Charge separation at nanoscale interfaces: energy-level alignment including two-quasiparticle interactions.

PubMed

Li, Huashan; Lin, Zhibin; Lusk, Mark T; Wu, Zhigang

2014-10-21

The universal and fundamental criteria for charge separation at interfaces involving nanoscale materials are investigated. In addition to the single-quasiparticle excitation, all the two-quasiparticle effects including exciton binding, Coulomb stabilization, and exciton transfer are considered, which play critical roles on nanoscale interfaces for optoelectronic applications. We propose a scheme allowing adding these two-quasiparticle interactions on top of the single-quasiparticle energy level alignment for determining and illuminating charge separation at nanoscale interfaces. Employing the many-body perturbation theory based on Green's functions, we quantitatively demonstrate that neglecting or simplifying these crucial two-quasiparticle interactions using less accurate methods is likely to predict qualitatively incorrect charge separation behaviors at nanoscale interfaces where quantum confinement dominates.

Tribo-charging properties of waste plastic granules in process of tribo-electrostatic separation.

PubMed

Li, Jia; Wu, Guiqing; Xu, Zhenming

2015-01-01

Plastic products can be found everywhere in people's daily life. With the consistent growth of plastic consumption, more and more plastic waste is generated. Considering the stable chemical and physics characteristics of plastic, regular waste management methods are not suitable for recycling economic strategy of each government, which has become a serious environmental problem. Recycling plastic waste is considered to be the best way to treat it, because it cannot only deduce the waste but also save the energy to produce new virgin plastic. Tribo-electrostatic separation is strongly recommended for plastic separation as it can preserve the original properties of plastic and has little additional pollution. In this study, plastic granules are generated by crushing plastic waste in waste electric and electronic equipment. The tribo-charging properties of plastic waste were studied by vibrating tribo-charging and cyclone tribo-charging. The triboelectric series obtained by vibrating was: (-)-PE-PS-PC-PVC-ABS-PP-(+), while the triboelectric series obtained by cyclone was (-)-PE-PS-PC-PVC-ABS-PP-(+). Further, the cyclone charging was more effective and stable than vibrating charging. The impact factors experiments showed that small particle size was better changed than large ones and were more suitable recycled by tribo-electrostatic separation. High relative humidity was identified as impede charging effect. The results of this study will help defining the operating parameters of subsequent separator. Copyright © 2014 Elsevier Ltd. All rights reserved.

Trypsin treatment of reaction centers from Rhodobacter sphaeroides in the dark and under illumination: protein structural changes follow charge separation.

PubMed

Brzezinski, P; Andréasson, L E

1995-06-06

Reaction centers from Rhodobacter sphaeroides R-26 were treated with trypsin in the dark and during illumination (in the charge-separated state). Trypsination resulted in a time-dependent modification of the reaction centers, reflected in changes in the charge recombination rate, in the inhibition of QA- to QB electron transfer, and eventually to inhibition of charge separation. Comparisons of centers with ubiquinone or anthraquinone in the QA site, in which the charge recombination pathways are different, indicate that trypsination affects charges close to the QA(-)-binding site. Studies of light-induced voltage changes from moving charges in reaction centers incorporated in lipid layers on a Teflon film, a technique which allows the discrimination of effects on donor and acceptor sides, indicate that the acceptor side is preferentially degraded by trypsin in the dark. Tryptic digestion during illumination generally resulted in a marked strengthening and acceleration of the effects seen already during dark treatment, but new effects were also detected in gel electrophoretic peptide patterns, in optical spectra, and in the kinetic measurements. Optical kinetic measurements revealed that the donor side of the reaction centers became susceptible to modification by trypsin during illumination as seen in the value of the binding constant for soluble cytochrome c2 which increased by a factor of 2, whereas it was much less affected after trypsination of reaction centers in the dark. The influence of illumination on the rate and mode by which trypsin acts on reaction centers indicates that changes in the protein conformation follow charge separation.(ABSTRACT TRUNCATED AT 250 WORDS)

Directional charge separation in isolated organic semiconductor crystalline nanowires

DOE PAGES

Labastide, J. A.; Thompson, H. B.; Marques, S. R.; ...

2016-02-25

One of the fundamental design paradigms in organic photovoltaic device engineering is based on the idea that charge separation is an extrinsically driven process requiring an interface for exciton fission. This idea has driven an enormous materials science engineering effort focused on construction of domain sizes commensurate with a nominal exciton diffusion length of order 10 nm. Here, we show that polarized optical excitation of isolated pristine crystalline nanowires of a small molecule n-type organic semiconductor, 7,8,15,16-tetraazaterrylene, generates a significant population of charge-separated polaron pairs along the π-stacking direction. Charge separation was signalled by pronounced power-law photoluminescence decay polarized alongmore » the same axis. In the transverse direction, we observed exponential decay associated with excitons localized on individual monomers. We propose that this effect derives from an intrinsic directional charge-transfer interaction that can ultimately be programmed by molecular packing geometry.« less

Multi-frequency inversion-charge pumping for charge separation and mobility analysis in high-k/InGaAs metal-oxide-semiconductor field-effect transistors

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

Djara, V.; Cherkaoui, K.; Negara, M. A.

2015-11-28

An alternative multi-frequency inversion-charge pumping (MFICP) technique was developed to directly separate the inversion charge density (N{sub inv}) from the trapped charge density in high-k/InGaAs metal-oxide-semiconductor field-effect transistors (MOSFETs). This approach relies on the fitting of the frequency response of border traps, obtained from inversion-charge pumping measurements performed over a wide range of frequencies at room temperature on a single MOSFET, using a modified charge trapping model. The obtained model yielded the capture time constant and density of border traps located at energy levels aligned with the InGaAs conduction band. Moreover, the combination of MFICP and pulsed I{sub d}-V{sub g}more » measurements enabled an accurate effective mobility vs N{sub inv} extraction and analysis. The data obtained using the MFICP approach are consistent with the most recent reports on high-k/InGaAs.« less

The effect of cosmic rays on thunderstorm electricity

NASA Technical Reports Server (NTRS)

Bragin, Y. A.

1975-01-01

The inflow of charges of small ions, formed by cosmic rays, into thunderstorm cells is estimated on the basis of rocket measurements of ionic concentrations below 90 km. Out of the two processes that form the thunderstorm charge (generation and separation of charges), the former is supposed to be caused by cosmic rays, and the nature of separation is assumed to be the same as in other thunderstorm theories.

Ewald Electrostatics for Mixtures of Point and Continuous Line Charges.

PubMed

Antila, Hanne S; Tassel, Paul R Van; Sammalkorpi, Maria

2015-10-15

Many charged macro- or supramolecular systems, such as DNA, are approximately rod-shaped and, to the lowest order, may be treated as continuous line charges. However, the standard method used to calculate electrostatics in molecular simulation, the Ewald summation, is designed to treat systems of point charges. We extend the Ewald concept to a hybrid system containing both point charges and continuous line charges. We find the calculated force between a point charge and (i) a continuous line charge and (ii) a discrete line charge consisting of uniformly spaced point charges to be numerically equivalent when the separation greatly exceeds the discretization length. At shorter separations, discretization induces deviations in the force and energy, and point charge-point charge correlation effects. Because significant computational savings are also possible, the continuous line charge Ewald method presented here offers the possibility of accurate and efficient electrostatic calculations.

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

Motion-based, high-yielding, and fast separation of different charged organics in water.

PubMed

Xuan, Mingjun; Lin, Xiankun; Shao, Jingxin; Dai, Luru; He, Qiang

2015-01-12

We report a self-propelled Janus silica micromotor as a motion-based analytical method for achieving fast target separation of polyelectrolyte microcapsules, enriching different charged organics with low molecular weights in water. The self-propelled Janus silica micromotor catalytically decomposes a hydrogen peroxide fuel and moves along the direction of the catalyst face at a speed of 126.3 μm s(-1) . Biotin-functionalized Janus micromotors can specifically capture and rapidly transport streptavidin-modified polyelectrolyte multilayer capsules, which could effectively enrich and separate different charged organics in water. The interior of the polyelectrolyte multilayer microcapsules were filled with a strong charged polyelectrolyte, and thus a Donnan equilibrium is favorable between the inner solution within the capsules and the bulk solution to entrap oppositely charged organics in water. The integration of these self-propelled Janus silica micromotors and polyelectrolyte multilayer capsules into a lab-on-chip device that enables the separation and analysis of charged organics could be attractive for a diverse range of applications. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Promoting Charge Separation and Injection by Optimizing the Interfaces of GaN:ZnO Photoanode for Efficient Solar Water Oxidation.

PubMed

Wang, Zhiliang; Zong, Xu; Gao, Yuying; Han, Jingfeng; Xu, Zhiqiang; Li, Zheng; Ding, Chunmei; Wang, Shengyang; Li, Can

2017-09-13

Photoelectrochemical water splitting provides an attractive way to store solar energy in molecular hydrogen as a kind of sustainable fuel. To achieve high solar conversion efficiency, the most stringent criteria are effective charge separation and injection in electrodes. Herein, efficient photoelectrochemical water oxidation is realized by optimizing charge separation and surface charge transfer of GaN:ZnO photoanode. The charge separation can be greatly improved through modified moisture-assisted nitridation and HCl acid treatment, by which the interfaces in GaN:ZnO solid solution particles are optimized and recombination centers existing at the interfaces are depressed in GaN:ZnO photoanode. Moreover, a multimetal phosphide of NiCoFeP was employed as water oxidation cocatalyst to improve the charge injection at the photoanode/electrolyte interface. Consequently, it significantly decreases the overpotential and brings the photocurrent to a benchmark of 3.9 mA cm -2 at 1.23 V vs RHE and a solar conversion efficiency over 1% was obtained.

The impact of long-range electron-hole interaction on the charge separation yield of molecular photocells

NASA Astrophysics Data System (ADS)

Nemati Aram, Tahereh; Ernzerhof, Matthias; Asgari, Asghar; Mayou, Didier

2017-01-01

We discuss the effects of charge carrier interaction and recombination on the operation of molecular photocells. Molecular photocells are devices where the energy conversion process takes place in a single molecular donor-acceptor complex attached to electrodes. Our investigation is based on the quantum scattering theory, in particular on the Lippmann-Schwinger equation; this minimizes the complexity of the problem while providing useful and non-trivial insight into the mechanism governing photocell operation. In this study, both exciton pair creation and dissociation are treated in the energy domain, and therefore there is access to detailed spectral information, which can be used as a framework to interpret the charge separation yield. We demonstrate that the charge carrier separation is a complex process that is affected by different parameters, such as the strength of the electron-hole interaction and the non-radiative recombination rate. Our analysis helps to optimize the charge separation process and the energy transfer in organic solar cells and in molecular photocells.

Separating large microscale particles by exploiting charge differences with dielectrophoresis.

PubMed

Polniak, Danielle V; Goodrich, Eric; Hill, Nicole; Lapizco-Encinas, Blanca H

2018-04-13

Dielectrophoresis (DEP), the migration of particles due to polarization effects under the influence of a nonuniform electric field, was employed for characterizing the behavior and achieving the separation of larger (diameter >5 μm) microparticles by exploiting differences in electrical charge. Usually, electrophoresis (EP) is the method of choice for separating particles based on differences in electrical charge; however, larger particles, which have low electrophoretic mobilities, cannot be easily separated with EP-based techniques. This study presents an alternative for the characterization, assessment, and separation of larger microparticles, where charge differences are exploited with DEP instead of EP. Polystyrene microparticles with sizes varying from 5 to 10 μm were characterized employing microdevices for insulator-based dielectrophoresis (iDEP). Particles within an iDEP microchannel were exposed simultaneously to DEP, EP, and electroosmotic (EO) forces. The electrokinetic behavior of four distinct types of microparticles was carefully characterized by means of velocimetry and dielectrophoretic capture assessments. As a final step, a dielectropherogram separation of two distinct types of 10 μm particles was devised by first characterizing the particles and then performing the separation. The two types of 10 μm particles were eluted from the iDEP device as two separate peaks of enriched particles in less than 80 s. It was demonstrated that particles with the same size, shape, surface functionalization, and made from the same bulk material can be separated with iDEP by exploiting slight differences in the magnitude of particle charge. The results from this study open the possibility for iDEP to be used as a technique for the assessment and separation of biological cells that have very similar characteristics (shape, size, similar make-up), but slight variance in surface electrical charge. Copyright © 2018 Elsevier B.V. All rights reserved.

Enhanced Internal Quantum Efficiency in Dye-Sensitized Solar Cells: Effect of Long-Lived Charge-Separated State of Sensitizers.

PubMed

Sun, Haiya; Liu, Dongzhi; Wang, Tianyang; Lu, Ting; Li, Wei; Ren, Siyao; Hu, Wenping; Wang, Lichang; Zhou, Xueqin

2017-03-22

Effective charge separation is one of the key determinants for the photovoltaic performance of the dye-sensitized solar cells (DSSCs). Herein, two charge-separated (CS) sensitizers, MTPA-Pyc and YD-Pyc, have been synthesized and applied in DSSCs to investigate the effect of the CS states of the sensitizers on the device's efficiency. The CS states with lifetimes of 64 and 177 ns for MTPA-Pyc and YD-Pyc, respectively, are formed via the photoinduced electron transfer (PET) from the 4-styryltriphenylamine (MTPA) or 4-styrylindoline (YD) donor to the pyrimidine cyanoacrylic acid (Pyc) acceptor. DSSCs based on MTPA-Pyc and YD-Pyc exhibit high internal quantum efficiency (IQE) values of over 80% from 400 to 600 nm. In comparison, the IQEs of the charge transfer (CT) sensitizer cells are 10-30% lower in the same wavelength range. The enhanced IQE values in the devices based on the CS sensitizers are ascribed to the higher electron injection efficiencies and slower charge recombination. The results demonstrate that taking advantage of the CS states in the sensitizers can be a promising strategy to improve the IQEs and further enhance the overall efficiencies of the DSSCs.

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

Enhanced charge separation of rutile TiO2 nanorods by trapping holes and transferring electrons for efficient cocatalyst-free photocatalytic conversion of CO2 to fuels.

PubMed

Wu, Jing; Lu, Hongwei; Zhang, Xuliang; Raziq, Fazal; Qu, Yang; Jing, Liqiang

2016-04-11

Modification with chloride and phosphate anions, and coupling with carbon nanotubes could effectively trap holes and transfer the electrons of rutile nanorods, respectively, so as to greatly promote photogenerated charge separation, leading to an obviously-improved cocatalyst-free photocatalytic conversion of CO2 to CH4 and CO, along with the positive effects of constructed phosphate bridges.

Strong coupling electrostatics for randomly charged surfaces: antifragility and effective interactions.

PubMed

Ghodrat, Malihe; Naji, Ali; Komaie-Moghaddam, Haniyeh; Podgornik, Rudolf

2015-05-07

We study the effective interaction mediated by strongly coupled Coulomb fluids between dielectric surfaces carrying quenched, random monopolar charges with equal mean and variance, both when the Coulomb fluid consists only of mobile multivalent counterions and when it consists of an asymmetric ionic mixture containing multivalent and monovalent (salt) ions in equilibrium with an aqueous bulk reservoir. We analyze the consequences that follow from the interplay between surface charge disorder, dielectric and salt image effects, and the strong electrostatic coupling that results from multivalent counterions on the distribution of these ions and the effective interaction pressure they mediate between the surfaces. In a dielectrically homogeneous system, we show that the multivalent counterions are attracted towards the surfaces with a singular, disorder-induced potential that diverges logarithmically on approach to the surfaces, creating a singular but integrable counterion density profile that exhibits an algebraic divergence at the surfaces with an exponent that depends on the surface charge (disorder) variance. This effect drives the system towards a state of lower thermal 'disorder', one that can be described by a renormalized temperature, exhibiting thus a remarkable antifragility. In the presence of an interfacial dielectric discontinuity, the singular behavior of counterion density at the surfaces is removed but multivalent counterions are still accumulated much more strongly close to randomly charged surfaces as compared with uniformly charged ones. The interaction pressure acting on the surfaces displays in general a highly non-monotonic behavior as a function of the inter-surface separation with a prominent regime of attraction at small to intermediate separations. This attraction is caused directly by the combined effects from charge disorder and strong coupling electrostatics of multivalent counterions, which dominate the surface-surface repulsion due to the (equal) mean charges on the two surfaces and the osmotic pressure of monovalent ions residing between them. These effects can be quite significant even with a small degree of surface charge disorder relative to the mean surface charge. The strong coupling, disorder-induced attraction is typically much stronger than the van der Waals interaction between the surfaces, especially within a range of several nanometers for the inter-surface separation, where such effects are predicted to be most pronounced.

Charge Weld Effects on High Cycle Fatigue Behavior of a Hollow Extruded AA6082 Profile

NASA Astrophysics Data System (ADS)

Nanninga, N.; White, C.; Dickson, R.

2011-10-01

Fatigue properties of specimens taken from different locations along the length of a hollow AA6082 extrusion, where charge weld (interface between successive billets in multi-billet extrusions) properties and the degree of coring (accumulation of highly sheared billet surface material at back end of billet) are expected to vary, have been evaluated. The fatigue strength of transverse specimens containing charge welds is lower near the front of the extrusion where the charge weld separation is relatively large. The relationship between fatigue failure and charge weld separation appears to be directly related to charge weld properties. The lower fatigue properties of the specimens are likely associated with early overload fatigue failure along the charge weld interface. Coring does not appear to have significantly affected fatigue behavior.

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.

Foam separation of Rhodamine-G and Evans Blue using a simple separatory bottle system.

PubMed

Dasarathy, Dhweeja; Ito, Yoichiro

2017-09-29

A simple separatory glass bottle was used to improve separation effectiveness and cost efficiency while simultaneously creating a simpler system for separating biological compounds. Additionally, it was important to develop a scalable separation method so this would be applicable to both analytical and preparative separations. Compared to conventional foam separation methods, this method easily forms stable dry foam which ensures high purity of yielded fractions. A negatively charged surfactant, sodium dodecyl sulfate (SDS), was used as the ligand to carry a positively charged Rhodamine-G, leaving a negatively charged Evans Blue in the bottle. The performance of the separatory bottle was tested for separating Rhodamine-G from Evans Blue with sample sizes ranged from 1 to 12mg in preparative separations and 1-20μg in analytical separations under optimum conditions. These conditions including N 2 gas pressure, spinning speed of contents with a magnetic stirrer, concentration of the ligand, volume of the solvent, and concentration of the sample, were all modified and optimized. Based on the calculations at their peak absorbances, Rhodamine-G and Evans Blue were efficiently separated in times ranging from 1h to 3h, depending on sample volume. Optimal conditions were found to be 60psi N 2 pressure and 2mM SDS for the affinity ligand. This novel separation method will allow for rapid separation of biological compounds while simultaneously being scalable and cost effective. Published by Elsevier B.V.

Poisson-Boltzmann theory of the charge-induced adsorption of semi-flexible polyelectrolytes.

PubMed

Ubbink, Job; Khokhlov, Alexei R

2004-03-15

A model is suggested for the structure of an adsorbed layer of a highly charged semi-flexible polyelectrolyte on a weakly charged surface of opposite charge sign. The adsorbed phase is thin, owing to the effective reversal of the charge sign of the surface upon adsorption, and ordered, owing to the high surface density of polyelectrolyte strands caused by the generally strong binding between polyelectrolyte and surface. The Poisson-Boltzmann equation for the electrostatic interaction between the array of adsorbed polyelectrolytes and the charged surface is solved for a cylindrical geometry, both numerically, using a finite element method, and analytically within the weak curvature limit under the assumption of excess monovalent salt. For small separations, repulsive surface polarization and counterion osmotic pressure effects dominate over the electrostatic attraction and the resulting electrostatic interaction curve shows a minimum at nonzero separations on the Angstrom scale. The equilibrium density of the adsorbed phase is obtained by minimizing the total free energy under the condition of equality of chemical potential and osmotic pressure of the polyelectrolyte in solution and in the adsorbed phase. For a wide range of ionic conditions and charge densities of the charged surface, the interstrand separation as predicted by the Poisson-Boltzmann model and the analytical theory closely agree. For low to moderate charge densities of the adsorbing surface, the interstrand spacing decreases as a function of the charge density of the charged surface. Above about 0.1 M excess monovalent salt, it is only weakly dependent on the ionic strength. At high charge densities of the adsorbing surface, the interstrand spacing increases with increasing ionic strength, in line with the experiments by Fang and Yang [J. Phys. Chem. B 101, 441 (1997)]. (c) 2004 American Institute of Physics.

Disentangling flow and signals of Chiral Magnetic Effect in U+U, Au+Au and p+Au collisions

NASA Astrophysics Data System (ADS)

Tribedy, Prithwish; STAR Collaboration

2017-11-01

We present STAR measurements of the charge-dependent three-particle correlator γ a , b = 〈 cos ⁡ (ϕ1a + ϕ2b - 2ϕ3) 〉 /v2 { 2 } and elliptic flow v2 { 2 } in U+U, Au+Au and p+Au collisions at RHIC. The difference Δγ = γ (opposite-sign) - γ (same-sign) measures charge separation across the reaction plane, a predicted signal of the Chiral Magnetic Effect (CME). Although charge separation has been observed, it has been argued that the measured separation can also be explained by elliptic flow related backgrounds. In order to separate the two effects we perform measurements of the γ-correlator where background expectations differ from magnetic field driven effects. A differential measurement of γ with the relative pseudorapidity (Δη) between the first and second particles indicate that Δγ in peripheral A+A and p+A collisions are dominated by short-range correlations in Δη. However, a relatively wider component of the correlation in Δη tends to vanish the same way as projected magnetic field as predicted by MC-Glauber simulations.

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.

Method development of enantiomer separations by affinity capillary electrophoresis, cyclodextrin electrokinetic chromatography and capillary electrophoresis-mass spectrometry.

PubMed

Tanaka, Yoshihide

2002-07-01

Capillary electrophoresis (CE) has become a powerful tool for enantiomer separations during the last decade. Since 1993, the author has investigated enantiomer separations by affinity capillary electrophoresis (affinity CE) with some proteins and by cyclodextrin electrokinetic chromatography (CDEKC) with some charged cyclodextrins (CDs). Many successful enantiomer separations are demonstrated from our study in this review article. In the enantiomer separations by affinity CE, the deterioration of detection sensitivity was observed under high concentration of the protein in running solutions. The partial filling technique was practically useful to solve the serious problem. It allowed operation at high protein concentrations, such as 500 mumol/L, without the detection problem. Charged CDs had several advantages for the enantiomer separations over neutral ones. Strong electrostatic interactions between a charged CD and oppositely charged analytes should be effective for the formation of the complex. A large difference in electrophoretic mobility between the free analyte and the inclusion complex should also enhance the enantiomeric resolution. In CE-mass spectrometry (CE-MS), the partial filling technique was applied to avoid the introduction of nonvolatile chiral selectors into the CE-MS interface. By replacing the nonvolatile electrolytes in the running buffer by volatile ones, the separation conditions employed in CE with the UV detection method could be transferred to CE-MS.

Effect of interstitial palladium on plasmon-driven charge transfer in nanoparticle dimers.

PubMed

Lerch, Sarah; Reinhard, Björn M

2018-04-23

Capacitive plasmon coupling between noble metal nanoparticles (NPs) is characterized by an increasing red-shift of the bonding dipolar plasmon mode (BDP) in the classical electromagnetic coupling regime. This model breaks down at short separations where plasmon-driven charge transfer induces a gap current between the NPs with a magnitude and separation dependence that can be modulated if molecules are present in the gap. Here, we use gap contained DNA as a scaffold for the growth of palladium (Pd) NPs in the gap between two gold NPs and investigate the effect of increasing Pd NP concentration on the BDP mode. Consistent with enhanced plasmon-driven charge transfer, the integration of discrete Pd NPs depolarizes the capacitive BDP mode over longer interparticle separations than is possible in only DNA-linked Au NPs. High Pd NP densities in the gap increases the gap conductance and induces the transition from capacitive to conductive coupling.

Effective Coulomb force modeling for spacecraft in Earth orbit plasmas

NASA Astrophysics Data System (ADS)

Seubert, Carl R.; Stiles, Laura A.; Schaub, Hanspeter

2014-07-01

Coulomb formation flight is a concept that utilizes electrostatic forces to control the separations of close proximity spacecraft. The Coulomb force between charged bodies is a product of their size, separation, potential and interaction with the local plasma environment. A fast and accurate analytic method of capturing the interaction of a charged body in a plasma is shown. The Debye-Hückel analytic model of the electrostatic field about a charged sphere in a plasma is expanded to analytically compute the forces. This model is fitted to numerical simulations with representative geosynchronous and low Earth orbit (GEO and LEO) plasma environments using an effective Debye length. This effective Debye length, which more accurately captures the charge partial shielding, can be up to 7 times larger at GEO, and as great as 100 times larger at LEO. The force between a sphere and point charge is accurately captured with the effective Debye length, as opposed to the electron Debye length solutions that have errors exceeding 50%. One notable finding is that the effective Debye lengths in LEO plasmas about a charged body are increased from centimeters to meters. This is a promising outcome, as the reduced shielding at increased potentials provides sufficient force levels for operating the electrostatically inflated membrane structures concept at these dense plasma altitudes.

Fast charge separation in a non-fullerene organic solar cell with a small driving force

NASA Astrophysics Data System (ADS)

Liu, Jing; Chen, Shangshang; Qian, Deping; Gautam, Bhoj; Yang, Guofang; Zhao, Jingbo; Bergqvist, Jonas; Zhang, Fengling; Ma, Wei; Ade, Harald; Inganäs, Olle; Gundogdu, Kenan; Gao, Feng; Yan, He

2016-07-01

Fast and efficient charge separation is essential to achieve high power conversion efficiency in organic solar cells (OSCs). In state-of-the-art OSCs, this is usually achieved by a significant driving force, defined as the offset between the bandgap (Egap) of the donor/acceptor materials and the energy of the charge transfer (CT) state (ECT), which is typically greater than 0.3 eV. The large driving force causes a relatively large voltage loss that hinders performance. Here, we report non-fullerene OSCs that exhibit ultrafast and efficient charge separation despite a negligible driving force, as ECT is nearly identical to Egap. Moreover, the small driving force is found to have minimal detrimental effects on charge transfer dynamics of the OSCs. We demonstrate a non-fullerene OSC with 9.5% efficiency and nearly 90% internal quantum efficiency despite a low voltage loss of 0.61 V. This creates a path towards highly efficient OSCs with a low voltage loss.

Greatly Increasing Trapped Ion Populations for Mobility Separations Using Traveling Waves in Structures for Lossless Ion Manipulations

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

Deng, Liulin; Ibrahim, Yehia M.; Garimella, Sandilya V. B.

The initial use of traveling waves (TW) for ion mobility (IM) separations using a structures for lossless ion manipulations (SLIM) employed an ion funnel trap (IFT) to accumulate ions from a continuous electrospray ionization source, and limited to injected ion populations of ~106 charges due to the onset of space charge effects in the trapping region. Additional limitations arise due to the loss of resolution for the injection of ions over longer periods (e.g. in extended pulses). In this work a new SLIM ‘flat funnel’ (FF) module has been developed and demonstrated to enable the accumulation of much larger ionmore » populations and their injection for IM separations. Ion current measurements indicate a capacity of ~3.2×108 charges for the extended trapping volume, over an order of magnitude greater than the IFT. The orthogonal ion injection into a funnel shaped separation region can greatly reduce space charge effects during the initial IM separation stage, and the gradually reduced width of the path allows the ion packet to be increasingly compressed in the lateral dimension as the separation progresses, allowing e.g. efficient transmission through conductance limits or compatibility with subsequent ion manipulations. This work examined the TW, RF, and DC confining field SLIM parameters involved in ion accumulation, injection, transmission and separation in the FF IM module using both direct ion current and MS measurements. Wide m/z range ion transmission is demonstrated, along with significant increases in signal to noise (S/N) ratios due to the larger ion populations injected. Additionally, we observed a reduction in the chemical background, which was attributed to more efficient desolvation of solvent related clusters over the extended ion accumulation periods. The TW SLIM FF IM module is anticipated to be especially effective as a front end for long path SLIM IM separation modules.« less

Use of cationic polymers to reduce pathogen levels during dairy manure separation.

PubMed

Liu, Zong; Carroll, Zachary S; Long, Sharon C; Gunasekaran, Sundaram; Runge, Troy

2016-01-15

Various separation technologies are used to deal with the enormous amounts of animal waste that large livestock operations generate. When the recycled waste stream is land applied, it is essential to lower the pathogen load to safeguard the health of livestock and humans. We investigated whether cationic polymers, used as a flocculent in the solid/liquid separation process, could reduce the pathogen indicator load in the animal waste stream. The effects of low charge density cationic polyacrylamide (CPAM) and high charge density cationic polydicyandiamide (PDCD) were investigated. Results demonstrated that CPAM was more effective than PDCD for manure coagulation and flocculation, while PDCD was more effective than CPAM in reducing the pathogen indicator loads. However, their combined use, CPAM followed by PDCD, resulted in both improved solids separation and pathogen indicator reduction. Copyright © 2015 The Authors. Published by Elsevier Ltd.. All rights reserved.

Capillary electrophoresis electrospray ionization mass spectrometry interface

DOEpatents

Smith, Richard D.; Severs, Joanne C.

1999-01-01

The present invention is an interface between a capillary electrophoresis separation capillary end and an electrospray ionization mass spectrometry emitter capillary end, for transporting an anolyte sample from a capillary electrophoresis separation capillary to a electrospray ionization mass spectrometry emitter capillary. The interface of the present invention has: (a) a charge transfer fitting enclosing both of the capillary electrophoresis capillary end and the electrospray ionization mass spectrometry emitter capillary end; (b) a reservoir containing an electrolyte surrounding the charge transfer fitting; and (c) an electrode immersed into the electrolyte, the electrode closing a capillary electrophoresis circuit and providing charge transfer across the charge transfer fitting while avoiding substantial bulk fluid transfer across the charge transfer fitting. Advantages of the present invention have been demonstrated as effective in providing high sensitivity and efficient analyses.

A more than six orders of magnitude UV-responsive organic field-effect transistor utilizing a benzothiophene semiconductor and Disperse Red 1 for enhanced charge separation.

PubMed

Smithson, Chad S; Wu, Yiliang; Wigglesworth, Tony; Zhu, Shiping

2015-01-14

A more than six orders of magnitude UV-responsive organic field-effect transistor is developed using a benzothiophene (BTBT) semiconductor and strong donor-acceptor Disperse Red 1 as the traps to enhance charge separation. The device can be returned to its low drain current state by applying a short gate bias, and is completely reversible with excellent stability under ambient conditions. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The Charging Events in Contact-Separation Electrification.

PubMed

Musa, Umar G; Cezan, S Doruk; Baytekin, Bilge; Baytekin, H Tarik

2018-02-06

Contact electrification (CE)-charging of surfaces that are contacted and separated, is a common phenomenon, however it is not completely understood yet. Recent studies using surface imaging techniques and chemical analysis revealed a 'spatial' bipolar distribution of charges at the nano dimension, which made a paradigm shift in the field. However, such analyses can only provide information about the charges that remained on the surface after the separation, providing limited information about the actual course of the CE event. Tapping common polymers and metal surfaces to each other and detecting the electrical potential produced on these surfaces 'in-situ' in individual events of contact and separation, we show that, charges are generated and transferred between the surfaces in both events; the measured potential is bipolar in contact and unipolar in separation. We show, the 'contact-charges' on the surfaces are indeed the net charges that results after the separation process, and a large contribution to tribocharge harvesting comes, in fact, from the electrostatic induction resulting from the generated CE charges. Our results refine the mechanism of CE providing information for rethinking the conventional ranking of materials' charging abilities, charge harvesting, and charge prevention.

Control of gel swelling and phase separation of weakly charged thermoreversible gels by salt addition

PubMed Central

Solis, Francisco J.; Vernon, Brent

2009-01-01

Doping of thermoreversible polymer gels with charged monomers provides a way to control phase separation and gelation conditions by coupling the properties of the gel with a tunable ionic environment. We analyze the dependence of the gelation and phase separation conditions on the amount of salt present using a mean field model of weakly charged associative polymers. The ions and co-ions present are explicitly considered at the mean field level, and we determine their concentrations in the different equilibrium phases when the system undergoes phase separation. For weak polymer charge, the entropic contributions of the ions to the free energy of the system play a central role in the determination of the location of phase equilibrium. In the simplest case, when the associative interaction responsible for gel formation is independent of the electrostatic interaction, the addition of salt changes the polymer equilibrium concentrations and indirectly changes the measurable swelling of the gel. We construct phase diagrams of these systems showing the location of the coexistence region, the gel-sol boundary and the location of the tie-lines. We determine the swelling of the gel within the co-existence region. Our main result is that the description of the effect of the salt on the properties of the weakly charged gel can be described through an extra contribution to the effective immiscibility parameter χ proportional to the square of the doping degree f2 and to the inverse square of the added salt concentration s−2. PMID:19759854

Charge and energy dynamics in photo-excited poly(para-phenylenevinylene) systems

NASA Astrophysics Data System (ADS)

Gisslén, L.; Johansson, A.˚.; Stafström, S.

2004-07-01

We report results from simulations of charge and energy dynamics in poly(para-phenylenevinylene) (PPV) and PPV interacting with C60. The simulations were performed by solving the time-dependent Schrödinger equation and the lattice equation of motion simultaneously and nonadiabatically. The electronic system and the coupling of the electrons to the lattice were described by an extended three-dimensional version of the Su-Schrieffer-Heeger model, which also included an external electric field. Electron and lattice dynamics following electronic excitations at different energies have been simulated. The effect of additional lattice energy was also included in the simulations. Our results show that both exciton diffusion and transitions from high to lower lying excitations are stimulated by increasing the lattice energy. Also field induced charge separation occurs faster if the lattice energy is increased. This separation process is highly nonadiabatic and involves a significant rearrangement of the electron distribution. In the case of PPV coupled to C60, we observe a spontaneous charge separation. The separation time is in this case limited by the local concentration of C60 molecules close to the PPV chain.

Simulations to Predict the Phase Behavior and Structure of Multipolar Colloidal Particles

NASA Astrophysics Data System (ADS)

Rutkowski, David Matthew

Colloidal particles with anisotropic charge distributions can assemble into a number of interesting structures including chains, lattices and micelles that could be useful in biotechnology, optics and electronics. The goal of this work is to understand how the properties of the colloidal particles, such as their charge distribution or shape, affect the selfassembly and phase behavior of collections of such particles. The specific aim of this work is to understand how the separation between a pair of oppositely signed charges affects the phase behavior and structure of assemblies of colloidal particles. To examine these particles, we have used both discontinuous molecular dynamics (DMD) and Monte Carlo (MC) simulation techniques. In our first study of colloidal particles with finite charge separation, we simulate systems of 2-D colloidal rods with four possible charge separations. Our simulations show that the charge separation does indeed have a large effect on the phase behavior as can be seen in the phase diagrams we construct for these four systems in the area fraction-reduced temperature plane. The phase diagrams delineate the boundaries between isotropic fluid, string-fluid and percolated fluid for all systems considered. In particular, we find that coarse gel-like structures tend to form at large charge separations while denser aggregates form at small charge separations, suggesting a route to forming low volume gels by focusing on systems with large charge separations. Next we examine systems of circular particles with four embedded charges of alternating sign fixed to a triangular lattice. This system is found to form a limit periodic structure, a theoretical structure with an infinite number of phase transitions, under specific conditions. The limit-periodic structure only forms when the rotation of the particles in the system is restricted to increments of pi/3. When the rotation is restricted to increments of th/6 or the rotation is continuous, related structures form including a striped phase and a phase with nematic order. Neither the distance from the point charges to the center of the particle nor the angle between the charges influences whether the system forms a limit-periodic structure, suggesting that point quadrupoles may also be able to form limit-periodic structures. Results from these simulations will likely aid in the quest to find an experimental realization of a limit-periodic structure. Next we examine the effect of charge separation on the self-assembly of systems of 2-D colloidal particles with off-center extended dipoles. We simulate systems with both small and large charge separations for a set of displacements of the dipole from the particle center. Upon cooling, these particles self-assemble into closed, cyclic structures at large displacements including dimers, triangular shapes and square shapes, and chain-like structures at small displacements. At extremely low temperatures, the cyclic structures form interesting lattices with particles of similar chirality grouped together. Results from this work could aid in the experimental construction of open lattice-like structures that could find use in photonic applications. Finally, we present work in collaboration with Drs. Bhuvnesh Bharti and Orlin Velev in which we investigate how the surface coverage affects the self-assembly of systems of Janus particles coated with both an iron oxide and fatty acid chain layer. We model these particles by decorating a sphere with evenly dispersed points that interact with points on other spheres through square-well interactions. The interactions are designed to mimic specific coverage values for the iron oxide/fatty acid chain layer. Structures similar to those found in experiment form readily in the simulations. The number of clusters formed as a function of surface coverage agrees well with experiment. The aggregation behavior of these novel particles can therefore, be described by a relatively simple model.

Event-shape-engineering study of charge separation in heavy-ion collisions

NASA Astrophysics Data System (ADS)

Wen, Fufang; Bryon, Jacob; Wen, Liwen; Wang, Gang

2018-01-01

Recent measurements of charge-dependent azimuthal correlations in high-energy heavy-ion collisions have indicated charge-separation signals perpendicular to the reaction plane, and have been related to the chiral magnetic effect (CME). However, the correlation signal is contaminated with the background caused by the collective motion (flow) of the collision system, and an effective approach is needed to remove the flow background from the correlation. We present a method study with simplified Monte Carlo simulations and a multi-phase transport model, and develop a scheme to reveal the true CME signal via event-shape engineering with the flow vector of the particles of interest. Supported by a grant (DE-FG02-88ER40424) from U.S. Department of Energy, Office of Nuclear Physics

Separation of Albumin, Ceruloplasmin, and Transferrin from Human Plasma.

ERIC Educational Resources Information Center

Barnes, Grady; Frieden, Earl

1982-01-01

Procedures are provided for separating the principal metalloproteins (albumin, ceruloplasmin, and transferrin) from plasma using column chromatographic techniques. The experiment can be completed in two separate three-hour laboratory periods during which column chromatography is illustrated and the effect of pH on charge and affinity of a protein…

Ion transport restriction in mechanically strained separator membranes

NASA Astrophysics Data System (ADS)

Cannarella, John; Arnold, Craig B.

2013-03-01

We use AC impedance methods to investigate the effect of mechanical deformation on ion transport in commercial separator membranes and lithium-ion cells as a whole. A Bruggeman type power law relationship is found to provide an accurate correlation between porosity and tortuosity of deformed separators, which allows the impedance of a separator membrane to be predicted as a function of deformation. By using mechanical compression to vary the porosity of the separator membranes during impedance measurements it is possible to determine both the α and γ parameters from the modified Bruggeman relation for individual separator membranes. From impedance testing of compressed pouch cells it is found that separator deformation accounts for the majority of the transport restrictions arising from compressive stress in a lithium-ion cell. Finally, a charge state dependent increase in the impedance associated with charge transfer is observed with increasing cell compression.

The impact of chemical structure and molecular packing on the electronic polarisation of fullerene arrays.

PubMed

Few, Sheridan; Chia, Cleaven; Teo, Daniel; Kirkpatrick, James; Nelson, Jenny

2017-07-19

Electronic polarisation contributes to the electronic landscape as seen by separating charges in organic materials. The nature of electronic polarisation depends on the polarisability, density, and arrangement of polarisable molecules. In this paper, we introduce a microscopic, coarse-grained model in which we treat each molecule as a polarisable site, and use an array of such polarisable dipoles to calculate the electric field and associated energy of any arrangement of charges in the medium. The model incorporates chemical structure via the molecular polarisability and molecular packing patterns via the structure of the array. We use this model to calculate energies of charge pairs undergoing separation in finite fullerene lattices of different chemical and crystal structures. The effective dielectric constants that we estimate from this approach are in good quantitative agreement with those measured experimentally in C 60 and phenyl-C 61 -butyric acid methyl ester (PCBM) films, but we find significant differences in dielectric constant depending on packing and on direction of separation, which we rationalise in terms of density of polarisable fullerene cages in regions of high field. In general, we find lattices containing molecules of more isotropic polarisability tensors exhibit higher dielectric constants. By exploring several model systems we conclude that differences in molecular polarisability (and therefore, chemical structure) appear to be less important than differences in molecular packing and separation direction in determining the energetic landscape for charge separation. We note that the results are relevant for finite lattices, but not necessarily for infinite systems. We propose that the model could be used to design molecular systems for effective electronic screening.

Capillary electrophoresis of covalently functionalized single-chirality carbon nanotubes.

PubMed

He, Pingli; Meany, Brendan; Wang, Chunyan; Piao, Yanmei; Kwon, Hyejin; Deng, Shunliu; Wang, YuHuang

2017-07-01

We demonstrate the separation of chirality-enriched single-walled carbon nanotubes (SWCNTs) by degree of surface functionalization using high-performance CE. Controlled amounts of negatively charged and positively charged functional groups were attached to the sidewall of chirality-enriched SWCNTs through covalent functionalization using 4-carboxybenzenediazonium tetrafluoroborate or 4-diazo-N,N-diethylaniline tetrafluoroborate, respectively. Surfactant- and pH-dependent studies confirmed that under conditions that minimized ionic screening effects, separation of these functionalized SWCNTs was strongly dependent on the surface charge density introduced through covalent surface chemistry. For both heterogeneous mixtures and single-chirality-enriched samples, covalently functionalized SWCNTs showed substantially increased peak width in electropherogram spectra compared to nonfunctionalized SWCNTs, which can be attributed to a distribution of surface charges along the functionalized nanotubes. Successful separation of functionalized single-chirality SWCNTs by functional density was confirmed with UV-Vis-NIR absorption and Raman scattering spectroscopies of fraction collected samples. These results suggest a high degree of structural heterogeneity in covalently functionalized SWCNTs, even for chirality-enriched samples, and show the feasibility of applying CE for high-performance separation of nanomaterials based on differences in surface functional density. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The effect of charged quantum dots on the mobility of a two-dimensional electron gas: How important is the Coulomb scattering?

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

Kurzmann, A., E-mail: annika.kurzmann@uni-due.de; Beckel, A.; Lorke, A.

2015-02-07

We have investigated the influence of a layer of charged self-assembled quantum dots (QDs) on the mobility of a nearby two-dimensional electron gas (2DEG). Time-resolved transconductance spectroscopy was used to separate the two contributions of the change in mobility, which are: (i) The electrons in the QDs act as Coulomb scatterers for the electrons in the 2DEG. (ii) The screening ability and, hence, the mobility of the 2DEG decreases when the charge carrier density is reduced by the charged QDs, i.e., the mobility itself depends on the charge carrier concentration. Surprisingly, we find a negligible influence of the Coulomb scatteringmore » on the mobility for a 2DEG, separated by a 30 nm tunneling barrier to the layer of QDs. This means that the mobility change is completely caused by depletion, i.e., reduction of the charge carrier density in the 2DEG, which indirectly influences the mobility.« less

Theory and practical understanding of the migration behavior of proteins and peptides in CE and related techniques.

PubMed

Freitag, Ruth; Hilbrig, Frank

2007-07-01

CEC is defined as an analytical method, where the analytes are separated on a chromatographic column in the presence of an applied voltage. The separation of charged analytes in CEC is complex, since chromatographic interaction, electroosmosis and electrophoresis contribute to the experimentally observed behavior. The putative contribution of effects such as surface electrodiffusion has been suggested. A sound theoretical treatment incorporating all effects is currently not available. The question of whether the different effects contribute in an independent or an interdependent manner is still under discussion. In this contribution, the state-of-the-art in the theoretical description of the individual contributions as well as models for the retention behavior and in particular possible dimensionless 'retention factors' is discussed, together with the experimental database for the separation of charged analytes, in particular proteins and peptides, by CEC and related techniques.

Modeling the Electric Potential and Surface Charge Density near Charged Thunderclouds

ERIC Educational Resources Information Center

Neel, Matthew Stephen

2018-01-01

Thundercloud charge separation, or the process by which the bottom portion of a cloud gathers charge and the top portion of the cloud gathers the opposite charge, is still not thoroughly understood. Whatever the mechanism, though, a charge separation definitely exists and can lead to electrostatic discharge via cloud-to-cloud lightning and…

Review on charge transfer and chemical activity of TiO2: Mechanism and applications

NASA Astrophysics Data System (ADS)

Cai, Yongqing; Feng, Yuan Ping

2016-12-01

Charge separation and transfer at the interface between two materials play a significant role in various atomic-scale processes and energy conversion systems. In this review, we present the mechanism and outcome of charge transfer in TiO2, which is extensively explored for photocatalytic applications in the field of environmental science. We list several experimental and computational methods to estimate the amount of charge transfer. The effects of the work function, defects and doping, and employment of external electric field on modulating the charge transfer are presented. The interplay between the band bending and carrier transport across the surface and interface consisting of TiO2 is discussed. We show that the charge transfer can also strongly affect the behavior of deposited nanoparticles on TiO2 through built-in electric field that it creates. This review encompasses several advances of composite materials where TiO2 is combined with two-dimensional materials like graphene, MoS2, phosphorene, etc. The charge transport in the TiO2-organohalide perovskite with respect to the electron-hole separation at the interface is also discussed.

Hexahedron Prism-Anchored Octahedronal CeO2: Crystal Facet-Based Homojunction Promoting Efficient Solar Fuel Synthesis.

PubMed

Li, Ping; Zhou, Yong; Zhao, Zongyan; Xu, Qinfeng; Wang, Xiaoyong; Xiao, Min; Zou, Zhigang

2015-08-05

An unprecedented, crystal facet-based CeO2 homojunction consisting of hexahedron prism-anchored octahedron with exposed prism surface of {100} facets and octahedron surface of {111} facets was fabricated through solution-based crystallographic-oriented epitaxial growth. The photocatalysis experiment reveals that growth of the prism arm on octahedron allows to activate inert CeO2 octahedron for an increase in phototocatalytic reduction of CO2 into methane. The pronounced photocatalytic performance is attributed to a synergistic effect of the following three factors: (1) band alignment of the {100} and {111} drives electrons and holes to octahedron and prism surfaces, respectively, aiming to reach the most stable energy configuration and leading to a spatial charge separation for long duration; (2) crystallographic-oriented epitaxial growth of the CeO2 hexahedron prism arm on the octahedron verified by the interfacial lattice fringe provides convenient and fast channels for the photogenerated carrier transportation between two units of homojuntion; (3) different effective mass of electrons and holes on {100} and {111} faces leads to high charge carrier mobility, more facilitating the charge separation. The proposed facet-based homojunction in this work may provide a new concept for the efficient separation and fast transfer of photoinduced charge carriers and enhancement of the photocatalytic performance.

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.

The influence of charge and the distribution of charge in the polar region of phospholipids on the activity of UDP-glucuronosyltransferase.

PubMed

Zakim, D; Eibl, H

1992-07-05

Studies of the mechanism of lipid-induced regulation of the microsomal enzyme UDP-glucuronosyltransferase have been extended by examining the influence of charge within the polar region on the ability of lipids to activate delipidated pure enzyme. The effects of net negative charge, of charge separation in phosphocholine, and of the distribution of charge in the polar region of lipids were studied using the GT2p isoform isolated from pig liver. Prior experiments have shown that lipids with net negative charge inhibit the enzyme (Zakim, D., Cantor, M., and Eibl, H. (1988) J. Biol. Chem. 263, 5164-5169). The current experiments show that the extent of inhibition on a molar basis increases as the net negative charge increases from -1 to -2. The inhibitory effect of negatively charged lipids is on the functional state of the enzyme and is not due to electrostatic repulsion of negatively charged substrates of the enzyme. Although the inhibitory effect of net negative charge is removed when negative charge is balanced by a positive charge due to a quaternary nitrogen, neutrality of the polar region is not a sufficient condition for activation of the enzyme. In addition to a balance of charge between Pi and the quaternary nitrogen, the distance between the negative and positive charges and the orientation of the dipole created by them are critical for activation of GT2p. The negative and positive charges must be separated by the equivalent of three -CH2- groups for optimal activation by a lipid. Shortening this distance by one -CH2- unit leads to a lipid that is ineffective in activating the enzyme. Reversal of the orientation of the dipole in which the negative charge is on the polymethylene side of the lipid-water interface and the positive charge extends into water also produces a lipid that is not effective for activating GT2p. On the other hand, lipids with phosphoserine as the polar region, which has the "normal" P-N distance but carries a net negative charge, do not inhibit GT2p. This result again illustrates the importance of the dipole of phosphocholine for modulating the functional state of GT2p.

Gate bias stress in pentacene field-effect-transistors: Charge trapping in the dielectric or semiconductor

NASA Astrophysics Data System (ADS)

Häusermann, R.; Batlogg, B.

2011-08-01

Gate bias stress instability in organic field-effect transistors (OFETs) is a major conceptual and device issue. This effect manifests itself by an undesirable shift of the transfer characteristics and is associated with long term charge trapping. We study the role of the dielectric and the semiconductor separately by producing OFETs with the same semiconductor (pentacene) combined with different dielectrics (SiO2 and Cytop). We show that it is possible to fabricate devices which are immune to gate bias stress. For other material combinations, charge trapping occurs in the semiconductor alone or in the dielectric.

Distinct exciton dissociation behavior of organolead trihalide perovskite and excitonic semiconductors studied in a same device

DOE PAGES

Hu, Miao; Bi, Cheng; Yuan, Yongbo; ...

2015-01-15

The nonexcitonic character for organometal trihalide perovskites is demonstrated by examining the field-dependent exciton dissociation behavior. Moreover, it is found that photogenerated excitons can be effectively dissociated into free charges inside perovskite without the assistance of charge extraction layer or external field, which is a stark contrast to the charge-separation behavior in excitonic materials in the same photovoltaic operation system.

Segregation in like-charged polyelectrolyte-surfactant mixtures can be precisely tuned via manipulation of the surfactant mass ratio.

PubMed

Wills, Peter W; Lopez, Sonia G; Burr, Jocelyn; Taboada, Pablo; Yeates, Stephen G

2013-04-09

In this study, we consider segregative phase separation in aqueous mixtures of quaternary ammonium surfactants didecyldimethylammonium chloride (DDQ) and alkyl (C12, 70%; C14 30%) dimethyl benzyl ammonium chloride (BAC) upon the addition of poly(diallyldimethylammonium) chloride (pDADMAC) as a function of both concentration and molecular weight. The nature of the surfactant type is dominant in determining the concentration at which separation into an upper essentially surfactant-rich phase and lower polyelectrolyte-rich phase is observed. However, for high-molecular-weight pDADMAC there is a clear indication of an additional depletion flocculation effect. When the BAC/DDQ ratio is tuned, the segregative phase separation point can be precisely controlled. We propose a phase separation mechanism for like-charged quaternary ammonium polyelectrolyte/surfactant/water mixtures induced by a reduction in the ionic atmosphere around the surfactant headgroup and possible ion pair formation. An additional polyelectrolyte-induced depletion flocculation effect was also observed.

Evaluation of newly synthesized and commercially available charged cyclomaltooligosaccharides (cyclodextrins) for capillary electrokinetic chromatography.

PubMed

Culha, Mustafa; Schell, Fred M; Fox, Shannon; Green, Thomas; Betts, Thomas; Sepaniak, Michael J

2004-01-22

A highly new charged cyclodextrin (CD) derivatives, (6-O-carboxymethyl-2,3-di-O-methyl)cyclomaltoheptaoses (CDM-beta-CDs), was synthesized and characterized as anionic reagents for capillary electrophoresis (CE) in an electrokinetic chromatography mode of separation. Substitution with dimethyl groups at the secondary hydroxyl sites of the CD is aimed at influencing the magnitude and selectivity of analyte-CD interactions, while substitution by carboxymethyl groups at the primary hydroxyl sites provides for high charge and electrophoretic mobility. Full regioselective methylation at the secondary hydroxyl sites was achieved in this work, while substitution at the primary hydroxyl sites generated a mixture of multiply charged products. The separation performance of CDM-beta-CD was evaluated using a variety of analyte mixtures. The results obtained from commercially available negatively charged cyclodextrins, heptakis(2,3-di-O-methyl-6-O-sulfo)cyclomaltoheptaose (HDMS-beta-CD) and O-(carboxymethyl)cyclomaltoheptaose (CM-beta-CD) with an average degree of substitution one (DS 1), were compared to CDM-beta-CD using a sample composed of eight positional isomers of dihydroxynaphthalene. Four hydroxylated polychlorobiphenyl derivatives, a group of chiral and isomeric catchecins, and chiral binaphthyl compounds were also separated with CDM-beta-CD. The effect of adding neutral beta-cyclodextrin (beta-CD) into the running buffer containing charged cyclodextrins was investigated and provided evidence of significant inter-CD interactions. Under certain running buffer conditions, the charged cyclodextrins also appear to adsorb to the capillary walls to various degrees.

A charge-polarized porous metal-organic framework for gas chromatographic separation of alcohols from water.

PubMed

Sun, Jian-Ke; Ji, Min; Chen, Cheng; Wang, Wu-Gen; Wang, Peng; Chen, Rui-Ping; Zhang, Jie

2013-02-25

A bipyridinium ligand with a charge separated skeleton has been introduced into a metal-organic framework to yield a porous material with charge-polarized pore space, which exhibits selective adsorption for polar guest molecules and can be further used in gas chromatography for the separation of alcohol-water mixtures.

Photo-electrochemical properties of graphene wrapped hierarchically branched nanostructures obtained through hydrothermally transformed TiO2 nanotubes

NASA Astrophysics Data System (ADS)

Rambabu, Y.; Jaiswal, Manu; Roy, Somnath C.

2017-10-01

Hierarchically structured nanomaterials play an important role in both light absorption and separation of photo-generated charges. In the present study, hierarchically branched TiO2 nanostructures (HB-MLNTs) are obtained through hydrothermal transformation of electrochemically anodized TiO2 multi-leg nanotubes (MLNT) arrays. Photo-anodes based on HB-MLNTs demonstrated 5 fold increase in applied bias to photo-conversion efficiency (%ABPE) over that of TiO2 MLNTs without branches. Further, such nanostructures are wrapped with reduced graphene oxide (rGO) films to enhance the charge separation, which resulted in ∼6.5 times enhancement in %ABPE over that of bare MLNTs. We estimated charge transport (η tr) and charge transfer (η ct) efficiencies by analyzing the photo-current data. The ultra-fine nano branches grown on the MLNTs are effective in increasing light absorption through multiple scattering and improving charge transport/transfer efficiencies by enlarging semiconductor/electrolyte interface area. The charge transfer resistance, interfacial capacitance and electron decay time have been estimated through electrochemical impedance measurements which correlate with the results obtained from photocurrent measurements.

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

PubMed

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

2012-09-06

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

Fabrication of High-Performance Polymer Bulk-Heterojunction Solar Cells by Interfacial Modifications II

DTIC Science & Technology

2010-08-25

coulombically bound electron-hole (e-h) pairs, commonly having a short range of the separation distance. [27, 31-34] Those excitons may undergo a...reactions causes a simultaneous reduction in the Isc and accounts for a negative MC response. The exciton-charge reaction is essentially Coulombic ...effect indicate that the excitons can interact with trapped charge carriers to de -trap the charge carriers. [46, 57, 58] Alternatively, the triplet

Protein Separation by Electrophoretic-Electroosmotic Focusing on Supported Lipid Bilayers

PubMed Central

Liu, Chunming; Monson, Christopher F.; Yang, Tinglu; Pace, Hudson; Cremer, Paul S.

2011-01-01

An electrophoretic-electroosmotic focusing (EEF) method was developed and used to separate membrane-bound proteins and charged lipids based on their charge-to-size ratio from an initially homogeneous mixture. EEF uses opposing electrophoretic and electroosmotic forces to focus and separate proteins and lipids into narrow bands on supported lipid bilayers (SLBs). Membrane-associated species were focused into specific positions within the SLB in a highly repeatable fashion. The steady-state focusing positions of the proteins could be predicted and controlled by tuning experimental conditions, such as buffer pH, ionic strength, electric field and temperature. Careful tuning of the variables should enable one to separate mixtures of membrane proteins with only subtle differences. The EEF technique was found to be an effective way to separate protein mixtures with low initial concentrations, and it overcame diffusive peak broadening to allow four bands to be separated simultaneously within a 380 μm wide isolated supported membrane patch. PMID:21958061

Wide size range fast integrated mobility spectrometer

DOEpatents

Wang, Jian

2013-10-29

A mobility spectrometer to measure a nanometer particle size distribution is disclosed. The mobility spectrometer includes a conduit and a detector. The conduit is configured to receive and provide fluid communication of a fluid stream having a charged nanometer particle mixture. The conduit includes a separator section configured to generate an electrical field of two dimensions transverse to a dimension associated with the flow of the charged nanometer particle mixture through the separator section to spatially separate charged nanometer particles of the charged nanometer particle mixture in said two dimensions. The detector is disposed downstream of the conduit to detect concentration and position of the spatially-separated nanometer particles.

Charge separation and transport of the n=2 instability in C-2 FRC plasmas

NASA Astrophysics Data System (ADS)

Deng, Bihe; Sun, Xuan; Tuszewski, Michel

2012-10-01

Charge separation is critical in the positive feedback loop for gravitational type instabilities to grow [1], such as in the case of the n=2 mode in the C-2 field reversed configuration (FRC) experiment [2]. A fast time response Langmuir probe with minimum perturbation to the plasma is inserted into the edge of the C-2 plasma to measure the plasma floating potential. With the combined plasma wobble motion and spin motion, 2-D scans of the plasma floating potential are obtained, and evidence of charge separation associated with the n=2 instability is observed. The transport due to charge separation is estimated. Charge neutralization can provide an alternative method to stabilize the n=2 mode. An experiment is proposed to test this method with two probes inserted into the plasma from two azimuthally separated ports and an external shorting circuit, to constantly neutralize the charge separation, thus suppress the growth of the n=2 mode. [4pt] [1] R.J. Goldston and P.H. Rutherford, Introduction to Plasma Physics (Institute of Physics Publishing, Bristol, 2000).[0pt] [2]. M.W. Binderbauer et al, Phys. Rev. Lett. 105, 045003 (2010).

Exploring what prompts ITIC to become a superior acceptor in organic solar cell by combining molecular dynamics simulation with quantum chemistry calculation.

PubMed

Pan, Qing-Qing; Li, Shuang-Bao; Duan, Ying-Chen; Wu, Yong; Zhang, Ji; Geng, Yun; Zhao, Liang; Su, Zhong-Min

2017-11-29

The interface characteristic is a crucial factor determining the power conversion efficiency of organic solar cells (OSCs). In this work, our aim is to conduct a comparative study on the interface characteristics between the very famous non-fullerene acceptor, ITIC, and a fullerene acceptor, PC71BM by combining molecular dynamics simulations with density functional theory. Based on some typical interface models of the acceptor ITIC or PC71BM and the donor PBDB-T selected from MD simulation, besides the evaluation of charge separation/recombination rates, the relative positions of Frenkel exciton (FE) states and the charge transfer states along with their oscillator strengths are also employed to estimate the charge separation abilities. The results show that, when compared with those for the PBDB-T/PC71BM interface, the CT states are more easily formed for the PBDB-T/ITIC interface by either the electron transfer from the FE state or direct excitation, indicating the better charge separation ability of the former. Moreover, the estimation of the charge separation efficiency manifests that although these two types of interfaces have similar charge recombination rates, the PBDB-T/ITIC interface possesses the larger charge separation rates than those of the PBDB-T/PC71BM interface. Therefore, the better match between PBDB-T and ITIC together with a larger charge separation efficiency at the interface are considered to be the reasons for the prominent performance of ITIC in OSCs.

Reducing charging effects in scanning electron microscope images by Rayleigh contrast stretching method (RCS).

PubMed

Wan Ismail, W Z; Sim, K S; Tso, C P; Ting, H Y

2011-01-01

To reduce undesirable charging effects in scanning electron microscope images, Rayleigh contrast stretching is developed and employed. First, re-scaling is performed on the input image histograms with Rayleigh algorithm. Then, contrast stretching or contrast adjustment is implemented to improve the images while reducing the contrast charging artifacts. This technique has been compared to some existing histogram equalization (HE) extension techniques: recursive sub-image HE, contrast stretching dynamic HE, multipeak HE and recursive mean separate HE. Other post processing methods, such as wavelet approach, spatial filtering, and exponential contrast stretching, are compared as well. Overall, the proposed method produces better image compensation in reducing charging artifacts. Copyright © 2011 Wiley Periodicals, Inc.

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.

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2012-11-19

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Charging of Basic Structural Shapes in a Simulated Lunar Environment

NASA Technical Reports Server (NTRS)

Craven, P.; Schneider, T.; Vaughn, J.; Wang, J.; Polansky, J.

2012-01-01

In order to understand the effect of the charging environment on and around structures on the lunar surface, we have exposed basic structural shapes to electrons and Vacuum Ultra-Violet (VUV) radiation. The objects were, in separate runs, isolated, grounded, and placed on dielectric surfaces. In this presentation, the effects of electron energy, VUV flux, and sample orientation, on the charging of the objects will be examined. The potential of each of the object surfaces was monitored in order to determine the magnitude of the ram and wake effects under different orientations relative to the incoming beams (solar wind). This is a part of, and complementary to, the study of the group at USC under Dr. J. Wang, the purpose of which is to model the effects of the charging environment on structures on the lunar surface.

Local Intermolecular Order Controls Photoinduced Charge Separation at Donor/Acceptor Interfaces in Organic Semiconductors

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

Feier, Hilary M.; Reid, Obadiah G.; Pace, Natalie A.

2016-03-23

How free charge is generated at organic donor-acceptor interfaces is an important question, as the binding energy of the lowest energy (localized) charge transfer states should be too high for the electron and hole to escape each other. Recently, it has been proposed that delocalization of the electronic states participating in charge transfer is crucial, and aggregated or otherwise locally ordered structures of the donor or the acceptor are the precondition for this electronic characteristic. The effect of intermolecular aggregation of both the polymer donor and fullerene acceptor on charge separation is studied. In the first case, the dilute electronmore » acceptor triethylsilylhydroxy-1,4,8,11,15,18,22,25-octabutoxyphthalocyaninatosilicon(IV) (SiPc) is used to eliminate the influence of acceptor aggregation, and control polymer order through side-chain regioregularity, comparing charge generation in 96% regioregular (RR-) poly(3-hexylthiophene) (P3HT) with its regiorandom (RRa-) counterpart. In the second case, ordered phases in the polymer are eliminated by using RRa-P3HT, and phenyl-C61-butyric acid methyl ester (PC61BM) is used as the acceptor, varying its concentration to control aggregation. Time-resolved microwave conductivity, time-resolved photoluminescence, and transient absorption spectroscopy measurements show that while ultrafast charge transfer occurs in all samples, long-lived charge carriers are only produced in films with intermolecular aggregates of either RR-P3HT or PC61BM, and that polymer aggregates are just as effective in this regard as those of fullerenes.« less

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

Tsvelik, A. M.; Yevtushenko, O. M.

We study the low energy physics of a Kondo chain where electrons from a one-dimensional band interact with magnetic moments via an anisotropic exchange interaction. It is demonstrated that the anisotropy gives rise to two different phases which are separated by a quantum phase transition. In the phase with easy plane anisotropy, Z2 symmetry between sectors with different helicity of the electrons is broken. As a result, localization effects are suppressed and the dc transport acquires (partial) symmetry protection. This effect is similar to the protection of the edge transport in time-reversal invariant topological insulators. The phase with easy axismore » anisotropy corresponds to the Tomonaga-Luttinger liquid with a pronounced spin-charge separation. The slow charge density wave modes have no protection against localizatioin.« less

Exceptionally Long-Lived Charge Separated State in Zeolitic Imidazolate Framework: Implication for Photocatalytic Applications

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

Pattengale, Brian; Yang, Sizhuo; Ludwig, John

2016-06-22

Zeolitic Imidazolate Frameworks (ZIFs) have emerged as a novel class of porous metal-organic frameworks (MOFs) for catalysis application because of their exceptional thermal and chemical stability. Inspired by the broad absorption of ZIF-67 in UV-visible-near IR region, we explored its excited state and charge separation dynamics, properties essential for photocatalytic applications, using optical (OTA) and X-ray transient absorption (XTA) spectroscopy. OTA results show that an exceptionally long-lived excited state is formed after photoexcitation. This long-lived excited state was confirmed to be the charge separated state with ligandto-metal charge transfer character using XTA. The surprisingly long-lived charge separated state, together withmore » its intrinsic hybrid nature, all point to its potential application in heterogeneous photocatalysis and energy conversion.« less

Spin-orbit induced electronic spin separation in semiconductor nanostructures.

PubMed

Kohda, Makoto; Nakamura, Shuji; Nishihara, Yoshitaka; Kobayashi, Kensuke; Ono, Teruo; Ohe, Jun-ichiro; Tokura, Yasuhiro; Mineno, Taiki; Nitta, Junsaku

2012-01-01

The demonstration of quantized spin splitting by Stern and Gerlach is one of the most important experiments in modern physics. Their discovery was the precursor of recent developments in spin-based technologies. Although electrical spin separation of charged particles is fundamental in spintronics, in non-uniform magnetic fields it has been difficult to separate the spin states of charged particles due to the Lorentz force, as well as to the insufficient and uncontrollable field gradients. Here we demonstrate electronic spin separation in a semiconductor nanostructure. To avoid the Lorentz force, which is inevitably induced when an external magnetic field is applied, we utilized the effective non-uniform magnetic field which originates from the Rashba spin-orbit interaction in an InGaAs-based heterostructure. Using a Stern-Gerlach-inspired mechanism, together with a quantum point contact, we obtained field gradients of 10(8) T m(-1) resulting in a highly polarized spin current.

Spin–orbit induced electronic spin separation in semiconductor nanostructures

PubMed Central

Kohda, Makoto; Nakamura, Shuji; Nishihara, Yoshitaka; Kobayashi, Kensuke; Ono, Teruo; Ohe, Jun-ichiro; Tokura, Yasuhiro; Mineno, Taiki; Nitta, Junsaku

2012-01-01

The demonstration of quantized spin splitting by Stern and Gerlach is one of the most important experiments in modern physics. Their discovery was the precursor of recent developments in spin-based technologies. Although electrical spin separation of charged particles is fundamental in spintronics, in non-uniform magnetic fields it has been difficult to separate the spin states of charged particles due to the Lorentz force, as well as to the insufficient and uncontrollable field gradients. Here we demonstrate electronic spin separation in a semiconductor nanostructure. To avoid the Lorentz force, which is inevitably induced when an external magnetic field is applied, we utilized the effective non-uniform magnetic field which originates from the Rashba spin–orbit interaction in an InGaAs-based heterostructure. Using a Stern–Gerlach-inspired mechanism, together with a quantum point contact, we obtained field gradients of 108 T m−1 resulting in a highly polarized spin current. PMID:23011136

Optical excitations dynamics at hetero-interfaces fullerene/quantum dots

NASA Astrophysics Data System (ADS)

Righetto, Marcello; Privitera, Alberto; Franco, Lorenzo; Bozio, Renato

2017-08-01

Embedding Semiconductor Quantum Dots (QDs) into hybrid organic-inorganic solar cell holds promises for improving photovoltaic performances. Thanks to their strong coupling with electro-magnetic radiation field, QDs represent paradigmatic photon absorbers. Nevertheless, the quest for suitable charge separating hetero-interfaces is still an open challenge. Within this framework, the excited state interactions between QDs and fullerene derivatives are of great interest for ternary solar cells (polymer:QDs:fullerene). In this work, we investigated the exciton dynamics of core/shell CdSe/CdS QDs both in solution and in blends with fullerene derivative (PCBM). By means of transient optical techniques, we aimed to unveil the dynamics of the QDs-PCBM interaction. Indeed, the observed excited state depopulation of QDs in blends is compatible with an excited state interaction living on picosecond timescale. Through electron paramagnetic resonance, we delved into the nature of this interaction, identifying the presence of charge separated states. The concurrence of these observations suggest a fast electron transfer process, where QDs act as donors and PCBM molecules as acceptors, followed by effective charge separation. Therefore, our experimental results indicate the QDs-PCBM heterointerface as suitable exciton separating interface, paving the way for possible applications in photovoltaics.

Statistical mechanics of light elements at high pressure. VI - Liquid-state calculations with Thomas-Fermi-Dirac theory

NASA Technical Reports Server (NTRS)

Macfarlane, J. J.

1984-01-01

A model free energy is developed for hydrogen-helium mixtures based on solid-state Thomas-Fermi-Dirac calculations at pressures relevant to the interiors of giant planets. Using a model potential similar to that for a two-component plasma, effective charges for the nuclei (which are in general smaller than the actual charges because of screening effects) are parameterized, being constrained by calculations at a number of densities, compositions, and lattice structures. These model potentials are then used to compute the equilibrium properties of H-He fluids using a charged hard-sphere model. The results find critical temperatures of about 0 K, 500 K, and 1500 K, for pressures of 10, 100, and 1000 Mbar, respectively. These phase separation temperatures are considerably lower (approximately 6,000-10,000 K) than those found from calculations using free electron perturbation theory, and suggest that H-He solutions should be stable against phase separation in the metallic zones of Jupiter and Saturn.

Photoinduced electron transfer in a ferrocene-distyryl BODIPY dyad and a ferrocene-distyryl BODIPY-C60 triad.

PubMed

Liu, Jian-Yong; El-Khouly, Mohamed E; Fukuzumi, Shunichi; Ng, Dennis K P

2012-06-04

A ferrocene-distyryl BODIPY dyad and a ferrocene-distyryl BODIPY-C(60) triad are synthesized and characterized. Upon photoexcitation at the distyryl BODIPY unit, these arrays undergo photoinduced electron transfer to form the corresponding charge-separated species. Based on their redox potentials, determined by cyclic voltammetry, the direction of the charge separation and the energies of these states are revealed. Femtosecond transient spectroscopic studies reveal that a fast charge separation (k(CS) =1.0×10(10) s(-1)) occurs for both the ferrocene-distyryl BODIPY dyad and the ferrocene-distyryl BODIPY-C(60) triad, but that a relatively slow charge recombination is observed only for the triad. The lifetime of the charge-separated state is 500 ps. Charge recombination of the dyad and triad leads to population of the triplet excited sate of ferrocene and the ground state, respectively. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Study of gain and photoresponse characteristics for back-illuminated separate absorption and multiplication GaN avalanche photodiodes

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

Wang, Xiaodong; Pan, Ming; Hou, Liwei

2014-01-07

The gain and photoresponse characteristics have been numerically studied for back-illuminated separate absorption and multiplication (SAM) GaN avalanche photodiodes (APDs). The parameters of fundamental models are calibrated by simultaneously comparing the simulated dark and light current characteristics with the experimental results. Effects of environmental temperatures and device dimensions on gain characteristics have been investigated, and a method to achieve the optimum thickness of charge layer is obtained. The dependence of gain characteristics and breakdown voltage on the doping concentration of the charge layer is also studied in detail to get the optimal charge layer. The bias-dependent spectral responsivity and quantummore » efficiency are then presented to study the photoresponse mechanisms inside SAM GaN APDs. It is found the responsivity peak red-shifts at first due to the Franz-Keldysh effect and then blue-shifts due to the reach-through effect of the absorption layer. Finally, a new SAM GaN/AlGaN heterojunction APD structure is proposed for optimizing SAM GaN APDs.« less

Control of mobility in molecular organic semiconductors by dendrimer generation

NASA Astrophysics Data System (ADS)

Lupton, J. M.; Samuel, I. D.; Beavington, R.; Frampton, M. J.; Burn, P. L.; Bässler, H.

2001-04-01

Conjugated dendrimers are of interest as novel materials for light-emitting diodes. They consist of a luminescent chromophore at the core with highly branched conjugated dendron sidegroups. In these materials, light emission occurs from the core and is independent of generation. The dendron branching controls the separation between the chromophores. We present here a family of conjugated dendrimers and investigate the effect of dendron branching on light emission and charge transport. We apply a number of transport measurement techniques to thin films of a conjugated dendrimer in a light-emitting diode configuration to determine the effect of chromophore spacing on charge transport. We find that the mobility is reduced by two orders of magnitude as the size of the molecule doubles with increased branching or dendrimer generation. The degree of branching allows a unique control of mobility by molecular structure. An increase in chromophore separation also results in a reduction of intermolecular interactions, which reduces the red emission tail in film photoluminescence. We find that the steady-state charge transport is well described by a simple device model incorporating the effect of generation, and use the materials to shed light on the interpretation of transient electroluminescence data. We demonstrate the significance of the ability to tune the mobility in bilayer devices, where a more balanced charge transport can be achieved.

