Orthogonality of embedded wave functions for different states in frozen-density embedding theory

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

Zech, Alexander; Wesolowski, Tomasz A.; Aquilante, Francesco

2015-10-28

Other than lowest-energy stationary embedded wave functions obtained in Frozen-Density Embedding Theory (FDET) [T. A. Wesolowski, Phys. Rev. A 77, 012504 (2008)] can be associated with electronic excited states but they can be mutually non-orthogonal. Although this does not violate any physical principles — embedded wave functions are only auxiliary objects used to obtain stationary densities — working with orthogonal functions has many practical advantages. In the present work, we show numerically that excitation energies obtained using conventional FDET calculations (allowing for non-orthogonality) can be obtained using embedded wave functions which are strictly orthogonal. The used method preserves the mathematicalmore » structure of FDET and self-consistency between energy, embedded wave function, and the embedding potential (they are connected through the Euler-Lagrange equations). The orthogonality is built-in through the linearization in the embedded density of the relevant components of the total energy functional. Moreover, we show formally that the differences between the expectation values of the embedded Hamiltonian are equal to the excitation energies, which is the exact result within linearized FDET. Linearized FDET is shown to be a robust approximation for a large class of reference densities.« less

Charmonium ground and excited states at finite temperature from complex Borel sum rules

NASA Astrophysics Data System (ADS)

Araki, Ken-Ji; Suzuki, Kei; Gubler, Philipp; Oka, Makoto

2018-05-01

Charmonium spectral functions in vector and pseudoscalar channels at finite temperature are investigated through the complex Borel sum rules and the maximum entropy method. Our approach enables us to extract the peaks corresponding to the excited charmonia, ψ‧ and ηc‧ , as well as those of the ground states, J / ψ and ηc, which has never been achieved in usual QCD sum rule analyses. We show the spectral functions in vacuum and their thermal modification around the critical temperature, which leads to the almost simultaneous melting (or peak disappearance) of the ground and excited states.

Tight-binding approximations to time-dependent density functional theory — A fast approach for the calculation of electronically excited states

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

Rüger, Robert, E-mail: rueger@scm.com; Department of Theoretical Chemistry, Vrije Universiteit Amsterdam, De Boelelaan 1083, 1081 HV Amsterdam; Wilhelm-Ostwald-Institut für Physikalische und Theoretische Chemie, Linnéstr. 2, 04103 Leipzig

2016-05-14

We propose a new method of calculating electronically excited states that combines a density functional theory based ground state calculation with a linear response treatment that employs approximations used in the time-dependent density functional based tight binding (TD-DFTB) approach. The new method termed time-dependent density functional theory TD-DFT+TB does not rely on the DFTB parametrization and is therefore applicable to systems involving all combinations of elements. We show that the new method yields UV/Vis absorption spectra that are in excellent agreement with computationally much more expensive TD-DFT calculations. Errors in vertical excitation energies are reduced by a factor of twomore » compared to TD-DFTB.« less

Excited-state lifetimes of far-infrared collective modes in proteins.

PubMed

Xie, Aihua; van der Meer, Alexander F G; Austin, Robert H

2002-01-07

Vibrational excitations of low frequency collective modes are essential for functionally important conformational transitions in proteins. Here we report the first direct measurement on the lifetime of vibrational excitations of the collective modes at 87 microm (115 cm(-1)) in bacteriorhodopsin, a transmembrane protein. The data show that these modes have extremely long lifetime of vibrational excitations, over 500 ps, accommodating 1500 vibrations. We suggest that there is a connection between this relatively slow anharmonic relaxation rate of approximately 10(9) sec(-1) and the similar observed rate of conformational transitions in proteins, which require multilevel vibrational excitations.

Extension of the Kohn-Sham formulation of density functional theory to finite temperature

NASA Astrophysics Data System (ADS)

Gonis, A.; Däne, M.

2018-05-01

Based on Mermin's extension of the Hohenberg and Kohn theorems to non-zero temperature, the Kohn-Sham formulation of density functional theory (KS-DFT) is generalized to finite temperature. We show that present formulations are inconsistent with Mermin's functional containing expressions, in particular describing the Coulomb energy, that defy derivation and are even in violation of rules of logical inference. More; current methodology is in violation of fundamental laws of both quantum and classical mechanics. Based on this feature, we demonstrate the impossibility of extending the KS formalism to finite temperature through the self-consistent solutions of the single-particle Schrödinger equation of T > 0. Guided by the form of Mermin's functional that depends on the eigenstates of a Hamiltonian, determined at T = 0, we base our extension of KS-DFT on the determination of the excited states of a non-interacting system at the zero of temperature. The resulting formulation is consistent with that of Mermin constructing the free energy at T > 0 in terms of the excited states of a non-interacting Hamiltonian (system) that, within the KS formalism, are described by Slater determinants. To determine the excited states at T = 0 use is made of the extension of the Hohenberg and Kohn theorems to excited states presented in previous work applied here to a non-interacting collection of replicas of a non-interacting N-particle system, whose ground state density is taken to match that of K non-interacting replicas of an interacting N-particle system at T = 0 . The formalism allows for an ever denser population of the excitation spectrum of a Hamiltonian, within the KS approximation. The form of the auxiliary potential, (Kohn-Sham potential), is formally identical to that in the ground state formalism with the contribution of the Coulomb energy provided by the derivative of the Coulomb energy in all excited states taken into account. Once the excited states are determined, the minimum of the free energy within the KS formalism follows immediately in the form of Mermin's functional, but with the exact excited states in that functional represented by Slater determinants obtained through self-consistency conditions at the zero of temperature. It is emphasized that, in departure from all existing formulations, no self-consistency conditions are implemented at finite T; as we show, in fact, such formulations are rigorously blocked.

Study of deuteron induced reactions on natural iron and copper and their use for monitoring beam parameters and for thin layer activation technique

NASA Astrophysics Data System (ADS)

Takács, S.; Tárkányi, F.; Sonck, M.; Hermanne, A.; Sudár, S.

1997-02-01

Excitation functions of deuteron induced nuclear reactions on natural iron and copper have been studied in the frame of a systematic investigation of charged particle induced nuclear reactions on metals for different applications. The excitation functions were measured up to 20 MeV deuteron energy by using stacked foil technique and activation method. The measured and the evaluated literature data showed that some reaction can be recommended for monitoring deuteron beams, and the excitation functions can be used to determine calibration curves for Thin Layer Activation Technique (TLA). Cross sections calculated by statistical model theory, STAPRE, taking into account preequilibrium effect are in reasonable agreement with the experimental results.

Neural evidence for cultural differences in the valuation of positive facial expressions

PubMed Central

Park, BoKyung; Chim, Louise; Blevins, Elizabeth; Knutson, Brian

2016-01-01

European Americans value excitement more and calm less than Chinese. Within cultures, European Americans value excited and calm states similarly, whereas Chinese value calm more than excited states. To examine how these cultural differences influence people’s immediate responses to excited vs calm facial expressions, we combined a facial rating task with functional magnetic resonance imaging. During scanning, European American (n = 19) and Chinese (n = 19) females viewed and rated faces that varied by expression (excited, calm), ethnicity (White, Asian) and gender (male, female). As predicted, European Americans showed greater activity in circuits associated with affect and reward (bilateral ventral striatum, left caudate) while viewing excited vs calm expressions than did Chinese. Within cultures, European Americans responded to excited vs calm expressions similarly, whereas Chinese showed greater activity in these circuits in response to calm vs excited expressions regardless of targets’ ethnicity or gender. Across cultural groups, greater ventral striatal activity while viewing excited vs. calm expressions predicted greater preference for excited vs calm expressions months later. These findings provide neural evidence that people find viewing the specific positive facial expressions valued by their cultures to be rewarding and relevant. PMID:26342220

Active Control of the Forced and Transient Response of a Finite Beam. M.S. Thesis

NASA Technical Reports Server (NTRS)

Post, John Theodore

1989-01-01

When studying structural vibrations resulting from a concentrated source, many structures may be modelled as a finite beam excited by a point source. The theoretical limit on cancelling the resulting beam vibrations by utilizing another point source as an active controller is explored. Three different types of excitation are considered, harmonic, random, and transient. In each case, a cost function is defined and minimized for numerous parameter variations. For the case of harmonic excitation, the cost function is obtained by integrating the mean squared displacement over a region of the beam in which control is desired. A controller is then found to minimize this cost function in the control interval. The control interval and controller location are continuously varied for several frequencies of excitation. The results show that control over the entire beam length is possible only when the excitation frequency is near a resonant frequency of the beam, but control over a subregion may be obtained even between resonant frequencies at the cost of increasing the vibration outside of the control region. For random excitation, the cost function is realized by integrating the expected value of the displacement squared over the interval of the beam in which control is desired. This is shown to yield the identical cost function as obtained by integrating the cost function for harmonic excitation over all excitation frequencies. As a result, it is always possible to reduce the cost function for random excitation whether controlling the entire beam or just a subregion, without ever increasing the vibration outside the region in which control is desired. The last type of excitation considered is a single, transient pulse. A cost function representative of the beam vibration is obtained by integrating the transient displacement squared over a region of the beam and over all time. The form of the controller is chosen a priori as either one or two delayed pulses. Delays constrain the controller to be causal. The best possible control is then examined while varying the region of control and the controller location. It is found that control is always possible using either one or two control pulses. The two pulse controller gives better performance than a single pulse controller, but finding the optimal delay time for the additional controllers increases as the square of the number of control pulses.

Highly efficient implementation of pseudospectral time-dependent density-functional theory for the calculation of excitation energies of large molecules.

PubMed

Cao, Yixiang; Hughes, Thomas; Giesen, Dave; Halls, Mathew D; Goldberg, Alexander; Vadicherla, Tati Reddy; Sastry, Madhavi; Patel, Bhargav; Sherman, Woody; Weisman, Andrew L; Friesner, Richard A

2016-06-15

We have developed and implemented pseudospectral time-dependent density-functional theory (TDDFT) in the quantum mechanics package Jaguar to calculate restricted singlet and restricted triplet, as well as unrestricted excitation energies with either full linear response (FLR) or the Tamm-Dancoff approximation (TDA) with the pseudospectral length scales, pseudospectral atomic corrections, and pseudospectral multigrid strategy included in the implementations to improve the chemical accuracy and to speed the pseudospectral calculations. The calculations based on pseudospectral time-dependent density-functional theory with full linear response (PS-FLR-TDDFT) and within the Tamm-Dancoff approximation (PS-TDA-TDDFT) for G2 set molecules using B3LYP/6-31G*(*) show mean and maximum absolute deviations of 0.0015 eV and 0.0081 eV, 0.0007 eV and 0.0064 eV, 0.0004 eV and 0.0022 eV for restricted singlet excitation energies, restricted triplet excitation energies, and unrestricted excitation energies, respectively; compared with the results calculated from the conventional spectral method. The application of PS-FLR-TDDFT to OLED molecules and organic dyes, as well as the comparisons for results calculated from PS-FLR-TDDFT and best estimations demonstrate that the accuracy of both PS-FLR-TDDFT and PS-TDA-TDDFT. Calculations for a set of medium-sized molecules, including Cn fullerenes and nanotubes, using the B3LYP functional and 6-31G(**) basis set show PS-TDA-TDDFT provides 19- to 34-fold speedups for Cn fullerenes with 450-1470 basis functions, 11- to 32-fold speedups for nanotubes with 660-3180 basis functions, and 9- to 16-fold speedups for organic molecules with 540-1340 basis functions compared to fully analytic calculations without sacrificing chemical accuracy. The calculations on a set of larger molecules, including the antibiotic drug Ramoplanin, the 46-residue crambin protein, fullerenes up to C540 and nanotubes up to 14×(6,6), using the B3LYP functional and 6-31G(**) basis set with up to 8100 basis functions show that PS-FLR-TDDFT CPU time scales as N(2.05) with the number of basis functions. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.

An Ab Initio Exciton Model Including Charge-Transfer Excited States

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

Li, Xin; Parrish, Robert M.; Liu, Fang

Here, the Frenkel exciton model is a useful tool for theoretical studies of multichromophore systems. We recently showed that the exciton model could be used to coarse-grain electronic structure in multichromophoric systems, focusing on singly excited exciton states. However, our previous implementation excluded charge-transfer excited states, which can play an important role in light-harvesting systems and near-infrared optoelectronic materials. Recent studies have also emphasized the significance of charge-transfer in singlet fission, which mediates the coupling between the locally excited states and the multiexcitonic states. In this work, we report on an ab initio exciton model that incorporates charge-transfer excited statesmore » and demonstrate that the model provides correct charge-transfer excitation energies and asymptotic behavior. Comparison with TDDFT and EOM-CC2 calculations shows that our exciton model is robust with respect to system size, screening parameter, and different density functionals. Inclusion of charge-transfer excited states makes the exciton model more useful for studies of singly excited states and provides a starting point for future construction of a model that also includes double-exciton states.« less

An Ab Initio Exciton Model Including Charge-Transfer Excited States

DOE PAGES

Li, Xin; Parrish, Robert M.; Liu, Fang; ...

2017-06-15

Here, the Frenkel exciton model is a useful tool for theoretical studies of multichromophore systems. We recently showed that the exciton model could be used to coarse-grain electronic structure in multichromophoric systems, focusing on singly excited exciton states. However, our previous implementation excluded charge-transfer excited states, which can play an important role in light-harvesting systems and near-infrared optoelectronic materials. Recent studies have also emphasized the significance of charge-transfer in singlet fission, which mediates the coupling between the locally excited states and the multiexcitonic states. In this work, we report on an ab initio exciton model that incorporates charge-transfer excited statesmore » and demonstrate that the model provides correct charge-transfer excitation energies and asymptotic behavior. Comparison with TDDFT and EOM-CC2 calculations shows that our exciton model is robust with respect to system size, screening parameter, and different density functionals. Inclusion of charge-transfer excited states makes the exciton model more useful for studies of singly excited states and provides a starting point for future construction of a model that also includes double-exciton states.« less

An Ab Initio Exciton Model Including Charge-Transfer Excited States.

PubMed

Li, Xin; Parrish, Robert M; Liu, Fang; Kokkila Schumacher, Sara I L; Martínez, Todd J

2017-08-08

The Frenkel exciton model is a useful tool for theoretical studies of multichromophore systems. We recently showed that the exciton model could be used to coarse-grain electronic structure in multichromophoric systems, focusing on singly excited exciton states [ Acc. Chem. Res. 2014 , 47 , 2857 - 2866 ]. However, our previous implementation excluded charge-transfer excited states, which can play an important role in light-harvesting systems and near-infrared optoelectronic materials. Recent studies have also emphasized the significance of charge-transfer in singlet fission, which mediates the coupling between the locally excited states and the multiexcitonic states. In this work, we report on an ab initio exciton model that incorporates charge-transfer excited states and demonstrate that the model provides correct charge-transfer excitation energies and asymptotic behavior. Comparison with TDDFT and EOM-CC2 calculations shows that our exciton model is robust with respect to system size, screening parameter, and different density functionals. Inclusion of charge-transfer excited states makes the exciton model more useful for studies of singly excited states and provides a starting point for future construction of a model that also includes double-exciton states.

Mark 4A DSN receiver-exciter and transmitter subsystems

NASA Technical Reports Server (NTRS)

Wick, M. R.

1986-01-01

The present configuration of the Mark 4A DSN Receiver-Exciter and Transmitter Subsystems is described. Functional requirements and key characteristics are given to show the differences in the capabilities required by the Networks Consolidation task for combined High Earth Orbiter and Deep Space Network tracking support.

Relative and absolute level populations in beam-foil-excited neutral helium

NASA Technical Reports Server (NTRS)

Davidson, J.

1975-01-01

Relative and absolute populations of 19 levels in beam-foil-excited neutral helium at 0.275 MeV have been measured. The singlet angular-momentum sequences show dependences on principal quantum number consistent with n to the -3rd power, but the triplet sequences do not. Singlet and triplet angular-momentum sequences show similar dependences on level excitation energy. Excitation functions for six representative levels were measured in the range from 0.160 to 0.500 MeV. The absolute level populations increase with energy, whereas the neutral fraction of the beam decreases with energy. Further, the P angular-momentum levels are found to be overpopulated with respect to the S and D levels. The overpopulation decreases with increasing principal quantum number.

Electron-Impact Cross Sections for Ground State to np Excitations of Sodium and Potassium.

PubMed

Stone, Philip M; Kim, Yong-Ki

2004-01-01

Cross sections for electron impact excitation of atoms are important for modeling of low temperature plasmas and gases. While there are many experimental and theoretical results for excitation to the first excited states, little information is available for excitation to higher states. We present here calculations of excitations from the ground state to the np levels of sodium (n = 3 through 11) and potassium (n = 4 through 12). We also present a calculation for a transition from the excited sodium level 3p to 3d to show the generality of the method. Scaling formulas developed earlier by Kim [Phys. Rev. A 64, 032713 (2001)] for plane-wave Born cross sections are used. These formulas have been shown to be remarkably accurate yet simple to use. We have used a core polarization potential in a Dirac-Fock wave function code to calculate target atom wave functions and a matching form of the dipole transition operator to calculate oscillator strengths and Born cross sections. The scaled Born results here for excitation to the first excited levels are in very good agreement with experimental and other theoretical data, and the results for excitation to the next few levels are in satisfactory agreement with the limited data available. The present results for excitation to the higher levels are believed to be the only data available.

Influence of excitation frequency on the metastable atoms and electron energy distribution function in a capacitively coupled argon discharge

NASA Astrophysics Data System (ADS)

Sharma, S.; Sirse, N.; Turner, M. M.; Ellingboe, A. R.

2018-06-01

One-dimensional particle-in-cell simulation is used to simulate the capacitively coupled argon plasma for a range of excitation frequency from 13.56 MHz to 100 MHz. The argon chemistry set can, selectively, include two metastable levels enabling multi-step ionization and metastable pooling. The results show that the plasma density decreases when metastable atoms are included with higher discrepancy at a higher excitation frequency. The contribution of multistep ionization to the overall density increases with the excitation frequency. The electron temperature increases with the inclusion of metastable atoms and decreases with the excitation frequency. At a lower excitation frequency, the density of Ar** (3p5 4p, 13.1 eV) is higher than that of Ar* (3p5 4s, 11.6 eV), whereas at higher excitation frequencies, the Ar* (3p5 4s, 11.6 eV) is the dominant metastable atom. The metastable and electron temperature profile evolve from a parabolic profile at a lower excitation frequency to a saddle type profile at a higher excitation frequency. With metastable, the electron energy distribution function (EEDF) changes its shape from Druyvesteyn type, at a low excitation frequency, to bi-Maxwellian, at a high frequency plasma excitation; however, a three-temperature EEDF is observed without metastable atoms.

Excitation energies of dissociating H2: A problematic case for the adiabatic approximation of time-dependent density functional theory

NASA Astrophysics Data System (ADS)

Gritsenko, O. V.; van Gisbergen, S. J. A.; Görling, A.; Baerends, E. J.

2000-11-01

Time-dependent density functional theory (TDDFT) is applied for calculation of the excitation energies of the dissociating H2 molecule. The standard TDDFT method of adiabatic local density approximation (ALDA) totally fails to reproduce the potential curve for the lowest excited singlet 1Σu+ state of H2. Analysis of the eigenvalue problem for the excitation energies as well as direct derivation of the exchange-correlation (xc) kernel fxc(r,r',ω) shows that ALDA fails due to breakdown of its simple spatially local approximation for the kernel. The analysis indicates a complex structure of the function fxc(r,r',ω), which is revealed in a different behavior of the various matrix elements K1c,1cxc (between the highest occupied Kohn-Sham molecular orbital ψ1 and virtual MOs ψc) as a function of the bond distance R(H-H). The effect of nonlocality of fxc(r,r') is modeled by using different expressions for the corresponding matrix elements of different orbitals. Asymptotically corrected ALDA (ALDA-AC) expressions for the matrix elements K12,12xc(στ) are proposed, while for other matrix elements the standard ALDA expressions are retained. This approach provides substantial improvement over the standard ALDA. In particular, the ALDA-AC curve for the lowest singlet excitation qualitatively reproduces the shape of the exact curve. It displays a minimum and approaches a relatively large positive energy at large R(H-H). ALDA-AC also produces a substantial improvement for the calculated lowest triplet excitation, which is known to suffer from the triplet instability problem of the restricted KS ground state. Failure of the ALDA for the excitation energies is related to the failure of the local density as well as generalized gradient approximations to reproduce correctly the polarizability of dissociating H2. The expression for the response function χ is derived to show the origin of the field-counteracting term in the xc potential, which is lacking in the local density and generalized gradient approximations and which is required to obtain a correct polarizability.

Comparison of the hydrological excitation functions HAM of polar motion for the period 1980.0-2007.0

NASA Astrophysics Data System (ADS)

Nastula, J.; Pasnicka, M.; Kolaczek, B.

2011-10-01

In this study we compared contributions of polar motion excitation determined from hydrological models and harmonic coefficients of the Earth gravity field obtained from Gravity Recovery and Climate Experiment (GRACE). Hydrological excitation function (hydrological angular momentum - HAM) has been estimated from models of global hydrology, based on the observed distribution of surface water, snow, ice and soil moisture. All of them were compared with observed Geodetic Angular Momentum (GAM), excitations of polar motion. The spectra of these excitation functions of polar motion and residual geodetic excitation function G-A-O obtained from GAM by elimination of atmospheric and oceanic excitation functions were computed too. Phasor diagrams of the seasonal components of the polar motion excitation functions of all HAM excitation functions as well as of two GRACE solutions: CSR, CNES were determined and discussed.

Changes in the Excitability of Neocortical Neurons in a Mouse Model of Amyotrophic Lateral Sclerosis Are Not Specific to Corticospinal Neurons and Are Modulated by Advancing Disease.

PubMed

Kim, Juhyun; Hughes, Ethan G; Shetty, Ashwin S; Arlotta, Paola; Goff, Loyal A; Bergles, Dwight E; Brown, Solange P

2017-09-13

Cell type-specific changes in neuronal excitability have been proposed to contribute to the selective degeneration of corticospinal neurons in amyotrophic lateral sclerosis (ALS) and to neocortical hyperexcitability, a prominent feature of both inherited and sporadic variants of the disease, but the mechanisms underlying selective loss of specific cell types in ALS are not known. We analyzed the physiological properties of distinct classes of cortical neurons in the motor cortex of hSOD1 G93A mice of both sexes and found that they all exhibit increases in intrinsic excitability that depend on disease stage. Targeted recordings and in vivo calcium imaging further revealed that neurons adapt their functional properties to normalize cortical excitability as the disease progresses. Although different neuron classes all exhibited increases in intrinsic excitability, transcriptional profiling indicated that the molecular mechanisms underlying these changes are cell type specific. The increases in excitability in both excitatory and inhibitory cortical neurons show that selective dysfunction of neuronal cell types cannot account for the specific vulnerability of corticospinal motor neurons in ALS. Furthermore, the stage-dependent alterations in neuronal function highlight the ability of cortical circuits to adapt as disease progresses. These findings show that both disease stage and cell type must be considered when developing therapeutic strategies for treating ALS. SIGNIFICANCE STATEMENT It is not known why certain classes of neurons preferentially die in different neurodegenerative diseases. It has been proposed that the enhanced excitability of affected neurons is a major contributor to their selective loss. We show using a mouse model of amyotrophic lateral sclerosis (ALS), a disease in which corticospinal neurons exhibit selective vulnerability, that changes in excitability are not restricted to this neuronal class and that excitability does not increase monotonically with disease progression. Moreover, although all neuronal cell types tested exhibited abnormal functional properties, analysis of their gene expression demonstrated cell type-specific responses to the ALS-causing mutation. These findings suggest that therapies for ALS may need to be tailored for different cell types and stages of disease. Copyright © 2017 the authors 0270-6474/17/379038-17$15.00/0.

Employment of sawtooth-shaped-function excitation signal and oversampling for improving resistance measurement accuracy

NASA Astrophysics Data System (ADS)

Lin, Ling; Li, Shujuan; Yan, Wenjuan; Li, Gang

2016-10-01

In order to achieve higher measurement accuracy of routine resistance without increasing the complexity and cost of the system circuit of existing methods, this paper presents a novel method that exploits a shaped-function excitation signal and oversampling technology. The excitation signal source for resistance measurement is modulated by the sawtooth-shaped-function signal, and oversampling technology is employed to increase the resolution and the accuracy of the measurement system. Compared with the traditional method of using constant amplitude excitation signal, this method can effectively enhance the measuring accuracy by almost one order of magnitude and reduce the root mean square error by 3.75 times under the same measurement conditions. The results of experiments show that the novel method can attain the aim of significantly improve the measurement accuracy of resistance on the premise of not increasing the system cost and complexity of the circuit, which is significantly valuable for applying in electronic instruments.

Fast metastable fragments produced by dissociative excitation of carbonyl sulfide

NASA Technical Reports Server (NTRS)

Van Brunt, R. J.; Mumma, M. J.

1975-01-01

Dissociative excitation of OCS by electron impact has been studied using the method of translational spectroscopy. Time-of-flight distributions and excitation functions of the fast metastable fragments have been measured. The results are compared with similar measurements on CO2 and show that a variety of metastable fragments including CO(a 3Pi), S(5S), O(5S) as well as long-lived high-lying atomic and molecular Rydberg fragments can contribute to dissociation.

Different equation-of-motion coupled cluster methods with different reference functions: The formyl radical

NASA Astrophysics Data System (ADS)

Kuś, Tomasz; Bartlett, Rodney J.

2008-09-01

The doublet and quartet excited states of the formyl radical have been studied by the equation-of-motion (EOM) coupled cluster (CC) method. The Sz spin-conserving singles and doubles (EOM-EE-CCSD) and singles, doubles, and triples (EOM-EE-CCSDT) approaches, as well as the spin-flipped singles and doubles (EOM-SF-CCSD) method have been applied, subject to unrestricted Hartree-Fock (HF), restricted open-shell HF, and quasirestricted HF references. The structural parameters, vertical and adiabatic excitation energies, and harmonic vibrational frequencies have been calculated. The issue of the reference function choice for the spin-flipped (SF) method and its impact on the results has been discussed using the experimental data and theoretical results available. The results show that if the appropriate reference function is chosen so that target states differ from the reference by only single excitations, then EOM-EE-CCSD and EOM-SF-CCSD methods give a very good description of the excited states. For the states that have a non-negligible contribution of the doubly excited configurations one is able to use the SF method with such a reference function, that in most cases the performance of the EOM-SF-CCSD method is better than that of the EOM-EE-CCSD approach.

Multi-photon excited luminescence of magnetic FePt core-shell nanoparticles.

PubMed

Seemann, K M; Kuhn, B

2014-07-01

We present magnetic FePt nanoparticles with a hydrophilic, inert, and biocompatible silico-tungsten oxide shell. The particles can be functionalized, optically detected, and optically manipulated. To show the functionalization the fluorescent dye NOPS was bound to the FePt core-shell nanoparticles with propyl-triethoxy-silane linkers and fluorescence of the labeled particles were observed in ethanol (EtOH). In aqueous dispersion the NOPS fluorescence is quenched making them invisible using 1-photon excitation. However, we observe bright luminescence of labeled and even unlabeled magnetic core-shell nanoparticles with multi-photon excitation. Luminescence can be detected in the near ultraviolet and the full visible spectral range by near infrared multi-photon excitation. For optical manipulation, we were able to drag clusters of particles, and maybe also single particles, by a focused laser beam that acts as optical tweezers by inducing an electric dipole in the insulated metal nanoparticles. In a first application, we show that the luminescence of the core-shell nanoparticles is bright enough for in vivo multi-photon imaging in the mouse neocortex down to cortical layer 5.

Neural evidence for cultural differences in the valuation of positive facial expressions.

PubMed

Park, BoKyung; Tsai, Jeanne L; Chim, Louise; Blevins, Elizabeth; Knutson, Brian

2016-02-01

European Americans value excitement more and calm less than Chinese. Within cultures, European Americans value excited and calm states similarly, whereas Chinese value calm more than excited states. To examine how these cultural differences influence people's immediate responses to excited vs calm facial expressions, we combined a facial rating task with functional magnetic resonance imaging. During scanning, European American (n = 19) and Chinese (n = 19) females viewed and rated faces that varied by expression (excited, calm), ethnicity (White, Asian) and gender (male, female). As predicted, European Americans showed greater activity in circuits associated with affect and reward (bilateral ventral striatum, left caudate) while viewing excited vs calm expressions than did Chinese. Within cultures, European Americans responded to excited vs calm expressions similarly, whereas Chinese showed greater activity in these circuits in response to calm vs excited expressions regardless of targets' ethnicity or gender. Across cultural groups, greater ventral striatal activity while viewing excited vs. calm expressions predicted greater preference for excited vs calm expressions months later. These findings provide neural evidence that people find viewing the specific positive facial expressions valued by their cultures to be rewarding and relevant. © The Author (2015). Published by Oxford University Press. For Permissions, please email: journals.permissions@oup.com.

High resolution multiple excitation spot optical microscopy

NASA Astrophysics Data System (ADS)

Dilipkumar, Shilpa; Mondal, Partha Pratim

2011-06-01

We propose fundamental improvements in three-dimensional (3D) resolution of multiple excitation spot optical microscopy. The excitation point spread function (PSF) is generated by two interfering counter-propagating depth-of-focus beams along the optical axis. Detection PSF is obtained by coherently interfering the emitted fluorescent light (collected by both the objectives) at the detector. System PSF shows upto 14-fold reduction in focal volume as compared to confocal, and almost 2-fold improvement in lateral resolution. Proposed PSF has the ability to simultaneously excite multiple 3D-spots of sub-femtoliter volume. Potential applications are in fluorescence microscopy and nanobioimaging.

Photophysical study of some 3-benzoylmethyleneindol-2-ones and estimation of ground and excited states dipole moments from solvatochromic methods using solvent polarity parameters

NASA Astrophysics Data System (ADS)

Saroj, Manju K.; Sharma, Neera; Rastogi, Ramesh C.

2012-03-01

3-Benzoylmethyleneindol-2-ones, isatin based chalcones containing donor and acceptor moieties that exhibit excited-state intramolecular charge transfer, have been studied in different solvents by absorption and emission spectroscopy. The excited state behavior of these compounds is strongly dependent on the nature of substituents and the environment. These compounds show multiple emissions arising from a locally excited state and the two states due to intramolecular processes viz. intramolecular charge transfer (ICT) and excited state intramolecular proton transfer (ESIPT). Excited-state dipole moments have been calculated using Stoke-shifts of LE and ICT states using solvatochromic methods. The higher values of dipole moments obtained lead to support the formation of ICT state as one of the prominent species in the excited states of all 3-benzoylmethyleneindol-2-ones. The correlation of the solvatochromic Stokes-shifts with the microscopic solvent polarity parameter (ETN) was found to be superior to that obtained using bulk solvent polarity functions. The absorption and florescence spectral characteristics have been also investigated as a function of acidity and basicity (Ho/pH) in aqueous phase.

Extension of the Kohn-Sham formulation of density functional theory to finite temperature

DOE PAGES

Gonis, A.; Dane, M.

2017-12-20

Based on Mermin's extension of the Hohenberg and Kohn theorems to non-zero temperature, the Kohn-Sham formulation of density functional theory (KS-DFT) is generalized to finite temperature. Here, we show that present formulations are inconsistent with Mermin's functional containing expressions, in particular describing the Coulomb energy, that defy derivation and are even in violation of rules of logical inference. More; current methodology is in violation of fundamental laws of both quantum and classical mechanics. Based on this feature, we demonstrate the impossibility of extending the KS formalism to finite temperature through the self-consistent solutions of the single-particle Schrödinger equation of T>0.more » Guided by the form of Mermin's functional that depends on the eigenstates of a Hamiltonian, determined at T>0 we base our extension of KS-DFT on the determination of the excited states of a non-interacting system at the zero of temperature. The resulting formulation is consistent with that of Mermin constructing the free energy at T>0 in terms of the excited states of a non-interacting Hamiltonian (system) that, within the KS formalism, are described by Slater determinants. To determine the excited states at T=0 use is made of the extension of the Hohenberg and Kohn theorems to excited states presented in previous work applied here to a non-interacting collection of replicas of a non-interacting N-particle system, whose ground state density is taken to match that of K non-interacting replicas of an interacting N-particle system at T>0. The formalism allows for an ever denser population of the excitation spectrum of a Hamiltonian, within the KS approximation. The form of the auxiliary potential, (Kohn-Sham potential), is formally identical to that in the ground state formalism with the contribution of the Coulomb energy provided by the derivative of the Coulomb energy in all excited states taken into account. Once the excited states are determined, the minimum of the free energy within the KS formalism follows immediately in the form of Mermin's functional, but with the exact excited states in that functional represented by Slater determinants obtained through self-consistency conditions at the zero of temperature. Lastly, it is emphasized that, in departure from all existing formulations, no self-consistency conditions are implemented at finite T; as we show, in fact, such formulations are rigorously blocked.« less

Extension of the Kohn-Sham formulation of density functional theory to finite temperature

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

Gonis, A.; Dane, M.

Based on Mermin's extension of the Hohenberg and Kohn theorems to non-zero temperature, the Kohn-Sham formulation of density functional theory (KS-DFT) is generalized to finite temperature. Here, we show that present formulations are inconsistent with Mermin's functional containing expressions, in particular describing the Coulomb energy, that defy derivation and are even in violation of rules of logical inference. More; current methodology is in violation of fundamental laws of both quantum and classical mechanics. Based on this feature, we demonstrate the impossibility of extending the KS formalism to finite temperature through the self-consistent solutions of the single-particle Schrödinger equation of T>0.more » Guided by the form of Mermin's functional that depends on the eigenstates of a Hamiltonian, determined at T>0 we base our extension of KS-DFT on the determination of the excited states of a non-interacting system at the zero of temperature. The resulting formulation is consistent with that of Mermin constructing the free energy at T>0 in terms of the excited states of a non-interacting Hamiltonian (system) that, within the KS formalism, are described by Slater determinants. To determine the excited states at T=0 use is made of the extension of the Hohenberg and Kohn theorems to excited states presented in previous work applied here to a non-interacting collection of replicas of a non-interacting N-particle system, whose ground state density is taken to match that of K non-interacting replicas of an interacting N-particle system at T>0. The formalism allows for an ever denser population of the excitation spectrum of a Hamiltonian, within the KS approximation. The form of the auxiliary potential, (Kohn-Sham potential), is formally identical to that in the ground state formalism with the contribution of the Coulomb energy provided by the derivative of the Coulomb energy in all excited states taken into account. Once the excited states are determined, the minimum of the free energy within the KS formalism follows immediately in the form of Mermin's functional, but with the exact excited states in that functional represented by Slater determinants obtained through self-consistency conditions at the zero of temperature. Lastly, it is emphasized that, in departure from all existing formulations, no self-consistency conditions are implemented at finite T; as we show, in fact, such formulations are rigorously blocked.« less

Identifying the T=5 states in 48Ca

NASA Astrophysics Data System (ADS)

Upadhyayula, Sriteja; Ahn, Sunghoon; Anastasiou, Maria; Bedoor, Shadi; Browne, Justin; Blackmon, Jeffrey; Deibel, Catherine; Hood, Ashley; Hooker, Joshua; Hunt, Curtis; Koshchiy, Yevgen; Lighthall, Jon; Ong, Wei Jia; Rijal, Nabin; Rogachev, Grigory; Santiago-Gonzalez, Daniel; Nscl, Michigan State University, Ingo

2017-09-01

Particle-hole excitations near closed shells carry information on single-particle energies and on two-body interactions. The particle-hole excitations near the doubly magic nuclei are of special interest. Information on the charge-changing particle-hole excitations (T=5 negative parity states) in 48Ca is not available. We performed an experiment to establish the level scheme of the low-lying negative parity T=5 states in 48Ca. Excitation functions for the 1H(47K,p)47K(g.s.) and 1H(47K,p)47K(3/2+) reactions in the c.m. energy range from 1 MeV to 4.5 MeV were measured. The T=5 states are expected to show up in the p+47K excitation function as narrow resonances. This experiment was performed at NSCL using the ReA3 beam of 47K at energy of 4.6 MeV/u. ANASEN, set in active target mode, was used for this experiment. Experimental results from this experiment will be presented.

On Emulation of Flueric Devices in Excitable Chemical Medium

PubMed Central

Adamatzky, Andrew

2016-01-01

Flueric devices are fluidic devices without moving parts. Fluidic devices use fluid as a medium for information transfer and computation. A Belousov-Zhabotinsky (BZ) medium is a thin-layer spatially extended excitable chemical medium which exhibits travelling excitation wave-fronts. The excitation wave-fronts transfer information. Flueric devices compute via jets interaction. BZ devices compute via excitation wave-fronts interaction. In numerical model of BZ medium we show that functions of key flueric devices are implemented in the excitable chemical system: signal generator, and, xor, not and nor Boolean gates, delay elements, diodes and sensors. Flueric devices have been widely used in industry since late 1960s and are still employed in automotive and aircraft technologies. Implementation of analog of the flueric devices in the excitable chemical systems opens doors to further applications of excitation wave-based unconventional computing in soft robotics, embedded organic electronics and living technologies. PMID:27997561

On Emulation of Flueric Devices in Excitable Chemical Medium.

PubMed

Adamatzky, Andrew

2016-01-01

Flueric devices are fluidic devices without moving parts. Fluidic devices use fluid as a medium for information transfer and computation. A Belousov-Zhabotinsky (BZ) medium is a thin-layer spatially extended excitable chemical medium which exhibits travelling excitation wave-fronts. The excitation wave-fronts transfer information. Flueric devices compute via jets interaction. BZ devices compute via excitation wave-fronts interaction. In numerical model of BZ medium we show that functions of key flueric devices are implemented in the excitable chemical system: signal generator, and, xor, not and nor Boolean gates, delay elements, diodes and sensors. Flueric devices have been widely used in industry since late 1960s and are still employed in automotive and aircraft technologies. Implementation of analog of the flueric devices in the excitable chemical systems opens doors to further applications of excitation wave-based unconventional computing in soft robotics, embedded organic electronics and living technologies.

A method for the direct measurement of electronic site populations in a molecular aggregate using two-dimensional electronic-vibrational spectroscopy

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

Lewis, Nicholas H. C.; Dong, Hui; Oliver, Thomas A. A.

2015-09-28

Two dimensional electronic spectroscopy has proven to be a valuable experimental technique to reveal electronic excitation dynamics in photosynthetic pigment-protein complexes, nanoscale semiconductors, organic photovoltaic materials, and many other types of systems. It does not, however, provide direct information concerning the spatial structure and dynamics of excitons. 2D infrared spectroscopy has become a widely used tool for studying structural dynamics but is incapable of directly providing information concerning electronic excited states. 2D electronic-vibrational (2DEV) spectroscopy provides a link between these domains, directly connecting the electronic excitation with the vibrational structure of the system under study. In this work, we derivemore » response functions for the 2DEV spectrum of a molecular dimer and propose a method by which 2DEV spectra could be used to directly measure the electronic site populations as a function of time following the initial electronic excitation. We present results from the response function simulations which show that our proposed approach is substantially valid. This method provides, to our knowledge, the first direct experimental method for measuring the electronic excited state dynamics in the spatial domain, on the molecular scale.« less

A method for the direct measurement of electronic site populations in a molecular aggregate using two-dimensional electronic-vibrational spectroscopy

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

Lewis, Nicholas H. C.; Dong, Hui; Oliver, Thomas A. A.

2015-09-28

Two dimensional electronic spectroscopy has proved to be a valuable experimental technique to reveal electronic excitation dynamics in photosynthetic pigment-protein complexes, nanoscale semiconductors, organic photovoltaic materials, and many other types of systems. It does not, however, provide direct information concerning the spatial structure and dynamics of excitons. 2D infrared spectroscopy has become a widely used tool for studying structural dynamics but is incapable of directly providing information concerning electronic excited states. 2D electronic-vibrational (2DEV) spectroscopy provides a link between these domains, directly connecting the electronic excitation with the vibrational structure of the system under study. In this work, we derivemore » response functions for the 2DEV spectrum of a molecular dimer and propose a method by which 2DEV spectra could be used to directly measure the electronic site populations as a function of time following the initial electronic excitation. We present results from the response function simulations which show that our proposed approach is substantially valid. This method provides, to our knowledge, the first direct experimental method for measuring the electronic excited state dynamics in the spatial domain, on the molecular scale.« less

A method for the direct measurement of electronic site populations in a molecular aggregate using two-dimensional electronic-vibrational spectroscopy.

PubMed

Lewis, Nicholas H C; Dong, Hui; Oliver, Thomas A A; Fleming, Graham R

2015-09-28

Two dimensional electronic spectroscopy has proved to be a valuable experimental technique to reveal electronic excitation dynamics in photosynthetic pigment-protein complexes, nanoscale semiconductors, organic photovoltaic materials, and many other types of systems. It does not, however, provide direct information concerning the spatial structure and dynamics of excitons. 2D infrared spectroscopy has become a widely used tool for studying structural dynamics but is incapable of directly providing information concerning electronic excited states. 2D electronic-vibrational (2DEV) spectroscopy provides a link between these domains, directly connecting the electronic excitation with the vibrational structure of the system under study. In this work, we derive response functions for the 2DEV spectrum of a molecular dimer and propose a method by which 2DEV spectra could be used to directly measure the electronic site populations as a function of time following the initial electronic excitation. We present results from the response function simulations which show that our proposed approach is substantially valid. This method provides, to our knowledge, the first direct experimental method for measuring the electronic excited state dynamics in the spatial domain, on the molecular scale.

Abnormal cell-intrinsic and network excitability in the neocortex of serotonin-deficient Pet-1 knockout mice.

PubMed

Puzerey, Pavel A; Kodama, Nathan X; Galán, Roberto F

2016-02-01

Neurons originating from the raphe nuclei of the brain stem are the exclusive source of serotonin (5-HT) to the cortex. Their serotonergic phenotype is specified by the transcriptional regulator Pet-1, which is also necessary for maintaining their neurotransmitter identity across development. Transgenic mice in which Pet-1 is genetically ablated (Pet-1(-/-)) show a dramatic reduction (∼80%) in forebrain 5-HT levels, yet no investigations have been carried out to assess the impact of such severe 5-HT depletion on the function of target cortical neurons. Using whole cell patch-clamp methods, two-dimensional (2D) multielectrode arrays (MEAs), 3D morphological neuronal reconstructions, and animal behavior, we investigated the impact of 5-HT depletion on cortical cell-intrinsic and network excitability. We found significant changes in several parameters of cell-intrinsic excitability in cortical pyramidal cells (PCs) as well as an increase in spontaneous synaptic excitation through 5-HT3 receptors. These changes are associated with increased local network excitability and oscillatory activity in a 5-HT2 receptor-dependent manner, consistent with previously reported hypersensitivity of cortical 5-HT2 receptors. PC morphology was also altered, with a significant reduction in dendritic complexity that may possibly act as a compensatory mechanism for increased excitability. Consistent with this interpretation, when we carried out experiments with convulsant-induced seizures to asses cortical excitability in vivo, we observed no significant differences in seizure parameters between wild-type and Pet-1(-/-) mice. Moreover, MEA recordings of propagating field potentials showed diminished propagation of activity across the cortical sheath. Together these findings reveal novel functional changes in neuronal and cortical excitability in mice lacking Pet-1. Copyright © 2016 the American Physiological Society.

Abnormal cell-intrinsic and network excitability in the neocortex of serotonin-deficient Pet-1 knockout mice

PubMed Central

Puzerey, Pavel A.; Kodama, Nathan X.

2015-01-01

Neurons originating from the raphe nuclei of the brain stem are the exclusive source of serotonin (5-HT) to the cortex. Their serotonergic phenotype is specified by the transcriptional regulator Pet-1, which is also necessary for maintaining their neurotransmitter identity across development. Transgenic mice in which Pet-1 is genetically ablated (Pet-1−/−) show a dramatic reduction (∼80%) in forebrain 5-HT levels, yet no investigations have been carried out to assess the impact of such severe 5-HT depletion on the function of target cortical neurons. Using whole cell patch-clamp methods, two-dimensional (2D) multielectrode arrays (MEAs), 3D morphological neuronal reconstructions, and animal behavior, we investigated the impact of 5-HT depletion on cortical cell-intrinsic and network excitability. We found significant changes in several parameters of cell-intrinsic excitability in cortical pyramidal cells (PCs) as well as an increase in spontaneous synaptic excitation through 5-HT3 receptors. These changes are associated with increased local network excitability and oscillatory activity in a 5-HT2 receptor-dependent manner, consistent with previously reported hypersensitivity of cortical 5-HT2 receptors. PC morphology was also altered, with a significant reduction in dendritic complexity that may possibly act as a compensatory mechanism for increased excitability. Consistent with this interpretation, when we carried out experiments with convulsant-induced seizures to asses cortical excitability in vivo, we observed no significant differences in seizure parameters between wild-type and Pet-1−/− mice. Moreover, MEA recordings of propagating field potentials showed diminished propagation of activity across the cortical sheath. Together these findings reveal novel functional changes in neuronal and cortical excitability in mice lacking Pet-1. PMID:26609119

Electronic structure and optical properties of CdSxSe1-x solid solution nanostructures from X-ray absorption near edge structure, X-ray excited optical luminescence, and density functional theory investigations

NASA Astrophysics Data System (ADS)

Murphy, M. W.; Yiu, Y. M.; Ward, M. J.; Liu, L.; Hu, Y.; Zapien, J. A.; Liu, Yingkai; Sham, T. K.

2014-11-01

The electronic structure and optical properties of a series of iso-electronic and iso-structural CdSxSe1-x solid solution nanostructures have been investigated using X-ray absorption near edge structure, extended X-ray absorption fine structure, and X-ray excited optical luminescence at various absorption edges of Cd, S, and Se. It is found that the system exhibits compositions, with variable local structure in-between that of CdS and CdSe accompanied by tunable optical band gap between that of CdS and CdSe. Theoretical calculation using density functional theory has been carried out to elucidate the observations. It is also found that luminescence induced by X-ray excitation shows new optical channels not observed previously with laser excitation. The implications of these observations are discussed.

Multiconfiguration Pair-Density Functional Theory Spectral Calculations Are Stable to Adding Diffuse Basis Functions.

PubMed

Hoyer, Chad E; Gagliardi, Laura; Truhlar, Donald G

2015-11-05

Time-dependent Kohn-Sham density functional theory (TD-KS-DFT) is useful for calculating electronic excitation spectra of large systems, but the low-energy spectra are often complicated by artificially lowered higher-energy states. This affects even the lowest energy excited states. Here, by calculating the lowest energy spin-conserving excited state for atoms from H to K and for formaldehyde, we show that this problem does not occur in multiconfiguration pair-density functional theory (MC-PDFT). We use the tPBE on-top density functional, which is a translation of the PBE exchange-correlation functional. We compare to a robust multireference method, namely, complete active space second-order perturbation theory (CASPT2), and to TD-KS-DFT with two popular exchange-correlation functionals, PBE and PBE0. We find for atoms that the mean unsigned error (MUE) of MC-PDFT with the tPBE functional improves from 0.42 to 0.40 eV with a double set of diffuse functions, whereas the MUEs for PBE and PBE0 drastically increase from 0.74 to 2.49 eV and from 0.45 to 1.47 eV, respectively.

Hydrological excitation of polar motion by different variables of the GLDAS models

NASA Astrophysics Data System (ADS)

Wińska, Małgorzata; Nastula, Jolanta

Continental hydrological loading, by land water, snow, and ice, is an element that is strongly needed for a full understanding of the excitation of polar motion. In this study we compute different estimations of hydrological excitation functions of polar motion (Hydrological Angular Momentum - HAM) using various variables from the Global Land Data Assimilation System (GLDAS) models of land hydrosphere. The main aim of this study is to show the influence of different variables for example: total evapotranspiration, runoff, snowmelt, soil moisture to polar motion excitations in annual and short term scale. In our consideration we employ several realizations of the GLDAS model as: GLDAS Common Land Model (CLM), GLDAS Mosaic Model, GLDAS National Centers for Environmental Prediction/Oregon State University/Air Force/Hydrologic Research Lab Model (Noah), GLDAS Variable Infiltration Capacity (VIC) Model. Hydrological excitation functions of polar motion, both global and regional, are determined by using selected variables of these GLDAS realizations. First we compare a timing, spectra and phase diagrams of different regional and global HAMs with each other. Next, we estimate, the hydrological signal in geodetically observed polar motion excitation by subtracting the atmospheric -- AAM (pressure + wind) and oceanic -- OAM (bottom pressure + currents) contributions. Finally, the hydrological excitations are compared to these hydrological signal in observed polar motion excitation series. The results help us understand which variables of considered hydrological models are the most important for the polar motion excitation and how well we can close polar motion excitation budget in the seasonal and inter-annual spectral ranges.

Wave Function and Emergent SU(2) Symmetry in the νT=1 Quantum Hall Bilayer

NASA Astrophysics Data System (ADS)

Lian, Biao; Zhang, Shou-Cheng

2018-02-01

We propose a trial wave function for the quantum Hall bilayer system of total filling factor νT=1 at a layer distance d to magnetic length ℓ ratio d /ℓ=κc 1≈1.1 , where the lowest charged excitation is known to have a level crossing. The wave function has two-particle correlations, which fit well with those in previous numerical studies, and can be viewed as a Bose-Einstein condensate of free excitons formed by composite bosons and anticomposite bosons in different layers. We show the free nature of these excitons indicating an emergent SU(2) symmetry for the composite bosons at d /ℓ=κc 1, which leads to the level crossing in low-lying charged excitations. We further show the overlap between the trial wave function, and the ground state of a small size exact diagonalization is peaked near d /ℓ=κc 1, which supports our theory.

Rapid activity-dependent modulation of the intrinsic excitability through up-regulation of KCNQ/Kv7 channel function in neonatal spinal motoneurons.

PubMed

Lombardo, Joseph; Sun, Jianli; Harrington, Melissa A

2018-01-01

Activity-dependent changes in the properties of the motor system underlie the necessary adjustments in its responsiveness on the basis of the environmental and developmental demands of the organism. Although plastic changes in the properties of the spinal cord have historically been neglected because of the archaic belief that the spinal cord is constituted by a hardwired network that simply relays information to muscles, plenty of evidence has been accumulated showing that synapses impinging on spinal motoneurons undergo short- and long-term plasticity. In the brain, brief changes in the activity level of the network have been shown to be paralleled by changes in the intrinsic excitability of the neurons and are suggested to either reinforce or stabilize the changes at the synaptic level. However, rapid activity-dependent changes in the intrinsic properties of spinal motoneurons have never been reported. In this study, we show that in neonatal mice the intrinsic excitability of spinal motoneurons is depressed after relatively brief but sustained changes in the spinal cord network activity. Using electrophysiological techniques together with specific pharmacological blockers of KCNQ/Kv7 channels, we demonstrate their involvement in the reduction of the intrinsic excitability of spinal motoneurons. This action results from an increased M-current, the product of the activation of KCNQ/Kv7 channels, which leads to a hyperpolarization of the resting membrane potential and a decrease in the input resistance of spinal motoneurons. Computer simulations showed that specific up-regulations in KCNQ/Kv7 channels functions lead to a modulation of the intrinsic excitability of spinal motoneurons as observed experimentally. These results indicate that KCNQ/Kv7 channels play a fundamental role in the activity-dependent modulation of the excitability of spinal motoneurons.

Combining extrapolation with ghost interaction correction in range-separated ensemble density functional theory for excited states

NASA Astrophysics Data System (ADS)

Alam, Md. Mehboob; Deur, Killian; Knecht, Stefan; Fromager, Emmanuel

2017-11-01

The extrapolation technique of Savin [J. Chem. Phys. 140, 18A509 (2014)], which was initially applied to range-separated ground-state-density-functional Hamiltonians, is adapted in this work to ghost-interaction-corrected (GIC) range-separated ensemble density-functional theory (eDFT) for excited states. While standard extrapolations rely on energies that decay as μ-2 in the large range-separation-parameter μ limit, we show analytically that (approximate) range-separated GIC ensemble energies converge more rapidly (as μ-3) towards their pure wavefunction theory values (μ → +∞ limit), thus requiring a different extrapolation correction. The purpose of such a correction is to further improve on the convergence and, consequently, to obtain more accurate excitation energies for a finite (and, in practice, relatively small) μ value. As a proof of concept, we apply the extrapolation method to He and small molecular systems (viz., H2, HeH+, and LiH), thus considering different types of excitations such as Rydberg, charge transfer, and double excitations. Potential energy profiles of the first three and four singlet Σ+ excitation energies in HeH+ and H2, respectively, are studied with a particular focus on avoided crossings for the latter. Finally, the extraction of individual state energies from the ensemble energy is discussed in the context of range-separated eDFT, as a perspective.

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

Davidson, J.

Relative and absolute populations of 19 levels in beam-foil--excited neutral helium at 0.275 MeV have been measured. The singlet angular-momentum sequences show dependences on principal quantum number consistent with n$sup -3$, but the triplet sequences do not. Singlet and triplet angular-momentum sequences show similar dependences on level excitation energy. Excitation functions for six representative levels were measured in the range 0.160 to 0.500 MeV. The absolute level populations increase with energy, whereas the neutral fraction of the beam decreases with energy. Further, the P angular-momentum levels are found to be overpopulated with respect to the S and D levels. Themore » overpopulation decreases with increasing principal quantum number.« less

Theory of spin-conserving excitation of the N-V(-) center in diamond.

PubMed

Gali, Adam; Janzén, Erik; Deák, Péter; Kresse, Georg; Kaxiras, Efthimios

2009-10-30

The negatively charged nitrogen-vacancy defect in diamond is an important atomic-scale structure that can be used as a qubit in quantum computing and as a marker in biomedical applications. Its usefulness relies on the ability to optically excite electrons between well-defined gap states, which requires a clear and detailed understanding of the relevant states and excitation processes. Here we show that by using hybrid density-functional-theory calculations in a large supercell we can reproduce the zero-phonon line and the Stokes and anti-Stokes shifts, yielding a complete picture of the spin-conserving excitation of this defect.

Transform-limited-pulse representation of excitation with natural incoherent light

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

Chenu, Aurélia, E-mail: aurelia.chenu@utoronto.ca; Brumer, Paul, E-mail: pbrumer@chem.utoronto.ca

2016-01-28

The excitation of molecular systems by natural incoherent light relevant, for example, to photosynthetic light-harvesting is examined. We show that the result of linear excitation with natural incoherent light can be obtained using incident light described in terms of transform limited pulses, as opposed to conventional classical representations with explicit random character. The derived expressions allow for computations to be done directly for any thermal light spectrum using a simple wave function formalism and provide a route to the experimental determination of natural incoherent excitation using pulsed laser techniques. Pulses associated with solar and cosmic microwave background radiation are providedmore » as examples.« less

Hot topics: Signal processing in acoustics

NASA Astrophysics Data System (ADS)

Gaumond, Charles F.

2005-09-01

Signal processing in acoustics is a multidisciplinary group of people that work in many areas of acoustics. We have chosen two areas that have shown exciting new applications of signal processing to acoustics or have shown exciting and important results from the use of signal processing. In this session, two hot topics are shown: the use of noiselike acoustic fields to determine sound propagation structure and the use of localization to determine animal behaviors. The first topic shows the application of correlation on geo-acoustic fields to determine the Greens function for propagation through the Earth. These results can then be further used to solve geo-acoustic inverse problems. The first topic also shows the application of correlation using oceanic noise fields to determine the Greens function through the ocean. These results also have utility for oceanic inverse problems. The second topic shows exciting results from the detection, localization, and tracking of marine mammals by two different groups. Results from detection and localization of bullfrogs are shown, too. Each of these studies contributed to the knowledge of animal behavior. [Work supported by ONR.

Multi-quasiparticle excitations in 145Tb

NASA Astrophysics Data System (ADS)

Zheng, Y.; Zhou, X. H.; Zhang, Y. H.; Hayakawa, T.; Oshima, M.; Toh, Y.; Shizuma, T.; Katakura, J.; Hatsukawa, Y.; Matsuda, M.; Kusakari, H.; Sugawara, M.; Furuno, K.; Komatsubara, T.

2004-04-01

High-spin states in 145Tb have been investigated by means of in-beam ggr-ray spectroscopy techniques with the 118Sn(32S, 1p4n) reaction. Excitation functions, X-ggr-t and ggr-ggr-t coincidences and ggr-ray anisotropies were measured. A level scheme of 145Tb was established up to Exap 7 MeV. The level structure shows characteristics of a spherical nucleus. Based on the systematics of level structure in the odd-A N = 80 isotones, the level structure below 2 MeV excitation is interpreted by coupling an h11/2 proton to the excitations in the even-even 144Gd core. Above 2 MeV excitation, most of the yrast levels are interpreted with multi-quasiparticle shell-model configurations.

Experimental evidence of exciton-plasmon coupling in densely packed dye doped core-shell nanoparticles obtained via microfluidic technique

NASA Astrophysics Data System (ADS)

De Luca, A.; Iazzolino, A.; Salmon, J.-B.; Leng, J.; Ravaine, S.; Grigorenko, A. N.; Strangi, G.

2014-09-01

The interplay between plasmons and excitons in bulk metamaterials are investigated by performing spectroscopic studies, including variable angle pump-probe ellipsometry. Gain functionalized gold nanoparticles have been densely packed through a microfluidic chip, representing a scalable process towards bulk metamaterials based on self-assembly approach. Chromophores placed at the hearth of plasmonic subunits ensure exciton-plasmon coupling to convey excitation energy to the quasi-static electric field of the plasmon states. The overall complex polarizability of the system, probed by variable angle spectroscopic ellipsometry, shows a significant modification under optical excitation, as demonstrated by the behavior of the ellipsometric angles Ψ and Δ as a function of suitable excitation fields. The plasmon resonances observed in densely packed gain functionalized core-shell gold nanoparticles represent a promising step to enable a wide range of electromagnetic properties and fascinating applications of plasmonic bulk systems for advanced optical materials.

Spillover-mediated feedforward-inhibition functionally segregates interneuron activity

PubMed Central

Coddington, Luke T.; Rudolph, Stephanie; Lune, Patrick Vande; Overstreet-Wadiche, Linda; Wadiche, Jacques I.

2013-01-01

Summary Neurotransmitter spillover represents a form of neural transmission not restricted to morphologically defined synaptic connections. Communication between climbing fibers (CFs) and molecular layer interneurons (MLIs) in the cerebellum is mediated exclusively by glutamate spillover. Here, we show how CF stimulation functionally segregates MLIs based on their location relative to glutamate release. Excitation of MLIs that reside within the domain of spillover diffusion coordinates inhibition of MLIs outside the diffusion limit. CF excitation of MLIs is dependent on extrasynaptic NMDA receptors that enhance the spatial and temporal spread of CF signaling. Activity mediated by functionally segregated MLIs converges onto neighboring Purkinje cells (PCs) to generate a long-lasting biphasic change in inhibition. These data demonstrate how glutamate release from single CFs modulates excitability of neighboring PCs, thus expanding the influence of CFs on cerebellar cortical activity in a manner not predicted by anatomical connectivity. PMID:23707614

Active Dendrites Enhance Neuronal Dynamic Range

PubMed Central

Gollo, Leonardo L.; Kinouchi, Osame; Copelli, Mauro

2009-01-01

Since the first experimental evidences of active conductances in dendrites, most neurons have been shown to exhibit dendritic excitability through the expression of a variety of voltage-gated ion channels. However, despite experimental and theoretical efforts undertaken in the past decades, the role of this excitability for some kind of dendritic computation has remained elusive. Here we show that, owing to very general properties of excitable media, the average output of a model of an active dendritic tree is a highly non-linear function of its afferent rate, attaining extremely large dynamic ranges (above 50 dB). Moreover, the model yields double-sigmoid response functions as experimentally observed in retinal ganglion cells. We claim that enhancement of dynamic range is the primary functional role of active dendritic conductances. We predict that neurons with larger dendritic trees should have larger dynamic range and that blocking of active conductances should lead to a decrease in dynamic range. PMID:19521531

Relaxation and collective excitations of cluster nano-plasmas

NASA Astrophysics Data System (ADS)

Reinholz, Heidi; Röpke, Gerd; Broda, Ingrid; Morozov, Igor; Bystryi, Roman; Lavrinenko, Yaroslav

2018-01-01

Nano-plasmas produced, for example, in clusters after short-pulse laser irradiation, can show collective excitations, as derived from the time evolution of fluctuations in thermodynamic equilibrium. Molecular dynamical simulations are performed for various cluster sizes. New data are obtained for the minimum value of the stationary cluster charge. The bi-local autocorrelation function gives the spatial structure of the eigenmodes, for which energy eigenvalues are obtained. By varying the cluster size, starting from a few-particle cluster, the emergence of macroscopic properties such as collective excitations is shown.

Excitation energies of molecules within time-independent density functional theory

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

Hemanadhan, M., E-mail: hemanadh@iitk.ac.in; Harbola, Manoj K., E-mail: hemanadh@iitk.ac.in

2014-04-24

Recently proposed exchange energy functional for excited-states is tested for obtaining excitation energies of diatomic molecules. The functional is the ground-state counterpart of the local-density approximation, the modified local spin density (MLSD). The MLSD functional is tested for the N{sub 2} and CO diatomic molecules. The excitation energy obtained with the MLSD functional for the N{sub 2} molecule is in close vicinity to that obtained from the exact exchange orbital functional, Krieger, Li and Iafrate (KLI). For the CO molecule, the departure in excitation energy is observed and is due to the overcorrection of self-interaction.

Excitation energies of molecules within time-independent density functional theory

NASA Astrophysics Data System (ADS)

Hemanadhan, M.; Harbola, Manoj K.

2014-04-01

Recently proposed exchange energy functional for excited-states is tested for obtaining excitation energies of diatomic molecules. The functional is the ground-state counterpart of the local-density approximation, the modified local spin density (MLSD). The MLSD functional is tested for the N2 and CO diatomic molecules. The excitation energy obtained with the MLSD functional for the N2 molecule is in close vicinity to that obtained from the exact exchange orbital functional, Krieger, Li and Iafrate (KLI). For the CO molecule, the departure in excitation energy is observed and is due to the overcorrection of self-interaction.

Variation in Differential and Total Cross Sections Due to Different Radial Wave Functions

ERIC Educational Resources Information Center

Williamson, W., Jr.; Greene, T.

1976-01-01

Three sets of analytical wave functions are used to calculate the Na (3s---3p) transition differential and total electron excitation cross sections by Born approximations. Results show expected large variations in values. (Author/CP)

Layer-specific excitation/inhibition balances during neuronal synchronization in the visual cortex.

PubMed

Adesnik, Hillel

2018-05-01

Understanding the balance between synaptic excitation and inhibition in cortical circuits in the brain, and how this contributes to cortical rhythms, is fundamental to explaining information processing in the cortex. This study used cortical layer-specific optogenetic activation in mouse cortex to show that excitatory neurons in any cortical layer can drive powerful gamma rhythms, while inhibition balances excitation. The net impact of this is to keep activity within each layer in check, but simultaneously to promote the propagation of activity to downstream layers. The data show that rhythm-generating circuits exist in all principle layers of the cortex, and provide layer-specific balances of excitation and inhibition that affect the flow of information across the layers. Rhythmic activity can synchronize neural ensembles within and across cortical layers. While gamma band rhythmicity has been observed in all layers, the laminar sources and functional impacts of neuronal synchronization in the cortex remain incompletely understood. Here, layer-specific optogenetic stimulation demonstrates that populations of excitatory neurons in any cortical layer of the mouse's primary visual cortex are sufficient to powerfully entrain neuronal oscillations in the gamma band. Within each layer, inhibition balances excitation and keeps activity in check. Across layers, translaminar output overcomes inhibition and drives downstream firing. These data establish that rhythm-generating circuits exist in all principle layers of the cortex, but provide layer-specific balances of excitation and inhibition that may dynamically shape the flow of information through cortical circuits. These data might help explain how excitation/inhibition (E/I) balances across cortical layers shape information processing, and shed light on the diverse nature and functional impacts of cortical gamma rhythms. © 2018 The Authors. The Journal of Physiology © 2018 The Physiological Society.

Homeostatic Scaling of Excitability in Recurrent Neural Networks

PubMed Central

Remme, Michiel W. H.; Wadman, Wytse J.

2012-01-01

Neurons adjust their intrinsic excitability when experiencing a persistent change in synaptic drive. This process can prevent neural activity from moving into either a quiescent state or a saturated state in the face of ongoing plasticity, and is thought to promote stability of the network in which neurons reside. However, most neurons are embedded in recurrent networks, which require a delicate balance between excitation and inhibition to maintain network stability. This balance could be disrupted when neurons independently adjust their intrinsic excitability. Here, we study the functioning of activity-dependent homeostatic scaling of intrinsic excitability (HSE) in a recurrent neural network. Using both simulations of a recurrent network consisting of excitatory and inhibitory neurons that implement HSE, and a mean-field description of adapting excitatory and inhibitory populations, we show that the stability of such adapting networks critically depends on the relationship between the adaptation time scales of both neuron populations. In a stable adapting network, HSE can keep all neurons functioning within their dynamic range, while the network is undergoing several (patho)physiologically relevant types of plasticity, such as persistent changes in external drive, changes in connection strengths, or the loss of inhibitory cells from the network. However, HSE cannot prevent the unstable network dynamics that result when, due to such plasticity, recurrent excitation in the network becomes too strong compared to feedback inhibition. This suggests that keeping a neural network in a stable and functional state requires the coordination of distinct homeostatic mechanisms that operate not only by adjusting neural excitability, but also by controlling network connectivity. PMID:22570604

Constraining nuclear photon strength functions by the decay properties of photo-excited states

NASA Astrophysics Data System (ADS)

Isaak, J.; Savran, D.; Krtička, M.; Ahmed, M. W.; Beller, J.; Fiori, E.; Glorius, J.; Kelley, J. H.; Löher, B.; Pietralla, N.; Romig, C.; Rusev, G.; Scheck, M.; Schnorrenberger, L.; Silva, J.; Sonnabend, K.; Tonchev, A. P.; Tornow, W.; Weller, H. R.; Zweidinger, M.

2013-12-01

A new approach for constraining the low-energy part of the electric dipole Photon Strength Function (E1-PSF) is presented. Experiments at the Darmstadt High-Intensity Photon Setup and the High Intensity γ→-Ray Source have been performed to investigate the decay properties of 130Te between 5.50 and 8.15 MeV excitation energy. In particular, the average γ-ray branching ratio to the ground state and the population intensity of low-lying excited states have been studied. A comparison to the statistical model shows that the latter is sensitive to the low-energy behavior of the E1-PSF, while the average ground state branching ratio cannot be described by the statistical model in the energy range between 5.5 and 6.5 MeV.

Temperature Effects of Electric Field on the First Excited State of Strong Coupling Polaron in a CsI Quantum Pseudodot

NASA Astrophysics Data System (ADS)

Sun, Yong; Ding, Zhao-Hua; Xiao, Jing-Lin

2017-03-01

Employing variational method of Pekar type (VMPT), this paper investigates the first-excited state energy (FESE), excitation energy and transition frequency of the strongly-coupled polaron in the CsI quantum pseudodot (QPD) with electric field. The temperature effects on the strong-coupling polaron in electric field are calculated by using the quantum statistical theory (QST). The results from the present investigation show that the FESE, excitation energy and transition frequency increase (decrease) firstly and then at lower (higher) temperature regions. They are decreasing functions of the electric field strength. Supported by the National Natural Science Foundation of China under Grant No. 11464033

Multireference Density Functional Theory with Generalized Auxiliary Systems for Ground and Excited States.

PubMed

Chen, Zehua; Zhang, Du; Jin, Ye; Yang, Yang; Su, Neil Qiang; Yang, Weitao

2017-09-21

To describe static correlation, we develop a new approach to density functional theory (DFT), which uses a generalized auxiliary system that is of a different symmetry, such as particle number or spin, from that of the physical system. The total energy of the physical system consists of two parts: the energy of the auxiliary system, which is determined with a chosen density functional approximation (DFA), and the excitation energy from an approximate linear response theory that restores the symmetry to that of the physical system, thus rigorously leading to a multideterminant description of the physical system. The electron density of the physical system is different from that of the auxiliary system and is uniquely determined from the functional derivative of the total energy with respect to the external potential. Our energy functional is thus an implicit functional of the physical system density, but an explicit functional of the auxiliary system density. We show that the total energy minimum and stationary states, describing the ground and excited states of the physical system, can be obtained by a self-consistent optimization with respect to the explicit variable, the generalized Kohn-Sham noninteracting density matrix. We have developed the generalized optimized effective potential method for the self-consistent optimization. Among options of the auxiliary system and the associated linear response theory, reformulated versions of the particle-particle random phase approximation (pp-RPA) and the spin-flip time-dependent density functional theory (SF-TDDFT) are selected for illustration of principle. Numerical results show that our multireference DFT successfully describes static correlation in bond dissociation and double bond rotation.

Dose-Dependent Effects of Theta Burst rTMS on Cortical Excitability and Resting-State Connectivity of the Human Motor System

PubMed Central

Nettekoven, Charlotte; Volz, Lukas J.; Kutscha, Martha; Pool, Eva-Maria; Rehme, Anne K.; Eickhoff, Simon B.; Fink, Gereon R.

2014-01-01

Theta burst stimulation (TBS), a specific protocol of repetitive transcranial magnetic stimulation (rTMS), induces changes in cortical excitability that last beyond stimulation. TBS-induced aftereffects, however, vary between subjects, and the mechanisms underlying these aftereffects to date remain poorly understood. Therefore, the purpose of this study was to investigate whether increasing the number of pulses of intermittent TBS (iTBS) (1) increases cortical excitability as measured by motor-evoked potentials (MEPs) and (2) alters functional connectivity measured using resting-state fMRI, in a dose-dependent manner. Sixteen healthy, human subjects received three serially applied iTBS blocks of 600 pulses over the primary motor cortex (M1 stimulation) and the parieto-occipital vertex (sham stimulation) to test for dose-dependent iTBS effects on cortical excitability and functional connectivity (four sessions in total). iTBS over M1 increased MEP amplitudes compared with sham stimulation after each stimulation block. Although the increase in MEP amplitudes did not differ between the first and second block of M1 stimulation, we observed a significant increase after three blocks (1800 pulses). Furthermore, iTBS enhanced resting-state functional connectivity between the stimulated M1 and premotor regions in both hemispheres. Functional connectivity between M1 and ipsilateral dorsal premotor cortex further increased dose-dependently after 1800 pulses of iTBS over M1. However, no correlation between changes in MEP amplitudes and functional connectivity was detected. In summary, our data show that increasing the number of iTBS stimulation blocks results in dose-dependent effects at the local level (cortical excitability) as well as at a systems level (functional connectivity) with a dose-dependent enhancement of dorsal premotor cortex-M1 connectivity. PMID:24828639

Topological determinants of self-sustained activity in a simple model of excitable dynamics on graphs

PubMed Central

Fretter, Christoph; Lesne, Annick; Hilgetag, Claus C.; Hütt, Marc-Thorsten

2017-01-01

Simple models of excitable dynamics on graphs are an efficient framework for studying the interplay between network topology and dynamics. This topic is of practical relevance to diverse fields, ranging from neuroscience to engineering. Here we analyze how a single excitation propagates through a random network as a function of the excitation threshold, that is, the relative amount of activity in the neighborhood required for the excitation of a node. We observe that two sharp transitions delineate a region of sustained activity. Using analytical considerations and numerical simulation, we show that these transitions originate from the presence of barriers to propagation and the excitation of topological cycles, respectively, and can be predicted from the network topology. Our findings are interpreted in the context of network reverberations and self-sustained activity in neural systems, which is a question of long-standing interest in computational neuroscience. PMID:28186182

Topological determinants of self-sustained activity in a simple model of excitable dynamics on graphs.

