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Sample records for electronic excitation effect

  1. Effect of electron excitation on radiation damage in fce metals

    NASA Astrophysics Data System (ADS)

    Iwase, A.; Iwata, T.

    1994-05-01

    Defect production, radiation annealing and defect recovery are studied in several fcc metals (Al, Cu, Ni, Ag and Pt) irradiated with low-energy (˜ 1 MeV) and high-energy (˜ 100 MeV) ions. Irradiation of the metals with strong electron-lattice interaction (Al, Ni and Pt) by ˜ 100 MeV ions causes an anomalous reduction, or even a complete disappearance of stage-I recovery. This experimental result shows that the energy transferred from excited electrons to lattice atoms through the electron-lattice interaction contributes to the annihilation of single interstitials. This effect is also observed in Ni as a large cross section for radiation annealing, and a decrease of the damage efficiency. On the other hand, in Cu and Ag thin foils, we find that lattice defects are produced not only through elastic interactions, but also through a process strongly associated with electron excitation. In the latter process, the defect production cross section is proportional to Se1.7 in Cu and Se1.5 in Ag. The nearly quadratic dependence of the cross section on Se suggests that the mutual Coulomb repulsion of ions positively charged by electron excitation causes the defect production.

  2. Different effects of electronic excitation on metals and semiconductors

    NASA Astrophysics Data System (ADS)

    Yan, Gai-Qin; Cheng, Xin-Lu; Zhang, Hong; Zhu, Zhi-Yang; Ren, Da-Hua

    2016-06-01

    We study the electronic excitation effect upon ultrafast and intense laser irradiation on the stability of target materials, using density functional perturbation theory. The target materials include metals (Li, Na, Mg, Al, K, W, Au), Bi as a semimetal, and Si as a semiconductor. We found that the electronic excitation had different effects on the two distinct materials. For metals, the electronic pressure induces an increase in the shear modulus and presents a negative effect on the phonon entropy, which increases the lattice vibration frequency and melting temperature, leading to a higher stability for the close-packed structure (Al, Au, Mg). Conversely, the electronic pressure induces a decreasing trend in all these quantities, leading to a lower degree of stability and even a structural destabilization in the case of bcc-structured metals (W, Na, K, and Li). For semimetals and semiconductors, the internal pressure induces a completely opposite behavior with respect to close-packed structure metals. This can lead to structural destabilization for semimetals and even collapse for semiconductors. Finally, a shift of the Raman and infrared active modes is revealed for semimetals and semiconductors.

  3. Effect of Electronic Excitation on Thin Film Growth

    SciTech Connect

    Elsayed-Ali, Hani E.

    2011-01-31

    The effect of nanosecond pulsed laser excitation on surface diffusion during growth of Ge on Si(100) at 250 degrees C was studied. In Situ reflection high-energy electron diffraction (RHEED) was used to measure the surface diffusion coefficient while ex situ atomic force microscopy (AFM) was used to probe the structure and morphology of the grown quantum dots. The results show that laser excitation of the substrate increases the surface diffusion during growth of Ge on Si(100), changes the growth morphology, improves crystalline structure of the grown quantum dots, and decreases their size distribution. A purely electronic mechanism of enhanced surface diffusion of the deposited Ge is proposed. Ge quantum dots were grown on Si(100)-(2x1) by pulsed laser deposition at various substrate temperatures using a femtosecond Ti:sapphire laser. In-situ reflection high-energy electron diffraction and ex-situ atomic force microscopy were used to analyze the fim structure and morphology. The morphology of germanium islands on silicon was studied at differect coverages. The results show that femtosecond pulsed laser depositon reduces the minimum temperature for epitaxial growth of Ge quantum dots to ~280 degrees C, which is 120 degrees C lower then previously observed in nanosecond pulsed laser deposition and more than 200 degrees C lower than that reported for molecular beam epitaxy and chemical vapor deposition.

  4. Solvent Effects on Electronic Excitations of an Organic Chromophore.

    PubMed

    Zuehlsdorff, T J; Haynes, P D; Hanke, F; Payne, M C; Hine, N D M

    2016-04-12

    In this work we study the solvatochromic shift of a selected low-energy excited state of alizarin in water by using a linear-scaling implementation of large-scale time-dependent density functional theory (TDDFT). While alizarin, a small organic dye, is chosen as a simple example of solute-solvent interactions, the findings presented here have wider ramifications for the realistic modeling of dyes, paints, and pigment-protein complexes. We find that about 380 molecules of explicit water need to be considered in order to yield an accurate representation of the solute-solvent interaction and a reliable solvatochromic shift. By using a novel method of constraining the TDDFT excitation vector, we confirm that the origin of the slow convergence of the solvatochromic shift with system size is due to two different effects. The first factor is a strong redshift of the excitation due to an explicit delocalization of a small fraction of the electron and the hole from the alizarin onto the water, which is mainly confined to within a distance of 7 Å from the alizarin molecule. The second factor can be identified as long-range electrostatic influences of water molecules beyond the 7 Å region on the ground-state properties of alizarin. We also show that these electrostatic influences are not well reproduced by a QM/MM model, suggesting that full QM studies of relatively large systems may be necessary in order to obtain reliable results. PMID:26967019

  5. Vibronic effects on the low-lying electronic excitations in N2O induced by electron impact

    NASA Astrophysics Data System (ADS)

    Watanabe, Noboru; Takahashi, Masahiko

    2014-08-01

    We report a theoretical study on the valence-shell electronic excitations of N2O induced by electron impact. Momentum transfer-dependent generalized oscillator strengths (GOSs) or GOS profiles have been calculated for the low-lying electronic excitations using theoretical wave functions at the equation-of-motion coupled-cluster singles and doubles level. In the calculation, Herzberg-Teller vibronic effects are taken into account. The computed results are in overall agreement with experimental GOS profiles reported in the literature and reveal prominent roles of the bending vibration of N2O in the B1Δ and C1Π transitions.

  6. Free electron degeneracy effects on collisional excitation, ionization, de-excitation and three-body recombination

    NASA Astrophysics Data System (ADS)

    Tallents, G. J.

    2016-09-01

    Collisional-radiative models enable average ionization and ionization populations, plus the rates of absorption and emission of radiation to be calculated for plasmas not in thermal equilbrium. At high densities and low temperatures, electrons may have a high occupancy of the free electron quantum states and evaluations of rate coefficients need to take into account the free electron degeneracy. We demonstrate that electron degeneracy can reduce collisional rate coefficients by orders-of-magnitude from values calculated neglecting degeneracy. We show that assumptions regarding the collisional differential cross-section can alter collisional ionization and recombination rate coefficients by a further factor two under conditions relevant to inertial fusion.

  7. Effects of Thermal Electronic Excitations on the Diffusion of Oxygen Adatoms on Graphene.

    PubMed

    Sun, Tao; Yao, Xinxin; Fabris, Stefano

    2016-05-01

    We conduct first-principles calculations to study oxygen diffusion on the graphene surface as a function of temperature up to 3000 K. The minimum energy migration path and the corresponding activation energy are determined by the nudged elastic band method with explicit inclusion of thermal electronic excitations. Below 1000 K the activation energy for epoxy oxygen to migrate remains close to its room temperature value (0.72 eV). Above 1000 K the activation energy decreases near linearly with temperature, from 0.70 eV at 1000 K to 0.47 eV at 3000 K. We show that this reduction originates from thermal electronic excitations. In particular, the effect is determined by the large contrasts in the electronic structures of the initial and transition states: the transition state exhibits much larger electronic density of states near the Fermi level and is more susceptible to thermal electronic excitations. The reduction in activation energy leads to appreciable enhancement in the diffusivity of oxygen adatoms. A moderate decrease in the vibrational prefactor, also caused by thermal electronic excitations, does not alter this trend. These findings may facilitate future works to accurately describe the dynamics of O adatoms on graphene at high T, which are critical for determining surface thermodynamic properties such as equilibrium coverage. PMID:27074529

  8. Plasma-screening effects on the electron-impact excitation of hydrogenic ions in dense plasmas

    NASA Technical Reports Server (NTRS)

    Jung, Young-Dae

    1993-01-01

    Plasma-screening effects are investigated on electron-impact excitation of hydrogenic ions in dense plasmas. Scaled cross sections Z(exp 4) sigma for 1s yields 2s and 1s yields 2p are obtained for a Debye-Hueckel model of the screened Coulomb interaction. Ground and excited bound wave functions are modified in the screened Coulomb potential (Debye-Hueckel model) using the Ritz variation method. The resulting atomic wave functions and their eigenenergies agree well with the numerical and high-order perturbation theory calculations for the interesting domain of the Debye length not less than 10. The Born approximation is used to describe the continuum states of the projectile electron. Plasma screening effects on the atomic electrons cannot be neglected in the high-density cases. Including these effects, the cross sections are appreciably increased for 1s yields 2s transitions and decreased for 1s yields 2p transitions.

  9. The effect of electron collisions on rotational excitation of cometary water

    NASA Technical Reports Server (NTRS)

    Xie, Xingfa; Mumma, Michael J.

    1991-01-01

    The e-H2O collisional rate for exciting rotational transitions in cometary water is evaluated for conditions found in Comet Halley. The e-H2O collisional rate exceeds that for excitation by neutral-neutral collisions at distances exceeding 3000 km from the cometary nucleus, in the case of the O sub 00 yields 1 sub 11 transition. The estimates are based on theoretical and experimental studies of e-H2O collisions, on ion and electron parameters acquired in-situ by instruments on the Giotto and Vega spacecraft, and on results obtained from models of the cometary ionosphere. The contribution of electron collisions may explain the need for large water-water cross-sections in models which neglect the effect of electrons. The importance of electron collisions is enhanced for populations of water molecules in regions where their rotational lines are optically thick.

  10. Distortion effects in electron excitation of hydrogen atoms by impact of heavy ions

    SciTech Connect

    Ramirez, C.A.; Rivarola, R.D.

    1995-12-01

    Electron excitation from the fundamental state of hydrogen atoms by impact of bare ions is studied at intermediate and high collision velocities. Total cross sections for final {ital np} states by impact of protons, alpha particles, and He{sup +} ions are calculated using the symmetric eikonal approximation and compared with experimental data. This comparison supports the existence of distortion effects recently predicted by Bugacov and co-workers [Phys. Rev. A {bold 47}, 1052 (1993)]. The validity of scaling laws is analyzed.

  11. Calculation of resonant effects in electron-impact excitation of positive ions Application to oxygen VII

    NASA Technical Reports Server (NTRS)

    Pindzola, M. S.; Temkin, A.; Bhatia, A. K.

    1979-01-01

    The general reaction theory of Feshbach is applied to the calculation of resonant effects in near-threshold electron-positive-ion excitation. The theory divides configuration space into open- and closed-channel parts, resonance effects being described by the closed-channel part. The open-channel part is handled in a distorted-wave approximation to the set of open-channel coupled equations. Various methods are suggested for handling the closed-channel part. However, an 'attached-excited-target approximation' is used explicitly, which is further approximated by a set of uncoupled closed-channel equations. As an example, the 1 1S-2 1P excitation cross section of O VII below the 3 3S threshold is calculated. Various distorted-wave approximations are investigated and results from most of them are quite similar. Resonant effects arising from the attachment of the colliding electron with the 3 3S state are found to be small, but other close-lying n = 3 states have not yet been included.

  12. Effective collision strengths for excitation and de-excitation of nebular [O III] optical and infrared lines with κ distributed electron energies

    NASA Astrophysics Data System (ADS)

    Storey, P. J.; Sochi, Taha

    2015-05-01

    We present effective collision strengths for electron excitation and de-excitation of the 10 forbidden transitions between the five lowest energy levels of the astronomically abundant doubly ionized oxygen ion, O2+. The raw collision strength data were obtained from an R-matrix intermediate coupling calculation using the Breit-Pauli relativistic approximation published previously by the authors. The effective collision strengths were calculated with κ-distributed electron energies and are tabulated as a function of the electron temperature and κ.

  13. Effective Collision Strengths for Electron Impact Excitation of Inelastic Transitions in S III

    NASA Technical Reports Server (NTRS)

    Tayal, S. S.

    1997-01-01

    We have calculated electron collisional excitation strengths for all electric dipole forbidden, semi-forbidden, and allowed transitions among the lowest 17 LS states 3s(exp 2)3p(exp 2) P-3, D-1, S-1, 3s3p(exp 3)S-5(exp 0), D-3(exp 0), P-3(exp 0), P-1(exp 0), S-3(exp 0), D-1(exp 0), 3S(exp 2)3p3d D-1(exp 0), F-3(exp 0), P-3(exp 0), D-3(exp 0), F-3(exp 0), P-1(exp 0), and 3S(exp 2)3p4S P-3(exp 0), P-l(exp 0) of S III using the R-matrix method. These S m states are represented by fairly extensive configuration-interaction wave functions that yield excited state energies in close agreement with recent laboratory measurements. Rydberg series of resonances converging to the excited state thresholds are explicitly included in the scattering calculation. The effective collision strengths are determined assuming Maxwellian distribution of electron energies. These are listed over a wide temperature range ([0.5-10] x 10(exp 4) K) and compared, where possible, with other available calculations. Subject headings: atomic data - atomic processes

  14. Benchmarks of electronically excited states: Basis set effects on CASPT2 results

    NASA Astrophysics Data System (ADS)

    Silva-Junior, Mario R.; Schreiber, Marko; Sauer, Stephan P. A.; Thiel, Walter

    2010-11-01

    Vertical excitation energies and one-electron properties are computed for the valence excited states of 28 medium-sized organic benchmark molecules using multistate multiconfigurational second-order perturbation theory (MS-CASPT2) and the augmented correlation-consistent aug-cc-pVTZ basis set. They are compared with previously reported MS-CASPT2 results obtained with the smaller TZVP basis. The basis set extension from TZVP to aug-cc-pVTZ causes rather minor and systematic shifts in the vertical excitation energies that are normally slightly reduced (on average by 0.11 eV for the singlets and by 0.09 eV for the triplets), whereas the changes in the calculated oscillator strengths and dipole moments are somewhat more pronounced on a relative scale. These basis set effects at the MS-CASPT2 level are qualitatively and quantitatively similar to those found at the coupled cluster level for the same set of benchmark molecules. The previously proposed theoretical best estimates (TBE-1) for the vertical excitation energies for 104 singlet and 63 triplet excited states of the benchmark molecules are upgraded by replacing TZVP with aug-cc-pVTZ data that yields a new reference set (TBE-2). Statistical evaluations of the performance of density functional theory (DFT) and semiempirical methods lead to the same ranking and very similar quantitative results for TBE-1 and TBE-2, with slightly better performance measures with respect to TBE-2. DFT/MRCI is most accurate among the investigated DFT-based approaches, while the OMx methods with orthogonalization corrections perform best at the semiempirical level.

  15. Entanglement entropy of electronic excitations

    NASA Astrophysics Data System (ADS)

    Plasser, Felix

    2016-05-01

    A new perspective into correlation effects in electronically excited states is provided through quantum information theory. The entanglement between the electron and hole quasiparticles is examined, and it is shown that the related entanglement entropy can be computed from the eigenvalue spectrum of the well-known natural transition orbital (NTO) decomposition. Non-vanishing entanglement is obtained whenever more than one NTO pair is involved, i.e., in the case of a multiconfigurational or collective excitation. An important implication is that in the case of entanglement it is not possible to gain a complete description of the state character from the orbitals alone, but more specific analysis methods are required to decode the mutual information between the electron and hole. Moreover, the newly introduced number of entangled states is an important property by itself giving information about excitonic structure. The utility of the formalism is illustrated in the cases of the excited states of two interacting ethylene molecules, the conjugated polymer para-phenylene vinylene, and the naphthalene molecule.

  16. Entanglement entropy of electronic excitations.

    PubMed

    Plasser, Felix

    2016-05-21

    A new perspective into correlation effects in electronically excited states is provided through quantum information theory. The entanglement between the electron and hole quasiparticles is examined, and it is shown that the related entanglement entropy can be computed from the eigenvalue spectrum of the well-known natural transition orbital (NTO) decomposition. Non-vanishing entanglement is obtained whenever more than one NTO pair is involved, i.e., in the case of a multiconfigurational or collective excitation. An important implication is that in the case of entanglement it is not possible to gain a complete description of the state character from the orbitals alone, but more specific analysis methods are required to decode the mutual information between the electron and hole. Moreover, the newly introduced number of entangled states is an important property by itself giving information about excitonic structure. The utility of the formalism is illustrated in the cases of the excited states of two interacting ethylene molecules, the conjugated polymer para-phenylene vinylene, and the naphthalene molecule. PMID:27208936

  17. The effect of electron beams on cyclotron maser emission excited by lower-energy cutoffs

    NASA Astrophysics Data System (ADS)

    Zhao, G. Q.; Feng, H. Q.; Wu, D. J.

    2016-05-01

    Electron-cyclotron maser (ECM) is one of the most important emission mechanisms in astrophysics and can be excited efficiently by lower-energy cutoffs of power-law electrons. These non-thermal electrons probably propagate as a directed collimated beam along ambient magnetic fields. This paper investigates the ECM, in which the effect of electron beams is emphasized. Results show the dependence of emission properties of the ECM on the beam feature. The maximum growth rate of the extraordinary mode (X2) rapidly decreases as the beam momentum increases, while the growth rate of the ordinary mode (O1) changes slightly. In particular, the ordinary mode can overcome the extraordinary mode and becomes the fastest growth mode once the beam momentum is large enough. This research presents an extension of the conventional studies on ECM driven by lower-energy cutoffs and may be helpful to understand better the emission process of solar type I radio bursts, which are dominated by the ordinary mode emission.

  18. Electronic excitations of slow ions in a free electron gas metal: evidence for charge exchange effects.

    PubMed

    Primetzhofer, D; Rund, S; Roth, D; Goebl, D; Bauer, P

    2011-10-14

    Electronic energy loss of light ions transmitted through nanometer films of Al has been studied at very low ion velocities. For hydrogen, the electronic stopping power S is found to be perfectly proportional to velocity, as expected for a free electron gas. For He, the same is anticipated, but S shows a transition between two distinct regimes, in both of which S is velocity proportional-however, with remarkably different slopes. This finding can be explained as a consequence of charge exchange in close encounters between He and Al atoms, which represents an additional energy loss channel. PMID:22107378

  19. Effect of collective response on electron capture and excitation in collisions of highly charged ions with fullerenes.

    PubMed

    Kadhane, U; Misra, D; Singh, Y P; Tribedi, Lokesh C

    2003-03-01

    Projectile deexcitation Lyman x-ray emission following electron capture and K excitation has been studied in collisions of bare and Li-like sulphur ions (of energy 110 MeV) with fullerenes (C(60)/C(70)) and different gaseous targets. The intensity ratios of different Lyman x-ray lines in collisions with fullerenes are found to be substantially lower than those for the gas targets, both for capture and excitation. This has been explained in terms of a model based on "solidlike" effect, namely, wakefield induced stark mixing of the excited states populated via electron capture or K excitation: a collective phenomenon of plasmon excitation in the fullerenes under the influence of heavy, highly charged ions. PMID:12689221

  20. Effect of electronic excitation on high-temperature flows behind strong shock waves

    SciTech Connect

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

    2014-12-09

    In the present paper, a strongly non-equilibrium one-dimensional steady-state flow behind the plane shock wave is studied. We consider a high-temperature chemically reacting five-component ionized mixture of nitrogen species (N{sub 2}/N{sub 2}{sup 2}/N/N{sup +}/e{sup −}) taking into account electronic degrees of freedom in N and N{sup +} (170 and 625 electronic energy levels respectively), and electronic-rotational-vibrational modes in N{sub 2} and N{sub 2}{sup +} (5 and 7 electronic terms). Non-equilibrium reactions of ionization, dissociation, recombination and charge-transfer are included to the kinetic scheme. The system of governing equations is written under the assumption that translation and internal energy relaxation is fast whereas chemical reactions and ionization proceed on the macroscopic gas-dynamics time-scale. The developed model is applied to simulate the flow behind a plane shock wave under initial conditions characteristic for the spacecraft re-entry from an interplanetary flight (Hermes and Fire II experiments). Fluid-dynamic parameters behind the shock wave as well as transport coefficients and the heat flux are calculated for the (N{sub 2}/N{sub 2}{sup +}/N/N{sup +}/e{sup −}) mixture. The effect of electronic excitation on kinetics, dynamics and heat transfer is analyzed. Whereas the contribution of electronic degrees of freedom to the flow macroparameters is negligible, their influence on the heat flux is found to be important under conditions of Hermes re-entry.

  1. Excitation of plasmonic terahertz photovoltaic effects in a periodic two-dimensional electron system by the attenuated total reflection method

    SciTech Connect

    Fateev, D. V. Mashinsky, K. V.; Bagaeva, T. Yu.; Popov, V. V.

    2015-01-15

    The problem of the rectification of terahertz radiation due to plasmonic nonlinearities in a periodic two-dimensional electron system upon the excitation of plasma oscillations by the attenuated total reflection method is solved. This model allows the independent study of different plasmonic rectification mechanisms, i.e., plasmonic electron drag and plasmonic ratchet effects.

  2. On The Effect of Electron Collisions in the Excitation of Cometary HCN

    NASA Technical Reports Server (NTRS)

    Lovell, Amy J.; Kallivayalil, Nitya; Schloerb, F. Peter; Combi, Michael R.; Hansen, Kenneth C.; Gombosi, T. I.

    2004-01-01

    The electron-HCN collision rate for the excitation of rotational transitions of the HCN molecule is evaluated in comets C/1995 01 (Hale-Bopp) and C/1996 B2 (Hyakutake). Based on theoretical models of the cometary atmosphere, we show that collisions with electrons can provide a significant excitation mechanism for rotational transitions in the HCN molecule. Computed values of the cross section sigma(sub e-HCN) can be as high as 1.3 x cm2, more than 2 orders of magnitude greater than the commonly assumed HCN-H2O cross section. For the ground rotational transitions of HCN, the electron-HCN collision rate is found to exceed the HCN-H2O collision rate at distances greater than 3000 km from the cometary nucleus of Hale-Bopp and 1000 km from that of Hyakutake. Collisional excitation processes dominate over radiative excitation processes up to a distance of 160,000 km from the cometary nucleus of Hale-Bopp and 50,000 km from that of Hyakutake. Excitation models that neglect electron collisions can underestimate the HCN gas production rates by as much as a factor of 2.

  3. Effect of Electronic Excitation on Hydrogen Atom Transfer (Tautomerization) Reactions for the DNA Base Adenine

    NASA Technical Reports Server (NTRS)

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

    2002-01-01

    Geometrical structures and energetic properties for four different tautomers of adenine are calculated in this study, using multi-configurational wave functions. Both the ground and the lowest single excited state potential energy surface are studied. The energetic order of the tautomers on the ground state potential surface is 9H less than 7H less than 3H less than 1H, while on the excited state surface this order is found to be different: 3H less than 1H less than 9H less than 7H. Minimum energy reaction paths are obtained for hydrogen atom transfer (9 yields 3 tautomerization) reactions in the ground and the lowest excited electronic state. It is found that the barrier heights and the shapes of the reaction paths are different for the ground and the excited electronic state, suggesting that the probability of such tautomerization reaction is higher on the excited state potential energy surface. The barrier for this reaction in the excited state may become very low in the presence of water or other polar solvent molecules, and therefore such tautomerization reaction may play an important role in the solution phase photochemistry of adenine.

  4. Nonequilibrium solvent effects in Born-Oppenheimer molecular dynamics for ground and excited electronic states

    NASA Astrophysics Data System (ADS)

    Bjorgaard, J. A.; Velizhanin, K. A.; Tretiak, S.

    2016-04-01

    The effects of solvent on molecular processes such as excited state relaxation and photochemical reaction often occurs in a nonequilibrium regime. Dynamic processes such as these can be simulated using excited state molecular dynamics. In this work, we describe methods of simulating nonequilibrium solvent effects in excited state molecular dynamics using linear-response time-dependent density functional theory and apparent surface charge methods. These developments include a propagation method for solvent degrees of freedom and analytical energy gradients for the calculation of forces. Molecular dynamics of acetaldehyde in water or acetonitrile are demonstrated where the solute-solvent system is out of equilibrium due to photoexcitation and emission.

  5. Nonequilibrium solvent effects in Born-Oppenheimer molecular dynamics for ground and excited electronic states.

    PubMed

    Bjorgaard, J A; Velizhanin, K A; Tretiak, S

    2016-04-21

    The effects of solvent on molecular processes such as excited state relaxation and photochemical reaction often occurs in a nonequilibrium regime. Dynamic processes such as these can be simulated using excited statemolecular dynamics. In this work, we describe methods of simulating nonequilibrium solvent effects in excited statemolecular dynamics using linear-response time-dependent density functional theory and apparent surface charge methods. These developments include a propagation method for solvent degrees of freedom and analytical energy gradients for the calculation of forces. Molecular dynamics of acetaldehyde in water or acetonitrile are demonstrated where the solute-solvent system is out of equilibrium due to photoexcitation and emission. PMID:27389206

  6. Selectivity of peptide bond dissociation on excitation of a core electron: Effects of a phenyl group

    NASA Astrophysics Data System (ADS)

    Tsai, Cheng-Cheng; Chen, Jien-Lian; Hu, Wei-Ping; Lin, Yi-Shiue; Lin, Huei-Ru; Lee, Tsai-Yun; Lee, Yuan T.; Ni, Chi-Kung; Liu, Chen-Lin

    2016-09-01

    The selective dissociation of a peptide bond upon excitation of a core electron in acetanilide and N-benzylacetamide was investigated. The total-ion-yield near-edge X-ray absorption fine structure spectra were recorded and compared with the predictions from time-dependent density functional theory. The branching ratios for the dissociation of a peptide bond are observed as 16-34% which is quite significant. This study explores the core-excitation, the X-ray photodissociation pathways, and the theoretical explanation of the NEXAFS spectra of organic molecules containing both a peptide bond and a phenyl group.

  7. Stark effect of interfering electronic states: Localization of the nπ* excitations in toluquinone

    NASA Astrophysics Data System (ADS)

    Galaup, J. P.; Trommsdorff, H. P.

    1984-04-01

    High-precision Stark measurements on oriented single crystals of toluquinone at low temperatures have been performed and lead to an assessment of the electronic parenthood of the levels giving rise to the complex spectral region of interference between the two nearby nπ* excited states. The origin bands of the lowest excited singlet and triplet states are characterized by a measure of their factor-group splittings and an evaluation of the change in dipole moment and in polarizability upon excitation. The value of the change in dipole moment is shown to vary strongly between different vibrational levels of the lower state and an evaluation of the degree of localization of the electronic excitation on one CO group is made. The previous assignment of the second nπ* state is confirmed by the sign of the corresponding Stark shift. From measurements on crystals having been oriented in an electric field the absolute orientation of the polar crystal as well as the sign of the pyroelectric coefficient are proposed.

  8. Dynamic screening and wake effects on electronic excitation in ion-solid and ion-surface collisions

    SciTech Connect

    Burgdoerfer, J. . Dept. of Physics Oak Ridge National Lab., TN )

    1991-01-01

    The collective electronic response in a solid effectively alters ionic and atomic potentials giving rise to dynamic screening and to a wake'' of density fluctuations trailing ions as they propagate through the solid. The presence of dynamic screening modifies electronic excitation processes of projectiles in ion-solid collisions as compared to binary ion-atom collisions. We review recent theoretical and experimental studies directed at the search for and identification of signatures of dynamic screening and wake effects. Examples include the formation of excited projectile bound states under channeling conditions, radiative electron capture, the search for wake riding'' electrons in antiproton-solid collisions, and the neutralization of highly charged ions near surfaces. 42 refs., 7 figs.

  9. Electronic Doppler effect in resonant Auger decay of CO molecules upon excitation near a shake-up {pi} resonance

    SciTech Connect

    Sorensen, S. L.; Kitajima, M.; Tanaka, T.; Hoshino, M.; Tanaka, H.; Tamenori, Y.; Sankari, R.; Piancastelli, M. N.; Ueda, K.; Velkov, Y.; Minkov, I.; Carravetta, V. |; Gel'mukhanov, F. |

    2007-12-15

    We present an experimental observation of the electronic Doppler effect in resonant Auger spectra upon core excitation slightly above the carbon K edge of the CO molecule. Thus the electronic Doppler effect has been identified in above-threshold excitation, and in a transition of {pi} symmetry. Ab initio calculations of the potential energy curves of the relevant states of CO and the wave packet technique have been employed to provide a theoretical background to the experimental studies. The weak feature around 299.4 eV in the photoabsorption spectrum, whose decay has been investigated by the present experiment, is assigned to double (core-valence) excitations to C 1s shake-up states |1s{sub C}{sup -1}1{pi}{sup -1}{pi}*{sup 2}> with a strong dissociative character, and the Doppler splitting of the atomic peak has been reproduced by the simulation.

  10. Q -dependent electronic excitations in osmium: Pressure- and temperature-induced effects

    NASA Astrophysics Data System (ADS)

    Ponosov, Yu. S.; Struzhkin, V. V.; Goncharov, A. F.; Streltsov, S. V.

    2008-12-01

    Raman scattering by electrons and phonons has been studied in single crystals of the 5d transition-metal osmium under pressures up to 60 GPa in the temperature range of 10-300 K. An anomalous increase in the electronic light-scattering cross section was found in the pressure range of 20-30 GPa with the use of green and blue excitation wavelengths. At these conditions, we observe an appearance of well-defined electronic peaks at ˜580cm-1 for the wave-vector direction q∥[0001] and at ˜350cm-1 for q∥[101¯0] . The comparison of q dependencies measured and calculated from the first-principles spectra suggests a strong volume- and temperature-dependent renormalization of the energies and damping of the electronic states near the Fermi level.

  11. Experimental evidence of excited electron number density and temperature effects on electron-phonon coupling in gold films

    SciTech Connect

    Giri, Ashutosh; Gaskins, John T.; Foley, Brian M.; Cheaito, Ramez; Hopkins, Patrick E.

    2015-01-28

    The electronic transport properties of metals with weak electron-phonon coupling can be influenced by non-thermal electrons. Relaxation processes involving non-thermal electrons competing with the thermalized electron system have led to inconsistencies in the understanding of how electrons scatter and relax with the less energetic lattice. Recent theoretical and computational works have shown that the rate of energy relaxation with the metallic lattice will change depending on the thermalization state of the electrons. Even though 20 years of experimental works have focused on understanding and isolating these electronic relaxation mechanisms with short pulsed irradiation, discrepancies between these existing works have not clearly answered the fundamental question of the competing effects between non-thermal and thermal electrons losing energy to the lattice. In this work, we demonstrate the ability to measure the electron relaxation for varying degrees of both electron-electron and electron-phonon thermalization. This series of measurements of electronic relaxation over a predicted effective electron temperature range up to ∼3500 K and minimum lattice temperatures of 77 K validate recent computational and theoretical works that theorize how a nonequilibrium distribution of electrons transfers energy to the lattice. Utilizing this wide temperature range during pump-probe measurements of electron-phonon relaxation, we explain discrepancies in the past two decades of literature of electronic relaxation rates. We experimentally demonstrate that the electron-phonon coupling factor in gold increases with increasing lattice temperature and laser fluences. Specifically, we show that at low laser fluences corresponding to small electron perturbations, energy relaxation between electrons and phonons is mainly governed by non-thermal electrons, while at higher laser fluences, non-thermal electron scattering with the lattice is less influential on the energy relaxation

  12. Solvent electronic polarization effects on a charge transfer excitation studied by the mean-field QM/MM method

    SciTech Connect

    Nakano, Hiroshi

    2015-12-31

    Electronic polarization effects of a medium can have a significant impact on a chemical reaction in condensed phases. We discuss the effects on the charge transfer excitation of a chromophore, N,N-dimethyl-4-nitroaniline, in various solvents using the mean-field QM/MM method with a polarizable force field. The results show that the explicit consideration of the solvent electronic polarization effects is important especially for a solvent with a low dielectric constant when we study the solvatochromism of the chromophore.

  13. High electronic excitations and ion beam mixing effects in high energy ion irradiated Fe/Si multilayers

    SciTech Connect

    Bauer, P.; Dufour, C.; Jaouen, C.; Marchal, G.; Pacaud, J.; Grilhe, J.; Jousset, J.C.

    1997-01-01

    M{umlt o}ssbauer spectroscopy ({sup 57}Fe) shows evidence for mixing effects induced by electronic energy deposition in nanoscale Fe/Si multilayers irradiated with swift heavy ions. A decrease in the mixing efficiency with electronic stopping power is reported; a threshold is found, under which iron environment modifications no longer occur. The kinetics of Fe{endash}Si phase formation after irradiation suggests the existence of three regimes: (i) for high excitation levels, a magnetic amorphous phase is formed directly in the wake of the incoming ion and an almost complete mixing is reached at low fluence (10{sup 13} U/cm{sup 2}); (ii) for low excitation levels, a paramagnetic Si-rich amorphous phase is favored at the interface while crystalline iron subsists at high fluences; (iii) for intermediate excitation levels, saturation effects are observed and the formation rate of both magnetic and paramagnetic phases points to direct mixing in the ion wake but with a reduced track length in comparison to U irradiation. The measured interfacial mixing cross section induced by electronic energy deposition suggests that a thermal diffusion process is mainly involved in addition to damage creation. {copyright} {ital 1997 American Institute of Physics.}

  14. One-electron excitations, correlation effects, and the plasmon in cesium metal

    SciTech Connect

    Fleszar, A. ||; Stumpf, R.; Eguiluz, A.G. ||

    1997-01-01

    We study the dynamical electronic response of Cs at a first-principles level. The spatially localized 5p semicore shell induces a physical interplay between crystal local fields and electron correlations, leading to a novel, and relatively large, many-body shift of the plasmon energy. This effect, combined with that of one-electron transitions into empty states near the plasmon energy, yields a plasmon dispersion curve which is in excellent agreement with experiment for small wave vectors. In addition, our results feature a flat dispersion for large wave vectors, in qualitative agreement with experiment. {copyright} {ital 1997} {ital The American Physical Society}

  15. Excitation of atomic nitrogen by electron impact.

    NASA Technical Reports Server (NTRS)

    Stone, E. J.; Zipf, E. C.

    1973-01-01

    Measurement of the absolute cross sections for the excitation of a number of N I multiplets by electron impact on atomic nitrogen. Two of these cross sections - 1134 and 1200 A - are found to be large, reaching 2.0 x 10 to the minus 16th and 2.5 x 10 to the minus 16th sq cm at their peaks, respectively. The presence of vibrationally excited molecular nitrogen in the discharged gas is confirmed, and its effect on the measurements is discussed. The ratio of the oscillator strengths of the 1200- and 1134-A resonance transitions is measured to be 2.6 plus or minus 0.3.

  16. Theoretical study of Raman chirped adiabatic passage by X-ray absorption spectroscopy: Highly excited electronic states and rotational effects

    SciTech Connect

    Engin, Selma; Sisourat, Nicolas Selles, Patricia; Taïeb, Richard; Carniato, Stéphane

    2014-06-21

    Raman Chirped Adiabatic Passage (RCAP) is an efficient method to climb the vibrational ladder of molecules. It was shown on the example of fixed-in-space HCl molecule that selective vibrational excitation can thus be achieved by RCAP and that population transfer can be followed by X-ray Photoelectron spectroscopy [S. Engin, N. Sisourat, P. Selles, R. Taïeb, and S. Carniato, Chem. Phys. Lett. 535, 192–195 (2012)]. Here, in a more detailed analysis of the process, we investigate the effects of highly excited electronic states and of molecular rotation on the efficiency of RCAP. Furthermore, we propose an alternative spectroscopic way to monitor the transfer by means of X-ray absorption spectra.

  17. Effect of Solvation on Electron Detachment and Excitation Energies of a Green Fluorescent Protein Chromophore Variant.

    PubMed

    Bose, Samik; Chakrabarty, Suman; Ghosh, Debashree

    2016-05-19

    Hybrid quantum mechanics/molecular mechanics (QM/MM) is applied to the fluorinated green fluorescent protein (GFP) chromophore (DFHBDI) in its deprotonated form to understand the solvatochromic shifts in its vertical detachment energy (VDE) and vertical excitation energy (VEE). This variant of the GFP chromophore becomes fluorescent in an RNA environment and has a wide range of applications in biomedical and biochemical fields. From microsolvation studies, we benchmark (with respect to full QM) the accuracy of our QM/MM calculations with effective fragment potential (EFP) as the MM method of choice. We show that while the solvatochromic shift in the VEE is minimal (0.1 eV blue shift) and its polarization component is only 0.03 eV, the effect of the solvent on the VDE is quite large (3.85 eV). We also show by accurate calculations on the solvatochromic shift of the VDE that polarization accounts for ∼0.23 eV and therefore cannot be neglected. The effect of the counterions on the VDE of the deprotonated chromophore in solvation is studied in detail, and a charge-smearing scheme is suggested for charged chromophores. PMID:27116477

  18. Electronic and Nuclear Factors in Charge and Excitation Transfer

    SciTech Connect

    Piotr Piotrowiak

    2004-09-28

    We report the and/or state of several subprojects of our DOE sponsored research on Electronic and Nuclear Factors in Electron and Excitation Transfer: (1) Construction of an ultrafast Ti:sapphire amplifier. (2) Mediation of electronic interactions in host-guest molecules. (3) Theoretical models of electrolytes in weakly polar media. (4) Symmetry effects in intramolecular excitation transfer.

  19. Theoretical studies of electronically excited states

    SciTech Connect

    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.

  20. Description of electronic excited states using electron correlation operator.

    PubMed

    Nichols, Bryan; Rassolov, Vitaly A

    2013-09-14

    The electron correlation energy in a chemical system is defined as a difference between the energy of an exact energy for a given Hamiltonian, and a mean-field, or single determinant, approximation to it. A promising way to model electron correlation is through the expectation value of a linear two-electron operator for the Kohn-Sham single determinant wavefunction. For practical reasons, it is desirable for such an operator to be universal, i.e., independent of the positions and types of nuclei in a molecule. The correlation operator models the effect of electron correlation on the interaction energy in a electron pair. We choose an operator expanded in a small number of Gaussians as a model for electron correlation, and test it by computing atomic and molecular adiabatic excited states. The computations are performed within the Δ Self-Consistent Field (ΔSCF) formalism, and are compared to the time-dependent density functional theory model with popular density functionals. The simplest form of the correlation operator contains only one parameter derived from the helium atom ground state correlation energy. The correlation operator approach significantly outperforms other methods in computation of atomic excitation energies. The accuracy of molecular excitation energies computed with the correlation operator is limited by the shortcomings of the ΔSCF methodology in describing excited states. PMID:24050332

  1. Investigation of effect of excitation frequency on electron energy distribution functions in low pressure radio frequency bounded plasmas

    NASA Astrophysics Data System (ADS)

    Bhattacharjee, Sudeep; Lafleur, Trevor; Charles, Christine; Boswell, Rod

    2011-07-01

    Particle in cell (PIC) simulations are employed to investigate the effect of excitation frequency ω on electron energy distribution functions (EEDFs) in a low pressure radio frequency (rf) discharge. The discharge is maintained over a length of 0.10 m, bounded by two infinite parallel plates, with the coherent heating field localized at the center of the discharge over a distance of 0.05 m and applied perpendicularly along the y and z directions. On varying the excitation frequency f (=ω/2π) in the range 0.01-50 MHz, it is observed that for f ≤ 5 MHz the EEDF shows a trend toward a convex (Druyvesteyn-like) distribution. For f > 5 MHz, the distribution resembles more like a Maxwellian with the familiar break energy visible in most of the distributions. A prominent "hot tail" is observed at f ≥ 20 MHz and the temperature of the tail is seen to decrease with further increase in frequency (e.g., at 30 MHz and 50 MHz). The mechanism for the generation of the "hot tail" is considered to be due to preferential transit time heating of energetic electrons as a function of ω, in the antenna heating field. There exists an optimum frequency for which high energy electrons are maximally heated. The occurrence of the Druyvesteyn-like distributions at lower ω may be explained by a balance between the heating of the electrons in the effective electric field and elastic cooling due to electron neutral collision frequency νen; the transition being dictated by ω ˜ 2πνen.

  2. Effect of the Bethe surface description on the electronic excitations induced by energetic proton beams in liquid water and DNA

    NASA Astrophysics Data System (ADS)

    Abril, Isabel; Denton, Cristian D.; de Vera, Pablo; Kyriakou, Ioanna; Emfietzoglou, Dimitris; Garcia-Molina, Rafael

    2010-06-01

    The irradiation of biological systems by energetic ion beams has multiple applications in medical physics and space radiation health, such as hadrontherapy for cancer treatment or protection of astronauts against space radiation. Therefore, for a better control and understanding of the effects of radiation damage in living tissues, it is necessary to advance an accurate description of the energy loss from the ion beam to the target. In the present work we use the dielectric formalism to calculate the probability for an energetic proton to produce electronic excitations in two targets of high biological interest, namely, liquid water and DNA. Also, the mean energy of the electronic excitations in these targets is found as a function of the incident proton energy. The electronic response of the target, characterized by its energy-loss function (ELF), is described by several models that fit the available experimental optical data (at zero momentum transfer), but use different approaches to obtain the Bethe surface, that is, to extend the ELF to any energy and momentum transferred.

  3. Pressure anisotropy effects on nonlinear electrostatic excitations in magnetized electron-positron-ion plasmas

    NASA Astrophysics Data System (ADS)

    Adnan, Muhammad; Williams, Gina; Qamar, Anisa; Mahmood, Shahzad; Kourakis, Ioannis

    2014-09-01

    The propagation of linear and nonlinear electrostatic waves is investigated in a magnetized anisotropic electron-positron-ion (e-p-i) plasma with superthermal electrons and positrons. A two-dimensional plasma geometry is assumed. The ions are assumed to be warm and anisotropic due to an external magnetic field. The anisotropic ion pressure is defined using the double adiabatic Chew-Golberger-Low (CGL) theory. In the linear regime, two normal modes are predicted, whose characteristics are investigated parametrically, focusing on the effect of superthermality of electrons and positrons, ion pressure anisotropy, positron concentration and magnetic field strength. A Zakharov-Kuznetsov (ZK) type equation is derived for the electrostatic potential (disturbance) via a reductive perturbation method. The parametric role of superthermality, positron content, ion pressure anisotropy and magnetic field strength on the characteristics of solitary wave structures is investigated. Following Allen and Rowlands [J. Plasma Phys. 53, 63 (1995)], we have shown that the pulse soliton solution of the ZK equation is unstable to oblique perturbations, and have analytically traced the dependence of the instability growth rate on superthermality and ion pressure anisotropy.

  4. Effect of fluoro substitution on the fragmentation of the K-shell excited/ionized pyridine studied by electron impact.

    PubMed

    Sakai, Masamichi; Okada, Kazumasa

    2011-07-01

    Fragmentation of the pyridine ring followed by K-shell excitation/ionization has been studied with 2-fluoropyridine (2FPy) by electron impact. Ab initio molecular orbital (MO) calculations were also carried out to investigate the electronic states correlating with specific fragment ions. The fragment ions are produced characteristically at the N 1s edge, while the spectra observed at the F 1s and C 1s edges exhibit a small difference from that at the valence ionization. The production of the C(4)H(2)(+), C(4)H(3)(+) and C(4)H(2)F(+) ions indicates that the cleavage of the N-C6 and C2-C3 bonds or the N-C2 and C5-C6 bonds is likely to occur after the N 1s excitation/ionization. Ab initio MO calculations indicate that the former fission is likely to proceed through the n(N)(1)π(2)(1)π(3)(2) and n(N)(0)π(2)(2)π(3)(2) excited states of the parent molecular dication. On the other hand, the breakage of the N-C2 and C4-C5 bonds, which specifically proceeds at the N 1s edge for 2-methylpyridine, does not occur for 2FPy. The present calculation reveals that the products of this channel are unstable by the electronegativity of fluorine and that the relative energy of the Auger-final states of 2FPy is lowered by the reorganization and electron correlation effects. PMID:21744416

  5. Nonlocal thermodynamic equilibrium effects in stratospheric HF by collisional energy transfer from electronically excited O2 and implications for infrared remote sensing

    NASA Technical Reports Server (NTRS)

    Kaye, Jack A.

    1989-01-01

    A possible nonlocal thermodynamic equilibrium (non-LTE) effect involving stratospheric HF arising from the direct photochemical excitation of vibrationally excited HF by collisional energy transfer from electronically excited O2 is presented. Although this non-LTE effect is smaller that one associated with the direct solar excitation of both HF(nv = 1) and HF(nv = 2), calculations show that inclusion of the mechanism into retrieval algorithms is necessary if correct daytime upper stratosphere HF profiles are to be inferred in future IR thermal emission measurements.

  6. Dissociative electron attachment and vibrational excitation of CF{sub 3}Cl: Effect of two vibrational modes revisited

    SciTech Connect

    Tarana, Michal; Houfek, Karel; Horacek, Jiri; Fabrikant, Ilya I.