Repulsion Between Finite Charged Plates with Strongly Overlapped Electric Double Layers.

PubMed

Ghosal, Sandip; Sherwood, John D

2016-09-20

Screened Coulomb interactions between uniformly charged flat plates are considered at very small plate separations for which the Debye layers are strongly overlapped, in the limit of small electrical potentials. If the plates are of infinite length, the disjoining pressure between the plates decays as an inverse power of the plate separation. If the plates are of finite length, we show that screening Debye layer charges close to the edge of the plates are no longer constrained to stay between the plates, but instead spill out into the surrounding electrolyte. The resulting change in the disjoining pressure is calculated analytically: the force between the plates is reduced by this edge correction when the charge density is uniform over the surface of the plates, and is increased when the surface is at constant potential. A similar change in disjoining pressure due to loss of lateral confinement of the Debye layer charges should occur whenever the sizes of the interacting charged objects become small enough to approach the Debye scale. We investigate the effect here in the context of a two-dimensional model problem that is sufficiently simple to yield analytical results.

One-dimension modeling on the parallel-plate ion extraction process based on a non-electron-equilibrium fluid model

NASA Astrophysics Data System (ADS)

Li, He-Ping; Chen, Jian; Guo, Heng; Jiang, Dong-Jun; Zhou, Ming-Sheng; Department of Engineering Physics Team

2017-10-01

Ion extraction from a plasma under an externally applied electric field involve multi-particle and multi-field interactions, and has wide applications in the fields of materials processing, etching, chemical analysis, etc. In order to develop the high-efficiency ion extraction methods, it is indispensable to establish a feasible model to understand the non-equilibrium transportation processes of the charged particles and the evolutions of the space charge sheath during the extraction process. Most of the previous studies on the ion extraction process are mainly based on the electron-equilibrium fluid model, which assumed that the electrons are in the thermodynamic equilibrium state. However, it may lead to some confusions with neglecting the electron movement during the sheath formation process. In this study, a non-electron-equilibrium model is established to describe the transportation of the charged particles in a parallel-plate ion extraction process. The numerical results show that the formation of the Child-Langmuir sheath is mainly caused by the charge separation. And thus, the sheath shielding effect will be significantly weakened if the charge separation is suppressed during the extraction process of the charged particles.

Nanoengineered field induced charge separation membranes manufacture thereof

DOEpatents

O'Brien, Kevin C.; Haslam, Jeffery J.; Bourcier, William L.; Floyd, III, William Clary

2016-08-02

A device according to one embodiment includes a porous membrane having a surface charge and pore configuration characterized by a double layer overlap effect being present in pores of the membrane, where the porous membrane includes functional groups that preferentially interact with either cations or anions. A device according to another embodiment includes a porous membrane having a surface charge in pores thereof sufficient to impart anion or cation selectivity in the pores. Additional devices, systems and methods are also presented.

Application of ion mobility-mass spectrometry to microRNA analysis.

PubMed

Takebayashi, Kosuke; Hirose, Kenji; Izumi, Yoshihiro; Bamba, Takeshi; Fukusaki, Eiichiro

2013-03-01

Liquid chromatography/mass spectrometry is widely used for studying sequence determination and modification analysis of small RNAs. However, the efficiency of liquid chromatography-based separation of intact small RNA species is insufficient, since the physiochemical properties among small RNAs are very similar. In this study, we focused on ion mobility-mass spectrometry (IM-MS), which is a gas-phase separation technique coupled with mass spectrometry; we have evaluated the utility of IM-MS for microRNA (miRNA) analysis. A multiply charged deprotonated ion derived from an 18-24-nt-long miRNA was formed by electrospray ionization, and then the time, called the "drift time", taken by each ion to migrate through a buffer gas was measured. Each multivalent ion was temporally separated on the basis of the charge state and structural formation; 3 types of unique mass-mobility correlation patterns (i.e., chainlike-form, hairpin-form, and dimer-form) were present on the two-dimensional mobility-mass spectrum. Moreover, we found that the ion size (sequence length) and the secondary structures of the small RNAs strongly contributed to the IM-MS-based separation, although solvent conditions such as pH had no effect. Therefore, sequence isomers could also be discerned by the selection of each specific charged ion, i.e., the 6(-) charged ion reflected a majority among chainlike-, hairpin-, and other structures. We concluded that the IM-MS provides additional capability for separation; thus, this analytical method will be a powerful tool for comprehensive small RNA analysis. Copyright © 2012. Published by Elsevier B.V.

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

NASA Astrophysics Data System (ADS)

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

2011-09-01

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

Formation of ion clusters in the phase separated structures of neutral-charged polymer blends

NASA Astrophysics Data System (ADS)

Kwon, Ha-Kyung; Olvera de La Cruz, Monica

2015-03-01

Polyelectrolyte blends, consisting of at least one charged species, are promising candidate materials for fuel cell membranes, for their mechanical stability and high selectivity for proton conduction. The phase behavior of the blends is important to understand, as this can significantly affect the performance of the device. The phase behavior is controlled by χN, the Flory-Huggins parameter multiplied by the number of mers, as well as the electrostatic interactions between the charged backbone and the counterions. It has recently been shown that local ionic correlations, incorporated via liquid state (LS) theory, enhance phase separation of the blend, even in the absence of polymer interactions. In this study, we show phase diagrams of neutral-charged polymer blends including ionic correlations via LS theory. In addition to enhanced phase separation at low χN, the blends show liquid-liquid phase separation at high electrostatic interaction strengths. Above the critical strength, the charged polymer phase separates into ion-rich and ion-poor regions, resulting in the formation of ion clusters within the charged polymer phase. This can be shown by the appearance of multiple spinodal and critical points, indicating the coexistence of several charge separated phases. This work was performed under the following financial assistance award 70NANB14H012 from U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD).

Photoelectrodes based on 2D opals assembled from Cu-delafossite double-shelled microspheres for an enhanced photoelectrochemical response.

PubMed

Oh, Yunjung; Yang, Wooseok; Tan, Jeiwan; Lee, Hyungsoo; Park, Jaemin; Moon, Jooho

2018-02-22

Although a unique light-harvesting property was recently demonstrated in a photocathode based on 2-dimensional (2D) opals of CuFeO 2 -shelled SiO 2 microspheres, the performance of a monolayer of ultra-thin CuFeO 2 -shelled microspheres is limited by ineffective charge separation. Herein, we propose an innovative design rule, in which an inner CuFeO 2 /outer CuAlO 2 double-shelled heterojunction is formed on each partially etched microsphere to obtain a hexagonally assembled 2D opal photoelectrode. Our Cu-delafossite double-shelled photocathode shows a dramatically improved charge separation capability, with a 9-fold increase in the photocurrent compared to that of the single-shelled counterpart. Electrochemical impedance spectroscopy clearly confirms the reduced charge transport/transfer resistance associated with the Cu-delafossite double-shelled photocathode, while surface photovoltage spectra reveal enhanced polarization of the photogenerated carrier, indicating improved charge separation capability with the aid of the heterojunction. Our finding sheds light on the importance of heterojunction interfaces in achieving optimal charge separation in opal architectures as well as the inner-shell/electrolyte interface to expedite charge separation/transport.

Quantum modeling of ultrafast photoinduced charge separation

NASA Astrophysics Data System (ADS)

Rozzi, Carlo Andrea; Troiani, Filippo; Tavernelli, Ivano

2018-01-01

Phenomena involving electron transfer are ubiquitous in nature, photosynthesis and enzymes or protein activity being prominent examples. Their deep understanding thus represents a mandatory scientific goal. Moreover, controlling the separation of photogenerated charges is a crucial prerequisite in many applicative contexts, including quantum electronics, photo-electrochemical water splitting, photocatalytic dye degradation, and energy conversion. In particular, photoinduced charge separation is the pivotal step driving the storage of sun light into electrical or chemical energy. If properly mastered, these processes may also allow us to achieve a better command of information storage at the nanoscale, as required for the development of molecular electronics, optical switching, or quantum technologies, amongst others. In this Topical Review we survey recent progress in the understanding of ultrafast charge separation from photoexcited states. We report the state-of-the-art of the observation and theoretical description of charge separation phenomena in the ultrafast regime mainly focusing on molecular- and nano-sized solar energy conversion systems. In particular, we examine different proposed mechanisms driving ultrafast charge dynamics, with particular regard to the role of quantum coherence and electron-nuclear coupling, and link experimental observations to theoretical approaches based either on model Hamiltonians or on first principles simulations.

Explicit Solvent Simulations of Friction between Brush Layers of Charged and Neutral Bottle-Brush Macromolecules

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

Carrillo, Jan-Michael; Brown, W Michael; Dobrynin, Andrey

2012-01-01

We study friction between charged and neutral brush layers of bottle-brush macromolecules using molecular dynamics simulations. In our simulations the solvent molecules were treated explicitly. The deformation of the bottle-brush macromolecules under the shear were studied as a function of the substrate separation and shear stress. For charged bottle-brush layers we study effect of the added salt on the brush lubricating properties to elucidate factors responsible for energy dissipation in charged and neutral brush systems. Our simulations have shown that for both charged and neutral brush systems the main deformation mode of the bottle-brush macromolecule is associated with the backbonemore » deformation. This deformation mode manifests itself in the backbone deformation ratio, , and shear viscosity, , to be universal functions of the Weissenberg number W. The value of the friction coefficient, , and viscosity, , are larger for the charged bottle-brush coatings in comparison with those for neutral brushes at the same separation distance, D, between substrates. The additional energy dissipation generated by brush sliding in charged bottle-brush systems is due to electrostatic coupling between bottle-brush and counterion motion. This coupling weakens as salt concentration, cs, increases resulting in values of the viscosity, , and friction coefficient, , approaching corresponding values obtained for neutral brush systems.« less

Acquisition of a High Performance Computer Cluster for Materials Research and Education

DTIC Science & Technology

2015-04-17

separation in all-organic and hybrid organic- inorganic solar cells. The outcome of the project 1. REPORT DATE (DD-MM-YYYY) 4. TITLE AND SUBTITLE 13...diffusion and interfacial charge separation in all-organic and hybrid organic- inorganic solar cells. The outcome of the project is the development...simulations to predict charge carrier mobilities, exciton diffusion and interfacial charge separation in all- organic and hybrid organic- inorganic solar

Complex coacervation of supercharged proteins with polyelectrolytes.

PubMed

Obermeyer, Allie C; Mills, Carolyn E; Dong, Xue-Hui; Flores, Romeo J; Olsen, Bradley D

2016-04-21

Complexation of proteins with polyelectrolytes or block copolymers can lead to phase separation to generate a coacervate phase or self-assembly of coacervate core micelles. However, many proteins do not coacervate at conditions near neutral pH and physiological ionic strength. Here, protein supercharging is used to systematically explore the effect of protein charge on the complex coacervation with polycations. Four model proteins were anionically supercharged to varying degrees as quantified by mass spectrometry. Proteins phase separated with strong polycations when the ratio of negatively charged residues to positively charged residues on the protein (α) was greater than 1.1-1.2. Efficient partitioning of the protein into the coacervate phase required larger α (1.5-2.0). The preferred charge ratio for coacervation was shifted away from charge symmetry for three of the four model proteins and indicated an excess of positive charge in the coacervate phase. The composition of protein and polymer in the coacervate phase was determined using fluorescently labeled components, revealing that several of the coacervates likely have both induced charging and a macromolecular charge imbalance. The model proteins were also encapsulated in complex coacervate core micelles and micelles formed when the protein charge ratio α was greater than 1.3-1.4. Small angle neutron scattering and transmission electron microscopy showed that the micelles were spherical. The stability of the coacervate phase in both the bulk and micelles improved to increased ionic strength as the net charge on the protein increased. The micelles were also stable to dehydration and elevated temperatures.

Improvement of calcium mineral separation contrast using anionic reagents: electrokinetics properties and flotation

NASA Astrophysics Data System (ADS)

Lafhaj, Z.; Filippov, L. O.; Filippova, I. V.

2017-07-01

The flotation separation of salt type calcium minerals is problematic, due to the similarities in their same active Ca2+ related site for interaction with anionic collectors and similar physicochemical characteristics such as solubility, zero-point charge, surface speciation and Ca-site density. The work was performed to achieve effective and selective separation of the calcium-minerals using pure minerals samples: orange calcite with Mg impurities, optic calcite with impurities level and an apatite. The pure samples surface was examined using techniques sensitive near-surface like infrared spectroscopy (FTIR) and chemical composition was obtained by ICPMS. The isoelectric point (IEP) and point of zero charge (PZC) in electrolyte were recorded using electrophoresis method at different ionic strengths of the solution. Mechanisms of charge development at the mineral-water interface are discussed. The time of contact as important parameter for the charge equilibrium was deduced from kinetics study and fixed to 30 minutes. The difference in the values obtained between IEP and PZSE can be explained by the presence of a specific adsorption of cations and anions on the surface. The effect of pure anionic collectors such as oleic and linoleic acid were studied. At low pH, both collectors lead to a good recovery for the calcites. The flotation recovery of optic calcite at pH 9 with sodium oleate is higher than with sodium linoleate. At alkaline pH, apatite showed a better recovery with sodium linoleate.

Theoretical Studies on InGaAs/InAlAs SAGCM Avalanche Photodiodes

NASA Astrophysics Data System (ADS)

Cao, Siyu; Zhao, Yue; ur Rehman, Sajid; Feng, Shuai; Zuo, Yuhua; Li, Chuanbo; Zhang, Lichun; Cheng, Buwen; Wang, Qiming

2018-05-01

In this paper, we provide a detailed insight on InGaAs/InAlAs separate absorption, grading, charge, and multiplication avalanche photodiodes (SAGCM APDs) and a theoretical model of APDs is built. Through theoretical analysis and two-dimensional (2D) simulation, the influence of charge layer and tunneling effect on the APDs is fully understood. The design of charge layer (including doping level and thickness) can be calculated by our predictive model for different multiplication thickness. We find that as the thickness of charge layer increases, the suitable doping level range in charge layer decreases. Compared to thinner charge layer, performance of APD varies significantly via several percent deviations of doping concentrations in thicker charge layer. Moreover, the generation rate ( G btt ) of band-to-band tunnel is calculated, and the influence of tunneling effect on avalanche field was analyzed. We confirm that avalanche field and multiplication factor ( M n ) in multiplication will decrease by the tunneling effect. The theoretical model and analysis are based on InGaAs/InAlAs APD; however, they are applicable to other APD material systems as well.

Means and method of detection in chemical separation procedures

DOEpatents

Yeung, Edward S.; Koutny, Lance B.; Hogan, Barry L.; Cheung, Chan K.; Ma, Yinfa

1993-03-09

A means and method for indirect detection of constituent components of a mixture separated in a chemical separation process. Fluorescing ions are distributed across the area in which separation of the mixture will occur to provide a generally uniform background fluorescence intensity. For example, the mixture is comprised of one or more charged analytes which displace fluorescing ions where its constituent components separate to. Fluorescing ions of the same charge as the charged analyte components cause a displacement. The displacement results in the location of the separated components having a reduced fluorescence intensity to the remainder of the background. Detection of the lower fluorescence intensity areas can be visually, by photographic means and methods, or by automated laser scanning.

Means and method of detection in chemical separation procedures

DOEpatents

Yeung, E.S.; Koutny, L.B.; Hogan, B.L.; Cheung, C.K.; Yinfa Ma.

1993-03-09

A means and method are described for indirect detection of constituent components of a mixture separated in a chemical separation process. Fluorescing ions are distributed across the area in which separation of the mixture will occur to provide a generally uniform background fluorescence intensity. For example, the mixture is comprised of one or more charged analytes which displace fluorescing ions where its constituent components separate to. Fluorescing ions of the same charge as the charged analyte components cause a displacement. The displacement results in the location of the separated components having a reduced fluorescence intensity to the remainder of the background. Detection of the lower fluorescence intensity areas can be visually, by photographic means and methods, or by automated laser scanning.

Electrophoretic sample insertion. [device for uniformly distributing samples in flow path

NASA Technical Reports Server (NTRS)

Mccreight, L. R. (Inventor)

1974-01-01

Two conductive screens located in the flow path of an electrophoresis sample separation apparatus are charged electrically. The sample is introduced between the screens, and the charge is sufficient to disperse and hold the samples across the screens. When the charge is terminated, the samples are uniformly distributed in the flow path. Additionally, a first separation by charged properties has been accomplished.

Freezing, fragmentation, and charge separation in sonic sprayed water droplets

NASA Astrophysics Data System (ADS)

Zilch, Lloyd W.; Maze, Joshua T.; Smith, John W.; Jarrold, Martin F.

2009-06-01

Water droplets are generated by sonic spray, transferred into vacuum through a capillary interface, and then passed through two image charge detectors separated by a drift region. The image charge detectors measure the charge and velocity of each droplet. For around 1% of the droplets, the charge changes significantly between the detectors. In some cases it increases, in others it decreases, and for some droplets the charge changes polarity. We attribute the charge changing behavior to fragmentation caused by freezing. Simulations indicate that the time required for a droplet to cool and freeze in vacuum depends on its size, and that droplets with radii of 1-2 [mu]m have the right size to freeze between the two detectors. These sizes correspond to the smaller end of the distribution present in the experiment. When the charge on a droplet increases or changes polarity, fragmentation must be accompanied by charge separation where fragments carry away opposite charges. In some cases, two fission fragments were observed in the second charge detector. We show examples where the droplet breaks apart to give fragments of the same charge and opposite charges. The fragmentation and charge changing behavior found here is consistent with what has been found in the freezing of larger suspended and supported droplets.

Device and method for separating minerals, carbon and cement additives from fly ash

DOEpatents

Link, Thomas A.; Schoffstall, Micael R.; Soong, Yee

2004-01-27

A process for separating organic and inorganic particles from a dry mixture by sizing the particles into isolated fractions, contacting the sized particles to a charged substrate and subjecting the charged particles to an electric field to separate the particles.

Inactivation of Gating Currents of L-Type Calcium Channels

PubMed Central

Shirokov, Roman; Ferreira, Gonzalo; Yi, Jianxun; Ríos, Eduardo

1998-01-01

In studies of gating currents of rabbit cardiac Ca channels expressed as α1C/β2a or α1C/β2a/α2δ subunit combinations in tsA201 cells, we found that long-lasting depolarization shifted the distribution of mobile charge to very negative potentials. The phenomenon has been termed charge interconversion in native skeletal muscle (Brum, G., and E. Ríos. 1987. J. Physiol. (Camb.). 387:489–517) and cardiac Ca channels (Shirokov, R., R. Levis, N. Shirokova, and E. Ríos. 1992. J. Gen. Physiol. 99:863–895). Charge 1 (voltage of half-maximal transfer, V1/2 ≃ 0 mV) gates noninactivated channels, while charge 2 (V1/2 ≃ −90 mV) is generated in inactivated channels. In α1C/β2a cells, the available charge 1 decreased upon inactivating depolarization with a time constant τ ≃ 8, while the available charge 2 decreased upon recovery from inactivation (at −200 mV) with τ ≃ 0.3 s. These processes therefore are much slower than charge movement, which takes <50 ms. This separation between the time scale of measurable charge movement and that of changes in their availability, which was even wider in the presence of α2δ, implies that charges 1 and 2 originate from separate channel modes. Because clear modal separation characterizes slow (C-type) inactivation of Na and K channels, this observation establishes the nature of voltage-dependent inactivation of L-type Ca channels as slow or C-type. The presence of the α2δ subunit did not change the V1/2 of charge 2, but sped up the reduction of charge 1 upon inactivation at 40 mV (to τ ≃ 2 s), while slowing the reduction of charge 2 upon recovery (τ ≃ 2 s). The observations were well simulated with a model that describes activation as continuous electrodiffusion (Levitt, D. 1989. Biophys. J. 55:489–498) and inactivation as discrete modal change. The effects of α2δ are reproduced assuming that the subunit lowers the free energy of the inactivated mode. PMID:9607938

Femtosecond Visible Transient Absorption Spectroscopy of Chlorophyll f-Containing Photosystem I.

PubMed

Kaucikas, Marius; Nürnberg, Dennis; Dorlhiac, Gabriel; Rutherford, A William; van Thor, Jasper J

2017-01-24

Photosystem I (PSI) from Chroococcidiopsis thermalis PCC 7203 grown under far-red light (FRL; >725 nm) contains both chlorophyll a and a small proportion of chlorophyll f. Here, we investigated excitation energy transfer and charge separation using this FRL-grown form of PSI (FRL-PSI). We compared femtosecond transient visible absorption changes of normal, white-light (WL)-grown PSI (WL-PSI) with those of FRL-PSI using excitation at 670 nm, 700 nm, and (in the case of FRL-PSI) 740 nm. The possibility that chlorophyll f participates in energy transfer or charge separation is discussed on the basis of spectral assignments. With selective pumping of chlorophyll f at 740 nm, we observe a final ∼150 ps decay assigned to trapping by charge separation, and the amplitude of the resulting P700 +• A 1 -• charge-separated state indicates that the yield is directly comparable to that of WL-PSI. The kinetics shows a rapid 2 ps time constant for almost complete transfer to chlorophyll f if chlorophyll a is pumped with a wavelength of 670 nm or 700 nm. Although the physical role of chlorophyll f is best supported as a low-energy radiative trap, the physical location should be close to or potentially within the charge-separating pigments to allow efficient transfer for charge separation on the 150 ps timescale. Target models can be developed that include a branching in the formation of the charge separation for either WL-PSI or FRL-PSI. Copyright © 2017 Biophysical Society. Published by Elsevier Inc. All rights reserved.

Position-dependent effects of polylysine on Sec protein transport.

PubMed

Liang, Fu-Cheng; Bageshwar, Umesh K; Musser, Siegfried M

2012-04-13

The bacterial Sec protein translocation system catalyzes the transport of unfolded precursor proteins across the cytoplasmic membrane. Using a recently developed real time fluorescence-based transport assay, the effects of the number and distribution of positive charges on the transport time and transport efficiency of proOmpA were examined. As expected, an increase in the number of lysine residues generally increased transport time and decreased transport efficiency. However, the observed effects were highly dependent on the polylysine position in the mature domain. In addition, a string of consecutive positive charges generally had a more significant effect on transport time and efficiency than separating the charges into two or more charged segments. Thirty positive charges distributed throughout the mature domain resulted in effects similar to 10 consecutive charges near the N terminus of the mature domain. These data support a model in which the local effects of positive charge on the translocation kinetics dominate over total thermodynamic constraints. The rapid translocation kinetics of some highly charged proOmpA mutants suggest that the charge is partially shielded from the electric field gradient during transport, possibly by the co-migration of counter ions. The transport times of precursors with multiple positively charged sequences, or "pause sites," were fairly well predicted by a local effect model. However, the kinetic profile predicted by this local effect model was not observed. Instead, the transport kinetics observed for precursors with multiple polylysine segments support a model in which translocation through the SecYEG pore is not the rate-limiting step of transport.

Position-dependent Effects of Polylysine on Sec Protein Transport*

PubMed Central

Liang, Fu-Cheng; Bageshwar, Umesh K.; Musser, Siegfried M.

2012-01-01

The bacterial Sec protein translocation system catalyzes the transport of unfolded precursor proteins across the cytoplasmic membrane. Using a recently developed real time fluorescence-based transport assay, the effects of the number and distribution of positive charges on the transport time and transport efficiency of proOmpA were examined. As expected, an increase in the number of lysine residues generally increased transport time and decreased transport efficiency. However, the observed effects were highly dependent on the polylysine position in the mature domain. In addition, a string of consecutive positive charges generally had a more significant effect on transport time and efficiency than separating the charges into two or more charged segments. Thirty positive charges distributed throughout the mature domain resulted in effects similar to 10 consecutive charges near the N terminus of the mature domain. These data support a model in which the local effects of positive charge on the translocation kinetics dominate over total thermodynamic constraints. The rapid translocation kinetics of some highly charged proOmpA mutants suggest that the charge is partially shielded from the electric field gradient during transport, possibly by the co-migration of counter ions. The transport times of precursors with multiple positively charged sequences, or “pause sites,” were fairly well predicted by a local effect model. However, the kinetic profile predicted by this local effect model was not observed. Instead, the transport kinetics observed for precursors with multiple polylysine segments support a model in which translocation through the SecYEG pore is not the rate-limiting step of transport. PMID:22367204

Core/shell colloidal quantum dot exciplex states for the development of highly efficient quantum-dot-sensitized solar cells.

PubMed

Wang, Jin; Mora-Seró, Iván; Pan, Zhenxiao; Zhao, Ke; Zhang, Hua; Feng, Yaoyu; Yang, Guang; Zhong, Xinhua; Bisquert, Juan

2013-10-23

Searching suitable panchromatic QD sensitizers for expanding the light-harvesting range, accelerating charge separation, and retarding charge recombination is an effective way to improve power conversion efficiency (PCE) of quantum-dot-sensitized solar cells (QDSCs). One possible way to obtain a wide absorption range is to use the exciplex state of a type-II core/shell-structured QDs. In addition, this system could also provide a fast charge separation and low charge-recombination rate. Herein, we report on using a CdTe/CdSe type-II core/shell QD sensitizer with an absorption range extending into the infrared region because of its exciplex state, which is covalently linked to TiO2 mesoporous electrodes by dropping a bifunctional linker molecule mercaptopropionic acid (MPA)-capped QD aqueous solution onto the film electrode. High loading and a uniform distribution of QD sensitizer throughout the film electrode thickness have been confirmed by energy dispersive X-ray (EDX) elemental mapping. The accelerated electron injection and retarded charge-recombination pathway in the built CdTe/CdSe QD cells in comparison with reference CdSe QD-based cells have been confirmed by impedance spectroscopy, fluorescence decay, and intensity-modulated photocurrent/photovoltage spectroscopy (IMPS/IMVS) analysis. With the combination of the high QD loading and intrinsically superior optoelectronic properties of type-II core/shell QD (wide absorption range, fast charge separation, and slow charge recombination), the resulting CdTe/CdSe QD-based regenerative sandwich solar cells exhibit a record PCE of 6.76% (J(sc) = 19.59 mA cm(-2), V(oc) = 0.606 V, and FF = 0.569) with a mask around the active film under a full 1 sun illumination (simulated AM 1.5), which is the highest reported to date for liquid-junction QDSCs.

Nanoimprinting-induced nanomorphological transition in polymer solar cells: enhanced electrical and optical performance.

PubMed

Jeong, Seonju; Cho, Changsoon; Kang, Hyunbum; Kim, Ki-Hyun; Yuk, Youngji; Park, Jeong Young; Kim, Bumjoon J; Lee, Jung-Yong

2015-03-24

We have investigated the effects of a directly nanopatterned active layer on the electrical and optical properties of inverted polymer solar cells (i-PSCs). The capillary force in confined molds plays a critical role in polymer crystallization and phase separation of the film. The nanoimprinting process induced improved crystallization and multidimensional chain alignment of polymers for more effective charge transfer and a fine phase-separation between polymers and [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) to favor exciton dissociation and increase the generation rate of charge transfer excitons. Consequently, the power conversion efficiency with a periodic nanostructure was enhanced from 7.40% to 8.50% and 7.17% to 9.15% in PTB7 and PTB7-Th based i-PSCs, respectively.

Effective charge separation in BiOI/Cu2O composites with enhanced photocatalytic activity

NASA Astrophysics Data System (ADS)

Xia, Yongmei; He, Zuming; Yang, Wei; Tang, Bin; Lu, Yalin; Hu, Kejun; Su, Jiangbin; Li, Xiaoping

2018-02-01

Novel BiOI/Cu2O composites were designed and synthesized for the first time by coupling reduction method at low temperature. The samples were characterized by XRD, XPS, SEM, EDS, HRTEM, UV-vis (DRS), FTIR and photo-electro-chemical (PEC) analysis. Results showed that the BiOI/Cu2O composites consisted of three-dimensional (3D), hierarchical cauliflower-like structure composed of BiOI nanosheet and Cu2O cubic submicrometer structure, the composite absorption band broadened, and the absorption intensity in the visible region strengthened. And the composites exhibited an excellent photocatalytic performance, which might be attributed to the improvement of the composite absorption and effective charge separation in BiOI/Cu2O composites. In addition, the possible photocatalytic mechanism was proposed.

High rate lithium-sulfur battery enabled by sandwiched single ion conducting polymer electrolyte

PubMed Central

Sun, Yubao; Li, Gai; Lai, Yuanchu; Zeng, Danli; Cheng, Hansong

2016-01-01

Lithium-sulfur batteries are highly promising for electric energy storage with high energy density, abundant resources and low cost. However, the battery technologies have often suffered from a short cycle life and poor rate stability arising from the well-known “polysulfide shuttle” effect. Here, we report a novel cell design by sandwiching a sp3 boron based single ion conducting polymer electrolyte film between two carbon films to fabricate a composite separator for lithium-sulfur batteries. The dense negative charges uniformly distributed in the electrolyte membrane inherently prohibit transport of polysulfide anions formed in the cathode inside the polymer matrix and effectively blocks polysulfide shuttling. A battery assembled with the composite separator exhibits a remarkably long cycle life at high charge/discharge rates. PMID:26898772

Quantum phase transition and protected ideal transport in a Kondo chain

DOE PAGES

Tsvelik, A. M.; Yevtushenko, O. M.

2015-11-30

We study the low energy physics of a Kondo chain where electrons from a one-dimensional band interact with magnetic moments via an anisotropic exchange interaction. It is demonstrated that the anisotropy gives rise to two different phases which are separated by a quantum phase transition. In the phase with easy plane anisotropy, Z2 symmetry between sectors with different helicity of the electrons is broken. As a result, localization effects are suppressed and the dc transport acquires (partial) symmetry protection. This effect is similar to the protection of the edge transport in time-reversal invariant topological insulators. The phase with easy axismore » anisotropy corresponds to the Tomonaga-Luttinger liquid with a pronounced spin-charge separation. The slow charge density wave modes have no protection against localizatioin.« less

Plasmon-induced charge separation: chemistry and wide applications.

PubMed

Tatsuma, Tetsu; Nishi, Hiroyasu; Ishida, Takuya

2017-05-01

Recent development of nanoplasmonics has stimulated chemists to utilize plasmonic nanomaterials for efficient and distinctive photochemical applications, and physicists to boldly go inside the "wet" chemistry world. The discovery of plasmon-induced charge separation (PICS) has even accelerated these trends. On the other hand, some confusion is found in discussions about PICS. In this perspective, we focus on differences between PICS and some other phenomena such as co-catalysis effect and plasmonic nanoantenna effect. In addition, materials and nanostructures suitable for PICS are shown, and characteristics and features unique to PICS are documented. Although it is well known that PICS has been applied to photovoltaics and photocatalysis, here light is shed on other applications that take better advantage of PICS, such as chemical sensing and biosensing, various photochromisms, photoswitchable functionalities and nanoscale photofabrication.

Early bacteriopheophytin reduction in charge separation in reaction centers of Rhodobacter sphaeroides.

PubMed

Zhu, Jingyi; van Stokkum, Ivo H M; Paparelli, Laura; Jones, Michael R; Groot, Marie Louise

2013-06-04

A question at the forefront of biophysical sciences is, to what extent do quantum effects and protein conformational changes play a role in processes such as biological sensing and energy conversion? At the heart of photosynthetic energy transduction lie processes involving ultrafast energy and electron transfers among a small number of tetrapyrrole pigments embedded in the interior of a protein. In the purple bacterial reaction center (RC), a highly efficient ultrafast charge separation takes place between a pair of bacteriochlorophylls: an accessory bacteriochlorophyll (B) and bacteriopheophytin (H). In this work, we applied ultrafast spectroscopy in the visible and near-infrared spectral region to Rhodobacter sphaeroides RCs to accurately track the timing of the electron on BA and HA via the appearance of the BA and HA anion bands. We observed an unexpectedly early rise of the HA⁻ band that challenges the accepted simple picture of stepwise electron transfer with 3 ps and 1 ps time constants. The implications for the mechanism of initial charge separation in bacterial RCs are discussed in terms of a possible adiabatic electron transfer step between BA and HA, and the effect of protein conformation on the electron transfer rate. Copyright © 2013 Biophysical Society. Published by Elsevier Inc. All rights reserved.

Are Separate Black and White MMPI Norms Needed?: An IQ-Controlled Comparison of Accused Murderers.

ERIC Educational Resources Information Center

Holcomb, William R.; And Others

1984-01-01

Investigated racial differences in the Minnesota Multiphasic Personality Inventory by comparing samples of Black and White men charged with murder (N=160). Results indicated Black murderers tend to deny symptoms of pathology and are more socially outgoing. The confounding effects of intelligence suggested separate Black and White norms are…

Eccentric superconducting RF cavity separator structure

DOEpatents

Aggus, John R.; Giordano, Salvatore T.; Halama, Henry J.

1976-01-01

Accelerator apparatus having an eccentric-shaped, iris-loaded deflecting cavity for an rf separator for a high energy high momentum, charged particle accelerator beam. In one embodiment, the deflector is superconducting, and the apparatus of this invention provides simplified machining and electron beam welding techniques. Model tests have shown that the electrical characteristics provide the desired mode splitting without adverse effects.

Improvement of charge separation in TiO{sub 2} by its modification with different tungsten compounds

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

Tryba, B., E-mail: beata.tryba@zut.edu.pl; Tygielska, M.; Grzeskowiak, M.

2016-04-15

Highlights: • Ammonium m-tungstate doped to TiO{sub 2} highly improved charge separation in TiO{sub 2}. • Negative electrokinetic potential of TiO{sub 2} facilitates holes migration to its surface. • Fast migration of holes to TiO{sub 2} surfaces increased yield of OH radicals formation. • Adsorption of dyes on photocatalyst increased its decomposition under visible light. - Abstract: Three different tungsten precursors were used for TiO{sub 2} modification: H{sub 2}WO{sub 4}, WO{sub 2}, and ammonium m-tungstate. It was proved that modification of TiO{sub 2} with tungsten compounds enhanced its photocatalytic activity through the improvement of charge separation. This effect was obtainedmore » by coating of TiO{sub 2} particles with tungsten compound, which changed their surficial electrokinetical potential from positive onto negative. The most efficient tungsten compound, which caused enhanced separation of free carriers was ammonium m-tungstate (AMT). Two dyes with different ionic potential were used for the photocatalytic decomposition. It appeared that cationic dye—Methylene Blue was highly adsorbed on the negatively charged surface of TiO{sub 2} modified by AMT and decomposed, however this photocatalyst was quickly deactivated whereas anionic dye—acid red was better adsorbed on the less acidic surface of TiO{sub 2} and was rapidly decomposed with almost the same rate in the five following cycles.« less

Utilization of photoinduced charge-separated state of donor-acceptor-linked molecules for regulation of cell membrane potential and ion transport.

PubMed

Numata, Tomohiro; Murakami, Tatsuya; Kawashima, Fumiaki; Morone, Nobuhiro; Heuser, John E; Takano, Yuta; Ohkubo, Kei; Fukuzumi, Shunichi; Mori, Yasuo; Imahori, Hiroshi

2012-04-11

The control of ion transport across cell membranes by light is an attractive strategy that allows targeted, fast control of precisely defined events in the biological membrane. Here we report a novel general strategy for the control of membrane potential and ion transport by using charge-separation molecules and light. Delivery of charge-separation molecules to the plasma membrane of PC12 cells by a membranous nanocarrier and subsequent light irradiation led to depolarization of the membrane potential as well as inhibition of the potassium ion flow across the membrane. Photoregulation of the cell membrane potential and ion transport by using charge-separation molecules is highly promising for control of cell functions. © 2012 American Chemical Society

Facile Synthesis of Ultrafine Hematite Nanowire Arrays in Mixed Water-Ethanol-Acetic Acid Solution for Enhanced Charge Transport and Separation.

PubMed

Wang, Jian; Wang, Menglong; Zhang, Tao; Wang, Zhiqiang; Guo, Penghui; Su, Jinzhan; Guo, Liejin

2018-04-18

Nanostructure engineering is of great significance for semiconductor electrode to achieve high photoelectrochemical performance. Herein, we report a novel strategy to fabricate ultrafine hematite (α-Fe 2 O 3 ) nanowire arrays in a mixed water-ethanol-acetic acid (WEA) solvent. To the best of our knowledge, this is the first report on direct growth of ultrafine (∼10 nm) α-Fe 2 O 3 nanowire arrays on fluorine-doped tin oxide substrates through solution-based fabrication process. The effect of WEA ratio on the morphology of nanowires has been systematically studied to understand the formation mechanism. Photoelectrochemical measurements were conducted on both Ti-treated α-Fe 2 O 3 nanowire and nanorod photoelectrodes. It reveals that α-Fe 2 O 3 nanowire electrode has higher photocurrent and charge separation efficiencies than nanorod electrode if the carrier concentration and space-charge carrier width are in the same order of magnitude. Normalized by electrochemically active surface area, the Ti-treated α-Fe 2 O 3 nanowire electrode obtains 6.4 times higher specific photocurrent density than nanorod electrode. This superiority of nanowires arises from the higher bulk and surface charge separation efficiencies, which could be partly attributed to reduced distance that holes must transfer to reach the semiconductor-liquid junction.

Superior visible light hydrogen evolution of Janus bilayer junctions via atomic-level charge flow steering

NASA Astrophysics Data System (ADS)

Li, Jie; Zhan, Guangming; Yu, Ying; Zhang, Lizhi

2016-05-01

Although photocatalytic hydrogen evolution (PHE) is ideal for solar-to-fuel conversion, it remains challenging to construct a highly efficient PHE system by steering the charge flow in a precise manner. Here we tackle this challenge by assembling 1T MoS2 monolayers selectively and chemically onto (Bi12O17) end-faces of Bi12O17Cl2 monolayers to craft two-dimensional (2D) Janus (Cl2)-(Bi12O17)-(MoS2) bilayer junctions, a new 2D motif different from van der Waals heterostructure. Electrons and holes from visible light-irradiated Bi12O17Cl2 are directionally separated by the internal electric field to (Bi12O17) and (Cl2) end-faces, respectively. The separated electrons can further migrate to MoS2 via Bi-S bonds formed between (Bi12O17) and MoS2 monolayers. This atomic-level directional charge separation endows the Janus bilayers with ultralong carrier lifetime of 3,446 ns and hence a superior visible-light PHE rate of 33 mmol h-1 g-1. Our delineated Janus bilayer junctions on the basis of the oriented assembly of monolayers presents a new design concept to effectively steer the charge flow for PHE.

A semiempirical study for the ground and excited states of free-base and zinc porphyrin-fullerene dyads

NASA Technical Reports Server (NTRS)

Parusel, A. B.

2000-01-01

The ground and excited states of a covalently linked porphyrin-fullerene dyad in both its free-base and zinc forms (D. Kuciauskas et al., J. Phys. Chem. 100 (1996) 15926) have been investigated by semiempirical methods. The excited-state properties are discussed by investigation of the character of the molecular orbitals. All frontier MOs are mainly localized on either the donor or the acceptor subunit. Thus, the absorption spectra of both systems are best described as the sum of the spectra of the single components. The experimentally observed spectra are well reproduced by the theoretical computations. Both molecules undergo efficient electron transfer in polar but not in apolar solvents. This experimental finding is explained theoretically by explicitly considering solvent effects. The tenth excited state in the gas phase is of charge-separated character where an electron is transferred from the porphyrin donor to the fullerene acceptor subunit. This state is stabilized in energy in polar solvents due to its large formal dipole moment. The stabilization energy for an apolar environment such as benzene is not sufficient to lower this state to become the first excited singlet state. Thus, no electron transfer is observed, in agreement with experiment. In a polar environment such as acetonitrile, the charge-separated state becomes the S, state and electron transfer takes place, as observed experimentally. The flexible single bond connecting both the donor and acceptor subunits allows free rotation by ca. +/- 30 degrees about the optimized ground-state conformation. For the charge-separated state this optimized geometry has a maximum dipole moment. The geometry of the charge-separated state thus does not change relatively to the ground-state conformation. The electron-donating properties of porphyrin are enhanced in the zinc derivative due to a reduced porphyrin HOMO-LUMO energy gap. This yields a lower energy for the charge-separated state compared to the free-base dyad.

Electron in higher-dimensional weakly charged rotating black hole spacetimes

NASA Astrophysics Data System (ADS)

Cariglia, Marco; Frolov, Valeri P.; Krtouš, Pavel; Kubizňák, David

2013-03-01

We demonstrate separability of the Dirac equation in weakly charged rotating black hole spacetimes in all dimensions. The electromagnetic field of the black hole is described by a test field approximation, with the vector potential proportional to the primary Killing vector field. It is shown that the demonstrated separability can be intrinsically characterized by the existence of a complete set of mutually commuting first-order symmetry operators generated from the principal Killing-Yano tensor. The presented results generalize the results on integrability of charged particle motion and separability of charged scalar field studied in V. P. Frolov and P. Krtous [Phys. Rev. D 83, 024016 (2011)].

Stability and charge separation of different CH3NH3SnI3/TiO2 interface: A first-principles study

NASA Astrophysics Data System (ADS)

Yang, Zhenzhen; Wang, Yuanxu; Liu, Yunyan

2018-05-01

Interface has an important effect on charge separation of perovskite solar cells. Using first-principles calculations, we studied several different interfaces between CH3NH3SnI3 and TiO2. The interfacial structure and electronic structure of these interfaces are thoroughly explored. We found that the SnI2/anatase (SnI2/A) system is more stable than the other three systems, because an anatase surface can make Snsbnd I bond faster restore to the pristine value than a rutile surface, and SnI2/A system has a smaller standard deviation. The calculated plane-averaged electrostatic potential and the density of states suggest that SnI2/anatase interface has a better separation of photo-generated electron-hole pairs.

Binary Oscillatory Crossflow Electrophoresis

NASA Technical Reports Server (NTRS)

Molloy, Richard F.; Gallagher, Christopher T.; Leighton, David T., Jr.

1997-01-01

Electrophoresis has long been recognized as an effective analytic technique for the separation of proteins and other charged species, however attempts at scaling up to accommodate commercial volumes have met with limited success. In this report we describe a novel electrophoretic separation technique - Binary Oscillatory Crossflow Electrophoresis (BOCE). Numerical simulations indicate that the technique has the potential for preparative scale throughputs with high resolution, while simultaneously avoiding many problems common to conventional electrophoresis. The technique utilizes the interaction of an oscillatory electric field and a transverse oscillatory shear flow to create an active binary filter for the separation of charged protein species. An oscillatory electric field is applied across the narrow gap of a rectangular channel inducing a periodic motion of charged protein species. The amplitude of this motion depends on the dimensionless electrophoretic mobility, alpha = E(sub o)mu/(omega)d, where E(sub o) is the amplitude of the electric field oscillations, mu is the dimensional mobility, omega is the angular frequency of oscillation and d is the channel gap width. An oscillatory shear flow is induced along the length of the channel resulting in the separation of species with different mobilities. We present a model that predicts the oscillatory behavior of charged species and allows estimation of both the magnitude of the induced convective velocity and the effective diffusivity as a function of a in infinitely long channels. Numerical results indicate that in addition to the mobility dependence, the steady state behavior of solute species may be strongly affected by oscillating fluid into and out of the active electric field region at the ends of the cell. The effect is most pronounced using time dependent shear flows of the same frequency (cos((omega)t)) flow mode) as the electric field oscillations. Under such conditions, experiments indicate that solute is drawn into the cell from reservoirs at both ends of the cell leading to a large mass build up. As a consequence, any initially induced mass flux will vanish after short times. This effect was not captured by the infinite channel model and hence numerical and experimental results deviated significantly. The revised model including finite cell lengths and reservoir volumes allowed quantitative predictions of the time history of the concentration profile throughout the system. This latter model accurately describes the fluxes observed for both oscillatory flow modes in experiments using single protein species. Based on the results obtained from research funded under NASA grant NAG-8-1080.S, we conclude that binary separations are not possible using purely oscillatory flow modes because of end effects associated with the cos((omega)t) mode. Our research shows, however, that a combination of cos(2(omega)t) and steady flow should lead to efficient separation free of end effects. This possibility is currently under investigation.

Effect of Charge Patterning on the Phase Behavior of Polymer Coacervates for Charge Driven Self Assembly

NASA Astrophysics Data System (ADS)

Radhakrishna, Mithun; Sing, Charles E.

Oppositely charged polymers can undergo associative liquid-liquid phase separation when mixed under suitable conditions of ionic strength, temperature and pH to form what are known as `polymeric complex coacervates'. Polymer coacervates find use in diverse array of applications like microencapsulation, drug delivery, membrane filtration and underwater adhesives. The similarity between complex coacervate environments and those in biological systems has also found relevance in areas of bio-mimicry. Our previous works have demonstrated how local charge correlations and molecular connectivity can drastically affect the phase behavior of coacervates. The precise location of charges along the chain therefore dramatically influences the local charge correlations, which consequently influences the phase behavior of coacervates. We investigate the effect of charge patterning along the polymer chain on the phase behavior of coacervates in the framework of the Restricted Primitive Model using Gibbs Ensemble Monte Carlo simulations. Our results show that charge patterning dramatically changes the phase behavior of polymer coacervates, which contrasts with the predictions of the classical Voorn-Overbeek theory. This provides the basis for designing new materials through charge driven self assembly by controlling the positioning of the charged monomers along the chain.

The CE-Way of Thinking: "All Is Relative!".

PubMed

Schmitt-Kopplin, Philippe; Fekete, Agnes

2016-01-01

Over the last two decades the development of capillary electrophoresis instruments lead to systems with programmable sampler, separation column, separation buffer, and detection devices comparable visually in many aspects to the setup of classical chromatography.Two processes make capillary electrophoresis essentially different from chromatography and are the basis of the CE-way of thinking, namely, the injection type and the liquid flow within the capillary. (1) When the injection is made hydrodynamically (such as in most of the found applications in the literature), the injected volumes are directly dependent on the type and size of the separation capillary. (2) The buffer velocity is not pressure driven as in liquid chromatography but electrokinetically governed by the quality of the capillary surface (separation buffer dependant surface charge) inducing an electroosmotic flow (EOF). The EOF undergoes small variations and is not necessarily identical from one separation or day to the other. The direct consequence is an apparent nonreproducible migration time of the analytes, even though the own velocity of the ions is the same.The effective mobility (field strength normalized velocity) of the ions is a possible parameterization from acquired timescale to effective mobility-scale electropherograms leading to a reproducible visualization and better quantification with a direct relation to structural characters of the analytes (i.e., charge and size-see chapter on semiempirical modelization).

Electric Double-Layer Interaction between Dissimilar Charge-Conserved Conducting Plates.

PubMed

Chan, Derek Y C

2015-09-15

Small metallic particles used in forming nanostructured to impart novel optical, catalytic, or tribo-rheological can be modeled as conducting particles with equipotential surfaces that carry a net surface charge. The value of the surface potential will vary with the separation between interacting particles, and in the absence of charge-transfer or electrochemical reactions across the particle surface, the total charge of each particle must also remain constant. These two physical conditions require the electrostatic boundary condition for metallic nanoparticles to satisfy an equipotential whole-of-particle charge conservation constraint that has not been studied previously. This constraint gives rise to a global charge conserved constant potential boundary condition that results in multibody effects in the electric double-layer interaction that are either absent or are very small in the familiar constant potential or constant charge or surface electrochemical equilibrium condition.

The physics of charge separation preceding lightning strokes in thunderclouds

NASA Technical Reports Server (NTRS)

Kyrala, Ali

1987-01-01

The physics of charge separation preceding lightning strokes in thunderclouds is presented by three types of arguments: An explanation is given for the aggregation of electrical charges of like sign overcoming Coulomb repulsion by attraction due to exchange interaction. The latter is well known in quantum mechanics from the theories of the nuclear bond and the covalent bond. A classical electrostatic model of charge balls of segregated positive and negative charges in the thundercloud is presented. These charge balls can only be maintained in temporarily stable locations by a containing vortex. Because they will be of different sizes and masses, they will stabilize at different altitudes when drag forces are included with the given electrostatic force. The question of how the charges become concentrated again after lightning discharges is approached by means of the collisional Boltzmann transport equation to explain quasi-periodic recharging. It is shown that solutions cannot be separable in both position and time if they are to represent aggregation.

Directional Charge Separation in Isolated Organic Semiconductor Crystalline Nanowires

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

Barnes, Michael; Labastide, Joelle; Bond-Thompson, Hilary

2017-03-01

In the conventional view of organic photovoltaics (OPV), localized electronic excitations (excitons) formed in the active layer are transported by random 3D diffusion to an interface where charge separation and extraction take place. Because radiative de-excitation is usually strongly allowed in organic semiconductors, efficient charge separation requires high exciton mobility, with much of the diffusive motion ‘wasted’ in directions that don’t result in an interface encounter. Our research efforts are focused on ways to enforce a preferred directionality in energy and/or charge transport using ordered crystalline nanowires in which the intermolecular interactions that facilitate transport along, for example, the pi-stackingmore » axis, can be made several orders of magnitude stronger than those in a transverse direction. The results presented in our recent work (Nature Communications) is a first step towards realizing the goal of directional control of both energy transport and charge separation, where excitons shared between adjacent molecules dissociate exclusively along the pi-stacking direction.« less

Charge-specific size-dependent separation of water-soluble organic molecules by fluorinated nanoporous networks

NASA Astrophysics Data System (ADS)

Byun, Jeehye; Patel, Hasmukh A.; Thirion, Damien; Yavuz, Cafer T.

2016-11-01

Molecular architecture in nanoscale spaces can lead to selective chemical interactions and separation of species with similar sizes and functionality. Substrate specific sorbent chemistry is well known through highly crystalline ordered structures such as zeolites, metal organic frameworks and widely available nanoporous carbons. Size and charge-dependent separation of aqueous molecular contaminants, on the contrary, have not been adequately developed. Here we report a charge-specific size-dependent separation of water-soluble molecules through an ultra-microporous polymeric network that features fluorines as the predominant surface functional groups. Treatment of similarly sized organic molecules with and without charges shows that fluorine interacts with charges favourably. Control experiments using similarly constructed frameworks with or without fluorines verify the fluorine-cation interactions. Lack of a σ-hole for fluorine atoms is suggested to be responsible for this distinct property, and future applications of this discovery, such as desalination and mixed matrix membranes, may be expected to follow.

Charge-specific size-dependent separation of water-soluble organic molecules by fluorinated nanoporous networks

PubMed Central

Byun, Jeehye; Patel, Hasmukh A.; Thirion, Damien; Yavuz, Cafer T.

2016-01-01

Molecular architecture in nanoscale spaces can lead to selective chemical interactions and separation of species with similar sizes and functionality. Substrate specific sorbent chemistry is well known through highly crystalline ordered structures such as zeolites, metal organic frameworks and widely available nanoporous carbons. Size and charge-dependent separation of aqueous molecular contaminants, on the contrary, have not been adequately developed. Here we report a charge-specific size-dependent separation of water-soluble molecules through an ultra-microporous polymeric network that features fluorines as the predominant surface functional groups. Treatment of similarly sized organic molecules with and without charges shows that fluorine interacts with charges favourably. Control experiments using similarly constructed frameworks with or without fluorines verify the fluorine-cation interactions. Lack of a σ-hole for fluorine atoms is suggested to be responsible for this distinct property, and future applications of this discovery, such as desalination and mixed matrix membranes, may be expected to follow. PMID:27830697

Effect of Reduced Flux Iron Ore Pellets on Removal of Impurities from Pig Iron During Induction Melting: A New Phenomenon

NASA Astrophysics Data System (ADS)

Dishwar, Raj Kumar; Agrawal, Shavi; Mandal, A. K.; Mahobia, G. S.; Sinha, O. P.

2018-06-01

The present work represents a comparative study of impurity removal (sulfur, phosphorus, and carbon) from pig iron melt by the addition of lime powder and reduced fluxed iron ore pellets separately in a 5-kg-capacity induction melting furnace. Two types of reduced flux pellets (80% and 50%) of similar basicity ( 3.06) were charged separately into the pool to obtain the different oxidizing atmospheres of the bath. Results showed that the rate of impurity removal increases up to 6 min of exposure time and decreases afterward. Only lime powder charging, sulfur ( 77%), and a small fraction of carbon were removed from pig iron. Phosphorous ( 41%), sulfur ( 53%), and carbon ( 96%) were removed simultaneously when 80% reduced fluxed pellets were used. The present study indicates that the optimum removal of impurities is possible by charging 80% reduced flux iron ore pellets from the pig iron melt.

Possible origin and roles of nano-porosity in ZrO2 scales for hydrogen pick-up in Zr alloys

NASA Astrophysics Data System (ADS)

Lindgren, Mikaela; Geers, Christine; Panas, Itai

2017-08-01

A mechanistic understanding of Wagnerian build-up and subsequent non-Wagnerian break-down of barrier oxide upon oxidation of zirconium alloys by water is reiterated. Hydrogen assisted build-up of nano-porosity is addressed. Growth of sub-nanometer wide stalactitic pores owing to increasing aggregation of neutral oxygen vacancies offering a means to permeate hydrogen into the alloy is explored by density functional theory. The Wagnerian channel utilizes charge separation allowing charged oxygen vacancies and electrons to move separately from nominal anode to nominal cathode. This process becomes increasingly controlled by the charging of the barrier oxide resulting in sub-parabolic rate law for oxide growth. The break-down of the barrier oxide is understood to be preceded by avalanching hydrogen pick-up in the alloy. Pore mediated diffusion allows water to effectively short circuit the barrier oxide.

Multiple exciton dissociation in CdSe quantum dots by ultrafast electron transfer to adsorbed methylene blue.

PubMed

Huang, Jier; Huang, Zhuangqun; Yang, Ye; Zhu, Haiming; Lian, Tianquan

2010-04-07

Multiexciton generation in quantum dots (QDs) may provide a new approach for improving the solar-to-electric power conversion efficiency in QD-based solar cells. However, it remains unclear how to extract these excitons before the ultrafast exciton-exciton annihilation process. In this study we investigate multiexciton dissociation dynamics in CdSe QDs adsorbed with methylene blue (MB(+)) molecules by transient absorption spectroscopy. We show that excitons in QDs dissociate by ultrafast electron transfer to MB(+) with an average time constant of approximately 2 ps. The charge separated state is long-lived (>1 ns), and the charge recombination rate increases with the number of dissociated excitons. Up to three MB(+) molecules per QD can be reduced by exciton dissociation. Our result demonstrates that ultrafast interfacial charge separation can effectively compete with exciton-exciton annihilation, providing a viable approach for utilizing short-lived multiple excitons in QDs.

Statistical patterns in the location of natural lightning

NASA Astrophysics Data System (ADS)

Zoghzoghy, F. G.; Cohen, M. B.; Said, R. K.; Inan, U. S.

2013-01-01

Lightning discharges are nature's way of neutralizing the electrical buildup in thunderclouds. Thus, if an individual discharge destroys a substantial fraction of the cloud charge, the probability of a subsequent flash is reduced until the cloud charge separation rebuilds. The temporal pattern of lightning activity in a localized region may thus inherently be a proxy measure of the corresponding timescales for charge separation and electric field buildup processes. We present a statistical technique to bring out this effect (as well as the subsequent recovery) using lightning geo-location data, in this case with data from the National Lightning Detection Network (NLDN) and from the GLD360 Network. We use this statistical method to show that a lightning flash can remove an appreciable fraction of the built up charge, affecting the neighboring lightning activity for tens of seconds within a ˜ 10 km radius. We find that our results correlate with timescales of electric field buildup in storms and suggest that the proposed statistical tool could be used to study the electrification of storms on a global scale. We find that this flash suppression effect is a strong function of flash type, flash polarity, cloud-to-ground flash multiplicity, the geographic location of lightning, and is proportional to NLDN model-derived peak stroke current. We characterize the spatial and temporal extent of the suppression effect as a function of these parameters and discuss various applications of our findings.

Electrostatic potential of B-DNA: effect of interionic correlations.

PubMed Central

Gavryushov, S; Zielenkiewicz, P

1998-01-01

Modified Poisson-Boltzmann (MPB) equations have been numerically solved to study ionic distributions and mean electrostatic potentials around a macromolecule of arbitrarily complex shape and charge distribution. Results for DNA are compared with those obtained by classical Poisson-Boltzmann (PB) calculations. The comparisons were made for 1:1 and 2:1 electrolytes at ionic strengths up to 1 M. It is found that ion-image charge interactions and interionic correlations, which are neglected by the PB equation, have relatively weak effects on the electrostatic potential at charged groups of the DNA. The PB equation predicts errors in the long-range electrostatic part of the free energy that are only approximately 1.5 kJ/mol per nucleotide even in the case of an asymmetrical electrolyte. In contrast, the spatial correlations between ions drastically affect the electrostatic potential at significant separations from the macromolecule leading to a clearly predicted effect of charge overneutralization. PMID:9826596

Stochastic heating of a single Brownian particle by charge fluctuations in a radio-frequency produced plasma sheath

NASA Astrophysics Data System (ADS)

Schmidt, Christian; Piel, Alexander

2015-10-01

The Brownian motion of a single particle in the plasma sheath is studied to separate the effect of stochastic heating by charge fluctuations from heating by collective effects. By measuring the particle velocities in the ballistic regime and by carefully determining the particle mass from the Epstein drag it is shown that for a pressure of 10 Pa, which is typical of many experiments, the proper kinetic temperature of the Brownian particle remains close to the gas temperature and rises only slightly with particle size. This weak effect is confirmed by a detailed model for charging and charge fluctuations in the sheath. A substantial temperature rise is found for decreasing pressure, which approximately shows the expected scaling with p-2. The system under study is an example for non-equilibrium Brownian motion under the influence of white noise without corresponding dissipation.

Electroosmotic flow in a microcavity with nonuniform surface charges.

PubMed

Halpern, David; Wei, Hsien-Hung

2007-08-28

In this work, we theoretically explore the characteristics of electroosmostic flow (EOF) in a microcavity with nonuniform surface charges. It is well known that a uniformly charged EOF does not give rise to flow separation because of its irrotational nature, as opposed to the classical problem of viscous flow past a cavity. However, if the cavity walls bear nonuniform surface charges, then the similitude between electric and flow fields breaks down, leading to the generation of vorticity in the cavity. Because this vorticity must necessarily diffuse into the exterior region that possesses a zero vorticity set by a uniform EOF, a new flow structure emerges. Assuming Stokes flow, we employ a boundary element method to explore how a nonuniform charge distribution along the cavity surface affects the flow structure. The results show that the stream can be susceptible to flow separation and exhibits a variety of flow structures, depending on the distributions of zeta potentials and the aspect ratio of the cavity. The interactions between patterned EOF vortices and Moffatt eddies are further demonstrated for deep cavities. This work not only has implications for electrokinetic flow induced by surface imperfections but also provides optimal strategies for achieving effective mixing in microgrooves.

Effects of granular charge on flow and mixing

NASA Astrophysics Data System (ADS)

Shinbrot, T.; Herrmann, H. J.

2008-12-01

Sandstorms in the desert have long been reported to produce sparks and other electrical disturbances - indeed as long ago as 1850, Faraday commented on the peculiarities of granular charging during desert sandstorms. Similarly, lightning strikes within volcanic dust plumes have been repeatedly reported for over half a century, but remain unexplained. The problem of granular charging has applied, as well as natural, implications, for charged particle clouds frequently generate spectacularly devastating dust explosions in granular processing plants, and sand becomes strongly electrified by helicopters traveling in desert environments. The issue even has implications for missions to the Moon and to Mars, where charged dust degrades solar cells viability and clings to spacesuits, limiting the lifetime of their joints. Despite the wide-ranging importance of granular charging, even the simplest aspects of its causes remain elusive. To take one example, sand grains in the desert manage to charge one another despite having only similar materials to rub against over expanses of many miles - thus existing theories of charging due to material differences fail entirely to account for the observed charging of desert sands. In this talk, we describe recent progress made in identifying underlying causes of granular charging, both in desert-like environments and in industrial applications, and we examine effects of granular charging on flow, mixing and separation of common granular materials. We find that charging of identical grains can occur under simple laboratory conditions, and we make new predictions for the effects of this charging on granular behaviours.

Charge and spin in low-dimensional cuprates

NASA Astrophysics Data System (ADS)

Maekawa, Sadamichi; Tohyama, Takami

2001-03-01

One of the central issues in the study of high-temperature superconducting cuprates which are composed of two-dimensional (2D) CuO2 planes is whether the 2D systems with strong electron correlation behave as a Fermi liquid or a non-Fermi-liquid-like one-dimensional (1D) system with electron correlation. In this article, we start with the detailed examination of the electronic structure in cuprates and study theoretically the spin and charge dynamics in 1D and 2D cuprates. The theoretical background of spin-charge separation in the 1D model systems including the Hubbard and t-J models is presented. The first direct observation of collective modes of spin and charge excitations in a 1D cuprate, which are called spinons and holons respectively, in angle-resolved photoemission spectroscopy (ARPES) experiments is reviewed in the light of the theoretical results based on the numerically exact-diagonalization method. The charge and spin dynamics in 1D insulating cuprates is also discussed in connection with the spin-charge separation. The arguments are extended to the 2D cuprates, and the unique aspects of the electronic properties of high-temperature superconductors are discussed. Special emphasis is placed on the d-wave-like excitations in insulating 2D cuprates observed in ARPES experiments. We explain how the excitations are caused by the spin-charge separation. The charge stripes observed in the underdoped cuprates are examined in connection with spin-charge separation in real space.

Computational modeling of electrostatic charge and fields produced by hypervelocity impact

DOE PAGES

Crawford, David A.

2015-05-19

Following prior experimental evidence of electrostatic charge separation, electric and magnetic fields produced by hypervelocity impact, we have developed a model of electrostatic charge separation based on plasma sheath theory and implemented it into the CTH shock physics code. Preliminary assessment of the model shows good qualitative and quantitative agreement between the model and prior experiments at least in the hypervelocity regime for the porous carbonate material tested. The model agrees with the scaling analysis of experimental data performed in the prior work, suggesting that electric charge separation and the resulting electric and magnetic fields can be a substantial effectmore » at larger scales, higher impact velocities, or both.« less

Plasmon-induced charge separation: chemistry and wide applications

PubMed Central

Nishi, Hiroyasu; Ishida, Takuya

2017-01-01

Recent development of nanoplasmonics has stimulated chemists to utilize plasmonic nanomaterials for efficient and distinctive photochemical applications, and physicists to boldly go inside the “wet” chemistry world. The discovery of plasmon-induced charge separation (PICS) has even accelerated these trends. On the other hand, some confusion is found in discussions about PICS. In this perspective, we focus on differences between PICS and some other phenomena such as co-catalysis effect and plasmonic nanoantenna effect. In addition, materials and nanostructures suitable for PICS are shown, and characteristics and features unique to PICS are documented. Although it is well known that PICS has been applied to photovoltaics and photocatalysis, here light is shed on other applications that take better advantage of PICS, such as chemical sensing and biosensing, various photochromisms, photoswitchable functionalities and nanoscale photofabrication. PMID:28507702

Cell and Particle Interactions and Aggregation During Electrophoretic Motion

NASA Technical Reports Server (NTRS)

Davis, Robert H.

2000-01-01

The objectives of this research were (i) to perform experiments for observing and quantifying electrophoretic aggregation, (ii) to develop a theoretical description to appropriately analyze and compare with the experimental results, (iii) to study the combined effects of electrophoretic and gravitational aggregation of large particles, and the combined effects of electrophoretic and Brownian aggregation of small particles, and (iv) to perform a preliminary design of a potential future flight experiment involving electrophoretic aggregation. Electrophoresis refers to the motion of charged particles, droplets or molecules in response to an applied electric field. Electrophoresis is commonly used for analysis and separation of biological particles or molecules. When particles have different surface charge densities or potentials, they will migrate at different velocities in an electric field. This differential migration leads to the possibility that they will collide and aggregate, thereby preventing separation.

A charge-stabilizing, multimodular, ferrocene-bis(triphenylamine)-zinc-porphyrin-fullerene polyad.

PubMed

Wijesinghe, Channa A; El-Khouly, Mohamed E; Zandler, Melvin E; Fukuzumi, Shunichi; D'Souza, Francis

2013-07-15

A novel multimodular donor-acceptor polyad featuring zinc porphyrin, fullerene, ferrocene, and triphenylamine entities was designed, synthesized, and studied as a charge-stabilizing, photosynthetic-antenna/reaction-center mimic. The ferrocene and fullerene entities, covalently linked to the porphyrin ring, were distantly separated to accomplish the charge-separation/hole-migration events leading to the creation of a long-lived charge-separated state. The geometry and electronic structures of the newly synthesized compound was deduced by B3LYP/3-21G(*) optimization, while the energy levels for different photochemical events was established using data from the optical absorption and emission, and electrochemical studies. Excitation of the triphenylamine entities revealed singlet-singlet energy transfer to the appended zinc porphyrin. As predicted from the energy levels, photoinduced electron transfer from both the singlet and triplet excited states of the zinc porphyrin to fullerene followed by subsequent hole migration involving ferrocene was witnessed from the transient absorption studies. The charge-separated state persisted for about 8.5 μs and was governed by the distance between the final charge-transfer product, that is, a species involving a ferrocenium cation and a fullerene radical anion, with additional influence from the charge-stabilizing triphenylamine entities located on the zinc-porphyrin macrocycle. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Interfacial disorder drives charge separation in molecular semiconductors

NASA Astrophysics Data System (ADS)

Willard, Adam

One of the fundamental microscopic processes in photocurrent generation is the dissociation of neutral photo-excitations (i.e., Frenkel excitons) into free charge carriers (i.e., electrons and holes). This process requires the physical separation of oppositely charged electrons and holes, which are held to together by an attractive electrostatic binding energy. In traditional inorganic-based photovoltaic (PV) materials, this binding energy is generally small and easily overcome, however, in organic-based PVs (OPVs) the exciton binding energy can significantly exceed thermal energies. The inability of bound charges to overcome this large binding energy has been implicated as a primary source of efficiency loss in OPVs. Here I present results from our recent efforts to explore the role of static molecular disorder in mediating this process. Using a simple lattice model of exciton dynamics we demonstrate that random spatial variations in the energetic landscape can mitigate the attractive Coulomb interaction between electrons and holes. We show that this effect manifests as a reduction in the free energy barrier for exciton dissociation that grows more pronounced with increasing disorder. By considering the competition between this thermodynamic effect and the disorder-induced slowing of dissociation kinetics we demonstrate that exciton dissociation yields are expected to depend non-monotonically on the degree of static disorder.

Photochemical charge separation in zeolites: Electron transfer dynamics, nanocrystals and zeolitic membranes. Final technical report

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

Dutta, Prabir K.

2001-09-30

Aluminosilicate zeolites provide an excellent host for photochemical charge separation. Because of the constraints provided by the zeolite, the back electron transfer from the reduced acceptor to the oxidized sensitizer is slowed down. This provides the opportunity to separate the charge and use it in a subsequent reaction for water oxidation and reduction. Zeolite-based ruthenium oxide catalysts have been found to be efficient for the water splitting process. This project has demonstrated the usefulness of zeolite hosts for photolytic splitting of water.

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.

Ultrafast photoinduced charge separation in metal-semiconductor nanohybrids.

PubMed

Mongin, Denis; Shaviv, Ehud; Maioli, Paolo; Crut, Aurélien; Banin, Uri; Del Fatti, Natalia; Vallée, Fabrice

2012-08-28

Hybrid nano-objects formed by two or more disparate materials are among the most promising and versatile nanosystems. A key parameter in their properties is interaction between their components. In this context we have investigated ultrafast charge separation in semiconductor-metal nanohybrids using a model system of gold-tipped CdS nanorods in a matchstick architecture. Experiments are performed using an optical time-resolved pump-probe technique, exciting either the semiconductor or the metal component of the particles, and probing the light-induced change of their optical response. Electron-hole pairs photoexcited in the semiconductor part of the nanohybrids are shown to undergo rapid charge separation with the electron transferred to the metal part on a sub-20 fs time scale. This ultrafast gold charging leads to a transient red-shift and broadening of the metal surface plasmon resonance, in agreement with results for free clusters but in contrast to observation for static charging of gold nanoparticles in liquid environments. Quantitative comparison with a theoretical model is in excellent agreement with the experimental results, confirming photoexcitation of one electron-hole pair per nanohybrid followed by ultrafast charge separation. The results also point to the utilization of such metal-semiconductor nanohybrids in light-harvesting applications and in photocatalysis.

Discrete space charge affected field emission: Flat and hemisphere emitters

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

Jensen, Kevin L., E-mail: kevin.jensen@nrl.navy.mil; Shiffler, Donald A.; Tang, Wilkin

Models of space-charge affected thermal-field emission from protrusions, able to incorporate the effects of both surface roughness and elongated field emitter structures in beam optics codes, are desirable but difficult. The models proposed here treat the meso-scale diode region separate from the micro-scale regions characteristic of the emission sites. The consequences of discrete emission events are given for both one-dimensional (sheets of charge) and three dimensional (rings of charge) models: in the former, results converge to steady state conditions found by theory (e.g., Rokhlenko et al. [J. Appl. Phys. 107, 014904 (2010)]) but show oscillatory structure as they do. Surfacemore » roughness or geometric features are handled using a ring of charge model, from which the image charges are found and used to modify the apex field and emitted current. The roughness model is shown to have additional constraints related to the discrete nature of electron charge. The ability of a unit cell model to treat field emitter structures and incorporate surface roughness effects inside a beam optics code is assessed.« less

Predictions for isobaric collisions at √{sN N}=200 GeV from a multiphase transport model

NASA Astrophysics Data System (ADS)

Deng, Wei-Tian; Huang, Xu-Guang; Ma, Guo-Liang; Wang, Gang

2018-04-01

The isobaric collisions of Ru9644+Ru9644 and Zr9640+Zr9640 have recently been proposed to discern the charge separation signal of the chiral magnetic effect (CME). In this article, we employ the string melting version of a multiphase transport model to predict various charged-particle observables, including d N /d η ,pT spectra, elliptic flow (v2), and particularly possible CME signals in Ru + Ru and Zr + Zr collisions at √{sNN}=200 GeV . Two sets of the nuclear structure parametrization have been explored, and the difference between the two isobaric collisions appears to be small, in terms of d N /d η ,pT spectra, and v2 for charged particles. We mimic the CME by introducing an initial charge separation that is proportional to the magnetic field produced in the collision, and study how the final-state interactions affect the CME observables. The relative difference in the CME signal between the two isobaric collisions is found to be robust, insensitive to the final-state interactions.

Simulations of stretching a flexible polyelectrolyte with varying charge separation

DOE PAGES

Stevens, Mark J.; Saleh, Omar A.

2016-07-22

We calculated the force-extension curves for a flexible polyelectrolyte chain with varying charge separations by performing Monte Carlo simulations of a 5000 bead chain using a screened Coulomb interaction. At all charge separations, the force-extension curves exhibit a Pincus-like scaling regime at intermediate forces and a logarithmic regime at large forces. As the charge separation increases, the Pincus regime shifts to a larger range of forces and the logarithmic regime starts are larger forces. We also found that force-extension curve for the corresponding neutral chain has a logarithmic regime. Decreasing the diameter of bead in the neutral chain simulations removedmore » the logarithmic regime, and the force-extension curve tends to the freely jointed chain limit. In conclusion, this result shows that only excluded volume is required for the high force logarithmic regime to occur.« less

Protein separation using an electrically tunable membrane

NASA Astrophysics Data System (ADS)

Jou, Ining; Melnikov, Dmitriy; Gracheva, Maria

Separation of small proteins by charge with a solid-state porous membrane requires control over the protein's movement. Semiconductor membrane has this ability due to the electrically tunable electric potential profile inside the nanopore. In this work we investigate the possibility to separate the solution of two similar sized proteins by charge. As an example, we consider two small globular proteins abundant in humans: insulin (negatively charged) and ubiquitin (neutral). We find that the localized electric field inside the pore either attracts or repels the charged protein to or from the pore wall which affects the delay time before a successful translocation of the protein through the nanopore. However, the motion of the uncharged ubiquitin is unaffected. The difference in the delay time (and hence the separation) can be further increased by the application of the electrolyte bias which induces an electroosmotic flow in the pore. NSF DMR and CBET Grant No. 1352218.