PubMed

Fretter, Christoph; Lesne, Annick; Hilgetag, Claus C; Hütt, Marc-Thorsten

2017-02-10

Simple models of excitable dynamics on graphs are an efficient framework for studying the interplay between network topology and dynamics. This topic is of practical relevance to diverse fields, ranging from neuroscience to engineering. Here we analyze how a single excitation propagates through a random network as a function of the excitation threshold, that is, the relative amount of activity in the neighborhood required for the excitation of a node. We observe that two sharp transitions delineate a region of sustained activity. Using analytical considerations and numerical simulation, we show that these transitions originate from the presence of barriers to propagation and the excitation of topological cycles, respectively, and can be predicted from the network topology. Our findings are interpreted in the context of network reverberations and self-sustained activity in neural systems, which is a question of long-standing interest in computational neuroscience.

Topological determinants of self-sustained activity in a simple model of excitable dynamics on graphs

NASA Astrophysics Data System (ADS)

Fretter, Christoph; Lesne, Annick; Hilgetag, Claus C.; Hütt, Marc-Thorsten

2017-02-01

Simple models of excitable dynamics on graphs are an efficient framework for studying the interplay between network topology and dynamics. This topic is of practical relevance to diverse fields, ranging from neuroscience to engineering. Here we analyze how a single excitation propagates through a random network as a function of the excitation threshold, that is, the relative amount of activity in the neighborhood required for the excitation of a node. We observe that two sharp transitions delineate a region of sustained activity. Using analytical considerations and numerical simulation, we show that these transitions originate from the presence of barriers to propagation and the excitation of topological cycles, respectively, and can be predicted from the network topology. Our findings are interpreted in the context of network reverberations and self-sustained activity in neural systems, which is a question of long-standing interest in computational neuroscience.

Non-empirical exchange-correlation parameterizations based on exact conditions from correlated orbital theory.

PubMed

Haiduke, Roberto Luiz A; Bartlett, Rodney J

2018-05-14

Some of the exact conditions provided by the correlated orbital theory are employed to propose new non-empirical parameterizations for exchange-correlation functionals from Density Functional Theory (DFT). This reparameterization process is based on range-separated functionals with 100% exact exchange for long-range interelectronic interactions. The functionals developed here, CAM-QTP-02 and LC-QTP, show mitigated self-interaction error, correctly predict vertical ionization potentials as the negative of eigenvalues for occupied orbitals, and provide nice excitation energies, even for challenging charge-transfer excited states. Moreover, some improvements are observed for reaction barrier heights with respect to the other functionals belonging to the quantum theory project (QTP) family. Finally, the most important achievement of these new functionals is an excellent description of vertical electron affinities (EAs) of atoms and molecules as the negative of appropriate virtual orbital eigenvalues. In this case, the mean absolute deviations for EAs in molecules are smaller than 0.10 eV, showing that physical interpretation can indeed be ascribed to some unoccupied orbitals from DFT.

Non-empirical exchange-correlation parameterizations based on exact conditions from correlated orbital theory

NASA Astrophysics Data System (ADS)

Haiduke, Roberto Luiz A.; Bartlett, Rodney J.

2018-05-01

Some of the exact conditions provided by the correlated orbital theory are employed to propose new non-empirical parameterizations for exchange-correlation functionals from Density Functional Theory (DFT). This reparameterization process is based on range-separated functionals with 100% exact exchange for long-range interelectronic interactions. The functionals developed here, CAM-QTP-02 and LC-QTP, show mitigated self-interaction error, correctly predict vertical ionization potentials as the negative of eigenvalues for occupied orbitals, and provide nice excitation energies, even for challenging charge-transfer excited states. Moreover, some improvements are observed for reaction barrier heights with respect to the other functionals belonging to the quantum theory project (QTP) family. Finally, the most important achievement of these new functionals is an excellent description of vertical electron affinities (EAs) of atoms and molecules as the negative of appropriate virtual orbital eigenvalues. In this case, the mean absolute deviations for EAs in molecules are smaller than 0.10 eV, showing that physical interpretation can indeed be ascribed to some unoccupied orbitals from DFT.

Molecular excited states from the SCAN functional

NASA Astrophysics Data System (ADS)

Tozer, David J.; Peach, Michael J. G.

2018-06-01

The performance of the strongly constrained and appropriately normed (SCAN) meta-generalised gradient approximation exchange-correlation functional is investigated for the calculation of time-dependent density-functional theory molecular excitation energies of local, charge-transfer and Rydberg character, together with the excited ? potential energy curve in H2. The SCAN results frequently resemble those obtained using a global hybrid functional, with either a standard or increased fraction of exact orbital exchange. For local excitations, SCAN can exhibit significant triplet instability problems, resulting in imaginary triplet excitation energies for a number of cases. The Tamm-Dancoff approximation offers a simple approach to improve the situation, but the excitation energies are still significantly underestimated. Understanding the origin of these (near)-triplet instabilities may provide useful insight into future functional development.

Evaluating excited state atomic polarizabilities of chromophores.

PubMed

Heid, Esther; Hunt, Patricia A; Schröder, Christian

2018-03-28

Ground and excited state dipoles and polarizabilities of the chromophores N-methyl-6-oxyquinolinium betaine (MQ) and coumarin 153 (C153) in solution have been evaluated using time-dependent density functional theory (TD-DFT). A method for determining the atomic polarizabilities has been developed; the molecular dipole has been decomposed into atomic charge transfer and polarizability terms, and variation in the presence of an electric field has been used to evaluate atomic polarizabilities. On excitation, MQ undergoes very site-specific changes in polarizability while C153 shows significantly less variation. We also conclude that MQ cannot be adequately described by standard atomic polarizabilities based on atomic number and hybridization state. Changes in the molecular polarizability of MQ (on excitation) are not representative of the local site-specific changes in atomic polarizability, thus the overall molecular polarizability ratio does not provide a good approximation for local atom-specific polarizability changes on excitation. Accurate excited state force fields are needed for computer simulation of solvation dynamics. The chromophores considered in this study are often used as molecular probes. The methods and data reported here can be used for the construction of polarizable ground and excited state force fields. Atomic and molecular polarizabilities (ground and excited states) have been evaluated over a range of functionals and basis sets. Different mechanisms for including solvation effects have been examined; using a polarizable continuum model, explicit solvation and via sampling of clusters extracted from a MD simulation. A range of different solvents have also been considered.

Analysis of axial compressive loaded beam under random support excitations

NASA Astrophysics Data System (ADS)

Xiao, Wensheng; Wang, Fengde; Liu, Jian

2017-12-01

An analytical procedure to investigate the response spectrum of a uniform Bernoulli-Euler beam with axial compressive load subjected to random support excitations is implemented based on the Mindlin-Goodman method and the mode superposition method in the frequency domain. The random response spectrum of the simply supported beam subjected to white noise excitation and to Pierson-Moskowitz spectrum excitation is investigated, and the characteristics of the response spectrum are further explored. Moreover, the effect of axial compressive load is studied and a method to determine the axial load is proposed. The research results show that the response spectrum mainly consists of the beam's additional displacement response spectrum when the excitation is white noise; however, the quasi-static displacement response spectrum is the main component when the excitation is the Pierson-Moskowitz spectrum. Under white noise excitation, the amplitude of the power spectral density function decreased as the axial compressive load increased, while the frequency band of the vibration response spectrum increased with the increase of axial compressive load.

Wavelet based comparison of high frequency oscillations in the geodetic and fluid excitation functions of polar motion

NASA Astrophysics Data System (ADS)

Kosek, W.; Popinski, W.; Niedzielski, T.

2011-10-01

It has been already shown that short period oscillations in polar motion, with periods less than 100 days, are very chaotic and are responsible for increase in short-term prediction errors of pole coordinates data. The wavelet technique enables to compare the geodetic and fluid excitation functions in the high frequency band in many different ways, e.g. by looking at the semblance function. The waveletbased semblance filtering enables determination the common signal in both geodetic and fluid excitation time series. In this paper the considered fluid excitation functions consist of the atmospheric, oceanic and land hydrology excitation functions from ECMWF atmospheric data produced by IERS Associated Product Centre Deutsches GeoForschungsZentrum, Potsdam. The geodetic excitation functions have been computed from the combined IERS pole coordinates data.

Comparison of regional hydrological excitation of polar motion derived from hydrological models and the GRACE gravity field data

NASA Astrophysics Data System (ADS)

Nastula, J.; Kolaczek, B.; Salstein, D. A.

2009-09-01

Global geophysical excitation functions of polar motion do not explain fully the observed polar motion as determined by geodetic techniques. The impact of continental hydrologic signals, from land water, snow, and ice, on polar motion excitation HAM (Hydrological Angular Momentum), is still inadequately estimated and not known so well as atmospheric and oceanic ones. Recently the GRACE (Gravity Recovery and Climate Experiment) satellite mission monitoring Earth's time variable gravity field has allowed us to determine global mass term of the polar motion excitation functions, which inherently includes the atmospheric, oceanic and hydrological portions. We use these terms to make comparisons with the mass term of the geodetic and geophysical excitation functions of polar motion on seasonal scales. Global GRACE excitation function of polar motion and hydrological excitation function of polar motion have been determined and were studied earlier

Wave Function and Emergent SU(2) Symmetry in the ν_{T}=1 Quantum Hall Bilayer.

PubMed

Lian, Biao; Zhang, Shou-Cheng

2018-02-16

We propose a trial wave function for the quantum Hall bilayer system of total filling factor ν_{T}=1 at a layer distance d to magnetic length ℓ ratio d/ℓ=κ_{c1}≈1.1, where the lowest charged excitation is known to have a level crossing. The wave function has two-particle correlations, which fit well with those in previous numerical studies, and can be viewed as a Bose-Einstein condensate of free excitons formed by composite bosons and anticomposite bosons in different layers. We show the free nature of these excitons indicating an emergent SU(2) symmetry for the composite bosons at d/ℓ=κ_{c1}, which leads to the level crossing in low-lying charged excitations. We further show the overlap between the trial wave function, and the ground state of a small size exact diagonalization is peaked near d/ℓ=κ_{c1}, which supports our theory.

CC2 oscillator strengths within the local framework for calculating excitation energies (LoFEx).

PubMed

Baudin, Pablo; Kjærgaard, Thomas; Kristensen, Kasper

2017-04-14

In a recent work [P. Baudin and K. Kristensen, J. Chem. Phys. 144, 224106 (2016)], we introduced a local framework for calculating excitation energies (LoFEx), based on second-order approximated coupled cluster (CC2) linear-response theory. LoFEx is a black-box method in which a reduced excitation orbital space (XOS) is optimized to provide coupled cluster (CC) excitation energies at a reduced computational cost. In this article, we present an extension of the LoFEx algorithm to the calculation of CC2 oscillator strengths. Two different strategies are suggested, in which the size of the XOS is determined based on the excitation energy or the oscillator strength of the targeted transitions. The two strategies are applied to a set of medium-sized organic molecules in order to assess both the accuracy and the computational cost of the methods. The results show that CC2 excitation energies and oscillator strengths can be calculated at a reduced computational cost, provided that the targeted transitions are local compared to the size of the molecule. To illustrate the potential of LoFEx for large molecules, both strategies have been successfully applied to the lowest transition of the bivalirudin molecule (4255 basis functions) and compared with time-dependent density functional theory.

Excitation-Power Dependence of the Near Band-Edge PL Spectra of CdMnTe with High Mn Concentrations

NASA Astrophysics Data System (ADS)

Hwang, Younghun; Um, Youngho; Park, Hyoyeol

2011-12-01

Temperature and excitation power dependences of photoluminescence (PL) measurements were studied for the CdMnTe crystal grown by the vertical Bridgman method. The near band-edge and intra-Mn2+ emissions were investigated as a function of temperature. The observed band-edge peak of the PL spectrum showed a clear blue-shift with decreasing temperature. However, the peak energy of the intra-Mn2+ transition did not decrease monotonically with changing temperature, as can be seen above 70 K. With increasing the excitation power, the intensity of the emission peak was increased.

Dissociative excitation of vacuum ultraviolet emission features by electron impact on molecular gases. 3: CO2

NASA Technical Reports Server (NTRS)

Mumma, M. J.; Borst, W. L.; Zipf, E. C.

1972-01-01

Vacuum ultraviolet multiplets of C I, C II, and O I were produced by electron impact of CO2. Absolute emission cross sections for these multiplets were measured from threshold to 350 eV. The electrostatically focussed electron gun used in this series of experiments is described in detail. The atomic multiplets which were produced by dissociative excitation of CO2 and the cross sections at 100 eV are given. The dependence of the excitation functions on electron energy shows that these multiplets are produced by electric-dipole-allowed transitions in CO2.

Self-pulsations and excitability in optically injected quantum-dot lasers: Impact of the excited states and spontaneous emission noise

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

Olejniczak, Lukasz; SUPELEC, OPTEL, and LMOPS EA 4423; Panajotov, Krassimir

2010-08-15

We study the dynamics of an optically injected quantum-dot laser accounting for excited states. Mapping of the bifurcations in the plane frequency detuning vs. injection strength shows that the relaxation rate scales the regions of locking and single- and double-period solutions, while the capture rate has a minor effect. Within the regions of time-periodic solutions, close to the saddle-node bifurcation boundary, we identify subregions where the output signal resembles excitable pulses as a result of the bottleneck phenomenon. We show that such emission is determined mainly by fluctuations in the occupation of the excited states. The interpulse time follows anmore » inverse square root scaling law as a function of the detuning. In a deterministic system the pulses are periodic regardless of the detuning, but in the presence of noise, close to the locking region, the interpulse time follows a positively skewed normal distribution. For a fixed frequency detuning, increasing the noise strength can shift the mean of the interpulse time distribution and make the pulsations more periodic.« less

Neutral and charged excitations in carbon fullerenes from first-principles many-body theories

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

Tiago, Murilo L; Kent, Paul R; Hood, Randolph Q.

2008-01-01

We use first-principles many-body theories to investigate the low energy excitations of the carbon fullerenes C_20, C_24, C_50, C_60, C_70, and C_80. Properties are calculated via the GW-Bethe-Salpeter Equation (GW-BSE) and diffusion Quantum Monte Carlo (QMC) methods. At a lower level of theoretical complexity, we also calculate these properties using static and time-dependent density-functional theory. We critically compare these theories and assess their accuracy against available experimental data. The first ionization potentials are consistently well reproduced and are similar for all the fullerenes and methods studied. The electron affinities and first triplet excitation energies show substantial method and geometry dependence.more » Compared to available experiment, GW-BSE underestimates excitation energies by approximately 0.3 eV while QMC overestimates them by approximately 0.5 eV. We show the GW-BSE errors result primarily from a systematic overestimation of the electron affinities, while the QMC errors likely result from nodal error in both ground and excited state calculations.« less

Development and Applications of Orthogonality Constrained Density Functional Theory for the Accurate Simulation of X-Ray Absorption Spectroscopy

NASA Astrophysics Data System (ADS)

Derricotte, Wallace D.

The aim of this dissertation is to address the theoretical challenges of calculating core-excited states within the framework of orthogonality constrained density functional theory (OCDFT). OCDFT is a well-established variational, time independent formulation of DFT for the computation of electronic excited states. In this work, the theory is first extended to compute core-excited states and generalized to calculate multiple excited state solutions. An initial benchmark is performed on a set of 40 unique core-excitations, highlighting that OCDFT excitation energies have a mean absolute error of 1.0 eV. Next, a novel implementation of the spin-free exact-two-component (X2C) one-electron treatment of scalar relativistic effects is presented and combined with OCDFT in an effort to calculate core excited states of transition metal complexes. The X2C-OCDFT spectra of three organotitanium complexes (TiCl4, TiCpCl3, and TiCp2Cl2) are shown to be in good agreement with experimental results and show a maximum absolute error of 5-6 eV. Next the issue of assigning core excited states is addressed by introducing an automated approach to analyzing the excited state MO by quantifying its local contributions using a unique orbital basis known as localized intrinsic valence virtual orbitals (LIVVOs). The utility of this approach is highlighted by studying sulfur core-excitations in ethanethiol and benzenethiol, as well as the hydrogen bonding in the water dimer. Finally, an approach to selectively target specic core-excited states in OCDFT based on atomic orbital subspace projection is presented in an effort to target core excited states of chemisorbed organic molecules. The core excitation spectrum of pyrazine chemisorbed on Si(100) is calculated using OCDFT and further characterized using the LIVVO approach.

Heteroclinic tangle phenomena in nanomagnets subject to time-harmonic excitations

NASA Astrophysics Data System (ADS)

Serpico, C.; Quercia, A.; Bertotti, G.; d'Aquino, M.; Mayergoyz, I.; Perna, S.; Ansalone, P.

2015-05-01

Magnetization dynamics in uniformly magnetized nanomagnets excited by time-harmonic (AC) external fields or spin-polarized injected currents is considered. The analysis is focused on the behaviour of the AC-excited dynamics near saddle equilibria. It turns out that this dynamics has a chaotic character at moderately low power level. This chaotic and fractal nature is due to the phenomenon of heteroclinic tangle which is produced by the combined effect of AC-excitations and saddle type dynamics. By using the perturbation technique based on Melnikov function, analytical formulas for the threshold AC excitation amplitudes necessary to create the heteroclinic tangle are derived. Both the cases of AC applied fields and AC spin-polarized injected currents are treated. Then, by means of numerical simulations, we show how heteroclinic tangle is accompanied by the erosion of the safe basin around the stable regimes.

Cortical excitability and neurology: insights into the pathophysiology

PubMed Central

Badawy, Radwa A.B.; Loetscher, Tobias; Macdonell, Richard A.L.; Brodtmann, Amy

2012-01-01

Summary Transcranial magnetic stimulation (TMS) is a technique developed to non-invasively investigate the integrity of human motor corticospinal tracts. Over the last three decades, the use of stimulation paradigms including single-pulse TMS, paired-pulse TMS, repetitive TMS, and integration with EEG and functional imaging have been developed to facilitate measurement of cortical excitability. Through the use of these protocols, TMS has evolved into an excellent tool for measuring cortical excitability. TMS has high sensitivity in detecting subtle changes in cortical excitability, and therefore it is also a good measure of disturbances associated with brain disorders. In this review, we appraise the current literature on cortical excitability studies using TMS in neurological disorders. We begin with a brief overview of current TMS measures and then show how these have added to our understanding of the underlying mechanisms of brain disorders. PMID:23402674

Full-field modal analysis during base motion excitation using high-speed 3D digital image correlation

NASA Astrophysics Data System (ADS)

Molina-Viedma, Ángel J.; López-Alba, Elías; Felipe-Sesé, Luis; Díaz, Francisco A.

2017-10-01

In recent years, many efforts have been made to exploit full-field measurement optical techniques for modal identification. Three-dimensional digital image correlation using high-speed cameras has been extensively employed for this purpose. Modal identification algorithms are applied to process the frequency response functions (FRF), which relate the displacement response of the structure to the excitation force. However, one of the most common tests for modal analysis involves the base motion excitation of a structural element instead of force excitation. In this case, the relationship between response and excitation is typically based on displacements, which are known as transmissibility functions. In this study, a methodology for experimental modal analysis using high-speed 3D digital image correlation and base motion excitation tests is proposed. In particular, a cantilever beam was excited from its base with a random signal, using a clamped edge join. Full-field transmissibility functions were obtained through the beam and converted into FRF for proper identification, considering a single degree-of-freedom theoretical conversion. Subsequently, modal identification was performed using a circle-fit approach. The proposed methodology facilitates the management of the typically large amounts of data points involved in the DIC measurement during modal identification. Moreover, it was possible to determine the natural frequencies, damping ratios and full-field mode shapes without requiring any additional tests. Finally, the results were experimentally validated by comparing them with those obtained by employing traditional accelerometers, analytical models and finite element method analyses. The comparison was performed by using the quantitative indicator modal assurance criterion. The results showed a high level of correspondence, consolidating the proposed experimental methodology.

Analytical and experimental comparisons of electromechanical vibration response of a piezoelectric bimorph beam for power harvesting

NASA Astrophysics Data System (ADS)

Lumentut, M. F.; Howard, I. M.

2013-03-01

Power harvesters that extract energy from vibrating systems via piezoelectric transduction show strong potential for powering smart wireless sensor devices in applications of health condition monitoring of rotating machinery and structures. This paper presents an analytical method for modelling an electromechanical piezoelectric bimorph beam with tip mass under two input base transverse and longitudinal excitations. The Euler-Bernoulli beam equations were used to model the piezoelectric bimorph beam. The polarity-electric field of the piezoelectric element is excited by the strain field caused by base input excitation, resulting in electrical charge. The governing electromechanical dynamic equations were derived analytically using the weak form of the Hamiltonian principle to obtain the constitutive equations. Three constitutive electromechanical dynamic equations based on independent coefficients of virtual displacement vectors were formulated and then further modelled using the normalised Ritz eigenfunction series. The electromechanical formulations include both the series and parallel connections of the piezoelectric bimorph. The multi-mode frequency response functions (FRFs) under varying electrical load resistance were formulated using Laplace transformation for the multi-input mechanical vibrations to provide the multi-output dynamic displacement, velocity, voltage, current and power. The experimental and theoretical validations reduced for the single mode system were shown to provide reasonable predictions. The model results from polar base excitation for off-axis input motions were validated with experimental results showing the change to the electrical power frequency response amplitude as a function of excitation angle, with relevance for practical implementation.

Optical properties of azobenzene-functionalized self-assembled monolayers: Intermolecular coupling and many-body interactions

NASA Astrophysics Data System (ADS)

Cocchi, Caterina; Moldt, Thomas; Gahl, Cornelius; Weinelt, Martin; Draxl, Claudia

2016-12-01

In a joint theoretical and experimental work, the optical properties of azobenzene-functionalized self-assembled monolayers (SAMs) are studied at different molecular packing densities. Our results, based on density-functional and many-body perturbation theory, as well as on differential reflectance (DR) spectroscopy, shed light on the microscopic mechanisms ruling photo-absorption in these systems. While the optical excitations are intrinsically excitonic in nature, regardless of the molecular concentration, in densely packed SAMs intermolecular coupling and local-field effects are responsible for a sizable weakening of the exciton binding strength. Through a detailed analysis of the character of the electron-hole pairs, we show that distinct excitations involved in the photo-isomerization at low molecular concentrations are dramatically broadened by intermolecular interactions. Spectral shifts in the calculated DR spectra are in good agreement with the experimental results. Our findings represent an important step forward to rationalize the excited-state properties of these complex materials.

Identifying and tracing potential energy surfaces of electronic excitations with specific character via their transition origins: application to oxirane.

PubMed

Li, Jian-Hao; Zuehlsdorff, T J; Payne, M C; Hine, N D M

2015-05-14

We show that the transition origins of electronic excitations identified by quantified natural transition orbital (QNTO) analysis can be employed to connect potential energy surfaces (PESs) according to their character across a wide range of molecular geometries. This is achieved by locating the switching of transition origins of adiabatic potential surfaces as the geometry changes. The transition vectors for analysing transition origins are provided by linear response time-dependent density functional theory (TDDFT) calculations under the Tamm-Dancoff approximation. We study the photochemical CO ring opening of oxirane as an example and show that the results corroborate the traditional Gomer-Noyes mechanism derived experimentally. The knowledge of specific states for the reaction also agrees well with that given by previous theoretical work using TDDFT surface-hopping dynamics that was validated by high-quality quantum Monte Carlo calculations. We also show that QNTO can be useful for considerably larger and more complex systems: by projecting the excitations to those of a reference oxirane molecule, the approach is able to identify and analyse specific excitations of a trans-2,3-diphenyloxirane molecule.

The use of gravimetric data from GRACE mission in the understanding of polar motion variations

NASA Astrophysics Data System (ADS)

Seoane, L.; Nastula, J.; Bizouard, C.; Gambis, D.

2009-08-01

Tesseral coefficients C21 and S21 derived from Gravity Recovery and Climate Experiment (GRACE) observations allow to compute the mass term of the polar-motion excitation function. This independent estimation can improve the geophysical models and, in addition, determine the unmodelled phenomena. In this paper, we intend to validate the polar motion excitation derived from GRACE's last release (GRACE Release 4) computed by different institutes: GeoForschungsZentrum (GFZ), Postdam, Germany; Center for Space Research (CSR), Austin, USA; Jet Propulsion Laboratory (JPL), Pasadena, USA, and the Groupe de Recherche en Géodésie Spatiale (GRGS), Toulouse, France. For this purpose, we compare these excitations functions first to the mass term obtained from observed Earth's rotation variations free of the motion term and, second, to the mass term estimated from geophysical fluids models. We confirm the large improvement of the CSR solution, and we show that the GRGS estimate is also well correlated with the geodetic observations. Significant discrepancies exist between the solutions of each centre. The source of these differences is probably related to the data processing strategy. We also consider residuals computed after removing the geophysical models or the gravimetric solutions from the geodetic mass term. We show that the residual excitation based on models is smoother than the gravimetric data, which are still noisy. Still, they are comparable for the χ2 component. It appears that χ2 residual signals using GFZ and JPL data have less variability. Finally, for assessing the impact of the geophysical fluids models choice on our results, we checked two different oceanic excitation series. We show the significant differences in the residuals correlations, especially for the χ1 more sensitive to the oceanic signals.

Functional Cooperation between the IP3 Receptor and Phospholipase C Secures the High Sensitivity to Light of Drosophila Photoreceptors In Vivo

PubMed Central

Kohn, Elkana; Katz, Ben; Yasin, Bushra; Peters, Maximilian; Rhodes, Elisheva; Zaguri, Rachel; Weiss, Shirley

2015-01-01

Drosophila phototransduction is a model system for the ubiquitous phosphoinositide signaling. In complete darkness, spontaneous unitary current events (dark bumps) are produced by spontaneous single Gqα activation, while single-photon responses (quantum bumps) arise from synchronous activation of several Gqα molecules. We have recently shown that most of the spontaneous single Gqα activations do not produce dark bumps, because of a critical phospholipase Cβ (PLCβ) activity level required for bump generation. Surpassing the threshold of channel activation depends on both PLCβ activity and cellular [Ca2+], which participates in light excitation via a still unclear mechanism. We show here that in IP3 receptor (IP3R)-deficient photoreceptors, both light-activated Ca2+ release from internal stores and light sensitivity were strongly attenuated. This was further verified by Ca2+ store depletion, linking Ca2+ release to light excitation. In IP3R-deficient photoreceptors, dark bumps were virtually absent and the quantum-bump rate was reduced, indicating that Ca2+ release from internal stores is necessary to reach the critical level of PLCβ catalytic activity and the cellular [Ca2+] required for excitation. Combination of IP3R knockdown with reduced PLCβ catalytic activity resulted in highly suppressed light responses that were partially rescued by cellular Ca2+ elevation, showing a functional cooperation between IP3R and PLCβ via released Ca2+. These findings suggest that in contrast to the current dogma that Ca2+ release via IP3R does not participate in light excitation, we show that released Ca2+ plays a critical role in light excitation. The positive feedback between PLCβ and IP3R found here may represent a common feature of the inositol-lipid signaling. PMID:25673847

K-shell excitation studied for H- and He-like bismuth ions in collisions with low-Z target atoms

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

Stoehlker, T.; Ionescu, D.C.; Rymuza, P.

1998-02-01

The formation of excited projectile states via Coulomb excitation is investigated for hydrogenlike and heliumlike bismuth projectiles (Z=83) in relativistic ion-atom collisions. The excitation process was unambiguously identified by observing the radiative decay of the excited levels to the vacant 1s shell in coincidence with ions that did not undergo charge exchange in the reaction target. In particular, owing to the large fine-structure splitting of Bi, the excitation cross sections to the various L-shell sublevels are determined separately. The results are compared with detailed relativistic calculations, showing that both the relativistic character of the bound-state wave functions and the magneticmore » interaction are of considerable importance for the K-shell excitation process in high-Z ions such as Bi. The experimental data confirm the result of the complete relativistic calculations, namely, that the magnetic part of the Li{acute e}nard-Wiechert interaction leads to a significant reduction of the K-shell excitation cross section. {copyright} {ital 1998} {ital The American Physical Society}« less

A long-range-corrected density functional that performs well for both ground-state properties and time-dependent density functional theory excitation energies, including charge-transfer excited states.

PubMed

Rohrdanz, Mary A; Martins, Katie M; Herbert, John M

2009-02-07

We introduce a hybrid density functional that asymptotically incorporates full Hartree-Fock exchange, based on the long-range-corrected exchange-hole model of Henderson et al. [J. Chem. Phys. 128, 194105 (2008)]. The performance of this functional, for ground-state properties and for vertical excitation energies within time-dependent density functional theory, is systematically evaluated, and optimal values are determined for the range-separation parameter, omega, and for the fraction of short-range Hartree-Fock exchange. We denote the new functional as LRC-omegaPBEh, since it reduces to the standard PBEh hybrid functional (also known as PBE0 or PBE1PBE) for a certain choice of its two parameters. Upon optimization of these parameters against a set of ground- and excited-state benchmarks, the LRC-omegaPBEh functional fulfills three important requirements: (i) It outperforms the PBEh hybrid functional for ground-state atomization energies and reaction barrier heights; (ii) it yields statistical errors comparable to PBEh for valence excitation energies in both small and medium-sized molecules; and (iii) its performance for charge-transfer excitations is comparable to its performance for valence excitations. LRC-omegaPBEh, with the parameters determined herein, is the first density functional that satisfies all three criteria. Notably, short-range Hartree-Fock exchange appears to be necessary in order to obtain accurate ground-state properties and vertical excitation energies using the same value of omega.

Luminescent rare earth vanadate nanoparticles doped with Eu3+ and Bi3 for sensing and imaging applications

NASA Astrophysics Data System (ADS)

Escudero, Alberto; Carrillo-Carrión, Carolina; Zyuzin, Mikhail; Hartmann, Raimo; Ashraf, Sumaira; Parak, Wolfgang J.

2016-03-01

Nanoparticles (NPs) are attracting interest in nanomedicine due to their potential medical applications, ranging from optical biolabels and contrast agents for magnetic resonance imaging to carriers for drug and gene delivery for disease therapy.[1] Rare earth (RE) based nanophosphors exhibit important advantages compared with other available luminescent materials, such as quantum dots and nanostructures functionalized with organic dyes, due to their lower toxicities, photostabilities, high thermal and chemical stabilities, high luminescence quantum yields, and sharp emission bands.[2] Yttrium orthovanadate NPs doped with Eu3+ and Bi3+, functionalized with poly acryl acid (PAA), and excitable by near-ultraviolet light have been synthesized by homogeneous precipitation at 120 °C from solutions of rare earth precursors (yttrium acetylacetonate and europium nitrate), bismuth nitrate, sodium orthovanadate, and PAA, in an ethylene glycol/water mixture. Quasispheres with sizes from 93 to 51 nm were obtained. The as synthesized NPs were already functionalized with PAA. The NPs showed the typical red luminescence of Eu3+, which can be excited with near-UV light through an energy transfer from the vanadate anion. The presence of Bi3+ shifts the maximum of the broad excitation band from 280 nm to 342 nm. This excitation path is much more efficient than the direct excitation of the Eu3+ electronic levels, and results in a much higher luminescence. The NPs can be uptaken by HeLa cells, and are eventually located in the lysosomes after being internalized. Finally, the functionalization with PAA provides -COOH anchors for adding functional ligands of biomedical interest that can be used for sensing applications.

Metabotropic glutamate receptor-mediated use-dependent down-regulation of synaptic excitability involves the fragile X mental retardation protein.

PubMed

Repicky, Sarah; Broadie, Kendal

2009-02-01

Loss of the mRNA-binding protein FMRP results in the most common inherited form of both mental retardation and autism spectrum disorders: fragile X syndrome (FXS). The leading FXS hypothesis proposes that metabotropic glutamate receptor (mGluR) signaling at the synapse controls FMRP function in the regulation of local protein translation to modulate synaptic transmission strength. In this study, we use the Drosophila FXS disease model to test the relationship between Drosophila FMRP (dFMRP) and the sole Drosophila mGluR (dmGluRA) in regulation of synaptic function, using two-electrode voltage-clamp recording at the glutamatergic neuromuscular junction (NMJ). Null dmGluRA mutants show minimal changes in basal synapse properties but pronounced defects during sustained high-frequency stimulation (HFS). The double null dfmr1;dmGluRA mutant shows repression of enhanced augmentation and delayed onset of premature long-term facilitation (LTF) and strongly reduces grossly elevated post-tetanic potentiation (PTP) phenotypes present in dmGluRA-null animals. Null dfmr1 mutants show features of synaptic hyperexcitability, including multiple transmission events in response to a single stimulus and cyclic modulation of transmission amplitude during prolonged HFS. The double null dfmr1;dmGluRA mutant shows amelioration of these defects but does not fully restore wildtype properties in dfmr1-null animals. These data suggest that dmGluRA functions in a negative feedback loop in which excess glutamate released during high-frequency transmission binds the glutamate receptor to dampen synaptic excitability, and dFMRP functions to suppress the translation of proteins regulating this synaptic excitability. Removal of the translational regulator partially compensates for loss of the receptor and, similarly, loss of the receptor weakly compensates for loss of the translational regulator.

Convergent close coupling versus the generalized Sturmian function approach: Wave-function analysis

NASA Astrophysics Data System (ADS)

Ambrosio, M.; Mitnik, D. M.; Gasaneo, G.; Randazzo, J. M.; Kadyrov, A. S.; Fursa, D. V.; Bray, I.

2015-11-01

We compare the physical information contained in the Temkin-Poet (TP) scattering wave function representing electron-impact ionization of hydrogen, calculated by the convergent close-coupling (CCC) and generalized Sturmian function (GSF) methodologies. The idea is to show that the ionization cross section can be extracted from the wave functions themselves. Using two different procedures based on hyperspherical Sturmian functions we show that the transition amplitudes contained in both GSF and CCC scattering functions lead to similar single-differential cross sections. The single-continuum channels were also a subject of the present studies, and we show that the elastic and excitation amplitudes are essentially the same as well.

Benchmarking the Performance of Exchange-Correlation Functionals for Predicting Two-Photon Absorption Strengths.

PubMed

Beerepoot, Maarten T P; Alam, Md Mehboob; Bednarska, Joanna; Bartkowiak, Wojciech; Ruud, Kenneth; Zaleśny, Robert

2018-06-15

The present work investigates the performance of exchange-correlation functionals in the prediction of two-photon absorption (2PA) strengths. For this purpose, we considered six common functionals used for studying 2PA processes and tested these on six organoboron chelates. The set consisted of two semilocal (PBE and BLYP), two hybrid (B3LYP and PBE0), and two range-separated (LC-BLYP and CAM-B3LYP) functionals. The RI-CC2 method was chosen as a reference level and was found to give results consistent with the experimental data that are available for three of the molecules considered. Of the six exchange-correlation functionals studied, only the range-separated functionals predict an ordering of the 2PA strengths that is consistent with experimental and RI-CC2 results. Even though the range-separated functionals predict correct relative trends, the absolute values for the 2PA strengths are underestimated by a factor of 2-6 for the molecules considered. An in-depth analysis, on the basis of the derived generalized few-state model expression for the 2PA strength for a coupled-cluster wave function, reveals that the problem with these functionals can be linked to underestimated excited-state dipole moments and, to a lesser extent, overestimated excitation energies. The semilocal and hybrid functionals exhibit less predictable errors and a variation in the 2PA strengths in disagreement with the reference results. The semilocal and hybrid functionals show smaller average errors than the range-separated functionals, but our analysis reveals that this is due to fortuitous error cancellation between excitation energies and the transition dipole moments. Our results constitute a warning against using currently available exchange-correlation functionals in the prediction of 2PA strengths and highlight the need for functionals that correctly describe the electron density of excited electronic states.

Coherent wavepackets in the Fenna-Matthews-Olson complex are robust to excitonic-structure perturbations caused by mutagenesis

NASA Astrophysics Data System (ADS)

Maiuri, Margherita; Ostroumov, Evgeny E.; Saer, Rafael G.; Blankenship, Robert E.; Scholes, Gregory D.

2018-02-01

Femtosecond pulsed excitation of light-harvesting complexes creates oscillatory features in their response. This phenomenon has inspired a large body of work aimed at uncovering the origin of the coherent beatings and possible implications for function. Here we exploit site-directed mutagenesis to change the excitonic level structure in Fenna-Matthews-Olson (FMO) complexes and compare the coherences using broadband pump-probe spectroscopy. Our experiments detect two oscillation frequencies with dephasing on a picosecond timescale—both at 77 K and at room temperature. By studying these coherences with selective excitation pump-probe experiments, where pump excitation is in resonance only with the lowest excitonic state, we show that the key contributions to these oscillations stem from ground-state vibrational wavepackets. These experiments explicitly show that the coherences—although in the ground electronic state—can be probed at the absorption resonances of other bacteriochlorophyll molecules because of delocalization of the electronic excitation over several chromophores.

Windows in direct dissociative recombination cross sections

NASA Technical Reports Server (NTRS)

Guberman, Steven L.

1986-01-01

Model potential curves are used to show that large windows are present in direct dissociative-recombination cross sections from excited molecular-ion vibrational levels. The windows are due to the overlap of vibrational wave functions of the repulsive neutral states with the nodes of the ion vibrational wave function.

Improving Rydberg Excitations within Time-Dependent Density Functional Theory with Generalized Gradient Approximations: The Exchange-Enhancement-for-Large-Gradient Scheme.

PubMed

Li, Shaohong L; Truhlar, Donald G

2015-07-14

Time-dependent density functional theory (TDDFT) with conventional local and hybrid functionals such as the local and hybrid generalized gradient approximations (GGA) seriously underestimates the excitation energies of Rydberg states, which limits its usefulness for applications such as spectroscopy and photochemistry. We present here a scheme that modifies the exchange-enhancement factor to improve GGA functionals for Rydberg excitations within the TDDFT framework while retaining their accuracy for valence excitations and for the thermochemical energetics calculated by ground-state density functional theory. The scheme is applied to a popular hybrid GGA functional and tested on data sets of valence and Rydberg excitations and atomization energies, and the results are encouraging. The scheme is simple and flexible. It can be used to correct existing functionals, and it can also be used as a strategy for the development of new functionals.

Improving Rydberg Excitations within Time-Dependent Density Functional Theory with Generalized Gradient Approximations: The Exchange-Enhancement-for-Large-Gradient Scheme

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

Li, Shaohong L.; Truhlar, Donald G.

Time-dependent density functional theory (TDDFT) with conventional local and hybrid functionals such as the local and hybrid generalized gradient approximations (GGA) seriously underestimates the excitation energies of Rydberg states, which limits its usefulness for applications such as spectroscopy and photochemistry. We present here a scheme that modifies the exchange-enhancement factor to improve GGA functionals for Rydberg excitations within the TDDFT framework while retaining their accuracy for valence excitations and for the thermochemical energetics calculated by ground-state density functional theory. The scheme is applied to a popular hybrid GGA functional and tested on data sets of valence and Rydberg excitations andmore » atomization energies, and the results are encouraging. The scheme is simple and flexible. It can be used to correct existing functionals, and it can also be used as a strategy for the development of new functionals.« less

Improving Rydberg Excitations within Time-Dependent Density Functional Theory with Generalized Gradient Approximations: The Exchange-Enhancement-for-Large-Gradient Scheme

DOE PAGES

Li, Shaohong L.; Truhlar, Donald G.

2015-05-22

Time-dependent density functional theory (TDDFT) with conventional local and hybrid functionals such as the local and hybrid generalized gradient approximations (GGA) seriously underestimates the excitation energies of Rydberg states, which limits its usefulness for applications such as spectroscopy and photochemistry. We present here a scheme that modifies the exchange-enhancement factor to improve GGA functionals for Rydberg excitations within the TDDFT framework while retaining their accuracy for valence excitations and for the thermochemical energetics calculated by ground-state density functional theory. The scheme is applied to a popular hybrid GGA functional and tested on data sets of valence and Rydberg excitations andmore » atomization energies, and the results are encouraging. The scheme is simple and flexible. It can be used to correct existing functionals, and it can also be used as a strategy for the development of new functionals.« less

Exciton-polariton dynamics in a GaAs bulk microcavity

NASA Astrophysics Data System (ADS)

Ceccherini, S.; Gurioli, M.; Bogani, F.; Colocci, M.; Tredicucci, A.; Bassani, F.; Beltram, F.; Sorba, L.

1998-01-01

We present a full analysis of exciton dynamics in a GaAs λ/2 bulk microcavity following excitation by ultrafast laser pulses. Coherent dynamics was probed by means of an interferometric technique; beating and dephasing times were studied for various excitation intensities. At high incident power, population effects begin to show up reducing exciton oscillator strength and suppressing Rabi splitting. This feature produces marked non-linearities in the input-output characteristic of the optical functions, which were studied in view of reaching bistable operation. Theoretical calculations performed within the transfer-matrix framework show good agreement with experimental results.

Assessment of Ab Initio and Density Functional Theory Methods for the Excitations of Donor-Acceptor Complexes: The Case of the Benzene-Tetracyanoethylene Model.

PubMed

Xu, Peng; Zhang, Cai-Rong; Wang, Wei; Gong, Ji-Jun; Liu, Zi-Jiang; Chen, Hong-Shan

2018-04-10

The understanding of the excited-state properties of electron donors, acceptors and their interfaces in organic optoelectronic devices is a fundamental issue for their performance optimization. In order to obtain a balanced description of the different excitation types for electron-donor-acceptor systems, including the singlet charge transfer (CT), local excitations, and triplet excited states, several ab initio and density functional theory (DFT) methods for excited-state calculations were evaluated based upon the selected model system of benzene-tetracyanoethylene (B-TCNE) complexes. On the basis of benchmark calculations of the equation-of-motion coupled-cluster with single and double excitations method, the arithmetic mean of the absolute errors and standard errors of the electronic excitation energies for the different computational methods suggest that the M11 functional in DFT is superior to the other tested DFT functionals, and time-dependent DFT (TDDFT) with the Tamm-Dancoff approximation improves the accuracy of the calculated excitation energies relative to that of the full TDDFT. The performance of the M11 functional underlines the importance of kinetic energy density, spin-density gradient, and range separation in the development of novel DFT functionals. According to the TDDFT results, the performances of the different TDDFT methods on the CT properties of the B-TCNE complexes were also analyzed.

Excited-State Deactivation of Branched Phthalocyanine Compounds.

PubMed

Zhu, Huaning; Li, Yang; Chen, Jun; Zhou, Meng; Niu, Yingli; Zhang, Xinxing; Guo, Qianjin; Wang, Shuangqing; Yang, Guoqiang; Xia, Andong

2015-12-21

The excited-state relaxation dynamics and chromophore interactions in two phthalocyanine compounds (bis- and trisphthalocyanines) are studied by using steady-state and femtosecond transient absorption spectral measurements, where the excited-state energy-transfer mechanism is explored. By exciting phthalocyanine compounds to their second electronically excited states and probing the subsequent relaxation dynamics, a multitude of deactivation pathways are identified. The transient absorption spectra show the relaxation pathway from the exciton state to excimer state and then back to the ground state in bisphthalocyanine (bis-Pc). In trisphthalocyanine (tris-Pc), the monomeric and dimeric subunits are excited and the excitation energy transfers from the monomeric vibrationally hot S1 state to the exciton state of a pre-associated dimer, with subsequent relaxation to the ground state through the excimer state. The theoretical calculations and steady-state spectra also show a face-to-face conformation in bis-Pc, whereas in tris-Pc, two of the three phthalocyanine branches form a pre-associated face-to-face dimeric conformation with the third one acting as a monomeric unit; this is consistent with the results of the transient absorption experiments from the perspective of molecular structure. The detailed structure-property relationships in phthalocyanine compounds is useful for exploring the function of molecular aggregates in energy migration of natural photosynthesis systems. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Producing coherent excitations in pumped Mott antiferromagnetic insulators

NASA Astrophysics Data System (ADS)

Wang, Yao; Claassen, Martin; Moritz, B.; Devereaux, T. P.

2017-12-01

Nonequilibrium dynamics in correlated materials has attracted attention due to the possibility of characterizing, tuning, and creating complex ordered states. To understand the photoinduced microscopic dynamics, especially the linkage under realistic pump conditions between transient states and remnant elementary excitations, we performed nonperturbative simulations of various time-resolved spectroscopies. We used the Mott antiferromagnetic insulator as a model platform. The transient dynamics of multiparticle excitations can be attributed to the interplay between Floquet virtual states and a modification of the density of states, in which interactions induce a spectral weight transfer. Using an autocorrelation of the time-dependent spectral function, we show that resonance of the virtual states with the upper Hubbard band in the Mott insulator provides the route towards manipulating the electronic distribution and modifying charge and spin excitations. Our results link transient dynamics to the nature of many-body excitations and provide an opportunity to design nonequilibrium states of matter via tuned laser pulses.

Asynchronous Cholinergic Drive Correlates with Excitation-Inhibition Imbalance via a Neuronal Ca2+ Sensor Protein.

PubMed

Zhou, Keming; Cherra, Salvatore J; Goncharov, Alexandr; Jin, Yishi

2017-05-09

Excitation-inhibition imbalance in neural networks is widely linked to neurological and neuropsychiatric disorders. However, how genetic factors alter neuronal activity, leading to excitation-inhibition imbalance, remains unclear. Here, using the C. elegans locomotor circuit, we examine how altering neuronal activity for varying time periods affects synaptic release pattern and animal behavior. We show that while short-duration activation of excitatory cholinergic neurons elicits a reversible enhancement of presynaptic strength, persistent activation results to asynchronous and reduced cholinergic drive, inducing imbalance between endogenous excitation and inhibition. We find that the neuronal calcium sensor protein NCS-2 is required for asynchronous cholinergic release in an activity-dependent manner and dampens excitability of inhibitory neurons non-cell autonomously. The function of NCS-2 requires its Ca 2+ binding and membrane association domains. These results reveal a synaptic mechanism implicating asynchronous release in regulation of excitation-inhibition balance. Copyright © 2017 The Author(s). Published by Elsevier Inc. All rights reserved.

Molecular Excitation Energies from Time-Dependent Density Functional Theory Employing Random-Phase Approximation Hessians with Exact Exchange.

PubMed

Heßelmann, Andreas

2015-04-14

Molecular excitation energies have been calculated with time-dependent density-functional theory (TDDFT) using random-phase approximation Hessians augmented with exact exchange contributions in various orders. It has been observed that this approach yields fairly accurate local valence excitations if combined with accurate asymptotically corrected exchange-correlation potentials used in the ground-state Kohn-Sham calculations. The inclusion of long-range particle-particle with hole-hole interactions in the kernel leads to errors of 0.14 eV only for the lowest excitations of a selection of three alkene, three carbonyl, and five azabenzene molecules, thus surpassing the accuracy of a number of common TDDFT and even some wave function correlation methods. In the case of long-range charge-transfer excitations, the method typically underestimates accurate reference excitation energies by 8% on average, which is better than with standard hybrid-GGA functionals but worse compared to range-separated functional approximations.

Analysis of the total kinetic energy of fission fragments with the Langevin equation

NASA Astrophysics Data System (ADS)

Usang, M. D.; Ivanyuk, F. A.; Ishizuka, C.; Chiba, S.

2017-12-01

We analyzed the total kinetic energy (TKE) of fission fragments with three-dimensional Langevin calculations for a series of actinides and Fm isotopes at various excitation energies. This allowed us to establish systematic trends of TKE with Z2/A1 /3 of the fissioning system and as a function of excitation energy. In the mass-energy distributions of fission fragments we see the contributions from the standard, super-long, and super-short (in the case of 258Fm) fission modes. For the fission fragments mass distribution of 258Fm we obtained a single peak mass distribution. The decomposition of TKE into the prescission kinetic energy and Coulomb repulsion showed that decrease of TKE with growing excitation energy is accompanied by a decrease of prescission kinetic energy. It was also found that transport coefficients (friction and inertia tensors) calculated by a microscopic model and by macroscopic models give drastically different behaviors of TKE as a function of excitation energy. The results obtained with microscopic transport coefficients are much closer to experimental data than those calculated with macroscopic ones.

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

Rose, Sunniva J.; Zeiser, Fabio; Wilson, J. N.

Prompt-fission γ rays are responsible for approximately 5% of the total energy released in fission, and therefore important to understand when modeling nuclear reactors. In this work we present prompt γ-ray emission characteristics in fission as a function of the nuclear excitation energy of the fissioning system. Emitted γ-ray spectra were measured, and γ-ray multiplicities and average and total γ energies per fission were determined for the 233U(d,pf) reaction for excitation energies between 4.8 and 10 MeV, and for the 239Pu(d,pf) reaction between 4.5 and 9 MeV. The spectral characteristics show no significant change as a function of excitation energymore » above the fission barrier, despite the fact that an extra ~5 MeV of energy is potentially available in the excited fragments for γ decay. The measured results are compared with model calculations made for prompt γ-ray emission with the fission model code gef. In conclusion, further comparison with previously obtained results from thermal neutron induced fission is made to characterize possible differences arising from using the surrogate (d,p) reaction.« less

Excitation of the Earth's Chandler wobble by southern oscillation/El Nino, 1900-1979

NASA Technical Reports Server (NTRS)

Chao, B. F.

1985-01-01

The southern oscillation/El Nino (ENSO) is the single most prominent interannual signal in global atmospheric/oceanic fluctuations. The following question is addressed: how important is the angular momentum carried by ENSO in exciting the Earth's Chandler wobble? The question is attacked through a statistical analysis of the coherence spectra (correlation as a function of frequency) between two data sets spanning 1900 to 1979-the southern oscillation index (SOI) time series and the excitation function psi (with x-component psi sub x and y-component psi sub y) of the Chandler wobble derived from the homogeneous ILS (International Latitude Service) polar motion data. The coherence power and phase in the Chandler frequency band (approx. 0.79 to 0.89 cpy) are studied. It is found that, during 1900 to 1979 the coherence between SOI and psi sub x is significant well over the 95% confidence threshold whereas that between SOI and psi sub y is practically nil. Quantitatively, the coherence study shows that ENSO provides some 20% of the observed Chandler wobble excitation power. Since earlier investigations have shown that the total atmospheric/oceanic variation can account for the Chandler wobble excitation at about 20% level, the implication is that ENSO maybe an important (interannual) part of the atmospheric/oceanic variation that is responsible for the Chandler wobble excitation during 1900 to 1979.

Dose-dependent effects of theta burst rTMS on cortical excitability and resting-state connectivity of the human motor system.

PubMed

Nettekoven, Charlotte; Volz, Lukas J; Kutscha, Martha; Pool, Eva-Maria; Rehme, Anne K; Eickhoff, Simon B; Fink, Gereon R; Grefkes, Christian

2014-05-14

Theta burst stimulation (TBS), a specific protocol of repetitive transcranial magnetic stimulation (rTMS), induces changes in cortical excitability that last beyond stimulation. TBS-induced aftereffects, however, vary between subjects, and the mechanisms underlying these aftereffects to date remain poorly understood. Therefore, the purpose of this study was to investigate whether increasing the number of pulses of intermittent TBS (iTBS) (1) increases cortical excitability as measured by motor-evoked potentials (MEPs) and (2) alters functional connectivity measured using resting-state fMRI, in a dose-dependent manner. Sixteen healthy, human subjects received three serially applied iTBS blocks of 600 pulses over the primary motor cortex (M1 stimulation) and the parieto-occipital vertex (sham stimulation) to test for dose-dependent iTBS effects on cortical excitability and functional connectivity (four sessions in total). iTBS over M1 increased MEP amplitudes compared with sham stimulation after each stimulation block. Although the increase in MEP amplitudes did not differ between the first and second block of M1 stimulation, we observed a significant increase after three blocks (1800 pulses). Furthermore, iTBS enhanced resting-state functional connectivity between the stimulated M1 and premotor regions in both hemispheres. Functional connectivity between M1 and ipsilateral dorsal premotor cortex further increased dose-dependently after 1800 pulses of iTBS over M1. However, no correlation between changes in MEP amplitudes and functional connectivity was detected. In summary, our data show that increasing the number of iTBS stimulation blocks results in dose-dependent effects at the local level (cortical excitability) as well as at a systems level (functional connectivity) with a dose-dependent enhancement of dorsal premotor cortex-M1 connectivity. Copyright © 2014 the authors 0270-6474/14/346849-11$15.00/0.

Exploring excited eigenstates of many-body systems using the functional renormalization group

NASA Astrophysics Data System (ADS)

Klöckner, Christian; Kennes, Dante Marvin; Karrasch, Christoph

2018-05-01

We introduce approximate, functional renormalization group based schemes to obtain correlation functions in pure excited eigenstates of large fermionic many-body systems at arbitrary energies. The algorithms are thoroughly benchmarked and their strengths and shortcomings are documented using a one-dimensional interacting tight-binding chain as a prototypical testbed. We study two "toy applications" from the world of Luttinger liquid physics: the survival of power laws in lowly excited states as well as the spectral function of high-energy "block" excitations, which feature several single-particle Fermi edges.

Plane-Wave Implementation and Performance of à-la-Carte Coulomb-Attenuated Exchange-Correlation Functionals for Predicting Optical Excitation Energies in Some Notorious Cases.

PubMed

Bircher, Martin P; Rothlisberger, Ursula

2018-06-12

Linear-response time-dependent density functional theory (LR-TD-DFT) has become a valuable tool in the calculation of excited states of molecules of various sizes. However, standard generalized-gradient approximation and hybrid exchange-correlation (xc) functionals often fail to correctly predict charge-transfer (CT) excitations with low orbital overlap, thus limiting the scope of the method. The Coulomb-attenuation method (CAM) in the form of the CAM-B3LYP functional has been shown to reliably remedy this problem in many CT systems, making accurate predictions possible. However, in spite of a rather consistent performance across different orbital overlap regimes, some pitfalls remain. Here, we present a fully flexible and adaptable implementation of the CAM for Γ-point calculations within the plane-wave pseudopotential molecular dynamics package CPMD and explore how customized xc functionals can improve the optical spectra of some notorious cases. We find that results obtained using plane waves agree well with those from all-electron calculations employing atom-centered bases, and that it is possible to construct a new Coulomb-attenuated xc functional based on simple considerations. We show that such a functional is able to outperform CAM-B3LYP in some cases, while retaining similar accuracy in systems where CAM-B3LYP performs well.

Self-Consistent Optimization of Excited States within Density-Functional Tight-Binding.

PubMed

Kowalczyk, Tim; Le, Khoa; Irle, Stephan

2016-01-12

We present an implementation of energies and gradients for the ΔDFTB method, an analogue of Δ-self-consistent-field density functional theory (ΔSCF) within density-functional tight-binding, for the lowest singlet excited state of closed-shell molecules. Benchmarks of ΔDFTB excitation energies, optimized geometries, Stokes shifts, and vibrational frequencies reveal that ΔDFTB provides a qualitatively correct description of changes in molecular geometries and vibrational frequencies due to excited-state relaxation. The accuracy of ΔDFTB Stokes shifts is comparable to that of ΔSCF-DFT, and ΔDFTB performs similarly to ΔSCF with the PBE functional for vertical excitation energies of larger chromophores where the need for efficient excited-state methods is most urgent. We provide some justification for the use of an excited-state reference density in the DFTB expansion of the electronic energy and demonstrate that ΔDFTB preserves many of the properties of its parent ΔSCF approach. This implementation fills an important gap in the extended framework of DFTB, where access to excited states has been limited to the time-dependent linear-response approach, and affords access to rapid exploration of a valuable class of excited-state potential energy surfaces.

Variability in Terrestrial Water Storage and its effect on polar motion

NASA Astrophysics Data System (ADS)

Śliwińska, Justyna; Nastula, Jolanta

2017-04-01

Explaining the hydrological part of observed polar motion excitation has been a major challenge over a dozen years. The terrestrial water storage (TWS) excitation of polar motion - hydrological angular momentum (HAM), has been investigated widely using global hydrological models mainly at seasonal timescales. Unfortunately, the results from the models do not fully explain the role of hydrological signal in polar motion excitation. The determination of TWS from the Earth's gravity field observations represents an indirect approach for estimating land hydrology. Throughout the past decade, the Gravity Recovery and Climate Experiment (GRACE) has given an unprecedented view on global variations in Terrestrial Water Storage. Our investigations are focused on the influence of Terrestrial Water Storage (TWS) variations obtained from Gravity Recovery and Climate Experiment (GRACE) mission on polar motion excitation functions at decadal and inter-annual timescales. The global and regional trend, seasonal cycle as well as some extremes in TWS variations are considered here. Here TWS are obtained from the monthly mass grids land GRACE Tellus data: GRACE CSR RL05, GRACE GFZ RL05 and GRACE JPL RL05. As a comparative dataset, we also use TWS estimates determined from the World Climate Research Programme's Coupled Model Intercomparison Project Phase 5 (CMIP5). GRACE data and state-of-the-art CMIP5 climate models allow us to show the variability of hydrological part of polar motion under climate changes. Our studies include two steps: first, the determination and comparisons of regional patterns of TWS obtained from GRACE data and climate models, and second, comparison of the regional and global hydrological excitation functions of polar motion with a hydrological signal in the geodetic excitation functions of polar motion.

A Semi-Analytical Method for the PDFs of A Ship Rolling in Random Oblique Waves

NASA Astrophysics Data System (ADS)

Liu, Li-qin; Liu, Ya-liu; Xu, Wan-hai; Li, Yan; Tang, You-gang

2018-03-01

The PDFs (probability density functions) and probability of a ship rolling under the random parametric and forced excitations were studied by a semi-analytical method. The rolling motion equation of the ship in random oblique waves was established. The righting arm obtained by the numerical simulation was approximately fitted by an analytical function. The irregular waves were decomposed into two Gauss stationary random processes, and the CARMA (2, 1) model was used to fit the spectral density function of parametric and forced excitations. The stochastic energy envelope averaging method was used to solve the PDFs and the probability. The validity of the semi-analytical method was verified by the Monte Carlo method. The C11 ship was taken as an example, and the influences of the system parameters on the PDFs and probability were analyzed. The results show that the probability of ship rolling is affected by the characteristic wave height, wave length, and the heading angle. In order to provide proper advice for the ship's manoeuvring, the parametric excitations should be considered appropriately when the ship navigates in the oblique seas.

A walk through the approximations of ab initio multiple spawning

NASA Astrophysics Data System (ADS)

Mignolet, Benoit; Curchod, Basile F. E.

2018-04-01

Full multiple spawning offers an in principle exact framework for excited-state dynamics, where nuclear wavefunctions in different electronic states are represented by a set of coupled trajectory basis functions that follow classical trajectories. The couplings between trajectory basis functions can be approximated to treat molecular systems, leading to the ab initio multiple spawning method which has been successfully employed to study the photochemistry and photophysics of several molecules. However, a detailed investigation of its approximations and their consequences is currently missing in the literature. In this work, we simulate the explicit photoexcitation and subsequent excited-state dynamics of a simple system, LiH, and we analyze (i) the effect of the ab initio multiple spawning approximations on different observables and (ii) the convergence of the ab initio multiple spawning results towards numerically exact quantum dynamics upon a progressive relaxation of these approximations. We show that, despite the crude character of the approximations underlying ab initio multiple spawning for this low-dimensional system, the qualitative excited-state dynamics is adequately captured, and affordable corrections can further be applied to ameliorate the coupling between trajectory basis functions.

Computational study of the electronic spectra of the rare gas fluorohydrides HRgF (Rg = Ar, Kr, Xe, Rn)

NASA Astrophysics Data System (ADS)

van Hoeve, Miriam D.; Klobukowski, Mariusz

2018-03-01

Simulation of the electronic spectra of HRgF (Rg = Ar, Kr, Xe, Rn) was carried out using the time-dependent density functional method, with the CAMB3LYP functional and several basis sets augmented with even-tempered diffuse functions. A full spectral assignment for the HRgF systems was done. The effect of the rare gas matrix on the HRgF (Rg = Ar and Kr) spectra was investigated and it was found that the matrix blue-shifted the spectra. Scalar relativistic effects on the spectra were also studied and it was found that while the excitation energies of HArF and HKrF were insignificantly affected by relativistic effects, most of the excitation energies of HXeF and HRnF were red-shifted. Spin-orbit coupling was found to significantly affect excitation energies in HRnF. Analysis of performance of the model core potential basis set relative to all-electron (AE) basis sets showed that the former basis set increased computational efficiency and gave results similar to those obtained with the AE basis set.

A walk through the approximations of ab initio multiple spawning.

PubMed

Mignolet, Benoit; Curchod, Basile F E

2018-04-07

Full multiple spawning offers an in principle exact framework for excited-state dynamics, where nuclear wavefunctions in different electronic states are represented by a set of coupled trajectory basis functions that follow classical trajectories. The couplings between trajectory basis functions can be approximated to treat molecular systems, leading to the ab initio multiple spawning method which has been successfully employed to study the photochemistry and photophysics of several molecules. However, a detailed investigation of its approximations and their consequences is currently missing in the literature. In this work, we simulate the explicit photoexcitation and subsequent excited-state dynamics of a simple system, LiH, and we analyze (i) the effect of the ab initio multiple spawning approximations on different observables and (ii) the convergence of the ab initio multiple spawning results towards numerically exact quantum dynamics upon a progressive relaxation of these approximations. We show that, despite the crude character of the approximations underlying ab initio multiple spawning for this low-dimensional system, the qualitative excited-state dynamics is adequately captured, and affordable corrections can further be applied to ameliorate the coupling between trajectory basis functions.

Evaluating excited state atomic polarizabilities of chromophores† †Electronic supplementary information (ESI) available: Basis set dependence, definition of bond charges, Romberg differentiation, python script to calculate atomic polarizabilities, influence of the cavity radius, atomic polarizabilities of coumarin 153, all tables in atomic units. See DOI: 10.1039/c7cp08549d

PubMed Central

Heid, Esther

2018-01-01

Ground and excited state dipoles and polarizabilities of the chromophores N-methyl-6-oxyquinolinium betaine (MQ) and coumarin 153 (C153) in solution have been evaluated using time-dependent density functional theory (TD-DFT). A method for determining the atomic polarizabilities has been developed; the molecular dipole has been decomposed into atomic charge transfer and polarizability terms, and variation in the presence of an electric field has been used to evaluate atomic polarizabilities. On excitation, MQ undergoes very site-specific changes in polarizability while C153 shows significantly less variation. We also conclude that MQ cannot be adequately described by standard atomic polarizabilities based on atomic number and hybridization state. Changes in the molecular polarizability of MQ (on excitation) are not representative of the local site-specific changes in atomic polarizability, thus the overall molecular polarizability ratio does not provide a good approximation for local atom-specific polarizability changes on excitation. Accurate excited state force fields are needed for computer simulation of solvation dynamics. The chromophores considered in this study are often used as molecular probes. The methods and data reported here can be used for the construction of polarizable ground and excited state force fields. Atomic and molecular polarizabilities (ground and excited states) have been evaluated over a range of functionals and basis sets. Different mechanisms for including solvation effects have been examined; using a polarizable continuum model, explicit solvation and via sampling of clusters extracted from a MD simulation. A range of different solvents have also been considered. PMID:29542743

The Impact of Structural Heterogeneity on Excitation-Inhibition Balance in Cortical Networks.

PubMed

Landau, Itamar D; Egger, Robert; Dercksen, Vincent J; Oberlaender, Marcel; Sompolinsky, Haim

2016-12-07

Models of cortical dynamics often assume a homogeneous connectivity structure. However, we show that heterogeneous input connectivity can prevent the dynamic balance between excitation and inhibition, a hallmark of cortical dynamics, and yield unrealistically sparse and temporally regular firing. Anatomically based estimates of the connectivity of layer 4 (L4) rat barrel cortex and numerical simulations of this circuit indicate that the local network possesses substantial heterogeneity in input connectivity, sufficient to disrupt excitation-inhibition balance. We show that homeostatic plasticity in inhibitory synapses can align the functional connectivity to compensate for structural heterogeneity. Alternatively, spike-frequency adaptation can give rise to a novel state in which local firing rates adjust dynamically so that adaptation currents and synaptic inputs are balanced. This theory is supported by simulations of L4 barrel cortex during spontaneous and stimulus-evoked conditions. Our study shows how synaptic and cellular mechanisms yield fluctuation-driven dynamics despite structural heterogeneity in cortical circuits. Copyright © 2016 The Author(s). Published by Elsevier Inc. All rights reserved.

AC electroosmosis in microchannels packed with a porous medium

NASA Astrophysics Data System (ADS)

Kang, Yuejun; Yang, Chun; Huang, Xiaoyang

2004-08-01

This paper presents a theoretical study on ac-driven electroosmotic flow in both open-end and closed-end microchannels packed with uniform charged spherical microparticles. The time-periodic oscillating electroosmotic flow in an open-end capillary in response to the application of an alternating (ac) electric field is obtained using the Green function approach. The analysis is based on the Carman-Kozeny theory. The backpressure associated with the counter-flow in a closed-end capillary is obtained by analytically solving the modified Brinkman momentum equation. It is demonstrated that in a microchannel with its two ends connected to reservoirs and subject to ambient pressure, the oscillating Darcy velocity profile depends on both the pore size and the excitation frequency; such effects are coupled through an important aspect ratio of the tubule radius to the Stokes penetration depth. For a fixed pore size, the magnitude of the ac electroosmotic flow decreases with increasing frequency. With increasing pore size, however, the magnitude of the maximum velocity shows two different trends with respect to the excitation frequency: it gets higher in the low frequency domain, and gets lower in the high frequency domain. In a microchannel with closed ends, for a fixed excitation frequency, use of smaller packing particles can generate higher backpressure. For a fixed pore size, the backpressure magnitude shows two different trends changing with the excitation frequency. When the excitation frequency is lower than the system characteristic frequency, the backpressure decreases with increasing excitation frequency. When the excitation frequency is higher than the system characteristic frequency, the backpressure increases with increasing excitation frequency.

Acceptor number-dependent ultrafast photo-physical properties of push-pull chromophores using time-resolved methods

NASA Astrophysics Data System (ADS)

Chi, Xiao-Chun; Wang, Ying-Hui; Gao, Yu; Sui, Ning; Zhang, Li-Quan; Wang, Wen-Yan; Lu, Ran; Ji, Wen-Yu; Yang, Yan-Qiang; Zhang, Han-Zhuang

2018-04-01

Three push-pull chromophores comprising a triphenylamine (TPA) as electron-donating moiety and functionalized β-diketones as electron acceptor units are studied by various spectroscopic techniques. The time-correlated single-photon counting data shows that increasing the number of electron acceptor units accelerates photoluminescence relaxation rate of compounds. Transient spectra data shows that intramolecular charge transfer (ICT) takes place from TPA units to β-diketones units after photo-excitation. Increasing the number of electron acceptor units would prolong the generation process of ICT state, and accelerate the excited molecule reorganization process and the relaxation process of ICT state.

Statistics of Fractionalized Excitations through Threshold Spectroscopy.

PubMed

Morampudi, Siddhardh C; Turner, Ari M; Pollmann, Frank; Wilczek, Frank

2017-06-02

We show that neutral anyonic excitations have a signature in spectroscopic measurements of materials: The low-energy onset of spectral functions near the threshold follows universal power laws with an exponent that depends only on the statistics of the anyons. This provides a route, using experimental techniques such as neutron scattering and tunneling spectroscopy, for detecting anyonic statistics in topologically ordered states such as gapped quantum spin liquids and hypothesized fractional Chern insulators. Our calculations also explain some recent theoretical results in spin systems.

Terahertz emission from thermally-managed square intrinsic Josephson junction microstrip antennas

NASA Astrophysics Data System (ADS)

Klemm, Richard; Davis, Andrew; Wang, Qing

We show for thin square microstrip antennas that the transverse magnetic electromagnetic cavity modes are greatly restricted in number due to the point group symmetry of a square. For the ten lowest frequency emissions, we present plots of the orthonormal wave functions and of the angular distributions of the emission power obtained from the uniform Josephson current source and from the excitation of an electromagnetic cavity mode excited in the intrinsic Josephson junctions between the layers of a highly anisotropic layered superconductor.

Enhancing transcranial direct current stimulation via motor imagery and kinesthetic illusion: crossing internal and external tools.

PubMed

Bodranghien, Florian; Manto, Mario; Lebon, Florent

2016-06-01

Transcranial direct current stimulation is a safe technique which is now part of the therapeutic armamentarium for the neuromodulation of motor functions and cognitive operations. It is currently considered that tDCS is an intervention that might promote functional recovery after a lesion in the central nervous system, thus reducing long-term disability and associated socio-economic burden. A recent study shows that kinesthetic illusion and motor imagery prolong the effects of tDCS on corticospinal excitability, overcoming one of the limitations of this intervention. Because changes in excitability anticipate changes in structural plasticity in the CNS, this interesting multi-modal approach might very soon find applications in neurorehabilitation.

Dynamics of a population of oscillatory and excitable elements.

PubMed

O'Keeffe, Kevin P; Strogatz, Steven H

2016-06-01

We analyze a variant of a model proposed by Kuramoto, Shinomoto, and Sakaguchi for a large population of coupled oscillatory and excitable elements. Using the Ott-Antonsen ansatz, we reduce the behavior of the population to a two-dimensional dynamical system with three parameters. We present the stability diagram and calculate several of its bifurcation curves analytically, for both excitatory and inhibitory coupling. Our main result is that when the coupling function is broad, the system can display bistability between steady states of constant high and low activity, whereas when the coupling function is narrow and inhibitory, one of the states in the bistable regime can show persistent pulsations in activity.

Nonperturbative Series Expansion of Green's Functions: The Anatomy of Resonant Inelastic X-Ray Scattering in the Doped Hubbard Model

NASA Astrophysics Data System (ADS)

Lu, Yi; Haverkort, Maurits W.

2017-12-01

We present a nonperturbative, divergence-free series expansion of Green's functions using effective operators. The method is especially suited for computing correlators of complex operators as a series of correlation functions of simpler forms. We apply the method to study low-energy excitations in resonant inelastic x-ray scattering (RIXS) in doped one- and two-dimensional single-band Hubbard models. The RIXS operator is expanded into polynomials of spin, density, and current operators weighted by fundamental x-ray spectral functions. These operators couple to different polarization channels resulting in simple selection rules. The incident photon energy dependent coefficients help to pinpoint main RIXS contributions from different degrees of freedom. We show in particular that, with parameters pertaining to cuprate superconductors, local spin excitation dominates the RIXS spectral weight over a wide doping range in the cross-polarization channel.

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

Singh, Varinderjit; Vadas, J.; Steinbach, T. K.

Measuring the fusion excitation function for an isotopic chain of projectile nuclei provides a stringent test of a microscopic description of fusion. We report the first measurement of the fusion excitation function at near-barrier energies for the 19O+ 12C system. The measured excitation function is compared with the fusion excitation function of 18O+ 12C. A significant enhancement in the fusion probability of 19O ions with a 12C target as compared to 18O ions is observed. As a result, the experimental cross-sections observed at near-barrier energies are compared with a state-of-the-art microscopic model.

Effect of Wii-based balance training on corticomotor excitability post stroke.

PubMed

Omiyale, Oluwabunmi; Crowell, Charles R; Madhavan, Sangeetha

2015-01-01

The objective was to examine the effectiveness of a 3-week balance training program using the Nintendo Wii Fit gaming system (Nintendo Wii Sports, Nintendo, Redmond, WA) on lower limb corticomotor excitability and other clinical measures in chronic stroke survivors. Ten individuals diagnosed with ischemic stroke with residual hemiparesis received balance training using the Wii Fit for 60 min/day, three times/week, for three weeks. At the end of training, an increase in interhemispheric symmetry of corticomotor excitability of the tibialis anterior muscle representations was noted (n = 9). Participants also showed improvements in reaction time, time to perform the Dual Timed-Up-and-Go test, and balance confidence. The training-induced balance in corticomotor excitability suggests that this Wii-based balance training paradigm has the potential to influence neural plasticity and thereby functional recovery.

Local symmetries and order-disorder transitions in small macroscopic Wigner islands.