    2011-11-15

    We present a study of dissociative electron attachment and vibrational excitation processes in electron collisions with the CF{sub 3}Cl molecule. The calculations are based on the two-dimensional nuclear dynamics including the C-Cl symmetric stretch coordinate and the CF{sub 3} symmetric deformation (umbrella) coordinate. The complex potential energy surfaces are calculated using the ab initio R-matrix method. The results for dissociative attachment and vibrational excitation of the umbrella mode agree quite well with experiment whereas the cross section for excitation of the C-Cl symmetric stretch vibrations is about a factor-of-three too low in comparison with experimental data.

  7. Monte Carlo simulation for Multi-Mode Elastic Peak Electron Spectroscopy of crystalline materials: Effects of surface structure and excitation

    NASA Astrophysics Data System (ADS)

    Gruzza, B.; Chelda, S.; Robert-Goumet, C.; Bideux, L.; Monier, G.

    2010-01-01

    The Multi-Mode Elastic Peak Electron Spectroscopy (MM-EPES) analysis is confined to incoherent electron elastic scattering and the use of variable primary energy. This experimental method is very sensitive to the surface region of the sample. However, for quantitative interpretation, the MM-EPES method needs jointly a Monte Carlo (MC) computer simulation of electron trajectories in the solid. In the present work, we proposed a new approach to calculate the percentage η e of elastic reflected electrons by the surface of a sample. This simulation takes into account the surface effects (i.e. surface plasmon), and the atoms arrangement in the substrate. The concept of the surface excitation parameter (SEP) is also presented. Computer simulations were performed on the three low index single crystals of Cu, Au, Si and Ag. The results confirm that the distribution of substrate atoms, according to the crystallographic structure, influences the intensity measured by EPES. A simple prediction formula was proposed to calculate η e for elastic electrons entering in a Retarding Field Analyzer (RFA) spectrometer which is the apparatus giving experimentally numerical values of the percentage η e.

  8. On the Electronically Excited States of Uracil

    SciTech Connect

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

    2008-10-09

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

  9. Electronic spectra and excited state dynamics of pentafluorophenol: Effects of low-lying πσ{sup ∗} states

    SciTech Connect

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

    2015-05-14

    Multiple fluorine atom substitution effect on photophysics of an aromatic chromophore has been investigated using phenol as the reference system. It has been noticed that the discrete vibronic structure of the S{sub 1}←S{sub 0} absorption system of phenol vapor is completely washed out for pentafluorophenol (PFP), and the latter also shows very large Stokes shift in the fluorescence spectrum. For excitations beyond S{sub 1} origin, the emission yield of PFP is reduced sharply with increase in excess vibronic energy. However, in a collisional environment like liquid hydrocarbon, the underlying dynamical process that drives the non-radiative decay is hindered drastically. Electronic structure theory predicts a number of low-lying dark electronic states of πσ{sup ∗} character in the vicinity of the lowest valence ππ{sup ∗} state of this molecule. Tentatively, we have attributed the excitation energy dependent non-radiative decay of the molecule observed only in the gas phase to an interplay between the lowest ππ{sup ∗} and a nearby dissociative πσ{sup ∗} state. Measurements in different liquids reveal that some of the dark excited states light up with appreciable intensity only in protic liquids like methanol and water due to hydrogen bonding between solute and solvents. Electronic structure theory methods indeed predict that for PFP-(H{sub 2}O){sub n} clusters (n = 1-11), intensities of a number of πσ{sup ∗} states are enhanced with increase in cluster size. In contrast with emitting behavior of the molecule in the gas phase and solutions of nonpolar and polar aprotic liquids, the fluorescence is completely switched off in polar protic liquids. This behavior is a chemically significant manifestation of perfluoro effect, because a very opposite effect occurs in the case of unsubstituted phenol for which fluorescence yield undergoes a very large enhancement in protic liquids. Several dynamical mechanisms have been suggested to interpret the

  10. Effective collision strengths for electron impact excitations in S II. [Plasma torus of Io

    SciTech Connect

    Tayal, S.S.; Henry, R.J.W.; Nakazaki, S.

    1987-02-01

    Electron impact collision strengths for forbidden, semiforbidden, and allowed transitions in S II calculated using the R-matrix method are presented. Configuration interaction wave functions are used to represent the six target states included in the calculation. At low impact energies the collision strengths are dominated by resonances for several transitions. The contribution from higher partial waves is obtained in the close-coupling approximation with exchange terms omitted. Results are presented for the effective collision strengths over a wide temperature range (5000-150,000 K) of astrophysical interest. The present results for the 4S(0) yields 2P(0) transition are 20-30 percent lower than previous calculations, while for the 4S(0) yields 2D(0) transition they are in good agreement. The results are approximately 30 percent higher than those of Ho and Henry (1983) for the 4S(0) yields 2P(0) transition at 80,000 K, and the difference between the two results increases with decreasing temperatures (under 80,000 K). 38 references.

  11. Collective Excitations in Electron-Hole Bilayers

    SciTech Connect

    Kalman, G. J.; Hartmann, P.; Donko, Z.; Golden, K. I.

    2007-06-08

    We report a combined analytic and molecular dynamics analysis of the collective mode spectrum of a bipolar (electron-hole) bilayer in the strong coupling classical limit. A robust, isotropic energy gap is identified in the out-of-phase spectra, generated by the combined effect of correlations and of the excitation of the bound dipoles. In the in-phase spectra we identify longitudinal and transverse acoustic modes wholly maintained by correlations. Strong nonlinear generation of higher harmonics of the fundamental dipole oscillation frequency and the transfer of harmonics between different modes is observed.

  12. Electron-impact excitation of holmium atoms

    SciTech Connect

    Smirnov, Yu M

    2000-06-30

    The electron-impact excitation of holmium atoms was studied by the method of extended crossing beams. The cross sections and the optical excitation functions were obtained for odd levels of Ho I, including the 22014 cm{sup -1} laser level. Over 99% of the atoms were shown to reside in the ground level prior to collisions with electrons. Also measured were the excitation cross sections for six even levels, which presumably participate in the formation of inversion population in a gas-discharge holmium vapour laser. (laser applications and other topics in quantum electronics)

  13. Simple model of bulk and surface excitation effects to inelastic scattering in low-energy electron beam irradiation of multi-walled carbon nanotubes

    SciTech Connect

    Kyriakou, Ioanna; Emfietzoglou, Dimitris; Garcia-Molina, Rafael; Abril, Isabel; Kostarelos, Kostas

    2011-09-01

    The effect of bulk and surface excitations to inelastic scattering in low-energy electron beam irradiation of multi-walled carbon nanotubes (MWNTs) is studied using the dielectric formalism. Calculations are based on a semiempirical dielectric response function for MWCNTs determined by means of a many-pole plasmon model with parameters adjusted to available experimental spectroscopic data under theoretical sum-rule constrains. Finite-size effects are considered in the context of electron gas theory via a boundary correction term in the plasmon dispersion relations, thus, allowing a more realistic extrapolation of the electronic excitation spectrum over the whole energy-momentum plane. Energy-loss differential and total inelastic scattering cross sections as a function of electron energy and distance from the surface, valid over the energy range {approx}50-30,000 eV, are calculated with the individual contribution of bulk and surface excitations separated and analyzed for the case of normally incident and escaping electrons. The sensitivity of the results to the various approximations for the spatial dispersion of the electronic excitations is quantified. Surface excitations are shown to have a strong influence upon the shape and intensity of the energy-loss differential cross section in the near surface region whereas the general notion of a spatially invariant inelastic mean free path inside the material is found to be of good approximation.

  14. Simple model of bulk and surface excitation effects to inelastic scattering in low-energy electron beam irradiation of multi-walled carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Kyriakou, Ioanna; Emfietzoglou, Dimitris; Garcia-Molina, Rafael; Abril, Isabel; Kostarelos, Kostas

    2011-09-01

    The effect of bulk and surface excitations to inelastic scattering in low-energy electron beam irradiation of multi-walled carbon nanotubes (MWNTs) is studied using the dielectric formalism. Calculations are based on a semiempirical dielectric response function for MWCNTs determined by means of a many-pole plasmon model with parameters adjusted to available experimental spectroscopic data under theoretical sum-rule constrains. Finite-size effects are considered in the context of electron gas theory via a boundary correction term in the plasmon dispersion relations, thus, allowing a more realistic extrapolation of the electronic excitation spectrum over the whole energy-momentum plane. Energy-loss differential and total inelastic scattering cross sections as a function of electron energy and distance from the surface, valid over the energy range ˜50-30,000 eV, are calculated with the individual contribution of bulk and surface excitations separated and analyzed for the case of normally incident and escaping electrons. The sensitivity of the results to the various approximations for the spatial dispersion of the electronic excitations is quantified. Surface excitations are shown to have a strong influence upon the shape and intensity of the energy-loss differential cross section in the near surface region whereas the general notion of a spatially invariant inelastic mean free path inside the material is found to be of good approximation.

  15. Rotational and translational effects in collisions of electronically excited diatomic hydrides

    NASA Technical Reports Server (NTRS)

    Crosley, David R.

    1988-01-01

    Collisional quenching and vibrational energy proceed competitively with rotational energy transfer for several excited states of the diatomic radicals OH, NH, and CH. This occurs for a wide variety of molecular collision partners. This phenomenon permits the examination of the influence of rotational motion on the collision dynamics of these theoretically tractable species. Measurements can also be made as a function of temperature, i.e., collision velocity. In OH (sup 2 sigma +), both vibrational transfer and quenching are found to decrease with an increase in rotational level, while quenching decreases with increasing temperature. This behavior indicates that for OH, anisotropic attractive forces govern the entrance channel dynamics for these collisions. The quenching of NH (sup 3 pi sub i) by many (although not all) collision partners also decreases with increasing rotational and translational energy, and NH (sup 1 pi) behaves much like OH (sup 2 sigma +). However, the quenching of CH (sup 2 delta) appears to decrease with increasing rotation but increases with increasing temperature, suggesting in this case anisotropic forces involving a barrier or repulsive wall. Such similarities and differences should furnish useful comparisons with both simple and detailed theoretical pictures of the appropriate collision dynamics.

  16. Electron impact vibrational excitation of methyl chloride

    NASA Astrophysics Data System (ADS)

    Sakaamini, Ahmad; Hargreaves, Leigh; Khakoo, Murtadha

    2016-05-01

    Low energy differential cross sections and excitation functions for vibrational excitation of CH3 Cl are presented for five vibrational features in the electron energy loss spectrum of this molecule. Electron energies range from 1 eV to 15 eV and scattering angles from 10o to 125o. Results will be compared to existing data for CH3 Cl in the literature. Funded by a NSF-AMOP-RUI Grant.

  17. Electronic excitation of CO by positron impact

    SciTech Connect

    Silva, Euclimar P. da; Varella, Marcio T. do N; Lima, Marco A. P.

    2005-12-15

    We report calculated cross sections for the electronic excitation of carbon monoxide by positron impact. The calculations were carried out with the Schwinger multichannel method and included six collision channels, namely the ground (X {sup 1}{sigma}{sup +}) and five electronically excited (A {sup 1}{pi}, I {sup 1}{sigma}{sup -} and D {sup 1}{delta}) states. Present calculated excitation cross sections to the A {sup 1}{pi} state did not present any resonant features, being in this sense consistent with previous calculations for the isoelectronic nitrogen molecule. The experimental a {sup 1}{pi}{sub g} excitation cross section of N{sub 2} presented a resonantlike structure which would also be expected in the A {sup 1}{pi} excitation of CO. We discuss possible reasons for the disagreement between experiment and theory.

  18. Effect of multipole excitations in electron energy-loss spectroscopy of surface plasmon modes in silver nanowires

    SciTech Connect

    Zhou, Xiuli; Norris, Theodore B.; Hörl, Anton; Trügler, Andreas; Hohenester, Ulrich; Herzing, Andrew A.

    2014-12-14

    We have characterized the surface plasmon resonance (SPR) in silver nanowires using spatially resolved electron energy loss spectroscopy (EELS) in the scanning transmission electron microscope. Non-symmetric EELS spectra due to high-k SPR propagation along the nanowire and spectral shifts due to higher-order mode excitation are observed when the beam is positioned near the tip of the nanowire. When the beam is far from the tip region and on the side of nanowire, no spectral shifts are observed as the beam is scanned in the radial direction of the nanowire. The experimental spectra are compared with three different theoretical approaches: direct numerical calculation of the energy loss, analytical models for energy loss, and numerical simulations using an optical model. All three models reproduce the spectral shifts as the electron beam approaches the cap of the nanowire. The analytical model reveals the origin of the shifts in high-order plasmon mode excitation.

  19. Electron-impact excitation of neon

    NASA Astrophysics Data System (ADS)

    Ballance, Connor; Griffin, Don

    2004-05-01

    A number of convergent close-coupling and R-matrix with pseudo-state (RMPS) calculations on H-like, He-like, Li-like, and Be-like ions have demonstrated that coupling to the target continuum can have large effects on the electron-impact excitation cross sections of neutral and low-charge species. However, no one has yet attempted such advanced calculations on a system as complex as neutral neon. We report on a series of RMPS calculations of electron-impact excitation of Ne using recently developed parallel Breit-Pauli (BP) R-matrix programs. Our largest calculation was a BP calculation with 235 spectroscopic and pseudo levels in the close-coupling expansion. Although the results of this calculation clearly reveal the importance of coupling to the target continuum in this atom, the pseudo-state expansion is not yet sufficiently complete to provide reliable cross sections for energies above the ionization limit. However, this is the largest BP calculation that can be performed with present computer resources. Thus, we have also carried out a series of RMPS calculations in LS coupling with different pseudo-state expansions. Comparisons of these results have allowed us to determine the approximate size of the pseudo-state expansion required to achieve convergence in future BP calculations for neon.

  20. Electronically excited states of PANH anions.

    PubMed

    Theis, Mallory L; Candian, Alessandra; Tielens, Alexander G G M; Lee, Timothy J; Fortenberry, Ryan C

    2015-06-14

    The singly deprotonated anion derivatives of nitrogenated polycyclic aromatic hydrocarbons (PANHs) are investigated for their electronically excited state properties. These include single deprotonation of the two unique arrangements of quinoline producing fourteen different isomers. This same procedure is also undertaken for single deprotonation of the three nitrogenation isomers of acridine and the three of pyrenidine. It is shown quantum chemically that the quinoline-class of PANH anion derivatives can only produce a candidate dipole-bound excited state each, a state defined as the interaction of an extra electron with the dipole moment of the corresponding neutral. However, the acridine- and pyrenidine-classes possess valence excited states as well as the possible dipole-bound excited states where the latter is only possible if the dipole moment is sufficiently large to retain the extra electron; the valence excitation is independent of the radical dipolar strength. As a result, the theoretical vertically computed electronic spectra of deprotonated PANH anion derivatives is fairly rich in the 1.5 eV to 2.5 eV range significantly opening the possibilities for these molecules to be applied to longer wavelength studies of visible and near-IR spectroscopy. Lastly, the study of these systems is also enhanced by the inclusion of informed orbital arrangements in a simply constructed basis set that is shown to be more complete and efficient than standard atom-centered functions. PMID:25975430

  1. ELECTRON-IMPACT EXCITATION OF Cr II: A THEORETICAL CALCULATION OF EFFECTIVE COLLISION STRENGTHS FOR OPTICALLY ALLOWED TRANSITIONS

    SciTech Connect

    Wasson, I. R.; Ramsbottom, C. A.; Scott, M. P.

    2011-10-01

    In this paper, we present electron-impact excitation collision strengths and Maxwellian averaged effective collision strengths for the complicated iron-peak ion Cr II. We consider specifically the allowed lines for transitions from the 3d {sup 5} and 3d {sup 4}4s even parity configuration states to the 3d {sup 4}4p odd parity configuration levels. The parallel suite of R-Matrix packages, RMATRX II, which have recently been extended to allow for the inclusion of relativistic effects, were used to compute the collision cross sections. A total of 108 LS{pi}/280 J{pi} levels from the basis configurations 3d {sup 5}, 3d {sup 4}4s, and 3d {sup 4}4p were included in the wavefunction representation of the target including all doublet, quartet, and sextet terms. Configuration interaction and correlation effects were carefully considered by the inclusion of seven more configurations and a pseudo-corrector 4d-bar type orbital. The 10 configurations incorporated into the Cr II model thus listed are 3d {sup 5}, 3d {sup 4}4s, 3d {sup 4}4p, 3d {sup 3}4s {sup 2}, 3d {sup 3}4p {sup 2}, 3d {sup 3}4s4p, 3d{sup 4}4d-bar, 3d{sup 3}4s4d-bar, 3d{sup 3}4p4d-bar, and 3d{sup 3}4d-bar{sup 2}, constituting the largest Cr II target model considered to date in a scattering calculation. The Maxwellian averaged effective collision strengths are computed for a wide range of electron temperatures 2000-100,000 K which are astrophysically significant. Care has been taken to ensure that the partial wave contributions to the collision strengths for these allowed lines have converged with 'top-up' from the Burgess-Tully sum rule incorporated. Comparisons are made with the results of Bautista et al. and significant differences are found for some of the optically allowed lines considered.

  2. Electronic excitation in bulk and nanocrystalline alkali halides.

    PubMed

    Bichoutskaia, Elena; Pyper, Nicholas C

    2012-11-14

    The lowest energy excitations in bulk alkali halides are investigated by considering five different excited state descriptions. It is concluded that excitation transfers one outermost halide electron in the fully ionic ground state to the lowest energy vacant s orbital of one closest cation neighbour to produce the excited state termed dipolar. The excitation energies of seven salts were computed using shell model description of the lattice polarization produced by the effective dipole moment of the excited state neutral halogen-neutral metal pair. Ab initio uncorrelated short-range inter-ionic interactions computed from anion wavefunctions adapted to the in-crystal environment were augmented by short-range electron correlation contributions derived from uniform electron-gas density functional theory. Dispersive attractions including wavefunction overlap damping were introduced using reliable semi-empirical dispersion coefficients. The good agreement between the predicted excitation energies and experiment provides strong evidence that the excited state is dipolar. In alkali halide nanocrystals in which each ionic plane contains only four ions, the Madelung energies are significantly reduced compared with the bulk. This predicts that the corresponding intra-crystal excitation energies in the nanocrystals, where there are two excited states depending on whether the halide electron is transferred to a cation in the same or in the neighbouring plane, will be reduced by almost 2 eV. For such an encapsulated KI crystal, it has been shown that the greater polarization in the excited state of the bulk crystal causes these reductions to be lowered to a 1.1 eV-1.5 eV range for the case of charge transfer to a neighbouring plane. For intra-plane charge transfer the magnitude of the polarization energy is further reduced thus causing the excitation in these encapsulated materials to be only 0.2 eV less than in the bulk crystal. PMID:23163361

  3. Collisional excitation of electron Landau levels in strong magnetic fields

    NASA Technical Reports Server (NTRS)

    Langer, S. H.

    1981-01-01

    The cross sections for the excitation and deexcitation of the quantized transverse energy levels of an electron in a magnetic field are calculated for electron-proton and electron-electron collisions in light of the importance of the cross sections for studies of X-ray pulsar emission. First-order matrix elements are calculated using the Dirac theory of the electron, thus taking into account relativistic effects, which are believed to be important in accreting neutron stars. Results for the collisional excitation of ground state electrons by protons are presented which demonstrate the importance of proton recoil and relativistic effects, and it is shown that electron-electron excitations may contribute 10 to 20% of the excitation rate from electron-proton scattering in a Maxwellian plasma. Finally, calculations of the cross section for electron-proton small-angle scattering are presented which lead to relaxation rates for the electron velocity distribution which are modified by the magnetic field, and to a possible increase in the value of the Coulomb logarithm.

  4. Electron-impact vibrational excitation of cyclopropane

    SciTech Connect

    Čurík, R. Čársky, P.; Allan, M.

    2015-04-14

    We report a very detailed test of the ab initio discrete momentum representation (DMR) method of calculating vibrational excitation of polyatomic molecules by electron impact, by comparison of its results with an extensive set of experimental data, covering the entire range of scattering angles from 10{sup ∘} to 180{sup ∘} and electron energies from 0.4 to 20 eV. The DMR calculations were carried out by solving the two-channel Lippmann-Schwinger equation in the momentum space, and the interaction between the scattered electron and the target molecule was described by exact static-exchange potential corrected by a density functional theory (DFT) correlation-polarization interaction that models target’s response to the field of incoming electron. The theory is found to quantitatively reproduce the measured spectra for all normal modes, even at the difficult conditions of extreme angles and at low energies, and thus provides full understanding of the excitation mechanism. It is shown that the overlap of individual vibrational bands caused by limited experimental resolution and rotational excitation must be properly taken into account for correct comparison of experiment and theory. By doing so, an apparent discrepancy between published experimental data could be reconciled. A substantial cross section is found for excitation of the non-symmetric HCH twisting mode ν{sub 4} of A{sub 1}{sup ″} symmetry by the 5.5 eV A{sub 2}{sup ′} resonance, surprisingly because the currently accepted selection rules predict this process to be forbidden. The DMR theory shows that the excitation is caused by an incoming electron in an f-wave of A{sub 2}{sup ′} symmetry which causes excitation of the non-symmetric HCH twisting mode ν{sub 4} of the A{sub 1}{sup ″} symmetry and departs in p- and f-waves of A{sub 2}{sup ″} symmetry.

  5. Reactive and internal contributions to the thermal conductivity of local thermodynamic equilibrium nitrogen plasma: The effect of electronically excited states

    NASA Astrophysics Data System (ADS)

    Bruno, D.; Colonna, G.; Laricchiuta, A.; Capitelli, M.

    2012-12-01

    Internal and reactive contributions to the thermal conductivity of a local thermodynamic equilibrium nitrogen plasma have been calculated using the Chapman-Enskog method. Low-lying (LL) electronically excited states (i.e., states with the same principal quantum number of the ground state) and high-lying (HL) ones (i.e., states with principal quantum number n > 2) have been considered. Several models have been developed, the most accurate being a model that treats the LL states as separate species while disregarding the presence of HL states, on account of their enormous transport cross sections.

  6. Reactive and internal contributions to the thermal conductivity of local thermodynamic equilibrium nitrogen plasma: The effect of electronically excited states

    SciTech Connect

    Bruno, D.; Colonna, G.; Laricchiuta, A.; Capitelli, M.

    2012-12-15

    Internal and reactive contributions to the thermal conductivity of a local thermodynamic equilibrium nitrogen plasma have been calculated using the Chapman-Enskog method. Low-lying (LL) electronically excited states (i.e., states with the same principal quantum number of the ground state) and high-lying (HL) ones (i.e., states with principal quantum number n> 2) have been considered. Several models have been developed, the most accurate being a model that treats the LL states as separate species while disregarding the presence of HL states, on account of their enormous transport cross sections.

  7. Electron-impact excitation of nitric oxide.

    NASA Technical Reports Server (NTRS)

    Stone, E. J.; Zipf, E. C.

    1972-01-01

    The absolute cross sections for the excitation of the nitrosyl cation Baer-Miescher bands, two nitric oxide bands, and several atomic nitrogen multiplets in the vacuum UV by electron impact on NO have been measured over an energy range extending from threshold to 300 eV. The variation of the dipole transition moment for the nitrosyl cation band system was also determined.

  8. Femtosecond Timescale Evolution of Pyrrole Electronic Excitation

    NASA Astrophysics Data System (ADS)

    Montero, Raul; Conde, Alvaro Peralta; Ovejas, Virginia; Castano, Fernando; Longarte, Asier

    2012-06-01

    Pyrrole is a simple aromatic molecule with relevantchromophoric properties in biology. Although its apparent simplicity, it shows a complicated dynamics after excitation in the near part of the UV absorption spectrum, which results from the interplay between the bright ππ^* and the dark dissociative πσ^* electronic transitions. Herein, we present a time resolved study with ultrafast resolution on the relaxation dynamics of isolated pyrrole, after excitation in the 265-217 nm range. Two lifetimes of 19 and 15 fs, which are associated with the internal conversion from the bright 1B2 ππ^* state and the propagation of the wavepacket on the πσ^* state, respectively, are found in the studied energy interval. The work also explores the consequences of non resonant adiabatic excitation of the system when broadband femtosecond pulses are employed to prepare the molecule in the targeted electronic states, revealing the key implication of this type of coherent phenomena. The collected data reveal that the bright 1B2 ππ^* state is adiabatically populated at excitation wavelengths far away from resonance, providing an efficient way to reach the πσ^* state. The recorded transients are fit employing a coherent model that provides a comprehensive view of the dynamical processes pyrrole undergoes after excitation by ultrashort light pulses. M. N. R. Ashfold, B. Cronin, A. L. Devine, R. N. Dixon and M. G. D. Nix Science, 312, 1637-1640, 2006.

  9. Electron-driven excitations and dissociation of molecules

    SciTech Connect

    Miller, Greg; Orel, Ann E.

    2015-02-13

    This program studied how energy is interchanged in electron and photon collisions with molecules leading to ex-citation and dissociation. Modern ab initio techniques, both for the photoionization and electron scattering, and the subsequent nuclear dynamics studies, are used to accurately treat these problems. This work addresses vibrational ex-citation and dissociative attachment following electron impact, and the dynamics following inner shell photoionzation. These problems are ones for which a full multi-dimensional treatment of the nuclear dynamics is essential and where non-adiabatic effects are expected to be important.

  10. Electron Impact Excitation Of Ti XIX

    NASA Astrophysics Data System (ADS)

    Aggarwal, Kanti M.; Keenan, F. P.

    2012-05-01

    Emission lines of Ti XIX are important for the modeling and diagnostics of lasing, fusion and astrophysical plasmas, for which atomic data are required for a variety of parameters, such as energy levels, radiative rates (A- values), and excitation rates or equivalently the effective collision strengths (Υ), which are obtained from the electron impact collision strengths (Ω). Experimentally, energy levels are available for Ti XIX on the NIST website, but there is paucity for accurate collisional atomic data. Therefore, here we report a complete set of results (namely energy levels, radiative rates, and effective collision strengths) for all transitions among the lowest 98 levels of Ti XIX. These levels belong to the (1s2) 2s2, 2s2p, 2p2, 2s3l, 2p3l, 2s4l, and 2p4l configurations. Finally, we also report the A- values for four types of transitions, namely electric dipole (E1), electric quadrupole (E2), magnetic dipole (M1), and magnetic quadrupole (M2), because these are also required for plasma modeling. For our calculations of wavefunctions, we have adopted the fully relativistic GRASP code, and for the calculations of Ω, the Dirac atomic R-matrix code (DARC) of PH Norrington and IP Grant. Additionally, parallel calculations have also been performed with the Flexible Atomic Code (FAC) of Gu, so that all atomic parameters can be rigorously assessed for accuracy.

  11. Concepts of Highly Excited Electronic Systems

    NASA Astrophysics Data System (ADS)

    Berakdar, Jamal

    2003-05-01

    Knowledge of the excitation characteristics of matter is decisive for the descriptions of a variety of dynamical processes, which are of significant technological interest. E.g. transport properties and the optical response are controlled by the excitation spectrum. This self-contained work is a coherent presentation of the quantum theory of correlated few-particle excitations in electronic systems. It begins with a compact resume of the quantum mechanics of single particle excitations. Particular emphasis is put on Green function methods, which offer a natural tool to unravel the relations between the physics of small and large electronic systems. The book contains explicit expressions for the Coulomb Green function of two charge particles and a generalization to three-body systems. Techniques for the many-body Green function of finite systems are introduced and some explicit calculations of the Green functions are given. Concrete examples are provided and the theories are contrasted with experimental data, when available. The second volume presents an up-to-date selection of applications of the developed concepts and a comparison with available experiments is made

  12. Solvent Effects on the Electronic Absorption and Fluorescence Spectra of HNP: Estimation of Ground and Excited State Dipole Moments.

    PubMed

    Desai, Vani R; Hunagund, Shirajahammad M; Basanagouda, Mahantesha; Kadadevarmath, Jagadish S; Sidarai, Ashok H

    2016-07-01

    We report the effect of solvents on absorption and fluorescence spectra of biologically active 3(2H)-pyridazinone namely 5-(2-hydroxy-naphthalen-1-yl)-2-phenyl-2H-pyridazin-3-one (HNP) in different solvents at room temperature. The ground and the excited state dipole moments of HNP molecule was estimated from Lippert's, Bakshiev's and Kawski-Chamma-Viallet's equations using the solvatochromic shift method. The ground state dipole moment (μ g ) was also estimated by Guggenheim and Higasi method using the dielectric constant and refractive index of solute at different concentrations, the μ g value obtained from these two methods are comparable to the μ g value obtained by the solvatochromic shift method. The excited state dipole moment (μ e ) is greater than the ground state dipole moment (μ g ), which indicates that the excited state is more polar than the ground state. Further, we have evaluated the change in dipole moment (Δμ) from the solvatochromic shift method and on the basis of molecular-microscopic solvent polarity parameter[Formula: see text], later on the values were compared. PMID:27220623

  13. Search for excited electrons at HERA

    NASA Astrophysics Data System (ADS)

    H1 Collaboration; Adloff, C.; Andreev, V.; Andrieu, B.; Anthonis, T.; Astvatsatourov, A.; Babaev, A.; Bähr, J.; Baranov, P.; Barrelet, E.; Bartel, W.; Baumgartner, S.; Becker, J.; Beckingham, M.; Beglarian, A.; Behnke, O.; Belousov, A.; Berger, Ch.; Berndt, T.; Bizot, J. C.; Böhme, J.; Boudry, V.; Braunschweig, W.; Brisson, V.; Bröker, H.-B.; Brown, D. P.; Bruncko, D.; Büsser, F. W.; Bunyatyan, A.; Burrage, A.; Buschhorn, G.; Bystritskaya, L.; Campbell, A. J.; Caron, S.; Cassol-Brunner, F.; Clarke, D.; Collard, C.; Contreras, J. G.; Coppens, Y. R.; Coughlan, J. A.; Cousinou, M.-C.; Cox, B. E.; Cozzika, G.; Cvach, J.; Dainton, J. B.; Dau, W. D.; Daum, K.; Davidsson, M.; Delcourt, B.; Delerue, N.; Demirchyan, R.; de Roeck, A.; de Wolf, E. A.; Diaconu, C.; Dingfelder, J.; Dixon, P.; Dodonov, V.; Dowell, J. D.; Droutskoi, A.; Dubak, A.; Duprel, C.; Eckerlin, G.; Eckstein, D.; Efremenko, V.; Egli, S.; Eichler, R.; Eisele, F.; Eisenhandler, E.; Ellerbrock, M.; Elsen, E.; Erdmann, M.; Erdmann, W.; Faulkner, P. J. W.; Favart, L.; Fedotov, A.; Felst, R.; Ferencei, J.; Ferron, S.; Fleischer, M.; Fleischmann, P.; Fleming, Y. H.; Flügge, G.; Fomenko, A.; Foresti, I.; Formánek, J.; Franke, G.; Frising, G.; Gabathuler, E.; Gabathuler, K.; Garvey, J.; Gassner, J.; Gayler, J.; Gerhards, R.; Gerlich, C.; Ghazaryan, S.; Goerlich, L.; Gogitidze, N.; Grab, C.; Grabski, V.; Grässler, H.; Greenshaw, T.; Grindhammer, G.; Hadig, T.; Haidt, D.; Hajduk, L.; Haller, J.; Heinemann, B.; Heinzelmann, G.; Henderson, R. C. W.; Hengstmann, S.; Henschel, H.; Heremans, R.; Herrera, G.; Herynek, I.; Hildebrandt, M.; Hilgers, M.; Hiller, K. H.; Hladký, J.; Höting, P.; Hoffmann, D.; Horisberger, R.; Hovhannisyan, A.; Hurling, S.; Ibbotson, M.; Işsever, Ç.; Jacquet, M.; Jaffre, M.; Janauschek, L.; Janssen, X.; Jemanov, V.; Jönsson, L.; Johnson, C.; Johnson, D. P.; Jones, M. A. S.; Jung, H.; Kant, D.; Kapichine, M.; Karlsson, M.; Karschnick, O.; Katzy, J.; Keil, F.; Keller, N.; Kennedy, J.; Kenyon, I. R.; Kiesling, C.; Kjellberg, P.; Klein, M.; Kleinwort, C.; Kluge, T.; Knies, G.; Koblitz, B.; Kolya, S. D.; Korbel, V.; Kostka, P.; Kotelnikov, S. K.; Koutouev, R.; Koutov, A.; Kroseberg, J.; Krüger, K.; Kuhr, T.; Lamb, D.; Landon, M. P. J.; Lange, W.; Laštovička, T.; Laycock, P.; Lebailly, E.; Lebedev, A.; Leißner, B.; Lemrani, R.; Lendermann, V.; Levonian, S.; List, B.; Lobodzinska, E.; Lobodzinski, B.; Loginov, A.; Loktionova, N.; Lubimov, V.; Lüders, S.; Lüke, D.; Lytkin, L.; Malden, N.; Malinovski, E.; Mangano, S.; Maraček, R.; Marage, P.; Marks, J.; Marshall, R.; Martyn, H.-U.; Martyniak, J.; Maxfield, S. J.; Meer, D.; Mehta, A.; Meier, K.; Meyer, A. B.; Meyer, H.; Meyer, J.; Michine, S.; Mikocki, S.; Milstead, D.; Mohrdieck, S.; Mondragon, M. N.; Moreau, F.; Morozov, A.; Morris, J. V.; Müller, K.; Murín, P.; Nagovizin, V.; Naroska, B.; Naumann, J.; Naumann, Th.; Newman, P. R.; Niebergall, F.; Niebuhr, C.; Nix, O.; Nowak, G.; Nozicka, M.; Olivier, B.; Olsson, J. E.; Ozerov, D.; Panassik, V.; Pascaud, C.; Patel, G. D.; Peez, M.; Perez, E.; Petrukhin, A.; Phillips, J. P.; Pitzl, D.; Pöschl, R.; Potachnikova, I.; Povh, B.; Rauschenberger, J.; Reimer, P.; Reisert, B.; Risler, C.; Rizvi, E.; Robmann, P.; Roosen, R.; Rostovtsev, A.; Rusakov, S.; Rybicki, K.; Sankey, D. P. C.; Schätzel, S.; Scheins, J.; Schilling, F.-P.; Schleper, P.; Schmidt, D.; Schmidt, D.; Schmidt, S.; Schmitt, S.; Schneider, M.; Schoeffel, L.; Schöning, A.; Schörner, T.; Schröder, V.; Schultz-Coulon, H.-C.; Schwanenberger, C.; Sedlák, K.; Sefkow, F.; Shekelyan, V.; Sheviakov, I.; Shtarkov, L. N.; Sirois, Y.; Sloan, T.; Smirnov, P.; Soloviev, Y.; South, D.; Spaskov, V.; Specka, A.; Spitzer, H.; Stamen, R.; Stella, B.; Stiewe, J.; Strauch, I.; Straumann, U.; Tchetchelnitski, S.; Thompson, G.; Thompson, P. D.; Tomasz, F.; Traynor, D.; Truöl, P.; Tsipolitis, G.; Tsurin, I.; Turnau, J.; Turney, J. E.; Tzamariudaki, E.; Uraev, A.; Urban, M.; Usik, A.; Valkár, S.; Valkárová, A.; Vallée, C.; van Mechelen, P.; Vargas Trevino, A.; Vassiliev, S.; Vazdik, Y.; Veelken, C.; Vest, A.; Vichnevski, A.; Wacker, K.; Wagner, J.; Wallny, R.; Waugh, B.; Weber, G.; Wegener, D.; Werner, C.; Werner, N.; Wessels, M.; White, G.; Wiesand, S.; Wilksen, T.; Winde, M.; Winter, G.-G.; Wissing, Ch.; Wobisch, M.; Woehrling, E.-E.; Wünsch, E.; Wyatt, A. C.; Žáček, J.; Zálešák, J.; Zhang, Z.; Zhokin, A.; Zomer, F.; Zur Nedden, M.

    2002-11-01

    A search for excited electron (e*) production is described in which the electroweak decays e*-->eγ, e*-->eZ and e*-->νW are considered. The data used correspond to an integrated luminosity of 120 pb-1 taken in e+/-p collisions from 1994 to 2000 with the H1 detector at HERA at centre-of-mass energies of 300 and 318 GeV. No evidence for a signal is found. Mass dependent exclusion limits are derived for the ratio of the couplings to the compositeness scale, /f/Λ. These limits extend the excluded region to higher masses than has been possible in previous direct searches for excited electrons.

  14. Search for excited electrons at HERA

    NASA Astrophysics Data System (ADS)

    Adloff, C.; Andreev, V.; Andrieu, B.; Anthonis, T.; Astvatsatourov, A.; Babaev, A.; Bähr, J.; Baranov, P.; Barrelet, E.; Bartel, W.; Baumgartner, S.; Becker, J.; Beckingham, M.; Beglarian, A.; Behnke, O.; Belousov, A.; Berger, Ch.; Berndt, T.; Bizot, J. C.; Böhme, J.; Boudry, V.; Braunschweig, W.; Brisson, V.; Bröker, H.-B.; Brown, D. P.; Bruncko, D.; Büsser, F. W.; Bunyatyan, A.; Burrage, A.; Buschhorn, G.; Bystritskaya, L.; Campbell, A. J.; Caron, S.; Cassol-Brunner, F.; Clarke, D.; Collard, C.; Contreras, J. G.; Coppens, Y. R.; Coughlan, J. A.; Cousinou, M.-C.; Cox, B. E.; Cozzika, G.; Cvach, J.; Dainton, J. B.; Dau, W. D.; Daum, K.; Davidsson, M.; Delcourt, B.; Delerue, N.; Demirchyan, R.; De Roeck, A.; De Wolf, E. A.; Diaconu, C.; Dingfelder, J.; Dixon, P.; Dodonov, V.; Dowell, J. D.; Droutskoi, A.; Dubak, A.; Duprel, C.; Eckerlin, G.; Eckstein, D.; Efremenko, V.; Egli, S.; Eichler, R.; Eisele, F.; Eisenhandler, E.; Ellerbrock, M.; Elsen, E.; Erdmann, M.; Erdmann, W.; Faulkner, P. J. W.; Favart, L.; Fedotov, A.; Felst, R.; Ferencei, J.; Ferron, S.; Fleischer, M.; Fleischmann, P.; Fleming, Y. H.; Flügge, G.; Fomenko, A.; Foresti, I.; Formánek, J.; Franke, G.; Frising, G.; Gabathuler, E.; Gabathuler, K.; Garvey, J.; Gassner, J.; Gayler, J.; Gerhards, R.; Gerlich, C.; Ghazaryan, S.; Goerlich, L.; Gogitidze, N.; Grab, C.; Grabski, V.; Grässler, H.; Greenshaw, T.; Grindhammer, G.; Hadig, T.; Haidt, D.; Hajduk, L.; Haller, J.; Heinemann, B.; Heinzelmann, G.; Henderson, R. C. W.; Hengstmann, S.; Henschel, H.; Heremans, R.; Herrera, G.; Herynek, I.; Hildebrandt, M.; Hilgers, M.; Hiller, K. H.; Hladký, J.; Höting, P.; Hoffmann, D.; Horisberger, R.; Hovhannisyan, A.; Hurling, S.; Ibbotson, M.; İşsever, Ç.; Jacquet, M.; Jaffre, M.; Janauschek, L.; Janssen, X.; Jemanov, V.; Jönsson, L.; Johnson, C.; Johnson, D. P.; Jones, M. A. S.; Jung, H.; Kant, D.; Kapichine, M.; Karlsson, M.; Karschnick, O.; Katzy, J.; Keil, F.; Keller, N.; Kennedy, J.; Kenyon, I. R.; Kiesling, C.; Kjellberg, P.; Klein, M.; Kleinwort, C.; Kluge, T.; Knies, G.; Koblitz, B.; Kolya, S. D.; Korbel, V.; Kostka, P.; Kotelnikov, S. K.; Koutouev, R.; Koutov, A.; Kroseberg, J.; Krüger, K.; Kuhr, T.; Lamb, D.; Landon, M. P. J.; Lange, W.; Laštovička, T.; Laycock, P.; Lebailly, E.; Lebedev, A.; Leißner, B.; Lemrani, R.; Lendermann, V.; Levonian, S.; List, B.; Lobodzinska, E.; Lobodzinski, B.; Loginov, A.; Loktionova, N.; Lubimov, V.; Lüders, S.; Lüke, D.; Lytkin, L.; Malden, N.; Malinovski, E.; Mangano, S.; Maraček, R.; Marage, P.; Marks, J.; Marshall, R.; Martyn, H.-U.; Martyniak, J.; Maxfield, S. J.; Meer, D.; Mehta, A.; Meier, K.; Meyer, A. B.; Meyer, H.; Meyer, J.; Michine, S.; Mikocki, S.; Milstead, D.; Mohrdieck, S.; Mondragon, M. N.; Moreau, F.; Morozov, A.; Morris, J. V.; Müller, K.; Murín, P.; Nagovizin, V.; Naroska, B.; Naumann, J.; Naumann, Th.; Newman, P. R.; Niebergall, F.; Niebuhr, C.; Nix, O.; Nowak, G.; Nozicka, M.; Olivier, B.; Olsson, J. E.; Ozerov, D.; Panassik, V.; Pascaud, C.; Patel, G. D.; Peez, M.; Perez, E.; Petrukhin, A.; Phillips, J. P.; Pitzl, D.; Pöschl, R.; Potachnikova, I.; Povh, B.; Rauschenberger, J.; Reimer, P.; Reisert, B.; Risler, C.; Rizvi, E.; Robmann, P.; Roosen, R.; Rostovtsev, A.; Rusakov, S.; Rybicki, K.; Sankey, D. P. C.; Schätzel, S.; Scheins, J.; Schilling, F.-P.; Schleper, P.; Schmidt, D.; Schmidt, D.; Schmidt, S.; Schmitt, S.; Schneider, M.; Schoeffel, L.; Schöning, A.; Schörner, T.; Schröder, V.; Schultz-Coulon, H.-C.; Schwanenberger, C.; Sedlák, K.; Sefkow, F.; Shekelyan, V.; Sheviakov, I.; Shtarkov, L. N.; Sirois, Y.; Sloan, T.; Smirnov, P.; Soloviev, Y.; South, D.; Spaskov, V.; Specka, A.; Spitzer, H.; Stamen, R.; Stella, B.; Stiewe, J.; Strauch, I.; Straumann, U.; Tchetchelnitski, S.; Thompson, G.; Thompson, P. D.; Tomasz, F.; Traynor, D.; Truöl, P.; Tsipolitis, G.; Tsurin, I.; Turnau, J.; Turney, J. E.; Tzamariudaki, E.; Uraev, A.; Urban, M.; Usik, A.; Valkár, S.; Valkárová, A.; Vallée, C.; Van Mechelen, P.; Vargas Trevino, A.; Vassiliev, S.; Vazdik, Y.; Veelken, C.; Vest, A.; Vichnevski, A.; Wacker, K.; Wagner, J.; Wallny, R.; Waugh, B.; Weber, G.; Wegener, D.; Werner, C.; Werner, N.; Wessels, M.; White, G.; Wiesand, S.; Wilksen, T.; Winde, M.; Winter, G.-G.; Wissing, Ch.; Wobisch, M.; Woehrling, E.-E.; Wünsch, E.; Wyatt, A. C.; Žáček, J.; Zálešák, J.; Zhang, Z.; Zhokin, A.; Zomer, F.; zur Nedden, M.; H1 Collaboration

    2002-11-01

    A search for excited electron (e∗) production is described in which the electroweak decays e∗→eγ, e∗→eZ and e∗→νW are considered. The data used correspond to an integrated luminosity of 120 pb-1 taken in e±p collisions from 1994 to 2000 with the H1 detector at HERA at centre-of-mass energies of 300 and 318 GeV. No evidence for a signal is found. Mass dependent exclusion limits are derived for the ratio of the couplings to the compositeness scale, f/Λ. These limits extend the excluded region to higher masses than has been possible in previous direct searches for excited electrons.

  15. Electron impact excitation of SF6

    NASA Technical Reports Server (NTRS)

    Trajmar, S.; Chutjian, A.

    1977-01-01

    A study of the electron impact energy-loss spectrum of SF6 under both optical (low scattering angle, high impact energy) and non-optical conditions (high scattering angle, low impact energy) has revealed a number of electronic excitation processes. With the help of theoretical calculations, several of these transitions have been assigned and approximate cross sections associated with four features have been determined. In addition, a strong resonance at 12 eV has been observed in both elastic and vibrationally inelastic (delta E = 0.092 eV) channels.

  16. Four-electron model for singlet and triplet excitation energy transfers with inclusion of coherence memory, inelastic tunneling and nuclear quantum effects

    NASA Astrophysics Data System (ADS)

    Suzuki, Yosuke; Ebina, Kuniyoshi; Tanaka, Shigenori

    2016-08-01

    A computational scheme to describe the coherent dynamics of excitation energy transfer (EET) in molecular systems is proposed on the basis of generalized master equations with memory kernels. This formalism takes into account those physical effects in electron-bath coupling system such as the spin symmetry of excitons, the inelastic electron tunneling and the quantum features of nuclear motions, thus providing a theoretical framework to perform an ab initio description of EET through molecular simulations for evaluating the spectral density and the temporal correlation function of electronic coupling. Some test calculations have then been carried out to investigate the dependence of exciton population dynamics on coherence memory, inelastic tunneling correlation time, magnitude of electronic coupling, quantum correction to temporal correlation function, reorganization energy and energy gap.