Improved solar-driven photocatalytic performance of Ag{sub 2}CO{sub 3}/(BiO){sub 2}CO{sub 3} prepared in-situ

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

Zhong, Junbo, E-mail: junbozhong@163.com; Li, Jianzhang, E-mail: lschmanuscript@163.com; Huang, Shengtian

Highlights: • Ag{sub 2}CO{sub 3}/(BiO){sub 2}CO{sub 3} photocatalysts were prepared in-situ. • The photo-induced charge separation rate has been greatly increased. • The photocatalytic activity has been greatly promoted. - Abstract: Ag{sub 2}CO{sub 3}/(BiO){sub 2}CO{sub 3} composites have been fabricated in-situ via a facile parallel flaw co-precipitation method. The specific surface area, structure, morphology, and the separation rate of photo-induced charge pairs of the photocatalysts were characterized by Brunauer–Emmett–Teller (BET) method, X-ray diffraction (XRD), UV–vis diffuse reflectance spectroscopy(DRS), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), and surface photovoltage (SPV) spectroscopy, respectively. XRD patterns and DRS demonstrated that Ag{submore » 2}CO{sub 3} has no effect on the crystal phase and bandgap of (BiO){sub 2}CO{sub 3}. The existence of Ag{sub 2}CO{sub 3} in the composites enhances the separation rate of photo-induced charge pairs of the photocatalysts. The photocatalytic performance of Ag{sub 2}CO{sub 3}/(BiO){sub 2}CO{sub 3} was evaluated by the decolorization of methyl orange (MO) aqueous solution under simulated solar irradiation. It was found that the simulated solar-induced photocatalytic activity of Ag{sub 2}CO{sub 3}/(BiO){sub 2}CO{sub 3} copmposites was significantly improved, which was mainly attributed to the enhanced surface area and the separation rate of photo-induced charge pairs.« less

Behavior of a spin-1/2 massive charged particle in Schwarzschild immersed in an electromagnetic universe

NASA Astrophysics Data System (ADS)

Al-Badawi, A.

2018-02-01

The Dirac equation is considered in a spacetime that represents a Schwarzschild metric coupled to a uniform external electromagnetic field. Due to the presence of electromagnetic field from the surroundings, the interaction with the spin-1/2 massive charged particle is considered. The equations of the spin-1/2 massive charged particle are separated into radial and angular equations by adopting the Newman-Penrose formalism. The angular equations obtained are similar to the Schwarzschild geometry. For the radial equations we manage to obtain the one dimensional Schrödinger-type wave equations with effective potentials. Finally, we study the behavior of the potentials by plotting them as a function of radial distance and expose the effect of the external parameter, charge and the frequency of the particle on them.

Charge pattern matching as a ‘fuzzy’ mode of molecular recognition for the functional phase separations of intrinsically disordered proteins

NASA Astrophysics Data System (ADS)

Lin, Yi-Hsuan; Brady, Jacob P.; Forman-Kay, Julie D.; Chan, Hue Sun

2017-11-01

Biologically functional liquid-liquid phase separation of intrinsically disordered proteins (IDPs) is driven by interactions encoded by their amino acid sequences. Little is currently known about the molecular recognition mechanisms for distributing different IDP sequences into various cellular membraneless compartments. Pertinent physics was addressed recently by applying random-phase-approximation (RPA) polymer theory to electrostatics, which is a major energetic component governing IDP phase properties. RPA accounts for charge patterns and thus has advantages over Flory-Huggins (FH) and Overbeek-Voorn mean-field theories. To make progress toward deciphering the phase behaviors of multiple IDP sequences, the RPA formulation for one IDP species plus solvent is hereby extended to treat polyampholyte solutions containing two IDP species plus solvent. The new formulation generally allows for binary coexistence of two phases, each containing a different set of volume fractions ({φ }1,{φ }2) for the two different IDP sequences. The asymmetry between the two predicted coexisting phases with regard to their {φ }1/{φ }2 ratios for the two sequences increases with increasing mismatch between their charge patterns. This finding points to a multivalent, stochastic, ‘fuzzy’ mode of molecular recognition that helps populate various IDP sequences differentially into separate phase compartments. An intuitive illustration of this trend is provided by FH models, whereby a hypothetical case of ternary coexistence is also explored. Augmentations of the present RPA theory with a relative permittivity {ɛ }{{r}}(φ ) that depends on IDP volume fraction φ ={φ }1+{φ }2 lead to higher propensities to phase separate, in line with the case with one IDP species we studied previously. Notably, the cooperative, phase-separation-enhancing effects predicted by the prescriptions for {ɛ }{{r}}(φ ) we deem physically plausible are much more prominent than that entailed by common effective medium approximations based on Maxwell Garnett and Bruggeman mixing formulas. Ramifications of our findings on further theoretical development for IDP phase separation are discussed.

Calculation of rates of exciton dissociation into hot charge-transfer states in model organic photovoltaic interfaces

NASA Astrophysics Data System (ADS)

Vázquez, Héctor; Troisi, Alessandro

2013-11-01

We investigate the process of exciton dissociation in ordered and disordered model donor/acceptor systems and describe a method to calculate exciton dissociation rates. We consider a one-dimensional system with Frenkel states in the donor material and states where charge transfer has taken place between donor and acceptor. We introduce a Green's function approach to calculate the generation rates of charge-transfer states. For disorder in the Frenkel states we find a clear exponential dependence of charge dissociation rates with exciton-interface distance, with a distance decay constant β that increases linearly with the amount of disorder. Disorder in the parameters that describe (final) charge-transfer states has little effect on the rates. Exciton dissociation invariably leads to partially separated charges. In all cases final states are “hot” charge-transfer states, with electron and hole located far from the interface.

Charge exchange molecular ion source

DOEpatents

Vella, Michael C.

2003-06-03

Ions, particularly molecular ions with multiple dopant nucleons per ion, are produced by charge exchange. An ion source contains a minimum of two regions separated by a physical barrier and utilizes charge exchange to enhance production of a desired ion species. The essential elements are a plasma chamber for production of ions of a first species, a physical separator, and a charge transfer chamber where ions of the first species from the plasma chamber undergo charge exchange or transfer with the reactant atom or molecules to produce ions of a second species. Molecular ions may be produced which are useful for ion implantation.

Characterization and correction of charge-induced pixel shifts in DECam

DOE PAGES

Gruen, D.; Bernstein, G. M.; Jarvis, M.; ...

2015-05-28

Interaction of charges in CCDs with the already accumulated charge distribution causes both a flux dependence of the point-spread function (an increase of observed size with flux, also known as the brighter/fatter effect) and pixel-to-pixel correlations of the Poissonian noise in flat fields. We describe these effects in the Dark Energy Camera (DECam) with charge dependent shifts of effective pixel borders, i.e. the Antilogus et al. (2014) model, which we fit to measurements of flat-field Poissonian noise correlations. The latter fall off approximately as a power-law r -2.5 with pixel separation r, are isotropic except for an asymmetry in themore » direct neighbors along rows and columns, are stable in time, and are weakly dependent on wavelength. They show variations from chip to chip at the 20% level that correlate with the silicon resistivity. The charge shifts predicted by the model cause biased shape measurements, primarily due to their effect on bright stars, at levels exceeding weak lensing science requirements. We measure the flux dependence of star images and show that the effect can be mitigated by applying the reverse charge shifts at the pixel level during image processing. Differences in stellar size, however, remain significant due to residuals at larger distance from the centroid.« less

Induced-Charge Enhancement of the Diffusion Potential in Membranes with Polarizable Nanopores

NASA Astrophysics Data System (ADS)

Ryzhkov, I. I.; Lebedev, D. V.; Solodovnichenko, V. S.; Shiverskiy, A. V.; Simunin, M. M.

2017-12-01

When a charged membrane separates two salt solutions of different concentrations, a potential difference appears due to interfacial Donnan equilibrium and the diffusion junction. Here, we report a new mechanism for the generation of a membrane potential in polarizable conductive membranes via an induced surface charge. It results from an electric field generated by the diffusion of ions with different mobilities. For uncharged membranes, this effect strongly enhances the diffusion potential and makes it highly sensitive to the ion mobilities ratio, electrolyte concentration, and pore size. Theoretical predictions on the basis of the space-charge model extended to polarizable nanopores fully agree with experimental measurements in KCl and NaCl aqueous solutions.

Separation of heat and charge currents for boosted thermoelectric conversion

NASA Astrophysics Data System (ADS)

Mazza, Francesco; Valentini, Stefano; Bosisio, Riccardo; Benenti, Giuliano; Giovannetti, Vittorio; Fazio, Rosario; Taddei, Fabio

2015-06-01

In a multiterminal device the (electronic) heat and charge currents can follow different paths. In this paper we introduce and analyze a class of multiterminal devices where this property is pushed to its extreme limits, with charge and heat currents flowing in different reservoirs. After introducing the main characteristics of this heat-charge current separation regime, we show how to realize it in a multiterminal device with normal and superconducting leads. We demonstrate that this regime allows us to control independently heat and charge flows and to greatly enhance thermoelectric performances at low temperatures. We analyze in detail a three-terminal setup involving a superconducting lead, a normal lead, and a voltage probe. For a generic scattering region we show that in the regime of heat-charge current separation both the power factor and the figure of merit Z T are highly increased with respect to a standard two-terminal system. These results are confirmed for the specific case of a system consisting of three coupled quantum dots.

Photoinduced Dynamics of Charge Separation: From Photosynthesis to Polymer–Fullerene Bulk Heterojunctions

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

Niklas, Jens; Beaupré, Serge; Leclerc, Mario

2015-06-18

Understanding charge separation and charge transport is crucial for improving the efficiency of organic solar cells. Their active media are based on organic molecules and polymers, serving as both light-absorbing and transport layers. The charge-transfer (CT) states play an important role, being intermediate for free carrier generation and charge recombination. Here, we use light-induced electron paramagnetic resonance spectroscopy to study the CT dynamics in blends of the polymers P3HT, PCDTBT, and PTB7 with the fullerene derivative C-60-PCBM. Time-resolved EPR measurements show strong spin-polarization patterns for all polymer-fullerene blends, confirming predominant generation of singlet CT states and partial orientation ordering nearmore » the donor-acceptor interface. These observations allow a comparison with charge separation processes in molecular donor-acceptor systems and in natural and artificial photosynthetic assemblies, and thus the elucidation of the initial steps of sequential CT in organic photovoltaic materials.« less

Superconductivity, phase separation, and charge-transfer instability in the U = infinity limit of the three-band model of the CuO sub 2 planes

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

Grilli, M.; Raimondi, R.; Castellani, C.

1991-07-08

The {ital U}={infinity} limit of the three-band Hubbard model with nearest-neighbor repulsion {ital V} is studied using the slave-boson approach and the large-{ital N} expansion technique to order 1/{ital N}. A charge-transfer instability is found as in weak-coupling theory. The charge-transfer instability is always associated with a diverging compressibility leading to a phase separation. Near the phase-separation, charge-transfer-instability region we find superconducting instabilities in the {ital s}- and {ital d}-wave channel. The requirement for superconductivity is that {ital V} be on the scale of the Cu-O hopping as suggested by Varma, Schmitt-Rink, and Abrahams.

Rapid preparative separation of monoclonal antibody charge variants using laterally-fed membrane chromatography.

PubMed

Sadavarte, Rahul; Madadkar, Pedram; Filipe, Carlos Dm; Ghosh, Raja

2018-01-15

Monoclonal antibodies undergo various forms of chemical transformation which have been shown to cause loss in efficacy and alteration in pharmacokinetic properties of these molecules. Such modified antibody molecules are known as variants. They also display physical properties such as charge that are different from intact antibody molecules. However, the difference in charge is very subtle and separation based on it is quite challenging. Charge variants are usually separated using ion-exchange column chromatography or isoelectric focusing. In this paper, we report a rapid and scalable method for fractionating monoclonal antibody charge variants, based on the use of cation exchange laterally-fed membrane chromatography (LFMC). Starting with a sample of monoclonal antibody hIgG1-CD4, three well-resolved fractions were obtained using either pH or salt gradient. These fractions were identified as acidic, neutral and basic variants. Each of these fractions contained intact heavy and light chains and so antibody fragmentation had no role in variant generation. The separation was comparable to that using column chromatography but was an order of magnitude faster. Copyright © 2017 Elsevier B.V. All rights reserved.

Non-aqueous capillary electrophoretic separation of cholesterol and 25-hydroxycholesterol after derivatization with Girard P reagent.

PubMed

Gregus, Michal; Roberg-Larsen, Hanne; Lundanes, Elsa; Foret, Frantisek; Kuban, Petr; Wilson, Steven Ray

2017-10-01

Capillary electrophoresis (CE) can provide high separation efficiency with very simple instrumentation, but has yet to be explored regarding oxysterols/cholesterol. Cholesterol and 25-hydroxycholesterol (both are 4-ene-3-ketosteroids) were quantitatively transformed into hydrazones using Girard P reagent after enzymatic oxidation by cholesterol oxidase. Separation was achieved using non-aqueous capillary electrophoresis with UV detection at 280nm; the "charge-tagging" Girard P reagent ensured both charge and chromophore (which are requirements for CE-UV). Excess reagent was also separated from the two analytes, eliminating the need for removal prior to the analysis. The compounds were separated in less than 5min with excellent separation efficiency, using separation electrolytes fully compatible with mass spectrometry. The CE-UV method was used to optimize steps for charge-tagging, revealing that the procedure is affected by the analyte/reagent ratio and reaction time, but also the analyte structure. Copyright © 2017 Elsevier B.V. All rights reserved.

Magnetic field enhancement of organic photovoltaic cells performance.

PubMed

Oviedo-Casado, S; Urbina, A; Prior, J

2017-06-27

Charge separation is a critical process for achieving high efficiencies in organic photovoltaic cells. The initial tightly bound excitonic electron-hole pair has to dissociate fast enough in order to avoid photocurrent generation and thus power conversion efficiency loss via geminate recombination. Such process takes place assisted by transitional states that lie between the initial exciton and the free charge state. Due to spin conservation rules these intermediate charge transfer states typically have singlet character. Here we propose a donor-acceptor model for a generic organic photovoltaic cell in which the process of charge separation is modulated by a magnetic field which tunes the energy levels. The impact of a magnetic field is to intensify the generation of charge transfer states with triplet character via inter-system crossing. As the ground state of the system has singlet character, triplet states are recombination-protected, thus leading to a higher probability of successful charge separation. Using the open quantum systems formalism we demonstrate that the population of triplet charge transfer states grows in the presence of a magnetic field, and discuss the impact on carrier population and hence photocurrent, highlighting its potential as a tool for research on charge transfer kinetics in this complex systems.

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.

Role of coherence and delocalization in photo-induced electron transfer at organic interfaces

NASA Astrophysics Data System (ADS)

Abramavicius, V.; Pranculis, V.; Melianas, A.; Inganäs, O.; Gulbinas, V.; Abramavicius, D.

2016-09-01

Photo-induced charge transfer at molecular heterojunctions has gained particular interest due to the development of organic solar cells (OSC) based on blends of electron donating and accepting materials. While charge transfer between donor and acceptor molecules can be described by Marcus theory, additional carrier delocalization and coherent propagation might play the dominant role. Here, we describe ultrafast charge separation at the interface of a conjugated polymer and an aggregate of the fullerene derivative PCBM using the stochastic Schrödinger equation (SSE) and reveal the complex time evolution of electron transfer, mediated by electronic coherence and delocalization. By fitting the model to ultrafast charge separation experiments, we estimate the extent of electron delocalization and establish the transition from coherent electron propagation to incoherent hopping. Our results indicate that even a relatively weak coupling between PCBM molecules is sufficient to facilitate electron delocalization and efficient charge separation at organic interfaces.

Self-assembled photosynthesis-inspired light harvesting material and solar cells containing the same

DOEpatents

Lindsey, Jonathan S [Raleigh, NC; Chinnasamy, Muthiah [Raleigh, NC; Fan, Dazhong [Raleigh, NC

2009-12-15

A solar cell is described that comprises: (a) a semiconductor charge separation material; (b) at least one electrode connected to the charge separation material; and (c) a light-harvesting film on the charge separation material, the light-harvesting film comprising non-covalently coupled, self-assembled units of porphyrinic macrocycles. The porphyrinic macrocycles preferably comprise: (i) an intramolecularly coordinated metal; (ii) a first coordinating substituent; and (iii) a second coordinating substituent opposite the first coordinating substituent. The porphyrinic macrocycles can be assembled by repeating intermolecular coordination complexes of the metal, the first coordinating substituent and the second coordinating substituent.

CHARGE BOTTLE FOR A MASS SEPARATOR

DOEpatents

Davidson, P.H.

1959-07-01

Improved mass separator charge bottles are described for containing a dense charge of a chemical compound of copper, nickel, lead or other useful substance which is to be vaporized, and to the method of utilizing such improvcd charge bottles so that the chemical compound is vaporized from the under surface of the charge and thus permits the non-volatile portion thereof to fall to the bottom of the charge bottle where it does not form an obstacle to further evaporation. The charge bottle comprises a vertically disposed cylindrical portion, an inner re-entrant cylindrical portion extending axially and downwardly into the same from the upper end thereof, and evaporative source material in the form of a chemical compound compacted within the upper annular pontion of the charge bottle formed by the re-entrant cylindrical portion, whereby vapor from the chemical compound will pass outwardly from the charge bottle through an apertured closure.

The CE way of thinking: "all is relative!".

PubMed

Schmitt-Kopplin, Philippe; Fekete, Agnes

2008-01-01

Over the last two decades, the development of capillary electrophoresis (CE) instruments has lead to systems with programmable samplers, separation columns, separation buffers, and detection devices comparable visually in many aspects to the setup of classical chromatography. Two characteristics make CE essentially different from chromatography and are the basis of the CE way of thinking: first is the injection type and the liquid flow within the capillary. When the injection is made hydrodynamically (such as in most of the applications found in the literature), the injected volumes are directly dependent on the type and size of the separation capillary. The second characteristic is that in CE, buffer velocity is not pressure-driven, as in liquid chromatography, but is electrokinetically governed by the quality of the capillary surface (separation buffer dependent surface charge) inducing an electroosmotic flow (EOF). The EOF undergoes small variations and is not necessarily identical from one separation or day to the other. The direct consequence is that the migration time of the analytes apparently nonreproducible, although the velocity of the ions is the same. The effective mobility (field strength normalized velocity) of the ions is a possible parameterization from acquired time-scale to effective mobility-scale electropherograms leading to a reproducible visualization and better quantification with a direct relation to structural characters of the analytes (i.e., charge and size; see Chapter 23).

A quantitative structure–function relationship for the Photosystem II reaction center: Supermolecular behavior in natural photosynthesis

PubMed Central

Barter, Laura M. C.; Durrant, James R.; Klug, David R.

2003-01-01

Light-induced charge separation is the primary photochemical event of photosynthesis. Efficient charge separation in photosynthetic reaction centers requires the balancing of electron and excitation energy transfer processes, and in Photosystem II (PSII), these processes are particularly closely entangled. Calculations that treat the cofactors of the PSII reaction center as a supermolecular complex allow energy and electron transfer reactions to be described in a unified way. This calculational approach is shown to be in good agreement with experimentally observed energy and electron transfer dynamics. This supermolecular view also correctly predicts the effect of changing the redox potentials of cofactors by site-directed mutagenesis, thus providing a unified and quantitative structure–function relationship for the PSII reaction center. PMID:12538865

Equivalent circuit model of Ge/Si separate absorption charge multiplication avalanche photodiode

NASA Astrophysics Data System (ADS)

Wang, Wei; Chen, Ting; Yan, Linshu; Bao, Xiaoyuan; Xu, Yuanyuan; Wang, Guang; Wang, Guanyu; Yuan, Jun; Li, Junfeng

2018-03-01

The equivalent circuit model of Ge/Si Separate Absorption Charge Multiplication Avalanche Photodiode (SACM-APD) is proposed. Starting from the carrier rate equations in different regions of device and considering the influences of non-uniform electric field, noise, parasitic effect and some other factors, the equivalent circuit model of SACM-APD device is established, in which the steady-state and transient current voltage characteristics can be described exactly. In addition, the proposed Ge/Si SACM APD equivalent circuit model is embedded in PSpice simulator. The important characteristics of Ge/Si SACM APD such as dark current, frequency response, shot noise are simulated, the simulation results show that the simulation with the proposed model are in good agreement with the experimental results.

Particle separation

NASA Technical Reports Server (NTRS)

Arnott, W. Patrick (Inventor); Chakrabarty, Rajan K. (Inventor); Moosmuller, Hans (Inventor)

2011-01-01

Embodiments of a method for selecting particles, such as based on their morphology, is disclosed. In a particular example, the particles are charged and acquire different amounts of charge, or have different charge distributions, based on their morphology. The particles are then sorted based on their flow properties. In a specific example, the particles are sorted using a differential mobility analyzer, which sorts particles, at least in part, based on their electrical mobility. Given a population of particles with similar electrical mobilities, the disclosed process can be used to sort particles based on the net charge carried by the particle, and thus, given the relationship between charge and morphology, separate the particles based on their morphology.

Particle separation

DOEpatents

Moosmuller, Hans [Reno, NV; Chakrabarty, Rajan K [Reno, NV; Arnott, W Patrick [Reno, NV

2011-04-26

Embodiments of a method for selecting particles, such as based on their morphology, is disclosed. In a particular example, the particles are charged and acquire different amounts of charge, or have different charge distributions, based on their morphology. The particles are then sorted based on their flow properties. In a specific example, the particles are sorted using a differential mobility analyzer, which sorts particles, at least in part, based on their electrical mobility. Given a population of particles with similar electrical mobilities, the disclosed process can be used to sort particles based on the net charge carried by the particle, and thus, given the relationship between charge and morphology, separate the particles based on their morphology.

Topological phase transition and the effect of Hubbard interactions on the one-dimensional topological Kondo insulator

NASA Astrophysics Data System (ADS)

Pillay, Jason C.; McCulloch, Ian P.

2018-05-01

The effect of a local Kondo coupling and Hubbard interaction on the topological phase of the one-dimensional topological Kondo insulator (TKI) is numerically investigated using the infinite matrix-product state density-matrix renormalization group algorithm. The ground state of the TKI is a symmetry-protected topological (SPT) phase protected by inversion symmetry. It is found that on its own, the Hubbard interaction that tends to force fermions into a one-charge per site order is insufficient to destroy the SPT phase. However, when the local Kondo Hamiltonian term that favors a topologically trivial ground state with a one-charge per site order is introduced, the Hubbard interaction assists in the destruction of the SPT phase. This topological phase transition occurs in the charge sector where the correlation length of the charge excitation diverges while the correlation length of the spin excitation remains finite. The critical exponents, central charge, and the phase diagram separating the SPT phase from the topologically trivial phase are presented.

Resonance Raman and excitation energy dependent charge transfer mechanism in halide-substituted hybrid perovskite solar cells.

PubMed

Park, Byung-wook; Jain, Sagar M; Zhang, Xiaoliang; Hagfeldt, Anders; Boschloo, Gerrit; Edvinsson, Tomas

2015-02-24

Organo-metal halide perovskites (OMHPs) are materials with attractive properties for optoelectronics. They made a recent introduction in the photovoltaics world by methylammonium (MA) lead triiodide and show remarkably improved charge separation capabilities when chloride and bromide are added. Here we show how halide substitution in OMHPs with the nominal composition CH3NH3PbI2X, where X is I, Br, or Cl, influences the morphology, charge quantum yield, and local interaction with the organic MA cation. X-ray diffraction and photoluminescence data demonstrate that halide substitution affects the local structure in the OMHPs with separate MAPbI3 and MAPbCl3 phases. Raman spectroscopies as well as theoretical vibration calculations reveal that this at the same time delocalizes the charge to the MA cation, which can liberate the vibrational movement of the MA cation, leading to a more adaptive organic phase. The resonance Raman effect together with quantum chemical calculations is utilized to analyze the change in charge transfer mechanism upon electronic excitation and gives important clues for the mechanism of the much improved photovoltage and photocurrent also seen in the solar cell performance for the materials when chloride compounds are included in the preparation.

Molecular design and nanoscale engineering of organic nanofibril donor-acceptor heterojunctions

NASA Astrophysics Data System (ADS)

Huang, Helin

Organic nanofibril heterojunction materials have gained increasing research interest due to their broad applications in organic semiconductor devices. In order to enhance the device performance, we have investigated the structure-property relationship of these nanostructures by designing and synthesizing functional building block molecules, selfassembling the molecules into well-defined nanofibers, fabricating the nanofibers into optical and electrical devices, and testing their photoconductivity and sensor properties. In Chapter 2, we present a simple approach to fabricate efficient nanofibril heterojunctions by interfacial engineering of electron donor (D) coating onto acceptor (A) nanofibers. The nanofibers both create a large D/A interface for increased charge separation and act as long-range transport pathways for photogenerated charge carriers towards the electrodes, and the alkyl groups modified at the A molecules not only enable effective surface adsorption of D molecules on the nanofibers for effective electron-transfer communication, but also spatially separate the photogenerated charge carriers to prevent their recombination. In Chapter 3, we further investigated the effect of D molecular structure and coating morphology on photoconductivity of organic nanofiber materials. A series of D molecules with varying side-chain modifications were synthesized and investigated for the different intermolecular arrangements caused by pi-pi stacking in balance with steric hindrance of side-chains. Different molecular assemblies of D resulted in distinctive phase segregation between D and A nanofiber, which significantly affects the interfacial charge separation. In Chapter 4, we developed an alternative nanofibril heterojunction structure that is composed of D as the nanofiber, onto which a monolayer of A molecule was coated. Due to the strong redox (charge transfer) interaction between D and A, the nanofibril junction demonstrated high conductivity even without light illumination, which makes this material suitable for applications in chemiresistor sensors for detection of amines. In Chapter 5, a series of perylene tetracarboxylic monoimides were synthesized through a one-step reaction between cycloalkyl amines and the parent perylene dianhydride. The selection of appropriate reaction medium is the most critical for achieving the high purity of product. This approach opens up a new way for large scale production of the monoimides, which are the precursor for making a variety of perylene based building block molecules.

Comparison between students and residents on determinants of willingness to separate waste and waste separation behaviour in Zhengzhou, China.

PubMed

Dai, Xiaoping; Han, Yuping; Zhang, Xiaohong; Hu, Wei; Huang, Liangji; Duan, Wenpei; Li, Siyi; Liu, Xiaolu; Wang, Qian

2017-09-01

A better understanding of willingness to separate waste and waste separation behaviour can aid the design and improvement of waste management policies. Based on the intercept questionnaire survey data of undergraduate students and residents in Zhengzhou City of China, this article compared factors affecting the willingness and behaviour of students and residents to participate in waste separation using two binary logistic regression models. Improvement opportunities for waste separation were also discussed. Binary logistic regression results indicate that knowledge of and attitude to waste separation and acceptance of waste education significantly affect the willingness of undergraduate students to separate waste, and demographic factors, such as gender, age, education level, and income, significantly affect the willingness of residents to do so. Presence of waste-specific bins and attitude to waste separation are drivers of waste separation behaviour for both students and residents. Improved education about waste separation and facilities are effective to stimulate waste separation, and charging on unsorted waste may be an effective way to improve it in Zhengzhou.

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

Hydrogen bonding effects on the reorganization energy for photoinduced charge separation reaction between porphyrin and quinone studied by nanosecond laser flash photolysis.

PubMed

Yago, Tomoaki; Gohdo, Masao; Wakasa, Masanobu

2010-02-25

Alcohol concentration dependences of photoinduced charge separation (CS) reaction of zinc tetraphenyl-porphyrin (ZnTPP) and duroquinone (DQ) were investigated in benzonitrile by a nanosecond laser flash photolysis technique. The photoinduced CS reaction was accelerated by the addition of alcohols, whereas the addition of acetonitrile caused little effect on the CS reactions. The simple theory was developed to calculate an increase in reorganization energies induced by the hydrogen bonding interactions between DQ and alcohols using the chemical equilibrium constants for the hydrogen bonding complexes through the concerted pathway and the stepwise one. The experimental results were analyzed by using the Marcus equation where we took into account the hydrogen bonding effects on the reorganization energy and the reaction free energy for the CS reaction. The observed alcohol concentration dependence of the CS reaction rates was well explained by the formation of the hydrogen bonding complexes through the concerted pathway, demonstrating the increase in the reorganization energy by the hydrogen bonding interactions.

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.

17 CFR 270.26a-2 - Exemptions from certain provisions of sections 26 and 27 for registered separate accounts and...

Code of Federal Regulations, 2010 CFR

2010-04-01

... deduction of certain fees and charges from the assets of such accounts. 270.26a-2 Section 270.26a-2... registered separate accounts and others regarding custodianship of and deduction of certain fees and charges... by any State or other governmental entity and, if the separate account is registered under the Act as...

Physical aspects of ferroelectric semiconductors for photovoltaic solar energy conversion

NASA Astrophysics Data System (ADS)

Lopez-Varo, Pilar; Bertoluzzi, Luca; Bisquert, Juan; Alexe, Marin; Coll, Mariona; Huang, Jinsong; Jimenez-Tejada, Juan Antonio; Kirchartz, Thomas; Nechache, Riad; Rosei, Federico; Yuan, Yongbo

2016-10-01

Solar energy conversion using semiconductors to fabricate photovoltaic devices relies on efficient light absorption, charge separation of electron-hole pair carriers or excitons, and fast transport and charge extraction to counter recombination processes. Ferroelectric materials are able to host a permanent electrical polarization which provides control over electrical field distribution in bulk and interfacial regions. In this review, we provide a critical overview of the physical principles and mechanisms of solar energy conversion using ferroelectric semiconductors and contact layers, as well as the main achievements reported so far. In a ferroelectric semiconductor film with ideal contacts, the polarization charge would be totally screened by the metal layers and no charge collection field would exist. However, real materials show a depolarization field, smooth termination of polarization, and interfacial energy barriers that do provide the control of interface and bulk electric field by switchable spontaneous polarization. We explore different phenomena as the polarization-modulated Schottky-like barriers at metal/ferroelectric interfaces, depolarization fields, vacancy migration, and the switchable rectifying behavior of ferroelectric thin films. Using a basic physical model of a solar cell, our analysis provides a general picture of the influence of ferroelectric effects on the actual power conversion efficiency of the solar cell device, and we are able to assess whether these effects or their combinations are beneficial or counterproductive. We describe in detail the bulk photovoltaic effect and the contact layers that modify the built-in field and the charge injection and separation in bulk heterojunction organic cells as well as in photocatalytic and water splitting devices. We also review the dominant families of ferroelectric materials that have been most extensively investigated and have provided the best photovoltaic performance.

Role of charge separation mechanism and local disorder at hybrid solar cell interfaces

NASA Astrophysics Data System (ADS)

Ehrenreich, Philipp; Pfadler, Thomas; Paquin, Francis; Dion-Bertrand, Laura-Isabelle; Paré-Labrosse, Olivier; Silva, Carlos; Weickert, Jonas; Schmidt-Mende, Lukas

2015-01-01

Dye-sensitized metal oxide polymer hybrid solar cells deliver a promising basis in organic solar cell development due to many conceptual advantages. Since the power conversion efficiency is still in a noncompetitive state, it has to be understood how the photocurrent contribution can be maximized (i.e., which dye-polymer properties are most beneficial for efficient charge generation in hybrid solar cells). By the comparison of three model systems for hybrid solar cells with Ti O2 -dye-polymer interfaces, this paper was aimed at elucidating the role of the exact mechanism of charge generation. In the exciton dissociation (ED) case, an exciton that is generated in the polymer is split at the dye-polymer interface. Alternatively, this exciton can be transferred to the dye via an energy transfer (ET), upon which charge separation occurs between dye and Ti O2 . For comparison, the third case is included in which the high lowest unoccupied molecular orbital of the dye does not allow exciton separation or ET from the dye to the polymer, so that the dye only is responsible for charge generation. To separate effects owing to differences in energy levels of the involved materials from the impact of local order and disorder in the polymer close to the interface, this paper further comprises a detailed analysis of the polymer crystallinity based on the H-aggregate model. While the massive impact of the poly(3-hexylthiophene) crystallinity on device function has been outlined for bare metal oxide-polymer interfaces, it has not been considered for hybrid solar cells with dye-sensitized Ti O2 . The results presented here indicate that all dye molecules in general influence the polymer morphology, which has to be taken into account for future optimization of hybrid solar cells. Apart from that, it can be suggested that ED on the polymer needs an additional driving force to work efficiently; thus, energy transfer seems to be currently the most promising strategy to increase the polymer photocurrent contribution.

Persistence time of charge carriers in defect states of molecular semiconductors.

PubMed

McMahon, David P; Troisi, Alessandro

2011-06-07

Charge carriers in organic crystals are often trapped in point defects. The persistence time of the charge in these defect states is evaluated by computing the escape rate from this state using non-adiabatic rate theory. Two cases are considered (i) the hopping between separate identical defect states and (ii) the hopping between a defect state and the bulk (delocalized) states. We show that only the second process is likely to happen with realistic defect concentrations and highlight that the inclusion of an effective quantum mode of vibration is essential for accurate computation of the rate. The computed persistence time as a function of the trap energy indicates that trap states shallower than ∼0.3 eV cannot be effectively investigated with some slow spectroscopic techniques such as THz spectroscopy or EPR commonly used to study the nature of excess charge in semiconductors.

Investigation of electric charge on inertial particle dynamics in turbulence

NASA Astrophysics Data System (ADS)

Lu, Jiang; Shaw, Raymond

2014-11-01

The behavior of electrically charged, inertial particles in homogeneous, isotropic turbulence is investigated. Both like-charged and oppositely-charged particle interactions are considered. Direct numerical simulations (DNS) of turbulence in a periodic box using the pseudospectral numerical method are performed, with Lagrangian tracking of the particles. We study effects of mutual electrostatic repulsion and attraction on the particle dynamics, as quantified by the radial distribution function (RDF) and the radial relative velocity. For the like-charged particle case, the Coulomb force leads to a short range repulsion behavior and an RDF reminiscent of that for a dilute gas. For the oppositely-charged particle case, the Coulomb force increases the RDF beyond that already occurring for neutral inertial particles. For both cases, the relative velocities are calculated as a function of particle separation distance and show distinct deviations from the expected scaling within the dissipation range. This research was supported by NASA Grant NNX113AF90G.

High-potential perfluorinated phthalocyanine-fullerene dyads for generation of high-energy charge-separated states: formation and photoinduced electron-transfer studies.

PubMed

Das, Sushanta K; Mahler, Andrew; Wilson, Angela K; D'Souza, Francis

2014-08-25

High oxidation potential perfluorinated zinc phthalocyanines (ZnF(n)Pcs) are synthesised and their spectroscopic, redox, and light-induced electron-transfer properties investigated systematically by forming donor-acceptor dyads through metal-ligand axial coordination of fullerene (C60) derivatives. Absorption and fluorescence spectral studies reveal efficient binding of the pyridine- (Py) and phenylimidazole-functionalised fullerene (C60Im) derivatives to the zinc centre of the F(n)Pcs. The determined binding constants, K, in o-dichlorobenzene for the 1:1 complexes are in the order of 10(4) to 10(5) M(-1); nearly an order of magnitude higher than that observed for the dyad formed from zinc phthalocyanine (ZnPc) lacking fluorine substituents. The geometry and electronic structure of the dyads are determined by using the B3LYP/6-31G* method. The HOMO and LUMO levels are located on the Pc and C60 entities, respectively; this suggests the formation of ZnF(n)Pc(.+)-C60Im(.-) and ZnF(n)Pc(.+)-C60Py(.-) (n=0, 8 or 16) intra-supramolecular charge-separated states during electron transfer. Electrochemical studies on the ZnPc-C60 dyads enable accurate determination of their oxidation and reduction potentials and the energy of the charge-separated states. The energy of the charge-separated state for dyads composed of ZnF(n)Pc is higher than that of normal ZnPc-C60 dyads and reveals their significance in harvesting higher amounts of light energy. Evidence for charge separation in the dyads is secured from femtosecond transient absorption studies in nonpolar toluene. Kinetic evaluation of the cation and anion radical ion peaks reveals ultrafast charge separation and charge recombination in dyads composed of perfluorinated phthalocyanine and fullerene; this implies their significance in solar-energy harvesting and optoelectronic device building applications. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Direct Observation of Photoinduced Charge Separation in Ruthenium Complex/Ni(OH) 2 Nanoparticle Hybrid

DOE PAGES

Tang, Yu; Pattengale, Brian A.; Ludwig, John M.; ...

2015-12-17

We report that Ni(OH) 2 have emerged as important functional materials for solar fuel conversion because of their potential as cost-effective bifunctional catalysts for both hydrogen and oxygen evolution reactions. However, their roles as photocatalysts in the photoinduced charge separation (CS) reactions remain unexplored. In this paper, we investigate the CS dynamics of a newly designed hybrid catalyst by integrating a Ru complex with Ni(OH) 2 nanoparticles (NPs). Using time resolved X-ray absorption spectroscopy (XTA), we directly observed the formation of the reduced Ni metal site (~60 ps), unambiguously demonstrating CS process in the hybrid through ultrafast electron transfer frommore » Ru complex to Ni(OH) 2 NPs. Compared to the ultrafast CS process, the charge recombination in the hybrid is ultraslow (>>50 ns). These results not only suggest the possibility of developing Ni(OH) 2 as solar fuel catalysts, but also represent the first time direct observation of efficient CS in a hybrid catalyst using XTA.« less

Magnetic Control of the Charge-Separated State Lifetime Realized by Covalent Attachment of a Platinum Complex.

PubMed

Miura, Tomoaki; Fujiwara, Dai; Akiyama, Kimio; Horikoshi, Takafumi; Suzuki, Shuichi; Kozaki, Masatoshi; Okada, Keiji; Ikoma, Tadaaki

2017-02-02

Dynamics of the photogenerated charge-separated (CS) state is studied for a newly synthesized molecular triad, in which the donor (D) dimethoxytriphenylamine, 1,3-bis(2-pyridylimino)isoindolate platinum (BPIPt), and the acceptor (A) naphthaldiimide are linked with a triethynylbenzene unit (BPIPt-DA). Photoexcitation of BPIPt gives rise to generation of a long-lived (∼4 μs) CS state BPIPt-D + A - , of which the lifetime is considerably increased by an applied magnetic field of 270 mT. The positive magnetic field effect (MFE) is in contrast to the negative MFE for the reference DA molecule, which indicates successful switching of the initial spin state of the CS state from singlet to triplet. Simulations of the MFE and time-resolved electron paramagnetic resonance show that spin-selective charge recombination and spin relaxation are unaffected by attachment of BPIPt. The minimum impact of heavy atom substitution on the electronic and magnetic properties has been realized by the small electronic coupling mediated by the rigid meta-triethynylbenzene.

Recent progress in the transition radiation detector techniques

NASA Technical Reports Server (NTRS)

Yuan, L. C. L.

1973-01-01

A list of some of the major experimental achievements involving charged particles in the relativistic region are presented. With the emphasis mainly directed to the X-ray region, certain modes of application of the transition radiation for the identification and separation of relativistic charged particles are discussed. Some recent developments in detection techniques and improvements in detector performances are presented. Experiments were also carried out to detect the dynamic radiation, but no evidence of such an effect was observed.

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

Elucidating the Ultrafast Dynamics of Photoinduced Charge Separation in Metalloporphyrin-Fullerene Dyads Across the Electromagnetic Spectrum

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

Zhang, J.; Pápai, M.; Hirsch, A.

Metalloporphyrins are prominent building blocks in the synthetic toolbox of advanced photodriven molecular devices. When the central ion is paramagnetic, the relaxation pathways within the manifold of excited states are highly intricate so that unravelling the intramolecular energy and electron transfer processes is usually a very complex task. This fact is critically hampering the development of applications based on the enhanced coupling offered by the electronic exchange interaction. In this work, the dynamics of charge separation in a copper porphyrin-fullerene are studied with several complementary spectroscopic tools across the electromagnetic spectrum (from near infra-red to X-ray wavelengths), each of themmore » providing specific diagnostics. Correlating the various rates clearly demonstrates that the lifetime of the photoinduced charge-separated state exceeds by about 10 fold that of the isolated photoexcited CuII porphyrin. As revealed by the spectral modifications in the XANES region, this stabilization is accompanied by a transient change in covalency around the CuII center, which is induced by an enhanced interaction with the C60 moiety. This experimental finding is further confirmed by state-of-the art calculations using DFT and TD-DFT including dispersion effects that explain the electrostatic and structural origins of this interaction, as the CuIIP cation becomes ruffled and approaches closer to the fullerene in the charge-separated state. From a methodological point of view, these results exemplify the potential of multielectron excitation features in transient X-ray spectra as future diagnostics of sub-femtosecond electronic dynamics. From a practical point of view, this work is paving the way for elucidating out-of-equilibrium electron transfer events coupled to magnetic interaction processes on their intrinsic time-scales.« less

Spin-orbit coupling, electron transport and pairing instabilities in two-dimensional square structures

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

Kocharian, Armen N.; Fernando, Gayanath W.; Fang, Kun

Rashba spin-orbit effects and electron correlations in the two-dimensional cylindrical lattices of square geometries are assessed using mesoscopic two-, three- and four-leg ladder structures. Here the electron transport properties are systematically calculated by including the spin-orbit coupling in tight binding and Hubbard models threaded by a magnetic flux. These results highlight important aspects of possible symmetry breaking mechanisms in square ladder geometries driven by the combined effect of a magnetic gauge field spin-orbit interaction and temperature. The observed persistent current, spin and charge polarizations in the presence of spin-orbit coupling are driven by separation of electron and hole charges andmore » opposite spins in real-space. The modeled spin-flip processes on the pairing mechanism induced by the spin-orbit coupling in assembled nanostructures (as arrays of clusters) engineered in various two-dimensional multi-leg structures provide an ideal playground for understanding spatial charge and spin density inhomogeneities leading to electron pairing and spontaneous phase separation instabilities in unconventional superconductors. Such studies also fall under the scope of current challenging problems in superconductivity and magnetism, topological insulators and spin dependent transport associated with numerous interfaces and heterostructures.« less

Accumulative charge separation for solar fuels production: coupling light-induced single electron transfer to multielectron catalysis.

PubMed

Hammarström, Leif

2015-03-17

The conversion and storage of solar energy into a fuel holds promise to provide a significant part of the future renewable energy demand of our societies. Solar energy technologies today generate heat or electricity, while the large majority of our energy is used in the form of fuels. Direct conversion of solar energy to a fuel would satisfy our needs for storable energy on a large scale. Solar fuels can be generated by absorbing light and converting its energy to chemical energy by electron transfer leading to separation of electrons and holes. The electrons are used in the catalytic reduction of a cheap substrate with low energy content into a high-energy fuel. The holes are filled by oxidation of water, which is the only electron source available for large scale solar fuel production. Absorption of a single photon typically leads to separation of a single electron-hole pair. In contrast, fuel production and water oxidation are multielectron, multiproton reactions. Therefore, a system for direct solar fuel production must be able to accumulate the electrons and holes provided by the sequential absorption of several photons in order to complete the catalytic reactions. In this Account, the process is termed accumulative charge separation. This is considerably more complicated than charge separation on a single electron level and needs particular attention. Semiconductor materials and molecular dyes have for a long time been optimized for use in photovoltaic devices. Efforts are made to develop new systems for light harvesting and charge separation that are better optimized for solar fuel production than those used in the early devices presented so far. Significant progress has recently been made in the discovery and design of better homogeneous and heterogeneous catalysts for solar fuels and water oxidation. While the heterogeneous ones perform better today, molecular catalysts based on transition metal complexes offer much greater tunability of electronic and structural properties, they are typically more amenable to mechanistic analysis, and they are small and therefore require less material. Therefore, they have arguably greater potential as future efficient catalysts but must be efficiently coupled to accumulative charge separation. This Account discusses accumulative charge separation with focus on molecular and molecule-semiconductor hybrid systems. The coupling between charge separation and catalysis involves many challenges that are often overlooked, and they are not always apparent when studying water oxidation and fuel formation as separate half-reactions with sacrificial agents. Transition metal catalysts, as well as other multielectron donors and acceptors, cycle through many different states that may quench the excited sensitizer by nonproductive pathways. Examples where this has been shown, often with ultrafast rates, are reviewed. Strategies to avoid these competing energy-loss reactions and still obtain efficient coupling of charge separation to catalysis are discussed. This includes recent examples of dye-sensitized semiconductor devices with molecular catalysts and dyes that realize complete water splitting, albeit with limited efficiency.

Charge Transfer Processes in OPV Materials as Revealed by EPR Spectroscopy

DOE PAGES

Niklas, Jens; Poluektov, Oleg

2017-03-03

Understanding charge separation and charge transport at a molecular level is crucial for improving the efficiency of organic photovoltaic (OPV) cells. Under illumination of Bulk Heterojunction (BHJ) blends of polymers and fullerenes, various paramagnetic species are formed including polymer and fullerene radicals, radical pairs, and photoexcited triplet states. Light-induced Electron Paramagnetic Resonance (EPR) spectroscopy is ideally suited to study these states in BHJ due to its selectivity in probing the paramagnetic intermediates. Some advanced EPR techniques like light-induced ENDOR spectroscopy and pulsed techniques allow the determination of hyperfine coupling tensors, while high-frequency EPR allows the EPR signals of the individualmore » species to be resolved and their g-tensors to be determined. In these magnetic resonance parameters reveal details about the delocalization of the positive polaron on the various polymer donors which is important for the efficient charge separation in BHJ systems. Time-resolved EPR can contribute to the study of the dynamics of charge separation, charge transfer and recombination in BHJ by probing the unique spectral signatures of charge transfer and triplet states. Furthermore, the potential of the EPR also allows characterization of the intermediates and products of BHJ degradation.« less

First-principles studies of interfacial charge separation in nano-materials photovoltaic heterojunction

NASA Astrophysics Data System (ADS)

Kanai, Yosuke

2009-03-01

Charge separation is a crucial process that must be understood in order to make substantial improvements in nano-materials based PV cells. In our work, first principles quantum mechanical calculations are employed to shed light on this process for some important nano-material heterojunctions. I will first present our work on the interfacial charge separation in Fullerene/P3HT and CNT/P3HT heterojunctions. Our findings indicate that in the fullerene system a two-step process is operative, involving an adiabatic electron transfer and an exciton dissociation via quasi-degenerate states localized on the fullerene. For the nanotubes, on the other hand, while such a two-step process is not necessary for efficient charge separation, the presence of metallic nanotubes lead to undesirable charge traps. Secondly, I will discuss how we are addressing the difficulty in employing standard DFT approaches for investigating inorganic-organic PV interfaces, which are composed of two distinct materials with very different electronic environments. I will discuss a QMC scheme for obtaining many-body corrections to the Kohn-Sham level alignments and its application to a CdSe/Oligothiophene hybrid PV interface, with the aim of tailoring its behavior by controlling the conjugation length.

Long-Lived Photoinduced Charge Separation in a Trinuclear Iron-μ 3 -oxo-based Metal–Organic Framework

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

Hanna, Lauren; Kucheryavy, Pavel; Liu, Cunming

2017-06-14

The presence of long-lived charge-separated excited states in metal-organic frameworks (MOFs) can enhance their photocatalytic activity by decreasing the probability that photogenerated electrons and holes recombine before accessing adsorbed reactants. Detecting these charge separated states via optical transient absorption, however, can be challenging when they lack definitive optical signatures. Here, we investigate the long-lived excited state of a MOF with such vague optical properties, MIL-100(Fe), comprised of Fe3-μ3-oxo clusters and trimesic acid linkers using Fe K-edge X-ray transient absorption (XTA) spectroscopy, to unambiguously determine its ligand-to-metal charge transfer character. Spectra measured at time delays up to 3.6 μs confirm themore » long lived nature of the charge separated excited state. Several trinuclear iron μ3- oxo carboxylate complexes, which model the trinuclear cores of the MOF structure, are measured for comparison using both steady state XAS and XTA to further support this assignment and corresponding decay time. The MOF is prepared as a colloidal nanoparticle suspension for these measurements so both its fabrication and particle size analysis are presented, as well.« less

Surface charge dependent separation of modified and hybrid ferritin in native PAGE: Impact of lysine 104.

PubMed

Subhadarshanee, Biswamaitree; Mohanty, Abhinav; Jagdev, Manas Kumar; Vasudevan, Dileep; Behera, Rabindra K

2017-10-01

Preparation of modified and hybrid ferritin provides a great opportunity to understand the mechanisms of iron loading/unloading, protein self-assembly, size constrained nanomaterial synthesis and targeted drug delivery. However, the large size (M.W.=490kDa) has been limiting the separation of different modified and/or hybrid ferritin nanocages from each other in their intact assembled form and further characterization. Native polyacrylamide gel electrophoresis (PAGE) separates proteins on the basis of both charge and mass, while maintaining their overall native structure and activity. Altering surface charge distribution by substitution of amino acid residues located at the external surface of ferritin (K104E & D40A) affected the migration rate in native PAGE while internal modification had little effect. Crystal structures confirmed that ferritin nanocages made up of subunits with single amino acid substitutions retain the overall structure of ferritin nanocage. Taking advantage of K104E migration behavior, formation of hybrid ferritins with subunits of wild type (WT) and K104E were confirmed and separated in native PAGE. Cage integrity and iron loading ability (ferritin activity) were also tested. The migration pattern of hybrid ferritins in native PAGE depends on the subunit ratio (WT: K104E) in the ferritin cage. Our work shows that native PAGE can be exploited in nanobiotechnology, by analyzing modifications of large proteins like ferritin. Native PAGE, a simple, straight-forward technique, can be used to analyze small modification (by altering external surface charge) in large proteins like ferritin, without disintegrating its self-assembled nanocage structure. In doing so, native PAGE can complement the information obtained from mass spectrometry. The confirmation and separation of modified and hybrid ferritin protein nanocages in native PAGE, opens up various prospects of bio-conjugation, which can be useful in targeted drug delivery, nanobiotechnology and in understanding nature's idea of synthesizing hybrid ferritins in different human tissues. Copyright © 2017 Elsevier B.V. All rights reserved.

Charge separation and charge delocalization identified in long-living states of photoexcited DNA

PubMed Central

Bucher, Dominik B.; Pilles, Bert M.; Carell, Thomas; Zinth, Wolfgang

2014-01-01

Base stacking in DNA is related to long-living excited states whose molecular nature is still under debate. To elucidate the molecular background we study well-defined oligonucleotides with natural bases, which allow selective UV excitation of one single base in the strand. IR probing in the picosecond regime enables us to dissect the contribution of different single bases to the excited state. All investigated oligonucleotides show long-living states on the 100-ps time scale, which are not observable in a mixture of single bases. The fraction of these states is well correlated with the stacking probabilities and reaches values up to 0.4. The long-living states show characteristic absorbance bands that can be assigned to charge-transfer states by comparing them to marker bands of radical cation and anion spectra. The charge separation is directed by the redox potential of the involved bases and thus controlled by the sequence. The spatial dimension of this charge separation was investigated in longer oligonucleotides, where bridging sequences separate the excited base from a sensor base with a characteristic marker band. After excitation we observe a bleach of all involved bases. The contribution of the sensor base is observable even if the bridge is composed of several bases. This result can be explained by a charge delocalization along a well-stacked domain in the strand. The presence of charged radicals in DNA strands after light absorption may cause reactions—oxidative or reductive damage—currently not considered in DNA photochemistry. PMID:24616517

a Moessbauer Effect and Fenske-Hall Molecular Orbital Study of the Electronic Properties of Organoiron Clusters.

NASA Astrophysics Data System (ADS)

Buhl, Margaret Linn

The electronic properties of trinuclear iron, tetranuclear iron butterfly, iron-cobalt, and iron-copper clusters have been studied experimentally at 78K by the Mossbauer effect and theoretically by Fenske-Hall molecular orbital calculations. The Mossbauer effect isomer shift is very sensitive to the differences in the iron s-electron densities in these clusters and, as expected, decreases as the sum of the iron 4s Mulliken population and the Clementi and Raimondi effective nuclear charge increases. The molecular orbital wave functions and the Mulliken atomic charges are used to calculate the electric field gradient at the metal nuclei and the iron Mossbauer effect quadrupole splittings. The valence contribution was found to be the major component of the electric field gradient in all the clusters studied. In general the calculated value of Delta E_ {Q} is larger than the observed value, as a result of neglect of the valence Sternheimer factor, R. The metal charge depends upon its electronegativity and upon the nature of its Lewis base ligands. The carbonyl ligand carbon charge becomes more positive as the metal electronegativity increases. The oxygen charge becomes more negative as the anionic cluster charge increases, and in so doing, yields the maximum anionic charge separation. The electronic properties of the terminal carbonyl ligands are similar to those of carbon monoxide, whereas the electronic properties of the bridging carbonyl ligands are similar to those of the carbonyl group found in aldehydes and ketones.

Method of minimizing the effects of parasitic currents

DOEpatents

Chi, Michael C.; Carr, Peter

1983-02-01

A method of minimizing the effect of parasitic currents in secondary batteries having a plurality of cells connected electrically in series and a common electrolyte in communication with the cells is described. Specifically, the parasitic currents flowing through the battery cause a cell imbalance over the charge/discharge cycle. This cell imbalance is minimized by first separating the cells of the battery into two equal groups. Then the battery is charged with the two groups of cells connected electrically in series, and subsequently discharged with the two groups of cells reconnected electrically in series in an inverted sequence.

Charge Dependence and Electric Quadrupole Effects on Single-Nucleon Removal in Relativistic and Intermediate Energy Nuclear Collisions

NASA Technical Reports Server (NTRS)

Norbury, John W.

1992-01-01

Single nucleon removal in relativistic and intermediate energy nucleus-nucleus collisions is studied using a generalization of Weizsacker-Williams theory that treats each electromagnetic multipole separately. Calculations are presented for electric dipole and quadrupole excitations and incorporate a realistic minimum impact parameter, Coulomb recoil corrections, and the uncertainties in the input photonuclear data. Discrepancies are discussed. The maximum quadrupole effect to be observed in future experiments is estimated and also an analysis of the charge dependence of the electromagnetic cross sections down to energies as low as 100 MeV/nucleon is made.

Charge dependence and electric quadrupole effects on single-nucleon removal in relativistic and intermediate energy nuclear collisions

NASA Technical Reports Server (NTRS)

Norbury, J. W.; Townsend, L. W. (Principal Investigator)

1990-01-01

Single-nucleon removal in relativistic and intermediate energy nucleus-nucleus collisions is studied using a generalization of Weizsacker-Williams theory that treats each electromagnetic multipole separately. Calculations are presented for electric dipole and quadrupole excitations and incorporate a realistic minimum impact parameter, Coulomb recoil corrections, and the uncertainties in the input photonuclear data. Discrepancies are discussed. The maximum quadrupole effect to be observed in future experiments is estimated and also an analysis of the charge dependence of the electromagnetic cross sections down to energies as low as 100 MeV/nucleon is made.

Impact of the titania nanostructure on charge transport and its application in hybrid solar cells

NASA Astrophysics Data System (ADS)

Koffman-Frischknecht, Alejandro; Gonzalez, Fernando; Plá, Juan; Violi, Ianina; Soler-Illia, Galo J. A. A.; Perez, M. Dolores

2018-02-01

Porous titania films are widely studied in a number of optoelectronic applications due to its favorable optical and electronic characteristics. Mesoporous titania thin films (MTTFs) with tunable pore size, pore order, accessibility and crystallinity are of interest in electronic devices due to the potential for optimization of the desired characteristics for charge separation and carrier transport. In this work, several MTTFs were prepared by sol-gel chemistry with different structural properties tuned by post-synthesis thermal treatment. The effect of the structural properties (pore diameter, order and accessibility) on the electrical properties of the material was studied by films fabrication onto a transparent conducting electrode, ITO, such that it enables optoelectronic applications. The performance as photoanode was explored by the fabrication of hybrid polymer (P3HT): titania solar cells. Not only does structural properties affect polymer impregnation inside the titania pores as expected and hence impacts charge separation at the interface, but also the thermal treatment affects crystallinity and the films electronic properties. A more complete picture about the electronic properties of the different MTTFs prepared in this work was studied by mobility measurement by space charge limited current and impedance spectroscopy.

Enhanced spin-dependent charge transport of Co-(Al-fluoride) granular nanocomposite by co-separate sputtering

NASA Astrophysics Data System (ADS)

Cao, Yang; Kobayashi, Nobukiyo; Zhang, Yi-Wen; Ohnuma, Shigehiro; Masumoto, Hiroshi

2017-10-01

Spin-dependent charge transport behavior involving the recently discovered tunnel-type magneto-dielectric (TMD) and magnetoresistance (TMR) effects was studied in Co-(Al-fluoride) granular nanocomposites. By setting a changeable partition height (t = 1-4 cm) on a substrate holder in a conventional co-sputtering (CS) deposition system, we developed a co-separate sputtering (CSS) method to fabricate Co-(Al-F) granular nanocomposites. XPS analysis shows that the Al content remains balanced between the Al metal and Al-F compounds by controlling t. This phenomenon can be attributed to the magnetron plasma interference from the two target sources. Fittings between TMR and normalized magnetization suggest that the CSS films with clear granular structures may have high spin polarization. Compared with the CS samples (t = 0 cm), the CSS films with t = 4 cm show enhanced charge transport properties with a maximum TMD ratio (0.5%) and TMR ratio (7.2%) under a magnetic field of H = 10 kOe. This study demonstrates that the Al-F tunnel barrier between Co granules plays an essential role in controlling the charge transport behavior and will be of significance for applications in field sensors and impedance-tunable devices with large magnetic-field response.

Mixed mosaic membranes prepared by layer-by-layer assembly for ionic separations.

PubMed

Rajesh, Sahadevan; Yan, Yu; Chang, Hsueh-Chia; Gao, Haifeng; Phillip, William A

2014-12-23

Charge mosaic membranes, which possess distinct cationic and anionic domains that traverse the membrane thickness, are capable of selectively separating dissolved salts from similarly sized neutral solutes. Here, the generation of charge mosaic membranes using facile layer-by-layer assembly methodologies is reported. Polymeric nanotubes with pore walls lined by positively charged polyethylenimine moieties or negatively charged poly(styrenesulfonate) moieties were prepared via layer-by-layer assembly using track-etched membranes as sacrificial templates. Subsequently, both types of nanotubes were deposited on a porous support in order to produce mixed mosaic membranes. Scanning electron microscopy demonstrates that the facile deposition techniques implemented result in nanotubes that are vertically aligned without overlap between adjacent elements. Furthermore, the nanotubes span the thickness of the mixed mosaic membranes. The effects of this unique nanostructure are reflected in the transport characteristics of the mixed mosaic membranes. The hydraulic permeability of the mixed mosaic membranes in piezodialysis operations was 8 L m(-2) h(-1) bar(-1). Importantly, solute rejection experiments demonstrate that the mixed mosaic membranes are more permeable to ionic solutes than similarly sized neutral molecules. In particular, negative rejection of sodium chloride is observed (i.e., the concentration of NaCl in the solution that permeates through a mixed mosaic membrane is higher than in the initial feed solution). These properties illustrate the ability of mixed mosaic membranes to permeate dissolved ions selectively without violating electroneutrality and suggest their utility in ionic separations.

Microscopic dynamics of charge separation at the aqueous electrochemical interface.

PubMed

Kattirtzi, John A; Limmer, David T; Willard, Adam P

2017-12-19

We have used molecular simulation and methods of importance sampling to study the thermodynamics and kinetics of ionic charge separation at a liquid water-metal interface. We have considered this process using canonical examples of two different classes of ions: a simple alkali-halide pair, Na + I - , or classical ions, and the products of water autoionization, H 3 O + OH - , or water ions. We find that for both ion classes, the microscopic mechanism of charge separation, including water's collective role in the process, is conserved between the bulk liquid and the electrode interface. However, the thermodynamic and kinetic details of the process differ between these two environments in a way that depends on ion type. In the case of the classical ion pairs, a higher free-energy barrier to charge separation and a smaller flux over that barrier at the interface result in a rate of dissociation that is 40 times slower relative to the bulk. For water ions, a slightly higher free-energy barrier is offset by a higher flux over the barrier from longer lived hydrogen-bonding patterns at the interface, resulting in a rate of association that is similar both at and away from the interface. We find that these differences in rates and stabilities of charge separation are due to the altered ability of water to solvate and reorganize in the vicinity of the metal interface.

Microscopic dynamics of charge separation at the aqueous electrochemical interface

PubMed Central

Kattirtzi, John A.; Limmer, David T.; Willard, Adam P.

2017-01-01

We have used molecular simulation and methods of importance sampling to study the thermodynamics and kinetics of ionic charge separation at a liquid water–metal interface. We have considered this process using canonical examples of two different classes of ions: a simple alkali–halide pair, Na+I−, or classical ions, and the products of water autoionization, H3O+OH−, or water ions. We find that for both ion classes, the microscopic mechanism of charge separation, including water’s collective role in the process, is conserved between the bulk liquid and the electrode interface. However, the thermodynamic and kinetic details of the process differ between these two environments in a way that depends on ion type. In the case of the classical ion pairs, a higher free-energy barrier to charge separation and a smaller flux over that barrier at the interface result in a rate of dissociation that is 40 times slower relative to the bulk. For water ions, a slightly higher free-energy barrier is offset by a higher flux over the barrier from longer lived hydrogen-bonding patterns at the interface, resulting in a rate of association that is similar both at and away from the interface. We find that these differences in rates and stabilities of charge separation are due to the altered ability of water to solvate and reorganize in the vicinity of the metal interface. PMID:28698368

Electrochemical force microscopy

DOEpatents

Kalinin, Sergei V.; Jesse, Stephen; Collins, Liam F.; Rodriguez, Brian J.

2017-01-10

A system and method for electrochemical force microscopy are provided. The system and method are based on a multidimensional detection scheme that is sensitive to forces experienced by a biased electrode in a solution. The multidimensional approach allows separation of fast processes, such as double layer charging, and charge relaxation, and slow processes, such as diffusion and faradaic reactions, as well as capturing the bias dependence of the response. The time-resolved and bias measurements can also allow probing both linear (small bias range) and non-linear (large bias range) electrochemical regimes and potentially the de-convolution of charge dynamics and diffusion processes from steric effects and electrochemical reactivity.

Solid state electrochromic light modulator

DOEpatents

Cogan, Stuart F.; Rauh, R. David

1993-01-01

An all solid-state variable transmission electrochromic device has a source of charge compensating ions. An inorganic oxide counterelectrode film which on reduction with the accompanying insertion of the charge compensating ions increases its transmission of light of predetermined wavelength is separated from a primary electrochromic film which on reduction with the accompanying insertion of the charge compensating ions decreases its transmission of light of predetermined wavelength by an insulating electrolyte film that transports the charge compensating ions. First and second electrodes are contiguous with the inorganic oxide counter electrode film and the primary electrochromic film, respectively, and separated by the three films.

Solid state electrochromic light modulator

DOEpatents

Cogan, Stuart F.; Rauh, R. David

1993-12-07

An all solid-state variable transmission electrochromic device has a source of charge compensating ions. An inorganic oxide counterelectrode film which on reduction with the accompanying insertion of the charge compensating ions increases its transmission of light of predetermined wavelength is separated from a primary electrochromic film which on reduction with the accompanying insertion of the charge compensating ions decreases its transmission of light of predetermined wavelength by an insulating electrolyte film that transports the charge compensating ions. First and second electrodes are contiguous with the inorganic oxide counter electrode film and the primary electrochromic film, respectively, and separated by the three films.

Solid state electrochromic light modulator

DOEpatents

Cogan, Stuart F.; Rauh, R. David

1990-01-01

An all solid-state variable transmission electrochromic device has a source of charge compensating ions. An inorganic oxide counterelectrode film which on reduction with the accompanying insertion of the charge compensating ions increases its transmission of light of predetermined wavelength is separated from a primary electrochromic film which on reduction with the accompanying insertion of the charge compensating ions decreases its transmission of light of predetermined wavelength by an insulating electrolyte film that transports the charge compensating ions. First and second electrodes are contiguous with the inorganic oxide counter electrode film and the primary electrochromic film, respectively, and separated by the three films.

Solid state electrochromic light modulator

DOEpatents

Cogan, S.F.; Rauh, R.D.

1990-07-03

An all solid-state variable transmission electrochromic device has a source of charge compensating ions. An inorganic oxide counter electrode film which on reduction with the accompanying insertion of the charge compensating ions increases its transmission of light of predetermined wavelength is separated from a primary electrochromic film which on reduction with the accompanying insertion of the charge compensating ions decreases its transmission of light of predetermined wavelength by an insulating electrolyte film that transports the charge compensating ions. First and second electrodes are contiguous with the inorganic oxide counter electrode film and the primary electrochromic film, respectively, and separated by the three films. 4 figs.

On the role of local charge carrier mobility in the charge separation mechanism of organic photovoltaics.

PubMed

Yoshikawa, Saya; Saeki, Akinori; Saito, Masahiko; Osaka, Itaru; Seki, Shu

2015-07-21

Although the charge separation (CS) and transport processes that compete with geminate and non-geminate recombination are commonly regarded as the governing factors of organic photovoltaic (OPV) efficiency, the details of the CS mechanism remain largely unexplored. Here we provide a systematic investigation on the role of local charge carrier mobility in bulk heterojunction films of ten different low-bandgap polymers and polythiophene analogues blended with methanofullerene (PCBM). By correlating with the OPV performances, we demonstrated that the local mobility of the blend measured by time-resolved microwave conductivity is more important for the OPV output than those of the pure polymers. Furthermore, the results revealed two separate trends for crystalline and semi-crystalline polymers. This work offers guidance in the design of high-performance organic solar cells.

Influence of Crystallinity and Energetics on Charge Separation in Polymer–Inorganic Nanocomposite Films for Solar Cells

PubMed Central

Bansal, Neha; Reynolds, Luke X.; MacLachlan, Andrew; Lutz, Thierry; Ashraf, Raja Shahid; Zhang, Weimin; Nielsen, Christian B.; McCulloch, Iain; Rebois, Dylan G.; Kirchartz, Thomas; Hill, Michael S.; Molloy, Kieran C.; Nelson, Jenny; Haque, Saif A.

2013-01-01

The dissociation of photogenerated excitons and the subsequent spatial separation of the charges are of crucial importance to the design of efficient donor-acceptor heterojunction solar cells. While huge progress has been made in understanding charge generation at all-organic junctions, the process in hybrid organic:inorganic systems has barely been addressed. Here, we explore the influence of energetic driving force and local crystallinity on the efficiency of charge pair generation at hybrid organic:inorganic semiconductor heterojunctions. We use x-ray diffraction, photoluminescence quenching, transient absorption spectroscopy, photovoltaic device and electroluminescence measurements to demonstrate that the dissociation of photogenerated polaron pairs at hybrid heterojunctions is assisted by the presence of crystalline electron acceptor domains. We propose that such domains encourage delocalization of the geminate pair state. The present findings suggest that the requirement for a large driving energy for charge separation is relaxed when a more crystalline electron acceptor is used. PMID:23524906

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.

Insulator charging limits direct current across tunneling metal-insulator-semiconductor junctions

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

Vilan, Ayelet

Molecular electronics studies how the molecular nature affects the probability of charge carriers to tunnel through the molecules. Nevertheless, transport is also critically affected by the contacts to the molecules, an aspect that is often overlooked. Specifically, the limited ability of non-metallic contacts to maintain the required charge balance across the fairly insulating molecule often have dramatic effects. This paper shows that in the case of lead/organic monolayer-silicon junctions, a charge balance is responsible for an unusual current scaling, with the junction diameter (perimeter), rather than its area. This is attributed to the balance between the 2D charging at themore » metal/insulator interface and the 3D charging of the semiconductor space-charge region. A derivative method is developed to quantify transport across tunneling metal-insulator-semiconductor junctions; this enables separating the tunneling barrier from the space-charge barrier for a given current-voltage curve, without complementary measurements. The paper provides practical tools to analyze specific molecular junctions compatible with existing silicon technology, and demonstrates the importance of contacts' physics in modeling charge transport across molecular junctions.« less

Fluid mechanics of electroosmotic flow and its effect on band broadening in capillary electrophoresis.

PubMed

Ghosal, Sandip

2004-01-01

Electroosmotic flow (EOF) usually accompanies electrophoretic migration of charged species in capillary electrophoresis unless special precautions are taken to suppress it. The presence of the EOF provides certain advantages in separations. It is an alternative to mechanical pumps, which are inefficient and difficult to build at small scales, for transporting reagents and analytes on microfluidic chips. The downside is that any imperfection that distorts the EOF profile reduces the separation efficiency. In this paper, the basic facts about EOF are reviewed from the perspective of fluid mechanics and its effect on separations in free solution capillary zone electrophoresis is discussed in the light of recent advances.

Charge-induced fluctuation forces in graphitic nanostructures

DOE PAGES

Drosdoff, D.; Bondarev, Igor V.; Widom, Allan; ...

2016-01-21

Charge fluctuations in nanocircuits with capacitor components are shown to give rise to a novel type of long-ranged interaction, which coexist with the regular Casimir–van derWaals force. The developed theory distinguishes between thermal and quantum mechanical effects, and it is applied to capacitors involving graphene nanostructures. The charge fluctuations mechanism is captured via the capacitance of the system with geometrical and quantum mechanical components. The dependence on the distance separation, temperature, size, and response properties of the system shows that this type of force can have a comparable and even dominant effect to the Casimir interaction. Lastly, our results stronglymore » indicate that fluctuation-induced interactions due to various thermodynamic quantities can have important thermal and quantum mechanical contributions at the microscale and the nanoscale.« less

Photoinduced charge separation at polymer-fullerene interfaces of BHJ solar cells (Conference Presentation)

NASA Astrophysics Data System (ADS)

Poluektov, Oleg G.; Niklas, Jens; Mardis, Kristy

2016-09-01

While photovoltaic cells are highly promising man-made devices for direct solar energy utilization, a number of fundamental questions about how the organic bulk heterojunction cell enables efficient long-lived and long-range charge separation remain unanswered. These questions were address by employing an advanced suite of EPR spectroscopy in combination with DFT calculations to study mechanism of charge separation at the polymer-fullerene interfaces of photo-active BHJ. Observed charge delocalization in BHJ upon photoinduced ET is analogous to that in organic donor-acceptor material. This is an efficient mechanism of charge stabilization in photosynthetic assemblies. Time-resolved EPR spectra show a strong polarization pattern for all polymer-fullerene blends under study, which is caused by non-Boltzmann population of the electron spin energy levels in the radical pairs. The first observation of this phenomenon was reported in natural and artificial photosynthetic assemblies, and comparison with these systems allows us to better understand charge separation processes in OPVs. The spectral analysis presented here, in combination with DFT calculations, shows that CS processes in OPV materials are similar to that in organic photosynthetic systems. This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract DE-AC02-06CH11357 at Argonne National Laboratory.

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.

Surface charge- and space-dependent transport of proteins in crowded environments of nanotailored posts.

PubMed

Choi, Chang Kyoung; Fowlkes, Jason D; Retterer, Scott T; Siuti, Piro; Iyer, Sukanya; Doktycz, Mitchel J

2010-06-22

The reaction and diffusion of molecules across barriers and through crowded environments is integral to biological system function and to separation technologies. Ordered, microfabricated post arrays are a promising route to creating synthetic barriers with controlled chemical and physical characteristics. They can be used to create crowded environments, to mimic aspects of cellular membranes, and to serve as engineered replacements of polymer-based separation media. Here, the translational diffusion of fluorescein isothiocyante and various forms of green fluorescent protein (GFP), including "supercharged" variants, are examined in a silicon-based post array environment. The technique of fluorescence recovery after photobleaching (FRAP) is combined with analytical approximations and numerical simulations to assess the relative effects of reaction and diffusion on molecular transport, respectively. FRAP experiments were conducted for 64 different cases where the molecular species, the density of the posts, and the chemical surface charge of the posts were varied. In all cases, the dense packing of the posts hindered the diffusive transport of the fluorescent species. The supercharged GFPs strongly interacted with oppositely charged surfaces. With similar molecular and surface charges, transport is primarily limited by hindered diffusion. For conventional, enhanced GFP in a positively charged surface environment, transport was limited by the coupled action of hindered diffusion and surface interaction with the posts. Quantification of the size-, space-, time-, and charge-dependent translational diffusion in the post array environments can provide insight into natural processes and guide the design and development of selective membrane systems.

Self assembly of oppositely charged latex particles at oil-water interface.