PubMed

Coupier, Gwennou; Guthmann, Claudine; Noat, Yves; Jean, Michel Saint

2005-04-01

The influence of local order on the disordering scenario of small Wigner islands is discussed. A first disordering step is put in evidence by the time correlation functions and is linked to individual excitations resulting in configuration transitions, which are very sensitive to the local symmetries. This is followed by two other transitions, corresponding to orthoradial and radial diffusion, for which both individual and collective excitations play a significant role. Finally, we show that, contrary to large systems, the focus that is commonly made on collective excitations for such small systems through the Lindemann criterion has to be made carefully in order to clearly identify the relative contributions in the whole disordering process.

Evolutionarily conserved coupling of adaptive and excitable networks mediates eukaryotic chemotaxis

NASA Astrophysics Data System (ADS)

Tang, Ming; Wang, Mingjie; Shi, Changji; Iglesias, Pablo A.; Devreotes, Peter N.; Huang, Chuan-Hsiang

2014-10-01

Numerous models explain how cells sense and migrate towards shallow chemoattractant gradients. Studies show that an excitable signal transduction network acts as a pacemaker that controls the cytoskeleton to drive motility. Here we show that this network is required to link stimuli to actin polymerization and chemotactic motility and we distinguish the various models of chemotaxis. First, signalling activity is suppressed towards the low side in a gradient or following removal of uniform chemoattractant. Second, signalling activities display a rapid shut off and a slower adaptation during which responsiveness to subsequent test stimuli decline. Simulations of various models indicate that these properties require coupled adaptive and excitable networks. Adaptation involves a G-protein-independent inhibitor, as stimulation of cells lacking G-protein function suppresses basal activities. The salient features of the coupled networks were observed for different chemoattractants in Dictyostelium and in human neutrophils, suggesting an evolutionarily conserved mechanism for eukaryotic chemotaxis.

Dynamic Optical Tuning of Interlayer Interactions in the Transition Metal Dichalcogenides

DOE PAGES

Mannebach, Ehren M.; Nyby, Clara; Ernst, Friederike; ...

2017-11-09

Modulation of weak interlayer interactions between quasi-two-dimensional atomic planes in the transition metal dichalcogenides (TMDCs) provides avenues for tuning their functional properties. Here we show that above-gap optical excitation in the TMDCs leads to an unexpected large-amplitude, ultrafast compressive force between the two-dimensional layers, as probed by in situ measurements of the atomic layer spacing at femtosecond time resolution. We show that this compressive response arises from a dynamic modulation of the interlayer van der Waals interaction and that this represents the dominant light-induced stress at low excitation densities. A simple analytic model predicts the magnitude and carrier density dependencemore » of the measured strains. Furthermore, this work establishes a new method for dynamic, nonequilibrium tuning of correlation-driven dispersive interactions and of the optomechanical functionality of TMDC quasi-two-dimensional materials.« less

TD-CI simulation of the electronic optical response of molecules in intense fields II: comparison of DFT functionals and EOM-CCSD.

PubMed

Sonk, Jason A; Schlegel, H Bernhard

2011-10-27

Time-dependent configuration interaction (TD-CI) simulations can be used to simulate molecules in intense laser fields. TD-CI calculations use the excitation energies and transition dipoles calculated in the absence of a field. The EOM-CCSD method provides a good estimate of the field-free excited states but is rather expensive. Linear-response time-dependent density functional theory (TD-DFT) is an inexpensive alternative for computing the field-free excitation energies and transition dipoles needed for TD-CI simulations. Linear-response TD-DFT calculations were carried out with standard functionals (B3LYP, BH&HLYP, HSE2PBE (HSE03), BLYP, PBE, PW91, and TPSS) and long-range corrected functionals (LC-ωPBE, ωB97XD, CAM-B3LYP, LC-BLYP, LC-PBE, LC-PW91, and LC-TPSS). These calculations used the 6-31G(d,p) basis set augmented with three sets of diffuse sp functions on each heavy atom. Butadiene was employed as a test case, and 500 excited states were calculated with each functional. Standard functionals yield average excitation energies that are significantly lower than the EOM-CC, while long-range corrected functionals tend to produce average excitation energies slightly higher. Long-range corrected functionals also yield transition dipoles that are somewhat larger than EOM-CC on average. The TD-CI simulations were carried out with a three-cycle Gaussian pulse (ω = 0.06 au, 760 nm) with intensities up to 1.26 × 10(14) W cm(-2) directed along the vector connecting the end carbons. The nonlinear response as indicated by the residual populations of the excited states after the pulse is far too large with standard functionals, primarily because the excitation energies are too low. The LC-ωPBE, LC-PBE, LC-PW91, and LC-TPSS long-range corrected functionals produce responses comparable to EOM-CC.

Synthesis and functionalization of monodisperse near-ultraviolet and visible excitable multifunctional Eu(3+), Bi(3+):REVO4 nanophosphors for bioimaging and biosensing applications.

PubMed

Escudero, Alberto; Carrillo-Carrión, Carolina; Zyuzin, Mikhail V; Ashraf, Sumaira; Hartmann, Raimo; Núñez, Nuria O; Ocaña, Manuel; Parak, Wolfgang J

2016-06-16

Near-ultraviolet and visible excitable Eu- and Bi-doped NPs based on rare earth vanadates (REVO4, RE = Y, Gd) have been synthesized by a facile route from appropriate RE precursors, europium and bismuth nitrate, and sodium orthovanadate, by homogeneous precipitation in an ethylene glycol/water mixture at 120 °C. The NPs can be functionalized either by a one-pot synthesis with polyacrylic acid (PAA) or by a Layer-by-Layer approach with poly(allylamine hydrochloride) (PAH) and PAA. In the first case, the particle size can also be tuned by adjusting the amount of PAA. The Eu- Bi-doped REVO4 based nanophosphors show the typical red luminescence of Eu(iii), which can be excited through an energy transfer process from the vanadate anions, resulting in a much higher luminescence intensity in comparison to the direct excitation of the europium cations. The incorporation of Bi into the REVO4 structure shifts the original absorption band of the vanadate anions towards longer wavelengths, giving rise to nanophosphors with an excitation maximum at 342 nm, which can also be excited in the visible range. The suitability of such nanophosphors for bioimaging and biosensing applications, as well as their colloidal stability in different buffer media of biological interest, their cytotoxicity, their degradability at low pH, and their uptake by HeLa cells have been evaluated. Their suitability for bioimaging and biosensing applications is also demonstrated.

The Importance of Short- and Long-Range Exchange on Various Excited State Properties of DNA Monomers, Stacked Complexes, and Watson-Crick Pairs.

PubMed

Raeber, Alexandra E; Wong, Bryan M

2015-05-12

We present a detailed analysis of several time-dependent DFT (TD-DFT) methods, including conventional hybrid functionals and two types of nonempirically tuned range-separated functionals, for predicting a diverse set of electronic excitations in DNA nucleobase monomers and dimers. This large and extensive set of excitations comprises a total of 50 different transitions (for each tested DFT functional) that includes several n → π and π → π* valence excitations, long-range charge-transfer excitations, and extended Rydberg transitions (complete with benchmark calculations from high-level EOM-CCSD(T) methods). The presence of localized valence excitations as well as extreme long-range charge-transfer excitations in these systems poses a serious challenge for TD-DFT methods that allows us to assess the importance of both short- and long-range exchange contributions for simultaneously predicting all of these various transitions. In particular, we find that functionals that do not have both short- and full long-range exchange components are unable to predict the different types of nucleobase excitations with the same accuracy. Most importantly, the current study highlights the importance of both short-range exchange and a nonempirically tuned contribution of long-range exchange for accurately predicting the diverse excitations in these challenging nucleobase systems.

Density functional study of the electronic structure of dye-functionalized fullerenes and their model donor-acceptor complexes containing P3HT

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

Baruah, Tunna; Garnica, Amanda; Paggen, Marina

2016-04-14

We study the electronic structure of C{sub 60} fullerenes functionalized with a thiophene-diketo-pyrrolopyrrole-thiophene based chromophore using density functional theory combined with large polarized basis sets. As the attached chromophore has electron donor character, the functionalization of the fullerene leads to a donor-acceptor (DA) system. We examine in detail the effect of the linker and the addition site on the electronic structure of the functionalized fullerenes. We further study the electronic structure of these DA complexes with a focus on the charge transfer excitations. Finally, we examine the interface of the functionalized fullerenes with the widely used poly(3-hexylthiophene-2,5-diyl) (P3HT) donor. Ourmore » results show that all functionalized fullerenes with an exception of the C{sub 60}-pyrrolidine [6,6], where the pyrrolidine is attached at a [6,6] site, have larger electron affinities relative to the pristine C{sub 60} fullerene. We also estimate the quasi-particle gap, lowest charge transfer excitation energy, and the exciton binding energies of the functionalized fullerene-P3MT model systems. Results show that the exciton binding energies in these model complexes are slightly smaller compared to a similarly prepared phenyl-C{sub 61}-butyric acid methyl ester (PCBM)-P3MT complex.« less

Local field effects in the energy transfer between a chromophore and a carbon nanotube: a single-nanocompound investigation.

PubMed

Roquelet, Cyrielle; Vialla, Fabien; Diederichs, Carole; Roussignol, Philippe; Delalande, Claude; Deleporte, Emmanuelle; Lauret, Jean-Sébastien; Voisin, Christophe

2012-10-23

Energy transfer in noncovalently bound porphyrin/carbon nanotube compounds is investigated at the single-nanocompound scale. Excitation spectroscopy of the luminescence of the nanotube shows two resonances arising from intrinsic excitation of the nanotube and from energy transfer from the porphyrin. Polarization diagrams show that both resonances are highly anisotropic, with a preferred direction along the tube axis. The energy transfer is thus strongly anisotropic despite the almost isotropic absorption of porphyrins. We account for this result by local field effects induced by the large optical polarizability of nanotubes. We show that the local field correction extends over several nanometers outside the nanotubes and drives the overall optical response of functionalized nanotubes.

Analysis of the geodetic residuals as differences between geodetic and sum of the atmospheric and ocean excitation of polar motion

NASA Astrophysics Data System (ADS)

Kolaczek, B.; Pasnicka, M.; Nastula, J.

2012-12-01

Up to now studies of geophysical excitation of polar motion containing AAM (Atmospheric Angular Momentum), OAM (Oceanic Angular Momentum) and HAM (Hydrological Angular Momentum) excitation functions of polar motion have not achieved the total agreement between geophysical and determined geodetic excitation (GAM, Geodetic AngularMomentum) functions of polar motion...

A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions

DOE PAGES

Wu, Guanhong; Zhou, Chenkun; Ming, Wenmei; ...

2018-05-23

Organic–inorganic metal halide hybrids have emerged as a new class of materials with fascinating optical and electronic properties. The exceptional structure tunability has enabled the development of materials with various dimensionalities at the molecular level, from three-dimensional (3D) to 2D, 1D, and 0D. Here, we report a new 1D lead chloride hybrid, C 4N 2H 14PbCl 4, which exhibits unusual inverse excitation-dependent broadband emission from bluish-green to yellow. Density functional theory calculations were performed to better understand the mechanism of this excitation-dependent broadband emission. This 1D hybrid material is found to have two emission centers, corresponding to the self-trapped excitonsmore » (STEs) and vacancy-bound excitons. The excitation-dependent emission is due to different populations of these two types of excitons generated at different excitation wavelengths. Furthermore, this work shows the rich chemistry and physics of organic–inorganic metal halide hybrids and paves the way to achieving novel light emitters with excitation-dependent broadband emissions at room temperature.« less

A One-Dimensional Organic Lead Chloride Hybrid with Excitation-Dependent Broadband Emissions

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

Wu, Guanhong; Zhou, Chenkun; Ming, Wenmei

Organic–inorganic metal halide hybrids have emerged as a new class of materials with fascinating optical and electronic properties. The exceptional structure tunability has enabled the development of materials with various dimensionalities at the molecular level, from three-dimensional (3D) to 2D, 1D, and 0D. Here, we report a new 1D lead chloride hybrid, C 4N 2H 14PbCl 4, which exhibits unusual inverse excitation-dependent broadband emission from bluish-green to yellow. Density functional theory calculations were performed to better understand the mechanism of this excitation-dependent broadband emission. This 1D hybrid material is found to have two emission centers, corresponding to the self-trapped excitonsmore » (STEs) and vacancy-bound excitons. The excitation-dependent emission is due to different populations of these two types of excitons generated at different excitation wavelengths. Furthermore, this work shows the rich chemistry and physics of organic–inorganic metal halide hybrids and paves the way to achieving novel light emitters with excitation-dependent broadband emissions at room temperature.« less

Regulating energy transfer of excited carriers and the case for excitation-induced hydrogen dissociation on hydrogenated graphene

PubMed Central

Bang, Junhyeok; Meng, Sheng; Sun, Yi-Yang; West, Damien; Wang, Zhiguo; Gao, Fei; Zhang, S. B.

2013-01-01

Understanding and controlling of excited carrier dynamics is of fundamental and practical importance, particularly in photochemistry and solar energy applications. However, theory of energy relaxation of excited carriers is still in its early stage. Here, using ab initio molecular dynamics (MD) coupled with time-dependent density functional theory, we show a coverage-dependent energy transfer of photoexcited carriers in hydrogenated graphene, giving rise to distinctively different ion dynamics. Graphene with sparsely populated H is difficult to dissociate due to inefficient transfer of the excitation energy into kinetic energy of the H. In contrast, H can easily desorb from fully hydrogenated graphane. The key is to bring down the H antibonding state to the conduction band minimum as the band gap increases. These results can be contrasted to those of standard ground-state MD that predict H in the sparse case should be much less stable than that in fully hydrogenated graphane. Our findings thus signify the importance of carrying out explicit electronic dynamics in excited-state simulations. PMID:23277576

Multiple hydrogen bonding in excited states of aminopyrazine in methanol solution: time-dependent density functional theory study.

PubMed

Chai, Shuo; Yu, Jie; Han, Yong-Chang; Cong, Shu-Lin

2013-11-01

Aminopyrazine (AP) and AP-methanol complexes have been theoretically studied by using density functional theory (DFT) and time-dependent density functional theory (TDDFT). The excited-state hydrogen bonds are discussed in detail. In the ground state the intermolecular multiple hydrogen bonds can be formed between AP molecule and protic solvents. The AP monomer and hydrogen-bonded complex of AP with one methanol are photoexcited initially to the S2 state, and then transferred to the S1 state via internal conversion. However the complex of AP with two methanol molecules is directly excited to the S1 state. From the calculated electronic excited energies and simulated absorption spectra, we find that the intermolecular hydrogen bonds are strengthened in the electronic excited states. The strengthening is confirmed by the optimized excited-state geometries. The photochemical processes in the electronic excited states are significantly influenced by the excited-state hydrogen bond strengthening. Copyright © 2013 Elsevier B.V. All rights reserved.

Solute-Solvent Charge-Transfer Excitations and Optical Absorption of Hydrated Hydroxide from Time-Dependent Density-Functional Theory.

PubMed

Opalka, Daniel; Sprik, Michiel

2014-06-10

The electronic structure of simple hydrated ions represents one of the most challenging problems in electronic-structure theory. Spectroscopic experiments identified the lowest excited state of the solvated hydroxide as a charge-transfer-to-solvent (CTTS) state. In the present work we report computations of the absorption spectrum of the solvated hydroxide ion, treating both solvent and solute strictly at the same level of theory. The average absorption spectrum up to 25 eV has been computed for samples taken from periodic ab initio molecular dynamics simulations. The experimentally observed CTTS state near the onset of the absorption threshold has been analyzed at the generalized-gradient approximation (GGA) and with a hybrid density-functional. Based on results for the lowest excitation energies computed with the HSE hybrid functional and a Davidson diagonalization scheme, the CTTS transition has been found 0.6 eV below the first absorption band of liquid water. The transfer of an electron to the solvent can be assigned to an excitation from the solute 2pπ orbitals, which are subject to a small energetic splitting due to the asymmetric solvent environment, to the significantly delocalized lowest unoccupied orbital of the solvent. The distribution of the centers of the excited state shows that CTTS along the OH(-) axis of the hydroxide ion is avoided. Furthermore, our simulations indicate that the systematic error arising in the calculated spectrum at the GGA originates from a poor description of the valence band energies in the solution.

Source mechanism of long-period events at Kusatsu-Shirane Volcano, Japan, inferred from waveform inversion of the effective excitation functions

USGS Publications Warehouse

Nakano, M.; Kumagai, H.; Chouet, B.A.

2003-01-01

We investigate the source mechanism of long-period (LP) events observed at Kusatsu-Shirane Volcano, Japan, based on waveform inversions of their effective excitation functions. The effective excitation function, which represents the apparent excitation observed at individual receivers, is estimated by applying an autoregressive filter to the LP waveform. Assuming a point source, we apply this method to seven LP events the waveforms of which are characterized by simple decaying and nearly monochromatic oscillations with frequency in the range 1-3 Hz. The results of the waveform inversions show dominant volumetric change components accompanied by single force components, common to all the events analyzed, and suggesting a repeated activation of a sub-horizontal crack located 300 m beneath the summit crater lakes. Based on these results, we propose a model of the source process of LP seismicity, in which a gradual buildup of steam pressure in a hydrothermal crack in response to magmatic heat causes repeated discharges of steam from the crack. The rapid discharge of fluid causes the collapse of the fluid-filled crack and excites acoustic oscillations of the crack, which produce the characteristic waveforms observed in the LP events. The presence of a single force synchronous with the collapse of the crack is interpreted as the release of gravitational energy that occurs as the slug of steam ejected from the crack ascends toward the surface and is replaced by cooler water flowing downward in a fluid-filled conduit linking the crack and the base of the crater lake. ?? 2003 Elsevier Science B.V. All rights reserved.

Extended Lagrangian Excited State Molecular Dynamics

DOE PAGES

Bjorgaard, Josiah August; Sheppard, Daniel Glen; Tretiak, Sergei; ...

2018-01-09

In this work, an extended Lagrangian framework for excited state molecular dynamics (XL-ESMD) using time-dependent self-consistent field theory is proposed. The formulation is a generalization of the extended Lagrangian formulations for ground state Born–Oppenheimer molecular dynamics [Phys. Rev. Lett. 2008 100, 123004]. The theory is implemented, demonstrated, and evaluated using a time-dependent semiempirical model, though it should be generally applicable to ab initio theory. The simulations show enhanced energy stability and a significantly reduced computational cost associated with the iterative solutions of both the ground state and the electronically excited states. Relaxed convergence criteria can therefore be used both formore » the self-consistent ground state optimization and for the iterative subspace diagonalization of the random phase approximation matrix used to calculate the excited state transitions. In conclusion, the XL-ESMD approach is expected to enable numerically efficient excited state molecular dynamics for such methods as time-dependent Hartree–Fock (TD-HF), Configuration Interactions Singles (CIS), and time-dependent density functional theory (TD-DFT).« less

Excitation of Love waves in a thin film layer by a line source.

NASA Technical Reports Server (NTRS)

Tuan, H.-S.; Ponamgi, S. R.

1972-01-01

The excitation of a Love surface wave guided by a thin film layer deposited on a semiinfinite substrate is studied in this paper. Both the thin film and the substrate are considered to be elastically isotropic. Amplitudes of the surface wave in the thin film region and the substrate are found in terms of the strength of a line source vibrating in a direction transverse to the propagating wave. In addition to the surface wave, the bulk shear wave excited by the source is also studied. Analytical expressions for the bulk wave amplitude as a function of the direction of propagation, the acoustic powers transported by the surface and bulk waves, and the efficiency of surface wave excitation are obtained. A numerical example is given to show how the bulk wave radiation pattern depends upon the source frequency, the film thickness and other important parameters of the problem. The efficiency of surface wave excitation is also calculated for various parameter values.

Extended Lagrangian Excited State Molecular Dynamics

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

Bjorgaard, Josiah August; Sheppard, Daniel Glen; Tretiak, Sergei

In this work, an extended Lagrangian framework for excited state molecular dynamics (XL-ESMD) using time-dependent self-consistent field theory is proposed. The formulation is a generalization of the extended Lagrangian formulations for ground state Born–Oppenheimer molecular dynamics [Phys. Rev. Lett. 2008 100, 123004]. The theory is implemented, demonstrated, and evaluated using a time-dependent semiempirical model, though it should be generally applicable to ab initio theory. The simulations show enhanced energy stability and a significantly reduced computational cost associated with the iterative solutions of both the ground state and the electronically excited states. Relaxed convergence criteria can therefore be used both formore » the self-consistent ground state optimization and for the iterative subspace diagonalization of the random phase approximation matrix used to calculate the excited state transitions. In conclusion, the XL-ESMD approach is expected to enable numerically efficient excited state molecular dynamics for such methods as time-dependent Hartree–Fock (TD-HF), Configuration Interactions Singles (CIS), and time-dependent density functional theory (TD-DFT).« less

Extended Lagrangian Excited State Molecular Dynamics.

PubMed

Bjorgaard, J A; Sheppard, D; Tretiak, S; Niklasson, A M N

2018-02-13

An extended Lagrangian framework for excited state molecular dynamics (XL-ESMD) using time-dependent self-consistent field theory is proposed. The formulation is a generalization of the extended Lagrangian formulations for ground state Born-Oppenheimer molecular dynamics [Phys. Rev. Lett. 2008 100, 123004]. The theory is implemented, demonstrated, and evaluated using a time-dependent semiempirical model, though it should be generally applicable to ab initio theory. The simulations show enhanced energy stability and a significantly reduced computational cost associated with the iterative solutions of both the ground state and the electronically excited states. Relaxed convergence criteria can therefore be used both for the self-consistent ground state optimization and for the iterative subspace diagonalization of the random phase approximation matrix used to calculate the excited state transitions. The XL-ESMD approach is expected to enable numerically efficient excited state molecular dynamics for such methods as time-dependent Hartree-Fock (TD-HF), Configuration Interactions Singles (CIS), and time-dependent density functional theory (TD-DFT).

Comparison of hydrological signal in polar motion excitation with those based on the FGOALS-g2 climate model

NASA Astrophysics Data System (ADS)

Wińska, Małgorzata; Nastula, Jolanta; Salstein, David

2016-04-01

Our investigations are focused on the influence of different land hydrosphere surface parameters (precipitation, evaporation, total runoff, soil moisture, accumulated snow) on polar motion excitation functions at seasonal and nonseasonal timescales. Here these different variables are obtained from the Flexible Global Ocean-Atmosphere-Land System Model, Grid point Version 2 (FGOALS-g2), which is a climate model from the fifth phase of the Coupled Model Intercomparison Project (CMIP5); with CMIP5 being composed of separate component models of the atmosphere, ocean, sea ice, and land surface. In this study Terrestrial Water Storage TWS changes were determined as: differences between the precipitation, evaporation and total surface runoff content, and as the total soil moisture content being a sum of soil moisture and snowfall flux changes. We compare the model-based data with those from estimates of the Equivalent Water Thickness determined by GRACE satellite observations from the Center for Space Research (CSR). The transfer of angular momentum from global geophysical fluids to the solid Earth is described by the equatorial components χ1 and χ2 of the polar motion excitation functions. Observationally, these so-called geodetic excitation functions of polar motion can be determined on the basis of the equations of motion by using observed x, y components of the pole. The second-degree, first-order coefficients of the Earth gravity field are proportional to variations of the equatorial component χ1, χ2 of the series of the gravimetric excitation function of polar motion. This gravimetric function can be compared with the mass term of geodetic excitation of polar motion. Our analysis comprises (1) determinations and comparisons of regional patterns of hydrological excitation functions of polar motion, and (2) comparison of the global hydrological function determined from the FGOALS-g2 and GRACE data with a hydrological signal in the geodetic excitation function of polar motion, determined as a residual geodetic and atmospheric plus oceanic excitations.

Investigating Female Sexual Concordance: Do Sexual Excitation and Sexual Inhibition Moderate the Agreement of Genital and Subjective Sexual Arousal in Women?

PubMed

Velten, Julia; Scholten, Saskia; Graham, Cynthia A; Adolph, Dirk; Margraf, Jürgen

2016-11-01

The agreement of subjective and genital sexual response, also referred to as sexual concordance, shows substantial variability between women. Identifying predictors of sexual arousal and sexual concordance is important to improve our understanding of female sexual response and its relationship to sexual function or dysfunction. The aim of this study was to assess the relevance of sexual excitation and sexual inhibition as predictors of subjective sexual arousal, genital arousal, and sexual concordance. In a laboratory setting, sexual arousal was induced by erotic video stimuli. Subjective sexual arousal was assessed continuously during stimulus presentation and genital arousal was measured with vaginal photoplethysmography. Data of 58 women (M age = 24.95, SD = 4.65) were analyzed using multilevel analyses (HLM). This data analytic technique estimates the within-subject associations of subjective and genital arousal, by controlling for between-subject differences. An interaction term of sexual excitation and sexual inhibition significantly predicted genital sexual arousal. In exploratory analyses, two lower order factors of sexual inhibition (Concerns about Sexual Function and Arousal Contingency) were predictive of sexual concordance. Further examination of these associations might increase our knowledge of female sexual function and deepen our understanding of how sexual excitation and sexual inhibition affect sexual arousal and consequently, impact sexual behaviors, in women.

Singlet and triplet excitons and charge polarons in cycloparaphenylenes. A density functional theory study

DOE PAGES

Liu, Jin; Adamska, Lyudmyla; Doorn, Stephen K.; ...

2015-05-14

Conformational structure and the electronic properties of various electronic excitations in cycloparaphenylenes (CPPs) are calculated using hybrid Density Functional Theory (DFT). The results demonstrate that wavefunctions of singlet and triplet excitons as well as the positive and negative polarons remain fully delocalized in CPPs. In contrast, these excitations in larger CPP molecules become localized on several phenyl rings, which are locally planarized, while the undeformed ground state geometry is preserved on the rest of the hoop. As evidenced by the measurements of bond-length alternation and dihedral angles, localized regions show stronger hybridization between neighboring bonds and thus enhanced electronic communication.more » This effect is even more significant in the smaller hoops, where phenyl rings have strong quinoid character in the ground state. Thus, upon excitation, electron–phonon coupling leads to the self-trapping of the electronic wavefunction and release of energy from fractions of an eV up to two eVs, depending on the type of excitation and the size of the hoop. The impact of such localization on electronic and optical properties of CPPs is systematically investigated and compared with the available experimental measurements.« less

Effect of the solvent environment on the spectroscopic properties and dynamics of the lowest excited states of carotenoids

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

Frank, H.A.; Bautista, J.A.; Josue, J.

2000-05-11

The spectroscopic properties and dynamics of the lowest excited singlet states of peridinin, fucoxanthin, neoxanthin, uriolide acetate, spheroidene, and spheroidenone in several different solvents have been studied by steady-state absorption and fast-transient optical spectroscopic techniques. Peridinin, fucoxanthin, uriolide acetate, and spheroidenone, which contain carbonyl functional groups in conjugation with the carbon-carbon {pi}-electron system, display broader absorption spectral features and are affected more by the solvent environment than neoxanthin and spheroidene, which do not contain carbonyl functional groups. The possible sources of the spectral broadening are explored by examining the absorption spectra at 77 K in glassy solvents. Also, carotenoids whichmore » contain carbonyls have complex transient absorption spectra and show a pronounced dependence of the excited singlet state lifetime on the solvent environment. It is postulated that these effects are related to the presence of an intramolecular charge transfer state strongly coupled to the S{sub 1} (2{sup 1}A{sub g}) excited singlet state. Structural variations in the series of carotenoids studied here make it possible to focus on the general molecular features that control the spectroscopic and dynamic properties of carotenoids.« less

Energy dependence of the prompt γ -ray emission from the ( d , p ) -induced fission of U * 234 and Pu * 240

DOE PAGES

Rose, Sunniva J.; Zeiser, Fabio; Wilson, J. N.; ...

2017-07-05

Prompt-fission γ rays are responsible for approximately 5% of the total energy released in fission, and therefore important to understand when modeling nuclear reactors. In this work we present prompt γ-ray emission characteristics in fission as a function of the nuclear excitation energy of the fissioning system. Emitted γ-ray spectra were measured, and γ-ray multiplicities and average and total γ energies per fission were determined for the 233U(d,pf) reaction for excitation energies between 4.8 and 10 MeV, and for the 239Pu(d,pf) reaction between 4.5 and 9 MeV. The spectral characteristics show no significant change as a function of excitation energymore » above the fission barrier, despite the fact that an extra ~5 MeV of energy is potentially available in the excited fragments for γ decay. The measured results are compared with model calculations made for prompt γ-ray emission with the fission model code gef. In conclusion, further comparison with previously obtained results from thermal neutron induced fission is made to characterize possible differences arising from using the surrogate (d,p) reaction.« less

Controlling plasmonic properties of epitaxial thin films of indium tin oxide in the near-infrared region

NASA Astrophysics Data System (ADS)

Kamakura, R.; Fujita, K.; Murai, S.; Tanaka, K.

2015-06-01

Epitaxial thin films of indium tin oxide (ITO) were grown on yttria-stabilized zirconia single-crystal substrates by using a pulsed laser deposition to examine their plasmonic properties. The dielectric function of ITO was characterized by spectroscopic ellipsometry. Through the concentration of SnO2 in the target, the carrier concentration in the films was modified, which directly leads to the tuning of the dielectric function in the near-infrared region. Variable-angle reflectance spectroscopy in the Kretschmann geometry shows the dip in the reflection spectrum of p-polarized light corresponding to the excitation of surface plasmon polaritions (SPPs) in the near-infrared region. The excitation wavelength of the SPPs was shifted with changing the dielectric functions of ITO, which is reproduced by the calculation using transfer matrix method.

Multiconfiguration pair-density functional theory investigation of the electronic spectrum of MnO4-

NASA Astrophysics Data System (ADS)

Sharma, Prachi; Truhlar, Donald G.; Gagliardi, Laura

2018-03-01

The electronic spectrum of permanganate ions contains various highly multiconfigurational ligand-to-metal charge transfer states and is notorious for being one of the most challenging systems to be treated by quantum-chemical methods. Here we studied the lowest nine vertical excitation energies using restricted active space second-order perturbation theory (RASPT2) and multiconfiguration pair-density functional theory (MC-PDFT) to test and compare these two theories in computing such a challenging spectrum. The results are compared to literature data, including time-dependent density functional theory, completely renormalized equation-of-motion couple-cluster theory with single and double excitations, symmetry-adapted-cluster configuration interaction, and experimental spectra in the gas phase and solution. Our results show that MC-PDFT accurately predicts the spectrum at a significantly reduced cost as compared to RASPT2.

Multiconfiguration pair-density functional theory investigation of the electronic spectrum of MnO4.

PubMed

Sharma, Prachi; Truhlar, Donald G; Gagliardi, Laura

2018-03-28

The electronic spectrum of permanganate ions contains various highly multiconfigurational ligand-to-metal charge transfer states and is notorious for being one of the most challenging systems to be treated by quantum-chemical methods. Here we studied the lowest nine vertical excitation energies using restricted active space second-order perturbation theory (RASPT2) and multiconfiguration pair-density functional theory (MC-PDFT) to test and compare these two theories in computing such a challenging spectrum. The results are compared to literature data, including time-dependent density functional theory, completely renormalized equation-of-motion couple-cluster theory with single and double excitations, symmetry-adapted-cluster configuration interaction, and experimental spectra in the gas phase and solution. Our results show that MC-PDFT accurately predicts the spectrum at a significantly reduced cost as compared to RASPT2.

Comment on de-averaged back-angle heavy-ion elastic scattering excitation functions

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

Hussein, M.S.; Canto, L.F.; Donangelo, R.

1984-06-01

It is suggested that the de-averaged 180/sup 0/ excitation function of /sup 16/O+ /sup 28/Si, recently considered by Frahn and Kaufmann, is strongly model dependent. Within a multistep ..cap alpha..-transfer description of the back-angle anomaly, we obtain a de-averaged 180/sup 0/ excitation function that exhibits a more regular gross structure.

Fusion enhancement at near and sub-barrier energies in 19O + 12C

DOE PAGES

Singh, Varinderjit; Vadas, J.; Steinbach, T. K.; ...

2016-12-12

Measuring the fusion excitation function for an isotopic chain of projectile nuclei provides a stringent test of a microscopic description of fusion. We report the first measurement of the fusion excitation function at near-barrier energies for the 19O+ 12C system. The measured excitation function is compared with the fusion excitation function of 18O+ 12C. A significant enhancement in the fusion probability of 19O ions with a 12C target as compared to 18O ions is observed. As a result, the experimental cross-sections observed at near-barrier energies are compared with a state-of-the-art microscopic model.

Theoretical studies of electronically excited states

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

Besley, Nicholas A.

2014-10-06

Time-dependent density functional theory is the most widely used quantum chemical method for studying molecules in electronically excited states. However, excited states can also be computed within Kohn-Sham density functional theory by exploiting methods that converge the self-consistent field equations to give excited state solutions. The usefulness of single reference self-consistent field based approaches for studying excited states is demonstrated by considering the calculation of several types of spectroscopy including the infrared spectroscopy of molecules in an electronically excited state, the rovibrational spectrum of the NO-Ar complex, core electron binding energies and the emission spectroscopy of BODIPY in water.

Excitation energies from range-separated time-dependent density and density matrix functional theory.

PubMed

Pernal, Katarzyna

2012-05-14

Time-dependent density functional theory (TD-DFT) in the adiabatic formulation exhibits known failures when applied to predicting excitation energies. One of them is the lack of the doubly excited configurations. On the other hand, the time-dependent theory based on a one-electron reduced density matrix functional (time-dependent density matrix functional theory, TD-DMFT) has proven accurate in determining single and double excitations of H(2) molecule if the exact functional is employed in the adiabatic approximation. We propose a new approach for computing excited state energies that relies on functionals of electron density and one-electron reduced density matrix, where the latter is applied in the long-range region of electron-electron interactions. A similar approach has been recently successfully employed in predicting ground state potential energy curves of diatomic molecules even in the dissociation limit, where static correlation effects are dominating. In the paper, a time-dependent functional theory based on the range-separation of electronic interaction operator is rigorously formulated. To turn the approach into a practical scheme the adiabatic approximation is proposed for the short- and long-range components of the coupling matrix present in the linear response equations. In the end, the problem of finding excitation energies is turned into an eigenproblem for a symmetric matrix. Assignment of obtained excitations is discussed and it is shown how to identify double excitations from the analysis of approximate transition density matrix elements. The proposed method used with the short-range local density approximation (srLDA) and the long-range Buijse-Baerends density matrix functional (lrBB) is applied to H(2) molecule (at equilibrium geometry and in the dissociation limit) and to Be atom. The method accounts for double excitations in the investigated systems but, unfortunately, the accuracy of some of them is poor. The quality of the other excitations is in general much better than that offered by TD-DFT-LDA or TD-DMFT-BB approximations if the range-separation parameter is properly chosen. The latter remains an open problem.

Effects of glutamate, substance P and eledoisin-related peptide on solitary tract neurones involved in respiration and respiratory reflexes.

PubMed

Henry, J L; Sessle, B J

1985-03-01

Recent studies have implicated glutamate and substance P in synaptic transmission in the nuclei tractus solitarii and in central regulation of cardiorespiratory functions. Consequently, in chloralose-anaesthetized cats that were artificially ventilated, we examined the effects of the microiontophoretic application of both chemicals (and the substance P homologue, eledoisin-related peptide) on single neurones of the nuclei tractus solitarii implicated in the control of respiration and respiratory tract reflexes. These neurones were functionally identified as either respiratory neurones or presumed reflex interneurones, and showed functional properties comparable to those previously documented for each of these two types. The iontophoretic application of glutamate produced an excitation of rapid onset in 23 or 25 reflex interneurones tested, but the respiratory neurones showed a differential sensitivity: one type (n = 32) was "glutamate-sensitive" and showed rapid excitation with glutamate applications of less than 30 nA, the other type of respiratory neurone (n = 26) was termed "glutamate-insensitive" since it either showed excitation only with applications of 60 nA or more or showed no response even with currents up to 94 nA. Each neurone studied was clearly of one type or the other. Glutamate could increase the number of spikes per rhythmic burst and the burst duration of respiratory neurones, it facilitated evoked activity in the reflex interneurones and in those respiratory neurones having a superior laryngeal nerve or vagus nerve afferent input, and the magnitude of the excitatory responses to glutamate varied directly with the amount of ejecting current. Substance P and eledoisin-related peptide also had excitatory effects on respiratory neurones and reflex interneurones, but compared with glutamate-induced effects the excitation was slower in onset and more prolonged in after-discharge. Both rhythmic and evoked activity could be facilitated, and the magnitude of the effect varied directly with the magnitude of the ejecting current. In showing that both glutamate and substance P (and its analogue, eledoisin-related peptide) have excitatory effects on the activity of respiratory neurones and reflex interneurones, this study provides evidence suggesting that these neurones have receptors for these neural chemicals, supportive of a role for each chemical in the regulation of respiration and respiratory tract reflexes.

Electronic-structure and quantum dynamical study of the photochromism of the aromatic Schiff base salicylideneaniline

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

Ortiz-Sanchez, Juan Manuel; Gelabert, Ricard; Moreno, Miquel

2008-12-07

The ultrafast proton transfer dynamics of salicylideneaniline has been theoretically analyzed in the ground and first singlet excited electronic states using density functional theory (DFT) and time-dependent DFT calculations, which predict a ({pi},{pi}*) barrierless excited state intramolecular proton transfer (ESIPT). In addition to this, the photochemistry of salicylideneaniline is experimentally known to present fast depopulation processes of the photoexcited species before and after the proton transfer reaction. Such processes are explained by means of conical intersections between the ground and first singlet ({pi},{pi}*) excited electronic states. The electronic energies obtained by the time-dependent density functional theory formalism have been fittedmore » to a monodimensional potential energy surface in order to perform quantum dynamics study of the processes. Our results show that the proton transfer and deactivation of the photoexcited species before the ESIPT processes are completed within 49.6 and 37.7 fs, respectively, which is in remarkable good agreement with experiments.« less

Watching excitons move: the time-dependent transition density matrix

NASA Astrophysics Data System (ADS)

Ullrich, Carsten

2012-02-01

Time-dependent density-functional theory allows one to calculate excitation energies and the associated transition densities in principle exactly. The transition density matrix (TDM) provides additional information on electron-hole localization and coherence of specific excitations of the many-body system. We have extended the TDM concept into the real-time domain in order to visualize the excited-state dynamics in conjugated molecules. The time-dependent TDM is defined as an implicit density functional, and can be approximately obtained from the time-dependent Kohn-Sham orbitals. The quality of this approximation is assessed in simple model systems. A computational scheme for real molecular systems is presented: the time-dependent Kohn-Sham equations are solved with the OCTOPUS code and the time-dependent Kohn-Sham TDM is calculated using a spatial partitioning scheme. The method is applied to show in real time how locally created electron-hole pairs spread out over neighboring conjugated molecular chains. The coupling mechanism, electron-hole coherence, and the possibility of charge separation are discussed.

Resonant photoluminescence studies of carrier localisation in c-plane InGaN/GaN quantum well structures

NASA Astrophysics Data System (ADS)

Blenkhorn, W. E.; Schulz, S.; Tanner, D. S. P.; Oliver, R. A.; Kappers, M. J.; Humphreys, C. J.; Dawson, P.

2018-05-01

In this paper we report on changes in the form of the low temperature (12 K) photoluminescence spectra of an InGaN/GaN quantum well structure as a function of excitation photon energy. As the photon energy is progressively reduced we observe at a critical energy a change in the form of the spectra from one which is determined by the occupation of the complete distribution of hole localisation centres to one which is determined by the resonant excitation of specific localisation sites. This change is governed by an effective mobility edge whereby the photo-excited holes remain localised at their initial energy and are prevented from scattering to other localisation sites. This assignment is confirmed by the results of atomistic tight binding calculations which show that the wave function overlap of the lowest lying localised holes with other hole states is low compared with the overlap of higher lying hole states with other higher lying hole states.

Effects of two-handed task training on upper limb function of chronic hemiplegic patients after stroke

PubMed Central

Yang, Byung Il; Song, Bo Kyoung; Joung, Sang Mi

2017-01-01

[Purpose] The purpose of this study was to determine whether two-handed task training is effective on motor learning of injured cerebral cortex activation and upper extremity function recovery after stroke. [Subjects and Methods] Two hemiplegic subjects participated in this study: one patient was affected on the dominant side of the body and the other was affected on the non-dominant side of the body, and both scored in the range of 58–66 in the Fugl-Meyer assessment. The excitability of the corticospinal tract and Manual Function Test were examined. [Results] The excitability of the corticospinal tract and the Manual Function Test showed significant differences in the activation of both sides of the cerebral cortex and in the variation in learning effect of upper extremity motor function recovery in patients with hemiplegic non-dominant hand (left). [Conclusion] The results suggested that two-handed task training had a different influence on dominant hand (right) and non-dominant hand (left) motor recovery. PMID:28210051

AKAP79/150 impacts intrinsic excitability of hippocampal neurons through phospho-regulation of A-type K+ channel trafficking.

PubMed

Lin, Lin; Sun, Wei; Kung, Faith; Dell'Acqua, Mark L; Hoffman, Dax A

2011-01-26

Kv4.2, as the primary α-subunit of rapidly inactivating, A-type voltage-gated K(+) (Kv) channels expressed in hippocampal CA1 pyramidal dendrites, plays a critical role in regulating their excitability. Activity-dependent trafficking of Kv4.2 relies on C-terminal protein kinase A (PKA) phosphorylation. A-kinase-anchoring proteins (AKAPs) target PKA to glutamate receptor and ion channel complexes to allow for discrete, local signaling. As part of a previous study, we showed that AKAP79/150 interacts with Kv4.2 complexes and that the two proteins colocalize in hippocampal neurons. However, the nature and functional consequence of their interaction has not been previously explored. Here, we report that the C-terminal domain of Kv4.2 interacts with an internal region of AKAP79/150 that overlaps with its MAGUK (membrane-associated guanylate kinase)-binding domain. We show that AKAP79/150-anchored PKA activity controls Kv4.2 surface expression in heterologous cells and hippocampal neurons. Consistent with these findings, disrupting PKA anchoring led to a decrease in neuronal excitability, while preventing dephosphorylation by the phosphatase calcineurin resulted in increased excitability. These results demonstrate that AKAP79/150 provides a platform for dynamic PKA regulation of Kv4.2 expression, fundamentally impacting CA1 excitability.

Calculation of total electron excitation cross-sections and partial electron ionization cross-sections for the elements. Ph.D. Thesis

NASA Technical Reports Server (NTRS)

Green, T. J.

1973-01-01

Computer programs were used to calculate the total electron excitation cross-section for atoms and the partial ionization cross-section. The approximations to the scattering amplitude used are as follows: (1) Born, Bethe, and Modified Bethe for non-exchange excitation; (2) Ochkur for exchange excitation; and (3) Coulomb-Born of non-exchange ionization. The amplitudes are related to the differential cross-sections which are integrated to give the total excitation (or partial ionization) cross-section for the collision. The atomic wave functions used are Hartree-Fock-Slater functions for bound states and the coulomb wave function for the continuum. The programs are presented and the results are examined.

SLEEPLESS is a bi-functional regulator of excitability and cholinergic synaptic transmission

PubMed Central

Wu, Meilin; Robinson, James E.; Joiner, William J.

2014-01-01

Summary Background Although sleep is conserved throughout evolution, the molecular basis of its control is still largely a mystery. We previously showed that the quiver/sleepless (qvr/sss) gene encodes a membrane-tethered protein that is required for normal sleep in Drosophila. SLEEPLESS (SSS) protein functions, at least in part, by upregulating the levels and open probability of Shaker (Sh) potassium channels to suppress neuronal excitability and enable sleep. Consistent with this proposed mechanism, loss-of-function mutations in Sh phenocopy qvr/sss null mutants. However, sleep is more genetically modifiable in Sh than in qvr/sss mutants, suggesting that sss may regulate additional molecules to influence sleep. Results Here we show that SSS also antagonizes nicotinic acetylcholine receptors (nAChRs) to reduce synaptic transmission and promote sleep. Mimicking this antagonism with the nAChR inhibitor mecamylamine or by RNAi knockdown of specific nAChR subunits is sufficient to restore sleep to qvr/sss mutants. Regulation of nAChR activity by SSS occurs post-transcriptionally since the levels of nAChR mRNAs are unchanged in qvr/sss mutants. Regulation of nAChR activity by SSS may in fact be direct, since SSS forms a stable complex with and antagonizes fly nAChR function in transfected cells. Intriguingly, lynx1, a mammalian homolog of SSS, can partially restore normal sleep to qvr/sss mutants, and lynx1 can form stable complexes with Shaker-type channels and nAChRs. Conclusions Together, our data point to an evolutionarily conserved, bi-functional role for SSS and its homologs in controlling excitability and synaptic transmission in fundamental processes of the nervous system such as sleep. PMID:24613312

Transient photothermal spectra of plasmonic nanobubbles.

PubMed

Lukianova-Hleb, Ekaterina Y; Sassaroli, Elisabetta; Jones, Alicia; Lapotko, Dmitri O

2012-03-13

The photothermal efficacy of near-infrared gold nanoparticles (NP), nanoshells, and nanorods was studied under pulsed high-energy optical excitation in plasmonic nanobubble (PNB) mode as a function of the wavelength and duration of the excitation laser pulse. PNBs, transient vapor nanobubbles, were generated around individual and clustered overheated NPs in water and living cells. Transient PNBs showed two photothermal features not previously observed for NPs: the narrowing of the spectral peaks to 1 nm and the strong dependence of the photothermal efficacy upon the duration of the laser pulse. Narrow red-shifted (relative to those of NPs) near-infrared spectral peaks were observed for 70 ps excitation laser pulses, while longer sub- and nanosecond pulses completely suppressed near-infrared peaks and blue shifted the PNB generation to the visual range. Thus, PNBs can provide superior spectral selectivity over gold NPs under specific optical excitation conditions.

Effects of Low-Energy Excitations on Spectral Properties at Higher Binding Energy: The Metal-Insulator Transition of VO2

NASA Astrophysics Data System (ADS)

Gatti, Matteo; Panaccione, Giancarlo; Reining, Lucia

2015-03-01

The effects of electron interaction on spectral properties can be understood in terms of coupling between excitations. In transition-metal oxides, the spectral function close to the Fermi level and low-energy excitations between d states have attracted particular attention. In this work we focus on photoemission spectra of vanadium dioxide over a wide (10 eV) range of binding energies. We show that there are clear signatures of the metal-insulator transition over the whole range due to a cross coupling of the delocalized s and p states with low-energy excitations between the localized d states. This coupling can be understood by advanced calculations based on many-body perturbation theory in the G W approximation. We also advocate the fact that tuning the photon energy up to the hard-x-ray range can help to distinguish fingerprints of correlation from pure band-structure effects.

UV fluorescence excitation imaging of healing of wounds in skin: Evaluation of wound closure in organ culture model.

PubMed

Wang, Ying; Gutierrez-Herrera, Enoch; Ortega-Martinez, Antonio; Anderson, Richard Rox; Franco, Walfre

2016-09-01

Molecules native to tissue that fluoresce upon light excitation can serve as reporters of cellular activity and protein structure. In skin, the fluorescence ascribed to tryptophan is a marker of cellular proliferation, whereas the fluorescence ascribed to cross-links of collagen is a structural marker. In this work, we introduce and demonstrate a simple but robust optical method to image the functional process of epithelialization and the exposed dermal collagen in wound healing of human skin in an organ culture model. Non-closing non-grafted, partial closing non-grafted, and grafted wounds were created in ex vivo human skin and kept in culture. A wide-field UV fluorescence excitation imaging system was used to visualize epithelialization of the exposed dermis and quantitate wound area, closure, and gap. Histology (H&E staining) was also used to evaluate epithelialization. The endogenous fluorescence excitation of cross-links of collagen at 335 nm clearly shows the dermis missing epithelium, while the endogenous fluorescence excitation of tryptophan at 295 nm shows keratinocytes in higher proliferating state. The size of the non-closing wound was 11.4 ± 1.8 mm and remained constant during the observation period, while the partial-close wound reached 65.5 ± 4.9% closure by day 16. Evaluations of wound gaps using fluorescence excitation images and histology images are in agreement. We have established a fluorescence imaging method for studying epithelialization processes, evaluating keratinocyte proliferation, and quantitating closure during wound healing of skin in an organ culture model: the dermal fluorescence of pepsin-digestible collagen cross-links can be used to quantitate wound size, closure extents, and gaps; and, the epidermal fluorescence ascribed to tryptophan can be used to monitor and quantitate functional states of epithelialization. UV fluorescence excitation imaging has the potential to become a valuable tool for research, diagnostic and educational purposes on evaluating the healing of wounds. Lasers Surg. Med. 48:678-685, 2016. © 2016 The Authors. Lasers in Surgery and Medicine Published by Wiley Periodicals, Inc. © 2016 The Authors. Lasers in Surgery and Medicine Published by Wiley Periodicals, Inc.

Excitations in the Yang–Gaudin Bose gas

DOE PAGES

Robinson, Neil J.; Konik, Robert M.

2017-06-01

Here, we study the excitation spectrum of two-component delta-function interacting bosons confined to a single spatial dimension, the Yang–Gaudin Bose gas. We show that there are pronounced finite-size effects in the dispersion relations of excitations, perhaps best illustrated by the spinon single particle dispersion which exhibits a gap at 2k F and a finite-momentum roton-like minimum. Such features occur at energies far above the finite volume excitation gap, vanish slowly as 1/L for fixed spinon number, and can persist to the thermodynamic limit at fixed spinon density. Features such as the 2k F gap also persist to multi-particle excitation continua. Our results show that excitations in the finite system can behave in a qualitatively different manner to analogous excitations in the thermodynamic limit. The Yang–Gaudin Bose gas is also host to multi-spinon bound states, known asmore » $$\\Lambda$$ -strings. We study these excitations both in the thermodynamic limit under the string hypothesis and in finite size systems where string deviations are taken into account. In the zero-temperature limit we present a simple relation between the length n $$\\Lambda$$-string dressed energies $$\\epsilon_n(\\lambda)$$ and the dressed energy $$\\epsilon(k)$$. We solve the Yang–Yang–Takahashi equations numerically and compare to the analytical solution obtained under the strong couple expansion, revealing that the length n $$\\Lambda$$ -string dressed energy is Lorentzian over a wide range of real string centers λ in the vicinity of $$\\lambda = 0$$ . We then examine the finite size effects present in the dispersion of the two-spinon bound states by numerically solving the Bethe ansatz equations with string deviations.« less

An ultrasound transient elastography system with coded excitation.

PubMed

Diao, Xianfen; Zhu, Jing; He, Xiaonian; Chen, Xin; Zhang, Xinyu; Chen, Siping; Liu, Weixiang

2017-06-28

Ultrasound transient elastography technology has found its place in elastography because it is safe and easy to operate. However, it's application in deep tissue is limited. The aim of this study is to design an ultrasound transient elastography system with coded excitation to obtain greater detection depth. The ultrasound transient elastography system requires tissue vibration to be strictly synchronous with ultrasound detection. Therefore, an ultrasound transient elastography system with coded excitation was designed. A central component of this transient elastography system was an arbitrary waveform generator with multi-channel signals output function. This arbitrary waveform generator was used to produce the tissue vibration signal, the ultrasound detection signal and the synchronous triggering signal of the radio frequency data acquisition system. The arbitrary waveform generator can produce different forms of vibration waveform to induce different shear wave propagation in the tissue. Moreover, it can achieve either traditional pulse-echo detection or a phase-modulated or a frequency-modulated coded excitation. A 7-chip Barker code and traditional pulse-echo detection were programmed on the designed ultrasound transient elastography system to detect the shear wave in the phantom excited by the mechanical vibrator. Then an elasticity QA phantom and sixteen in vitro rat livers were used for performance evaluation of the two detection pulses. The elasticity QA phantom's results show that our system is effective, and the rat liver results show the detection depth can be increased more than 1 cm. In addition, the SNR (signal-to-noise ratio) is increased by 15 dB using the 7-chip Barker coded excitation. Applying 7-chip Barker coded excitation technique to the ultrasound transient elastography can increase the detection depth and SNR. Using coded excitation technology to assess the human liver, especially in obese patients, may be a good choice.

Characterization of Different Types of Excitability in Large Somatosensory Neurons and Its Plastic Changes in Pathological Pain States

PubMed Central

Xie, Rou-Gang; Chu, Wen-Guang; Hu, San-Jue; Luo, Ceng

2018-01-01

Sensory neuron types have been distinguished by distinct morphological and transcriptional characteristics. Excitability is the most fundamental functional feature of neurons. Mathematical models described by Hodgkin have revealed three types of neuronal excitability based on the relationship between firing frequency and applied current intensity. However, whether natural sensory neurons display different functional characteristics in terms of excitability and whether this excitability type undergoes plastic changes under pathological pain states have remained elusive. Here, by utilizing whole-cell patch clamp recordings, behavioral and pharmacological assays, we demonstrated that large dorsal root ganglion (DRG) neurons can be classified into three classes and four subclasses based on their excitability patterns, which is similar to mathematical models raised by Hodgkin. Analysis of hyperpolarization-activated cation current (Ih) revealed different magnitude of Ih in different excitability types of large DRG neurons, with higher Ih in Class 2-1 than that in Class 1, 2-2 and 3. This indicates a crucial role of Ih in the determination of excitability type of large DRG neurons. More importantly, this pattern of excitability displays plastic changes and transition under pathological pain states caused by peripheral nerve injury. This study sheds new light on the functional characteristics of large DRG neurons and extends functional classification of large DRG neurons by integration of transcriptomic and morphological characteristics. PMID:29303989

sp-d Exchange Interactions in Wave Function Engineered Colloidal CdSe/Mn:CdS Hetero-Nanoplatelets.

PubMed

Muckel, Franziska; Delikanli, Savas; Hernández-Martínez, Pedro Ludwig; Priesner, Tamara; Lorenz, Severin; Ackermann, Julia; Sharma, Manoj; Demir, Hilmi Volkan; Bacher, Gerd

2018-03-14

In two-dimensional (2D) colloidal semiconductor nanoplatelets, which are atomically flat nanocrystals, the precise control of thickness and composition on the atomic scale allows for the synthesis of heterostructures with well-defined electron and hole wave function distributions. Introducing transition metal dopants with a monolayer precision enables tailored magnetic exchange interactions between dopants and band states. Here, we use the absorption based technique of magnetic circular dichroism (MCD) to directly prove the exchange coupling of magnetic dopants with the band charge carriers in hetero-nanoplatelets with CdSe core and manganese-doped CdS shell (CdSe/Mn:CdS). We show that the strength of both the electron as well as the hole exchange interactions with the dopants can be tuned by varying the nanoplatelets architecture with monolayer accuracy. As MCD is highly sensitive for excitonic resonances, excited level spectroscopy allows us to resolve and identify, in combination with wave function calculations, several excited state transitions including spin-orbit split-off excitonic contributions. Thus, our study not only demonstrates the possibility to expand the extraordinary physical properties of colloidal nanoplatelets toward magneto-optical functionality by transition metal doping but also provides an insight into the excited state electronic structure in this novel two-dimensional material.

Physical Meaning of Virtual Kohn-Sham Orbitals and Orbital Energies: An Ideal Basis for the Description of Molecular Excitations.

PubMed

van Meer, R; Gritsenko, O V; Baerends, E J

2014-10-14

In recent years, several benchmark studies on the performance of large sets of functionals in time-dependent density functional theory (TDDFT) calculations of excitation energies have been performed. The tested functionals do not approximate exact Kohn-Sham orbitals and orbital energies closely. We highlight the advantages of (close to) exact Kohn-Sham orbitals and orbital energies for a simple description, very often as just a single orbital-to-orbital transition, of molecular excitations. Benchmark calculations are performed for the statistical average of orbital potentials (SAOP) functional for the potential [J. Chem. Phys. 2000, 112, 1344; 2001, 114, 652], which approximates the true Kohn-Sham potential much better than LDA, GGA, mGGA, and hybrid potentials do. An accurate Kohn-Sham potential does not only perform satisfactorily for calculated vertical excitation energies of both valence and Rydberg transitions but also exhibits appealing properties of the KS orbitals including occupied orbital energies close to ionization energies, virtual-occupied orbital energy gaps very close to excitation energies, realistic shapes of virtual orbitals, leading to straightforward interpretation of most excitations as single orbital transitions. We stress that such advantages are completely lost in time-dependent Hartree-Fock and partly in hybrid approaches. Many excitations and excitation energies calculated with local density, generalized gradient, and hybrid functionals are spurious. There is, with an accurate KS, or even the LDA or GGA potentials, nothing problematic about the "band gap" in molecules: the HOMO-LUMO gap is close to the first excitation energy (the optical gap).

Influence of Force Fields and Quantum Chemistry Approach on Spectral Densities of BChl a in Solution and in FMO Proteins

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

Chandrasekaran, Suryanarayanan; Aghtar, Mortaza; Valleau, Stéphanie

2015-08-06

Studies on light-harvesting (LH) systems have attracted much attention after the finding of long-lived quantum coherences in the exciton dynamics of the Fenna–Matthews–Olson (FMO) complex. In this complex, excitation energy transfer occurs between the bacteriochlorophyll a (BChl a) pigments. Two quantum mechanics/molecular mechanics (QM/MM) studies, each with a different force-field and quantum chemistry approach, reported different excitation energy distributions for the FMO complex. To understand the reasons for these differences in the predicted excitation energies, we have carried out a comparative study between the simulations using the CHARMM and AMBER force field and the Zerner intermediate neglect of differential orbitalmore » (ZINDO)/S and time-dependent density functional theory (TDDFT) quantum chemistry methods. The calculations using the CHARMM force field together with ZINDO/S or TDDFT always show a wider spread in the energy distribution compared to those using the AMBER force field. High- or low-energy tails in these energy distributions result in larger values for the spectral density at low frequencies. A detailed study on individual BChl a molecules in solution shows that without the environment, the density of states is the same for both force field sets. Including the environmental point charges, however, the excitation energy distribution gets broader and, depending on the applied methods, also asymmetric. The excitation energy distribution predicted using TDDFT together with the AMBER force field shows a symmetric, Gaussian-like distribution.« less

Osteogenic and chondrogenic master genes expression is dependent on the Kir2.1 potassium channel through the bone morphogenetic protein pathway.

PubMed

Pini, Jonathan; Giuliano, Serena; Matonti, Julia; Simkin, Dina; Rouleau, Matthieu; Bendahhou, Saïd

2018-05-29

Andersen's syndrome is a rare disorder affecting muscle, heart, and bone, that is associated with mutations leading to a loss of function of the inwardly rectifying K + channel Kir2.1. While the Kir2.1 function can be anticipated in excitable cells by controlling the electrical activity, its role in non-excitable cells remains to be investigated. Using Andersen's syndrome induced Pluripotent Stem cells, we investigated the cellular and molecular events during the osteoblastic and chondrogenic differentiation that are affected by the loss of the Ik1 current. We show that loss of Kir2.1 channel function impairs both osteoblastic and chondrogenic processes through the down regulation master gene expression. This down regulation is due to an impairment of the bone morphogenetic proteins signaling pathway through de-phosphorylation of the Smad proteins. Restoring Kir2.1 channel function in Andersen's syndrome cells rescued master genes expression, and restored normal osteoblasts and chondrocytes behavior. Our results show that Kir2.1-mediated activity controls endochondral and intramembranous ossification signaling pathways. This article is protected by copyright. All rights reserved. This article is protected by copyright. All rights reserved.

Simulation of femtosecond two-dimensional electronic spectra of conical intersections

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

Krčmář, Jindřich; Gelin, Maxim F.; Domcke, Wolfgang

2015-08-21

We have simulated femtosecond two-dimensional (2D) electronic spectra for an excited-state conical intersection using the wave-function version of the equation-of-motion phase-matching approach. We show that 2D spectra at fixed values of the waiting time provide information on the structure of the vibronic eigenstates of the conical intersection, while the evolution of the spectra with the waiting time reveals predominantly ground-state wave-packet dynamics. The results show that 2D spectra of conical intersection systems differ significantly from those obtained for chromophores with well separated excited-state potential-energy surfaces. The spectral signatures which can be attributed to conical intersections are discussed.

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

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

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

2014-09-14

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

Synthesis and functionalization of monodisperse near-ultraviolet and visible excitable multifunctional Eu3+, Bi3+:REVO4 nanophosphors for bioimaging and biosensing applications

NASA Astrophysics Data System (ADS)

Escudero, Alberto; Carrillo-Carrión, Carolina; Zyuzin, Mikhail V.; Ashraf, Sumaira; Hartmann, Raimo; Núñez, Nuria O.; Ocaña, Manuel; Parak, Wolfgang J.

2016-06-01

Near-ultraviolet and visible excitable Eu- and Bi-doped NPs based on rare earth vanadates (REVO4, RE = Y, Gd) have been synthesized by a facile route from appropriate RE precursors, europium and bismuth nitrate, and sodium orthovanadate, by homogeneous precipitation in an ethylene glycol/water mixture at 120 °C. The NPs can be functionalized either by a one-pot synthesis with polyacrylic acid (PAA) or by a Layer-by-Layer approach with poly(allylamine hydrochloride) (PAH) and PAA. In the first case, the particle size can also be tuned by adjusting the amount of PAA. The Eu- Bi-doped REVO4 based nanophosphors show the typical red luminescence of Eu(iii), which can be excited through an energy transfer process from the vanadate anions, resulting in a much higher luminescence intensity in comparison to the direct excitation of the europium cations. The incorporation of Bi into the REVO4 structure shifts the original absorption band of the vanadate anions towards longer wavelengths, giving rise to nanophosphors with an excitation maximum at 342 nm, which can also be excited in the visible range. The suitability of such nanophosphors for bioimaging and biosensing applications, as well as their colloidal stability in different buffer media of biological interest, their cytotoxicity, their degradability at low pH, and their uptake by HeLa cells have been evaluated. Their suitability for bioimaging and biosensing applications is also demonstrated.Near-ultraviolet and visible excitable Eu- and Bi-doped NPs based on rare earth vanadates (REVO4, RE = Y, Gd) have been synthesized by a facile route from appropriate RE precursors, europium and bismuth nitrate, and sodium orthovanadate, by homogeneous precipitation in an ethylene glycol/water mixture at 120 °C. The NPs can be functionalized either by a one-pot synthesis with polyacrylic acid (PAA) or by a Layer-by-Layer approach with poly(allylamine hydrochloride) (PAH) and PAA. In the first case, the particle size can also be tuned by adjusting the amount of PAA. The Eu- Bi-doped REVO4 based nanophosphors show the typical red luminescence of Eu(iii), which can be excited through an energy transfer process from the vanadate anions, resulting in a much higher luminescence intensity in comparison to the direct excitation of the europium cations. The incorporation of Bi into the REVO4 structure shifts the original absorption band of the vanadate anions towards longer wavelengths, giving rise to nanophosphors with an excitation maximum at 342 nm, which can also be excited in the visible range. The suitability of such nanophosphors for bioimaging and biosensing applications, as well as their colloidal stability in different buffer media of biological interest, their cytotoxicity, their degradability at low pH, and their uptake by HeLa cells have been evaluated. Their suitability for bioimaging and biosensing applications is also demonstrated. Electronic supplementary information (ESI) available: Additional details of experiments and results (NP characterization, NPs' uptake and imaging). See DOI: 10.1039/c6nr03369e

Interacting Genes Required for Pharyngeal Excitation by Motor Neuron Mc in Caenorhabditis Elegans

PubMed Central

Raizen, D. M.; Lee, RYN.; Avery, L.

1995-01-01

We studied the control of pharyngeal excitation in Caenorhabditis elegans. By laser ablating subsets of the pharyngeal nervous system, we found that the MC neuron type is necessary and probably sufficient for rapid pharyngeal pumping. Electropharyngeograms showed that MC transmits excitatory postsynaptic potentials, suggesting that MC acts as a neurogenic pacemaker for pharyngeal pumping. Mutations in genes required for acetylcholine (ACh) release and an antagonist of the nicotinic ACh receptor (nAChR) reduced pumping rates, suggesting that a nAChR is required for MC transmission. To identify genes required for MC neurotransmission, we screened for mutations that cause slow pumping but no other defects. Mutations in two genes, eat-2 and eat-18, eliminated MC neurotransmission. A gain-of-function eat-18 mutation, ad820sd, and a putative loss-of-function eat-18 mutation, ad1110, both reduced the excitation of pharyngeal muscle in response to the nAChR agonists nicotine and carbachol, suggesting that eat-18 is required for the function of a pharyngeal nAChR. Fourteen recessive mutations in eat-2 fell into five complementation classes. We found allele-specific genetic interactions between eat-2 and eat-18 that correlated with complementation classes of eat-2. We propose that eat-18 and eat-2 function in a multisubunit protein complex involved in the function of a pharyngeal nAChR. PMID:8601480

Profilin2 contributes to synaptic vesicle exocytosis, neuronal excitability, and novelty-seeking behavior

PubMed Central

Pilo Boyl, Pietro; Di Nardo, Alessia; Mulle, Christophe; Sassoè-Pognetto, Marco; Panzanelli, Patrizia; Mele, Andrea; Kneussel, Matthias; Costantini, Vivian; Perlas, Emerald; Massimi, Marzia; Vara, Hugo; Giustetto, Maurizio; Witke, Walter

2007-01-01

Profilins are actin binding proteins essential for regulating cytoskeletal dynamics, however, their function in the mammalian nervous system is unknown. Here, we provide evidence that in mouse brain profilin1 and profilin2 have distinct roles in regulating synaptic actin polymerization with profilin2 preferring a WAVE-complex-mediated pathway. Mice lacking profilin2 show a block in synaptic actin polymerization in response to depolarization, which is accompanied by increased synaptic excitability of glutamatergic neurons due to higher vesicle exocytosis. These alterations in neurotransmitter release correlate with a hyperactivation of the striatum and enhanced novelty-seeking behavior in profilin2 mutant mice. Our results highlight a novel, profilin2-dependent pathway, regulating synaptic physiology, neuronal excitability, and complex behavior. PMID:17541406

Improving the precision of linear optics measurements based on turn-by-turn beam position monitor data after a pulsed excitation in lepton storage rings

NASA Astrophysics Data System (ADS)

Malina, L.; Coello de Portugal, J.; Persson, T.; Skowroński, P. K.; Tomás, R.; Franchi, A.; Liuzzo, S.

2017-08-01

Beam optics control is of critical importance for machine performance and protection. Nowadays, turn-by-turn (TbT) beam position monitor (BPM) data are increasingly exploited as they allow for fast and simultaneous measurement of various optics quantities. Nevertheless, so far the best documented uncertainty of measured β -functions is of about 10‰ rms. In this paper we compare the β -functions of the ESRF storage ring measured from two different TbT techniques—the N-BPM and the Amplitude methods—with the ones inferred from a measurement of the orbit response matrix (ORM). We show how to improve the precision of TbT techniques by refining the Fourier transform of TbT data with properly chosen excitation amplitude. The precision of the N-BPM method is further improved by refining the phase advance measurement. This represents a step forward compared to standard TbT measurements. First experimental results showing the precision of β -functions pushed down to 4‰ both in TbT and ORM techniques are reported and commented.

Transfer couplings and hindrance far below the barrier for 40 Ca + 96 Zr

DOE PAGES

Stefanini, A. M.; Montagnoli, G.; Esbensen, H.; ...

2015-01-29

The sub-barrier fusion excitation function of 40Ca + 96Zr has been measured down to cross sections ≃2.4µb, i.e. two orders of magnitude smaller than obtained in the previous experiment, where the sub-barrier fusion of this system was found to be greatly enhanced with respect to 40Ca + 90Zr, and the need of coupling to transfer channels was suggested. The purpose of this work was to investigate the behavior of 40Ca + 96Zr fusion far below the barrier. The smooth trend of the excitation function has been found to continue, and the logarithmic slope increases very slowly. No indication of hindrancemore » shows up, and a comparison with 48Ca + 96Zr is very useful in this respect. A new CC analysis of the complete excitation function has been performed, including explicitly one- and two-nucleon Q >0 transfer channels. Such transfer couplings bring significant cross section enhancements, even at the level of a few µb. Locating the hindrance threshold, if any, in 40Ca + 96Zr would require challenging measurements of cross sections in the sub-µb range.« less

Spin excitations in the deformed nuclei 154Sm, 158Gd and 168Er

NASA Astrophysics Data System (ADS)

Frekers, D.; Wörtche, H. J.; Richter, A.; Abegg, R.; Azuma, R. E.; Celler, A.; Chan, C.; Drake, T. E.; Helmer, R.; Jackson, K. P.; King, J. D.; Miller, C. A.; Schubank, R.; Vetterli, M. C.; Yen, S.

1990-07-01

An intermediate energy proton scattering experiment has been performed to probe spin excitation in the deformed rare earth nuclei 154Sm, 158Gd and 168Er for energies up to 12 MeV. A concentration of spin M1 strength is observed between 6 and 10MeV with a total strength of about 11 μN2 independent of the nucleus. The strength function shows two distinct structures separated by about 2.5 MeV and each having a width of about 2 MeV.

Violation of the zero-force theorem in the time-dependent Krieger-Li-Iafrate approximation

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

Mundt, Michael; Kuemmel, Stephan; Leeuwen, Robert van

2007-05-15

We demonstrate that the time-dependent Krieger-Li-Iafrate approximation in combination with the exchange-only functional violates the zero-force theorem. By analyzing the time-dependent dipole moment of Na{sub 5} and Na{sub 9}{sup +}, we furthermore show that this can lead to an unphysical self-excitation of the system depending on the system properties and the excitation strength. Analytical aspects, especially the connection between the zero-force theorem and the generalized-translation invariance of the potential, are discussed.

System and method for characterizing voiced excitations of speech and acoustic signals, removing acoustic noise from speech, and synthesizing speech

DOEpatents

Burnett, Greg C [Livermore, CA; Holzrichter, John F [Berkeley, CA; Ng, Lawrence C [Danville, CA

2006-08-08

The present invention is a system and method for characterizing human (or animate) speech voiced excitation functions and acoustic signals, for removing unwanted acoustic noise which often occurs when a speaker uses a microphone in common environments, and for synthesizing personalized or modified human (or other animate) speech upon command from a controller. A low power EM sensor is used to detect the motions of windpipe tissues in the glottal region of the human speech system before, during, and after voiced speech is produced by a user. From these tissue motion measurements, a voiced excitation function can be derived. Further, the excitation function provides speech production information to enhance noise removal from human speech and it enables accurate transfer functions of speech to be obtained. Previously stored excitation and transfer functions can be used for synthesizing personalized or modified human speech. Configurations of EM sensor and acoustic microphone systems are described to enhance noise cancellation and to enable multiple articulator measurements.

System and method for characterizing voiced excitations of speech and acoustic signals, removing acoustic noise from speech, and synthesizing speech

DOEpatents

Burnett, Greg C.; Holzrichter, John F.; Ng, Lawrence C.

2004-03-23

The present invention is a system and method for characterizing human (or animate) speech voiced excitation functions and acoustic signals, for removing unwanted acoustic noise which often occurs when a speaker uses a microphone in common environments, and for synthesizing personalized or modified human (or other animate) speech upon command from a controller. A low power EM sensor is used to detect the motions of windpipe tissues in the glottal region of the human speech system before, during, and after voiced speech is produced by a user. From these tissue motion measurements, a voiced excitation function can be derived. Further, the excitation function provides speech production information to enhance noise removal from human speech and it enables accurate transfer functions of speech to be obtained. Previously stored excitation and transfer functions can be used for synthesizing personalized or modified human speech. Configurations of EM sensor and acoustic microphone systems are described to enhance noise cancellation and to enable multiple articulator measurements.

System and method for characterizing voiced excitations of speech and acoustic signals, removing acoustic noise from speech, and synthesizing speech

DOEpatents

Burnett, Greg C.; Holzrichter, John F.; Ng, Lawrence C.