  17. The electronic couplings in electron transfer and excitation energy transfer.

    PubMed

    Hsu, Chao-Ping

    2009-04-21

    The transport of charge via electrons and the transport of excitation energy via excitons are two processes of fundamental importance in diverse areas of research. Characterization of electron transfer (ET) and excitation energy transfer (EET) rates are essential for a full understanding of, for instance, biological systems (such as respiration and photosynthesis) and opto-electronic devices (which interconvert electric and light energy). In this Account, we examine one of the parameters, the electronic coupling factor, for which reliable values are critical in determining transfer rates. Although ET and EET are different processes, many strategies for calculating the couplings share common themes. We emphasize the similarities in basic assumptions between the computational methods for the ET and EET couplings, examine the differences, and summarize the properties, advantages, and limits of the different computational methods. The electronic coupling factor is an off-diagonal Hamiltonian matrix element between the initial and final diabatic states in the transport processes. ET coupling is essentially the interaction of the two molecular orbitals (MOs) where the electron occupancy is changed. Singlet excitation energy transfer (SEET), however, contains a Frster dipole-dipole coupling as its most important constituent. Triplet excitation energy transfer (TEET) involves an exchange of two electrons of different spin and energy; thus, it is like an overlap interaction of two pairs of MOs. Strategies for calculating ET and EET couplings can be classified as (1) energy-gap-based approaches, (2) direct calculation of the off-diagonal matrix elements, or (3) use of an additional operator to describe the extent of charge or excitation localization and to calculate the coupling value. Some of the difficulties in calculating the couplings were recently resolved. Methods were developed to remove the nondynamical correlation problem from the highly precise coupled cluster

  18. Effect of Size and Structure on the Ground-State and Excited-State Electronic Structure of TiO2 Nanoparticles.

    PubMed

    Cho, Daeheum; Ko, Kyoung Chul; Lamiel-García, Oriol; Bromley, Stefan T; Lee, Jin Yong; Illas, Francesc

    2016-08-01

    We investigated the influence of size and structure on the electronic structure of TiO2 nanoparticles 0.5-3.2 nm in diameter, in both vacuum and water, using density functional theory (DFT) calculations. Specifically, we tracked the optical and electronic energy gap of a set of (TiO2)n nanoparticles ranging from small non-bulklike clusters with n = 4, 8, and 16, to larger nanoparticles derived from the anatase bulk crystal with n = 35 and 84. As the difference between these two energy gaps (the exciton binding energy) becomes negligible in the bulk, this magnitude provides an indicator of the bulklike character of the electronic structure of the nanoparticles under study. Extrapolating our results to larger sizes, we obtain a rough estimate of the nanoparticle size at which the electronic structure will begin to be effectively bulklike. Our results generally confirmed that the electronic structure of the nanoparticle ground state and excited state has a more pronounced structure dependency than size dependency within a size range of 0.5-1.5 nm. We also showed that the thermodynamic preference for the photocatalytic species is the first S1 exciton. This S1 exciton is stable under vacuum but may evolve to free charge carriers upon structural relaxation in an aqueous environment for particles 0.5-1.5 nm in size studied in the present article. An analysis of ionization potentials and electron affinities, relative to the standard reduction potential for the water splitting half-reactions, revealed the importance of considering the structural relaxation in the excited states and the presence of water for assessing the thermodynamic conditions for photocatalytic water splitting. PMID:27379415

  19. Separation of ionization and subsequent electronic excitation for formation of electronically excited ethanol cation in intense laser fields

    NASA Astrophysics Data System (ADS)

    Ikuta, T.; Hosaka, K.; Akagi, H.; Yokoyama, A.; Yamanouchi, K.; Kannari, F.; Itakura, R.

    2011-10-01

    Ionization and subsequent electronic excitation occurring within the same laser pulse (400 nm, 96 fs, 1.3 ~ 18 TW cm-2) are separately investigated by measuring in coincidence an electron and a product ion produced from C2H5OH. It is revealed that the nascent population in the electronically excited C2H5OH+ prepared by the ionization decreases as the laser intensity increases, while the subsequent electronic excitation is enhanced through the resonant electronic transitions. Ionization and electronic excitation mechanisms are described based on the electronic-state distributions of C2H5OH+.

  20. Excited S 1 state dipole moments of nitrobenzene and p-nitroaniline from thermochromic effect on electronic absorption spectra

    NASA Astrophysics Data System (ADS)

    Kawski, A.; Kukliński, B.; Bojarski, P.

    2006-11-01

    The effect of temperature on the absorption spectra of nitrobenzene (NB) and p-nitroaniline (NA) in 1,2-dichloroethane was studied for temperature ranging from 295 K to 378 K and from 296 K to 408 K, respectively. With temperature increase the absorption bands of both compounds are blue shifted, which is caused by the decrease of permittivity ɛ and refractive index n. From the band shifts and by using the Bilot and Kawski theory [ L. Bilot, A. Kawski, Z. Naturforsch. 17a (1962) 621] the dipole moments in the excited singlet state μe = 6.59 D of NB and μe = 13.35 D of NA were determined. The influence of polarizability α, the Onsager cavity radius a and dipole moment in the ground state μg on the determined values of μe are discussed. A comparison of the obtained μe values with those of other authors is given. In the case of p-NA a strong intramolecular charge transfer (ICT) was confirmed.

  1. Comparison of the quadratic configuration interaction and coupled cluster approaches to electron correlation including the effect of triple excitations

    NASA Technical Reports Server (NTRS)

    Taylor, Peter R.; Lee, Timothy J.; Rendell, Alistair P.

    1990-01-01

    The recently proposed quadratic configuration interaction (QCI) method is compared with the more rigorous coupled cluster (CC) approach for a variety of chemical systems. Some of these systems are well represented by a single-determinant reference function and others are not. The finite order singles and doubles correlation energy, the perturbational triples correlation energy, and a recently devised diagnostic for estimating the importance of multireference effects are considered. The spectroscopic constants of CuH, the equilibrium structure of cis-(NO)2 and the binding energies of Be3, Be4, Mg3, and Mg4 were calculated using both approaches. The diagnostic for estimating multireference character clearly demonstrates that the QCI method becomes less satisfactory than the CC approach as non-dynamical correlation becomes more important, in agreement with a perturbational analysis of the two methods and the numerical estimates of the triple excitation energies they yield. The results for CuH show that the differences between the two methods become more apparent as the chemical systems under investigation becomes more multireference in nature and the QCI results consequently become less reliable. Nonetheless, when the system of interest is dominated by a single reference determinant both QCI and CC give very similar results.

  2. 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.

  3. Tracing molecular electronic excitation dynamics in real time and space.

    PubMed

    Dutoi, Anthony D; Cederbaum, Lorenz S; Wormit, Michael; Starcke, Jan Hendrik; Dreuw, Andreas

    2010-04-14

    We present a method for studying the movement of electrons and energy within and between electronically excited molecules. The dynamically changing state is a many-electron wavepacket, for which we numerically integrate the Schrodinger equation using the ADC(2) effective Hamiltonian for the particle-hole propagator. We develop the tools necessary for following the separate motions of the particles and holes. Total particle and hole densities can be used to give an overview of the dynamics, which can be atomically decomposed in a Mulliken fashion, or individual particle and hole states give a more detailed look at the structure of an excitation. We apply our model to a neon chain, as an illustrative example, projecting an excited eigenstate of an isolated atom onto the coupled system as the initial state. In addition to demonstrating our propagation and analysis machinery, the results show a dramatic difference in excitation-energy transfer rates as a consequence of initial polarization. Furthermore, already in a system with three constituents, an important aspect of multiple coupled systems appears, in that one absorbing system essentially shields another, changing the effective sitewise coupling parameters. PMID:20405991

  4. Excitation of local magnetic moments by tunneling electrons

    NASA Astrophysics Data System (ADS)

    Gauyacq, Jean-Pierre; Lorente, Nicolás; Novaes, Frederico Dutilh

    2012-05-01

    The advent of milli-kelvin scanning tunneling microscopes (STM) with inbuilt magnetic fields has opened access to the study of magnetic phenomena with atomic resolution at surfaces. In the case of single atoms adsorbed on a surface, the existence of different magnetic energy levels localized on the adsorbate is due to the breaking of the rotational invariance of the adsorbate spin by the interaction with its environment, leading to energy terms in the meV range. These structures were revealed by STM experiments in IBM Almaden in the early 2000s for atomic adsorbates on CuN surfaces. The experiments consisted in the study of the changes in conductance caused by inelastic tunneling of electrons (IETS, inelastic electron tunneling spectroscopy). Manganese and Iron adatoms were shown to have different magnetic anisotropies induced by the substrate. More experiments by other groups followed up, showing that magnetic excitations could be detected in a variety of systems: e.g. complex organic molecules showed that their magnetic anisotropy was dependent on the molecular environment, piles of magnetic molecules showed that they interact via intermolecular exchange interaction, spin waves were excited on ferromagnetic surfaces and in Mn chains, and magnetic impurities have been analyzed on semiconductors. These experiments brought up some intriguing questions: the efficiency of magnetic excitations was very high, the excitations could or could not involve spin flip of the exciting electron and singular-like behavior was sometimes found at the excitation thresholds. These facts called for extended theoretical analysis; perturbation theories, sudden-approximation approaches and a strong coupling scheme successfully explained most of the magnetic inelastic processes. In addition, many-body approaches were also used to decipher the interplay between inelastic processes and the Kondo effect. Spin torque transfer has been shown to be effective in changing spin orientations of an

  5. Cumulant approach for electronic excitations in x-ray and electron spectra

    NASA Astrophysics Data System (ADS)

    Rehr, J. J.

    A quantitative treatment of electronic excitations and other many-body effects in x-ray and electron spectra has long been challenging. Physically, electronic correlations and atomic vibrations lead to inelastic losses and damping effects that are ignored in ground state methods or approximations such as TDDFT. Quasi-particle (QP) approaches such as the GW approximation yield significant improvements, as demonstrated in real-space Green's function and GW/Bethe-Salpeter equation calculations, but still ignore multi-electron excitations. Recently such excitations have been treated with considerable success using cumulant expansion techniques and the quasi-boson approximation. In this beyond QP approach, excitations such as plasmons and electron-hole excitations appear as satellites in the spectral function. The method naturally accounts for multiple-satellites and can be extended to include extrinsic losses and interference effects. Extensions for effects of vibrations and strong correlations including charge-transfer satellites may also be possible. These advances are illustrated with a number of applications. Supported by DOE Grant DE-FG02-97ER45623.

  6. High temperature electronic excitation and ionization rates in gases

    NASA Technical Reports Server (NTRS)

    Hansen, Frederick

    1991-01-01

    The relaxation times for electronic excitation due to electron bombardment of atoms was found to be quite short, so that electron kinetic temperature (T sub e) and the electron excitation temperature (T asterisk) should equilibrate quickly whenever electrons are present. However, once equilibrium has been achieved, further energy to the excited electronic states and to the kinetic energy of free electrons must be fed in by collisions with heavy particles that cause vibrational and electronic state transitions. The rate coefficients for excitation of electronic states produced by heavy particle collision have not been well known. However, a relatively simple semi-classical theory has been developed here which is analytic up to the final integration over a Boltzmann distribution of collision energies; this integral can then be evaluated numerically by quadrature. Once the rate coefficients have been determined, the relaxation of electronic excitation energy can be evaluated and compared with the relaxation rates of vibrational excitation. Then the relative importance of these two factors, electronic excitation and vibrational excitation by heavy particle collision, on the transfer of energy to free electron motion, can be assessed.

  7. Dynamics and spectroscopy of CH₂OO excited electronic states.

    PubMed

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

    2016-04-28

    The excited states of the Criegee intermediate CH2OO are studied in molecular dynamics simulations using directly potentials from multi-reference perturbation theory (MR-PT2). The photoexcitation of the species is simulated, and trajectories are propagated in time on the excited state. Some of the photoexcitation events lead to direct fragmentation of the molecule, but other trajectories describe at least several vibrations in the excited state, that may terminate by relaxation to the ground electronic state. Limits on the role of non-adiabatic contributions to the process are estimated by two different simulations, one that forces surface-hopping at potential crossings, and another that ignores surface hopping altogether. The effect of non-adiabatic transitions is found to be small. Spectroscopic implications and consequences for the interpretation of experimental results are discussed. PMID:27040614

  8. Nuclear excitation by electronic transition of 235U

    DOE PAGESBeta

    Chodash, P. A.; Norman, E. B.; Burke, J. T.; Casperson, R. J.; Fisher, S. E.; Holliday, K. S.; Jeffries, J. R.; Wakeling, M. A.; Wilks, S. C.

    2016-03-11

    Here, nuclear excitation by electronic transition (NEET) is a rare nuclear excitation that can occur in isotopes containing a low-lying nuclear excited state. Over the past 40 yr, several experiments have attempted to measure NEET of 235U and those experiments have yielded conflicting results.

  9. Electron impact excitation of helium atom

    NASA Astrophysics Data System (ADS)

    Han, Xiao-Ying; Zeng, De-Ling; Gao, Xiang; Li, Jia-Ming

    2015-08-01

    A method to deal with the electron impact excitation cross sections of an atom from low to high incident energies are presented. This method combines the partial wave method and the first Born approximation (FBA), i.e., replacing the several lowest partial wave cross sections of the total cross sections within FBA by the corresponding exact partial wave cross sections. A new set of codes are developed to calculate the FBA partial wave cross sections. Using this method, the convergent e-He collision cross sections of optical-forbidden and optical-allowed transitions at low to high incident energies are obtained. The calculation results demonstrate the validity and efficiency of the method. Project supported by the National Basic Research Program of China (Grant Nos. 2011CB921501 and 2013CB922200), the National Natural Science Foundation of China (Grant Nos. 11274035, 11275029, 11328401, 11371218, 11474031, 11474032, and 11474034), and the Foundation of Development of Science and Technology of Chinese Academy of Engineering Physics (Grant Nos. 2013A0102005 and 2014A0102005).

  10. Convoy electron emission following ionization of highly-charged ions excited by resonant coherent excitation

    NASA Astrophysics Data System (ADS)

    Suda, S.; Nakano, Y.; Metoki, K.; Shindo, T.; Ohtsuki, S.; Azuma, T.; Hatakeyama, A.; Komaki, K.; Nakai, Y.; Takada, E.; Murakami, T.

    2012-11-01

    Projectile ionization of highly-charged Ar and Fe ions in the excited states passing relativistically fast through a thin crystalline foil was experimentally studied. We selectively controlled the population of the excited states of the projectiles, and their alignment by choosing a specific m-state through three-dimensional resonant coherent excitation technique by periodical electric fields in a crystalline. We measured energy-differential spectra of electron emission released from projectiles at zero degree. Under the resonance condition, we found an evident enhancement of the convoy electron yield, which reflects the electron momentum distribution of the initial bound state of the excited ions.

  11. Effect of high-optical excitation on the ultrafast electron dynamics in stacked-monolayer graphene samples

    NASA Astrophysics Data System (ADS)

    Castañeda, Juan A.; Guimarães Rosa, Henrique; Gomes, José C. V.; Thoroh de Souza, Eunezio A.; de Brito-Cruz, Carlos H.; Fragnito, Hugo L.; Padilha, Lázaro A.

    2016-05-01

    We report on transient absorption experiments performed at high optical excitation fluences and used to study the ultrafast dynamics in graphene. We employed a degenerated scheme of pump and probe at 800 nm (1.55 eV). The time resolution of our measurements was limited by the pulse duration ~ 100 fs. The samples were prepared by chemical vapor deposition (CVD) as single-layers on silica and, then staked layer-by-layer in order to make a stack of up to 5 graphene monolayers. We observed saturable absorption (SA) and fluence-dependent relaxation times. We see that the ultrafast carrier dynamics is composed by two decay mechanisms, one with response time of about 200 fs and a slower process of about 1 ps. The fast decay, due to both carrier-carrier and carrier-optical phonon scattering, becomes slower when the density of excited carrier was increased. We implemented a theoretical model and found that both the optical phonon rate emission and the optical phonon lifetime are affect by the pump fluence.

  12. Electron impact excitation cross sections for carbon

    NASA Astrophysics Data System (ADS)

    Ganas, P. S.

    1981-04-01

    A realistic analytic atomic independent particle model is used to generate wave functions for the valence and excited states of carbon. Using these wave functions in conjunction with the Born approximation and the Russell-Saunders LS-coupling scheme, we calculate generalized oscillator strengths and integrated cross sections for various excitations from the 2p 2( 3P O) valence state.

  13. CW silver ion laser with electron beam excitation

    NASA Astrophysics Data System (ADS)

    Wernsman, B.; Prabhuram, T.; Lewis, K.; Gonzalez, F.; Villagran, M.

    1988-08-01

    A CW laser power of 140 mW was obtained in the 840.39-nm transition of Ag II by electron-beam excitation. The electron-beam excited metal-vapor ion laser is capable of operating using metals with high vaporization temperatures, and is of interest for generation of CW coherent radiation in the 220-260-nm spectral region.

  14. Initial state dependence of convoy electrons emitted from the excited ions by resonant coherent excitation

    NASA Astrophysics Data System (ADS)

    Azuma, T.; Nakano, Y.; Metoki, K.; Hatakeyama, A.; Nakai, Y.; Komaki, K.; Yamazaki, Y.; Takada, E.; Murakami, T.

    2009-11-01

    Convoy electrons emitted from 416 MeV/u heliumlike Ar16+ ions excited by three-dimensional resonant coherent excitation (3D-RCE) have been explored. The 1s electron in the ground state was excited to the 2p state by a periodic crystal field during the passage through a Si crystal and released into the continuum by collisions with target atoms to form a cusp-shaped peak in the energy distribution, referred to as convoy electron. Under the resonance condition, we found not only enhancement of the convoy electron yield but also significant narrowing in the energy distribution, reflecting the initial bound state momentum distribution of the excited ions. This suggests that RCE is well-suited to study fast ion collisions involving the specific excited state.

  15. Plasmoelectronics: coupling plasmonic excitation with electron flow.

    PubMed

    Warren, Scott C; Walker, David A; Grzybowski, Bartosz A

    2012-06-19

    Explorations of the coupling of light and charge via localized surface plasmons have led to the discovery that plasmonic excitation can influence macroscopic flows of charge and, conversely, that charging events can change the plasmonic excitation. We discuss recent theory and experiments in the emerging field of plasmoelectronics, with particular emphasis on the application of these materials to challenges in nanotechnology, energy use, and sensing. PMID:22385329

  16. VUV study of electron impact dissociative excitation of thymine

    NASA Astrophysics Data System (ADS)

    Tiessen, C. J.; Trocchi, J. A.; Hein, J. D.; Dech, J.; Kedzierski, W.; McConkey, J. W.

    2016-06-01

    Dissociative excitation of thymine following electron impact was studied in the energy range up to 430 eV. Emissions in the vacuum ultra-violet spectral region below 150 nm were studied and found to be dominated by the hydrogen Lyman series. Emission cross section data reveal that Lyman-α excitation displays a broad maximum at an electron impact energy of 160 eV. The probability of extracting other excited atoms from the parent molecule is found to be insignificant. Possible excitation and dissociation mechanisms in the parent molecule are discussed.

  17. Electronic excitation of the surface of UV-irradiated solids in heterogeneous recombination of hydrogen atoms

    NASA Astrophysics Data System (ADS)

    Grankin, V. P.; Grankin, D. V.

    2016-06-01

    The reaction energy transfer to electrons and release of electrons from traps under the action of the recombination of H atoms on the surface of light-sum-storing crystals (Zn2SiO4-Mn, ZnS, ZnS,CdS-Ag) was studied. This effect is associated with the reaction energy accommodation via the electronic channel. The transfer of electronic excitations to the atomic recombination event is independent of the reaction rate, but depends on the electron transition energy in a solid. The possibility of electronic excitation per heterogeneous recombination event of H atoms increased exponentially as the electron transition energy decreased.

  18. Nuclear Excitation by Electronic Transition - NEET

    SciTech Connect

    Becker, J.A.

    2002-06-10

    Experiments seeking to demonstrate nuclear excitation induced by synchrotron radiation have been enabled by the development of intense synchrotron radiation. The phenomena has been demonstrated in {sup 197}Au, while realistic upper limits for {sup 189}Os have been established. A new experiment in {sup 189}Os is described. The experimental claim of NEET in isomeric {sup 178}Hf is not credible.

  19. Electronic Excitations and Metal-Insulator Transition inPoly(3-hexylthiophene) Organic Field-Effect Transistors

    SciTech Connect

    Sai, N.; Li, Z.Q.; Martin, M.C.; Basov, D.N.; Di Ventra, M.

    2006-11-07

    We carry out a comprehensive theoretical and experimentalstudy of charge injection in poly(3-hexylthiophene) (P3HT) to determinethe most likely scenario for metal-insulator transition in this system.Wecalculate the optical-absorption frequencies corresponding to a polaronand a bipolaron lattice in P3HT. We also analyze the electronicexcitations for three possible scenarios under which a first- or asecond-order metal-insulator transition can occur in doped P3HT. Thesetheoretical scenarios are compared with data from infrared absorptionspectroscopy on P3HT thin-film field-effect transistors (FETs). Ourmeasurements and theoretical predictions suggest that charge-inducedlocalized states in P3HT FETs are bipolarons and that the highest dopinglevel achieved in our experiments approaches that required for afirst-order metal-insulator transition.

  20. Theoretical Studies of Chemical Reactions following Electronic Excitation

    NASA Technical Reports Server (NTRS)

    Chaban, Galina M.

    2003-01-01

    The use of multi-configurational wave functions is demonstrated for several processes: tautomerization reactions in the ground and excited states of the DNA base adenine, dissociation of glycine molecule after electronic excitation, and decomposition/deformation of novel rare gas molecules HRgF. These processes involve bond brealung/formation and require multi-configurational approaches that include dynamic correlation.

  1. Electron impact excitation of Kr XXVIII

    SciTech Connect

    Aggarwal, K.M.; Keenan, F.P.; Lawson, K.D.

    2011-05-15

    Collision strengths ({Omega}) are calculated for all 6328 transitions among the lowest 113 levels belonging to the 2s{sup 2}2p{sup 5},2s2p{sup 6},2s{sup 2}2p{sup 4}3l,2s2p{sup 5}3l, and 2p{sup 6}3l configurations of fluorine-like krypton, Kr XXVIII, using the Dirac Atomic R-matrix Code. All partial waves with angular momentum J{<=}40 are included, sufficient for the convergence of {Omega} for forbidden transitions. For allowed transitions a top-up is employed to obtain converged values of {Omega} up to an energy of 400 Ryd. Resonances in the thresholds region are resolved on a narrow energy mesh, and results for effective collision strengths (Y) are obtained after averaging the values of {Omega} over a Maxwellian distribution of electron velocities. Values of Y are reported over a wide temperature range below 10{sup 7.1}K, and the accuracy of the results is assessed. In addition, effective collision strengths are listed for the temperature range 7.0{<=}logT{sub e}(K){<=}9.0, obtained from non-resonant collision strengths generated with the FAC code.

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

    NASA Astrophysics Data System (ADS)

    Ramon, John Glenn Santos

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-03-01

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

  4. Experimental apparatus for measurements of electron impact excitation

    NASA Technical Reports Server (NTRS)

    Lafyatis, G. P.; Kohl, J. L.; Gardner, L. D.

    1987-01-01

    An ion beam apparatus for the absolute measurement of collision cross sections in singly and multiply charged ions is described. An inclined electron and ion beams arrangement is used. Emitted photons from the decay of collision produced excited states are collected by a mirror and imaged onto a photomultiplier. Absolute measurements of the electron impact excitation of the 2s-2p transition in C(3+) were used to demonstrate the reliability of the apparatus.

  5. Electron impact excitation of Kr XXXII

    SciTech Connect

    Aggarwal, K.M. Keenan, F.P.; Lawson, K.D.

    2009-09-15

    Collision strengths ({omega}) have been calculated for all 7750 transitions among the lowest 125 levels belonging to the 2s{sup 2}2p,2s2p{sup 2},2p{sup 3},2s{sup 2}3l,2s2p3l, and 2p{sup 2}3l configurations of boron-like krypton, Kr XXXII, for which the Dirac Atomic R-matrix Code has been adopted. All partial waves with angular momentum J{<=}40 have been included, sufficient for the convergence of {omega} for forbidden transitions. For allowed transitions, a top-up has been included in order to obtain converged values of {omega} up to an energy of 500 Ryd. Resonances in the thresholds region have been resolved in a narrow energy mesh, and results for effective collision strengths (Y) have been obtained after averaging the values of {omega} over a Maxwellian distribution of electron velocities. Values of Y are reported over a wide temperature range below 10{sup 7.3}K, and the accuracy of the results is assessed. Values of Y are also listed in the temperature range 7.3{<=}logT{sub e}(K){<=}9.0, obtained from the nonresonant collision strengths from the Flexible Atomic Code.

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

    SciTech Connect

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

    2006-02-10

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

  7. Theory of nuclear excitation by electron capture for heavy ions

    SciTech Connect

    Palffy, Adriana; Scheid, Werner; Harman, Zoltan

    2006-01-15

    We investigate the resonant process of nuclear excitation by electron capture (NEEC), in which a continuum electron is captured into a bound state of an ion with the simultaneous excitation of the nucleus. In order to derive the cross section a Feshbach projection operator formalism is introduced. Nuclear states and transitions are described by a nuclear collective model and making use of experimental data. Transition rates and total cross sections for NEEC followed by the radiative decay of the excited nucleus are calculated for various heavy-ion collision systems.

  8. Dissociative excitation of molecular hydrogen by electron impact.

    NASA Technical Reports Server (NTRS)

    Misakian, M.; Zorn, J. C.

    1972-01-01

    A pulsed electron beam was employed in the experiment to excite a diffuse gas of hydrogen molecules. The energy resolution of the electron gun permitted careful measurements of the thresholds for the production of slow and fast H(2s) atoms. The experiment was conducted in a vacuum system that facilitated a systematic study of the angular distribution of the fragments in the dissociative excitation process. The results permit the identification of the several excited states that are involved in the production of the H(2s) fragments.

  9. Electron-impact excitation of ions

    SciTech Connect

    Crandall, D.H.

    1981-01-01

    A review of electron-ion beam experiments is given. Techniques, difficulties, and present trends in this area are discussed. Measured cross sections are compared with theoretical results and the current level of agreement is assessed. 74 references. (WHK)

  10. Electron-pair excitations and the molecular Coulomb continuum

    SciTech Connect

    Colgan, James

    2009-01-01

    Electron-pair excitations in the molecular hydrogen continuum are described by quantizing rotations of the momentum plane of the electron pair about by the pair's relative momentum. A helium-like description of the molecular pi.Joto double ionization is thus extended to higher angular momenta of the electron pair. A simple three-state superposition is found to account surprisingly well for recent observations of noncoplanar electron-pair, molecular-axis angular distributions.

  11. Dynamics Of Electronic Excitation Of Solids With Ultrashort Laser Pulse

    SciTech Connect

    Medvedev, Nikita; Rethfeld, Baerbel

    2010-10-08

    When ultrashort laser pulses irradiate a solid, photoabsorption by electrons in conduction band produces nonequilibrium highly energetic free electrons gas. We study the ionization and excitation of the electronic subsystem in a semiconductor and a metal (solid silicon and aluminum, respectively). The irradiating femtosecond laser pulse has a duration of 10 fs and a photon energy of h-bar {omega} = 38 eV. The classical Monte Carlo method is extended to take into account the electronic band structure and Pauli's principle for electrons excited to the conduction band. In the case of semiconductors this applies to the holes as well. Conduction band electrons and valence band holes induce secondary excitation and ionization processes which we simulate event by event. We discuss the transient electron dynamics with respect to the differences between semiconductors and metals. For metals the electronic distribution is split up into two branches: a low energy distribution as a slightly distorted Fermi-distribution and a long high energy tail. For the case of semiconductors it is split into two parts by the band gap. To thermalize, these excited electronic subsystems need longer times than the characteristic pulse duration. Therefore, the analysis of experimental data with femtosecond lasers must be based on non-equilibrium concepts.

  12. Atomic electron excitation probabilities during orbital electron capture by the nucleus

    NASA Technical Reports Server (NTRS)

    Crasemann, B.; Chen, M. H.; Briand, J. P.; Chevallier, P.; Chetioui, A.; Tavernier, M.

    1979-01-01

    Approximate probabilities of electron excitation (shakeup/shakeoff) from various atomic states during nuclear ns electron capture have been calculated in the sudden approximation, using Hartree-Fock wave functions. Total excitation probabilities are much lower than during inner-shell ionization by photons or electrons, and ns states are more likely to be excited than np states. This latter result is borne out by K-alpha X-ray satellite spectra.

  13. Detection of excited-state electron bubbles in superfluid helium.

    PubMed

    Konstantinov, Denis; Maris, Humphrey J

    2003-01-17

    We report on experiments in which the pressure oscillation associated with a sound wave is used to explode electron bubbles in liquid helium. Using this technique, we are able to detect the presence of electron bubbles in excited states. PMID:12570553

  14. "Delta Plots"--A New Way to Visualize Electronic Excitation.

    ERIC Educational Resources Information Center

    Morrison, Harry; And Others

    1985-01-01

    Presents procedures for obtaining and examples of delta plots (a way of illustrating electron density changes associated with electronic excitation). These plots are pedagogically useful for visualizing simple and complex transitions and provide a way of "seeing" the origin of highest occupied molecular orbital (HOMO)-dictated carbonyl…

  15. Axial- and radial-resolved electron density and excitation temperature of aluminum plasma induced by nanosecond laser: Effect of the ambient gas composition and pressure

    SciTech Connect

    Dawood, Mahmoud S.; Hamdan, Ahmad E-mail: Joelle.margot@umontreal.ca; Margot, Joëlle E-mail: Joelle.margot@umontreal.ca

    2015-11-15

    The spatial variation of the characteristics of an aluminum plasma induced by a pulsed nanosecond XeCl laser is studied in this paper. The electron density and the excitation temperature are deduced from time- and space- resolved Stark broadening of an ion line and from a Boltzmann diagram, respectively. The influence of the gas pressure (from vacuum up to atmospheric pressure) and compositions (argon, nitrogen and helium) on these characteristics is investigated. It is observed that the highest electron density occurs near the laser spot and decreases by moving away both from the target surface and from the plume center to its edge. The electron density increases with the gas pressure, the highest values being occurred at atmospheric pressure when the ambient gas has the highest mass, i.e. in argon. The excitation temperature is determined from the Boltzmann plot of line intensities of iron impurities present in the aluminum target. The highest temperature is observed close to the laser spot location for argon at atmospheric pressure. It decreases by moving away from the target surface in the axial direction. However, no significant variation of temperature occurs along the radial direction. The differences observed between the axial and radial direction are mainly due to the different plasma kinetics in both directions.

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

    NASA Technical Reports Server (NTRS)

    Chutjian, A.

    1974-01-01

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

  17. Electronic excitation spectrum of ABC-stacked multilayer graphene

    NASA Astrophysics Data System (ADS)

    Henni, Y.; Nogajewski, K.; Ojeda Collado, H. P.; Usaj, G.; Balseiro, C. A.; Potemski, M.; Faugeras, C.

    The electronic properties of ABC graphene trilayers has attracted lot of attention recently due to their potential applications in engineering carbon-based devices with gate tunable electrical conductivity. Morever,ABC-stacked thin layers of graphite are predicted to host peculiar surface electronic states, with a flat dispersion over most of the Brillouin zone. The associated high density of states is likely to favour the emergence of exotic electronic phases, such as charge density waves or even superconductivity. We present a micro-magneto-Raman scattering study of a thin graphite flake produced by exfoliation of natural graphite, composed of ~15graphene layers, and including a large ABC-stacked domain. Exploring the low temperature Raman scattering spectrum of this domain up to B=29T,we identify inter Landau level electronic excitations within the surface flat bands,together with electronic excitations involving the gapped states in the bulk. This interband electronic excitation at B=0T can be observed,up to room temperature, directly in the Raman scattering spectrum as a broad(~ 180 cm-1) feature. Because the energy gap strongly depends on the number of layers,this electronic excitation can be used to identify and characterize ABC-stacked graphite thin layers.

  18. Raman scattering in high-{Tc} superconductors: Electronic excitations

    SciTech Connect

    Cardona, M.; Strohm, T.; Kircher, J.

    1996-12-31

    Since the discovery of the high {Tc} superconductors Raman scattering has proven to be an excellent technique to characterize them and to investigate basic physical properties relevant to the elusive mechanism responsible for their superconductivity. The authors discuss here several aspects of the technique as applied to superconductivity, including scattering by lattice vibrations, magnetic excitations, and electronic excitations, with particular emphasis on the latter, both in the normal and the superconducting state. 47 refs., 8 figs., 1 tab.

  19. Electronic excitation energy transfer between nucleobases of natural DNA.

    PubMed

    Vayá, Ignacio; Gustavsson, Thomas; Douki, Thierry; Berlin, Yuri; Markovitsi, Dimitra

    2012-07-18

    Transfer of the electronic excitation energy in calf thymus DNA is studied by time-resolved fluorescence spectroscopy. The fluorescence anisotropy, after an initial decay starting on the femtosecond time scale, dwindles down to ca. 0.1. The in-plane depolarized fluorescence decays are described by a stretched exponential law. Our observations are consistent with one-dimensional transfer mediated by charge-transfer excited states. PMID:22765050

  20. Fast-electron-impact study on excitations of 4d electron of xenon

    NASA Astrophysics Data System (ADS)

    Zhang, Xin; Liu, Ya-Wei; Peng, Yi-Geng; Xu, Long-Quan; Ni, Dong-Dong; Kang, Xu; Wang, Yang-Yang; Qi, Yue-Ying; Zhu, Lin-Fan

    2015-12-01

    The electron energy loss spectrum of the 4d excitations of xenon was measured at an incident electron energy of 1500 eV and a scattering angle of 6°. Besides the optically allowed transitions of and the optically forbidden transitions of and were observed. The measured features are assigned with the help of the calculation by the Cowan Code. The line profile parameters of both optically allowed transitions and optically forbidden ones were determined and compared with the previous available data. It is found that the natural widths of both dipole-allowed and dipole-forbidden excitations are approximately identical, which means the spectator transitions dominate the resonant Auger effect for both dipole-allowed and dipole-forbidden transitions. Project supported by the National Natural Science Foundation of China (Grant Nos. U1332204, 11274291, 11504361, and 11320101003).

  1. Electronic excitation and isentropic coefficients of high temperature planetary atmosphere plasmas

    SciTech Connect

    Colonna, Gianpiero; Capitelli, Mario

    2012-07-15

    In this paper, we have discussed the effects of electronically excited states of atomic species in affecting the isentropic coefficients of plasmas, focusing on mixtures representing the atmospheres of Jupiter, Mars, and Earth. General behaviors have been rationalized on the basis of simplified approaches. The contribution of the electronically excited states has been evidenced by comparing results obtained considering only the ground state and those obtained using either Fermi or Griem cutoff criteria.

  2. Electron-irradiation-induced crystallization at metallic amorphous/silicon oxide interfaces caused by electronic excitation

    NASA Astrophysics Data System (ADS)

    Nagase, Takeshi; Yamashita, Ryo; Lee, Jung-Goo

    2016-04-01

    Irradiation-induced crystallization of an amorphous phase was stimulated at a Pd-Si amorphous/silicon oxide (a(Pd-Si)/SiOx) interface at 298 K by electron irradiation at acceleration voltages ranging between 25 kV and 200 kV. Under irradiation, a Pd-Si amorphous phase was initially formed at the crystalline face-centered cubic palladium/silicon oxide (Pd/SiOx) interface, followed by the formation of a Pd2Si intermetallic compound through irradiation-induced crystallization. The irradiation-induced crystallization can be considered to be stimulated not by defect introduction through the electron knock-on effects and electron-beam heating, but by the electronic excitation mechanism. The observed irradiation-induced structural change at the a(Pd-Si)/SiOx and Pd/SiOx interfaces indicates multiple structural modifications at the metal/silicon oxide interfaces through electronic excitation induced by the electron-beam processes.

  3. Superelastic electron scattering from laser-excited cesium atoms

    SciTech Connect

    Slaughter, D. S.; Karaganov, V.; Brunger, M. J.; Teubner, P. J. O.; Bray, I.; Bartschat, K.

    2007-06-15

    We present results from a joint experimental and theoretical investigation of superelastic electron scattering from laser-excited Cs atoms in the (6p){sup 2}P{sub 3/2} state. Comparison of the measured pseudo-Stokes parameters P{sub 1}, P{sub 2}, and P{sub 3} and the total degree of polarization P{sup +} for incident energies of 5.5 eV and 13.5 eV, respectively, with theoretical predictions based upon a nonrelativistic convergent close-coupling method and a 24-state semirelativistic Breit-Pauli R-matrix approach indicates that driving channel coupling to convergence for these observables is more important than accounting for relativistic effects.

  4. Resonant vibrational excitation of CO by low-energy electrons

    SciTech Connect

    Poparic, G. B.; Belic, D. S.; Vicic, M. D.

    2006-06-15

    Electron impact vibrational excitation of the CO molecule, via the {sup 2}{pi} resonance, in the 0-4 eV energy region has been investigated. The energy dependence of the resonant excitation of the first ten vibrational levels, v=1 to v=10, has been measured by use of a crossed-beams double trochoidal electron spectrometer. Obtained relative differential cross sections are normalized to the absolute values. Integral cross sections are determined by using our recent results on scattered electrons angular distributions, which demonstrate clear p-partial wave character of this resonance. Substructures appear in the {sup 2}{pi} resonant excitation of the CO molecule which have not been previously observed.

  5. Imaging Excited Orbitals of Quantum Dots: Experiment and Electronic Structure Theory.

    PubMed

    Nienhaus, Lea; Goings, Joshua J; Nguyen, Duc; Wieghold, Sarah; Lyding, Joseph W; Li, Xiaosong; Gruebele, Martin

    2015-11-25

    Electronically excited orbitals play a fundamental role in chemical reactivity and spectroscopy. In nanostructures, orbital shape is diagnostic of defects that control blinking, surface carrier dynamics, and other important optoelectronic properties. We capture nanometer resolution images of electronically excited PbS quantum dots (QDs) by single molecule absorption scanning tunneling microscopy (SMA-STM). Dots with a bandgap of ∼1 eV are deposited on a transparent gold surface and optically excited with red or green light to produce hot carriers. The STM tip-enhanced laser light produces a large excited-state population, and the Stark effect allows transitions to be tuned into resonance by changing the sample voltage. Scanning the QDs under laser excitation, we were able to image electronic excitation to different angular momentum states depending on sample bias. The shapes differ from idealized S- or P-like orbitals due to imperfections of the QDs. Excitation of adjacent QD pairs reveals orbital alignment, evidence for electronic coupling between dots. Electronic structure modeling of a small PbS QD, when scaled for size, reveals Stark tuning and variation in the transition moment of different parity states, supporting the simple one-electron experimental interpretation in the hot carrier limit. The calculations highlight the sensitivity of orbital density to applied field, laser wavelength, and structural fluctuations of the QD. PMID:26518039

  6. Integrating proton coupled electron transfer (PCET) and excited states

    SciTech Connect

    Gagliardi, Christopher J.; Westlake, Brittany C.; Kent, Caleb A.; Paul, Jared J.; Papanikolas, John M.; Meyer, Thomas J.

    2010-11-01

    In many of the chemical steps in photosynthesis and artificial photosynthesis, proton coupled electron transfer (PCET) plays an essential role. An important issue is how excited state reactivity can be integrated with PCET to carry out solar fuel reactions such as water splitting into hydrogen and oxygen or water reduction of CO2 to methanol or hydrocarbons. The principles behind PCET and concerted electron–proton transfer (EPT) pathways are reasonably well understood. In Photosystem II antenna light absorption is followed by sensitization of chlorophyll P680 and electron transfer quenching to give P680+. The oxidized chlorophyll activates the oxygen evolving complex (OEC), a CaMn4 cluster, through an intervening tyrosine–histidine pair, YZ. EPT plays a major role in a series of four activation steps that ultimately result in loss of 4e-/4H+ from the OEC with oxygen evolution. The key elements in photosynthesis and artificial photosynthesis – light absorption, excited state energy and electron transfer, electron transfer activation of multiple-electron, multiple-proton catalysis – can also be assembled in dye sensitized photoelectrochemical synthesis cells (DS-PEC). In this approach, molecular or nanoscale assemblies are incorporated at separate electrodes for coupled, light driven oxidation and reduction. Separate excited state electron transfer followed by proton transfer can be combined in single semi-concerted steps (photo-EPT) by photolysis of organic charge transfer excited states with H-bonded bases or in metal-to-ligand charge transfer (MLCT) excited states in pre-associated assemblies with H-bonded electron transfer donors or acceptors. In these assemblies, photochemically induced electron and proton transfer occur in a single, semi-concerted event to give high-energy, redox active intermediates.

  7. Excitation of symmetric surface wavesby electron tubular beams

    NASA Astrophysics Data System (ADS)

    Akimov, Yu A.; Olefir, V. P.; Azarenkov, N. A.

    2006-08-01

    The nonlinear theory of symmetric surface wave excitation by a low-density electron tubular beam in a cylindrical plasma-vacuum-metal waveguide is presented. A set of nonlinear equations is derived that describes the time evolution of the plasma-beam interaction. The influence of the beam and waveguide structure parameters on the saturation amplitude and excitation efficiency of the surface wave is investigated both numerically and analytically. Thermalization of the electron beam in the wave-fields is studied as well.

  8. Inelastic X-ray Scattering Studies of Electronic Excitations

    NASA Astrophysics Data System (ADS)

    Ishii, Kenji; Tohyama, Takami; Mizuki, Jun'ichiro

    2013-02-01

    Inelastic x-ray scattering (IXS) has developed into one of the most powerful momentum-resolved spectroscopies. Especially in the last decade, it has achieved significant progress utilizing brilliant x-rays from third-generation synchrotron radiation facilities. Simultaneously, theoretical efforts have been made to predict or interpret the experimental spectra. One of the scientific fields studied intensively by IXS is strongly correlated electron systems, where the interplay of charge, spin, and orbital degrees of freedom determines their physical properties. IXS can provide a new insight into the electron dynamics of the systems through the observation of charge, spin, and orbital excitations. Focusing on the momentum-resolved electronic excitations in strongly correlated electron systems, we review IXS studies and the present capabilities of IXS for the study of the dynamics of materials. With nonresonant inelastic x-ray scattering (NIXS), one can directly obtain dynamical charge correlation and we discuss its complementary aspects with inelastic neutron scattering. NIXS also has a unique capability of measuring higher multipole transitions, which are usually forbidden in conventional optical absorption. Resonant inelastic x-ray scattering (RIXS) is now established as a valuable tool for measuring charge, spin, and orbital excitations in a momentum-resolved manner. We describe RIXS works on cuprates in detail and show what kind of electronic excitations have been observed. We also discuss RIXS studies on other transition-metal compounds. Finally, we conclude with an outlook on IXS using next-generation x-ray sources.

  9. Electron excitation collision strengths for positive atomic ions: a collection of theoretical data

    SciTech Connect

    Merts, A.L.; Mann, J.B.; Robb, W.D.; Magee, N.H. Jr.

    1980-03-01

    This report contains data on theoretical and experimental cross sections for electron impact excitation of positive atomic ions. It is an updated and corrected version of a preliminary manuscript which was used during an Atomic Data Workshop on Electron Excitation of Ions held at Los Alamos in November 1978. The current status of quantitative knowledge of collisional excitation collision strengths is shown for highly stripped ions where configuration mixing, relativistic and resonance effects may be important. The results show a reasonably satisfactory state for first-row isoelectronic ions and indicate that a considerable amount of work remains to be done for second-row and heavier ions.

  10. Minimal-excitation states for electron quantum optics using levitons

    NASA Astrophysics Data System (ADS)

    Dubois, J.; Jullien, T.; Portier, F.; Roche, P.; Cavanna, A.; Jin, Y.; Wegscheider, W.; Roulleau, P.; Glattli, D. C.

    2013-10-01

    The on-demand generation of pure quantum excitations is important for the operation of quantum systems, but it is particularly difficult for a system of fermions. This is because any perturbation affects all states below the Fermi energy, resulting in a complex superposition of particle and hole excitations. However, it was predicted nearly 20 years ago that a Lorentzian time-dependent potential with quantized flux generates a minimal excitation with only one particle and no hole. Here we report that such quasiparticles (hereafter termed levitons) can be generated on demand in a conductor by applying voltage pulses to a contact. Partitioning the excitations with an electronic beam splitter generates a current noise that we use to measure their number. Minimal-excitation states are observed for Lorentzian pulses, whereas for other pulse shapes there are significant contributions from holes. Further identification of levitons is provided in the energy domain with shot-noise spectroscopy, and in the time domain with electronic Hong-Ou-Mandel noise correlations. The latter, obtained by colliding synchronized levitons on a beam splitter, exemplifies the potential use of levitons for quantum information: using linear electron quantum optics in ballistic conductors, it is possible to imagine flying-qubit operation in which the Fermi statistics are exploited to entangle synchronized electrons emitted by distinct sources. Compared with electron sources based on quantum dots, the generation of levitons does not require delicate nanolithography, considerably simplifying the circuitry for scalability. Levitons are not limited to carrying a single charge, and so in a broader context n-particle levitons could find application in the study of full electron counting statistics. But they can also carry a fraction of charge if they are implemented in Luttinger liquids or in fractional quantum Hall edge channels; this allows the study of Abelian and non-Abelian quasiparticles in the

  11. Excitations and benchmark ensemble density functional theory for two electrons

    SciTech Connect

    Pribram-Jones, Aurora; Burke, Kieron; Yang, Zeng-hui; Ullrich, Carsten A.; Trail, John R.; Needs, Richard J.