PubMed

Nallamilli, Trivikram; Ragothaman, Srikanth; Basavaraj, Madivala G

2017-01-15

In this study we explore the self assembly of oppositely charged latex particles at decane water interfaces. Two spreading protocols have been proposed in this context. In the first method oppositely charged particles are mixed prior to spreading at the interface, this is called "premixed-mixtures". In the second protocol negatively charged particles are first spread at the interface at known coverage followed by spreading positively charged particles at known coverage and this is called "sequential-mixtures". In premixed mixtures depending on particle mixing ratio (composition) and total surface coverage a number of 2d structures ranging from 2d crystals, aggregate-crystal coexistence and 2d-gels are observed. A detailed phase diagram of this system has been explored. In sequential-mixtures for the first time we observed a new phase in colloidal monolayers called 2d-bi crystalline domains. These structures consisted regions of two crystal phases of oppositely charged particles separated by a one dimensional chain of alternating positive and negative particles. Phase diagram of this system has also been explored at various combinations of first spread and second spread particles. A possible mechanism leading to formation of these 2d bi crystalline structures has been discussed. A direct visualization of breakage and reformation of particle barriers separating the crystal phases has been demonstrated through videos. Effect of salt in the water sub phase and particle hydrophobicity on domain formation is also investigated. Copyright © 2016 Elsevier Inc. All rights reserved.

Characterization of Boron Contamination in Fluorine Implantation using Boron Trifluoride as a Source Material

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

Schmeide, Matthias; Kondratenko, Serguei

2011-01-07

Fluorine implantation process purity was considered on different types of high current implanters. It was found that implanters equipped with an indirectly heated cathode ion source show an enhanced deep boron contamination compared to a high current implanter using a cold RF-driven multicusp ion source when boron trifluoride is used for fluorine implantations. This contamination is directly related to the source technology and thus, should be considered potentially for any implanter design using hot cathode/hot filament ion source, independently of the manufacturer.The boron contamination results from the generation of double charged boron ions in the arc chamber and the subsequentmore » charge exchange reaction to single charged boron ions taking place between the arc chamber and the extraction electrode. The generation of the double charged boron ions depends mostly on the source parameters, whereas the pressure in the region between the arc chamber and the extraction electrode is mostly responsible for the charge exchange from double charged to single charged ions. The apparent mass covers a wide range, starting at mass 11. A portion of boron ions with energies of (19/11) times higher than fluorine energy has the same magnetic rigidity as fluorine beam and cannot be separated by the analyzer magnet. The earlier described charge exchange effects between the extraction electrode and the entrance to the analyzer magnet, however, generates boron beam with a higher magnetic rigidity compared to fluorine beam and cannot cause boron contamination after mass-separation.The energetic boron contamination was studied as a function of the ion source parameters, such as gas flow, arc voltage, and source magnet settings, as well as analyzing magnet aperture resolution. This allows process optimization reducing boron contamination to the level acceptable for device performance.« less

Surface morphology effects in a vibration based triboelectric energy harvester

NASA Astrophysics Data System (ADS)

Nafari, A.; Sodano, H. A.

2018-01-01

Despite the abundance of ambient mechanical energy in our environment, it is often neglected and left unused. However, recent studies have demonstrated that mechanical vibrations can be harvested and used to power small wireless electronic devices, such as micro electromechanical sensors (MEMS) and actuators. Most commonly, these energy harvesters convert vibration into electrical energy by utilizing piezoelectric, electromagnetic or electrostatic effects. Recently, triboelectric based energy harvesters have shown to be among the simplest and most cost-effective techniques for scavenging mechanical energy. The basis of triboelectric energy harvesters is the periodic contact and separation of two surfaces with opposite triboelectric properties which results in induced charge flow through an external load. Here, a vibration driven triboelectric nanogenerator (TENG) is fabricated and the effect of micro/nano scale surface modification is studied. The TENG produces electrical energy on the basis of periodic out-of-plane charge separation between gold and polydimethylsiloxane (PDMS) with opposite triboelectric charge polarities. By introducing micro/nano scale surface modifications to the PDMS and gold, the TENG’s power output is further enhanced. This work demonstrates that the morphology of the surfaces in a TENG device is important and by increasing the effective surface area through micro/nano scale modification, the power output of the device can increase by 118%. Moreover, it is shown that unlike many TENGs proposed in the literature, the fabricated device has a high RMS open circuit voltage and short circuit current and can perform for an extended period of time.

The rate of separation of magnetic lines of force in a random magnetic field.

NASA Technical Reports Server (NTRS)

Jokipii, J. R.

1973-01-01

The mixing of magnetic lines of force, as represented by their rate of separation, as a function of distance along the magnetic field, is considered with emphasis on neighboring lines of force. This effect is particularly important in understanding the transport of charged particles perpendicular to the average magnetic field. The calculation is carried out in the approximation that the separation changes by an amount small compared with the correlation scale normal to the field, in a distance along the field of a few correlation scales. It is found that the rate of separation is very sensitive to the precise form of the power spectrum. Application to the interplanetary and interstellar magnetic fields is discussed, and it is shown that in some cases field lines, much closer together than the correlation scale, separate at a rate which is effectively as rapid as if they were many correlation lengths apart.

Collision-Induced Dissociation of Electrosprayed Protein Complexes: An All-Atom Molecular Dynamics Model with Mobile Protons.

PubMed

Popa, Vlad; Trecroce, Danielle A; McAllister, Robert G; Konermann, Lars

2016-06-16

Electrospray ionization mass spectrometry (ESI-MS) has become an indispensable technique for examining noncovalent protein complexes. Collision-induced dissociation (CID) of these multiply protonated gaseous ions usually culminates in ejection of a single subunit with a disproportionately large amount of charge. Experiments suggest that this process involves subunit unfolding prior to separation from the residual complex, as well as H(+) migration onto the unravelling chain. Molecular dynamics (MD) simulations are a promising avenue for gaining detailed insights into these CID events. Unfortunately, typical MD algorithms do not allow for mobile protons. Here we address this limitation by implementing a strategy that combines atomistic force fields (such as OPLS/AA and CHARMM36) with a proton hopping algorithm, focusing on the tetrameric complexes transthyretin and streptavidin. Protons are redistributed over all acidic and basic sites in 20 ps intervals, subject to an energy function that reflects electrostatic interactions and proton affinities. Our simulations predict that nativelike conformers at the onset of collisional heating contain multiple salt bridges. Collisional heating initially causes subtle structural changes that lead to a gradual decline of these zwitterionic patterns. Many of the MD runs show gradual unfolding of a single subunit in conjunction with H(+) migration, culminating in subunit separation from the complex. However, there are also instances where two or more chains start to unfold simultaneously, giving rise to charge competition. The scission point where the "winning" subunit separates from the complex can be attained for different degrees of unfolding, giving rise to product ions in various charge states. The simulated product ion distributions are in close agreement with experimental CID data. Proton enrichment in the departing subunit is driven by charge-charge repulsion, but the combination of salt bridge depletion, charge migration, and proton affinity causes surprising compensation effects among the various energy terms. It appears that this work provides the most detailed account to date of the mechanism whereby noncovalent protein complexes disassemble during CID.

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

Enhanced Solar Cell Conversion Efficiency of InGaN/GaN Multiple Quantum Wells by Piezo-Phototronic Effect.

PubMed

Jiang, Chunyan; Jing, Liang; Huang, Xin; Liu, Mengmeng; Du, Chunhua; Liu, Ting; Pu, Xiong; Hu, Weiguo; Wang, Zhong Lin

2017-09-26

The piezo-phototronic effect is the tuning of piezoelectric polarization charges at the interface to largely enhance the efficiency of optoelectronic processes related to carrier separation or recombination. Here, we demonstrated the enhanced short-circuit current density and the conversion efficiency of InGaN/GaN multiple quantum well solar cells with an external stress applied on the device. The external-stress-induced piezoelectric charges generated at the interfaces of InGaN and GaN compensate the piezoelectric charges induced by lattice mismatch stress in the InGaN wells. The energy band realignment is calculated with a self-consistent numerical model to clarify the enhancement mechanism of optical-generated carriers. This research not only theoretically and experimentally proves the piezo-phototronic effect modulated the quantum photovoltaic device but also provides a great promise to maximize the use of solar energy in the current energy revolution.

State of charge indicators for a battery

DOEpatents

Rouhani, S. Zia

1999-01-01

The present invention relates to state of charge indicators for a battery. One aspect of the present invention utilizes expansion and contraction displacements of an electrode plate of a battery to gauge the state of charge in the battery. One embodiment of a battery of the present invention includes an anodic plate; a cathodic plate; an electrolyte in contact with the anodic and cathodic plates; plural terminals individually coupled with one of the anodic and cathodic plates; a separator intermediate the anodic and cathodic plates; an indicator configured to indicate an energy level of the battery responsive to movement of the separator; and a casing configured to house the anodic and cathodic plates, electrolyte, and separator.

Charge Transfer from n-Doped Nanocrystals: Mimicking Intermediate Events in Multielectron Photocatalysis.

PubMed

Wang, Junhui; Ding, Tao; Wu, Kaifeng

2018-06-12

In multielectron photocatalytic reactions, an absorbed photon triggers charge transfer from the light-harvester to the attached catalyst, leaving behind a charge of the opposite sign in the light-harvester. If this charge is not scavenged before the absorption of the following photons, photoexcitation generates not neutral but charged excitons from which the extraction of charges should become more difficult. This is potentially an efficiency-limiting intermediate event in multielectron photocatalysis. To study the charge dynamics in this event, we doped CdS nanocrystal quantum dots (QDs) with an extra electron and measured hole transfer from n-doped QDs to attached acceptors. We find that the Auger decay of charged excitons lowers the charge separation yield to 68.6% from 98.4% for neutral excitons. In addition, the hole transfer rate in the presence of two electrons (1290 ps) is slower than that in the presence one electron (776 ps), and the recombination rate of charge separated states is about 2 times faster in the former case. This model study provides important insights into possible efficiency-limiting intermediate events involved in photocatalysis.

Transient and modulated charge separation at CuInSe2/C60 and CuInSe2/ZnPc hybrid interfaces

NASA Astrophysics Data System (ADS)

von Morzé, Natascha; Dittrich, Thomas; Calvet, Wolfram; Lauermann, Iver; Rusu, Marin

2017-02-01

Spectral dependent charge transfer and exciton dissociation have been investigated at hybrid interfaces between inorganic polycrystalline CuInSe2 (untreated and Na-conditioned) thin films and organic C60 as well as zinc phthalocyanine (ZnPc) layers by transient and modulated surface photovoltage measurements. The stoichiometry and electronic properties of the bare CuInSe2 surface were characterized by photoelectron spectroscopy which revealed a Cu-poor phase with n-type features. After the deposition of the C60 layer, a strong band bending at the CuInSe2 surface was observed. Evidence for dissociation of excitons followed by charge separation was found at the CuInSe2/ZnPc interface. The Cu-poor layer at the CuInSe2 surface was found to be crucial for transient and modulated charge separation at CuInSe2/organic hybrid interfaces.

Tracking the coherent generation of polaron pairs in conjugated polymers

NASA Astrophysics Data System (ADS)

de Sio, Antonietta; Troiani, Filippo; Maiuri, Margherita; Réhault, Julien; Sommer, Ephraim; Lim, James; Huelga, Susana F.; Plenio, Martin B.; Rozzi, Carlo Andrea; Cerullo, Giulio; Molinari, Elisa; Lienau, Christoph

2016-12-01

The optical excitation of organic semiconductors not only generates charge-neutral electron-hole pairs (excitons), but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. We observe multi-period peak oscillations persisting for up to about 1 ps as distinct signatures of vibronic quantum coherence at room temperature. The measured two-dimensional spectra show pronounced peak splittings revealing that the elementary optical excitations of this polymer are hybridized exciton-polaron-pairs, strongly coupled to a dominant underdamped vibrational mode. Coherent vibronic coupling induces ultrafast polaron pair formation, accelerates the charge separation dynamics and makes it insensitive to disorder. These findings open up new perspectives for tailoring light-to-current conversion in organic materials.

AlInAsSb separate absorption, charge, and multiplication avalanche photodiodes

NASA Astrophysics Data System (ADS)

Ren, Min; Maddox, Scott J.; Woodson, Madison E.; Chen, Yaojia; Bank, Seth R.; Campbell, Joe C.

2016-05-01

We report AlxIn1-xAsySb1-y separate absorption, charge, and multiplication avalanche photodiodes (APDs) that operate in the short-wavelength infrared spectrum. They exhibit excess noise factor less or equal to that of Si and the low dark currents typical of III-V compound APDs.

Molecular approaches to solar energy conversion: the energetic cost of charge separation from molecular-excited states.

PubMed

Durrant, James R

2013-08-13

This review starts with a brief overview of the technological potential of molecular-based solar cell technologies. It then goes on to focus on the core scientific challenge associated with using molecular light-absorbing materials for solar energy conversion, namely the separation of short-lived, molecular-excited states into sufficiently long-lived, energetic, separated charges capable of generating an external photocurrent. Comparisons are made between different molecular-based solar cell technologies, with particular focus on the function of dye-sensitized photoelectrochemical solar cells as well as parallels with the function of photosynthetic reaction centres. The core theme of this review is that generating charge carriers with sufficient lifetime and a high quantum yield from molecular-excited states comes at a significant energetic cost-such that the energy stored in these charge-separated states is typically substantially less than the energy of the initially generated excited state. The role of this energetic loss in limiting the efficiency of solar energy conversion by such devices is emphasized, and strategies to minimize this energy loss are compared and contrasted.

Charge-dependent flow and the search for the chiral magnetic wave in Pb-Pb collisions at s N N = 2.76 TeV

DOE PAGES

Adam, J.; Adamová, D.; Aggarwal, M. M.; ...

2016-04-08

We report on measurements of a charge-dependent flow using a novel three-particle correlator with ALICE in Pb-Pb collisions at the CERN Large Hadron Collider (LHC), and discuss the implications for observation of local parity violation and the chiral magnetic wave (CMW) in heavy-ion collisions. Charge-dependent flow is reported for different collision centralities as a function of the event charge asymmetry. While our results are in qualitative agreement with expectations based on the CMW, the nonzero signal observed in higher harmonics correlations indicates a possible significant background contribution. We also present results on a differential correlator, where the flow of positivemore » and negative charges is reported as a function of the mean charge of the particles and their pseudorapidity separation. We argue that this differential correlator is better suited to distinguish the differences in positive and negative charges expected due to the CMW and the background effects, such as local charge conservation coupled with strong radial and anisotropic flow.« less

Charge-dependent flow and the search for the chiral magnetic wave in Pb-Pb collisions at √{sN N}=2.76 TeV

NASA Astrophysics Data System (ADS)

Adam, J.; Adamová, D.; Aggarwal, M. M.; Aglieri Rinella, G.; Agnello, M.; Agrawal, N.; Ahammed, Z.; Ahn, S. U.; Aiola, S.; Akindinov, A.; Alam, S. N.; Aleksandrov, D.; Alessandro, B.; Alexandre, D.; Alfaro Molina, R.; Alici, A.; Alkin, A.; Almaraz, J. R. M.; Alme, J.; Alt, T.; Altinpinar, S.; Altsybeev, I.; Alves Garcia Prado, C.; Andrei, C.; Andronic, A.; Anguelov, V.; Anielski, J.; Antičić, T.; Antinori, F.; Antonioli, P.; 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.; Balasubramanian, S.; Baldisseri, A.; Baral, R. C.; Barbano, A. M.; Barbera, R.; Barile, F.; Barnaföldi, G. G.; Barnby, L. S.; Barret, V.; Bartalini, P.; Barth, K.; Bartke, J.; Bartsch, E.; Basile, M.; Bastid, N.; Basu, S.; Bathen, B.; Batigne, G.; Batista Camejo, A.; Batyunya, B.; Batzing, P. C.; Bearden, I. G.; Beck, H.; Bedda, C.; Behera, N. K.; Belikov, I.; Bellini, F.; Bello Martinez, H.; Bellwied, R.; Belmont, R.; Belmont-Moreno, E.; Belyaev, V.; Benacek, P.; Bencedi, G.; Beole, S.; Berceanu, I.; 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, L.; Bianchi, N.; Bianchin, C.; Bielčík, J.; Bielčíková, J.; Bilandzic, A.; Biro, G.; Biswas, R.; Biswas, S.; Bjelogrlic, S.; Blair, J. T.; Blau, D.; Blume, C.; Bock, F.; Bogdanov, A.; Bøggild, H.; Boldizsár, L.; Bombara, M.; Book, J.; Borel, H.; Borissov, A.; Borri, M.; Bossú, F.; Botta, E.; Bourjau, C.; Braun-Munzinger, P.; Bregant, M.; Breitner, T.; Broker, T. A.; Browning, T. A.; Broz, M.; Brucken, E. J.; Bruna, E.; Bruno, G. E.; Budnikov, D.; Buesching, H.; Bufalino, S.; Buncic, P.; Busch, O.; Buthelezi, Z.; Butt, J. B.; Buxton, J. T.; Caffarri, D.; Cai, X.; Caines, H.; Calero Diaz, L.; Caliva, A.; Calvo Villar, E.; Camerini, P.; Carena, F.; Carena, W.; Carnesecchi, F.; Castillo Castellanos, J.; Castro, A. J.; Casula, E. A. R.; Ceballos Sanchez, C.; Cerello, P.; Cerkala, J.; Chang, B.; Chapeland, S.; Chartier, M.; Charvet, J. L.; Chattopadhyay, S.; Chattopadhyay, S.; Chauvin, A.; Chelnokov, V.; Cherney, M.; Cheshkov, C.; Cheynis, B.; Chibante Barroso, V.; Chinellato, D. D.; Cho, S.; Chochula, P.; Choi, K.; Chojnacki, M.; Choudhury, S.; 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.; 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.; Crochet, P.; Cruz Albino, R.; Cuautle, E.; Cunqueiro, L.; Dahms, T.; Dainese, A.; 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.; Deisting, A.; Deloff, A.; Dénes, E.; Deplano, C.; Dhankher, P.; di Bari, D.; di Mauro, A.; di Nezza, P.; Diaz Corchero, M. A.; Dietel, T.; Dillenseger, P.; Divià, R.; Djuvsland, Ø.; Dobrin, A.; Domenicis Gimenez, D.; Dönigus, B.; Dordic, O.; Drozhzhova, T.; Dubey, A. K.; Dubla, A.; Ducroux, L.; Dupieux, P.; Ehlers, R. J.; Elia, D.; Endress, E.; Engel, H.; Epple, E.; Erazmus, B.; Erdemir, I.; Erhardt, F.; Espagnon, B.; Estienne, M.; Esumi, S.; Eum, J.; Evans, D.; Evdokimov, S.; Eyyubova, G.; Fabbietti, L.; Fabris, D.; Faivre, J.; Fantoni, A.; Fasel, M.; Feldkamp, L.; Feliciello, A.; Feofilov, G.; Ferencei, J.; 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.; Fiore, E. M.; Fleck, M. G.; Floris, M.; Foertsch, S.; Foka, P.; Fokin, S.; Fragiacomo, E.; Francescon, A.; Frankenfeld, U.; Fronze, G. G.; Fuchs, U.; Furget, C.; Furs, A.; Fusco Girard, M.; Gaardhøje, J. J.; Gagliardi, M.; Gago, A. M.; Gallio, M.; Gangadharan, D. R.; Ganoti, P.; Gao, C.; Garabatos, C.; Garcia-Solis, E.; Gargiulo, C.; Gasik, P.; Gauger, E. F.; Germain, M.; Gheata, A.; Gheata, M.; Ghosh, P.; Ghosh, S. K.; Gianotti, P.; Giubellino, P.; Giubilato, P.; Gladysz-Dziadus, E.; Glässel, P.; Goméz Coral, D. M.; Gomez Ramirez, A.; Gonzalez, V.; González-Zamora, P.; Gorbunov, S.; Görlich, L.; Gotovac, S.; Grabski, V.; Grachov, O. A.; Graczykowski, L. K.; Graham, K. L.; Grelli, A.; Grigoras, A.; Grigoras, C.; Grigoriev, V.; Grigoryan, A.; Grigoryan, S.; Grinyov, B.; Grion, N.; Gronefeld, J. M.; Grosse-Oetringhaus, J. F.; Grossiord, J.-Y.; Grosso, R.; Guber, F.; Guernane, R.; Guerzoni, B.; Gulbrandsen, K.; Gunji, T.; Gupta, A.; Gupta, R.; Haake, R.; Haaland, Ø.; Hadjidakis, C.; Haiduc, M.; Hamagaki, H.; Hamar, G.; Hamon, J. C.; Harris, J. W.; Harton, A.; Hatzifotiadou, D.; Hayashi, S.; Heckel, S. T.; Helstrup, H.; Herghelegiu, A.; Herrera Corral, G.; Hess, B. A.; Hetland, K. F.; Hillemanns, H.; Hippolyte, B.; Horak, D.; Hosokawa, R.; Hristov, P.; Huang, M.; Humanic, T. J.; Hussain, N.; Hussain, T.; Hutter, D.; Hwang, D. S.; Ilkaev, R.; Inaba, M.; Incani, E.; Ippolitov, M.; Irfan, M.; Ivanov, M.; Ivanov, V.; Izucheev, V.; Jacazio, N.; Jacobs, P. M.; Jadhav, M. B.; Jadlovska, S.; Jadlovsky, J.; Jahnke, C.; Jakubowska, M. J.; Jang, H. J.; Janik, M. A.; Jayarathna, P. H. S. Y.; Jena, C.; Jena, S.; Jimenez Bustamante, R. T.; Jones, P. G.; Jung, H.; Jusko, A.; Kalinak, P.; Kalweit, A.; Kamin, J.; Kang, J. H.; Kaplin, V.; Kar, S.; Karasu Uysal, A.; Karavichev, O.; Karavicheva, T.; Karayan, L.; Karpechev, E.; Kebschull, U.; Keidel, R.; Keijdener, D. L. D.; Keil, M.; Mohisin Khan, M.; Khan, P.; Khan, S. A.; Khanzadeev, A.; Kharlov, Y.; Kileng, B.; Kim, D. W.; Kim, D. J.; Kim, D.; Kim, H.; Kim, J. S.; 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.; Kollegger, T.; Kolojvari, A.; Kondratiev, V.; Kondratyeva, N.; Kondratyuk, E.; Konevskikh, A.; Kopcik, M.; Kour, M.; Kouzinopoulos, C.; Kovalenko, O.; Kovalenko, V.; Kowalski, M.; Koyithatta Meethaleveedu, G.; Králik, I.; Kravčáková, A.; Kretz, M.; 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.; Kurashvili, P.; Kurepin, A.; Kurepin, A. B.; Kuryakin, A.; Kweon, M. J.; Kwon, Y.; La Pointe, S. L.; La Rocca, P.; Ladron de Guevara, P.; Lagana Fernandes, C.; Lakomov, I.; Langoy, R.; Lara, C.; Lardeux, A.; Lattuca, A.; Laudi, E.; Lea, R.; Leardini, L.; Lee, G. R.; Lee, S.; Lehas, F.; Lemmon, R. C.; Lenti, V.; Leogrande, E.; León Monzón, I.; León Vargas, H.; Leoncino, M.; Lévai, P.; Li, S.; Li, X.; Lien, J.; Lietava, R.; Lindal, S.; Lindenstruth, V.; Lippmann, C.; Lisa, M. A.; Ljunggren, H. M.; Lodato, D. F.; Loenne, P. I.; Loginov, V.; Loizides, C.; Lopez, X.; López Torres, E.; Lowe, A.; Luettig, P.; Lunardon, M.; Luparello, G.; Lutz, T. H.; Maevskaya, A.; Mager, M.; Mahajan, S.; Mahmood, S. M.; Maire, A.; Majka, R. D.; Malaev, M.; Maldonado Cervantes, I.; Malinina, L.; Mal'Kevich, D.; Malzacher, P.; Mamonov, A.; Manko, V.; Manso, F.; Manzari, V.; Marchisone, M.; Mareš, J.; Margagliotti, G. V.; Margotti, A.; Margutti, J.; Marín, A.; Markert, C.; Marquard, M.; Martin, N. A.; Martin Blanco, J.; Martinengo, P.; Martínez, M. I.; Martínez García, G.; Martinez Pedreira, M.; Mas, A.; Masciocchi, S.; Masera, M.; Masoni, A.; Massacrier, L.; Mastroserio, A.; Matyja, A.; Mayer, C.; Mazer, J.; Mazzoni, M. A.; McDonald, D.; Meddi, F.; Melikyan, Y.; Menchaca-Rocha, A.; Meninno, E.; Mercado Pérez, J.; Meres, M.; Miake, Y.; Mieskolainen, M. M.; Mikhaylov, K.; Milano, L.; Milosevic, J.; Minervini, L. M.; Mischke, A.; Mishra, A. N.; Miśkowiec, D.; Mitra, J.; Mitu, C. M.; Mohammadi, N.; Mohanty, B.; Molnar, L.; Montaño Zetina, L.; 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.; Munzer, R. H.; Murakami, H.; Murray, S.; Musa, L.; Musinsky, J.; Naik, B.; Nair, R.; Nandi, B. K.; Nania, R.; Nappi, E.; Naru, M. U.; Natal da Luz, H.; Nattrass, C.; Navarro, S. R.; Nayak, K.; Nayak, R.; Nayak, T. K.; Nazarenko, S.; Nedosekin, A.; Nellen, L.; 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.; Oh, S. K.; Ohlson, A.; Okatan, A.; Okubo, T.; Olah, L.; Oleniacz, J.; Oliveira da Silva, A. C.; Oliver, M. H.; Onderwaater, J.; Oppedisano, C.; Orava, R.; Ortiz Velasquez, A.; Oskarsson, A.; Otwinowski, J.; Oyama, K.; Ozdemir, M.; Pachmayer, Y.; Pagano, P.; Paić, G.; Pal, S. K.; Pan, J.; Pandey, A. K.; Papcun, P.; Papikyan, V.; Pappalardo, G. S.; Pareek, P.; Park, W. J.; Parmar, S.; Passfeld, A.; Paticchio, V.; Patra, R. N.; Paul, B.; Pei, H.; Peitzmann, T.; Pereira da Costa, H.; Peresunko, D.; Pérez Lara, C. E.; Perez Lezama, E.; Peskov, V.; Pestov, Y.; Petráček, V.; Petrov, V.; Petrovici, M.; Petta, C.; Piano, S.; Pikna, M.; Pillot, P.; Pimentel, L. O. D. L.; Pinazza, O.; Pinsky, L.; Piyarathna, D. B.; Płoskoń, M.; Planinic, M.; Pluta, J.; Pochybova, S.; Podesta-Lerma, P. L. M.; Poghosyan, M. G.; Polichtchouk, B.; Poljak, N.; Poonsawat, W.; Pop, A.; Porteboeuf-Houssais, S.; Porter, J.; Pospisil, J.; Prasad, S. K.; Preghenella, R.; Prino, F.; Pruneau, C. A.; Pshenichnov, I.; Puccio, M.; Puddu, G.; Pujahari, P.; Punin, V.; Putschke, J.; Qvigstad, H.; Rachevski, A.; Raha, S.; Rajput, S.; Rak, J.; Rakotozafindrabe, A.; Ramello, L.; Rami, F.; Raniwala, R.; Raniwala, S.; Räsänen, S. S.; Rascanu, B. T.; Rathee, D.; Read, K. F.; Redlich, K.; Reed, R. J.; Rehman, A.; Reichelt, P.; Reidt, F.; Ren, X.; Renfordt, R.; Reolon, A. R.; Reshetin, A.; Revol, J.-P.; Reygers, K.; Riabov, V.; Ricci, R. A.; Richert, T.; Richter, M.; Riedler, P.; Riegler, W.; Riggi, F.; Ristea, C.; Rocco, E.; Rodríguez Cahuantzi, M.; Rodriguez Manso, A.; Røed, K.; Rogochaya, E.; Rohr, D.; Röhrich, D.; Romita, R.; Ronchetti, F.; Ronflette, L.; Rosnet, P.; Rossi, A.; Roukoutakis, F.; Roy, A.; Roy, C.; Roy, P.; Rubio Montero, A. J.; Rui, R.; Russo, R.; Ryabinkin, E.; Ryabov, Y.; Rybicki, A.; Sadovsky, S.; Šafařík, K.; Sahlmuller, B.; Sahoo, P.; Sahoo, R.; Sahoo, S.; Sahu, P. K.; Saini, J.; Sakai, S.; Saleh, M. A.; Salzwedel, J.; Sambyal, S.; Samsonov, V.; Šándor, L.; Sandoval, A.; Sano, M.; Sarkar, D.; Sarma, P.; Scapparone, E.; Scarlassara, F.; Schiaua, C.; Schicker, R.; Schmidt, C.; Schmidt, H. R.; Schuchmann, S.; Schukraft, J.; Schulc, M.; Schuster, T.; Schutz, Y.; Schwarz, K.; Schweda, K.; Scioli, G.; Scomparin, E.; Scott, R.; Šefčík, M.; Seger, J. E.; Sekiguchi, Y.; Sekihata, D.; Selyuzhenkov, I.; Senosi, K.; Senyukov, S.; Serradilla, E.; Sevcenco, A.; Shabanov, A.; Shabetai, A.; Shadura, O.; Shahoyan, R.; Shangaraev, A.; Sharma, A.; Sharma, M.; Sharma, M.; Sharma, N.; Shigaki, K.; Shtejer, K.; Sibiriak, Y.; Siddhanta, S.; Sielewicz, K. M.; Siemiarczuk, T.; Silvermyr, D.; Silvestre, C.; Simatovic, G.; Simonetti, G.; Singaraju, R.; Singh, R.; Singha, S.; Singhal, V.; Sinha, B. C.; Sinha, T.; Sitar, B.; Sitta, M.; Skaali, T. B.; Slupecki, M.; Smirnov, N.; Snellings, R. J. M.; Snellman, T. W.; Søgaard, C.; Song, J.; Song, M.; Song, Z.; Soramel, F.; Sorensen, S.; de Souza, R. D.; Sozzi, F.; Spacek, M.; Spiriti, E.; Sputowska, I.; Spyropoulou-Stassinaki, M.; Stachel, J.; Stan, I.; Stankus, P.; Stefanek, G.; Stenlund, E.; Steyn, G.; Stiller, J. H.; Stocco, D.; Strmen, P.; Suaide, A. A. P.; Sugitate, T.; Suire, C.; Suleymanov, M.; Suljic, M.; Sultanov, R.; Šumbera, M.; Szabo, A.; Szanto de Toledo, A.; Szarka, I.; Szczepankiewicz, A.; Szymanski, M.; Tabassam, U.; Takahashi, J.; Tambave, G. J.; Tanaka, N.; Tangaro, M. A.; Tarhini, M.; Tariq, M.; Tarzila, M. G.; Tauro, A.; Tejeda Muñoz, G.; Telesca, A.; Terasaki, K.; Terrevoli, C.; Teyssier, B.; Thäder, J.; Thomas, D.; Tieulent, R.; Timmins, A. R.; Toia, A.; Trogolo, S.; Trombetta, G.; Trubnikov, V.; Trzaska, W. H.; Tsuji, T.; Tumkin, A.; Turrisi, R.; Tveter, T. S.; Ullaland, K.; Uras, A.; Usai, G. L.; Utrobicic, A.; Vajzer, M.; Vala, M.; Valencia Palomo, L.; Vallero, S.; 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.; Vechernin, V.; Veen, A. M.; Veldhoen, M.; Velure, A.; Venaruzzo, M.; Vercellin, E.; Vergara Limón, S.; Vernet, R.; Verweij, M.; Vickovic, L.; Viesti, G.; Viinikainen, J.; Vilakazi, Z.; Villalobos Baillie, O.; Villatoro Tello, A.; Vinogradov, A.; Vinogradov, L.; Vinogradov, Y.; Virgili, T.; Vislavicius, V.; Viyogi, Y. P.; Vodopyanov, A.; Völkl, M. A.; Voloshin, K.; Voloshin, S. A.; Volpe, G.; von Haller, B.; Vorobyev, I.; Vranic, D.; Vrláková, J.; Vulpescu, B.; Wagner, B.; Wagner, J.; Wang, H.; Wang, M.; Watanabe, D.; Watanabe, Y.; Weber, M.; Weber, S. G.; Weiser, D. F.; Wessels, J. P.; Westerhoff, U.; Whitehead, A. M.; Wiechula, J.; Wikne, J.; Wilde, M.; Wilk, G.; Wilkinson, J.; Williams, M. C. S.; Windelband, B.; Winn, M.; Yaldo, C. G.; Yang, H.; Yang, P.; Yano, S.; Yasar, C.; Yin, Z.; Yokoyama, H.; Yoo, I.-K.; Yoon, J. H.; Yurchenko, V.; Yushmanov, I.; Zaborowska, A.; Zaccolo, V.; Zaman, A.; Zampolli, C.; Zanoli, H. J. C.; Zaporozhets, S.; Zardoshti, N.; Zarochentsev, A.; Závada, P.; Zaviyalov, N.; Zbroszczyk, H.; Zgura, I. S.; 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.; Zyzak, M.; Alice Collaboration

2016-04-01

We report on measurements of a charge-dependent flow using a novel three-particle correlator with ALICE in Pb-Pb collisions at the CERN Large Hadron Collider (LHC), and discuss the implications for observation of local parity violation and the chiral magnetic wave (CMW) in heavy-ion collisions. Charge-dependent flow is reported for different collision centralities as a function of the event charge asymmetry. While our results are in qualitative agreement with expectations based on the CMW, the nonzero signal observed in higher harmonics correlations indicates a possible significant background contribution. We also present results on a differential correlator, where the flow of positive and negative charges is reported as a function of the mean charge of the particles and their pseudorapidity separation. We argue that this differential correlator is better suited to distinguish the differences in positive and negative charges expected due to the CMW and the background effects, such as local charge conservation coupled with strong radial and anisotropic flow.

Evolved phase separation toward balanced charge transport and high efficiency in polymer solar cells.

PubMed

Fan, Haijun; Zhang, Maojie; Guo, Xia; Li, Yongfang; Zhan, Xiaowei

2011-09-01

Understanding effect of morphology on charge carrier transport within polymer/fullerene bulk heterojunction is necessary to develop high-performance polymer solar cells. In this work, we synthesized a new benzodithiophene-based polymer with good self-organization behavior as well as favorable morphology evolution of its blend films with PC(71)BM under improved processing conditions. Charge carrier transport behavior of blend films was characterized by space charge limited current method. Evolved blend film morphology by controlling blend composition and additive content gradually reaches an optimized state, featured with nanoscale fibrilla polymer phase in moderate size and balanced mobility ratio close to 1:1 for hole and electron. This optimized morphology toward more balanced charge carrier transport accounts for the best power conversion efficiency of 3.2%, measured under simulated AM 1.5 solar irradiation 100 mW/cm(2), through enhancing short circuit current and reducing geminate recombination loss.

Functional Two-Dimensional Coordination Polymeric Layer as a Charge Barrier in Li-S Batteries.

PubMed

Huang, Jing-Kai; Li, Mengliu; Wan, Yi; Dey, Sukumar; Ostwal, Mayur; Zhang, Daliang; Yang, Chih-Wen; Su, Chun-Jen; Jeng, U-Ser; Ming, Jun; Amassian, Aram; Lai, Zhiping; Han, Yu; Li, Sean; Li, Lain-Jong

2018-01-23

Ultrathin two-dimensional (2D) polymeric layers are capable of separating gases and molecules based on the reported size exclusion mechanism. What is equally important but missing today is an exploration of the 2D layers with charge functionality, which enables applications using the charge exclusion principle. This work demonstrates a simple and scalable method of synthesizing a free-standing 2D coordination polymer Zn 2 (benzimidazolate) 2 (OH) 2 at the air-water interface. The hydroxyl (-OH) groups are stoichiometrically coordinated and implement electrostatic charges in the 2D structures, providing powerful functionality as a charge barrier. Electrochemical performance of the Li-S battery shows that the Zn 2 (benzimidazolate) 2 (OH) 2 coordination polymer layers efficiently mitigate the polysulfide shuttling effects and largely enhance the battery capacity and cycle performance. The synthesis of the proposed coordination polymeric layers is simple, scalable, cost saving, and promising for practical use in batteries.

Guest and solvent modulated photo-driven charge separation and triplet generation in a perylene bisimide cyclophane

DOE PAGES

Spenst, Peter; Young, Ryan M.; Wasielewski, Michael R.; ...

2016-05-18

Cofacial positioning of two perylene bisimide (PBI) chromophores at a distance of 6.5 Å in a cyclophane structure prohibits the otherwise common excimer formation and directs photoexcited singlet state relaxation towards intramolecular symmetry-breaking charge separation (τ CS = 161 ± 4 ps) in polar CH 2Cl 2, which is thermodynamically favored with a Gibbs free energy of ΔG CS = –0.32 eV. The charges then recombine slowly in τ CR = 8.90 ± 0.06 ns to form the PBI triplet excited state, which can be used subsequently to generate singlet oxygen in 27% quantum yield. This sequence of events ismore » eliminated by dissolving the PBI cyclophane in non-polar toluene, where only excited singlet state decay occurs. In contrast, complexation of electron-rich aromatic hydrocarbons by the host PBI cyclophane followed by photoexcitation of PBI results in ultrafast electron transfer (<10 ps) from the guest to the PBI in CH 2Cl 2. As a result, the rate constants for charge separation and recombination increase as the guest molecules become easier to oxidize, demonstrating that charge separation occurs close to the peak of the Marcus curve and the recombination lies far into the Marcus inverted region.« less

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 Effects on Coacervate-Driven Block Copolymer Self Assembly

NASA Astrophysics Data System (ADS)

Lytle, Tyer; Radhakrishna, Mithun; Sing, Charles

Two oppositely charged polymers can undergo associative phase separation in a salt solution in a process known as \\x98complex coacervation. Recent work has used this as a motif to control the self-assembly behavior of a mixture of oppositely-charged block copolymers which form nanoscale structures. The materials formed from these complex coacervate-block copolymers (BCPs) have potential use as drug delivery systems, gels, and sensors. We have developed a hybrid Monte Carlo-Single Chain in a Mean Field (MC-SCMF) simulation method that is able to determine morphological phase diagrams for BCPs. This technique is an efficient way to calculate morphological phase diagrams and provides a clear link between molecular level features and self-assembly behaviors. Morphological phase diagrams showing the effects of polymer concentration, salt concentration, chain length, and charge-block fraction at large charge densities on self-assembly behavior have been determined. An unexpected phase transition from disorder to hexagonal packing at large salt concentrations has been observed for charge-block fractions equal to and larger than 0.5. This is attributed to the salt filling space stabilizing the morphology of the BCP.

Charge Separation and Triplet Exciton Formation Pathways in Small-Molecule Solar Cells as Studied by Time-Resolved EPR Spectroscopy

DOE PAGES

Thomson, Stuart A. J.; Niklas, Jens; Mardis, Kristy L.; ...

2017-09-13

Organic solar cells are a promising renewable energy technology, offering the advantages of mechanical flexibility and solution processability. An understanding of the electronic excited states and charge separation pathways in these systems is crucial if efficiencies are to be further improved. Here we use light induced electron paramagnetic resonance (LEPR) spectroscopy and density functional theory calculations (DFT) to study the electronic excited states, charge transfer (CT) dynamics and triplet exciton formation pathways in blends of the small molecule donors (DTS(FBTTh 2) 2, DTS(F2BTTh 2) 2, DTS(PTTh 2) 2, DTG(FBTTh 2) 2 and DTG(F2BTTh 2) 2) with the fullerene derivative PCmore » 61BM. Using high frequency EPR the g-tensor of the positive polaron on the donor molecules was determined. The experimental results are compared with DFT calculations which reveal that the spin density of the polaron is distributed over a dimer or trimer. Time-resolved EPR (TR-EPR) spectra attributed to singlet CT states were identified and the polarization patterns revealed similar charge separation dynamics in the four fluorobenzothiadiazole donors, while charge separation in the DTS(PTTh 2) 2 blend is slower. Using TR-EPR we also investigated the triplet exciton formation pathways in the blend. The polarization patterns reveal that the excitons originate from both intersystem crossing (ISC) and back electron transfer (BET) processes. The DTS(PTTh 2) 2 blend was found to contain substantially more triplet excitons formed by BET than the fluorobenzothiadiazole blends. As a result, the higher BET triplet exciton population in the DTS(PTTh 2) 2 blend is in accordance with the slower charge separation dynamics observed in this blend.« less

Charge Separation and Triplet Exciton Formation Pathways in Small Molecule Solar Cells as Studied by Time-resolved EPR Spectroscopy.

PubMed

Thomson, Stuart A J; Niklas, Jens; Mardis, Kristy L; Mallares, Christopher; Samuel, Ifor D W; Poluektov, Oleg G

2017-10-19

Organic solar cells are a promising renewable energy technology, offering the advantages of mechanical flexibility and solution processability. An understanding of the electronic excited states and charge separation pathways in these systems is crucial if efficiencies are to be further improved. Here we use light induced electron paramagnetic resonance (LEPR) spectroscopy and density functional theory calculations (DFT) to study the electronic excited states, charge transfer (CT) dynamics and triplet exciton formation pathways in blends of the small molecule donors (DTS(FBTTh 2 ) 2 , DTS(F 2 BTTh 2 ) 2 , DTS(PTTh 2 ) 2 , DTG(FBTTh 2 ) 2 and DTG(F 2 BTTh 2 ) 2 ) with the fullerene derivative PC 61 BM. Using high frequency EPR the g-tensor of the positive polaron on the donor molecules was determined. The experimental results are compared with DFT calculations which reveal that the spin density of the polaron is distributed over a dimer or trimer. Time-resolved EPR (TR-EPR) spectra attributed to singlet CT states were identified and the polarization patterns revealed similar charge separation dynamics in the four fluorobenzothiadiazole donors, while charge separation in the DTS(PTTh 2 ) 2 blend is slower. Using TR-EPR we also investigated the triplet exciton formation pathways in the blend. The polarization patterns reveal that the excitons originate from both intersystem crossing (ISC) and back electron transfer (BET) processes. The DTS(PTTh 2 ) 2 blend was found to contain substantially more triplet excitons formed by BET than the fluorobenzothiadiazole blends. The higher BET triplet exciton population in the DTS(PTTh 2 ) 2 blend is in accordance with the slower charge separation dynamics observed in this blend.

Charge Separation and Triplet Exciton Formation Pathways in Small-Molecule Solar Cells as Studied by Time-Resolved EPR Spectroscopy

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

Thomson, Stuart A. J.; Niklas, Jens; Mardis, Kristy L.

Organic solar cells are a promising renewable energy technology, offering the advantages of mechanical flexibility and solution processability. An understanding of the electronic excited states and charge separation pathways in these systems is crucial if efficiencies are to be further improved. Here we use light induced electron paramagnetic resonance (LEPR) spectroscopy and density functional theory calculations (DFT) to study the electronic excited states, charge transfer (CT) dynamics and triplet exciton formation pathways in blends of the small molecule donors (DTS(FBTTh 2) 2, DTS(F2BTTh 2) 2, DTS(PTTh 2) 2, DTG(FBTTh 2) 2 and DTG(F2BTTh 2) 2) with the fullerene derivative PCmore » 61BM. Using high frequency EPR the g-tensor of the positive polaron on the donor molecules was determined. The experimental results are compared with DFT calculations which reveal that the spin density of the polaron is distributed over a dimer or trimer. Time-resolved EPR (TR-EPR) spectra attributed to singlet CT states were identified and the polarization patterns revealed similar charge separation dynamics in the four fluorobenzothiadiazole donors, while charge separation in the DTS(PTTh 2) 2 blend is slower. Using TR-EPR we also investigated the triplet exciton formation pathways in the blend. The polarization patterns reveal that the excitons originate from both intersystem crossing (ISC) and back electron transfer (BET) processes. The DTS(PTTh 2) 2 blend was found to contain substantially more triplet excitons formed by BET than the fluorobenzothiadiazole blends. As a result, the higher BET triplet exciton population in the DTS(PTTh 2) 2 blend is in accordance with the slower charge separation dynamics observed in this blend.« less

Nanotribological Properties of Positively and Negatively charged nanodiamonds as additives to solutions

NASA Astrophysics Data System (ADS)

Liu, Zijian; Corley, Steven; Shenderova, Olga; Brenner, Donald; Krim, Jacqueline

2013-03-01

Nano-diamond (ND) particles are known to be beneficial for wear and friction reduction when used as additives in liquids, but the fundamental origins of the improvement in tribological properties has not been established. In order to explore this issue, we have investigated the nanotribological properties of ND coated with self-assembled monolayers (SAM) as additives to solutions, employing gold/chrome coated quartz crystal microbalances (QCM). Measurements were performed with the QCM initially immersed in deionized water. ND particles with positively and negatively charged SAM end groups were then added to the water, while the frequency and amplitude of the QCM were monitored. Negative shifts in both the QCM frequency and amplitude were observed when ND with positively charged SAM end groups were added, while positive shifts in both the QCM frequency and amplitude were observed when ND with negatively charged ND end groups were added. The results are consistent with a lubricating effect for the negatively charged ND, but were only observed for sufficiently small negative ND particle size. Experiments on QCM surfaces with differing textures and roughness are in progress, to determine the separate contributing effects of surface roughness charge-water interactions. Funding provided by NSF DMR.

Gradient Self-Doped CuBi2O4 with Highly Improved Charge Separation Efficiency.

PubMed

Wang, Fuxian; Septina, Wilman; Chemseddine, Abdelkrim; Abdi, Fatwa F; Friedrich, Dennis; Bogdanoff, Peter; van de Krol, Roel; Tilley, S David; Berglund, Sean P

2017-10-25

A new strategy of using forward gradient self-doping to improve the charge separation efficiency in metal oxide photoelectrodes is proposed. Gradient self-doped CuBi 2 O 4 photocathodes are prepared with forward and reverse gradients in copper vacancies using a two-step, diffusion-assisted spray pyrolysis process. Decreasing the Cu/Bi ratio of the CuBi 2 O 4 photocathodes introduces Cu vacancies that increase the carrier (hole) concentration and lowers the Fermi level, as evidenced by a shift in the flat band toward more positive potentials. Thus, a gradient in Cu vacancies leads to an internal electric field within CuBi 2 O 4 , which can facilitate charge separation. Compared to homogeneous CuBi 2 O 4 photocathodes, CuBi 2 O 4 photocathodes with a forward gradient show highly improved charge separation efficiency and enhanced photoelectrochemical performance for reduction reactions, while CuBi 2 O 4 photocathodes with a reverse gradient show significantly reduced charge separation efficiency and photoelectrochemical performance. The CuBi 2 O 4 photocathodes with a forward gradient produce record AM 1.5 photocurrent densities for CuBi 2 O 4 up to -2.5 mA/cm 2 at 0.6 V vs RHE with H 2 O 2 as an electron scavenger, and they show a charge separation efficiency of 34% for 550 nm light. The gradient self-doping accomplishes this without the introduction of external dopants, and therefore the tetragonal crystal structure and carrier mobility of CuBi 2 O 4 are maintained. Lastly, forward gradient self-doped CuBi 2 O 4 photocathodes are protected with a CdS/TiO 2 heterojunction and coated with Pt as an electrocatalyst. These photocathodes demonstrate photocurrent densities on the order of -1.0 mA/cm 2 at 0.0 V vs RHE and evolve hydrogen with a faradaic efficiency of ∼91%.

Alloy and heterostructure architectures as promising tools for controlling electronic properties of semiconductor quantum dots

NASA Astrophysics Data System (ADS)

Vaxenburg, Roman; Lifshitz, Efrat

2012-02-01

Tunability of energy levels and wavefunctions of carriers in colloidal quantum dots (CQDs) has a marked effect on numerous physical aspects, such as Coulomb interactions and charge separation, which in turn has a direct impact on the functioning of CQD-based opto-electronic devices. The electronic properties of CQDs are conventionally controlled by variation of their size. Here we demonstrate a theoretical approach to engineer the electronic properties of IV-VI CQDs by introducing an alloy composition in core and core/shell heterostructures, having the general chemical formula PbSexS1-x/PbSeyS1-y (0 ≤ x ≤ 1, 0 ≤ y ≤ 1), while maintaining a constant size. The theoretical model considered an effective mass anisotropy and smooth potential step at the core/shell interface. The model revealed the influence induced by variation of chemical composition and core-to-shell division on the band-gap energy, remote states’ density, internal charge separation, electron-hole Coulomb interaction, and optical transition oscillator strength.

Energy exchange between a laser beam and charged particles using inverse transition radiation and method for its use

DOEpatents

Kimura, Wayne D.; Romea, Richard D.; Steinhauer, Loren C.

1998-01-01

A method and apparatus for exchanging energy between relativistic charged particles and laser radiation using inverse diffraction radiation or inverse transition radiation. The beam of laser light is directed onto a particle beam by means of two optical elements which have apertures or foils through which the particle beam passes. The two apertures or foils are spaced by a predetermined distance of separation and the angle of interaction between the laser beam and the particle beam is set at a specific angle. The separation and angle are a function of the wavelength of the laser light and the relativistic energy of the particle beam. In a diffraction embodiment, the interaction between the laser and particle beams is determined by the diffraction effect due to the apertures in the optical elements. In a transition embodiment, the interaction between the laser and particle beams is determined by the transition effect due to pieces of foil placed in the particle beam path.

Facile fabrication of BiVO4 nanofilms with controlled pore size and their photoelectrochemical performances

NASA Astrophysics Data System (ADS)

Feng, Chenchen; Jiao, Zhengbo; Li, Shaopeng; Zhang, Yan; Bi, Yingpu

2015-12-01

We demonstrate a facile method for the rational fabrication of pore-size controlled nanoporous BiVO4 photoanodes, and confirmed that the optimum pore-size distributions could effectively absorb visible light through light diffraction and confinement functions. Furthermore, in situ X-ray photoelectron spectroscopy (XPS) reveals more efficient photoexcited electron-hole separation than conventional particle films, induced by light confinement and rapid charge transfer in the inter-crossed worm-like structures.We demonstrate a facile method for the rational fabrication of pore-size controlled nanoporous BiVO4 photoanodes, and confirmed that the optimum pore-size distributions could effectively absorb visible light through light diffraction and confinement functions. Furthermore, in situ X-ray photoelectron spectroscopy (XPS) reveals more efficient photoexcited electron-hole separation than conventional particle films, induced by light confinement and rapid charge transfer in the inter-crossed worm-like structures. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr06584d

Nano-TiO2 decorated carbon coating on the separator to physically and chemically suppress the shuttle effect for lithium-sulfur battery

NASA Astrophysics Data System (ADS)

Shao, Hongyuan; Wang, Weikun; Zhang, Hao; Wang, Anbang; Chen, Xiaonong; Huang, Yaqin

2018-02-01

Despite recent progress in designing modified separators for lithium-sulfur (Li-S) batteries, detail in optimizing the synergistic effect between chemical and physical immobilization for lithium polysulfides (LiPS) in modified separator hasn't been investigated totally. Here, a nano-TiO2 decorated carbon layer (T-DCL) has been successfully applied to modify separator for the Li-S battery. The results indicate that appropriate weight percentage of nano-TiO2 uniformly distributed in conductive carbon layer is effective to chemically and physically immobilize for LiPS, and promote the electron transfer during discharge/charge process. The performance of the modified Li-S battery with T-DCL separator are significantly enhanced, with a specific capacity of 883 mAh g-1 retained after 180 cycles at 0.1 C and 762 mAh g-1 retained after 200 cycles at 0.5C, which are much higher than that of separators only coated with TiO2 layer or conductive carbon layer. Besides, the separator coated with T-DCL also shows low electrochemical impedance and good lithium anode protection. These results indicate that separator with T-DCL is promising to balance the physical and chemical LiPS trapping effect, and optimize the electrochemical performance for Li-S battery.

Effects of Magnetic Nanoparticles and External Magnetostatic Field on the Bulk Heterojunction Polymer Solar Cells

DOE PAGES

Wang, Kai; Yi, Chao; Liu, Chang; ...

2015-03-18

The price of energy to separate tightly bound electron-hole pair (or charge-transfer state) and extract freely movable charges from low-mobility materials represents fundamental losses for many low-cost photovoltaic devices. In bulk heterojunction (BHJ) polymer solar cells (PSCs), approximately 50% of the total efficiency lost among all energy loss pathways is due to the photogenerated charge carrier recombination within PSCs and low charge carrier mobility of disordered organic materials. To address these issues, we introduce magnetic nanoparticles (MNPs) and orientate these MNPS within BHJ composite by an external magnetostatic field. Over 50% enhanced efficiency was observed from BHJ PSCs incorporated withmore » MNPs and an external magnetostatic field alignment when compared to the control BHJ PSCs. The optimization of BHJ thin film morphology, suppression of charge carrier recombination, and enhancement in charge carrier collection result in a greatly increased short-circuit current density and fill factor, as a result, enhanced power conversion efficiency.« less

Measurement of the charged-particle multiplicity inside jets from $$\\sqrt{s}=8$$ $${\\mathrm{TeV}}$$ pp collisions with the ATLAS detector

DOE PAGES

Aad, G.; Abbott, B.; Abdallah, J.; ...

2016-06-13

The number of charged particles inside jets is a widely used discriminant for identifying the quark or gluon nature of the initiating parton and is sensitive to both the perturbative and non-perturbative components of fragmentation. This paper presents a measurement of the average number of charged particles with p T > 500 MeV inside high-momentum jets in dijet events using 20.3 fb -1 of data recorded with the ATLAS detector in pp collisions at √s=8 TeV collisions at the LHC. The jets considered have transverse momenta from 50 GeV up to and beyond 1.5 TeV . The reconstructed charged-particle trackmore » multiplicity distribution is unfolded to remove distortions from detector effects and the resulting charged-particle multiplicity is compared to several models. Lastly, quark and gluon jet fractions are used to extract the average charged-particle multiplicity for quark and gluon jets separately.« less

Thermal analysis of the vertical bridgman semiconductor crystal growth technique. Ph.D. Thesis

NASA Technical Reports Server (NTRS)

Jasinski, T. J.

1982-01-01

The quality of semiconductor crystals grown by the vertical Bridgman technique is strongly influenced by the axial and radial variations of temperature within the charge. The relationship between the thermal parameters of the vertical Bridgman system and the thermal behavior of the charge are examined. Thermal models are developed which are capable of producing results expressable in analytical form and which can be used without recourse to extensive computer work for the preliminary thermal design of vertical Bridgman crystal growth systems. These models include the effects of thermal coupling between the furnace and the charge, charge translation rate, charge diameter, thickness and thermal conductivity of the confining crucible, thermal conductivity change and liberation of latent heat at the growth interface, and infinite charge length. The hot and cold zone regions, considered to be at spatially uniform temperatures, are separated by a gradient control region which provides added thermal design flexibility for controlling the temperature variations near the growth interface.

The Effect of Voltage Charging on the Transport Properties of Gold Nanotube Membranes.

PubMed

Experton, Juliette; Martin, Charles R

2018-05-01

Porous membranes are used in chemical separations and in many electrochemical processes and devices. Research on the transport properties of a unique class of porous membranes that contain monodisperse gold nanotubes traversing the entire membrane thickness is reviewed here. These gold nanotubes can act as conduits for ionic and molecular transports through the membrane. Because the tubes are electronically conductive, they can be electrochemically charged by applying a voltage to the membrane. How this "voltage charging" affects the transport properties of gold nanotube membranes is the subject of this Review. Experiments showing that voltage charging can be used to reversibly switch the membrane between ideally cation- and anion-transporting states are reviewed. Voltage charging can also be used to enhance the ionic conductivity of gold nanotube membranes. Finally, voltage charging to accomplish electroporation of living bacteria as they pass through gold nanotube membranes is reviewed. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Stark tuning and electrical charge state control of single divacancies in silicon carbide

NASA Astrophysics Data System (ADS)

de las Casas, Charles F.; Christle, David J.; Ul Hassan, Jawad; Ohshima, Takeshi; Son, Nguyen T.; Awschalom, David D.

2017-12-01

Neutrally charged divacancies in silicon carbide (SiC) are paramagnetic color centers whose long coherence times and near-telecom operating wavelengths make them promising for scalable quantum communication technologies compatible with existing fiber optic networks. However, local strain inhomogeneity can randomly perturb their optical transition frequencies, which degrades the indistinguishability of photons emitted from separate defects and hinders their coupling to optical cavities. Here, we show that electric fields can be used to tune the optical transition frequencies of single neutral divacancy defects in 4H-SiC over a range of several GHz via the DC Stark effect. The same technique can also control the charge state of the defect on microsecond timescales, which we use to stabilize unstable or non-neutral divacancies into their neutral charge state. Using fluorescence-based charge state detection, we show that both 975 nm and 1130 nm excitation can prepare their neutral charge state with near unity efficiency.

Out-of-equilibrium chiral magnetic effect from chiral kinetic theory

NASA Astrophysics Data System (ADS)

Huang, Anping; Jiang, Yin; Shi, Shuzhe; Liao, Jinfeng; Zhuang, Pengfei

2018-02-01

Recently there has been significant interest in the macroscopic manifestation of chiral anomaly in many-body systems of chiral fermions. A notable example is the Chiral Magnetic Effect (CME). Enthusiastic efforts have been made to search for the CME in the quark-gluon plasma created in heavy ion collisions. A crucial challenge is that the extremely strong magnetic field in such collisions may last only for a brief moment and the CME current may have to occur at so early a stage that the quark-gluon matter is still far from thermal equilibrium. This thus requires modeling of the CME in an out-of-equilibrium setting. With the recently developed theoretical tool of chiral kinetic theory, we make a first phenomenological study of the CME-induced charge separation during the pre-thermal stage in heavy ion collisions. The effect is found to be very sensitive to the time dependence of the magnetic field and also influenced by the initial quark momentum spectrum as well as the relaxation time of the system evolution toward thermal equilibrium. Within the present approach, such pre-thermal charge separation is found to be modest.

Effect of charge ordering and phase separation on the electrical and magnetoresistive properties of polycrystalline La0.4Eu0.1Ca0.5MnO3

NASA Astrophysics Data System (ADS)

Krichene, A.; Boujelben, W.; Mukherjee, S.; Shah, N. A.; Solanki, P. S.

2018-03-01

We have investigated the effect of charge ordering and phase separation on the electrical and magnetotransport properties of La0.4Eu0.1Ca0.5MnO3 polycrystalline sample. Temperature dependence of resistivity shows a metal-insulator transition at transition temperature Tρ. A hysteretic behavior is observed for zero field resistivity curves with Tρ = 128 K on cooling process and Tρ = 136 K on warming process. Zero field resistivity curves follow Zener polynomial law in the metallic phase with unusual n exponent value ∼9. Presence of resistivity minimum at low temperatures has been ascribed to the coulombic electron-electron scattering process. Resistivity modification due to the magnetic field cycling testifies the presence of the training effect. Magnetization and resistivity appear to be highly correlated. Magnetoresistive study reveals colossal values of negative magnetoresistance reaching about 75% at 132 K under only 2T applied field. Colossal values of magnetoresistance suggest the possibility of using this sample for magnetic field sensing and spintronic applications.

An Analytical Model of Tribocharging in Regolith

NASA Astrophysics Data System (ADS)

Carter, D. P.; Hartzell, C. M.

2015-12-01

Nongravitational forces, including electrostatic forces and cohesion, can drive the behavior of regolith in low gravity environments such as the Moon and asteroids. Regolith is the 'skin' of solid planetary bodies: it is the outer coating that is observed by orbiters and the first material contacted by landers. Triboelectric charging, the phenomenon by which electrical charge accumulates during the collision or rubbing of two surfaces, has been found to occur in initially electrically neutral granular mixtures. Although charge transfer is often attributed to chemical differences between the different materials, charge separation has also been found to occur in mixtures containing grains of a single material, but with a variety of grain sizes. In such cases, the charge always separates according to grain size; typically the smaller grains acquire a more negative charge than the larger grains. Triboelectric charging may occur in a variety of planetary phenomena (including mass wasting and dust storms) as well as during spacecraft-surface interactions (including sample collection and wheel motion). Interactions between charged grains or with the solar wind plasma could produce regolith motion. However, a validated, predictive model of triboelectric charging between dielectric grains has not yet been developed. A model for such size-dependent charge separation will be presented, demonstrating how random collisions between initially electrically neutral grains lead to net migration of electrons toward the smaller grains. The model is applicable to a wide range of single-material granular mixtures, including those with unusual or wildly varying size distributions, and suggests a possible mechanism for the reversal of the usual size-dependent charge polarity described above. This is a significant improvement over existing charge exchange models, which are restricted to two discrete grains sizes and provide severely limited estimates for charge magnitude. We will also discuss the design of an experiment planned to test the charging estimates provided by the model presented and the potential implications for our understanding of regolith behavior.

Strong field gravitational lensing by a charged Galileon black hole

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

Zhao, Shan-Shan; Xie, Yi, E-mail: clefairy035@163.com, E-mail: yixie@nju.edu.cn

Strong field gravitational lensings are dramatically disparate from those in the weak field by representing relativistic images due to light winds one to infinity loops around a lens before escaping. We study such a lensing caused by a charged Galileon black hole, which is expected to have possibility to evade no-hair theorem. We calculate the angular separations and time delays between different relativistic images of the charged Galileon black hole. All these observables can potentially be used to discriminate a charged Galileon black hole from others. We estimate the magnitudes of these observables for the closest supermassive black hole Sgrmore » A*. The strong field lensing observables of the charged Galileon black hole can be close to those of a tidal Reissner-Nordström black hole or those of a Reissner-Nordström black hole. It will be helpful to distinguish these black holes if we can separate the outermost relativistic images and determine their angular separation, brightness difference and time delay, although it requires techniques beyond the current limit.« less

Substituent effects on photosensitized splitting of thymine cyclobutane dimer by an attached indole.

PubMed

Tang, Wenjian; Zhou, Hongmei; Wang, Jing; Pan, Chunxiao; Shi, Jingbo; Song, Qinhua

2012-12-21

In chromophore-containing cyclobutane pyrimidine dimer (CPD) model systems, solvent effects on the splitting efficiency may depend on the length of the linker, the molecular conformation, and the oxidation potential of the donor. To further explore the relationship between chromophore structure and splitting efficiency, we prepared a series of substituted indole-T< >T model compounds 2 a-2 g and measured their splitting quantum yields in various solvents. Two reverse solvent effects were observed: an increase in splitting efficiency in solvents of lower polarity for models 2 a-2 d with an electron-donating group (EDG), and vice versa for models 2 e-2 g with an electron-withdrawing group (EWG). According to the Hammett equation, the negative value of the slope of the Hammett plot indicates that the indole moiety during the T< >T-splitting reaction loses negative charge, and the larger negative value implies that the repair reaction is more sensitive to substituent effects in low-polarity solvents. The EDGs of the models 2 a-2 d can delocalize the charge-separated state, and low-polarity solvents make it more stable, which leads to higher splitting efficiency in low-polarity solvents. Conversely, the EWGs of models 2 e-2 g favor destabilization of the charge-separated state, and high-polarity solvents decrease the destabilization and hence lead to more efficient splitting in high-polarity solvents. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Graphene supported silver@silver chloride & ferroferric oxide hybrid, a magnetically separable photocatalyst with high performance under visible light irradiation

NASA Astrophysics Data System (ADS)

Zhong, Suting; Jiang, Wei; Han, Mei; Liu, Gongzong; Zhang, Na; Lu, Yue

2015-08-01

A stable magnetic separable plasmonic photocatalyst was successfully fabricated by grafting silver@silver chloride (Ag@AgCl) and ferroferric oxide (Fe3O4) nanoparticles on graphene sheets. The composite exhibited high activity degrading methylene blue (MB) and rhodamine B (RB) under visible light irradiation: decomposition 97.4% of MB in 100 min and 97.9% of RB in 120 min. The enhanced photocatalytic activities can be attributed to synergistic effect between Ag@AgCl and graphene: the effective charge transfer from Ag@AgCl to graphene thus promotes the separation of electron-hole pairs. Moreover, the excellent magnetic property gives a more convenient way to recycle the photocatalysts.

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.

Edge effects in vertically-oriented graphene based electric double-layer capacitors

NASA Astrophysics Data System (ADS)

Yang, Huachao; Yang, Jinyuan; Bo, Zheng; Zhang, Shuo; Yan, Jianhua; Cen, Kefa

2016-08-01

Vertically-oriented graphenes (VGs) have been demonstrated as a promising active material for electric double-layer capacitors (EDLCs), partially due to their edge-enriched structure. In this work, the 'edge effects', i.e., edges as the promoters of high capacitance, in VG based EDLCs are investigated with experimental research and numerical simulations. VGs with diverse heights (i.e., edge-to-basal ratios) and edge densities are prepared with varying the plasma-enabled growth time and employing different plasma sources. Electrochemical measurements show that the edges play a predominant role on the charge storage behavior of VGs. A simulation is further conducted to unveil the roles of the edges on the separation and adsorption of ions within VG channels. The initial charge distribution of a VG plane is obtained with density functional theory (DFT) calculations, which is subsequently applied to a molecular dynamics (MD) simulation system to gain the insights into the microscope EDLC structures. Compared with the basal planes, the edges present higher initial charge density (by 4.2 times), higher ion packing density (by 2.6 times), closer ion packing location (by 0.8 Å), and larger ion separation degree (by 14%). The as-obtained findings will be instructive in designing the morphology and structure of VGs for enhanced capacitive performances.

Hierarchical FeTiO3-TiO2 hollow spheres for efficient simulated sunlight-driven water oxidation.

PubMed

Han, Taoran; Chen, Yajie; Tian, Guohui; Wang, Jian-Qiang; Ren, Zhiyu; Zhou, Wei; Fu, Honggang

2015-10-14

Oxygen generation is the key step for the photocatalytic overall water splitting and considered to be kinetically more challenging than hydrogen generation. Here, an effective water oxidation catalyst of hierarchical FeTiO3-TiO2 hollow spheres are prepared via a two-step sequential solvothermal processes and followed by thermal treatment. The existence of an effective heterointerface and built-in electric field in the surface space charge region in FeTiO3-TiO2 hollow spheres plays a positive role in promoting the separation of photoinduced electron-hole pairs. Surface photovoltage, transient-state photovoltage, fluorescence and electrochemical characterization are used to investigate the transfer process of photoinduced charge carriers. The photogenerated charge carriers in the hierarchical FeTiO3-TiO2 hollow spheres with a proper molar ratio display much higher separation efficiency and longer lifetime than those in the FeTiO3 alone. Moreover, it is suggested that the hierarchical porous hollow structure can contribute to the enhancement of light utilization, surface active sites and material transportation through the framework walls. This specific synergy significantly contributes to the remarkable improvement of the photocatalytic water oxidation activity of the hierarchical FeTiO3-TiO2 hollow spheres under simulated sunlight (AM1.5).

Graphene assisted effective hole-extraction on In2O3:H/CH3NH3PbI3 interface: Studied by modulated surface spectroscopy

NASA Astrophysics Data System (ADS)

Vinoth Kumar, Sri Hari Bharath; Muydinov, Ruslan; Kol'tsova, Tat‘yana; Erfurt, Darja; Steigert, Alexander; Tolochko, Oleg; Szyszka, Bernd

2018-01-01

Charge separation in CH3NH3PbI3 (MAPbI3) films deposited on a hydrogen doped indium oxide (In2O3:H) photoelectrode was investigated by modulated surface photovoltage (SPV) spectroscopy in a fixed capacitor arrangement. It was found that In2O3:H reproducibly extracts photogenerated-holes from MAPbI3 films. The oxygen-plasma treatment of the In2O3:H surface is suggested to be a reason for this phenomenon. Introducing graphene interlayer increased charge separation nearly 6 times as compared to that on the In2O3:H/MAPbI3 interface. Furthermore, it is confirmed by SPV spectroscopy that the defects of the MAPbI3 interface are passivated by graphene.

Energy storage device with large charge separation

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

Holme, Timothy P.; Prinz, Friedrich B.; Iancu, Andrei T.

High density energy storage in semiconductor devices is provided. There are two main aspects of the present approach. The first aspect is to provide high density energy storage in semiconductor devices based on formation of a plasma in the semiconductor. The second aspect is to provide high density energy storage based on charge separation in a p-n junction.

Energy storage device with large charge separation

DOEpatents

Holme, Timothy P.; Prinz, Friedrich B.; Iancu, Andrei

2016-04-12

High density energy storage in semiconductor devices is provided. There are two main aspects of the present approach. The first aspect is to provide high density energy storage in semiconductor devices based on formation of a plasma in the semiconductor. The second aspect is to provide high density energy storage based on charge separation in a p-n junction.

Ligand-modulated interactions between charged monolayer-protected Au144 (SR)60 gold nanoparticles in physiological saline

NASA Astrophysics Data System (ADS)

Villarreal, Oscar; Chen, Liao; Whetten, Robert; Yacaman, Miguel

2015-03-01

We studied the interactions of functionalized Au144 nanoparticles (NPs) in a near-physiological environment through all-atom molecular dynamics simulations. The AuNPs were coated with a homogeneous selection of 60 thiolates: 11-mercapto-1-undecanesulfonate, 5-mercapto-1-pentanesulfonate, 5-mercapto-1-pentane-amine, 4-mercapto-benzoate or 4-mercapto-benzamide. These ligands were selected to elucidate how the aggregation behavior depends on the ligands' sign of charge, length, and flexibility. Simulating the dynamics of a pair of identical AuNPs in a cell of saline of 150 mM NaCl in addition to 120 Na+/Cl- counter-ions, we computed the aggregation affinities from the potential of mean force as a function of the pair separation. We found that NPs coated with negatively charged, short ligands have the strongest affinities mediated by multiple Na+ counter-ions residing on a plane in-between the pair and forming ``salt bridges'' to both NPs. Positively charged NPs have weaker affinities, as Cl counter-ions form fewer and weaker salt bridges. The longer ligands' large fluctuations disfavor the forming of salt bridges, enable hydrophobic contact between the exposed hydrocarbon chains and interact at greater separations due to the fact that the screening effect is rather incomplete. Supported by the CONACYT, NIH, NSF and TACC.

32 CFR 776.85 - Effect of separate proceeding.

Code of Federal Regulations, 2010 CFR

2010-07-01

... that issue during an ethics investigation. A subsequent ethics investigation based on such misconduct... the basis for ethics charges under this instruction, the Rules Counsel may dispense with the preliminary inquiry and proceed directly with an ethics investigation. (c) In those cases in which a covered...

Final Technical Report for the Energy Frontier Research Center Understanding Charge Separation and Transfer at Interfaces in Energy Materials (EFRC:CST)

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

Vanden Bout, David A.

2015-09-14

Our EFRC was founded with the vision of creating a broadly collaborative and synergistic program that would lead to major breakthroughs in the molecular-level understanding of the critical interfacial charge separation and charge transfer (CST) processes that underpin the function of candidate materials for organic photovoltaic (OPV) and electrical-energy-storage (EES) applications. Research in these energy contexts shares an imposing challenge: How can we understand charge separation and transfer mechanisms in the presence of immense materials complexity that spans multiple length scales? To address this challenge, our 50-member Center undertook a total of 28 coordinated research projects aimed at unraveling themore » CST mechanisms that occur at interfaces in these nanostructured materials. This rigorous multi-year study of CST interfaces has greatly illuminated our understanding of early-timescale processes (e.g., exciton generation and dissociation dynamics at OPV heterojunctions; control of Li+-ion charging kinetics by surface chemistry) occurring in the immediate vicinity of interfaces. Program outcomes included: training of 72 graduate student and postdoctoral energy researchers at 5 institutions and spanning 7 academic disciplines in science and engineering; publication of 94 peer-reviewed journal articles; and dissemination of research outcomes via 340 conference, poster and other presentations. Major scientific outcomes included: implementation of a hierarchical strategy for understanding the electronic communication mechanisms and ultimate fate of charge carriers in bulk heterojunction OPV materials; systematic investigation of ion-coupled electron transfer processes in model Li-ion battery electrode/electrolyte systems; and the development and implementation of 14 unique technologies and instrumentation capabilities to aid in probing sub-ensemble charge separation and transfer mechanisms.« less

Electrokinetic dispersion in microfluidic separation systems

NASA Astrophysics Data System (ADS)

Molho, Joshua Irving

Numerous efforts have focused on engineering miniaturized chemical analysis devices that are faster, more portable and consume smaller volumes of expensive reagents than their macroscale counterparts. Many of these analysis devices employ electrokinetic effects to transport picoliter volumes of liquids and to separate chemical species from an initially mixed sample volume. In these microfluidic separation systems, dispersion must be minimized to obtain the highest resolution separation possible. This work focuses on modeling, simulation and experimental measurement of two electrokinetic dispersion mechanisms that can reduce the effectiveness of microfluidic separation systems: dispersion resulting from non-uniform wall zeta-potential, and dispersion caused by microchannel turns. When the surface of a microchannel has non-uniform zeta-potential (e.g., if the surface charge varies along the length of the microchannel), an applied electric field creates both electroosmotic and pressure-driven flow. A caged-fluorescence imaging technique was used to visualize the dispersion caused by this electrokinetically induced pressure-driven flow. A simple model for a single channel with an axially varying surface charge is presented and compared to experimental measurements. Microchannel turns have been shown to create dispersion of electrokinetically transported analyte bands. Using a method of moments analysis, a model is developed that quantifies this dispersion and identifies the conditions under which turn dispersion limits the resolution of a microfluidic separation system. Measurements using the caged-fluorescence visualization technique were used to verify this model. New turn geometries are presented and were optimized using both a reduced parameter technique as well as a more generalized, numerical shape optimization approach. These improved turn designs were manufactured using two fabrication techniques and then tested experimentally. The turn optimization approaches and resulting turn geometries described here are shown to reduce turn dispersion to less than 1% of the dispersion caused by unoptimized, constant-width turns.