2006-02-14

The present invention is a system and method for characterizing human (or animate) speech voiced excitation functions and acoustic signals, for removing unwanted acoustic noise which often occurs when a speaker uses a microphone in common environments, and for synthesizing personalized or modified human (or other animate) speech upon command from a controller. A low power EM sensor is used to detect the motions of windpipe tissues in the glottal region of the human speech system before, during, and after voiced speech is produced by a user. From these tissue motion measurements, a voiced excitation function can be derived. Further, the excitation function provides speech production information to enhance noise removal from human speech and it enables accurate transfer functions of speech to be obtained. Previously stored excitation and transfer functions can be used for synthesizing personalized or modified human speech. Configurations of EM sensor and acoustic microphone systems are described to enhance noise cancellation and to enable multiple articulator measurements.

System And Method For Characterizing Voiced Excitations Of Speech And Acoustic Signals, Removing Acoustic Noise From Speech, And Synthesizi

DOEpatents

Burnett, Greg C.; Holzrichter, John F.; Ng, Lawrence C.

2006-04-25

The present invention is a system and method for characterizing human (or animate) speech voiced excitation functions and acoustic signals, for removing unwanted acoustic noise which often occurs when a speaker uses a microphone in common environments, and for synthesizing personalized or modified human (or other animate) speech upon command from a controller. A low power EM sensor is used to detect the motions of windpipe tissues in the glottal region of the human speech system before, during, and after voiced speech is produced by a user. From these tissue motion measurements, a voiced excitation function can be derived. Further, the excitation function provides speech production information to enhance noise removal from human speech and it enables accurate transfer functions of speech to be obtained. Previously stored excitation and transfer functions can be used for synthesizing personalized or modified human speech. Configurations of EM sensor and acoustic microphone systems are described to enhance noise cancellation and to enable multiple articulator measurements.

Inferring muscle functional roles of the ostrich pelvic limb during walking and running using computer optimization.

PubMed

Rankin, Jeffery W; Rubenson, Jonas; Hutchinson, John R

2016-05-01

Owing to their cursorial background, ostriches (Struthio camelus) walk and run with high metabolic economy, can reach very fast running speeds and quickly execute cutting manoeuvres. These capabilities are believed to be a result of their ability to coordinate muscles to take advantage of specialized passive limb structures. This study aimed to infer the functional roles of ostrich pelvic limb muscles during gait. Existing gait data were combined with a newly developed musculoskeletal model to generate simulations of ostrich walking and running that predict muscle excitations, force and mechanical work. Consistent with previous avian electromyography studies, predicted excitation patterns showed that individual muscles tended to be excited primarily during only stance or swing. Work and force estimates show that ostrich gaits are partially hip-driven with the bi-articular hip-knee muscles driving stance mechanics. Conversely, the knee extensors acted as brakes, absorbing energy. The digital extensors generated large amounts of both negative and positive mechanical work, with increased magnitudes during running, providing further evidence that ostriches make extensive use of tendinous elastic energy storage to improve economy. The simulations also highlight the need to carefully consider non-muscular soft tissues that may play a role in ostrich gait. © 2016 The Authors.

Derivation of the RPA (Random Phase Approximation) Equation of ATDDFT (Adiabatic Time Dependent Density Functional Ground State Response Theory) from an Excited State Variational Approach Based on the Ground State Functional.

PubMed

Ziegler, Tom; Krykunov, Mykhaylo; Autschbach, Jochen

2014-09-09

The random phase approximation (RPA) equation of adiabatic time dependent density functional ground state response theory (ATDDFT) has been used extensively in studies of excited states. It extracts information about excited states from frequency dependent ground state response properties and avoids, thus, in an elegant way, direct Kohn-Sham calculations on excited states in accordance with the status of DFT as a ground state theory. Thus, excitation energies can be found as resonance poles of frequency dependent ground state polarizability from the eigenvalues of the RPA equation. ATDDFT is approximate in that it makes use of a frequency independent energy kernel derived from the ground state functional. It is shown in this study that one can derive the RPA equation of ATDDFT from a purely variational approach in which stationary states above the ground state are located using our constricted variational DFT (CV-DFT) method and the ground state functional. Thus, locating stationary states above the ground state due to one-electron excitations with a ground state functional is completely equivalent to solving the RPA equation of TDDFT employing the same functional. The present study is an extension of a previous work in which we demonstrated the equivalence between ATDDFT and CV-DFT within the Tamm-Dancoff approximation.

Daily iTBS worsens hand motor training--a combined TMS, fMRI and mirror training study.

PubMed

Läppchen, C H; Ringer, T; Blessin, J; Schulz, K; Seidel, G; Lange, R; Hamzei, F

2015-02-15

Repetitive transcranial magnetic stimulation (rTMS) is used to increase regional excitability to improve motor function in combination with training after neurological diseases or events such as stroke. We investigated whether a daily application of intermittent theta burst stimulation (iTBS; a short-duration rTMS that increases regional excitability) improves the training effect compared with sham stimulation in association with a four-day hand training program using a mirror (mirror training, MT). The right dorsal premotor cortex (dPMC right) was chosen as the target region for iTBS because this region has recently been emphasized as a node within a network related to MT. Healthy subjects were randomized into the iTBS group or sham group (control group CG). In the iTBS group, iTBS was applied daily over dPMC right, which was functionally determined in an initial fMRI session prior to starting MT. MT involved 20 min of hand training daily in a mirror over four days. The hand tests, the intracortical excitability and fMRI were evaluated prior to and at the end of MT. The results of the hand training tests of the iTBS group were surprisingly significantly poorer compared with those from the CG group. Both groups showed a different course of excitability in both M1 and a different course of fMRI activation within the supplementary motor area and M1 left. We suggest the inter-regional functional balance was affected by daily iTBS over dPMC right. Maybe an inter-regional connectivity within a network is differentially balanced. An excitability increase within an inhibitory-balanced network would therefore disturb the underlying network. Copyright © 2014 Elsevier Inc. All rights reserved.

Rotation of a Single Acetylene Molecule on Cu(001) by Tunneling Electrons in STM

NASA Astrophysics Data System (ADS)

Shchadilova, Yulia E.; Tikhodeev, Sergei G.; Paulsson, Magnus; Ueba, Hiromu

2013-11-01

We study the elementary processes behind one of the pioneering works on scanning tunneling microscope controlled reactions of single molecules [Stipe et al., Phys. Rev. Lett. 81, 1263 (1998)]. Using the Keldysh-Green function approach for the vibrational generation rate in combination with density functional theory calculations to obtain realistic parameters we reproduce the experimental rotation rate of an acetylene molecule on a Cu(100) surface as a function of bias voltage and tunneling current. This combined approach allows us to identify the reaction coordinate mode of the acetylene rotation and its anharmonic coupling with the C-H stretch mode. We show that three different elementary processes, the excitation of C-H stretch, the overtone ladder climbing of the hindered rotational mode, and the combination band excitation together explain the rotation of the acetylene molecule on Cu(100).

Efficient time-dependent density functional theory approximations for hybrid density functionals: analytical gradients and parallelization.

PubMed

Petrenko, Taras; Kossmann, Simone; Neese, Frank

2011-02-07

In this paper, we present the implementation of efficient approximations to time-dependent density functional theory (TDDFT) within the Tamm-Dancoff approximation (TDA) for hybrid density functionals. For the calculation of the TDDFT/TDA excitation energies and analytical gradients, we combine the resolution of identity (RI-J) algorithm for the computation of the Coulomb terms and the recently introduced "chain of spheres exchange" (COSX) algorithm for the calculation of the exchange terms. It is shown that for extended basis sets, the RIJCOSX approximation leads to speedups of up to 2 orders of magnitude compared to traditional methods, as demonstrated for hydrocarbon chains. The accuracy of the adiabatic transition energies, excited state structures, and vibrational frequencies is assessed on a set of 27 excited states for 25 molecules with the configuration interaction singles and hybrid TDDFT/TDA methods using various basis sets. Compared to the canonical values, the typical error in transition energies is of the order of 0.01 eV. Similar to the ground-state results, excited state equilibrium geometries differ by less than 0.3 pm in the bond distances and 0.5° in the bond angles from the canonical values. The typical error in the calculated excited state normal coordinate displacements is of the order of 0.01, and relative error in the calculated excited state vibrational frequencies is less than 1%. The errors introduced by the RIJCOSX approximation are, thus, insignificant compared to the errors related to the approximate nature of the TDDFT methods and basis set truncation. For TDDFT/TDA energy and gradient calculations on Ag-TB2-helicate (156 atoms, 2732 basis functions), it is demonstrated that the COSX algorithm parallelizes almost perfectly (speedup ~26-29 for 30 processors). The exchange-correlation terms also parallelize well (speedup ~27-29 for 30 processors). The solution of the Z-vector equations shows a speedup of ~24 on 30 processors. The parallelization efficiency for the Coulomb terms can be somewhat smaller (speedup ~15-25 for 30 processors), but their contribution to the total calculation time is small. Thus, the parallel program completes a Becke3-Lee-Yang-Parr energy and gradient calculation on the Ag-TB2-helicate in less than 4 h on 30 processors. We also present the necessary extension of the Lagrangian formalism, which enables the calculation of the TDDFT excited state properties in the frozen-core approximation. The algorithms described in this work are implemented into the ORCA electronic structure system.

Low-lying excited states by constrained DFT

NASA Astrophysics Data System (ADS)

Ramos, Pablo; Pavanello, Michele

2018-04-01

Exploiting the machinery of Constrained Density Functional Theory (CDFT), we propose a variational method for calculating low-lying excited states of molecular systems. We dub this method eXcited CDFT (XCDFT). Excited states are obtained by self-consistently constraining a user-defined population of electrons, Nc, in the virtual space of a reference set of occupied orbitals. By imposing this population to be Nc = 1.0, we computed the first excited state of 15 molecules from a test set. Our results show that XCDFT achieves an accuracy in the predicted excitation energy only slightly worse than linear-response time-dependent DFT (TDDFT), but without incurring into problems of variational collapse typical of the more commonly adopted ΔSCF method. In addition, we selected a few challenging processes to test the limits of applicability of XCDFT. We find that in contrast to TDDFT, XCDFT is capable of reproducing energy surfaces featuring conical intersections (azobenzene and H3) with correct topology and correct overall energetics also away from the intersection. Venturing to condensed-phase systems, XCDFT reproduces the TDDFT solvatochromic shift of benzaldehyde when it is embedded by a cluster of water molecules. Thus, we find XCDFT to be a competitive method among single-reference methods for computations of excited states in terms of time to solution, rate of convergence, and accuracy of the result.

Tuning Ag29 nanocluster light emission from red to blue with one and two-photon excitation.

PubMed

Russier-Antoine, Isabelle; Bertorelle, Franck; Hamouda, Ramzi; Rayane, Driss; Dugourd, Philippe; Sanader, Željka; Bonačić-Koutecký, Vlasta; Brevet, Pierre-François; Antoine, Rodolphe

2016-02-07

We demonstrate that the tuning of the light emission from red to blue in dihydrolipoic acid (DHLA) capped Ag29 nanoclusters can be trigged with one and two photon excitations. The cluster stoichiometry was determined with mass spectrometry and found to be Ag29(DHLA)12. In a detailed optical investigation, we show that these silver nanoclusters exhibit a strong red photoluminescence visible to the naked eye and characterized by a quantum yield of nearly ∼2% upon one-photon excitation. In the nonlinear optical (NLO) study of the properties of the clusters, the two-photon excited fluorescence spectra were recorded and their first hyperpolarizability obtained. The two-photon absorption cross-section at ∼800 nm for Ag29(DHLA)12 is higher than 10(4) GM and the hyperpolarizability is 106 × 10(-30) esu at the same excitation wavelength. The two-photon excited fluorescence spectrum appears strongly blue-shifted as compared to the one-photon excited spectrum, displaying a broad band between 400 and 700 nm. The density functional theory (DFT) provides insight into the structural and electronic properties of Ag29(DHLA)12 as well as into interplay between metallic subunit or core and ligands which is responsible for unique optical properties.

Nonequilibrium excitations and transport of Dirac electrons in electric-field-driven graphene

NASA Astrophysics Data System (ADS)

Li, Jiajun; Han, Jong E.

2018-05-01

We investigate nonequilibrium excitations and charge transport in charge-neutral graphene driven with dc electric field by using the nonequilibrium Green's-function technique. Due to the vanishing Fermi surface, electrons are subject to nontrivial nonequilibrium excitations such as highly anisotropic momentum distribution of electron-hole pairs, an analog of the Schwinger effect. We show that the electron-hole excitations, initiated by the Landau-Zener tunneling with a superlinear I V relation I ∝E3 /2 , reaches a steady state dominated by the dissipation due to optical phonons, resulting in a marginally sublinear I V with I ∝E , in agreement with recent experiments. The linear I V starts to show the sign of current saturation as the graphene is doped away from the Dirac point, and recovers the semiclassical relation for the saturated velocity. We give a detailed discussion on the nonequilibrium charge creation and the relation between the electron-phonon scattering rate and the electric field in the steady-state limit. We explain how the apparent Ohmic I V is recovered near the Dirac point. We propose a mechanism where the peculiar nonequilibrium electron-hole creation can be utilized in a infrared device.

Depth-dependent autofluorescence photobleaching using 325, 473, 633, and 785 nm of porcine ear skin ex vivo

NASA Astrophysics Data System (ADS)

Schleusener, Johannes; Lademann, Jürgen; Darvin, Maxim E.

2017-09-01

Autofluorescence photobleaching describes the decrease of fluorescence intensity of endogenous fluorophores in biological tissue upon light irradiation. The origin of autofluorescence photobleaching is not fully understood. In the skin, the spatial distribution of various endogenous fluorophores varies within the skin layers. Most endogenous fluorophores are excited in the ultraviolet and short visible wavelength range, and only a few, such as porphyrins (red) and melanin (near-infrared), are excited at longer wavelengths. The excitation wavelength- and depth-dependent irradiation of skin will therefore excite different fluorophores, which will likely influence the photobleaching characteristics. The autofluorescence photobleaching of porcine ear skin has been measured ex vivo using 325, 473, 633, and 785 nm excitation at different skin depths from the surface to the dermis at 150 μm. Confocal Raman microscopes were used to achieve sufficient spatial resolution of the measurements. The autofluorescence area under the curve was measured for 21 consecutive acquisitions of 15 s. In all cases, the photobleaching follows a two-exponential decay function approximated by nonlinear regression. The results show that photobleaching can be applied to improve the signal-to-noise ratio in Raman spectroscopy for all of the applied excitation wavelengths and skin depths.

Quantification of Na+,K+ pumps and their transport rate in skeletal muscle: Functional significance

PubMed Central

2013-01-01

During excitation, muscle cells gain Na+ and lose K+, leading to a rise in extracellular K+ ([K+]o), depolarization, and loss of excitability. Recent studies support the idea that these events are important causes of muscle fatigue and that full use of the Na+,K+-ATPase (also known as the Na+,K+ pump) is often essential for adequate clearance of extracellular K+. As a result of their electrogenic action, Na+,K+ pumps also help reverse depolarization arising during excitation, hyperkalemia, and anoxia, or from cell damage resulting from exercise, rhabdomyolysis, or muscle diseases. The ability to evaluate Na+,K+-pump function and the capacity of the Na+,K+ pumps to fill these needs require quantification of the total content of Na+,K+ pumps in skeletal muscle. Inhibition of Na+,K+-pump activity, or a decrease in their content, reduces muscle contractility. Conversely, stimulation of the Na+,K+-pump transport rate or increasing the content of Na+,K+ pumps enhances muscle excitability and contractility. Measurements of [3H]ouabain binding to skeletal muscle in vivo or in vitro have enabled the reproducible quantification of the total content of Na+,K+ pumps in molar units in various animal species, and in both healthy people and individuals with various diseases. In contrast, measurements of 3-O-methylfluorescein phosphatase activity associated with the Na+,K+-ATPase may show inconsistent results. Measurements of Na+ and K+ fluxes in intact isolated muscles show that, after Na+ loading or intense excitation, all the Na+,K+ pumps are functional, allowing calculation of the maximum Na+,K+-pumping capacity, expressed in molar units/g muscle/min. The activity and content of Na+,K+ pumps are regulated by exercise, inactivity, K+ deficiency, fasting, age, and several hormones and pharmaceuticals. Studies on the α-subunit isoforms of the Na+,K+-ATPase have detected a relative increase in their number in response to exercise and the glucocorticoid dexamethasone but have not involved their quantification in molar units. Determination of ATPase activity in homogenates and plasma membranes obtained from muscle has shown ouabain-suppressible stimulatory effects of Na+ and K+. PMID:24081980

A five-primary photostimulator suitable for studying intrinsically photosensitive retinal ganglion cell functions in humans

PubMed Central

Cao, Dingcai; Nicandro, Nathaniel; Barrionuevo, Pablo A.

2015-01-01

Intrinsically photosensitive retinal ganglion cells (ipRGCs) can respond to light directly through self-contained photopigment, melanopsin. IpRGCs also receive synaptic inputs from rods and cones. Thus, studying ipRGC functions requires a novel photostimulating method that can account for all of the photoreceptor inputs. Here, we introduced an inexpensive LED-based five-primary photostimulator that can control the excitations of rods, S-, M-, L-cones, and melanopsin-containing ipRGCs in humans at constant background photoreceptor excitation levels, a critical requirement for studying the adaptation behavior of ipRGCs with rod, cone, or melanopsin input. We described the theory and technical aspects (including optics, electronics, software, and calibration) of the five-primary photostimulator. Then we presented two preliminary studies using the photostimulator we have implemented to measure melanopsin-mediated pupil responses and temporal contrast sensitivity function (TCSF). The results showed that the S-cone input to pupil responses was antagonistic to the L-, M- or melanopsin inputs, consistent with an S-OFF and (L + M)-ON response property of primate ipRGCs (Dacey et al., 2005). In addition, the melanopsin-mediated TCSF had a distinctive pattern compared with L + M or S-cone mediated TCSF. Other than controlling individual photoreceptor excitation independently, the five-primary photostimulator has the flexibility in presenting stimuli modulating any combination of photoreceptor excitations, which allows researchers to study the mechanisms by which ipRGCs combine various photoreceptor inputs. PMID:25624466

Gentlest ascent dynamics for calculating first excited state and exploring energy landscape of Kohn-Sham density functionals.

PubMed

Li, Chen; Lu, Jianfeng; Yang, Weitao

2015-12-14

We develop the gentlest ascent dynamics for Kohn-Sham density functional theory to search for the index-1 saddle points on the energy landscape of the Kohn-Sham density functionals. These stationary solutions correspond to excited states in the ground state functionals. As shown by various examples, the first excited states of many chemical systems are given by these index-1 saddle points. Our novel approach provides an alternative, more robust way to obtain these excited states, compared with the widely used ΔSCF approach. The method can be easily generalized to target higher index saddle points. Our results also reveal the physical interest and relevance of studying the Kohn-Sham energy landscape.

Two-color two-photon excited fluorescence of indole: Determination of wavelength-dependent molecular parameters

NASA Astrophysics Data System (ADS)

Herbrich, Sebastian; Al-Hadhuri, Tawfik; Gericke, Karl-Heinz; Shternin, Peter S.; Smolin, Andrey G.; Vasyutinskii, Oleg S.

2015-01-01

We present a detailed study of two-color two-photon excited fluorescence in indole dissolved in propylene glycol. Femtosecond excitation pulses at effective wavelengths from 268 to 293.33 nm were used to populate the two lowest indole excited states 1La and 1Lb and polarized fluorescence was then detected. All seven molecular parameters and the two-photon polarization ratio Ω containing information on two-photon absorption dynamics, molecular lifetime τf, and rotation correlation time τrot have been determined from experiment and analyzed as a function of the excitation wavelength. The analysis of the experimental data has shown that 1Lb-1La inversion occurred under the conditions of our experiment. The two-photon absorption predominantly populated the 1La state at all excitation wavelengths but in the 287-289 nm area which contained an absorption hump of the 1Lb state 0-0 origin. The components of the two-photon excitation tensor S were analyzed giving important information on the principal tensor axes and absorption symmetry. The results obtained are in a good agreement with the results reported by other groups. The lifetime τf and the rotation correlation time τrot showed no explicit dependence on the effective excitation wavelength. Their calculated weighted average values were found to be τf = 3.83 ± 0.14 ns and τrot = 0.74 ± 0.06 ns.

Interplay between plasmon and single-particle excitations in a metal nanocluster

DOE PAGES

Ma, Jie; Wang, Zhi; Wang, Lin-Wang

2015-12-17

Plasmon-generated hot carriers are used in photovoltaic or photochemical applications. However, the interplays between the plasmon and single-particle excitations in nanosystems have not been theoretically addressed using ab initio methods. Here we show such interplays in a Ag 55 nanocluster using real-time time-dependent density functional theory simulations. We find that the disappearance of the zero-frequency peak in the Fourier transform of the band-to-band transition coefficient is a hallmark of the plasmon. We show the importance of the d-states for hot-carrier generations. If the single-particle d-to-s excitations are resonant to the plasmon frequency, the majority of the plasmon energy will bemore » converted into hot carriers, and the overall hot-carrier generation is enhanced by the plasmon; if such resonance does not exist, we observe an intriguing Rabi oscillation between the plasmon and hot carriers. Phonons play a minor role in plasmonic dynamics in such small systems. Ultimately, this study provides guidance on improving plasmonic applications.« less

Insights into the Mechanism of a Covalently Linked Organic Dye–Cobaloxime Catalyst System for Dye‐Sensitized Solar Fuel Devices

PubMed Central

Pati, Palas Baran; Zhang, Lei; Philippe, Bertrand; Fernández‐Terán, Ricardo; Ahmadi, Sareh; Tian, Lei; Rensmo, Håkan; Hammarström, Leif

2017-01-01

Abstract A covalently linked organic dye–cobaloxime catalyst system based on mesoporous NiO is synthesized by a facile click reaction for mechanistic studies and application in a dye‐sensitized solar fuel device. The system is systematically investigated by photoelectrochemical measurements, density functional theory, time‐resolved fluorescence, transient absorption spectroscopy, and photoelectron spectroscopy. The results show that irradiation of the dye–catalyst on NiO leads to ultrafast hole injection into NiO from the excited dye, followed by a fast electron transfer process to reduce the catalyst. Moreover, the dye adopts different structures with different excited state energies, and excitation energy transfer occurs between neighboring molecules on the semiconductor surface. The photoelectrochemical experiments also show hydrogen production by this system. The axial chloride ligands of the catalyst are released during photocatalysis to create the active sites for proton reduction. A working mechanism of the dye–catalyst system on the photocathode is proposed on the basis of this study. PMID:28338295

Interplay between plasmon and single-particle excitations in a metal nanocluster

PubMed Central

Ma, Jie; Wang, Zhi; Wang, Lin-Wang

2015-01-01

Plasmon-generated hot carriers are used in photovoltaic or photochemical applications. However, the interplays between the plasmon and single-particle excitations in nanosystems have not been theoretically addressed using ab initio methods. Here we show such interplays in a Ag55 nanocluster using real-time time-dependent density functional theory simulations. We find that the disappearance of the zero-frequency peak in the Fourier transform of the band-to-band transition coefficient is a hallmark of the plasmon. We show the importance of the d-states for hot-carrier generations. If the single-particle d-to-s excitations are resonant to the plasmon frequency, the majority of the plasmon energy will be converted into hot carriers, and the overall hot-carrier generation is enhanced by the plasmon; if such resonance does not exist, we observe an intriguing Rabi oscillation between the plasmon and hot carriers. Phonons play a minor role in plasmonic dynamics in such small systems. This study provides guidance on improving plasmonic applications. PMID:26673449

Quasiclassical trajectory studies of the O(3P) + CX4(vk = 0, 1) → OXv + CX3(n1n2n3n4) [X = H and D] reactions on an ab initio potential energy surface.

PubMed

Czakó, Gábor; Liu, Rui; Yang, Minghui; Bowman, Joel M; Guo, Hua

2013-08-01

We report quasiclassical trajectory calculations of the integral and differential cross sections and the mode-specific product state distributions for the "central-barrier" O((3)P) + CH4/CD4(vk = 0, 1) [k = 1, 2, 3, 4] reactions using a full-dimensional ab initio potential energy surface. The mode-specific vibrational distributions for the polyatomic methyl products are obtained by doing a normal-mode analysis in the Eckart frame, followed by standard histogram binning (HB) and energy-based Gaussian binning (1GB). The reactant bending excitations slightly enhance the reactivity, whereas stretching excitations activate the reaction more efficiently. None of the reactant vibrational excitations is as efficient as an equivalent amount of translational energy to promote the reactions. The excitation functions without product zero-point energy (ZPE) constraint are in good agreement with previous 8-dimensional quantum mechanical (QM) results for the ground-state and stretching-excited O + CH4 reactions, whereas for the bending-excited reactions the soft ZPE constraint, which is applied to the sum of the product vibrational energies, provides better agreement with the QM cross sections. All angular distributions show the dominance of backward scattering indicating a direct rebound mechanism, in agreement with experiment. The title reactions produce mainly OH/OD(v = 0) products for all the initial states. HB significantly overestimates the populations of OH/OD(v = 1), especially in the energetic threshold regions, whereas 1GB provides physically correct results. The CH3/CD3 vibrational distributions show dominant populations for ground (v = 0), umbrella-excited (v2 = 1, 2), in-plane-bending-excited (v4 = 1), and v2 + v4 methyl product states. Neither translational energy nor reactant vibrational excitation transfers significantly into product vibrations.

Excited-State Effective Masses in Lattice QCD

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

George Fleming, Saul Cohen, Huey-Wen Lin

2009-10-01

We apply black-box methods, i.e. where the performance of the method does not depend upon initial guesses, to extract excited-state energies from Euclidean-time hadron correlation functions. In particular, we extend the widely used effective-mass method to incorporate multiple correlation functions and produce effective mass estimates for multiple excited states. In general, these excited-state effective masses will be determined by finding the roots of some polynomial. We demonstrate the method using sample lattice data to determine excited-state energies of the nucleon and compare the results to other energy-level finding techniques.

Synthesis and characterization of Na(Gd0.5Lu0.5)F4: Nd3+,a core-shell free multifunctional contrast agent.

PubMed

Mimun, L Christopher; Ajithkumar, G; Rightsell, Chris; Langloss, Brian W; Therien, Michael J; Sardar, Dhiraj K

2017-02-25

Compared to conventional core-shell structures, core-shell free nanoparticles with multiple functionalities offer several advantages such as minimal synthetic complexity and low production cost. In this paper, we present the synthesis and characterization of Nd 3+ doped Na(Gd 0.5 Lu 0.5 )F 4 as a core-shell free nanoparticle system with three functionalities. Nanocrystals with 20 nm diameter, high crystallinity and a narrow particle size distributions were synthesized by the solvothermal method and characterized by various analytical techniques to understand their phase and morphology. Fluorescence characteristics under near infrared (NIR) excitation at 808 nm as well as X-ray excitation were studied to explore their potential in NIR optical and X-ray imaging. At 1.0 mol% Nd concentration, we observed a quantum yield of 25% at 1064 nm emission with 13 W/cm 2 excitation power density which is sufficiently enough for imaging applications. Under 130 kVp (5 mA) power of X-ray excitation, Nd 3+ doped Na(Gd 0.5 Lu 0.5 )F 4 shows the characteristic emission bands of Gd 3+ and Nd 3+ with the strongest emission peak at 1064 nm due to Nd 3+ . Furthermore, magnetization measurements show that the nanocrystals are paramagnetic in nature with a calculated magnetic moment per particle of ~570 μB at 2T. These preliminary results support the suitability of the present nanophosphor as a multimodal contrast agent with three imaging features viz. optical, magnetic and X-ray.

Excitation Function of the Reaction Al$sup 27$(d,p)Al$sup 28$ from 2.2 to 12.6 Mev. Report No. 65; FUNCION DE EXCITACION DE LA REACCION AL$sup 27$(d,p)Al$sup 28$ ENTRE 2,2 Y 12,6 Mev. INFORME NO. 65

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

Flores, J.M.

1962-01-01

The excitation function is measured for the reaction Al/sup 27/(d,p)Al/ sup 28/ between 2.2 and 12.6 Mev. The calibration of the excitation function in absolute form is carried out by measuring simultaneously the excitation function of the reactions Al/sup 27/(d,p) and (d, alpha p) and comparing the results obtained with those of Batzel et al. The maximum of the function is between 7 and 8 Mev, and is 239 plus or minus 29 mb. The half life of Al/sup 28/ was determined as 2.28 plus or minus 0.06 min. (tr-auth)

Proton-Proton Elastic Scattering Excitation Functions at Intermediate Energies: Cross Sections and Analyzing Powers

NASA Astrophysics Data System (ADS)

Hinterberger, F.; Rohdjeß, H.; Altmeier, M.; Bauer, F.; Bisplinghoff, J.; Büßer, K.; Busch, M.; Colberg, T.; Diehl, O.; Dohrmann, F.; Engelhardt, H. P.; Eversheim, P. D.; Felden, O.; Gebel, R.; Glende, M.; Greiff, J.; Groß-Hardt, R.; Hinterberger, F.; Jahn, R.; Jonas, E.; Krause, H.; Langkau, R.; Lindemann, T.; Lindlein, J.; Maier, R.; Maschuw, R.; Mayer-Kuckuk, T.; Meinerzhagen, A.; Nähle, O.; Prasuhn, D.; Rohdjeß, H.; Rosendaal, D.; von Rossen, P.; Schirm, N.; Schulz-Rojahn, M.; Schwarz, V.; Scobel, W.; Trelle, H. J.; Weise, E.; Wellinghausen, A.; Woller, K.; Ziegler, R.

2000-01-01

The EDDA experiment at the cooler synchrotron COSY measures proton-proton elastic scattering excitation functions in the momentum range 0.8 - 3.4 GeV/c. In phase 1 of the experiment, spin-averaged differential cross sections were measured continuously during acceleration with an internal polypropylene (CH2) fiber target, taking particular care to monitor luminosity as a function of beam momentum. In phase 2, excitation functions of the analyzing power AN and the polarization correlation parameters ANN, ASS and ASL are measured using a polarized proton beam and a polarized atomic hydrogen beam target. The paper presents recent dσ/dΩ and AN data. The results provide excitation functions and angular distributions of high precision and internal consistency. No evidence for narrow structures was found. The data are compared to recent phase shift solutions.

How to precisely measure the volume velocity transfer function of physical vocal tract models by external excitation

PubMed Central

Mainka, Alexander; Kürbis, Steffen; Birkholz, Peter

2018-01-01

Recently, 3D printing has been increasingly used to create physical models of the vocal tract with geometries obtained from magnetic resonance imaging. These printed models allow measuring the vocal tract transfer function, which is not reliably possible in vivo for the vocal tract of living humans. The transfer functions enable the detailed examination of the acoustic effects of specific articulatory strategies in speaking and singing, and the validation of acoustic plane-wave models for realistic vocal tract geometries in articulatory speech synthesis. To measure the acoustic transfer function of 3D-printed models, two techniques have been described: (1) excitation of the models with a broadband sound source at the glottis and measurement of the sound pressure radiated from the lips, and (2) excitation of the models with an external source in front of the lips and measurement of the sound pressure inside the models at the glottal end. The former method is more frequently used and more intuitive due to its similarity to speech production. However, the latter method avoids the intricate problem of constructing a suitable broadband glottal source and is therefore more effective. It has been shown to yield a transfer function similar, but not exactly equal to the volume velocity transfer function between the glottis and the lips, which is usually used to characterize vocal tract acoustics. Here, we revisit this method and show both, theoretically and experimentally, how it can be extended to yield the precise volume velocity transfer function of the vocal tract. PMID:29543829

Is the Bethe–Salpeter Formalism Accurate for Excitation Energies? Comparisons with TD-DFT, CASPT2, and EOM-CCSD

PubMed Central

2017-01-01

Developing ab initio approaches able to provide accurate excited-state energies at a reasonable computational cost is one of the biggest challenges in theoretical chemistry. In that framework, the Bethe–Salpeter equation approach, combined with the GW exchange-correlation self-energy, which maintains the same scaling with system size as TD-DFT, has recently been the focus of a rapidly increasing number of applications in molecular chemistry. Using a recently proposed set encompassing excitation energies of many kinds [J. Phys. Chem. Lett.2016, 7, 586–591], we investigate here the performances of BSE/GW. We compare these results to CASPT2, EOM-CCSD, and TD-DFT data and show that BSE/GW provides an accuracy comparable to the two wave function methods. It is particularly remarkable that the BSE/GW is equally efficient for valence, Rydberg, and charge-transfer excitations. In contrast, it provides a poor description of triplet excited states, for which EOM-CCSD and CASPT2 clearly outperform BSE/GW. This contribution therefore supports the use of the Bethe–Salpeter approach for spin-conserving transitions. PMID:28301726

New two-photon excitation chromophores for cellular imaging

NASA Astrophysics Data System (ADS)

D'Alfonso, Laura; Chirico, Giuseppe; Collini, Maddalena; Baldini, Giancarlo; Diaspro, Alberto; Ramoino, Paola; Abbotto, Alessandro; Beverina, Luca; Pagani, Giorgio A.

2003-10-01

The one photon and two photon excitation spectral properties (absorption, emission spectra, singlet lifetime) of a very efficient two photon absorber, dimethyl-pepep, have been measured in solution. The one photon excitation peak lye near 525 nm and the emission falls at 600 nm, where autofluorescence of cells is weak. The value of the singlet-triplet conversion rate, obtained by two-photon excitation fluorescence correlation spectroscopy, has a quadratic dependence on the excitation power and is comparable to that shown by the dye rhodamine. Preliminary results on stained cells from yeast Saccaromices cerevisiae and Paramecium primaurelia show that the dye preferentially stains DNA in the cell. A direct comparison with a DNA stainer, Dapi, is also performed. Some measurements of the dye functionalized to react with lysine and n-terminal residues of protein are presented. Moreover, this dye can be employed in order to follow in detail some cellular processes such as nuclei division. In vitro fluorescence titration of dimethyl-pepep with calf thymus DNA allowed to estimate the values of the dye-DNA association constant versus ionic strength, and an affinity close to that of ethidium bromide is found.

The performance and relationship among range-separated schemes for density functional theory

NASA Astrophysics Data System (ADS)

Nguyen, Kiet A.; Day, Paul N.; Pachter, Ruth

2011-08-01

The performance and relationship among different range-separated (RS) hybrid functional schemes are examined using the Coulomb-attenuating method (CAM) with different values for the fractions of exact Hartree-Fock (HF) exchange (α), long-range HF (β), and a range-separation parameter (μ), where the cases of α + β = 1 and α + β = 0 were designated as CA and CA0, respectively. Attenuated PBE exchange-correlation functionals with α = 0.20 and μ = 0.20 (CA-PBE) and α = 0.25 and μ = 0.11 (CA0-PBE) are closely related to the LRC-ωPBEh and HSE functionals, respectively. Time-dependent density functional theory calculations were carried out for a number of classes of molecules with varying degrees of charge-transfer (CT) character to provide an assessment of the accuracy of excitation energies from the CA functionals and a number of other functionals with different exchange hole models. Functionals that provided reasonable estimates for local and short-range CT transitions were found to give large errors for long-range CT excitations. In contrast, functionals that afforded accurate long-range CT excitation energies significantly overestimated energies for short-range CT and local transitions. The effects of exchange hole models and parameters developed for RS functionals for CT excitations were analyzed in detail. The comparative analysis across compound classes provides a useful benchmark for CT excitations.

Influence of Wall Material on VUV Emission from Hydrogen Plasma in H- Source

NASA Astrophysics Data System (ADS)

Bacal, M.; Glass-Maujean, M.; Ivanov, A. A., Jr; Nishiura, M.; Sasao, M.; Wada, M.

2002-11-01

The study of VUV emission from a hydrogen plasma produced in a filament discharge in a magnetic multicusp device showed that the use of tantalum and tungsten filaments leads to significant differences in the spectra. The effect of the filament material is interpreted in terms of the fresh film of this material, deposited on the wall. The synthetic spectrum convoluted with our apparatus function for the conditions of this experiment (gas temperature 500 K, electron energy 100 eV) agrees roughly well with the spectrum obtained with tungsten covered walls, but not with the spectrum obtained with tantalum covered walls. We show that in the case of tungsten covered walls the E-V singlet excitation is indeed a two-step Franck-Condon transition, going through either B or C state from an initial H2 molecule with v"=0, added to a Franck-Condon transition to highly excited states cascading to the B or C states. The excitation process to high v" states in the case of tantalum covered walls is a three step process, in which the first step is the formation by recombinative desorption on the wall of a vibrationally excited molecule with v"=1 or 2, which serves as the initial molecule in the subsequent E-V excitation through the B state. The results indicate a larger recombination coefficient of atoms on the tantalum covered wall.

Mechanism of resonant electron emission from the deprotonated GFP chromophore and its biomimetics.

PubMed

Bochenkova, Anastasia V; Mooney, Ciarán R S; Parkes, Michael A; Woodhouse, Joanne L; Zhang, Lijuan; Lewin, Ross; Ward, John M; Hailes, Helen C; Andersen, Lars H; Fielding, Helen H

2017-04-01

The Green Fluorescent Protein (GFP), which is widely used in bioimaging, is known to undergo light-induced redox transformations. Electron transfer is thought to occur resonantly through excited states of its chromophore; however, a detailed understanding of the electron gateway states of the chromophore is still missing. Here, we use photoelectron spectroscopy and high-level quantum chemistry calculations to show that following UV excitation, the ultrafast electron dynamics in the chromophore anion proceeds via an excited shape resonance strongly coupled to the open continuum. The impact of this state is found across the entire 355-315 nm excitation range, from above the first bound-bound transition to below the opening of higher-lying continua. By disentangling the electron dynamics in the photodetachment channels, we provide an important reference for the adiabatic position of the electron gateway state, which is located at 348 nm, and discover the source of the curiously large widths of the photoelectron spectra that have been reported in the literature. By introducing chemical modifications to the GFP chromophore, we show that the detachment threshold and the position of the gateway state, and hence the underlying excited-state dynamics, can be changed systematically. This enables a fine tuning of the intrinsic electron emission properties of the GFP chromophore and has significant implications for its function, suggesting that the biomimetic GFP chromophores are more stable to photooxidation.

Three-dimensional spectroscopy of vibrational energy in liquids: nitromethane and acetonitrile.

PubMed

Sun, Yuxiao; Pein, Brandt C; Dlott, Dana D

2013-12-12

We introduce a novel type of three-dimensional (3D) spectroscopy to study vibrational energy transfer, where an IR pulse tunable through the CH-stretching and CD-stretching regions was used to create parent vibrational excitations in liquids and a visible probe pulse was used to generate both Stokes and anti-Stokes Raman spectra as a function of delay time. The Raman spectra determine how much vibrational excitation was present in each probed state. The three dimensions are the wavenumber of the pumped state, the wavenumber of the probed state, and the time interval. The technique was used to study nitromethane (NM) and acetonitrile (ACN) and their deuterated analogues at ambient temperature. The 3D spectra were quite complicated. Three types of artifacts due to nonlinear light scattering were observed. Along the diagonal were two fundamental CH-stretch (or CD-stretch) transitions and several weaker combination bands or overtone transitions. Because Raman spectroscopy allows us to simultaneously probe a wide wavenumber region, for every diagonal peak, there were ∼10 off-diagonal peaks. The cross-peaks at shorter delay times reveal the nature of the initial excitation by showing which lower-wavenumber excitations were produced along with the pumped CH-stretch or CD-stretch. The longer-time spectra characterized vibrational energy relaxation processes, and showed how daughter vibrations were generated by different parent excitations.

Hydrological signal in polar motion excitation from a combination of geophysical and gravimetric series

NASA Astrophysics Data System (ADS)

Nastula, Jolanta; Winska, Malgorzata; Salstein, David A.

2015-08-01

One can estimate the hydrological signal in polar motion excitation as a residual, namely the difference between observed geodetic excitation functions (Geodetic Angular Momentum, GAM) and the sum of Atmospheric Angular Momentum (AAM) and Oceanic Angular Momentum (OAM).The aim of this study is to find the optimal model and results for hydrological excitation functions in terms of their agreement with the computed difference between GAM and atmospheric and oceanic signals.The atmospheric and oceanic model-based data that we use in this study are the geophysical excitation functions of AAM, OAM available from the Special Bureaus for the Atmosphere and Oceans of the Geophysical Global Fluids Center (GGFC) of the International Earth Rotation and Reference Systems Service (IERS). For the atmosphere and ocean, these functions are based on the mass and motion fields of the fluids.Global models of land hydrology are used to estimate hydrological excitation functions of polar motion (Hydrological Angular Momentum - HAM). These HAM series are the mass of water substance determined from the various types of land-based hydrological reservoirs. In addition the HAM are estimated from spherical harmonic coefficients of the Earth’s gravity field. We use several sets of degree-2, order-1 harmonics of the Earth’s gravity field, derived from the Gravity Recovery and Climate Experiment (GRACE), Satellite Laser Ranging (SLR), and Global Navigation Satellite Systems (GNSS) data.Finally, these several different HAM series are used to determine the best model of hydrological excitation of polar motion. The model is found by looking for the combination of these series that fits the geodetic residuals using the least-square method.In addition, we will access model results from the Coupled Model Intercomparison Project, fifth experiment (CMIP-5) to examine atmospheric excitations from the twentieth century and estimates for the twenty-first century to see the possible signals and trends of these excitation series to help understand the potential range in the derived of hydrological excitation results.

Extended methods using thick-targets for nuclear reaction data of radioactive isotopes

NASA Astrophysics Data System (ADS)

Ebata, Shuichiro; Aikawa, Masayuki; Imai, Shotaro

2017-09-01

The nuclear transmutation is a technology to dispose of radioactive wastes. However, we do not have enough basic data for its developments, such as thick-target yields (TTY) and the interaction cross sections for radioactive material. We suggest two methods to estimate the TTY using inverse kinematics and to obtain the excitation function of the interaction cross sections which is named the thick-target transmission (T3) method. We deduce the energy-dependent conversion relation between the TTYs of the original system and its inverse kinematics, which can be replaced to a constant coefficient in the high energy region. Furthermore we show the usefulness of the T3 method to investigate the excitation function of the 12C + 27Al reaction in the simulation.

Designing graphene absorption in a multispectral plasmon-enhanced infrared detector

DOE PAGES

Goldflam, Michael D.; Fei, Zhe; Ruiz, Isaac; ...

2017-05-18

Here, we have examined graphene absorption in a range of graphene-based infrared devices that combine either monolayer or bilayer graphene with three different gate dielectrics. Electromagnetic simulations show that the optical absorption in graphene in these devices, an important factor in a functional graphene-based detector, is strongly dielectric-dependent. Our simulations reveal that plasmonic excitation in graphene can significantly influence the percentage of light absorbed in the entire device, as well as the graphene layer itself, with graphene absorption exceeding 25% in regions where plasmonic excitation occurs. Notably, the dielectric environment of graphene has a dramatic influence on the strength andmore » wavelength range over which the plasmons can be excited, making dielectric choice paramount to final detector tunability and sensitivity.« less

Designing graphene absorption in a multispectral plasmon-enhanced infrared detector

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

Goldflam, Michael D.; Fei, Zhe; Ruiz, Isaac

Here, we have examined graphene absorption in a range of graphene-based infrared devices that combine either monolayer or bilayer graphene with three different gate dielectrics. Electromagnetic simulations show that the optical absorption in graphene in these devices, an important factor in a functional graphene-based detector, is strongly dielectric-dependent. Our simulations reveal that plasmonic excitation in graphene can significantly influence the percentage of light absorbed in the entire device, as well as the graphene layer itself, with graphene absorption exceeding 25% in regions where plasmonic excitation occurs. Notably, the dielectric environment of graphene has a dramatic influence on the strength andmore » wavelength range over which the plasmons can be excited, making dielectric choice paramount to final detector tunability and sensitivity.« less

Energy dissipation in a friction-controlled slide of a body excited by random motions of the foundation

NASA Astrophysics Data System (ADS)

Berezin, Sergey; Zayats, Oleg

2018-01-01

We study a friction-controlled slide of a body excited by random motions of the foundation it is placed on. Specifically, we are interested in such quantities as displacement, traveled distance, and energy loss due to friction. We assume that the random excitation is switched off at some time (possibly infinite) and show that the problem can be treated in an analytic, explicit, manner. Particularly, we derive formulas for the moments of the displacement and distance, and also for the average energy loss. To accomplish that we use the Pugachev-Sveshnikov equation for the characteristic function of a continuous random process given by a system of SDEs. This equation is solved by reduction to a parametric Riemann boundary value problem of complex analysis.

Excited-state potential-energy surfaces of metal-adsorbed organic molecules from linear expansion Δ-self-consistent field density-functional theory (ΔSCF-DFT).

PubMed

Maurer, Reinhard J; Reuter, Karsten

2013-07-07

Accurate and efficient simulation of excited state properties is an important and much aspired cornerstone in the study of adsorbate dynamics on metal surfaces. To this end, the recently proposed linear expansion Δ-self-consistent field method by Gavnholt et al. [Phys. Rev. B 78, 075441 (2008)] presents an efficient alternative to time consuming quasi-particle calculations. In this method, the standard Kohn-Sham equations of density-functional theory are solved with the constraint of a non-equilibrium occupation in a region of Hilbert-space resembling gas-phase orbitals of the adsorbate. In this work, we discuss the applicability of this method for the excited-state dynamics of metal-surface mounted organic adsorbates, specifically in the context of molecular switching. We present necessary advancements to allow for a consistent quality description of excited-state potential-energy surfaces (PESs), and illustrate the concept with the application to Azobenzene adsorbed on Ag(111) and Au(111) surfaces. We find that the explicit inclusion of substrate electronic states modifies the topologies of intra-molecular excited-state PESs of the molecule due to image charge and hybridization effects. While the molecule in gas phase shows a clear energetic separation of resonances that induce isomerization and backreaction, the surface-adsorbed molecule does not. The concomitant possibly simultaneous induction of both processes would lead to a significantly reduced switching efficiency of such a mechanism.

Pharmacological modulation of the voltage-gated neuronal Kv7/KCNQ/M-channel alters the intrinsic excitability and synaptic responses of pyramidal neurons in rat prefrontal cortex slices.

PubMed

Peng, Hui; Bian, Xi-Ling; Ma, Fu-Cui; Wang, Ke-Wei

2017-09-01

The prefrontal cortex (PFC) critical for higher cognition is implicated in neuropsychiatric diseases, such as Alzheimer's disease, depression and schizophrenia. The voltage-activated Kv7/KCNQ/M-channel or M-current modulates the neuronal excitability that defines the fundamental mechanism of brain function. However, whether M-current functions to regulate the excitability of PFC neurons remains elusive. In this study, we recorded the native M-current from PFC layer V pyramidal neurons in rat brain slices and showed that it modulated the intrinsic excitability and synaptic responses of PFC pyramidal neurons. Application of a specific M-channel blocker XE991 (40 μmol/L) or opener retigabine (10 μmol/L) resulted in inhibition or activation of M-current, respectively. In the current-clamp recordings, inhibition of M-current was evidenced by the increased average spike frequency and the reduced first inter-spike interval (ISI), spike onset latency and fast afterhyperpolarization (fAHP), whereas activation of M-current caused opposite responses. Furthermore, inhibition of M-current significantly increased the amplitude of excitatory postsynaptic potentials (EPSPs) and depolarized the resting membrane potential (RMP) without affecting the miniature EPSC (mEPSC) frequency. These data demonstrate that voltage-gated neuronal Kv7/KCNQ/M-current modulates the excitability and synaptic transmission of PFC neurons, suggesting that pharmacological modulation of M-current in the PFC may exert beneficial effects on cognitive deficits implicated in the pathophysiology of neuropsychiatric disorders.

The excitation and characteristic frequency of the long-period volcanic event: An approach based on an inhomogeneous autoregressive model of a linear dynamic system

USGS Publications Warehouse

Nakano, M.; Kumagai, H.; Kumazawa, M.; Yamaoka, K.; Chouet, B.A.

1998-01-01

We present a method to quantify the source excitation function and characteristic frequencies of long-period volcanic events. The method is based on an inhomogeneous autoregressive (AR) model of a linear dynamic system, in which the excitation is assumed to be a time-localized function applied at the beginning of the event. The tail of an exponentially decaying harmonic waveform is used to determine the characteristic complex frequencies of the event by the Sompi method. The excitation function is then derived by operating an AR filter constructed from the characteristic frequencies to the entire seismogram of the event, including the inhomogeneous part of the signal. We apply this method to three long-period events at Kusatsu-Shirane Volcano, central Japan, whose waveforms display simple decaying monochromatic oscillations except for the beginning of the events. We recover time-localized excitation functions lasting roughly 1 s at the start of each event and find that the estimated functions are very similar to each other at all the stations of the seismic network for each event. The phases of the characteristic oscillations referred to the estimated excitation function fall within a narrow range for almost all the stations. These results strongly suggest that the excitation and mode of oscillation are both dominated by volumetric change components. Each excitation function starts with a pronounced dilatation consistent with a sudden deflation of the volumetric source which may be interpreted in terms of a choked-flow transport mechanism. The frequency and Q of the characteristic oscillation both display a temporal evolution from event to event. Assuming a crack filled with bubbly water as seismic source for these events, we apply the Van Wijngaarden-Papanicolaou model to estimate the acoustic properties of the bubbly liquid and find that the observed changes in the frequencies and Q are consistently explained by a temporal change in the radii of the bubbles characterizing the bubbly water in the crack.

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

Robinson, Neil J.; Konik, Robert M.

Here, we study the excitation spectrum of two-component delta-function interacting bosons confined to a single spatial dimension, the Yang–Gaudin Bose gas. We show that there are pronounced finite-size effects in the dispersion relations of excitations, perhaps best illustrated by the spinon single particle dispersion which exhibits a gap at 2k F and a finite-momentum roton-like minimum. Such features occur at energies far above the finite volume excitation gap, vanish slowly as 1/L for fixed spinon number, and can persist to the thermodynamic limit at fixed spinon density. Features such as the 2k F gap also persist to multi-particle excitation continua. Our results show that excitations in the finite system can behave in a qualitatively different manner to analogous excitations in the thermodynamic limit. The Yang–Gaudin Bose gas is also host to multi-spinon bound states, known asmore » $$\\Lambda$$ -strings. We study these excitations both in the thermodynamic limit under the string hypothesis and in finite size systems where string deviations are taken into account. In the zero-temperature limit we present a simple relation between the length n $$\\Lambda$$-string dressed energies $$\\epsilon_n(\\lambda)$$ and the dressed energy $$\\epsilon(k)$$. We solve the Yang–Yang–Takahashi equations numerically and compare to the analytical solution obtained under the strong couple expansion, revealing that the length n $$\\Lambda$$ -string dressed energy is Lorentzian over a wide range of real string centers λ in the vicinity of $$\\lambda = 0$$ . We then examine the finite size effects present in the dispersion of the two-spinon bound states by numerically solving the Bethe ansatz equations with string deviations.« less

Multiresolution quantum chemistry in multiwavelet bases: excited states from time-dependent Hartree–Fock and density functional theory via linear response

DOE PAGES

Yanai, Takeshi; Fann, George I.; Beylkin, Gregory; ...

2015-02-25

Using the fully numerical method for time-dependent Hartree–Fock and density functional theory (TD-HF/DFT) with the Tamm–Dancoff (TD) approximation we use a multiresolution analysis (MRA) approach to present our findings. From a reformulation with effective use of the density matrix operator, we obtain a general form of the HF/DFT linear response equation in the first quantization formalism. It can be readily rewritten as an integral equation with the bound-state Helmholtz (BSH) kernel for the Green's function. The MRA implementation of the resultant equation permits excited state calculations without virtual orbitals. Moreover, the integral equation is efficiently and adaptively solved using amore » numerical multiresolution solver with multiwavelet bases. Our implementation of the TD-HF/DFT methods is applied for calculating the excitation energies of H 2, Be, N 2, H 2O, and C 2H 4 molecules. The numerical errors of the calculated excitation energies converge in proportion to the residuals of the equation in the molecular orbitals and response functions. The energies of the excited states at a variety of length scales ranging from short-range valence excitations to long-range Rydberg-type ones are consistently accurate. It is shown that the multiresolution calculations yield the correct exponential asymptotic tails for the response functions, whereas those computed with Gaussian basis functions are too diffuse or decay too rapidly. Finally, we introduce a simple asymptotic correction to the local spin-density approximation (LSDA) so that in the TDDFT calculations, the excited states are correctly bound.« less

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

Escartín, J. M.; CNRS, UMR5152, F-31062 Toulouse Cedex; Theory of Condensed Matter Group, Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, Cambridge CB3 0HE

Time-Dependent Density-Functional Theory (TDDFT) is a well-established theoretical approach to describe and understand irradiation processes in clusters and molecules. However, within the so-called adiabatic local density approximation (ALDA) to the exchange-correlation (xc) potential, TDDFT can show insufficiencies, particularly in violently dynamical processes. This is because within ALDA the xc potential is instantaneous and is a local functional of the density, which means that this approximation neglects memory effects and long-range effects. A way to go beyond ALDA is to use Time-Dependent Current-Density-Functional Theory (TDCDFT), in which the basic quantity is the current density rather than the density as in TDDFT.more » This has been shown to offer an adequate account of dissipation in the linear domain when the Vignale-Kohn (VK) functional is used. Here, we go beyond the linear regime and we explore this formulation in the time domain. In this case, the equations become very involved making the computation out of reach; we hence propose an approximation to the VK functional which allows us to calculate the dynamics in real time and at the same time to keep most of the physics described by the VK functional. We apply this formulation to the calculation of the time-dependent dipole moment of Ca, Mg and Na{sub 2}. Our results show trends similar to what was previously observed in model systems or within linear response. In the non-linear domain, our results show that relaxation times do not decrease with increasing deposited excitation energy, which sets some limitations to the practical use of TDCDFT in such a domain of excitations.« less

Electron-phonon relaxation and excited electron distribution in gallium nitride

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

Zhukov, V. P.; Donostia International Physics Center; Tyuterev, V. G., E-mail: valtyut00@mail.ru

2016-08-28

We develop a theory of energy relaxation in semiconductors and insulators highly excited by the long-acting external irradiation. We derive the equation for the non-equilibrium distribution function of excited electrons. The solution for this function breaks up into the sum of two contributions. The low-energy contribution is concentrated in a narrow range near the bottom of the conduction band. It has the typical form of a Fermi distribution with an effective temperature and chemical potential. The effective temperature and chemical potential in this low-energy term are determined by the intensity of carriers' generation, the speed of electron-phonon relaxation, rates ofmore » inter-band recombination, and electron capture on the defects. In addition, there is a substantial high-energy correction. This high-energy “tail” largely covers the conduction band. The shape of the high-energy “tail” strongly depends on the rate of electron-phonon relaxation but does not depend on the rates of recombination and trapping. We apply the theory to the calculation of a non-equilibrium distribution of electrons in an irradiated GaN. Probabilities of optical excitations from the valence to conduction band and electron-phonon coupling probabilities in GaN were calculated by the density functional perturbation theory. Our calculation of both parts of distribution function in gallium nitride shows that when the speed of the electron-phonon scattering is comparable with the rate of recombination and trapping then the contribution of the non-Fermi “tail” is comparable with that of the low-energy Fermi-like component. So the high-energy contribution can essentially affect the charge transport in the irradiated and highly doped semiconductors.« less

Thick-target transmission method for excitation functions of interaction cross sections

NASA Astrophysics Data System (ADS)

Aikawa, M.; Ebata, S.; Imai, S.

2016-09-01

We propose a method, called as thick-target transmission (T3) method, to obtain an excitation function of interaction cross sections. In an ordinal experiment to measure the excitation function of interaction cross sections by the transmission method, we need to change the beam energy for each cross section. In the T3 method, the excitation function is derived from the beam attenuations measured at the targets of different thicknesses without changing the beam energy. The advantage of the T3 method is the simplicity and availability for radioactive beams. To confirm the availability, we perform a simulation for the 12C + 27Al system with the PHITS code instead of actual experiments. Our results have large uncertainties but well reproduce the tendency of the experimental data.

Non-linear dynamic characteristics and optimal control of giant magnetostrictive film subjected to in-plane stochastic excitation

NASA Astrophysics Data System (ADS)

Zhu, Z. W.; Zhang, W. D.; Xu, J.

2014-03-01

The non-linear dynamic characteristics and optimal control of a giant magnetostrictive film (GMF) subjected to in-plane stochastic excitation were studied. Non-linear differential items were introduced to interpret the hysteretic phenomena of the GMF, and the non-linear dynamic model of the GMF subjected to in-plane stochastic excitation was developed. The stochastic stability was analysed, and the probability density function was obtained. The condition of stochastic Hopf bifurcation and noise-induced chaotic response were determined, and the fractal boundary of the system's safe basin was provided. The reliability function was solved from the backward Kolmogorov equation, and an optimal control strategy was proposed in the stochastic dynamic programming method. Numerical simulation shows that the system stability varies with the parameters, and stochastic Hopf bifurcation and chaos appear in the process; the area of the safe basin decreases when the noise intensifies, and the boundary of the safe basin becomes fractal; the system reliability improved through stochastic optimal control. Finally, the theoretical and numerical results were proved by experiments. The results are helpful in the engineering applications of GMF.

A simple derivation of the exact quasiparticle theory and its extension to arbitrary initial excited eigenstates.

PubMed

Ohno, Kaoru; Ono, Shota; Isobe, Tomoharu

2017-02-28

The quasiparticle (QP) energies, which are minus of the energies required by removing or produced by adding one electron from/to the system, corresponding to the photoemission or inverse photoemission (PE/IPE) spectra, are determined together with the QP wave functions, which are not orthonormal and even not linearly independent but somewhat similar to the normal spin orbitals in the theory of the configuration interaction, by self-consistently solving the QP equation coupled with the equation for the self-energy. The electron density, kinetic, and all interaction energies can be calculated using the QP wave functions. We prove in a simple way that the PE/IPE spectroscopy and therefore this QP theory can be applied to an arbitrary initial excited eigenstate. In this proof, we show that the energy-dependence of the self-energy is not an essential difficulty, and the QP picture holds exactly if there is no relaxation mechanism in the system. The validity of the present theory for some initial excited eigenstates is tested using the one-shot GW approximation for several atoms and molecules.

Matrix product state representation of quasielectron wave functions

NASA Astrophysics Data System (ADS)

Kjäll, J.; Ardonne, E.; Dwivedi, V.; Hermanns, M.; Hansson, T. H.

2018-05-01

Matrix product state techniques provide a very efficient way to numerically evaluate certain classes of quantum Hall wave functions that can be written as correlators in two-dimensional conformal field theories. Important examples are the Laughlin and Moore-Read ground states and their quasihole excitations. In this paper, we extend the matrix product state techniques to evaluate quasielectron wave functions, a more complex task because the corresponding conformal field theory operator is not local. We use our method to obtain density profiles for states with multiple quasielectrons and quasiholes, and to calculate the (mutual) statistical phases of the excitations with high precision. The wave functions we study are subject to a known difficulty: the position of a quasielectron depends on the presence of other quasiparticles, even when their separation is large compared to the magnetic length. Quasielectron wave functions constructed using the composite fermion picture, which are topologically equivalent to the quasielectrons we study, have the same problem. This flaw is serious in that it gives wrong results for the statistical phases obtained by braiding distant quasiparticles. We analyze this problem in detail and show that it originates from an incomplete screening of the topological charges, which invalidates the plasma analogy. We demonstrate that this can be remedied in the case when the separation between the quasiparticles is large, which allows us to obtain the correct statistical phases. Finally, we propose that a modification of the Laughlin state, that allows for local quasielectron operators, should have good topological properties for arbitrary configurations of excitations.

Existence of a new emitting singlet state of proflavine: femtosecond dynamics of the excited state processes and quantum chemical studies in different solvents.

PubMed

Kumar, Karuppannan Senthil; Selvaraju, Chellappan; Malar, Ezekiel Joy Padma; Natarajan, Paramasivam

2012-01-12

Proflavine (3,6-diaminoacridine) shows fluorescence emission with lifetime, 4.6 ± 0.2 ns, in all the solvents irrespective of the solvent polarity. To understand this unusual photophysical property, investigations were carried out using steady state and time-resolved fluorescence spectroscopy in the pico- and femtosecond time domain. Molecular geometries in the ground and low-lying excited states of proflavine were examined by complete structural optimization using ab initio quantum chemical computations at HF/6-311++G** and CIS/6-311++G** levels. Time dependent density functional theory (TDDFT) calculations were performed to study the excitation energies in the low-lying excited states. The steady state absorption and emission spectral details of proflavine are found to be influenced by solvents. The femtosecond fluorescence decay of the proflavine in all the solvents follows triexponential function with two ultrafast decay components (τ(1) and τ(2)) in addition to the nanosecond component. The ultrafast decay component, τ(1), is attributed to the solvation dynamics of the particular solvent used. The second ultrafast decay component, τ(2), is found to vary from 50 to 215 ps depending upon the solvent. The amplitudes of the ultrafast decay components vary with the wavelength and show time dependent spectral shift in the emission maximum. The observation is interpreted that the time dependent spectral shift is not only due to solvation dynamics but also due to the existence of more than one emitting state of proflavine in the solvent used. Time resolved area normalized emission spectral (TRANES) analysis shows an isoemissive point, indicating the presence of two emitting states in homogeneous solution. Detailed femtosecond fluorescence decay analysis allows us to isolate the two independent emitting components of the close lying singlet states. The CIS and TDDFT calculations also support the existence of the close lying emitting states. The near constant lifetime observed for proflavine in different solvents is suggested to be due to the similar dipole moments of the ground and the evolved emitting singlet state of the dye from the Franck-Condon excited state.

First-principles electron dynamics control simulation of diamond under femtosecond laser pulse train irradiation.

PubMed

Wang, Cong; Jiang, Lan; Wang, Feng; Li, Xin; Yuan, Yanping; Xiao, Hai; Tsai, Hai-Lung; Lu, Yongfeng

2012-07-11

A real-time and real-space time-dependent density functional is applied to simulate the nonlinear electron-photon interactions during shaped femtosecond laser pulse train ablation of diamond. Effects of the key pulse train parameters such as the pulse separation, spatial/temporal pulse energy distribution and pulse number per train on the electron excitation and energy absorption are discussed. The calculations show that photon-electron interactions and transient localized electron dynamics can be controlled including photon absorption, electron excitation, electron density, and free electron distribution by the ultrafast laser pulse train.

Experimental and computational studies on the electronic excited states of nitrobenzene

NASA Astrophysics Data System (ADS)

Krishnakumar, Sunanda; Das, Asim Kumar; Singh, Param Jeet; Shastri, Aparna; Rajasekhar, B. N.

2016-11-01

The gas phase electronic absorption spectrum of nitrobenzene (C6H5NO2) in the 4.5-11.2 eV region is recorded using synchrotron radiation with a view to comprehend the nature of the excited states. Electronic excited states of nitrobenzene are mainly classified as local excitations within the benzene ring or nitro group and charge transfer excitations between the benzene and nitro group, with some transitions showing percentage from both. The nature of molecular orbitals, their orderings and energies are obtained from density functional theory calculations which help in assigning partially assigned/unassigned features in earlier photoelectron spectroscopy studies. Optimized geometry of ionic nitrobenzene predicts redistribution of charge density in the benzene ring rather than the nitro group resulting in stabilization of the benzene ring π orbitals in comparison to the neutral molecule. Time dependent density functional theory computations are found to describe the experimental spectra well with respect to energies, relative intensities and nature of the observed transitions in terms of valence, Rydberg or charge transfer type. New insights into the interpretation of 1B2u←1A1g and 1B1u←1A1g shifted benzene transitions in light of the present computational calculations are presented. The first few members of the ns, np and nd type Rydberg series in nitrobenzene, converging to the first six ionization potentials, identified in the spectra as weak but sharp peaks are reported for the first time. In general, transitions to the lowest three unoccupied molecular orbitals 4b1, 3a2 and 5b1 are valence or charge transfer in nature, while excitations to higher orbitals are predominantly Rydberg in nature. This work presents a consolidated experimental study and theoretical interpretation of the electronic absorption spectrum of nitrobenzene.

Total photoionization cross-sections of excited electronic states by the algebraic diagrammatic construction-Stieltjes-Lanczos method.

PubMed

Ruberti, M; Yun, R; Gokhberg, K; Kopelke, S; Cederbaum, L S; Tarantelli, F; Averbukh, V

2014-05-14

Here, we extend the L2 ab initio method for molecular photoionization cross-sections introduced in Gokhberg et al. [J. Chem. Phys. 130, 064104 (2009)] and benchmarked in Ruberti et al. [J. Chem. Phys. 139, 144107 (2013)] to the calculation of total photoionization cross-sections of molecules in electronically excited states. The method is based on the ab initio description of molecular electronic states within the many-electron Green's function approach, known as algebraic diagrammatic construction (ADC), and on the application of Stieltjes-Chebyshev moment theory to Lanczos pseudospectra of the ADC electronic Hamiltonian. The intermediate state representation of the dipole operator in the ADC basis is used to compute the transition moments between the excited states of the molecule. We compare the results obtained using different levels of the many-body theory, i.e., ADC(1), ADC(2), and ADC(2)x for the first two excited states of CO, N2, and H2O both at the ground state and the excited state equilibrium or saddle point geometries. We find that the single excitation ADC(1) method is not adequate even at the qualitative level and that the inclusion of double electronic excitations for description of excited state photoionization is essential. Moreover, we show that the use of the extended ADC(2)x method leads to a substantial systematic difference from the strictly second-order ADC(2). Our calculations demonstrate that a theoretical modelling of photoionization of excited states requires an intrinsically double excitation theory with respect to the ground state and cannot be achieved by the standard single excitation methods with the ground state as a reference.

Total photoionization cross-sections of excited electronic states by the algebraic diagrammatic construction-Stieltjes-Lanczos method

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

Ruberti, M.; Yun, R.; Averbukh, V.

2014-05-14

Here, we extend the L{sup 2} ab initio method for molecular photoionization cross-sections introduced in Gokhberg et al. [J. Chem. Phys. 130, 064104 (2009)] and benchmarked in Ruberti et al. [J. Chem. Phys. 139, 144107 (2013)] to the calculation of total photoionization cross-sections of molecules in electronically excited states. The method is based on the ab initio description of molecular electronic states within the many-electron Green's function approach, known as algebraic diagrammatic construction (ADC), and on the application of Stieltjes-Chebyshev moment theory to Lanczos pseudospectra of the ADC electronic Hamiltonian. The intermediate state representation of the dipole operator in themore » ADC basis is used to compute the transition moments between the excited states of the molecule. We compare the results obtained using different levels of the many-body theory, i.e., ADC(1), ADC(2), and ADC(2)x for the first two excited states of CO, N{sub 2}, and H{sub 2}O both at the ground state and the excited state equilibrium or saddle point geometries. We find that the single excitation ADC(1) method is not adequate even at the qualitative level and that the inclusion of double electronic excitations for description of excited state photoionization is essential. Moreover, we show that the use of the extended ADC(2)x method leads to a substantial systematic difference from the strictly second-order ADC(2). Our calculations demonstrate that a theoretical modelling of photoionization of excited states requires an intrinsically double excitation theory with respect to the ground state and cannot be achieved by the standard single excitation methods with the ground state as a reference.« less

System and method for characterizing voiced excitations of speech and acoustic signals, removing acoustic noise from speech, and synthesizing speech

DOEpatents

Burnett, Greg C.; Holzrichter, John F.; Ng, Lawrence C.

2002-01-01

Low power EM waves are used to detect motions of vocal tract tissues of the human speech system before, during, and after voiced speech. A voiced excitation function is derived. The excitation function provides speech production information to enhance speech characterization and to enable noise removal from human speech.

Production of vibrationally excited N 2 by electron impact

NASA Astrophysics Data System (ADS)

Campbell, L.; Brunger, M. J.; Cartwright, D. C.; Teubner, P. J. O.

2004-08-01

Energy transfer from electrons to neutral gases and ions is one of the dominant electron cooling processes in the ionosphere, and the role of vibrationally excited N 2 in this is particularly significant. We report here the results from a new calculation of electron energy transfer rates ( Q) for vibrational excitation of N 2, as a function of the electron temperature Te. The present study was motivated by the development of a new cross-section compilation for vibrational excitation processes in N 2 which supercedes those used in the earlier calculations of the electron energy transfer rates. We show that the energy dependence and magnitude of these cross sections, particularly in the region of the well-known 2Π g resonance in N 2, significantly affect the calculated values of Q. A detailed comparison between the current and previous calculated electron energy transfer rates is made and coefficients are provided so that these rates for transitions from level 0 to levels 1-10 can be calculated for electron temperatures less than 6000 K.

Energy-filtered cold electron transport at room temperature.

PubMed

Bhadrachalam, Pradeep; Subramanian, Ramkumar; Ray, Vishva; Ma, Liang-Chieh; Wang, Weichao; Kim, Jiyoung; Cho, Kyeongjae; Koh, Seong Jin

2014-09-10

Fermi-Dirac electron thermal excitation is an intrinsic phenomenon that limits functionality of various electron systems. Efforts to manipulate electron thermal excitation have been successful when the entire system is cooled to cryogenic temperatures, typically <1 K. Here we show that electron thermal excitation can be effectively suppressed at room temperature, and energy-suppressed electrons, whose energy distribution corresponds to an effective electron temperature of ~45 K, can be transported throughout device components without external cooling. This is accomplished using a discrete level of a quantum well, which filters out thermally excited electrons and permits only energy-suppressed electrons to participate in electron transport. The quantum well (~2 nm of Cr2O3) is formed between source (Cr) and tunnelling barrier (SiO2) in a double-barrier-tunnelling-junction structure having a quantum dot as the central island. Cold electron transport is detected from extremely narrow differential conductance peaks in electron tunnelling through CdSe quantum dots, with full widths at half maximum of only ~15 mV at room temperature.

Study of cumulative fatigue damage detection for used parts with nonlinear output frequency response functions based on NARMAX modelling

NASA Astrophysics Data System (ADS)

Huang, Honglan; Mao, Hanying; Mao, Hanling; Zheng, Weixue; Huang, Zhenfeng; Li, Xinxin; Wang, Xianghong

2017-12-01

Cumulative fatigue damage detection for used parts plays a key role in the process of remanufacturing engineering and is related to the service safety of the remanufactured parts. In light of the nonlinear properties of used parts caused by cumulative fatigue damage, the based nonlinear output frequency response functions detection approach offers a breakthrough to solve this key problem. First, a modified PSO-adaptive lasso algorithm is introduced to improve the accuracy of the NARMAX model under impulse hammer excitation, and then, an effective new algorithm is derived to estimate the nonlinear output frequency response functions under rectangular pulse excitation, and a based nonlinear output frequency response functions index is introduced to detect the cumulative fatigue damage in used parts. Then, a novel damage detection approach that integrates the NARMAX model and the rectangular pulse is proposed for nonlinear output frequency response functions identification and cumulative fatigue damage detection of used parts. Finally, experimental studies of fatigued plate specimens and used connecting rod parts are conducted to verify the validity of the novel approach. The obtained results reveal that the new approach can detect cumulative fatigue damages of used parts effectively and efficiently and that the various values of the based nonlinear output frequency response functions index can be used to detect the different fatigue damages or working time. Since the proposed new approach can extract nonlinear properties of systems by only a single excitation of the inspected system, it shows great promise for use in remanufacturing engineering applications.

Towards time-dependent current-density-functional theory in the non-linear regime

NASA Astrophysics Data System (ADS)

Escartín, J. M.; Vincendon, M.; Romaniello, P.; Dinh, P. M.; Reinhard, P.-G.; Suraud, E.