    2014-05-14

    A new method for extracting ensemble Kohn-Sham potentials from accurate excited state densities is applied to a variety of two-electron systems, exploring the behavior of exact ensemble density functional theory. The issue of separating the Hartree energy and the choice of degenerate eigenstates is explored. A new approximation, spin eigenstate Hartree-exchange, is derived. Exact conditions that are proven include the signs of the correlation energy components and the asymptotic behavior of the potential for small weights of the excited states. Many energy components are given as a function of the weights for two electrons in a one-dimensional flat box, in a box with a large barrier to create charge transfer excitations, in a three-dimensional harmonic well (Hooke's atom), and for the He atom singlet-triplet ensemble, singlet-triplet-singlet ensemble, and triplet bi-ensemble.

  12. Electron impact excitation of argon in the extreme vacuum ultraviolet

    NASA Technical Reports Server (NTRS)

    Mentall, J. E.; Morgan, H. D.

    1976-01-01

    Polarization-free excitation cross sections in the extreme vacuum ultraviolet have been measured for electron impact on Ar. Observed spectral features were those lines of Ar I and Ar II which lie between 700 and 1100 A. Excitation functions were measured for the Ar I resonance line at 1048 A and the Ar II resonance line at 920 A. Peak cross sections for these two lines were found to be (39.4 plus or minus 7.9) x 10 to the -18th and (6.9 plus or minus 1.4) x 10 to the -18th, respectively. At low energies, excitation of the Ar II resonance line is dominated by an electron exchange transition.

  13. Electron impact elastic scattering and vibrational excitation of ethylene

    NASA Astrophysics Data System (ADS)

    Khakoo, Murtadha; Khakoo, Sabaha; Sakaamini, Ahmad; Hargreaves, Leigh; Winstead, Carl; McKoy, Vince

    2015-09-01

    Experimental and theoretical (Schwinger Multi-Channel model) differential scattering cross sections for low energy electron elastic scattering plus vibrational excitation (4 energy loss features) of ethylene are presented. The incident electron energy range is from 0.5eV to 100eV and scattering angles of 5 to 130 degrees. Comparisons with theory and past available measurements show good agreement in general. Funded by a National Science Foundation Collaborative Research Grant to CSUF and Caltech.

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

    SciTech Connect

    Campbell, Luke W.; Gao, Fei

    2013-05-01

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

  15. Photoionization of furan from the ground and excited electronic states

    NASA Astrophysics Data System (ADS)

    Ponzi, Aurora; Sapunar, Marin; Angeli, Celestino; Cimiraglia, Renzo; Došlić, Nada; Decleva, Piero

    2016-02-01

    Here we present a comparative computational study of the photoionization of furan from the ground and the two lowest-lying excited electronic states. The study aims to assess the quality of the computational methods currently employed for treating bound and continuum states in photoionization. For the ionization from the ground electronic state, we show that the Dyson orbital approach combined with an accurate solution of the continuum one particle wave functions in a multicenter B-spline basis, at the density functional theory (DFT) level, provides cross sections and asymmetry parameters in excellent agreement with experimental data. On the contrary, when the Dyson orbitals approach is combined with the Coulomb and orthogonalized Coulomb treatments of the continuum, the results are qualitatively different. In excited electronic states, three electronic structure methods, TDDFT, ADC(2), and CASSCF, have been used for the computation of the Dyson orbitals, while the continuum was treated at the B-spline/DFT level. We show that photoionization observables are sensitive probes of the nature of the excited states as well as of the quality of excited state wave functions. This paves the way for applications in more complex situations such as time resolved photoionization spectroscopy.

  16. Tuning ground states and excitations in complex electronic materials

    SciTech Connect

    Bishop, A.R.

    1996-09-01

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

  17. Low energy electron impact vibrational excitation of acetylene

    NASA Astrophysics Data System (ADS)

    Patra, Sigma; Hargreaves, Leigh; Khakoo, Murtadha

    2016-05-01

    Experimental differential cross sections for the vibration excitation of the four fundamental modes of acetylene at low incident electron energies from 1 eV to 20 eV and scattering angles of 10o to 130o will be presented. The results will be compared to results available in the literature. Funded by NSF-AMOP-RUI Grant.

  18. Electron impact excitation coefficients for laboratory and astrophysical plasmas

    NASA Technical Reports Server (NTRS)

    Davis, J.; Kepple, P. C.; Blaha, M.

    1976-01-01

    Electron impact excitation rate coefficients have been obtained for a number of transitions in highly ionized ions of interest to astrophysical and laboratory plasmas. The calculations were done using the method of distorted waves. Results are presented for various transitions in highly ionized Ne, Na, Al, Si, A, Ca, Ni and Fe.

  19. Excitation of electron Langmuir frequency harmonics in the solar atmosphere

    SciTech Connect

    Fomichev, V. V.; Fainshtein, S. M.; Chernov, G. P.

    2013-05-15

    An alternative mechanism for the excitation of electron Langmuir frequency harmonics as a result of the development of explosive instability in a weakly relativistic beam-plasma system in the solar atmosphere is proposed. The efficiency of the new mechanism as compared to the previously discussed ones is analyzed.

  20. The coupling of condensed matter excitations to electron probes

    SciTech Connect

    Ritchie, R.H.

    1988-01-01

    Aspects of coupling of a classical electron with bulk and surface excitations in condensed matter have been sketched. Some considerations of a self-energy approach to the complete quantal treatment of this coupling have been given. 19 refs., 3 figs.

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

    PubMed Central

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

    2015-01-01

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

  2. Influence of collective effects on lifetimes of condensed excited states

    NASA Technical Reports Server (NTRS)

    Zmuidzinas, Jonas Stasys

    1987-01-01

    The possibility that collective effects may dramatically influence autoionization-limited lifetimes of condensed excited states is investigated in the context of a two-band model of an insulator in a strong magnetic field. Two different mechanisms for suppressing autoionization are discussed which may prevent the potentially catastrophic destruction of the excited state. Under appropriate circumstances, the residual low-density Auger electrons may be confined in a superconducting state and paired by excitonic fluctuations in the conduction band.

  3. Excitation of the surface flute waves in electron cyclotron frequency range by internal rotating electron beam in a coaxial waveguide

    NASA Astrophysics Data System (ADS)

    Blednov, O.; Girka, I.; Girka, V.; Pavlenko, I.; Sydora, R.

    2014-12-01

    The initial stage of interaction between a gyrating beam of electrons, which move along Larmor orbits in a narrow gap between a cylindrical plasma layer and an internal screen of a metal coaxial waveguide and electromagnetic eigen waves, is studied theoretically. These waves are extraordinary polarized ones; they propagate along the azimuthal angle across an axial external steady magnetic field in the electron cyclotron frequency range. The numerical analysis shows that the excitation process is stable enough in respect to changing plasma waveguide parameters. The wider the plasma layer, the broader the range of plasma waveguide parameters within which effective wave excitation takes place. The main influence on the excitation of these modes is performed by the applied axial magnetic field, namely: its increase leads to an increase of growth rate and a broadening of the range of the waveguide parameters within which wave excitation is effective.

  4. Dynamics of two-electron excitations in helium

    SciTech Connect

    Caldwell, C.D.; Menzel, A.; Frigo, S.P.

    1997-04-01

    Excitation of both electrons in helium offers a unique window for studying electron correlation at the most basic level in an atom in which these two electrons and the nucleus form a three-body system. The authors utilized the first light available at the U-8 undulator-SGM monochromator beamline to investigate the dynamic parameters, partial cross sections, differential cross sections, and photoelectron angular distribution parameters ({beta}), with a high resolving power for the photon beam and at the highly differential level afforded by the use of their electron spectrometer. In parallel, they carried out detailed calculations of the relevant properties by a theoretical approach that is based on the hyperspherical close-coupling method. Partial photoionization cross sections {sigma}{sub n}, and photoelectron angular distributions {beta}{sub n} were measured for all possible final ionic states He{sup +}(n) in the region of the double excitations N(K,T){sup A} up to the N=5 threshold. At a photon energy bandpass of 12 meV below the thresholds N=3, 4, and 5, this level of differentiation offers the most critical assessment of the dynamics of the two-electron excitations to date. The experimental data were seen to be very well described by the most advanced theoretical calculations.

  5. Electron-impact excitation and ionization cross sections for ground state and excited helium atoms

    SciTech Connect

    Ralchenko, Yu. Janev, R.K.; Kato, T.; Fursa, D.V.; Bray, I.; Heer, F.J. de

    2008-07-15

    Comprehensive and critically assessed cross sections for the electron-impact excitation and ionization of ground state and excited helium atoms are presented. All states (atomic terms) with n{<=}4 are treated individually, while the states with n{>=}5 are considered degenerate. For the processes involving transitions to and from n{>=}5 levels, suitable cross section scaling relations are presented. For a large number of transitions, from both ground and excited states, convergent close coupling calculations were performed to achieve a high accuracy of the data. The evaluated/recommended cross section data are presented by analytic fit functions, which preserve the correct asymptotic behavior of the cross sections. The cross sections are also displayed in graphical form.

  6. Chemical excitation of electrons: A dark path to melanoma.

    PubMed

    Premi, Sanjay; Brash, Douglas E

    2016-08-01

    Sunlight's ultraviolet wavelengths induce cyclobutane pyrimidine dimers (CPDs), which then cause mutations that lead to melanoma or to cancers of skin keratinocytes. In pigmented melanocytes, we found that CPDs arise both instantaneously and for hours after UV exposure ends. Remarkably, the CPDs arising in the dark originate by a novel pathway that resembles bioluminescence but does not end in light: First, UV activates the enzymes nitric oxide synthase (NOS) and NADPH oxidase (NOX), which generate the radicals nitric oxide (NO) and superoxide (O2(-)); these combine to form the powerful oxidant peroxynitrite (ONOO(-)). A fragment of the skin pigment melanin is then oxidized, exciting an electron to an energy level so high that it is rarely seen in biology. This process of chemically exciting electrons, termed "chemiexcitation", is used by fireflies to generate light but it had never been seen in mammalian cells. In melanocytes, the energy transfers radiationlessly to DNA, inducing CPDs. Chemiexcitation is a new source of genome instability, and it calls attention to endogenous mechanisms of genome maintenance that prevent electronic excitation or dissipate the energy of excited states. Chemiexcitation may also trigger pathogenesis in internal tissues because the same chemistry should arise wherever superoxide and nitric oxide arise near cells that contain melanin. PMID:27262612

  7. Electronic excitations in electron-doped cuprate superconductors

    NASA Astrophysics Data System (ADS)

    Unger, P.; Fulde, P.

    1995-04-01

    We calculate the electronic single-particle spectrum of an electron-doped cuprate superconductor such as Nd2-xCexCuO4-y. The dynamics of holes in the Cu-O planes is described by the extended Hubbard or Emery model. We consider the system at half-filling (one hole per unit cell, nh=1) and in the case of electron doping where the ground state is paramagnetic. The projection technique of Mori and Zwanzig is applied to derive the equations of motion for the Green's functions of Cu and O holes. These equations are solved self-consistently as in a previous calculation, where we considered the case of hole doping. At half-filling the system exhibits a charge-transfer gap bounded by Zhang-Rice singlet states and the upper Hubbard band. Upon electron doping the upper Hubbard band crosses the Fermi level and the system becomes metallic. With increasing electron doping the singlet band loses intensity and finally vanishes for nh=0. The corresponding spectral weight is transferred to the upper Hubbard band, which becomes a usual tight-binding band for zero hole concentration. The shape of the flat band crossing the Fermi level fits well to angle-resolved photoemission spectra of Nd2-xCexCuO4-y for x=0.15 and 0.22. Furthermore, our findings are in excellent agreement with exact diagonalization studies of 2×2 CuO2 cluster with periodic boundary conditions.

  8. Isomer Triggering via Nuclear Excitation by Electron Capture

    SciTech Connect

    Palffy, Adriana; Evers, Joerg; Keitel, Christoph H.

    2007-10-26

    Triggering of long-lived nuclear isomeric states via coupling to the atomic shells in the process of nuclear excitation by electron capture (NEEC) is studied. NEEC occurring in highly charged ions can excite the isomeric state to a triggering level that subsequently decays to the ground state. We present total cross sections for NEEC isomer triggering considering experimentally confirmed low-lying triggering levels and reaction rates based on realistic experimental parameters in ion storage rings. A comparison with other isomer triggering mechanisms shows that, among these, NEEC is the most efficient.

  9. Electron scattering by laser-excited barium atoms

    NASA Technical Reports Server (NTRS)

    Register, D. F.; Trajmar, S.; Jensen, S. W.; Poe, R. T.

    1978-01-01

    Inelastic and superelastic scattering of 30- and 100-eV electrons by laser-excited 6s 6p 1P and subsequent cascade-populated 6s 6p 3P, 6s 5d 1D, and 6s 5d 3D Ba atoms have been observed. Absolute differential cross sections for the singlet and relative scattering intensities for the triplet species have been determined in the 5 to 20 deg angular region. Under the present conditions excitations dominate over deexcitations.

  10. Mechanisms for Ultrafast Nonradiative Relaxation in Electronically Excited Eumelanin Constituents

    PubMed Central

    Meng, Sheng; Kaxiras, Efthimios

    2008-01-01

    We investigate the relaxation dynamics of melanin model constituents including monomers, dimers, and tetramers, upon excitation, using state-of-the-art, time-dependent, density functional theory calculations. The results explain the ability of these molecules to transform photon energy into thermal energy in a remarkably short timescale of ∼100 fs. We find that after electronic excitation by light absorption, ultrafast energy conversion takes place through two novel mechanisms: proton transfer on a timescale of 110 fs and state mixing upon oligomerization on a timescale of <50 fs. These results are in good agreement with available experiments and help elucidate melanin's role in photoprotection against ultraviolet radiation. PMID:18676639

  11. Eucken correction in high-temperature gases with electronic excitation

    SciTech Connect

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

    2014-05-14

    In the present paper, thermal conductivity coefficient of high-temperature molecular and atomic gases with excited electronic states is studied using both the kinetic theory algorithm developed by authors earlier and the well known simple expression for the thermal conductivity coefficient proposed by Eucken and generalized by Hirschfelder. The influence of large collision diameters of excited states on the thermal conductivity is discussed. The limit of validity of the Eucken correction is evaluated on the basis of the kinetic theory calculations; an improved model suitable for air species under high-temperature conditions is proposed.

  12. Effects of core turbulence on jet excitability

    NASA Technical Reports Server (NTRS)

    Mankbadi, Reda R.; Raman, Ganesh; Rice, Edward J.

    1989-01-01

    The effects of varying freestream core turbulence on the evolution of a circular jet with and without tonal excitation are examined. Measurements are made on an 8.8 cm diameter jet at a Mach number of 0.3. The jet is excitated by plane waves at Strouhal number 0.5. For the excited and unexcited cases the turbulence level is varied by screens and grids placed upstream of the nozzle exit. The experiment results are compared with a theoretical model which incorporates a variable core turbulence and considers the energy interactions between the mean flow, the turbulence and the forced component. Both data and theory indicate that increasing the freestream turbulence diminishes the excitability of the jet and reduces the effect of excitation on the spreading rate of the jet.

  13. Excitation of low-frequency waves by auroral electron beams

    NASA Technical Reports Server (NTRS)

    Lin, C. S.; Wong, H. K.; Koga, J.; Burch, J. L.

    1989-01-01

    The electron distribution functions measured by the Dynamics Explorer 1 satellite during an auroral pass in 1981 are used in a linear instability analysis of low-frequency electromagnetic and electrostatic waves near and below the hydrogen gyrofrequency. It is suggested that the low-frequency electric and magnetic noise in the auroral zone might be explained by O and H electromagnetic ion cyclotron waves excited by energetic electron beams. An instability analysis suggests that upward and downward streaming electrons throughout the central plasma sheet region provide the free energy for heating oxygen ion through oxygen electrostatic ion cyclotron waves.

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

    NASA Astrophysics Data System (ADS)

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

    2016-05-01

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

  15. Theoretical studies on the reaction pathways of electronically excited DAAF

    SciTech Connect

    Quenneville, Jason M; Moore, David S

    2009-01-01

    The use of temporally and spectrally shaped ultrafast laser pulses to initiate, as well as detect, high explosives is being explored at Los Alamos. High level ab initio calculations, presented here, are employed to help guide and interpret the experiments. The ground and first excited electronic states of 3,3{prime}-diamino-4,4{prime}-azoxyfurazan (DAAF) are investigated using complete active space self-consistent field (CASSCF) and time-dependent density functional theory (TD-DFT). The geometrical and energetic character of the excited state minima, conical intersections and reaction pathways of DAAF are described. Two radiative and two non-radiative excited state population quenching mechanisms are outlined, and possible pathways for photochemical and spectroscopic control are discussed. The use of laser light to control chemical reactions has many applications. The initiation and the detection of explosives are two such applications currently under development at Los Alamos. Though inherently experimental, the project can be aided by theory through both prediction and interpretation. When the laser light is in the UV/visible region of the electromagnetic spectrum, the absorbing molecule is excited electronically and excitation decay may occur either radiatively (fluorescence or phosphorescence) or non-radiatively (through internal conversion). In many cases decay of the excitation occurs through a mixture of processes, and maximizing the desired result requires sophisticated laser pulses whose amplitude has been optimally modulated in time and/or frequency space. Control of cis-stilbene photochemistry was recently demonstrated in our group, and we aim to extend this work to high explosive compounds. Maximizing radiative decay leads to increased fluorescence quantum yields and enhances the possibility of spectral detection of the absorbing molecule. Maximizing non-radiative decay can lead to chemistry, heating of the sample and possibly detonation initiation in

  16. Nuclear excitation by electronic transition of 235U

    NASA Astrophysics Data System (ADS)

    Chodash, P. A.; Burke, J. T.; Norman, E. B.; Wilks, S. C.; Casperson, R. J.; Fisher, S. E.; Holliday, K. S.; Jeffries, J. R.; Wakeling, M. A.

    2016-03-01

    Background: Nuclear excitation by electronic transition (NEET) is a rare nuclear excitation that can occur in isotopes containing a low-lying nuclear excited state. Over the past 40 yr, several experiments have attempted to measure NEET of 235U and those experiments have yielded conflicting results. Purpose: An experiment was performed to determine whether NEET of 235U occurs and to determine its excitation rate. Method: A pulsed Nd:YAG laser operating at 1064 nm with a pulse energy of 790 mJ and a pulse width of 9 ns was used to generate a uranium plasma. The plasma was collected on a catcher plate and electrons from the catcher plate were accelerated and focused onto a microchannel plate detector. An observation of a decay with a 26-min half-life would suggest the creation of Um235 and the possibility that NEET of 235U occurred. Results: A 26-min decay consistent with the decay of Um235 was not observed and there was no evidence that NEET occurred. An upper limit for the NEET rate of 235U was determined to be λNEET<1.8 ×10-4 s-1, with a confidence level of 68.3%. Conclusions: The upper limit determined from this experiment is consistent with most of the past measurements. Discrepancies between this experiment and past measurements can be explained by assuming that past experiments misinterpreted the data.

  17. Electron delocalization and electron density of small polycyclic aromatic hydrocarbons in singlet excited states.

    PubMed

    Estévez-Fregoso, Mar; Hernández-Trujillo, Jesús

    2016-04-28

    The four lowest singlet electronic states of benzene, the acenes from naphthalene to pentacene, phenanthrene and pyrene were studied by means of theoretical methods. Their vertical excitation energies from the ground electronic states were computed at the CASPT2 approximation. As an attempt to explain the trends observed in the excitation energies, several descriptors based on the electron density were used and the similarity of these molecules with their ground state counterparts was analyzed. It was found that the changes of the topological properties at the C-C bond critical points do not explain the decreasing trends for the excitation energies with the increase of the number of rings, in part because the small changes that take place in the electron density occur above and below the molecular plane. A similarity index based on electron delocalization between quantum topological atoms was defined to compare a molecule in two different electronic states. It was found that, mainly for the acenes, this index goes in line with the excitation energies to the first excited state. Implications of the changes in electron delocalization on the aromatic character of these molecules are also discussed. In general, local aromaticity decreases upon excitation. PMID:26795361

  18. Photonically excited electron emission from modified graphitic nanopetal arrays

    SciTech Connect

    McCarthy, Patrick T.; Fisher, Timothy S.; School of Mechanical Engineering, Purdue University, West Lafayette, Indiana 47907 ; Vander Laan, Scott J.; Janes, David B.; School of Electrical and Computer Engineering, Purdue University, West Lafayette, Indiana 47907

    2013-05-21

    Efficient electron emission for energy conversion requires a low work function and a stable emitter material. The work function of graphene-based carbon materials can decrease significantly by intercalation with alkali metals, thus increasing their emission current. In this work, electron emission from potassium-intercalated carbon nanosheet extensions grown on electrode graphite is investigated. These petal-like structures, composed of 5-25 layers of graphene, are synthesized using microwave plasma chemical vapor deposition. Samples are intercalated with potassium, and a hemispherical energy analyzer is used to measure the emission intensity caused by both thermal and photonic excitation. The emission from the potassium-intercalated structures is found to consistently decrease the work function by 2.4 to 2.8 eV relative to non-intercalated samples. High emission intensity induced by photonic excitation from a solar simulator, with a narrow electron energy distribution relative to established theory, suggests that electron scattering decreases emitted electron energy as compared to surface photoemission. A modified photoemission theory is applied to account for electron scattering, and the sample work function and mean number of scattering events are used as parameters to fit theory to experimental data. The thermal stability of the intercalated nanopetals is investigated, and after an initial heating and cooling cycle, the samples are stable at low temperatures.

  19. Electron doping evolution of the magnetic excitations in NaFe1 xCoxAs

    DOE PAGESBeta

    Carr, Scott V.; Zhang, Chenglin; Song, Yu; Tan, Guotai; Li, Yu; Abernathy, Douglas L.; Stone, Matthew B.; Granroth, Garrett E.; Perring, T. G.; Dai, Pengcheng

    2016-06-13

    We use time-of-flight (TOF) inelastic neutron scattering (INS) spectroscopy to investigate the doping dependence of magnetic excitations across the phase diagram of NaFe1-xCoxAs with x = 0, 0.0175, 0.0215, 0.05, and 0.11. The effect of electron-doping by partially substituting Fe by Co is to form resonances that couple with superconductivity, broaden and suppress low energy (E 80 meV) spin excitations compared with spin waves in undoped NaFeAs. However, high energy (E > 80 meV) spin excitations are weakly Co-doping dependent. Integration of the local spin dynamic susceptibility "(!) of NaFe1-xCoxAs reveals a total fluctuating moment of 3.6 μ2 B/Fe andmore » a small but systematic reduction with electron doping. The presence of a large spin gap in the Cooverdoped nonsuperconducting NaFe0.89Co0.11As suggests that Fermi surface nesting is responsible for low-energy spin excitations. These results parallel Ni-doping evolution of spin excitations in BaFe2-xNixAs2, confirming the notion that low-energy spin excitations coupling with itinerant electrons are important for superconductivity, while weakly doping dependent high-energy spin excitations result from localized moments.« less

  20. Electron densities and the excitation of CN in molecular clouds

    NASA Technical Reports Server (NTRS)

    Black, John H.; Van Dishoeck, Ewine F.

    1991-01-01

    In molecular clouds of modest density and relatively high fractional ionization, the rotational excitation of CN is controlled by a competition among electron impact, neutral impact and the interaction with the cosmic background radiation. The degree of excitation can be measured through optical absorption lines and millimeter-wave emission lines. The available, accurate data on CN in diffuse and translucent molecular clouds are assembled and used to determine electron densities. The derived values, n(e) = roughly 0.02 - 0.5/cu cm, imply modest neutral densities, which generally agree well with determinations by other techniques. The absorption- and emission-line measurements of CN both exclude densities higher than n(H2) = roughly 10 exp 3.5/cu cm on scales varying from 0.001 to 60 arcsec in these clouds.

  1. The role of electron-impact vibrational excitation in electron transport through gaseous tetrahydrofuran

    SciTech Connect

    Duque, H. V.; Do, T. P. T.; Konovalov, D. A.; White, R. D.; Brunger, M. J. E-mail: darryl.jones@flinders.edu.au; Jones, D. B. E-mail: darryl.jones@flinders.edu.au

    2015-03-28

    In this paper, we report newly derived integral cross sections (ICSs) for electron impact vibrational excitation of tetrahydrofuran (THF) at intermediate impact energies. These cross sections extend the currently available data from 20 to 50 eV. Further, they indicate that the previously recommended THF ICS set [Garland et al., Phys. Rev. A 88, 062712 (2013)] underestimated the strength of the electron-impact vibrational excitation processes. Thus, that recommended vibrational cross section set is revised to address those deficiencies. Electron swarm transport properties were calculated with the amended vibrational cross section set, to quantify the role of electron-driven vibrational excitation in describing the macroscopic swarm phenomena. Here, significant differences of up to 17% in the transport coefficients were observed between the calculations performed using the original and revised cross section sets for vibrational excitation.

  2. Excitation of plasmonic nanoantennas by nonresonant and resonant electron tunnelling.

    PubMed

    Uskov, Alexander V; Khurgin, Jacob B; Protsenko, Igor E; Smetanin, Igor V; Bouhelier, Alexandre

    2016-08-14

    A rigorous theory of photon emission generated by inelastic electron tunnelling inside the gap of plasmonic nanoantennas is developed. The disappointingly low efficiency of the electrical excitation of surface plasmon polaritons in these structures can be increased by orders of magnitude when a resonant tunnelling structure is incorporated inside the gap. A resonant tunnelling assisted surface plasmon emitter may become a key element in future electrically-driven plasmonic nanocircuits. PMID:27427159

  3. Electron acceleration by parametrically excited Langmuir waves. [in ionospheric modification

    NASA Technical Reports Server (NTRS)

    Fejer, J. A.; Graham, K. N.

    1974-01-01

    Simple physical arguments are used to estimate the downward-going energetic electron flux due to parametrically excited Langmuir waves in ionospheric modification experiments. The acceleration mechanism is a single velocity reversal as seen in the frame of the Langmuir wave. The flux is sufficient to produce the observed ionospheric airglow if focusing-type instabilities are invoked to produce moderate local enhancements of the pump field.

  4. Ultrafast Structural Dynamics of Tertiary Amines upon Electronic Excitation

    NASA Astrophysics Data System (ADS)

    Cheng, Xinxin; Minitti, Michael P.; Deb, Sanghamitra; Zhang, Yao; Budarz, James; Weber, Peter M.

    2011-06-01

    The structural response of several tertiary amines to electronic excitation has been investigated using Rydberg Fingerprint Spectroscopy. The 3p Rydberg states are reached by excitation with a 5.93 eV photon while 3s states are populated by electronic relaxation from 3p state. We observe binding energy shifts on ultrafast time scales in all peaks that reflect the structural change of the molecular ion cores. The shifts are in the range of 15 meV to 30 meV, within time scales of less than 500 fs, depending on the specific molecular systems and the nature of the electronic state. In cases where the p states are spectrally separate, the trends of the energy shifts are different for the p_z and p_x_y Rydberg states whereas the p_z and s states are similar. This suggests that the response of the Rydberg states to structural displacements depends on the symmetry. Very fast binding energy shifts, observed on sub-picosecond time scales, are attributed to the structural adjustment from a pyramidal to a planar structure upon Rydberg excitation. The quantitative values of the binding energy shifts can also be affected by laser chirp, which we model using simulations.

  5. Collisional energy transfer and quenching of electronic excitation

    PubMed Central

    Lin, S. H.; Eyring, H.

    1975-01-01

    The purpose of this paper has been to explore in a preliminary way the nature and mechanism of collisional energy transfer and quenching of electronic excitation. For this purpose, the Born approximation has been used, and the triplet-triplet and singlet-singlet transfer, and the triplet-triplet and singlet-singlet quenching have been studied. It has been shown theoretically that (i) the singlet-singlet transfer constants (or cross sections) are always larger than the triplet-triplet transfer constants (or cross sections) for the same system of donor and acceptor; (ii) for the singlet-singlet transfer, the observed cross section varies linearly with respect to the spectral overlap between the donor emission and the acceptor absorption; (iii) the reason that the quenching constants (or cross sections) are always smaller than the energy transfer constants (or cross sections) is due to the fact that for the quenching the vibration of the acceptor hardly participates in accepting the electronic excitation and for the energy transfer only part of the excited electron energy of the donor is converted into the energy of nuclear motion; and (iv) the polar acceptor molecules are better quenchers than nonpolar acceptor molecules. PMID:16592281

  6. Search for Nuclear Excitation by Electronic Transition in U-235

    NASA Astrophysics Data System (ADS)

    Chodash, P. A.; Norman, E. B.; Burke, J. T.; Wilks, S. C.; Casperson, R. J.; Swanberg, E. L.; Wakeling, M. A.; Cordeiro, T. J.

    2013-10-01

    Nuclear excitation by electronic transition (NEET) is a rare nuclear excitation that is predicted to occur in numerous isotopes, including U-235. When a nuclear transition matches the energy and the multipolarity of an electronic transition, there is a possibility that NEET will occur. If NEET were to occur in U-235, the nucleus would be excited to its 1/2 + isomeric state that subsequently decays by internal conversion with a decay energy of 77 eV and a half-life of 26 minutes. Theory predicts that NEET can occur in partially ionized uranium plasma with a charge state of 23 +. A pulsed Nd:YAG laser operating at 1064 nm with a pulse energy of 780 mJ and a pulse width of 9 ns was used to generate the uranium plasma. The plasma was collected on a plate and the internal conversion electrons were focused onto a microchannel plate detector by a series of electrostatic lenses. Depleted uranium and highly enriched uranium samples were used for the experiment. Preliminary results will be presented. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344. This work was further supported by the U.S. DHS, UC Berkeley, and the NNIS Fellowship.

  7. Explicit calculation of the excited electronic states of the photosystem II reaction centre.

    PubMed

    Frankcombe, Terry J

    2015-02-01

    The excited states of sets of the cofactors found in the photosystem II reaction centre have been calculated directly as a multi-monomer supermolecule for the first time. Time-dependent density functional theory was used with the CAM-B3LYP functional. Multiple excited states for each cofactor were found at lower energies than the lowest energy state corresponding to charge transfer states (in which an electron is shifted from one cofactor to another). The electrostatic environment was found to have a dramatic impact on the excited state energies, with the effect of a surrounding dielectric medium being less significant. PMID:25523136

  8. Electron plasma dynamics during autoresonant excitation of the diocotron mode

    SciTech Connect

    Baker, C. J. Danielson, J. R. Hurst, N. C. Surko, C. M.

    2015-02-15

    Chirped-frequency autoresonant excitation of the diocotron mode is used to move electron plasmas confined in a Penning-Malmberg trap across the magnetic field for advanced plasma and antimatter applications. Plasmas of 10{sup 8} electrons, with radii small compared to that of the confining electrodes, can be moved from the magnetic axis to ≥90% of the electrode radius with near unit efficiency and reliable angular positioning. Translations of ≥70% of the wall radius are possible for a wider range of plasma parameters. Details of this process, including phase and displacement oscillations in the plasma response and plasma expansion, are discussed, as well as possible extensions of the technique.

  9. Excitation of whistler waves by reflected auroral electrons

    NASA Technical Reports Server (NTRS)

    Wu, C. S.; Dillenburg, D.; Ziebell, L. F.; Freund, H. P.

    1983-01-01

    Excitation of electron waves and whistlers by reflected auroral electrons which possess a loss-cone distribution is investigated. Based on a given magnetic field and density model, the instability problem is studied over a broad region along the auroral field lines. This region covers altitudes ranging from one quarter of an earth radius to five earth radii. It is found that the growth rate is significant only in the region of low altitude, say below the source region of the auroral kilometric radiation. In the high altitude region the instability is insignificant either because of low refractive indices or because of small loss cone angles.

  10. Electronic properties of solids excited with intermediate laser power densities

    NASA Astrophysics Data System (ADS)

    Sirotti, Fausto; Tempo Beamline Team

    Intermediate laser power density up to about 100 GW/cm2 is below the surface damage threshold is currently used to induce modification in the physical properties on short time scales. The absorption of a short laser pulse induces non-equilibrium electronic distributions followed by lattice-mediated equilibrium taking place only in the picosecond range. The role of the hot electrons is particularly important in several domains as for example fast magnetization and demagnetization processes, laser induced phase transitions, charge density waves. Angular resolved photoelectron spectroscopy measuring directly energy and momentum of electrons is the most adapted tool to study the electronic excitations at short time scales during and after fast laser excitations. The main technical problem is the space charge created by the pumping laser pulse. I will present angular resolved multiphoton photoemission results obtained with 800 nm laser pulses showing how space charge electrons emitted during fast demagnetization processes can be measured. Unable enter Affiliation: CNRS-SOLEIL Synchrotron L'Orme des Merisiers , Saint Aubin 91192 Gif sur Yvette France.

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

    PubMed

    Yang, Yang; Davidson, Ernest R; Yang, Weitao

    2016-08-30

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

  12. Quantitative Measurements of Electronically Excited CH Concentration in Normal Gravity and Microgravity Coflow Laminar Diffusion Flames

    NASA Technical Reports Server (NTRS)

    Giassi, D.; Cao, S.; Stocker, D. P.; Takahashi, F.; Bennett, B. A. V.; Smooke, M. D.; Long, M. B.

    2015-01-01

    With the conclusion of the SLICE campaign aboard the ISS in 2012, a large amount of data was made available for the analysis of the effect of microgravity on laminar coflow diffusion flames. Previous work focused on the study of sooty flames in microgravity as well as the ability of numerical models to predict its formation in a simplified buoyancy-free environment. The current work shifts the investigation to soot-free flames, putting an emphasis on the chemiluminescence emission from electronically excited CH (CH*). This radical species is of significant interest in combustion studies: it has been shown that the electronically excited CH spatial distribution is indicative of the flame front position and, given the relatively simple diagnostic involved with its measurement, several works have been done trying to understand the ability of electronically excited CH chemiluminescence to predict the total and local flame heat release rate. In this work, a subset of the SLICE nitrogen-diluted methane flames has been considered, and the effect of fuel and coflow velocity on electronically excited CH concentration is discussed and compared with both normal gravity results and numerical simulations. Experimentally, the spectral characterization of the DSLR color camera used to acquire the flame images allowed the signal collected by the blue channel to be considered representative of the electronically excited CH emission centered around 431 nm. Due to the axisymmetric flame structure, an Abel deconvolution of the line-of-sight chemiluminescence was used to obtain the radial intensity profile and, thanks to an absolute light intensity calibration, a quantification of the electronically excited CH concentration was possible. Results show that, in microgravity, the maximum flame electronically excited CH concentration increases with the coflow velocity, but it is weakly dependent on the fuel velocity; normal gravity flames, if not lifted, tend to follow the same trend

  13. Optically Induced Nuclear Spin Polarization in the Quantum Hall Regime: The Effect of Electron Spin Polarization through Exciton and Trion Excitations

    NASA Astrophysics Data System (ADS)

    Akiba, K.; Kanasugi, S.; Yuge, T.; Nagase, K.; Hirayama, Y.

    2015-07-01

    We study nuclear spin polarization in the quantum Hall regime through the optically pumped electron spin polarization in the lowest Landau level. The nuclear spin polarization is measured as a nuclear magnetic field BN by means of the sensitive resistive detection. We find the dependence of BN on the filling factor nonmonotonic. The comprehensive measurements of BN with the help of the circularly polarized photoluminescence measurements indicate the participation of the photoexcited complexes, i.e., the exciton and trion (charged exciton), in nuclear spin polarization. On the basis of a novel estimation method of the equilibrium electron spin polarization, we analyze the experimental data and conclude that the filling factor dependence of BN is understood by the effect of electron spin polarization through excitons and trions.

  14. Optically Induced Nuclear Spin Polarization in the Quantum Hall Regime: The Effect of Electron Spin Polarization through Exciton and Trion Excitations.

    PubMed

    Akiba, K; Kanasugi, S; Yuge, T; Nagase, K; Hirayama, Y

    2015-07-10

    We study nuclear spin polarization in the quantum Hall regime through the optically pumped electron spin polarization in the lowest Landau level. The nuclear spin polarization is measured as a nuclear magnetic field B(N) by means of the sensitive resistive detection. We find the dependence of B(N) on the filling factor nonmonotonic. The comprehensive measurements of B(N) with the help of the circularly polarized photoluminescence measurements indicate the participation of the photoexcited complexes, i.e., the exciton and trion (charged exciton), in nuclear spin polarization. On the basis of a novel estimation method of the equilibrium electron spin polarization, we analyze the experimental data and conclude that the filling factor dependence of B(N) is understood by the effect of electron spin polarization through excitons and trions. PMID:26207494

  15. Review of electron impact excitation cross sections for copper atom

    SciTech Connect

    Winter, N.W.; Hazi, A.U.

    1982-02-01

    Excitation of atomic copper by electron impact plays an important role in the copper vapor laser and accurate cross sections are needed for understanding and modeling laser performance. During the past seven years, there have been several attempts to normalize the relative elastic and inelastic cross sections measured by Trajmar and coworkers. However, each of these efforts have yielded different cross sections, and the uncertainty in the correct normalization of the data has been a source of confusion and concern for the kinetic modeling efforts. This difficulty has motivated us to review previous work on the electron impact excitation of copper atom and to perform new calculations of the inelastic cross sections using the impact parameter method. In this memorandum we review the previous attempts to normalize the experimental data and provide a critical assessment of the accuracy of the resulting cross sections. We also present new theoretical cross sections for the electron impact excitation of the /sup 2/S ..-->.. /sup 2/P/sup 0/ and /sup 2/S ..-->.. /sup 2/D transitions in copper. When the experimental cross sections are renormalized to the results of the impact parameter calculations, they are a factor of three smaller than those published in the latest paper of Trajmar et. al. At impact energies above 60 eV the excitation cross sections obtained with the impact parameter method agree well with the results of the very recent, unpublished, close-coupling calculations of Henry. This agreement suggests that the present normalization of the experimental cross sections is probably the most reliable one obtained to date.

  16. Validation of local hybrid functionals for TDDFT calculations of electronic excitation energies

    NASA Astrophysics Data System (ADS)

    Maier, Toni M.; Bahmann, Hilke; Arbuznikov, Alexei V.; Kaupp, Martin

    2016-02-01

    The first systematic evaluation of local hybrid functionals for the calculation of electronic excitation energies within linear-response time-dependent density functional theory (TDDFT) is reported. Using our recent efficient semi-numerical TDDFT implementation [T. M. Maier et al., J. Chem. Theory Comput. 11, 4226 (2015)], four simple, thermochemically optimized one-parameter local hybrid functionals based on local spin-density exchange are evaluated against a database of singlet and triplet valence excitations of organic molecules, and against a mixed database including also Rydberg, intramolecular charge-transfer (CT) and core excitations. The four local hybrids exhibit comparable performance to standard global or range-separated hybrid functionals for common singlet valence excitations, but several local hybrids outperform all other functionals tested for the triplet excitations of the first test set, as well as for relative energies of excited states. Evaluation for the combined second test set shows that local hybrids can also provide excellent Rydberg and core excitations, in the latter case rivaling specialized functionals optimized specifically for such excitations. This good performance of local hybrids for different excitation types could be traced to relatively large exact-exchange (EXX) admixtures in a spatial region intermediate between valence and asymptotics, as well as close to the nucleus, and lower EXX admixtures in the valence region. In contrast, the tested local hybrids cannot compete with the best range-separated hybrids for intra- and intermolecular CT excitation energies. Possible directions for improvement in the latter category are discussed. As the used efficient TDDFT implementation requires essentially the same computational effort for global and local hybrids, applications of local hybrid functionals to excited-state problems appear promising in a wide range of fields. Influences of current-density dependence of local kinetic

  17. Electronically Excited C2 from Laser Photodissociated C60

    NASA Technical Reports Server (NTRS)

    Arepalli, Sivaram; Scott, Carl D.; Nikolaev, Pavel; Smalley, Richard E.

    1999-01-01

    Spectral and transient emission measurements are made of radiation from products of laser excitation of buckminsterfullerene (C60) vapor diluted in argon at 973 K. The principal radiation is from the Swan band system of C2 and, at early times, also from a black body continuum. The C2 radiation is observed only when C60 is excited by green (532 nm) and not with IR (1064 nm) laser radiation at energy densities of about 1.5 J/square cm. Transient measurements indicate that there are two characteristic periods of decay of radiation. The first period, lasting about 2 micro seconds, has a characteristic decay time of about 0.3 micro seconds. The second period, lasting at least 50 micro seconds, has a characteristic decay time of about 5 micro seconds. These characteristic times are thought to be associated with cooling of C60 molecules or nanosized carbon particles during the early period; and with electronically excited C2 that is a decomposition product of laser excited C60, C58, ... molecules during the later period.

  18. Complete Solution of Electronic Excitation and Ionization in Electron-Hydrogen Molecule Scattering.

    PubMed

    Zammit, Mark C; Savage, Jeremy S; Fursa, Dmitry V; Bray, Igor

    2016-06-10

    The convergent close-coupling method has been used to solve the electron-hydrogen molecule scattering problem in the fixed-nuclei approximation. Excellent agreement with experiment is found for the grand total, elastic, electronic-excitation, and total ionization cross sections from the very low to the very high energies. This shows that for the electronic degrees of freedom the method provides a complete treatment of electron scattering on molecules as it does for atoms. PMID:27341229

  19. Complete solution of electronic excitation and ionization in electron-hydrogen molecule scattering

    DOE PAGESBeta

    Zammit, Mark C.; Savage, Jeremy S.; Fursa, Dmitry V.; Bray, Igor

    2016-06-01

    The convergent close-coupling method has been used to solve the electron-hydrogen molecule scattering problem in the fixed-nuclei approximation. Excellent agreement with experiment is found for the grand total, elastic, electronic-excitation, and total ionization cross sections from the very low to the very high energies. This shows that for the electronic degrees of freedom the method provides a complete treatment of electron scattering on molecules as it does for atoms.

  20. Complete Solution of Electronic Excitation and Ionization in Electron-Hydrogen Molecule Scattering

    NASA Astrophysics Data System (ADS)

    Zammit, Mark C.; Savage, Jeremy S.; Fursa, Dmitry V.; Bray, Igor

    2016-06-01

    The convergent close-coupling method has been used to solve the electron-hydrogen molecule scattering problem in the fixed-nuclei approximation. Excellent agreement with experiment is found for the grand total, elastic, electronic-excitation, and total ionization cross sections from the very low to the very high energies. This shows that for the electronic degrees of freedom the method provides a complete treatment of electron scattering on molecules as it does for atoms.

  1. Absolute cross sections for electronic excitation of pyrimidine by electron impact.

    PubMed

    Regeta, Khrystyna; Allan, Michael; Mašín, Zdeněk; Gorfinkiel, Jimena D

    2016-01-14

    We measured differential cross sections for electron-impact electronic excitation of pyrimidine, both as a function of electron energy up to 18 eV, and of scattering angle up to 180°. The emphasis of the present work is on recording detailed excitation functions revealing resonances in the excitation process. The differential cross sections were summed to obtain integral cross sections. These are compared to results of R-matrix calculations, which successfully reproduce both the magnitude of the cross section and the major resonant features. Comparison of the experiment to the calculated contributions of different symmetries to the integral cross section permitted assignment of several features to specific core-excited resonances. Comparison of the resonant structure of pyrimidine with that of benzene revealed pronounced similarities and thus a dominant role of π-π(∗) excited states and resonances. Electron energy loss spectra were measured as a preparation for the cross section measurements and vibrational structure was observed for some of the triplet states. A detailed analysis of the electronic excited states of pyrimidine is also presented. PMID:26772566

  2. Excitation of plasmonic nanoantennas by nonresonant and resonant electron tunnelling

    NASA Astrophysics Data System (ADS)

    Uskov, Alexander V.; Khurgin, Jacob B.; Protsenko, Igor E.; Smetanin, Igor V.; Bouhelier, Alexandre

    2016-07-01

    A rigorous theory of photon emission generated by inelastic electron tunnelling inside the gap of plasmonic nanoantennas is developed. The disappointingly low efficiency of the electrical excitation of surface plasmon polaritons in these structures can be increased by orders of magnitude when a resonant tunnelling structure is incorporated inside the gap. A resonant tunnelling assisted surface plasmon emitter may become a key element in future electrically-driven plasmonic nanocircuits.A rigorous theory of photon emission generated by inelastic electron tunnelling inside the gap of plasmonic nanoantennas is developed. The disappointingly low efficiency of the electrical excitation of surface plasmon polaritons in these structures can be increased by orders of magnitude when a resonant tunnelling structure is incorporated inside the gap. A resonant tunnelling assisted surface plasmon emitter may become a key element in future electrically-driven plasmonic nanocircuits. Electronic supplementary information (ESI) available: Plasmonic mode in nanowires, the probability of stimulated emission in tunnelling through the Fermi's Golden Rule and electron wave functions in tunnelling structures with nonresonant and resonant tunnelling. See DOI: 10.1039/c6nr01931e

  3. Experimental investigation of the ionospheric hysteresis effect on the threshold excitation level of the Stimulated Electromagnetic Emission (SEE) during heating at the second electron gyro-harmonic frequency

    NASA Astrophysics Data System (ADS)

    Samimi, A.; Scales, W.; Cruz, M.; Isham, B.; Bernhardt, P. A.