Separation and Purification of Mineral Salts from Spacecraft Wastewater Processing via Electrostatic Beneficiation

NASA Technical Reports Server (NTRS)

Miles, John D., II; Lunn, Griffin

2013-01-01

Electrostatic separation is a class of material processing technologies commonly used for the sorting of coarse mixtures by means of electrical forces acting on charged or polarized particles. Most if not all of the existing tribo-electrostatic separators had been initially developed for mineral ores beneficiation. It is a well-known process that has been successfully used to separate coal from minerals. Potash (potassium) enrichment where underground salt mines containing large amounts of sodium is another use of this techno logy. Through modification this technology can be used for spacecraft wastewater brine beneficiation. This will add in closing the gap beeen traveling around Earth's Gravity well and long-term space explorations. Food has been brought on all man missions, which is why plant growth for food crops continues to be of interest to NASA. For long-term mission considerations food productions is one of the top priorities. Nutrient recovery is essential for surviving in or past low earth orbit. In our advance bio-regenerative process instead of nitrogen gas produced; soluble nitrate salts that can be recovered for plant fertilizer would be produced instead. The only part missing is the beneficiation of brine to separate the potassium from the sodium. The use of electrostatic beneficiation in this experiment utilizes the electrical charge differences between aluminum and dried brine by surface contact. The helixes within the aluminum tribocharger allows for more surface contact when being agitated. When two materials are in contact, the material with the highest affinity for electrons becomes negatively charged, while the other becomes positively charged. This contact exchange of charge may cause the particles to agglomerate depending on their residence time within the tribocharger, compromising the efficiency of separation. The aim of this experiment is to further the development in electrostatic beneficiation by optimizing the separation of ersatz and possibly real wastewater brine residues. In doing so, ideally it will yield a high potassium enrichment for use in spacecraft plant systems.

Electrokinetic Response of Charge-Selective Nanostructured Polymeric Membranes

NASA Astrophysics Data System (ADS)

Schiffbauer, Jarrod; Li, Diya; Gao, Feng; Phillip, William; Chang, Hsueh-Chia

2017-11-01

Nanostructured polymeric membranes, with a tunable pore size and ease of surface molecular functionalization, are a promising material for separations, filtration, and sensing applications. Recently, such membranes have been fabricated wherein the ion selectivity is imparted by self-assembled functional groups through a two-step process. Amine groups are used to provide a positive surface charge and acid groups are used to yield a negative charge. The membranes can be fabricated as either singly-charged or patterned/mosaic membranes, where there are alternating regions of amine- lined or acid-lined pores. We demonstrate that such membranes, in addition to having many features in common with other charge selective membranes (i.e. AMX or Nafion), display a unique single-membrane rectification behavior. This is due to the asymmetric distribution of charged functional groups during the fabrication process. We demonstrate this rectification effect using both dc current-voltage characteristics as well as dc-biased electrical impedance spectroscopy. Furthermore, surface charge changes due to dc concentration polarization and generation of localized pH shifts are monitored using electrical impedance spectroscopy. (formerly at University of Notre Dame).

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.

A lithium oxygen secondary battery

NASA Technical Reports Server (NTRS)

Semkow, Krystyna W.; Sammells, Anthony F.

1987-01-01

Some recent work on a lithium-oxygen secondary battery is reported in which stabilized zirconia oxygen vacancy conducting solid electrolytes were used for the effective separation of respective half-cell reactions. The electroactive material consisted of alloys possessing the general composition Li(x)FeSi2 immersed in a ternary molten salt comprising LiF, LiCl, and Li2O. The manufacture of the cell is described, and discharge-current voltage curves for partially charged cells are shown and discussed. A galvanostatic IR free-changing curve and an IR-free charge-discharge curve are also shown.

Specific ion effects on membrane potential and the permselectivity of ion exchange membranes.

PubMed

Geise, Geoffrey M; Cassady, Harrison J; Paul, Donald R; Logan, Bruce E; Hickner, Michael A

2014-10-21

Membrane potential and permselectivity are critical parameters for a variety of electrochemically-driven separation and energy technologies. An electric potential is developed when a membrane separates electrolyte solutions of different concentrations, and a permselective membrane allows specific species to be transported while restricting the passage of other species. Ion exchange membranes are commonly used in applications that require advanced ionic electrolytes and span technologies such as alkaline batteries to ammonium bicarbonate reverse electrodialysis, but membranes are often only characterized in sodium chloride solutions. Our goal in this work was to better understand membrane behaviour in aqueous ammonium bicarbonate, which is of interest for closed-loop energy generation processes. Here we characterized the permselectivity of four commercial ion exchange membranes in aqueous solutions of sodium chloride, ammonium chloride, sodium bicarbonate, and ammonium bicarbonate. This stepwise approach, using four different ions in aqueous solution, was used to better understand how these specific ions affect ion transport in ion exchange membranes. Characterization of cation and anion exchange membrane permselectivity, using these ions, is discussed from the perspective of the difference in the physical chemistry of the hydrated ions, along with an accompanying re-derivation and examination of the basic equations that describe membrane potential. In general, permselectivity was highest in sodium chloride and lowest in ammonium bicarbonate solutions, and the nature of both the counter- and co-ions appeared to influence measured permselectivity. The counter-ion type influences the binding affinity between counter-ions and polymer fixed charge groups, and higher binding affinity between fixed charge sites and counter-ions within the membrane decreases the effective membrane charge density. As a result permselectivity decreases. The charge density and polarizability of the co-ions also appeared to influence permselectivity leading to ion-specific effects; co-ions that are charge dense and have low polarizability tended to result in high membrane permselectivity.

Pi-Pi contacts are an overlooked protein feature relevant to phase separation

PubMed Central

Vernon, Robert McCoy; Chong, Paul Andrew; Tsang, Brian; Kim, Tae Hun; Bah, Alaji; Farber, Patrick; Lin, Hong

2018-01-01

Protein phase separation is implicated in formation of membraneless organelles, signaling puncta and the nuclear pore. Multivalent interactions of modular binding domains and their target motifs can drive phase separation. However, forces promoting the more common phase separation of intrinsically disordered regions are less understood, with suggested roles for multivalent cation-pi, pi-pi, and charge interactions and the hydrophobic effect. Known phase-separating proteins are enriched in pi-orbital containing residues and thus we analyzed pi-interactions in folded proteins. We found that pi-pi interactions involving non-aromatic groups are widespread, underestimated by force-fields used in structure calculations and correlated with solvation and lack of regular secondary structure, properties associated with disordered regions. We present a phase separation predictive algorithm based on pi interaction frequency, highlighting proteins involved in biomaterials and RNA processing. PMID:29424691

Encapsulating Bi2Ti2O7 (BTO) with reduced graphene oxide (RGO): an effective strategy to enhance photocatalytic and photoelectrocatalytic activity of BTO.

PubMed

Gupta, Satyajit; Subramanian, Vaidyanathan Ravi

2014-11-12

Multimetal oxides (AxByOz) offer a higher degree of freedom compared to single metal oxides (AOx) in that these oxides facilitate (i) designing nanomaterials with greater stability, (ii) tuning of the optical bandgap, and (iii) promoting visible light absorption. However, all AxByOz materials such as pyrochlores (A2B2O7)--referred to here as band-gap engineered composite oxide nanomaterials or BECONs--are traditionally prone to severe charge recombination at their surface. To alleviate the charge recombination, an effective strategy is to employ reduced graphene oxide (RGO) as a charge separator. The BECON and the RGO with oppositely charged functional groups attached to them can be integrated at the interface by employing a simple electrostatic self-assembly approach. As a case study, the approach is demonstrated using the Pt-free pyrochlore bismuth titanate (BTO) with RGO, and the application of the composite is investigated for the first time. When tested as a photocatalyst toward hydrogen production, an increase of ∼ 250% using BTO in the presence of RGO was observed. Further, photoelectrochemical measurements indicate an enhancement of ∼ 130% in the photocurrent with RGO inclusion. These two results firmly establish the viability of the electrostatic approach and the inclusion of RGO. The merits of the RGO addition is identified as (i) the RGO-assisted improvement in the separation of the photogenerated charges of BTO, (ii) the enhanced utilization of the charges in a photocatalytic process, and (iii) the maintenance of the BTO/RGO structural integrity after repeated use (established through reusability analysis). The success of the self-assembly strategy presented here lays the foundation for developing other forms of BECONs, belonging to perovskites (ABO3), sillenite (A12BO20), or delafossite (ABO2) groups, hitherto written off due to limited or no photoelectrochemicalactivity.

Composite tin and zinc oxide nanocrystalline particles for enhanced charge separation in sensitized degradation of dyes.

PubMed

Bandara, J; Tennakone, K; Jayatilaka, P P B

2002-10-01

Composite ZnO/SnO2 catalyst has been studied for the sensitized degradation of dyes e.g. Eosin Y (2', 4', 5', 7'-tetrabromofluorescein disodium salt) in relation to efficient charge separation properties of the catalyst. Improved photocatalytic activity was observed in the case of ZnO/SnO2 composite catalyst compared to the catalytic activity of ZnO, SnO2 or TiO2 powder. The suppression of charge recombination in the composite ZnO/SnO2 catalyst led to higher catalytic activity for the degradation of Eosin Y. Degradation of Eosin follows concomitant formation of CO2 and formation of CO2 followed a pseudo-first-order rate. Photoelectrochemical cells constructed using SnO2, ZnO, ZnO/SnO2 sensitized with Eosin Y showed V(oc) of 175, 306, 512 mV/cm2 and I(sc) of 50, 70, 200 microA/cm2 respectively. A higher irreversible degradation of Eosin Y and higher V(oc) observed on composite ZnO/SnO2 than ZnO and SnO2 separately can be considered as a proof of enhanced charge separation of ZnO/SnO2 catalyst. Eosin Y showed a higher emission decreases on ZnO/SnO2 composite than on individual ZnO, SnO2 or TiO2 indicating dominance of the charge injection process. Photoinjected electrons are tunneled from ZnO to SnO2 particles accumulating injected electrons in the conduction bands allowing wider separation of excited carriers.

Isotope separation by selective charge conversion and field deflection

DOEpatents

Hickman, Robert G.

1978-01-01

A deuterium-tritium separation system wherein a source beam comprised of positively ionized deuterium (D.sup.+) and tritium (T.sup.+) is converted at different charge-exchange cell sections of the system to negatively ionized deuterium (D.sup.-) and tritium (T.sup.-). First, energy is added to the beam to accelerate the D.sup.+ ions to the velocity that is optimum for conversion of the D.sup.+ ions to D.sup.- ions in a charge-exchange cell. The T.sup.+ ions are accelerated at the same time, but not to the optimum velocity since they are heavier than the D.sup.+ ions. The T.sup.+ ions are, therefore, not converted to T.sup.- ions when the D.sup.+ ions are converted to D.sup.- ions. This enables effective separation of the beam by deflection of the isotopes with an electrostatic field, the D.sup.- ions being deflected in one direction and the T.sup.+ ions being deflected in the opposite direction. Next, more energy is added to the deflected beam of T.sup.+ ions to bring the T.sup.+ ions to the optimum velocity for their conversion to T.sup.- ions. In a particular use of the invention, the beams of D.sup.- and T.sup.- ions are separately further accelerated and then converted to energetic neutral particles for injection as fuel into a thermonuclear reactor. The reactor exhaust of D.sup.+ and T.sup.+ and the D.sup.+ and T.sup.+ that was not converted in the respective sections is combined with the source beam and recycled through the system to increase the efficiency of the system.

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

Schneider, T

Purpose: Since 2008 the Physikalisch-Technische Bundesanstalt (PTB) has been offering the calibration of {sup 125}I-brachytherapy sources in terms of the reference air-kerma rate (RAKR). The primary standard is a large air-filled parallel-plate extrapolation chamber. The measurement principle is based on the fact that the air-kerma rate is proportional to the increment of ionization per increment of chamber volume at chamber depths greater than the range of secondary electrons originating from the electrode x{sub 0}. Methods: Two methods for deriving the RAKR from the measured ionization charges are: (1) to determine the RAKR from the slope of the linear fit tomore » the so-called ’extrapolation curve’, the measured ionization charges Q vs. plate separations x or (2) to differentiate Q(x) and to derive the RAKR by a linear extrapolation towards zero plate separation. For both methods, correcting the measured data for all known influencing effects before the evaluation method is applied is a precondition. However, the discrepancy of their results is larger than the uncertainty given for the determination of the RAKR with both methods. Results: A new approach to derive the RAKR from the measurements is investigated as an alternative. The method was developed from the ground up, based on radiation transport theory. A conversion factor C(x{sub 1}, x{sub 2}) is applied to the difference of charges measured at the two plate separations x{sub 1} and x{sub 2}. This factor is composed of quotients of three air-kerma values calculated for different plate separations in the chamber: the air kerma Ka(0) for plate separation zero, and the mean air kermas at the plate separations x{sub 1} and x{sub 2}, respectively. The RAKR determined with method (1) yields 4.877 µGy/h, and with method (2) 4.596 µGy/h. The application of the alternative approach results in 4.810 µGy/h. Conclusion: The alternative method shall be established in the future.« less

First Observation of a Hall Effect in a Dusty Plasma: A Charged Granular Flow with Relevance to Planetary Rings

NASA Astrophysics Data System (ADS)

Eiskowitz, Skylar; Ballew, Nolan; Rojas, Rubén; Lathrop, Daniel

2017-11-01

The particles in Saturn's rings exhibit complex dynamic behavior. They experience solar radiation pressure, electromagnetic forces, and granular collisions. To investigate the possibility of the Hall Effect in the dusty plasma that comprise Saturn's rings, we have built an experiment that demonstrates the Hall Effect in granular matter. We focus on the Hall Effect because the rings' grains become collisionally charged and experience Saturn's dipolar magnetic field and Lorentz forces as they orbit. The experimental setup includes a closed ring-like track where granular matter is forced to circulate driven by compressed air. The structure sits between two electromagnets so that a portion of the track experiences up to a 0.2 T magnetic field. We vary the strength of the field and the speed of the particles. We report the voltage differences between two conducting plates on opposite sides of the track. If Saturn's rings do experience the Hall Effect, the inside and outside of the rings will develop a charge separation that can lead to a radial electric field and various phenomena including orbital effects due to the additional electric forces. Observational evidence from Cassini suggests that Saturn's rings exhibit lighting, supporting the notion that they are electrically charged. TREND REU program sponsored by the National Science Foundation.

Large silver-cadmium technology program

NASA Technical Reports Server (NTRS)

Charlip, S.; Lerner, S.

1971-01-01

The effects of varying cell design on operation factors on the electrochemical performance of sealed, silver-cadmium cells were determined. A factorial experiment was conducted for all test cells constructed with organic separators. Three operating factors were evaluated: temperature, depth of discharge, and charge rate. The six construction factors considered were separator, absorber, electrolyte quantity, cadmium electrode type, cadmium-to-silver ratio, and auxiliary electrode. Test cells of 4 ampere-hour capacity were fabricated and cycled. The best performing cells, on a 94 minute orbit, at 40% depth of discharge, were those containing silver-treated fibrous sausage casings as the separator, and Teflon-ated, pressed cadmium electrodes. Cycling data of cells with inorganic separators (Astroset) are given. Best performance was shown by cells with nonwoven nylon absorbers. Rigid inorganic separators provided the best barrier to silver migration.

Charge separation at disordered semiconductor heterojunctions from random walk numerical simulations.

PubMed

Mandujano-Ramírez, Humberto J; González-Vázquez, José P; Oskam, Gerko; Dittrich, Thomas; Garcia-Belmonte, Germa; Mora-Seró, Iván; Bisquert, Juan; Anta, Juan A

2014-03-07

Many recent advances in novel solar cell technologies are based on charge separation in disordered semiconductor heterojunctions. In this work we use the Random Walk Numerical Simulation (RWNS) method to model the dynamics of electrons and holes in two disordered semiconductors in contact. Miller-Abrahams hopping rates and a tunnelling distance-dependent electron-hole annihilation mechanism are used to model transport and recombination, respectively. To test the validity of the model, three numerical "experiments" have been devised: (1) in the absence of constant illumination, charge separation has been quantified by computing surface photovoltage (SPV) transients. (2) By applying a continuous generation of electron-hole pairs, the model can be used to simulate a solar cell under steady-state conditions. This has been exploited to calculate open-circuit voltages and recombination currents for an archetypical bulk heterojunction solar cell (BHJ). (3) The calculations have been extended to nanostructured solar cells with inorganic sensitizers to study, specifically, non-ideality in the recombination rate. The RWNS model in combination with exponential disorder and an activated tunnelling mechanism for transport and recombination is shown to reproduce correctly charge separation parameters in these three "experiments". This provides a theoretical basis to study relevant features of novel solar cell technologies.

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)

Agarose gel electrophoresis for the separation of DNA fragments.

PubMed

Lee, Pei Yun; Costumbrado, John; Hsu, Chih-Yuan; Kim, Yong Hoon

2012-04-20

Agarose gel electrophoresis is the most effective way of separating DNA fragments of varying sizes ranging from 100 bp to 25 kb(1). Agarose is isolated from the seaweed genera Gelidium and Gracilaria, and consists of repeated agarobiose (L- and D-galactose) subunits(2). During gelation, agarose polymers associate non-covalently and form a network of bundles whose pore sizes determine a gel's molecular sieving properties. The use of agarose gel electrophoresis revolutionized the separation of DNA. Prior to the adoption of agarose gels, DNA was primarily separated using sucrose density gradient centrifugation, which only provided an approximation of size. To separate DNA using agarose gel electrophoresis, the DNA is loaded into pre-cast wells in the gel and a current applied. The phosphate backbone of the DNA (and RNA) molecule is negatively charged, therefore when placed in an electric field, DNA fragments will migrate to the positively charged anode. Because DNA has a uniform mass/charge ratio, DNA molecules are separated by size within an agarose gel in a pattern such that the distance traveled is inversely proportional to the log of its molecular weight(3). The leading model for DNA movement through an agarose gel is "biased reptation", whereby the leading edge moves forward and pulls the rest of the molecule along(4). The rate of migration of a DNA molecule through a gel is determined by the following: 1) size of DNA molecule; 2) agarose concentration; 3) DNA conformation(5); 4) voltage applied, 5) presence of ethidium bromide, 6) type of agarose and 7) electrophoresis buffer. After separation, the DNA molecules can be visualized under uv light after staining with an appropriate dye. By following this protocol, students should be able to: Understand the mechanism by which DNA fragments are separated within a gel matrix Understand how conformation of the DNA molecule will determine its mobility through a gel matrix Identify an agarose solution of appropriate concentration for their needs Prepare an agarose gel for electrophoresis of DNA samples Set up the gel electrophoresis apparatus and power supply Select an appropriate voltage for the separation of DNA fragments Understand the mechanism by which ethidium bromide allows for the visualization of DNA bands Determine the sizes of separated DNA fragments.

Zeta potential control for electrophoresis cells

NASA Technical Reports Server (NTRS)

Fogal, G. L.

1973-01-01

Zeta potential arises from fact that ions tend to be adsorbed on surface of cell walls. This potential interfaces with electric field sensed by migrating particles and degrades resolution of separation. By regulating sign and magnitude of applied potential induced charge can be used to increase or decrease effective wall zeta potential.

Chiral separation of β-blockers by MEEKC using neutral microemulsion: Analysis of separation mechanism and further elucidation of resolution equation.

PubMed

Hu, Shao-Qiang; Lü, Wen-Juan; Ma, Yan-Hua; Hu, Qin; Dong, Li-Jun; Chen, Xing-Guo

2013-01-01

Based on the investigation of the effect of microemulsion charge on the chiral separation, a new chiral separation method with MEEKC employing neutral microemulsion was established. The method used a microemulsion containing 3.0% (w/v) neutral surfactant Tween 20 and 0.8% (w/v, 30 mM) dibutyl l-tartrate in 40 mM sodium tetraborate buffer to separate the enantiomers of β-blockers. The effect of major parameters on the chiral separation was investigated. The applied voltage had little effect on the resolution, but the chiral separation could be improved by suppressing the EOF. Nine racemic β-blockers obtained relatively good enantioseparation after appropriate concentrations of tetradecyl trimethyl ammonium bromide were added into the microemulsion to suppress the EOF. These results were explained based on the analysis of the separation mechanism of the method and deduced separation equations. The resolution equation of the method was further elucidated. It was found that the fourth term in the resolution equation, an additional term compared to the conventional resolution equation for column chromatography, represents the ratio of the relative movement distance between the analyte and microemulsion droplets relative to the effective capillary length. It can be regarded as a correction for the effective capillary length. These findings are significant for the development of the theory of MEEKC and the development of new chiral MEEKC method. © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

Stevens, Mark J.; Saleh, Omar A.

We calculated the force-extension curves for a flexible polyelectrolyte chain with varying charge separations by performing Monte Carlo simulations of a 5000 bead chain using a screened Coulomb interaction. At all charge separations, the force-extension curves exhibit a Pincus-like scaling regime at intermediate forces and a logarithmic regime at large forces. As the charge separation increases, the Pincus regime shifts to a larger range of forces and the logarithmic regime starts are larger forces. We also found that force-extension curve for the corresponding neutral chain has a logarithmic regime. Decreasing the diameter of bead in the neutral chain simulations removedmore » the logarithmic regime, and the force-extension curve tends to the freely jointed chain limit. In conclusion, this result shows that only excluded volume is required for the high force logarithmic regime to occur.« less

Separations by supported liquid membrane cascades

DOEpatents

Danesi, P.R.

1983-09-01

The invention describes a new separation technique which leads to multi-stage operations by the use of a series (a cascade) of alternated carrier-containing supported-liquid cation exchanger extractant and a liquid anion exchanger extractant (or a neutral extractant) as carrier. The membranes are spaced between alternated aqueous electrolytic solutions of different composition which alternatively provide positively charged extractable species and negatively charged (or zero charged) extractable species, of the chemical species to be separated. The alternated aqueous electrolytic solutions in addition to providing the driving force to the process, simultaneously function as a stripping solution from one type of membrane and as an extraction-promoting solution for the other type of membrane. The aqueous electrolytic solution and the supported liquid membranes are arranged to provide a continuous process.

Electrostatic attraction between overall neutral surfaces.

PubMed

Adar, Ram M; Andelman, David; Diamant, Haim

2016-08-01

Two overall neutral surfaces with positively and negatively charged domains ("patches") have been shown in recent experiments to exhibit long-range attraction when immersed in an ionic solution. Motivated by the experiments, we calculate analytically the osmotic pressure between such surfaces within the Poisson-Boltzmann framework, using a variational principle for the surface-averaged free energy. The electrostatic potential, calculated beyond the linear Debye-Hückel theory, yields an overall attraction at large intersurface separations, over a wide range of the system's controlled length scales. In particular, the attraction is stronger and occurs at smaller separations for surface patches of larger size and charge density. In this large patch limit, we find that the attraction-repulsion crossover separation is inversely proportional to the square of the patch-charge density and to the Debye screening length.

Separator for lithium-sulfur battery based on polymer blend membrane

NASA Astrophysics Data System (ADS)

Freitag, Anne; Stamm, Manfred; Ionov, Leonid

2017-09-01

In this work we report a novel way of reducing the polysulfide shuttle in lithium-sulfur batteries by a new separator material. Polyvinylsulfate potassium salt (PVSK) as polymeric additive is introduced into a polyvinylidene fluoride-hexafluoropropylene (PVdF-HFP) matrix membrane to improve the battery performance. PVSK is expected to lower the polysulfide mobility due to interaction with the sulfonic group. PVdF-HFP/PVSK blend membranes are prepared and an UV/Vis polysulfide diffusion test clearly demonstrates the positive effect of PVSK. Electrochemical testing reveals a significant improvement of cycling stability up to more than 200 cycles. In addition, the effect of separator porosity to the polysulfide shuttle is investigated with PVdF-HFP membranes of different porosity. A simple polysulfide diffusion test and potentiostatic charge/discharge cycling clearly demonstrate that low separator porosity is favorable in a lithium-sulfur cell.

Enhanced Photocarrier Separation in Hierarchical Graphitic-C3N4-Supported CuInS2 for Noble-Metal-Free Z-Scheme Photocatalytic Water Splitting.

PubMed

Li, Xiaoxue; Xie, Keyu; Song, Long; Zhao, Mengjia; Zhang, Zhipan

2017-07-26

The effective separation of photogenerated electrons and holes in photocatalysts is a prerequisite for efficient photocatalytic water splitting. CuInS 2 (CIS) is a widely used light absorber that works properly in photovoltaics but only shows limited performance in solar-driven hydrogen evolution due to its intrinsically severe charge recombination. Here, we prepare hierarchical graphitic C 3 N 4 -supported CuInS 2 (denoted as GsC) by an in situ growth of CIS directly on exfoliated thin graphitic C 3 N 4 nanosheets (g-C 3 N 4 NS) and demonstrate efficient separation of photoinduced charge carriers in the GsC by forming the Z-scheme system for the first time in CIS-catalyzed water splitting. Under visible light illumination, the GsC features an enhanced hydrogen evolution rate up to 1290 μmol g -1 h -1 , which is 3.3 and 6.1 times higher than that of g-C 3 N 4 NS and bare-CIS, respectively, thus setting a new performance benchmark for CIS-based water-splitting photocatalysts.

A Nonmetal Plasmonic Z-Scheme Photocatalyst with UV- to NIR-Driven Photocatalytic Protons Reduction.

PubMed

Zhang, Zhenyi; Huang, Jindou; Fang, Yurui; Zhang, Mingyi; Liu, Kuichao; Dong, Bin

2017-05-01

Ultrabroad-spectrum absorption and highly efficient generation of available charge carriers are two essential requirements for promising semiconductor-based photocatalysts, towards achieving the ultimate goal of solar-to-fuel conversion. Here, a fascinating nonmetal plasmonic Z-scheme photocatalyst with the W 18 O 49 /g-C 3 N 4 heterostructure is reported, which can effectively harvest photon energies spanning from the UV to the nearinfrared region and simultaneously possesses improved charge-carrier dynamics to boost the generation of long-lived active electrons for the photocatalytic reduction of protons into H 2 . By combining with theoretical simulations, a unique synergistic photocatalysis effect between the semiconductive Z-scheme charge-carrier separation and metal-like localized-surface-plasmon-resonance-induced "hot electrons" injection process is demonstrated within this binary heterostructure. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Influence of Coulomb interaction of tunable shapes on the collective transport of ultradilute two-dimensional holes.

PubMed

Huang, Jian; Pfeiffer, L N; West, K W

2014-01-24

In high quality updoped GaAs field-effect transistors, the two-dimensional charge carrier concentrations can be tuned to very low values similar to the density of electrons on helium surfaces. An important interaction effect, screening of the Coulomb interaction by the gate, rises as a result of the large charge spacing comparable to the distance between the channel and the gate. Based on the results of the temperature (T) dependence of the resistivity from measuring four different samples, a power-law characteristic is found for charge densities ≤2×10(9)  cm(-2). Moreover, the exponent exhibits a universal dependence on a single dimensionless parameter, the ratio between the mean carrier separation and the distance to the metallic gate that screens the Coulomb interaction. Thus, the electronic properties are tuned through varying the shape of the interaction potential.

Effects of Coulomb Repulsion on the Phase Diagram of the Asakura-Oosawa Model

NASA Astrophysics Data System (ADS)

Haaga, Jason; Pemberton, Elizabeth; Gunton, James; Rickman, Jeffrey

We investigate the effect of adding a screened Coulomb charge to a model colloidal system interacting via the Asakura-Oosawa depletion potential. This model has previously been used to study the early stages of amelogenin self-assembly, a crucial process in the formation of dental enamel, by Li et al (BiophysicalJournal 101, 2502 (2011). By employing Monte Carlo simulations, we explore the role of interaction strengths and ranges on phase behavior. We find that charge strength and range have a strong influence on the stable, in the case of long range depletion potential, or metastable, in the case of short range depletion, fluid-fluid phase separation. Coulomb repulsion narrows and flattens the coexistence curve with increasing charge. This talk will also discuss solid-solid transitions present for certain interaction ranges. This work is supported by the G. Harold and Leila Y. Mathers Foundation.

Interaction between like-charged polyelectrolyte-colloid complexes in electrolyte solutions: a Monte Carlo simulation study in the Debye-Hückel approximation.

PubMed

Truzzolillo, D; Bordi, F; Sciortino, F; Sennato, S

2010-07-14

We study the effective interaction between differently charged polyelectrolyte-colloid complexes in electrolyte solutions via Monte Carlo simulations. These complexes are formed when short and flexible polyelectrolyte chains adsorb onto oppositely charged colloidal spheres, dispersed in an electrolyte solution. In our simulations the bending energy between adjacent monomers is small compared to the electrostatic energy, and the chains, once adsorbed, do not exchange with the solution, although they rearrange on the particles surface to accommodate further adsorbing chains or due to the electrostatic interaction with neighbor complexes. Rather unexpectedly, when two interacting particles approach each other, the rearrangement of the surface charge distribution invariably produces antiparallel dipolar doublets that invert their orientation at the isoelectric point. These findings clearly rule out a contribution of dipole-dipole interactions to the observed attractive interaction between the complexes, pointing out that such suspensions cannot be considered dipolar fluids. On varying the ionic strength of the electrolyte, we find that a screening length kappa(-1), short compared with the size of the colloidal particles, is required in order to observe the attraction between like-charged complexes due to the nonuniform distribution of the electric charge on their surface ("patch attraction"). On the other hand, by changing the polyelectrolyte/particle charge ratio xi(s), the interaction between like-charged polyelectrolyte-decorated particles, at short separations, evolves from purely repulsive to strongly attractive. Hence, the effective interaction between the complexes is characterized by a potential barrier, whose height depends on the net charge and on the nonuniformity of their surface charge distribution.

Fractional charge and emergent mass hierarchy in diagonal two-leg t – J cylinders

DOE PAGES

Jiang, Yi-Fan; Jiang, Hong-Chen; Yao, Hong; ...

2017-06-06

Here, we define a class of “diagonal” tmore » $-$ J ladders rotated by π / 4 relative to the canonical lattice directions of the square lattice, and study it using density matrix renormalization group. Here, we focus on the two-leg cylinder with a doped hole concentration near x = $$\\frac{1}{4}$$ . At exactly x = $$\\frac{1}{4}$$, the system forms a period 4 charge density wave and exhibits spin-charge separation. Slightly away from $$\\frac{1}{4}$$ doping, we observe several topologically distinct types of solitons with well-defined fractionalized quantum numbers. Remarkably, given the absence of any obvious small parameter, the effective masses of the emergent solitons differ by several orders of magnitude.« less

A solution-processed binary cathode interfacial layer facilitates electron extraction for inverted polymer solar cells.

PubMed

Zhang, Xinyuan; Li, Zhiqi; Liu, Chunyu; Guo, Jiaxin; Shen, Liang; Guo, Wenbin

2018-03-15

The charge transfer and separation are significantly affected by the electron properties of the interface between the electron-donor layer and the carrier-transporting layer in polymer solar cells (PSCs). In this study, we investigate the electron extraction mechanism of PSCs with a low temperature solution-processed ZnO/PEI as electron transport layer. The incorporation of PEI layer can decrease the work function of ZnO and reduce interfacial barrier, which facilitates electron extraction and suppresses bimolecular recombination, leading to a significant performance enhancement. Furthermore, PEI layer can induce phase separation and passivite inorganic surface trap states as well as shift the interfacial energy offset between metal oxide and organic materials. This work offers a simple and effective way to improve the charge transporting property of organic photovoltaic devices. Copyright © 2017 Elsevier Inc. All rights reserved.

Three-dimensional thin film for lithium-ion batteries and supercapacitors.

PubMed

Yang, Yang; Peng, Zhiwei; Wang, Gunuk; Ruan, Gedeng; Fan, Xiujun; Li, Lei; Fei, Huilong; Hauge, Robert H; Tour, James M

2014-07-22

Three-dimensional heterogeneously nanostructured thin-film electrodes were fabricated by using Ta2O5 nanotubes as a framework to support carbon-onion-coated Fe2O3 nanoparticles along the surface of the nanotubes. Carbon onion layers function as microelectrodes to separate the two different metal oxides and form a nanoscale 3-D sandwich structure. In this way, space-charge layers were formed at the phase boundaries, and it provides additional energy storage by charge separation. These 3-D nanostructured thin films deliver both excellent Li-ion battery properties (stabilized at 800 mAh cm(–3)) and supercapacitor (up to 18.2 mF cm(–2)) performance owing to the synergistic effects of the heterogeneous structure. Thus, Li-ion batteries and supercapacitors are successfully assembled into the same electrode, which is promising for next generation hybrid energy storage and delivery devices.

Energy Conversion Mechanism for Electron Perpendicular Energy in High Guide-Field Reconnection

NASA Astrophysics Data System (ADS)

Guo, Xuehan; Horiuchi, Ritoku; Kaminou, Yasuhiro; Cheng, Frank; Ono, Yasushi

2016-10-01

The energy conversion mechanism for electron perpendicular energy, both the thermal and the kinetic energy, is investigated by means of two-dimensional, full-particle simulations in an open system. It is shown that electron perpendicular heating is mainly due to the breaking of magnetic moment conservation in separatrix region because the charge separation generates intense variation of electric field within the electron Larmor radius. Meanwhile, electron perpendicular acceleration takes place manly due to the polarization drift term as well as the curvature drift term of E . u⊥ in the downstream near the X-point. The enhanced electric field due to the charge separation there results in a significant effect of the polarization drift term on the dissipation of magnetic energy within the ion inertia length in the downstream. Japan Society for the Promotion of Science (JSPS) Fellows 15J03758.

Effective Tuning of Ketocyanine Derivatives through Acceptor Substitution.

PubMed

Poe, Ambata; Della Pelle, Andrea; Byrnes, Sean; Thayumanavan, S

2015-05-18

A series of ketocyanine derivatives possessing bis(diarylamino)fluorenyl donors and variable acceptors installed at the bridging carbon atom were synthesized to investigate how the electronic structure of the dye can be systemically tuned through stabilization of the cyanine-like character of the donor by increasing the acceptor strength. Analysis of the (1) H NMR spectra indicates that the "charge-separated" species dominates in these dyes, given that carbons possessing a positive or negative charge in the resonance structures of this state purposefully shift downfield or upfield, respectively, depending on the strength of the acceptor moiety. In DAA-Fl-PI, the acceptor strength and the gain of acceptor aromaticity indicates a predisposition of the separated state, indicated by asymmetry in the (1) H NMR spectrum, as well as uneven distribution of the HOMO on the fluorenyl donor. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

ELECTROSTATIC SURFACE STRUCTURES OF COAL AND MINERAL PARTICLES

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

NONE

It is the purpose of this research to study electrostatic charging mechanisms related to electrostatic beneficiation of coal with the goal of improving models of separation and the design of electrostatic separators. Areas addressed in this technical progress report are (a) electrostatic beneficiation of Pittsburgh #8 coal powders as a function of grind size and processing atmosphere; (b) the use of fluorescent micro-spheres to probe the charge distribution on the surfaces of coal particles; (c) the use of electrostatic beneficiation to recover unburned carbon from flyash; (d) the development of research instruments for investigation of charging properties of coal. Pittsburghmore » #8 powders were beneficiated as a function of grind size and under three atmosphere conditions: fresh ground in air , after 24 hours of air exposure, or under N2 atmosphere. The feed and processed powders were analyzed by a variety of methods including moisture, ash, total sulfur, and pyritic sulfur content. Mass distribution and cumulative charge of the processed powders were also measured. Fresh ground coal performed the best in electrostatic beneficiation. Results are compared with those of similar studies conducted on Pittsburgh #8 powders last year (April 1, 1997 to September 30, 1997). Polystyrene latex spheres were charged and deposited onto coal particles that had been passed through the electrostatic separator and collected onto insulating filters. The observations suggest bipolar charging of individual particles and patches of charge on the particles which may be associated with particular maceral types or with mineral inclusions. A preliminary investigation was performed on eletrostatic separation of unburned carbon particles from flyash. Approximately 25% of the flyash acquired positive charge in the copper tribocharger. This compares with 75% of fresh ground coal. The negatively charged material had a slightly reduced ash content suggesting some enrichment of carbonaceous material. There was also evidence that the carbon is present at a higher ratio in larger particles than in small particles. An ultraviolet photoelectron counter for use in ambient atmosphere is nearing completion. The counter will be used to measure work functions of different maceral and mineral types in the coal matrix. A Particle Image Analyzer for measuring size and charge of airborne particles is also under contruction and its current status is presented. A charged, monodisperse, droplet generator is also being constructed for calibration of the Particle Image Analyzer and other airborne particle analyzers in our labs.« less

Enhancing the Efficiency of Silicon-Based Solar Cells by the Piezo-Phototronic Effect.

PubMed

Zhu, Laipan; Wang, Longfei; Pan, Caofeng; Chen, Libo; Xue, Fei; Chen, Baodong; Yang, Leijing; Su, Li; Wang, Zhong Lin

2017-02-28

Although there are numerous approaches for fabricating solar cells, the silicon-based photovoltaics are still the most widely used in industry and around the world. A small increase in the efficiency of silicon-based solar cells has a huge economic impact and practical importance. We fabricate a silicon-based nanoheterostructure (p + -Si/p-Si/n + -Si (and n-Si)/n-ZnO nanowire (NW) array) photovoltaic device and demonstrate the enhanced device performance through significantly enhanced light absorption by NW array and effective charge carrier separation by the piezo-phototronic effect. The strain-induced piezoelectric polarization charges created at n-doped Si-ZnO interfaces can effectively modulate the corresponding band structure and electron gas trapped in the n + -Si/n-ZnO NW nanoheterostructure and thus enhance the transport process of local charge carriers. The efficiency of the solar cell was improved from 8.97% to 9.51% by simply applying a static compress strain. This study indicates that the piezo-phototronic effect can enhance the performance of a large-scale silicon-based solar cell, with great potential for industrial applications.

Blue Thermally Activated Delayed Fluorescence Polymers with Nonconjugated Backbone and Through-Space Charge Transfer Effect.

PubMed

Shao, Shiyang; Hu, Jun; Wang, Xingdong; Wang, Lixiang; Jing, Xiabin; Wang, Fosong

2017-12-13

We demonstrate novel molecular design for thermally activated delayed fluorescence (TADF) polymers based on a nonconjugated polyethylene backbone with through-space charge transfer effect between pendant electron donor (D) and acceptor (A) units. Different from conventional conjugated D-A polymers with through-bond charge transfer effect, the nonconjugated architecture avoids direct conjugation between D and A units, enabling blue emission. Meanwhile, spatial π-π interaction between the physically separated D and A units results in both small singlet-triplet energy splitting (0.019 eV) and high photoluminescence quantum yield (up to 60% in film state). The resulting polymer with 5 mol % acceptor unit gives efficient blue electroluminescence with Commission Internationale de l'Eclairage coordinates of (0.176, 0.269), together with a high external quantum efficiency of 12.1% and low efficiency roll-off of 4.9% (at 1000 cd m -2 ), which represents the first example of blue TADF nonconjugated polymer.

The effect of charged groups on hydrophilic monolithic stationary phases on their chromatographic properties.

PubMed

Li, Haibin; Liu, Chusheng; Wang, Qiqin; Zhou, Haibo; Jiang, Zhengjin

2016-10-21

In order to investigate the effect of charged groups present in hydrophilic monolithic stationary phases on their chromatographic properties, three charged hydrophilic monomers, i.e. N,N-dimethyl-N-acryloyloxyethyl-N-(3-sulfopropyl)ammonium betaine (SPDA), [2-(acryloyloxy)ethyl]trimethylammonium chloride (AETA), and 3-sulfopropyl acrylate potassium salt (SPA) were co-polymerized with the crosslinker N,N'-methylenebisacrylamide (MBA), respectively. The physicochemical properties of the three resulting charged hydrophilic monolithic columns were evaluated using scanning electron microscopy, ζ-potential analysis and micro-HPLC. High column efficiency was obtained on the three monolithic columns at a linear velocity of 1mm/s using thiourea as test compound. Comparative characterization of the three charged HILIC phases was then carried out using a set of model compounds, including nucleobases, nucleosides, benzoic acid derivatives, phenols, β-blockers and small peptides. Depending on the combination of stationary phase/mobile phase/solute, both hydrophilic interaction and other potential secondary interactions, including electrostatic interaction, hydrogen-bonding interaction, molecular shape selectivity, could contribute to the over-all retention of the analytes. Because of the strong electrostatic interaction provided by the quaternary ammonium groups in the poly (AETA-co-MBA) monolith, this cationic HILIC monolith exhibited the strongest retention for benzoic acid derivatives and small peptides with distorted peak shapes and the weakest retention for basic β-blockers. The sulfonyl groups on the poly (SPA-co-MBA) hydrophilic monolith could provide strong electrostatic attraction and hydrogen bonding for positively charged analytes and hydrogen-donor/acceptor containing analytes, respectively. Therefore, basic drugs, nucleobases and nucleotides exhibited the strongest retention on this anionic monolith. Because of the weak but distinct cation exchange properties of the zwitterionic poly (SPDA-co-MBA) hydrophilic monolith, it exhibited the best separation for most test analytes (including phenols, β-blockers and small peptides) in terms of selectivity, peak shape and analysis time. The poly (AETA-co-MBA) hydrophilic monolithic column provides the best separation of nucleobases and nucleosides. These results could guide the selection and application of these charged HILIC monoliths in the future. Copyright © 2016 Elsevier B.V. All rights reserved.

Extension of the charge separated-state lifetime by supramolecular association of a tetrathiafulvalene electron donor to a zinc/gold bisporphyrin.

PubMed

Boixel, Julien; Fortage, Jérôme; Blart, Errol; Pellegrin, Yann; Hammarström, Leif; Becker, Hans-Christian; Odobel, Fabrice

2010-02-14

Supramolecular triads were prepared by self-assembly of 4'-pyridyl-2-tetrathiafulvalene axially bound on ZnP-spacer-AuP(+) dyads; the lifetime of the charge separated state ((+)TTF-ZnP-Spacer-AuP ) formed upon light excitation of the triad is greatly increased with respect to that found in the parent dyad.

Therapeutic Antibody Engineering To Improve Viscosity and Phase Separation Guided by Crystal Structure.

PubMed

Chow, Chi-Kin; Allan, Barrett W; Chai, Qing; Atwell, Shane; Lu, Jirong

2016-03-07

Antibodies at high concentrations often reveal unanticipated biophysical properties suboptimal for therapeutic development. The purpose of this work was to explore the use of point mutations based on crystal structure information to improve antibody physical properties such as viscosity and phase separation (LLPS) at high concentrations. An IgG4 monoclonal antibody (Mab4) that exhibited high viscosity and phase separation at high concentration was used as a model system. Guided by the crystal structure, four CDR point mutants were made to evaluate the role of hydrophobic and charge interactions on solution behavior. Surprisingly and unpredictably, two of the charge mutants, R33G and N35E, showed a reduction in viscosity and a lower propensity to form LLPS at high concentration compared to the wild-type (WT), while a third charge mutant S28K showed an increased propensity to form LLPS compared to the WT. A fourth mutant, F102H, had reduced hydrophobicity, but unchanged viscosity and phase separation behavior. We further evaluated the correlation of various biophysical measurements including second virial coefficient (A2), interaction parameter (kD), weight-average molecular weight (WAMW), and hydrodynamic diameters (DH), at relatively low protein concentration (4 to 15 mg/mL) to physical properties, such as viscosity and liquid-liquid phase separation (LLPS), at high concentration. Surprisingly, kD measured using dynamic light scattering (DLS) at low antibody concentration correlated better with viscosity and phase separation than did A2 for Mab4. Our results suggest that the high viscosity and phase separation observed at high concentration for Mab4 are mainly driven by charge and not hydrophobicity.

A FOUR-FLUID MHD MODEL OF THE SOLAR WIND/INTERSTELLAR MEDIUM INTERACTION WITH TURBULENCE TRANSPORT AND PICKUP PROTONS AS SEPARATE FLUID

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

Usmanov, Arcadi V.; Matthaeus, William H.; Goldstein, Melvyn L., E-mail: arcadi.usmanov@nasa.gov

2016-03-20

We have developed a four-fluid, three-dimensional magnetohydrodynamic model of the solar wind interaction with the local interstellar medium. The unique features of the model are: (a) a three-fluid description for the charged components of the solar wind and interstellar plasmas (thermal protons, electrons, and pickup protons), (b) the built-in turbulence transport equations based on Reynolds decomposition and coupled with the mean-flow Reynolds-averaged equations, and (c) a solar corona/solar wind model that supplies inner boundary conditions at 40 au by computing solar wind and magnetic field parameters outward from the coronal base. The three charged species are described by separate energy equationsmore » and are assumed to move with the same velocity. The fourth fluid in the model is the interstellar hydrogen which is treated by separate continuity, momentum, and energy equations and is coupled with the charged components through photoionization and charge exchange. We evaluate the effects of turbulence transport and pickup protons on the global heliospheric structure and compute the distribution of plasma, magnetic field, and turbulence parameters throughout the heliosphere for representative solar minimum and maximum conditions. We compare our results with Voyager 1 observations in the outer heliosheath and show that the relative amplitude of magnetic fluctuations just outside the heliopause is in close agreement with the value inferred from Voyager 1 measurements by Burlaga et al. The simulated profiles of magnetic field parameters in the outer heliosheath are in qualitative agreement with the Voyager 1 observations and with the analytical model of magnetic field draping around the heliopause of Isenberg et al.« less

Charge carrier concentration dependence of encounter-limited bimolecular recombination in phase-separated organic semiconductor blends

NASA Astrophysics Data System (ADS)

Heiber, Michael C.; Nguyen, Thuc-Quyen; Deibel, Carsten

2016-05-01

Understanding how the complex intermolecular configurations and nanostructure present in organic semiconductor donor-acceptor blends impacts charge carrier motion, interactions, and recombination behavior is a critical fundamental issue with a particularly major impact on organic photovoltaic applications. In this study, kinetic Monte Carlo (KMC) simulations are used to numerically quantify the complex bimolecular charge carrier recombination behavior in idealized phase-separated blends. Recent KMC simulations have identified how the encounter-limited bimolecular recombination rate in these blends deviates from the often used Langevin model and have been used to construct the new power mean mobility model. Here, we make a challenging but crucial expansion to this work by determining the charge carrier concentration dependence of the encounter-limited bimolecular recombination coefficient. In doing so, we find that an accurate treatment of the long-range electrostatic interactions between charge carriers is critical, and we further argue that many previous KMC simulation studies have used a Coulomb cutoff radius that is too small, which causes a significant overestimation of the recombination rate. To shed more light on this issue, we determine the minimum cutoff radius required to reach an accuracy of less than ±10 % as a function of the domain size and the charge carrier concentration and then use this knowledge to accurately quantify the charge carrier concentration dependence of the recombination rate. Using these rigorous methods, we finally show that the parameters of the power mean mobility model are determined by a newly identified dimensionless ratio of the domain size to the average charge carrier separation distance.

Theoretical study on the cooperative exciton dissociation process based on dimensional and hot charge-transfer state effects in an organic photocell

NASA Astrophysics Data System (ADS)

Shimazaki, Tomomi; Nakajima, Takahito

2016-06-01

This paper discusses the exciton dissociation process at the donor-acceptor interface in organic photocells. In our previous study, we introduced a local temperature to handle the hot charge-transfer (CT) state and calculated the exciton dissociation probability based on the 1D organic semiconductor model [T. Shimazaki and T. Nakajima, Phys. Chem. Chem. Phys. 17, 12538 (2015)]. Although the hot CT state plays an essential role in exciton dissociations, the probabilities calculated are not high enough to efficiently separate bound electron-hole pairs. This paper focuses on the dimensional (entropy) effect together with the hot CT state effect and shows that cooperative behavior between both effects can improve the exciton dissociation process. In addition, we discuss cooperative effects with site-disorders and external-electric-fields.

An experimental and modeling study of isothermal charge/discharge behavior of commercial Ni-MH cells

NASA Astrophysics Data System (ADS)

Pan, Y. H.; Srinivasan, V.; Wang, C. Y.

In this study, a previously developed nickel-metal hydride (Ni-MH) battery model is applied in conjunction with experimental characterization. Important geometric parameters, including the active surface area and micro-diffusion length for both electrodes, are measured and incorporated in the model. The kinetic parameters of the oxygen evolution reaction are also characterized using constant potential experiments. Two separate equilibrium equations for the Ni electrode, one for charge and the other for discharge, are determined to provide a better description of the electrode hysteresis effect, and their use results in better agreement of simulation results with experimental data on both charge and discharge. The Ni electrode kinetic parameters are re-calibrated for the battery studied. The Ni-MH cell model coupled with the updated electrochemical properties is then used to simulate a wide range of experimental discharge and charge curves with satisfactory agreement. The experimentally validated model is used to predict and compare various charge algorithms so as to provide guidelines for application-specific optimization.

Engineering and Probing Topological Properties of Dirac Semimetal Films by Asymmetric Charge Transfer.

PubMed

Villanova, John W; Barnes, Edwin; Park, Kyungwha

2017-02-08

Dirac semimetals (DSMs) have topologically robust three-dimensional Dirac (doubled Weyl) nodes with Fermi-arc states. In heterostructures involving DSMs, charge transfer occurs at the interfaces, which can be used to probe and control their bulk and surface topological properties through surface-bulk connectivity. Here we demonstrate that despite a band gap in DSM films, asymmetric charge transfer at the surface enables one to accurately identify locations of the Dirac-node projections from gapless band crossings and to examine and engineer properties of the topological Fermi-arc surface states connecting the projections, by simulating adatom-adsorbed DSM films using a first-principles method with an effective model. The positions of the Dirac-node projections are insensitive to charge transfer amount or slab thickness except for extremely thin films. By varying the amount of charge transfer, unique spin textures near the projections and a separation between the Fermi-arc states change, which can be observed by gating without adatoms.

Cascading electron and hole transfer dynamics in a CdS/CdTe core-shell sensitized with bromo-pyrogallol red (Br-PGR): slow charge recombination in type II regime.

PubMed

Maity, Partha; Debnath, Tushar; Chopra, Uday; Ghosh, Hirendra Nath

2015-02-14

Ultrafast cascading hole and electron transfer dynamics have been demonstrated in a CdS/CdTe type II core-shell sensitized with Br-PGR using transient absorption spectroscopy and the charge recombination dynamics have been compared with those of CdS/Br-PGR composite materials. Steady state optical absorption studies suggest that Br-PGR forms strong charge transfer (CT) complexes with both the CdS QD and CdS/CdTe core-shell. Hole transfer from the photo-excited QD and QD core-shell to Br-PGR was confirmed by both steady state and time-resolved emission spectroscopy. Charge separation was also confirmed by detecting electrons in the conduction band of the QD and the cation radical of Br-PGR as measured from femtosecond transient absorption spectroscopy. Charge separation in the CdS/Br-PGR composite materials was found to take place in three different pathways, by transferring the photo-excited hole of CdS to Br-PGR, electron injection from the photo-excited Br-PGR to the CdS QD, and direct electron transfer from the HOMO of Br-PGR to the conduction band of the CdS QD. However, in the CdS/CdTe/Br-PGR system hole transfer from the photo-excited CdS to Br-PGR and electron injection from the photo-excited Br-PGR to CdS take place after cascading through the CdTe shell QD. Charge separation also takes place via direct electron transfer from the Br-PGR HOMO to the conduction band of CdS/CdTe. Charge recombination (CR) dynamics between the electron in the conduction band of the CdS QD and the Br-PGR cation radical were determined by monitoring the bleach recovery kinetics. The CR dynamics were found to be much slower in the CdS/CdTe/Br-PGR system than in the CdS/Br-PGR system. The formation of the strong CT complex and the separation of charges cascading through the CdTe shell help to slow down charge recombination in the type II regime.

A computational approach to predicting ligand selectivity for the size-based separation of trivalent lanthanides

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

Ivanov, Alexander S.; Bryantsev, Vyacheslav S.

An accurate description of solvation effects for trivalent lanthanide ions is a main stumbling block to the qualitative prediction of selectivity trends along the lanthanide series. In this work, we propose a simple model to describe the differential effect of solvation in the competitive binding of a ligand by lanthanide ions by including weakly co-ordinated counterions in the complexes of more than a +1 charge. The success of the approach to quantitatively reproduce selectivities obtained from aqueous phase complexation studies demonstrates its potential for the design and screening of new ligands for efficient size-based separation.

A computational approach to predicting ligand selectivity for the size-based separation of trivalent lanthanides

DOE PAGES

Ivanov, Alexander S.; Bryantsev, Vyacheslav S.

2016-06-20

An accurate description of solvation effects for trivalent lanthanide ions is a main stumbling block to the qualitative prediction of selectivity trends along the lanthanide series. In this work, we propose a simple model to describe the differential effect of solvation in the competitive binding of a ligand by lanthanide ions by including weakly co-ordinated counterions in the complexes of more than a +1 charge. The success of the approach to quantitatively reproduce selectivities obtained from aqueous phase complexation studies demonstrates its potential for the design and screening of new ligands for efficient size-based separation.

Effects of exchanged cation and layer charge on the sorption of water and EGME vapors on montmorillonite clays

USGS Publications Warehouse

Chiou, Cary T.; Rutherford, David W.

1997-01-01

The effects of exchanged cation and layer charge on the sorption of water and ethylene glycol monoethyl ether (EGME) vapors on montmorillonite have been studied on SAz-1 and SWy-1 source clays, each exchanged respectively with Ca, Na, K, Cs and tetramethylammonium (TMA) cations. The corresponding lattice expansions were also determined, and the corresponding N2 adsorption data were provided for comparison. For clays exchanged with cations of low hydrating powers (such as K, Cs and TMA), water shows a notably lower uptake than does N2 at low relative pressures (P/P0). By contrast, EGME shows higher uptakes than N2 on all exchanged clays at all P/P0. The anomaly for water is attributed to its relatively low attraction for siloxane surfaces of montmorillonite because of its high cohesive energy density. In addition to solvating cations and expanding interlayers, water and EGME vapors condense into small clay pores and interlayer voids created by interlayer expansion. The initial (dry) interlayer separation varies more significantly with cation type than with layer charge; the water-saturated interlayer separation varies more with cation type than the EGME-saturated interlayer separation. Because of the differences in surface adsorption and interlayer expansion for water and EGME, no general correspondence is found between the isotherms of water and EGME on exchanged clays, nor is a simple relation observed between the overall uptake of either vapor and the cation solvating power. The excess interlayer capacities of water and of EGME that result from lattice expansion of the exchanged clays are estimated by correcting for amounts of vapor adsorption on planar clay surfaces and of vapor condensation into intrinsic clay pores. The resulting data follow more closely the relative solvating powers of the exchanged cations.

Double heterojunction nanowire photocatalysts for hydrogen generation.

PubMed

Tongying, P; Vietmeyer, F; Aleksiuk, D; Ferraudi, G J; Krylova, G; Kuno, M

2014-04-21

Charge separation and charge transfer across interfaces are key aspects in the design of efficient photocatalysts for solar energy conversion. In this study, we investigate the hydrogen generating capabilities and underlying photophysics of nanostructured photocatalysts based on CdSe nanowires (NWs). Systems studied include CdSe, CdSe/CdS core/shell nanowires and their Pt nanoparticle-decorated counterparts. Femtosecond transient differential absorption measurements reveal how semiconductor/semiconductor and metal/semiconductor heterojunctions affect the charge separation and hydrogen generation efficiencies of these hybrid photocatalysts. In turn, we unravel the role of surface passivation, charge separation at semiconductor interfaces and charge transfer to metal co-catalysts in determining photocatalytic H2 generation efficiencies. This allows us to rationalize why Pt nanoparticle decorated CdSe/CdS NWs, a double heterojunction system, performs best with H2 generation rates of ∼434.29 ± 27.40 μmol h(-1) g(-1) under UV/Visible irradiation. In particular, we conclude that the CdS shell of this double heterojunction system serves two purposes. The first is to passivate CdSe NW surface defects, leading to long-lived charges at the CdSe/CdS interface capable of carrying out reduction chemistries. Upon photoexcitation, we also find that CdS selectively injects charges into Pt NPs, enabling simultaneous reduction chemistries at the Pt NP/solvent interface. Pt nanoparticle decorated CdSe/CdS NWs thus enable reduction chemistries at not one, but rather two interfaces, taking advantage of each junction's optimal catalytic activities.

Revealing the Double-Edged Sword Role of Graphene on Boosted Charge Transfer versus Active Site Control in TiO2 Nanotube Arrays@RGO/MoS2 Heterostructure.

PubMed

Quan, Quan; Xie, Shunji; Weng, Bo; Wang, Ye; Xu, Yi-Jun

2018-05-01

Charge separation/transfer is generally believed to be the most key factor affecting the efficiency of photocatalysis, which however will be counteracted if not taking the active site engineering into account for a specific photoredox reaction. Here, a 3D heterostructure composite is designed consisting of MoS 2 nanoplatelets decorated on reduced graphene oxide-wrapped TiO 2 nanotube arrays (TNTAs@RGO/MoS 2 ). Such a cascade configuration renders a directional migration of charge carriers and controlled immobilization of active sites, thereby showing much higher photoactivity for water splitting to H 2 than binary TNTAs@RGO and TNTAs/MoS 2 . The photoactivity comparison and mechanistic analysis reveal the double-edged sword role of RGO on boosted charge separation/transfer versus active site control in this composite system. The as-observed inconsistency between boosted charge transfer and lowered photoactivity over TNTAs@RGO is attributed to the decrease of active sites for H 2 evolution, which is significantly different from the previous reports in literature. The findings of the intrinsic relationship of balanced benefits from charge separation/transfer and active site control could promote the rational optimization of photocatalyst design by cooperatively manipulating charge flow and active site control, thereby improving the efficiency of photocatalysis for target photoredox processes. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Pi-Pi contacts are an overlooked protein feature relevant to phase separation.

PubMed

Vernon, Robert McCoy; Chong, Paul Andrew; Tsang, Brian; Kim, Tae Hun; Bah, Alaji; Farber, Patrick; Lin, Hong; Forman-Kay, Julie Deborah

2018-02-09

Protein phase separation is implicated in formation of membraneless organelles, signaling puncta and the nuclear pore. Multivalent interactions of modular binding domains and their target motifs can drive phase separation. However, forces promoting the more common phase separation of intrinsically disordered regions are less understood, with suggested roles for multivalent cation-pi, pi-pi, and charge interactions and the hydrophobic effect. Known phase-separating proteins are enriched in pi-orbital containing residues and thus we analyzed pi-interactions in folded proteins. We found that pi-pi interactions involving non-aromatic groups are widespread, underestimated by force-fields used in structure calculations and correlated with solvation and lack of regular secondary structure, properties associated with disordered regions. We present a phase separation predictive algorithm based on pi interaction frequency, highlighting proteins involved in biomaterials and RNA processing. © 2018, Vernon et al.

Ionic Structure at Dielectric Interfaces

NASA Astrophysics Data System (ADS)

Jing, Yufei

The behavior of ions in liquids confined between macromolecules determines the outcome of many nanoscale assembly processes in synthetic and biological materials such as colloidal dispersions, emulsions, hydrogels, DNA, cell membranes, and proteins. Theoretically, the macromolecule-liquid boundary is often modeled as a dielectric interface and an important quantity of interest is the ionic structure in a liquid confined between two such interfaces. The knowledge gleaned from the study of ionic structure in such models can be useful in several industrial applications, such as biosensors, lithium-ion batteries double-layer supercapacitors for energy storage and seawater desalination. Electrostatics plays a critical role in the development of such functional materials. Many of the functions of these materials, result from charge and composition heterogeneities. There are great challenges in solving electrostatics problems in heterogeneous media with arbitrary shapes because electrostatic interactions remains unknown but depend on the particular density of charge distributions. Charged molecules in heterogeneous media affect the media's dielectric response and hence the interaction between the charges is unknown since it depends on the media and on the geometrical properties of the interfaces. To determine the properties of heterogeneous systems including crucial effects neglected in classical mean field models such as the hard core of the ions, the dielectric mismatch and interfaces with arbitrary shapes. The effect of hard core interactions accounts properly for short range interactions and the effect of local dielectric heterogeneities in the presence of ions and/or charged molecules for long-range interactions are both analyzed via an energy variational principle that enables to update charges and the medium's response in the same simulation time step. In particular, we compute the ionic structure in a model system of electrolyte confined by two planar dielectric interfaces using molecular dynamics(MD) simulations and compared it with liquid state theory result. We explore the effects of high electrolyte concentrations, multivalent ions, and dielectric contrasts on the ionic distributions. We observe the presence of non-monotonous ionic density profiles leading to structure deformation in the fluid which is attributed to the competition between electrostatic and steric (entropic) interactions. We find that thermal forces that arise from symmetry breaking at the interfaces can have a profound effect on the ionic structure and can oftentimes overwhelm the influence of dielectric discontinuity. The combined effect of ionic correlations and inhomogeneous dielectric permittivity significantly changes the character of effective interaction between two interfaces. We show that, in concentrated electrolytes with confinement, it is imperative to take into account the finite-size of the ions as well as proper description of electrostatic interactions in heterogeneous media, which is not fully fulfilled by Poisson-Boltzmann based approaches. The effect of electric field at interface between two immiscible electrolyte solutions is studied as well. The classical Poisson-Boltzmann theory has been widely used to describe the corresponding ionic distribution, even though it neglects the polarization and ion correlations typical of these charged systems. Using Monte Carlo simulations, we provide an enhanced description of an oil-water interface in the presence of an electric field without needing any adjustable parameter, including realistic ionic sizes, ion correlations, and image charges. Our data agree with experimental measurements of excess surface tension for a wide range of electrolyte concentrations of LiCl and TBATPB (tetrabutylammonium-tetraphenylborate), contrasting with the result of the classical non-linear Poisson-Boltzmann theory. More importantly, we show that the size-asymmetry between small Li+ and large Cl- ions can significantly increase the electric field near the liquid interface, or can even reverse it locally, at high salt concentrations in the aqueous phase. These observations suggest a novel trapping/release mechanism of charged nanoparticles at oil-water interfaces in the vicinity of the point of zero charge. In addition, we study the effects of size asymmetry and charge asymmetry on ion distribution at a dielectric interface using coarse-grained MD based on an energy variational principle. The goal is to explore charge amplification with exact consideration of surface polarization. We find that both size asymmetry and charge asymmetry lead to charge separation at the interfaces. In addition, charge separation is enhanced by interface polarization. We are currently extending the research to charged interfaces that has broad applications such as batteries and supercapacitors for energy storage.

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

NASA Astrophysics Data System (ADS)

Hendrickson, Heidi Phillips

A fundamental understanding of charge separation in organic materials is necessary for the rational design of optoelectronic devices suited for renewable energy applications and requires a combination of theoretical, computational, and experimental methods. Density functional theory (DFT) and time-dependent (TD)DFT are cost effective ab-initio approaches for calculating fundamental properties of large molecular systems, however conventional DFT methods have been known to fail in accurately characterizing frontier orbital gaps and charge transfer states in molecular systems. In this dissertation, these shortcomings are addressed by implementing an optimally-tuned range-separated hybrid (OT-RSH) functional approach within DFT and TDDFT. The first part of this thesis presents the way in which RSH-DFT addresses the shortcomings in conventional DFT. Environmentally-corrected RSH-DFT frontier orbital energies are shown to correspond to thin film measurements for a set of organic semiconducting molecules. Likewise, the improved RSH-TDDFT description of charge transfer excitations is benchmarked using a model ethene dimer and silsesquioxane molecules. In the second part of this thesis, RSH-DFT is applied to chromophore-functionalized silsesquioxanes, which are currently investigated as candidates for building blocks in optoelectronic applications. RSH-DFT provides insight into the nature of absorptive and emissive states in silsesquioxanes. While absorption primarily involves transitions localized on one chromophore, charge transfer between chromophores and between chromophore and silsesquioxane cage have been identified. The RSH-DFT approach, including a protocol accounting for complex environmental effects on charge transfer energies, was tested and validated against experimental measurements. The third part of this thesis addresses quantum transport through nano-scale junctions. The ability to quantify a molecular junction via spectroscopic methods is crucial to their technological design and development. Time dependent perturbation theory, employed by non-equilibrium Green's function formalism, is utilized to study the effect of quantum coherences on electron transport and the effect of symmetry breaking on the electronic spectra of model molecular junctions. The fourth part of this thesis presents the design of a physical chemistry course based on a pedagogical approach called Writing-to-Teach. The nature of inaccuracies expressed in student-generated explanations of quantum chemistry topics, and the ability of a peer review process to engage these inaccuracies, is explored within this context.

Versatile organic (fullerene)-inorganic (CdTe nanoparticle) nanoensembles.

PubMed

Guldi, Dirk M; Zilbermann, Israel; Anderson, Greg; Kotov, Nicholas A; Tagmatarchis, Nikos; Prato, Maurizio

2004-11-10

Novel organic (positively charged fullerene)-inorganic (negatively charged CdTe nanoparticle) nanoensembles were devised through electrostatic interactions and probed as versatile donor-acceptor hybrids. Photoirradiation of their homogeneous solutions, containing the electrostatically packed components, let to very long-lived (1.3 ms) charge separated states.

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

Electrostatic Separator for Beneficiation of Lunar Soil

NASA Technical Reports Server (NTRS)

Quinn, Jacqueline; Arens, Ellen; Trigwell, Steve; Captain, James

2010-01-01

A charge separator has been constructed for use in a lunar environment that will allow for separation of minerals from lunar soil. In the present experiments, whole lunar dust as received was used. The approach taken here was that beneficiation of ores into an industrial feedstock grade may be more efficient. Refinement or enrichment of specific minerals in the soil before it is chemically processed may be more desirable as it would reduce the size and energy requirements necessary to produce the virgin material, and it may significantly reduce the process complexity. The principle is that minerals of different composition and work function will charge differently when tribocharged against different materials, and hence be separated in an electric field.

Correlated scattering states of N-body Coulomb systems

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

Berakdar, J.

1997-03-01

For N charged particles of equal masses moving in the field of a heavy residual charge, an approximate analytical solution of the many-body time-independent Schr{umlt o}dinger equation is derived at a total energy above the complete fragmentation threshold. All continuum particles are treated on equal footing. The proposed correlated wave function represents, to leading order, an exact solution of the many-body Schr{umlt o}dinger equation in the asymptotic region defined by large interparticle separations. Thus, in this asymptotic region the N-body Coulomb modifications to the plane-wave motion of free particles are rigorously estimated. It is shown that the Kato cusp conditionsmore » are satisfied by the derived wave function at all two-body coalescence points. An expression of the normalization of this wave function is also given. To render possible the calculations of scattering amplitudes for transitions leading to a four-body scattering state, an effective-charge method is suggested in which the correlations between the continuum particles are completely subsumed into effective interactions with the residual charge. Analytical expressions for these effective interactions are derived and discussed for physical situations. {copyright} {ital 1997} {ital The American Physical Society}« less

Charged-pion cross sections and double-helicity asymmetries in polarized p + p collisions at √s = 200 GeV

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

Adare, A.; Aidala, C.; Ajitanand, N. N.

2015-02-02

We present midrapidity charged-pion invariant cross sections, the ratio of the π⁻ to π⁺ cross sections and the charge-separated double-spin asymmetries in polarized p+p collisions at √s = 200 GeV. While the cross section measurements are consistent within the errors of next-to-leadingorder (NLO) perturbative quantum chromodynamics predictions (pQCD), the same calculations over estimate the ratio of the charged-pion cross sections. This discrepancy arises from the cancellation of the substantial systematic errors associated with the NLO-pQCD predictions in the ratio and highlights the constraints these data will place on flavor dependent pion fragmentation functions. Thus, the charge-separated pion asymmetries presented heremore » sample an x range of ~0.03–0.16 and provide unique information on the sign of the gluon-helicity distribution.« less

Charged-pion cross sections and double-helicity asymmetries in polarized p +p collisions at √{s }=200 GeV

NASA Astrophysics Data System (ADS)

Adare, A.; Aidala, C.; Ajitanand, N. N.; Akiba, Y.; Akimoto, R.; Al-Ta'Ani, H.; Alexander, J.; Andrews, K. R.; Angerami, A.; Aoki, K.; Apadula, N.; Appelt, E.; Aramaki, Y.; Armendariz, R.; Aschenauer, E. C.; Atomssa, E. T.; Awes, T. C.; Azmoun, B.; Babintsev, V.; Bai, M.; Bannier, B.; Barish, K. N.; Bassalleck, B.; Basye, A. T.; Bathe, S.; Baublis, V.; Baumann, C.; Bazilevsky, A.; Belmont, R.; Ben-Benjamin, J.; Bennett, R.; Blau, D. S.; Bok, J. S.; Boyle, K.; Brooks, M. L.; Broxmeyer, D.; Buesching, H.; Bumazhnov, V.; Bunce, G.; Butsyk, S.; Campbell, S.; Castera, P.; Chen, C.-H.; Chi, C. Y.; Chiu, M.; Choi, I. J.; Choi, J. B.; Choudhury, R. K.; Christiansen, P.; Chujo, T.; Chvala, O.; Cianciolo, V.; Citron, Z.; Cole, B. A.; Conesa Del Valle, Z.; Connors, M.; Csanád, M.; Csörgő, T.; Dairaku, S.; Datta, A.; David, G.; Dayananda, M. K.; Denisov, A.; Deshpande, A.; Desmond, E. J.; Dharmawardane, K. V.; Dietzsch, O.; Dion, A.; Donadelli, M.; Drapier, O.; Drees, A.; Drees, K. A.; Durham, J. M.; Durum, A.; D'Orazio, L.; Efremenko, Y. V.; Engelmore, T.; Enokizono, A.; En'yo, H.; Esumi, S.; Fadem, B.; Fields, D. E.; Finger, M.; Finger, M.; Fleuret, F.; Fokin, S. L.; Frantz, J. E.; Franz, A.; Frawley, A. D.; Fukao, Y.; Fusayasu, T.; Gal, C.; Garishvili, I.; Giordano, F.; Glenn, A.; Gong, X.; Gonin, M.; Goto, Y.; Granier de Cassagnac, R.; Grau, N.; Greene, S. V.; Grosse Perdekamp, M.; Gunji, T.; Guo, L.; Gustafsson, H.-Å.; Haggerty, J. S.; Hahn, K. I.; Hamagaki, H.; Hamblen, J.; Han, R.; Hanks, J.; Harper, C.; Hashimoto, K.; Haslum, E.; Hayano, R.; He, X.; Hemmick, T. K.; Hester, T.; Hill, J. C.; Hollis, R. S.; Holzmann, W.; Homma, K.; Hong, B.; Horaguchi, T.; Hori, Y.; Hornback, D.; Huang, S.; Ichihara, T.; Ichimiya, R.; Iinuma, H.; Ikeda, Y.; Imai, K.; Inaba, M.; Iordanova, A.; Isenhower, D.; Ishihara, M.; Issah, M.; Ivanischev, D.; Iwanaga, Y.; Jacak, B. V.; Jia, J.; Jiang, X.; John, D.; Johnson, B. M.; Jones, T.; Joo, K. S.; Jouan, D.; Kamin, J.; Kaneti, S.; Kang, B. H.; Kang, J. H.; Kang, J. S.; Kapustinsky, J.; Karatsu, K.; Kasai, M.; Kawall, D.; Kazantsev, A. V.; Kempel, T.; Khanzadeev, A.; Kijima, K. M.; Kim, B. I.; Kim, D. J.; Kim, E.-J.; Kim, Y.-J.; Kim, Y. K.; Kinney, E.; Kiss, Á.; Kistenev, E.; Kleinjan, D.; Kline, P.; Kochenda, L.; Komkov, B.; Konno, M.; Koster, J.; Kotov, D.; Král, A.; Kunde, G. J.; Kurita, K.; Kurosawa, M.; Kwon, Y.; Kyle, G. S.; Lacey, R.; Lai, Y. S.; Lajoie, J. G.; Lebedev, A.; Lee, D. M.; Lee, J.; Lee, K. B.; Lee, K. S.; Lee, S. H.; Lee, S. R.; Leitch, M. J.; Leite, M. A. L.; Li, X.; Lim, S. H.; Linden Levy, L. A.; Liu, H.; Liu, M. X.; Love, B.; Lynch, D.; Maguire, C. F.; Makdisi, Y. I.; Manion, A.; Manko, V. I.; Mannel, E.; Mao, Y.; Masui, H.; McCumber, M.; McGaughey, P. L.; McGlinchey, D.; McKinney, C.; Means, N.; Mendoza, M.; Meredith, B.; Miake, Y.; Mibe, T.; Mignerey, A. C.; Miki, K.; Milov, A.; Mitchell, J. T.; Miyachi, Y.; Mohanty, A. K.; Moon, H. J.; Morino, Y.; Morreale, A.; Morrison, D. P.; Motschwiller, S.; Moukhanova, T. V.; Murakami, T.; Murata, J.; Nagamiya, S.; Nagle, J. L.; Naglis, M.; Nagy, M. I.; Nakagawa, I.; Nakamiya, Y.; Nakamura, K. R.; Nakamura, T.; Nakano, K.; Newby, J.; Nguyen, M.; Nihashi, M.; Nouicer, R.; Nyanin, A. S.; Oakley, C.; O'Brien, E.; Ogilvie, C. A.; Oka, M.; Okada, K.; Oskarsson, A.; Ouchida, M.; Ozawa, K.; Pak, R.; Pantuev, V.; Papavassiliou, V.; Park, B. H.; Park, I. H.; Park, S. K.; Pate, S. F.; Patel, L.; Pei, H.; Peng, J.-C.; Pereira, H.; Peressounko, D. Yu.; Petti, R.; Pinkenburg, C.; Pisani, R. P.; Proissl, M.; Purschke, M. L.; Qu, H.; Rak, J.; Ravinovich, I.; Read, K. F.; Reygers, K.; Riabov, V.; Riabov, Y.; Richardson, E.; Roach, D.; Roche, G.; Rolnick, S. D.; Rosati, M.; Rosendahl, S. S. E.; Rubin, J. G.; Sahlmueller, B.; Saito, N.; Sakaguchi, T.; Samsonov, V.; Sano, S.; Sarsour, M.; Sato, T.; Savastio, M.; Sawada, S.; Sedgwick, K.; Seidl, R.; Seto, R.; Sharma, D.; Shein, I.; Shibata, T.-A.; Shigaki, K.; Shim, H. H.; Shimomura, M.; Shoji, K.; Shukla, P.; Sickles, A.; Silva, C. L.; Silvermyr, D.; Silvestre, C.; Sim, K. S.; Singh, B. K.; Singh, C. P.; Singh, V.; Slunečka, M.; Sodre, T.; Soltz, R. A.; Sondheim, W. E.; Sorensen, S. P.; Sourikova, I. V.; Stankus, P. W.; Stenlund, E.; Stoll, S. P.; Sugitate, T.; Sukhanov, A.; Sun, J.; Sziklai, J.; Takagui, E. M.; Takahara, A.; Taketani, A.; Tanabe, R.; Tanaka, Y.; Taneja, S.; Tanida, K.; Tannenbaum, M. J.; Tarafdar, S.; Taranenko, A.; Tennant, E.; Themann, H.; Thomas, D.; Togawa, M.; Tomášek, L.; Tomášek, M.; Torii, H.; Towell, R. S.; Tserruya, I.; Tsuchimoto, Y.; Utsunomiya, K.; Vale, C.; van Hecke, H. W.; Vazquez-Zambrano, E.; Veicht, A.; Velkovska, J.; Vértesi, R.; Virius, M.; Vossen, A.; Vrba, V.; Vznuzdaev, E.; Wang, X. R.; Watanabe, D.; Watanabe, K.; Watanabe, Y.; Watanabe, Y. S.; Wei, F.; Wei, R.; Wessels, J.; White, S. N.; Winter, D.; Woody, C. L.; Wright, R. M.; Wysocki, M.; Yamaguchi, Y. L.; Yang, R.; Yanovich, A.; Ying, J.; Yokkaichi, S.; Yoo, J. S.; You, Z.; Young, G. R.; Younus, I.; Yushmanov, I. E.; Zajc, W. A.; Zelenski, A.; Zhou, S.; Phenix Collaboration

2015-02-01

We present midrapidity charged-pion invariant cross sections, the ratio of the π- to π+ cross sections and the charge-separated double-spin asymmetries in polarized p +p collisions at √{s }=200 GeV . While the cross section measurements are consistent within the errors of next-to-leading-order (NLO) perturbative quantum chromodynamics predictions (pQCD), the same calculations overestimate the ratio of the charged-pion cross sections. This discrepancy arises from the cancellation of the substantial systematic errors associated with the NLO-pQCD predictions in the ratio and highlights the constraints these data will place on flavor-dependent pion fragmentation functions. The charge-separated pion asymmetries presented here sample an x range of ˜0.03 - 0.16 and provide unique information on the sign of the gluon-helicity distribution.