2015-02-01

Time-Dependent Density-Functional Theory (TDDFT) is a well-established theoretical approach to describe and understand irradiation processes in clusters and molecules. However, within the so-called adiabatic local density approximation (ALDA) to the exchange-correlation (xc) potential, TDDFT can show insufficiencies, particularly in violently dynamical processes. This is because within ALDA the xc potential is instantaneous and is a local functional of the density, which means that this approximation neglects memory effects and long-range effects. A way to go beyond ALDA is to use Time-Dependent Current-Density-Functional Theory (TDCDFT), in which the basic quantity is the current density rather than the density as in TDDFT. This has been shown to offer an adequate account of dissipation in the linear domain when the Vignale-Kohn (VK) functional is used. Here, we go beyond the linear regime and we explore this formulation in the time domain. In this case, the equations become very involved making the computation out of reach; we hence propose an approximation to the VK functional which allows us to calculate the dynamics in real time and at the same time to keep most of the physics described by the VK functional. We apply this formulation to the calculation of the time-dependent dipole moment of Ca, Mg and Na2. Our results show trends similar to what was previously observed in model systems or within linear response. In the non-linear domain, our results show that relaxation times do not decrease with increasing deposited excitation energy, which sets some limitations to the practical use of TDCDFT in such a domain of excitations.

Towards time-dependent current-density-functional theory in the non-linear regime.

PubMed

Escartín, J M; Vincendon, M; Romaniello, P; Dinh, P M; Reinhard, P-G; Suraud, E

2015-02-28

Time-Dependent Density-Functional Theory (TDDFT) is a well-established theoretical approach to describe and understand irradiation processes in clusters and molecules. However, within the so-called adiabatic local density approximation (ALDA) to the exchange-correlation (xc) potential, TDDFT can show insufficiencies, particularly in violently dynamical processes. This is because within ALDA the xc potential is instantaneous and is a local functional of the density, which means that this approximation neglects memory effects and long-range effects. A way to go beyond ALDA is to use Time-Dependent Current-Density-Functional Theory (TDCDFT), in which the basic quantity is the current density rather than the density as in TDDFT. This has been shown to offer an adequate account of dissipation in the linear domain when the Vignale-Kohn (VK) functional is used. Here, we go beyond the linear regime and we explore this formulation in the time domain. In this case, the equations become very involved making the computation out of reach; we hence propose an approximation to the VK functional which allows us to calculate the dynamics in real time and at the same time to keep most of the physics described by the VK functional. We apply this formulation to the calculation of the time-dependent dipole moment of Ca, Mg and Na2. Our results show trends similar to what was previously observed in model systems or within linear response. In the non-linear domain, our results show that relaxation times do not decrease with increasing deposited excitation energy, which sets some limitations to the practical use of TDCDFT in such a domain of excitations.

Transient extracellular application of gold nanostars increases hippocampal neuronal activity.

PubMed

Salinas, Kirstie; Kereselidze, Zurab; DeLuna, Frank; Peralta, Xomalin G; Santamaria, Fidel

2014-08-20

With the increased use of nanoparticles in biomedical applications there is a growing need to understand the effects that nanoparticles may have on cell function. Identifying these effects and understanding the mechanism through which nanoparticles interfere with the normal functioning of a cell is necessary for any therapeutic or diagnostic application. The aim of this study is to evaluate if gold nanoparticles can affect the normal function of neurons, namely their activity and coding properties. We synthesized star shaped gold nanoparticles of 180 nm average size. We applied the nanoparticles to acute mouse hippocampal slices while recording the action potentials from single neurons in the CA3 region. Our results show that CA3 hippocampal neurons increase their firing rate by 17% after the application of gold nanostars. The increase in excitability lasted for as much as 50 minutes after a transient 5 min application of the nanoparticles. Further analyses of the action potential shape and computational modeling suggest that nanoparticles block potassium channels responsible for the repolarization of the action potentials, thus allowing the cell to increase its firing rate. Our results show that gold nanoparticles can affect the coding properties of neurons by modifying their excitability.

Low-lying excited states by constrained DFT.

PubMed

Ramos, Pablo; Pavanello, Michele

2018-04-14

Exploiting the machinery of Constrained Density Functional Theory (CDFT), we propose a variational method for calculating low-lying excited states of molecular systems. We dub this method eXcited CDFT (XCDFT). Excited states are obtained by self-consistently constraining a user-defined population of electrons, N c , in the virtual space of a reference set of occupied orbitals. By imposing this population to be N c = 1.0, we computed the first excited state of 15 molecules from a test set. Our results show that XCDFT achieves an accuracy in the predicted excitation energy only slightly worse than linear-response time-dependent DFT (TDDFT), but without incurring into problems of variational collapse typical of the more commonly adopted ΔSCF method. In addition, we selected a few challenging processes to test the limits of applicability of XCDFT. We find that in contrast to TDDFT, XCDFT is capable of reproducing energy surfaces featuring conical intersections (azobenzene and H 3 ) with correct topology and correct overall energetics also away from the intersection. Venturing to condensed-phase systems, XCDFT reproduces the TDDFT solvatochromic shift of benzaldehyde when it is embedded by a cluster of water molecules. Thus, we find XCDFT to be a competitive method among single-reference methods for computations of excited states in terms of time to solution, rate of convergence, and accuracy of the result.

Transition rate diagrams - A new approach to the study of selective excitation processes: The spectrum of manganese in a Grimm-type glow discharge

NASA Astrophysics Data System (ADS)

Weiss, Zdeněk; Steers, Edward B. M.; Pickering, Juliet C.; Mushtaq, Sohail

2014-02-01

The emission spectra of manganese observed using a Grimm-type glow discharge in pure argon, argon with 0.3% v/v hydrogen and pure neon were studied in order to identify major excitation and ionization processes of manganese in the plasma. A new procedure is proposed, in which each observed emission line is associated with the corresponding transition between different states of the Mn atom or Mn ion, and, by considering all the observed transitions from and into a specific state, a measure of the total rate is determined at which this state is radiatively populated and depopulated. These resulting population/depopulation rates are then plotted as function of level energy. Such plots, called here “transition rate diagrams”, show the role of individual states in the formation of the observed spectrum and can be used to identify possible selective excitation processes. Also, cascade excitation by radiative decay of higher excited states can be conveniently evaluated in this way. A detailed description of the observed Mn I and Mn II spectra is given for Ar, Ar-H2 and Ne plasmas and relevant excitation/ionization mechanisms are discussed. Matrix effects in analysis of manganese by glow discharge spectroscopy are discussed. A list of important Mn I and Mn II lines excited in the glow discharge plasma is given.

Electron Transport and Nonlinear Optical Properties of Substituted Aryldimesityl Boranes: A DFT Study

PubMed Central

Pandith, Altaf Hussain; Islam, Nasarul

2014-01-01

A comprehensive theoretical study was carried out on a series of aryldimesityl borane (DMB) derivatives using Density Functional theory. Optimized geometries and electronic parameters like electron affinity, reorganization energy, frontiers molecular contours, polarizability and hyperpolarizability have been calculated by employing B3PW91/6-311++G (d, p) level of theory. Our results show that the Hammett function and geometrical parameters correlates well with the reorganization energies and hyperpolarizability for the series of DMB derivatives studied in this work. The orbital energy study reveals that the electron releasing substituents increase the LUMO energies and electron withdrawing substituents decrease the LUMO energies, reflecting the electron transport character of aryldimesityl borane derivatives. From frontier molecular orbitals diagram it is evident that mesityl rings act as the donor, while the phenylene and Boron atom appear as acceptors in these systems. The calculated hyperpolarizability of secondary amine derivative of DMB is 40 times higher than DMB (1). The electronic excitation contributions to the hyperpolarizability studied by using TDDFT calculation shows that hyperpolarizability correlates well with dipole moment in ground and excited state and excitation energy in terms of the two-level model. Thus the results of these calculations can be helpful in designing the DMB derivatives for efficient electron transport and nonlinear optical material by appropriate substitution with electron releasing or withdrawing substituents on phenyl ring of DMB system. PMID:25479382

In vivo, two-color multiphoton microscopy using a femtosecond diamond Raman laser

NASA Astrophysics Data System (ADS)

Jarrett, Jeremy W.; Perillo, Evan P.; Hassan, Ahmed; Miller, David R.; Dunn, Andrew K.

2018-02-01

Multiphoton microscopy is an essential tool for detailed study of neurovascular structure and function. Wavelength mixing of synchronized laser sources—two-color multiphoton microscopy—increases the spectral window of excitable fluorophores without the need for wavelength tuning. However, implementation of two-color microscopy requires a dual output laser source, which is typically costly and complicated. We have developed a relatively simple and low-cost diamond Raman laser pumped with a ytterbium fiber amplifier. The dual output system generates excitation light at both 1060 nm (pump wavelength) and 1250 nm (first Stokes emission of diamond laser) which, when temporally and spatially overlapped, yield an effective two-color excitation wavelength of 1160 nm. This source provides an almost complete coverage of fluorophores excitable within the range of 1000-1300 nm. When compared with 1060 nm excitation, twocolor excitation at 1160 nm offers a 90% increase in signal for many far-red emitting fluorescent proteins (e.g. tdKatushka2). We demonstrate multicolor imaging of tdKatushka2 and Hoechst 33342 via simultaneous two-color twophoton, and two-color three-photon microscopy in engineered 3-D multicellular spheroids. Additionally, we show that this laser system is capable of in vivo imaging in mouse cortex to nearly 1 mm in depth with two-color excitation. This system can also be used to excite genetically encoded calcium indicators (e.g. RCaMP and GCaMP), which will be paramount in studying neuronal activity.

Pair-correlation function of a metastable helium Bose-Einstein condensate

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

Zin, Pawel; Trippenbach, Marek; Gajda, Mariusz

2004-02-01

The pair-correlation function is one of the basic quantities to characterize the coherence properties of a Bose-Einstein condensate. We calculate this function in the experimentally important case of a zero temperature Bose-Einstein condensate in a metastable triplet helium state using the variational method with a pair-excitation ansatz. We compare our result with a pair-correlation function obtained for the hard-sphere potential with the same scattering length. Both functions are practically indistinguishable for distances greater than the scattering length. At smaller distances, due to interatomic interactions, the helium condensate shows strong correlations.

Self-potential response to periodic pumping test: a numerical study

NASA Astrophysics Data System (ADS)

Konosavsky, Pavel; Maineult, Alexis; Narbut, Mikhail; Titov, Konstantin

2017-09-01

We numerically model self-potential responses associated with periodic pumping test experiments by sequential calculation of the hydraulic response and the coupled electrical potential. We assume the pumping test experiments with a fully saturated confined aquifer. Application of different excitation functions leads to quasi-linear trends in electrical records whose direction and intensity depend on the form of the excitation function. The hydraulic response is phase shifted compared to the excitation function; the phase shift increases quasi-linearly with the distance from the pumping well. For the electrical signals, we investigated separately the cases of conducting and insulating casings of the pumping well. For the conducting casing the electrical signals are larger in magnitude than that for the insulating casing; they reproduce the drawdown signals in the pumping well at any distance from the well and exhibit any phase shift with the increased distance. For the insulating casing, the electrical signals are phase shifted and their shape depends on the distance from the pumping well. Three characteristic regimes were found for the phase shift, φ, with the increased distance and for various hydraulic diffusivity values. At small distances φ increases quasi-linearly; at intermediate distances φ attends the value of π/2 and stay about this value (for relatively small diffusivity values); and at large distances φ attends the value of π and, stay about this value at larger distances. This behaviour of the electrical signals can be explained by two electrical sources of reverse polarity. They are (i) linear, time independent, and located at the pumping interval of the well; and (ii) volumetric, time dependent, with maximum value located in the aquifer at the distance corresponding to maximum variation of the hydraulic head magnitude with time. We also model the variation of the amplitude and phase of the hydraulic and electrical signals with increased excitation function period, and we show the characteristic periods corresponding to transition of the periodic pumping test regime to the classical pumping test regime, when the excitation function is considered as the step-function. This transition depends on the distance from the pumping well and the hydraulic diffusivity value of aquifer. Finally, with this modelling of saturated flow we reproduced in sufficient details the field data previously obtained by Maineult et al.

Probabilistic solutions of nonlinear oscillators excited by combined colored and white noise excitations

NASA Astrophysics Data System (ADS)

Siu-Siu, Guo; Qingxuan, Shi

2017-03-01

In this paper, single-degree-of-freedom (SDOF) systems combined to Gaussian white noise and Gaussian/non-Gaussian colored noise excitations are investigated. By expressing colored noise excitation as a second-order filtered white noise process and introducing colored noise as an additional state variable, the equation of motion for SDOF system under colored noise is then transferred artificially to multi-degree-of-freedom (MDOF) system under white noise excitations with four-coupled first-order differential equations. As a consequence, corresponding Fokker-Planck-Kolmogorov (FPK) equation governing the joint probabilistic density function (PDF) of state variables increases to 4-dimension (4-D). Solution procedure and computer programme become much more sophisticated. The exponential-polynomial closure (EPC) method, widely applied for cases of SDOF systems under white noise excitations, is developed and improved for cases of systems under colored noise excitations and for solving the complex 4-D FPK equation. On the other hand, Monte Carlo simulation (MCS) method is performed to test the approximate EPC solutions. Two examples associated with Gaussian and non-Gaussian colored noise excitations are considered. Corresponding band-limited power spectral densities (PSDs) for colored noise excitations are separately given. Numerical studies show that the developed EPC method provides relatively accurate estimates of the stationary probabilistic solutions, especially the ones in the tail regions of the PDFs. Moreover, statistical parameter of mean-up crossing rate (MCR) is taken into account, which is important for reliability and failure analysis. Hopefully, our present work could provide insights into the investigation of structures under random loadings.

Excitations of single-beauty hadrons

NASA Astrophysics Data System (ADS)

Burch, Tommy; Hagen, Christian; Lang, Christian B.; Limmer, Markus; Schäfer, Andreas

2009-01-01

In this work we study the predominantly orbital and radial excitations of hadrons containing a single heavy quark. We present meson and baryon mass splittings and ratios of meson decay constants (e.g., fBs/fB and fBs'/fBs) resulting from quenched and dynamical two-flavor configurations. Light quarks are simulated using the chirally improved lattice Dirac operator at valence masses as light as Mπ≈350MeV. The heavy quark is approximated by a static propagator, appropriate for the b quark on our lattices (1/ã1-2GeV). We also include some preliminary calculations of the O(1/mQ) kinetic corrections to the states, showing, in the process, a viable way of applying the variational method to three-point functions involving excited states. We compare our results with recent experimental findings.

Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons

PubMed Central

Soavi, Giancarlo; Dal Conte, Stefano; Manzoni, Cristian; Viola, Daniele; Narita, Akimitsu; Hu, Yunbin; Feng, Xinliang; Hohenester, Ulrich; Molinari, Elisa; Prezzi, Deborah; Müllen, Klaus; Cerullo, Giulio

2016-01-01

Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron–hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton–exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ≈250 meV, in very good agreement with theoretical results from quantum Monte Carlo simulations. These observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics. PMID:26984281

Isgur-Karl model revisited

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

Galeta, Leonardo; Pirjol, Dan; Schat, Carlos

2009-12-01

We show how to match the Isgur-Karl model to the spin-flavor quark operator expansion used in the 1/N{sub c} studies of the nonstrange negative parity L=1 excited baryons. Using the transformation properties of states and interactions under the permutation group S{sub 3} we are able to express the operator coefficients as overlap integrals, without making any assumption on the spatial dependence of the quark wave functions. The general mass operator leads to parameter free mass relations and constraints on the mixing angles that are valid beyond the usual harmonic oscillator approximation. The Isgur-Karl model with harmonic oscillator wave functions providesmore » a simple counterexample that demonstrates explicitly that the alternative operator basis for the 1/N{sub c} expansion for excited baryons recently proposed by Matagne and Stancu is incomplete.« less

Macular autofluorescence in eyes with cystoid macula edema, detected with 488 nm-excitation but not with 580 nm-excitation.

PubMed

Bessho, Kenichiro; Gomi, Fumi; Harino, Seiyo; Sawa, Miki; Sayanagi, Kaori; Tsujikawa, Motokazu; Tano, Yasuo

2009-06-01

Fundus autofluorescence (AF) derives from lipofuscin in the retinal pigment epithelium (RPE). Because lipofuscin is a by-product of phagocytosis of photoreceptors by RPE, AF imaging is expected to describe some functional aspect of the retina. In this study we report distribution of AF in patients showing macular edema. Three eyes with diabetic macular edema (DME) and 11 with retinal vein occlusion (RVO), associated with macular edema (ME) were examined. ME was determined by standard fundus examination, fluorescein angiography (FA) and optical coherence tomography (OCT). AF was recorded using a Heidelberg confocal scanning laser ophthalmoscope (cSLO) with 488 nm laser exciter (488 nm-AF), and a conventional Topcon fundus camera with halogen lamp exciter and 580 nm band-pass filter (580 nm-AF). Color fundus picture, FA image and these two AF images were analyzed by superimposing all images. All subjects presented cystoid macular edema (CME) with petaloid pattern hyperfluorescence in FA. In 488 nm-AF, all eyes (100%) showed macular autofluorescence of a similar shape to that of the CME in FA. In contrast, in 580 nm-AF only one eye (7%) presented this corresponding petaloid-shaped autofluorescence. In all cases, peripheral retinal edemas did not show autofluorescence corresponding to the leakage in FA. In eyes with CME, analogous hyperautofluorescence to the CME was always observed in 488 nm-AF, while it was rarely observed in 580 nm-AF. Moreover, this CME hyperautofluorescence was only seen in the macular area. We hypothesize that autofluorescence from CME may be considered as a "pseudo" or "relative" autofluorescence, due to macular stretching following CME that may result in lateral displacement of macular pigments (MPs) and subsequent reduction of MPs density, as MPs block 488 nm-AF more intensely than 580 nm-AF. Although this phenomenon may not directly indicate change of RPE function, it may be used as a method to assess or track CME non-invasively.

Ground and excited states of CaSH through electron propagator calculations

NASA Astrophysics Data System (ADS)

Ortiz, J. V.

1990-05-01

Electron propagator calculations of electron affinities of CaSH + produce ground and excited state energies at the optimized, C s minimum of the neutral ground state and at a C ∞v geometry. Feynman-Dyson amplitudes (FDAs) describe the distribution of the least bound electron in various states. The neutral ground state differs from the cation by the occupation of a one-electron state dominated by Ca s functions. Described by FDAs with Ca-S π pseudosymmetry, corresponding excited states have unpaired electrons in orbitals displaying interference between Ca p and d functions. Above these lies a σ pseudosymmetry FDA with principal contributions from Ca d functions. Two FDAs with σ pseudosymmetry follow. Higher excited states exhibit considerable delocalization onto S.

Hidden multiparticle excitation in a weakly interacting Bose-Einstein condensate

NASA Astrophysics Data System (ADS)

Watabe, Shohei

2018-03-01

We investigate multiparticle excitation effect on a collective density excitation as well as a single-particle excitation in a weakly interacting Bose-Einstein condensate (BEC). We find that although the weakly interacting BEC offers weak multiparticle excitation spectrum at low temperatures, this multiparticle excitation effect may not remain hidden, but emerges as bimodality in the density response function through the single-particle excitation. Identification of spectra in the BEC between the single-particle excitation and the density excitation is also assessed at nonzero temperatures, which has been known to be unique nature in the BEC at absolute zero temperature.

Cluster decomposition of full configuration interaction wave functions: A tool for chemical interpretation of systems with strong correlation

NASA Astrophysics Data System (ADS)

Lehtola, Susi; Tubman, Norm M.; Whaley, K. Birgitta; Head-Gordon, Martin

2017-10-01

Approximate full configuration interaction (FCI) calculations have recently become tractable for systems of unforeseen size, thanks to stochastic and adaptive approximations to the exponentially scaling FCI problem. The result of an FCI calculation is a weighted set of electronic configurations, which can also be expressed in terms of excitations from a reference configuration. The excitation amplitudes contain information on the complexity of the electronic wave function, but this information is contaminated by contributions from disconnected excitations, i.e., those excitations that are just products of independent lower-level excitations. The unwanted contributions can be removed via a cluster decomposition procedure, making it possible to examine the importance of connected excitations in complicated multireference molecules which are outside the reach of conventional algorithms. We present an implementation of the cluster decomposition analysis and apply it to both true FCI wave functions, as well as wave functions generated from the adaptive sampling CI algorithm. The cluster decomposition is useful for interpreting calculations in chemical studies, as a diagnostic for the convergence of various excitation manifolds, as well as as a guidepost for polynomially scaling electronic structure models. Applications are presented for (i) the double dissociation of water, (ii) the carbon dimer, (iii) the π space of polyacenes, and (iv) the chromium dimer. While the cluster amplitudes exhibit rapid decay with an increasing rank for the first three systems, even connected octuple excitations still appear important in Cr2, suggesting that spin-restricted single-reference coupled-cluster approaches may not be tractable for some problems in transition metal chemistry.

Electron impact excitation of highly charged sodium-like ions

NASA Technical Reports Server (NTRS)

Blaha, M.; Davis, J.

1978-01-01

Optical transition probabilities and electron collision strengths for Ca X, Fe XVI, Zn XX, Kr XXVI and Mo XXXII are calculated for transitions between n equal to 3 and n equal to 4 levels. The calculations neglect relativistic effects on the radial functions. A semi-empirical approach provides wave functions of the excited states; a distorted wave function without exchange is employed to obtain the excitation cross sections. The density dependence of the relative intensities of certain emission lines in the sodium isoelectronic sequence is also discussed.

Computing correct truncated excited state wavefunctions

NASA Astrophysics Data System (ADS)

Bacalis, N. C.; Xiong, Z.; Zang, J.; Karaoulanis, D.

2016-12-01

We demonstrate that, if a wave function's truncated expansion is small, then the standard excited states computational method, of optimizing one "root" of a secular equation, may lead to an incorrect wave function - despite the correct energy according to the theorem of Hylleraas, Undheim and McDonald - whereas our proposed method [J. Comput. Meth. Sci. Eng. 8, 277 (2008)] (independent of orthogonality to lower lying approximants) leads to correct reliable small truncated wave functions. The demonstration is done in He excited states, using truncated series expansions in Hylleraas coordinates, as well as standard configuration-interaction truncated expansions.

Design, assembly, and metrology of an oil-immersion microscope objective with long working distance

NASA Astrophysics Data System (ADS)

Peng, Wei-Jei; Lin, Wen-Lung; Kuo, Hui-Jean; Ho, Cheng-Fang; Hsu, Wei-Yao

2016-10-01

The design, tolerance sensitivity reduction, assembly, and optical bench test for an oil-immersion microscope objective with long working distance employed in a lattice light-sheet microscope is presented in this paper. In this application, the orthogonal excitation and detection objectives are dipped in an oil medium. The excitation objective focuses the incident laser beam to generate fluorescence on specimen for collecting by detection objective. The excitation objective is custom-designed to meet the requirement specification such as oil-immersion, the long working distance, and numerical aperture (NA) of 0.5, etc. To produce an acceptable point spread function (PSF) for effective excitation, the performance of the objective needs to be close to diffraction limit. Because the tolerance of the modulation transfer function (MTF) is more and more sensitive at higher spatial frequency, it is extremely critical to keep the performance after manufacture. Consequently, an insensitive optical design is very important for relaxing tolerance. We compare the design with and without tolerance sensitivity reduction, and the as-built MTF shows the result. Furthermore, the method for sensitivity reduction is presented. The opto-mechanical design and assembly method are also discussed. Eventually, the objective with five spherical lenses was fabricated. In optical bench test, the depth of the oil is sensitive to MTF, and it leads to the complicated adjustment. For solving this issue, we made an index-matching lens to replace oil for measurement easily. Finally, the measured MTF of the excitation objective can accomplish the requirement specification and successfully employed in a lattice light-sheet microscope.

Portable vibration exciter

NASA Technical Reports Server (NTRS)

Beecher, L. C.; Williams, F. T.

1970-01-01

Gas-driven vibration exciter produces a sinusoidal excitation function controllable in frequency and in amplitude. It allows direct vibration testing of components under normal loads, removing the possibility of component damage due to high static pressure.

Predicting Near Edge X-ray Absorption Spectra with the Spin-Free Exact-Two-Component Hamiltonian and Orthogonality Constrained Density Functional Theory.

PubMed

Verma, Prakash; Derricotte, Wallace D; Evangelista, Francesco A

2016-01-12

Orthogonality constrained density functional theory (OCDFT) provides near-edge X-ray absorption (NEXAS) spectra of first-row elements within one electronvolt from experimental values. However, with increasing atomic number, scalar relativistic effects become the dominant source of error in a nonrelativistic OCDFT treatment of core-valence excitations. In this work we report a novel implementation of the spin-free exact-two-component (X2C) one-electron treatment of scalar relativistic effects and its combination with a recently developed OCDFT approach to compute a manifold of core-valence excited states. The inclusion of scalar relativistic effects in OCDFT reduces the mean absolute error of second-row elements core-valence excitations from 10.3 to 2.3 eV. For all the excitations considered, the results from X2C calculations are also found to be in excellent agreement with those from low-order spin-free Douglas-Kroll-Hess relativistic Hamiltonians. The X2C-OCDFT NEXAS spectra of three organotitanium complexes (TiCl4, TiCpCl3, TiCp2Cl2) are in very good agreement with unshifted experimental results and show a maximum absolute error of 5-6 eV. In addition, a decomposition of the total transition dipole moment into partial atomic contributions is proposed and applied to analyze the nature of the Ti pre-edge transitions in the three organotitanium complexes.

Correlation of near-infrared spectroscopy and transcranial magnetic stimulation of the motor cortex in overt reading and musical tasks.

PubMed

Lo, Y L; Zhang, H H; Wang, C C; Chin, Z Y; Fook-Chong, S; Gabriel, C; Guan, C T

2009-01-01

In overt reading and singing tasks, actual vocalization of words in a rhythmic fashion is performed. During execution of these tasks, the role of underlying vascular processes in relation to cortical excitability changes in a spatial manner is uncertain. Our objective was to investigate cortical excitability changes during reading and singing with transcranial magnetic stimulation (TMS), as well as vascular changes with nearinfrared spectroscopy (NIRS). Findings with TMS and NIRS were correlated. TMS and NIRS recordings were performed in 5 normal subjects while they performed reading and singing tasks separately. TMS was applied over the left motor cortex at 9 positions 2.5 cm apart. NIRS recordings were made over these identical positions. Although both TMS and NIRS showed significant mean cortical excitability and hemodynamic changes from baseline during vocalization tasks, there was no significant spatial correlation of these changes evaluated with the 2 techniques over the left motor cortex. Our findings suggest that increased left-sided cortical excitability from overt vocalization tasks in the corresponding "hand area" were the result of "functional connectivity," rather than an underlying "vascular overflow mechanism" from the adjacent speech processing or face/mouth areas. Our findings also imply that functional neurophysiological and vascular methods may evaluate separate underlying processes, although subjects performed identical vocalization tasks. Future research combining similar methodologies should embrace this aspect and harness their separate capabilities.

Chemical Approaches for Structure and Function of RNA in Postgenomic Era

PubMed Central

Ro-Choi, Tae Suk; Choi, Yong Chun

2012-01-01

In the study of cellular RNA chemistry, a major thrust of research focused upon sequence determinations for decades. Structures of snRNAs (4.5S RNA I (Alu), U1, U2, U3, U4, U5, and U6) were determined at Baylor College of Medicine, Houston, Tex, in an earlier time of pregenomic era. They show novel modifications including base methylation, sugar methylation, 5′-cap structures (types 0–III) and sequence heterogeneity. This work offered an exciting problem of posttranscriptional modification and underwent numerous significant advances through technological revolutions during pregenomic, genomic, and postgenomic eras. Presently, snRNA research is making progresses involved in enzymology of snRNA modifications, molecular evolution, mechanism of spliceosome assembly, chemical mechanism of intron removal, high-order structure of snRNA in spliceosome, and pathology of splicing. These works are destined to reach final pathway of work “Function and Structure of Spliceosome” in addition to exciting new exploitation of other noncoding RNAs in all aspects of regulatory functions. PMID:22347623

Excitations in a spin-polarized two-dimensional electron gas

NASA Astrophysics Data System (ADS)

Kreil, Dominik; Hobbiger, Raphael; Drachta, Jürgen T.; Böhm, Helga M.

2015-11-01

A remarkably long-lived spin plasmon may exist in two-dimensional electron liquids with imbalanced spin-up and spin-down population. The predictions for this interesting mode by Agarwal et al. [Phys. Rev. B 90, 155409 (2014), 10.1103/PhysRevB.90.155409] are based on the random phase approximation. Here, we show how to account for spin-dependent correlations from known ground-state pair correlation functions and study the consequences on the various spin-dependent longitudinal response functions. The spin-plasmon dispersion relation and its critical wave vector for Landau damping by minority spins turn out to be significantly lower. We further demonstrate that spin-dependent effective interactions imply a rich structure in the excitation spectrum of the partially spin-polarized system. Most notably, we find a "magnetic antiresonance," where the imaginary part of both, the spin-spin as well as the density-spin response function vanish. The resulting minimum in the double-differential cross section is awaiting experimental confirmation.

Excited state characterization of carbonyl containing carotenoids: a comparison between single and multireference descriptions

NASA Astrophysics Data System (ADS)

Spezia, Riccardo; Knecht, Stefan; Mennucci, Benedetta

Carotenoids can play multiple roles in biological photoreceptors thanks to their rich photophysics. In the present work, we have investigated six of the most common carbonyl containing carotenoids: Echinenone, Canthaxanthin, Astaxanthin, Fucoxanthin, Capsanthin and Capsorubin. Their excitation properties are investigated by means of a hybrid density functional theory (DFT) and multireference configuration interaction (MRCI) approach to elucidate the role of the carbonyl group: the bright transition is of {\\pi}{\\pi}* character, as expected, but the presence of a C=O moiety reduces the energy of n{\\pi}* transitions which may become closer to the {\\pi}{\\pi}* transition, in particular as the conjugation chain decreases. This can be related to the presence of a low-lying charge transfer state typical of short carbonyl- containing carotenoids. The DFT/MRCI results are finally used to benchmark single- reference time-dependent DFT-based methods: among the investigated functionals, the meta- GGA (and in particular M11L and MN12L) functionals show to perform the best for all six investigated systems.

Electronic and transport properties of Cobalt-based valence tautomeric molecules and polymers

NASA Astrophysics Data System (ADS)

Chen, Yifeng; Calzolari, Arrigo; Buongiorno Nardelli, Marco

2011-03-01

The advancement of molecular spintronics requires further understandings of the fundamental electronic structures and transport properties of prototypical spintronics molecules and polymers. Here we present a density functional based theoretical study of the electronic structures of Cobalt-based valence tautomeric molecules Co III (SQ)(Cat)L Co II (SQ)2 L and their polymers, where SQ refers to the semiquinone ligand, and Cat the catecholate ligand, while L is a redox innocent backbone ligand. The conversion from low-spin Co III ground state to high-spin Co II excited state is realized by imposing an on-site potential U on the Co atom and elongating the Co-N bond. Transport properties are subsequently calculated by extracting electronic Wannier functions from these systems and computing the charge transport in the ballistic regime using a Non-Equilibrium Green's Function (NEGF) approach. Our transport results show distinct charge transport properties between low-spin ground state and high-spin excited state, hence suggesting potential spintronics devices from these molecules and polymers such as spin valves.

The Researches on Damage Detection Method for Truss Structures

NASA Astrophysics Data System (ADS)

Wang, Meng Hong; Cao, Xiao Nan

2018-06-01

This paper presents an effective method to detect damage in truss structures. Numerical simulation and experimental analysis were carried out on a damaged truss structure under instantaneous excitation. The ideal excitation point and appropriate hammering method were determined to extract time domain signals under two working conditions. The frequency response function and principal component analysis were used for data processing, and the angle between the frequency response function vectors was selected as a damage index to ascertain the location of a damaged bar in the truss structure. In the numerical simulation, the time domain signal of all nodes was extracted to determine the location of the damaged bar. In the experimental analysis, the time domain signal of a portion of the nodes was extracted on the basis of an optimal sensor placement method based on the node strain energy coefficient. The results of the numerical simulation and experimental analysis showed that the damage detection method based on the frequency response function and principal component analysis could locate the damaged bar accurately.

Novel use of UV broad-band excitation and stretched exponential function in the analysis of fluorescent dissolved organic matter: study of interaction between protein and humic-like components

NASA Astrophysics Data System (ADS)

Panigrahi, Suraj Kumar; Mishra, Ashok Kumar

2017-09-01

A combination of broad-band UV radiation (UV A and UV B; 250-400 nm) and a stretched exponential function (StrEF) has been utilised in efforts towards convenient and sensitive detection of fluorescent dissolved organic matter (FDOM). This approach enables accessing the gross fluorescence spectral signature of both protein-like and humic-like components in a single measurement. Commercial FDOM components are excited with the broad-band UV excitation; the variation of spectral profile as a function of varying component ratio is analysed. The underlying fluorescence dynamics and non-linear quenching of amino acid moieties are studied with the StrEF (exp(-V[Q] β )). The complex quenching pattern reflects the inner filter effect (IFE) as well as inter-component interactions. The inter-component interactions are essentially captured through the ‘sphere of action’ and ‘dark complex’ models. The broad-band UV excitation ascertains increased excitation energy, resulting in increased population density in the excited state and thereby resulting in enhanced sensitivity.

Chromophore twisting in the excited state of a photoswitchable fluorescent protein captured by time-resolved serial femtosecond crystallography

NASA Astrophysics Data System (ADS)

Coquelle, Nicolas; Sliwa, Michel; Woodhouse, Joyce; Schirò, Giorgio; Adam, Virgile; Aquila, Andrew; Barends, Thomas R. M.; Boutet, Sébastien; Byrdin, Martin; Carbajo, Sergio; de La Mora, Eugenio; Doak, R. Bruce; Feliks, Mikolaj; Fieschi, Franck; Foucar, Lutz; Guillon, Virginia; Hilpert, Mario; Hunter, Mark S.; Jakobs, Stefan; Koglin, Jason E.; Kovacsova, Gabriela; Lane, Thomas J.; Lévy, Bernard; Liang, Mengning; Nass, Karol; Ridard, Jacqueline; Robinson, Joseph S.; Roome, Christopher M.; Ruckebusch, Cyril; Seaberg, Matthew; Thepaut, Michel; Cammarata, Marco; Demachy, Isabelle; Field, Martin; Shoeman, Robert L.; Bourgeois, Dominique; Colletier, Jacques-Philippe; Schlichting, Ilme; Weik, Martin

2018-01-01

Chromophores absorb light in photosensitive proteins and thereby initiate fundamental biological processes such as photosynthesis, vision and biofluorescence. An important goal in their understanding is the provision of detailed structural descriptions of the ultrafast photochemical events that they undergo, in particular of the excited states that connect chemistry to biological function. Here we report on the structures of two excited states in the reversibly photoswitchable fluorescent protein rsEGFP2. We populated the states through femtosecond illumination of rsEGFP2 in its non-fluorescent off state and observed their build-up (within less than one picosecond) and decay (on the several picosecond timescale). Using an X-ray free-electron laser, we performed picosecond time-resolved crystallography and show that the hydroxybenzylidene imidazolinone chromophore in one of the excited states assumes a near-canonical twisted configuration halfway between the trans and cis isomers. This is in line with excited-state quantum mechanics/molecular mechanics and classical molecular dynamics simulations. Our new understanding of the structure around the twisted chromophore enabled the design of a mutant that displays a twofold increase in its off-to-on photoswitching quantum yield.

Relative energies and collisional kinetics of the B(. cap omega. = 1/2) and C(. cap omega. = 3/2) excited states of xenon fluoride as studied by laser-induced fluorescence

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

Gedanken, A.; Smith, A.L.

1981-09-17

A pulsed nitrogen laser photodissociated F/sub 2/ in the presence of Xe, and the resulting ground-state XeF was excited by a second pulsed, tunable dye laser in the 0,4 and 0,5 bands of the B(1/2)-X(1/2) transition. Both dispersed fluorescence spectra and tunable laser excitation spectra, taken by using a gated detection system, show that the C state is lower in energy than the lowest vibrational level of the B state. The ratio of fluorescence intensities in the C-A and B-X transitions was measured as a function of xenon and argon pressure. An analytical model was developed for the time dependencemore » of the B and C state concentrations after instantaneous excitation and in the presence of intersystem crossing, quenching, and radiative decay. Published rate constants for the excited state kinetics of XeF(B) and XeF(C) are reviewed, and model calculations of the measured intensity ratio are used to assess these rate constants.« less

The measurement of molecular fragments from DNA components using synchrotron radiation

NASA Astrophysics Data System (ADS)

Fujii, K.; Akamatsu, K.; Yokoya, A.

2003-03-01

Photon-stimulated desorption of positive ions from thin film DNA components, 2-deoxy- D-ribose, thymine and guanine, were investigated in the oxygen K-edge excitation region. H +, CH 2+, C 2H 2+, CHO +, C 3H 3+ and C 2HO + were desorbed mainly from the 2-deoxy- D-ribose thin film following oxygen K-edge excitation. The ion yields were obtained as a function of the photon energy. Each spectrum showed a prominent peak structure coinciding with the O 1 s→ σ∗(C-O) excitation energy. These results indicate that the observed ions are produced not only by direct photodecomposition but also by the impact of secondary electrons that the core excitation generates. On the other hand, H + has been observed by irradiation of thymine and guanine thin films, while only insignificant amounts of the other ions were observed. It is shown that the core excitation more drastically degraded the 2-deoxy- D-ribose molecule into small fragments than is the case with the nucleobases. The sugar moiety in DNA is likely to be one of the nor fragile molecular sites, conducive to a single-strand DNA break.

Chromophore twisting in the excited state of a photoswitchable fluorescent protein captured by time-resolved serial femtosecond crystallography

DOE PAGES

Coquelle, Nicolas; Sliwa, Michel; Woodhouse, Joyce; ...

2017-09-11

Chromophores absorb light in photosensitive proteins and thereby initiate fundamental biological processes such as photosynthesis, vision and biofluorescence. An important goal in their understanding is the provision of detailed structural descriptions of the ultrafast photochemical events that they undergo, in particular of the excited states that connect chemistry to biological function. Here in this paper we report on the structures of two excited states in the reversibly photoswitchable fluorescent protein rsEGFP2. We populated the states through femtosecond illumination of rsEGFP2 in its non-fluorescent off state and observed their build-up (within less than one picosecond) and decay (on the several picosecondmore » timescale). Using an X-ray free-electron laser, we performed picosecond time-resolved crystallography and show that the hydroxybenzylidene imidazolinone chromophore in one of the excited states assumes a near-canonical twisted configuration halfway between the trans and cis isomers. This is in line with excited-state quantum mechanics/molecular mechanics and classical molecular dynamics simulations. Our new understanding of the structure around the twisted chromophore enabled the design of a mutant that displays a twofold increase in its off-to-on photoswitching quantum yield.« less

Chromophore twisting in the excited state of a photoswitchable fluorescent protein captured by time-resolved serial femtosecond crystallography

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

Coquelle, Nicolas; Sliwa, Michel; Woodhouse, Joyce

Chromophores absorb light in photosensitive proteins and thereby initiate fundamental biological processes such as photosynthesis, vision and biofluorescence. An important goal in their understanding is the provision of detailed structural descriptions of the ultrafast photochemical events that they undergo, in particular of the excited states that connect chemistry to biological function. Here in this paper we report on the structures of two excited states in the reversibly photoswitchable fluorescent protein rsEGFP2. We populated the states through femtosecond illumination of rsEGFP2 in its non-fluorescent off state and observed their build-up (within less than one picosecond) and decay (on the several picosecondmore » timescale). Using an X-ray free-electron laser, we performed picosecond time-resolved crystallography and show that the hydroxybenzylidene imidazolinone chromophore in one of the excited states assumes a near-canonical twisted configuration halfway between the trans and cis isomers. This is in line with excited-state quantum mechanics/molecular mechanics and classical molecular dynamics simulations. Our new understanding of the structure around the twisted chromophore enabled the design of a mutant that displays a twofold increase in its off-to-on photoswitching quantum yield.« less

Combined TDDFT and AIM Insights into Photoinduced Excited State Intramolecular Proton Transfer (ESIPT) Mechanism in Hydroxyl- and Amino-Anthraquinone Solution.

PubMed

Zheng, Daoyuan; Zhang, Mingzhen; Zhao, Guangjiu

2017-10-23

Time-dependent density functional theory (TDDFT) and atoms in molecules (AIM) theory are combined to study the photoinduced excited state intramolecular proton transfer (ESIPT) dynamics for eight anthraquinones (AQs) derivatives in solution. The calculated absorption and emission spectra are consistent with the available experimental data, verifying the suitability of the theory selected. The systems with the excited-state exothermic proton transfer, such as 1-HAQ, 1,5-DHAQ and TFAQ, emit completely from transfer structure (T), while the reactions for those without ESIPT including 1,4-DHAQ and AAAQ appear to be endothermic. Three reaction properties of three systems (1,8-DHAQ, DCAQ and CAAQ) are between the exothermic and endothermic, sensitive to the solvent. Energy scanning shows that 1,4-DHAQ and AAAQ exhibit the higher ESIPT energy barriers compared to 1-HAQ, 1,5-DHAQ and TFAQ with the "barrierless" ESIPT process. The ESIPT process is facilitated by the strengthening of hydrogen bonds in excited state. With AIM theory, it is observed that the change in electrons density ρ(r) and potential energy density V(r) at BCP position between ground state and excited state are crucial factors to quantitatively elucidate the ESIPT.

Spin-polarized density-matrix functional theory of the single-impurity Anderson model

NASA Astrophysics Data System (ADS)

Töws, W.; Pastor, G. M.

2012-12-01

Lattice density functional theory (LDFT) is used to investigate spin excitations in the single-impurity Anderson model. In this method, the single-particle density matrix γijσ with respect to the lattice sites replaces the wave function as the basic variable of the many-body problem. A recently developed two-level approximation (TLA) to the interaction-energy functional W[γ] is extended to systems having spin-polarized density distributions and bond orders. This allows us to investigate the effect of external magnetic fields and, in particular, the important singlet-triplet gap ΔE, which determines the Kondo temperature. Applications to finite Anderson rings and square lattices show that the gap ΔE as well as other ground-state and excited-state properties are very accurately reproduced. One concludes that the spin-polarized TLA is reliable in all interaction regimes, from weak to strong correlations, for different hybridization strengths and for all considered impurity valence states. In this way the efficiency of LDFT to account for challenging electron-correlation effects is demonstrated.

Coupled-cluster and density functional theory studies of the electronic 0-0 transitions of the DNA bases.

PubMed

Ovchinnikov, Vasily A; Sundholm, Dage

2014-04-21

The 0-0 transitions of the electronic excitation spectra of the lowest tautomers of the four nucleotide (DNA) bases have been studied using linear-response approximate coupled-cluster singles and doubles (CC2) calculations. Excitation energies have also been calculated at the linear-response time-dependent density functional theory (TDDFT) level using the B3LYP functional. Large basis sets have been employed for ensuring that the obtained excitation energies are close to the basis-set limit. Zero-point vibrational energy corrections have been calculated at the B3LYP and CC2 levels for the ground and excited states rendering direct comparisons with high-precision spectroscopy measurements feasible. The obtained excitation energies for the 0-0 transitions of the first excited states of guanine tautomers are in good agreement with experimental values confirming the experimental assignment of the energetic order of the tautomers of the DNA bases. For the experimentally detected guanine tautomers, the first excited state corresponds to a π→π* transition, whereas for the tautomers of adenine, thymine, and the lowest tautomer of cytosine the transition to the first excited state has n →π* character. The calculations suggest that the 0-0 transitions of adenine, thymine, and cytosine are not observed in the absorption spectrum due to the weak oscillator strength of the formally symmetry-forbidden transitions, while 0-0 transitions of thymine have been detected in fluorescence excitation spectra.

Estimation of the auto frequency response function at unexcited points using dummy masses

NASA Astrophysics Data System (ADS)

Hosoya, Naoki; Yaginuma, Shinji; Onodera, Hiroshi; Yoshimura, Takuya

2015-02-01

If structures with complex shapes have space limitations, vibration tests using an exciter or impact hammer for the excitation are difficult. Although measuring the auto frequency response function at an unexcited point may not be practical via a vibration test, it can be obtained by assuming that the inertia acting on a dummy mass is an external force on the target structure upon exciting a different excitation point. We propose a method to estimate the auto frequency response functions at unexcited points by attaching a small mass (dummy mass), which is comparable to the accelerometer mass. The validity of the proposed method is demonstrated by comparing the auto frequency response functions estimated at unexcited points in a beam structure to those obtained from numerical simulations. We also consider random measurement errors by finite element analysis and vibration tests, but not bias errors. Additionally, the applicability of the proposed method is demonstrated by applying it to estimate the auto frequency response function of the lower arm in a car suspension.

Insights into the Mechanism of a Covalently Linked Organic Dye-Cobaloxime Catalyst System for Dye-Sensitized Solar Fuel Devices.

PubMed

Pati, Palas Baran; Zhang, Lei; Philippe, Bertrand; Fernández-Terán, Ricardo; Ahmadi, Sareh; Tian, Lei; Rensmo, Håkan; Hammarström, Leif; Tian, Haining

2017-06-09

A covalently linked organic dye-cobaloxime catalyst system based on mesoporous NiO is synthesized by a facile click reaction for mechanistic studies and application in a dye-sensitized solar fuel device. The system is systematically investigated by photoelectrochemical measurements, density functional theory, time-resolved fluorescence, transient absorption spectroscopy, and photoelectron spectroscopy. The results show that irradiation of the dye-catalyst on NiO leads to ultrafast hole injection into NiO from the excited dye, followed by a fast electron transfer process to reduce the catalyst. Moreover, the dye adopts different structures with different excited state energies, and excitation energy transfer occurs between neighboring molecules on the semiconductor surface. The photoelectrochemical experiments also show hydrogen production by this system. The axial chloride ligands of the catalyst are released during photocatalysis to create the active sites for proton reduction. A working mechanism of the dye-catalyst system on the photocathode is proposed on the basis of this study. © 2017 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.

Luminescent single-walled carbon nanotube-sensitized europium nanoprobes for cellular imaging

PubMed Central

Avti, Pramod K; Sitharaman, Balaji

2012-01-01

Lanthanoid-based optical probes with excitation wavelengths in the ultra-violet (UV) range (300–325 nm) have been widely developed as imaging probes. Efficient cellular imaging requires that lanthanoid optical probes be excited at visible wavelengths, to avoid UV damage to cells. The efficacy of europium-catalyzed single-walled carbon nanotubes (Eu-SWCNTs), as visible nanoprobes for cellular imaging, is reported in this study. Confocal fluorescence microscopy images of breast cancer cells (SK-BR-3 and MCF-7) and normal cells (NIH 3T3), treated with Eu-SWCNT at 0.2 μg/mL concentration, showed bright red luminescence after excitation at 365 nm and 458 nm wavelengths. Cell viability analysis showed no cytotoxic effects after the incubation of cells with Eu-SWCNTs at this concentration. Eu-SWCNT uptake is via the endocytosis mechanism. Labeling efficiency, defined as the percentage of incubated cells that uptake Eu-SWCNT, was 95%–100% for all cell types. The average cellular uptake concentration was 6.68 ng Eu per cell. Intracellular localization was further corroborated by transmission electron microscopy and Raman microscopy. The results indicate that Eu-SWCNT shows potential as a novel cellular imaging probe, wherein SWCNT sensitizes Eu3+ ions to allow excitation at visible wavelengths, and stable time-resolved red emission. The ability to functionalize biomolecules on the exterior surface of Eu-SWCNT makes it an excellent candidate for targeted cellular imaging. PMID:22619533

Active control of the forced and transient response of a finite beam. M.S. Thesis

NASA Technical Reports Server (NTRS)

Post, John T.

1990-01-01

Structural vibrations from a point force are modelled on a finite beam. This research explores the theoretical limit on controlling beam vibrations utilizing another point source as an active controller. Three different types of excitation are considered, harmonic, random, and transient. For harmonic excitation, control over the entire beam length is possible only when the excitation frequency is near a resonant frequency of the beam. Control over a subregion may be obtained even between resonant frequencies at the cost of increasing the vibration outside of the control region. For random excitation, integrating the expected value of the displacement squared over the required interval, is shown to yield the identical cost function as obtained by integrating the cost function for harmonic excitation over all excitation frequencies. As a result, it is always possible to reduce the cost function for random excitation whether controlling the entire beam or just a subregion, without ever increasing the vibration outside the region in which control is desired. The last type of excitation considered is a single, transient pulse. The form of the controller is specified as either one or two delayed pulses, thus constraining the controller to be casual. The best possible control is examined while varying the region of control and the controller location. It is found that control is always possible using either one or two control pulses.

Manual therapy directed at the knee or lumbopelvic region does not influence quadriceps spinal reflex excitability.

PubMed

Grindstaff, Terry L; Pietrosimone, Brian G; Sauer, Lindsay D; Kerrigan, D Casey; Patrie, James T; Hertel, Jay; Ingersoll, Christopher D

2014-08-01

Manual therapies, directed to the knee and lumbopelvic region, have demonstrated the ability to improve neuromuscular quadriceps function in individuals with knee pathology. It remains unknown if manual therapies may alter impaired spinal reflex excitability, thus identifying a potential mechanism in which manual therapy may improve neuromuscular function following knee injury. To determine the effect of local and distant mobilisation/manipulation interventions on quadriceps spinal reflex excitability. Seventy-five individuals with a history of knee joint injury and current quadriceps inhibition volunteered for this study. Participants were randomised to one of five intervention groups: lumbopelvic manipulation (grade V), lumbopelvic manipulation positioning (no thrust), grade IV patellar mobilisation, grade I patellar mobilisation, and control (no treatment). Changes in spinal reflex excitability were quantified by assessing the Hoffmann reflex (H-reflex), presynaptic, and postsynaptic excitability. A hierarchical linear-mixed model for repeated measures was performed to compare changes in outcome variables between groups over time (pre, post 0, 30, 60, 90 min). There were no significant differences in H-reflex, presynaptic, or postsynaptic excitability between groups across time. Manual therapies directed to the knee or lumbopelvic region did not acutely change quadriceps spinal reflex excitability. Although manual therapies may improve impairments and functional outcomes the underlying mechanism does not appear to be related to changes in spinal reflex excitability. Copyright © 2014 Elsevier Ltd. All rights reserved.

Does the regulation of local excitation-inhibition balance aid in recovery of functional connectivity? A computational account.

PubMed

Vattikonda, Anirudh; Surampudi, Bapi Raju; Banerjee, Arpan; Deco, Gustavo; Roy, Dipanjan

2016-08-01

Computational modeling of the spontaneous dynamics over the whole brain provides critical insight into the spatiotemporal organization of brain dynamics at multiple resolutions and their alteration to changes in brain structure (e.g. in diseased states, aging, across individuals). Recent experimental evidence further suggests that the adverse effect of lesions is visible on spontaneous dynamics characterized by changes in resting state functional connectivity and its graph theoretical properties (e.g. modularity). These changes originate from altered neural dynamics in individual brain areas that are otherwise poised towards a homeostatic equilibrium to maintain a stable excitatory and inhibitory activity. In this work, we employ a homeostatic inhibitory mechanism, balancing excitation and inhibition in the local brain areas of the entire cortex under neurological impairments like lesions to understand global functional recovery (across brain networks and individuals). Previous computational and empirical studies have demonstrated that the resting state functional connectivity varies primarily due to the location and specific topological characteristics of the lesion. We show that local homeostatic balance provides a functional recovery by re-establishing excitation-inhibition balance in all areas that are affected by lesion. We systematically compare the extent of recovery in the primary hub areas (e.g. default mode network (DMN), medial temporal lobe, medial prefrontal cortex) as well as other sensory areas like primary motor area, supplementary motor area, fronto-parietal and temporo-parietal networks. Our findings suggest that stability and richness similar to the normal brain dynamics at rest are achievable by re-establishment of balance. Copyright © 2016 Elsevier Inc. All rights reserved.

Collision energy dependent cross section and rotational alignment of NO (A 2Σ+) in the energy-transfer reaction of N2 (A 3Σu+) + NO (X 2Π) → N2 (X 1Σg+) + NO (A 2Σ+).

PubMed

Ohoyama, H

2014-10-16

We have studied the collision energy dependent cross section and alignment of NO (A (2)Σ(+)) rotation in the energy-transfer reaction of N2 (A (3)Σ(u)(+)) + NO (X (2)Π) → N2 (X (1)Σ(g)(+)) + NO (A (2)Σ(+)) at the collision energy (E) region of 0.03-0.2 eV. NO (A (2)Σ(+)) emission in two linear polarization directions in the collision frame (parallel (∥) and perpendicular (⊥) with respect to the relative velocity vector (vR)) has been measured as a function of collision energy. NO (A (2)Σ(+)) rotation (J-vector) turns out to be aligned perpendicular to vR. In addition, collision energy is found to enhance the degree of alignment of NO (A (2)Σ(+)) rotation. The collision energy dependent cross sections σ(∥,(⊥))(E) (excitation functions) show a rapid fall-off following an initial rise with a threshold less than 0.02 eV. The excitation function at the parallel alignment of NO (A (2)Σ(+)) rotation, σ(J∥v(R), (E), is slightly shifted to the low collision energy region as compared with σ(J ⊥ vR, E). We propose that the rapid fall-off feature in the excitation function is attributed to the multidimensional nonadiabatic transitions.

Phosphorene quantum dot-fullerene nanocomposites for solar energy conversion: An unexplored inorganic-organic nanohybrid with novel photovoltaic properties

NASA Astrophysics Data System (ADS)

Rajbanshi, Biplab; Kar, Moumita; Sarkar, Pallavi; Sarkar, Pranab

2017-10-01

Using the self-consistent charge density-functional based tight-binding (SCC-DFTB) method, coupled with time-dependent density functional theory (TDDFT) calculations, for the first time we explore the possibility of use of phosphorene quantum dots in solar energy harvesting devices. The phosphorene quantum dots-fullerene (PQDs-PCBA) nanocomposites show type-II band alignment indicating spatial separation of charge carriers. The TDDFT calculations also show that the PQD-fullerene nanocomposites seem to be exciting material for future generation solar energy harvester, with extremely fast charge transfer and very poor recombination rate.

QPM Analysis of 205Tl Nuclear Excitations below the Giant Dipole Resonance

NASA Astrophysics Data System (ADS)

Benouaret, N.; Beller, J.; Isaak, J.; Kelley, J. H.; Pai, H.; Pietralla, N.; Ponomarev, V. Yu.; Raut, R.; Romig, C.; Rusev, G.; Savran, D.; Scheck, M.; Schnorrenberger, L.; Sonnabend, K.; Tonchev, A. P.; Tornow, W.; Weller, H. R.; Zweidinger, M.

2015-05-01

We analysed our experimental recent findings of the dipole response of the odd-mass stable nucleus 205Tl within the quasi-particle phonon model. Using the phonon basis constructed for the neighbouring 204Hg and wave function configurations for 205Tl consisting of a mixture of quasiparticle ⊗ N-phonon configurations (N=0,1,2), only one group of fragmented dipole excited states has been reproduced at 5.5 MeV in comparison to the experimental distribution which shows a second group at about 5 MeV. The computed dipole transition strengths are mainly of E1 character which could be associated to the pygmy dipole resonance.

Bosonic excitations and electron pairing in an electron-doped cuprate superconductor

NASA Astrophysics Data System (ADS)

Wang, M. C.; Yu, H. S.; Xiong, J.; Yang, Y.-F.; Luo, S. N.; Jin, K.; Qi, J.

2018-04-01

By applying ultrafast optical spectroscopy to electron-doped La1.9Ce0.1CuO4 ±δ , we discern a bosonic mode of electronic origin and provide the evolution of its coupling with the charge carriers as a function of temperature. Our results show that it has the strongest coupling strength near Tc and can fully account for the superconducting pairing. This mode can be associated with the two-dimensional antiferromagnetic spin correlations emerging below a critical temperature T† larger than Tc. Our work may help to establish a quantitative relation between bosonic excitations and superconducting pairing in electron-doped cuprates.

Classification of the nonlinear dynamics and bifurcation structure of ultrasound contrast agents excited at higher multiples of their resonance frequency

NASA Astrophysics Data System (ADS)

Sojahrood, Amin Jafari; Kolios, Michael C.

2012-07-01

Through numerical simulation of the Hoff model we show that when ultrasound contrast agents (UCAs) are excited at frequencies which are close to integer (m>2) multiples of their natural resonance frequency, the bifurcation structure of the UCA oscillations as a function of pressure may be characterized by 3 general distinct regions. The UCA behavior starts with initial period one oscillations which undergoes a saddle node bifurcation to m coexisting attractors for an acoustic pressure above a threshold, P. Further increasing the pressure above a second threshold P, is followed by a sudden transition to period 1 oscillations.

The Peep Show

ERIC Educational Resources Information Center

Gamble, David L.

2010-01-01

Three years ago, the author and Linda Arbuckle (University of Florida ceramic professor and internationally known majolica clay artist) were on the phone discussing how electric kilns just don't have any artistic design flair to them. The round kiln has basic properties that allow it to function properly, but its looks are far from exciting. They…

Maximum-Entropy Inference with a Programmable Annealer

PubMed Central

Chancellor, Nicholas; Szoke, Szilard; Vinci, Walter; Aeppli, Gabriel; Warburton, Paul A.

2016-01-01

Optimisation problems typically involve finding the ground state (i.e. the minimum energy configuration) of a cost function with respect to many variables. If the variables are corrupted by noise then this maximises the likelihood that the solution is correct. The maximum entropy solution on the other hand takes the form of a Boltzmann distribution over the ground and excited states of the cost function to correct for noise. Here we use a programmable annealer for the information decoding problem which we simulate as a random Ising model in a field. We show experimentally that finite temperature maximum entropy decoding can give slightly better bit-error-rates than the maximum likelihood approach, confirming that useful information can be extracted from the excited states of the annealer. Furthermore we introduce a bit-by-bit analytical method which is agnostic to the specific application and use it to show that the annealer samples from a highly Boltzmann-like distribution. Machines of this kind are therefore candidates for use in a variety of machine learning applications which exploit maximum entropy inference, including language processing and image recognition. PMID:26936311

Non-invasive brain stimulation: a new strategy to improve neurorehabilitation after stroke?

PubMed

Hummel, Friedhelm C; Cohen, Leonardo G

2006-08-01

Motor impairment resulting from chronic stroke can have extensive physical, psychological, financial, and social implications despite available neurorehabilitative treatments. Recent studies in animals showed that direct epidural stimulation of the primary motor cortex surrounding a small infarct in the lesioned hemisphere (M1(lesioned hemisphere)) elicits improvements in motor function. In human beings, proof of principle studies from different laboratories showed that non-invasive transcranial magnetic stimulation and direct current stimulation that upregulate excitability within M1(lesioned hemisphere) or downregulate excitability in the intact hemisphere (M1(intact hemisphere)) results in improvement in motor function in patients with stroke. Possible mechanisms mediating these effects can include the correction of abnormally persistent interhemispheric inhibitory drive from M1(intact hemisphere) to M1(lesioned hemisphere) in the process of generation of voluntary movements by the paretic hand, a disorder correlated with the magnitude of impairment. In this paper we review these mechanistically oriented interventional approaches. WHAT NEXT?: These findings suggest that transcranial magnetic stimulation and transcranial direct current stimulation could develop into useful adjuvant strategies in neurorehabilitation but have to be further assessed in multicentre clinical trials.

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

Holdaway, David I. H., E-mail: d.holdaway@ucl.ac.uk; Olaya-Castro, Alexandra, E-mail: a.olaya@ucl.ac.uk; Collini, Elisabetta, E-mail: elisabetta.collini@unipd.it

We examine transient circular dichroism (TRCD) spectroscopy as a technique to investigate signatures of exciton coherence dynamics under the influence of structured vibrational environments. We consider a pump-probe configuration with a linearly polarized pump and a circularly polarized probe, with a variable angle θ between the two directions of propagation. In our theoretical formalism the signal is decomposed in chiral and achiral doorway and window functions. Using this formalism, we show that the chiral doorway component, which beats during the population time, can be isolated by comparing signals with different values of θ. As in the majority of time-resolved pump-probemore » spectroscopy, the overall TRCD response shows signatures of both excited and ground state dynamics. However, we demonstrate that the chiral doorway function has only a weak ground state contribution, which can generally be neglected if an impulsive pump pulse is used. These findings suggest that the pump-probe configuration of optical TRCD in the impulsive limit has the potential to unambiguously probe quantum coherence beating in the excited state. We present numerical results for theoretical signals in an example dimer system.« less

Coherence specific signal detection via chiral pump-probe spectroscopy.

PubMed

Holdaway, David I H; Collini, Elisabetta; Olaya-Castro, Alexandra

2016-05-21

We examine transient circular dichroism (TRCD) spectroscopy as a technique to investigate signatures of exciton coherence dynamics under the influence of structured vibrational environments. We consider a pump-probe configuration with a linearly polarized pump and a circularly polarized probe, with a variable angle θ between the two directions of propagation. In our theoretical formalism the signal is decomposed in chiral and achiral doorway and window functions. Using this formalism, we show that the chiral doorway component, which beats during the population time, can be isolated by comparing signals with different values of θ. As in the majority of time-resolved pump-probe spectroscopy, the overall TRCD response shows signatures of both excited and ground state dynamics. However, we demonstrate that the chiral doorway function has only a weak ground state contribution, which can generally be neglected if an impulsive pump pulse is used. These findings suggest that the pump-probe configuration of optical TRCD in the impulsive limit has the potential to unambiguously probe quantum coherence beating in the excited state. We present numerical results for theoretical signals in an example dimer system.

Stochastic resonance energy harvesting for a rotating shaft subject to random and periodic vibrations: influence of potential function asymmetry and frequency sweep

NASA Astrophysics Data System (ADS)

Kim, Hongjip; Che Tai, Wei; Zhou, Shengxi; Zuo, Lei

2017-11-01

Stochastic resonance is referred to as a physical phenomenon that is manifest in nonlinear systems whereby a weak periodic signal can be significantly amplified with the aid of inherent noise or vice versa. In this paper, stochastic resonance is considered to harvest energy from two typical vibrations in rotating shafts: random whirl vibration and periodic stick-slip vibration. Stick-slip vibrations impose a constant offset in centrifugal force and distort the potential function of the harvester, leading to potential function asymmetry. A numerical analysis based on a finite element method was conducted to investigate stochastic resonance with potential function asymmetry. Simulation results revealed that a harvester with symmetric potential function generates seven times higher power than that with asymmetric potential function. Furthermore, a frequency-sweep analysis also showed that stochastic resonance has hysteretic behavior, resulting in frequency difference between up-sweep and down-sweep excitations. An electromagnetic energy harvesting system was constructed to experimentally verify the numerical analysis. In contrast to traditional stochastic resonance harvesters, the proposed harvester uses magnetic force to compensate the offset in the centrifugal force. System identification was performed to obtain the parameters needed in the numerical analysis. With the identified parameters, the numerical simulations showed good agreement with the experiment results with around 10% error, which verified the effect of potential function asymmetry and frequency sweep excitation condition on stochastic resonance. Finally, attributed to compensating the centrifugal force offset, the proposed harvester generated nearly three times more open-circuit output voltage than its traditional counterpart.

Cerebellum tunes the excitability of the motor system: evidence from peripheral motor axons.

PubMed

Nodera, Hiroyuki; Manto, Mario

2014-12-01

Cerebellum is highly connected with the contralateral cerebral cortex. So far, the motor deficits observed in acute focal cerebellar lesions in human have been mainly explained on the basis of a disruption of the cerebello-thalamo-cortical projections. Cerebellar circuits have also numerous anatomical and functional interactions with brainstem nuclei and projects also directly to the spinal cord. Cerebellar lesions alter the excitability of peripheral motor axons as demonstrated by peripheral motor threshold-tracking techniques in cerebellar stroke. The biophysical changes are correlated with the functional scores. Nerve excitability measurements represent an attractive tool to extract the rules underlying the tuning of excitability of the motor pathways by the cerebellum and to discover the contributions of each cerebellar nucleus in this key function, contributing to early plasticity and sensorimotor learning.

Vastus Medialis Hoffmann Reflex Excitability Is Associated With Pain Level, Self-Reported Function, and Chronicity in Women With Patellofemoral Pain.

PubMed

de Oliveira Silva, Danilo; Magalhães, Fernando Henrique; Faria, Nathálie Clara; Ferrari, Deisi; Pazzinatto, Marcella Ferraz; Pappas, Evangelos; de Azevedo, Fábio Mícolis

2017-01-01

To determine the association between the amplitude of vastus medialis (VM) Hoffmann reflex (H-reflex) and pain level, self-reported physical function, and chronicity of pain in women with patellofemoral pain (PFP). Cross-sectional study. Laboratory of biomechanics and motor control. Women diagnosed with PFP (N=15) aged 18 to 35 years. Not applicable. Data on worst pain level during the previous month, self-reported physical function, and symptom duration (chronicity) were collected from the participants. Maximum evoked responses were obtained by electrical stimulation applied to the femoral nerve and peak-to-peak amplitudes of normalized maximal H-reflexes (maximal Hoffmann reflex/maximal motor wave ratios) of the VM were calculated. A Pearson product-moment correlation matrix (r) was used to explore the relations between the amplitude of VM H-reflex and worst pain during the previous month, self-reported function, and chronicity of pain. Strong negative correlations were found between the amplitude of VM H-reflex and worst pain in the previous month (r=-.71; P=.003) and chronicity (r=-.74; P=.001). A strong positive correlation was found between the amplitude of VM H-reflex and self-reported physical function (r=.62; P=.012). The strong and significant relations reported in this study suggest that women with PFP showing greater VM H-reflex excitability tend to have lower pain, better physical function, and more recent symptoms. Therefore, rehabilitation strategies designed to increase the excitability of the monosynaptic stretch reflex should be considered in the treatment of women with PFP if their effectiveness is demonstrated in future studies. Copyright © 2016 American Congress of Rehabilitation Medicine. Published by Elsevier Inc. All rights reserved.

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

Yanai, Takeshi; Fann, George I.; Beylkin, Gregory

Using the fully numerical method for time-dependent Hartree–Fock and density functional theory (TD-HF/DFT) with the Tamm–Dancoff (TD) approximation we use a multiresolution analysis (MRA) approach to present our findings. From a reformulation with effective use of the density matrix operator, we obtain a general form of the HF/DFT linear response equation in the first quantization formalism. It can be readily rewritten as an integral equation with the bound-state Helmholtz (BSH) kernel for the Green's function. The MRA implementation of the resultant equation permits excited state calculations without virtual orbitals. Moreover, the integral equation is efficiently and adaptively solved using amore » numerical multiresolution solver with multiwavelet bases. Our implementation of the TD-HF/DFT methods is applied for calculating the excitation energies of H 2, Be, N 2, H 2O, and C 2H 4 molecules. The numerical errors of the calculated excitation energies converge in proportion to the residuals of the equation in the molecular orbitals and response functions. The energies of the excited states at a variety of length scales ranging from short-range valence excitations to long-range Rydberg-type ones are consistently accurate. It is shown that the multiresolution calculations yield the correct exponential asymptotic tails for the response functions, whereas those computed with Gaussian basis functions are too diffuse or decay too rapidly. Finally, we introduce a simple asymptotic correction to the local spin-density approximation (LSDA) so that in the TDDFT calculations, the excited states are correctly bound.« less

Electronic π-to-π* Excitations of Rhodamine Dyes Exhibit a Time-Dependent Kohn-Sham Theory “Cyanine Problem”

DOE PAGES

Moore, II, Barry; Schrader, Robert L.; Kowalski, Karol; ...

2017-05-02

The longest-wavelength π-to-π* electronic excitations of rhodamine-like dyes (RDs) with different group16 heteroatoms (O, S, Se, Te) have been investigated. Time-dependent Kohn–Sham theory (TDKST) calculations were compared with coupled-cluster (CC) and equations-of-motion (EOM) CC results for π-to-π* singlet and triplet excitations. The RDs exhibit characteristics in the TDKST calculations that are very similar to previously investigated cyanine dyes, in the sense that the singlet energies obtained with nonhybrid functionals are too high compared with the CC results at the SD(T) level. The errors became increasingly larger for functionals with increasing amounts of exact exchange. TDKST with all tested functionals ledmore » to severe underestimations of the corresponding triplet excitations and overestimations of the singlet--triplet gaps. Long-range-corrected range-separated exchange and "optimal tuning" of the range separation parameter did not significantly improve the TDKST results. A detailed analysis suggests that the problem is differential electron correlation between the ground and excited states, which is not treated sufficiently by the relatively small integrals over the exchange-correlation response kernel that enters the excitation energy expression. As a result, numerical criteria are suggested that may help identify "cyanine-like" problems in TDKST calculations of excitation spectra.« less

Comparison of hydrological and GRACE-based excitation functions of polar motion in the seasonal spectral band

NASA Astrophysics Data System (ADS)

Nastula, J.; Kolaczek, B.; Salstein, D. A.

2008-04-01

Understanding changes in the global balance of the Earths angular momentum due to the mass redistribution of geophysical fluids is needed to explain the observed polar motion. The impact of continental hydrologic signals, from land water, snow, and ice, on polar motion excitation (hydrological angular momentum-HAM), is still inadequately known. Although estimates of HAM have been made from several models of global hydrology based upon the observed distribution of surface water, snow, and soil moisture, the relatively sparse observation network and the presence of errors in the data and the geophysical fluid models preclude a full understanding of the HAM influence on polar motion variations. Recently the GRACE mission monitoring Earths time variable gravity field has allowed us to determine the mass term of polar motion excitation functions and compare them with the mass term derivable as a residual from the geodetic excitation functions and geophysical fluid motion terms on seasonal time scales. Differences between these mass terms in the years 2004 - 2005.5 are still on the order of 20 mas. Besides the overall mass excitation of polar motion comparisons with GRACE (RL04-release), we also intercompare the non-atmospheric, non-oceanic signals in the mass term of geodetic polar motion excitation with hydrological excitation of polar motion.

Comparison of high-voltage ac and pulsed operation of a surface dielectric barrier discharge

NASA Astrophysics Data System (ADS)

Williamson, James M.; Trump, Darryl D.; Bletzinger, Peter; Ganguly, Biswa N.

2006-10-01

A surface dielectric barrier discharge (DBD) in atmospheric pressure air was excited either by low frequency (0.3-2 kHz) high-voltage ac or by short, high-voltage pulses at repetition rates from 50 to 600 pulses s-1. The short-pulse excited discharge was more diffuse and did not have the pronounced bright multiple cathode spots observed in the ac excited discharge. The discharge voltage, current and average power deposited into the discharge were calculated for both types of excitation. As a measure of plasma-chemical efficiency, the ozone number density was measured by UV absorption as a function of average deposited power. The density of ozone produced by ac excitation did not increase so rapidly as that produced by short-pulse excitation as a function of average power, with a maximum measured density of ~3 × 1015 cm-3 at 25 W. The maximum ozone production achieved by short-pulse excitation was ~8.5 × 1015 cm-3 at 20 W, which was four times greater than that achieved by ac excitation at the same power level.