    2012-12-01

    Recent experimental observations of the stimulated electromagnetic emission (SEE) spectrum during heating at the second electron gyro-harmonic show structures ordered by ion gyro-frequency. The proposed generation mechanism considers parametric decay of a pump upper hybrid/electron Bernstein (UH/EB) wave into another UH/EB and a group of neutralized ion Bernstein waves. The presumption of the proposed mechanism is that the pump electromagnetic wave is converted into the UH/EB wave. This conversion process generates field aligned irregularity which exhibits hysteresis effect. The predicted ionospheric hysteresis effect is studied during the PARS 2012 at HAARP. The preliminary results are presented for the first time. Also, experimental study of the effects of 1) the transmitter beam angle and 2) the transmitter frequency offset relative to the second electron gyro-harmonic frequency on the ion gyro-harmonic structures in the SEE spectrum are provided. The aforementioned observations are compared to the predictions of the analytical model. Possible connection of the SEE spectral features and artificially generated ionospheric descending layer is also discussed

  4. Model for the hyperfine structure of electronically excited KCs molecules

    NASA Astrophysics Data System (ADS)

    Orbán, A.; Vexiau, R.; Krieglsteiner, O.; Nägerl, H.-C.; Dulieu, O.; Crubellier, A.; Bouloufa-Maafa, N.

    2015-09-01

    A model for determining the hyperfine structure of the excited electronic states of diatomic bialkali heteronuclear molecules is formulated from the atomic hyperfine interactions and is applied to the case of bosonic 39KCs and fermionic 40KCs molecules. The hyperfine structure of the potential-energy curves of the states correlated to the K (4 s 2S1 /2) +Cs (6 p 2P1 /2 ,3 /2) dissociation limits is described in terms of different coupling schemes depending on the internuclear distance R . These results provide a step in the calculation of the hyperfine structure of rovibrational levels of these excited molecular states in the perspective of the identification of efficient paths for creating ultracold ground-state KCs molecules.

  5. Electron impact collision strengths for excitation of highly charged ions

    SciTech Connect

    Sampson, D.H. . Dept. of Astronomy and Astrophysics)

    1990-08-20

    The principle task given us by the Lawrence Livermore National Laboratory (LLNL) to perform under Subcontract 6181405 was to develop a method and corresponding computer programs to make very rapid, yet accurate, fully relativistic and quasirelativistic calculations of cross sections or collision strengths for electron impact excitation of highly charged ions with any value for the nuclear charge number Z. Also while this major code development was being done we were asked to calculate cross sections of interest using our previous rapid, more approximate codes, which used hydrogenic basis functions and screening constants with both the electron-electron Coulomb interaction and relativistic interactions included by perturbation theory. We were also asked to determine the branching ratio for ionization to various final states in complex cases, where two or more states corresponding to the final configuration of the ion were possible.

  6. Does electron-transfer theory explain large rate differences in singlet and triplet excited state electron-transfer reactions?

    SciTech Connect

    Zusman, L.D.; Kurnikov, I.V.; Beratan, D.N.

    1995-12-31

    Gray and coworkers have shown that intramolecular electron-transfer rates from singlet and triplet excited states in iridium(spacer)pyridinium complexes can be vastly different (>5 orders of magnitude). We have analyzed the possible sources of these differences, including effects that may arise from reorganization energies, free energies, and tunneling matrix elements. When distance dependent reorganization energies and energy dependent tunneling matrix elements are included, a systematic framework emerges to describe these electron-transfer reactions.

  7. Electronic Ground and Excited State Spectral Diffusion of a Photocatalyst

    NASA Astrophysics Data System (ADS)

    Kiefer, Laura M.; King, John T.; Kubarych, Kevin J.

    2014-06-01

    Re(bpy)(CO)_3Cl is a well studied CO_2 reduction catalyst, known for its ability as both a photosensitizer and a catalyst with a high quantum yield and product selectivity. The catalysis reaction is initiated by a 400 nm excitation, followed by an intersystem crossing (ISC) and re-equilibration in the lowest triplet state. We utilize the quasi-equilibrium nature of this long-lived triplet metal-to-ligand charge-transfer (3MLCT) state to completely characterize the solvent dynamics using the technique of transient two-dimensional infrared (t-2DIR) spectroscopy to extract observables such as the frequency-frequency correlation function (FFCF), an equilibrium function. The electronic ground state solvent dynamics are characterized using equilibrium two-dimensional infrared spectroscopy (2D IR). Our technique allows us to independently observe the solvent dynamics of different electronic states and compare them. In this study, three carbonyl stretching modes were utilized to probe both the intramolecular and solvent environments in each electronic state. In the electronic ground state, the totally symmetric mode exhibits pure homogeneous broadening and a lack of spectral dynamics, while the two other modes have similar FFCF decay times of ˜ 1.5 ps. In the 3MLCT, however, all three modes experience similar spectral dynamics and have a FFCF decay time of ˜ 4.5 ps, three times slower than in the electronic ground state. Our technique allows us to directly observe the differences in spectral dynamics of the ground and excited electronic states and allows us to attribute the differences to specific origins such as solvent-solute coupling and molecular flexibility.

  8. An amorphous phase formation at palladium / silicon oxide (Pd/SiOx) interface through electron irradiation - electronic excitation process

    NASA Astrophysics Data System (ADS)

    Nagase, Takeshi; Yamashita, Ryo; Yabuuchi, Atsushi; Lee, Jung-Goo

    2015-11-01

    A Pd-Si amorphous phase was formed at a palladium/silicon oxide (Pd/SiOx) interface at room temperature by electron irradiation at acceleration voltages ranging between 25 kV and 200 kV. Solid-state amorphization was stimulated without the electron knock-on effects. The total dose required for the solid-state amorphization decreases with decreasing acceleration voltage. This is the first report on electron irradiation induced metallic amorphous formation caused by the electronic excitation at metal/silicon oxide interface.

  9. Influence of surface excitations on electrons elastically backscattered from copper and silver surfaces

    NASA Astrophysics Data System (ADS)

    Chen, Y. F.; Su, P.; Kwei, C. M.; Tung, C. J.

    1994-12-01

    The influence of surface excitations on electrons elastically backscattered from solid surfaces is investigated. Elastic-scattering differential cross sections are calculated using the partial-wave expansion method and the finite difference techique for solid atoms with the Hartree-Fock-Wigner-Seitz potential. An extended Drude dielectric function which allows the characteristic oscillator strength, damping constant, and critical-point energy for each subband of valence electrons is employed to estimate electron inelastic mean free paths for volume excitations. The same dielectric function is applied to evaluate the probability of surface excitations for incident and escape electrons by including the recoil effect without the small-angle approximation. Results of Monte Carlo simulations on the elastic reflection coefficient and the angular distribution of electrons elastically backscattered from Cu and Ag surfaces are presented. It is revealed that surface excitations significantly reduce the elastic reflection coefficient for low-energy electrons, but less significantly influence the angular distribution for large escape angles. Our results agree very well with experimental data.

  10. Study of intermediates from transition metal excited-state electron- transfer reactions

    SciTech Connect

    Hoffman, M.Z.

    1993-03-31

    Progress on 6 projects is reported: excited state absorption spectrum of Ru(bpy)[sub 3][sup 2+], solvent cage model for electron transfer quenching, reductive quenching of [sup *]Cr(III) complexes, solution medium effects in oxidative quenching of [sup *]Ru(II) complexes, photosensitized oxidation of phenol in aqueous solution, and quenching of Ru(II) complexes by oxygen.

  11. Electronically excited rubidium atom in a helium cluster or film

    NASA Astrophysics Data System (ADS)

    Leino, Markku; Viel, Alexandra; Zillich, Robert E.

    2008-11-01

    We present theoretical studies of helium droplets and films doped with one electronically excited rubidium atom Rb∗ (P2). Diffusion and path integral Monte Carlo approaches are used to investigate the energetics and the structure of clusters containing up to 14 helium atoms. The surface of large clusters is approximated by a helium film. The nonpair additive potential energy surface is modeled using a diatomic in molecule scheme. Calculations show that the stable structure of Rb∗Hen consists of a seven helium atom ring centered at the rubidium, surrounded by a tirelike second solvation shell. A very different structure is obtained when performing a "vertical Monte Carlo transition." In this approach, a path integral Monte Carlo equilibration starts from the stable configuration of a rubidium atom in the electronic ground state adsorbed to the helium surface after switching to the electronically excited surface. In this case, Rb∗Hen relaxes to a weakly bound metastable state in which Rb∗ sits in a shallow dimple. The interpretation of the results is consistent with the recent experimental observations [G. Auböck et al., Phys. Rev. Lett. 101, 035301 (2008)].

  12. Excitation of surface modes by electron beam in semi-bounded quantum plasma

    SciTech Connect

    Mohamed, B. F.; Elbasha, N. M.

    2015-10-15

    The excitation of the TM surface modes due to the interaction of electron beam with a semi-bounded quantum magnetized plasma is investigated. The generated current and the perturbed densities of the electron beam and plasma are obtained. The wave equation that describes the excited fields has been solved to obtain the dispersion relation for these modes. It is found that the quantum effects play important role for frequencies less and bigger than plasma frequency such that the phase velocity of modes increases with increasing the quantum effects compared to the classical case. It has also been displayed that in the absence of external magnetic field, the surface modes appear in the all regions of the wavelength while they have been only excited for high wavenumber in the presence of the magnetic field. Besides, it has been shown that the dispersion curves of the modes depend essentially on the density ratio of beam and plasma.

  13. Thermally excited modes in a pure electron plasma.

    PubMed

    Anderegg, F; Shiga, N; Danielson, J R; Dubin, D H E; Driscoll, C F; Gould, R W

    2003-03-21

    Thermally excited plasma modes are observed in near-thermal-equilibrium pure electron plasmas over a temperature range of 0.05

  14. Inner-shell excitation of acetylene by electron impact

    SciTech Connect

    Michelin, S.E.; Pessoa, O.; Oliveira, H.L.; Veiteinheimer, E.; Santos, A.M.S.; Fujimoto, M.M.; Iga, I.; Lee, M.-T.

    2005-08-15

    The distorted-wave approximation (DWA) is applied to study K-shell excitation in C{sub 2}H{sub 2} by electron impact. More specifically, calculated differential and integral cross sections for the X {sup 1}{sigma}{sub g}{sup +}{yields}{sup 1,3}{pi}{sub g}(1s{sigma}{sub g}{yields}1p{pi}{sub g}) and X {sup 1}{sigma}{sub g}{sup +}{yields}{sup 1,3}{pi}{sub u}(1s{sigma}{sub u}{yields}1p{pi}{sub g}) transitions in this target in the 300-800 eV incident energy range are reported. The triplet-to-singlet ratios of respective integral cross sections, namely, RI(3:1), calculated by dividing the integral cross sections for transitions leading to the triplet core-excited states by those leading to the corresponding singlet states, are also reported as a function of incident energies. In general, our calculated sums of the generalized oscillator strength for transitions leading to the {sup 1}{pi}{sub g} and {sup 1}{pi}{sub u} excited states are in good agreement with the available experimental data. On the other hand, the present calculated integral cross sections and the corresponding data for its isoelectronic species CO are significantly different. Possible physical origins for this difference are discussed.

  15. High resolution fluorescent bio-imaging with electron beam excitation.

    PubMed

    Kawata, Yoshimasa; Nawa, Yasunori; Inami, Wataru

    2014-11-01

    We have developed electron beam excitation assisted (EXA) optical microscope[1-3], and demonstrated its resolution higher than 50 nm. In the microscope, a light source in a few nanometers size is excited by focused electron beam in a luminescent film. The microscope makes it possible to observe dynamic behavior of living biological specimens in various surroundings, such as air or liquids. Scan speed of the nanometric light source is faster than that in conventional near-field scanning optical microscopes. The microscope enables to observe optical constants such as absorption, refractive index, polarization, and their dynamic behavior on a nanometric scale. The microscope opens new microscopy applications in nano-technology and nano-science.Figure 1(a) shows schematic diagram of the proposed EXA microscope. An electron beam is focused on a luminescent film. A specimen is put on the luminescent film directly. The inset in Fig. 1(a) shows magnified image of the luminescent film and the specimen. Nanometric light source is excited in the luminescent film by the focused electron beam. The nanometric light source illuminates the specimen, and the scattered or transmitted radiation is detected with a photomultiplier tube (PMT). The light source is scanned by scanning of the focused electron beam in order to construct on image. Figure 1(b) shows a luminescence image of the cells acquired with the EXA microscope, and Fig. 1(c) shows a phase contrast microscope image. Cells were observed in culture solution without any treatments, such as fixation and drying. The shape of each cell was clearly recognized and some bright spots were observed in cells. We believe that the bright spots indicated with arrows were auto-fluorescence of intracellular granules and light- grey regions were auto-fluorescence of cell membranes. It is clearly demonstrated that the EXA microscope is useful tool for observation of living biological cells in physiological conditions.jmicro;63/suppl_1/i

  16. Spin-orbit coupling induced magnetic field effects in electron-transfer reactions with excited triplets: The role of triplet exciplexes and radical pairs in geminate recombination

    SciTech Connect

    Steiner, U.E.; Haas, W. )

    1991-03-07

    The magnetic field dependence of free-radical yield in the electron-transfer quenching of methylene blue triplet by p-iodoaniline has been determined between 0.00 and 3.30 T in methanol/ethylene glycol mixtures of various viscosities by using laser flash spectroscopy and a photostationary flow technique. The observed decrease of the free-radical yield with the magnetic field is interpreted by heavy-atom-induced spin-orbit coupling causing magnetic field sensitivity according to the triplet mechanism (TM) in intermediate triplet exciplexes and to the {Delta}g type radical pair mechanism (RPM) in germinate triplet radical pairs originating from dissociation of the triplet exciplexes. Analytical expressions are provided for a treatment of a combination of both mechanisms including the case of reversible formation of the triplet exciplex from the geminate radical pair. The formalism of Pedersen developed for the high field radical pair mechanism and modified by Vollenweider and Fischer to account for effects of exchange interaction is generalized to include various boundary conditions for the electron spin density matrix suggested in the literature to describe the effects of encounters and chemical reaction. With a physically consistent choice of TM and RPM parameters model calculations provide a very good quantitative fit of the observed magnetic field and viscosity dependence of the yield of free radicals.

  17. Direct and secondary nuclear excitation with x-ray free-electron lasers

    SciTech Connect

    Gunst, Jonas; Wu, Yuanbin Kumar, Naveen; Keitel, Christoph H.; Pálffy, Adriana

    2015-11-15

    The direct and secondary nuclear excitation produced by an x-ray free electron laser when interacting with a solid-state nuclear target is investigated theoretically. When driven at the resonance energy, the x-ray free electron laser can produce direct photoexcitation. However, the dominant process in that interaction is the photoelectric effect producing a cold and very dense plasma in which also secondary processes such as nuclear excitation by electron capture may occur. We develop a realistic theoretical model to quantify the temporal dynamics of the plasma and the magnitude of the secondary excitation therein. Numerical results show that depending on the nuclear transition energy and the temperature and charge states reached in the plasma, secondary nuclear excitation by electron capture may dominate the direct photoexcitation by several orders of magnitude, as it is the case for the 4.8 keV transition from the isomeric state of {sup 93}Mo, or it can be negligible, as it is the case for the 14.4 keV Mössbauer transition in {sup 57}Fe. These findings are most relevant for future nuclear quantum optics experiments at x-ray free electron laser facilities.

  18. Direct and secondary nuclear excitation with x-ray free-electron lasers

    NASA Astrophysics Data System (ADS)

    Gunst, Jonas; Wu, Yuanbin; Kumar, Naveen; Keitel, Christoph H.; Pálffy, Adriana

    2015-11-01

    The direct and secondary nuclear excitation produced by an x-ray free electron laser when interacting with a solid-state nuclear target is investigated theoretically. When driven at the resonance energy, the x-ray free electron laser can produce direct photoexcitation. However, the dominant process in that interaction is the photoelectric effect producing a cold and very dense plasma in which also secondary processes such as nuclear excitation by electron capture may occur. We develop a realistic theoretical model to quantify the temporal dynamics of the plasma and the magnitude of the secondary excitation therein. Numerical results show that depending on the nuclear transition energy and the temperature and charge states reached in the plasma, secondary nuclear excitation by electron capture may dominate the direct photoexcitation by several orders of magnitude, as it is the case for the 4.8 keV transition from the isomeric state of 93Mo, or it can be negligible, as it is the case for the 14.4 keV Mössbauer transition in 57Fe. These findings are most relevant for future nuclear quantum optics experiments at x-ray free electron laser facilities.

  19. Excited-State Energies and Electronic Couplings of DNA Base Dimers

    SciTech Connect

    Kozak, Christopher R.; Kistler, Kurt A.; Lu, Zhen; Matsika, Spiridoula

    2010-02-04

    The singlet excited electronic states of two π-stacked thymine molecules and their splittings due to electronic coupling have been investigated with a variety of computational methods. Focus has been given on the effect of intermolecular distance on these energies and couplings. Single-reference methods, CIS, CIS(2), EOMCCSD, TDDFT, and the multireference method CASSCF, have been used, and their performance has been compared. It is found that the excited-state energies are very sensitive to the applied method but the couplings are not as sensitive. Inclusion of diffuse functions in the basis set also affects the excitation energies significantly but not the couplings. TDDFT is inadequate in describing the states and their coupling, while CIS(2) gives results very similar to EOM-CCSD. Excited states of cytosine and adenine π-stacked dimers were also obtained and compared with those of thymine dimers to gain a more general picture of excited states in π-stacked DNA base dimers. The coupling is very sensitive to the relative position and orientation of the bases, indicating great variation in the degree of delocalization of the excited states between stacked bases in natural DNA as it fluctuates.

  20. Cold chemistry with electronically excited Ca+ Coulomb crystals.

    PubMed

    Gingell, Alexander D; Bell, Martin T; Oldham, James M; Softley, Timothy P; Harvey, Jeremy N

    2010-11-21

    Rate constants for chemical reactions of laser-cooled Ca(+) ions and neutral polar molecules (CH(3)F, CH(2)F(2), or CH(3)Cl) have been measured at low collision energies (/k(B)=5-243 K). Low kinetic energy ensembles of (40)Ca(+) ions are prepared through Doppler laser cooling to form "Coulomb crystals" in which the ions form a latticelike arrangement in the trapping potential. The trapped ions react with translationally cold beams of polar molecules produced by a quadrupole guide velocity selector or with room-temperature gas admitted into the vacuum chamber. Imaging of the Ca(+) ion fluorescence allows the progress of the reaction to be monitored. Product ions are sympathetically cooled into the crystal structure and are unambiguously identified through resonance-excitation mass spectrometry using just two trapped ions. Variations of the laser-cooling parameters are shown to result in different steady-state populations of the electronic states of (40)Ca(+) involved in the laser-cooling cycle, and these are modeled by solving the optical Bloch equations for the eight-level system. Systematic variation of the steady-state populations over a series of reaction experiments allows the extraction of bimolecular rate constants for reactions of the ground state ((2)S(1/2)) and the combined excited states ((2)D(3/2) and (2)P(1/2)) of (40)Ca(+). These results are analyzed in the context of capture theories and ab initio electronic structure calculations of the reaction profiles. In each case, suppression of the ground state rate constant is explained by the presence of a submerged or real barrier on the ground state potential surface. Rate constants for the excited states are generally found to be in line with capture theories. PMID:21090857

  1. Cold chemistry with electronically excited Ca+ Coulomb crystals

    NASA Astrophysics Data System (ADS)

    Gingell, Alexander D.; Bell, Martin T.; Oldham, James M.; Softley, Timothy P.; Harvey, Jeremy N.

    2010-11-01

    Rate constants for chemical reactions of laser-cooled Ca+ ions and neutral polar molecules (CH3F, CH2F2, or CH3Cl) have been measured at low collision energies (⟨Ecoll⟩/kB=5-243 K). Low kinetic energy ensembles of C40a+ ions are prepared through Doppler laser cooling to form "Coulomb crystals" in which the ions form a latticelike arrangement in the trapping potential. The trapped ions react with translationally cold beams of polar molecules produced by a quadrupole guide velocity selector or with room-temperature gas admitted into the vacuum chamber. Imaging of the Ca+ ion fluorescence allows the progress of the reaction to be monitored. Product ions are sympathetically cooled into the crystal structure and are unambiguously identified through resonance-excitation mass spectrometry using just two trapped ions. Variations of the laser-cooling parameters are shown to result in different steady-state populations of the electronic states of C40a+ involved in the laser-cooling cycle, and these are modeled by solving the optical Bloch equations for the eight-level system. Systematic variation of the steady-state populations over a series of reaction experiments allows the extraction of bimolecular rate constants for reactions of the ground state (S21/2) and the combined excited states (D23/2 and P21/2) of C40a+. These results are analyzed in the context of capture theories and ab initio electronic structure calculations of the reaction profiles. In each case, suppression of the ground state rate constant is explained by the presence of a submerged or real barrier on the ground state potential surface. Rate constants for the excited states are generally found to be in line with capture theories.

  2. Electron impact excitation of resonance transitions in atomic potassium

    SciTech Connect

    Tayal, S.S.; Msezane, A.Z.

    1993-05-01

    Cross sections for electron impact excitation of the 4 s{sup 2}S - 4p {sup 2}P{sup o} and 4s {sup 2}S - 5p {sup 2}P{sup o} transitions in atomic potassium are calculated in the low-energy region from 1.5 to 30 eV using the R-matrix method. We included eight target states (4s {sup 2}S, 4p {sup 2}P{sup o}, 5s {sup 2}S, 3d {sup 2}D, 5p {sup 2}P{sup o}, 4d {sup 2}D, 6S {sup 2}S, and 4f {sup 2}F{sup o}) in the close-coupling expansion. These states are represented by extensive configuration- interaction wavefunctions constructed from the orthogonal one-electron orbitals: 1s, 2s, 2p, 3s, 3p, 3d, 4s, 4p, 4d, 4f, 5s, 5p, and 6s. The calculated results are compared with the available experiments and other calculations. The present calculation shows a resonance structure in the cross section for the excitation of the resonance 4s {sup 2}S - 4p {sup 2}P{sup o} transition around 2.5 eV.

  3. Controlling multipolar surface plasmon excitation through the azimuthal phase structure of electron vortex beams

    NASA Astrophysics Data System (ADS)

    Ugarte, Daniel; Ducati, Caterina

    2016-05-01

    We have theoretically studied how the azimuthal phase structure of an electron vortex beam excites surface plasmons on metal particles of different geometries as observed in electron energy loss spectroscopy (EELS). We have developed a semiclassical approximation combining a ring-shaped beam and the dielectric formalism. Our results indicate that for the case of total orbital angular momentum transfer, we can manipulate surface plasmon multipole excitation and even attain an enhancement factor of several orders of magnitude. Since electron vortex beams interact with particles mostly through effects due to azimuthal symmetry, i.e., in the plane perpendicular to the electron beam, anisotropy information (longitudinal and transversal) of the sample may be derived in EELS studies by comparing nonvortex and vortex beam measurements.

  4. Ultrafast electronic relaxation of excited state vitamin B 12 in the gas phase

    NASA Astrophysics Data System (ADS)

    Shafizadeh, Niloufar; Poisson, Lionel; Soep, Benoıˆt

    2008-06-01

    The time evolution of electronically excited vitamin B 12 (cyanocobalamin) has been observed for the first time in the gas phase. It reveals an ultrafast decay to a state corresponding to metal excitation. This decay is interpreted as resulting from a ring to metal electron transfer. This opens the observation of the excited state of other complex biomimetic systems in the gas phase, the key to the characterisation of their complex evolution through excited electronic states.

  5. Vertical and adiabatic excitations in anthracene from quantum Monte Carlo: Constrained energy minimization for structural and electronic excited-state properties in the JAGP ansatz

    SciTech Connect

    Dupuy, Nicolas; Bouaouli, Samira; Mauri, Francesco Casula, Michele; Sorella, Sandro

    2015-06-07

    We study the ionization energy, electron affinity, and the π → π{sup ∗} ({sup 1}L{sub a}) excitation energy of the anthracene molecule, by means of variational quantum Monte Carlo (QMC) methods based on a Jastrow correlated antisymmetrized geminal power (JAGP) wave function, developed on molecular orbitals (MOs). The MO-based JAGP ansatz allows one to rigorously treat electron transitions, such as the HOMO → LUMO one, which underlies the {sup 1}L{sub a} excited state. We present a QMC optimization scheme able to preserve the rank of the antisymmetrized geminal power matrix, thanks to a constrained minimization with projectors built upon symmetry selected MOs. We show that this approach leads to stable energy minimization and geometry relaxation of both ground and excited states, performed consistently within the correlated QMC framework. Geometry optimization of excited states is needed to make a reliable and direct comparison with experimental adiabatic excitation energies. This is particularly important in π-conjugated and polycyclic aromatic hydrocarbons, where there is a strong interplay between low-lying energy excitations and structural modifications, playing a functional role in many photochemical processes. Anthracene is an ideal benchmark to test these effects. Its geometry relaxation energies upon electron excitation are of up to 0.3 eV in the neutral {sup 1}L{sub a} excited state, while they are of the order of 0.1 eV in electron addition and removal processes. Significant modifications of the ground state bond length alternation are revealed in the QMC excited state geometry optimizations. Our QMC study yields benchmark results for both geometries and energies, with values below chemical accuracy if compared to experiments, once zero point energy effects are taken into account.

  6. Vertical and adiabatic excitations in anthracene from quantum Monte Carlo: Constrained energy minimization for structural and electronic excited-state properties in the JAGP ansatz.

    PubMed

    Dupuy, Nicolas; Bouaouli, Samira; Mauri, Francesco; Sorella, Sandro; Casula, Michele

    2015-06-01

    We study the ionization energy, electron affinity, and the π → π(∗) ((1)La) excitation energy of the anthracene molecule, by means of variational quantum Monte Carlo (QMC) methods based on a Jastrow correlated antisymmetrized geminal power (JAGP) wave function, developed on molecular orbitals (MOs). The MO-based JAGP ansatz allows one to rigorously treat electron transitions, such as the HOMO → LUMO one, which underlies the (1)La excited state. We present a QMC optimization scheme able to preserve the rank of the antisymmetrized geminal power matrix, thanks to a constrained minimization with projectors built upon symmetry selected MOs. We show that this approach leads to stable energy minimization and geometry relaxation of both ground and excited states, performed consistently within the correlated QMC framework. Geometry optimization of excited states is needed to make a reliable and direct comparison with experimental adiabatic excitation energies. This is particularly important in π-conjugated and polycyclic aromatic hydrocarbons, where there is a strong interplay between low-lying energy excitations and structural modifications, playing a functional role in many photochemical processes. Anthracene is an ideal benchmark to test these effects. Its geometry relaxation energies upon electron excitation are of up to 0.3 eV in the neutral (1)La excited state, while they are of the order of 0.1 eV in electron addition and removal processes. Significant modifications of the ground state bond length alternation are revealed in the QMC excited state geometry optimizations. Our QMC study yields benchmark results for both geometries and energies, with values below chemical accuracy if compared to experiments, once zero point energy effects are taken into account. PMID:26049481

  7. Electron-impact excitation of diatomic hydride cations - I. HeH+, CH+, ArH+

    NASA Astrophysics Data System (ADS)

    Hamilton, James R.; Faure, Alexandre; Tennyson, Jonathan

    2016-01-01

    R-matrix calculations combined with the adiabatic nuclei approximation are used to compute electron-impact rotational excitation rates for three closed-shell diatomic cations, HeH+, CH+, ArH+. Comparisons with previous studies show that an improved treatment of threshold effects leads to significant changes in the low temperature rates; furthermore the new calculations suggest that excitation of CH+ is dominated by ΔJ = 1 transitions as is expected for cations with a large dipole moment. A model for ArH+ excitation in the Crab nebula is presented which gives results consistent with the observations for electron densities in the range 2-3 × 103 cm-3.

  8. Excitation of Plasma Waves in Aurora by Electron Beams

    NASA Technical Reports Server (NTRS)

    daSilva, C. E.; Vinas, A. F.; deAssis, A. S.; deAzevedo, C. A.

    1996-01-01

    In this paper, we study numerically the excitation of plasma waves by electron beams, in the auroral region above 2000 km of altitude. We have solved the fully kinetic dispersion relation, using numerical method and found the real frequency and the growth rate of the plasma wave modes. We have examined the instability properties of low-frequency waves such as the Electromagnetic Ion Cyclotron (EMIC) wave as well as Lower-Hybrid (LH) wave in the range of high-frequency. In all cases, the source of free energy are electron beams propagating parallel to the geomagnetic field. We present some features of the growth rate modes, when the cold plasma parameters are changed, such as background electrons and ions species (H(+) and O(+)) temperature, density or the electron beam density and/or drift velocity. These results can be used in a test-particle simulation code, to investigate the ion acceleration and their implication in the auroral acceleration processes, by wave-particle interaction.

  9. Benzonitrile: Electron affinity, excited states, and anion solvation

    NASA Astrophysics Data System (ADS)

    Dixon, Andrew R.; Khuseynov, Dmitry; Sanov, Andrei

    2015-10-01

    We report a negative-ion photoelectron imaging study of benzonitrile and several of its hydrated, oxygenated, and homo-molecularly solvated cluster anions. The photodetachment from the unsolvated benzonitrile anion to the X ˜ 1 A 1 state of the neutral peaks at 58 ± 5 meV. This value is assigned as the vertical detachment energy (VDE) of the valence anion and the upper bound of adiabatic electron affinity (EA) of benzonitrile. The EA of the lowest excited electronic state of benzonitrile, a ˜ 3 A 1 , is determined as 3.41 ± 0.01 eV, corresponding to a 3.35 eV lower bound for the singlet-triplet splitting. The next excited state, the open-shell singlet A ˜ 1 A 1 , is found about an electron-volt above the triplet, with a VDE of 4.45 ± 0.01 eV. These results are in good agreement with ab initio calculations for neutral benzonitrile and its valence anion but do not preclude the existence of a dipole-bound state of similar energy and geometry. The step-wise and cumulative solvation energies of benzonitrile anions by several types of species were determined, including homo-molecular solvation by benzonitrile, hydration by 1-3 waters, oxygenation by 1-3 oxygen molecules, and mixed solvation by various combinations of O2, H2O, and benzonitrile. The plausible structures of the dimer anion of benzonitrile were examined using density functional theory and compared to the experimental observations. It is predicted that the dimer anion favors a stacked geometry capitalizing on the π-π interactions between the two partially charged benzonitrile moieties.

  10. Electron doping evolution of the magnetic excitations in NaFe1 -xCoxAs

    NASA Astrophysics Data System (ADS)

    Carr, Scott V.; Zhang, Chenglin; Song, Yu; Tan, Guotai; Li, Yu; Abernathy, D. L.; Stone, M. B.; Granroth, G. E.; Perring, T. G.; Dai, Pengcheng

    2016-06-01

    We use time-of-flight (TOF) inelastic-neutron-scattering (INS) spectroscopy to investigate the doping dependence of magnetic excitations across the phase diagram of NaFe1 -xCoxAs with x =0 , 0.0175, 0.0215, 0.05, and 0.11 . The effect of electron doping by partially substituting Fe by Co is to form resonances that couple with superconductivity, broaden, and suppress low-energy (E ≤80 meV) spin excitations compared with spin waves in undoped NaFeAs. However, high-energy (E >80 meV) spin excitations are weakly Co-doping-dependent. Integration of the local spin dynamic susceptibility χ''(ω ) of NaFe1 -xCoxAs reveals a total fluctuating moment of 3.6 μB2/Fe and a small but systematic reduction with electron doping. The presence of a large spin gap in Co-overdoped nonsuperconducting NaFe0.89Co0.11As suggests that Fermi surface nesting is responsible for low-energy spin excitations. These results parallel the Ni-doping evolution of spin excitations in BaFe2 -xNixAs2 in spite of the differences in crystal structures and Fermi surface evolution in these two families of iron pnictides, thus confirming the notion that low-energy spin excitations coupling with itinerant electrons are important for superconductivity, while weakly doping-dependent high-energy spin excitations result from localized moments.

  11. Resonance enhanced electron impact excitation for P-like Cu XV

    NASA Astrophysics Data System (ADS)

    Li, Shuang; Yan, Jun; Li, Chuan-Ying; Huang, Min; Chen, Chong-Yang

    2015-11-01

    Employing both the Dirac R-matrix and the relativistic distorted wave with independent process and isolated resonance approaches, we report resonance enhanced electron impact excitation data (specifically, effective collision strengths) among the lowest 41 levels from the n = 3 configurations of Cu XV. The results show that the latter approach can obtain resonance contributions reasonably well for most excitations of Cu XV, though a comparison between the two approaches shows that the close-coupling effects are truly significant for rather weak excitations, especially for two-electron excitations from the 3s3p4 to 3s23p23d configuration. Resonance contributions are significant (more than two orders of magnitude) for many excitations and dramatically influence the line intensity ratios associated with density diagnostics. Project supported by the National Natural Science Foundation of China (Grant Nos. 11076009 and 11374062), the Chinese Association of Atomic and Molecular Data, the Chinese National Fusion Project for ITER (Grant No. 2015GB117000), and the Leading Academic Discipline Project of Shanghai, China (Grant No. B107).

  12. Properties of Auger electrons following excitation of polarized atoms by polarized electrons

    NASA Astrophysics Data System (ADS)

    Kupliauskienė, A.; Tutlys, V.

    2009-01-01

    In non-relativistic approximation, the most general expression for differential cross sections describing the properties of Auger-electron emission induced in the excitation of polarized atoms by polarized electrons is obtained for the first time. The ways of the application of the general expressions suitable for the specific experimental conditions are outlined by deriving the expressions for the asymmetry parameters and the magnetic dichroism of the angular distribution of the Auger electrons as well as of the angular correlations between the scattered and Auger electrons.

  13. Perturbation method to calculate the interaction potentials and electronic excitation spectra of atoms in He nanodroplets.

    PubMed

    Callegari, Carlo; Ancilotto, Francesco

    2011-06-30

    A method is proposed for the calculation of potential energy curves and related electronic excitation spectra of dopant atoms captured in/on He nanodroplets and is applied to alkali metal atoms. The method requires knowledge of the droplet density distribution at equilibrium (here calculated within a bosonic-He density functional approach) and of a set of valence electron orbitals of the bare dopant atom (here calculated by numeric solution of the Schrödinger equation in a suitably parametrized model potential). The electron-helium interaction is added as a perturbation, and potential energy curves are obtained by numeric diagonalization of the resulting Hamiltonian as a function of an effective coordinate z(A) (here the distance between the dopant atom and center of mass of the droplet, resulting in a pseudodiatomic potential). Excitation spectra are calculated for Na in the companion paper as the Franck-Condon factors between the v = 0 vibrational state in the ground electronic state and excited states of the pseudodiatomic molecule. They agree well with available experimental data, even for highly excited states where a more traditional approach fails. PMID:21434657

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

    PubMed

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

    2015-05-21

    We report on measurements of integral cross sections (ICSs) for electron impact excitation of a series of composite vibrational modes and electronic-states in phenol, where the energy range of those experiments was 15-250 eV. There are currently no other results against which we can directly compare those measured data. We also report results from our independent atom model with screened additivity rule correction computations, namely, for the inelastic ICS (all discrete electronic states and neutral dissociation) and the total ionisation ICS. In addition, for the relevant dipole-allowed excited electronic states, we also report f-scaled Born-level and energy-corrected and f-scaled Born-level (BEf-scaled) ICS. Where possible, our measured and calculated ICSs are compared against one another with the general level of accord between them being satisfactory to within the measurement uncertainties. PMID:26001459

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

    SciTech Connect

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

    2015-05-21

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

  16. General active space commutator-based coupled cluster theory of general excitation rank for electronically excited states: Implementation and application to ScH

    NASA Astrophysics Data System (ADS)

    Hubert, Mickaël; Olsen, Jeppe; Loras, Jessica; Fleig, Timo

    2013-11-01

    We present a new implementation of general excitation rank coupled cluster theory for electronically excited states based on the single-reference multi-reference formalism. The method may include active-space selected and/or general higher excitations by means of the general active space concept. It may employ molecular integrals over the four-component Lévy-Leblond Hamiltonian or the relativistic spin-orbit-free four-component Hamiltonian of Dyall. In an initial application to ground- and excited states of the scandium monohydride molecule we report spectroscopic constants using basis sets of up to quadruple-zeta quality and up to full iterative triple excitations in the cluster operators. Effects due to spin-orbit interaction are evaluated using two-component multi-reference configuration interaction for assessing the accuracy of the coupled cluster results.

  17. General active space commutator-based coupled cluster theory of general excitation rank for electronically excited states: Implementation and application to ScH

    SciTech Connect

    Hubert, Mickaël; Loras, Jessica; Fleig, Timo; Olsen, Jeppe

    2013-11-21

    We present a new implementation of general excitation rank coupled cluster theory for electronically excited states based on the single-reference multi-reference formalism. The method may include active-space selected and/or general higher excitations by means of the general active space concept. It may employ molecular integrals over the four-component Lévy-Leblond Hamiltonian or the relativistic spin-orbit-free four-component Hamiltonian of Dyall. In an initial application to ground- and excited states of the scandium monohydride molecule we report spectroscopic constants using basis sets of up to quadruple-zeta quality and up to full iterative triple excitations in the cluster operators. Effects due to spin-orbit interaction are evaluated using two-component multi-reference configuration interaction for assessing the accuracy of the coupled cluster results.

  18. Ballistic effects and intersubband excitations in multiple quantum well structures

    NASA Astrophysics Data System (ADS)

    Schneider, H.; Schönbein, C.; Schwarz, K.; Walther, M.

    1998-07-01

    We have studied the transport properties of electrons in asymmetric quantum well structures upon far-infrared optical excitation of carriers from the lowest subband into the continuum. Here the photocurrent consists of a coherent component originating from ballistic transport upon excitation, and of an incoherent part associated with asymmetric diffusion and relaxation processes, which occur after the coherence has been lost. The signature of the coherent contribution is provided by a sign reversal of the photocurrent upon changing the excitation energy. This sign reversal arises from the energy-dependent interference between continuum states, which have a twofold degeneracy characterized by positive and negative momenta. The interference effect also allows us to estimate the coherent mean free path ( >20 nm at 77K). In specifically designed device structures, we use both the coherent and incoherent components in order to achieve a pronounced photovoltaic infrared response for detector applications.

  19. Electronic excitation of condensed CO: Sputtering and chemical change

    NASA Astrophysics Data System (ADS)

    Chrisey, D. B.; Brown, W. L.; Boring, J. W.

    1990-01-01

    We have bombarded condensed CO "ice" films with keV and MeV ions at low temperatures to investigate the physical sputtering mechanisms and chemical modifications of the ice. The sputtering yield measured for keV and MeV H + and He + ions indicates that the yield has a quadratic dependence on the electronic stopping power of the ions. Energy spectra of CO molecules sputtered by bombardment with 53 keV He + and 34 keV Ar + ions are very similar and show a collision-cascade-like behavior. We explore the origin of this quadratic dependence in terms of several models proposed for sputtering by electronic excitation and conclude that the quadratic dependence is intrinsic to the electronic relaxation process for CO. RBS measurements of the residue produced from sputtering various thicknesses of the initial CO film (˜ (3-25) × 10 17 CO/cm 2) indicate the production of the residue is approximately proportional to the initial thickness, accounts for ˜ 2% of the initial mass, and has a stoichiometric composition of approximately C 3O. The production and composition of the residue is discussed in terms of existing mechanisms for the radiolysis of gas phase CO.

  20. Effect of frequency on microplasmas driven by microwave excitation

    SciTech Connect

    Levko, Dmitry; Raja, Laxminarayan L.

    2015-07-28

    The effect of excitation frequency on the breakdown voltage of a microwave (mw) microdischarge and its steady-state plasma parameters is studied by the self-consistent one-dimensional Particle-in-Cell Monte Carlo collisions model. It is found that for microdischarges in which the electron wall losses are significant, an increase in the mw frequency results in a decrease in the breakdown voltage. For conditions in which the electron wall losses become negligible, an increase in the frequency does not influence significantly the breakdown voltage. At the same time, for both regimes, the increase in the frequency results in an increase in the steady-state plasma density. The analysis of the steady-state plasma parameters have shown that the dominant electron heating mechanism is the Joule heating while the stochastic heating is negligible. Also, it is found that the electron energy distribution function consists of two electron groups, namely, slow and fast electrons. The presence of fast electrons in the plasma bulk indicates the non-local nature of microwave excited microdischarges.

  1. Nuclear Excitation by Electronic Transition of U-235

    NASA Astrophysics Data System (ADS)

    Chodash, Perry Adam

    Nuclear excitation by electronic transition (NEET) is a rare nuclear excitation that is theorized to occur in numerous isotopes. One isotope in particular, U-235, has been studied several times over the past 40 years and NEET of U-235 has never been conclusively observed. These past experiments generated conflicting results with some experiments claiming to observe NEET of U-235 and others setting limits for the NEET rate. This dissertation discusses the latest attempt to measure NEET of U-235. If NEET of U-235 were to occur, U-235m would be created. U-235m decays by internal conversion with a decay energy of 76 eV and a half-life of 26 minutes. A pulsed Nd:YAG laser operating at 1064 nm with a pulse energy of 789 mJ and a pulse width of 9 ns was used to generate a uranium plasma. The plasma was captured on a catcher plate and electrons emitted from the catcher plate were accelerated and focused onto a microchannel plate detector. A decay of 26 minutes would suggest the creation of U-235m and the possibility that NEET occurred. However, measurements performed using a variety of uranium targets spanning depleted uranium up to 99.4% enriched uranium did not observe a 26 minute decay. Numerous other decays were observed with half-lives ranging from minutes up to hundreds of minutes. While NEET of U-235 was not observed during this experiment, an upper limit for the NEET rate of U-235 was determined. In addition, explanations for the conflicting results from previous experiments are given. Based on the results of this experiment and the previous experiments looking for NEET of U-235, it is likely that NEET of U-235 has never been observed.

  2. Electronic excitation of ground state atoms by collision with heavy gas particles

    NASA Technical Reports Server (NTRS)

    Hansen, C. Frederick

    1993-01-01

    Most of the important chemical reactions which occur in the very high temperature air produced around space vehicles as they enter the atmosphere were investigated both experimentally and theoretically, to some extent at least. One remaining reaction about which little is known, and which could be quite important at the extremely high temperatures that will be produced by the class of space vehicles now contemplated - such as the AOTV - is the excitation of bound electron states due to collisions between heavy gas particles. Rates of electronic excitation due to free electron collisions are known to be very rapid, but because these collisions quickly equilibrate the free and bound electron energy, the approach to full equilibrium with the heavy particle kinetic energy will depend primarily on the much slower process of bound electron excitation in heavy particle collisions and the subsequent rapid transfer to free electron energy. This may be the dominant mechanism leading to full equilibrium in the gas once the dissociation process has depleted the molecular states so the transfer between molecular vibrational energy and free electron energy is no longer available as a channel for equilibration of free electron and heavy particle kinetic energies. Two mechanisms seem probable in electronic excitation by heavy particle impact. One of these is the collision excitation and deexcitation of higher electronic states which are Rydberg like. A report, entitled 'Semi-Classical Theory of Electronic Excitation Rates', was submitted previously. This presented analytic expressions for the transition probabilities, assuming that the interaction potential is an exponential repulsion with a perturbation ripple due to the dipole-induced dipole effect in the case of neutral-neutral collisions, and to the ion-dipole interaction in the case of ion-neutral collisions. However the above may be, there is little doubt that excitation of ground state species by collision occurs at the

  3. Fluorescence polarization of helium negative-ion resonances excited by polarized electron impact

    NASA Astrophysics Data System (ADS)

    Maseberg, J. W.; Gay, T. J.

    2006-12-01

    We have investigated helium (1s3d) 3D → (1s2p) 3P (588 nm) fluorescence produced by electron impact excitation in the vicinity of the (2s22p) 2P and (2s2p2) 2D negative-ion resonances at 57.2 and 58.3 eV, respectively. In contrast to previous work, we use spin-polarized incident electrons and report the relative Stokes parameters P1, P2 and P3 in the 55-60 eV region. Our failure to see discernable resonance effects in P2 indicates that even though the lifetime of these resonances is significant (~10 fs), magnetic forces acting on the temporarily captured electron are small. Resonant structures in the values of P1 and P3 are observed because the polarization contributions of resonant states are generally different than those from direct excitation of the 3 3D state.