Study of Velocity and Materials on Tribocharging of Polymer Powders for Powder Coating Applications

NASA Technical Reports Server (NTRS)

Biris, Alex S.; Trigwell, Steve; Sims, Robert A.; Mazumder, Malay K.

2005-01-01

Electrostatic powder deposition is widely used in a plethora of industrial-applications ranging from the pharmaceutical and food.industries, to farm equipment and automotive applications. The disadvantages of this technique are possible back corona (pin-like formations) onset and the Faraday penetration limitation (when the powder does not penetrate in some recessed areas). A possible solution to overcome these problems is to use tribochargers to electrostatically charge the powder. Tribocharging, or contact charging while two materials are in contact, is related to the work function difference between the contacting materials and generates bipolarly charged particles. The generation of an ion-free powder cloud by tribocharging with high bipolar charge and an overall charge density of almost zero, provides a better coverage of the recessed areas. In this study, acrylic and epoxy powders were fluidized and charged by passing through stainless steel, copper, aluminum, and polycarbonate static mixers, respectively. The particle velocity was varied to determine its effect on the net charge-to-mass ratio (QIM) acquired by the powders. In general, the Q/M increases rapidly when the velocity was increased from 1.5 to 2.5 m/s, remaining almost constant for higher velocities. Charge separation experiments showed bipolar charging for all chargers.

Mixed Metal Phosphonate- Phosphate Resins for Separation of Lanthanides from Actinides

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

Clearfield, Abraham

As indicated in the previous annual report the goals of this project are to develop procedures for efficient separation of lanthanides from actinides and curium from americium. These processes are required for the nuclear fuel cycle to minimize the waste and recover the valuable actinides. The basis for our study is that we have prepared a group of compounds that are porous and favor the uptake of ions with charges 3+ and 4+ over ions of lesser charge. The general formula for these materials is M(O 3PC 6H 4PO 3) 1-x/2(APO 4)x·nH 2O: where M=Zr 4+, Sn 4+, A=H, Na,more » or K and X=O, 0.5, 0.8, 1.0, 1.33 and 1.61-3. One of our tasks is to determine which members of this group of compounds are effective in carrying out the required separations. A difficulty in obtaining this required information is that the compounds are amorphous. That is they are not crystalline, therefore we need to resort to synchrotron data to obtain structural data which will be presented in detail. This information will be provided as a separate section.« less

A Novel, In-solution Separation of Endogenous Cardiac Sarcomeric Proteins and Identification of Distinct Charged Variants of Regulatory Light Chain*

PubMed Central

Scruggs, Sarah B.; Reisdorph, Rick; Armstrong, Mike L.; Warren, Chad M.; Reisdorph, Nichole; Solaro, R. John; Buttrick, Peter M.

2010-01-01

The molecular conformation of the cardiac myosin motor is modulated by intermolecular interactions among the heavy chain, the light chains, myosin binding protein-C, and titin and is governed by post-translational modifications (PTMs). In-gel digestion followed by LC/MS/MS has classically been applied to identify cardiac sarcomeric PTMs; however, this approach is limited by protein size, pI, and difficulties in peptide extraction. We report a solution-based work flow for global separation of endogenous cardiac sarcomeric proteins with a focus on the regulatory light chain (RLC) in which specific sites of phosphorylation have been unclear. Subcellular fractionation followed by OFFGEL electrophoresis resulted in isolation of endogenous charge variants of sarcomeric proteins, including regulatory and essential light chains, myosin heavy chain, and myosin-binding protein-C of the thick filament. Further purification of RLC using reverse-phase HPLC separation and UV detection enriched for RLC PTMs at the intact protein level and provided a stoichiometric and quantitative assessment of endogenous RLC charge variants. Digestion and subsequent LC/MS/MS unequivocally identified that the endogenous charge variants of cardiac RLC focused in unique OFFGEL electrophoresis fractions were unphosphorylated (78.8%), singly phosphorylated (18.1%), and doubly phosphorylated (3.1%) RLC. The novel aspects of this study are that 1) milligram amounts of endogenous cardiac sarcomeric subproteome were focused with resolution comparable with two-dimensional electrophoresis, 2) separation and quantification of post-translationally modified variants were achieved at the intact protein level, 3) separation of intact high molecular weight thick filament proteins was achieved in solution, and 4) endogenous charge variants of RLC were separated; a novel doubly phosphorylated form was identified in mouse, and singly phosphorylated, singly deamidated, and deamidated/phosphorylated forms were identified and quantified in human non-failing and failing heart samples, thus demonstrating the clinical utility of the method. PMID:20445002

Interfacial charge separation and photovoltaic efficiency in Fe(ii)-carbene sensitized solar cells.

PubMed

Pastore, Mariachiara; Duchanois, Thibaut; Liu, Li; Monari, Antonio; Assfeld, Xavier; Haacke, Stefan; Gros, Philippe C

2016-10-12

The first combined theoretical and photovoltaic characterization of both homoleptic and heteroleptic Fe(ii)-carbene sensitized photoanodes in working dye sensitized solar cells (DSSCs) has been performed. Three new heteroleptic Fe(ii)-NHC dye sensitizers have been synthesized, characterized and tested. Despite an improved interfacial charge separation in comparison to the homoleptic compounds, the heteroleptic complexes did not show boosted photovoltaic performances. The ab initio quantitative analysis of the interfacial electron and hole transfers and the measured photovoltaic data clearly evidenced fast recombination reactions for heteroleptics, even associated with un unfavorable directional electron flow, and hence slower injection rates, in the case of homoleptics. Notably, quantum mechanics calculations revealed that deprotonation of the not anchored carboxylic function in the homoleptic complex can effectively accelerate the electron injection rate and completely suppress the electron recombination to the oxidized dye. This result suggests that introduction of strong electron-donating substituents on the not-anchored carbene ligand in heteroleptic complexes, in such a way of mimicking the electronic effects of the carboxylate functionality, should yield markedly improved interfacial charge generation properties. The present results, providing for the first time a detailed understanding of the interfacial electron transfers and photovoltaic characterization in Fe(ii)-carbene sensitized solar cells, open the way to a rational molecular engineering of efficient iron-based dyes for photoelectrochemical applications.

Effect of solvent and subsequent thermal annealing on the performance of phenylenevinylene copolymer: PCBM solar cells.

PubMed

Sharma, G D; Suresh, P; Sharma, S S; Vijay, Y K; Mikroyannidis, John A

2010-02-01

The morphology of the photoactive layer used in the bulk heterojunction photovoltaic devices is crucial for efficient charge generation and their collection at the electrodes. We investigated the solvent vapor annealing and thermal annealing effect of an alternating phenylenevinylene copolymer P:PCBM blend on its morphology and optical properties. The UV-visible absorption spectroscopy shows that both solvent and thermal annealing can result in self-assembling of copolymer P to form an ordered structure, leading to enhanced absorption in the red region and hole transport enhancement. By combining the solvent and thermal annealing of the devices, the power conversion efficiency is improved. This feature was attributed to the fact that the PCBM molecules begin to diffuse into aggregates and together with the ordered copolymer P phase form bicontinuous pathways in the entire layer for efficient charge separation and transport. Furthermore, the measured photocurrent also suggests that the space charges no longer limit the values of the short circuit current (J(sc)) and fill factor (FF) for solvent-treated and thermally annealed devices. These results indicate that the higher J(sc) and PCE for the solvent-treated and thermally annealed devices can be attributed to the phase separation of active layers, which leads to a balanced carrier mobility. The overall PCE of the device based on the combination of solvent annealing and thermal annealing is about 3.7 %.

Exciplexes versus Loose Ion Pairs: How Does the Driving Force Impact the Initial Product Ratio of Photoinduced Charge Separation Reactions?

PubMed Central

2014-01-01

Many donor–acceptor systems can undergo a photoinduced charge separation reaction, yielding loose ion pairs (LIPs). LIPs can be formed either directly via (distant) electron transfer (ET) or indirectly via the dissociation of an initially formed exciplex or tight ion pair. Establishing the prevalence of one of the reaction pathways is challenging because differentiating initially formed exciplexes from LIPs is difficult due to similar spectroscopic footprints. Hence, no comprehensive reaction model has been established for moderately polar solvents. Here, we employ an approach based on the time-resolved magnetic field effect (MFE) of the delayed exciplex luminescence to distinguish the two reaction channels. We focus on the effects of the driving force of ET and the solvent permittivity. We show that, surprisingly, the exciplex channel is significant even for an exergonic ET system with a free energy of ET of −0.58 eV and for the most polar solutions studied (butyronitrile). Our findings demonstrate that exciplexes play a crucial role even in polar solvents and at moderate driving forces, contrary to what is usually assumed. PMID:25243054

Search for the Chiral Magnetic Effect in Heavy-Ion Collisions and Quantification of the Background with the AMPT Model

NASA Astrophysics Data System (ADS)

Bryon, Jacob

2017-09-01

The chiral magnetic effect (CME) arises from the chirality imbalance of quarks and its interaction to the strong magnetic field generated in non-central heavy-ion collisions. Possible formation of domains of quarks with chirality imbalances is an intrinsic property of the Quantum ChromoDynamics (QCD), which describes the fundamental strong interactions among quarks and gluons. Azimuthal-angle correlations have been used to measure the magnitude of charge- separation across the reaction plane, which was predicted to arise from the CME. However, backgrounds from collective motion (flow) of the collision system can also contribute to the correlation observable. In this poster, we investigate the magnitude of the background utilizing the AMPT model, which contains no CME signals. We demonstrate, for Au +Au collisions at 200 and 39 GeV, a scheme to remove the flow background via the event-shape engineering with the vanishing magnitude of the flow vector. We also calculate the ensemble average of the charge-separation observable, and provide a background baseline for the experimental data.

Rapid detection of cardiac troponin I using antibody-immobilized gate-pulsed AlGaN/GaN high electron mobility transistor structures

NASA Astrophysics Data System (ADS)

Yang, Jiancheng; Carey, Patrick; Ren, Fan; Wang, Yu-Lin; Good, Michael L.; Jang, Soohwan; Mastro, Michael A.; Pearton, S. J.

2017-11-01

We report a comparison of two different approaches to detecting cardiac troponin I (cTnI) using antibody-functionalized AlGaN/GaN High Electron Mobility Transistors (HEMTs). If the solution containing the biomarker has high ionic strength, there can be difficulty in detection due to charge-screening effects. To overcome this, in the first approach, we used a recently developed method involving pulsed biases applied between a separate functionalized electrode and the gate of the HEMT. The resulting electrical double layer produces charge changes which are correlated with the concentration of the cTnI biomarker. The second approach fabricates the sensing area on a glass slide, and the pulsed gate signal is externally connected to the nitride HEMT. This produces a larger integrated change in charge and can be used over a broader range of concentrations without suffering from charge-screening effects. Both approaches can detect cTnI at levels down to 0.01 ng/ml. The glass slide approach is attractive for inexpensive cartridge-type sensors.

The rates of charge separation and energy destructive charge recombination processes within an organic dyad in presence of metal-semiconductor core shell nanocomposites.

PubMed

Mandal, Gopa; Bhattacharya, Sudeshna; Das, Subrata; Ganguly, Tapan

2012-01-01

Steady state and time resolved spectroscopic measurements were made at the ambient temperature on an organic dyad, 1-(4-Chloro-phenyl)-3-(4-methoxy-naphthalen-1-yl)-propenone (MNCA), where the donor 1-methoxynaphthalene (1 MNT) is connected with the acceptor p-chloroacetophenone (PCA) by an unsaturated olefinic bond, in presence of Ag@TiO2 nanoparticles. Time resolved fluorescence and absorption measurements reveal that the rate parameters associated with charge separation, k(CS), within the dyad increases whereas charge recombination rate k(CR) reduces significantly when the surrounding medium is changed from only chloroform to mixture of chloroform and Ag@TiO2 (noble metal-semiconductor) nanocomposites. The observed results indicate that the dyad being combined with core-shell nanocomposites may form organic-inorganic nanocomposite system useful for developing light energy conversion devices. Use of metal-semiconductor nanoparticles may provide thus new ways to modulate charge recombination processes in light energy conversion devices. From comparison with the results obtained in our earlier investigations with only TiO2 nanoparticles, it is inferred that much improved version of light energy conversion device, where charge-separated species could be protected for longer period of time of the order of millisecond, could be designed by using metal-semiconductor core-shell nanocomposites rather than semiconductor nanoparticles only.

High yield of secondary B-side electron transfer in mutant Rhodobacter capsulatus reaction centers

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

Kressel, Lucas; Faries, Kaitlyn M.; Wander, Marc J.

2014-08-01

From the crystal structures of reaction centers (RCs) from purple photosynthetic bacteria, two pathways for electron transfer (ET) are apparent but only one pathway (the A side) operates in the native protein-cofactor complex. Partial activation of the B-side pathway has unveiled the true inefficiencies of ET processes on that side in comparison to analogous reactions on the A side. Of significance are the relative rate constants for forward ET and the competing charge recombination reactions. On the B side, these rate constants are nearly equal for the secondary charge-separation step (ET from bacteriopheophytin to quinone), relegating the yield of thismore » process to < 50%. Herein we report efforts to optimize this step. In surveying all possible residues at position 131 in the M subunit, we discovered that when glutamic acid replaces the native valine the efficiency of the secondary ET is nearly two-fold higher than in the wild-type RC. The positive effect of M131 Glu is likely due to formation of a hydrogen bond with the ring V keto group of the B-side bacteriopheophytin leading to stabilization of the charge-separated state involving this cofactor. In conclusion, this change slows charge recombination by roughly a factor of two and affords the improved yield of the desired forward ET to the B-side quinone terminal acceptor.« less

Two possible improvements for mass spectrometry analysis of intact biomolecules.

PubMed

Raznikov, Valeriy V; Zelenov, Vladislav V; Aparina, Elena V; Pikhtelev, Alexander R; Sulimenkov, Ilia V; Raznikova, Marina O

2017-08-01

The goals of our study were to investigate abilities of two approaches to eliminate possible errors in electrospray mass spectrometry measurements of biomolecules. Passing of a relatively dense supersonic gas jet through ionization region followed by its hitting the spray of the analyzed solution in low vacuum may be effective to keep an initial biomolecule structure in solution. Provided that retention of charge carriers for some sites in the biomolecule cannot be changed noticeably in electrospray ion source, decomposition and separation of charge-state distributions of electrosprayed ions may give additional information about native structure of biomolecules in solution.

Electrospun nylon 6/zinc doped hydroxyapatite membrane for protein separation: Mechanism of fouling and blocking model.

PubMed

Esfahani, Hamid; Prabhakaran, Molamma P; Salahi, Esmaeil; Tayebifard, Ali; Rahimipour, Mohamad Reza; Keyanpour-Rad, Mansour; Ramakrishna, Seeram

2016-02-01

Development of composite nanofibrous membrane via electrospinning a polymer with ceramic nanoparticles (NPs) for application in protein separation systems is explored during this study. Positively charged zinc doped hydroxyapatite (xZH) NPs were prepared in three different compositions via chemical precipitation method. Herein, we created a positively charged surface containing nanoparticles on electrospun Nylon-6 nanofibers (NFs) to improve the separation and selectivity properties for adsorption of negatively charged protein, namely bovine serum albumin (BSA). The decline in permeate flux was analyzed using the framework of classical blocking models and fitting, demonstrated that the transition of fouling mechanisms was dominated during the filtration process. The standard blocking model provided the best fit of the experimental results during the mid-filtration period. The membrane decorated by NPs containing 4at.% zinc cations not only provided maximum BSA separation but also capable of separating higher amounts of BSA molecules (even after 1h filtration) than the pure Nylon membrane. Protein separation was achieved through this membrane with the incorporation of NPs that had high zeta potential (+5.9±0.2mV) and lower particle area (22,155nm(2)). The developed membrane has great potential to act as a high efficiency membrane for capturing BSA. Copyright © 2015 Elsevier B.V. All rights reserved.

Simultaneous separation and analysis of water- and fat-soluble vitamins on multi-modal reversed-phase weak anion exchange material by HPLC-UV.

PubMed

Dabre, Romain; Azad, Nazanin; Schwämmle, Achim; Lämmerhofer, Michael; Lindner, Wolfgang

2011-04-01

Several methods for the separation of vitamins on HPLC columns were already validated in the last 20 years. However, most of the techniques focus on separating either fat- or water-soluble vitamins and only few methods are intended to separate lipophilic and hydrophilic vitamins simultaneously. A mixed-mode reversed-phase weak anion exchange (RP-WAX) stationary phase was developed in our laboratory in order to address such mixture of analytes with different chemical characteristics, which are difficult to separate on standard columns. The high versatility in usage of the RP-WAX chromatographic material allowed a baseline separation of ten vitamins within a single run, seven water-soluble and three fat-soluble, using three different chromatographic modes: some positively charged vitamins are eluted in ion exclusion and ion repulsion modes whereas the negatively charged molecules are eluted in the ion exchange mechanism. The non-charged molecules are eluted in a classical reversed-phase mode, regarding their polarities. The method was validated for the vitamin analysis in tablets, evaluating selectivity, robustness, linearity, accuracy, and precision. The validated method was finally employed for the analysis of the vitamin content of some commercially available supplement tablets. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Sequence-Specific Model for Peptide Retention Time Prediction in Strong Cation Exchange Chromatography.

PubMed

Gussakovsky, Daniel; Neustaeter, Haley; Spicer, Victor; Krokhin, Oleg V

2017-11-07

The development of a peptide retention prediction model for strong cation exchange (SCX) separation on a Polysulfoethyl A column is reported. Off-line 2D LC-MS/MS analysis (SCX-RPLC) of S. cerevisiae whole cell lysate was used to generate a retention dataset of ∼30 000 peptides, sufficient for identifying the major sequence-specific features of peptide retention mechanisms in SCX. In contrast to RPLC/hydrophilic interaction liquid chromatography (HILIC) separation modes, where retention is driven by hydrophobic/hydrophilic contributions of all individual residues, SCX interactions depend mainly on peptide charge (number of basic residues at acidic pH) and size. An additive model (incorporating the contributions of all 20 residues into the peptide retention) combined with a peptide length correction produces a 0.976 R 2 value prediction accuracy, significantly higher than the additive models for either HILIC or RPLC. Position-dependent effects on peptide retention for different residues were driven by the spatial orientation of tryptic peptides upon interaction with the negatively charged surface functional groups. The positively charged N-termini serve as a primary point of interaction. For example, basic residues (Arg, His, Lys) increase peptide retention when located closer to the N-terminus. We also found that hydrophobic interactions, which could lead to a mixed-mode separation mechanism, are largely suppressed at 20-30% of acetonitrile in the eluent. The accuracy of the final Sequence-Specific Retention Calculator (SSRCalc) SCX model (∼0.99 R 2 value) exceeds all previously reported predictors for peptide LC separations. This also provides a solid platform for method development in 2D LC-MS protocols in proteomics and peptide retention prediction filtering of false positive identifications.

Evaluation of differences between dual salt-pH gradient elution and mono gradient elution using a thermodynamic model: Simultaneous separation of six monoclonal antibody charge and size variants on preparative-scale ion exchange chromatographic resin.

PubMed

Lee, Yi Feng; Jöhnck, Matthias; Frech, Christian

2018-02-21

The efficiencies of mono gradient elution and dual salt-pH gradient elution for separation of six mAb charge and size variants on a preparative-scale ion exchange chromatographic resin are compared in this study. Results showed that opposite dual salt-pH gradient elution with increasing pH gradient and simultaneously decreasing salt gradient is best suited for the separation of these mAb charge and size variants on Eshmuno ® CPX. Besides giving high binding capacity, this type of opposite dual salt-pH gradient also provides better resolved mAb variant peaks and lower conductivity in the elution pools compared to single pH or salt gradients. To have a mechanistic understanding of the differences in mAb variants retention behaviors of mono pH gradient, parallel dual salt-pH gradient, and opposite dual salt-pH gradient, a linear gradient elution model was used. After determining the model parameters using the linear gradient elution model, 2D plots were used to show the pH and salt dependencies of the reciprocals of distribution coefficient, equilibrium constant, and effective ionic capacity of the mAb variants in these gradient elution systems. Comparison of the 2D plots indicated that the advantage of opposite dual salt-pH gradient system with increasing pH gradient and simultaneously decreasing salt gradient is the noncontinuous increased acceleration of protein migration. Furthermore, the fitted model parameters can be used for the prediction and optimization of mAb variants separation in dual salt-pH gradient and step elution. © 2018 American Institute of Chemical Engineers Biotechnol. Prog., 2018. © 2018 American Institute of Chemical Engineers.

Comparing Positively and Negatively Charged Distonic Radical Ions in Phenylperoxyl Forming Reactions.

PubMed

Williams, Peggy E; Marshall, David L; Poad, Berwyck L J; Narreddula, Venkateswara R; Kirk, Benjamin B; Trevitt, Adam J; Blanksby, Stephen J

2018-06-04

In the gas phase, arylperoxyl forming reactions play a significant role in low-temperature combustion and atmospheric processing of volatile organic compounds. We have previously demonstrated the application of charge-tagged phenyl radicals to explore the outcomes of these reactions using ion trap mass spectrometry. Here, we present a side-by-side comparison of rates and product distributions from the reaction of positively and negatively charge tagged phenyl radicals with dioxygen. The negatively charged distonic radical ions are found to react with significantly greater efficiency than their positively charged analogues. The product distributions of the anion reactions favor products of phenylperoxyl radical decomposition (e.g., phenoxyl radicals and cyclopentadienone), while the comparable fixed-charge cations yield the stabilized phenylperoxyl radical. Electronic structure calculations rationalize these differences as arising from the influence of the charged moiety on the energetics of rate-determining transition states and reaction intermediates within the phenylperoxyl reaction manifold and predict that this influence could extend to intra-molecular charge-radical separations of up to 14.5 Å. Experimental observations of reactions of the novel 4-(1-carboxylatoadamantyl)phenyl radical anion confirm that the influence of the charge on both rate and product distribution can be modulated by increasing the rigidly imposed separation between charge and radical sites. These findings provide a generalizable framework for predicting the influence of charged groups on polarizable radicals in gas phase distonic radical ions. Graphical Abstract.

Comparing Positively and Negatively Charged Distonic Radical Ions in Phenylperoxyl Forming Reactions

NASA Astrophysics Data System (ADS)

Williams, Peggy E.; Marshall, David L.; Poad, Berwyck L. J.; Narreddula, Venkateswara R.; Kirk, Benjamin B.; Trevitt, Adam J.; Blanksby, Stephen J.

2018-06-01

In the gas phase, arylperoxyl forming reactions play a significant role in low-temperature combustion and atmospheric processing of volatile organic compounds. We have previously demonstrated the application of charge-tagged phenyl radicals to explore the outcomes of these reactions using ion trap mass spectrometry. Here, we present a side-by-side comparison of rates and product distributions from the reaction of positively and negatively charge tagged phenyl radicals with dioxygen. The negatively charged distonic radical ions are found to react with significantly greater efficiency than their positively charged analogues. The product distributions of the anion reactions favor products of phenylperoxyl radical decomposition (e.g., phenoxyl radicals and cyclopentadienone), while the comparable fixed-charge cations yield the stabilized phenylperoxyl radical. Electronic structure calculations rationalize these differences as arising from the influence of the charged moiety on the energetics of rate-determining transition states and reaction intermediates within the phenylperoxyl reaction manifold and predict that this influence could extend to intra-molecular charge-radical separations of up to 14.5 Å. Experimental observations of reactions of the novel 4-(1-carboxylatoadamantyl)phenyl radical anion confirm that the influence of the charge on both rate and product distribution can be modulated by increasing the rigidly imposed separation between charge and radical sites. These findings provide a generalizable framework for predicting the influence of charged groups on polarizable radicals in gas phase distonic radical ions.

Molecular Structure and Sequence in Complex Coacervates

NASA Astrophysics Data System (ADS)

Sing, Charles; Lytle, Tyler; Madinya, Jason; Radhakrishna, Mithun

Oppositely-charged polyelectrolytes in aqueous solution can undergo associative phase separation, in a process known as complex coacervation. This results in a polyelectrolyte-dense phase (coacervate) and polyelectrolyte-dilute phase (supernatant). There remain challenges in understanding this process, despite a long history in polymer physics. We use Monte Carlo simulation to demonstrate that molecular features (charge spacing, size) play a crucial role in governing the equilibrium in coacervates. We show how these molecular features give rise to strong monomer sequence effects, due to a combination of counterion condensation and correlation effects. We distinguish between structural and sequence-based correlations, which can be designed to tune the phase diagram of coacervation. Sequence effects further inform the physical understanding of coacervation, and provide the basis for new coacervation models that take monomer-level features into account.

Polyelectrolyte assisted charge titration spectrometry: Applications to latex and oxide nanoparticles.

PubMed

Mousseau, F; Vitorazi, L; Herrmann, L; Mornet, S; Berret, J-F

2016-08-01

The electrostatic charge density of particles is of paramount importance for the control of the dispersion stability. Conventional methods use potentiometric, conductometric or turbidity titration but require large amount of samples. Here we report a simple and cost-effective method called polyelectrolyte assisted charge titration spectrometry or PACTS. The technique takes advantage of the propensity of oppositely charged polymers and particles to assemble upon mixing, leading to aggregation or phase separation. The mixed dispersions exhibit a maximum in light scattering as a function of the volumetric ratio X, and the peak position XMax is linked to the particle charge density according to σ∼D0XMax where D0 is the particle diameter. The PACTS is successfully applied to organic latex, aluminum and silicon oxide particles of positive or negative charge using poly(diallyldimethylammonium chloride) and poly(sodium 4-styrenesulfonate). The protocol is also optimized with respect to important parameters such as pH and concentration, and to the polyelectrolyte molecular weight. The advantages of the PACTS technique are that it requires minute amounts of sample and that it is suitable to a broad variety of charged nano-objects. Copyright © 2016 Elsevier Inc. All rights reserved.

Ultrafast photoinduced charge transport in Pt(II) donor-acceptor assembly bearing naphthalimide electron acceptor and phenothiazine electron donor.

PubMed

Sazanovich, Igor V; Best, Jonathan; Scattergood, Paul A; Towrie, Michael; Tikhomirov, Sergei A; Bouganov, Oleg V; Meijer, Anthony J H M; Weinstein, Julia A

2014-12-21

Visible light-induced charge transfer dynamics were investigated in a novel transition metal triad acceptor-chromophore-donor, (NDI-phen)Pt(II)(-C≡C-Ph-CH2-PTZ)2 (1), designed for photoinduced charge separation using a combination of time-resolved infrared (TRIR) and femtosecond electronic transient absorption (TA) spectroscopy. In 1, the electron acceptor is 1,4,5,8-naphthalene diimide (NDI), and the electron donor is phenothiazine (PTZ), and [(phen)Pt(-C≡C-Ph-)], where phen is 1,10-phenanthroline, represents the chromophoric core. The first excited state observed in 1 is a (3)MLCT/LL'CT, with {Pt(II)-acetylide}-to-phen character. Following that, charge transfer from the phen-anion onto the NDI subunit to form NDI(-)-phen-[Pt-(C≡C)2](+)-PTZ2 occurs with a time constant of 2.3 ps. This transition is characterised by appearance of the prominent NDI-anion features in both TRIR and TA spectra. The final step of the charge separation in 1 proceeds with a time constant of ∼15 ps during which the hole migrates from the [Pt-(C≡C)2] subunit to one of the PTZ groups. Charge recombination in 1 then occurs with two distinct time constants of 36 ns and 107 ns, corresponding to the back electron transfer to each of the two donor groups; a rather rare occurrence which manifests that the hole in the final charge-separated state is localised on one of the two donor PTZ groups. The assignment of the nature of the excited states and dynamics in 1 was assisted by TRIR investigations of the analogous previously reported ((COOEt)2bpy)Pt(C≡C-Ph-CH2-PTZ)2 (2), (J. E. McGarrah and R. Eisenberg, Inorg. Chem., 2003, 42, 4355; J. E. McGarrah, J. T. Hupp and S. N. Smirnov, J. Phys. Chem. A, 2009, 113, 6430) as well as (bpy)Pt(C≡C-Ph-C7H15)2, which represent the acceptor-free dyad, and the chromophoric core, respectively. Thus, the step-wise formation of the full charge-separated state on the picosecond time scale and charge recombination via tunnelling have been established; and the presence of two distinct charge recombination pathways has been observed.

Electrokinetic Supercapacitor for Simultaneous Harvesting and Storage of Mechanical Energy.

PubMed

Yang, Peihua; Qu, Xiaopeng; Liu, Kang; Duan, Jiangjiang; Li, Jia; Chen, Qian; Xue, Guobin; Xie, Wenke; Xu, Zhimou; Zhou, Jun

2018-03-07

Energy harvesting and storage are two distinct processes that are generally achieved using two separated parts based on different physical and chemical principles. Here we report a self-charging electrokinetic supercapacitor that directly couples the energy harvesting and storage processes into one device. The device consists of two identical carbon nanotube/titanium electrodes, separated by a piece of anodic aluminum oxide nanochannels membrane. Pressure-driven electrolyte flow through the nanochannels generates streaming potential, which can be used to charge the capacitive electrodes, accomplishing simultaneous energy generation and storage. The device stores electric charge density of 0.4 mC cm -2 after fully charging under pressure of 2.5 bar. This work may offer a train of thought for the development of a new type of energy unit for self-powered systems.

Field-modulation spectroscopy of pentacene thin films using field-effect devices: Reconsideration of the excitonic structure

NASA Astrophysics Data System (ADS)

Haas, Simon; Matsui, Hiroyuki; Hasegawa, Tatsuo

2010-10-01

We report pure electric-field effects on the excitonic absorbance of pentacene thin films as measured by unipolar field-effect devices that allowed us to separate the charge accumulation effects. The field-modulated spectra between 1.8 and 2.6 eV can be well fitted with the first derivative curve of Frenkel exciton absorption and its vibronic progression, and at higher energy a field-induced feature appears at around 2.95 eV. The results are in sharp contrast to the electroabsorption spectra reported by Sebastian in previous studies [Chem. Phys. 61, 125 (1981)10.1016/0301-0104(81)85055-0], and leads us to reconsider the excitonic structure including the location of charge-transfer excitons. Nonlinear π -electronic response is discussed based on second-order electro-optic (Kerr) spectra.

Organic phototransistors with nanoscale phase-separated polymer/polymer bulk heterojunction layers

NASA Astrophysics Data System (ADS)

Hwang, Hyemin; Kim, Hwajeong; Nam, Sungho; Bradley, Donal D. C.; Ha, Chang-Sik; Kim, Youngkyoo

2011-05-01

Low-cost detectors for sensing photons at a low light intensity are of crucial importance in modern science. Phototransistors can deliver better signals of low-intensity light by electrical amplification, but conventional inorganic phototransistors have a limitation owing to their high temperature processes in vacuum. In this work, we demonstrate organic phototransistors with polymer/polymer bulk heterojunction blend films (mixtures of p-type and n-type semiconducting polymers), which can be fabricated by inexpensive solution processes at room temperature. The key idea here is to effectively exploit hole charges (from p-type polymer) as major signaling carriers by employing p-type transistor geometry, while the n-type polymer helps efficient charge separation from excitons generated by incoming photons. Results showed that the present organic transistors exhibited proper functions as p-type phototransistors with ~4.3 A W-1 responsivity at a low light intensity (1 µW cm-2), which supports their encouraging potential to replace conventional cooled charge coupled devices (CCD) for low-intensity light detection applications.Low-cost detectors for sensing photons at a low light intensity are of crucial importance in modern science. Phototransistors can deliver better signals of low-intensity light by electrical amplification, but conventional inorganic phototransistors have a limitation owing to their high temperature processes in vacuum. In this work, we demonstrate organic phototransistors with polymer/polymer bulk heterojunction blend films (mixtures of p-type and n-type semiconducting polymers), which can be fabricated by inexpensive solution processes at room temperature. The key idea here is to effectively exploit hole charges (from p-type polymer) as major signaling carriers by employing p-type transistor geometry, while the n-type polymer helps efficient charge separation from excitons generated by incoming photons. Results showed that the present organic transistors exhibited proper functions as p-type phototransistors with ~4.3 A W-1 responsivity at a low light intensity (1 µW cm-2), which supports their encouraging potential to replace conventional cooled charge coupled devices (CCD) for low-intensity light detection applications. Electronic supplementary information (ESI) available: XPS spectra of P3HT:F8BT nanolayers and pristine P3HT and F8BT films, HRTEM images of P3HT:F8BT blend film detached from the substrate, and 1D GIXD profiles of P3HT:F8BT nanolayers and PI layer coated on the ITO-glass substrates. See DOI: 10.1039/c0nr00915f

Separations by supported liquid membrane cascades

DOEpatents

Danesi, Pier R.

1986-01-01

The invention describes a new separation technique which leads to multi-stage operations by the use of a series (a cascade) of alternated carrier-containing supported-liquid membranes. The membranes contain alternatively a liquid cation exchanger extractant and a liquid anion exchanger extractant (or a neutral extractant) as carrier. The membranes are spaced between alternated aqueous electrolytic solutions of different composition which alternatively provide positively charged extractable species and negatively charged (or zero charged) extractable species, of the chemical species to be separated. The alternated aqueous electrolytic solutions in addition to providing the driving force to the process, simultaneously function as a stripping solution from one type of membrane and as an extraction-promoting solution for the other type of membrane. The aqueous electrolytic solutions and the supported liquid membranes are arranged in such a way to provide a continuous process which leads to the continuous enrichment of the species which show the highest permeability coefficients. By virtue of the very high number of stages which can be arranged, even chemical species having very similar chemical behavior (and consequently very similar permeability coefficients) can be completely separated. The invention also provide a way to concentrate the separated species.

48 CFR 871.201-2 - Requirements when contracts are not required.

Code of Federal Regulations, 2010 CFR

2010-10-01

..., fees, and charges for books, supplies, or services necessary to train or educate an eligible veteran..., including the rate of tuition, fees, and separate charges, if any, for books, supplies, and equipment... accordance with catalog or other published document (identify publication). The statement of charges may not...

Magnetic Separator Enhances Treatment Possibilities

NASA Technical Reports Server (NTRS)

2008-01-01

Since the earliest missions in space, NASA specialists have performed experiments in low gravity. Protein crystal growth, cell and tissue cultures, and separation technologies such as electrophoresis and magnetophoresis have been studied on Apollo 14, Apollo 16, STS-107, and many other missions. Electrophoresis and magnetophoresis, respectively, are processes that separate substances based on the electrical charge and magnetic field of a molecule or particle. Electrophoresis has been studied on over a dozen space shuttle flights, leading to developments in electrokinetics, which analyzes the effects of electric fields on mass transport (atoms, molecules, and particles) in fluids. Further studies in microgravity will continue to improve these techniques, which researchers use to extract cells for various medical treatments and research.

Stacked white OLED having separate red, green and blue sub-elements

DOEpatents

Forrest, Stephen; Qi, Xiangfei; Slootsky, Michael

2014-07-01

The present invention relates to efficient organic light emitting devices (OLEDs). The devices employ three emissive sub-elements, typically emitting red, green and blue, to sufficiently cover the visible spectrum. Thus, the devices may be white-emitting OLEDs, or WOLEDs. Each sub-element comprises at least one organic layer which is an emissive layer--i.e., the layer is capable of emitting light when a voltage is applied across the stacked device. The sub-elements are vertically stacked and are separated by charge generating layers. The charge-generating layers are layers that inject charge carriers into the adjacent layer(s) but do not have a direct external connection.

Delayed bunching for multi-reflection time-of-flight mass separation

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

Rosenbusch, M.; Marx, G.; Schweikhard, L.

2015-06-29

Many experiments are handicapped when the ion sources do not only deliver the ions of interest but also contaminations, i.e., unwanted ions of similar mass. In the recent years, multi-reflection time-of-flight mass separation has become a promising method to isolate the ions of interest from the contaminants, in particular for measurements with low-energy short-lived nuclides. To further improve the performance of multi-reflection mass separators with respect to the limitations by space-charge effects, the simultaneously trapped ions are spatially widely distributed in the apparatus. Thus, the ions can propagate with reduced Coulomb interactions until, finally, they are bunched by a changemore » in the trapping conditions for high-resolution mass separation. Proof-of-principle measurements are presented.« less

Separation of charge-regulated polyelectrolytes by pH-assisted diffusiophoresis.

PubMed

Hsu, Jyh-Ping; Hsu, Yen-Rei; Shang-Hung, Hsieh; Tseng, Shiojenn

2017-03-29

The potential of separating colloidal particles through simultaneous application of a salt gradient and a pH gradient, or pH-assisted diffusiophoresis, is evaluated by considering the case of spherical polyelectrolytes (PEs) having different equilibrium dissociation constants in an aqueous solution with KCl as the background salt. The simulation results gathered reveal that the dependence of the particle velocity on pH is more sensitive than that in pH-assisted electrophoresis, where an electric field and a pH gradient are applied simultaneously. This implies that the separation efficiency of pH-assisted diffusiophoresis can be better than that of pH-assisted electrophoresis. In particular, two types of PE having different equilibrium dissociation constants can be separated effectively by applying the former by enhancing/reducing their diffusiophoretic velocities.

Room-temperature in situ fabrication of Bi2O3/g-C3N4 direct Z-scheme photocatalyst with enhanced photocatalytic activity

NASA Astrophysics Data System (ADS)

He, Rongan; Zhou, Jiaqian; Fu, Huiqing; Zhang, Shiying; Jiang, Chuanjia

2018-02-01

Constructing direct Z-scheme heterojunction is an effective approach to separating photogenerated charge carriers and improving the activity of semiconductor photocatalysts. Herein, a composite of bismuth(III) oxide (Bi2O3) and graphitic carbon nitride (g-C3N4) was in situ fabricated at room temperature by photoreductive deposition of Bi3+ and subsequent air-oxidation of the resultant metallic Bi. Quantum-sized ω-Bi2O3 nanoparticles approximately 6 nm in diameter were uniformly distributed on the surface of mesoporous g-C3N4. The as-prepared Bi2O3/g-C3N4 composite exhibited higher photocatalytic activity than pure Bi2O3 and g-C3N4 for photocatalytic degradation of phenol under visible light. Reactive species trapping experiments revealed that superoxide radicals and photogenerated holes played important roles in the photocatalytic degradation of phenol. The enhanced photocatalytic activity, identification of reactive species and higher rate of charge carrier recombination (as indicated by stronger photoluminescence intensity) collectively suggest that the charge migration within the Bi2O3/g-C3N4 composite followed a Z-scheme mechanism. Photogenerated electrons on the conduction band of Bi2O3 migrate to the valence band of g-C3N4 and combine with photogenerated holes therein. At the cost of these less reactive charge carriers, the Z-scheme heterojunction enables efficient charge separation, while preserving the photogenerated electrons and holes with stronger redox abilities, which is beneficial for enhanced photocatalytic activity.

Electrostatic Explorations.

ERIC Educational Resources Information Center

Gallai, Ditta; Stewart, Gay

1998-01-01

Presents a set of hands-on electrostatics experiments in the form of an activity guide and worksheet through which students discover the different types of electric charge, Coulomb's Law, induced charge separation, and grounding. (DDR)

Electrostatic Beneficiation of Lunar Simulant

NASA Technical Reports Server (NTRS)

Trigwell, Steve; Captain, James; Captain, Janine; Arens, Ellen; Quinn, Jacqueline; Calle, Carlos

2006-01-01

Electrostatic beneficiation of lunar regolith is a method allowing refinement of specific minerals in the material for processing on the moon. The use of tribocharging the regolith prior to separation was investigated on the lunar simulant MLS-I by passing the dust through static mixers constructed from different materials; aluminum, copper, stainless steel, and polytetrafluoroethylene (PTFE). The amount of charge acquired by the simulant was dependent upon the difference in the work function of the dust and the charging material. XPS and SEM were used to characterize the simulant after it was sieved into five size fractions (> 100 pm, 75-100 pm, 50- 75 pm, 50-25 pm, and < 25 pm), where very little difference in surface composition was observed between the sizes. Samples of the smallest (< 25 pm) and largest (> 100 pm) size fractions were beneficiated through a charge separator using the aluminum (charged the simulant negatively) and PTFE (charged positively) mixers. The mass fractions of the separated simulant revealed that for the larger particle size, significant unipolar charging was observed for both mixers, whereas for the smaller particle sizes, more bipolar charging was observed, probably due to the finer simulant adhering to the inside of the mixers shielding the dust from the charging material. Subsequent XPS analysis of the beneficiated fractions showed the larger particle size fraction having some species differentiation, but very little difference for the smaller.size. Although MLS-1 was made to have similar chemistry to actual lunar dust, its mineralogy is quite different. On-going experiments are using NASA JSC-1 lunar simulant. A vacuum chamber has been constructed, and future experiments are planned in a simulated lunar environment.

Modular Homogeneous Chromophore–Catalyst Assemblies

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

Mulfort, Karen L.; Utschig, Lisa M.

2016-05-17

Photosynthetic reaction center (RC) proteins convert incident solar energy to chemical energy through a network of molecular cofactors which have been evolutionarily tuned to couple efficient light-harvesting, directional electron transfer, and long-lived charge separation with secondary reaction sequences. These molecular cofactors are embedded within a complex protein environment which precisely positions each cofactor in optimal geometries along efficient electron transfer pathways with localized protein environments facilitating sequential and accumulative charge transfer. By contrast, it is difficult to approach a similar level of structural complexity in synthetic architectures for solar energy conversion. However, by using appropriate self-assembly strategies, we anticipate thatmore » molecular modules, which are independently synthesized and optimized for either light-harvesting or redox catalysis, can be organized into spatial arrangements that functionally mimic natural photosynthesis. In this Account, we describe a modular approach to new structural designs for artificial photosynthesis which is largely inspired by photosynthetic RC proteins. We focus on recent work from our lab which uses molecular modules for light-harvesting or proton reduction catalysis in different coordination geometries and different platforms, spanning from discrete supramolecular assemblies to molecule–nanoparticle hybrids to protein-based biohybrids. Molecular modules are particularly amenable to high-resolution characterization of the ground and excited state of each module using a variety of physical techniques; such spectroscopic interrogation helps our understanding of primary artificial photosynthetic mechanisms. In particular, we discuss the use of transient optical spectroscopy, EPR, and X-ray scattering techniques to elucidate dynamic structural behavior and light-induced kinetics and the impact on photocatalytic mechanism. Two different coordination geometries of supramolecular photocatalyst based on the [Ru(bpy)3]2+ (bpy = 2,2'-bipyridine) light-harvesting module with cobaloxime-based catalyst module are compared, with progress in stabilizing photoinduced charge separation identified. These same modules embedded in the small electron transfer protein ferredoxin exhibit much longer charge-separation, enabled by stepwise electron transfer through the native [2Fe-2S] cofactor. We anticipate that the use of interchangeable, molecular modules which can interact in different coordination geometries or within entirely different structural platforms will provide important fundamental insights into the effect of environment on parameters such as electron transfer and charge separation, and ultimately drive more efficient designs for artificial photosynthesis.« less

Report of investigations into charge cadmium reactivity: Nickel-cadmium cell ESD 91-86

NASA Technical Reports Server (NTRS)

Lewis, Harlan L.

1992-01-01

In Aug. 1990, a presentation was given at the 25th Ann. IECEC meeting on the results of Destructive Physical Analysis (DPA) on two successive sets of Ni-Cd cells. The cells were of two different separator types, Pellon 2505 and 2536. One cell of each separator type was analyzed on two occasions; the first pair were analyzed to establish baseline data on essentially new cells; the second pair were analyzed after the cells had been on charge-discharge cycling for a year in connection with a satellite simulation study. The gas composition found in the cells, the absence of charged cadmium in the analytical data, and the appearance of dried out portions on the Cd plates in the one year cell S/N 7 which used Pellon 2505 as its separator material, were questions which arose. These concerns are answered and the observational results are clarified.

Worm Algorithm simulations of the hole dynamics in the t-J model

NASA Astrophysics Data System (ADS)

Prokof'ev, Nikolai; Ruebenacker, Oliver

2001-03-01

In the limit of small J << t, relevant for HTSC materials and Mott-Hubbard systems, computer simulations have to be performed for large systems and at low temperatures. Despite convincing evidence against spin-charge separation obtained by various methods for J > 0.4t there is an ongoing argument that at smaller J spin-charge separation is still possible. Worm algorithm Monte Carlo simulations of the hole Green function for 0.1 < J/t < 0.4 were performed on lattices with up to 32x32 sites, and at temperature J/T = 40 (for the largest size). Spectral analysis reveals a single, delta-function sharp quasiparticle peak at the lowest edge of the spectrum and two distinct peaks above it at all studied J. We rule out the possibility of spin-charge separation in this parameter range, and present, apparently, the hole spectral function in the thermodynamic limit.

Picosecond absorption studies of photoinduced charge separation in polyelectrolyte bound aromatic chromophores

NASA Astrophysics Data System (ADS)

Shand, M. A.; Rodgers, M. A. J.; Webber, S. E.

1991-02-01

Picosecond absorption studies of photoinduced electron transfer between aromatic chromophores bound to polymethacrylic acid (P) and methylviologen (MV 2+ have been carried out in aqueous solution. The diphenylanthracene copolymer/viologen system at pH 2.8 shows the corresponding redox products DPA + rad and MV + rad arising from the singlet state of DPA with a forward rate constant of electron transfer of 2.6 × 10 9 s -1. At pH 9.0 the quenching of the S 1 state of DPA occurs with no charge separated products being observed. The pyrene copolymer shows no evidence of charge separated products at any pH in the range 2.8-9.0. It is proposed that the differences in the radical pair kinetics arise from differences in the degree of binding of the ground state complexes formed by the donor and acceptor species.

Theoretical study on the cooperative exciton dissociation process based on dimensional and hot charge-transfer state effects in an organic photocell

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

Shimazaki, Tomomi; Nakajima, Takahito

2016-06-21

This paper discusses the exciton dissociation process at the donor–acceptor interface in organic photocells. In our previous study, we introduced a local temperature to handle the hot charge-transfer (CT) state and calculated the exciton dissociation probability based on the 1D organic semiconductor model [T. Shimazaki and T. Nakajima, Phys. Chem. Chem. Phys. 17, 12538 (2015)]. Although the hot CT state plays an essential role in exciton dissociations, the probabilities calculated are not high enough to efficiently separate bound electron–hole pairs. This paper focuses on the dimensional (entropy) effect together with the hot CT state effect and shows that cooperative behaviormore » between both effects can improve the exciton dissociation process. In addition, we discuss cooperative effects with site-disorders and external-electric-fields.« less

Twenty-First Century Research Needs in Electrostatic Processes Applied to Industry and Medicine

NASA Technical Reports Server (NTRS)

Mazumder, M. K.; Sims, R. A.; Biris, A. S.; Srirama, P. K.; Saini, D.; Yurteri, C. U.; Trigwell, S.; De, S.; Sharma, R.

2005-01-01

From the early century Nobel Prize winning (1923) experiments with charged oil droplets, resulting in the discovery of the elementary electronic charge by Robert Millikan, to the early 21st century Nobel Prize (2002) awarded to John Fenn for his invention of electrospray ionization mass spectroscopy and its applications to proteomics, electrostatic processes have been successfully applied to many areas of industry and medicine. Generation, transport, deposition, separation, analysis, and control of charged particles involved in the four states of matter: solid, liquid, gas, and plasma are of interest in many industrial and biomedical processes. In this paper, we briefly discuss some of the applications and research needs involving charged particles in industrial and medical applications including: (1) Generation and deposition of unipolarly charged dry powder without the presence of ions or excessive ozone, (2) Control of tribocharging process for consistent and reliable charging, (3) Thin film (less than 25 micrometers) powder coating and Powder coating on insulative surfaces, (4) Fluidization and dispersion of fine powders, (5) Mitigation of Mars dust, (6) Effect of particle charge on the lung deposition of inhaled medical aerosols, (7) Nanoparticle deposition, and (8) Plasma/Corona discharge processes. A brief discussion on the measurements of charged particles and suggestions for research needs are also included.

Influence of natural organic matter on equilibrium adsorption of neutral and charged pharmaceuticals onto activated carbon.

PubMed

de Ridder, D J; Verliefde, A R D; Heijman, S G J; Verberk, J Q J C; Rietveld, L C; van der Aa, L T J; Amy, G L; van Dijk, J C

2011-01-01

Natural organic matter (NOM) can influence pharmaceutical adsorption onto granular activated carbon (GAC) by direct adsorption competition and pore blocking. However, in the literature there is limited information on which of these mechanisms is more important and how this is related to NOM and pharmaceutical properties. Adsorption batch experiments were carried out in ultrapure, waste- and surface water and fresh and NOM preloaded GAC was used. Twenty-one pharmaceuticals were selected with varying hydrophobicity and with neutral, negative or positive charge. The influence of NOM competition and pore blocking could not be separated. However, while reduction in surface area was similar for both preloaded GACs, up to 50% lower pharmaceutical removal was observed on wastewater preloaded GAC. This was attributed to higher hydrophobicity of wastewater NOM, indicating that NOM competition may influence pharmaceutical removal more than pore blocking. Preloaded GAC was negatively charged, which influenced removal of charged pharmaceuticals significantly. At a GAC dose of 6.7 mg/L, negatively charged pharmaceuticals were removed for 0-58%, while removal of positively charged pharmaceuticals was between 32-98%. Charge effects were more pronounced in ultrapure water, as it contained no ions to shield the surface charge. Solutes with higher log D could compete better with NOM, resulting in higher removal.

Electron beam induced strong organic/inorganic grafting for thermally stable lithium-ion battery separators

NASA Astrophysics Data System (ADS)

Choi, Yunah; Kim, Jin Il; Moon, Jungjin; Jeong, Jongyeob; Park, Jong Hyeok

2018-06-01

A tailored interface between organic and inorganic materials is of great importance to maximize the synergistic effects from hybridization. Polyethylene separators over-coated with inorganic thin films are the state-of-the art technology for preparing various secondary batteries with high safety. Unfortunately, the organic/inorganic hybrid separators have the drawback of a non-ideal interface, thus causing poor thermal/dimensional stability. Here, we report a straightforward method to resolve the drawback of the non-ideal interface between vapor deposited SiO2 and polyethylene separators, to produce a highly stable lithium-ion battery separator through strong chemical linking generated by direct electron beam irradiation. The simple treatment with an electron beam with an optimized dose generates thermally stable polymer separators, which may enhance battery safety under high-temperature conditions. Additionally, the newly formed Si-O-C or Si-CH3 chemical bonding enhances electrolyte-separator compatibility and thus may provide a better environment for ionic transport between the cathode and anode, thereby leading to better charge/discharge behaviors.

Efficient Solar-Induced Photoelectrochemical Response Using Coupling Semiconductor TiO2-ZnO Nanorod Film

PubMed Central

Abd Samad, Nur Azimah; Lai, Chin Wei; Lau, Kung Shiuh; Abd Hamid, Sharifah Bee

2016-01-01

Efficient solar driven photoelectrochemical (PEC) response by enhancing charge separation has attracted great interest in the hydrogen generation application. The formation of one-dimensional ZnO nanorod structure without bundling is essential for high efficiency in PEC response. In this present research work, ZnO nanorod with an average 500 nm in length and average diameter of about 75 nm was successfully formed via electrodeposition method in 0.05 mM ZnCl2 and 0.1 M KCl electrolyte at 1 V for 60 min under 70 °C condition. Continuous efforts have been exerted to further improve the solar driven PEC response by incorporating an optimum content of TiO2 into ZnO nanorod using dip-coating technique. It was found that 0.25 at % of TiO2 loaded on ZnO nanorod film demonstrated a maximum photocurrent density of 19.78 mA/cm2 (with V vs. Ag/AgCl) under UV illumination and 14.75 mA/cm2 (with V vs. Ag/AgCl) under solar illumination with photoconversion efficiency ~2.9% (UV illumination) and ~4.3% (solar illumination). This performance was approximately 3–4 times higher than ZnO film itself. An enhancement of photocurrent density and photoconversion efficiency occurred due to the sufficient Ti element within TiO2-ZnO nanorod film, which acted as an effective mediator to trap the photo-induced electrons and minimize the recombination of charge carriers. Besides, phenomenon of charge-separation effect at type-II band alignment of Zn and Ti could further enhance the charge carrier transportation during illumination. PMID:28774068

Charge-dependent azimuthal correlations in pPb collisions with CMS experiment

NASA Astrophysics Data System (ADS)

Tu, Zhoudunming; CMS Collaboration

2017-11-01

Charge-dependent azimuthal correlations relative to the event plane in AA collisions have been suggested as providing evidence for the chiral magnetic effect (CME) caused by local strong parity violation. However, the observation of the CME remains inconclusive because of several possible sources of background correlations that may account for part or all of the observed signals. This talk will present the first application of three-particle, charge-dependent azimuthal correlation analysis in proton-nucleus collisions, using pPb data collected with the CMS experiment at the LHC at √{sNN} = 5.02 TeV. The differences found in comparing same and opposite sign correlations are studied as a function of event multiplicity and the pseudorapidity gap between two of the particles detected in the CMS tracker detector. After selecting events with comparable charge-particle multiplicities, the results for pPb collisions are found to be similar to those for PbPb collisions collected at the same collision energy. With a reduced magnetic field strength and a random field orientation in high multiplicity pPb events, the CME contribution to any charge separation signal is expected to be much smaller than found in peripheral PbPb events. These results pose a challenge for the interpretation of charge-dependent azimuthal correlations in heavy ion collisions in terms of the chiral magnetic effect.

Theory of linear sweep voltammetry with diffuse charge: Unsupported electrolytes, thin films, and leaky membranes

NASA Astrophysics Data System (ADS)

Yan, David; Bazant, Martin Z.; Biesheuvel, P. M.; Pugh, Mary C.; Dawson, Francis P.

2017-03-01

Linear sweep and cyclic voltammetry techniques are important tools for electrochemists and have a variety of applications in engineering. Voltammetry has classically been treated with the Randles-Sevcik equation, which assumes an electroneutral supported electrolyte. In this paper, we provide a comprehensive mathematical theory of voltammetry in electrochemical cells with unsupported electrolytes and for other situations where diffuse charge effects play a role, and present analytical and simulated solutions of the time-dependent Poisson-Nernst-Planck equations with generalized Frumkin-Butler-Volmer boundary conditions for a 1:1 electrolyte and a simple reaction. Using these solutions, we construct theoretical and simulated current-voltage curves for liquid and solid thin films, membranes with fixed background charge, and cells with blocking electrodes. The full range of dimensionless parameters is considered, including the dimensionless Debye screening length (scaled to the electrode separation), Damkohler number (ratio of characteristic diffusion and reaction times), and dimensionless sweep rate (scaled to the thermal voltage per diffusion time). The analysis focuses on the coupling of Faradaic reactions and diffuse charge dynamics, although capacitive charging of the electrical double layers is also studied, for early time transients at reactive electrodes and for nonreactive blocking electrodes. Our work highlights cases where diffuse charge effects are important in the context of voltammetry, and illustrates which regimes can be approximated using simple analytical expressions and which require more careful consideration.

47 CFR 69.121 - Connection charges for expanded interconnection.

Code of Federal Regulations, 2010 CFR

2010-10-01

... separations. (2) Charges for subelements associated with physical collocation or virtual collocation, other... of the virtual collocation equipment described in § 64.1401(e)(1) of this chapter, may reasonably...

77 FR 19425 - Prescription Drugs Not Administered During Treatment; Update to Administrative Cost for Calendar...

Federal Register 2010, 2011, 2012, 2013, 2014

2012-03-30

... that requires automobile accident reparations insurance. This updated administrative cost charge was... automobile accident reparations insurance, ``charges billed separately for such prescription drugs will...

Charging YOYO-1 on Capillary Wall for Online DNA Intercalation and Integrating This Approach with Multiplex PCR and Bare Narrow Capillary–Hydrodynamic Chromatography for Online DNA Analysis

PubMed Central

2016-01-01

Multiplex polymerase chain reaction (PCR) has been widely utilized for high-throughput pathogen identification. Often, a dye is used to intercalate the amplified DNA fragments, and identifications of the pathogens are carried out by DNA melting curve analysis or gel electrophoresis. Integrating DNA amplification and identification is a logic path toward maximizing the benefit of multiplex PCR. Although PCR and gel electrophoresis have been integrated, replenishing the gels after each run is tedious and time-consuming. In this technical note, we develop an approach to address this issue. We perform multiplex PCR inside a capillary, transfer the amplified fragments to a bare narrow capillary, and measure their lengths online using bare narrow capillary–hydrodynamic chromatography (BaNC-HDC), a new technique recently developed in our laboratory for free-solution DNA separation. To intercalate the DNA with YOYO-1 (a fluorescent dye) for BaNC-HDC, we flush the capillary column with a YOYO-1 solution; positively charged YOYO-1 is adsorbed (or charged) onto the negatively charged capillary wall. As DNA molecules are driven down the column for separation, they react with the YOYO-1 stored on the capillary wall and are online-intercalated with the dye. With a single YOYO-1 charging, the column can be used for more than 40 runs, although the fluorescence signal intensities of the DNA peaks decrease gradually. Although the dye-DNA intercalation occurs during the separation, it does not affect the retention times, separation efficiencies, or resolutions. PMID:25555111

Pentachlorophenol removal from water using surfactant-enhanced filtration through low-pressure thin film composite membranes.

PubMed

Kumar, Yogesh; Popat, K M; Brahmbhatt, H; Ganguly, B; Bhattacharya, A

2008-06-15

Removal of pentachlorophenol from water is investigated using the surfactant-enhanced cross-flow membrane filtration technique in which anionic surfactant; sodium dodecyl sulfate (SDS) is the carrier of pentachlorophenol. The separation performances are studied by varying SDS concentrations (

Numerical Simulations of Plasma Based Flow Control Applications

NASA Technical Reports Server (NTRS)

Suzen, Y. B.; Huang, P. G.; Jacob, J. D.; Ashpis, D. E.

2005-01-01

A mathematical model was developed to simulate flow control applications using plasma actuators. The effects of the plasma actuators on the external flow are incorporated into Navier Stokes computations as a body force vector. In order to compute this body force vector, the model solves two additional equations: one for the electric field due to the applied AC voltage at the electrodes and the other for the charge density representing the ionized air. The model is calibrated against an experiment having plasma-driven flow in a quiescent environment and is then applied to simulate a low pressure turbine flow with large flow separation. The effects of the plasma actuator on control of flow separation are demonstrated numerically.

A Mussel-Derived One-Component Adhesive Coacervate

PubMed Central

Wei, Wei; Tan, Yerpeng; Rodriguez, N. Martinez; Yu, Jing; Israelachvili, Jacob N.; Waite, J. Herbert

2013-01-01

Marine organisms process and deliver many of their underwater coatings and adhesives as complex fluids. In marine mussels, one such fluid, secreted during the formation of adhesive plaques, consists of a concentrated colloidal suspension of a mussel foot protein (mfp) known as Mfp-3S. Results of this study suggest that Mfp-3S becomes a complex fluid by a liquid-liquid phase separation from equilibrium solution at a pH and ionic strength reminiscent of conditions created by the mussel foot during plaque formation. The pH dependence of phase separation and its sensitivity indicate that inter/intra-molecular electrostatic interactions are partially responsible for driving the phase separation. Hydrophobic interactions between the nonpolar Mfp-3S proteins provide another important driving force for coacervation. As complex coacervation typically results from charge-charge interactions between polyanions and polycations, Mfp-3S is thus unique in being the only known protein that coacervates with itself. The Mfp-3S coacervate was shown to have an effective interfacial energy of ≤ 1 mJ/m2 which explains its tendency to spread over or engulf most surfaces. Of particular interest to biomedical applications is the extremely high adsorption capacity of coacervated Mfp-3S on hydroxyapatite. PMID:24060881

The electrification of stratiform anvils

NASA Astrophysics Data System (ADS)

Boccippio, Dennis J.

1997-10-01

Stratiform precipitation regions accompany convective activity on many spatial scales. The electrification of these regions is anomalous in a number of ways. Surface and above-cloud fields are often 'inverted' from normal thunderstorm conditions. Unusually large, bright, horizontal 'spider' lightning and high current and charge transfer positive cloud-to-ground (CC) lightning dominates in these regions. Mesospheric 'red sprite' emissions have to date been observed exclusively over stratiform cloud shields. We postulate that a dominant 'inverted dipole' charge structure may account for this anomalous electrification. This is based upon laboratory observations of charge separation which show that in low liquid water content (LWC) environments, or dry but ice- supersaturated environments, precipitation ice tends to charge positively (instead of negatively) upon collision with smaller crystals. Under typical stratiform cloud conditions, liquid water should be depleted and this charging regime favored. An inverted dipole would be the natural consequence of large-scale charge separation (net flux divergence of charged ice), given typical hydrometeor profiles. The inverted dipole hypothesis is tested using radar and electrical observations of four weakly organized, late- stage systems in Orlando, Albuquerque and the Western Pacific. Time-evolving, area-average vertical velocity profiles are inferred from single Doppler radar data. These profiles provide the forcing for a 1-D steady state micro-physical retrieval, which yields vertical hydrometeor profiles and ice/water saturation conditions. The retrieved microphysical parameters are then combined with laboratory charge transfer measurements to infer the instantaneous charging behavior of the systems. Despite limitations in the analysis technique, the retrievals yield useful results. Total charge transfer drops only modestly as the storm enters the late (stratiform) stage, suggesting a continued active generator is plausible. Generator currents show an enhanced lowermost inverted dipole charging structure, which we may infer will result in a comparable inverted dipole charge structure, consistent with surface, in-situ and remote observations. Fine-scale vertical variations in ice and liquid water content may yield multipolar generator current profiles, despite unipolar charge transfer regimes. This suggests that multipoles observed in balloon soundings may not necessarily conflict with the simple ice-ice collisional charge separation mechanism. Overall, the results are consistent with, but not proof of, the inverted dipole model. (Copies available exclusively from MIT Libraries, Rm. 14-0551, Cambridge, MA 02139-4307. Ph. 617-253-5668; Fax 617-253- 1690.)

Modeling the Electric Potential and Surface Charge Density Near Charged Thunderclouds

NASA Astrophysics Data System (ADS)

Neel, Matthew Stephen

2018-03-01

Thundercloud charge separation, or the process by which the bottom portion of a cloud gathers charge and the top portion of the cloud gathers the opposite charge, is still not thoroughly understood. Whatever the mechanism, though, a charge separation definitely exists and can lead to electrostatic discharge via cloud-to-cloud lightning and cloud-to-ground lightning. We wish to examine the latter form, in which upward leaders from Earth connect with downward leaders from the cloud to form a plasma channel and produce lightning. Much of the literature indicates that the lower part of a thundercloud becomes negatively charged while the upper part becomes positively charged via convective charging, although the opposite polarity can certainly exist along with various, complex intra-cloud currents. It is estimated that >90% of cloud-to-ground lightning is "negative lightning," or the flow of charges from the bottom of the cloud, while the remaining <10% of lightning strikes is "positive lightning," or the flow of charges from the top of the cloud. We wish to understand the electric potential surrounding charged thunderclouds as well as the resulting charge density on the surface of Earth below them. In this paper we construct a simple and adaptable model that captures the very basic features of the cloud/ground system and that exhibits conditions favorable for both forms of lightning. In this way, we provide a practical application of electrostatic dipole physics as well as the method of images that can serve as a starting point for further modeling and analysis by students.

Non-Faradaic Li + Migration and Chemical Coordination across Solid-State Battery Interfaces

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

Gittleson, Forrest S.; El Gabaly, Farid

Efficient and reversible charge transfer is essential to realizing high-performance solid-state batteries. Efforts to enhance charge transfer at critical electrode–electrolyte interfaces have proven successful, yet interfacial chemistry and its impact on cell function remains poorly understood. Using X-ray photoelectron spectroscopy combined with electrochemical techniques, we elucidate chemical coordination near the LiCoO 2–LIPON interface, providing experimental validation of space-charge separation. Space-charge layers, defined by local enrichment and depletion of charges, have previously been theorized and modeled, but the unique chemistry of solid-state battery interfaces is now revealed. Here we highlight the non-Faradaic migration of Li+ ions from the electrode to themore » electrolyte, which reduces reversible cathodic capacity by ~15%. Inserting a thin, ion-conducting LiNbO 3 interlayer between the electrode and electrolyte, however, can reduce space-charge separation, mitigate the loss of Li+ from LiCoO 2, and return cathodic capacity to its theoretical value. This work illustrates the importance of interfacial chemistry in understanding and improving solid-state batteries.« less

5 CFR 842.404 - Reductions in basic annuity.

Code of Federal Regulations, 2010 CFR

2010-01-01

... by removal for cause on charges of misconduct or delinquency; (2) A firefighter and/or law enforcement officer, except one separated by removal for cause on charges of misconduct of delinquency; or (3...

Excellent photocatalytic hydrogen production over CdS nanorods via using noble metal-free copper molybdenum sulfide (Cu2MoS4) nanosheets as co-catalysts

NASA Astrophysics Data System (ADS)

Hong, Sangyeob; Kumar, D. Praveen; Reddy, D. Amaranatha; Choi, Jiha; Kim, Tae Kyu

2017-02-01

Charge carrier recombination and durability issues are major problems in photocatalytic hydrogen (H2) evolution processes. Thus, there is a very important necessitate to extend an efficient photocatalyst to control charge-carrier dynamics in the photocatalytic system. We have developed copper molybdenum sulfide (Cu2MoS4) nanosheets as co-catalysts with CdS nanorods for controlling charge carriers without recombination for use in photocatalytic H2 evolution under simulated solar light irradiation. Effective control and utilization of charge carriers are possible by loading Cu2MoS4 nanosheets onto the CdS nanorods. The loading compensates for the restrictions of CdS, and stimulated synergistic effects, such as efficient photoexcited charge separation, lead to an improvement in photostability because of the layered structure of the Cu2MoS4nanosheets. These layered Cu2MoS4 nanosheets have emerged as novel and active replacements for precious noble metal co-catalysts in photocatalytic H2 production by water splitting. We have obtained superior H2 production rates by using Cu2MoS4 loaded CdS nanorods. The physicochemical properties of the composites are analyzed by diverse characterization techniques.

Stick slip, charge separation and decay

USGS Publications Warehouse

Lockner, D.A.; Byerlee, J.D.; Kuksenko, V.S.; Ponomarev, A.V.

1986-01-01

Measurements of charge separation in rock during stable and unstable deformation give unexpectedly large decay times of 50 sec. Time-domain induced polarization experiments on wet and dry rocks give similar decay times and suggest that the same decay mechanisms operate in the induced polarization response as in the relaxation of charge generated by mechanical deformation. These large decay times are attributed to electrochemical processes in the rocks, and they require low-frequency relative permittivity to be very large, in excess of 105. One consequence of large permittivity, and therefore long decay times, is that a significant portion of any electrical charge generated during an earthquake can persist for tens or hundreds of seconds. As a result, electrical disturbances associated with earthquakes should be observable for these lengths of time rather than for the milliseconds previously suggested. ?? 1986 Birka??user Verlag.

Efficient charge-carrier extraction from Ag₂S quantum dots prepared by the SILAR method for utilization of multiple exciton generation.

PubMed

Zhang, Xiaoliang; Liu, Jianhua; Johansson, Erik M J

2015-01-28

The utilization of electron-hole pairs (EHPs) generated from multiple excitons in quantum dots (QDs) is of great interest toward efficient photovoltaic devices and other optoelectronic devices; however, extraction of charge carriers remains difficult. Herein, we extract photocharges from Ag2S QDs and investigate the dependence of the electric field on the extraction of charges from multiple exciton generation (MEG). Low toxic Ag2S QDs are directly grown on TiO2 mesoporous substrates by employing the successive ionic layer adsorption and reaction (SILAR) method. The contact between QDs is important for the initial charge separation after MEG and for the carrier transport, and the space between neighbor QDs decreases with more SILAR cycles, resulting in better charge extraction. At the optimal electric field for extraction of photocharges, the results suggest that the threshold energy (hνth) for MEG is 2.41Eg. The results reveal that Ag2S QD is a promising material for efficient extraction of charges from MEG and that QDs prepared by SILAR have an advantageous electrical contact facilitating charge separation and extraction.