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

Bouchard, Chris; Chang, Chia Cheng; Kurth, Thorsten

In this paper, the Feynman-Hellmann theorem can be derived from the long Euclidean-time limit of correlation functions determined with functional derivatives of the partition function. Using this insight, we fully develop an improved method for computing matrix elements of external currents utilizing only two-point correlation functions. Our method applies to matrix elements of any external bilinear current, including nonzero momentum transfer, flavor-changing, and two or more current insertion matrix elements. The ability to identify and control all the systematic uncertainties in the analysis of the correlation functions stems from the unique time dependence of the ground-state matrix elements and the fact that all excited states and contact terms are Euclidean-time dependent. We demonstrate the utility of our method with a calculation of the nucleon axial charge using gradient-flowed domain-wall valence quarks on themore » $$N_f=2+1+1$$ MILC highly improved staggered quark ensemble with lattice spacing and pion mass of approximately 0.15 fm and 310 MeV respectively. We show full control over excited-state systematics with the new method and obtain a value of $$g_A = 1.213(26)$$ with a quark-mass-dependent renormalization coefficient.« less

Two-color two-photon excited fluorescence of indole: Determination of wavelength-dependent molecular parameters

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

Herbrich, Sebastian; Al-Hadhuri, Tawfik; Gericke, Karl-Heinz, E-mail: k.Gericke@tu-bs.de

2015-01-14

We present a detailed study of two-color two-photon excited fluorescence in indole dissolved in propylene glycol. Femtosecond excitation pulses at effective wavelengths from 268 to 293.33 nm were used to populate the two lowest indole excited states {sup 1}L{sub a} and {sup 1}L{sub b} and polarized fluorescence was then detected. All seven molecular parameters and the two-photon polarization ratio Ω containing information on two-photon absorption dynamics, molecular lifetime τ{sub f}, and rotation correlation time τ{sub rot} have been determined from experiment and analyzed as a function of the excitation wavelength. The analysis of the experimental data has shown that {supmore » 1}L{sub b}–{sup 1}L{sub a} inversion occurred under the conditions of our experiment. The two-photon absorption predominantly populated the {sup 1}L{sub a} state at all excitation wavelengths but in the 287–289 nm area which contained an absorption hump of the {sup 1}L{sub b} state 0-0 origin. The components of the two-photon excitation tensor S were analyzed giving important information on the principal tensor axes and absorption symmetry. The results obtained are in a good agreement with the results reported by other groups. The lifetime τ{sub f} and the rotation correlation time τ{sub rot} showed no explicit dependence on the effective excitation wavelength. Their calculated weighted average values were found to be τ{sub f} = 3.83 ± 0.14 ns and τ{sub rot} = 0.74 ± 0.06 ns.« less

Orientation-dependent imaging of electronically excited quantum dots

NASA Astrophysics Data System (ADS)

Nguyen, Duc; Goings, Joshua J.; Nguyen, Huy A.; Lyding, Joseph; Li, Xiaosong; Gruebele, Martin

2018-02-01

We previously demonstrated that we can image electronic excitations of quantum dots by single-molecule absorption scanning tunneling microscopy (SMA-STM). With this technique, a modulated laser beam periodically saturates an electronic transition of a single nanoparticle, and the resulting tunneling current modulation ΔI(x0, y0) maps out the SMA-STM image. In this paper, we first derive the basic theory to calculate ΔI(x0, y0) in the one-electron approximation. For near-resonant tunneling through an empty orbital "i" of the nanostructure, the SMA-STM signal is approximately proportional to the electron density |φi) (x0,y0)|

Orientation-dependent imaging of electronically excited quantum dots.

PubMed

Nguyen, Duc; Goings, Joshua J; Nguyen, Huy A; Lyding, Joseph; Li, Xiaosong; Gruebele, Martin

2018-02-14

We previously demonstrated that we can image electronic excitations of quantum dots by single-molecule absorption scanning tunneling microscopy (SMA-STM). With this technique, a modulated laser beam periodically saturates an electronic transition of a single nanoparticle, and the resulting tunneling current modulation ΔI(x 0 , y 0 ) maps out the SMA-STM image. In this paper, we first derive the basic theory to calculate ΔI(x 0 , y 0 ) in the one-electron approximation. For near-resonant tunneling through an empty orbital "i" of the nanostructure, the SMA-STM signal is approximately proportional to the electron density φ i x 0 ,y 0 2 of the excited orbital in the tunneling region. Thus, the SMA-STM signal is approximated by an orbital density map (ODM) of the resonantly excited orbital at energy E i . The situation is more complex for correlated electron motion, but either way a slice through the excited electronic state structure in the tunneling region is imaged. We then show experimentally that we can nudge quantum dots on the surface and roll them, thus imaging excited state electronic structure of a single quantum dot at different orientations. We use density functional theory to model ODMs at various orientations, for qualitative comparison with the SMA-STM experiment. The model demonstrates that our experimentally observed signal monitors excited states, localized by defects near the surface of an individual quantum dot. The sub-nanometer super-resolution imaging technique demonstrated here could become useful for mapping out the three-dimensional structure of excited states localized by defects within nanomaterials.

Functional Interaction between the Scaffold Protein Kidins220/ARMS and Neuronal Voltage-Gated Na+ Channels.

PubMed

Cesca, Fabrizia; Satapathy, Annyesha; Ferrea, Enrico; Nieus, Thierry; Benfenati, Fabio; Scholz-Starke, Joachim

2015-07-17

Kidins220 (kinase D-interacting substrate of 220 kDa)/ankyrin repeat-rich membrane spanning (ARMS) acts as a signaling platform at the plasma membrane and is implicated in a multitude of neuronal functions, including the control of neuronal activity. Here, we used the Kidins220(-/-) mouse model to study the effects of Kidins220 ablation on neuronal excitability. Multielectrode array recordings showed reduced evoked spiking activity in Kidins220(-/-) hippocampal networks, which was compatible with the increased excitability of GABAergic neurons determined by current-clamp recordings. Spike waveform analysis further indicated an increased sodium conductance in this neuronal subpopulation. Kidins220 association with brain voltage-gated sodium channels was shown by co-immunoprecipitation experiments and Na(+) current recordings in transfected HEK293 cells, which revealed dramatic alterations of kinetics and voltage dependence. Finally, an in silico interneuronal model incorporating the Kidins220-induced Na(+) current alterations reproduced the firing phenotype observed in Kidins220(-/-) neurons. These results identify Kidins220 as a novel modulator of Nav channel activity, broadening our understanding of the molecular mechanisms regulating network excitability. © 2015 by The American Society for Biochemistry and Molecular Biology, Inc.

GABA receptors and T-type Ca2+ channels crosstalk in thalamic networks.

PubMed

Leresche, Nathalie; Lambert, Régis C

2017-06-07

Although the thalamus presents a rather limited repertoire of GABAergic cell types compare to other CNS area, this structure is a privileged system to study how GABA impacts neuronal network excitability. Indeed both glutamatergic thalamocortical (TC) and GABAergic nucleus reticularis thalami (NRT) neurons present a high expression of T-type voltage-dependent Ca 2+ channels whose activation that shapes the output of the thalamus critically depends upon a preceding hyperpolarisation. Because of this strict dependence, a tight functional link between GABA mediated hyperpolarization and T-currents characterizes the thalamic network excitability. In this review we summarize a number of studies showing that the relationships between the various thalamic GABA A/B receptors and T-channels are complex and bidirectional. We discuss how this dynamic interaction sets the global intrathalamic network activity and its long-term plasticity and highlight how the functional relationship between GABA release and T-channel-dependent excitability is finely tuned by the T-channel activation itself. Finally, we illustrate how an impaired balance between T-channels and GABA receptors can lead to pathologically abnormal cellular and network behaviours. Copyright © 2017 Elsevier Ltd. All rights reserved.

Examining the role of transfer coupling in sub-barrier fusion of Ti 46 , 50 + Sn 124

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

Liang, J. Felix; Allmond, J. M.; Gross, C. J.

2016-08-24

In this study, the presence of neutron transfer channels with positive Q values can enhance sub-barrier fusion cross sections. Recent measurements of the fusion excitation functions for 58Ni+ 132,124Sn found that the fusion enhancement due to the influence of neutron transfer is smaller than that in 40Ca + 132,124Sn although the Q values for multineutron transfer are comparable. The purpose of this study is to investigate the differences observed between the fusion of Sn + Ni and Sn + Ca. Methods: Fusion excitation functions for 46,50Ti + 124Sn have been measured at energies near the Coulomb barrier. As a result,more » a comparison of the barrier distributions for 46Ti+ 124Sn and 40Ca+ 124Sn shows that the 40Ca+ 124Sn system has a barrier strength resulting from the coupling to the very collective octupole state in 40Ca at an energy significantly lower than the uncoupled barrier. In conclusion, the large sub-barrier fusion enhancement in 40Ca induced reactions is attributed to both couplings to neutron transfer and inelastic excitation, with the octupole vibration of 40Ca playing a major role.« less

Non-linear dynamic characteristics and optimal control of giant magnetostrictive film subjected to in-plane stochastic excitation

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

Zhu, Z. W., E-mail: zhuzhiwen@tju.edu.cn; Tianjin Key Laboratory of Non-linear Dynamics and Chaos Control, 300072, Tianjin; Zhang, W. D., E-mail: zhangwenditju@126.com

2014-03-15

The non-linear dynamic characteristics and optimal control of a giant magnetostrictive film (GMF) subjected to in-plane stochastic excitation were studied. Non-linear differential items were introduced to interpret the hysteretic phenomena of the GMF, and the non-linear dynamic model of the GMF subjected to in-plane stochastic excitation was developed. The stochastic stability was analysed, and the probability density function was obtained. The condition of stochastic Hopf bifurcation and noise-induced chaotic response were determined, and the fractal boundary of the system's safe basin was provided. The reliability function was solved from the backward Kolmogorov equation, and an optimal control strategy was proposedmore » in the stochastic dynamic programming method. Numerical simulation shows that the system stability varies with the parameters, and stochastic Hopf bifurcation and chaos appear in the process; the area of the safe basin decreases when the noise intensifies, and the boundary of the safe basin becomes fractal; the system reliability improved through stochastic optimal control. Finally, the theoretical and numerical results were proved by experiments. The results are helpful in the engineering applications of GMF.« less

A low-cost approach to electronic excitation energies based on the driven similarity renormalization group

NASA Astrophysics Data System (ADS)

Li, Chenyang; Verma, Prakash; Hannon, Kevin P.; Evangelista, Francesco A.

2017-08-01

We propose an economical state-specific approach to evaluate electronic excitation energies based on the driven similarity renormalization group truncated to second order (DSRG-PT2). Starting from a closed-shell Hartree-Fock wave function, a model space is constructed that includes all single or single and double excitations within a given set of active orbitals. The resulting VCIS-DSRG-PT2 and VCISD-DSRG-PT2 methods are introduced and benchmarked on a set of 28 organic molecules [M. Schreiber et al., J. Chem. Phys. 128, 134110 (2008)]. Taking CC3 results as reference values, mean absolute deviations of 0.32 and 0.22 eV are observed for VCIS-DSRG-PT2 and VCISD-DSRG-PT2 excitation energies, respectively. Overall, VCIS-DSRG-PT2 yields results with accuracy comparable to those from time-dependent density functional theory using the B3LYP functional, while VCISD-DSRG-PT2 gives excitation energies comparable to those from equation-of-motion coupled cluster with singles and doubles.

Properties of electronically excited states of four squaraine dyes and their complexes with fullerene C70: A theoretical investigation

NASA Astrophysics Data System (ADS)

Zhang, Jian; Li, Tingyu

2017-09-01

Solar cells sensitized by polypyridyl Ru(II) complexes exhibit relatively high efficiency, however those photo-sensitizers did not absorb the photons in the far-red and near-infrared region. At present, squaraine dyes have received considerable attention as their attractively intrinsic red light absorption and unusual high molar extinction coefficient. Here we applied density functional theory and time dependent density functional theory to investigate the properties of electronically excited states of four squaraine dyes and their complexes with fullerene C70. The influences of different functionals, basis sets and solvent effects are evaluated. To understand the photophysical properties, the investigations are basing on a classification method which splits the squaraine dyes and their complexes with fullerene C70 into two units to characterize the intramolecular density distribution. We present the signatures of their electronically excited states which are characterized as local excitation or charge-transfer excitation. The relationship between open-circuit voltage and the number of intramolecular hydrogen bonds in squaraine dyes are discussed.

Multicomponent Time-Dependent Density Functional Theory: Proton and Electron Excitation Energies.

PubMed

Yang, Yang; Culpitt, Tanner; Hammes-Schiffer, Sharon

2018-04-05

The quantum mechanical treatment of both electrons and protons in the calculation of excited state properties is critical for describing nonadiabatic processes such as photoinduced proton-coupled electron transfer. Multicomponent density functional theory enables the consistent quantum mechanical treatment of more than one type of particle and has been implemented previously for studying ground state molecular properties within the nuclear-electronic orbital (NEO) framework, where all electrons and specified protons are treated quantum mechanically. To enable the study of excited state molecular properties, herein the linear response multicomponent time-dependent density functional theory (TDDFT) is derived and implemented within the NEO framework. Initial applications to FHF - and HCN illustrate that NEO-TDDFT provides accurate proton and electron excitation energies within a single calculation. As its computational cost is similar to that of conventional electronic TDDFT, the NEO-TDDFT approach is promising for diverse applications, particularly nonadiabatic proton transfer reactions, which may exhibit mixed electron-proton vibronic excitations.

Variation in the thermionic work function of semiconductor powders exposed to electromagnetic radiation

NASA Technical Reports Server (NTRS)

Bourasseau, S.; Martin, J. R.; Juillet, F.; Teichner, S. J.

1977-01-01

The study of the variation of thermoelectronic work function potential of TiO2 in the presence of isobutane shows that this gas is not adsorbed on this solid, in either the presence or the absence of ultraviolet radiation. These results, as well as those obtained in a previous work, lead to the mechanism of the photo-oxidation of isobutane at room temperature, in which excited atomic oxygen is the active species.

The Measurement of the Evaporation Residues Excitation Functions in the Fusion Reactions 144Sm (40Ar,xn) and 166Er(40Ar,xn)

NASA Astrophysics Data System (ADS)

Chernysheva, E. V.; Rodin, A. M.; Belozerov, A. V.; Dmitriev, S. N.; Gulyaev, A. V.; Gulyaeva, A. V.; Itkis, M. G.; Novoselov, A. S.; Oganessian, Yu. Ts.; Salamatin, V. S.; Stepantsov, S. V.; Vedeneev, V. Yu.; Yukhimchuk, S. A.; Krupa, L.; Kliman, J.; Motycak, S.; Sivacek, I.

2015-06-01

The evaporation residues excitation functions for the reactions 40Ar+144Sm→184Hg and 40Ar+166Er→206Rn were measured at the energies below and above the Coulomb barrier (Elab=142-207 MeV) using a mass-separator MASHA. The experimental data were compared with theoretical calculations using a Channel Coupling Model. The influence of experimental beam energy spread on the excitation functions was taking into account. It was found that structure of xn-cross sections correlate strongly with the nuclear structure of colliding nuclei.

Investigation deuteron-induced reactions on cobalt

NASA Astrophysics Data System (ADS)

Ditrói, F.; Tárkányi, F.; Takács, S.; Hermanne, A.; Baba, M.; Ignatyuk, A. V.

2010-09-01

The excitation functions of deuteron-induced reactions were measured on metallic cobalt. Beyond the 56,57,58,60Co cobalt isotopes, we also identified 57Ni, 54Mn, 56Mn and 59Fe in the deuteron experiments. For the above radionuclides, the excitation functions in the measured energy range were determined and compared with the data found in the literature and with the results of model calculations (ALICE-IPPE, EMPIRE-D, EAF, and TALYS (TENDL)). The excitation functions agree with previous measurements; furthermore, we calculated the yield and thin layer activation (TLA) curves that are necessary for practical and industrial applications.

Multiple Types of Topological Fermions in Transition Metal Silicides

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

Tang, Peizhe; Zhou, Quan; Zhang, Shou -Cheng

Exotic massless fermionic excitations with nonzero Berry flux, other than the Dirac and Weyl fermions, could exist in condensed matter systems under the protection of crystalline symmetries, such as spin-1 excitations with threefold degeneracy and spin-3/2 Rarita-Schwinger-Weyl fermions. Herein, by using the ab initio density functional theory, we show that these unconventional quasiparticles coexist with type-I and type-II Weyl fermions in a family of transition metal silicides, including CoSi, RhSi, RhGe, and CoGe, when spin-orbit coupling is considered. Their nontrivial topology results in a series of extensive Fermi arcs connecting projections of these bulk excitations on the side surface, whichmore » is confirmed by (001) surface electronic spectra of CoSi. Additionally, these stable arc states exist within a wide energy window around the Fermi level, which makes them readily accessible in angle-resolved photoemission spectroscopy measurements.« less

Probing the symmetry of the potential of localized surface plasmon resonances with phase-shaped electron beams.

PubMed

Guzzinati, Giulio; Béché, Armand; Lourenço-Martins, Hugo; Martin, Jérôme; Kociak, Mathieu; Verbeeck, Jo

2017-04-12

Plasmonics, the science and technology of the interaction of light with metallic objects, is fundamentally changing the way we can detect, generate and manipulate light. Although the field is progressing swiftly, thanks to the availability of nanoscale manufacturing and analysis methods, fundamental properties such as the plasmonic excitations' symmetries cannot be accessed directly, leading to a partial, sometimes incorrect, understanding of their properties. Here we overcome this limitation by deliberately shaping the wave function of an electron beam to match a plasmonic excitations' symmetry in a modified transmission electron microscope. We show experimentally and theoretically that this offers selective detection of specific plasmon modes within metallic nanoparticles, while excluding modes with other symmetries. This method resembles the widespread use of polarized light for the selective excitation of plasmon modes with the advantage of locally probing the response of individual plasmonic objects and a far wider range of symmetry selection criteria.

The electronically excited states of LH2 complexes from Rhodopseudomonas acidophila strain 10050 studied by time-resolved spectroscopy and dynamic Monte Carlo simulations. I. Isolated, non-interacting LH2 complexes.

PubMed

Pflock, Tobias J; Oellerich, Silke; Southall, June; Cogdell, Richard J; Ullmann, G Matthias; Köhler, Jürgen

2011-07-21

We have employed time-resolved spectroscopy on the picosecond time scale in combination with dynamic Monte Carlo simulations to investigate the photophysical properties of light-harvesting 2 (LH2) complexes from the purple photosynthetic bacterium Rhodopseudomonas acidophila. The variations of the fluorescence transients were studied as a function of the excitation fluence, the repetition rate of the excitation and the sample preparation conditions. Here we present the results obtained on detergent solubilized LH2 complexes, i.e., avoiding intercomplex interactions, and show that a simple four-state model is sufficient to grasp the experimental observations quantitatively without the need for any free parameters. This approach allows us to obtain a quantitative measure for the singlet-triplet annihilation rate in isolated, noninteracting LH2 complexes.

The splicing regulator Rbfox1 (A2BP1) controls neuronal excitation in the mammalian brain

PubMed Central

Gehman, Lauren T.; Stoilov, Peter; Maguire, Jamie; Damianov, Andrey; Lin, Chia-Ho; Shiue, Lily; Ares, Manuel; Mody, Istvan; Black, Douglas L.

2011-01-01

The Rbfox family of RNA binding proteins regulates alternative splicing of many important neuronal transcripts but their role in neuronal physiology is not clear1. We show here that central nervous system (CNS)-specific deletion of the Rbfox1 gene results in heightened susceptibility to spontaneous and kainic acid-induced seizures. Electrophysiological recording reveals a corresponding increase in neuronal excitability in the dentate gyrus of the knockout mice. Whole transcriptome analyses identify multiple splicing changes in the Rbfox1−/− brain with few changes in overall transcript abundance. These splicing changes alter proteins that mediate synaptic transmission and membrane excitation, some of which are implicated in human epilepsy. Thus, Rbfox1 directs a genetic program required in the prevention of neuronal hyperexcitation and seizures. The Rbfox1 knockout mice provide a new model to study the post-transcriptional regulation of synaptic function. PMID:21623373

Membrane Cholesterol in Skeletal Muscle: A Novel Player in Excitation-Contraction Coupling and Insulin Resistance

PubMed Central

Barrientos, G.; Sánchez-Aguilera, P.; Jaimovich, E.; Hidalgo, C.

2017-01-01

Membrane cholesterol is critical for signaling processes in a variety of tissues. We will address here current evidence supporting an emerging role of cholesterol on excitation-contraction coupling and glucose transport in skeletal muscle. We have centered our review on the transverse tubule system, a complex network of narrow plasma membrane invaginations that propagate membrane depolarization into the fiber interior and allow nutrient delivery into the fibers. We will discuss current evidence showing that transverse tubule membranes have remarkably high cholesterol levels and we will address how modifications of cholesterol content influence excitation-contraction coupling. In addition, we will discuss how membrane cholesterol levels affect glucose transport by modulating the insertion into the membrane of the main insulin-sensitive glucose transporter GLUT4. Finally, we will address how the increased membrane cholesterol levels displayed by obese animals, which also present insulin resistance, affect these two particular skeletal muscle functions. PMID:28367451

Exciton–exciton annihilation and biexciton stimulated emission in graphene nanoribbons

DOE PAGES

Soavi, Giancarlo; Dal Conte, Stefano; Manzoni, Cristian; ...

2016-03-17

Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron–hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton–exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ≈250meV, in very goodmore » agreement with theoretical results from quantum Monte Carlo simulations. As a result, these observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics.« less

Ab Initio Multiple Spawning Photochemical Dynamics of DMABN Using GPUs

DOE PAGES

Curchod, Basile F. E.; Sisto, Aaron; Martinez, Todd J.

2016-12-15

The ultrafast decay dynamics of 4-( N,N-dimethylamino)benzonitrile (DMABN) following photoexcitation was studied with the ab initio multiple spawning (AIMS) method, combined with GPU-accelerated linear-response time-dependent density functional theory (LR-TDDFT). We validate the LR-TDDFT method for this case and then present a detailed analysis of the first ≈200 fs of DMABN excited-state dynamics. Almost complete nonadiabatic population transfer from S 2 (the initially populated bright state) to S 1 takes place in less than 50 fs, without significant torsion of the dimethylamino (DMA) group. Significant torsion of the DMA group is only observed after the nuclear wavepacket reaches S 1 andmore » acquires locally excited electronic character. Here, our results show that torsion of the DMA group is not prerequisite for nonadiabatic transitions in DMABN, although such motion is indeed relevant on the lowest excited state (S 1).« less

Single pulse two photon fluorescence lifetime imaging (SP-FLIM) with MHz pixel rate.

PubMed

Eibl, Matthias; Karpf, Sebastian; Weng, Daniel; Hakert, Hubertus; Pfeiffer, Tom; Kolb, Jan Philip; Huber, Robert

2017-07-01

Two-photon-excited fluorescence lifetime imaging microscopy (FLIM) is a chemically specific 3-D sensing modality providing valuable information about the microstructure, composition and function of a sample. However, a more widespread application of this technique is hindered by the need for a sophisticated ultra-short pulse laser source and by speed limitations of current FLIM detection systems. To overcome these limitations, we combined a robust sub-nanosecond fiber laser as the excitation source with high analog bandwidth detection. Due to the long pulse length in our configuration, more fluorescence photons are generated per pulse, which allows us to derive the lifetime with a single excitation pulse only. In this paper, we show high quality FLIM images acquired at a pixel rate of 1 MHz. This approach is a promising candidate for an easy-to-use and benchtop FLIM system to make this technique available to a wider research community.

Multiple Types of Topological Fermions in Transition Metal Silicides

DOE PAGES

Tang, Peizhe; Zhou, Quan; Zhang, Shou -Cheng

2017-11-17

Exotic massless fermionic excitations with nonzero Berry flux, other than the Dirac and Weyl fermions, could exist in condensed matter systems under the protection of crystalline symmetries, such as spin-1 excitations with threefold degeneracy and spin-3/2 Rarita-Schwinger-Weyl fermions. Herein, by using the ab initio density functional theory, we show that these unconventional quasiparticles coexist with type-I and type-II Weyl fermions in a family of transition metal silicides, including CoSi, RhSi, RhGe, and CoGe, when spin-orbit coupling is considered. Their nontrivial topology results in a series of extensive Fermi arcs connecting projections of these bulk excitations on the side surface, whichmore » is confirmed by (001) surface electronic spectra of CoSi. Additionally, these stable arc states exist within a wide energy window around the Fermi level, which makes them readily accessible in angle-resolved photoemission spectroscopy measurements.« less

Towards two-photon excited endogenous fluorescence lifetime imaging microendoscopy

PubMed Central

Hage, C. H.; Leclerc, P.; Brevier, J.; Fabert, M.; Le Nézet, C.; Kudlinski, A.; Héliot, L.; Louradour, F.

2017-01-01

In situ fluorescence lifetime imaging microscopy (FLIM) in an endoscopic configuration of the endogenous biomarker nicotinamide adenine dinucleotide (NADH) has a great potential for malignant tissue diagnosis. Moreover, two-photon nonlinear excitation provides intrinsic optical sectioning along with enhanced imaging depth. We demonstrate, for the first time to our knowledge, nonlinear endogenous FLIM in a fibered microscope with proximal detection, applied to NADH in cultured cells, as a first step to a nonlinear endomicroscope, using a double-clad microstructured fiber with convenient fiber length (> 3 m) and excitation pulse duration (≈50 fs). Fluorescence photons are collected by the fiber inner cladding and we show that its contribution to the impulse response function (IRF), which originates from its intermodal and chromatic dispersions, is small (< 600 ps) and stable for lengths up to 8 m and allows for short lifetime measurements. We use the phasor representation as a quick visualization tool adapted to the endoscopy speed requirements. PMID:29359093

Na, K-ATPase activity regulates AMPA receptor turnover through proteasome-mediated proteolysis

PubMed Central

Zhang, Dawei; Hou, Qingming; Wang, Min; Lin, Amy; Jarzylo, Larissa; Navis, Allison; Raissi, Aram; Liu, Fang; Man, Heng-Ye

2009-01-01

Neuronal activity largely depends on two key components on the membrane: the Na, K-ATPase (NKA) that maintains the ion gradients and sets the foundation of excitability, and the ionotropic glutamatergic AMPA receptors (AMPARs) through which sodium influx forms the driving force for excitation. Because the frequent sodium transients from glutamate receptor activity need to be efficiently extruded, a functional coupling between NKA and AMPARs should be a necessary cellular device for synapse physiology. We show that NKA is enriched at synapses and associates with AMPARs. NKA dysfunction induces a rapid reduction in AMPAR cell-surface expression as well as total protein abundance, leading to a long-lasting depression in synaptic transmission. AMPAR proteolysis requires sodium influx, proteasomal activity and receptor internalization. These data elucidate a novel mechanism by which NKA regulates AMPAR turnover and thereby synaptic strength and brain function. PMID:19357275

Scattering of targets over layered half space using a semi-analytic method in conjunction with FDTD algorithm.

PubMed

Cao, Le; Wei, Bing

2014-08-25

Finite-difference time-domain (FDTD) algorithm with a new method of plane wave excitation is used to investigate the RCS (Radar Cross Section) characteristics of targets over layered half space. Compare with the traditional excitation plane wave method, the calculation memory and time requirement is greatly decreased. The FDTD calculation is performed with a plane wave incidence, and the RCS of far field is obtained by extrapolating the currently calculated data on the output boundary. However, methods available for extrapolating have to evaluate the half space Green function. In this paper, a new method which avoids using the complex and time-consuming half space Green function is proposed. Numerical results show that this method is in good agreement with classic algorithm and it can be used in the fast calculation of scattering and radiation of targets over layered half space.

Vectorial model for guided-mode resonance gratings

NASA Astrophysics Data System (ADS)

Fehrembach, A.-L.; Gralak, B.; Sentenac, A.

2018-04-01

We propose a self-consistent vectorial method, based on a Green's function technique, to describe the resonances that appear in guided-mode resonance gratings. The model provides intuitive expressions of the reflectivity and transmittivity matrices of the structure, involving coupling integrals between the modes of a planar reference structure and radiative modes. When one mode is excited, the diffracted field for a suitable polarization can be written as the sum of a resonant and a nonresonant term, thus extending the intuitive approach used to explain the Fano shape of the resonance in scalar configurations. When two modes are excited, we derive a physical analysis in a configuration which requires a vectorial approach. We provide numerical validations of our model. From a technical point of view, we show how the Green's tensor of our planar reference structure can be expressed as two scalar Green's functions, and how to deal with the singularity of the Green's tensor.

Decoupling indirect topographic cross-talk in band excitation piezoresponse force microscopy imaging and spectroscopy

DOE PAGES

Mazet, Lucie; Jesse, Stephen; Niu, Gang; ...

2016-06-20

Here, all scanning probe microscopies are subjected to topographic cross-talk, meaning the topography-related contrast in functional images. Here, we investigate the signatures of indirect topographic cross-talk in piezoresponse force microscopy (PFM) imaging and spectroscopy and its decoupling using band excitation (BE) method in ferroelectric BaTiO 3 deposited on the Si substrates with free standing nanopillars of diameter 50 nm. Comparison between the single-frequency PFM and BE-PFM results shows that the measured signal can be significantly distorted by topography-induced shifts in the contact resonance frequency and cantilever transfer function. However, with proper correction, such shifts do not affect PFM imaging andmore » hysteresis loop measurements. This suggests the necessity of an advanced approach, such as BE-PFM, for detection of intrinsic sample piezoresponse on the topographically non-uniform surfaces.« less

Maternal creatine supplementation affects the morpho-functional development of hippocampal neurons in rat offspring.

PubMed

Sartini, S; Lattanzi, D; Ambrogini, P; Di Palma, M; Galati, C; Savelli, D; Polidori, E; Calcabrini, C; Rocchi, M B L; Sestili, P; Cuppini, R

2016-01-15

Creatine supplementation has been shown to protect neurons from oxidative damage due to its antioxidant and ergogenic functions. These features have led to the hypothesis of creatine supplementation use during pregnancy as prophylactic treatment to prevent CNS damage, such as hypoxic-ischemic encephalopathy. Unfortunately, very little is known on the effects of creatine supplementation during neuron differentiation, while in vitro studies revealed an influence on neuron excitability, leaving the possibility of creatine supplementation during the CNS development an open question. Using a multiple approach, we studied the hippocampal neuron morphological and functional development in neonatal rats born by dams supplemented with 1% creatine in drinking water during pregnancy. CA1 pyramidal neurons of supplemented newborn rats showed enhanced dendritic tree development, increased LTP maintenance, larger evoked-synaptic responses, and higher intrinsic excitability in comparison to controls. Moreover, a faster repolarizing phase of action potential with the appearance of a hyperpolarization were recorded in neurons of the creatine-treated group. Consistently, CA1 neurons of creatine exposed pups exhibited a higher maximum firing frequency than controls. In summary, we found that creatine supplementation during pregnancy positively affects morphological and electrophysiological development of CA1 neurons in offspring rats, increasing neuronal excitability. Altogether, these findings emphasize the need to evaluate the benefits and the safety of maternal intake of creatine in humans. Copyright © 2015 IBRO. Published by Elsevier Ltd. All rights reserved.

Competition between the compound and the pre-compound emission processes in α-induced reactions at near astrophysical energy to well above it

NASA Astrophysics Data System (ADS)

Sharma, Manoj Kumar; Sharma, Vijay Raj; Yadav, Abhiskek; Singh, Pushpendra P.; Singh, B. P.; Prasad, R.

2016-04-01

The study of pre-compound emission in α-induced reactions, particularly at the low incident energies, is of considerable interest as the pre-compound emission is more likely to occur at higher energies. With a view to study the competition between the compound and the pre-compound emission processes in α-induced reactions at different energies and with different targets, a systematics for neutron emission channels in targets 51V, 55Mn, 93Nb, 121, 123Sb and 141Pr at energy ranging from astrophysical interest to well above it, has been developed. The off-line γ-ray-spectrometry based activation technique has been adopted to measure the excitation functions. The experimental excitation functions have been analysed within the framework of the compound nucleus mechanism based on the Weisskopf-Ewing model and the pre-compound emission calculations based on the geometry dependent hybrid model. The analysis of the data shows that experimental excitation functions could be reproduced only when the pre-compound emission, simulated theoretically, is taken into account. The strength of pre-compound emission process for each system has been obtained by deducing the pre-compound fraction. Analysis of data indicates that in α-induced reactions, the pre-compound emission process plays an important role, particularly at the low incident energies, where the pure compound nucleus process is likely to dominate.

Effects of cluster-shell competition and BCS-like pairing in 12C

NASA Astrophysics Data System (ADS)

Matsuno, H.; Itagaki, N.

2017-12-01

The antisymmetrized quasi-cluster model (AQCM) was proposed to describe α-cluster and jj-coupling shell models on the same footing. In this model, the cluster-shell transition is characterized by two parameters, R representing the distance between α clusters and Λ describing the breaking of α clusters, and the contribution of the spin-orbit interaction, very important in the jj-coupling shell model, can be taken into account starting with the α-cluster model wave function. Not only the closure configurations of the major shells but also the subclosure configurations of the jj-coupling shell model can be described starting with the α-cluster model wave functions; however, the particle-hole excitations of single particles have not been fully established yet. In this study we show that the framework of AQCM can be extended even to the states with the character of single-particle excitations. For ^{12}C, two-particle-two-hole (2p2h) excitations from the subclosure configuration of 0p_{3/2} corresponding to a BCS-like pairing are described, and these shell model states are coupled with the three α-cluster model wave functions. The correlation energy from the optimal configuration can be estimated not only in the cluster part but also in the shell model part. We try to pave the way to establish a generalized description of the nuclear structure.

HAL® exoskeleton training improves walking parameters and normalizes cortical excitability in primary somatosensory cortex in spinal cord injury patients.

PubMed

Sczesny-Kaiser, Matthias; Höffken, Oliver; Aach, Mirko; Cruciger, Oliver; Grasmücke, Dennis; Meindl, Renate; Schildhauer, Thomas A; Schwenkreis, Peter; Tegenthoff, Martin

2015-08-20

Reorganization in the sensorimotor cortex accompanied by increased excitability and enlarged body representations is a consequence of spinal cord injury (SCI). Robotic-assisted bodyweight supported treadmill training (BWSTT) was hypothesized to induce reorganization and improve walking function. To assess whether BWSTT with hybrid assistive limb® (HAL®) exoskeleton affects cortical excitability in the primary somatosensory cortex (S1) in SCI patients, as measured by paired-pulse somatosensory evoked potentials (ppSEP) stimulated above the level of injury. Eleven SCI patients took part in HAL® assisted BWSTT for 3 months. PpSEP were conducted before and after this training period, where the amplitude ratios (SEP amplitude following double pulses - SEP amplitude following single pulses) were assessed and compared to eleven healthy control subjects. To assess improvement in walking function, we used the 10-m walk test, timed-up-and-go test, the 6-min walk test, and the lower extremity motor score. PpSEPs were significantly increased in SCI patients as compared to controls at baseline. Following training, ppSEPs were increased from baseline and no longer significantly differed from controls. Walking parameters also showed significant improvements, yet there was no significant correlation between ppSEP measures and walking parameters. The findings suggest that robotic-assisted BWSTT with HAL® in SCI patients is capable of inducing cortical plasticity following highly repetitive, active locomotive use of paretic legs. While there was no significant correlation of excitability with walking parameters, brain areas other than S1 might reflect improvement of walking functions. EEG and neuroimaging studies may provide further information about supraspinal plastic processes and foci in SCI rehabilitation.

Two-Component Structure in the Entanglement Spectrum of Highly Excited States

NASA Astrophysics Data System (ADS)

Yang, Zhi-Cheng; Chamon, Claudio; Hamma, Alioscia; Mucciolo, Eduardo R.

2015-12-01

We study the entanglement spectrum of highly excited eigenstates of two known models that exhibit a many-body localization transition, namely the one-dimensional random-field Heisenberg model and the quantum random energy model. Our results indicate that the entanglement spectrum shows a "two-component" structure: a universal part that is associated with random matrix theory, and a nonuniversal part that is model dependent. The nonuniversal part manifests the deviation of the highly excited eigenstate from a true random state even in the thermalized phase where the eigenstate thermalization hypothesis holds. The fraction of the spectrum containing the universal part decreases as one approaches the critical point and vanishes in the localized phase in the thermodynamic limit. We use the universal part fraction to construct an order parameter for measuring the degree of randomness of a generic highly excited state, which is also a promising candidate for studying the many-body localization transition. Two toy models based on Rokhsar-Kivelson type wave functions are constructed and their entanglement spectra are shown to exhibit the same structure.

Deciphering excited state evolution in halorhodopsin with stimulated emission pumping.

PubMed

Bismuth, Oshrat; Komm, Pavel; Friedman, Noga; Eliash, Tamar; Sheves, Mordechai; Ruhman, Sanford

2010-03-04

The primary photochemical dynamics of Hb. pharaonis Halorhodopsin (pHR) are investigated by femtosecond visible pump-near IR dump-hyperspectral probe spectroscopy. The efficiency of excited state depletion is deduced from transient changes in absorption, recorded with and without stimulated emission pumping (SEP), as a function of the dump delay. The concomitant reduction of photocycle population is assessed by probing the "K" intermediate difference spectrum. Results show that the cross section for stimulating emission is nearly constant throughout the fluorescent state lifetime. Probing "K" demonstrates that dumping produces a proportionate reduction in photocycle yields. We conclude that, despite its nonexponential internal conversion (IC) kinetics, the fluorescent state in pHR constitutes a single intermediate in the photocycle. This contrasts with conclusions drawn from the study of primary events in the related chloride pump from Hb. salinarum (sHR), believed to produce the "K" intermediate from a distinct short-lived subpopulation in the excited state. Our discoveries concerning internal conversion dynamics in pHR are discussed in light of recent expectations for similar excited state dynamics in both proteins.

Energy-filtered cold electron transport at room temperature

PubMed Central

Bhadrachalam, Pradeep; Subramanian, Ramkumar; Ray, Vishva; Ma, Liang-Chieh; Wang, Weichao; Kim, Jiyoung; Cho, Kyeongjae; Koh, Seong Jin

2014-01-01

Fermi-Dirac electron thermal excitation is an intrinsic phenomenon that limits functionality of various electron systems. Efforts to manipulate electron thermal excitation have been successful when the entire system is cooled to cryogenic temperatures, typically <1 K. Here we show that electron thermal excitation can be effectively suppressed at room temperature, and energy-suppressed electrons, whose energy distribution corresponds to an effective electron temperature of ~45 K, can be transported throughout device components without external cooling. This is accomplished using a discrete level of a quantum well, which filters out thermally excited electrons and permits only energy-suppressed electrons to participate in electron transport. The quantum well (~2 nm of Cr2O3) is formed between source (Cr) and tunnelling barrier (SiO2) in a double-barrier-tunnelling-junction structure having a quantum dot as the central island. Cold electron transport is detected from extremely narrow differential conductance peaks in electron tunnelling through CdSe quantum dots, with full widths at half maximum of only ~15 mV at room temperature. PMID:25204839

A bright cyan-excitable orange fluorescent protein facilitates dual-emission microscopy and enhances bioluminescence imaging in vivo

PubMed Central

Chu, Jun; Oh, Young-Hee; Sens, Alex; Ataie, Niloufar; Dana, Hod; Macklin, John J.; Laviv, Tal; Welf, Erik S.; Dean, Kevin M.; Zhang, Feijie; Kim, Benjamin B.; Tang, Clement Tran; Hu, Michelle; Baird, Michelle A.; Davidson, Michael W.; Kay, Mark A.; Fiolka, Reto; Yasuda, Ryohei; Kim, Douglas S.; Ng, Ho-Leung; Lin, Michael Z.

2016-01-01

Orange-red fluorescent proteins (FPs) are widely used in biomedical research for multiplexed epifluorescence microscopy with GFP-based probes, but their different excitation requirements make multiplexing with new advanced microscopy methods difficult. Separately, orange-red FPs are useful for deep-tissue imaging in mammals due to the relative tissue transmissibility of orange-red light, but their dependence on illumination limits their sensitivity as reporters in deep tissues. Here we describe CyOFP1, a bright engineered orange-red FP that is excitable by cyan light. We show that CyOFP1 enables single-excitation multiplexed imaging with GFP-based probes in single-photon and two-photon microscopy, including time-lapse imaging in light-sheet systems. CyOFP1 also serves as an efficient acceptor for resonance energy transfer from the highly catalytic blue-emitting luciferase NanoLuc. An optimized fusion of CyOFP1 and NanoLuc, called Antares, functions as a highly sensitive bioluminescent reporter in vivo, producing substantially brighter signals from deep tissues than firefly luciferase and other bioluminescent proteins. PMID:27240196

Pygmy dipole mode in deformed neutron-rich Mg isotopes close to the drip line

NASA Astrophysics Data System (ADS)

Yoshida, Kenichi

2009-10-01

We investigate the microscopic structure of the low-lying isovector-dipole excitation mode in neutron-rich Mg36,38,40 close to the drip line by means of the deformed quasiparticle random-phase approximation employing the Skyrme and the local pairing energy-density functionals. It is found that the low-lying bump structure above the neutron emission-threshold energy develops when the drip line is approached, and that the isovector dipole strength at Ex<10 MeV exhausts about 6.0% of the classical Thomas-Reiche-Kuhn dipole sum rule in Mg40. We obtained the collective dipole modes at around 8-10 MeV in Mg isotopes, that consist of many two-quasiparticle excitations of the neutron. The transition density clearly shows an oscillation of the neutron skin against the isoscalar core. We found significant coupling effects between the dipole and octupole excitation modes due to the nuclear deformation. It is also found that the responses for the compressional dipole and isoscalar octupole excitations are much enhanced in the lower energy region.

The triplet excited state of Bodipy: formation, modulation and application.

PubMed

Zhao, Jianzhang; Xu, Kejing; Yang, Wenbo; Wang, Zhijia; Zhong, Fangfang

2015-12-21

Boron dipyrromethene (Bodipy) is one of the most extensively investigated organic chromophores. Most of the investigations are focused on the singlet excited state of Bodipy, such as fluorescence. In stark contrast, the study of the triplet excited state of Bodipy is limited, but it is an emerging area, since the triplet state of Bodipy is tremendously important for several areas, such as the fundamental photochemistry study, photodynamic therapy (PDT), photocatalysis and triplet-triplet annihilation (TTA) upconversion. The recent developments in the study of the production, modulation and application of the triplet excited state of Bodipy are discussed in this review article. The formation of the triplet state of Bodipy upon photoexcitation, via the well known approach such as the heavy atom effect (including I, Br, Ru, Ir, etc.), and the new methods, such as using a spin converter (e.g. C60), charge recombination, exciton coupling and the doubly substituted excited state, are summarized. All the Bodipy-based triplet photosensitizers show strong absorption of visible or near IR light and the long-lived triplet excited state, which are important for the application of the triplet excited state in PDT or photocatalysis. Moreover, the methods for switching (or modulation) of the triplet excited state of Bodipy were discussed, such as those based on the photo-induced electron transfer (PET), by controlling the competing Förster-resonance-energy-transfer (FRET), or the intermolecular charge transfer (ICT). Controlling the triplet excited state will give functional molecules such as activatable PDT reagents or molecular devices. It is worth noting that switching of the singlet excited state and the triplet state of Bodipy may follow different principles. Application of the triplet excited state of Bodipy in PDT, hydrogen (H2) production, photoredox catalytic organic reactions and TTA upconversion were discussed. The challenges and the opportunities in these areas were briefly discussed.

Correlated wave functions for three-particle systems with Coulomb interaction - The muonic helium atom

NASA Technical Reports Server (NTRS)

Huang, K.-N.

1977-01-01

A computational procedure for calculating correlated wave functions is proposed for three-particle systems interacting through Coulomb forces. Calculations are carried out for the muonic helium atom. Variational wave functions which explicitly contain interparticle coordinates are presented for the ground and excited states. General Hylleraas-type trial functions are used as the basis for the correlated wave functions. Excited-state energies of the muonic helium atom computed from 1- and 35-term wave functions are listed for four states.

Gonadal Steroids: Effects on Excitability of Hippocampal Pyramidal Cells

NASA Astrophysics Data System (ADS)

Teyler, Timothy J.; Vardaris, Richard M.; Lewis, Deborah; Rawitch, Allen B.

1980-08-01

Electrophysiological field potentials from hippocampal slices of rat brain show sex-linked differences in response to 1 × 10-10M concentrations of estradiol and testosterone added to the incubation medium. Slices from male rats show increased excitability to estradiol and not to testosterone. Slices from female rats are not affected by estradiol, but slices from female rats in diestrus show increased excitability in response to testosterone whereas slices from females in proestrus show decreased excitability.

Changes in neural network homeostasis trigger neuropsychiatric symptoms.

PubMed

Winkelmann, Aline; Maggio, Nicola; Eller, Joanna; Caliskan, Gürsel; Semtner, Marcus; Häussler, Ute; Jüttner, René; Dugladze, Tamar; Smolinsky, Birthe; Kowalczyk, Sarah; Chronowska, Ewa; Schwarz, Günter; Rathjen, Fritz G; Rechavi, Gideon; Haas, Carola A; Kulik, Akos; Gloveli, Tengis; Heinemann, Uwe; Meier, Jochen C

2014-02-01

The mechanisms that regulate the strength of synaptic transmission and intrinsic neuronal excitability are well characterized; however, the mechanisms that promote disease-causing neural network dysfunction are poorly defined. We generated mice with targeted neuron type-specific expression of a gain-of-function variant of the neurotransmitter receptor for glycine (GlyR) that is found in hippocampectomies from patients with temporal lobe epilepsy. In this mouse model, targeted expression of gain-of-function GlyR in terminals of glutamatergic cells or in parvalbumin-positive interneurons persistently altered neural network excitability. The increased network excitability associated with gain-of-function GlyR expression in glutamatergic neurons resulted in recurrent epileptiform discharge, which provoked cognitive dysfunction and memory deficits without affecting bidirectional synaptic plasticity. In contrast, decreased network excitability due to gain-of-function GlyR expression in parvalbumin-positive interneurons resulted in an anxiety phenotype, but did not affect cognitive performance or discriminative associative memory. Our animal model unveils neuron type-specific effects on cognition, formation of discriminative associative memory, and emotional behavior in vivo. Furthermore, our data identify a presynaptic disease-causing molecular mechanism that impairs homeostatic regulation of neural network excitability and triggers neuropsychiatric symptoms.

Analytical excited state forces for the time-dependent density-functional tight-binding method.

PubMed

Heringer, D; Niehaus, T A; Wanko, M; Frauenheim, Th

2007-12-01

An analytical formulation for the geometrical derivatives of excitation energies within the time-dependent density-functional tight-binding (TD-DFTB) method is presented. The derivation is based on the auxiliary functional approach proposed in [Furche and Ahlrichs, J Chem Phys 2002, 117, 7433]. To validate the quality of the potential energy surfaces provided by the method, adiabatic excitation energies, excited state geometries, and harmonic vibrational frequencies were calculated for a test set of molecules in excited states of different symmetry and multiplicity. According to the results, the TD-DFTB scheme surpasses the performance of configuration interaction singles and the random phase approximation but has a lower quality than ab initio time-dependent density-functional theory. As a consequence of the special form of the approximations made in TD-DFTB, the scaling exponent of the method can be reduced to three, similar to the ground state. The low scaling prefactor and the satisfactory accuracy of the method makes TD-DFTB especially suitable for molecular dynamics simulations of dozens of atoms as well as for the computation of luminescence spectra of systems containing hundreds of atoms. (c) 2007 Wiley Periodicals, Inc.

Dynamics of Functionalized Surface Molecular Monolayers Studied with Ultrafast Infrared Vibrational Spectroscopy

PubMed Central

Rosenfeld, Daniel E.; Nishida, Jun; Yan, Chang; Gengeliczki, Zsolt; Smith, Brian J.; Fayer, Michael D.

2012-01-01

The structural dynamics of thin films consisting of tricarbonyl (1,10-phenanthroline)rhenium chloride (RePhen(CO)3Cl) linked to an alkyl silane monolayer through a triazole linker synthesized on silica-on-calcium-fluoride substrates are investigated using ultrafast infrared (IR) techniques. Ultrafast 2D IR vibrational echo experiments and polarization selective heterodyne detected transient grating (HDTG) measurements, as well as polarization dependent FT-IR and AFM experiments are employed to study the samples. The vibrational echo experiments measure spectral diffusion, while the HDTG experiments measure the vibrational excited state population relaxation and investigate the vibrational transition dipole orientational anisotropy decay. To investigate the anticipated impact of vibrational excitation transfer, which can be caused by the high concentration of RePhen(CO)3Cl in the monolayer, a concentration dependence of the spectral diffusion is measured. To generate a range of concentrations, mixed monolayers consisting of both hydrogen terminated and triazole/RePhen(CO)3Cl terminated alkyl silanes are synthesized. It is found that the measured rate of spectral diffusion is independent of concentration, with all samples showing spectral diffusion of 37 ± 6 ps. To definitively test for vibrational excitation transfer, polarization selective HDTG experiments are conducted. Excitation transfer will cause anisotropy decay. Polarization resolved heterodyne detected transient grating spectroscopy is sensitive to anisotropy decay (depolarization) caused by excitation transfer and molecular reorientation. The HDTG experiments show no evidence of anisotropy decay on the appropriate time scale, demonstrating the absence of excitation transfer the RePhen(CO)3Cl. Therefore the influence of excitation transfer on spectral diffusion is inconsequential in these samples, and the vibrational echo measurements of spectral diffusion report solely on structural dynamics. A small amount of very fast (~2 ps time scale) anisotropy decay is observed. The decay is concentration independent, and is assigned to wobbling-in-a-cone orientational motions of the RePhen(CO)3Cl. Theoretical calculations reported previously for experiments on a single concentration of the same type of sample suggested the presence of some vibrational excitation transfer and excitation transfer induced spectral diffusion. Possible reasons for the experimentally observed lack of excitation transfer in these high concentration samples are discussed. PMID:23259027

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

Moore, II, Barry; Schrader, Robert L.; Kowalski, Karol

The longest-wavelength π-to-π* electronic excitations of rhodamine-like dyes (RDs) with different group16 heteroatoms (O, S, Se, Te) have been investigated. Time-dependent Kohn–Sham theory (TDKST) calculations were compared with coupled-cluster (CC) and equations-of-motion (EOM) CC results for π-to-π* singlet and triplet excitations. The RDs exhibit characteristics in the TDKST calculations that are very similar to previously investigated cyanine dyes, in the sense that the singlet energies obtained with nonhybrid functionals are too high compared with the CC results at the SD(T) level. The errors became increasingly larger for functionals with increasing amounts of exact exchange. TDKST with all tested functionals ledmore » to severe underestimations of the corresponding triplet excitations and overestimations of the singlet--triplet gaps. Long-range-corrected range-separated exchange and "optimal tuning" of the range separation parameter did not significantly improve the TDKST results. A detailed analysis suggests that the problem is differential electron correlation between the ground and excited states, which is not treated sufficiently by the relatively small integrals over the exchange-correlation response kernel that enters the excitation energy expression. As a result, numerical criteria are suggested that may help identify "cyanine-like" problems in TDKST calculations of excitation spectra.« less

Jet noise modification by the 'whistler nozzle'

NASA Technical Reports Server (NTRS)

Hasan, M. A. Z.; Islam, O.; Hussain, A. K. M. F.

1984-01-01

The farfield noise characteristics of a subsonic whistler nozzle jet are measured as a function of Mach number (0.25, 0.37, and, 0.51), emission angle, and excitation mode. It is shown that a whistler nozzle has greater total and broadband acoustic power than an excited contraction nozzle; and that the intensity of far-field noise is a function of emission angle, Mach number, and whistler excitation stage. The whistler nozzle excitation produces broadband noise amplification with constant spectral shape; the broadband noise amplification (without associated whistler tones and harmonics) increases omnidirectionally with emission angle at all Mach numbers; and the broadband amplification factor decreases as Mach number and emission angle increase. Finally the whistler nozzle is described as a very efficient but inexpensive siren with applications in not only jet excitation but also acoustics.

Electronic and Structural Elements That Regulate the Excited-State Dynamics in Purine Nucleobase Derivatives

PubMed Central

2015-01-01

The excited-state dynamics of the purine free base and 9-methylpurine are investigated using experimental and theoretical methods. Femtosecond broadband transient absorption experiments reveal that excitation of these purine derivatives in aqueous solution at 266 nm results primarily in ultrafast conversion of the S2(ππ*) state to the vibrationally excited 1nπ* state. Following vibrational and conformational relaxation, the 1nπ* state acts as a doorway state in the efficient population of the triplet manifold with an intersystem crossing lifetime of hundreds of picoseconds. Experiments show an almost 2-fold increase in the intersystem crossing rate on going from polar aprotic to nonpolar solvents, suggesting that a solvent-dependent energy barrier must be surmounted to access the singlet-to-triplet crossing region. Ab initio static and surface-hopping dynamics simulations lend strong support to the proposed relaxation mechanism. Collectively, the experimental and computational results demonstrate that the accessibility of the nπ* states and the topology of the potential energy surfaces in the vicinity of conical intersections are key elements in controlling the excited-state dynamics of the purine derivatives. From a structural perspective, it is shown that the purine chromophore is not responsible for the ultrafast internal conversion in the adenine and guanine monomers. Instead, C6 functionalization plays an important role in regulating the rates of radiative and nonradiative relaxation. C6 functionalization inhibits access to the 1nπ* state while simultaneously facilitating access to the 1ππ*(La)/S0 conical intersection, such that population of the 1nπ* state cannot compete with the relaxation pathways to the ground state involving ring puckering at the C2 position. PMID:25763596

Brain Distribution and Modulation of Neuronal Excitability by Indicaxanthin From Opuntia Ficus Indica Administered at Nutritionally-Relevant Amounts

PubMed Central

Gambino, Giuditta; Allegra, Mario; Sardo, Pierangelo; Attanzio, Alessandro; Tesoriere, Luisa; Livrea, Maria A.; Ferraro, Giuseppe; Carletti, Fabio

2018-01-01

Several studies have recently investigated the role of nutraceuticals in complex pathophysiological processes such as oxidative damages, inflammatory conditions and excitotoxicity. In this regard, the effects of nutraceuticals on basic functions of neuronal cells, such as excitability, are still poorly investigated. For this reason, the possible modulation of neuronal excitability by phytochemicals (PhC) could represent an interesting field of research given that excitotoxicity phenomena are involved in neurodegenerative alterations leading, for example, to Alzheimer’s disease. The present study was focused on indicaxanthin from Opuntia ficus indica, a bioactive betalain pigment, with a proven antioxidant and anti-inflammatory potential, previously found to cross blood-brain barrier (BBB) and to modulate the bioelectric activity of hippocampal neurons. On this basis, we aimed at detecting the specific brain areas where indicaxanthin localizes after oral administration at dietary-achievable amounts and highlighting eventual local effects on the excitability of single neuronal units. HPLC analysis of brain tissue 1 h after ingestion of 2 μmol/kg indicaxanthin indicated that the phytochemical accumulates in cortex, hippocampus, diencephalon, brainstem and cerebellum, but not in the striato-pallidal complex. Then, electrophysiological recordings, applying the microiontophoretic technique, were carried out with different amounts of indicaxanthin (0.34, 0.17, 0.085 ng/neuron) to assess whether indicaxanthin influenced the neuronal firing rate. The data showed that the bioelectric activity of neurons belonging to different brain areas was modulated after local injection of indicaxanthin, mainly with dose-related responses. A predominating inhibitory effect was observed, suggesting a possible novel beneficial effect of indicaxanthin in reducing cell excitability. These findings can constitute a new rationale for exploring biological mechanisms through which PhC could modulate neuronal function with a relapse on complex cognitive brain process and related neurodegenerative conditions. PMID:29867444

Reduced-cost linear-response CC2 method based on natural orbitals and natural auxiliary functions

PubMed Central

Mester, Dávid

2017-01-01

A reduced-cost density fitting (DF) linear-response second-order coupled-cluster (CC2) method has been developed for the evaluation of excitation energies. The method is based on the simultaneous truncation of the molecular orbital (MO) basis and the auxiliary basis set used for the DF approximation. For the reduction of the size of the MO basis, state-specific natural orbitals (NOs) are constructed for each excited state using the average of the second-order Møller–Plesset (MP2) and the corresponding configuration interaction singles with perturbative doubles [CIS(D)] density matrices. After removing the NOs of low occupation number, natural auxiliary functions (NAFs) are constructed [M. Kállay, J. Chem. Phys. 141, 244113 (2014)], and the NAF basis is also truncated. Our results show that, for a triple-zeta basis set, about 60% of the virtual MOs can be dropped, while the size of the fitting basis can be reduced by a factor of five. This results in a dramatic reduction of the computational costs of the solution of the CC2 equations, which are in our approach about as expensive as the evaluation of the MP2 and CIS(D) density matrices. All in all, an average speedup of more than an order of magnitude can be achieved at the expense of a mean absolute error of 0.02 eV in the calculated excitation energies compared to the canonical CC2 results. Our benchmark calculations demonstrate that the new approach enables the efficient computation of CC2 excitation energies for excited states of all types of medium-sized molecules composed of up to 100 atoms with triple-zeta quality basis sets. PMID:28527453

Prefrontal cortex-projecting glutamatergic thalamic paraventricular nucleus-excited by hypocretin: a feedforward circuit that may enhance cognitive arousal.

PubMed

Huang, Hao; Ghosh, Prabhat; van den Pol, Anthony N

2006-03-01

The paraventricular thalamic nucleus (PVT) receives one of the most dense innervations by hypothalamic hypocretin/orexin (Hcrt) neurons, which play important roles in sleep-wakefulness, attention, and autonomic function. The PVT projects to several loci, including the medial prefrontal cortex (mPFC), a cortical region involved in associative function and attention. To study the effect of Hcrt on excitatory PVT neurons that project to the mPFC, we used a new line of transgenic mice expressing green fluorescent protein (GFP) under the control of the vesicular glutamate-transporter-2 promoter. These neurons were retrogradely labeled with cholera toxin subunit B that had been microinjected into the mPFC. Membrane characteristics and responses to hypocretin-1 and -2 (Hcrt-1 and -2) were studied using whole cell recording (n > 300). PVT neurons showed distinct membrane properties including inward rectification, H-type potassium currents, low threshold spikes, and spike frequency adaptation. Cortically projecting neurons were depolarized and excited by Hcrt-2. Hcrt-2 actions were stronger than those of Hcrt-1, and the action persisted in TTX and in low calcium/high magnesium artificial cerebrospinal fluid, consistent with direct actions mediated by Hcrt receptor-2. Two mechanisms of Hcrt excitation were found: an increase in input resistance caused by closure of potassium channels and activation of nonselective cation channels. The robust excitation evoked by Hcrt-2 on cortically projecting glutamate PVT neurons could generate substantial excitation in multiple layers of the mPFC, adding to the more selective direct excitatory actions of Hcrt in the mPFC and potentially increasing cortical arousal and attention to limbic or visceral states.

Prestimulus Network Integration of Auditory Cortex Predisposes Near-Threshold Perception Independently of Local Excitability

PubMed Central

Leske, Sabine; Ruhnau, Philipp; Frey, Julia; Lithari, Chrysa; Müller, Nadia; Hartmann, Thomas; Weisz, Nathan

2015-01-01

An ever-increasing number of studies are pointing to the importance of network properties of the brain for understanding behavior such as conscious perception. However, with regards to the influence of prestimulus brain states on perception, this network perspective has rarely been taken. Our recent framework predicts that brain regions crucial for a conscious percept are coupled prior to stimulus arrival, forming pre-established pathways of information flow and influencing perceptual awareness. Using magnetoencephalography (MEG) and graph theoretical measures, we investigated auditory conscious perception in a near-threshold (NT) task and found strong support for this framework. Relevant auditory regions showed an increased prestimulus interhemispheric connectivity. The left auditory cortex was characterized by a hub-like behavior and an enhanced integration into the brain functional network prior to perceptual awareness. Right auditory regions were decoupled from non-auditory regions, presumably forming an integrated information processing unit with the left auditory cortex. In addition, we show for the first time for the auditory modality that local excitability, measured by decreased alpha power in the auditory cortex, increases prior to conscious percepts. Importantly, we were able to show that connectivity states seem to be largely independent from local excitability states in the context of a NT paradigm. PMID:26408799

Real time observation of the excimer formation dynamics of a gas phase benzene dimer by picosecond pump-probe spectroscopy.

PubMed

Miyazaki, Mitsuhiko; Fujii, Masaaki

2015-10-21

We observed the real-time excimer (EXC) formation dynamics of a gas phase benzene dimer (Bz2) cluster after photo-excitation to the S1 state by applying an ionization detected picosecond transient absorption method for probing the visible EXC absorption for the first time. The time evolution of the EXC absorption from the S1 0(0) level shows a rise that is well fitted by a single exponential function with a time constant of 18 ± 2 ps. The structure of the Bz dimer has a T-shaped structure in the ground electronic state, and that in the EXC state is a parallel sandwich (SW) structure. Thus, the observed rise time corresponds to the structural change from the T to the SW structures, which directly shows the EXC formation. On the other hand, the EXC formation after excitation of the S1 6(1) vibrational level of the stem site showed a faster rise of the time constant of 10 ± 2 ps. Supposing equilibrium between the EXC and the local excited states, it followed that the intramolecular vibrational energy redistribution rate of the 6(1) level is largely enhanced and becomes faster than the EXC formation reaction.

Multiphonon contribution to the polaron formation in cuprates with strong electron correlations and strong electron-phonon interaction

NASA Astrophysics Data System (ADS)

Ovchinnikov, Sergey G.; Makarov, Ilya A.; Kozlov, Peter A.

2017-03-01

In this work dependences of the electron band structure and spectral function in the HTSC cuprates on magnitude of electron-phonon interaction (EPI) and temperature are investigated. We use three-band p-d model with diagonal and offdiagonal EPI with breathing and buckling phonon mode in the frameworks of polaronic version of the generalized tight binding (GTB) method. The polaronic quasiparticle excitation in the system with EPI within this approach is formed by a hybridization of the local multiphonon Franck-Condon excitations with lower and upper Hubbard bands. Increasing EPI leads to transfer of spectral weight to high-energy multiphonon excitations and broadening of the spectral function. Temperature effects are taken into account by occupation numbers of local excited polaronic states and variations in the magnitude of spin-spin correlation functions. Increasing the temperature results in band structure reconstruction, spectral weight redistribution, broadening of the spectral function peak at the top of the valence band and the decreasing of the peak intensity. The effect of EPI with two phonon modes on the polaron spectral function is discussed.

Benchmarking singlet and triplet excitation energies of molecular semiconductors for singlet fission: Tuning the amount of HF exchange and adjusting local correlation to obtain accurate functionals for singlet-triplet gaps

NASA Astrophysics Data System (ADS)

Brückner, Charlotte; Engels, Bernd

2017-01-01

Vertical and adiabatic singlet and triplet excitation energies of molecular p-type semiconductors calculated with various DFT functionals and wave-function based approaches are benchmarked against MS-CASPT2/cc-pVTZ reference values. A special focus lies on the singlet-triplet gaps that are very important in the process of singlet fission. Singlet fission has the potential to boost device efficiencies of organic solar cells, but the scope of existing singlet-fission compounds is still limited. A computational prescreening of candidate molecules could enlarge it; yet it requires efficient methods accurately predicting singlet and triplet excitation energies. Different DFT formulations (Tamm-Dancoff approximation, linear response time-dependent DFT, Δ-SCF) and spin scaling schemes along with several ab initio methods (CC2, ADC(2)/MP2, CIS(D), CIS) are evaluated. While wave-function based methods yield rather reliable singlet-triplet gaps, many DFT functionals are shown to systematically underestimate triplet excitation energies. To gain insight, the impact of exact exchange and correlation is in detail addressed.

Molecular reorganization of selected quinoline derivatives in the ground and excited states—Investigations via static DFT

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

Błaziak, Kacper; Panek, Jarosław J.; Jezierska, Aneta, E-mail: aneta.jezierska@chem.uni.wroc.pl

2015-07-21

Quinoline derivatives are interesting objects to study internal reorganizations due to the observed excited-state-induced intramolecular proton transfer (ESIPT). Here, we report on computations for selected 12 quinoline derivatives possessing three kinds of intramolecular hydrogen bonds. Density functional theory was employed for the current investigations. The metric and electronic structure simulations were performed for the ground state and first excited singlet and triplet states. The computed potential energy profiles do not show a spontaneous proton transfer in the ground state, whereas excited states exhibit this phenomenon. Atoms in Molecules (AIM) theory was applied to study the nature of hydrogen bonding, whereasmore » Harmonic Oscillator Model of aromaticity index (HOMA) provided data of aromaticity evolution as a derivative of the bridge proton position. The AIM-based topological analysis confirmed the presence of the intramolecular hydrogen bonding. In addition, using the theory, we were able to provide a quantitative illustration of bonding transformation: from covalent to the hydrogen. On the basis of HOMA analysis, we showed that the aromaticity of both rings is dependent on the location of the bridge proton. Further, the computed results were compared with experimental data available. Finally, ESIPT occurrence was compared for the three investigated kinds of hydrogen bridges, and competition between two bridges in one molecule was studied.« less

Lithium-functionalized germanene: A promising media for CO2 capture

NASA Astrophysics Data System (ADS)

Mehdi Aghaei, S.; Monshi, M. M.; Torres, I.; Banakermani, M.; Calizo, I.

2018-02-01

Density functional theory (DFT) is employed to investigate the interactions of CO2 gas molecules with pristine and lithium-functionalized germanene. It is discovered that although a single CO2 molecule is weakly physisorbed on pristine germanene, a significant improvement on its adsorption energy is found by utilizing Li-functionalized germanene as the adsorbent. Excitingly, the moderate adsorption energy at high CO2 coverage secures an easy release step. Moreover, the structure of Li-functionalized germanene can be fully recovered after removal of CO2 gas molecules. Our results suggest that Li-functionalized germanene show promise for CO2 sensing and capture with a storage capacity of 12.57 mol/kg.

UV-Light Exposure of Insulin: Pharmaceutical Implications upon Covalent Insulin Dityrosine Dimerization and Disulphide Bond Photolysis

PubMed Central

Correia, Manuel; Neves-Petersen, Maria Teresa; Jeppesen, Per Bendix; Gregersen, Søren; Petersen, Steffen B.

2012-01-01

In this work we report the effects of continuous UV-light (276 nm, ∼2.20 W.m−2) excitation of human insulin on its absorption and fluorescence properties, structure and functionality. Continuous UV-excitation of the peptide hormone in solution leads to the progressive formation of tyrosine photo-product dityrosine, formed upon tyrosine radical cross-linkage. Absorbance, fluorescence emission and excitation data confirm dityrosine formation, leading to covalent insulin dimerization. Furthermore, UV-excitation of insulin induces disulphide bridge breakage. Near- and far-UV-CD spectroscopy shows that UV-excitation of insulin induces secondary and tertiary structure losses. In native insulin, the A and B chains are held together by two disulphide bridges. Disruption of either of these bonds is likely to affect insulin’s structure. The UV-light induced structural changes impair its antibody binding capability and in vitro hormonal function. After 1.5 and 3.5 h of 276 nm excitation there is a 33.7% and 62.1% decrease in concentration of insulin recognized by guinea pig anti-insulin antibodies, respectively. Glucose uptake by human skeletal muscle cells decreases 61.7% when the cells are incubated with pre UV-illuminated insulin during 1.5 h. The observations presented in this work highlight the importance of protecting insulin and other drugs from UV-light exposure, which is of outmost relevance to the pharmaceutical industry. Several drug formulations containing insulin in hexameric, dimeric and monomeric forms can be exposed to natural and artificial UV-light during their production, packaging, storage or administration phases. We can estimate that direct long-term exposure of insulin to sunlight and common light sources for indoors lighting and UV-sterilization in industries can be sufficient to induce irreversible changes to human insulin structure. Routine fluorescence and absorption measurements in laboratory experiments may also induce changes in protein structure. Structural damage includes insulin dimerization via dityrosine cross-linking or disulphide bond disruption, which affects the hormone’s structure and bioactivity. PMID:23227203

UV-light exposure of insulin: pharmaceutical implications upon covalent insulin dityrosine dimerization and disulphide bond photolysis.

PubMed

Correia, Manuel; Neves-Petersen, Maria Teresa; Jeppesen, Per Bendix; Gregersen, Søren; Petersen, Steffen B

2012-01-01

In this work we report the effects of continuous UV-light (276 nm, ~2.20 W.m(-2)) excitation of human insulin on its absorption and fluorescence properties, structure and functionality. Continuous UV-excitation of the peptide hormone in solution leads to the progressive formation of tyrosine photo-product dityrosine, formed upon tyrosine radical cross-linkage. Absorbance, fluorescence emission and excitation data confirm dityrosine formation, leading to covalent insulin dimerization. Furthermore, UV-excitation of insulin induces disulphide bridge breakage. Near- and far-UV-CD spectroscopy shows that UV-excitation of insulin induces secondary and tertiary structure losses. In native insulin, the A and B chains are held together by two disulphide bridges. Disruption of either of these bonds is likely to affect insulin's structure. The UV-light induced structural changes impair its antibody binding capability and in vitro hormonal function. After 1.5 and 3.5 h of 276 nm excitation there is a 33.7% and 62.1% decrease in concentration of insulin recognized by guinea pig anti-insulin antibodies, respectively. Glucose uptake by human skeletal muscle cells decreases 61.7% when the cells are incubated with pre UV-illuminated insulin during 1.5 h. The observations presented in this work highlight the importance of protecting insulin and other drugs from UV-light exposure, which is of outmost relevance to the pharmaceutical industry. Several drug formulations containing insulin in hexameric, dimeric and monomeric forms can be exposed to natural and artificial UV-light during their production, packaging, storage or administration phases. We can estimate that direct long-term exposure of insulin to sunlight and common light sources for indoors lighting and UV-sterilization in industries can be sufficient to induce irreversible changes to human insulin structure. Routine fluorescence and absorption measurements in laboratory experiments may also induce changes in protein structure. Structural damage includes insulin dimerization via dityrosine cross-linking or disulphide bond disruption, which affects the hormone's structure and bioactivity.

The vibrational excitation of hot molecules by low energy electron impact

NASA Astrophysics Data System (ADS)

Kato, H.; Ohkawa, M.; Hoshino, M.; Campbell, L.; Brunger, M. J.; Tanaka, H.

2010-01-01

We report vibrational excitation functions and angular distributions for electron scattering from the ground vibrational quantum (000), the bending vibrational quantum (010) and the unresolved first bending overtone (020) and symmetric stretch (100) modes of the ground-electronic state in hot (750 K) carbon dioxide (CO2) molecules. The excitation function measurements were carried out at incident electron energies in the range of 1-9 eV, and at the electron scattering angles of 30°, 60°, 90° and 120°.

Two-cluster structure of some alpha-scattering resonances in the sd shell

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

Budzanowski, A.; Grotowski, K.; Strzalkowski, A.

1975-01-01

The excitation functions of the elastic scattering of alpha particles at backward angles on $sup 24$Mg and $sup 28$Si nuclei in the energy range from 23 to 28 MeV measured by Bobrowska et al. exhibit distinct maxima. It was shown that these maxima are not correlated with the structures seen in the excitation functions of the ($alpha$,$alpha$') and ($alpha$,p) reactions leading to low- lying excited states of the final nucleus possibly indicating the presence of Ericson fluctuations. (auth)

Electronic structure of single crystalline Bi 2(Sr,Ca,La) 3Cu 2O 8

NASA Astrophysics Data System (ADS)

Lindberg, P. A. P.; Shen, Z.-X.; Dessau, D. S.; Wells, B. O.; Borg, A.; Mitzi, D. B.; Lindau, I.; Spicer, W. E.; Kapitulnik, A.

1989-12-01

Angle-resolved photoemission experiments on single crystals of Bi 2(Sr,Ca,La) 3Cu 2O 8 are reported. The data show a dispersionless behaviour of the valence band states as a function of the perpendicular component of the wave vector (along the c-axis), while as a function of the parallel component (in the a-b plane) clear dispersion occurs. Furthermore, polarization-dependent excitations reveal information on the symmetry of the unoccupied states.

Lifetimes of the Vibrational States of DNA Molecules in Functionalized Complexes of Semiconductor Quantum Dots

NASA Astrophysics Data System (ADS)

Bayramov, F. B.; Poloskin, E. D.; Chernev, A. L.; Toporov, V. V.; Dubina, M. V.; Sprung, C.; Lipsanen, H. K.; Bairamov, B. Kh.