  4. Cross Sections for Electron Impact Excitation of Astrophysically Abundant Atoms and Ions

    NASA Technical Reports Server (NTRS)

    Tayal, S. S.

    2006-01-01

    Electron collisional excitation rates and transition probabilities are important for computing electron temperatures and densities, ionization equilibria, and for deriving elemental abundances from emission lines formed in the collisional and photoionized astrophysical plasmas. Accurate representation of target wave functions that properly account for the important correlation and relaxation effects and inclusion of coupling effects including coupling to the continuum are essential components of a reliable collision calculation. Non-orthogonal orbitals technique in multiconfiguration Hartree-Fock approach is used to calculate oscillator strengths and transition probabilities. The effect of coupling to the continuum spectrum is included through the use of pseudostates which are chosen to account for most of the dipole polarizabilities of target states. The B-spline basis is used in the R-matrix approach to calculate electron excitation collision strengths and rates. Results for oscillator strengths and electron excitation collision strengths for transitions in N I, O I, O II, O IV, S X and Fe XIV have been produced

  5. Investigation of Multiconfigurational Short-Range Density Functional Theory for Electronic Excitations in Organic Molecules.

    PubMed

    Hubert, Mickaël; Hedegård, Erik D; Jensen, Hans Jørgen Aa

    2016-05-10

    Computational methods that can accurately and effectively predict all types of electronic excitations for any molecular system are missing in the toolbox of the computational chemist. Although various Kohn-Sham density-functional methods (KS-DFT) fulfill this aim in some cases, they become inadequate when the molecule has near-degeneracies and/or low-lying double-excited states. To address these issues we have recently proposed multiconfiguration short-range density-functional theory-MC-srDFT-as a new tool in the toolbox. While initial applications for systems with multireference character and double excitations have been promising, it is nevertheless important that the accuracy of MC-srDFT is at least comparable to the best KS-DFT methods also for organic molecules that are typically of single-reference character. In this paper we therefore systematically investigate the performance of MC-srDFT for a selected benchmark set of electronic excitations of organic molecules, covering the most common types of organic chromophores. This investigation confirms the expectation that the MC-srDFT method is accurate for a broad range of excitations and comparable to accurate wave function methods such as CASPT2, NEVPT2, and the coupled cluster based CC2 and CC3. PMID:27058733

  6. Photoelectron Spectroscopy of Hexachloroplatinate-Nucleobase Complexes: Nucleobase Excited State Decay Observed via Delayed Electron Emission

    SciTech Connect

    Sen, Ananya; Matthews, Edward M.; Hou, Gao-Lei; Wang, Xue B.; Dessent, Caroline

    2015-11-14

    We report low-temperature photoelectron spectra of isolated gas-phase complexes of the hexachloroplatinate dianion bound to the nucleobases uracil, thymine, cytosine and adenine. The spectra display well-resolved, distinct peaks that are consistent with complexes where the hexachloroplatinate dianion is largely intact. Adiabatic electron detachment energies for the hexachloroplatinate-nucleobase complexes are measured as 2.26-2.36 eV. The magnitudes of the repulsive Coulomb barriers (RCBs) of the complexes are all ~1.7 eV, values that are lower than the RCB of the uncomplexed PtCl6 2- dianion as a result of charge solvation by the nucleobases. In addition to the resolved spectral features, broad featureless bands indicative of delayed electron detachment are observed in the 193 nm photoelectron spectra of the four clusters. The 266 nm spectra of the PtCl6 2-∙thymine and PtCl6 2-∙adenine complexes also display very prominent delayed electron emission bands. These results mirror recent results on the related Pt(CN)4 2-∙nucleobase complexes [Sen et al, J. Phys. Chem. B, 119, 11626, 2015]. The observation of delayed electron emission bands in the PtCl6 2-∙nucleobase spectra obtained in this work, as for the previously studied Pt(CN)4 2-∙nucleobase complexes, is attributed to onephoton excitation of nucleobase-centred excited states that can effectively couple to the electron detachment continuum, producing strong electron detachment. Moreover, the selective, strong excitation of the delayed emission bands in the 266 nm spectra is linked to fundamental differences in the individual nucleobase photophysics at this excitation energy. This strongly supports our previous suggestion that the dianion within these clusters can be viewed as a “dynamic tag” which has the propensity to emit electrons when the attached nucleobase decays over a timescale long enough to allow autodetachment.

  7. Application of DSMC Electronic Excitation Modeling to Radiation Calculation of Hypersonic Reentry Flows

    NASA Astrophysics Data System (ADS)

    Li, Zheng; Sohn, Ilyoup; Levin, Deborah A.; Modest, Michael F.

    2011-05-01

    The current work implemented excited levels of atomic N and corresponding electron impact excitation/de-excitation and ionization processes in DSMC. Results show that when excitation models are included, the Stardust 68.9 km re-entry flow has an observable change in the ion number densities and electron temperature. Adding in the excited levels of atoms improves the degree of ionization by providing additional intermediate steps to ionization. The extra ionization reactions consume the electron energy and reduce the electron temperature. The DSMC results of number densities of excited levels are lower than the prediction of quasi steady state calculation. Comparison of radiation calculations using electronic excited populations from DSMC and QSS indicates that, at the stagnation point, there is about 20% difference of the radiative heat flux between DSMC and QSS.

  8. Ensemble density functional theory method correctly describes bond dissociation, excited state electron transfer, and double excitations

    SciTech Connect

    Filatov, Michael; Huix-Rotllant, Miquel; Burghardt, Irene

    2015-05-14

    State-averaged (SA) variants of the spin-restricted ensemble-referenced Kohn-Sham (REKS) method, SA-REKS and state-interaction (SI)-SA-REKS, implement ensemble density functional theory for variationally obtaining excitation energies of molecular systems. In this work, the currently existing version of the SA-REKS method, which included only one excited state into the ensemble averaging, is extended by adding more excited states to the averaged energy functional. A general strategy for extension of the REKS-type methods to larger ensembles of ground and excited states is outlined and implemented in extended versions of the SA-REKS and SI-SA-REKS methods. The newly developed methods are tested in the calculation of several excited states of ground-state multi-reference systems, such as dissociating hydrogen molecule, and excited states of donor–acceptor molecular systems. For hydrogen molecule, the new method correctly reproduces the distance dependence of the lowest excited state energies and describes an avoided crossing between the doubly excited and singly excited states. For bithiophene–perylenediimide stacked complex, the SI-SA-REKS method correctly describes crossing between the locally excited state and the charge transfer excited state and yields vertical excitation energies in good agreement with the ab initio wavefunction methods.

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

    NASA Technical Reports Server (NTRS)

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

    1977-01-01

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

  10. TlII excitation cross-sections in collisions of slow electrons with thallium atoms

    NASA Astrophysics Data System (ADS)

    Smirnov, Yu M.

    2016-09-01

    Excitation of a singly-charged thallium ion in electron collisions with thallium atoms has been studied experimentally. Seventy excitation cross sections have been measured at an exciting electron energy of 30 eV. Ten optical excitation functions (OEFs) have been recorded in the incident electron energy range of 0–200 eV. For seven TlII spectral series, the dependence of excitation cross-sections on the principal quantum numbers of upper levels has been studied. A comparison of findings with data from preceding publications is presented.

  11. Double electron excitation in He ions interacting with an aluminum surface

    NASA Astrophysics Data System (ADS)

    Riccardi, P.; Sindona, A.; Dukes, C. A.

    2016-04-01

    Observation of Auger electron emission from Al under the impact of He ions, at energies below the excitation threshold of Al-Al collisions, gives evidence for charge transfer in He-Al collisions. Excitation of 2 p -shell electrons in Al is produced by vacancy transfer, following double excitation of He by promotion of its 1 s level. Studies of ion scattering from surfaces currently neglect the double excitation of He. We discuss implications on the debate about electronic excitations and energy deposition, which is relevant to many fields, since helium ions are applied in the characterization and imaging of materials.

  12. Dissociative excitation of NO2 by electron impact

    NASA Astrophysics Data System (ADS)

    Young, J. A.; Malone, C. P.; Johnson, P. V.; Liu, X.; Ajello, J. M.; Kanik, I.

    2009-09-01

    Electron-impact-induced vacuum ultraviolet emissions are measured for NO2, a species important to discharge phenomena and ozone decomposition in the Earth's atmosphere. A calibrated spectrum for 100 eV incident electrons is presented, along with cross sections for strong emission features between 80 and 160 nm. The dominant N i (2p3 4S°-3s 4P) emission at 120.1 nm is compared with that of N2 and used to provide an absolute calibration for all measured cross sections. In addition, 10-300 eV excitation functions for the N i (120.1 nm) and O i (130.4 nm) emissions are presented and interpreted. Comparisons are made with similar measurements of related species, in particular N2O and NO. Of interest, it was found that, on average, the variation in the intensity of oxygen and nitrogen emissions could be reasonably explained by the difference in the number of constituent oxygen and nitrogen atoms in each target.

  13. Ultrafast electron injection into photo-excited organic molecules.

    PubMed

    Cvetko, Dean; Fratesi, Guido; Kladnik, Gregor; Cossaro, Albano; Brivio, Gian Paolo; Venkataraman, Latha; Morgante, Alberto

    2016-08-10

    Charge transfer rates at metal/organic interfaces affect the efficiencies of devices for organic based electronics and photovoltaics. A quantitative study of electron transfer rates, which take place on the femtosecond timescale, is often difficult, especially since in most systems the molecular adsorption geometry is unknown. Here, we use X-ray resonant photoemission spectroscopy to measure ultrafast charge transfer rates across pyridine/Au(111) interfaces while also controlling the molecular orientation on the metal. We demonstrate that a bi-directional charge transfer across the molecule/metal interface is enabled upon creation of a core-exciton on the molecule with a rate that has a strong dependence on the molecular adsorption angle. Through density functional theory calculations, we show that the alignment of molecular levels relative to the metal Fermi level is dramatically altered when a core-hole is created on the molecule, allowing the lowest unoccupied molecular orbital to fall partially below the metal Fermi level. We also calculate charge transfer rates as a function of molecular adsorption geometry and find a trend that agrees with the experiment. These findings thus give insight into the charge transfer dynamics of a photo-excited molecule on a metal surface. PMID:27444572

  14. Electron impact excitation collision strengths for extreme ultraviolet lines of Fe VII

    SciTech Connect

    Tayal, S. S.; Zatsarinny, O. E-mail: oleg.zatsarinny@drake.edu

    2014-06-10

    Extensive calculations have been performed for electron impact excitation collision strengths and oscillator strengths for the Fe VII extreme ultraviolet lines of astrophysical importance. The collision strengths for fine-structure transitions are calculated in the B-spline Breit-Pauli R-matrix approach. The target wavefunctions have been calculated in the multiconfiguration Hartree-Fock method with term-dependent non-orthogonal orbitals. The close-coupling expansion includes 189 fine-structure levels of Fe VII belonging to terms of the ground 3p {sup 6}3d {sup 2} and excited 3p {sup 5}3d {sup 3}, 3p {sup 6}3d4l, 3p {sup 6}3d5s, and 3p {sup 6}3d5p configurations. The effective collision strengths are determined from the electron excitation collision strengths by integration over a Maxwellian distribution of electron velocities. The effective collision strengths are provided for 17766 fine-structure transitions at electron temperatures from 10{sup 4} to 10{sup 7} K. Our results normally agree with the previous R-matrix frame-transformation calculations by Witthoeft and Badnell. However, there are important differences for some transitions with the previous calculations. The corrections to the previous results are mainly due to more extensive expansions for the Fe VII target states.

  15. 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.

  16. Energy shift of collective electron excitations in highly corrugated graphitic nanostructures: Experimental and theoretical investigation

    NASA Astrophysics Data System (ADS)

    Sedelnikova, O. V.; Bulusheva, L. G.; Asanov, I. P.; Yushina, I. V.; Okotrub, A. V.

    2014-04-01

    Effect of corrugation of hexagonal carbon network on the collective electron excitations has been studied using optical absorption and X-ray photoelectron spectroscopy in conjunction with density functional theory calculations. Onion-like carbon (OLC) was taken as a material, where graphitic mantle enveloping agglomerates of multi-shell fullerenes is strongly curved. Experiments showed that positions of π and π + σ plasmon modes as well as π → π* absorption peak are substantially redshifted for OLC as compared with those of highly ordered pyrolytic graphite and thermally exfoliated graphite consisted of planar sheets. This effect was reproduced in behavior of dielectric functions of rippled graphite models calculated within the random phase approximation. We conclude that the energy of electron excitations in graphitic materials could be precisely tuned by a simple bending of hexagonal network without change of topology. Moreover, our investigation suggests that in such materials optical exciton can transfer energy to plasmon non-radiatively.

  17. Energy shift of collective electron excitations in highly corrugated graphitic nanostructures: Experimental and theoretical investigation

    SciTech Connect

    Sedelnikova, O. V. Bulusheva, L. G.; Okotrub, A. V.; Asanov, I. P.; Yushina, I. V.

    2014-04-21

    Effect of corrugation of hexagonal carbon network on the collective electron excitations has been studied using optical absorption and X-ray photoelectron spectroscopy in conjunction with density functional theory calculations. Onion-like carbon (OLC) was taken as a material, where graphitic mantle enveloping agglomerates of multi-shell fullerenes is strongly curved. Experiments showed that positions of π and π + σ plasmon modes as well as π → π* absorption peak are substantially redshifted for OLC as compared with those of highly ordered pyrolytic graphite and thermally exfoliated graphite consisted of planar sheets. This effect was reproduced in behavior of dielectric functions of rippled graphite models calculated within the random phase approximation. We conclude that the energy of electron excitations in graphitic materials could be precisely tuned by a simple bending of hexagonal network without change of topology. Moreover, our investigation suggests that in such materials optical exciton can transfer energy to plasmon non-radiatively.

  18. Adsorbate-induced absorption redshift in an organic-inorganic cluster conjugate: Electronic effects of surfactants and organic adsorbates on the lowest excited states of a methanethiol-CdSe conjugate

    NASA Astrophysics Data System (ADS)

    Liu, Christopher; Chung, Sang-Yoon; Lee, Sungyul; Weiss, Shimon; Neuhauser, Daniel

    2009-11-01

    Bioconjugated CdSe quantum dots are promising reagents for bioimaging applications. Experimentally, the binding of a short peptide has been found to redshift the optical absorption of nanoclusters [J. Tsay et al., J. Phys. Chem. B 109, 1669 (2005)]. This study examines this issue by performing density functional theory (DFT) and time-dependent-DFT calculations to study the ground state and low-lying excited states of (CdSe)6[SCH3]-, a transition metal complex built by binding methanethiolate to a CdSe molecular cluster. Natural bond orbital results show that the redshift is caused by ligand-inorganic cluster orbital interaction. The highest occupied molecular orbital (HOMO) of (CdSe)6 is dominated by selenium 4p orbitals; in contrast, the HOMO of (CdSe)6[SCH3]- is dominated by sulfur 3p orbitals. This difference shows that [SCH3]- binding effectively introduces filled sulfur orbitals above the selenium 4p orbitals of (CdSe)6. The resulting smaller HOMO-LUMO gap of (CdSe)6[SCH3]- indeed leads to redshifts in its excitation energies compared to (CdSe)6. In contrast, binding of multiple NH3 destabilizes cadmium 5p orbitals, which contribute significantly to the lowest unoccupied molecular orbital (LUMO) of (CdSe)6, while leaving the selenium 4p orbitals near the HOMO relatively unaffected. This has the effect of widening the HOMO-LUMO gap of (CdSe)6ṡ6NH3 compared to (CdSe)6. As expected, the excitation energies of the passivated (CdSe)6ṡ6NH3 are also blueshifted compared to (CdSe)6. As far as NH3 is a faithful representation of a surfactant, the results clearly illustrate the differences between the electronic effects of an alkylthiolate versus those of surfactant molecules. Surface passivation of (CdSe)6[SCH3]- is then simulated by coating it with multiple NH3 molecules. The results suggest that the [SCH3]- adsorption induces a redshift in the excitation energies in a surfactant environment.

  19. Excitation of plasmons in Ag/Fe/W structure by spin-polarized electrons

    SciTech Connect

    Samarin, Sergey N.; Kostylev, Mikhail; Williams, J. F.; Artamonov, Oleg M.; Baraban, Alexander P.; Guagliardo, Paul

    2015-09-07

    Using Spin-polarized Electron-Energy Loss Spectroscopy (SPEELS), the plasmon excitations were probed in a few atomic layers thick Ag film deposited on an Fe layer or on a single crystal of W(110). The measurements were performed at two specular geometries with either a 25° or 72° angle of incidence. On a clean Fe layer (10 atomic layers thick), Stoner excitation asymmetry was observed, as expected. Deposition of a silver film on top of the Fe layer dramatically changed the asymmetry of the SPEELS spectra. The spin-effect depends on the kinematics of the scattering: angles of incidence and detection. The spin-dependence of the plasmon excitations in the silver film on the W(110) surface and on the ferromagnetic Fe film is suggested to arise from the spin-active Ag/W or Ag/Fe interfaces.

  20. Calculation of the lowest electronic excitations of the alkaline earth metals using the relativistic polarization propagator

    NASA Astrophysics Data System (ADS)

    Brandt, Sven; Pernpointner, Markus

    2015-07-01

    In this work we use the recently implemented four-component polarization propagator for accurate single excitation calculations of alkaline earth metals and compare our results to experimental data. Various approximations to the Dirac-Coulomb Hamiltonian are additionally tested. In Ca spin-orbit coupling already leads to noticeable zero field splitting, which gradually increases for the heavier homologs finally invalidating the singlet and triplet state characterizations. For all systems we observe a very good agreement with experimental transition energies in the considered energy range. For Sr, Ba and Ra non-relativistic approaches already exhibit unacceptable deviations in the reproduction of transition energies and spectral structure. The obtained excited final states are analyzed in terms of atomic donor and acceptor orbital contributions. Our results stress the necessity to use relativistic implementations of the polarization propagator for an accurate description of both electron correlation and relativistic effects contributing to excitation spectra of heavy systems.

  1. Electronic excitation and quenching of atoms at insulator surfaces

    NASA Technical Reports Server (NTRS)

    Swaminathan, P. K.; Garrett, Bruce C.; Murthy, C. S.

    1988-01-01

    A trajectory-based semiclassical method is used to study electronically inelastic collisions of gas atoms with insulator surfaces. The method provides for quantum-mechanical treatment of the internal electronic dynamics of a localized region involving the gas/surface collision, and a classical treatment of all the nuclear degrees of freedom (self-consistently and in terms of stochastic trajectories), and includes accurate simulation of the bath-temperature effects. The method is easy to implement and has a generality that holds promise for many practical applications. The problem of electronically inelastic dynamics is solved by computing a set of stochastic trajectories that on thermal averaging directly provide electronic transition probabilities at a given temperature. The theory is illustrated by a simple model of a two-state gas/surface interaction.

  2. Electronic structure and excited state dynamics in optically excited PTCDA films investigated with two-photon photoemission.

    PubMed

    Marks, M; Sachs, S; Schwalb, C H; Schöll, A; Höfer, U

    2013-09-28

    We present an investigation of the electronic structure and excited state dynamics of optically excited 3,4,9,10-perylene-tetracarboxylic acid dianhydride (PTCDA) thin films adsorbed on Ag(111) using two-photon photoemission spectroscopy (2PPE). 2PPE allows us to study both occupied and unoccupied electronic states, and we are able to identify signals from the highest occupied and the two lowest unoccupied electronic states of the PTCDA thin film in the 2PPE spectra. The energies for occupied states are identical to values from ultraviolet photoelectron spectroscopy. Compared to results from inverse photoelectron spectroscopy (IPES), the 2PPE signals from the two lowest unoccupied electronic states, LUMO and LUMO+1, are found at 0.8 eV and 1.0 eV lower energies, respectively. We attribute this deviation to the different final states probed in 2PPE and IPES and the attractive interaction of the photoexcited electron and the remaining hole. Furthermore, we present a time-resolved investigation of the excited state dynamics of the PTCDA film in the femtosecond time regime. We observe a significantly shorter inelastic excited state lifetime compared to findings from time-resolved photoluminescence spectroscopy of PTCDA single crystals which could originate from excitation quenching by the metal substrate. PMID:24089789

  3. Electronic structure and excited state dynamics in optically excited PTCDA films investigated with two-photon photoemission

    NASA Astrophysics Data System (ADS)

    Marks, M.; Sachs, S.; Schwalb, C. H.; Schöll, A.; Höfer, U.

    2013-09-01

    We present an investigation of the electronic structure and excited state dynamics of optically excited 3,4,9,10-perylene-tetracarboxylic acid dianhydride (PTCDA) thin films adsorbed on Ag(111) using two-photon photoemission spectroscopy (2PPE). 2PPE allows us to study both occupied and unoccupied electronic states, and we are able to identify signals from the highest occupied and the two lowest unoccupied electronic states of the PTCDA thin film in the 2PPE spectra. The energies for occupied states are identical to values from ultraviolet photoelectron spectroscopy. Compared to results from inverse photoelectron spectroscopy (IPES), the 2PPE signals from the two lowest unoccupied electronic states, LUMO and LUMO+1, are found at 0.8 eV and 1.0 eV lower energies, respectively. We attribute this deviation to the different final states probed in 2PPE and IPES and the attractive interaction of the photoexcited electron and the remaining hole. Furthermore, we present a time-resolved investigation of the excited state dynamics of the PTCDA film in the femtosecond time regime. We observe a significantly shorter inelastic excited state lifetime compared to findings from time-resolved photoluminescence spectroscopy of PTCDA single crystals which could originate from excitation quenching by the metal substrate.

  4. Coherence, Energy and Charge Transfers in De-Excitation Pathways of Electronic Excited State of Biomolecules in Photosynthesis

    NASA Astrophysics Data System (ADS)

    Bohr, Henrik G.; Malik, F. Bary

    2013-11-01

    The observed multiple de-excitation pathways of photo-absorbed electronic excited state in the peridinin-chlorophyll complex, involving both energy and charge transfers among its constituents, are analyzed using the bio-Auger (B-A) theory. It is also shown that the usually used Förster-Dexter theory, which does not allow for charge transfer, is a special case of B-A theory. The latter could, under appropriate circumstances, lead to excimers.

  5. Nuclear Excitation by Electronic Transition of U-235

    SciTech Connect

    Chodash, Perry Adam

    2015-07-14

    Nuclear excitation by electronic transition (NEET) is a rare nuclear excitation that is theorized to occur in numerous isotopes. One isotope in particular, 235U, has been studied several times over the past 40 years and NEET of 235U has never been conclusively observed. These past experiments generated con icting results with some experiments claiming to observe NEET of 235U and others setting limits for the NEET rate. This dissertation discusses the latest attempt to measure NEET of 235U. If NEET of 235U were to occur, 235mU would be created. 235mU decays by internal conversion with a decay energy of 76 eV and a half-life of 26 minutes. A pulsed Nd:YAG laser operating at 1064 nm with a pulse energy of 789 mJ and a pulse width of 9 ns was used to generate a uranium plasma. The plasma was captured on a catcher plate and electrons emitted from the catcher plate were accelerated and focused onto a microchannel plate detector. A decay of 26 minutes would suggest the creation of 235mU and the possibility that NEET occurred. However, measurements performed using a variety of uranium targets spanning depleted uranium up to 99.4% enriched uranium did not observe a 26 minute decay. Numerous other decays were observed with half-lives ranging from minutes up to hundreds of minutes. While NEET of 235U was not observed during this experiment, an upper limit for the NEET rate of 235U was determined. In addition, explanations for the con icting results from previous experiments are given. Based on the results of this experiment and the previous experiments looking for NEET of 235U, it is likely that NEET of 235U has never been observed.

  6. Excitation and ionization of highly charged ions by electron impact

    SciTech Connect

    Sampson, D.H.

    1989-11-15

    Two approaches for very rapid calculation of atomic data for high temperature plasma modeling have been developed. The first uses hydrogenic basis states and has been developed and applied in many papers discussed in previous progress reports. Hence, it is only briefly discussed here. The second is a very rapid, yet accurate, fully relativistic approach that has been developed over the past two or three years. It is described in more detail. Recently it has been applied to large scale production of atomic data. Specifically, it has been used to calculate relativistic distorted wave collision strengths and oscillator strengths for the following: all transitions from the ground level to the n=3 and 4 excited levels in the 71 Neon-like ions with nuclear charge number Z in the range 22 {le} Z {le} 92; all transitions among the 2s{sub {1/2}}, 2p{sub {1/2}} and 2p{sub 3/2} levels and from them to all nlj levels with n=3,4 and 5 in the 85 Li-like ions with 8 {le} Z {le} 92; all transitions among the 3s{sub {1/2}}, 3p{sub 3/2}, 3d{sub 3/2} and 3d{sub 5/2} levels and from them to all nlj levels with n=4 and 5 in the 71 Na-like ions with 22 {le} Z {le} 92; and all transitions among 4s{sub {1/2}}, 4p{sub {1/2}}, 4p{sub 3/2}, 4d{sub 3/2}, 4d{sub 5/2}, 4f{sub 5/2} and 4f{sub 7/2} levels and from them to all nlj levels with n=5 in the 33 Cu-like ions with 60 {le} Z {le} 92. Also the program has been extended to give cross-sections for excitation to specific magnetic sublevels of the target ion by an electron beam and very recently it has been extended to give relativistic distorted wave cross sections for ionization of highly charged ions by electron impact.

  7. A benchmark study of electronic excitation energies, transition moments, and excited-state energy gradients on the nicotine molecule

    NASA Astrophysics Data System (ADS)

    Egidi, Franco; Segado, Mireia; Koch, Henrik; Cappelli, Chiara; Barone, Vincenzo

    2014-12-01

    In this work, we report a comparative study of computed excitation energies, oscillator strengths, and excited-state energy gradients of (S)-nicotine, chosen as a test case, using multireference methods, coupled cluster singles and doubles, and methods based on time-dependent density functional theory. This system was chosen because its apparent simplicity hides a complex electronic structure, as several different types of valence excitations are possible, including n-π*, π-π*, and charge-transfer states, and in order to simulate its spectrum it is necessary to describe all of them consistently well by the chosen method.

  8. A benchmark study of electronic excitation energies, transition moments, and excited-state energy gradients on the nicotine molecule

    SciTech Connect

    Egidi, Franco Segado, Mireia; Barone, Vincenzo; Koch, Henrik; Cappelli, Chiara

    2014-12-14

    In this work, we report a comparative study of computed excitation energies, oscillator strengths, and excited-state energy gradients of (S)-nicotine, chosen as a test case, using multireference methods, coupled cluster singles and doubles, and methods based on time-dependent density functional theory. This system was chosen because its apparent simplicity hides a complex electronic structure, as several different types of valence excitations are possible, including n-π{sup *}, π-π{sup *}, and charge-transfer states, and in order to simulate its spectrum it is necessary to describe all of them consistently well by the chosen method.

  9. I. Concepts of Highly Excited Electronic Systems / II. Electronic Correlation Mapping from Finite to Extended Systems

    NASA Astrophysics Data System (ADS)

    Berakdar, Jamal

    2003-09-01

    Knowledge of the excitation characteristics of matter is decisive for the descriptions of a variety of dynamical processes, which are of significant technological interest. E.g. transport properties and the optical response are controlled by the excitation spectrum. This self-contained work is a coherent presentation of the quantum theory of correlated few-particle excitations in electronic systems. It begins with a compact resume of the quantum mechanics of single particle excitations. Particular emphasis is put on Green function methods, which offer a natural tool to unravel the relations between the physics of small and large electronic systems. The book contains explicit expressions for the Coulomb Green function of two charge particles and a generalization to three-body systems. Techniques for the many-body Green function of finite systems are introduced and some explicit calculations of the Green functions are given. Concrete examples are provided and the theories are contrasted with experimental data, when available. A complimentary volume presents an up-to-date selection of applications of the developed concepts and a comparison with available experiments is made

  10. I. Concepts of Highly Excited Electronic Systems / II. Electronic Correlation Mapping from Finite to Extended Systems

    NASA Astrophysics Data System (ADS)

    Berakdar, Jamal

    2006-02-01

    Knowledge of the excitation characteristics of matter is decisive for the descriptions of a variety of dynamical processes, which are of significant technological interest. E.g. transport properties and the optical response are controlled by the excitation spectrum. This self-contained work is a coherent presentation of the quantum theory of correlated few-particle excitations in electronic systems. It begins with a compact resume of the quantum mechanics of single particle excitations. Particular emphasis is put on Green function methods, which offer a natural tool to unravel the relations between the physics of small and large electronic systems. The book contains explicit expressions for the Coulomb Green function of two charge particles and a generalization to three-body systems. Techniques for the many-body Green function of finite systems are introduced and some explicit calculations of the Green functions are given. Concrete examples are provided and the theories are contrasted with experimental data, when available. A complimentary volume presents an up-to-date selection of applications of the developed concepts and a comparison with available experiments is made

  11. Theoretical and experimental differential cross sections for electron impact excitation of the electronic bands of furfural.

    PubMed

    Jones, D B; Neves, R F C; Lopes, M C A; da Costa, R F; do N Varella, M T; Bettega, M H F; Lima, M A P; García, G; Limão-Vieira, P; Brunger, M J

    2016-03-28

    We report results from a joint experimental and theoretical investigation into electron scattering from the important industrial species furfural (C5H4O2). Specifically, differential cross sections (DCSs) have been measured and calculated for the electron-impact excitation of the electronic states of C5H4O2. The measurements were carried out at energies in the range 20-40 eV, and for scattered-electron angles between 10° and 90°. The energy resolution of those experiments was typically ∼80 meV. Corresponding Schwinger multichannel method with pseudo-potential calculations, for energies between 6-50 eV and with and without Born-closure, were also performed for a sub-set of the excited electronic-states that were accessed in the measurements. Those calculations were undertaken at the static exchange plus polarisation-level using a minimum orbital basis for single configuration interaction (MOB-SCI) approach. Agreement between the measured and calculated DCSs was qualitatively quite good, although to obtain quantitative accord, the theory would need to incorporate even more channels into the MOB-SCI. The role of multichannel coupling on the computed electronic-state DCSs is also explored in some detail. PMID:27036450

  12. Theoretical and experimental differential cross sections for electron impact excitation of the electronic bands of furfural

    NASA Astrophysics Data System (ADS)

    Jones, D. B.; Neves, R. F. C.; Lopes, M. C. A.; da Costa, R. F.; do N. Varella, M. T.; Bettega, M. H. F.; Lima, M. A. P.; García, G.; Limão-Vieira, P.; Brunger, M. J.

    2016-03-01

    We report results from a joint experimental and theoretical investigation into electron scattering from the important industrial species furfural (C5H4O2). Specifically, differential cross sections (DCSs) have been measured and calculated for the electron-impact excitation of the electronic states of C5H4O2. The measurements were carried out at energies in the range 20-40 eV, and for scattered-electron angles between 10° and 90°. The energy resolution of those experiments was typically ˜80 meV. Corresponding Schwinger multichannel method with pseudo-potential calculations, for energies between 6-50 eV and with and without Born-closure, were also performed for a sub-set of the excited electronic-states that were accessed in the measurements. Those calculations were undertaken at the static exchange plus polarisation-level using a minimum orbital basis for single configuration interaction (MOB-SCI) approach. Agreement between the measured and calculated DCSs was qualitatively quite good, although to obtain quantitative accord, the theory would need to incorporate even more channels into the MOB-SCI. The role of multichannel coupling on the computed electronic-state DCSs is also explored in some detail.

  13. Detailed glycan structural characterization by electronic excitation dissociation.

    PubMed

    Yu, Xiang; Jiang, Yan; Chen, Yajie; Huang, Yiqun; Costello, Catherine E; Lin, Cheng

    2013-11-01

    The structural complexity and diversity of glycans parallel their multilateral functions in living systems. To better understand the vital roles glycans play in biological processes, it is imperative to develop analytical tools that can provide detailed glycan structural information. This was conventionally achieved by multistage tandem mass spectrometry (MS(n)) analysis using collision-induced dissociation (CID) as the fragmentation method. However, the MS(n) approach lacks the sensitivity and throughput needed to analyze complex glycan mixtures from biological sources, often available in limited quantities. We define herein the critical parameters for a recently developed fragmentation technique, electronic excitation dissociation (EED), which can yield rich structurally informative fragment ions during liquid chromatographic (LC)-MS/MS analysis of glycans. We further demonstrate that permethylation, reducing end labeling and judicious selection of the metal charge carrier, can greatly facilitate spectral interpretation. With its high sensitivity, throughput, and compatibility with online chromatographic separation techniques, EED appears to hold great promise for large-scale glycomics studies. PMID:24080071

  14. Differential cross sections for electron impact excitation of the electronic bands of phenol

    SciTech Connect

    Neves, R. F. C.; Jones, D. B.; Lopes, M. C. A.; Nixon, K. L.; Silva, G. B. da; Duque, H. V.; Oliveira, E. M. de; Lima, M. A. P.; Costa, R. F. da; Varella, M. T. do N.; Bettega, M. H. F.; and others

    2015-03-14

    We report results from a joint theoretical and experimental investigation into electron scattering from the important organic species phenol (C{sub 6}H{sub 5}OH). Specifically, differential cross sections (DCSs) have been measured and calculated for the electron-impact excitation of the electronic states of C{sub 6}H{sub 5}OH. The measurements were carried out at energies in the range 15–40 eV, and for scattered-electron angles between 10{sup ∘} and 90{sup ∘}. The energy resolution of those experiments was typically ∼80 meV. Corresponding Schwinger multichannel method with pseudo-potentials calculations, with and without Born-closure, were also performed for a sub-set of the excited electronic-states that were accessed in the measurements. Those calculations were conducted at the static exchange plus polarisation (SEP)-level using a minimum orbital basis for single configuration interaction (MOBSCI) approach. Agreement between the measured and calculated DCSs was typically fair, although to obtain quantitative accord, the theory would need to incorporate even more channels into the MOBSCI.

  15. Random strain effects in optical and EPR spectra of electron-nuclear excitations in CaWO4:Ho(3+) single crystals.

    PubMed

    Shakurov, G S; Chukalina, E P; Popova, M N; Malkin, B Z; Tkachuk, A M

    2014-12-01

    We study paramagnetic Ho(3+) centers in CaWO4, a promising material for applications in quantum electronics and quantum information devices. Oriented single crystals with nominal holmium concentrations 0.05, 0.5, and 1 at% were investigated at 4.2 K using EPR spectroscopy in the frequency range 37-850 GHz at temperatures 5-40 K and high-resolution optical transmission spectroscopy in the infrared and visible wave-length ranges. Along with the tetragonal Ho(3+) centers of the S4 point symmetry, four different types of low-symmetry centers were identified in the EPR spectra and their spectral parameters were determined. A well resolved hyperfine structure exhibiting holmium concentration dependent features was observed in optical spectra. Modeling of the spectra taking into account random lattice strains gave a possibility of reproducing satisfactorily the measured hyperfine structure of the EPR signals, in particular, at anticrossings of the electron-nuclear sublevels of the ground non-Kramers doublet, and the envelopes of the hyperfine structure of optical transitions. The widths of the probability distribution of random deformations related to the point lattice defects in the samples with different concentrations of the impurity Ho(3+) ions were estimated from a comparison of the simulated spectra with the experimental data. PMID:25315262

  16. Spectroscopic and dynamical differences between exciplex and electronically excited EDA complex

    NASA Astrophysics Data System (ADS)

    Lim, B. T.; Okajima, S.; Lim, E. C.

    1986-02-01

    We demonstrate here that the electronically excited electron donor-acceptor (EDA) complex can be different from the corresponding exciplex even in the absence of viscosity constraints that prevent the attainment of preferred donor-acceptor orientation.

  17. Persistent order due to transiently enhanced nesting in an electronically excited charge density wave

    PubMed Central

    Rettig, L.; Cortés, R.; Chu, J.-H.; Fisher, I. R.; Schmitt, F.; Moore, R. G.; Shen, Z.-X.; Kirchmann, P. S.; Wolf, M.; Bovensiepen, U.

    2016-01-01

    Non-equilibrium conditions may lead to novel properties of materials with broken symmetry ground states not accessible in equilibrium as vividly demonstrated by non-linearly driven mid-infrared active phonon excitation. Potential energy surfaces of electronically excited states also allow to direct nuclear motion, but relaxation of the excess energy typically excites fluctuations leading to a reduced or even vanishing order parameter as characterized by an electronic energy gap. Here, using femtosecond time- and angle-resolved photoemission spectroscopy, we demonstrate a tendency towards transient stabilization of a charge density wave after near-infrared excitation, counteracting the suppression of order in the non-equilibrium state. Analysis of the dynamic electronic structure reveals a remaining energy gap in a highly excited transient state. Our observation can be explained by a competition between fluctuations in the electronically excited state, which tend to reduce order, and transiently enhanced Fermi surface nesting stabilizing the order. PMID:26804717

  18. Electronic excitation as a mode of heat dissipation in laser-driven cluster plasmas

    SciTech Connect

    Rajeev, R.; Rishad, K. P. M.; Madhu Trivikram, T.; Krishnamurthy, M.

    2013-12-15

    Electrons streaming out of laser plasma are known for non-local heat transport and energy deposition by the ionization wave. At 100 eV electron temperature, since the electronic excitation cross section is comparable to that of ionization for Ar and CO{sub 2}, a non-local excitation wave akin to the ionization wave is envisaged where energy deposition in excitations forms a excited cluster sheath beyond the laser focus. Here, we show that nano-cluster systems have the right parameters to form such an exciton sheath and experimentally demonstrate this via charge transfer reactions.

  19. A technique for the measurement of electron attachment to short-lived excited species

    SciTech Connect

    Christophorou, L.G.; Pinnaduwage, L.A. ); Bitouni, A.P. . Dept. of Physics)

    1990-01-01

    A technique is described for the measurement of electron attachment to short-lived ({approx lt}10{sup {minus}9} s) excited species. Preliminary results are presented for photoenhanced electron attachment to short-lived electronically-excited states of triethylamine molecules produced by laser two-photon excitation. The attachment cross sections for these excited states are estimated to be >10{sup {minus}11} cm{sup 2} and are {approximately}10{sup 7} larger compared to those for the unexcited (ground-state) molecules. 8 refs., 4 figs.

  20. Doppler effect in fragment autoionization following core-to-valence excitation in O{sub 2}

    SciTech Connect

    Guillemin, Renaud; Simon, Marc; Shigemasa, Eiji

    2010-11-15

    Atomic autoionization following O 1s resonant excitation in O{sub 2} is studied using high-resolution electron spectroscopy. The resonant Auger spectrum showing evidence of ultrafast dissociation as well as the autoionization of oxygen atoms is measured and discussed. Evidence of the electronic Doppler effect is observed in both electronic decay mechanisms.

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

    PubMed

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

    2016-06-30

    To tune the efficiency of organic semiconductor devices it is important to understand limiting factors as trapping mechanisms for excitons or charges. An understanding of such mechanisms deserves an accurate description of the involved electronical states in the given environment. In this study, we investigate how a polarizable surrounding influences the relative positions of electronically excited states of dimers of different perylene dyes. Polarization effects are particularly interesting for these systems, because gas phase computations predict that the CT states lie slightly above the corresponding Frenkel states. A polarizable environment may change this energy order because CT states are thought to be more sensitive to a polarizable surrounding than Frenkel states. A first insight we got via a TD-HF approach in combination with a polarizable continuum model (PCM). These give limited insights because TD-HF overestimates excitation energies of CT states. However, SCS-CC2 approaches, which are sufficiently accurate, cannot easily be used in combination with continuum solvent models. Hence, we developed two approaches to combine gas phase SCS-CC2 results with solvent effects based on TD-HF computations. Their accuracies were finally checked via ADC(2)//COSMO computations. The results show that for perylene dyes a polarizable surrounding alone does not influence the energetic ordering of CT and Frenkel states. Variations in the energy order of the states only result from nuclear relaxation effects after the excitation process. © 2016 Wiley Periodicals, Inc. PMID:27030658

  2. New tools for the systematic analysis and visualization of electronic excitations. II. Applications.

    PubMed

    Plasser, Felix; Bäppler, Stefanie A; Wormit, Michael; Dreuw, Andreas

    2014-07-14

    The excited states of a diverse set of molecules are examined using a collection of newly implemented analysis methods. These examples expose the particular power of three of these tools: (i) natural difference orbitals (the eigenvectors of the difference density matrix) for the description of orbital relaxation effects, (ii) analysis of the one-electron transition density matrix in terms of an electron-hole picture to identify charge resonance and excitonic correlation effects, and (iii) state-averaged natural transition orbitals for a compact simultaneous representation of several states. Furthermore, the utility of a wide array of additional analysis methods is highlighted. Five molecules with diverse excited state characteristics are chosen for these tasks: pyridine as a prototypical small heteroaromatic molecule, a model system of six neon atoms to study charge resonance effects, hexatriene in its neutral and radical cation forms to exemplify the cases of double excitations and spin-polarization, respectively, and a model iridium complex as a representative metal organic compound. Using these examples a number of phenomena, which are at first sight unexpected, are highlighted and their physical significance is discussed. Moreover, the generality of the conclusions of this paper is verified by a comparison of single- and multireference ab initio methods. PMID:25027999

  3. New tools for the systematic analysis and visualization of electronic excitations. II. Applications

    SciTech Connect

    Plasser, Felix Bäppler, Stefanie A.; Wormit, Michael; Dreuw, Andreas

    2014-07-14

    The excited states of a diverse set of molecules are examined using a collection of newly implemented analysis methods. These examples expose the particular power of three of these tools: (i) natural difference orbitals (the eigenvectors of the difference density matrix) for the description of orbital relaxation effects, (ii) analysis of the one-electron transition density matrix in terms of an electron-hole picture to identify charge resonance and excitonic correlation effects, and (iii) state-averaged natural transition orbitals for a compact simultaneous representation of several states. Furthermore, the utility of a wide array of additional analysis methods is highlighted. Five molecules with diverse excited state characteristics are chosen for these tasks: pyridine as a prototypical small heteroaromatic molecule, a model system of six neon atoms to study charge resonance effects, hexatriene in its neutral and radical cation forms to exemplify the cases of double excitations and spin-polarization, respectively, and a model iridium complex as a representative metal organic compound. Using these examples a number of phenomena, which are at first sight unexpected, are highlighted and their physical significance is discussed. Moreover, the generality of the conclusions of this paper is verified by a comparison of single- and multireference ab initio methods.

  4. Metallic bond effects on mean excitation energies for stopping powers

    NASA Technical Reports Server (NTRS)

    Wilson, J. W.; Xu, Y. J.

    1982-01-01

    Mean excitation energies for first row metals are evaluated by means of the local plasma approximation. Particle corrections based on Pines' (1953) procedure and the Wigner Seitz (1934) model of the metallic state are included. The agreement with experimental values is remarkably good. In contrast to previous work, the calculations given here estimate shifts in the plasma frequency according to the theory for plane wave states in an extended plasma as calculated by Pines. It is demonstrated that the effects of the metallic bond in lithium and beryllium are quite large and that they appear mainly as a result of collective oscillations in the 'free' electron gas formed from the valence electrons. The usefulness of the plasma frequency shift derived for a degenerate electron gas in predicting the plasma frequency shift within the ion core is considered surprising.

  5. Ultrafast Excitation of an Inner-Shell Electron by Laser-Induced Electron Recollision

    NASA Astrophysics Data System (ADS)

    Deng, Yunpei; Zeng, Zhinan; Jia, Zhengmao; Komm, Pavel; Zheng, Yinhui; Ge, Xiaochun; Li, Ruxin; Marcus, Gilad

    2016-02-01

    Extreme ultraviolet attosecond pulses, generated by a process known as laser-induced electron recollision, are a key ingredient for attosecond metrology, providing a tool to precisely initiate and probe subfemtosecond dynamics in atoms, molecules, and solids. However, extending attosecond metrology to scrutinize the dynamics of the inner-shell electrons is a challenge, that is because of the lower efficiency in generating the required soft x-ray (ℏω >300 eV ) attosecond bursts. A way around this problem is to use the recolliding electron to directly initiate the desired inner-shell process, instead of using the currently low flux x-ray attosecond sources. Such an excitation process occurs in a subfemtosecond time scale, and may provide the necessary "pump" step in a pump-probe experiment. Here we used a few cycle infrared (λ0≈1800 nm ) source and observed direct evidence for inner-shell excitations through the laser-induced electron recollision process. It is the first step toward time-resolved core-hole studies in the keV energy range with subfemtosecond time resolution.