An exploration into municipal waste charges for environmental management at local level: The case of Spain.

PubMed

Puig-Ventosa, Ignasi; Sastre Sanz, Sergio

2017-11-01

Municipal waste charges have been widely acknowledged as a crucial tool for waste management at the local level. This is because they contribute to financing the costly provision of waste collection and treatment services and they can be designed to provide an economic stimulus to encourage citizens and local businesses to improve separate collection and recycling. This work presents a methodology to evaluate a sample of 125 municipal waste charges in Spain for the year 2015, covering 33.91% of the Spanish population. The qualitative benchmarking of municipal waste charges shows that flat fees are frequent, whereas variable fees are set according to criteria that are weakly related to waste generation. The average fee per household is €82.2 per year, which does not provide full cost recovery. The current configuration of municipal waste charges penalises taxpayers contributing to source separation of waste, while subsidising less environmentally friendly behaviours. In this sense, municipal waste charges in Spain are far from applying the polluter pays principle. Furthermore, it is argued that municipal waste charges are ineffective for promoting the proper application of the so-called 'waste hierarchy'.

An improved model for computing the trajectories of conductive particles in roll-type electrostatic separator for recycling metals from WEEE.

PubMed

Wu, Jiang; Li, Jia; Xu, Zhenming

2009-08-15

Electrostatic separation presents an effective and environmentally friendly way for recycling metals and nonmetals from ground waste electrical and electronic equipment (WEEE). For this process, the trajectory of conductive particle is significant and some models have been established. However, the results of previous researches are limited by some simplifying assumptions and lead to a notable discrepancy between the model prediction and the experimental results. In the present research, a roll-type corona-electrostatic separator and ground printed circuit board (PCB) wastes were used to investigate the trajectory of the conductive particle. Two factors, the air drag force and the different charging situation, were introduced into the improved model. Their effects were analyzed and an improved model for the theoretical trajectory of conductive particle was established. Compared with the previous one, the improved model shows a good agreement with the experimental results. It provides a positive guidance for designing of separator and makes a progress for recycling the metals and nonmetals from WEEE.

Single-hole spectral function and spin-charge separation in the t-J model

NASA Astrophysics Data System (ADS)

Mishchenko, A. S.; Prokof'ev, N. V.; Svistunov, B. V.

2001-07-01

Worm algorithm Monte Carlo simulations of the hole Green function with subsequent spectral analysis were performed for 0.1<=J/t<=0.4 on lattices with up to L×L=32×32 sites at a temperature as low as T=J/40, and present, apparently, the hole spectral function in the thermodynamic limit. Spectral analysis reveals a δ-function-sharp quasiparticle peak at the lower edge of the spectrum that is incompatible with the power-law singularity and thus rules out the possibility of spin-charge separation in this parameter range. Spectral continuum features two peaks separated by a gap ~4÷5 t.

Charge recombination in organic photovoltaic devices with high open-circuit voltages.

PubMed

Westenhoff, Sebastian; Howard, Ian A; Hodgkiss, Justin M; Kirov, Kiril R; Bronstein, Hugo A; Williams, Charlotte K; Greenham, Neil C; Friend, Richard H

2008-10-15

A detailed charge recombination mechanism is presented for organic photovoltaic devices with a high open-circuit voltage. In a binary blend comprised of polyfluorene copolymers, the performance-limiting process is found to be the efficient recombination of tightly bound charge pairs into neutral triplet excitons. We arrive at this conclusion using optical transient absorption (TA) spectroscopy with visible and IR probes and over seven decades of time resolution. By resolving the polarization of the TA signal, we track the movement of polaronic states generated at the heterojunction not only in time but also in space. It is found that the photogenerated charge pairs are remarkably immobile at the heterojunction during their lifetime. The charge pairs are shown to be subject to efficient intersystem crossing and terminally recombine into F8BT triplet excitons within approximately 40 ns. Long-range charge separation competes rather unfavorably with intersystem crossing--75% of all charge pairs decay into triplet excitons. Triplet exciton states are thermodynamically accessible in polymer solar cells with high open circuit voltage, and we therefore suggest this loss mechanism to be general. We discuss guidelines for the design of the next generation of organic photovoltaic materials where separating the metastable interfacial charge pairs within approximately 40 ns is paramount.

How to harvest solar energy with the photosynthetic reaction center

NASA Astrophysics Data System (ADS)

Balaeff, Alexander; Reyes, Justin

Photosynthetic reaction center (PRC) is a protein complex that performs a key step in photosynthesis: the electron-hole separation driven by photon absorbtion. The PRC has a great promise for applications in solar energy harvesting and photosensing. Such applications, however, are hampered by the difficulty in extracting the photogenerated electric charge from the PRC. To that end, it was proposed to attach the PRC to a molecular wire through which the charge could be collected. In order to find the attachment point for the wire that would maximize the rate of charge outflow from the PRC, we performed a computational study of the PRC from the R. virdis bacterium. An ensemble of PRC structures generated by a molecular dynamics simulation was used to calculate the rate of charge transport from the site of initial charge separation to several trial sites on the protein surface. The Pathways model was used to calculate the charge transfer rate in each step of the network of heme co-factors through which the charge transport was presumed to proceed. A simple kinetic model was then used to determine the overall rate of the multistep charge transport. The calculations revealed several candidate sites for the molecular wire attachment, recommended for experimental verification.

Explicit symplectic algorithms based on generating functions for charged particle dynamics.

PubMed

Zhang, Ruili; Qin, Hong; Tang, Yifa; Liu, Jian; He, Yang; Xiao, Jianyuan

2016-07-01

Dynamics of a charged particle in the canonical coordinates is a Hamiltonian system, and the well-known symplectic algorithm has been regarded as the de facto method for numerical integration of Hamiltonian systems due to its long-term accuracy and fidelity. For long-term simulations with high efficiency, explicit symplectic algorithms are desirable. However, it is generally believed that explicit symplectic algorithms are only available for sum-separable Hamiltonians, and this restriction limits the application of explicit symplectic algorithms to charged particle dynamics. To overcome this difficulty, we combine the familiar sum-split method and a generating function method to construct second- and third-order explicit symplectic algorithms for dynamics of charged particle. The generating function method is designed to generate explicit symplectic algorithms for product-separable Hamiltonian with form of H(x,p)=p_{i}f(x) or H(x,p)=x_{i}g(p). Applied to the simulations of charged particle dynamics, the explicit symplectic algorithms based on generating functions demonstrate superiorities in conservation and efficiency.

Explicit symplectic algorithms based on generating functions for charged particle dynamics

NASA Astrophysics Data System (ADS)

Zhang, Ruili; Qin, Hong; Tang, Yifa; Liu, Jian; He, Yang; Xiao, Jianyuan

2016-07-01

Dynamics of a charged particle in the canonical coordinates is a Hamiltonian system, and the well-known symplectic algorithm has been regarded as the de facto method for numerical integration of Hamiltonian systems due to its long-term accuracy and fidelity. For long-term simulations with high efficiency, explicit symplectic algorithms are desirable. However, it is generally believed that explicit symplectic algorithms are only available for sum-separable Hamiltonians, and this restriction limits the application of explicit symplectic algorithms to charged particle dynamics. To overcome this difficulty, we combine the familiar sum-split method and a generating function method to construct second- and third-order explicit symplectic algorithms for dynamics of charged particle. The generating function method is designed to generate explicit symplectic algorithms for product-separable Hamiltonian with form of H (x ,p ) =pif (x ) or H (x ,p ) =xig (p ) . Applied to the simulations of charged particle dynamics, the explicit symplectic algorithms based on generating functions demonstrate superiorities in conservation and efficiency.

Plasmonic Landau damping in active environments

NASA Astrophysics Data System (ADS)

Thakkar, Niket; Montoni, Nicholas P.; Cherqui, Charles; Masiello, David J.

2018-03-01

Optical manipulation of charge on the nanoscale is of fundamental importance to an array of proposed technologies from selective photocatalysis to nanophotonics. Open plasmonic systems where collective electron oscillations release energy and charge to their environments offer a potential means to this end as plasmons can rapidly decay into energetic electron-hole pairs; however, isolating this decay from other plasmon-environment interactions remains a challenge. Here we present an analytic theory of noble-metal nanoparticles that quantitatively models plasmon decay into electron-hole pairs, demonstrates that this decay depends significantly on the nanoparticle's dielectric environment, and disentangles this effect from competing decay pathways. Using our approach to incorporate embedding material and substrate effects on plasmon-electron interaction, we show that predictions from the model agree with four separate experiments. Finally, examination of coupled nanoparticle-emitter systems further shows that the hybridized in-phase mode more efficiently decays to photons whereas the out-of-phase mode more efficiently decays to electron-hole pairs, offering a strategy to tailor open plasmonic systems for charge manipulation.

Molecular orbital evaluation of charge flow dynamics in natural pigments based photosensitizers.

PubMed

Heera, Thekinneydath Rajan; Cindrella, Louis

2010-03-01

The relationship between structure and photo electrochemical property of ten natural pigments from plants, insects and microbes has been analyzed using density functional theory (DFT) at the B3LYP/6-31G(d) level. The essential parameters for their photoelectrochemical behaviour such as ground state geometries, electronic transition energies and oxidation potentials are computed. The attachment tendency of the anchoring groups, expressed as the deprotonation order, is determined by calculating the proton affinities at different sites of the molecules. A thorough analysis of the charge flow dynamics in the molecular orbitals (HOMO and LUMO) of these molecules has been carried out and presented to emphasize the role of these orbitals in effective charge separation, the important feature of photosensitizers for DSSC. This study highlights that the flexible spatial orientation provided by the bridging aliphatic unsaturation favours the oscillator strength and the hydroxyl anchor group attached to the ring of delocalized pi electron cloud acts as the effective anchor.

Tuning Light Emission of a Pressure-Sensitive Silicon/ZnO Nanowires Heterostructure Matrix through Piezo-phototronic Effects.

PubMed

Chen, Mengxiao; Pan, Caofeng; Zhang, Taiping; Li, Xiaoyi; Liang, Renrong; Wang, Zhong Lin

2016-06-28

Based on white light emission at silicon (Si)/ZnO hetrerojunction, a pressure-sensitive Si/ZnO nanowires heterostructure matrix light emitting diode (LED) array is developed. The light emission intensity of a single heterostructure LED is tuned by external strain: when the applied stress keeps increasing, the emission intensity first increases and then decreases with a maximum value at a compressive strain of 0.15-0.2%. This result is attributed to the piezo-phototronic effect, which can efficiently modulate the LED emission intensity by utilizing the strain-induced piezo-polarization charges. It could tune the energy band diagrams at the junction area and regulate the optoelectronic processes such as charge carriers generation, separation, recombination, and transport. This study achieves tuning silicon based devices through piezo-phototronic effect.

Constraints on the chiral magnetic effect using charge-dependent azimuthal correlations in p Pb and PbPb collisions at the CERN Large Hadron Collider

NASA Astrophysics Data System (ADS)

Sirunyan, A. M.; Tumasyan, A.; Adam, W.; Ambrogi, F.; Asilar, E.; Bergauer, T.; Brandstetter, J.; Brondolin, E.; Dragicevic, M.; Erö, J.; Flechl, M.; Friedl, M.; Frühwirth, R.; Ghete, V. M.; Grossmann, J.; Hrubec, J.; Jeitler, M.; König, A.; Krammer, N.; Krätschmer, I.; Liko, D.; Madlener, T.; Mikulec, I.; Pree, E.; Rad, N.; Rohringer, H.; Schieck, J.; Schöfbeck, R.; Spanring, M.; Spitzbart, D.; Waltenberger, W.; Wittmann, J.; Wulz, C.-E.; Zarucki, M.; Chekhovsky, V.; Mossolov, V.; Suarez Gonzalez, J.; De Wolf, E. A.; Di Croce, D.; Janssen, X.; Lauwers, J.; Van Haevermaet, H.; Van Mechelen, P.; Van Remortel, N.; Abu Zeid, S.; Blekman, F.; D'Hondt, J.; De Bruyn, I.; De Clercq, J.; Deroover, K.; Flouris, G.; Lontkovskyi, D.; Lowette, S.; Moortgat, S.; Moreels, L.; Python, Q.; Skovpen, K.; Tavernier, S.; Van Doninck, W.; Van Mulders, P.; Van Parijs, I.; Beghin, D.; Brun, H.; Clerbaux, B.; De Lentdecker, G.; Delannoy, H.; Dorney, B.; Fasanella, G.; Favart, L.; Goldouzian, R.; Grebenyuk, A.; Karapostoli, G.; Lenzi, T.; Luetic, J.; Maerschalk, T.; Marinov, A.; Randle-conde, A.; Seva, T.; Starling, E.; Vander Velde, C.; Vanlaer, P.; Vannerom, D.; Yonamine, R.; Zenoni, F.; Zhang, F.; Cimmino, A.; Cornelis, T.; Dobur, D.; Fagot, A.; Gul, M.; Khvastunov, I.; Poyraz, D.; Roskas, C.; Salva, S.; Tytgat, M.; Verbeke, W.; Zaganidis, N.; Bakhshiansohi, H.; Bondu, O.; Brochet, S.; Bruno, G.; Caputo, C.; Caudron, A.; David, P.; De Visscher, S.; Delaere, C.; Delcourt, M.; Francois, B.; Giammanco, A.; Komm, M.; Krintiras, G.; Lemaitre, V.; Magitteri, A.; Mertens, A.; Musich, M.; Piotrzkowski, K.; Quertenmont, L.; Saggio, A.; Vidal Marono, M.; Wertz, S.; Zobec, J.; Beliy, N.; Aldá Júnior, W. L.; Alves, F. L.; Alves, G. A.; Brito, L.; Correa Martins Junior, M.; Hensel, C.; Moraes, A.; Pol, M. E.; Rebello Teles, P.; Belchior Batista Das Chagas, E.; Carvalho, W.; Chinellato, J.; Coelho, E.; Da Costa, E. M.; Da Silveira, G. G.; De Jesus Damiao, D.; Fonseca De Souza, S.; Huertas Guativa, L. M.; Malbouisson, H.; Melo De Almeida, M.; Mora Herrera, C.; Mundim, L.; Nogima, H.; Sanchez Rosas, L. J.; Santoro, A.; Sznajder, A.; Thiel, M.; Tonelli Manganote, E. J.; Torres Da Silva De Araujo, F.; Vilela Pereira, A.; Ahuja, S.; Bernardes, C. A.; Tomei, T. R. Fernandez Perez; Gregores, E. M.; Mercadante, P. G.; Novaes, S. F.; Padula, Sandra S.; Romero Abad, D.; Ruiz Vargas, J. C.; Aleksandrov, A.; Hadjiiska, R.; Iaydjiev, P.; Misheva, M.; Rodozov, M.; Shopova, M.; Sultanov, G.; Dimitrov, A.; Glushkov, I.; Litov, L.; Pavlov, B.; Petkov, P.; Fang, W.; Gao, X.; Yuan, L.; Ahmad, M.; Bian, J. G.; Chen, G. M.; Chen, H. S.; Chen, M.; Chen, Y.; Jiang, C. H.; Leggat, D.; Liao, H.; Liu, Z.; Romeo, F.; Shaheen, S. M.; Spiezia, A.; Tao, J.; Wang, C.; Wang, Z.; Yazgan, E.; Zhang, H.; Zhang, S.; Zhao, J.; Ban, Y.; Chen, G.; Li, Q.; Liu, S.; Mao, Y.; Qian, S. J.; Wang, D.; Xu, Z.; Avila, C.; Cabrera, A.; Chaparro Sierra, L. F.; Florez, C.; González Hernández, C. F.; Ruiz Alvarez, J. D.; Courbon, B.; Godinovic, N.; Lelas, D.; Puljak, I.; Ribeiro Cipriano, P. M.; Sculac, T.; Antunovic, Z.; Kovac, M.; Brigljevic, V.; Ferencek, D.; Kadija, K.; Mesic, B.; Starodumov, A.; Susa, T.; Ather, M. W.; Attikis, A.; Mavromanolakis, G.; Mousa, J.; Nicolaou, C.; Ptochos, F.; Razis, P. A.; Rykaczewski, H.; Finger, M.; Finger, M.; Carrera Jarrin, E.; Assran, Y.; Elgammal, S.; Mahrous, A.; Dewanjee, R. K.; Kadastik, M.; Perrini, L.; Raidal, M.; Tiko, A.; Veelken, C.; Eerola, P.; Kirschenmann, H.; Pekkanen, J.; Voutilainen, M.; Järvinen, T.; Karimäki, V.; Kinnunen, R.; Lampén, T.; Lassila-Perini, K.; Lehti, S.; Lindén, T.; Luukka, P.; Tuominen, E.; Tuominiemi, J.; Talvitie, J.; Tuuva, T.; Besancon, M.; Couderc, F.; Dejardin, M.; Denegri, D.; Faure, J. L.; Ferri, F.; Ganjour, S.; Ghosh, S.; Givernaud, A.; Gras, P.; Hamel de Monchenault, G.; Jarry, P.; Kucher, I.; Leloup, C.; Locci, E.; Machet, M.; Malcles, J.; Negro, G.; Rander, J.; Rosowsky, A.; Sahin, M. Ö.; Titov, M.; Abdulsalam, A.; Amendola, C.; Antropov, I.; Baffioni, S.; Beaudette, F.; Busson, P.; Cadamuro, L.; Charlot, C.; Granier de Cassagnac, R.; Jo, M.; Lisniak, S.; Lobanov, A.; Martin Blanco, J.; Nguyen, M.; Ochando, C.; Ortona, G.; Paganini, P.; Pigard, P.; Salerno, R.; Sauvan, J. B.; Sirois, Y.; Stahl Leiton, A. G.; Strebler, T.; Yilmaz, Y.; Zabi, A.; Zghiche, A.; Agram, J.-L.; Andrea, J.; Bloch, D.; Brom, J.-M.; Buttignol, M.; Chabert, E. C.; Chanon, N.; Collard, C.; Conte, E.; Coubez, X.; Fontaine, J.-C.; Gelé, D.; Goerlach, U.; Jansová, M.; Le Bihan, A.-C.; Tonon, N.; Van Hove, P.; Gadrat, S.; Beauceron, S.; Bernet, C.; Boudoul, G.; Chierici, R.; Contardo, D.; Depasse, P.; El Mamouni, H.; Fay, J.; Finco, L.; Gascon, S.; Gouzevitch, M.; Grenier, G.; Ille, B.; Lagarde, F.; Laktineh, I. B.; Lethuillier, M.; Mirabito, L.; Pequegnot, A. L.; Perries, S.; Popov, A.; Sordini, V.; Vander Donckt, M.; Viret, S.; Khvedelidze, A.; Tsamalaidze, Z.; Autermann, C.; Feld, L.; Kiesel, M. K.; Klein, K.; Lipinski, M.; Preuten, M.; Schomakers, C.; Schulz, J.; Zhukov, V.; Albert, A.; Dietz-Laursonn, E.; Duchardt, D.; Endres, M.; Erdmann, M.; Erdweg, S.; Esch, T.; Fischer, R.; Güth, A.; Hamer, M.; Hebbeker, T.; Heidemann, C.; Hoepfner, K.; Knutzen, S.; Merschmeyer, M.; Meyer, A.; Millet, P.; Mukherjee, S.; Pook, T.; Radziej, M.; Reithler, H.; Rieger, M.; Scheuch, F.; Teyssier, D.; Thüer, S.; Flügge, G.; Kargoll, B.; Kress, T.; Künsken, A.; Müller, T.; Nehrkorn, A.; Nowack, A.; Pistone, C.; Pooth, O.; Stahl, A.; Aldaya Martin, M.; Arndt, T.; Asawatangtrakuldee, C.; Beernaert, K.; Behnke, O.; Behrens, U.; Bermúdez Martínez, A.; Bin Anuar, A. A.; Borras, K.; Botta, V.; Campbell, A.; Connor, P.; Contreras-Campana, C.; Costanza, F.; Diez Pardos, C.; Eckerlin, G.; Eckstein, D.; Eichhorn, T.; Eren, E.; Gallo, E.; Garay Garcia, J.; Geiser, A.; Gizhko, A.; Grados Luyando, J. M.; Grohsjean, A.; Gunnellini, P.; Guthoff, M.; Harb, A.; Hauk, J.; Hempel, M.; Jung, H.; Kalogeropoulos, A.; Kasemann, M.; Keaveney, J.; Kleinwort, C.; Korol, I.; Krücker, D.; Lange, W.; Lelek, A.; Lenz, T.; Leonard, J.; Lipka, K.; Lohmann, W.; Mankel, R.; Melzer-Pellmann, I.-A.; Meyer, A. B.; Mittag, G.; Mnich, J.; Mussgiller, A.; Ntomari, E.; Pitzl, D.; Raspereza, A.; Roland, B.; Savitskyi, M.; Saxena, P.; Shevchenko, R.; Spannagel, S.; Stefaniuk, N.; Van Onsem, G. P.; Walsh, R.; Wen, Y.; Wichmann, K.; Wissing, C.; Zenaiev, O.; Aggleton, R.; Bein, S.; Blobel, V.; Centis Vignali, M.; Dreyer, T.; Garutti, E.; Gonzalez, D.; Haller, J.; Hinzmann, A.; Hoffmann, M.; Karavdina, A.; Klanner, R.; Kogler, R.; Kovalchuk, N.; Kurz, S.; Lapsien, T.; Marchesini, I.; Marconi, D.; Meyer, M.; Niedziela, M.; Nowatschin, D.; Pantaleo, F.; Peiffer, T.; Perieanu, A.; Scharf, C.; Schleper, P.; Schmidt, A.; Schumann, S.; Schwandt, J.; Sonneveld, J.; Stadie, H.; Steinbrück, G.; Stober, F. M.; Stöver, M.; Tholen, H.; Troendle, D.; Usai, E.; Vanelderen, L.; Vanhoefer, A.; Vormwald, B.; Akbiyik, M.; Barth, C.; Baur, S.; Butz, E.; Caspart, R.; Chwalek, T.; Colombo, F.; De Boer, W.; Dierlamm, A.; Freund, B.; Friese, R.; Giffels, M.; Haitz, D.; Harrendorf, M. A.; Hartmann, F.; Heindl, S. M.; Husemann, U.; Kassel, F.; Kudella, S.; Mildner, H.; Mozer, M. U.; Müller, Th.; Plagge, M.; Quast, G.; Rabbertz, K.; Schröder, M.; Shvetsov, I.; Sieber, G.; Simonis, H. J.; Ulrich, R.; Wayand, S.; Weber, M.; Weiler, T.; Williamson, S.; Wöhrmann, C.; Wolf, R.; Anagnostou, G.; Daskalakis, G.; Geralis, T.; Giakoumopoulou, V. A.; Kyriakis, A.; Loukas, D.; Topsis-Giotis, I.; Karathanasis, G.; Kesisoglou, S.; Panagiotou, A.; Saoulidou, N.; Kousouris, K.; Evangelou, I.; Foudas, C.; Kokkas, P.; Mallios, S.; Manthos, N.; Papadopoulos, I.; Paradas, E.; Strologas, J.; Triantis, F. A.; Csanad, M.; Filipovic, N.; Pasztor, G.; Surányi, O.; Veres, G. I.; Bencze, G.; Hajdu, C.; Horvath, D.; Hunyadi, Á.; Sikler, F.; Veszpremi, V.; Zsigmond, A. J.; Beni, N.; Czellar, S.; Karancsi, J.; Makovec, A.; Molnar, J.; Szillasi, Z.; Bartók, M.; Raics, P.; Trocsanyi, Z. L.; Ujvari, B.; Choudhury, S.; Komaragiri, J. R.; Bahinipati, S.; Bhowmik, S.; Mal, P.; Mandal, K.; Nayak, A.; Sahoo, D. K.; Sahoo, N.; Swain, S. K.; Bansal, S.; Beri, S. B.; Bhatnagar, V.; Chawla, R.; Dhingra, N.; Kalsi, A. K.; Kaur, A.; Kaur, M.; Kaur, S.; Kumar, R.; Kumari, P.; Mehta, A.; Singh, J. B.; Walia, G.; Kumar, Ashok; Shah, Aashaq; Bhardwaj, A.; Chauhan, S.; Choudhary, B. C.; Garg, R. B.; Keshri, S.; Kumar, A.; Malhotra, S.; Naimuddin, M.; Ranjan, K.; Sharma, R.; Bhardwaj, R.; Bhattacharya, R.; Bhattacharya, S.; Bhawandeep, U.; Dey, S.; Dutt, S.; Dutta, S.; Ghosh, S.; Majumdar, N.; Modak, A.; Mondal, K.; Mukhopadhyay, S.; Nandan, S.; Purohit, A.; Roy, A.; Roy, D.; Roy Chowdhury, S.; Sarkar, S.; Sharan, M.; Thakur, S.; Behera, P. K.; Chudasama, R.; Dutta, D.; Jha, V.; Kumar, V.; Mohanty, A. K.; Netrakanti, P. K.; Pant, L. M.; Shukla, P.; Topkar, A.; Aziz, T.; Dugad, S.; Mahakud, B.; Mitra, S.; Mohanty, G. B.; Sur, N.; Sutar, B.; Banerjee, S.; Bhattacharya, S.; Chatterjee, S.; Das, P.; Guchait, M.; Jain, Sa.; Kumar, S.; Maity, M.; Majumder, G.; Mazumdar, K.; Sarkar, T.; Wickramage, N.; Chauhan, S.; Dube, S.; Hegde, V.; Kapoor, A.; Kothekar, K.; Pandey, S.; Rane, A.; Sharma, S.; Chenarani, S.; Eskandari Tadavani, E.; Etesami, S. M.; Khakzad, M.; Mohammadi Najafabadi, M.; Naseri, M.; Paktinat Mehdiabadi, S.; Rezaei Hosseinabadi, F.; Safarzadeh, B.; Zeinali, M.; Felcini, M.; Grunewald, M.; Abbrescia, M.; Calabria, C.; Colaleo, A.; Creanza, D.; Cristella, L.; De Filippis, N.; De Palma, M.; Errico, F.; Fiore, L.; Iaselli, G.; Lezki, S.; Maggi, G.; Maggi, M.; Miniello, G.; My, S.; Nuzzo, S.; Pompili, A.; Pugliese, G.; Radogna, R.; Ranieri, A.; Selvaggi, G.; Sharma, A.; Silvestris, L.; Venditti, R.; Verwilligen, P.; Abbiendi, G.; Battilana, C.; Bonacorsi, D.; Borgonovi, L.; Braibant-Giacomelli, S.; Campanini, R.; Capiluppi, P.; Castro, A.; Cavallo, F. R.; Chhibra, S. S.; Codispoti, G.; Cuffiani, M.; Dallavalle, G. M.; Fabbri, F.; Fanfani, A.; Fasanella, D.; Giacomelli, P.; Grandi, C.; Guiducci, L.; Marcellini, S.; Masetti, G.; Montanari, A.; Navarria, F. L.; Perrotta, A.; Rossi, A. M.; Rovelli, T.; Siroli, G. P.; Tosi, N.; Albergo, S.; Costa, S.; Di Mattia, A.; Giordano, F.; Potenza, R.; Tricomi, A.; Tuve, C.; Barbagli, G.; Chatterjee, K.; Ciulli, V.; Civinini, C.; D'Alessandro, R.; Focardi, E.; Lenzi, P.; Meschini, M.; Paoletti, S.; Russo, L.; Sguazzoni, G.; Strom, D.; Viliani, L.; Benussi, L.; Bianco, S.; Fabbri, F.; Piccolo, D.; Primavera, F.; Calvelli, V.; Ferro, F.; Robutti, E.; Tosi, S.; Benaglia, A.; Brianza, L.; Brivio, F.; Ciriolo, V.; Dinardo, M. E.; Fiorendi, S.; Gennai, S.; Ghezzi, A.; Govoni, P.; Malberti, M.; Malvezzi, S.; Manzoni, R. A.; Menasce, D.; Moroni, L.; Paganoni, M.; Pauwels, K.; Pedrini, D.; Pigazzini, S.; Ragazzi, S.; Redaelli, N.; Tabarelli de Fatis, T.; Buontempo, S.; Cavallo, N.; Di Guida, S.; Fabozzi, F.; Fienga, F.; Iorio, A. O. M.; Khan, W. A.; Lista, L.; Meola, S.; Paolucci, P.; Sciacca, C.; Thyssen, F.; Azzi, P.; Bacchetta, N.; Benato, L.; Biasotto, M.; Bisello, D.; Boletti, A.; Carlin, R.; Checchia, P.; Dall'Osso, M.; De Castro Manzano, P.; Dorigo, T.; Dosselli, U.; Gasparini, F.; Gasparini, U.; Lacaprara, S.; Lujan, P.; Margoni, M.; Meneguzzo, A. T.; Pozzobon, N.; Ronchese, P.; Rossin, R.; Simonetto, F.; Torassa, E.; Zanetti, M.; Zotto, P.; Zumerle, G.; Braghieri, A.; Magnani, A.; Montagna, P.; Ratti, S. P.; Re, V.; Ressegotti, M.; Riccardi, C.; Salvini, P.; Vai, I.; Vitulo, P.; Alunni Solestizi, L.; Biasini, M.; Bilei, G. M.; Cecchi, C.; Ciangottini, D.; Fanò, L.; Lariccia, P.; Leonardi, R.; Manoni, E.; Mantovani, G.; Mariani, V.; Menichelli, M.; Rossi, A.; Santocchia, A.; Spiga, D.; Androsov, K.; Azzurri, P.; Bagliesi, G.; Boccali, T.; Borrello, L.; Castaldi, R.; Ciocci, M. A.; Dell'Orso, R.; Fedi, G.; Giannini, L.; Giassi, A.; Grippo, M. 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M.; Evans, A.; Hansen, P.; Hiltbrand, J.; Kalafut, S.; Kubota, Y.; Lesko, Z.; Mans, J.; Nourbakhsh, S.; Ruckstuhl, N.; Rusack, R.; Turkewitz, J.; Wadud, M. A.; Acosta, J. G.; Oliveros, S.; Avdeeva, E.; Bloom, K.; Claes, D. R.; Fangmeier, C.; Gonzalez Suarez, R.; Kamalieddin, R.; Kravchenko, I.; Monroy, J.; Siado, J. E.; Snow, G. R.; Stieger, B.; Dolen, J.; Godshalk, A.; Harrington, C.; Iashvili, I.; Nguyen, D.; Parker, A.; Rappoccio, S.; Roozbahani, B.; Alverson, G.; Barberis, E.; Hortiangtham, A.; Massironi, A.; Morse, D. M.; Orimoto, T.; Teixeira De Lima, R.; Trocino, D.; Wood, D.; Bhattacharya, S.; Charaf, O.; Hahn, K. A.; Mucia, N.; Odell, N.; Pollack, B.; Schmitt, M. H.; Sung, K.; Trovato, M.; Velasco, M.; Dev, N.; Hildreth, M.; Hurtado Anampa, K.; Jessop, C.; Karmgard, D. J.; Kellams, N.; Lannon, K.; Loukas, N.; Marinelli, N.; Meng, F.; Mueller, C.; Musienko, Y.; Planer, M.; Reinsvold, A.; Ruchti, R.; Smith, G.; Taroni, S.; Wayne, M.; Wolf, M.; Woodard, A.; Alimena, J.; Antonelli, L.; Bylsma, B.; Durkin, L. S.; Flowers, S.; Francis, B.; Hart, A.; Hill, C.; Ji, W.; Liu, B.; Luo, W.; Puigh, D.; Winer, B. L.; Wulsin, H. W.; Cooperstein, S.; Driga, O.; Elmer, P.; Hardenbrook, J.; Hebda, P.; Higginbotham, S.; Lange, D.; Luo, J.; Marlow, D.; Mei, K.; Ojalvo, I.; Olsen, J.; Palmer, C.; Piroué, P.; Stickland, D.; Tully, C.; Malik, S.; Norberg, S.; Barker, A.; Barnes, V. E.; Das, S.; Folgueras, S.; Gutay, L.; Jha, M. K.; Jones, M.; Jung, A. W.; Khatiwada, A.; Miller, D. H.; Neumeister, N.; Peng, C. C.; Qiu, H.; Schulte, J. F.; Sun, J.; Wang, F.; Xie, W.; Cheng, T.; Parashar, N.; Stupak, J.; Adair, A.; Chen, Z.; Ecklund, K. M.; Freed, S.; Geurts, F. J. M.; Guilbaud, M.; Kilpatrick, M.; Li, W.; Michlin, B.; Northup, M.; Padley, B. P.; Roberts, J.; Rorie, J.; Shi, W.; Tu, Z.; Zabel, J.; Zhang, A.; Bodek, A.; de Barbaro, P.; Demina, R.; Duh, Y. t.; Ferbel, T.; Galanti, M.; Garcia-Bellido, A.; Han, J.; Hindrichs, O.; Khukhunaishvili, A.; Lo, K. H.; Tan, P.; Verzetti, M.; Ciesielski, R.; Goulianos, K.; Mesropian, C.; Agapitos, A.; Chou, J. P.; Gershtein, Y.; Gómez Espinosa, T. A.; Halkiadakis, E.; Heindl, M.; Hughes, E.; Kaplan, S.; Kunnawalkam Elayavalli, R.; Kyriacou, S.; Lath, A.; Montalvo, R.; Nash, K.; Osherson, M.; Saka, H.; Salur, S.; Schnetzer, S.; Sheffield, D.; Somalwar, S.; Stone, R.; Thomas, S.; Thomassen, P.; Walker, M.; Delannoy, A. G.; Foerster, M.; Heideman, J.; Riley, G.; Rose, K.; Spanier, S.; Thapa, K.; Bouhali, O.; Castaneda Hernandez, A.; Celik, A.; Dalchenko, M.; De Mattia, M.; Delgado, A.; Dildick, S.; Eusebi, R.; Gilmore, J.; Huang, T.; Kamon, T.; Mueller, R.; Pakhotin, Y.; Patel, R.; Perloff, A.; Perniè, L.; Rathjens, D.; Safonov, A.; Tatarinov, A.; Ulmer, K. A.; Akchurin, N.; Damgov, J.; De Guio, F.; Dudero, P. R.; Faulkner, J.; Gurpinar, E.; Kunori, S.; Lamichhane, K.; Lee, S. W.; Libeiro, T.; Mengke, T.; Muthumuni, S.; Peltola, T.; Undleeb, S.; Volobouev, I.; Wang, Z.; Greene, S.; Gurrola, A.; Janjam, R.; Johns, W.; Maguire, C.; Melo, A.; Ni, H.; Padeken, K.; Sheldon, P.; Tuo, S.; Velkovska, J.; Xu, Q.; Arenton, M. W.; Barria, P.; Cox, B.; Hirosky, R.; Joyce, M.; Ledovskoy, A.; Li, H.; Neu, C.; Sinthuprasith, T.; Wang, Y.; Wolfe, E.; Xia, F.; Harr, R.; Karchin, P. E.; Poudyal, N.; Sturdy, J.; Thapa, P.; Zaleski, S.; Brodski, M.; Buchanan, J.; Caillol, C.; Dasu, S.; Dodd, L.; Duric, S.; Gomber, B.; Grothe, M.; Herndon, M.; Hervé, A.; Hussain, U.; Klabbers, P.; Lanaro, A.; Levine, A.; Long, K.; Loveless, R.; Polese, G.; Ruggles, T.; Savin, A.; Smith, N.; Smith, W. H.; Taylor, D.; Woods, N.; CMS Collaboration

2018-04-01

Charge-dependent azimuthal correlations of same- and opposite-sign pairs with respect to the second- and third-order event planes have been measured in p Pb collisions at √{s NN}=8.16 TeV and PbPb collisions at 5.02 TeV with the CMS experiment at the LHC. The measurement is motivated by the search for the charge separation phenomenon predicted by the chiral magnetic effect (CME) in heavy ion collisions. Three- and two-particle azimuthal correlators are extracted as functions of the pseudorapidity difference, the transverse momentum (pT) difference, and the pT average of same- and opposite-charge pairs in various event multiplicity ranges. The data suggest that the charge-dependent three-particle correlators with respect to the second- and third-order event planes share a common origin, predominantly arising from charge-dependent two-particle azimuthal correlations coupled with an anisotropic flow. The CME is expected to lead to a v2-independent three-particle correlation when the magnetic field is fixed. Using an event shape engineering technique, upper limits on the v2-independent fraction of the three-particle correlator are estimated to be 13% for p Pb and 7% for PbPb collisions at 95% confidence level. The results of this analysis, both the dominance of two-particle correlations as a source of the three-particle results and the similarities seen between PbPb and p Pb , provide stringent constraints on the origin of charge-dependent three-particle azimuthal correlations and challenge their interpretation as arising from a chiral magnetic effect in heavy ion collisions.

Constraints on the chiral magnetic effect using charge-dependent azimuthal correlations in $$p\\mathrm{Pb}$$ and PbPb collisions at the CERN Large Hadron Collider

DOE PAGES

Sirunyan, Albert M; et al.

2018-04-24

Charge-dependent azimuthal correlations of same- and opposite-sign pairs with respect to the second- and third-order event planes have been measured in pPb collisions at sNN=8.16TeV and PbPb collisions at 5.02 TeV with the CMS experiment at the LHC. The measurement is motivated by the search for the charge separation phenomenon predicted by the chiral magnetic effect (CME) in heavy ion collisions. Three- and two-particle azimuthal correlators are extracted as functions of the pseudorapidity difference, the transverse momentum (pT) difference, and the pT average of same- and opposite-charge pairs in various event multiplicity ranges. The data suggest that the charge-dependent three-particle correlatorsmore » with respect to the second- and third-order event planes share a common origin, predominantly arising from charge-dependent two-particle azimuthal correlations coupled with an anisotropic flow. The CME is expected to lead to a v2-independent three-particle correlation when the magnetic field is fixed. Using an event shape engineering technique, upper limits on the v2-independent fraction of the three-particle correlator are estimated to be 13% for pPb and 7% for PbPb collisions at 95% confidence level. The results of this analysis, both the dominance of two-particle correlations as a source of the three-particle results and the similarities seen between PbPb and pPb, provide stringent constraints on the origin of charge-dependent three-particle azimuthal correlations and challenge their interpretation as arising from a chiral magnetic effect in heavy ion collisions.« less

Constraints on the chiral magnetic effect using charge-dependent azimuthal correlations in $$p\\mathrm{Pb}$$ and PbPb collisions at the CERN Large Hadron Collider

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

Sirunyan, Albert M; et al.

Charge-dependent azimuthal correlations of same- and opposite-sign pairs with respect to the second- and third-order event planes have been measured in pPb collisions at sNN=8.16TeV and PbPb collisions at 5.02 TeV with the CMS experiment at the LHC. The measurement is motivated by the search for the charge separation phenomenon predicted by the chiral magnetic effect (CME) in heavy ion collisions. Three- and two-particle azimuthal correlators are extracted as functions of the pseudorapidity difference, the transverse momentum (pT) difference, and the pT average of same- and opposite-charge pairs in various event multiplicity ranges. The data suggest that the charge-dependent three-particle correlatorsmore » with respect to the second- and third-order event planes share a common origin, predominantly arising from charge-dependent two-particle azimuthal correlations coupled with an anisotropic flow. The CME is expected to lead to a v2-independent three-particle correlation when the magnetic field is fixed. Using an event shape engineering technique, upper limits on the v2-independent fraction of the three-particle correlator are estimated to be 13% for pPb and 7% for PbPb collisions at 95% confidence level. The results of this analysis, both the dominance of two-particle correlations as a source of the three-particle results and the similarities seen between PbPb and pPb, provide stringent constraints on the origin of charge-dependent three-particle azimuthal correlations and challenge their interpretation as arising from a chiral magnetic effect in heavy ion collisions.« less

Quasiparticle-mediated spin Hall effect in a superconductor.

PubMed

Wakamura, T; Akaike, H; Omori, Y; Niimi, Y; Takahashi, S; Fujimaki, A; Maekawa, S; Otani, Y

2015-07-01

In some materials the competition between superconductivity and magnetism brings about a variety of unique phenomena such as the coexistence of superconductivity and magnetism in heavy-fermion superconductors or spin-triplet supercurrent in ferromagnetic Josephson junctions. Recent observations of spin-charge separation in a lateral spin valve with a superconductor evidence that these remarkable properties are applicable to spintronics, although there are still few works exploring this possibility. Here, we report the experimental observation of the quasiparticle-mediated spin Hall effect in a superconductor, NbN. This compound exhibits the inverse spin Hall (ISH) effect even below the superconducting transition temperature. Surprisingly, the ISH signal increases by more than 2,000 times compared with that in the normal state with a decrease of the injected spin current. The effect disappears when the distance between the voltage probes becomes larger than the charge imbalance length, corroborating that the huge ISH signals measured are mediated by quasiparticles.

The first radial-mode Lorentzian Landau damping of dust acoustic space-charge waves

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

Lee, Myoung-Jae; Jung, Young-Dae, E-mail: ydjung@hanyang.ac.kr; Department of Applied Physics and Department of Bionanotechnology, Hanyang University, Ansan, Kyunggi-Do 15588

2016-05-15

The dispersion properties and the first radial-mode Lorentzian Landau damping of a dust acoustic space-charge wave propagating in a cylindrical waveguide dusty plasma which contains nonthermal electrons and ions are investigated by employing the normal mode analysis and the method of separation of variables. It is found that the frequency of dust acoustic space-charge wave increases as the wave number increases as well as the radius of cylindrical plasma does. However, the nonthermal property of the Lorentzian plasma is found to suppress the wave frequency of the dust acoustic space-charge wave. The Landau damping rate of the dust acoustic space-chargemore » wave is derived in a cylindrical waveguide dusty plasma. The damping of the space-charge wave is found to be enhanced as the radius of cylindrical plasma and the nonthermal property increase. The maximum Lorentzian Landau damping rate is also found in a cylindrical waveguide dusty plasma. The variation of the wave frequency and the Landau damping rate due to the nonthermal character and geometric effects are also discussed.« less

2D coherent charge transport in highly ordered conducting polymers doped by solid state diffusion

NASA Astrophysics Data System (ADS)

Kang, Keehoon; Watanabe, Shun; Broch, Katharina; Sepe, Alessandro; Brown, Adam; Nasrallah, Iyad; Nikolka, Mark; Fei, Zhuping; Heeney, Martin; Matsumoto, Daisuke; Marumoto, Kazuhiro; Tanaka, Hisaaki; Kuroda, Shin-Ichi; Sirringhaus, Henning

2016-08-01

Doping is one of the most important methods to control charge carrier concentration in semiconductors. Ideally, the introduction of dopants should not perturb the ordered microstructure of the semiconducting host. In some systems, such as modulation-doped inorganic semiconductors or molecular charge transfer crystals, this can be achieved by spatially separating the dopants from the charge transport pathways. However, in conducting polymers, dopants tend to be randomly distributed within the conjugated polymer, and as a result the transport properties are strongly affected by the resulting structural and electronic disorder. Here, we show that in the highly ordered lamellar microstructure of a regioregular thiophene-based conjugated polymer, a small-molecule p-type dopant can be incorporated by solid state diffusion into the layers of solubilizing side chains without disrupting the conjugated layers. In contrast to more disordered systems, this allows us to observe coherent, free-electron-like charge transport properties, including a nearly ideal Hall effect in a wide temperature range, a positive magnetoconductance due to weak localization and the Pauli paramagnetic spin susceptibility.

Controlling Gas-Phase Reactions for Efficient Charge Reduction Electrospray Mass Spectrometry of Intact Proteins

PubMed Central

Frey, Brian L.; Lin, Yuan; Westphall, Michael S.; Smith, Lloyd M.

2006-01-01

Charge reduction electrospray mass spectrometry (CREMS) reduces the charge states of electrospray-generated ions, which concentrates the ions from a protein into fewer peaks spread over a larger m/z range, thereby increasing peak separation and decreasing spectral congestion. An optimized design for a CREMS source is described that provides an order-of-magnitude increase in sensitivity compared to previous designs and provides control over the extent of charge reduction. Either a corona discharge or an α-particle source was employed to generate anions that abstract protons from electrosprayed protein cations. These desired ion/ion proton transfer reactions predominated, but some oxidation and ion-attachment reactions also occurred leading to new peaks or mass-shifted broader peaks while decreasing signal intensity. The species producing these deleterious side-reactions were identified, and conditions were found that prevented their formation. Spectrometer m/z biases were examined because of their effect upon the signal intensity of higher m/z charge-reduced protein ions. The utility of this atmospheric pressure CREMS was demonstrated using a cell lysate fraction from E. coli. The spectral simplification afforded by CREMS reveals more proteins than are observed without charge reduction. PMID:16198118

Numerical Simulations of Flow Separation Control in Low-Pressure Turbines using Plasma Actuators

NASA Technical Reports Server (NTRS)

Suzen, Y. B.; Huang, P. G.; Ashpis, D. E.

2007-01-01

A recently introduced phenomenological model to simulate flow control applications using plasma actuators has been further developed and improved in order to expand its use to complicated actuator geometries. The new modeling approach eliminates the requirement of an empirical charge density distribution shape by using the embedded electrode as a source for the charge density. The resulting model is validated against a flat plate experiment with quiescent environment. The modeling approach incorporates the effect of the plasma actuators on the external flow into Navier Stokes computations as a body force vector which is obtained as a product of the net charge density and the electric field. The model solves the Maxwell equation to obtain the electric field due to the applied AC voltage at the electrodes and an additional equation for the charge density distribution representing the plasma density. The new modeling approach solves the charge density equation in the computational domain assuming the embedded electrode as a source therefore automatically generating a charge density distribution on the surface exposed to the flow similar to that observed in the experiments without explicitly specifying an empirical distribution. The model is validated against a flat plate experiment with quiescent environment.

Communication: a density functional with accurate fractional-charge and fractional-spin behaviour for s-electrons.

PubMed

Johnson, Erin R; Contreras-García, Julia

2011-08-28

We develop a new density-functional approach combining physical insight from chemical structure with treatment of multi-reference character by real-space modeling of the exchange-correlation hole. We are able to recover, for the first time, correct fractional-charge and fractional-spin behaviour for atoms of groups 1 and 2. Based on Becke's non-dynamical correlation functional [A. D. Becke, J. Chem. Phys. 119, 2972 (2003)] and explicitly accounting for core-valence separation and pairing effects, this method is able to accurately describe dissociation and strong correlation in s-shell many-electron systems. © 2011 American Institute of Physics

Adverse Effects of Excess Residual PbI2 on Photovoltaic Performance, Charge Separation, and Trap-State Properties in Mesoporous Structured Perovskite Solar Cells.

PubMed

Wang, Hao-Yi; Hao, Ming-Yang; Han, Jun; Yu, Man; Qin, Yujun; Zhang, Pu; Guo, Zhi-Xin; Ai, Xi-Cheng; Zhang, Jian-Ping

2017-03-17

Organic-inorganic halide perovskite solar cells have rapidly come to prominence in the photovoltaic field. In this context, CH 3 NH 3 PbI 3 , as the most widely adopted active layer, has been attracting great attention. Generally, in a CH 3 NH 3 PbI 3 layer, unreacted PbI 2 inevitably coexists with the perovskite crystals, especially following a two-step fabrication process. There appears to be a consensus that an appropriate amount of unreacted PbI 2 is beneficial to the overall photovoltaic performance of a device, the only disadvantageous aspect of excess residual PbI 2 being viewed as its insulating nature. However, the further development of such perovskite-based devices requires a deeper understanding of the role of residual PbI 2 . In this work, PbI 2 -enriched and PbI 2 -controlled perovskite films, as two extreme cases, have been prepared by modulating the crystallinity of a pre-deposited PbI 2 film. The effects of excess residual PbI 2 have been elucidated on the basis of spectroscopic and optoelectronic studies. The initial charge separation, the trap-state density, and the trap-state distribution have all been found to be adversely affected in PbI 2 -enriched devices, to the detriment of photovoltaic performance. This leads to a biphasic recombination process and accelerates the charge carrier recombination dynamics. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Design Flexibility of Redox Flow Systems. [for energy storage applications

NASA Technical Reports Server (NTRS)

Hagedorn, N. H.; Thaller, L. H.

1982-01-01

The characteristics inherent in Redox flow systems permit considerable latitude in designing systems for specific storage applications. The first of these characteristics is the absence of plating/deplating reactions with their attendant morphology changes at the electrodes. This permits a given Redox system to operate over a wide range of depths of discharge and charge/discharge rates. The second characteristic is the separation of power generating components (stacks) from the energy storage components (tanks). This results in cost effective system design, ease of system growth via modularization, and freedom from sizing restraints so that the whole spectrum of applications, from utilities down to single residence can be considered. The final characteristic is the commonality of the reactant fluids which assures that all cells at all times are receiving reactants at the same state of charge. Since no cell can be out of balance with respect to any other cell, it is possible for some cells to be charged while others are discharging, in effect creating a DC to DC transformer. It is also possible for various groups of cells to be connected to separate loads, thus supplying a range of output voltages. Also, trim cells can be used to maintain constant bus voltage as the load is changed or as the depth of discharge increases. The commonality of reactant fluids also permits any corrective measures such as rebalancing to occur at the system level instead of at the single cell level.

Combined electrophoretic-separation and electrospray method and system

DOEpatents

Smith, Richard D.; Olivares, Jose A.

1989-01-01

A system and method for analyzing molecular constituents of a composition sample includes: forming a solution of the sample, separating the solution by capillary zone electrophoresis into an eluent of constituents longitudinally separated according to their relative electrophoretic mobilities, electrospraying the eluent to form a charged spray in which the molecular constituents have a temporal distribution; and detecting or collecting the separated constituents in accordance with the temporal distribution in the spray. A first high-voltage (e.g., 5-100 KVDC) is applied to the solution. The spray is charged by applying a second high voltage (e.g., .+-.2-8 KVDC) between the eluent at the capillary exit and a cathode spaced in front of the exit. A complete electrical circuit is formed by a conductor which directly contacts the eluent at the capillary exit.

Electrical Contacts to Individual Colloidal Semiconductor Nanorods

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

Trudeau, Paul-Emile; Sheldon, Matt; Altoe, Virginia

We report the results of charge transport studies on single CdTe nanocrystals contacted via evaporated Pd electrodes. Device charging energy, E{sub c}, monitored as a function of electrode separation drops suddenly at separations below {approx}55 nm. This drop can be explained by chemical changes induced by the metal electrodes. This explanation is corroborated by ensemble X-Ray photoelectron spectroscopy (XPS) studies of CdTe films as well as single particle measurements by transmission electron microscopy (TEM) and energy dispersive X-Rays (EDX). Similar to robust optical behavior obtained when Nanocrystals are coated with a protective shell, we find that a protective SiO2 layermore » deposited between the nanocrystal and the electrode prevents interface reactions and an associated drop in E{sub c,max}. This observation of interface reactivity and its effect on electrical properties has important implications for the integration of nanocrystals into conventional fabrication techniques and may enable novel nano-materials.« less

Enhancement of plasmon-induced charge separation efficiency by coupling silver nanocubes with a thin gold film

NASA Astrophysics Data System (ADS)

Akiyoshi, Kazutaka; Saito, Koichiro; Tatsuma, Tetsu

2016-10-01

Plasmon-induced charge separation (PICS), in which an energetic electron is injected from a plasmonic nanoparticle (NP) to a semiconductor on contact, is often inhibited by a protecting agent adsorbed on the NP. We addressed this issue for an Ag nanocube-TiO2 system by coating it with a thin Au layer or by inserting the Au layer between the nanocubes (NCs) and TiO2. Both of the electrodes exhibit much higher photocurrents due to PICS than the electrodes without the Au film or the Ag NCs. These photocurrent enhancements can be explained in terms of PICS with accelerated electron transfer, in which electron injection from the Ag NCs or Ag@Au core-shell NCs to TiO2 is promoted by the Au film, or PICS enhanced by a nanoantenna effect, in which the electron injection from the Au film to TiO2 is enhanced by optical near field generated by the Ag NC.

Ca2+-induced phase separation in black lipid membranes and its effect on the transport of a hydrophobic ion.

PubMed

Miller, A; Schmidt, G; Eibl, H; Knoll, W

1985-03-14

Voltage jump-current relaxation studies have been performed with dipicrylamine-doped black membranes of binary lipid mixtures. As in the case of the carrier-mediated ion transport (Schmidt, G., Eibl, H. and Knoll, W. (1982) J. Membrane Biol. 70, 147-155) no evidence was found that the neutral lipid phosphatidylcholine (DPMPC) and the charged phosphatidic acid (DPMPA) are heterogeneously distributed in the membrane over the whole range of composition. However, besides a continuous dilution of the surface charges of DPMPA by the addition of DPMPC molecules, different structural properties of mixed membranes influence the kinetics of the dipicrylamine transport. The addition of Ca2+ to the electrolyte induces a lipid phase separation within the membrane into two fluid phases of distinctly different characteristics of the translocation of hydrophobic ions. Thus, it is possible to determine a preliminary composition phase diagram for the DPMPA/DPMPC mixtures as a function of the Ca2+ concentration.

Structure and functionality of bromine doped graphite.

PubMed

Hamdan, Rashid; Kemper, A F; Cao, Chao; Cheng, H P

2013-04-28

First-principles calculations are used to study the enhanced in-plane conductivity observed experimentally in Br-doped graphite, and to study the effect of external stress on the structure and functionality of such systems. The model used in the numerical calculations is that of stage two doped graphite. The band structure near the Fermi surface of the doped systems with different bromine concentrations is compared to that of pure graphite, and the charge transfer between carbon and bromine atoms is analyzed to understand the conductivity change along different high symmetry directions. Our calculations show that, for large interlayer separation between doped graphite layers, bromine is stable in the molecular form (Br2). However, with increased compression (decreased layer-layer separation) Br2 molecules tend to dissociate. While in both forms, bromine is an electron acceptor. The charge exchange between the graphite layers and Br atoms is higher than that with Br2 molecules. Electron transfer to the Br atoms increases the number of hole carriers in the graphite sheets, resulting in an increase of conductivity.

System and method for charging a plug-in electric vehicle

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

Bassham, Marjorie A.; Spigno, Jr., Ciro A.; Muller, Brett T.

2017-05-02

A charging system and method that may be used to automatically apply customized charging settings to a plug-in electric vehicle, where application of the settings is based on the vehicle's location. According to an exemplary embodiment, a user may establish and save a separate charging profile with certain customized charging settings for each geographic location where they plan to charge their plug-in electric vehicle. Whenever the plug-in electric vehicle enters a new geographic area, the charging method may automatically apply the charging profile that corresponds to that area. Thus, the user does not have to manually change or manipulate themore » charging settings every time they charge the plug-in electric vehicle in a new location.« less

Integration of Semiconducting Sulfides for Full-Spectrum Solar Energy Absorption and Efficient Charge Separation.

PubMed

Zhuang, Tao-Tao; Liu, Yan; Li, Yi; Zhao, Yuan; Wu, Liang; Jiang, Jun; Yu, Shu-Hong

2016-05-23

The full harvest of solar energy by semiconductors requires a material that simultaneously absorbs across the whole solar spectrum and collects photogenerated electrons and holes separately. The stepwise integration of three semiconducting sulfides, namely ZnS, CdS, and Cu2-x S, into a single nanocrystal, led to a unique ternary multi-node sheath ZnS-CdS-Cu2-x S heteronanorod for full-spectrum solar energy absorption. Localized surface plasmon resonance (LSPR) in the nonstoichiometric copper sulfide nanostructures enables effective NIR absorption. More significantly, the construction of pn heterojunctions between Cu2-x S and CdS leads to staggered gaps, as confirmed by first-principles simulations. This band alignment causes effective electron-hole separation in the ternary system and hence enables efficient solar energy conversion. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Electrolyte transport in neutral polymer gels embedded with charged inclusions

NASA Astrophysics Data System (ADS)

Hill, Reghan

2005-11-01

Ion permeable membranes are the basis of a variety of molecular separation technologies, including ion exchange, gel electrophoresis and dialysis. This work presents a theoretical model of electrolyte transport in membranes comprised of a continuous polymer gel embedded with charged spherical inclusions, e.g., biological cells and synthetic colloids. The microstructure mimics immobilized cell cultures, where electric fields have been used to promote nutrient transport. Because several important characteristics can, in principle, be carefully controlled, the theory provides a quantitative framework to help tailor the bulk properties for enhanced molecular transport, microfluidic pumping, and physicochemical sensing applications. This talk focuses on the electroosmotic flow driven by weak electric fields and electrolyte concentration gradients. Also of importance is the influence of charge on the effective ion diffusion coefficients, bulk electrical conductivity, and membrane diffusion potential.

Characterization of TiO2-based semiconductors for photocatalysis by electrochemical impedance spectroscopy

NASA Astrophysics Data System (ADS)

Ângelo, Joana; Magalhães, Pedro; Andrade, Luísa; Mendes, Adélio

2016-11-01

The photocatalytic activity of a commercial titanium dioxide (P25) and of an in-house prepared P25/graphene composite is assessed according to standard ISO 22197-1:2007. The photoactivity performances of bare and composite TiO2-based materials were further studied by electrochemical impedance spectroscopy (EIS) technique to better understand the function of the graphene in the composite. EIS experiments were performed using a three-electrode configuration, which allows obtaining more detailed information about the complex charge transfer phenomena at the semiconductor/electrolyte interface. The Randles equivalent circuit was selected as the most suitable for modelling the present photocatalysts. The use of the graphene composite allows a more effective charge separation with lower charge transfer resistance and less e-/h+ recombination on the composite photocatalyst, reflected in the higher values of NO conversion.

Detuning dependence of Rabi oscillations in an InAs self-assembled quantum dot ensemble

NASA Astrophysics Data System (ADS)

Suzuki, Takeshi; Singh, Rohan; Bayer, Manfred; Ludzwig, Arne; Wieck, Andreas D.; Cundiff, Steven T.

2018-04-01

We study the coherent evolution of an InAs self-assembled quantum dot (QD) ensemble in the ultrafast regime. The evolution of the entire frequency distribution is revealed by performing prepulse two-dimensional (2D) coherent spectroscopy. Charged and neutral QDs display distinct nonlinear responses arising from two-level trion and four-level exciton-biexciton systems, respectively, and each signal is clearly separated in 2D spectra. Whereas the signals for charged QDs are symmetric with respect to the detuning, those for neutral QDs are asymmetric due to the asymmetric four-level energy structure. Experimental results for charged and neutral QDs are well reproduced by solving the optical Bloch equations, including detuning and excitation-induced dephasing (EID) effects. The temperature dependence suggests that wetting-layer carriers play an important role in EID.

Electrostatic Interactions and Self-Assembly in Polymeric Systems

NASA Astrophysics Data System (ADS)

Dobrynin, Andrey

Electrostatic interactions between macroions play an important role in different areas ranging from materials science to biophysics. They are main driving forces behind layer-by-layer assembly technique that allows self-assembly of multilayer films from synthetic polyelectrolytes, DNA, proteins and nanoparticles. They are responsible for complexation and reversible gelation between polyelectrolytes and proteins. In this talk, using results of the molecular dynamics simulations and analytical calculations, I will demonstrate what effect electrostatic interactions, counterion condensation and polymer solvent affinity have on a collapse of polyelectrolyte chain in a poor solvent conditions for the polymer backbone, on complexations and reversible gelation between polyelectrolytes and polyamholytes (unstructured proteins), on microphase separation transitions in spherical and planar charged brushes, and on a layer-by-layer assembly of charged nanoparticles and linear polyelectrolytes on charged surfaces. NSF DMR-1004576 DMR-1409710.

Interfacial charge separation and recombination in InP and quasi-type II InP/CdS core/shell quantum dot-molecular acceptor complexes.

PubMed

Wu, Kaifeng; Song, Nianhui; Liu, Zheng; Zhu, Haiming; Rodríguez-Córdoba, William; Lian, Tianquan

2013-08-15

Recent studies of group II-VI colloidal semiconductor heterostuctures, such as CdSe/CdS core/shell quantum dots (QDs) or dot-in-rod nanorods, show that type II and quasi-type II band alignment can facilitate electron transfer and slow down charge recombination in QD-molecular electron acceptor complexes. To explore the general applicability of this wave function engineering approach for controlling charge transfer properties, we investigate exciton relaxation and dissociation dynamics in InP (a group III-V semiconductor) and InP/CdS core/shell (a heterostructure beween group III-V and II-VI semiconductors) QDs by transient absorption spectroscopy. We show that InP/CdS QDs exhibit a quasi-type II band alignment with the 1S electron delocalized throughout the core and shell and the 1S hole confined in the InP core. In InP-methylviologen (MV(2+)) complexes, excitons in the QD can be dissociated by ultrafast electron transfer to MV(2+) from the 1S electron level (with an average time constant of 11.4 ps) as well as 1P and higher electron levels (with a time constant of 0.39 ps), which is followed by charge recombination to regenerate the complex in its ground state (with an average time constant of 47.1 ns). In comparison, InP/CdS-MV(2+) complexes show similar ultrafast charge separation and 5-fold slower charge recombination rates, consistent with the quasi-type II band alignment in these heterostructures. This result demonstrates that wave function engineering in nanoheterostructures of group III-V and II-VI semiconductors provides a promising approach for optimizing their light harvesting and charge separation for solar energy conversion applications.

27 CFR 53.91 - Charges to be included in sale price.

Code of Federal Regulations, 2010 CFR

2010-04-01

... the Code and § 53.100. In the case of sales on credit, a carrying, finance, or service charge is... connection with collection). (b) Tools and dies. Separate charges for tools and dies used in the manufacture... manufacture taxable articles, the tools and dies used in production pass to the purchaser, only the amount of...

Energy level engineering in ternary organic solar cells: Evaluating exciton dissociation at organic semiconductor interfaces

NASA Astrophysics Data System (ADS)

Feron, Krishna; Thameel, Mahir N.; Al-Mudhaffer, Mohammed F.; Zhou, Xiaojing; Belcher, Warwick J.; Fell, Christopher J.; Dastoor, Paul C.

2017-03-01

Electronic energy level engineering, with the aim to improve the power conversion efficiency in ternary organic solar cells, is a complex problem since multiple charge transfer steps and exciton dissociation driving forces must be considered. Here, we examine exciton dissociation in the ternary system poly(3-hexylthiophene): [6,6]-phenyl-C61-butyric acid methyl ester:2,4-bis[4-(N,N-diisobutylamino)-2,6-dihydroxyphenyl] squaraine (P3HT:PCBM:DIBSq). Even though the energy level diagram suggests that exciton dissociation at the P3HT:DIBSq interface should be efficient, electron paramagnetic resonance and external quantum efficiency measurements of planar devices show that this interface is not capable of generating separated charge carriers. Efficient exciton dissociation is still realised via energy transfer, which transports excitons from the P3HT:DIBSq interface to the DIBSq:PCBM interface, where separated charge carriers can be generated efficiently. This work demonstrates that energy level diagrams alone cannot be relied upon to predict the exciton dissociation and charge separation capability of an organic semiconductor interface and that energy transfer relaxes the energy level constraints for optimised multi-component organic solar cells.

Analysis of pharmaceutical impurities using multi-heartcutting 2D LC coupled with UV-charged aerosol MS detection.

PubMed

Zhang, Kelly; Li, Yi; Tsang, Midco; Chetwyn, Nik P

2013-09-01

To overcome challenges in HPLC impurity analysis of pharmaceuticals, we developed an automated online multi-heartcutting 2D HPLC system with hyphenated UV-charged aerosol MS detection. The first dimension has a primary column and the second dimension has six orthogonal columns to enhance flexibility and selectivity. The two dimensions were interfaced by a pair of switching valves equipped with six trapping loops that allow multi-heartcutting of peaks of interest in the first dimension and also allow "peak parking." The hyphenated UV-charged aerosol MS detection provides comprehensive detection for compounds with and without UV chromophores, organics, and inorganics. It also provides structural information for impurity identification. A hidden degradation product that co-eluted with the drug main peak was revealed by RP × RP separation and thus enabled the stability-indicating method development. A poorly retained polar component with no UV chromophores was analyzed by RP × hydrophilic interaction liquid chromatography separation with charged aerosol detection. Furthermore, using this system, the structures of low-level impurities separated by a method using nonvolatile phosphate buffer were identified and tracked by MS in the second dimension. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The Martian Dust Devil Electron Avalanche: Laboratory Measurements of the E-Field Fortifying Effects of Dust-Electron Absorption

NASA Technical Reports Server (NTRS)

Farrell, W. M.; McLain, J. L.; Collier, M. R.; Keller, J. W.

2017-01-01

Analogous to terrestrial dust devils, charged dust in Mars dust devils should become vertically stratified in the convective features, creating large scale E-fields. This E-field in a Martian-like atmosphere has been shown to stimulate the development of a Townsend discharge (electron avalanche) that acts to dissipate charge in regions where charge build-up occurs. While the stratification of the charged dust is a source of the electrical energy, the uncharged particulates in the dust population may absorb a portion of these avalanching electrons, thereby inhibiting dissipation and leading to the development of anomalously large E-field values. We performed a laboratory study that does indeed show the presence of enhanced E-field strengths between an anode and cathode when dust-absorbing filaments (acting as particulates) are placed in the avalanching electron flow. Further, the E-field threshold condition to create an impulsive spark discharge increases to larger values as more filaments are placed between the anode and cathode. We conclude that the spatially separated charged dust creates the charge centers and E-fields in a dust devil, but the under-charged portion of the population acts to reduce Townsend electron dissipation currents, further fortifying the development of larger-than-expected E-fields.

Dissociation of hydrophobic and charged nano particles in aqueous guanidinium chloride and urea solutions: A molecular dynamics study

NASA Astrophysics Data System (ADS)

Li, Weifeng; Mu, Yuguang

2012-02-01

It has been a long history that urea and guanidinium chloride (GdmCl) are used as agents for denaturing proteins. The underlying mechanism has been extensively studied in the past several decades. However, the question regarding why GdmCl is much stronger than urea has seldom been touched. Here, through molecular dynamics simulations, we show that a 4 M GdmCl solution is more able than 7 M urea solution to dissociate both hydrophobic and charged nano-particles (NP). Both urea and GdmCl affect the NPs' aggregation through direct binding to the NP surface. The advantages of GdmCl originate from the net charge of bound guanidinium ions which can generate a local positively charged environment around hydrophobic and negatively charged NPs. This effective coating can introduce Coulombic repulsion between all the NPs. Urea shows certain ability to dissociate hydrophobic NPs. However, in the case of charged NPs, urea molecules located between two opposite-charged NPs will form ordered hydrogen bonds, acting like ``glue'' which prevents separation of the NPs. Although urea can form hydrogen bonds with either hydrophilic amino acids or the protein backbone, which are believed to contribute to protein denaturation, our findings strongly suggest that this property does not always contribute positively to urea's denaturation power.

Charge redistribution in QM:QM ONIOM model systems: a constrained density functional theory approach

NASA Astrophysics Data System (ADS)

Beckett, Daniel; Krukau, Aliaksandr; Raghavachari, Krishnan

2017-11-01

The ONIOM hybrid method has found considerable success in QM:QM studies designed to approximate a high level of theory at a significantly reduced cost. This cost reduction is achieved by treating only a small model system with the target level of theory and the rest of the system with a low, inexpensive, level of theory. However, the choice of an appropriate model system is a limiting factor in ONIOM calculations and effects such as charge redistribution across the model system boundary must be considered as a source of error. In an effort to increase the general applicability of the ONIOM model, a method to treat the charge redistribution effect is developed using constrained density functional theory (CDFT) to constrain the charge experienced by the model system in the full calculation to the link atoms in the truncated model system calculations. Two separate CDFT-ONIOM schemes are developed and tested on a set of 20 reactions with eight combinations of levels of theory. It is shown that a scheme using a scaled Lagrange multiplier term obtained from the low-level CDFT model calculation outperforms ONIOM at each combination of levels of theory from 32% to 70%.

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.

Terahertz Emission from Hybrid Perovskites Driven by Ultrafast Charge Separation and Strong Electron-Phonon Coupling.

PubMed

Guzelturk, Burak; Belisle, Rebecca A; Smith, Matthew D; Bruening, Karsten; Prasanna, Rohit; Yuan, Yakun; Gopalan, Venkatraman; Tassone, Christopher J; Karunadasa, Hemamala I; McGehee, Michael D; Lindenberg, Aaron M

2018-03-01

Unusual photophysical properties of organic-inorganic hybrid perovskites have not only enabled exceptional performance in optoelectronic devices, but also led to debates on the nature of charge carriers in these materials. This study makes the first observation of intense terahertz (THz) emission from the hybrid perovskite methylammonium lead iodide (CH 3 NH 3 PbI 3 ) following photoexcitation, enabling an ultrafast probe of charge separation, hot-carrier transport, and carrier-lattice coupling under 1-sun-equivalent illumination conditions. Using this approach, the initial charge separation/transport in the hybrid perovskites is shown to be driven by diffusion and not by surface fields or intrinsic ferroelectricity. Diffusivities of the hot and band-edge carriers along the surface normal direction are calculated by analyzing the emitted THz transients, with direct implications for hot-carrier device applications. Furthermore, photogenerated carriers are found to drive coherent terahertz-frequency lattice distortions, associated with reorganizations of the lead-iodide octahedra as well as coupled vibrations of the organic and inorganic sublattices. This strong and coherent carrier-lattice coupling is resolved on femtosecond timescales and found to be important both for resonant and far-above-gap photoexcitation. This study indicates that ultrafast lattice distortions play a key role in the initial processes associated with charge transport. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ultrafast Exciton Dissociation and Long-Lived Charge Separation in a Photovoltaic Pentacene-MoS2 van der Waals Heterojunction.

PubMed

Bettis Homan, Stephanie; Sangwan, Vinod K; Balla, Itamar; Bergeron, Hadallia; Weiss, Emily A; Hersam, Mark C

2017-01-11

van der Waals heterojunctions between two-dimensional (2D) layered materials and nanomaterials of different dimensions present unique opportunities for gate-tunable optoelectronic devices. Mixed-dimensional p-n heterojunction diodes, such as p-type pentacene (0D) and n-type monolayer MoS 2 (2D), are especially interesting for photovoltaic applications where the absorption cross-section and charge transfer processes can be tailored by rational selection from the vast library of organic molecules and 2D materials. Here, we study the kinetics of excited carriers in pentacene-MoS 2 p-n type-II heterojunctions by transient absorption spectroscopy. These measurements show that the dissociation of MoS 2 excitons occurs by hole transfer to pentacene on the time scale of 6.7 ps. In addition, the charge-separated state lives for 5.1 ns, up to an order of magnitude longer than the recombination lifetimes from previously reported 2D material heterojunctions. By studying the fractional amplitudes of the MoS 2 decay processes, the hole transfer yield from MoS 2 to pentacene is found to be ∼50%, with the remaining holes undergoing trapping due to surface defects. Overall, the ultrafast charge transfer and long-lived charge-separated state in pentacene-MoS 2 p-n heterojunctions suggest significant promise for mixed-dimensional van der Waals heterostructures in photovoltaics, photodetectors, and related optoelectronic technologies.

Terahertz Emission from Hybrid Perovskites Driven by Ultrafast Charge Separation and Strong Electron-Phonon Coupling

DOE PAGES

Guzelturk, Burak; Belisle, Rebecca A.; Smith, Matthew D.; ...

2018-01-23

Unusual photophysical properties of organic–inorganic hybrid perovskites have not only enabled exceptional performance in optoelectronic devices, but also led to debates on the nature of charge carriers in these materials. This study makes the first observation of intense terahertz (THz) emission from the hybrid perovskite methylammonium lead iodide (CH 3NH 3PbI 3) following photoexcitation, enabling an ultrafast probe of charge separation, hot–carrier transport, and carrier–lattice coupling under 1–sun–equivalent illumination conditions. Using this approach, the initial charge separation/transport in the hybrid perovskites is shown to be driven by diffusion and not by surface fields or intrinsic ferroelectricity. Diffusivities of the hotmore » and band–edge carriers along the surface normal direction are calculated by analyzing the emitted THz transients, with direct implications for hot–carrier device applications. Furthermore, photogenerated carriers are found to drive coherent terahertz–frequency lattice distortions, associated with reorganizations of the lead–iodide octahedra as well as coupled vibrations of the organic and inorganic sublattices. This strong and coherent carrier–lattice coupling is resolved on femtosecond timescales and found to be important both for resonant and far–above–gap photoexcitation. As a result, this study indicates that ultrafast lattice distortions play a key role in the initial processes associated with charge transport.« less

Particle astronomy with a superconducting magnet.