2018-01-01

Results of studying nanocrystalline nc-Si/SiO2 quantum dots (QDs) functionalized by short oligonucleotides show that complexes of isolated crystalline semiconductor QDs are unique objects for detecting the manifestation of new quantum confinement phenomena. It is established that narrow lines observed in high-resolution spectra of inelastic light scattering can be used for determining the characteristic time scale of vibrational excitations of separate nucleotide molecules and for studying structural-dynamic properties of fast oscillatory processes in biomacromolecules.

Gravitational radiation during plunge - a Green's function approach

NASA Astrophysics Data System (ADS)

Nampalliwar, Sourabh; Price, Richard; Khanna, Gaurav

2015-04-01

During the merger of binary compact objects, an important stage is the plunge. A short part of the Gravitational waveform, it marks the end of early inspiral and determines the quasinormal ringing (QNR) of the final product of the merger. In this talk, we describe the approach of using the Fourier domain Green's function in the particle perturbation approximation to understand the excitation of QNR. We show that the resulting understanding is successful in explaining QNR in toy models and in the Schwarzschild background.

Remeasurement and compilation of excitation function of proton induced reactions on iron for activation techniques

NASA Astrophysics Data System (ADS)

Takács, S.; Vasváry, L.; Tárkányi, F.

1994-05-01

Excitation functions of proton induced reactions on natFe(p, xn) 56Co have been remeasured in the energy region up to 18 MeV using stacked foil technique and standard high resolution gamma-ray spectrometry at the Debrecen MGC-20E cyclotron. Compilation of the available data measured between 1959 and 1993 has been made. The corresponding excitation functions have been reviewed, critical comparison of all the available data was done to obtain the most accurate data set. The feasibility of the evaluated data set was checked by reproducing experimental calibration curves for TLA by calculation.

Molecular and Cellular Mechanisms for Trapping and Activating Emotional Memories

PubMed Central

Cai, Denise J.; Sano, Yoshitake; Lee, Yong-Seok; Zhou, Yu; Bekal, Pallavi; Deisseroth, Karl; Silva, Alcino J.

2016-01-01

Recent findings suggest that memory allocation to specific neurons (i.e., neuronal allocation) in the amygdala is not random, but rather the transcription factor cAMP-response element binding protein (CREB) modulates this process, perhaps by regulating the transcription of channels that control neuronal excitability. Here, optogenetic studies in the mouse lateral amygdala (LA) were used to demonstrate that CREB and neuronal excitability regulate which neurons encode an emotional memory. To test the role of CREB in memory allocation, we overexpressed CREB in the lateral amygdala to recruit the encoding of an auditory-fear conditioning (AFC) memory to a subset of neurons. Then, post-training activation of these neurons with Channelrhodopsin-2 was sufficient to trigger recall of the memory for AFC, suggesting that CREB regulates memory allocation. To test the role of neuronal excitability in memory allocation, we used a step function opsin (SFO) to transiently increase neuronal excitability in a subset of LA neurons during AFC. Post-training activation of these neurons with Volvox Channelrhodopsin-1 was able to trigger recall of that memory. Importantly, our studies show that activation of the SFO did not affect AFC by either increasing anxiety or by strengthening the unconditioned stimulus. Our findings strongly support the hypothesis that CREB regulates memory allocation by modulating neuronal excitability. PMID:27579481

Broadband spectroscopy of dynamic impedances with short chirp pulses.

PubMed

Min, M; Land, R; Paavle, T; Parve, T; Annus, P; Trebbels, D

2011-07-01

An impedance spectrum of dynamic systems is time dependent. Fast impedance changes take place, for example, in high throughput microfluidic devices and in operating cardiovascular systems. Measurements must be as short as possible to avoid significant impedance changes during the spectrum analysis, and as long as possible for enlarging the excitation energy and obtaining a better signal-to-noise ratio (SNR). The authors propose to use specific short chirp pulses for excitation. Thanks to the specific properties of the chirp function, it is possible to meet the needs for a spectrum bandwidth, measurement time and SNR so that the most accurate impedance spectrogram can be obtained. The chirp wave excitation can include thousands of cycles when the impedance changes slowly, but in the case of very high speed changes it can be shorter than a single cycle, preserving the same excitation bandwidth. For example, a 100 kHz bandwidth can be covered by the chirp pulse with durations from 10 µs to 1 s; only its excitation energy differs also 10(5) times. After discussing theoretical short chirp properties in detail, the authors show how to generate short chirps in the microsecond range with a bandwidth up to a few MHz by using digital synthesis architectures developed inside a low-cost standard field programmable gate array.

Magnetic and Electrical Characteristics of Permalloy Thin Tape Bobbin Cores

NASA Technical Reports Server (NTRS)

Schwarze, Gene E.; Wieserman, William R.; Niedra, Janis M.

2005-01-01

The core loss, that is, the power loss, of a soft ferromagnetic material is a function of the flux density, frequency, temperature, excitation type (voltage or current), excitation waveform (sine, square, etc.) and lamination or tape thickness. In previously published papers we have reported on the specific core loss and dynamic B-H loop results for several polycrystalline, nanocrystalline, and amorphous soft magnetic materials. In this previous research we investigated the effect of flux density, frequency, temperature, and excitation waveform for voltage excitation on the specific core loss and dynamic B-H loop. In this paper, we will report on an experimental study to investigate the effect of tape thicknesses of 1, 1/2, 1/4, and 1/8-mil Permalloy type magnetic materials on the specific core loss. The test cores were fabricated by winding the thin tapes on ceramic bobbin cores. The specific core loss tests were conducted at room temperature and over the frequency range of 10 kHz to 750 kHz using sine wave voltage excitation. The results of this experimental investigation will be presented primarily in graphical form to show the effect of tape thickness, frequency, and magnetic flux density on the specific core loss. Also, the experimental results when applied to power transformer design will be briefly discussed.

Modeling Excited States in TiO2 Nanoparticles: On the Accuracy of a TD-DFT Based Description

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

Berardo, Enrico; Hu, Hanshi; Shevlin, S. A.

2014-03-11

We have investigated the suitability of Time-Dependent Density Functional Theory (TD-DFT) to describe vertical low-energy excitations in naked and hydrated titanium dioxide nanoparticles through a comparison with results from Equation-of-Motion Coupled Cluster (EOM-CC) quantum chemistry methods. We demonstrate that for most TiO2 nanoparticles TD-DFT calculations with commonly used exchange-correlation (XC-)potentials (e.g. B3LYP) and EOM-CC methods give qualitatively similar results. Importantly, however, we also show that for an important subset of structures, TD-DFT gives qualitatively different results depending upon the XC-potential used and that in this case only TD-CAM-B3LYP and TD-BHLYP calculations yield results that are consistent with those obtained usingmore » EOM-CC theory. Moreover, we demonstrate that the discrepancies for such structures arise from a particular combination of defects, excitations involving which are charge-transfer excitations and hence are poorly described by XC-potentials that contain no or low fractions of Hartree-Fock like exchange. Finally, we discuss that such defects are readily healed in the presence of ubiquitously present water and that as a result the description of vertical low-energy excitations for hydrated TiO2 nanoparticles is hence non-problematic.« less

Energy transfer of highly vibrationally excited naphthalene: collisions with CHF3, CF4, and Kr.

PubMed

Chen Hsu, Hsu; Tsai, Ming-Tsang; Dyakov, Yuri A; Ni, Chi-Kung

2011-08-07

Energy transfer of highly vibrationally excited naphthalene in the triplet state in collisions with CHF(3), CF(4), and Kr was studied using a crossed-beam apparatus along with time-sliced velocity map ion imaging techniques. Highly vibrationally excited naphthalene (2.0 eV vibrational energy) was formed via the rapid intersystem crossing of naphthalene initially excited to the S(2) state by 266 nm photons. The shapes of the collisional energy-transfer probability density functions were measured directly from the scattering results of highly vibrationally excited naphthalene. In comparison to Kr atoms, the energy transfer in collisions between CHF(3) and naphthalene shows more forward scatterings, larger cross section for vibrational to translational (V → T) energy transfer, smaller cross section for translational to vibrational and rotational (T → VR) energy transfer, and more energy transferred from vibration to translation, especially in the range -ΔE(d) = -100 to -800 cm(-1). On the other hand, the difference of energy transfer properties between collisional partners Kr and CF(4) is small. The enhancement of the V → T energy transfer in collisions with CHF(3) is attributed to the large attractive interaction between naphthalene and CHF(3) (1-3 kcal/mol).

Alterations in gap junction connexin43/connexin45 ratio mediate a transition from quiescence to excitation in a mathematical model of the myometrium

PubMed Central

Sheldon, Rachel E.; Mashayamombe, Chipo; Shi, Shao-Qing; Garfield, Robert E.; Shmygol, Anatoly; Blanks, Andrew M.; van den Berg, Hugo A.

2014-01-01

The smooth muscle cells of the uterus contract in unison during delivery. These cells achieve coordinated activity via electrical connections called gap junctions which consist of aggregated connexin proteins such as connexin43 and connexin45. The density of gap junctions governs the excitability of the myometrium (among other factors). An increase in gap junction density occurs immediately prior to parturition. We extend a mathematical model of the myometrium by incorporating the voltage-dependence of gap junctions that has been demonstrated in the experimental literature. Two functional subtypes exist, corresponding to systems with predominantly connexin43 and predominantly connexin45, respectively. Our simulation results indicate that the gap junction protein connexin45 acts as a negative modulator of uterine excitability, and hence, activity. A network with a higher proportion of connexin45 relative to connexin43 is unable to excite every cell. Connexin45 has much more rapid gating kinetics than connexin43 which we show limits the maximum duration of a local burst of activity. We propose that this effect regulates the degree of synchronous excitation attained during a contraction. Our results support the hypothesis that as labour approaches, connexin45 is downregulated to allow action potentials to spread more readily through the myometrium. PMID:25401181

Magneto-acoustic imaging by continuous-wave excitation.

PubMed

Shunqi, Zhang; Zhou, Xiaoqing; Tao, Yin; Zhipeng, Liu

2017-04-01

The electrical characteristics of tissue yield valuable information for early diagnosis of pathological changes. Magneto-acoustic imaging is a functional approach for imaging of electrical conductivity. This study proposes a continuous-wave magneto-acoustic imaging method. A kHz-range continuous signal with an amplitude range of several volts is used to excite the magneto-acoustic signal and improve the signal-to-noise ratio. The magneto-acoustic signal amplitude and phase are measured to locate the acoustic source via lock-in technology. An optimisation algorithm incorporating nonlinear equations is used to reconstruct the magneto-acoustic source distribution based on the measured amplitude and phase at various frequencies. Validation simulations and experiments were performed in pork samples. The experimental and simulation results agreed well. While the excitation current was reduced to 10 mA, the acoustic signal magnitude increased up to 10 -7  Pa. Experimental reconstruction of the pork tissue showed that the image resolution reached mm levels when the excitation signal was in the kHz range. The signal-to-noise ratio of the detected magneto-acoustic signal was improved by more than 25 dB at 5 kHz when compared to classical 1 MHz pulse excitation. The results reported here will aid further research into magneto-acoustic generation mechanisms and internal tissue conductivity imaging.

3. INTERIOR OF POWERHOUSE BUILDING SHOWING EXCITER No. 2 (FOREGROUND), ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

3. INTERIOR OF POWERHOUSE BUILDING SHOWING EXCITER No. 2 (FOREGROUND), EXCITER No. 1, AND GENERATOR UNIT No. 2. BAYS FOR TRANSFORMERS No. 1 AND 2 ARE VISIBLE ALONG SIDE-WALL IN BACKGROUND. VIEW TO SOUTHWEST. - Kern County No. 1 Hydroelectric System, Powerhouse Exciters, Kern River Canyon, Bakersfield, Kern County, CA

Dynamics of hot rotating nuclei

NASA Astrophysics Data System (ADS)

Garcias, F.; de La Mota, V.; Remaud, B.; Royer, G.; Sébille, F.

1991-02-01

The deexcitation of hot rotating nuclei is studied within a microscopic semiclassical transport formalism. This framework allows the study of the competition between the fission and evaporation channels of deexcitation, including the mean-field and two-body interactions, without shape constraint for the fission channel. As a function of initial angular momenta and excitation energies, the transitions between three regimes is analyzed [particle evaporation, binary (ternary) fussion and multifragmentation], which correspond to well-defined symmetry breakings in the inertia tensor of the system. The competition between evaporation and binary fission is studied, showing the progressive disappearance of the fission process with increasing excitation energies, up to a critical point where nuclei pass directly from evaporation to multifragmentation channels.

Continuum theory of edge states of topological insulators: variational principle and boundary conditions.

PubMed

Medhi, Amal; Shenoy, Vijay B

2012-09-05

We develop a continuum theory to model low energy excitations of a generic four-band time reversal invariant electronic system with boundaries. We propose a variational energy functional for the wavefunctions which allows us to derive natural boundary conditions valid for such systems. Our formulation is particularly suited for developing a continuum theory of the protected edge/surface excitations of topological insulators both in two and three dimensions. By a detailed comparison of our analytical formulation with tight binding calculations of ribbons of topological insulators modelled by the Bernevig-Hughes-Zhang (BHZ) Hamiltonian, we show that the continuum theory with a natural boundary condition provides an appropriate description of the low energy physics.

Coupled-mode theory and Fano resonances in guided-mode resonant gratings: the conical diffraction mounting.

PubMed

Bykov, Dmitry A; Doskolovich, Leonid L; Soifer, Victor A

2017-01-23

We study resonances of guided-mode resonant gratings in conical mounting. By developing 2D time-dependent coupled-mode theory we obtain simple approximations of the transmission and reflection coefficients. Being functions of the incident light's frequency and in-plane wave vector components, the obtained approximations can be considered as multi-variable generalizations of the Fano line shape. We show that the approximations are in good agreement with the rigorously calculated transmission and reflection spectra. We use the developed theory to investigate angular tolerances of the considered structures and to obtain mode excitation conditions. In particular, we obtain the cross-polarization mode excitation conditions in the case of conical mounting.

Fast and accurate image recognition algorithms for fresh produce food safety sensing

NASA Astrophysics Data System (ADS)

Yang, Chun-Chieh; Kim, Moon S.; Chao, Kuanglin; Kang, Sukwon; Lefcourt, Alan M.

2011-06-01

This research developed and evaluated the multispectral algorithms derived from hyperspectral line-scan fluorescence imaging under violet LED excitation for detection of fecal contamination on Golden Delicious apples. The algorithms utilized the fluorescence intensities at four wavebands, 680 nm, 684 nm, 720 nm, and 780 nm, for computation of simple functions for effective detection of contamination spots created on the apple surfaces using four concentrations of aqueous fecal dilutions. The algorithms detected more than 99% of the fecal spots. The effective detection of feces showed that a simple multispectral fluorescence imaging algorithm based on violet LED excitation may be appropriate to detect fecal contamination on fast-speed apple processing lines.

Coulomb energy differences in isobaric multiplets

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

Lenzi, S. M.; Farnea, E.; Bazzacco, D.

2007-02-12

By comparing the excitation energies of analogue states in isobaric multiplets, several nuclear structure properties can be studied as a function of the angular momentum up to high spin states. In particular, the mirror nuclei 35Ar and 35Cl show large differences between the excitation energies of analogue negative-parity states at high spin, confirming the important contribution of the relativistic electromagnetic spin-orbit interaction to the Coulomb energy. The single-particle character of the configuration of these states is reproduced with very good accuracy by shell model calculations in the sd and pf shells valence space. In addition, evidence of isospin mixing ismore » deduced from the El transitions linking positive and negative parity states.« less

Excitation of the Earth's Chandler wobble by a turbulent oceanic double-gyre

NASA Astrophysics Data System (ADS)

Naghibi, S. E.; Jalali, M. A.; Karabasov, S. A.; Alam, M.-R.

2017-04-01

We develop a layer-averaged, multiple-scale spectral ocean model and show how an oceanic double-gyre can communicate with the Earth's Chandler wobble. The overall transfers of energy and angular momentum from the double-gyre to the Chandler wobble are used to calibrate the turbulence parameters of the layer-averaged model. Our model is tested against a multilayer quasi-geostrophic ocean model in turbulent regime, and base states used in parameter identification are obtained from mesoscale eddy resolving numerical simulations. The Chandler wobble excitation function obtained from the model predicts a small role of North Atlantic ocean region on the wobble dynamics as compared to all oceans, in agreement with the existing observations.

The Raman and SERS spectra of indigo and indigo-Ag2 complex: DFT calculation and comparison with experiment.

PubMed

Ricci, Marilena; Lofrumento, Cristiana; Becucci, Maurizio; Castellucci, Emilio M

2018-01-05

Using time-dependent density functional theory in conjunction with B3LYP functional and LANL2DZ/6-31+g(d,p) basis sets, static and pre-resonance Raman spectra of the indigo-Ag 2 complex have been calculated. Structure optimization, excitation energies and pre-resonance Raman spectra of the indigo molecule have been obtained at the same level of theory. The available experimental Raman spectra at 1064, 785 and 514nm and the SERS spectra at 785 and 514nm have been well reproduced by the calculation. Experimental SERS spectra are confronted with the calculated pre-resonance Raman spectra obtained for the indigo-Ag 2 complex. The Raman activities calculated under the infinite lifetime approximation show a strong dependence upon the proximity to the energy and the oscillator strength of the excitation electronic transition. The comparison of the integrated EFs for indigo and indigo-Ag 2 calculated Raman spectra, gave some hints as to the enhancement mechanisms acting for the different excitation wavelengths. Whereas for excitation at a wavelength corresponding to 785nm, the enhancement mechanism for the Raman spectrum of the metal complex seems the chemical one, the strong increment (ten times) of the integrated EF of the Raman spectra of the complex in the case of 514nm excitation, suggests the onset of other enhancement mechanisms. Assuming that intra-cluster transitions with high oscillator strength can be thought of as to mimic surface plasmons excitations, we suggest the onset of the electromagnetic mechanisms (EM) as the origin of the Raman spectrum enhancement. Nevertheless, other enhancement effects cannot be ruled out, as a new molecular transition gains strength in the proximity of the excitation wavelength, as a consequence of the symmetry lowering of the molecule in the complex. A large variation across vibrational modes, by a factor of at least 10 4 , was found for the EFs. This large variation in the EFs can indicate that B-term Herzberg-Teller scattering, due to metal and/or charge transfer states, can feed intensity to the inactive (in the molecule) and/or non totally symmetric modes. Copyright © 2017 Elsevier B.V. All rights reserved.

The Raman and SERS spectra of indigo and indigo-Ag2 complex: DFT calculation and comparison with experiment

NASA Astrophysics Data System (ADS)

Ricci, Marilena; Lofrumento, Cristiana; Becucci, Maurizio; Castellucci, Emilio M.

2018-01-01

Using time-dependent density functional theory in conjunction with B3LYP functional and LANL2DZ/6-31+g(d,p) basis sets, static and pre-resonance Raman spectra of the indigo-Ag2 complex have been calculated. Structure optimization, excitation energies and pre-resonance Raman spectra of the indigo molecule have been obtained at the same level of theory. The available experimental Raman spectra at 1064, 785 and 514 nm and the SERS spectra at 785 and 514 nm have been well reproduced by the calculation. Experimental SERS spectra are confronted with the calculated pre-resonance Raman spectra obtained for the indigo-Ag2 complex. The Raman activities calculated under the infinite lifetime approximation show a strong dependence upon the proximity to the energy and the oscillator strength of the excitation electronic transition. The comparison of the integrated EFs for indigo and indigo-Ag2 calculated Raman spectra, gave some hints as to the enhancement mechanisms acting for the different excitation wavelengths. Whereas for excitation at a wavelength corresponding to 785 nm, the enhancement mechanism for the Raman spectrum of the metal complex seems the chemical one, the strong increment (ten times) of the integrated EF of the Raman spectra of the complex in the case of 514 nm excitation, suggests the onset of other enhancement mechanisms. Assuming that intra-cluster transitions with high oscillator strength can be thought of as to mimic surface plasmons excitations, we suggest the onset of the electromagnetic mechanisms (EM) as the origin of the Raman spectrum enhancement. Nevertheless, other enhancement effects cannot be ruled out, as a new molecular transition gains strength in the proximity of the excitation wavelength, as a consequence of the symmetry lowering of the molecule in the complex. A large variation across vibrational modes, by a factor of at least 104, was found for the EFs. This large variation in the EFs can indicate that B-term Herzberg-Teller scattering, due to metal and/or charge transfer states, can feed intensity to the inactive (in the molecule) and/or non totally symmetric modes.

Interhemispheric modulation of dual-mode, noninvasive brain stimulation on motor function.

PubMed

Park, Eunhee; Kim, Yun-Hee; Chang, Won Hyuk; Kwon, Tae Gun; Shin, Yong-Il

2014-06-01

To investigate the effects of simultaneous, bihemispheric, dual-mode stimulation using repetitive transcranial magnetic stimulation (rTMS) and transcranial direct current stimulation (tDCS) on motor functions and cortical excitability in healthy individuals. Twenty-five healthy, right-handed volunteers (10 men, 15 women; mean age, 25.5 years) were enrolled. All participants received four randomly arranged, dual-mode, simultaneous stimulations under the following conditions: condition 1, high-frequency rTMS over the right primary motor cortex (M1) and sham tDCS over the left M1; condition 2, high-frequency rTMS over the right M1 and anodal tDCS over the left M1; condition 3, high-frequency rTMS over the right M1 and cathodal tDCS over the left M1; and condition 4, sham rTMS and sham tDCS. The cortical excitability of the right M1 and motor functions of the left hand were assessed before and after each simulation. Motor evoked potential (MEP) amplitudes after stimulation were significantly higher than before stimulation, under the conditions 1 and 2. The MEP amplitude in condition 2 was higher than both conditions 3 and 4, while the MEP amplitude in condition 1 was higher than condition 4. The results of the Purdue Pegboard test and the box and block test showed significant improvement in conditions 1 and 2 after stimulation. Simultaneous stimulation by anodal tDCS over the left M1 with high-frequency rTMS over the right M1 could produce interhemispheric modulation and homeostatic plasticity, which resulted in modulation of cortical excitability and motor functions.

5. POWERHOUSE INTERIOR SHOWING EXCITER No. 1. SMALL PELTONDOBLE IMPULSE ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

5. POWERHOUSE INTERIOR SHOWING EXCITER No. 1. SMALL PELTON-DOBLE IMPULSE WHEEL IN FOREGROUND. VIEW TO NORTHWEST. - Rush Creek Hydroelectric System, Powerhouse Exciters, Rush Creek, June Lake, Mono County, CA

Loss of MeCP2 From Forebrain Excitatory Neurons Leads to Cortical Hyperexcitation and Seizures

PubMed Central

Zhang, Wen; Peterson, Matthew; Beyer, Barbara; Frankel, Wayne N.

2014-01-01

Mutations of MECP2 cause Rett syndrome (RTT), a neurodevelopmental disorder leading to loss of motor and cognitive functions, impaired social interactions, and seizure at young ages. Defects of neuronal circuit development and function are thought to be responsible for the symptoms of RTT. The majority of RTT patients show recurrent seizures, indicating that neuronal hyperexcitation is a common feature of RTT. However, mechanisms underlying hyperexcitation in RTT are poorly understood. Here we show that deletion of Mecp2 from cortical excitatory neurons but not forebrain inhibitory neurons in the mouse leads to spontaneous seizures. Selective deletion of Mecp2 from excitatory but not inhibitory neurons in the forebrain reduces GABAergic transmission in layer 5 pyramidal neurons in the prefrontal and somatosensory cortices. Loss of MeCP2 from cortical excitatory neurons reduces the number of GABAergic synapses in the cortex, and enhances the excitability of layer 5 pyramidal neurons. Using single-cell deletion of Mecp2 in layer 2/3 pyramidal neurons, we show that GABAergic transmission is reduced in neurons without MeCP2, but is normal in neighboring neurons with MeCP2. Together, these results suggest that MeCP2 in cortical excitatory neurons plays a critical role in the regulation of GABAergic transmission and cortical excitability. PMID:24523563

Orthodontic treatment-induced temporal alteration of jaw-opening reflex excitability.

PubMed

Sasaki, Au; Hasegawa, Naoya; Adachi, Kazunori; Sakagami, Hiroshi; Suda, Naoto

2017-10-01

The impairment of orofacial motor function during orthodontic treatment needs to be addressed, because most orthodontic patients experience pain and motor excitability would be affected by pain. In the present study, the temporal alteration of the jaw-opening reflex excitability was investigated to determine if orthodontic treatment affects orofacial motor function. The excitability of jaw-opening reflex evoked by electrical stimulation on the gingiva and recorded bilaterally in the anterior digastric muscles was evaluated at 1 (D1), 3 (D3), and 7 days (D7) after orthodontic force application to the teeth of right side; morphological features (e.g., osteoclast genesis and tooth movement) were also evaluated. To clarify the underlying mechanism of orthodontic treatment-induced alteration of orofacial motor excitability, analgesics were administrated for 1 day. At D1 and D3, orthodontic treatment significantly decreased the threshold for inducing the jaw-opening reflex but significantly increased the threshold at D7. Other parameters of the jaw-opening reflex were also evaluated (e.g., latency, duration and area under the curve of anterior digastric muscles activity), and only the latency of the D1 group was significantly different from that of the other groups. Temporal alteration of the jaw-opening reflex excitability was significantly correlated with changes in morphological features. Aspirin (300 mg·kg -1 ·day -1 ) significantly increased the threshold for inducing the jaw-opening reflex, whereas a lower dose (75-150 mg·kg -1 ·day -1 ) of aspirin or acetaminophen (300 mg·kg -1 ·day -1 ) failed to alter the jaw-opening reflex excitability. These results suggest that an increase of the jaw-opening reflex excitability can be induced acutely by orthodontic treatment, possibly through the cyclooxygenase activation. NEW & NOTEWORTHY It is well known that motor function is affected by pain, but the effect of orthodontic treatment-related pain on the trigeminal motor excitability has not been fully understood. We found that, during orthodontic treatment, trigeminal motor excitability is acutely increased and then decreased in a week. Because alteration of trigeminal motor function can be evaluated quantitatively by jaw-opening reflex excitability, the present animal model may be useful to search for alternative approaches to attenuate orthodontic pain. Copyright © 2017 the American Physiological Society.

Engineering biosynthetic excitable tissues from unexcitable cells for electrophysiological and cell therapy studies.

PubMed

Kirkton, Robert D; Bursac, Nenad

2011-01-01

Patch-clamp recordings in single-cell expression systems have been traditionally used to study the function of ion channels. However, this experimental setting does not enable assessment of tissue-level function such as action potential (AP) conduction. Here we introduce a biosynthetic system that permits studies of both channel activity in single cells and electrical conduction in multicellular networks. We convert unexcitable somatic cells into an autonomous source of electrically excitable and conducting cells by stably expressing only three membrane channels. The specific roles that these expressed channels have on AP shape and conduction are revealed by different pharmacological and pacing protocols. Furthermore, we demonstrate that biosynthetic excitable cells and tissues can repair large conduction defects within primary 2- and 3-dimensional cardiac cell cultures. This approach enables novel studies of ion channel function in a reproducible tissue-level setting and may stimulate the development of new cell-based therapies for excitable tissue repair.

A chloroplast "wake up" mechanism: Illumination with weak light activates the photosynthetic antenna function in dark-adapted plants.

PubMed

Janik, Ewa; Bednarska, Joanna; Zubik, Monika; Luchowski, Rafal; Mazur, Radoslaw; Sowinski, Karol; Grudzinski, Wojciech; Garstka, Maciej; Gruszecki, Wieslaw I

2017-03-01

The efficient and fluent operation of photosynthesis in plants relies on activity of pigment-protein complexes called antenna, absorbing light and transferring excitations toward the reaction centers. Here we show, based on the results of the fluorescence lifetime imaging analyses of single chloroplasts, that pigment-protein complexes, in dark-adapted plants, are not able to act effectively as photosynthetic antennas, due to pronounced, adverse excitation quenching. It appeared that the antenna function could be activated by a short (on a minute timescale) illumination with light of relatively low intensity, substantially below the photosynthesis saturation threshold. The low-light-induced activation of the antenna function was attributed to phosphorylation of the major accessory light-harvesting complex LHCII, based on the fact that such a mechanism was not observed in the stn7 Arabidopsis thaliana mutant, with impaired LHCII phosphorylation. It is proposed that the protein phosphorylation-controlled change in the LHCII clustering ability provides mechanistic background for this regulatory process. Copyright © 2016 Elsevier GmbH. All rights reserved.

SrMoO4:Er3+-Yb3+ upconverting phosphor for photonic and forensic applications

NASA Astrophysics Data System (ADS)

Soni, Abhishek Kumar; Rai, Vineet Kumar

2016-08-01

The Er3+-Yb3+ codoped strontium molybdate (SrMoO4) phosphors have been synthesized via chemical co-precipitation method by adding ammonium hydroxide as a base reagent. The phase, crystal structure and formation of spindle-like particles present in the prepared phosphors have been recognized by using the X-ray powder diffraction (XRPD) and Field emission scanning electron microscopy (FE-SEM) techniques. The Fourier transform infrared (FTIR) spectroscopy of the developed phosphors has been analyzed to mark the different functional groups present in synthesized phosphors. The multicolour upconversion emissions observed upon excitation with 980 nm and 808 nm laser diode have been explained on the basis of dopants ions concentration, pump power dependence, energy level structure and decay curve analysis. The colour co-ordinate study confirmed that the codoped phosphor emits non-tunable green colour when excited with the 980 nm laser diode, whereas it shows the colour tunability from yellow to green region upon excitation with the 808 nm laser diode. The applicability of non-tunable green colour emission has been demonstrated in the security ink and latent finger print detection. This shows the utility of the developed phosphors in the photonic and forensic applications.

Intrinsic Gilbert Damping in Metallic Ferromagnets in Ballistic Regime and the Effect of Inelastic Electron Scattering from Magnetic Moments: A Time Dependent Keldysh Green Function Approach

NASA Astrophysics Data System (ADS)

Mahfouzi, Farzad; Kioussis, Nicholas

Gilbert damping in metallic ferromagnets is mainly governed by the exchange coupling between the electrons and the magnetic degree of freedom, where the time dependent evolution of the magnetization leads to the excitation of electrons and loss of energy as a result of flow of spin and charge currents. However, it turns out that when the magnetization evolves slowly in time, in the presence of spin-orbit interaction (SOI), the resonant electronic excitations has a major contribution to the damping which leads to infinite result in ballistic regime. In this work we consider the inelastic spin-flip scattering of electrons from the magnetic moments and show that in the presence of SOI it leads to the relaxation of the excited electrons. We show that in the case of clean crystal systems such scattering leads to a linear dependence of the Gilbert on the SOI strength and in the limit of diffusive systems we get the Gilbert damping expression obtained from Kambersky's Fermi breathing approach. This research was supported by NSF-PREM Grant No. DMR-1205734

Time-dependent Gutzwiller theory of magnetic excitations in the Hubbard model

NASA Astrophysics Data System (ADS)

Seibold, G.; Becca, F.; Rubin, P.; Lorenzana, J.

2004-04-01

We use a spin-rotational invariant Gutzwiller energy functional to compute random-phase-approximation-like (RPA) fluctuations on top of the Gutzwiller approximation (GA). The method can be viewed as an extension of the previously developed GA+RPA approach for the charge sector [G. Seibold and J. Lorenzana, Phys. Rev. Lett. 86, 2605 (2001)] with respect to the inclusion of the magnetic excitations. Unlike the charge case, no assumptions about the time evolution of the double occupancy are needed in this case. Interestingly, in a spin-rotational invariant system, we find the correct degeneracy between triplet excitations, showing the consistency of both computations. Since no restrictions are imposed on the symmetry of the underlying saddle-point solution, our approach is suitable for the evaluation of the magnetic susceptibility and dynamical structure factor in strongly correlated inhomogeneous systems. We present a detailed study of the quality of our approach by comparing with exact diagonalization results and show its much higher accuracy compared to the conventional Hartree-Fock+RPA theory. In infinite dimensions, where the GA becomes exact for the Gutzwiller variational energy, we evaluate ferromagnetic and antiferromagnetic instabilities from the transverse magnetic susceptibility. The resulting phase diagram is in complete agreement with previous variational computations.

Distinguishing between relaxation pathways by combining dissociative ionization pump probe spectroscopy and ab initio calculations: a case study of cytosine.

PubMed

Kotur, Marija; Weinacht, Thomas C; Zhou, Congyi; Kistler, Kurt A; Matsika, Spiridoula

2011-05-14

We present a general method for tracking molecular relaxation along different pathways from an excited state down to the ground state. We follow the excited state dynamics of cytosine pumped near the S(0)-S(1) resonance using ultrafast laser pulses in the deep ultraviolet and probed with strong field near infrared pulses which ionize and dissociate the molecules. The fragment ions are detected via time of flight mass spectroscopy as a function of pump probe delay and probe pulse intensity. Our measurements reveal that different molecular fragments show different timescales, indicating that there are multiple relaxation pathways down to the ground state. We interpret our measurements with the help of ab initio electronic structure calculations of both the neutral molecule and the molecular cation for different conformations en route to relaxation back down to the ground state. Our measurements and calculations show passage through two seams of conical intersections between ground and excited states and demonstrate the ability of dissociative ionization pump probe measurements in conjunction with ab initio electronic structure calculations to track molecular relaxation through multiple pathways.

2. INTERIOR OF POWERHOUSE BUILDING SHOWING EXCITER No. 1 (FOREGROUND), ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

2. INTERIOR OF POWERHOUSE BUILDING SHOWING EXCITER No. 1 (FOREGROUND), EXCITER No 2, AND GENERATOR UNIT No. 3. BAYS FOR TRANSFORMERS No. 3 AND 4 ARE VISIBLE ALONG SIDE-WALL IN BACKGROUND. STAIRS LEAD TO OFFICE. VIEW TO SOUTHEAST. - Kern County No. 1 Hydroelectric System, Powerhouse Exciters, Kern River Canyon, Bakersfield, Kern County, CA

UV absorption in metal decorated boron nitride flakes: a theoretical analysis of excited states

NASA Astrophysics Data System (ADS)

Chopra, Siddheshwar; Plasser, Felix

2017-10-01

The excited states of single metal atom (X = Co, Al and Cu) doped boron nitride flake (MBNF) B15N14H14-X and pristine boron nitride (B15N15H14) are studied by time-dependent density functional theory. The immediate effect of metal doping is a red shift of the onset of absorption from about 220 nm for pristine BNF to above 300 nm for all metal-doped variants with the biggest effect for MBNF-Co, which shows appreciable intensity even above 400 nm. These energy shifts are analysed by detailed wavefunction analysis protocols using visualisation methods, such as the natural transition orbital analysis and electron-hole correlation plots, as well as quantitative analysis of the exciton size and electron-hole populations. The analysis shows that the Co and Cu atoms provide strong contributions to the relevant states whereas the aluminium atom is only involved to a lesser extent.

Prenatal choline availability alters the context sensitivity of Pavlovian conditioning in adult rats

PubMed Central

Lamoureux, Jeffrey A.; Meck, Warren H.; Williams, Christina L.

2008-01-01

The effects of prenatal choline availability on Pavlovian conditioning were assessed in adult male rats (3–4 mo). Neither supplementation nor deprivation of prenatal choline affected the acquisition and extinction of simple Pavlovian conditioned excitation, or the acquisition and retardation of conditioned inhibition. However, prenatal choline availability significantly altered the contextual control of these learned behaviors. Both control and choline-deprived rats exhibited context specificity of conditioned excitation as exhibited by a loss in responding when tested in an alternate context after conditioning; in contrast, choline-supplemented rats showed no such effect. When switched to a different context following extinction, however, both choline-supplemented and control rats showed substantial contextual control of responding, whereas choline-deficient rats did not. These data support the view that configural associations that rely on hippocampal function are selectively sensitive to prenatal manipulations of dietary choline during prenatal development. PMID:19050158

Pet-1 Switches Transcriptional Targets Postnatally to Regulate Maturation of Serotonin Neuron Excitability.

PubMed

Wyler, Steven C; Spencer, W Clay; Green, Noah H; Rood, Benjamin D; Crawford, LaTasha; Craige, Caryne; Gresch, Paul; McMahon, Douglas G; Beck, Sheryl G; Deneris, Evan

2016-02-03

Newborn neurons enter an extended maturation stage, during which they acquire excitability characteristics crucial for development of presynaptic and postsynaptic connectivity. In contrast to earlier specification programs, little is known about the regulatory mechanisms that control neuronal maturation. The Pet-1 ETS (E26 transformation-specific) factor is continuously expressed in serotonin (5-HT) neurons and initially acts in postmitotic precursors to control acquisition of 5-HT transmitter identity. Using a combination of RNA sequencing, electrophysiology, and conditional targeting approaches, we determined gene expression patterns in maturing flow-sorted 5-HT neurons and the temporal requirements for Pet-1 in shaping these patterns for functional maturation of mouse 5-HT neurons. We report a profound disruption of postmitotic expression trajectories in Pet-1(-/-) neurons, which prevented postnatal maturation of 5-HT neuron passive and active intrinsic membrane properties, G-protein signaling, and synaptic responses to glutamatergic, lysophosphatidic, and adrenergic agonists. Unexpectedly, conditional targeting revealed a postnatal stage-specific switch in Pet-1 targets from 5-HT synthesis genes to transmitter receptor genes required for afferent modulation of 5-HT neuron excitability. Five-HT1a autoreceptor expression depended transiently on Pet-1, thus revealing an early postnatal sensitive period for control of 5-HT excitability genes. Chromatin immunoprecipitation followed by sequencing revealed that Pet-1 regulates 5-HT neuron maturation through direct gene activation and repression. Moreover, Pet-1 directly regulates the 5-HT neuron maturation factor Engrailed 1, which suggests Pet-1 orchestrates maturation through secondary postmitotic regulatory factors. The early postnatal switch in Pet-1 targets uncovers a distinct neonatal stage-specific function for Pet-1, during which it promotes maturation of 5-HT neuron excitability. The regulatory mechanisms that control functional maturation of neurons are poorly understood. We show that in addition to inducing brain serotonin (5-HT) synthesis and reuptake, the Pet-1 ETS (E26 transformation-specific) factor subsequently globally coordinates postmitotic expression trajectories of genes necessary for maturation of 5-HT neuron excitability. Further, Pet-1 switches its transcriptional targets as 5-HT neurons mature from 5-HT synthesis genes to G-protein-coupled receptors, which are necessary for afferent synaptic modulation of 5-HT neuron excitability. Our findings uncover gene-specific switching of downstream targets as a previously unrecognized regulatory strategy through which continuously expressed transcription factors control acquisition of neuronal identity at different stages of development. Copyright © 2016 the authors 0270-6474/16/361758-17$15.00/0.

Effects of acamprosate on attentional set-shifting and cellular function in the prefrontal cortex of chronic alcohol-exposed mice

NASA Astrophysics Data System (ADS)

Hu, Wei

Background: The medial prefrontal cortex (mPFC) inhibits impulsive and compulsive behaviors that characterize drug abuse and dependence. Acamprosate is the leading medication approved for the maintenance of abstinence, shown to reduce craving and relapse in animal models and human alcoholics. Whether acamprosate can modulate executive functions that are impaired by chronic ethanol exposure is unknown. Here we explored the effects of acamprosate on an attentional set-shifting task, and tested whether these behavioral effects are correlated with modulation of glutamatergic synaptic transmission and intrinsic excitability of mPFC neurons. Methods: We induced alcohol dependence in mice via chronic intermittent ethanol (CIE) exposure in vapor chambers and measured changes in alcohol consumption in a limited access 2-bottle choice paradigm. Impairments of executive function were assessed in an attentional set-shifting task. Acamprosate was applied subchronically for 2 days during withdrawal before the final behavioral test. Alcohol-induced changes in cellular function of layer 5/6 pyramidal neurons, and the potential modulation of these changes by acamprosate, were measured using patch clamp recordings in brain slices. Results: Chronic ethanol exposure impaired cognitive flexibility in the attentional set-shifting task. Acamprosate improved overall performance and reduced perseveration. Recordings of mPFC neurons showed that chronic ethanol exposure increased use-dependent presynaptic transmitter release and enhanced postsynaptic N-methyl-D-aspartate receptor (NMDAR) function. Moreover, CIE-treatment lowered input resistance, and decreased the threshold and the afterhyperpolarization (AHP) of action potentials, suggesting chronic ethanol exposure also impacted membrane excitability of mPFC neurons. However, acamprosate treatment did not reverse these ethanol-induced changes cellular function. Conclusion: Acamprosate improved attentional control of ethanol exposed animals, but did not alter the concurrent changes in synaptic transmission or membrane excitability of mPFC neurons, indicating that these changes are not the pharmacological targets of acamprosate in the recovery of mPFC functions affected by chronic ethanol exposure.

Domiciliary VR-Based Therapy for Functional Recovery and Cortical Reorganization: Randomized Controlled Trial in Participants at the Chronic Stage Post Stroke.

PubMed

Ballester, Belén Rubio; Nirme, Jens; Camacho, Irene; Duarte, Esther; Rodríguez, Susana; Cuxart, Ampar; Duff, Armin; Verschure, Paul F M J

2017-08-07

Most stroke survivors continue to experience motor impairments even after hospital discharge. Virtual reality-based techniques have shown potential for rehabilitative training of these motor impairments. Here we assess the impact of at-home VR-based motor training on functional motor recovery, corticospinal excitability and cortical reorganization. The aim of this study was to identify the effects of home-based VR-based motor rehabilitation on (1) cortical reorganization, (2) corticospinal tract, and (3) functional recovery after stroke in comparison to home-based occupational therapy. We conducted a parallel-group, controlled trial to compare the effectiveness of domiciliary VR-based therapy with occupational therapy in inducing motor recovery of the upper extremities. A total of 35 participants with chronic stroke underwent 3 weeks of home-based treatment. A group of subjects was trained using a VR-based system for motor rehabilitation, while the control group followed a conventional therapy. Motor function was evaluated at baseline, after the intervention, and at 12-weeks follow-up. In a subgroup of subjects, we used Navigated Brain Stimulation (NBS) procedures to measure the effect of the interventions on corticospinal excitability and cortical reorganization. Results from the system's recordings and clinical evaluation showed significantly greater functional recovery for the experimental group when compared with the control group (1.53, SD 2.4 in Chedoke Arm and Hand Activity Inventory). However, functional improvements did not reach clinical significance. After the therapy, physiological measures obtained from a subgroup of subjects revealed an increased corticospinal excitability for distal muscles driven by the pathological hemisphere, that is, abductor pollicis brevis. We also observed a displacement of the centroid of the cortical map for each tested muscle in the damaged hemisphere, which strongly correlated with improvements in clinical scales. These findings suggest that, in chronic stages, remote delivery of customized VR-based motor training promotes functional gains that are accompanied by neuroplastic changes. International Standard Randomized Controlled Trial Number NCT02699398 (Archived by ClinicalTrials.gov at https://clinicaltrials.gov/ct2/show/NCT02699398?term=NCT02699398&rank=1). ©Belén Rubio Ballester, Jens Nirme, Irene Camacho, Esther Duarte, Susana Rodríguez, Ampar Cuxart, Armin Duff, Paul F.M.J. Verschure. Originally published in JMIR Serious Games (http://games.jmir.org), 07.08.2017.

Atomic, Molecular, and Optical Physics: Optical Excitation Function of H(1s-2p) Produced by electron Impact from Threshold to 1.8 keV

NASA Technical Reports Server (NTRS)

James, G. K.; Slevin, J. A.; Shemansky, D. E.; McConkey, J. W.; Bray, I.; Dziczek, D.; Kanik, I.; Ajello, J. M.

1997-01-01

The optical excitation function of prompt Lyman-Alpha radiation, produced by electron impact on atomic hydrogen, has been measured over the extended energy range from threshold to 1.8 keV. Measurements were obtained in a crossed-beams experiment using both magnetically confined and electrostatically focused electrons in collision with atomic hydrogen produced by an intense discharge source. A vacuum-ultraviolet mono- chromator system was used to measure the emitted Lyman-Alpha radiation. The absolute H(1s-2p) electron impact excitation cross section was obtained from the experimental optical excitation function by normalizing to the accepted optical oscillator strength, with corrections for polarization and cascade. Statistical and known systematic uncertainties in our data range from +/- 4% near threshold to +/- 2% at 1.8 keV. Multistate coupling affecting the shape of the excitation function up to 1 keV impact energy is apparent in both the present experimental data and present theoretical results obtained with convergent close- coupling (CCC) theory. This shape function effect leads to an uncertainty in absolute cross sections at the 10% level in the analysis of the experimental data. The derived optimized absolute cross sections are within 7% of the CCC calculations over the 14 eV-1.8 keV range. The present CCC calculations converge on the Bethe- Fano profile for H(1s-2p) excitation at high energy. For this reason agreement with the CCC values to within 3% is achieved in a nonoptimal normalization of the experimental data to the Bethe-Fano profile. The fundamental H(1s-2p) electron impact cross section is thereby determined to an unprecedented accuracy over the 14 eV - 1.8 keV energy range.

Mechanism of orientation of stimulating currents in magnetic brain stimulation (abstract)

NASA Astrophysics Data System (ADS)

Ueno, S.; Matsuda, T.

1991-04-01

We made a functional map of the human motor cortex related to the hand and foot areas by stimulating the human brain with a focused magnetic pulse. We observed that each functional area in the cortex has an optimum direction for which stimulating currents can produce neural excitation. The present report focuses on the mechanism which is responsible for producing this anisotropic response to brain stimulation. We first obtained a functional map of the brain related to the left ADM (abductor digiti minimi muscles). When the stimulating currents were aligned in the direction from the left to the right hemisphere, clear EMG (electromyographic) responses were obtained only from the left ADM to magnetic stimulation of both hemisphere. When the stimulating currents were aligned in the direction from the right to the left hemisphere, clear EMG signals were obtained only from the right ADM to magnetic stimulation of both hemisphere. The functional maps of the brain were sensitive to changes in the direction of the stimulating currents. To explain the phenomena obtained in the experiments, we developed a model of neural excitation elicited by magnetic stimulation. When eddy currents which are induced by pulsed magnetic fields flow in the direction from soma to the distal part of neural fiber, depolarized area in the distal part are excited, and the membrane excitation propagates along the nerve fiber. In contrast, when the induced currents flow in the direction from the distal part to soma, hyperpolarized parts block or inhibit neural excitation even if the depolarized parts near the soma can be excited. The model explains our observation that the orientation of the induced current vectors reflect both the functional and anatomical organization of the neural fibers in the brain.

12. POWERHOUSE INTERIOR SHOWING EXCITER No. 2 SMALL PELTONDOBLE IMPULSE ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

12. POWERHOUSE INTERIOR SHOWING EXCITER No. 2 SMALL PELTON-DOBLE IMPULSE WHEEL, HAND-CONTROLLED GATE VALVE, AND NOZZLE. VIEW TO SOUTHWEST. - Rush Creek Hydroelectric System, Powerhouse Exciters, Rush Creek, June Lake, Mono County, CA

6. POWERHOUSE INTERIOR SHOWING EXCITER No. 1. HANDCONTROLLED GATE VALVE ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

6. POWERHOUSE INTERIOR SHOWING EXCITER No. 1. HAND-CONTROLLED GATE VALVE SHOWN ON NOZZLE TO PELTON-DOBLE IMPULSE WHEEL. VIEW TO NORTHEAST. - Rush Creek Hydroelectric System, Powerhouse Exciters, Rush Creek, June Lake, Mono County, CA

On the Feynman-Hellmann theorem in quantum field theory and the calculation of matrix elements

DOE PAGES

Bouchard, Chris; Chang, Chia Cheng; Kurth, Thorsten; ...

2017-07-12

In this paper, the Feynman-Hellmann theorem can be derived from the long Euclidean-time limit of correlation functions determined with functional derivatives of the partition function. Using this insight, we fully develop an improved method for computing matrix elements of external currents utilizing only two-point correlation functions. Our method applies to matrix elements of any external bilinear current, including nonzero momentum transfer, flavor-changing, and two or more current insertion matrix elements. The ability to identify and control all the systematic uncertainties in the analysis of the correlation functions stems from the unique time dependence of the ground-state matrix elements and the fact that all excited states and contact terms are Euclidean-time dependent. We demonstrate the utility of our method with a calculation of the nucleon axial charge using gradient-flowed domain-wall valence quarks on themore » $$N_f=2+1+1$$ MILC highly improved staggered quark ensemble with lattice spacing and pion mass of approximately 0.15 fm and 310 MeV respectively. We show full control over excited-state systematics with the new method and obtain a value of $$g_A = 1.213(26)$$ with a quark-mass-dependent renormalization coefficient.« less

Green's function of multi-layered poroelastic half-space for models of ground vibration due to railway traffic

NASA Astrophysics Data System (ADS)

Wang, Futong; Tao, Xiaxin; Xie, Lili; Raj, Siddharthan

2017-04-01

This study proposes a Green's function, an essential representation of water-saturated ground under moving excitation, to simulate ground borne vibration from trains. First, general solutions to the governing equations of poroelastic medium are derived by means of integral transform. Secondly, the transmission and reflection matrix approach is used to formulate the relationship between displacement and stress of the stratified ground, which results in the matrix of the Green's function. Then the Green's function is combined into a train-track-ground model, and is verified by typical examples and a field test. Additional simulations show that the computed ground vibration attenuates faster in the immediate vicinity of the track than in the surrounding area. The wavelength of wheel-rail unevenness has a notable effect on computed displacement and pore pressure. The variation of vibration intensity with the depth of ground is significantly influenced by the layering of the strata soil. When the train speed is equal to the velocity of the Rayleigh wave, the Mach cone appears in the simulated wave field. The proposed Green's function is an appropriate representation for a layered ground with shallow ground water table, and will be helpful to understand the dynamic responses of the ground to complicated moving excitation.

Measurement of excitation functions in alpha induced reactions on natCu

NASA Astrophysics Data System (ADS)

Shahid, Muhammad; Kim, Kwangsoo; Kim, Guinyun; Zaman, Muhammad; Nadeem, Muhammad

2015-09-01

The excitation functions of 66,67,68Ga, 62,63,65Zn, 61,64Cu, and 58,60Co radionuclides in the natCu(α, x) reaction were measured in the energy range from 15 to 42 MeV by using a stacked-foil activation method at the MC-50 cyclotron of the Korean Institute of Radiological and Medical Sciences. The measured results were compared with the literature data as well as the theoretical values obtained from the TENDL-2013 and TENDL-2014 libraries based on the TALYS-1.6 code. The integral yields for thick targets of the produced radionuclides were also determined from the measured excitation functions and the stopping power of natural copper.

Non-equilibrium plasma kinetics of reacting CO: an improved state to state approach

NASA Astrophysics Data System (ADS)

Pietanza, L. D.; Colonna, G.; Capitelli, M.

2017-12-01

Non-equilibrium plasma kinetics of reacting CO for conditions typically met in microwave discharges have been developed based on the coupling of excited state kinetics and the Boltzmann equation for the electron energy distribution function (EEDF). Particular attention is given to the insertion in the vibrational kinetics of a complete set of electron molecule resonant processes linking the whole vibrational ladder of the CO molecule, as well as to the role of Boudouard reaction, i.e. the process of forming CO2 by two vibrationally excited CO molecules, in shaping the vibrational distribution of CO and promoting reaction channels assisted by vibrational excitation (pure vibrational mechanisms, PVM). PVM mechanisms can become competitive with electron impact dissociation processes (DEM) in the activation of CO. A case study reproducing the conditions of a microwave discharge has been considered following the coupled kinetics also in the post discharge conditions. Results include the evolution of EEDF in discharge and post discharge conditions highlighting the role of superelastic vibrational and electronic collisions in shaping the EEDF. Moreover, PVM rate coefficients and DEM ones are studied as a function of gas temperature, showing a non-Arrhenius behavior, i.e. the rate coefficients increase with decreasing gas temperature as a result of a vibrational-vibrational (V-V) pumping up mechanism able to form plateaux in the vibrational distribution function. The accuracy of the results is discussed in particular in connection to the present knowledge of the activation energy of the Boudouard process.

Learning about protein solubility from bacterial inclusion bodies

PubMed Central

Martínez-Alonso, Mónica; González-Montalbán, Nuria; García-Fruitós, Elena; Villaverde, Antonio

2009-01-01

The progressive solving of the conformation of aggregated proteins and the conceptual understanding of the biology of inclusion bodies in recombinant bacteria is providing exciting insights on protein folding and quality. Interestingly, newest data also show an unexpected functional and structural complexity of soluble recombinant protein species and picture the whole bacterial cell factory scenario as more intricate than formerly believed. PMID:19133126

Dissociative excitation of the N(+)(5S) state by electron impact on N2 - Excitation function and quenching

NASA Technical Reports Server (NTRS)

Erdman, P. W.; Zipf, E. C.

1986-01-01

Metastable N(+)(5S) ions were produced in the laboratory by dissociative excitation of N2 with energetic electrons. The resulting radiative decay of the N(+)(5S) state was observed with sufficient resolution to completely resolve the doublet from the nearby N2 molecular radiation. The excitation function was measured from threshold to 500 eV. The cross section peaks at a high electron energy and also exhibits a high threshold energy both of which are typical of dissociative excitation-ionization processes. This finding complicates the explanation of electron impact on N2 as the mechanism for the source of the 2145 A 'auroral mystery feature' by further increasing the required peak cross section. It is suggested that the apparent N(+)(5S) quenching in auroras may be an artifact due to the softening of the electron energy spectrum in the auroral E region.

Faraday waves under time-reversed excitation.

PubMed

Pietschmann, Dirk; Stannarius, Ralf; Wagner, Christian; John, Thomas

2013-03-01

Do parametrically driven systems distinguish periodic excitations that are time mirrors of each other? Faraday waves in a Newtonian fluid are studied under excitation with superimposed harmonic wave forms. We demonstrate that the threshold parameters for the stability of the ground state are insensitive to a time inversion of the driving function. This is a peculiarity of some dynamic systems. The Faraday system shares this property with standard electroconvection in nematic liquid crystals [J. Heuer et al., Phys. Rev. E 78, 036218 (2008)]. In general, time inversion of the excitation affects the asymptotic stability of a parametrically driven system, even when it is described by linear ordinary differential equations. Obviously, the observed symmetry has to be attributed to the particular structure of the underlying differential equation system. The pattern selection of the Faraday waves above threshold, on the other hand, discriminates between time-mirrored excitation functions.

THz-circuits driven by photo-thermoelectric, gate-tunable graphene-junctions

NASA Astrophysics Data System (ADS)

Brenneis, Andreas; Schade, Felix; Drieschner, Simon; Heimbach, Florian; Karl, Helmut; Garrido, Jose A.; Holleitner, Alexander W.

2016-10-01

For future on-chip communication schemes, it is essential to integrate nanoscale materials with an ultrafast optoelectronic functionality into high-frequency circuits. The atomically thin graphene has been widely demonstrated to be suitable for photovoltaic and optoelectronic devices because of its broadband optical absorption and its high electron mobility. Moreover, the ultrafast relaxation of photogenerated charge carriers has been verified in graphene. Here, we show that dual-gated graphene junctions can be functional parts of THz-circuits. As the underlying optoelectronic process, we exploit ultrafast photo-thermoelectric currents. We describe an immediate photo-thermoelectric current of the unbiased device following a femtosecond laser excitation. For a picosecond time-scale after the optical excitation, an additional photo-thermoelectric contribution shows up, which exhibits the fingerprint of a spatially inverted temperature profile. The latter can be understood by the different time-constants and thermal coupling mechanisms of the electron and phonon baths within graphene to the substrate and the metal contacts. The interplay of the processes gives rise to ultrafast electromagnetic transients in high-frequency circuits, and it is equally important for a fundamental understanding of graphene-based ultrafast photodetectors and switches.

THz-circuits driven by photo-thermoelectric, gate-tunable graphene-junctions

PubMed Central

Brenneis, Andreas; Schade, Felix; Drieschner, Simon; Heimbach, Florian; Karl, Helmut; Garrido, Jose A.; Holleitner, Alexander W.

2016-01-01

For future on-chip communication schemes, it is essential to integrate nanoscale materials with an ultrafast optoelectronic functionality into high-frequency circuits. The atomically thin graphene has been widely demonstrated to be suitable for photovoltaic and optoelectronic devices because of its broadband optical absorption and its high electron mobility. Moreover, the ultrafast relaxation of photogenerated charge carriers has been verified in graphene. Here, we show that dual-gated graphene junctions can be functional parts of THz-circuits. As the underlying optoelectronic process, we exploit ultrafast photo-thermoelectric currents. We describe an immediate photo-thermoelectric current of the unbiased device following a femtosecond laser excitation. For a picosecond time-scale after the optical excitation, an additional photo-thermoelectric contribution shows up, which exhibits the fingerprint of a spatially inverted temperature profile. The latter can be understood by the different time-constants and thermal coupling mechanisms of the electron and phonon baths within graphene to the substrate and the metal contacts. The interplay of the processes gives rise to ultrafast electromagnetic transients in high-frequency circuits, and it is equally important for a fundamental understanding of graphene-based ultrafast photodetectors and switches. PMID:27762291

THz-circuits driven by photo-thermoelectric, gate-tunable graphene-junctions.

PubMed

Brenneis, Andreas; Schade, Felix; Drieschner, Simon; Heimbach, Florian; Karl, Helmut; Garrido, Jose A; Holleitner, Alexander W

2016-10-20

For future on-chip communication schemes, it is essential to integrate nanoscale materials with an ultrafast optoelectronic functionality into high-frequency circuits. The atomically thin graphene has been widely demonstrated to be suitable for photovoltaic and optoelectronic devices because of its broadband optical absorption and its high electron mobility. Moreover, the ultrafast relaxation of photogenerated charge carriers has been verified in graphene. Here, we show that dual-gated graphene junctions can be functional parts of THz-circuits. As the underlying optoelectronic process, we exploit ultrafast photo-thermoelectric currents. We describe an immediate photo-thermoelectric current of the unbiased device following a femtosecond laser excitation. For a picosecond time-scale after the optical excitation, an additional photo-thermoelectric contribution shows up, which exhibits the fingerprint of a spatially inverted temperature profile. The latter can be understood by the different time-constants and thermal coupling mechanisms of the electron and phonon baths within graphene to the substrate and the metal contacts. The interplay of the processes gives rise to ultrafast electromagnetic transients in high-frequency circuits, and it is equally important for a fundamental understanding of graphene-based ultrafast photodetectors and switches.

Two-Photon Absorption Properties of Gold Fluorescent Protein: A Combined Molecular Dynamics and Quantum Chemistry Study.

PubMed

Şimşek, Yusuf; Brown, Alex

2018-06-07

Molecular dynamics (MD) simulations were carried out to obtain the conformational changes of the chromophore in the gold fluorescent protein (PDB ID: 1OXF ). To obtain two-photon absorption (TPA) cross-sections, time dependent density functional theory (TD-DFT) computations were performed for chromophore geometries sampled along the trajectory. The TD-DFT computations used the CAM-B3LYP functional and 6-31+G(d) basis set. Results showed that two dihedral angles change remarkably over the simulation time. TPA cross-sections were found to average 13.82 GM for the excitation to S 1 computed from the equilibrium geometries; however, extending the structures with a water molecule and GLU residue, which make H bonds with the chromophore molecule, increased excitation energies and TPA cross-sections significantly. Besides the effects of the surrounding residues and the dihedrals on the spectroscopic properties, some bond lengths affected the excitation energies and the TPA cross-sections significantly (up to ±25-30%), while the effects of the bond angles were smaller (±5%). Overall the present results provide insight into the effects of the conformational flexibility on TPA (with gold fluorescent protein as a specific example) and suggest that further experimental measurements of TPA for the gold fluorescent protein should be undertaken.

The generalized Hill model: A kinematic approach towards active muscle contraction

NASA Astrophysics Data System (ADS)

Göktepe, Serdar; Menzel, Andreas; Kuhl, Ellen

2014-12-01

Excitation-contraction coupling is the physiological process of converting an electrical stimulus into a mechanical response. In muscle, the electrical stimulus is an action potential and the mechanical response is active contraction. The classical Hill model characterizes muscle contraction though one contractile element, activated by electrical excitation, and two non-linear springs, one in series and one in parallel. This rheology translates into an additive decomposition of the total stress into a passive and an active part. Here we supplement this additive decomposition of the stress by a multiplicative decomposition of the deformation gradient into a passive and an active part. We generalize the one-dimensional Hill model to the three-dimensional setting and constitutively define the passive stress as a function of the total deformation gradient and the active stress as a function of both the total deformation gradient and its active part. We show that this novel approach combines the features of both the classical stress-based Hill model and the recent active-strain models. While the notion of active stress is rather phenomenological in nature, active strain is micro-structurally motivated, physically measurable, and straightforward to calibrate. We demonstrate that our model is capable of simulating excitation-contraction coupling in cardiac muscle with its characteristic features of wall thickening, apical lift, and ventricular torsion.

Nonlinear electron-phonon coupling in doped manganites

DOE PAGES

Esposito, Vincent; Fechner, M.; Mankowsky, R.; ...

2017-06-15

Here, we employ time-resolved resonant x-ray diffraction to study the melting of charge order and the associated insulator-to-metal transition in the doped manganite Pr 0.5Ca 0.5MnO 3 after resonant excitation of a high-frequency infrared-active lattice mode. We find that the charge order reduces promptly and highly nonlinearly as function of excitation fluence. Density-functional theory calculations suggest that direct anharmonic coupling between the excited lattice mode and the electronic structure drives these dynamics, highlighting a new avenue of nonlinear phonon control.

Nonlinear Electron-Phonon Coupling in Doped Manganites.

PubMed

Esposito, V; Fechner, M; Mankowsky, R; Lemke, H; Chollet, M; Glownia, J M; Nakamura, M; Kawasaki, M; Tokura, Y; Staub, U; Beaud, P; Först, M

2017-06-16

We employ time-resolved resonant x-ray diffraction to study the melting of charge order and the associated insulator-to-metal transition in the doped manganite Pr_{0.5}Ca_{0.5}MnO_{3} after resonant excitation of a high-frequency infrared-active lattice mode. We find that the charge order reduces promptly and highly nonlinearly as function of excitation fluence. Density-functional theory calculations suggest that direct anharmonic coupling between the excited lattice mode and the electronic structure drives these dynamics, highlighting a new avenue of nonlinear phonon control.

Excitation power quantities in phase resonance testing of nonlinear systems with phase-locked-loop excitation

NASA Astrophysics Data System (ADS)

Peter, Simon; Leine, Remco I.

2017-11-01

Phase resonance testing is one method for the experimental extraction of nonlinear normal modes. This paper proposes a novel method for nonlinear phase resonance testing. Firstly, the issue of appropriate excitation is approached on the basis of excitation power considerations. Therefore, power quantities known from nonlinear systems theory in electrical engineering are transferred to nonlinear structural dynamics applications. A new power-based nonlinear mode indicator function is derived, which is generally applicable, reliable and easy to implement in experiments. Secondly, the tuning of the excitation phase is automated by the use of a Phase-Locked-Loop controller. This method provides a very user-friendly and fast way for obtaining the backbone curve. Furthermore, the method allows to exploit specific advantages of phase control such as the robustness for lightly damped systems and the stabilization of unstable branches of the frequency response. The reduced tuning time for the excitation makes the commonly used free-decay measurements for the extraction of backbone curves unnecessary. Instead, steady-state measurements for every point of the curve are obtained. In conjunction with the new mode indicator function, the correlation of every measured point with the associated nonlinear normal mode of the underlying conservative system can be evaluated. Moreover, it is shown that the analysis of the excitation power helps to locate sources of inaccuracies in the force appropriation process. The method is illustrated by a numerical example and its functionality in experiments is demonstrated on a benchmark beam structure.

A Preliminary Transcranial Magnetic Stimulation Study of Cortical Inhibition and Excitability in High-Functioning Autism and Asperger Disorder

ERIC Educational Resources Information Center

Enticott, Peter G.; Rinehart, Nicole J.; Tonge, Bruce J.; Bradshaw, John L.; Fitzgerald, Paul B.

2010-01-01

Aim: Controversy surrounds the distinction between high-functioning autism (HFA) and Asperger disorder, but motor abnormalities are associated features of both conditions. This study examined motor cortical inhibition and excitability in HFA and Asperger disorder using transcranial magnetic stimulation (TMS). Method: Participants were diagnosed by…

Calculation of Vibrational and Electronic Excited-State Absorption Spectra of Arsenic-Water Complexes Using Density Functional Theory

DTIC Science & Technology

2016-06-03

Naval Research Laboratory Washington, DC 20375-5320 NRL/MR/6390--16-9681 Calculation of Vibrational and Electronic Excited-State Absorption Spectra...NUMBER OF PAGES 17. LIMITATION OF ABSTRACT Calculation of Vibrational and Electronic Excited-State Absorption Spectra of Arsenic-Water Complexes Using...Unclassified Unlimited Unclassified Unlimited 59 Samuel G. Lambrakos (202) 767-2601 Calculations are presented of vibrational and electronic excited-state

Luminescence studies and infrared emission of erbium-doped calcium zirconate phosphor.

PubMed

Tiwari, Neha; Dubey, Vikas

2016-05-01

The near-infrared-to-visible upconversion luminescence behaviour of Er(3+)-doped CaZrO3 phosphor is discussed in this manuscript. The phosphor was prepared by a combustion synthesis technique that is suitable for less-time-taking techniques for nanophosphors. The starting materials used for sample preparation were Ca(NO3)2.4H2O, Zr(NO3)4 and Er(NO3)2, and urea was used as a fuel. The prepared sample was characterized by X-ray diffraction (XRD). The surface morphology of prepared phosphor was determined by field emission gun scanning electron microscopy (FEGSEM). The functional group analysis was determined by Fourier transform infrared (FTIR) spectroscopy. All prepared phosphors with variable Er(3+) concentrations (0.5-2.5 mol%) were studied by photoluminescence analysis. It was found that the excitation spectra of the prepared phosphor showed a sharp excitation peak centred at 980 nm. The emission spectra with variable Er(3+) concentrations showed strong peaks in the 555 nm and 567 nm range, with a dominant peak at 555 nm due to the ((2)H(11/2),(4)S(3/2)) transition and a weaker transition at 567 nm associated with 527 nm. Spectrophotometric determination of the peak was evaluated by the Commission Internationale de I'Eclairage (CIE) method These upconverted emissions were attributed to a two-photon process. The excitation wavelength dependence of the upconverted luminescence, together with its time evolution after infrared pulsed excitation, suggested that energy transfer upconversion processes were responsible for the upconversion luminescence. The upconversion mechanisms were studied in detail through laser power dependence. Excited state absorption and energy transfer processes were discussed as possible upconversion mechanisms. The cross-relaxation process in Er(3+) was also investigated. Copyright © 2015 John Wiley & Sons, Ltd.

Calculations of stopping powers of 100 eV-30 keV electrons in 31 elemental solids

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

Tanuma, S.; Powell, C. J.; Penn, D. R.

We present calculated electron stopping powers (SPs) for 31 elemental solids (Li, Be, glassy C, graphite, diamond, Na, Mg, K, Sc, Ti, V, Fe, Y, Zr, Nb, Mo, Ru, Rh, In, Sn, Cs, Gd, Tb, Dy, Hf, Ta, W, Re, Os, Ir, and Bi). These SPs were determined with an algorithm previously used for the calculation of electron inelastic mean free paths and from energy-loss functions (ELFs) derived from experimental optical data. The SP calculations were made for electron energies between 100 eV and 30 keV and supplement our earlier SP calculations for ten additional solids (Al, Si, Cr, Ni,more » Cu, Ge, Pd, Ag, Pt, and Au). Plots of SP versus atomic number for the group of 41 solids show clear trends. Multiple peaks and shoulders are seen that result from the contributions of valence-electron and various inner-shell excitations. Satisfactory agreement was found between the calculated SPs and values from the relativistic Bethe SP equation with recommended values of the mean excitation energy (MEE) for energies above 10 keV. We determined effective MEEs versus maximum excitation energy from the ELFs for each solid. Plots of effective MEE versus atomic number showed the relative contributions of valence-electron and different core-electron excitations to the MEE. For a maximum excitation energy of 30 keV, our effective MEEs agreed well for Be, graphite, Na, Al, and Si with recommended MEEs; a difference for Li was attributed to sample oxidation in the SP measurements for the recommended MEE. Substantially different effective MEEs were found for the three carbon allotropes (graphite, diamond, and glassy C)« less

Brain-robot interface driven plasticity: Distributed modulation of corticospinal excitability.

PubMed

Kraus, Dominic; Naros, Georgios; Bauer, Robert; Leão, Maria Teresa; Ziemann, Ulf; Gharabaghi, Alireza

2016-01-15

Brain-robot interfaces (BRI) are studied as novel interventions to facilitate functional restoration in patients with severe and persistent motor deficits following stroke. They bridge the impaired connection in the sensorimotor loop by providing brain-state dependent proprioceptive feedback with orthotic devices attached to the hand or arm of the patients. The underlying neurophysiology of this BRI neuromodulation is still largely unknown. We investigated changes of corticospinal excitability with transcranial magnetic stimulation in thirteen right-handed healthy subjects who performed 40min of kinesthetic motor imagery receiving proprioceptive feedback with a robotic orthosis attached to the left hand contingent to event-related desynchronization of the right sensorimotor cortex in the β-band (16-22Hz). Neural correlates of this BRI intervention were probed by acquiring the stimulus-response curve (SRC) of both motor evoked potential (MEP) peak-to-peak amplitudes and areas under the curve. In addition, a motor mapping was obtained. The specificity of the effects was studied by comparing two neighboring hand muscles, one BRI-trained and one control muscle. Robust changes of MEP amplitude but not MEP area occurred following the BRI intervention, but only in the BRI-trained muscle. The steep part of the SRC showed an MEP increase, while the plateau of the SRC showed an MEP decrease. MEP mapping revealed a distributed pattern with a decrease of excitability in the hand area of the primary motor cortex, which controlled the BRI, but an increase of excitability in the surrounding somatosensory and premotor cortex. In conclusion, the BRI intervention induced a complex pattern of modulated corticospinal excitability, which may boost subsequent motor learning during physiotherapy. Copyright © 2015 Elsevier Inc. All rights reserved.

Dependence of Excited State Potential Energy Surfaces on the Spatial Overlap of the Kohn-Sham Orbitals and the Amount of Nonlocal Hartree-Fock Exchange in Time-Dependent Density Functional Theory.

PubMed

Plötner, Jürgen; Tozer, David J; Dreuw, Andreas

2010-08-10

Time-dependent density functional theory (TDDFT) with standard GGA or hybrid exchange-correlation functionals is not capable of describing the potential energy surface of the S1 state of Pigment Yellow 101 correctly; an additional local minimum is observed at a twisted geometry with substantial charge transfer (CT) character. To investigate the influence of nonlocal exact orbital (Hartree-Fock) exchange on the shape of the potential energy surface of the S1 state in detail, it has been computed along the twisting coordinate employing the standard BP86, B3LYP, and BHLYP xc-functionals as well as the long-range separated (LRS) exchange-correlation (xc)-functionals LC-BOP, ωB97X, ωPBE, and CAM-B3LYP and compared to RI-CC2 benchmark results. Additionally, a recently suggested Λ-parameter has been employed that measures the amount of CT in an excited state by calculating the spatial overlap of the occupied and virtual molecular orbitals involved in the transition. Here, the error in the calculated S1 potential energy curves at BP86, B3LYP, and BHLYP can be clearly related to the Λ-parameter, i.e., to the extent of charge transfer. Additionally, it is demonstrated that the CT problem is largely alleviated when the BHLYP xc-functional is employed, although it still exhibits a weak tendency to underestimate the energy of CT states. The situation improves drastically when LRS-functionals are employed within TDDFT excited state calculations. All tested LRS-functionals give qualitatively the correct potential energy curves of the energetically lowest excited states of P. Y. 101 along the twisting coordinate. While LC-BOP and ωB97X overcorrect the CT problem and now tend to give too large excitation energies compared to other non-CT states, ωPBE and CAM-B3LYP are in excellent agreement with the RI-CC2 results, with respect to both the correct shape of the potential energy curve as well as the absolute values of the calculated excitation energies.