  6. Ultrafast Excitation of an Inner-Shell Electron by Laser-Induced Electron Recollision.

    PubMed

    Deng, Yunpei; Zeng, Zhinan; Jia, Zhengmao; Komm, Pavel; Zheng, Yinhui; Ge, Xiaochun; Li, Ruxin; Marcus, Gilad

    2016-02-19

    Extreme ultraviolet attosecond pulses, generated by a process known as laser-induced electron recollision, are a key ingredient for attosecond metrology, providing a tool to precisely initiate and probe subfemtosecond dynamics in atoms, molecules, and solids. However, extending attosecond metrology to scrutinize the dynamics of the inner-shell electrons is a challenge, that is because of the lower efficiency in generating the required soft x-ray (ℏω>300  eV) attosecond bursts. A way around this problem is to use the recolliding electron to directly initiate the desired inner-shell process, instead of using the currently low flux x-ray attosecond sources. Such an excitation process occurs in a subfemtosecond time scale, and may provide the necessary "pump" step in a pump-probe experiment. Here we used a few cycle infrared (λ_{0}≈1800  nm) source and observed direct evidence for inner-shell excitations through the laser-induced electron recollision process. It is the first step toward time-resolved core-hole studies in the keV energy range with subfemtosecond time resolution. PMID:26943536

  7. Spin excitations in systems with hopping electron transport and strong position disorder in a large magnetic field.

    PubMed

    Shumilin, A V

    2016-10-01

    We discuss the spin excitations in systems with hopping electron conduction and strong position disorder. We focus on the problem in a strong magnetic field when the spin Hamiltonian can be reduced to the effective single-particle Hamiltonian and treated with conventional numerical technics. It is shown that in a 3D system with Heisenberg exchange interaction the spin excitations have a delocalized part of the spectrum even in the limit of strong disorder, thus leading to the possibility of the coherent spin transport. The spin transport provided by the delocalized excitations can be described by a diffusion coefficient. Non-homogenous magnetic fields lead to the Anderson localization of spin excitations while anisotropy of the exchange interaction results in the Lifshitz localization of excitations. We discuss the possible effect of the additional exchange-driven spin diffusion on the organic spin-valve devices. PMID:27484892

  8. Peroxyacetyl radical: Electronic excitation energies, fundamental vibrational frequencies, and symmetry breaking in the first excited state

    SciTech Connect

    Copan, Andreas V.; Wiens, Avery E.; Nowara, Ewa M.; Schaefer, Henry F.; Agarwal, Jay

    2015-02-07

    Peroxyacetyl radical [CH{sub 3}C(O)O{sub 2}] is among the most abundant peroxy radicals in the atmosphere and is involved in OH-radical recycling along with peroxyacetyl nitrate formation. Herein, the ground (X{sup ~}) and first (A{sup ~}) excited state surfaces of cis and trans peroxyacetyl radical are characterized using high-level ab initio methods. Geometries, anharmonic vibrational frequencies, and adiabatic excitation energies extrapolated to the complete basis-set limit are reported from computations with coupled-cluster theory. Excitation of the trans conformer is found to induce a symmetry-breaking conformational change due to second-order Jahn-Teller interactions with higher-lying excited states. Additional benchmark computations are provided to aid future theoretical work on peroxy radicals.

  9. Excitation, propagation, and damping of electron Bernstein waves in tokamaks

    NASA Astrophysics Data System (ADS)

    Ram, A. K.; Schultz, S. D.

    2000-10-01

    The conventional ordinary O-mode and the extraordinary X-mode in the electron cyclotron range of frequencies are not suitable for core heating in high-β spherical tokamak plasmas, like the National Spherical Torus Experiment [M. Ono, S. Kaye, M. Peng et al., in Proceedings of the 17th International Atomic Energy Agency Fusion Energy Conference (International Atomic Energy Agency, Vienna, 1999), Vol. 3, p. 1135], as they are weakly damped at high harmonics of the electron cyclotron frequency. However, electron Bernstein waves (EBW) can be effective for heating and driving currents in spherical tokamak plasmas. Power can be coupled to EBWs via mode conversion of either the X-mode or the O-mode. The two mode conversions are optimized in different regions of the parameter space spanned by the parallel wavelength and wave frequency. The conditions for optimized mode conversion to EBWs are evaluated analytically and numerically using a cold plasma model and an approximate kinetic model. From geometric optics ray tracing it is found that the EBWs damp strongly near the Doppler-broadened resonance at harmonics of the electron cyclotron frequency.

  10. Intermediate energy cross sections for electron-impact vibrational-excitation of pyrimidine

    SciTech Connect

    Jones, D. B.; Ellis-Gibbings, L.; García, G.; Nixon, K. L.; Lopes, M. C. A.; Brunger, M. J.

    2015-09-07

    We report differential cross sections (DCSs) and integral cross sections (ICSs) for electron-impact vibrational-excitation of pyrimidine, at incident electron energies in the range 15–50 eV. The scattered electron angular range for the DCS measurements was 15°–90°. The measurements at the DCS-level are the first to be reported for vibrational-excitation in pyrimidine via electron impact, while for the ICS we extend the results from the only previous condensed-phase study [P. L. Levesque, M. Michaud, and L. Sanche, J. Chem. Phys. 122, 094701 (2005)], for electron energies ⩽12 eV, to higher energies. Interestingly, the trend in the magnitude of the lower energy condensed-phase ICSs is much smaller when compared to the corresponding gas phase results. As there is no evidence for the existence of any shape-resonances, in the available pyrimidine total cross sections [Baek et al., Phys. Rev. A 88, 032702 (2013); Fuss et al., ibid. 88, 042702 (2013)], between 10 and 20 eV, this mismatch in absolute magnitude between the condensed-phase and gas-phase ICSs might be indicative for collective-behaviour effects in the condensed-phase results.

  11. Decoherence dynamics of coherent electronic excited states in the photosynthetic purple bacterium Rhodobacter sphaeroides

    NASA Astrophysics Data System (ADS)

    Liang, Xian-Ting; Zhang, Wei-Min; Zhuo, Yi-Zhong

    2010-01-01

    In this paper, we present a theoretical description to the quantum coherence and decoherence phenomena of energy transfer in photosynthesis observed in a recent experiment [Science 316, 1462 (2007)]. As a successive two-color laser pulses with selected frequencies cast on a sample of the photosynthetic purple bacterium Rb. sphaeroides two resonant excitations of electrons in chromophores can be generated. However, this effective two-level subsystem will interact with its protein environment and decoherence is inevitable. We describe this subsystem coupled with its environment as a dynamical spin-boson model. The non-Markovian decoherence dynamics is described using a quasiadiabatic propagator path integral (QUAPI) approach. With the photon-induced effective time-dependent level splitting energy and level flip coupling coefficient between the two excited states and the environment-induced non-Markovian decoherence dynamics, our theoretical result is in good agreement with the experimental data.

  12. Vibronic structure and coupling of higher excited electronic states in carotenoids

    NASA Astrophysics Data System (ADS)

    Krawczyk, Stanisław; Luchowski, Rafał

    2013-03-01

    Absorption spectra of all-trans carotenoids (lycopene, violaxanthin, ζ-carotene) at low temperature exhibit peculiar features in the UV range. The transition to the 11Ag+ state ('cis-band') weakens on cooling, indicating that it is induced by thermal deformations of the conjugated chain. The higher energy band has unique vibrational structure indicating the vibronic coupling of nBu with another electronic state. The electroabsorption spectra point to the electric field-induced mixing of the nBu state with the vibrational continuum of a lower-lying excited state (Fano effect). These observations widen the basis for elucidation of the vibronic coupling effects in the lower excited states.

  13. Spin radical enhanced magnetocapacitance effect in intermolecular excited states.

    PubMed

    Zang, Huidong; Wang, Jianguo; Li, Mingxing; He, Lei; Liu, Zitong; Zhang, Deqing; Hu, Bin

    2013-11-14

    This article reports the magnetocapacitance effect (MFC) based on both pristine polymer MEH-PPV and its composite system doped with spin radicals (6R-BDTSCSB). We observed that a photoexcitation leads to a significant positive MFC in the pristine MEH-PPV. Moreover, we found that a low doping of spin radicals in polymer MEH-PPV causes a significant change on the MFC signal: an amplitude increase and a line-shape narrowing under light illumination at room temperature. However, no MFC signal was observed under dark conditions in either the pristine MEH-PPV or the radical-doped MEH-PPV. Furthermore, the magnitude increase and line-shape narrowing caused by the doped spin radicals are very similar to the phenomena induced by increasing the photoexcitation intensity. Our studies suggest that the MFC is essentially originated from the intermolecular excited states, namely, intermolecular electron-hole pairs, generated by a photoexcitation in the MEH-PPV. More importantly, by comparing the effects of spin radicals and electrically polar molecules on the MFC magnitude and line shape, we concluded that the doped spin radicals can have the spin interaction with intermolecular excited states and consequently affect the internal spin-exchange interaction within intermolecular excited states in the development of MFC. Clearly, our experimental results indicate that dispersing spin radicals forms a convenient method to enhance the magnetocapacitance effect in organic semiconducting materials. PMID:24144347

  14. Differential cross sections for electron-impact excitation of the electronic states of N sub 2

    SciTech Connect

    Brunger, M.J.; Teubner, P.J.O. )

    1990-02-01

    Differential cross sections for the electron-impact excitation of the first ten electronic states of N{sub 2} have been determined at five incident energies ranging from 15 to 50 eV. These differential cross sections were obtained for the scattering range 10{degree}--90{degree} by analyzing electron-energy-loss spectra in N{sub 2} at a number of fixed scattering angles within that range. The present study represents a comprehensive remeasurement of the earlier work of Cartwright and co-workers (Phys. Rev. A 16, 1013 (1977)) and was undertaken with a view to resolving certain anomalies which have been reported in the literature when the earlier cross-section set has been applied to model calculations of swarm parameters.

  15. Cross Sections for Electron Impact Excitation of Ions Relevant to Planetary Atmospheres Observation

    NASA Technical Reports Server (NTRS)

    Tayal, Swaraj S.

    1998-01-01

    The goal of this research grant was to calculate accurate oscillator strengths and electron collisional excitation strengths for inelastic transitions in atomic species of relevance to Planetary Atmospheres. Large scale configuration-interaction atomic structure calculations have been performed to obtain oscillator strengths and transition probabilities for transitions among the fine-structure levels and R-matrix method has been used in the calculations of electron-ion collision cross sections of C II, S I, S II, S III, and Ar II. A number of strong features due to ions of sulfur have been detected in the spectra of Jupiter satellite Io. The electron excitation cross sections for the C II and S II transitions are studied in collaboration with the experimental atomic physics group at the Jet Propulsion Laboratory. There is excellent agreement between experiment and theory which provide an accurate and broad-base test of the ability of theoretical methods used in the calculation of atomic processes. Specifically, research problems have been investigated for: electron impact excitation cross sections of C II: electron impact excitation cross sections of S III; energy levels and oscillator strengths for transitions in S III; collision strengths for electron collisional excitation of S II; electron impact excitation of inelastic transitions in Ar II; oscillator strengths of fine-structure transitions in neutral sulfur; cross sections for inelastic scattering of electrons from atomic nitrogen; and excitation of atomic ions by electron impact.

  16. Mitigation of electron attachment to oxygen in high pressure air plasmas by vibrational excitation

    NASA Astrophysics Data System (ADS)

    Frederickson, K.; Lee, W.; Palm, P.; Adamovich, I. V.; Rich, J. W.; Lempert, W. R.

    2007-05-01

    A series of time resolved microwave attenuation measurements are performed of the electron number density of an electron beam generated, CO laser excited nonequilibrium O2/N2 plasma. Resonant absorption of infrared radiation from the CO laser produces the nonequilibrium state, in which the heavy species vibrational modes are disproportionately excited, compared to the rotational and translational modes (Tvib≈2000-3000K vs TR /T≈300K). It is shown that this results in an increase in the plasma free electron lifetime by two orders of magnitude compared to the unexcited cold gas, an effect which is ascribed to complete mitigation of rapid three-body electron attachment to molecular oxygen. A series of heavy species filtered pure rotational Raman scattering measurements are also presented, which exhibit minimal temperature change (+50K), indicating that the observed lifetime increase cannot be due to heavy-species thermal effects. Finally, computational modeling results infer an increase in the rate of O2- detachment by four to five orders of magnitude, compared to the equilibrium value.

  17. On the character of the coherent and incoherent excitations of electron-doped SrTiO3

    NASA Astrophysics Data System (ADS)

    Ishida, Yukiaki; Eguchi, Ritsuko; Matsunami, Masaharu; Horiba, Koji; Taguchi, Munetaka; Chainani, Ashishi; Senba, Yasunori; Ohashi, Haruhiko; Ohta, Hiromichi; Shin, Shik

    2007-03-01

    Lightly-electron-doped SrTiO3 shows little sign of electron correlation effects in the transport and thermodynamic properties, but photoemission spectra show not only coherent excitations from the Fermi level but also broad incoherent excitations positioned ˜1.5 eV below the Fermi level [1]. We have investigated the near-EF electronic structures of Nb-doped SrTiO3 thin film [2] by performing resonant photoemission at the Ti 2p and O 1s absorption edges. Both the coherent and incoherent excitations showed giant resonances at the Ti 2p edge, while at the O 1s edge, resonance occurred mainly in the incoherent excitations. This indicates that the coherent excitations have mainly Ti 3d character, while the incoherent excitations have mixed character of Ti 3d and O 2p states. We attribute the incoherent and coherent excitations to locally and non-locally screened final states, respectively, similar to that argued in Ca1-xSrxVO3 [3]. [1] A. Fujimori et al., Phys. Rev. B 46, 9841 (1992). [2] S. Ohta, H. Ohta et al., Appl. Phys. Lett. 87, 092108 (2006). [3] R.J.O. Mossanek, M. Abbate, and A. Fujimori, cond-mat/0606253.

  18. Absolute cross sections for electronic excitations of cytosine by low energy electron impact

    PubMed Central

    Bazin, M.; Michaud, M.; Sanche, L.

    2013-01-01

    The absolute cross sections (CS) for electronic excitations of cytosine by electron impact between 5 and 18 eV were measured by electron-energy loss (EEL) spectroscopy of the molecule deposited at low coverage on an inert Ar substrate. The lowest EEL features found at 3.55 and 4.02 eV are ascribed to transitions from the ground state to the two lowest triplet 1 3A′(π→π*) and 2 3A′(π→π*) valence states of the molecule. Their energy dependent CS exhibit essentially a common maximum at about 6 eV with a value of 1.84 × 10−17 cm2 for the former and 4.94 × 10−17 cm2 for the latter. In contrast, the CS for the next EEL feature at 4.65 eV, which is ascribed to the optically allowed transition to the 2 1A′(π→π*) valence state, shows only a steep rise to about 1.04 × 10−16 cm2 followed by a monotonous decrease with the incident electron energy. The higher EEL features at 5.39, 6.18, 6.83, and 7.55 eV are assigned to the excitations of the 3 3, 1A′(π→π*), 4 1A′(π→π*), 5 1A′(π→π*), and 6 1A′(π→π*) valence states, respectively. The CS for the 3 3, 1A′ and 4 1A′ states exhibit a common enhancement at about 10 eV superimposed on a more or less a steep rise, reaching respectively a maximum of 1.27 and 1.79 × 10−16 cm2, followed by a monotonous decrease. This latter enhancement and the maximum seen at about 6 eV in the lowest triplet states correspond to the core-excited electron resonances that have been found by dissociative electron attachment experiments with cytosine in the gas phase. The weak EEL feature found at 5.01 eV with a maximum CS of 3.8 × 10−18 cm2 near its excitation threshold is attributed to transitions from the ground state to the 1 3, 1A″(n→π*) states. The monotonous rise of the EEL signal above 8 eV is attributed to the ionization of the molecule. It is partitioned into four excitation energy regions at about 8.55, 9.21, 9.83, and 11.53 eV, which correspond closely to the ionization energies of

  19. Nuclear fission fragment excitation of electronic transition laser media

    NASA Technical Reports Server (NTRS)

    Lorents, D. C.; Mccusker, M. V.; Rhodes, C. K.

    1976-01-01

    Specific characteristics of the media including density, excitation rates, wavelength, kinetics, fissile material, scale size, and medium uniformity are assessed. The use of epithermal neutrons, homogeneously mixed fissile material, and special high cross section nuclear isotopes to optimize coupling of the energy to the medium are shown to be important considerations maximizing the scale size, energy deposition, and medium uniformity. It is demonstrated that e-beam excitation can be used to simulate nuclear pumping conditions to facilitate the search for candidate media.

  20. Electron Impact Excitation of Polarised Sodium and Potassium.

    NASA Astrophysics Data System (ADS)

    Bukhari, Muhammad Abdul-Hakim

    Available from UMI in association with The British Library. Requires signed TDF. A beam of unpolarised electrons is crossed at right angles with a beam of partially polarised sodium or potassium atoms (degree of polarisation { bf P}_{bf A} = 21%). The resonance radiation from excited ^2P_{3/2,1/2} states is observed in a direction perpendicular to both beams, and the Stokes parameters {bf P}_ {bf 1}, {bf P }_{bf 2} and {bf P}_{bf 3} of the emitted photons are measured, {bf P}_{bf 1} = {I(0^circ)-I(90^circ)over I(0^circ)+I(90^circ)}, {bf P}_{bf 2} = {I(45^circ)-I(135^circ)over I(45^circ)+I(135^circ)}, {bf P}_{bf 3} = {I(RHC)-I(LHC)over I(RHC)+I(LHC)} where 0^circ, 45 ^circ, 90^circ and 135^circ corresponds to the polariser angle measured from the electron beam direction and RHC, LHC to right and left hand circular polarisation in the spectroscopic definition. Because of reflection symmetries, only {bf P }_{bf 1} is expected to be non-zero for unpolarised atoms. If polarised atoms are used with their spins parallel to the direction of the observed photons, {bf P}_ {bf 3} should also become non-zero (in addition to {bf P}_ {bf 1}) while {bf P}_{bf 2} remains zero. We report here an independent measurement on the neutral sodium NaI (3^2{bf P }_{3/2,1/2} - 3^2{bf S}_{1/2}) transition ( lambda=589.0, 589.6 nm) and present new results for the neutral potassium KI (5^2{ bf P}_{3/2,1/2} - 4^2 {bf S}_{1/2}) transition (lambda=404.4, 404.7 nm). The potassium results for {bf P}_{ bf 2} agree well with the theoretical prediction of zero and the results for {bf P}_{bf 1} show close similarities to those of sodium results at high and intermediate energies, while at low energy especially close to threshold they differ. The threshold polarisation ({ bf P}_{bf 1}) in the case of potassium is about 10%. Our { bf P}_{bf 3} values for sodium are somewhat higher than the results of Osimitsch and Jitschin. The trend of {bf P} _{bf 3} for potassium is similar to that of sodium in such a

  1. The separation of vibrational coherence from ground- and excited-electronic states in P3HT film

    SciTech Connect

    Song, Yin; Hellmann, Christoph; Stingelin, Natalie; Scholes, Gregory D.

    2015-06-07

    Concurrence of the vibrational coherence and ultrafast electron transfer has been observed in polymer/fullerene blends. However, it is difficult to experimentally investigate the role that the excited-state vibrational coherence plays during the electron transfer process since vibrational coherence from the ground- and excited-electronic states is usually temporally and spectrally overlapped. Here, we performed 2-dimensional electronic spectroscopy (2D ES) measurements on poly(3-hexylthiophene) (P3HT) films. By Fourier transforming the whole 2D ES datasets (S(λ{sub 1},T{sup ~}{sub 2},λ{sub 3})) along the population time (T{sup ~}{sub 2}) axis, we develop and propose a protocol capable of separating vibrational coherence from the ground- and excited-electronic states in 3D rephasing and nonrephasing beating maps (S(λ{sub 1},ν{sup ~}{sub 2},λ{sub 3})). We found that the vibrational coherence from pure excited electronic states appears at positive frequency (+ν{sup ~}{sub 2}) in the rephasing beating map and at negative frequency (−ν{sup ~}{sub 2}) in the nonrephasing beating map. Furthermore, we also found that vibrational coherence from excited electronic state had a long dephasing time of 244 fs. The long-lived excited-state vibrational coherence indicates that coherence may be involved in the electron transfer process. Our findings not only shed light on the mechanism of ultrafast electron transfer in organic photovoltaics but also are beneficial for the study of the coherence effect on photoexcited dynamics in other systems.

  2. Electron emission from fast heavy ions associated with resonant coherent excitation

    NASA Astrophysics Data System (ADS)

    Suda, S.; Nakano, Y.; Metoki, K.; Azuma, T.; Takano, Y.; Hatakeyama, A.; Nakai, Y.; Komaki, K.; Takada, E.; Murakami, T.

    2011-06-01

    We observed convoy electrons emitted from 416 MeV/u He-like Ar16+ passing through a thin Si crystal under the condition of three-dimensional resonant coherent excitation (3D-RCE). The convoy electrons, which originate from electrons released from ions into the continuum by collisions with target atoms, emerged in the forward direction and formed a cusp-shaped peak in the energy distribution. We selectively controlled the population of the ground and excited states of ions traveling through the crystal by using 3D-RCE, where the 1s electron was excited to the 2p state by a periodic crystal field. Under the resonance condition, we found an enhancement of the convoy electrons with a narrowing in the energy distribution, which reflects the electron momentum distribution of the initial bound state of the excited ions.

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

    NASA Technical Reports Server (NTRS)

    Hall, R. I.; Trajmar, S.

    1973-01-01

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

  4. Photoelectron spectroscopy of hexachloroplatinate-nucleobase complexes: Nucleobase excited state decay observed via delayed electron emission

    SciTech Connect

    Sen, Ananya; Matthews, Edward M.; Dessent, Caroline E. H. E-mail: xuebin.wang@pnnl.gov; Hou, Gao-Lei; Wang, Xue-Bin E-mail: xuebin.wang@pnnl.gov

    2015-11-14

    We report low-temperature photoelectron spectra of isolated gas-phase complexes of the hexachloroplatinate dianion bound to the nucleobases uracil, thymine, cytosine, and adenine. The spectra display well-resolved, distinct peaks that are consistent with complexes where the hexachloroplatinate dianion is largely intact. Adiabatic electron detachment energies for the hexachloroplatinate-nucleobase complexes are measured as 2.26-2.36 eV. The magnitudes of the repulsive Coulomb barriers (RCBs) of the complexes are all ∼1.7 eV, values that are lower than the RCB of the uncomplexed PtCl{sub 6}{sup 2−} dianion as a result of charge solvation by the nucleobases. In addition to the resolved spectral features, broad featureless bands indicative of delayed electron detachment are observed in the 193 nm photoelectron spectra of the four clusters. The 266 nm spectra of the PtCl{sub 6}{sup 2−} ⋅ thymine and PtCl{sub 6}{sup 2−} ⋅ adenine complexes also display very prominent delayed electron emission bands. These results mirror recent results on the related Pt(CN){sub 4}{sup 2−} ⋅ nucleobase complexes [A. Sen et al., J. Phys. Chem. B 119, 11626 (2015)]. The observation of delayed electron emission bands in the PtCl{sub 6}{sup 2−} ⋅ nucleobase spectra obtained in this work, as for the previously studied Pt(CN){sub 4}{sup 2−} ⋅ nucleobase complexes, is attributed to one-photon excitation of nucleobase-centred excited states that can effectively couple to the electron detachment continuum, producing strong electron detachment. Moreover, the selective, strong excitation of the delayed emission bands in the 266 nm spectra is linked to fundamental differences in the individual nucleobase photophysics at this excitation energy. This strongly supports our previous suggestion that the dianion within these clusters can be viewed as a “dynamic tag” which has the propensity to emit electrons when the attached nucleobase decays over a time scale long enough to

  5. Probing core-electron orbitals by scanning transmission electron microscopy and measuring the delocalization of core-level excitations

    NASA Astrophysics Data System (ADS)

    Jeong, Jong Seok; Odlyzko, Michael L.; Xu, Peng; Jalan, Bharat; Mkhoyan, K. Andre

    2016-04-01

    By recording low-noise energy-dispersive x-ray spectroscopy maps from crystalline specimens using aberration-corrected scanning transmission electron microscopy, it is possible to probe core-level electron orbitals in real space. Both the 1 s and 2 p orbitals of Sr and Ti atoms in SrTi O3 are probed, and their projected excitation potentials are determined. This paper also demonstrates experimental measurement of the electronic excitation impact parameter and the delocalization of an excitation due to Coulombic beam-orbital interaction.

  6. Excitation and ionization of outer shells in Rb by electron impact

    NASA Astrophysics Data System (ADS)

    Roman, V.; Kupliauskienė, A.; Borovik, A.

    2015-10-01

    The relativistic distorted-wave and binary-encounter-dipole approximations were employed for calculating the electron-impact single ionization cross sections of the 5s, 4p6, 4s2, 3d10 shells and 4p6 excitation cross section for Rb atom taking into account both configuration interaction and relativistic effects. The capabilities of the most used theoretical approaches in describing the single ionization of Rb atom were considered by comparing the present and other available calculated data with the experimental total ionization and total direct single ionization cross sections over the electron-impact energy range from the 5s threshold to 600 eV. The best agreement within experimental uncertainty was obtained by using the non-relativistic binary-encounter-dipole approximation included in the LANL Atomic Physics Codes package. At present none of the used approximations (plane-wave Born or relativistic distorted wave) can satisfactorily describe the experimental excitation-autoionization cross section in rubidium because the efficient formation of the 4p6 core-excited negative-ion rubidium states at near-threshold impact energies is ignored in calculations.

  7. Radiative association of LiH(X 1Σ+) from electronically excited lithium atoms

    NASA Astrophysics Data System (ADS)

    Gianturco, F. A.; Gori Giorgi, P.

    1996-11-01

    Full quantum calculations are carried out for the collisional processes involving H atoms in their ground electronic state and electronically excited lithium atoms, Li(1s22p). The channels that are being considered are those leading to the formation of bound rotovibrational states of LiH(X 1Σ+). The effects of both the specific features of the involved electronic potential-energy curves and of the transition moments coupling bound and continuum states during the process are studied in relation to the low-energy behavior of the corresponding cross sections. The role of the multitude of open channel resonances on the final rate constants is also analyzed and discussed over a broad range of bath temperatures.

  8. Anharmonicity Effects in IR Spectra of [Re(X)(CO)3(α-diimine)] (α-diimine = 2,2'-bipyridine or pyridylimidazo[1,5-a]pyridine; X = Cl or NCS) Complexes in Ground and Excited Electronic States.

    PubMed

    Kvapilová, Hana; Vlček, Antonín; Barone, Vincenzo; Biczysko, Malgorzata; Záliš, Stanislav

    2015-10-01

    Infrared spectra of [Re(X)(CO)(3)(α-diimine)] (α-diimine = 2,2'-bipyridine, X = Cl, NCS, or pyridylimidazo[1,5-a]pyridine, X = Cl) in the ground and the lowest triplet electronic states were calculated by a global hybrid density functional going beyond the harmonic level by means of second-order vibrational perturbation theory (VPT2) and including bulk solvent effects by the polarizable continuum model (PCM). The full-dimensionality (FD) VPT2 is compared with the reduced-dimensionality (RD) model, where only selected vibrational modes are calculated anharmonically. The simulated difference IR spectra (excited state minus ground state) in the ν(CO) region closely match experimental time-resolved infrared (TRIR) spectra. Very good agreement was also obtained for ground-state spectra in the fingerprint region. In comparison with the harmonic simulated spectra, the calculated anharmonic frequencies are closer to experimental values and do not require scaling when the B3LYP functional is used. Several spectral features due to combination bands have been identified by VPT2 simulations in the ν(CO) spectral region, which are of importance for a correct interpretation of TRIR experiments. PMID:26367031

  9. Impact excitation of neon atoms by heated seed electrons in filamentary plasma gratings.

    PubMed

    Shi, Liping; Li, Wenxue; Zhou, Hui; Ding, Liang'en; Zeng, Heping

    2013-02-15

    We demonstrate impact ionization and dissociative recombination of neon (Ne) atoms by means of seeded-electron heating and subsequent electron-atom collisions in an ultraviolet plasma grating, allowing for a substantial fraction of the neutral Ne atomic population to reside in high-lying excited states. A buffer gas with relatively low ionization potential (nitrogen or argon) was used to provide high-density seed electrons. A three-step excitation model is verified by the fluorescence emission from the impact excitation of Ne atoms. PMID:23455081

  10. Remote lasing in air by recombination and electron impact excitation of molecular nitrogen

    NASA Astrophysics Data System (ADS)

    Peñano, Joseph; Sprangle, Phillip; Hafizi, Bahman; Gordon, Daniel; Fernsler, Richard; Scully, Marlan

    2012-02-01

    We analyze and simulate the physical mechanisms for a remote atmospheric lasing configuration which utilizes a combination of an ultrashort pulse laser to form a plasma filament of seed electrons, and a heater beam to heat the seed electrons. Nitrogen molecules are excited by electron impact and recombination processes to induce lasing in the ultraviolet. Recombination excitation, thermal excitation, gain, and saturation are analyzed and simulated. The lasing gain is sufficiently high to reach saturation within the length of the plasma filament. A remotely generated ultraviolet source may have applications for standoff detection of biological and chemical agents.

  11. Excitation of positive ions by low-energy electrons - Relevance to the Io Torus

    NASA Technical Reports Server (NTRS)

    Smith, Steven J.; Chutjian, A.; Mawhorter, R. J.; Williams, I. D.; Shemansky, D. E.

    1993-01-01

    The importance of measuring electron-ion excitation cross sections in singly and multiply charged positive ions is outlined, and recent results for Mg II and O II ions are given using the JPL's electron energy-loss merged-beams apparatus. Theoretical comparisons are given with two five-state close-coupling calculations. The energy variation of the collision strength is fitted with a semiempirical analytic function which includes approximations to polarization, resonance, and exchange contributions. In O II, first spectra anywhere of electron excitation of the optically allowed transitions are presented. In addition, excitations of two low lying, optically forbidden transitions are detected for the first time.

  12. Ultrafast spectroscopy of electron transfer dynamics in liquids; excitation transfer studies of phase transitions

    NASA Astrophysics Data System (ADS)

    Goun, Alexei A.

    The transfer of an electron from a donor to an acceptor is the fundamental step in a wide range of chemical and biological processes. As a result, electron-transfer reactions have been the focus of numerous theoretical and experimental efforts aimed at understanding the kinetics and mechanism of the transfer event. Liquid solvents are an important medium for electron-transfer processes. The influences of the distance dependence, diffusion, the radial distribution function, and the hydrodynamic effect have been incorporated into the theory of electron transfer in solution, as well as into the theory of electron transfer between donors and acceptors in the head group regions of micelles. The development of new laser system with a pulse duration of tens of femtoseconds, with tunable wavelength allowed us to study these processes on a considerably shorter time scale than previous studies. This allowed us to observe not only the diffusion controlled but also the kinetics of electron transfer for donor/acceptor pairs that are in close proximity. In one set of experiments we have studied the kinetics of electron transfer in electron accepting molecule (rhodamine 3B) dissolved in electron donating solvent (N,N-dimethylaniline). The data for the forward electron transfer and geminate recombination are approximated by the statistical theory of the electron transfer. Optical anisotropy observed in the experiment demonstrates the orientation dependence of the electron transfer rate. In further experiments we investigated the electron transfer in non-hydrogen bonding liquids of increasing viscosity. The effective value of the donor/acceptor electronic coupling was found to decrease with viscosity. Electron transfer experiments were also carried out on the surface of micelles. The systems studied are the hole donor octadecyl-rhodamine B (ODRB) and the hole acceptor N,N-dimethyl-aniline (DMA) in micelles made of dodecyltrimethylammonium bromide (DTAB) and

  13. Electron-impact vibrational excitation rates in the flow field of aeroassisted orbital transfer vehicles

    NASA Technical Reports Server (NTRS)

    Lee, J.-H.

    1985-01-01

    This paper examines the vibrational excitation rate processes expected in the flow field of aeroassisted orbital transfer vehicles (AOTVs). An analysis of the multiple-quantum vibrational excitation processes by electron impact is made to predict the vibrational excitation cross sections, rate coefficients, and relaxation times which control vibrational temperature. The expression for the rate of electron-vibration energy transfer is derived by solving the system of master equations which account for the multiple-level transitions. The vibrational excitation coefficients, which are the prerequisite physical quantities in solving the obtained vibrational equation, are calculated based on the theoretically predicted cross sections. These cross sections are obtained from quantum mechanical calculations, based on the concept that vibrational excitation of molecules by electron impact occurs through formation of an intermediate negative ion state. Finally, the modified Landau-Teller-type rate equation, which is suitable for the numerical calculations for the AOTV flow fields, is suggested.

  14. Comparative analysis of the optical spectra of the holmium atom excited by electron impact and ionic bombardment

    SciTech Connect

    Vasileva, E.K.; Morozov, S.N.; Ryskin, B.V.

    1988-02-01

    A comparative analysis of the optical spectra of holmium excited by electron impact and ionic bombardment is given. It is shown that under ionic bombardment, the probability of excitation of screened transitions is significantly higher than under electron impact.

  15. Coulombic Effects on Excited States in a Small Quantum Dot

    NASA Astrophysics Data System (ADS)

    Goldhaber-Gordon, David; Duncan, David; Westervelt, R. M.; Maranowski, K. M.; Gossard, A. C.

    2000-03-01

    The excitation spectrum of a quantum dot varies with the addition of electrons, as successive single-particle eigenstates become filled in the ground state and so cannot accomodate additional electrons. Previous experiments have observed that each spatial state becomes unavailable for transport of further electrons after only one electron has occupied it. We have investigated state occupancy in the excitation spectrum of a small (200 nm X 200 nm) quantum dot laterally defined by capacitively coupled gate electrodes in a GaAs/AlGaAs heterostructure. For our dots, quantized level spacing Δ E ≈ 300 μeV and charging energy Ec ≈ 2 meV. We have studied the evolution of features in the excitation spectrum with magnetic field and equilibrium occupancy and have identified the pattern of spins for the added electrons. These results test the applicability of the spin-degenerate constant interaction picture as well as its limitations.

  16. Direct Electron Impact Excitation of Rydberg-Valence States of Molecular Nitrogen

    NASA Astrophysics Data System (ADS)

    Malone, C. P.; Johnson, P. V.; Liu, X.; Ajdari, B.; Muleady, S.; Kanik, I.; Khakoo, M. A.

    2012-12-01

    Collisions between electrons and neutral N2 molecules result in emissions that provide an important diagnostic probe for understanding the ionospheric energy balance and the effects of space weather in upper atmospheres. Also, transitions to singlet ungerade states cause N2 to be a strong absorber of solar radiation in the EUV spectral range where many ro-vibrational levels of these Rydberg-valence (RV) states are predissociative. Thus, their respective excitation and emission cross sections are important parameters for understanding the [N]/[N2] ratio in the thermosphere of nitrogen dominated atmospheres. The following work provides improved constraints on absolute and relative excitation cross sections of numerous RV states of N2, enabling more physically accurate atmospheric modeling. Here, we present recent integral cross sections (ICSs) for electron impact excitation of RV states of N2 [6], which were based on the differential cross sections (DCSs) derived from electron energy-loss (EEL) spectra of [5]. This work resulted in electronic excitation cross sections over the following measured vibrational levels: b 1Πu (v‧=0-14), c3 1Πu (v‧=0-3), o3 1Πu (v‧=0-3), b‧ 1Σu+ (v‧=0-10), c‧4 1Σu+ (v‧=0-3), G 3Πu (v‧=0-3), and F 3Πu (v‧=0-3). We further adjusted the cross sections of the RV states by extending the vibronic contributions to unmeasured v‧-levels via the relative excitation probabilities (REPs) as discussed in [6]. This resulted in REP-scaled ICSs over the following vibrational levels for the singlet ungerade states: b(0-19), c3(0-4), o3(0-4), b‧(0-16), and c‧4(0-8). Comparison of the ICSs of [6] with available EEL based measurements, theoretical calculations, and emission based work generally shows good agreement within error estimations, except with the recent reevaluation provided by [1]. Further, we have extended these results, using the recent EEL data of [3], to include the unfolding of better resolved features above ~13

  17. Vacuum ultraviolet studies of electron impact of helium Excitation of He n1P0 Rydberg series and ionization-excitation of He(+) nl Rydberg series

    NASA Technical Reports Server (NTRS)

    Shemansky, D. E.; Hall, D. T.; Ajello, J. M.; Franklin, B.

    1985-01-01

    The cross sections for the He I 1s2 1S-1snp 1P0 series have been measured using a relative flow method, with the absolute scale fixed by the H Ly-alpha dissociative excitation cross section standard. The results are compared with those obtained using a relative cross section data analysis by modified Born approximation, and good agreement is found. Cross sections for the ionization-excitation of the He II 121.51 nm and He II 164.04 nm transmissions have been measured, and the results strongly suggest that theoretical calculations of the reactions differ fundamentally from physical reality. The failure of the theory to describe experimental results stems from the neglect in the theory of electron correlation effects between the two orbital electrons.

  18. Excited-State Effective Masses in Lattice QCD

    SciTech Connect

    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.

  19. Study of intermediates from transition metal excited-state electron- transfer reactions. Progress report, January 1, 1992--March 31, 1993

    SciTech Connect

    Hoffman, M.Z.

    1993-03-31

    Progress on 6 projects is reported: excited state absorption spectrum of Ru(bpy){sub 3}{sup 2+}, solvent cage model for electron transfer quenching, reductive quenching of {sup *}Cr(III) complexes, solution medium effects in oxidative quenching of {sup *}Ru(II) complexes, photosensitized oxidation of phenol in aqueous solution, and quenching of Ru(II) complexes by oxygen.

  20. Electron impact excitation of helium in Debye plasma

    SciTech Connect

    Diallo, S.; Gomis, L.; Faye, I. G.; Tall, M. S.; Diédhiou, I.; Diatta, C. S.; Zammit, M.

    2015-03-15

    The probability, differential, and integral scattering cross sections of the 1{sup 1}S→2{sup 1}S and 1{sup 1}S→2{sup 1}P transitions of helium have been calculated in the first Born approximation. The projectile-target interactions depending on the temperature and the density of plasma are described by the Debye-Hückel model. Wave functions of the target before and after collision were modeled by non orthogonal Hartree-Fock orbitals. The wave functions parameters are calculated with the Ritz variational method. We improve our unscreened first Born approximation integral cross sections by using the BE-scaled (B stands for binding energy and E excitation energy) method. The second Born approximation has also been used to calculate the excitation cross sections in Debye plasma. Our calculations are compared to other theoretical and experimental results where applicable.

  1. Electron impact excitation of helium in Debye plasma

    NASA Astrophysics Data System (ADS)

    Diallo, S.; Gomis, L.; Faye, I. G.; Tall, M. S.; Diédhiou, I.; Diatta, C. S.; Zammit, M.

    2015-03-01

    The probability, differential, and integral scattering cross sections of the 11S →21S and 11S →21P transitions of helium have been calculated in the first Born approximation. The projectile-target interactions depending on the temperature and the density of plasma are described by the Debye-Hückel model. Wave functions of the target before and after collision were modeled by non orthogonal Hartree-Fock orbitals. The wave functions parameters are calculated with the Ritz variational method. We improve our unscreened first Born approximation integral cross sections by using the BE-scaled (B stands for binding energy and E excitation energy) method. The second Born approximation has also been used to calculate the excitation cross sections in Debye plasma. Our calculations are compared to other theoretical and experimental results where applicable.

  2. Dynamics of electron injection from the excited state of anchored molecules into semiconductors

    NASA Astrophysics Data System (ADS)

    Gundlach, L.; Ernstorfer, R.; Willig, F.

    A complete picture of different interfacial electron transfer dynamics has been obtained from transient absorption and two-photon photoemission data when inserting different anchor/bridge groups between the excited organic donor and the electrode surface.

  3. Carotenoid Excited State Kinetics in Bacterial RCs with the Primary Electron Donor Oxidized

    NASA Astrophysics Data System (ADS)

    Lin, Su; Katilius, Evaldas; Woodbury, Neal W.

    Carotenoid singlet excited state kinetics in wild type reaction centers from Rhodobacter sphaeroides was investigated using ultrafast laser spectroscopy under conditions where the primary electron donor is either neutral or oxidized.

  4. Modeling of electronic excitation and radiation in non-continuum hypersonic reentry flows

    NASA Astrophysics Data System (ADS)

    Li, Zheng; Ozawa, Takashi; Sohn, Ilyoup; Levin, Deborah A.

    2011-06-01

    The modeling of hypersonic radiation in non-equilibrium, non-continuum flows is considered in the framework of the direct simulation Monte Carlo (DSMC) approach. The study explores the influence of electronic states on the flow chemistry and degree of ionization as well as the assumption that the electronic states can be described by a steady state solution to a system of rate equations of excitation, de-excitation, and radiative transfer processes. The work implements selected excited levels of atomic nitrogen and oxygen and the corresponding electron impact excitation/de-excitation and ionization processes in DSMC. The simulations show that when excitation models are included, the degree of ionization in the Stardust transitional re-entry flow increases due to additional intermediate steps to ionization. The extra ionization reactions consume the electron energy to reduce the electron temperature. The DSMC predicted excited state level populations are lower than those predicted by a quasi steady state calculation, but the differences can be understood in terms of the flow distribution functions.

  5. Imaging Excited State Dynamics with 2d Electronic Spectroscopy

    NASA Astrophysics Data System (ADS)

    Engel, Gregory S.

    2012-06-01

    Excited states in the condensed phase have extremely high chemical potentials making them highly reactive and difficult to control. Yet in biology, excited state dynamics operate with exquisite precision driving solar light harvesting in photosynthetic complexes though excitonic transport and photochemistry through non-radiative relaxation to photochemical products. Optimized by evolution, these biological systems display manifestly quantum mechanical behaviors including coherent energy transfer, steering wavepacket trajectories through conical intersections and protection of long-lived quantum coherence. To image the underlying excited state dynamics, we have developed a new spectroscopic method allowing us to capture excitonic structure in real time. Through this method and other ultrafast multidimensional spectroscopies, we have captured coherent dynamics within photosynthetic antenna complexes. The data not only reveal how biological systems operate, but these same spectral signatures can be exploited to create new spectroscopic tools to elucidate the underlying Hamiltonian. New data on the role of the protein in photosynthetic systems indicates that the chromophores mix strongly with some bath modes within the system. The implications of this mixing for excitonic transport will be discussed along with prospects for transferring underlying design principles to synthetic systems.

  6. Plasmon-resonant Raman spectroscopy in metallic nanoparticles: Surface-enhanced scattering by electronic excitations

    NASA Astrophysics Data System (ADS)

    Carles, R.; Bayle, M.; Benzo, P.; Benassayag, G.; Bonafos, C.; Cacciato, G.; Privitera, V.

    2015-11-01

    Since the discovery of surface-enhanced Raman scattering (SERS) 40 years ago, the origin of the "background" that is systematically observed in SERS spectra has remained questionable. To deeply analyze this phenomenon, plasmon-resonant Raman scattering was recorded under specific experimental conditions on a panel of composite multilayer samples containing noble metal (Ag and Au) nanoparticles. Stokes, anti-Stokes, and wide, including very low, frequency ranges have been explored. The effects of temperature, size (in the nm range), embedding medium (SiO2, Si3N4, or TiO2) or ligands have been successively analyzed. Both lattice (Lamb modes and bulk phonons) and electron (plasmon mode and electron-hole excitations) dynamics have been investigated. This work confirms that in Ag-based nanoplasmonics composite layers, only Raman scattering by single-particle electronic excitations accounts for the background. This latter appears as an intrinsic phenomenon independently of the presence of molecules on the metallic surface. Its spectral shape is well described by revisiting a model developed in the 1990s for analyzing electron scattering in dirty metals, and used later in superconductors. The gs factor, that determines the effective mean-free path of free carriers, is evaluated, gsexpt=0.33 ±0.04 , in good agreement with a recent evaluation based on time-dependent local density approximation gstheor=0.32 . Confinement and interface roughness effects at the nanometer range thus appear crucial to understand and control SERS enhancement and more generally plasmon-enhanced processes on metallic surfaces.

  7. Analytic energy gradient of excited electronic state within TDDFT/MMpol framework: Benchmark tests and parallel implementation

    SciTech Connect

    Zeng, Qiao; Liang, WanZhen

    2015-10-07

    The time-dependent density functional theory (TDDFT) has become the most popular method to calculate the electronic excitation energies, describe the excited-state properties, and perform the excited-state geometric optimization of medium and large-size molecules due to the implementation of analytic excited-state energy gradient and Hessian in many electronic structure software packages. To describe the molecules in condensed phase, one usually adopts the computationally efficient hybrid Quantum Mechanics/Molecular Mechanics (QM/MM) models. Here, we extend our previous work on the energy gradient of TDDFT/MM excited state to account for the mutual polarization effects between QM and MM regions, which is believed to hold a crucial position in the potential energy surface of molecular systems when the photoexcitation-induced charge rearrangement in the QM region is drastic. The implementation of a simple polarizable TDDFT/MM (TDDFT/MMpol) model in Q-Chem/CHARMM interface with both the linear response and the state-specific features has been realized. Several benchmark tests and preliminary applications are exhibited to confirm our implementation and assess the effects of different treatment of environmental polarization on the excited-state properties, and the efficiency of parallel implementation is demonstrated as well.

  8. Analytic energy gradient of excited electronic state within TDDFT/MMpol framework: Benchmark tests and parallel implementation.