NASA Technical Reports Server (NTRS)

Buffington, A.

1972-01-01

The magnetic spectrometer measures deflections of charged particles moving in a magnetic field and provides a direct means of determining the rigidity of charged primary cosmic rays up to about 100 GV/c rigidity. The underlying concepts of the method are reviewed, and factors delineating the applicable momentum range and accuracy are described along with calibration techniques. Previous experiments employing this technique are summarized, and prospects for future applications are evaluated with emphasis on separate measurement of electron and positron spectra and on isotopic separation.

Simplified charge separation energetics in a two-dimensional model for polymer-based photovoltaic cells.

PubMed

Sylvester-Hvid, Kristian O; Ratner, Mark A

2005-01-13

An extension of our two-dimensional working model for photovoltaic behavior in binary polymer and/or molecular photoactive blends is presented. The objective is to provide a more-realistic description of the charge generation and charge separation processes in the blend system. This is achieved by assigning an energy to each of the possible occupation states, describing the system according to a simple energy model for exciton and geminate electron-hole pair configurations. The energy model takes as primary input the ionization potential, electron affinity and optical gap of the components of the blend. The underlying photovoltaic model considers a nanoscopic subvolume of a photoactive blend and represents its p- and n-type domain morphology, in terms of a two-dimensional network of donor and acceptor sites. The nearest-neighbor hopping of charge carriers in the illuminated system is described in terms of transitions between different occupation states. The equations governing the dynamics of these states are cast into a linear master equation, which can be solved for arbitrary two-dimensional donor-acceptor networks, assuming stationary conditions. The implications of incorporating the energy model into the photovoltaic model are illustrated by simulations of the short circuit current versus thickness of the photoactive blend layer for different choices of energy parameters and donor-acceptor topology. The results suggest the existence of an optimal thickness of the photoactive film in bulk heterojunctions, based on kinetic considerations alone, and that this optimal thickness is very sensitive to the choice of energy parameters. The results also indicate space-charge limiting effects for interpenetrating donor-acceptor networks with characteristic domain sizes in the nanometer range and high driving force for the photoinduced electron transfer across the donor-acceptor internal interface.

Macroparticle separation and plasma collimation in positively biased ducts in filtered vacuum arc deposition systems

NASA Astrophysics Data System (ADS)

Beilis, I. I.; Keidar, M.; Boxman, R. L.; Goldsmith, S.

1999-02-01

The objective of the present work was to determine the influence of positive bias on plasma and macroparticle (MP) flow in curved magnetized plasma ducts. The plasma bulk and sheath regions were analyzed. In the plasma bulk, the current density and electrical field component normal to the wall were obtained and used as boundary conditions for the near wall sheath region. In the sheath, a nonstationary model for MP charging and motion was developed. The solution of the hydrodynamic equations in the plasma when a positive bias is applied to the wall result in a radial electrical current. The electric field in the plasma bulk is generated by the separation between the magnetically confined electrons, and the ions, which are thrown outwards by the centrifugal force. The field increases with increasing positive bias. It was shown that MPs traveling in the sheath accumulate a charge which depends on the potential distribution, in contrast to MP charging in the quasineutral plasma where the charge depends on plasma density and electron temperature. MP trapping in the near-wall sheath was found. MPs may move in the sheath region along the wall by a repetitive process of electrostatic attraction to the wall, mechanical reflection and neutralization, followed by MP charging and attraction, etc. For example, titanium MPs with a radius less than 0.4 μm and with a velocity component normal to the wall of about 20 m/s are trapped if the sheath potential drop exceeds 20 V. It was obtained that the MP transmission fraction through filter decreases by more than few orders of magnitude due to the trapping effect when a bias potential of +100 V is applied between the wall and the plasma.

Ultrafast exciton dynamics and light-driven H2 evolution in colloidal semiconductor nanorods and Pt-tipped nanorods.

PubMed

Wu, Kaifeng; Zhu, Haiming; Lian, Tianquan

2015-03-17

Colloidal quantum confined one-dimensional (1D) semiconductor nanorods (NRs) and related semiconductor-metal heterostructures are promising new materials for efficient solar-to-fuel conversion because of their unique physical and chemical properties. NRs can simultaneously exhibit quantum confinement effects in the radial direction and bulk like carrier transport in the axial direction. The former implies that concepts well-established in zero-dimensional quantum dots, such as size-tunable energetics and wave function engineering through band alignment in heterostructures, can also be applied to NRs; while the latter endows NRs with fast carrier transport to achieve long distance charge separation. Selective growth of catalytic metallic nanoparticles, such as Pt, at the tips of NRs provides convenient routes to multicomponent heterostructures with photocatalytic capabilities and controllable charge separation distances. The design and optimization of such materials for efficient solar-to-fuel conversion require the understanding of exciton and charge carrier dynamics. In this Account, we summarize our recent studies of ultrafast charge separation and recombination kinetics and their effects on steady-state photocatalytic efficiencies of colloidal CdS and CdSe/CdS NRs and related NR-Pt heterostructures. After a brief introduction of their electronic structure, we discuss exciton dynamics of CdS NRs. By transient absorption and time-resolved photoluminescence decay, it is shown that although the conduction band electrons are long-lived, photogenerated holes in CdS NRs are trapped on an ultrafast time scale (∼0.7 ps), which forms localized excitons due to strong Coulomb interaction in 1D NRs. In quasi-type II CdSe/CdS dot-in-rod NRs, a large valence band offset drives the ultrafast localization of holes to the CdSe core, and the competition between this process and ultrafast hole trapping on a CdS rod leads to three types of exciton species with distinct spatial distributions. The effect of the exciton dynamics on photoreduction reactions is illustrated using methyl viologen (MV(2+)) as a model electron acceptor. The steady-state MV(2+) photoreduction quantum yield of CdSe/CdS dot-in-rod NRs approaches unity under rod excitation, much larger than CdSe QDs and CdSe/CdS core/shell QDs. Detailed time-resolved studies show that in quasi-type II CdSe/CdS NRs and type II ZnSe/CdS NRs strong quantum confinement in the radial direction facilitates fast electron transfer and hole removal, whereas the fast carrier mobility along the axial direction enables long distance charge separation and slow charge recombination, which is essential for efficient MV(2+) photoreduction. The NR/MV(2+) relay system can be coupled to Pt nanoparticles in solution for light-driven H2 generation. Alternatively, Pt-tipped CdS and CdSe/CdS NRs provide fully integrated all inorganic systems for light-driven H2 generation. In CdS-Pt and CdSe/CdS-Pt hetero-NRs, ultrafast hole trapping on the CdS rod surface or in CdSe core enables efficient electron transfer from NRs to Pt tips by suppressing hole and energy transfer. It is shown that the quantum yields of photodriven H2 generation using these heterostructures correlate well with measured hole transfer rates from NRs to sacrificial donors, revealing that hole removal is the key efficiency-limiting step. These findings provide important insights for designing more efficient quantum confined NR and NR-Pt based systems for solar-to-fuel conversion.

Solids and nutrient removal from flushed swine manure using polyacrylamides

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

Vanotti, M.B.; Hunt, P.G.

1999-12-01

Most of the organic nutrients and reduced carbon (C) materials in liquid swine manure are contained in fine suspended particles that are not separated by available mechanical separators. Treatment with polyacrylamide (PAM) polymers prior to mechanical removal or gravity settling has the potential for enhancing solids-liquid separation, thus concentrating nitrogen (N), phosphorus (P), and organic C. In this work, the authors determined PAM charge and density characteristics most desirable for swine wastewater applications and established the optimum chemical requirement. Treatments were applied to flushed manure from two swine operations in North Carolina. Cationic PAMs significantly increased solids separation while performancemore » of neutral and anionic types was not different from a control. Cationic PAMs with moderate-charge density (20%) were more effective than polymers with higher charge density. Flocs were large and effectively retained with a 1-mm screen. Optimum PAM rate varied with the amount of total suspended solids (TSS) in the liquid manure; 26 and 79 mg PAM/L for samples containing 1.5 and 4.1 g TSS/L, respectively. Corresponding TSS removal efficiencies were 90 to 94%. In contrast, screening without PAM treatment captured only 5 to 14% of the suspended solids. Polymer usage rate was consistent and averaged 2.0{degree} based on weight of dry solids produced. Volatile suspended solids (VSS) were highly correlated with TSS and comprised 79.5% of TSS. Chemical oxygen demand (COD) and organic nutrient concentrations in the effluent were also significantly decreased by PAM treatment. The decrease of COD concentration, an important consideration for odor control, was linearly related with removal of suspended solids, at a rate of 2.0 g COD/g TSS and 2.6 g COD/g VSS. Removal efficiency of organic N and P followed approximately a 1:1 relationship with removal efficiency of TSS. Chemical cost to capture 90% of the suspended solids was estimated to be $0.026 per hog per day ($2.79 per finished hog). Results obtained indicate that PAM treatment is very effective for removal of manure solids, COD, and organic nutrients from flushed swine effluents. The technology provides an attractive alternative to existing liquid manure handling methods for conserving nutrients and avoiding excessive nutrient application in areas where swine production is concentrated.« less

Self-Assembly Strategies for Integrating Light Harvesting and Charge Separation in Artificial Photosynthetic Systems

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

Wasielewski, Michael R.

In natural photosynthesis, organisms optimize solar energy conversion through organized assemblies of photofunctional chromophores and catalysts within proteins that provide specifically tailored environments for chemical reactions. As with their natural counterparts, artificial photosynthetic systems for practical solar fuels production must collect light energy, separate charge, and transport charge to catalytic sites where multielectron redox processes will occur. While encouraging progress has been made on each aspect of this complex problem, researchers have not yet developed self-ordering and self-assembling components and the tailored environments necessary to realize a fully-functional artificial system. Previously researchers have used complex, covalent molecular systems comprised ofmore » chromophores, electron donors, and electron acceptors to mimic both the light-harvesting and the charge separation functions of photosynthetic proteins. These systems allow for study of the dependencies of electron transfer rate constants on donor?acceptor distance and orientation, electronic interaction, and the free energy of the reaction. The most useful and informative systems are those in which structural constraints control both the distance and the orientation between the electron donors and acceptors. Self-assembly provides a facile means for organizing large numbers of molecules into supramolecular structures that can bridge length scales from nanometers to macroscopic dimensions. The resulting structures must provide pathways for migration of light excitation energy among antenna chromophores, and from antennas to reaction centers. They also must incorporate charge conduits, that is, molecular 'wires' that can efficiently move electrons and holes between reaction centers and catalytic sites. The central scientific challenge is to develop small, functional building blocks with a minimum number of covalent linkages, which also have the appropriate molecular recognition properties to facilitate self-assembly of complete, functional artificial photosynthetic systems. In this Account, we explore how self-assembly strategies involving ?-stacking can be used to integrate light harvesting with charge separation and transport.« less

Direct evidence of charge separation in a metal-organic framework: efficient and selective photocatalytic oxidative coupling of amines via charge and energy transfer.

PubMed

Xu, Caiyun; Liu, Hang; Li, Dandan; Su, Ji-Hu; Jiang, Hai-Long

2018-03-28

The selective aerobic oxidative coupling of amines under mild conditions is an important laboratory and commercial procedure yet a great challenge. In this work, a porphyrinic metal-organic framework, PCN-222, was employed to catalyze the reaction. Upon visible light irradiation, the semiconductor-like behavior of PCN-222 initiates charge separation, evidently generating oxygen-centered active sites in Zr-oxo clusters indicated by enhanced porphyrin π-cation radical signals. The photogenerated electrons and holes further activate oxygen and amines, respectively, to give the corresponding redox products, both of which have been detected for the first time. The porphyrin motifs generate singlet oxygen based on energy transfer to further promote the reaction. As a result, PCN-222 exhibits excellent photocatalytic activity, selectivity and recyclability, far superior to its organic counterpart, for the reaction under ambient conditions via combined energy and charge transfer.

A submicron device to rectify a square-wave angular velocity.

PubMed

Moradian, A; Miri, M F

2011-02-01

We study a system composed of two thick dielectric disks separated by a thin layer of an electrolyte solution. Initially both plates have the same surface charge distribution. The surface charge distribution has no rotational symmetry. We show that the top plate experiences a torque [Formula: see text]([Formula: see text]) if it rotates about its axis by an angle [Formula: see text] . The torque can be controlled by varying the electrolyte concentration, the separation and the surface charge density of the plates. For a specific example of charged rods attached to the plates, we find [Formula: see text]([Formula: see text]) [Formula: see text] sin(4[Formula: see text]) . We also study the dynamics of the system. We consider the case where the angular velocity of the bottom disk is a square-wave signal. We find that the average angular velocity of the top disk is not zero.

Emergence of a Stern Layer from the Incorporation of Hydration Interactions into the Gouy-Chapman Model of the Electrical Double Layer.

PubMed

Brown, Matthew A; Bossa, Guilherme Volpe; May, Sylvio

2015-10-27

In one of the most commonly used phenomenological descriptions of the electrical double layer, a charged solid surface and a diffuse region of mobile ions are separated from each other by a thin charge-depleted Stern layer. The Stern layer acts as a capacitor that improves the classical Gouy-Chapman model by increasing the magnitude of the surface potential and limiting the maximal counterion concentration. We show that very similar Stern-like properties of the diffuse double layer emerge naturally from adding a nonelectrostatic hydration repulsion to the electrostatic Coulomb potential. The interplay of electrostatic attraction and hydration repulsion of the counterions and the surface leads to the formation of a diffuse counterion layer that remains well separated from the surface. In addition, hydration repulsions between the ions limit and control the maximal ion concentration and widen the width of the diffuse double layer. Our mean-field model, which we express in terms of electrostatic and hydration potentials, is physically consistent and conceptually similar to the classical Gouy-Chapman model. It allows the incorporation of ion specificity, accounts for hydration properties of charged surfaces, and predicts Stern layer properties, which we analyze in terms of the effective size of the hydrated counterions.

Cationic flocculants carrying hydrophobic functionalities: applications for solid/liquid separation.

PubMed

Schwarz, S; Jaeger, W; Paulke, B-R; Bratskaya, S; Smolka, N; Bohrisch, J

2007-07-26

The flocculation behaviors of three series of polycations with narrow molecular weight distributions carrying hydrophobic substituents on their backbones [poly(N-vinylbenzyl-N,N,N-trimethylammonium chloride), poly(N-vinylbenzyl-N,N-dimethyl-N-butylammonium chloride), and poly(N-vinylbenzylpyridinium chloride)] were investigated in dispersions of monodisperse polystyrene latexes and kaolin. Apparently, the charge density of the polycations decreases with increasing substituent hydrophobicity and increasing molecular weight of the polyelectrolytes. The necessary amount of flocculant for phase separation in dispersions with high substrate surface charge densities increases with increasing hydrophobicity of the polyelectrolyte. Nevertheless, the introduction of hydrophobic functionalities is beneficial, resulting in a substantial broadening of the range between the minimum and maximum amounts of flocculant necessary for efficient flocculation (flocculation window). An increase in ionic strength supports this effect. When the substrate has a low charge density, the hydrophobic interactions play a much more significant role in the flocculation process. Here, the minimum efficient doses remained the same for all three polyelectrolytes investigated, but the width of the flocculation window increased as the polycation hydrophobicity and the molecular weight increased. The necessary amount of flocculant increased with an increase in particle size at constant solid content of the dispersion, as well as with a decreasing number of particles at a constant particle size.

Influence of polarization and self-polarization charges on impurity binding energy in spherical quantum dot with parabolic confinement

NASA Astrophysics Data System (ADS)

Sarkar, Supratik; Sarkar, Samrat; Bose, Chayanika

2018-07-01

We present a general formulation of the ground state binding energy of a shallow hydrogenic impurity in spherical quantum dot with parabolic confinement, considering the effects of polarization and self energy. The variational approach within the effective mass approximation is employed here. The binding energy of an on-center impurity is computed for a GaAs/AlxGa1-xAs quantum dot as a function of the dot size with the dot barrier as parameter. The influence of polarization and self energy are also treated separately. Results indicate that the binding energy increases due to the presence of polarization charge, while decreases due to the self energy of the carrier. An overall enhancement in impurity binding energy, especially for small dots is noted.

A simulated lightning effects test facility for testing live and inert missiles and components

NASA Technical Reports Server (NTRS)

Craven, Jeffery D.; Knaur, James A.; Moore, Truman W., Jr.; Shumpert, Thomas H.

1991-01-01

Details of a simulated lightning effects test facility for testing live and inert missiles, motors, and explosive components are described. The test facility is designed to simulate the high current, continuing current, and high rate-of-rise current components of an idealized direct strike lightning waveform. The Lightning Test Facility was in operation since May, 1988, and consists of: 3 separate capacitor banks used to produce the lightning test components; a permanently fixed large steel safety cage for retaining the item under test (should it be ignited during testing); an earth covered bunker housing the control/equipment room; a charge/discharge building containing the charging/discharging switching; a remotely located blockhouse from which the test personnel control hazardous testing; and interconnecting cables.

Magnetic field effect on the optoelectronic response of amorphous hydrogenated silicon

NASA Astrophysics Data System (ADS)

McLaughlin, Ryan; Sun, Dali; Zhang, Chuang; Ehrenfreund, Eitan; Vardeny, Zeev Valy

We have studied the magneto-photoluminescence and magneto photoconductivity in amorphous hydrogenated silicon (a-Si:H) thin films and devices as a function of temperature up to field of 5 Tesla. The magnetic field effects (MFE) are interpreted as spin mixing between spin-singlet and spin-triplet charge pairs due to the ''delta- g'' mechanism that is based on the g-value difference between the paired electron and hole, which directly affects the rate of radiative recombination and charge carrier separation, respectively. We found that the MFE(B) response does not form a Lorentzian (that is expected from the ''delta- g'' mechanism) due to disorder in the film that results in a broad distribution of e-h recombination rates, which could be extracted directly by time-resolved photoluminescence.

Swelling of biological and semiflexible polyelectrolytes.

PubMed

Dobrynin, Andrey V; Carrillo, Jan-Michael Y

2009-10-21

We have developed a theoretical model of swelling of semiflexible (biological) polyelectrolytes in salt solutions. Our approach is based on separation of length scales which allowed us to split a chain's electrostatic energy into two parts that describe local and remote electrostatic interactions along the polymer backbone. The local part takes into account interactions between charged monomers that are separated by distances along the polymer backbone shorter than the chain's persistence length. These electrostatic interactions renormalize chain persistence length. The second part includes electrostatic interactions between remote charged pairs along the polymer backbone located at distances larger than the chain persistence length. These interactions are responsible for chain swelling. In the framework of this approach we calculated effective chain persistence length and chain size as a function of the Debye screening length, chain degree of ionization, bare persistence length and chain degree of polymerization. Our crossover expression for the effective chain's persistence length is in good quantitative agreement with the experimental data on DNA. We have been able to fit experimental datasets by using two adjustable parameters: DNA ionization degree (α = 0.15-0.17) and a bare persistence length (l(p) = 40-44 nm).

Multibit Polycristalline Silicon-Oxide-Silicon Nitride-Oxide-Silicon Memory Cells with High Density Designed Utilizing a Separated Control Gate

NASA Astrophysics Data System (ADS)

Rok Kim, Kyeong; You, Joo Hyung; Dal Kwack, Kae; Kim, Tae Whan

2010-10-01

Unique multibit NAND polycrystalline silicon-oxide-silicon nitride-oxide-silicon (SONOS) memory cells utilizing a separated control gate (SCG) were designed to increase memory density. The proposed NAND SONOS memory device based on a SCG structure was operated as two bits, resulting in an increase in the storage density of the NVM devices in comparison with conventional single-bit memories. The electrical properties of the SONOS memory cells with a SCG were investigated to clarify the charging effects in the SONOS memory cells. When the program voltage was supplied to each gate of the NAND SONOS flash memory cells, the electrons were trapped in the nitride region of the oxide-nitride-oxide layer under the gate to supply the program voltage. The electrons were accumulated without affecting the other gate during the programming operation, indicating the absence of cross-talk between two trap charge regions. It is expected that the inference effect will be suppressed by the lower program voltage than the program voltage of the conventional NAND flash memory. The simulation results indicate that the proposed unique NAND SONOS memory cells with a SCG can be used to increase memory density.

Separability of massive field equations for spin-0 and spin-1/2 charged particles in the general nonextremal rotating charged black hole spacetimes in minimal five-dimensional gauged supergravity

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

Wu Shuangqing

We continue to investigate the separability of massive field equations for spin-0 and spin-1/2 charged particles in the general, nonextremal, rotating, charged, Chong-Cvetic-Lue-Pope black holes with two independent angular momenta and a nonzero cosmological constant in minimal D=5 gauged supergravity theory. We show that the complex Klein-Gordon equation and the modified Dirac equation with the inclusion of an extra counterterm can be separated by variables into purely radial and purely angular parts in this general Einstein-Maxwell-Chern-Simons background spacetime. A second-order symmetry operator that commutes with the complex Laplacian operator is constructed from the separated solutions and expressed compactly in termsmore » of a rank-2 Staeckel-Killing tensor which admits a simple diagonal form in the chosen pentad one-forms so that it can be understood as the square of a rank-3 totally antisymmetric tensor. A first-order symmetry operator that commutes with the modified Dirac operator is expressed in terms of a rank-3 generalized Killing-Yano tensor and its covariant derivative. The Hodge dual of this generalized Killing-Yano tensor is a generalized principal conformal Killing-Yano tensor of rank-2, which can generate a 'tower' of generalized (conformal) Killing-Yano and Staeckel-Killing tensors that are responsible for the whole hidden symmetries of this general, rotating, charged, Kerr-anti-de Sitter black hole geometry. In addition, the first laws of black hole thermodynamics have been generalized to the case that the cosmological constant can be viewed as a thermodynamical variable.« less

Trapping in irradiated p +-n-n - silicon sensors at fluences anticipated at the HL-LHC outer tracker

DOE PAGES

Adam, W.

2016-04-22

The degradation of signal in silicon sensors is studied under conditions expected at the CERN High-Luminosity LHC. 200μm thick n-type silicon sensors are irradiated with protons of different energies to fluences of up to 3 x 10 15 neq/cm 2. Pulsed red laser light with a wavelength of 672 nm is used to generate electron-hole pairs in the sensors. The induced signals are used to determine the charge collection efficiencies separately for electrons and holes drifting through the sensor. The effective trapping rates are extracted by comparing the results to simulation. The electric field is simulated using Synopsys device simulationmore » assuming two effective defects. The generation and drift of charge carriers are simulated in an independent simulation based on PixelAV. The effective trapping rates are determined from the measured charge collection efficiencies and the simulated and measured time-resolved current pulses are compared. Furthermore, the effective trapping rates determined for both electrons and holes are about 50% smaller than those obtained using standard extrapolations of studies at low fluences and suggests an improved tracker performance over initial expectations.« less

Direct observation of metal nanoparticles as heterogeneous nuclei for the condensation of supersaturated organic vapors: nucleation of size-selected aluminum nanoparticles in acetonitrile and n-hexane vapors.

PubMed

Abdelsayed, Victor; El-Shall, M Samy

2014-08-07

This work reports the direct observation and separation of size-selected aluminum nanoparticles acting as heterogeneous nuclei for the condensation of supersaturated vapors of both polar and nonpolar molecules. In the experiment, we study the condensation of supersaturated acetonitrile and n-hexane vapors on charged and neutral Al nanoparticles by activation of the metal nanoparticles to act as heterogeneous nuclei for the condensation of the organic vapor. Aluminum seed nanoparticles with diameters of 1 and 2 nm are capable of acting as heterogeneous nuclei for the condensation of supersaturated acetonitrile and hexane vapors. The comparison between the Kelvin and Fletcher diameters indicates that for the heterogeneous nucleation of both acetonitrile and hexane vapors, particles are activated at significantly smaller sizes than predicted by the Kelvin equation. The activation of the Al nanoparticles occurs at nearly 40% and 65% of the onset of homogeneous nucleation of acetonitrile and hexane supersaturated vapors, respectively. The lower activation of the charged Al nanoparticles in acetonitrile vapor is due to the charge-dipole interaction which results in rapid condensation of the highly polar acetonitrile molecules on the charged Al nanoparticles. The charge-dipole interaction decreases with increasing the size of the Al nanoparticles and therefore at low supersaturations, most of the heterogeneous nucleation events are occurring on neutral nanoparticles. No sign effect has been observed for the condensation of the organic vapors on the positively and negatively charged Al nanoparticles. The present approach of generating metal nanoparticles by pulsed laser vaporization within a supersaturated organic vapor allows for efficient separation between nucleation and growth of the metal nanoparticles and, consequently controls the average particle size, particle density, and particle size distribution within the liquid droplets of the condensing vapor. Strong correlation is found between the seed nanoparticle's size and the degree of the supersaturation of the condensing vapor. This result and the agreement among the calculated Kelvin diameters and the size of the nucleating Al nanoparticles determined by transmission electron microscopy provide strong proof for the development of a new approach for the separation and characterization of heterogeneous nuclei formed in organic vapors. These processes can take place in the atmosphere by a combination of several organic species including polar compounds which could be very efficient in activating charged nanoparticles and cluster ions of atmospheric relevance.

Direct observation of metal nanoparticles as heterogeneous nuclei for the condensation of supersaturated organic vapors: Nucleation of size-selected aluminum nanoparticles in acetonitrile and n-hexane vapors

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

Abdelsayed, Victor; Samy El-Shall, M., E-mail: mselshal@vcu.edu

This work reports the direct observation and separation of size-selected aluminum nanoparticles acting as heterogeneous nuclei for the condensation of supersaturated vapors of both polar and nonpolar molecules. In the experiment, we study the condensation of supersaturated acetonitrile and n-hexane vapors on charged and neutral Al nanoparticles by activation of the metal nanoparticles to act as heterogeneous nuclei for the condensation of the organic vapor. Aluminum seed nanoparticles with diameters of 1 and 2 nm are capable of acting as heterogeneous nuclei for the condensation of supersaturated acetonitrile and hexane vapors. The comparison between the Kelvin and Fletcher diameters indicatesmore » that for the heterogeneous nucleation of both acetonitrile and hexane vapors, particles are activated at significantly smaller sizes than predicted by the Kelvin equation. The activation of the Al nanoparticles occurs at nearly 40% and 65% of the onset of homogeneous nucleation of acetonitrile and hexane supersaturated vapors, respectively. The lower activation of the charged Al nanoparticles in acetonitrile vapor is due to the charge-dipole interaction which results in rapid condensation of the highly polar acetonitrile molecules on the charged Al nanoparticles. The charge-dipole interaction decreases with increasing the size of the Al nanoparticles and therefore at low supersaturations, most of the heterogeneous nucleation events are occurring on neutral nanoparticles. No sign effect has been observed for the condensation of the organic vapors on the positively and negatively charged Al nanoparticles. The present approach of generating metal nanoparticles by pulsed laser vaporization within a supersaturated organic vapor allows for efficient separation between nucleation and growth of the metal nanoparticles and, consequently controls the average particle size, particle density, and particle size distribution within the liquid droplets of the condensing vapor. Strong correlation is found between the seed nanoparticle's size and the degree of the supersaturation of the condensing vapor. This result and the agreement among the calculated Kelvin diameters and the size of the nucleating Al nanoparticles determined by transmission electron microscopy provide strong proof for the development of a new approach for the separation and characterization of heterogeneous nuclei formed in organic vapors. These processes can take place in the atmosphere by a combination of several organic species including polar compounds which could be very efficient in activating charged nanoparticles and cluster ions of atmospheric relevance.« less

Ion-mediated interactions in suspensions of oppositely charged nanoparticles

NASA Astrophysics Data System (ADS)

Dahirel, Vincent; Hansen, Jean Pierre

2009-08-01

The structure of oppositely charged spherical nanoparticles (polyions), dispersed in ionic solutions with continuous solvent (primitive model), is investigated by Monte Carlo (MC) simulations, within explicit and implicit microion representations, over a range of polyion valences and densities, and microion concentrations. Systems with explicit microions are explored by semigrand canonical MC simulations, and allow density-dependent effective polyion pair potentials vαβeff(r ) to be extracted from measured partial pair distribution functions. Implicit microion MC simulations are based on pair potentials of mean force vαβ(2)(r ) computed by explicit microion simulations of two charged polyions, in the low density limit. In the vicinity of the liquid-gas separation expected for oppositely charged polyions, the implicit microion representation leads to an instability against density fluctuations for polyion valences |Z| significantly below those at which the instability sets in within the exact explicit microion representation. Far from this instability region, the vαβ(2)(r ) are found to be fairly close to but consistently more repulsive than the effective pair potentials vαβeff(r ). This is corroborated by additional calculations of three-body forces between polyion triplets, which are repulsive when one polyion is of opposite charge to the other two. The explicit microion MC data were exploited to determine the ratio of salt concentrations c and co within the dispersion and the reservoir (Donnan effect). c /co is found to first increase before finally decreasing as a function of the polyion packing fraction.

Photoinitated charge separation in a hybrid titanium dioxide metalloporphyrin peptide material

NASA Astrophysics Data System (ADS)

Fry, H. Christopher; Liu, Yuzi; Dimitrijevic, Nada M.; Rajh, Tijana

2014-08-01

In natural systems, electron flow is mediated by proteins that spatially organize donor and acceptor molecules with great precision. Achieving this guided, directional flow of information is a desirable feature in photovoltaic media. Here, we design self-assembled peptide materials that organize multiple electronic components capable of performing photoinduced charge separation. Two peptides, c16-AHL3K3-CO2H and c16-AHL3K9-CO2H, self-assemble into fibres and provide a scaffold capable of binding a metalloporphyrin via histidine axial ligation and mineralize titanium dioxide (TiO2) on the lysine-rich surface of the resulting fibrous structures. Electron paramagnetic resonance studies of this self-assembled material under continuous light excitation demonstrate charge separation induced by excitation of the metalloporphyrin and mediated by the peptide assembly structure. This approach to dye-sensitized semiconducting materials offers a means to spatially control the dye molecule with respect to the semiconducting material through careful, strategic peptide design.

Charge separation and carrier dynamics in donor-acceptor heterojunction photovoltaic systems.

PubMed

Teuscher, Joël; Brauer, Jan C; Stepanov, Andrey; Solano, Alicia; Boziki, Ariadni; Chergui, Majed; Wolf, Jean-Pierre; Rothlisberger, Ursula; Banerji, Natalie; Moser, Jacques-E

2017-11-01

Electron transfer and subsequent charge separation across donor-acceptor heterojunctions remain the most important areas of study in the field of third-generation photovoltaics. In this context, it is particularly important to unravel the dynamics of individual ultrafast processes (such as photoinduced electron transfer, carrier trapping and association, and energy transfer and relaxation), which prevail in materials and at their interfaces. In the frame of the National Center of Competence in Research "Molecular Ultrafast Science and Technology," a research instrument of the Swiss National Science Foundation, several groups active in the field of ultrafast science in Switzerland have applied a number of complementary experimental techniques and computational simulation tools to scrutinize these critical photophysical phenomena. Structural, electronic, and transport properties of the materials and the detailed mechanisms of photoinduced charge separation in dye-sensitized solar cells, conjugated polymer- and small molecule-based organic photovoltaics, and high-efficiency lead halide perovskite solar energy converters have been scrutinized. Results yielded more than thirty research articles, an overview of which is provided here.

New Techniques to Evaluate the Incendiary Behavior of Insulators

NASA Technical Reports Server (NTRS)

Buhler, Charles; Calle, Carlos; Clements, Sid; Trigwell, Steve; Ritz, Mindy

2008-01-01

New techniques for evaluating the incendiary behavior of insulators is presented. The onset of incendive brush discharges in air is evaluated using standard spark probe techniques for the case simulating approaches of an electrically grounded sphere to a charged insulator in the presence of a flammable atmosphere. However, this standard technique is unsuitable for the case of brush discharges that may occur during the charging-separation process for two insulator materials. We present experimental techniques to evaluate this hazard in the presence of a flammable atmosphere which is ideally suited to measure the incendiary nature of micro-discharges upon separation, a measurement never before performed. Other measurement techniques unique to this study include; surface potential measurements of insulators before, during and after contact and separation, as well as methods to verify fieldmeter calibrations using a charge insulator surface opposed to standard high voltage plates. Key words: Kapton polyimide film, incendiary discharges, brush discharges, contact and frictional electrification, ignition hazards, insulators, contact angle, surface potential measurements.

Voltage-dependent gating and gating charge measurements in the Kv1.2 potassium channel

PubMed Central

Ishida, Itzel G.; Rangel-Yescas, Gisela E.; Carrasco-Zanini, Julia

2015-01-01

Much has been learned about the voltage sensors of ion channels since the x-ray structure of the mammalian voltage-gated potassium channel Kv1.2 was published in 2005. High resolution structural data of a Kv channel enabled the structural interpretation of numerous electrophysiological findings collected in various ion channels, most notably Shaker, and permitted the development of meticulous computational simulations of the activation mechanism. The fundamental premise for the structural interpretation of functional measurements from Shaker is that this channel and Kv1.2 have the same characteristics, such that correlation of data from both channels would be a trivial task. We tested these assumptions by measuring Kv1.2 voltage-dependent gating and charge per channel. We found that the Kv1.2 gating charge is near 10 elementary charges (eo), ∼25% less than the well-established 13–14 eo in Shaker. Next, we neutralized positive residues in the Kv1.2 S4 transmembrane segment to investigate the cause of the reduction of the gating charge and found that, whereas replacing R1 with glutamine decreased voltage sensitivity to ∼50% of the wild-type channel value, mutation of the subsequent arginines had a much smaller effect. These data are in marked contrast to the effects of charge neutralization in Shaker, where removal of the first four basic residues reduces the gating charge by roughly the same amount. In light of these differences, we propose that the voltage-sensing domains (VSDs) of Kv1.2 and Shaker might undergo the same physical movement, but the septum that separates the aqueous crevices in the VSD of Kv1.2 might be thicker than Shaker’s, accounting for the smaller Kv1.2 gating charge. PMID:25779871

Design and Synthesis of Novel Block Copolymers for Efficient Opto-Electronic Applications

NASA Technical Reports Server (NTRS)

Sun, Sam-Shajing; Fan, Zhen; Wang, Yiqing; Taft, Charles; Haliburton, James; Maaref, Shahin

2002-01-01

It has been predicted that nano-phase separated block copolymer systems containing electron rich donor blocks and electron deficient acceptor blocks may facilitate the charge carrier separation and migration in organic photovoltaic devices due to improved morphology in comparison to polymer blend system. This paper presents preliminary data describing the design and synthesis of a novel Donor-Bridge-Acceptor (D-B-A) block copolymer system for potential high efficient organic optoelectronic applications. Specifically, the donor block contains an electron donating alkyloxy derivatized polyphenylenevinylene (PPV), the acceptor block contains an electron withdrawing alkyl-sulfone derivatized polyphenylenevinylene (PPV), and the bridge block contains an electronically neutral non-conjugated aliphatic hydrocarbon chain. The key synthetic strategy includes the synthesis of each individual block first, then couple the blocks together. While the donor block stabilizes and facilitates the transport of the holes, the acceptor block stabilizes and facilitates the transport of the electrons, the bridge block is designed to hinder the probability of electron-hole recombination. Thus, improved charge separation and stability are expected with this system. In addition, charge migration toward electrodes may also be facilitated due to the potential nano-phase separated and highly ordered block copolymer ultra-structure.

Cadmium migration in aerospace nickel cadmium cells

NASA Technical Reports Server (NTRS)

Mcdermott, P. P.

1976-01-01

The effects of temperature, the nature of separator material, charge and discharge, carbonate contamination, and the mode of storage are studied with respect to the migration of active material from the negative toward the positive plate. A theoretical model is proposed which takes into account the solubility of cadmium in various concentrations of hydroxide and carbonate at different temperatures, the generation of the cadmiate ion, Cd(OH)3(-), during discharge, the migration of the cadmiate ion and particulate Cd(OH)2 due to electrophoretic effects and the movement of electrolyte in and out of the negative plate and, finally, the recrystallization of cadmiate ion in the separator as Cd(OH)2. Application of the theoretical model to observations of cadmium migration in cycled cells is also discussed.

Fine mist versus large droplets in phase separated manganites

NASA Astrophysics Data System (ADS)

Khomskii, D.; Khomskii, L.

2003-02-01

The properties of phase-separated systems, e.g., manganites close to a first-order phase transition between charge-ordered insulator and ferromagnetic metal, are usually described by percolation picture. We argue that the correlated occupation of metallic sites leads to the preferential formation of larger metallic clusters, and their size distribution depends on the thermal history. This can explain several puzzling effects in manganites, such as the often observed inverse, or “overshot” hysteresis, and the recently discovered thermal cycling effect. Thus in treating this and similar systems in percolation picture, not only the total concentration of metallic phase, but also the distribution of metallic clusters by shape and size may significantly influence the properties of the system and has to be taken into account.

The Rocket Electric Field Sounding (REFS) Program: Prototype Design and Successful First Launch

DTIC Science & Technology

1992-01-15

insulators surrounding the stators, and stator edges themselves, are fully covered by the rotor , so that any effects of charge on the insulators are...Jumper performed a separate analysis of the aerodynamics (primarily the " Magnus effect ") induced by the relative rotation of rocket body and shell. The...significant advantages over an aircraft in simplicity and calibration. A single cylindrical rotor covering most of the payload acts as the shutter for all

Through-Space Charge Interaction Substituent Effects in Molecular Catalysis Leading to the Design of the Most Efficient Catalyst of CO2-to-CO Electrochemical Conversion.

PubMed

Azcarate, Iban; Costentin, Cyrille; Robert, Marc; Savéant, Jean-Michel

2016-12-28

The starting point of this study of through-space substituent effects on the catalysis of the electrochemical CO 2 -to-CO conversion by iron(0) tetraphenylporphyrins is the linear free energy correlation between through-structure electronic effects and the iron(I/0) standard potential that we established separately. The introduction of four positively charged trimethylanilinium groups at the para positions of the tetraphenylporphyrin (TPP) phenyls results in an important positive deviation from the correlation and a parallel improvement of the catalytic Tafel plot. The assignment of this catalysis boosting effect to the Coulombic interaction of these positive charges with the negative charge borne by the initial Fe 0 -CO 2 adduct is confirmed by the negative deviation observed when the four positive charges are replaced by four negative charges borne by sulfonate groups also installed in the para positions of the TPP phenyls. The climax of this strategy of catalysis boosting by means of Coulombic stabilization of the initial Fe 0 -CO 2 adduct is reached when four positively charged trimethylanilinium groups are introduced at the ortho positions of the TPP phenyls. The addition of a large concentration of a weak acid-phenol-helps by cleaving one of the C-O bonds of CO 2 . The efficiency of the resulting catalyst is unprecedented, as can be judged by the catalytic Tafel plot benchmarking with all presently available catalysts of the electrochemical CO 2 -to-CO conversion. The maximal turnover frequency (TOF) is as high as 10 6 s -1 and is reached at an overpotential of only 220 mV; the extrapolated TOF at zero overpotential is larger than 300 s -1 . This catalyst leads to a highly selective formation of CO (practically 100%) in spite of the presence of a high concentration of phenol, which could have favored H 2 evolution. It is also very stable, showing no significant alteration after more than 80 h of electrolysis.

Engine Tune-up Service. Unit 2: Charging System. Review Exercise Book. Automotive Mechanics Curriculum.

ERIC Educational Resources Information Center

Richardson, Roger L.; Bacon, E. Miles

This book of pretests and review exercises is designed to accompany the Engine Tune-Up Service Student Guide for Unit 2, Charging System, available separately as CE 031 208. Focus of the exercises and pretests is testing the charging system. Pretests and performance checklists are provided for each of the three performance objectives contained in…

Engine Tune-up Service. Unit 2: Charging System. Posttests. Automotive Mechanics Curriculum.

ERIC Educational Resources Information Center

Richardson, Roger L.; Bacon, E. Miles

This book of posttests is designed to accompany the Engine Tune-Up Service Student Guide for Unit 2, Charging System, available separately as CE 031 208. Focus of the posttest is on the testing of the charging system. One multiple choice posttest is provided, that covers the three performance objectives contained in the unit. (No answer key is…

26 CFR 48.4216(a)-1 - Charges to be included in sale price.

Code of Federal Regulations, 2010 CFR

2010-04-01

... sales promotion programs, or otherwise. With respect to the rules relating to exclusion (in the case of... section 4216(e) and § 48.4216(e)-1. In the case of sales on credit, a carrying, finance, or service charge... communication in connection with collection). (b) Tools and dies. Separate charges for tools and dies used in...

Hot kinetic model as a guide to improve organic photovoltaic materials.

PubMed

Sosorev, Andrey Yu; Godovsky, Dmitry Yu; Paraschuk, Dmitry Yu

2018-01-31

The modeling of organic solar cells (OSCs) can provide a roadmap for their further improvement. Many OSC models have been proposed in recent years; however, the impact of the key intermediates from photons to electricity-hot charge-transfer (CT) states-on the OSC efficiency is highly ambiguous. In this study, we suggest an analytical kinetic model for OSC that considers a two-step charge generation via hot CT states. This hot kinetic model allowed us to evaluate the impact of different material parameters on the OSC performance: the driving force for charge separation, optical bandgap, charge mobility, geminate recombination rate, thermalization rate, average electron-hole separation distance in the CT state, dielectric permittivity, reorganization energy and charge delocalization. In contrast to a widespread trend of lowering the material bandgap, the model predicts that this approach is only efficient along with improvement of the other material properties. The most promising ways to increase the OSC performance are decreasing the reorganization energy, i.e., an energy change accompanying CT from the donor molecule to the acceptor, increasing the dielectric permittivity and charge delocalization. The model suggests that there are no fundamental limitations that can prevent achieving the OSC efficiency above 20%.

Modulating interactions between ligand-coated nanoparticles and phase-separated lipid bilayers by varying the ligand density and the surface charge.

PubMed

Chen, Xiaojie; Tieleman, D Peter; Liang, Qing

2018-02-01

The interactions between nanoparticles and lipid bilayers are critical in applications of nanoparticles in nanomedicine, cell imaging, toxicology, and elsewhere. Here, we investigate the interactions between nanoparticles coated with neutral and/or charged ligands and phase-separated lipid bilayers using coarse-grained molecular dynamics simulation. Both penetration and adsorption processes as well as the final distribution of the nanoparticles can be readily modulated by varying the ligand density and the surface charge of the nanoparticles. Completely hydrophobic (neutral) nanoparticles with larger size initially preferentially penetrate into the liquid-disordered region of the lipid bilayer and finally transfer into the liquid-ordered region; partially hydrophilic nanoparticles with low or moderate surface charge tend to either distribute in the liquid-disordered region or be adsorbed on the surface of the lipid bilayer, while strongly hydrophilic nanoparticles with high surface charge always reside on the surface of the lipid bilayer. Interactions of the nanoparticles with the lipid bilayers are affected by the surface charge of nanoparticles, hydrophobic mismatch, bending of the ligands, and the packing state of the lipids. Insight in these factors can be used to improve the efficiency of designing nanoparticles for specific applications.

Combined electrophoretic-separation and electrospray method and system

DOEpatents

Smith, R.D.; Olivares, J.A.

1989-06-27

A system and method for analyzing molecular constituents of a composition sample includes: forming a solution of the sample, separating the solution by capillary zone electrophoresis into an eluent of constituents longitudinally separated according to their relative electrophoretic mobilities, electrospraying the eluent to form a charged spray in which the molecular constituents have a temporal distribution; and detecting or collecting the separated constituents in accordance with the temporal distribution in the spray. A first high-voltage (e.g., 5--100 kVDC) is applied to the solution. The spray is charged by applying a second high voltage (e.g., [+-]2--8 kVDC) between the eluent at the capillary exit and a cathode spaced in front of the exit. A complete electrical circuit is formed by a conductor which directly contacts the eluent at the capillary exit. 10 figs.

Using Ion Exchange Chromatography to Separate and Quantify Complex Ions

ERIC Educational Resources Information Center

Johnson, Brian J.

2014-01-01

Ion exchange chromatography is an important technique in the separation of charged species, particularly in biological, inorganic, and environmental samples. In this experiment, students are supplied with a mixture of two substitution-inert complex ions. They separate the complexes by ion exchange chromatography using a "flash"…

Ru–protein–Co biohybrids designed for solar hydrogen production: understanding electron transfer pathways related to photocatalytic function† †Electronic supplementary information (ESI) available: Time traces of photocatalysis, additional EPR spectra and parameters, UV-visible spectroscopy data, and kinetic fits of TA traces. See DOI: 10.1039/c6sc03121h Click here for additional data file.

PubMed Central

Soltau, Sarah R.; Dahlberg, Peter D.; Niklas, Jens; Poluektov, Oleg G.; Mulfort, Karen L.

2016-01-01

A series of Ru–protein–Co biohybrids have been prepared using the electron transfer proteins ferredoxin (Fd) and flavodoxin (Fld) as scaffolds for photocatalytic hydrogen production. The light-generated charge separation within these hybrids has been monitored by transient optical and electron paramagnetic resonance spectroscopies. Two distinct electron transfer pathways are observed. The Ru–Fd–Co biohybrid produces up to 650 turnovers of H2 utilizing an oxidative quenching mechanism for Ru(ii)* and a sequential electron transfer pathway via the native [2Fe–2S] cluster to generate a Ru(iii)–Fd–Co(i) charge separated state that lasts for ∼6 ms. In contrast, a direct electron transfer pathway occurs for the Ru–ApoFld–Co biohybrid, which lacks an internal electron relay, generating Ru(i)–ApoFld–Co(i) charge separated state that persists for ∼800 μs and produces 85 turnovers of H2 by a reductive quenching mechanism for Ru(ii)*. This work demonstrates the utility of protein architectures for linking donor and catalytic function via direct or sequential electron transfer pathways to enable stabilized charge separation which facilitates photocatalysis for solar fuel production. PMID:28451142

THE CONTRIBUTIONS OF NORMAL AND ANOMALOUS OSMOSIS TO THE OSMOTIC EFFECTS ARISING ACROSS CHARGED MEMBRANES WITH SOLUTIONS OF ELECTROLYTES

PubMed Central

Grim, Eugene; Sollner, Karl

1957-01-01

The osmotic effect arising across a porous membrane separating the solution of an electrolyte from water (or a more dilute solution) is ordinarily due to both normal osmosis, as it occurs also with non-electrolytes, and to "anomalous" osmosis. It is shown that the normal osmotic component cannot be measured quantitatively by the conventional comparison with a non-electrolytic reference solute. Anomalous osmosis does not occur with electroneutral membranes. Accordingly, with membranes which can be charged and discharged reversibly (without changes in geometrical structure), such as many proteinized membranes, the osmotic effects caused by an electrolyte can be measured both when only normal osmosis arises (with the membrane in the electroneutral state) and when normal as well as anomalous osmosis occurs (with the membrane in a charged state). The difference between these two effects is the true anomalous osmosis. Data are presented on the osmotic effects across an oxyhemoglobin membrane in the uncharged state at pH 6.75 and in two charged states, positive at pH 4.0 and negative at pH 10.0, with solutions of a variety of electrolytes using a concentration ratio of 2:1 over a wide range of concentrations. The rates of the movement of liquid across the membrane against an inconsequentially small hydrostatic head are recorded instead of, as conventional, the physiologically less significant pressure rises after a standard time. PMID:13439166

Microphysical and Kinematic Characteristics of Regions of Flash Initiation in a Supercell Storm and a Multicell Storm Observed During the DC3 Field Program

NASA Astrophysics Data System (ADS)

DiGangi, E.; MacGorman, D. R.; Ziegler, C.; Betten, D.; Biggerstaff, M. I.

2017-12-01

Lightning initiation in thunderstorms requires that the local electric field magnitude exceed breakdown values somewhere, and this tends to occur between regions of positive and negative charge, where the largest electric field magnitudes tend to occur. Past studies have demonstrated that, near updrafts, storms with very strong updrafts tend to elevate regions of charge and of flash initiations higher, as well as to have more flashes initiated by small pockets of charge, than in storms with much weaker updrafts. In all thunderstorms, the source of these charge regions is generally thought to be microscopic charge separation via the relative growth rate noninductive mechanism, followed by macroscopic charge separation via sedimentation, although other charge generation mechanisms can contribute to charge in some regions. Charge generation and lightning initiation are therefore inherently dependent on the microphysical and kinematic characteristics of a given storm. This study compares the results of a hydrometeor classification algorithm applied to C-band mobile radar data with mixing ratios calculated by a diabatic Lagrangian analysis retrieval from the dual-Doppler wind fields for two storms, the 29-30 May 2012 supercell storm and the 21 June 2012 multicell storm, observed during the Deep Convective Clouds and Chemistry experiment. Using these data, we then compare the inferred microphysical and kinematic characteristics of regions in which the Oklahoma Lightning Mapping Array indicated that flashes were initiated in these two very different storms.

An Electrostatic Charge Partitioning Model for the Dissociation of Protein Complexes in the Gas Phase

NASA Astrophysics Data System (ADS)

Sciuto, Stephen V.; Liu, Jiangjiang; Konermann, Lars

2011-10-01

Electrosprayed multi-protein complexes can be dissociated by collisional activation in the gas phase. Typically, these processes follow a mechanism whereby a single subunit gets ejected with a disproportionately high amount of charge relative to its mass. This asymmetric behavior suggests that the departing subunit undergoes some degree of unfolding prior to being separated from the residual complex. These structural changes occur concomitantly with charge (proton) transfer towards the subunit that is being unraveled. Charge accumulation takes place up to the point where the subunit loses physical contact with the residual complex. This work develops a simple electrostatic model for studying the relationship between conformational changes and charge enrichment during collisional activation. Folded subunits are described as spheres that carry continuum surface charge. The unfolded chain is envisioned as random coil bead string. Simulations are guided by the principle that the system will adopt the charge configuration with the lowest potential energy for any backbone conformation. A finite-difference gradient algorithm is used to determine the charge on each subunit throughout the dissociation process. Both dimeric and tetrameric protein complexes are investigated. The model reproduces the occurrence of asymmetric charge partitioning for dissociation events that are preceded by subunit unfolding. Quantitative comparisons of experimental MS/MS data with model predictions yield estimates of the structural changes that occur during collisional activation. Our findings suggest that subunit separation can occur over a wide range of scission point structures that correspond to different degrees of unfolding.

Progressive Design of Plasmonic Metal-Semiconductor Ensemble toward Regulated Charge Flow and Improved Vis-NIR-Driven Solar-to-Chemical Conversion.

PubMed

Han, Chuang; Quan, Quan; Chen, Hao Ming; Sun, Yugang; Xu, Yi-Jun

2017-04-01

Surface plasmon resonance (SPR)-mediated photocatalysis without the bandgap limitations of traditional semiconductor has aroused significant attention in solar-to-chemical energy conversion. However, the photocatalytic efficiency barely initiated by the SPR effects is still challenged by the low concentration and ineffective extraction of energetic hot electrons, slow charge migration rates, random charge diffusion directions, and the lack of highly active sites for redox reactions. Here, the tunable, progressive harvesting of visible-to-near infrared light (vis-NIR, λ > 570 nm) by designing plasmonic Au nanorods and metal (Au, Ag, or Pt) nanoparticle codecorated 1D CdS nanowire (1D CdS NW) ensemble is reported. The intimate integration of these metal nanostructures with 1D CdS NWs promotes the extraction and manipulated directional separation and migration of hot charge carriers in a more effective manner. Such cooperative synergy with tunable control of interfacial interaction, morphology optimization, and cocatalyst strategy results in the distinctly boosted performance for vis-NIR-driven plasmonic photocatalysis. This work highlights the significance of rationally progressive design of plasmonic metal-semiconductor-based composite system for boosting the regulated directional flow of hot charge carrier and thus the more efficient use of broad-spectrum solar energy conversion. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Conserved interdomain linker promotes phase separation of the multivalent adaptor protein Nck

PubMed Central

Banjade, Sudeep; Wu, Qiong; Mittal, Anuradha; Peeples, William B.; Pappu, Rohit V.; Rosen, Michael K.

2015-01-01

The organization of membranes, the cytosol, and the nucleus of eukaryotic cells can be controlled through phase separation of lipids, proteins, and nucleic acids. Collective interactions of multivalent molecules mediated by modular binding domains can induce gelation and phase separation in several cytosolic and membrane-associated systems. The adaptor protein Nck has three SRC-homology 3 (SH3) domains that bind multiple proline-rich segments in the actin regulatory protein neuronal Wiskott-Aldrich syndrome protein (N-WASP) and an SH2 domain that binds to multiple phosphotyrosine sites in the adhesion protein nephrin, leading to phase separation. Here, we show that the 50-residue linker between the first two SH3 domains of Nck enhances phase separation of Nck/N-WASP/nephrin assemblies. Two linear motifs within this element, as well as its overall positively charged character, are important for this effect. The linker increases the driving force for self-assembly of Nck, likely through weak interactions with the second SH3 domain, and this effect appears to promote phase separation. The linker sequence is highly conserved, suggesting that the sequence determinants of the driving forces for phase separation may be generally important to Nck functions. Our studies demonstrate that linker regions between modular domains can contribute to the driving forces for self-assembly and phase separation of multivalent proteins. PMID:26553976

Z-M in Lightning Forecasting

DTIC Science & Technology

2009-03-01

hydrometers create a charge separation. Inductive processes rely on a preexisting external electric field to induce charges on polarized particles, which...frozen hydrometers . A. FLORIDA CLIMATE Florida is often referred to as the lightning capital of the United States (Hodanish et al. 1997) or

Breaking the barriers of all-polymer solar cells: Solving electron transporter and morphology problems

NASA Astrophysics Data System (ADS)

Gavvalapalli, Nagarjuna

All-polymer solar cells (APSC) are a class of organic solar cells in which hole and electron transporting phases are made of conjugated polymers. Unlike polymer/fullerene solar cell, photoactive material of APSC can be designed to have hole and electron transporting polymers with complementary absorption range and proper frontier energy level offset. However, the highest reported PCE of APSC is 5 times less than that of polymer/fullerene solar cell. The low PCE of APSC is mainly due to: i) low charge separation efficiency; and ii) lack of optimal morphology to facilitate charge transfer and transport; and iii) lack of control over the exciton and charge transport in each phase. My research work is focused towards addressing these issues. The charge separation efficiency of APSC can be enhanced by designing novel electron transporting polymers with: i) broad absorption range; ii) high electron mobility; and iii) high dielectric constant. In addition to with the above parameters chemical and electronic structure of the repeating unit of conjugated polymer also plays a role in charge separation efficiency. So far only three classes of electron transporting polymers, CN substituted PPV, 2,1,3-benzothiadiazole derived polymers and rylene diimide derived polymers, are used in APSC. Thus to enhance the charge separation efficiency new classes of electron transporting polymers with the above characteristics need to be synthesized. I have developed a new straightforward synthetic strategy to rapidly generate new classes of electron transporting polymers with different chemical and electronic structure, broad absorption range, and high electron mobility from readily available electron deficient monomers. In APSCs due to low entropy of mixing, polymers tend to micro-phase segregate rather than forming the more useful nano-phase segregation. Optimizing the polymer blend morphology to obtain nano-phase segregation is specific to the system under study, time consuming, and not trivial. Thus to avoid micro-phase segregation, nanoparticles of hole and electron transporters are synthesized and blended. But the PCE of nanoparticle blends are far less than those of polymer blends. This is mainly due to the: i) lack of optimal assembly of nanoparticles to facilitate charge transfer and transport processes; and ii) lack of control over the exciton and charge transport properties within the nanoparticles. Polymer packing within the nanoparticle controls the optoelectronic and charge transport properties of the nanoparticle. In this work I have shown that the solvent used to synthesize nanoparticles plays a crucial role in determining the assembly of polymer chains inside the nanoparticle there by affecting its exciton and charge transport processes. To obtain the optimal morphology for better charge transfer and transport, we have also synthesized nanoparticles of different radius with surfactants of opposite charge. We propose that depending on the radius and/or Coulombic interactions these nanoparticles can be assembled into mineral structure-types that are useful for photovoltaic devices.

Symmetry-protected topological phases of one-dimensional interacting fermions with spin-charge separation

NASA Astrophysics Data System (ADS)

Montorsi, Arianna; Dolcini, Fabrizio; Iotti, Rita C.; Rossi, Fausto

2017-06-01

The low energy behavior of a huge variety of one-dimensional interacting spinful fermionic systems exhibits spin-charge separation, described in the continuum limit by two sine-Gordon models decoupled in the charge and spin channels. Interaction is known to induce, besides the gapless Luttinger liquid phase, eight possible gapped phases, among which are the Mott, Haldane, charge-/spin-density, and bond-ordered wave insulators, and the Luther Emery liquid. Here we prove that some of these physically distinct phases have nontrivial topological properties, notably the presence of degenerate protected edge modes with fractionalized charge/spin. Moreover, we show that the eight gapped phases are in one-to-one correspondence with the symmetry-protected topological (SPT) phases classified by group cohomology theory in the presence of particle-hole symmetry P. The latter result is also exploited to characterize SPT phases by measurable nonlocal order parameters which follow the system evolution to the quantum phase transition. The implications on the appearance of exotic orders in the class of microscopic Hubbard Hamiltonians, possibly without P symmetry at higher energies, are discussed.

Effect of the molecular weight of a neutral polysaccharide on soy protein gelation.

PubMed

Monteiro, Sónia R; Lopes-da-Silva, José A

2017-12-01

The effects of galactomannans with different molecular weights on the heat-induced gelation characteristics of soybean protein were investigated using dynamic small-strain rheometry, under conditions where the proteins carry a net negative charge (pH7). Microstructure of the resulting gels was investigated by confocal laser scanning microscopy. Phase-separated systems were obtained with different morphologies and degree of phase separation, depending on both biopolymer concentrations and polysaccharide molecular weight. In general, a gelling enhancing effect on soy proteins was verified, despite extensive phase-separation processes observed at the higher polysaccharide molecular weight. This effect was demonstrated by an increase of the gelation rate, a decrease in the temperature at the onset of gelation, and an increase of gel stiffness and elastic character, with the length of polysaccharide chains. Overall, the results obtained established that the judicious selection of the galactomannan molecular weight may be used to modify the structure and gelation properties of soy proteins, originating a diversity of rheological characteristics and microstructures that will impact on the design of novel food formulations. Copyright © 2017 Elsevier Ltd. All rights reserved.

Photovoltaic Performance of Inverted Polymer Solar Cells Using Hybrid Carbon Quantum Dots and Absorption Polymer Materials

NASA Astrophysics Data System (ADS)

Lim, Hwain; Lee, Kyu Seung; Liu, Yang; Kim, Hak Yong; Son, Dong Ick

2018-05-01

We report the synthesis and characterization of the carbon quantum dots (C-dots) easily obtained from citric acid and ethanediamine, and also investigated structural, optical and electrical properties. The C-dots have extraordinary optical and electrical features such as absorption of ultraviolet range and effective interface for charge separation and transport in active layer, which make them attractive materials for applications in photovoltaic devices (PV). The C-dots play important roles in charge extraction in the PV structures, they can be synthesized by a simple method and used to insert in active layer of polymer solar cells. In this study, we demonstrate that improve charge transport properties of inverted polymer solar cells (iPSCs) with C-dots and structural, optical and electrical properties of C-dots. As a result, iPSCs with C-dots showed enhancement of more than 30% compared with that of the contrast device in power conversion efficiency.

Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites

DOE PAGES

Gélvez-Rueda, María C.; Hutter, Eline M.; Cao, Duyen H.; ...

2017-11-03

The optoelectronic properties of hybrid perovskites can be easily tailored by varying their components. Specifically, mixing the common short organic cation (methylammonium (MA)) with a larger one (e.g., butyl ammonium (BA)) results in 2-dimensional perovskites with varying thicknesses of inorganic layers separated by the large organic cation. In both of these applications, a detailed understanding of the dissociation and recombination of electron–hole pairs is of prime importance. Here in this work, we give a clear experimental demonstration of the interconversion between bound excitons and free charges as a function of temperature by combining microwave conductivity techniques with photoluminescence measurements. Wemore » demonstrate that the exciton binding energy varies strongly (between 80 and 370 meV) with the thickness of the inorganic layers. Additionally, we show that the mobility of charges increases with the layer thickness, in agreement with calculated effective masses from electronic structure calculations.« less

Electrification of Shaken Granular Flows as a Model of Natural Storm Charging

NASA Astrophysics Data System (ADS)

Kara, O.; Nordsiek, F.; Lathrop, D. P.

2015-12-01

The charging of particulates in nature is widespread and observed in thunderstorms, volcanic ash clouds, thunder-snow, and dust storms. However the mechanism of charge separation at large (> 1km) scale is poorly understood. We perform simple laboratory experiments to better understand the collective phenomena involved in granular electrification. We confine granular particles in an oscillating cylindrical chamber which is enclosed and sealed by two conducting plates. The primary measurement is the voltage difference between the two plates. We find that collective effects occurring in the bulk of the material play a significant role in the electrification process. We extend that by addition of photodetection capabilities to the experimental chamber to detect electrical discharges between the particles and each other and the plates. We present measurements of electrical discharges in addition to the slower dynamics of voltage variation in the system.

Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites.

PubMed

Gélvez-Rueda, María C; Hutter, Eline M; Cao, Duyen H; Renaud, Nicolas; Stoumpos, Constantinos C; Hupp, Joseph T; Savenije, Tom J; Kanatzidis, Mercouri G; Grozema, Ferdinand C

2017-11-30

The optoelectronic properties of hybrid perovskites can be easily tailored by varying their components. Specifically, mixing the common short organic cation (methylammonium (MA)) with a larger one (e.g., butyl ammonium (BA)) results in 2-dimensional perovskites with varying thicknesses of inorganic layers separated by the large organic cation. In both of these applications, a detailed understanding of the dissociation and recombination of electron-hole pairs is of prime importance. In this work, we give a clear experimental demonstration of the interconversion between bound excitons and free charges as a function of temperature by combining microwave conductivity techniques with photoluminescence measurements. We demonstrate that the exciton binding energy varies strongly (between 80 and 370 meV) with the thickness of the inorganic layers. Additionally, we show that the mobility of charges increases with the layer thickness, in agreement with calculated effective masses from electronic structure calculations.

Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites

PubMed Central

2017-01-01

The optoelectronic properties of hybrid perovskites can be easily tailored by varying their components. Specifically, mixing the common short organic cation (methylammonium (MA)) with a larger one (e.g., butyl ammonium (BA)) results in 2-dimensional perovskites with varying thicknesses of inorganic layers separated by the large organic cation. In both of these applications, a detailed understanding of the dissociation and recombination of electron–hole pairs is of prime importance. In this work, we give a clear experimental demonstration of the interconversion between bound excitons and free charges as a function of temperature by combining microwave conductivity techniques with photoluminescence measurements. We demonstrate that the exciton binding energy varies strongly (between 80 and 370 meV) with the thickness of the inorganic layers. Additionally, we show that the mobility of charges increases with the layer thickness, in agreement with calculated effective masses from electronic structure calculations. PMID:29218073

Non-monotonic spatial distribution of the interstellar dust in astrospheres: finite gyroradius effect

NASA Astrophysics Data System (ADS)

Katushkina, O. A.; Alexashov, D. B.; Izmodenov, V. V.; Gvaramadze, V. V.

2017-02-01

High-resolution mid-infrared observations of astrospheres show that many of them have filamentary (cirrus-like) structure. Using numerical models of dust dynamics in astrospheres, we suggest that their filamentary structure might be related to specific spatial distribution of the interstellar dust around the stars, caused by a gyrorotation of charged dust grains in the interstellar magnetic field. Our numerical model describes the dust dynamics in astrospheres under an influence of the Lorentz force and assumption of a constant dust charge. Calculations are performed for the dust grains with different sizes separately. It is shown that non-monotonic spatial dust distribution (viewed as filaments) appears for dust grains with the period of gyromotion comparable with the characteristic time-scale of the dust motion in the astrosphere. Numerical modelling demonstrates that the number of filaments depends on charge-to-mass ratio of dust.

Nucleon Charges from 2+1+1-flavor HISQ and 2+1-flavor clover lattices

DOE PAGES

Gupta, Rajan

2016-07-24

Precise estimates of the nucleon charges g A, g S and g T are needed in many phenomenological analyses of SM and BSM physics. In this talk, we present results from two sets of calculations using clover fermions on 9 ensembles of 2+1+1-flavor HISQ and 4 ensembles of 2+1-flavor clover lattices. In addition, we show that high statistics can be obtained cost-effectively using the truncated solver method with bias correction and the coherent source sequential propagator technique. By performing simulations at 4–5 values of the source-sink separation t sep, we demonstrate control over excited-state contamination using 2- and 3-state fits.more » Using the high-precision 2+1+1-flavor data, we perform a simultaneous fit in a, M π and M πL to obtain our final results for the charges.« less

Hole-Accepting-Ligand-Modified CdSe QDs for Dramatic Enhancement of Photocatalytic and Photoelectrochemical Hydrogen Evolution by Solar Energy.

PubMed

Li, Xu-Bing; Liu, Bin; Wen, Min; Gao, Yu-Ji; Wu, Hao-Lin; Huang, Mao-Yong; Li, Zhi-Jun; Chen, Bin; Tung, Chen-Ho; Wu, Li-Zhu

2016-04-01

Solar H 2 evolution of CdSe QDs can be significantly enhanced simply by introducing a suitable hole-accepting-ligand for achieving efficient hole extraction and transfer at the nanoscale interfaces, which opens an effective pathway for dissociation of excitons to generate long-lived charge separation, thus improving the solar-to-fuel conversion efficiency.

Charge sniffer for electrostatics demonstrations

NASA Astrophysics Data System (ADS)

Dinca, Mihai P.

2011-02-01

An electronic electroscope with a special design for demonstrations and experiments on static electricity is described. It operates as an electric charge sniffer by detecting slightly charged objects when they are brought to the front of its sensing electrode. The sniffer has the advantage of combining high directional sensitivity with a logarithmic bar display. It allows for the identification of electric charge polarity during charge separation by friction, peeling, electrostatic induction, batteries, or secondary coils of power transformers. Other experiments in electrostatics, such as observing the electric field of an oscillating dipole and the distance dependence of the electric field generated by simple charge configurations, are also described.

Continuous-Time Monitoring of Landau-Zener Interference in a Cooper-Pair Box

NASA Astrophysics Data System (ADS)

Sillanpää, Mika; Lehtinen, Teijo; Paila, Antti; Makhlin, Yuriy; Hakonen, Pertti

2006-05-01

Landau-Zener (LZ) tunneling can occur with a certain probability when crossing energy levels of a quantum two-level system are swept across the minimum energy separation. Here we present experimental evidence of quantum interference effects in solid-state LZ tunneling. We used a Cooper-pair box qubit where the LZ tunneling occurs at the charge degeneracy. By employing a weak nondemolition monitoring, we observe interference between consecutive LZ-tunneling events; we find that the average level occupancies depend on the dynamical phase. The system’s unusually strong linear response is explained by interband relaxation. Our interferometer can be used as a high-resolution Mach-Zehnder type detector for phase and charge.

Continuous-time monitoring of Landau-Zener interference in a cooper-pair box.

PubMed

Sillanpää, Mika; Lehtinen, Teijo; Paila, Antti; Makhlin, Yuriy; Hakonen, Pertti

2006-05-12

Landau-Zener (LZ) tunneling can occur with a certain probability when crossing energy levels of a quantum two-level system are swept across the minimum energy separation. Here we present experimental evidence of quantum interference effects in solid-state LZ tunneling. We used a Cooper-pair box qubit where the LZ tunneling occurs at the charge degeneracy. By employing a weak nondemolition monitoring, we observe interference between consecutive LZ-tunneling events; we find that the average level occupancies depend on the dynamical phase. The system's unusually strong linear response is explained by interband relaxation. Our interferometer can be used as a high-resolution Mach-Zehnder-type detector for phase and charge.

Electron beam influence on the carbon contamination of electron irradiated hydroxyapatite thin films

NASA Astrophysics Data System (ADS)

Hristu, Radu; Stanciu, Stefan G.; Tranca, Denis E.; Stanciu, George A.

2015-08-01

Electron beam irradiation which is considered a reliable method for tailoring the surface charge of hydroxyapatite is hindered by carbon contamination. Separating the effects of the carbon contamination from those of irradiation-induced trapped charge is important for a wide range of biological applications. In this work we focus on the understanding of the electron-beam-induced carbon contamination with special emphasis on the influence of the electron irradiation parameters on this phenomenon. Phase imaging in atomic force microscopy is used to evaluate the influence of electron energy, beam current and irradiation time on the shape and size of the resulted contamination patterns. Different processes involved in the carbon contamination of hydroxyapatite are discussed.

Concurrent DNA Preconcentration and Separation in Bipolar Electrode-Based Microfluidic Device

PubMed Central

Song, Hongjun; Wang, Yi; Garson, Charles; Pant, Kapil

2015-01-01

This paper presents a bipolar electrode (BPE) device in a microfluidic dual-channel design for concurrent preconcentration and separation of composite DNA containing samples. The novelty of the present effort relies on the combination of BPE-induced ion concentration polarization (ICP) and end-labeled free-solution electrophoresis (ELFSE). The ion concentration polarization effect arising from the faradaic reaction on the BPE is utilized to exert opposing electrophoretic and electroosmotic forces on the DNA samples. Meanwhile, end-labeled free-solution electrophoresis alters the mass-charge ratio to enable simultaneous DNA separation in free solution. The microfluidic device was fabricated using standard and soft lithography techniques to form gold-on-glass electrode capped with a PDMS microfluidic channel. Experimental testing with various DNA samples was carried out over a range of applied electric field. Concentration ratios up to 285× within 5 minutes for a 102-mer DNA, and concurrent preconcentration and free-solution separation of binary mixture of free and bound 102-mer DNA within 6 minutes was demonstrated. The effect of applied electric field was also interrogated with respect to pertinent performance metrics of preconcentration and separation. PMID:26005497

Energetics of bacterial photosynthesis.

PubMed

Lebard, David N; Matyushov, Dmitry V

2009-09-10

We report the results of extensive numerical simulations and theoretical calculations of electronic transitions in the reaction center of Rhodobacter sphaeroides photosynthetic bacterium. The energetics and kinetics of five electronic transitions related to the kinetic scheme of primary charge separation have been analyzed and compared to experimental observations. Nonergodic formulation of the reaction kinetics is required for the calculation of the rates due to a severe breakdown of the system ergodicity on the time scale of primary charge separation, with the consequent inapplicability of the standard canonical prescription to calculate the activation barrier. Common to all reactions studied is a significant excess of the charge-transfer reorganization energy from the width of the energy gap fluctuations over that from the Stokes shift of the transition. This property of the hydrated proteins, breaking the linear response of the thermal bath, allows the reaction center to significantly reduce the reaction free energy of near-activationless electron hops and thus raise the overall energetic efficiency of the biological charge-transfer chain. The increase of the rate of primary charge separation with cooling is explained in terms of the temperature variation of induction solvation, which dominates the average donor-acceptor energy gap for all electronic transitions in the reaction center. It is also suggested that the experimentally observed break in the Arrhenius slope of the primary recombination rate, occurring near the temperature of the dynamical transition in proteins, can be traced back to a significant drop of the solvent reorganization energy close to that temperature.

Enhanced specific heat jump in electron-doped CaMnO3: Spin ordering driven by charge separation

NASA Astrophysics Data System (ADS)

Moritomo, Y.; Machida, A.; Nishibori, E.; Takata, M.; Sakata, M.

2001-12-01

Temperature variation of the magnetic susceptibility χ, resistivity ρ, specific heat C, and lattice constants has been investigated in electron-doped CaMnO3. The parent CaMnO3 is an antiferromagnetic band insulator, and shows an insulator-metal crossover with electron doping, together with an enhanced ferromagnetic component. We have found an enhancement of the specific heat jump ΔC at the spin-ordering temperature Tspin and interpreted the enhancement in terms of the intrinsic charge separation.

Engine Tune-up Service. Unit 2: Charging System. Student Guide. Automotive Mechanics Curriculum.

ERIC Educational Resources Information Center

Richardson, Roger L.; Bacon, E. Miles

This student guide is for Unit 2, Charging System, in the Engine Tune-Up Service portion of the Automotive Mechanics Curriculum. It deals with how to test the charging system. A companion review exercise book and posttests are available separately as CE 031 209-210. An introduction tells how this unit fits into the total tune-up service, defines…