Spin-1 Kitaev model in one dimension

NASA Astrophysics Data System (ADS)

Sen, Diptiman; Shankar, R.; Dhar, Deepak; Ramola, Kabir

2010-11-01

We study a one-dimensional version of the Kitaev model on a ring of size N , in which there is a spin S>1/2 on each site and the Hamiltonian is J∑nSnxSn+1y . The cases where S is integer and half-odd integer are qualitatively different. We show that there is a Z2 -valued conserved quantity Wn for each bond (n,n+1) of the system. For integer S , the Hilbert space can be decomposed into 2N sectors, of unequal sizes. The number of states in most of the sectors grows as dN , where d depends on the sector. The largest sector contains the ground state, and for this sector, for S=1 , d=(5+1)/2 . We carry out exact diagonalization for small systems. The extrapolation of our results to large N indicates that the energy gap remains finite in this limit. In the ground-state sector, the system can be mapped to a spin-1/2 model. We develop variational wave functions to study the lowest energy states in the ground state and other sectors. The first excited state of the system is the lowest energy state of a different sector and we estimate its excitation energy. We consider a more general Hamiltonian, adding a term λ∑nWn , and show that this has gapless excitations in the range λ1c≤λ≤λ2c . We use the variational wave functions to study how the ground-state energy and the defect density vary near the two critical points λ1c and λ2c .

Dendritic excitability modulates dendritic information processing in a purkinje cell model.

PubMed

Coop, Allan D; Cornelis, Hugo; Santamaria, Fidel

2010-01-01

Using an electrophysiological compartmental model of a Purkinje cell we quantified the contribution of individual active dendritic currents to processing of synaptic activity from granule cells. We used mutual information as a measure to quantify the information from the total excitatory input current (I(Glu)) encoded in each dendritic current. In this context, each active current was considered an information channel. Our analyses showed that most of the information was encoded by the calcium (I(CaP)) and calcium activated potassium (I(Kc)) currents. Mutual information between I(Glu) and I(CaP) and I(Kc) was sensitive to different levels of excitatory and inhibitory synaptic activity that, at the same time, resulted in the same firing rate at the soma. Since dendritic excitability could be a mechanism to regulate information processing in neurons we quantified the changes in mutual information between I(Glu) and all Purkinje cell currents as a function of the density of dendritic Ca (g(CaP)) and Kca (g(Kc)) conductances. We extended our analysis to determine the window of temporal integration of I(Glu) by I(CaP) and I(Kc) as a function of channel density and synaptic activity. The window of information integration has a stronger dependence on increasing values of g(Kc) than on g(CaP), but at high levels of synaptic stimulation information integration is reduced to a few milliseconds. Overall, our results show that different dendritic conductances differentially encode synaptic activity and that dendritic excitability and the level of synaptic activity regulate the flow of information in dendrites.

Nonlinear electronic excitations in crystalline solids using meta-generalized gradient approximation and hybrid functional in time-dependent density functional theory

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

Sato, Shunsuke A.; Taniguchi, Yasutaka; Department of Medical and General Sciences, Nihon Institute of Medical Science, 1276 Shimogawara, Moroyama-Machi, Iruma-Gun, Saitama 350-0435

2015-12-14

We develop methods to calculate electron dynamics in crystalline solids in real-time time-dependent density functional theory employing exchange-correlation potentials which reproduce band gap energies of dielectrics; a meta-generalized gradient approximation was proposed by Tran and Blaha [Phys. Rev. Lett. 102, 226401 (2009)] (TBm-BJ) and a hybrid functional was proposed by Heyd, Scuseria, and Ernzerhof [J. Chem. Phys. 118, 8207 (2003)] (HSE). In time evolution calculations employing the TB-mBJ potential, we have found it necessary to adopt the predictor-corrector step for a stable time evolution. We have developed a method to evaluate electronic excitation energy without referring to the energy functionalmore » which is unknown for the TB-mBJ potential. For the HSE functional, we have developed a method for the operation of the Fock-like term in Fourier space to facilitate efficient use of massive parallel computers equipped with graphic processing units. We compare electronic excitations in silicon and germanium induced by femtosecond laser pulses using the TB-mBJ, HSE, and a simple local density approximation (LDA). At low laser intensities, electronic excitations are found to be sensitive to the band gap energy: they are close to each other using TB-mBJ and HSE and are much smaller in LDA. At high laser intensities close to the damage threshold, electronic excitation energies do not differ much among the three cases.« less

Radiofrequency pulse design using nonlinear gradient magnetic fields.

PubMed

Kopanoglu, Emre; Constable, R Todd

2015-09-01

An iterative k-space trajectory and radiofrequency (RF) pulse design method is proposed for excitation using nonlinear gradient magnetic fields. The spatial encoding functions (SEFs) generated by nonlinear gradient fields are linearly dependent in Cartesian coordinates. Left uncorrected, this may lead to flip angle variations in excitation profiles. In the proposed method, SEFs (k-space samples) are selected using a matching pursuit algorithm, and the RF pulse is designed using a conjugate gradient algorithm. Three variants of the proposed approach are given: the full algorithm, a computationally cheaper version, and a third version for designing spoke-based trajectories. The method is demonstrated for various target excitation profiles using simulations and phantom experiments. The method is compared with other iterative (matching pursuit and conjugate gradient) and noniterative (coordinate-transformation and Jacobian-based) pulse design methods as well as uniform density spiral and EPI trajectories. The results show that the proposed method can increase excitation fidelity. An iterative method for designing k-space trajectories and RF pulses using nonlinear gradient fields is proposed. The method can either be used for selecting the SEFs individually to guide trajectory design, or can be adapted to design and optimize specific trajectories of interest. © 2014 Wiley Periodicals, Inc.

Motor excitability measurements: the influence of gender, body mass index, age and temperature in healthy controls.

PubMed

Casanova, I; Diaz, A; Pinto, S; de Carvalho, M

2014-04-01

The technique of threshold tracking to test axonal excitability gives information about nodal and internodal ion channel function. We aimed to investigate variability of the motor excitability measurements in healthy controls, taking into account age, gender, body mass index (BMI) and small changes in skin temperature. We examined the left median nerve of 47 healthy controls using the automated threshold-tacking program, QTRAC. Statistical multiple regression analysis was applied to test relationship between nerve excitability measurements and subject variables. Comparisons between genders did not find any significant difference (P>0.2 for all comparisons). Multiple regression analysis showed that motor amplitude decreases with age and temperature, stimulus-response slope decreases with age and BMI, and that accommodation half-time decrease with age and temperature. The changes related to demographic features on TRONDE protocol parameters are small and less important than in conventional nerve conduction studies. Nonetheless, our results underscore the relevance of careful temperature control, and indicate that interpretation of stimulus-response slope and accommodation half-time should take into account age and BMI. In contrast, gender is not of major relevance to axonal threshold findings in motor nerves. Copyright © 2014 Elsevier Masson SAS. All rights reserved.

Ultralong-range Rydberg Molecules: Investigation of a Novel Binding Mechanism

NASA Astrophysics Data System (ADS)

Butscher, Björn; Bendkowsky, Vera; Nipper, Johannes; Balewski, Jonathan; Shaffer, James P.; Löw, Robert; Pfau, Tilman

2010-03-01

For highly excited Rydberg atoms, the scattering of the Rydberg electron from a nearby polarizable ground state atom can generate an attractive mean-field potential which is able to bind the ground state atom to the Rydberg atom within the Rydberg electron wave function at binding energies ranging from a few MHz to hundreds of MHz[1]. We present spectroscopic data on the observation of various bound states including the vibrational ground and excited states of rubidium dimers Rb(5S)-Rb(nS) as well as those of trimer states. Furthermore, we show calculations that reproduce the observed binding energies remarkably well and reveal that some of the excited states are purely bound by quantum reflection at a shape resonance for p-wave scattering [2]. To further characterize the coherent excitation of the molecular states, we performed echo experiments. [0pt] [1] V. Bendkowsky, B. Butscher, J. Nipper, J. P. Shaffer, R. Löw, T. Pfau, Nature 458, 1005 (2009); [2] V. Bendkowsky, B. Butscher, J. Nipper, J. Balewski, J. P. Shaffer, R. Löw, T. Pfau, W. Li, J. Stanojevic, T. Pohl,and J. M. Rost, arXiv:0912.4058 (2009)

Hydrogen bonding interaction of small acetaldehyde clusters studied with core-electron excitation spectroscopy in the oxygen K-edge region

NASA Astrophysics Data System (ADS)

Tabayashi, K.; Chohda, M.; Yamanaka, T.; Tsutsumi, Y.; Takahashi, O.; Yoshida, H.; Taniguchi, M.

2010-06-01

In order to examine inner-shell electron excitation spectra of molecular clusters with strong multipole interactions, excitation spectra and time-of-flight (TOF) fragment-mass spectra of small acetaldehyde (AA) clusters have been studied under the beam conditions. The TOF spectra at the oxygen K-edge region showed an intense growth of the protonated clusters, MnH+ (M=CH3CHO) in the cluster beams. "cluster-specific" excitation spectra could be generated by monitoring partial-ion-yields of the protonated clusters. The most intense band of O1s→π*CO was found to shift to a higher energy by 0.15 eV relative to the monomer band upon clusterization. X-ray absorption spectra (XAS) were also calculated for the representative dimer configurations using a computer modelling program based on the density functional theory. The XAS prediction for the most stable (non-planar) configuration was found to give a close comparison with the cluster-band shift observed. The band shift was interpreted as being due to the HOMO-LUMO interaction within the complex where a contribution of vibrationally blue-shifting hydrogen bonding could be identified.

TMS measures of motor cortex function after stroke: A meta-analysis.

PubMed

McDonnell, Michelle N; Stinear, Cathy M

Transcranial magnetic stimulation (TMS) is commonly used to measure the effects of stroke on corticomotor excitability, intracortical function, and interhemispheric interactions. The interhemispheric inhibition model posits that recovery of motor function after stroke is linked to rebalancing of asymmetric interhemispheric inhibition and corticomotor excitability. This model forms the rationale for using neuromodulation techniques to suppress unaffected motor cortex excitability, and facilitate affected motor cortex excitability. However, the evidence base for using neuromodulation techniques to promote post-stroke motor recovery is inconclusive. The aim of this meta-analysis was to compare measures of corticomotor excitability, intracortical function, and interhemispheric inhibition, between the affected and unaffected hemispheres of people with stroke, and measures made in healthy adults. A literature search was conducted to identify studies that made TMS measures of the motor cortex in adult stroke patients. Two authors independently extracted data, and the quality of included studies was assessed. TMS measures were compared between the affected and unaffected hemispheres of stroke patients, between the affected hemisphere and healthy controls, and between the unaffected hemisphere and healthy controls. Analyses were carried out with data grouped according to the muscle from which responses were recorded, and separately according to time post-stroke (<3 months, and ≥6 months). Meta-analyses were carried out using a random effects model. There were 844 studies identified, and 112 studies included in the meta-analysis. Results were very similar across muscle groups. Affected hemisphere M1 excitability is lower than unaffected and healthy control M1 excitability after stroke. Affected hemisphere short interval intracortical inhibition (SICI) is lower than unaffected and healthy control SICI early after stroke, and not different in the chronic phase. There were no differences detected between the unaffected hemisphere and healthy controls. There were only seven studies of interhemispheric inhibition that could be included, with no clear effects of hemisphere or time post-stroke. The neurophysiological effects of stroke are primarily localised to the affected hemisphere, and there is no clear evidence for hyper-excitability of the unaffected hemisphere or imbalanced interhemispheric inhibition. This indicates that facilitating affected M1 excitability directly may be more beneficial than suppressing unaffected M1 excitability for promoting post-stroke recovery. Copyright © 2017 Elsevier Inc. All rights reserved.

The nestin-expressing and non-expressing neurons in rat basal forebrain display different electrophysiological properties and project to hippocampus

PubMed Central

2011-01-01

Background Nestin-immunoreactive (nestin-ir) neurons have been identified in the medial septal/diagonal band complex (MS/DBB) of adult rat and human, but the significance of nestin expression in functional neurons is not clear. This study investigated electrophysiological properties and neurochemical phenotypes of nestin-expressing (nestin+) neurons using whole-cell recording combined with single-cell RT-PCR to explore the significance of nestin expression in functional MS/DBB neurons. The retrograde labelling and immunofluorescence were used to investigate the nestin+ neuron related circuit in the septo-hippocampal pathway. Results The results of single-cell RT-PCR showed that 87.5% (35/40) of nestin+ cells expressed choline acetyltransferase mRNA (ChAT+), only 44.3% (35/79) of ChAT+ cells expressed nestin mRNA. Furthermore, none of the nestin+ cells expressed glutamic acid decarboxylases 67 (GAD67) or vesicular glutamate transporters (VGLUT) mRNA. All of the recorded nestin+ cells were excitable and demonstrated slow-firing properties, which were distinctive from those of GAD67 or VGLUT mRNA-positive neurons. These results show that the MS/DBB cholinergic neurons could be divided into nestin-expressing cholinergic neurons (NEChs) and nestin non-expressing cholinergic neurons (NNChs). Interestingly, NEChs had higher excitability and received stronger spontaneous excitatory synaptic inputs than NNChs. Retrograde labelling combined with choline acetyltransferase and nestin immunofluorescence showed that both of the NEChs and NNChs projected to hippocampus. Conclusions These results suggest that there are two parallel cholinergic septo-hippocampal pathways that may have different functions. The significance of nestin expressing in functional neurons has been discussed. PMID:22185478

14. POWERHOUSE INTERIOR, EXCITER No. 2 SHOWING GENERAL ELECTRIC INDUCTION ...

Library of Congress Historic Buildings Survey, Historic Engineering Record, Historic Landscapes Survey

14. POWERHOUSE INTERIOR, EXCITER No. 2 SHOWING GENERAL ELECTRIC INDUCTION MOTOR IN SERIES BETWEEN PELTON-DOBLE IMPULSE WHEEL AND GENERAL ELECTRIC GENERATOR. VIEW TO EAST. - Rush Creek Hydroelectric System, Powerhouse Exciters, Rush Creek, June Lake, Mono County, CA

Molecular and excited state properties of isomeric scarlet disperse dyes

NASA Astrophysics Data System (ADS)

Lim, Jihye; Szymczyk, Malgorzata; Mehraban, Nahid; Ding, Yi; Parrillo-Chapman, Lisa; El-Shafei, Ahmed; Freeman, Harold S.

2018-06-01

This work was part of an investigation aimed at characterizing the molecular and excited state properties of currently available disperse dyes developed to provide stability to extensive sunlight exposures when adsorbed on poly(ethylene terephthalate) (PET) fibers. Having completed the characterization of yellow, magenta, and cyan disperse dyes for PET-based fabrics used outdoors, our attention turned to the colors designed to enhance the color gamut of a standard 4-member (cyan/yellow/magenta/black) color set. The present study pertained specifically to the characterization of commercially available scarlet dyes. In this regard, HPLC analysis showed that a scarlet product used for PET coloration was mainly a 70/30 mixture of dyes, and the use of HRMS and single crystal X-ray diffraction analyses indicated that these two dyes were azo compounds derived from isomeric pyridine-based couplers which differed in the location of the primary amino (sbnd NH2) and anilino (sbnd NHPh) groups attached to the pyridine ring. One dye structure has the sbnd NHPh group para to the azo group (Sc2), while the other has that group in the ortho position (Sc3). The presence of either ortho substituent provides photostabilization through intramolecular H-bonding with the azo moiety. Further, results from molecular modeling studies showed that the lower excited state oxidation potential of Sc3 relative to that of Sc2 allows Sc3 to function as an energy quencher for the excited state of Sc2 - through thermodynamically favorable electron transfer.

Impact of wavefront distortion and scattering on 2-photon microscopy in mammalian brain tissue

PubMed Central

Chaigneau, Emmanuelle; Wright, Amanda J.; Poland, Simon P.; Girkin, John M.; Silver, R. Angus

2011-01-01

Two-photon (2P) microscopy is widely used in neuroscience, but the optical properties of brain tissue are poorly understood. We have investigated the effect of brain tissue on the 2P point spread function (PSF2P) by imaging fluorescent beads through living cortical slices. By combining this with measurements of the mean free path of the excitation light, adaptive optics and vector-based modeling that includes phase modulation and scattering, we show that tissue-induced wavefront distortions are the main determinant of enlargement and distortion of the PSF2P at intermediate imaging depths. Furthermore, they generate surrounding lobes that contain more than half of the 2P excitation. These effects reduce the resolution of fine structures and contrast and they, together with scattering, limit 2P excitation. Our results disentangle the contributions of scattering and wavefront distortion in shaping the cortical PSF2P, thereby providing a basis for improved 2P microscopy. PMID:22109156

Probing the symmetry of the potential of localized surface plasmon resonances with phase-shaped electron beams

PubMed Central

Guzzinati, Giulio; Béché, Armand; Lourenço-Martins, Hugo; Martin, Jérôme; Kociak, Mathieu; Verbeeck, Jo

2017-01-01

Plasmonics, the science and technology of the interaction of light with metallic objects, is fundamentally changing the way we can detect, generate and manipulate light. Although the field is progressing swiftly, thanks to the availability of nanoscale manufacturing and analysis methods, fundamental properties such as the plasmonic excitations' symmetries cannot be accessed directly, leading to a partial, sometimes incorrect, understanding of their properties. Here we overcome this limitation by deliberately shaping the wave function of an electron beam to match a plasmonic excitations' symmetry in a modified transmission electron microscope. We show experimentally and theoretically that this offers selective detection of specific plasmon modes within metallic nanoparticles, while excluding modes with other symmetries. This method resembles the widespread use of polarized light for the selective excitation of plasmon modes with the advantage of locally probing the response of individual plasmonic objects and a far wider range of symmetry selection criteria. PMID:28401942

Electromagnon dispersion probed by inelastic X-ray scattering in LiCrO2

PubMed Central

Tóth, Sándor; Wehinger, Björn; Rolfs, Katharina; Birol, Turan; Stuhr, Uwe; Takatsu, Hiroshi; Kimura, Kenta; Kimura, Tsuyoshi; Rønnow, Henrik M.; Rüegg, Christian

2016-01-01

Inelastic X-ray scattering with meV energy resolution (IXS) is an ideal tool to measure collective excitations in solids and liquids. In non-resonant scattering condition, the cross-section is strongly dominated by lattice vibrations (phonons). However, it is possible to probe additional degrees of freedom such as magnetic fluctuations that are strongly coupled to the phonons. The IXS spectrum of the coupled system contains not only the phonon dispersion but also the so far undetected magnetic correlation function. Here we report the observation of strong magnon–phonon coupling in LiCrO2 that enables the measurement of magnetic correlations throughout the Brillouin zone via IXS. We find electromagnon excitations and electric dipole active two-magnon excitations in the magnetically ordered phase and heavily damped electromagnons in the paramagnetic phase of LiCrO2. We predict that several (frustrated) magnets with dominant direct exchange and non-collinear magnetism show surprisingly large IXS cross-section for magnons and multi-magnon processes. PMID:27882928

A class of parametrically excited calcium oscillation detectors.

PubMed Central

Izu, L T; Spangler, R A

1995-01-01

Intracellular Ca2+ oscillations are often a response to external signals such as hormones. Changes in the external signal can alter the frequency, amplitude, or form of the oscillations suggesting that information is encoded in the pattern of Ca2+ oscillations. How might a cell decode this signal? We show that an excitable system whose kinetic parameters are modulated by the Ca2+ concentration can function as a Ca2+ oscillation detector. Such systems have the following properties: (1) They are more sensitive to an oscillatory than to a steady Ca2+ signal. (2) Their response is largely independent of the signal amplitude. (3) They can extract information from a noisy signal. (4) Unlike other frequency sensitive detectors, they have a flat frequency response. These properties make a Ca(2+)-sensitive excitable system nearly ideal for detecting and decoding Ca2+ oscillations. We suggest that Ca2+ oscillations, in concert with these detectors, can act as cellular timekeepers to coordinate related biochemical reactions and enhance their overall efficiency. PMID:7787048

Ambra1 Shapes Hippocampal Inhibition/Excitation Balance: Role in Neurodevelopmental Disorders.

PubMed

Nobili, Annalisa; Krashia, Paraskevi; Cordella, Alberto; La Barbera, Livia; Dell'Acqua, Maria Concetta; Caruso, Angela; Pignataro, Annabella; Marino, Ramona; Sciarra, Francesca; Biamonte, Filippo; Scattoni, Maria Luisa; Ammassari-Teule, Martine; Cecconi, Francesco; Berretta, Nicola; Keller, Flavio; Mercuri, Nicola Biagio; D'Amelio, Marcello

2018-02-27

Imbalances between excitatory and inhibitory synaptic transmission cause brain network dysfunction and are central to the pathogenesis of neurodevelopmental disorders. Parvalbumin interneurons are highly implicated in this imbalance. Here, we probed the social behavior and hippocampal function of mice carrying a haploinsufficiency for Ambra1, a pro-autophagic gene crucial for brain development. We show that heterozygous Ambra1 mice (Ambra +/- ) are characterized by loss of hippocampal parvalbumin interneurons, decreases in the inhibition/excitation ratio, and altered social behaviors that are solely restricted to the female gender. Loss of parvalbumin interneurons in Ambra1 +/- females is further linked to reductions of the inhibitory drive onto principal neurons and alterations in network oscillatory activity, CA1 synaptic plasticity, and pyramidal neuron spine density. Parvalbumin interneuron loss is underlined by increased apoptosis during the embryonic development of progenitor neurons in the medial ganglionic eminence. Together, these findings identify an Ambra1-dependent mechanism that drives inhibition/excitation imbalance in the hippocampus, contributing to abnormal brain activity reminiscent of neurodevelopmental disorders.

Controlling the motion of solitons in 1-D magnonic crystal

NASA Astrophysics Data System (ADS)

Giridharan, D.; Sabareesan, P.; Daniel, M.

2018-04-01

We investigate nonlinear localized magnetic excitations in a simple form of one dimensional magnonic crystal by considering a ferromagnetic medium under periodic applied magnetic field of spatially varying strength. The governing Landau-Lifshitz equation is transformed into nonlinear evolution equation of a complex function through stereographic projection technique. The associated evolution equation numerically solved by using split-step Fourier method (SSFM). From the obtained results it is observed that the excitations appear in the form of solitons and the periodic magnetic field of spatially varying strength perturbs the soliton propagation. Bright and dark soliton solutions are constructed and studied the effect of tuning the strength of spatially periodic applied magnetic field on the nonlinear excitation of magnetization. The results show that the amplitude and velocity of the soliton can be effectively managed by varying the strength of spatially periodic applied magnetic field and it act as periodic potential which provides an additional degree of freedom to control the nature of soliton propagation in a ferromagnetic medium.

Selective far-field addressing of coupled quantum dots in a plasmonic nanocavity.

PubMed

Tang, Jianwei; Xia, Juan; Fang, Maodong; Bao, Fanglin; Cao, Guanjun; Shen, Jianqi; Evans, Julian; He, Sailing

2018-04-27

Plasmon-emitter hybrid nanocavity systems exhibit strong plasmon-exciton interactions at the single-emitter level, showing great potential as testbeds and building blocks for quantum optics and informatics. However, reported experiments involve only one addressable emitting site, which limits their relevance for many fundamental questions and devices involving interactions among emitters. Here we open up this critical degree of freedom by demonstrating selective far-field excitation and detection of two coupled quantum dot emitters in a U-shaped gold nanostructure. The gold nanostructure functions as a nanocavity to enhance emitter interactions and a nanoantenna to make the emitters selectively excitable and detectable. When we selectively excite or detect either emitter, we observe photon emission predominantly from the target emitter with up to 132-fold Purcell-enhanced emission rate, indicating individual addressability and strong plasmon-exciton interactions. Our work represents a step towards a broad class of plasmonic devices that will enable faster, more compact optics, communication and computation.

Combined Molecular and Spin Dynamics Simulation of Lattice Vacancies in BCC Iron

NASA Astrophysics Data System (ADS)

Mudrick, Mark; Perera, Dilina; Eisenbach, Markus; Landau, David P.

Using an atomistic model that treats translational and spin degrees of freedom equally, combined molecular and spin dynamics simulations have been performed to study dynamic properties of BCC iron at varying levels of defect impurity. Atomic interactions are described by an empirical many-body potential, and spin interactions with a Heisenberg-like Hamiltonian with a coordinate dependent exchange interaction. Equations of motion are solved numerically using the second-order Suzuki-Trotter decomposition for the time evolution operator. We analyze the spatial and temporal correlation functions for atomic displacements and magnetic order to obtain the effect of vacancy defects on the phonon and magnon excitations. We show that vacancy clusters in the material cause splitting of the characteristic transverse spin-wave excitations, indicating the production of additional excitation modes. Additionally, we investigate the coupling of the atomic and magnetic modes. These modes become more distinct with increasing vacancy cluster size. This material is based upon work supported by the U.S. Department of Energy Office of Science Graduate Student Research (SCGSR) program.

Recombination dynamics in In{sub x}Ga{sub 1−x}N quantum wells—Contribution of excited subband recombination to carrier leakage

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

Schulz, T.; Markurt, T.; Albrecht, M.

2014-11-03

The recombination dynamics of In{sub x}Ga{sub 1−x}N single quantum wells are investigated. By comparing the photoluminescence (PL) decay spectra with simulated emission spectra obtained by a Schrödinger-Poisson approach, we give evidence that recombination from higher subbands contributes the emission of the quantum well at high excitation densities. This recombination path appears as a shoulder on the high energy side of the spectrum at high charge carrier densities and exhibits decay in the range of ps. Due to the lower confinement of the excited subband states, a distinct proportion of the probability density function lies outside the quantum well, thus contributingmore » to charge carrier loss. By estimating the current density in our time resolved PL experiments, we show that the onset of this loss mechanism occurs in the droop relevant regime above 20 A/cm{sup 2}.« less

Influence of primary fragment excitation energy and spin distributions on fission observables

NASA Astrophysics Data System (ADS)

Litaize, Olivier; Thulliez, Loïc; Serot, Olivier; Chebboubi, Abdelaziz; Tamagno, Pierre

2018-03-01

Fission observables in the case of 252Cf(sf) are investigated by exploring several models involved in the excitation energy sharing and spin-parity assignment between primary fission fragments. In a first step the parameters used in the FIFRELIN Monte Carlo code "reference route" are presented: two parameters for the mass dependent temperature ratio law and two constant spin cut-off parameters for light and heavy fragment groups respectively. These parameters determine the initial fragment entry zone in excitation energy and spin-parity (E*, Jπ). They are chosen to reproduce the light and heavy average prompt neutron multiplicities. When these target observables are achieved all other fission observables can be predicted. We show here the influence of input parameters on the saw-tooth curve and we discuss the influence of a mass and energy-dependent spin cut-off model on gamma-rays related fission observables. The part of the model involving level densities, neutron transmission coefficients or photon strength functions remains unchanged.

Absorption and emission spectra of Li atoms trapped in rare gas matrices

NASA Astrophysics Data System (ADS)

Wright, J. J.; Balling, L. C.

1980-10-01

Pulsed-dye-laser excitation has been used to investigate the optical absorption and emission spectra of Li atoms trapped in Ar, Kr, and Xe matrices at 10 °K. Attempts to stabilize Li atoms in a Ne matrix at 2 °K were unsuccessful. Results for all three rare gases were qualitatively the same. White light absorption scans showed a single absorption with three peaks centered near the free-atom 2s→2p transition wavelength. The intensity of fluorescence produced by dye-laser excitation within this absorption band was measured as a function of emission wavelength. Excitation of the longest- and shortest-wavelength absorption peaks produced identical emission profiles, but no distinct fluorescence signal was detected when the laser was tuned to the central absorption peaks, indicating that the apparent absorption triplet is actually the superposition of a singlet and a doublet absorption originating from two different trapping sites. No additional absorption bands were detected.

Transverse excitations in liquid Fe, Cu and Zn

NASA Astrophysics Data System (ADS)

Hosokawa, S.; Inui, M.; Kajihara, Y.; Tsutsui, S.; Baron, A. Q. R.

2015-05-01

Transverse acoustic (TA) excitation modes were observed in inelastic x-ray scattering spectra of liquid Fe, Cu and Zn. From the analysis of current correlation functions, we concluded that TA excitation modes can experimentally be detected through the quasi-TA branches in the longitudinal current correlation spectra in these liquid metals. The microscopic elastic constants are estimated and a characteristic difference from macroscopic polycrystalline value was found in Poisson's ratio of liquid Fe, which shows an extremely softer value of ∼0.38 compared with the macroscopic value of ∼0.275. The lifetime of the TA modes were determined to be ∼0.45 ps for liquid Fe and Cu and ∼0.55 ps for liquid Zn, reflecting different interatomic correlations between liquid transition metals and non-transition metals. The propagation length of the TA modes are ∼0.85 nm in all of liquid metals, corresponding to the size of icosahedral or similar size of cages formed instantaneously in these liquid metals.

Kinetics of plasma formation in sodium vapor excited by nanosecond resonant laser pulses

NASA Astrophysics Data System (ADS)

Mahmoud, M. A.; Gamal, Y. E. E.

2012-07-01

We have studied theoretically formation of molecular ion Na2 + and the atomic ion Na+ which are created in laser excited sodium vapor at the first resonance transition, 3S1/2-3P1/2. A set of rate equations, which describe the temporal variation of the electron energy distribution function (EEDF), the electron density, the population density of the excited states as well as the atomic Na+ and molecular ion Na2 +, are solved numerically. The calculations are carried out at different laser energy and different sodium atomic vapor densities. The numerical calculations of the EEDF show that a deviation from the Maxwellian distribution due to the superelastic collisions effect. In addition to the competition between associative ionization (3P-3P), associative ionization (3P-3D) and Molnar-Hornbeck ionization processes for producing Na2 +, the calculations have also shown that the atomic ions Na+ are formed through the Penning ionization and photoionization processes. These results are found to be consistent with the experimental observations.

Fluorescent properties of a hybrid cadmium sulfide-dendrimer nanocomposite and its quenching with nitromethane.

PubMed

Campos, Bruno B; Algarra, Manuel; Esteves da Silva, Joaquim C G

2010-01-01

A fluorescent hybrid cadmium sulphide quantum dots (QDs) dendrimer nanocomposite (DAB-CdS) synthesised in water and stable in aqueous solution is described. The dendrimer, DAB-G5 dendrimer (polypropylenimine tetrahexacontaamine) generation 5, a diaminobutene core with 64 amine terminal primary groups. The maximum of the excitation and emission spectra, Stokes' shift and the emission full width of half maximum of this nanocomposite are, respectively: 351, 535, 204 and 212 nm. The fluorescence time decay was complex and a four component decay time model originated a good fit (chi = 1.20) with the following lifetimes: tau (1) = 657 ps; tau (2) = 10.0 ns; tau (3) = 59.42 ns; and tau (4) = 265 ns. The fluorescence intensity of the nanocomposite is markedly quenched by the presence of nitromethane with a dynamic Stern-Volmer constant of 25 M(-1). The quenching profiles show that about 81% of the CdS QDs are located in the external layer of the dendrimer accessible to the quencher. PARAFAC analysis of the excitation emission matrices (EEM) acquired as function of the nitromethane concentration showed a trilinear data structure with only one linearly independent component describing the quenching which allows robust estimation of the excitation and emission spectra and of the quenching profiles. This water soluble and fluorescent nanocomposite shows a set of favourable properties to its use in sensor applications.

Circular dichroism and site-directed spin labeling reveal structural and dynamical features of high-pressure states of myoglobin

PubMed Central

Lerch, Michael T.; Horwitz, Joseph; McCoy, John; Hubbell, Wayne L.

2013-01-01

Excited states of proteins may play important roles in function, yet are difficult to study spectroscopically because of their sparse population. High hydrostatic pressure increases the equilibrium population of excited states, enabling their characterization [Akasaka K (2003) Biochemistry 42:10875–85]. High-pressure site-directed spin-labeling EPR (SDSL-EPR) was developed recently to map the site-specific structure and dynamics of excited states populated by pressure. To monitor global secondary structure content by circular dichroism (CD) at high pressure, a modified optical cell using a custom MgF2 window with a reduced aperture is introduced. Here, a combination of SDSL-EPR and CD is used to map reversible structural transitions in holomyoglobin and apomyoglobin (apoMb) as a function of applied pressure up to 2 kbar. CD shows that the high-pressure excited state of apoMb at pH 6 has helical content identical to that of native apoMb, but reversible changes reflecting the appearance of a conformational ensemble are observed by SDSL-EPR, suggesting a helical topology that fluctuates slowly on the EPR time scale. Although the high-pressure state of apoMb at pH 6 has been referred to as a molten globule, the data presented here reveal significant differences from the well-characterized pH 4.1 molten globule of apoMb. Pressure-populated states of both holomyoglobin and apoMb at pH 4.1 have significantly less helical structure, and for the latter, that may correspond to a transient folding intermediate. PMID:24248390

Excited state intramolecular proton transfer reaction of 4'-N,N-diethylamino-3-hydroxyflavone and solvation dynamics in room temperature ionic liquids studied by optical Kerr gate fluorescence measurement.

PubMed

Kimura, Yoshifumi; Fukuda, Masanori; Suda, Kayo; Terazima, Masahide

2010-09-16

Fluorescence dynamics of 4'-N,N-diethylamino-3-hydroxyflavone (DEAHF) and its methoxy derivative (DEAMF) in various room temperature ionic liquids (RTILs) have been studied mainly by an optical Kerr gate method. DEAMF showed a single band fluorescence whose peak shifted with time by the solvation dynamics. The averaged solvation time determined by the fluorescence peak shift was proportional to the viscosity of the solvent except for tetradecyltrihexylphosphonium bis(trifluoromethanesulfonyl)amide. The solvation times were consistent with reported values determined with different probe molecules. DEAHF showed dual fluorescence due to the normal and tautomer forms produced by the excited state intramolecular proton transfer (ESIPT), and the relative intensities were dependent on the time and the solvent cation or anion species. By using the information of the fluorescence spectrum of DEAMF, the fluorescence spectrum of DEAHF at each delay time after the photoexcitation was decomposed into the normal and the tautomer fluorescence components, respectively. The normal component showed a very fast decay simulated by a biexponential function (2-3 and 20-30 ps) with an additional slower decay component. The tautomer component showed a rise with the time constants corresponding to the faster decay of the normal form with an additional instantaneous rise. The faster dynamics of the normal and tautomer population changes were assigned to the ESIPT process, while the slower decay of the fluorescence was attributed to the population decay from the excited state through the radiative and nonradiative processes. The average ESIPT time was much faster than the averaged solvation time of RTILs. Basically, the ESIPT kinetics in RTILs is similar to those in conventional liquid solvents like acetonitrile (Chou et al. J. Phys. Chem. A 2005, 109, 3777). The faster ESIPT is interpreted in terms of the activation barrierless process from the Franck-Condon state before the solvation of the normal state in the electronic excited state. With the advance of the solvation in the excited state, the normal form becomes relatively more stable than the tautomer form, which makes the ESIPT become an activation process.

Potassium Channels in Peripheral Pain Pathways: Expression, Function and Therapeutic Potential

PubMed Central

Du, Xiaona; Gamper, Nikita

2013-01-01

Electrical excitation of peripheral somatosensory nerves is a first step in generation of most pain signals in mammalian nervous system. Such excitation is controlled by an intricate set of ion channels that are coordinated to produce a degree of excitation that is proportional to the strength of the external stimulation. However, in many disease states this coordination is disrupted resulting in deregulated peripheral excitability which, in turn, may underpin pathological pain states (i.e. migraine, neuralgia, neuropathic and inflammatory pains). One of the major groups of ion channels that are essential for controlling neuronal excitability is potassium channel family and, hereby, the focus of this review is on the K+ channels in peripheral pain pathways. The aim of the review is threefold. First, we will discuss current evidence for the expression and functional role of various K+ channels in peripheral nociceptive fibres. Second, we will consider a hypothesis suggesting that reduced functional activity of K+ channels within peripheral nociceptive pathways is a general feature of many types of pain. Third, we will evaluate the perspectives of pharmacological enhancement of K+ channels in nociceptive pathways as a strategy for new analgesic drug design. PMID:24396338

Chaotic sources of noise in machine acoustics

NASA Astrophysics Data System (ADS)

Moon, F. C., Prof.; Broschart, Dipl.-Ing. T.

1994-05-01

In this paper a model is posited for deterministic, random-like noise in machines with sliding rigid parts impacting linear continuous machine structures. Such problems occur in gear transmission systems. A mathematical model is proposed to explain the random-like structure-borne and air-borne noise from such systems when the input is a periodic deterministic excitation of the quasi-rigid impacting parts. An experimental study is presented which supports the model. A thin circular plate is impacted by a chaotically vibrating mass excited by a sinusoidal moving base. The results suggest that the plate vibrations might be predicted by replacing the chaotic vibrating mass with a probabilistic forcing function. Prechaotic vibrations of the impacting mass show classical period doubling phenomena.

Optical Excitation of Carbon Nanotubes Drives Localized Diazonium Reactions

PubMed Central

2016-01-01

Covalent chemistries have been widely used to modify carbon nanomaterials; however, they typically lack the precision and efficiency required to directly engineer their optical and electronic properties. Here, we show, for the first time, that visible light which is tuned into resonance with carbon nanotubes can be used to drive their functionalization by aryldiazonium salts. The optical excitation accelerates the reaction rate 154-fold (±13) and makes it possible to significantly improve the efficiency of covalent bonding to the sp2 carbon lattice. Control experiments suggest that the reaction is dominated by a localized photothermal effect. This light-driven reaction paves the way for precise nanochemistry that can directly tailor carbon nanomaterials at the optical and electronic levels. PMID:27588432

Using Time-Dependent Density Functional Theory to Probe the Nature of Donor-Acceptor Stenhouse Adduct Photochromes.

PubMed

Laurent, Adèle D; Medveď, Miroslav; Jacquemin, Denis

2016-06-17

We present the first theoretical investigation of a recently proposed class of photochromes, namely donor-acceptor Stenhouse adduct (DASA) switches [J. Am. Chem. Soc. 2014, 136, 8169-8172]. By using density functional theory and its time-dependent counterpart, we investigate the ground- and excited-state structures, electronic transition energies, and several properties of the two isomeric forms. In addition to demonstrating that the selected level of theory is able to reproduce the main experimental facts, we show that 1) the two forms of the DASA photochromes are close to isoenergetic; 2) the two isomers possess similar total dipole moments, in spite of their very different sizes; 3) both isomers have a zwitterionic nature; 4) the nature of the dipole-allowed electronic excited state is vastly different in the two forms; and 5) the specific band shape of the extended DASA can be reproduced by vibronic calculations. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Hadronic production of the P-wave excited B{sub c} states (B{sub cJ,L=1}*)

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

Chang, C.-H.; Institute of Theoretical Physics, Chinese Academy of Sciences, P.O. Box 2735, Beijing 100080; Wang, J.-X.

2004-12-01

Adopting the complete {alpha}{sub s}{sup 4} approach of the perturbative QCD and the updated parton distribution functions, we have estimated the hadronic production of the P-wave excited B{sub c} states (B{sub cJ,L=1}*). In the estimate, special care has been paid to the dependence of the production amplitude on the derivative of the wave function at origin which is obtained by the potential model. For experimental references, main theoretical uncertainties are discussed, and the total cross section as well as the distributions of the production with reasonable cuts at the energies of Tevatron and CERN LHC are computed and presented properly.more » The results show that the P-wave production may contribute to the B{sub c}-meson production indirectly by a factor of about 0.5 of the direct production, and according to the estimated cross section, it is further worthwhile to study the possibility of observing the P-wave production itself experimentally.« less

Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements.

PubMed

Heilpern, Tal; Manjare, Manoj; Govorov, Alexander O; Wiederrecht, Gary P; Gray, Stephen K; Harutyunyan, Hayk

2018-05-10

Developing a fundamental understanding of ultrafast non-thermal processes in metallic nanosystems will lead to applications in photodetection, photochemistry and photonic circuitry. Typically, non-thermal and thermal carrier populations in plasmonic systems are inferred either by making assumptions about the functional form of the initial energy distribution or using indirect sensors like localized plasmon frequency shifts. Here we directly determine non-thermal and thermal distributions and dynamics in thin films by applying a double inversion procedure to optical pump-probe data that relates the reflectivity changes around Fermi energy to the changes in the dielectric function and in the single-electron energy band occupancies. When applied to normal incidence measurements our method uncovers the ultrafast excitation of a non-Fermi-Dirac distribution and its subsequent thermalization dynamics. Furthermore, when applied to the Kretschmann configuration, we show that the excitation of propagating plasmons leads to a broader energy distribution of electrons due to the enhanced Landau damping.

Electron beam-generated Ar/N{sub 2} plasmas: The effect of nitrogen addition on the brightest argon emission lines

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

Lock, E. H., E-mail: evgeniya.lock@nrl.navy.mil, E-mail: scott.walton@nrl.navy.mil; Petrova, Tz. B.; Petrov, G. M.

2016-04-15

The effect of nitrogen addition on the emission intensities of the brightest argon lines produced in a low pressure argon/nitrogen electron beam-generated plasmas is characterized using optical emission spectroscopy. In particular, a decrease in the intensities of the 811.5 nm and 763.5 nm lines is observed, while the intensity of the 750.4 nm line remains unchanged as nitrogen is added. To explain this phenomenon, a non-equilibrium collisional-radiative model is developed and used to compute the population of argon excited states and line intensities as a function of gas composition. The results show that the addition of nitrogen to argon modifies the electron energymore » distribution function, reduces the electron temperature, and depopulates Ar metastables in exchange reactions with electrons and N{sub 2} molecules, all of which lead to changes in argon excited states population and thus the emission originating from the Ar 4p levels.« less

Menthol Enhances Nicotine Reward-Related Behavior by Potentiating Nicotine-Induced Changes in nAChR Function, nAChR Upregulation, and DA Neuron Excitability.

PubMed

Henderson, Brandon J; Wall, Teagan R; Henley, Beverley M; Kim, Charlene H; McKinney, Sheri; Lester, Henry A

2017-11-01

Understanding why the quit rate among smokers of menthol cigarettes is lower than non-menthol smokers requires identifying the neurons that are altered by nicotine, menthol, and acetylcholine. Dopaminergic (DA) neurons in the ventral tegmental area (VTA) mediate the positive reinforcing effects of nicotine. Using mouse models, we show that menthol enhances nicotine-induced changes in nicotinic acetylcholine receptors (nAChRs) expressed on midbrain DA neurons. Menthol plus nicotine upregulates nAChR number and function on midbrain DA neurons more than nicotine alone. Menthol also enhances nicotine-induced changes in DA neuron excitability. In a conditioned place preference (CPP) assay, we observed that menthol plus nicotine produces greater reward-related behavior than nicotine alone. Our results connect changes in midbrain DA neurons to menthol-induced enhancements of nicotine reward-related behavior and may help explain how smokers of menthol cigarettes exhibit reduced cessation rates.

Thermally activated delayed photoluminescence from pyrenyl-functionalized CdSe quantum dots

NASA Astrophysics Data System (ADS)

Mongin, Cédric; Moroz, Pavel; Zamkov, Mikhail; Castellano, Felix N.

2018-02-01

The generation and transfer of triplet excitons across semiconductor nanomaterial-molecular interfaces will play an important role in emerging photonic and optoelectronic technologies, and understanding the rules that govern such phenomena is essential. The ability to cooperatively merge the photophysical properties of semiconductor quantum dots with those of well-understood and inexpensive molecular chromophores is therefore paramount. Here we show that 1-pyrenecarboxylic acid-functionalized CdSe quantum dots undergo thermally activated delayed photoluminescence. This phenomenon results from a near quantitative triplet-triplet energy transfer from the nanocrystals to 1-pyrenecarboxylic acid, producing a molecular triplet-state 'reservoir' that thermally repopulates the photoluminescent state of CdSe through endothermic reverse triplet-triplet energy transfer. The photoluminescence properties are systematically and predictably tuned through variation of the quantum dot-molecule energy gap, temperature and the triplet-excited-state lifetime of the molecular adsorbate. The concepts developed are likely to be applicable to semiconductor nanocrystals interfaced with molecular chromophores, enabling potential applications of their combined excited states.

Dynamics of the quantum search and quench-induced first-order phase transitions.

PubMed

Coulamy, Ivan B; Saguia, Andreia; Sarandy, Marcelo S

2017-02-01

We investigate the excitation dynamics at a first-order quantum phase transition (QPT). More specifically, we consider the quench-induced QPT in the quantum search algorithm, which aims at finding out a marked element in an unstructured list. We begin by deriving the exact dynamics of the model, which is shown to obey a Riccati differential equation. Then, we discuss the probabilities of success by adopting either global or local adiabaticity strategies. Moreover, we determine the disturbance of the quantum criticality as a function of the system size. In particular, we show that the critical point exponentially converges to its thermodynamic limit even in a fast evolution regime, which is characterized by both entanglement QPT estimators and the Schmidt gap. The excitation pattern is manifested in terms of quantum domain walls separated by kinks. The kink density is then shown to follow an exponential scaling as a function of the evolution speed, which can be interpreted as a Kibble-Zurek mechanism for first-order QPTs.

Serotonergic neurons signal reward and punishment on multiple timescales

PubMed Central

Cohen, Jeremiah Y; Amoroso, Mackenzie W; Uchida, Naoshige

2015-01-01

Serotonin's function in the brain is unclear. One challenge in testing the numerous hypotheses about serotonin's function has been observing the activity of identified serotonergic neurons in animals engaged in behavioral tasks. We recorded the activity of dorsal raphe neurons while mice experienced a task in which rewards and punishments varied across blocks of trials. We ‘tagged’ serotonergic neurons with the light-sensitive protein channelrhodopsin-2 and identified them based on their responses to light. We found three main features of serotonergic neuron activity: (1) a large fraction of serotonergic neurons modulated their tonic firing rates over the course of minutes during reward vs punishment blocks; (2) most were phasically excited by punishments; and (3) a subset was phasically excited by reward-predicting cues. By contrast, dopaminergic neurons did not show firing rate changes across blocks of trials. These results suggest that serotonergic neurons signal information about reward and punishment on multiple timescales. DOI: http://dx.doi.org/10.7554/eLife.06346.001 PMID:25714923

Menthol Enhances Nicotine Reward-Related Behavior by Potentiating Nicotine-Induced Changes in nAChR Function, nAChR Upregulation, and DA Neuron Excitability

PubMed Central

Henderson, Brandon J; Wall, Teagan R; Henley, Beverley M; Kim, Charlene H; McKinney, Sheri; Lester, Henry A

2017-01-01

Understanding why the quit rate among smokers of menthol cigarettes is lower than non-menthol smokers requires identifying the neurons that are altered by nicotine, menthol, and acetylcholine. Dopaminergic (DA) neurons in the ventral tegmental area (VTA) mediate the positive reinforcing effects of nicotine. Using mouse models, we show that menthol enhances nicotine-induced changes in nicotinic acetylcholine receptors (nAChRs) expressed on midbrain DA neurons. Menthol plus nicotine upregulates nAChR number and function on midbrain DA neurons more than nicotine alone. Menthol also enhances nicotine-induced changes in DA neuron excitability. In a conditioned place preference (CPP) assay, we observed that menthol plus nicotine produces greater reward-related behavior than nicotine alone. Our results connect changes in midbrain DA neurons to menthol-induced enhancements of nicotine reward-related behavior and may help explain how smokers of menthol cigarettes exhibit reduced cessation rates. PMID:28401925

Dynamical analysis of relaxation luminescence in ZnS:Er3+ thin film devices

NASA Astrophysics Data System (ADS)

Wang, Yu-Jiang; Wu, Chen-Xu; Chen, Mou-Zhi; Huang, Mei-Chun

2003-06-01

The relaxation luminescence of ZnS:Er3+ thin film devices fabricated by thermal evaporation with two boats is studied. The dynamical processes of the luminescence of Er3+ in ZnS are described in terms of a resonant energy transfer model, assuming that the probability of collision excitation of injected electrons with luminescence centers is expressed as a Gaussian function. It is found that the frequency distribution depends on the Lorentzian function by considering the emission from excited states as a damped oscillator. Taking into consideration the energy storing effect of traps, an expression is obtained to describe a profile that contains multiple relaxation luminescence peaks using the convolution theorem. Fitting of experimental results shows that the relaxation characteristics of the electroluminescence are related to the carriers captured by bulk traps as well as by interface states. The numerical calculation carried out agrees well with the dynamical characteristics of relaxation luminescence obtained by experiments.

Two-photon interference and coherent control of single InAs quantum dot emissions in an Ag-embedded structure

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

Liu, X., E-mail: iu.xiangming@nims.go.jp; National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044; Kumano, H.

2014-07-28

We have recently reported the successful fabrication of bright single-photon sources based on Ag-embedded nanocone structures that incorporate InAs quantum dots. The source had a photon collection efficiency as high as 24.6%. Here, we show the results of various types of photonic characterizations of the Ag-embedded nanocone structures that confirm their versatility as regards a broad range of quantum optical applications. We measure the first-order autocorrelation function to evaluate the coherence time of emitted photons, and the second-order correlation function, which reveals the strong suppression of multiple photon generation. The high indistinguishability of emitted photons is shown by the Hong-Ou-Mandel-typemore » two-photon interference. With quasi-resonant excitation, coherent population flopping is demonstrated through Rabi oscillations. Extremely high single-photon purity with a g{sup (2)}(0) value of 0.008 is achieved with π-pulse quasi-resonant excitation.« less

Nonadiabatic Molecular Dynamics and Orthogonality Constrained Density Functional Theory

NASA Astrophysics Data System (ADS)

Shushkov, Philip Georgiev

The exact quantum dynamics of realistic, multidimensional systems remains a formidable computational challenge. In many chemical processes, however, quantum effects such as tunneling, zero-point energy quantization, and nonadiabatic transitions play an important role. Therefore, approximate approaches that improve on the classical mechanical framework are of special practical interest. We propose a novel ring polymer surface hopping method for the calculation of chemical rate constants. The method blends two approaches, namely ring polymer molecular dynamics that accounts for tunneling and zero-point energy quantization, and surface hopping that incorporates nonadiabatic transitions. We test the method against exact quantum mechanical calculations for a one-dimensional, two-state model system. The method reproduces quite accurately the tunneling contribution to the rate and the distribution of reactants between the electronic states for this model system. Semiclassical instanton theory, an approach related to ring polymer molecular dynamics, accounts for tunneling by the use of periodic classical trajectories on the inverted potential energy surface. We study a model of electron transfer in solution, a chemical process where nonadiabatic events are prominent. By representing the tunneling electron with a ring polymer, we derive Marcus theory of electron transfer from semiclassical instanton theory after a careful analysis of the tunneling mode. We demonstrate that semiclassical instanton theory can recover the limit of Fermi's Golden Rule rate in a low-temperature, deep-tunneling regime. Mixed quantum-classical dynamics treats a few important degrees of freedom quantum mechanically, while classical mechanics describes affordably the rest of the system. But the interface of quantum and classical description is a challenging theoretical problem, especially for low-energy chemical processes. We therefore focus on the semiclassical limit of the coupled nuclear-electronic dynamics. We show that the time-dependent Schrodinger equation for the electrons employed in the widely used fewest switches surface hopping method is applicable only in the limit of nearly identical classical trajectories on the different potential energy surfaces. We propose a short-time decoupling algorithm that restricts the use of the Schrodinger equation only to the interaction regions. We test the short-time approximation on three model systems against exact quantum-mechanical calculations. The approximation improves the performance of the surface hopping approach. Nonadiabatic molecular dynamics simulations require the efficient and accurate computation of ground and excited state potential energy surfaces. Unlike the ground state calculations where standard methods exist, the computation of excited state properties is a challenging task. We employ time-independent density functional theory, in which the excited state energy is represented as a functional of the total density. We suggest an adiabatic-like approximation that simplifies the excited state exchange-correlation functional. We also derive a set of minimal conditions to impose exactly the orthogonality of the excited state Kohn-Sham determinant to the ground state determinant. This leads to an efficient, variational algorithm for the self-consistent optimization of the excited state energy. Finally, we assess the quality of the excitation energies obtained by the new method on a set of 28 organic molecules. The new approach provides results of similar accuracy to time-dependent density functional theory.

Excited state absorption spectra of dissolved and aggregated distyrylbenzene: A TD-DFT state and vibronic analysis

NASA Astrophysics Data System (ADS)

Oliveira, Eliezer Fernando; Shi, Junqing; Lavarda, Francisco Carlos; Lüer, Larry; Milián-Medina, Begoña; Gierschner, Johannes

2017-07-01

A time-dependent density functional theory study is performed to reveal the excited state absorption (ESA) features of distyrylbenzene (DSB), a prototype π-conjugated organic oligomer. Starting with a didactic insight to ESA based on simple molecular orbital and configuration considerations, the performance of various density functional theory functionals is tested to reveal the full vibronic ESA features of DSB at short and long probe delay times.

Analytical second derivatives of excited-state energy within the time-dependent density functional theory coupled with a conductor-like polarizable continuum model.

PubMed

Liu, Jie; Liang, WanZhen

2013-01-14

This work extends our previous works [J. Liu and W. Z. Liang, J. Chem. Phys. 135, 014113 (2011); J. Liu and W. Z. Liang, J. Chem. Phys. 135, 184111 (2011)] on analytical excited-state Hessian within the framework of time-dependent density functional theory (TDDFT) to couple with a conductor-like polarizable continuum model (CPCM). The formalism, implementation, and application of analytical first and second energy derivatives of TDDFT/CPCM excited state with respect to the nuclear and electric perturbations are presented. Their performances are demonstrated by the calculations of excitation energies, excited-state geometries, and harmonic vibrational frequencies for a number of benchmark systems. The calculated results are in good agreement with the corresponding experimental data or other theoretical calculations, indicating the reliability of the current computer implementation of the developed algorithms. Then we made some preliminary applications to calculate the resonant Raman spectrum of 4-hydroxybenzylidene-2,3-dimethyl-imidazolinone in ethanol solution and the infrared spectra of ground and excited states of 9-fluorenone in methanol solution.

Ab initio calculation of the electronic structures of the (7)Sigma+ ground and A (7)Pi and a (5)Sigma+ excited states of MnH.

PubMed

Tomonari, Mutsumi; Nagashima, Umpei; Hirano, Tsuneo

2009-04-21

Electronic structures and molecular constants of the ground (7)Sigma(+) and low-lying A (7)Pi and a (5)Sigma(+) electronic excited states of the MnH molecule were studied by multireference single and double excitation configuration interaction (MR-SDCI) with Davidson's correction (+Q) calculations under exact C(infinity v) symmetry using Slater-type basis sets. To correctly describe the (7)Sigma(+) electronic ground state, X (7)Sigma(+), at the MR-SDCI+Q calculation, we employed a large number of reference configurations in terms of the state-averaged complete active space self-consistent field (CASSCF) orbitals, taking into account the contribution from the B (7)Sigma(+) excited state. The A (7)Pi and a (5)Sigma(+) states can well be described by the MR-SDCI wave functions based on the CASSCF orbitals obtained for the lowest state only. In the MR-SDCI+Q, calculations of the X (7)Sigma(+), A (7)Pi, and a (5)Sigma(+) states required 16, 7, and 17 reference configurations, respectively. Molecular constants, i.e., r(e) and omega(e) of these states and excitation energy from the X (7)Sigma(+) state, obtained at the MR-SDCI+Q level, showed a good agreement with experimental values. The small remaining differences may be accounted for by taking relativistic effects into account.

Ab initio calculation of the electronic structures of the 7∑+ ground and A 7Π and a 5∑+ excited states of MnH

NASA Astrophysics Data System (ADS)

Tomonari, Mutsumi; Nagashima, Umpei; Hirano, Tsuneo

2009-04-01

Electronic structures and molecular constants of the ground ∑7+ and low-lying A 7Π and a ∑5+ electronic excited states of the MnH molecule were studied by multireference single and double excitation configuration interaction (MR-SDCI) with Davidson's correction (+Q) calculations under exact C∞v symmetry using Slater-type basis sets. To correctly describe the ∑7+ electronic ground state, X ∑7+, at the MR-SDCI+Q calculation, we employed a large number of reference configurations in terms of the state-averaged complete active space self-consistent field (CASSCF) orbitals, taking into account the contribution from the B ∑7+ excited state. The A 7Π and a ∑5+ states can well be described by the MR-SDCI wave functions based on the CASSCF orbitals obtained for the lowest state only. In the MR-SDCI+Q, calculations of the X ∑7+, A 7Π, and a ∑5+ states required 16, 7, and 17 reference configurations, respectively. Molecular constants, i.e., re and ωe of these states and excitation energy from the X ∑7+ state, obtained at the MR-SDCI+Q level, showed a good agreement with experimental values. The small remaining differences may be accounted for by taking relativistic effects into account.

Three-Photon Luminescence of Gold Nanorods and Its Applications for High Contrast Tissue and Deep In Vivo Brain Imaging

PubMed Central

Wang, Shaowei; Xi, Wang; Cai, Fuhong; Zhao, Xinyuan; Xu, Zhengping; Qian, Jun; He, Sailing

2015-01-01

Gold nanoparticles can be used as contrast agents for bio-imaging applications. Here we studied multi-photon luminescence (MPL) of gold nanorods (GNRs), under the excitation of femtosecond (fs) lasers. GNRs functionalized with polyethylene glycol (PEG) molecules have high chemical and optical stability, and can be used as multi-photon luminescent nanoprobes for deep in vivo imaging of live animals. We have found that the depth of in vivo imaging is dependent upon the transmission and focal capability of the excitation light interacting with the GNRs. Our study focused on the comparison of MPL from GNRs with two different aspect ratios, as well as their ex vivo and in vivo imaging effects under 760 nm and 1000 nm excitation, respectively. Both of these wavelengths were located at an optically transparent window of biological tissue (700-1000 nm). PEGylated GNRs, which were intravenously injected into mice via the tail vein and accumulated in major organs and tumor tissue, showed high image contrast due to distinct three-photon luminescence (3PL) signals upon irradiation of a 1000 nm fs laser. Concerning in vivo mouse brain imaging, the 3PL imaging depth of GNRs under 1000 nm fs excitation could reach 600 μm, which was approximately 170 μm deeper than the two-photon luminescence (2PL) imaging depth of GNRs with a fs excitation of 760 nm. PMID:25553113

AKAP-scaffolding proteins and regulation of cardiac physiology

PubMed Central

Mauban, JRH; O'Donnell, M; Warrier, S; Manni, S; Bond, M

2009-01-01

A kinase anchoring proteins (AKAPs) compose a growing list of diverse but functionally related proteins defined by their ability to bind to the regulatory subunit of protein kinase A. AKAPs perform an integral role in the spatiotemporal modulation of a multitude of cellular signaling pathways. This review highlights the extensive role of AKAPs in cardiac excitation/contraction coupling and cardiac physiology. The literature shows that particular AKAPs are involved in cardiac Ca2+ influx, release, re-uptake, and myocyte repolarization. Studies have also suggested roles for AKAPs in cardiac remodeling. Transgenic studies show functional effects of AKAPs, not only in the cardiovascular system, but in other organ systems as well. PMID:19364910

Multiple-photon excitation of nitrogen vacancy centers in diamond

NASA Astrophysics Data System (ADS)

Ji, Peng; Balili, R.; Beaumariage, J.; Mukherjee, S.; Snoke, D.; Dutt, M. V. Gurudev

2018-04-01

We report the observation of multiphoton photoluminescence excitation (PLE) below the resonant energies of nitrogen vacancy (NV) centers in diamond. The quadratic and cubic dependence of the integrated fluorescence intensity as a function of excitation power indicates a two-photon excitation pathway for the NV- charge state and a three-photon process involved for the neutral NV0 charge state, respectively. Comparing the total multiphoton energy with its single-photon equivalent, the PLE spectra follows the absorption spectrum of single photon excitation. We also observed that the efficiency of photoluminescence for different charge states, as well as the decay time constant, was dependent on the excitation wavelength and power.

Solid-state radiation-emitting compositions and devices

DOEpatents

Ashley, Carol S.; Brinker, C. Jeffrey; Reed, Scott; Walko, Robert J.

1992-01-01

The invention relates to a composition for the volumetric generation of radiation, wherein a first substance functions as a source of exciting radiation, and a second substance interacts with the exciting radiation to provide a second radiation. The compositions comprise a porous substrate which is loaded with: a source of exciting radiation, a component capable of emitting radiation upon interaction with the exciting radiation, or both. Preferably, the composition is an aerogel substrate loaded with both a source of exciting radiation, such as tritium, and a component capable of interacting with the exciting radiation, e.g., a phosphor, to produce radiation of a second energy.

Solid-state radiation-emitting compositions and devices

DOEpatents

Ashley, C.S.; Brinker, C.J.; Reed, S.; Walko, R.J.

1992-08-11

The invention relates to a composition for the volumetric generation of radiation, wherein a first substance functions as a source of exciting radiation, and a second substance interacts with the exciting radiation to provide a second radiation. The compositions comprise a porous substrate which is loaded with: a source of exciting radiation, a component capable of emitting radiation upon interaction with the exciting radiation, or both. Preferably, the composition is an aerogel substrate loaded with both a source of exciting radiation, such as tritium, and a component capable of interacting with the exciting radiation, e.g., a phosphor, to produce radiation of a second energy. 4 figs.

Condensates of p-wave pairs are exact solutions for rotating two-component Bose gases.

PubMed

Papenbrock, T; Reimann, S M; Kavoulakis, G M

2012-02-17

We derive exact analytical results for the wave functions and energies of harmonically trapped two-component Bose-Einstein condensates with weakly repulsive interactions under rotation. The isospin symmetric wave functions are universal and do not depend on the matrix elements of the two-body interaction. The comparison with the results from numerical diagonalization shows that the ground state and low-lying excitations consist of condensates of p-wave pairs for repulsive contact interactions, Coulomb interactions, and the repulsive interactions between aligned dipoles.

Vibrational excitation functions for inelastic and superelastic electron scattering from the ground-electronic state in hot CO2

NASA Astrophysics Data System (ADS)

Kato, H.; Kawahara, H.; Hoshino, M.; Tanaka, H.; Campbell, L.; Brunger, M. J.

2008-11-01

We report inelastic and superelastic excitation function measurements for electron scattering from the ground vibrational quantum (0 0 0), the bending vibrational quantum (0 1 0) and the unresolved first bending overtone (0 2 0) and symmetric stretch (1 0 0) modes of the ground-electronic state in hot (700 K) carbon dioxide ( CO) molecules. The incident electron energy range of these measurements was 1-9 eV, with the relevant excitation functions being measured at the respective electron scattering angles of 30°, 60°, 90° and 120°. Where possible comparison is made to the often quite limited earlier data, with satisfactory agreement typically being found to within the cited experimental errors.

Enhanced optical limiting effect in fluorine-functionalized graphene oxide

NASA Astrophysics Data System (ADS)

Zhang, Fang; Wang, Zhengping; Wang, Duanliang; Wang, Shenglai; Xu, Xinguang

2017-09-01

Nonlinear optical absorption of fluorine-functionalized graphene oxide (F-GO) solution was researched by the open-aperture Z-scan method using 1064 and 532 nm lasers as the excitation sources. The F-GO dispersion exhibited strong optical limiting property and the fitted results demonstrated that the optical limiting behavior was the result of a two-photon absorption process. For F-GO nanosheets, the two-photon absorption coefficients at 1064 nm excitation are 20% larger than the values at 532 nm excitation and four times larger than that of pure GO nanosheets. It indicates that the doping of fluorine can effectively improve the nonlinear optical property of GO especially in infrared waveband, and fluorine-functionalized graphene oxide is an excellent nonlinear absorption material in infrared waveband.

Targeting the Cerebellum by Noninvasive Neurostimulation: a Review.

PubMed

van Dun, Kim; Bodranghien, Florian; Manto, Mario; Mariën, Peter

2017-06-01

Transcranial magnetic and electric stimulation of the brain are novel and highly promising techniques currently employed in both research and clinical practice. Improving or rehabilitating brain functions by modulating excitability with these noninvasive tools is an exciting new area in neuroscience. Since the cerebellum is closely connected with the cerebral regions subserving motor, associative, and affective functions, the cerebello-thalamo-cortical pathways are an interesting target for these new techniques. Targeting the cerebellum represents a novel way to modulate the excitability of remote cortical regions and their functions. This review brings together the studies that have applied cerebellar stimulation, magnetic and electric, and presents an overview of the current knowledge and unsolved issues. Some recommendations for future research are implemented as well.

Excitation Functions of Helion-Induced Nuclear Reactions for the Production of the Medical Radioisotope 103Pd

NASA Astrophysics Data System (ADS)

Skakun, Ye.; Qaim, S. M.

2005-05-01

Excitation functions were measured by the stacked-foil technique for the reactions 100Ru(α,n)103Pd, 101Ru(α,2n)103Pd, 101Ru(3He,n)103Pd, and 102Ru(3He,2n)103Pd for incident energies up to 25 and 34 MeV for α-particles and 3He ions, respectively. The integral thick target yields of the product radionuclide 103Pd calculated from the excitation functions of the above-named four reactions amount to 960, 1050, 50, and 725 KBq/μAh, respectively, at the maximum energy of the incident particle. The data are compared with the results of statistical model calculations and other charged particle induced reaction investigations.

Engineering biosynthetic excitable tissues from unexcitable cells for electrophysiological and cell therapy studies

PubMed Central

Kirkton, Robert D.; Bursac, Nenad

2012-01-01

Patch-clamp recordings in single-cell expression systems have been traditionally used to study the function of ion channels. However, this experimental setting does not enable assessment of tissue-level function such as action potential (AP) conduction. Here we introduce a biosynthetic system that permits studies of both channel activity in single cells and electrical conduction in multicellular networks. We convert unexcitable somatic cells into an autonomous source of electrically excitable and conducting cells by stably expressing only three membrane channels. The specific roles that these expressed channels have on AP shape and conduction are revealed by different pharmacological and pacing protocols. Furthermore, we demonstrate that biosynthetic excitable cells and tissues can repair large conduction defects within primary 2- and 3-dimensional cardiac cell cultures. This approach enables novel studies of ion channel function in a reproducible tissue-level setting and may stimulate the development of new cell-based therapies for excitable tissue repair. PMID:21556054

Photophysical properties of blue – emitting silicon nanoparticles

PubMed Central

Portolés, Manuel J. Llansola; Nieto, Felipe Rodriguez; Soria, Delia B.; Amalvy, Javier I.; Peruzzo, Pablo J.; Mártire, Daniel O.; Kotler, Mónica; Holub, Oliver; Gonzalez, Mónica C.

2012-01-01

Silicon nanoparticles with strong blue photoluminescence were synthesized by electrochemical etching of silicon wafers and ultrasonically removed under N2 atmosphere in organic solvents to produce colloids. Thermal treatment leads to the formation of colloidal Si particles of 3 ± 1 nm diameter, which upon excitation with 340 – 380 nm light exhibited room temperature luminescence in the range from 400 to 500 nm. The emission and the one- and two-photon excitation spectra of the particles are not sensitive to surface functionalization with methyl 2-methylprop-2-enoate. However, the derivatized particles show higher emission quantum yields in air-saturated suspensions (44%) than the underivatized particles (27%), as well as higher stability of its dispersions. FTIR and XPS spectra indicate a significant surface oxidation of the particles. The Si:O:C ratio at the surface of the derivatized particles estimated from XPS is Si3O6(C5O2Hy)1, with y = 7 - 8. Vibronic spacing is observed in both the emission and excitation spectra. The information obtained from one-photon excitation experiments (emission and excitation spectra, photoluminescence quantum yields, luminescence decay lifetimes and anisotropy correlation lifetimes), as well as from two-photon excitation fluorescence correlation spectroscopy (brightness and diffusion coefficients) and TEM indicate that the blue-emitting particles are monodisperse and ball-shaped. Particle size clearly determines the emission and excitation spectral region, as expected from quantum confinement, but the presence and extent of Si-O species on the silicon networks seem crucial for determining the spectrum features and intensity of emission. The nanoparticles could hold great potential as quantum dots for applications as luminescence sensors in biology and environmental science. PMID:22866180

Ab initio study of excited state electronic circular dichroism. Two prototype cases: methyl oxirane and R-(+)-1,1'-bi(2-naphthol).

PubMed

Rizzo, Antonio; Vahtras, Olav

2011-06-28

A computational approach to the calculation of excited state electronic circular dichroism (ESECD) spectra of chiral molecules is discussed. Frequency dependent quadratic response theory is employed to compute the rotatory strength for transitions between excited electronic states, by employing both a magnetic gauge dependent and a (velocity-based) magnetic gauge independent approach. Application is made to the lowest excited states of two prototypical chiral molecules, propylene oxide, also known as 1,2-epoxypropane or methyl oxirane, and R-(+)-1,1'-bi(2-naphthol), or BINOL. The dependence of the rotatory strength for transitions between the lowest three excited states of methyl oxirane upon the quality and extension of the basis set is analyzed, by employing a hierarchy of correlation consistent basis sets. Once established that basis sets of at least triple zeta quality, and at least doubly augmented, are sufficient to ensure sufficiently converged results, at least at the Hartree-Fock self-consistent field (HF-SCF) level, the rotatory strengths for all transitions between the lowest excited electronic states of methyl oxirane are computed and analyzed, employing HF-SCF, and density functional theory (DFT) electronic structure models. For DFT, both the popular B3LYP and its recently highly successful CAM-B3LYP extension are exploited. The strong dependence of the spectra upon electron correlation is highlighted. A HF-SCF and DFT study is carried out also for BINOL, a system where excited states show the typical pairing structure arising from the interaction of the two monomeric moieties, and whose conformational changes following photoexcitation were studied recently with via time-resolved CD.

Excitation spectra of aromatic molecules within a real-space G W -BSE formalism: Role of self-consistency and vertex corrections

DOE PAGES

Hung, Linda; da Jornada, Felipe H.; Souto-Casares, Jaime; ...

2016-08-15

Here, we present first-principles calculations on the vertical ionization potentials (IPs), electron affinities (EAs), and singlet excitation energies on an aromatic-molecule test set (benzene, thiophene, 1,2,5-thiadiazole, naphthalene, benzothiazole, and tetrathiafulvalene) within the GW and Bethe-Salpeter equation (BSE) formalisms. Our computational framework, which employs a real-space basis for ground-state and a transition-space basis for excited-state calculations, is well suited for high-accuracy calculations on molecules, as we show by comparing against G0W0 calculations within a plane-wave-basis formalism. We then generalize our framework to test variants of the GW approximation that include a local density approximation (LDA)–derived vertex function (Γ LDA ) andmore » quasiparticle-self-consistent (QS) iterations. We find that Γ LDA and quasiparticle self-consistency shift IPs and EAs by roughly the same magnitude, but with opposite sign for IPs and the same sign for EAs. G0W0 and QS GWΓ LDA are more accurate for IPs, while G 0W 0Γ LDA and QS GW are best for EAs. For optical excitations, we find that perturbative GW-BSE underestimates the singlet excitation energy, while self-consistent GW-BSE results in good agreement with previous best-estimate values for both valence and Rydberg excitations. Finally, our work suggests that a hybrid approach, in which G0W0 energies are used for occupied orbitals and G0W0Γ LDA for unoccupied orbitals, also yields optical excitation energies in good agreement with experiment but at a smaller computational cost.« less