    PubMed

    Zeng, Qiao; Liang, WanZhen

    2015-10-01

    The time-dependent density functional theory (TDDFT) has become the most popular method to calculate the electronic excitation energies, describe the excited-state properties, and perform the excited-state geometric optimization of medium and large-size molecules due to the implementation of analytic excited-state energy gradient and Hessian in many electronic structure software packages. To describe the molecules in condensed phase, one usually adopts the computationally efficient hybrid Quantum Mechanics/Molecular Mechanics (QM/MM) models. Here, we extend our previous work on the energy gradient of TDDFT/MM excited state to account for the mutual polarization effects between QM and MM regions, which is believed to hold a crucial position in the potential energy surface of molecular systems when the photoexcitation-induced charge rearrangement in the QM region is drastic. The implementation of a simple polarizable TDDFT/MM (TDDFT/MMpol) model in Q-Chem/CHARMM interface with both the linear response and the state-specific features has been realized. Several benchmark tests and preliminary applications are exhibited to confirm our implementation and assess the effects of different treatment of environmental polarization on the excited-state properties, and the efficiency of parallel implementation is demonstrated as well. PMID:26450289

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

    NASA Astrophysics Data System (ADS)

    Okhrimenko, Albert N.

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

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

    NASA Technical Reports Server (NTRS)

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

    1973-01-01

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

  11. Excited electronic states of MnO4-: Challenges for wavefunction and density functional response theories

    NASA Astrophysics Data System (ADS)

    Almeida, Nuno M. S.; McKinlay, Russell G.; Paterson, Martin J.

    2015-01-01

    The lowest excited electronic states of the permanganate ion MnO4- are calculated using a hierarchy of coupled cluster response approaches, as well as time-dependent density functional theory. It is shown that while full linear response coupled cluster with singles and doubles (or higher) performs well, that permanganate represents a stern test for approximate coupled cluster response models, and that problems can be traced to very large orbital relaxation effects. TD-DFT is reasonably robust although errors around 0.6 eV are still observed. In order to further investigate the strong correlations prevalent in the electronic ground state large-scale RASSCF calculations were also performed. Again very large orbital relaxation in the correlated wavefunction is observed. Although the system can qualitatively be described by a single configuration, multi-reference diagnostic values show that care must be taken in this and similar metal complexes.

  12. Theory of ultrafast heterogeneous electron transfer: Contributions of direct charge transfer excitations to the absorbance

    NASA Astrophysics Data System (ADS)

    Wang, Luxia; Willig, Frank; May, Volkhard

    2007-04-01

    Absorption spectra related to heterogeneous electron transfer are analyzed with the focus on direct charge transfer transition from the surface attached molecule into the semiconductor band states. The computations are based on a model of reduced dimensionality with a single intramolecular vibrational coordinate but a complete account for the continuum of conduction band states. The applicability of this model to perylene on TiO2 has been demonstrated in a series of earlier papers. Here, based on a time-dependent formulation, the absorbance is calculated with the inclusion of charge transfer excitations. A broad parameter set inspired by the perylene TiO2 systems is considered. In particular, the description generalizes the Fano effect to heterogeneous electron transfer reactions. Preliminary simulations of measured spectra are presented for perylene-catechol attached to TiO2.

  13. Electron impact excitation of 5p states of rubidium at 20 eV incident energy

    NASA Astrophysics Data System (ADS)

    Hou Chin, Jia; Ratnavelu, Kuru; Zhou, Yajun

    2014-06-01

    The coupled-channel optical method (CCOM) is implemented in this work to study the scattering of electron on rubidium atom at 20 eV. In order to provide a realistic calculation, the continuum effect of the scattering system is accounted by incorporate an ab initio optical potential into the CCOM calculation. The differential cross sections (DCS), as well as the reduced Stokes parameters of 5p excitation are reported and compared to the available experimental and theoretical data. Contribution to the Topical Issue "Electron and Positron Induced Processes", edited by Michael Brunger, Radu Campeanu, Masamitsu Hoshino, Oddur Ingólfsson, Paulo Limão-Vieira, Nigel Mason, Yasuyuki Nagashima and Hajime Tanuma.

  14. Lifetimes of electronic excitations in unoccupied surface states and the image potential states on Pd(110)

    SciTech Connect

    Tsirkin, S. S. Eremeev, S. V.; Chulkov, E. V.

    2012-10-15

    The contribution of inelastic electron-electron scattering to the decay rate of excitations in the surface states and first two image potential states at the Y-bar point on the surface is calculated in the GW approximation, and the quasi-momentum dependence of the corresponding contribution for the surface states is analyzed. The mechanisms of electron scattering in these states are studied, and the temperature dependence of the excitation lifetime is analyzed with allowance for the contribution of the electron-phonon interaction calculated earlier.

  15. Differential cross sections for electron-impact vibrational-excitation of tetrahydrofuran at intermediate impact energies

    SciTech Connect

    Do, T. P. T.; Lopes, M. C. A.; Konovalov, D. A.; White, R. D.; Brunger, M. J. E-mail: darryl.jones@flinders.edu.au; Jones, D. B. E-mail: darryl.jones@flinders.edu.au

    2015-03-28

    We report differential cross sections (DCSs) for electron-impact vibrational-excitation of tetrahydrofuran, at intermediate incident electron energies (15-50 eV) and over the 10°-90° scattered electron angular range. These measurements extend the available DCS data for vibrational excitation for this species, which have previously been obtained at lower incident electron energies (≤20 eV). Where possible, our data are compared to the earlier measurements in the overlapping energy ranges. Here, quite good agreement was generally observed where the measurements overlapped.

  16. Electron-avalanche amplifier based on the electronic Venturi effect

    NASA Astrophysics Data System (ADS)

    Taubert, D.; Schinner, G. J.; Tranitz, H. P.; Wegscheider, W.; Tomaras, C.; Kehrein, S.; Ludwig, S.

    2010-10-01

    Scattering of otherwise ballistic electrons far from equilibrium is investigated in a cold two-dimensional electron system. The interaction between excited electrons and the degenerate Fermi liquid induces a positive charge in a nanoscale region which would be negatively charged for diffusive transport at local thermal equilibrium. In a three-terminal device we observe avalanche amplification of electrical current, resulting in a situation comparable to the Venturi effect in hydrodynamics. Numerical calculations using a random-phase approximation are in agreement with our data and suggest Coulomb interaction as the dominant scattering mechanism.

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

    NASA Technical Reports Server (NTRS)

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

    2002-01-01

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

  18. Electron-Photon Polarization Correlation Study of Neon, Argon and Krypton Excitation by Electron Impact

    NASA Astrophysics Data System (ADS)

    Zheng, Shuanghai

    1993-01-01

    The electron impact excitation of the 3s ^' (1/2) ^0_1 state in neon, the 4s^' (1/2) ^0_1 state in argon and the 5s (3/2) ^0_1 state in krypton have been studied using the electron-photon polarization correlation technique. The two linear coherence parameters P_1 and P_2 have been measured and the alignment angle gamma and the linear polarization P ^+_{rm lin} of the angular part of the collisionally induced excited state charge cloud were extracted from the measured P _1 and P_2 parameters. We measured P_1 and P_2 in neon at an impact energy of 50 eV, in argon at impact energies of 50 eV, 40 eV, 30 eV and 25 eV, and in krypton at impact energies of 50 eV and 30 eV and electron scattering angles up to 55^circ in all cases. A comparison with theoretical predictions from first-order perturbative theories such as a Distorted Wave Born Approximation (DWBA) and a First Order Many Body Theory (FOMBT) was made. At 50 eV in neon and argon, the agreement between experiment and theory is generally good at small scattering angles up to 25^circ and somewhat poorer at larger scattering angles. At 50 eV in krypton, the agreement between experiment and theory is generally good at scattering angles up to 40 ^circ. The measurements in argon (40 eV, 30 eV, and 25 eV) generally follow the trend of the theoretical predictions, but it was found that the experimentally measured coherence parameters appear to be shifted towards larger scattering angles compared to the theoretical predictions as the impact energy is decreased. At 30 eV in krypton, very good agreement between experiment and theory was found over the entire range of electron scattering angles (up to 55^circ). The level of agreement between experiment and theory indicates that the DWBA and FOMBT appear to provide a better description of the collision process for a more complex target. We also found that the alignment angle gamma is the parameter which is perhaps least sensitive to the details of the collision.

  19. Studies of metastable neon atoms produced by electron-beam excitation

    SciTech Connect

    Schulman, M.B.

    1988-01-01

    In the optical method, electron-excitation cross sections of radiative atomic or molecular levels are measured by absolutely calibrating the optical radiation emitted when the excited species are produced by electron-beam excitation of a high-purity gas sample, However, this method is not applicable to metastable (nonradiating) excited levels. With a continuous-wave dye-laser beam intersecting the electron beam, the metastable species produced can be pumped to a higher, radiative level. The intensity of the resulting laser-induced fluorescence from the higher level can be measured to obtain the excitation cross section for production of the metastable level. The absolute number density of the metastable species can be determined by a similar method which uses a pulsed dye laser. This work describes the application of the pulsed-laser technique to the investigation of several aspects of electron-beam excitation of neon atoms in a static gas sample to the metastable 1s{sub 5} (2p{sup 5}3s{sup 3}P{sub 2}) level. In addition to spatially resolved number-density measurements, the temporal disappearance of the metastables from the collision region has been investigated. In the first 50 {mu}s after a fast cutoff of the electron beam, the decay curve of the metastable density is close to a single exponential form, with a time constant of 20 {mu}s. The magnitude of the laser-induced fluorescence per unit electron-beam current has been studied as a function of electron energy and ground-state neon density. Attempts to measure the cross section for exciting form the metastable levels to the higher excited 2p{sub 9} level (2p{sup 5}3p, J = 3) are also described.

  20. Calculation of Ground State Rotational Populations for Kinetic Gas Homonuclear Diatomic Molecules including Electron-Impact Excitation and Wall Collisions

    SciTech Connect

    David R. Farley

    2010-08-19

    A model has been developed to calculate the ground-state rotational populations of homonuclear diatomic molecules in kinetic gases, including the effects of electron-impact excitation, wall collisions, and gas feed rate. The equations are exact within the accuracy of the cross sections used and of the assumed equilibrating effect of wall collisions. It is found that the inflow of feed gas and equilibrating wall collisions can significantly affect the rotational distribution in competition with non-equilibrating electron-impact effects. The resulting steady-state rotational distributions are generally Boltzmann for N≥3, with a rotational temperature between the wall and feed gas temperatures. The N=0,1,2 rotational level populations depend sensitively on the relative rates of electron-impact excitation versus wall collision and gas feed rates.

  1. Excitation and electron transfer from selectively excited primary donor chlorophyll (P700) in a photosystem I reaction center

    SciTech Connect

    Kumazaki, Shigeichi; Yoshihara, Keitaro; Ikegami, Isamu

    1997-01-23

    The primary processes in a photosystem I reaction center were studied by fluorescence up-conversion with a subpicosecond time resolution at room temperature. The samples were P700(primary donor chlorophyll)-enriched particles which retained {approx}14 chlorophylls per P700. Upon selective excitation of P700 at 701 nm at {approx}5{degree}C, anisotropy of the fluorescence at 749 nm decayed from {approx}0.3 to {approx}0.15 with a time constant of 1 ps. The dynamic depolarization is attributed to electronic excitation equilibration between P700 and the surrounding chlorophylls. In the isotropic fluorescence kinetics, at least two decaying components of 2.2 ps ({approx}35%) and 15 ps ({approx}55%) were found. The fast and slow components indicate the charge separation before and after full equilibration of excitation energy, respectively. A kinetic model calculation based on the above results suggests that the intrinsic rate constant of the primary electron transfer from P700{sup *} is > 0.25 ps{sup -1}. 51 refs., 4 figs., 1 tab.

  2. Contribution of electronic excitation to the structural evolution of ultrafast laser-irradiated tungsten nanofilms

    NASA Astrophysics Data System (ADS)

    Murphy, Samuel T.; Giret, Yvelin; Daraszewicz, Szymon L.; Lim, Anthony C.; Shluger, Alexander L.; Tanimura, Katsumi; Duffy, Dorothy M.

    2016-03-01

    The redistribution of the electron density in a material during laser irradiation can have a significant impact on its structural dynamics. This electronic excitation can be incorporated into two temperature molecular dynamics (2T-MD) simulations through the use of electronic temperature dependent potentials. Here, we study the structural dynamics of laser irradiated tungsten nanofilms using 2T-MD simulations with an electronic temperature dependent potential and compare the results to equivalent simulations that employ a ground-state interatomic potential. Electronic excitation leads to an expansion of the crystal and a decrease in the melting point of tungsten. During laser irradiation these factors ensure that the threshold fluences to the different melting regimes are reduced. Furthermore, both heterogenous and homogeneous melting are predicted to occur more rapidly due to excitation and oscillations in the film thickness will be accentuated.

  3. Back-action-induced excitation of electrons in a silicon quantum dot with a single-electron transistor charge sensor

    SciTech Connect

    Horibe, Kosuke; Oda, Shunri; Kodera, Tetsuo

    2015-02-02

    Back-action in the readout of quantum bits is an area that requires a great deal of attention in electron spin based-quantum bit architecture. We report here back-action measurements in a silicon device with quantum dots and a single-electron transistor (SET) charge sensor. We observe the back-action-induced excitation of electrons from the ground state to an excited state in a quantum dot. Our measurements and theoretical fitting to the data reveal conditions under which both suitable SET charge sensor sensitivity for qubit readout and low back-action-induced transition rates (less than 1 kHz) can be achieved.

  4. Helicon wave excitation to produce energetic electrons for manufacturing semiconductors

    DOEpatents

    Molvik, Arthur W.; Ellingboe, Albert R.

    1998-01-01

    A helicon plasma source is controlled by varying the axial magnetic field or rf power controlling the formation of the helicon wave. An energetic electron current is carried on the wave when the magnetic field is 90 G; but there is minimal energetic electron current when the magnetic field is 100 G in one particular plasma source. Similar performance can be expected from other helicon sources by properly adjusting the magnetic field and power to the particular geometry. This control for adjusting the production of energetic electrons can be used in the semiconductor and thin-film manufacture process. By applying energetic electrons to the insulator layer, such as silicon oxide, etching ions are attracted to the insulator layer and bombard the insulator layer at higher energy than areas that have not accumulated the energetic electrons. Thus, silicon and metal layers, which can neutralize the energetic electron currents will etch at a slower or non-existent rate. This procedure is especially advantageous in the multilayer semiconductor manufacturing because trenches can be formed that are in the range of 0.18-0.35 mm or less.

  5. Helicon wave excitation to produce energetic electrons for manufacturing semiconductors

    DOEpatents

    Molvik, A.W.; Ellingboe, A.R.

    1998-10-20

    A helicon plasma source is controlled by varying the axial magnetic field or rf power controlling the formation of the helicon wave. An energetic electron current is carried on the wave when the magnetic field is 90 G; but there is minimal energetic electron current when the magnetic field is 100 G in one particular plasma source. Similar performance can be expected from other helicon sources by properly adjusting the magnetic field and power to the particular geometry. This control for adjusting the production of energetic electrons can be used in the semiconductor and thin-film manufacture process. By applying energetic electrons to the insulator layer, such as silicon oxide, etching ions are attracted to the insulator layer and bombard the insulator layer at higher energy than areas that have not accumulated the energetic electrons. Thus, silicon and metal layers, which can neutralize the energetic electron currents will etch at a slower or non-existent rate. This procedure is especially advantageous in the multilayer semiconductor manufacturing because trenches can be formed that are in the range of 0.18--0.35 mm or less. 16 figs.

  6. An amorphous phase formation at palladium / silicon oxide (Pd/SiO{sub x}) interface through electron irradiation - electronic excitation process

    SciTech Connect

    Nagase, Takeshi; Yamashita, Ryo; Yabuuchi, Atsushi; Lee, Jung-Goo

    2015-11-15

    A Pd-Si amorphous phase was formed at a palladium/silicon oxide (Pd/SiO{sub x}) interface at room temperature by electron irradiation at acceleration voltages ranging between 25 kV and 200 kV. Solid-state amorphization was stimulated without the electron knock-on effects. The total dose required for the solid-state amorphization decreases with decreasing acceleration voltage. This is the first report on electron irradiation induced metallic amorphous formation caused by the electronic excitation at metal/silicon oxide interface.

  7. Determination of the geometry change of benzimidazole upon electronic excitation from a combined Franck-Condon/rotational constants fit

    NASA Astrophysics Data System (ADS)

    Stuhlmann, Benjamin; Gmerek, Felix; Krügler, Daniel; Schmitt, Michael

    2014-08-01

    Single vibronic level fluorescence spectra of the electronic origin and of seven vibronic bands between 0,0 and 0,0 + 1265 cm-1 have been measured and analyzed by means of a combined Franck-Condon/rotational constants fit. The rotational constants in ground and lowest electronically excited singlet state of four different isotopologues have been taken from previous rotationally resolved measurements of Schmitt et al. (2006). The intensities of 182 vibronic emission bands and of 8 rotational constants have been used for a fit of the complete heavy atom geometry changes upon electronic excitation. Vibronic modes, about 1000 cm-1 above the electronic origin, show strong deviations from Franck-Condon behavior in emission. Herzberg-Teller coupling contributes to this effect. 1300 cm-1 above the origin, we observe the onset of intramolecular vibrational redistribution in the emission spectra.

  8. The relativistic polarization propagator for the calculation of electronic excitations in heavy systems

    SciTech Connect

    Pernpointner, Markus

    2014-02-28

    In this work, we present a new four-component implementation of the polarization propagator for accurate calculations of excited states in heavy systems. Differences to existing nonrelativistic realizations are detailed and the energetically lowest final states of the ns{sup 2}np{sup 6} → ns{sup 2}np{sup 5}(n + 1)s{sup 1} and ns{sup 2}np{sup 6} → ns{sup 2}np{sup 5}(n + 1)p{sup 1} transitions in noble gases are calculated and compared with experimental data. Already for the light atoms Ne and Ar spin-orbit coupling leads to noticeable zero field splitting that gradually increases in the heavier homologues and eventually invalidates the LS-based description of singlet and triplet excited states. For all four noble gases Ne through Xe, we observe a very good agreement with experimental transition energies in the considered energetic range where the extended version of the propagator implementation in general yields better excitation energy differences than the strict variant. In the extended version, off-diagonal first-order contributions in the two-particle-two-hole block are included that are not present in the strict variant. In case of Kr and Xe, nonrelativistic approaches already exhibit unacceptable deviations in the reproduction of transition energies and the spectral structure. The obtained excited final states are analyzed in terms of atomic contributions to the donor and acceptor orbitals constituting the corresponding wave functions. The relativistic polarization propagator provides a consistent description of electron correlation and relativistic effects especially relevant for the heavier systems where these two contributions are no longer separable.

  9. Electron-impact excitation of neon: a pseudo-state convergence study

    NASA Astrophysics Data System (ADS)

    Ballance, C. P.; Griffin, D. C.

    2004-07-01

    A number of convergent close-coupling and R-matrix with pseudo-state (RMPS) calculations for H-like, He-like, Li-like and Be-like ions have demonstrated that coupling to the target continuum can have large effects on the electron-impact excitation cross sections of neutral and low-charge species. However, no one has yet attempted such advanced calculations on a system as complex as neutral neon. We report on a series of RMPS calculations of electron-impact excitation of Ne using recently developed parallel Breit-Pauli R-matrix programs. Our largest calculation included 235 spectroscopic and pseudo-state levels in the close-coupling expansion of the target. Although the results clearly reveal the importance of coupling to the target continuum in this atom, the pseudo-state expansion is not yet sufficiently complete to provide reliable cross sections for energies above the ionization limit. However, this is the largest intermediate-coupling calculation that can be performed with present computer resources. Thus, we have also carried out a series of RMPS calculations in LS coupling with different pseudo-state expansions. Comparisons of these results have allowed us to determine the approximate size of the pseudo-state expansion required to achieve convergence in future intermediate-coupling calculations for neon.

  10. New tools for the systematic analysis and visualization of electronic excitations. I. Formalism

    SciTech Connect

    Plasser, Felix Wormit, Michael; Dreuw, Andreas

    2014-07-14

    A variety of density matrix based methods for the analysis and visualization of electronic excitations are discussed and their implementation within the framework of the algebraic diagrammatic construction of the polarization propagator is reported. Their mathematical expressions are given and an extensive phenomenological discussion is provided to aid the interpretation of the results. Starting from several standard procedures, e.g., population analysis, natural orbital decomposition, and density plotting, we proceed to more advanced concepts of natural transition orbitals and attachment/detachment densities. In addition, special focus is laid on information coded in the transition density matrix and its phenomenological analysis in terms of an electron-hole picture. Taking advantage of both the orbital and real space representations of the density matrices, the physical information in these analysis methods is outlined, and similarities and differences between the approaches are highlighted. Moreover, new analysis tools for excited states are introduced including state averaged natural transition orbitals, which give a compact description of a number of states simultaneously, and natural difference orbitals (defined as the eigenvectors of the difference density matrix), which reveal details about orbital relaxation effects.

  11. Imaging Electronic Excitation of NO by Ultrafast Laser Tunneling Ionization.

    PubMed

    Endo, Tomoyuki; Matsuda, Akitaka; Fushitani, Mizuho; Yasuike, Tomokazu; Tolstikhin, Oleg I; Morishita, Toru; Hishikawa, Akiyoshi

    2016-04-22

    Tunneling-ionization imaging of photoexcitation of NO has been demonstrated by using few-cycle near-infrared intense laser pulses (8 fs, 800 nm, 1.1×10^{14}  W/cm^{2}). The ion image of N^{+} fragment ions produced by dissociative ionization of NO in the ground state, NO (X^{2}Π,2π)→NO^{+}+e^{-}→N^{+}+O+e^{-}, exhibits a characteristic momentum distribution peaked at 45° with respect to the laser polarization direction. On the other hand, a broad distribution centered at ∼0° appears when the A^{2}Σ^{+} (3sσ) excited state is prepared as the initial state by deep-UV photoexcitation. The observed angular distributions are in good agreement with the corresponding theoretical tunneling ionization yields, showing that the fragment anisotropy reflects changes of the highest-occupied molecular orbital by photoexcitation. PMID:27152798

  12. Imaging Electronic Excitation of NO by Ultrafast Laser Tunneling Ionization

    NASA Astrophysics Data System (ADS)

    Endo, Tomoyuki; Matsuda, Akitaka; Fushitani, Mizuho; Yasuike, Tomokazu; Tolstikhin, Oleg I.; Morishita, Toru; Hishikawa, Akiyoshi

    2016-04-01

    Tunneling-ionization imaging of photoexcitation of NO has been demonstrated by using few-cycle near-infrared intense laser pulses (8 fs, 800 nm, 1.1 ×1014 W /cm2 ). The ion image of N+ fragment ions produced by dissociative ionization of NO in the ground state, NO (X2Π ,2 π )→NO+ +e-→N+ +O +e- , exhibits a characteristic momentum distribution peaked at 45° with respect to the laser polarization direction. On the other hand, a broad distribution centered at ˜0 ° appears when the A2Σ+ (3 s σ ) excited state is prepared as the initial state by deep-UV photoexcitation. The observed angular distributions are in good agreement with the corresponding theoretical tunneling ionization yields, showing that the fragment anisotropy reflects changes of the highest-occupied molecular orbital by photoexcitation.

  13. Effects of abnormal excitation on the dynamics of spiral waves

    NASA Astrophysics Data System (ADS)

    Min-Yi, Deng; Xue-Liang, Zhang; Jing-Yu, Dai

    2016-01-01

    The effect of physiological and pathological abnormal excitation of a myocyte on the spiral waves is investigated based on the cellular automaton model. When the excitability of the medium is high enough, the physiological abnormal excitation causes the spiral wave to meander irregularly and slowly. When the excitability of the medium is low enough, the physiological abnormal excitation leads to a new stable spiral wave. On the other hand, the pathological abnormal excitation destroys the spiral wave and results in the spatiotemporal chaos, which agrees with the clinical conclusion that the early after depolarization is the pro-arrhythmic mechanism of some anti-arrhythmic drugs. The mechanisms underlying these phenomena are analyzed. Project supported by the National Natural Science Foundation of China (Grant Nos. 11365003 and 11165004).

  14. Exploring the vibrational fingerprint of the electronic excitation energy via molecular dynamics

    SciTech Connect

    Deyne, Andy Van Yperen-De; Pauwels, Ewald; Ghysels, An; Waroquier, Michel; Van Speybroeck, Veronique; Hemelsoet, Karen; De Meyer, Thierry; De Clerck, Karen

    2014-04-07

    A Fourier-based method is presented to relate changes of the molecular structure during a molecular dynamics simulation with fluctuations in the electronic excitation energy. The method implies sampling of the ground state potential energy surface. Subsequently, the power spectrum of the velocities is compared with the power spectrum of the excitation energy computed using time-dependent density functional theory. Peaks in both spectra are compared, and motions exhibiting a linear or quadratic behavior can be distinguished. The quadratically active motions are mainly responsible for the changes in the excitation energy and hence cause shifts between the dynamic and static values of the spectral property. Moreover, information about the potential energy surface of various excited states can be obtained. The procedure is illustrated with three case studies. The first electronic excitation is explored in detail and dominant vibrational motions responsible for changes in the excitation energy are identified for ethylene, biphenyl, and hexamethylbenzene. The proposed method is also extended to other low-energy excitations. Finally, the vibrational fingerprint of the excitation energy of a more complex molecule, in particular the azo dye ethyl orange in a water environment, is analyzed.

  15. Semiempirical Quantum-Chemical Orthogonalization-Corrected Methods: Benchmarks of Electronically Excited States.

    PubMed

    Tuna, Deniz; Lu, You; Koslowski, Axel; Thiel, Walter

    2016-09-13

    The semiempirical orthogonalization-corrected OMx methods have recently been shown to perform well in extensive ground-state benchmarks. They can also be applied to the computation of electronically excited states when combined with a suitable multireference configuration interaction (MRCI) treatment. We report on a comprehensive evaluation of the performance of the OMx/MRCI methods for electronically excited states. The present benchmarks cover vertical excitation energies, excited-state equilibrium geometries (including an analysis of significant changes between ground- and excited-state geometries), minimum-energy conical intersections, ground- and excited-state zero-point vibrational energies, and 0-0 transition energies for a total of 520 molecular structures and 412 excited states. For comparison, we evaluate the TDDFT/B3LYP method for all benchmark sets, and the CC2, MRCISD, and CASPT2 methods for some of them. We find that the current OMx/MRCI methods perform reasonably well for many of the excited-state properties. However, in comparison to the first-principles methods, there are also a number of shortcomings that should be addressed in future developments. PMID:27380455

  16. Low-lying electronic excited states of pentacene oligomers: a comparative electronic structure study in the context of singlet fission.

    PubMed

    Coto, Pedro B; Sharifzadeh, Sahar; Neaton, Jeffrey B; Thoss, Michael

    2015-01-13

    The lowest-lying electronic excited states of pentacene and its oligomers are investigated using accurate multireference wave function methods (CASPT2/CASSCF) and the many-body Greens's function approach (GW/BSE). The results obtained for dimers and trimers of different geometry reveal a complex electronic structure, which includes locally excited, charge transfer, and multiexciton states. For singlets of single-excitation character, both approaches yield excitation energies that are in good overall quantitative agreement. While the multiexciton states are located relatively high in energy in all systems investigated, charge transfer states exist in close proximity to the lowest-lying absorbing states. The implications of the results for the mechanisms of singlet fission in pentacene are discussed. PMID:26574213

  17. Double-hybrid density functional theory for excited electronic states of molecules

    NASA Astrophysics Data System (ADS)

    Grimme, Stefan; Neese, Frank

    2007-10-01

    Double-hybrid density functionals are based on a mixing of standard generalized gradient approximations (GGAs) for exchange and correlation with Hartree-Fock (HF) exchange and a perturbative second-order correlation part (PT2) that is obtained from the Kohn-Sham (GGA) orbitals and eigenvalues. This virtual orbital-dependent functional (dubbed B2PLYP) contains only two empirical parameters that describe the mixture of HF and GGA exchange (ax) and of the PT2 and GGA correlation (ac), respectively. Extensive testing has recently demonstrated the outstanding accuracy of this approach for various ground state problems in general chemistry applications. The method is extended here without any further empirical adjustments to electronically excited states in the framework of time-dependent density functional theory (TD-DFT) or the closely related Tamm-Dancoff approximation (TDA-DFT). In complete analogy to the ground state treatment, a scaled second-order perturbation correction to configuration interaction with singles (CIS(D)) wave functions developed some years ago by Head-Gordon et al. [Chem. Phys. Lett. 219, 21 (1994)] is computed on the basis of density functional data and added to the TD(A)-DFT/GGA excitation energy. The method is implemented by applying the resolution of the identity approximation and the efficiency of the code is discussed. Extensive tests for a wide variety of molecules and excited states (of singlet, triplet, and doublet multiplicities) including electronic spectra are presented. In general, rather accurate excitation energies (deviations from reference data typically <0.2eV) are obtained that are mostly better than those from standard functionals. Still, systematic errors are obtained for Rydberg (too low on average by about 0.3eV) and charge-transfer transitions but due to the relatively large ax parameter (0.53), B2PLYP outperforms most other functionals in this respect. Compared to conventional HF-based CIS(D), the method is more robust in

  18. A steadying effect of acoustic excitation on transitory stall

    NASA Technical Reports Server (NTRS)

    Zaman, K. B. M. Q.

    1991-01-01

    The effect of acoustic excitation on a class of separated flows with a transitional boundary layer at the point of separation is considered. Experimental results on the flow over airfoils, a two-dimensional backward-facing step, and through large angle conical diffusers are presented. In all cases, the separated flow undergoes large amplitude fluctuations, much of the energy being concentrated at unusually low frequencies. In each case, an appropriate high frequency acoustic excitation is found to be effective in reducing the fluctuations substantially. The effective excitation frequency scales on the initial boundary layer thickness and the effect is apparently achieved through acoustic tripping of the separating boundary layer.

  19. Electron Exciter Speeds Associated with Interplanetary Type III Solar Radio Bursts

    NASA Astrophysics Data System (ADS)

    Reiner, M. J.; MacDowall, R. J.

    2015-10-01

    This article provides a comprehensive quantitative investigation of the kinematics of the electron exciters associated with interplanetary type III solar radio bursts. Detailed multispacecraft analyses of the radio and plasma wave data from the widely separated Wind and STEREO spacecraft are provided for five interplanetary type III bursts that illustrate different aspects of the problems involved in establishing the electron exciter speeds. The exciter kinematics are determined from the observed frequency drift and in-situ radiation characteristics for each type III burst. The analysis assumes propagation of the electron exciters along a Parker spiral, with origin at the associated solar active region, and curvature determined by the measured solar wind speed. The analyses take fully into account the appropriate light-propagation-time corrections from the radio source to the observing spacecraft as the exciters propagate along the Parker spiral path. For the five in-situ type III bursts analyzed in detail here, we found that their initial exciter speeds, near the Sun, ranged from 0.2c to 0.38c, where c is the speed of light. This is significantly higher than the exciter speeds derived from other recent analyses. The results presented here further suggest that the type III electron exciters normally decelerate as they propagate through the interplanetary medium. We argue based on the observations by the widely separated spacecraft that the initial part of the type III radiation usually occurs at the fundamental of the plasma frequency. Finally, we compare the results for the exciter speeds to all previous determinations and provide quantitative arguments to explain the differences.

  20. Beat wave excitation of electron plasma wave by relativistic cross focusing of cosh-Gaussian laser beams in plasma

    NASA Astrophysics Data System (ADS)

    Singh, Arvinder; Gupta, Naveen

    2015-06-01

    A scheme for beat wave excitation of electron plasma wave (EPW) is proposed by relativistic cross-focusing of two coaxial Cosh-Gaussian (ChG) laser beams in an under dense plasma. The plasma wave is generated on account of beating of two coaxial laser beams of frequencies ω1 and ω2 . The mechanism for laser produced nonlinearity is assumed to be relativistic nonlinearity in electron mass. Following moment theory approach in Wentzel Kramers Brillouin (W.K.B) approximation, the coupled differential equations governing the evolution of spot size of laser beams with distance of propagation have been derived. The relativistic nonlinearity depends not only on the intensity of first laser beam but also on the intensity of second laser beam. Therefore, propagation dynamics of one laser beam affect that of second beam and hence cross-focusing of the two laser beams takes place. Due to non uniform intensity distribution of pump laser beams, the background electron concentration gets modified. The amplitude of EPW, which depends on the background electron concentration, thus gets nonlinearly coupled with the laser beams. The effects of relativistic electron mass nonlinearity and the cross-focusing of pump beams on excitation of EPW have been incorporated. Numerical simulations have been carried out to investigate the effect of laser as well as plasma parameters on cross-focusing of laser beams and further its effect on power of excited EPW.

  1. Measurements of electron excitation and recombination for Ne-like Ba/sup 46 +/

    SciTech Connect

    Marrs, R.E.; Levine, M.A.; Knapp, D.A.; Henderson, J.R.

    1987-07-01

    A new facility at Lawrence Livermore National Laboratory has been used to obtain measurements for electron-impact excitation, dielectronic recombination and radiative recombination for the neon-like Ba/sup 46 +/ ion. The experimental technique consists of trapping highly charged ions inside the space charge of an electron beam and measuring their x-ray emission spectra.

  2. Electron heating via self-excited plasma series resonance in geometrically symmetric multi-frequency capacitive plasmas

    NASA Astrophysics Data System (ADS)

    Schüngel, E.; Brandt, S.; Donkó, Z.; Korolov, I.; Derzsi, A.; Schulze, J.

    2015-08-01

    The self-excitation of plasma series resonance (PSR) oscillations plays an important role in the electron heating dynamics in capacitively coupled radio-frequency (CCRF) plasmas. In a combined approach of PIC/MCC simulations and a theoretical model based on an equivalent circuit, we investigate the self-excitation of PSR oscillations and their effect on the electron heating in geometrically symmetric CCRF plasmas driven by multiple consecutive harmonics. The discharge symmetry is controlled via the electrical asymmetry effect (EAE), i.e. by varying the total number of harmonics and tuning the phase shifts between them. It is demonstrated that PSR oscillations will be self-excited under both symmetric and asymmetric conditions, if (i) the charge-voltage relation of the plasma sheaths deviates from a simple quadratic behavior and (ii) the inductance of the plasma bulk exhibits a temporal modulation. These two effects have been neglected up to now, but we show that they must be included in the model in order to properly describe the nonlinear series resonance circuit and reproduce the self-excitation of PSR oscillations, which are observed in the electron current density resulting from simulations of geometrically symmetric CCRF plasmas. Furthermore, the effect of PSR self-excitation on the discharge current and the plasma properties, such as the potential profile, is illustrated by applying Fourier analysis. High-frequency oscillations in the entire spectrum between the applied frequencies and the local electron plasma frequency are observed. As a consequence, the electron heating is strongly enhanced by the presence of PSR oscillations. A complex electron heating dynamics is found during the expansion phase of the sheath, which is fully collapsed, when the PSR is initially self-excited. The nonlinear electron resonance heating (NERH) associated with the PSR oscillations causes a spatial asymmetry in the electron heating. By discussing the resulting ionization

  3. Electron Spectroscopy: Ultraviolet and X-Ray Excitation.

    ERIC Educational Resources Information Center

    Baker, A. D.; And Others

    1980-01-01

    Reviews recent growth in electron spectroscopy (54 papers cited). Emphasizes advances in instrumentation and interpretation (52); photoionization, cross-sections and angular distributions (22); studies of atoms and small molecules (35); transition, lanthanide and actinide metal complexes (50); organometallic (12) and inorganic compounds (2);…

  4. Measurements of Electron Impact Excitation Cross Sections at the Harvard-Smithsonian Center for Astrophysics

    NASA Technical Reports Server (NTRS)

    Gardner, L. D.; Kohl, J. L.

    2006-01-01

    The analysis of absolute spectral line intensities and intensity ratios with spectroscopic diagnostic techniques provides empirical determinations of chemical abundances, electron densities and temperatures in astrophysical objects. Since spectral line intensities and their ratios are controlled by the excitation rate coefficients for the electron temperature of the observed astrophysical structure, it is imperative that one have accurate values for the relevant rate coefficients. Here at the Harvard-Smithsonian Center for Astrophysics, we have been carrying out measurements of electron impact excitation (EIE) for more than 25 years.

  5. Study of intermediates from transition metal excited-state electron-transfer reactions

    SciTech Connect

    Hoffman, M.Z.

    1992-07-31

    Conventional and fast-kinetics techniques of photochemistry, photophysics, radiation chemistry, and electrochemistry were used to study the intermediates involved in transition metal excited-state electron-transfer reactions. These intermediates were excited state of Ru(II) and Cr(III) photosensitizers, their reduced forms, and species formed in reactions of redox quenchers and electron-transfer agents. Of particular concern was the back electron-transfer reaction between the geminate pair formed in the redox quenching of the photosensitizers, and the dependence of its rate on solution medium and temperature in competition with transformation and cage escape processes. (DLC)

  6. Excitation of the ligand-to-metal charge transfer band induces electron tunnelling in azurin

    SciTech Connect

    Baldacchini, Chiara; Bizzarri, Anna Rita; Cannistraro, Salvatore

    2014-03-03

    Optical excitation of azurin blue copper protein immobilized on indium-tin oxide, in resonance with its ligand-to-metal charge transfer absorption band, resulted in a light-induced current tunnelling within the protein milieu. The related electron transport rate is estimated to be about 10{sup 5} s{sup −1}. A model based on resonant tunnelling through an azurin excited molecular state is proposed. The capability of controlling electron transfer processes through light pulses opens interesting perspectives for implementation of azurin in bio-nano-opto-electronic devices.

  7. 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 on CO2. Absolute emission cross sections for these multiplets were measured from threshold to 350 eV. The electrostatically focused electron gun used is described in detail. The atomic multiplets which were produced by dissociative excitation of CO2 and the cross sections at 100 eV are presented. The dependence of the excitation functions on electron energy shows that these multiplets are produced by electric-dipole-allowed transitions in CO2.

  8. Persistent order due to transiently enhanced nesting in an electronically excited charge density wave

    DOE PAGESBeta

    Rettig, L.; Cortés, R.; Chu, J. -H.; Fisher, I. R.; Schmitt, F.; Moore, R. G.; Shen, Z. -X.; Kirchmann, P. S.; Wolf, M.; Bovensiepen, U.

    2016-01-25

    Non-equilibrium conditions may lead to novel properties of materials with broken symmetry ground states not accessible in equilibrium as vividly demonstrated by non-linearly driven mid-infrared active phonon excitation. Potential energy surfaces of electronically excited states also allow to direct nuclear motion, but relaxation of the excess energy typically excites fluctuations leading to a reduced or even vanishing order parameter as characterized by an electronic energy gap. Here, using femtosecond time-and angle-resolved photoemission spectroscopy, we demonstrate a tendency towards transient stabilization of a charge density wave after near-infrared excitation, counteracting the suppression of order in the non-equilibrium state. Analysis of themore » dynamic electronic structure reveals a remaining energy gap in a highly excited transient state. In conclusion, our observation can be explained by a competition between fluctuations in the electronically excited state, which tend to reduce order, and transiently enhanced Fermi surface nesting stabilizing the order.« less

  9. Low-energy electron elastic scattering cross sections for excited Au and Pt atoms

    NASA Astrophysics Data System (ADS)

    Felfli, Zineb; Eure, Amanda R.; Msezane, Alfred Z.; Sokolovski, Dmitri

    2010-05-01

    Electron elastic total cross sections (TCSs) and differential cross sections (DCSs) in both impact energy and scattering angle for the excited Au and Pt atoms are calculated in the electron impact energy range 0 ⩽ E ⩽ 4.0 eV. The cross sections are found to be characterized by very sharp long-lived resonances whose positions are identified with the binding energies of the excited anions formed during the collisions. The recent novel Regge-pole methodology wherein is embedded through the Mulholland formula the electron-electron correlations is used together with a Thomas-Fermi type potential incorporating the crucial core-polarization interaction for the calculations of the TCSs. The DCSs are evaluated using a partial wave expansion. The Ramsauer-Townsend minima, the shape resonances and the binding energies of the excited Au - and Pt - anions are extracted from the cross sections, while the critical minima are determined from the DCSs.

  10. Ultrafast Electron Dynamics in Gold in the Presence of Laser Excited Surface Plasma Waves

    SciTech Connect

    Raynaud, M.

    2010-02-02

    Surface plasmon excitation with ultrashort intense laser pulses enhances efficiently laser absorption in metals and creates local high fields and non-equilibrium hot electrons population that have attractivity for numerous applications such as the development of intense sources of high-energy particles or photons and in the fast ignitor scheme in the framework of inertial fusion. In this context, the knowledge of the dynamics of relaxation of the collective electrons behavior is of importance. Using gold grating, we have investigated electrons relaxation in the presence of laser excited surface plasmon waves using a multiple-wavelengh femtosecond pump-probe technique. The results yield evidence of longer relaxation time in the presence of the collective excitation than that of individual electronic states.

  11. Electronic excitation induced amorphization in titanate pyrochlores: an ab initio molecular dynamics study

    DOE PAGESBeta

    Xiao, Haiyan Y.; Weber, William J.; Zhang, Yanwen; Zu, X. T.; Li, Sean

    2015-02-09

    In this study, the response of titanate pyrochlores (A2Ti2O7, A = Y, Gd and Sm) to electronic excitation is investigated utilizing an ab initio molecular dynamics method. All the titanate pyrochlores are found to undergo a crystalline-to-amorphous structural transition under a low concentration of electronic excitations. The transition temperature at which structural amorphization starts to occur depends on the concentration of electronic excitations. During the structural transition, O2-like molecules are formed, and this anion disorder further drives cation disorder that leads to an amorphous state. This study provides new insights into the mechanisms of amorphization in titanate pyrochlores under laser,more » electron and ion irradiations.« less

  12. Apparatus for measuring electron-impact excitation cross sections using fast metastable atoms produced via charge exchange

    SciTech Connect

    Boffard, J.B.; Lagus, M.E.; Anderson, L.W.; Lin, C.C.

    1996-08-01

    An apparatus for measuring absolute cross sections due to electron-impact excitation out of the metastable levels of rare-gas atoms via the optical method is described with the focus specifically on excitation out of the 2{sup 3}{ital S} metastable helium level. The metastable helium target (He{asterisk}) is prepared by charge exchange between 1.6 keV He{sup +} ions and cesium vapor. An electron beam crosses the fast metastable beam target at a right angle and the fluorescence is collected at right angles to both beams. The charge transfer reaction produces He atoms mainly in the {ital n}=2 He levels. Because the target contains a negligible ground state He fraction, we can measure excitation cross sections from excitation threshold up to an arbitrarily high energy (keV regime) which represents a major improvement over previous metastable excitation cross sections measurements. The He{asterisk} target density is extremely small ({approximately}10{sup 6} atoms/cm{sup 3}) yielding minuscule signal rates. We describe steps taken to maximize the signal-to-noise ratio. We discuss the implications of using a fast beam target including both the finite flight time of the excited atoms across the light gathering region and the reduction of the cascade contributions to the apparent cross sections. A discussion of the identification and elimination of various systematic effects is also given. To measure absolute cross sections, we explicitly determine the spatial distributions of both the electron and metastable beams, as well as the spatially dependent response of the fluorescence gathering region. We determine the absolute flux of fast metastable atoms using a thermal detector calibrated with a He{sup +} ion beam. As examples, we present absolute cross sections for excitation out of the 2{sup 3}{ital S} metastable level into the 3{sup 3}{ital D} and 4{sup 3}{ital D} levels. {copyright} {ital 1996 American Institute of Physics.}

  13. Final Technical Report [Scalable methods for electronic excitations and optical responses of nanostructures: mathematics to algorithms to observables

    SciTech Connect

    Saad, Yousef

    2014-03-19

    The master project under which this work is funded had as its main objective to develop computational methods for modeling electronic excited-state and optical properties of various nanostructures. The specific goals of the computer science group were primarily to develop effective numerical algorithms in Density Functional Theory (DFT) and Time Dependent Density Functional Theory (TDDFT). There were essentially four distinct stated objectives. The first objective was to study and develop effective numerical algorithms for solving large eigenvalue problems such as those that arise in Density Functional Theory (DFT) methods. The second objective was to explore so-called linear scaling methods or Methods that avoid diagonalization. The third was to develop effective approaches for Time-Dependent DFT (TDDFT). Our fourth and final objective was to examine effective solution strategies for other problems in electronic excitations, such as the GW/Bethe-Salpeter method, and quantum transport problems.

  14. Scalable Methods for Electronic Excitations and Optical Responses of Nanostructures: Mathematics to Algorithms to Observables

    SciTech Connect

    Carter, Emily A

    2013-02-02

    Kohn-Sham density functional theory (DFT) is a powerful, well-established tool for the study of condensed phase electronic structure. However, there are still a number of situations where its applicability is limited. The basic theme of our research is the development of first principles electronic structure approaches for condensed matter that goes beyond what can currently be done with standard implementations ofKohn-Sham DFT. Our efforts to this end have focused on two classes or' methods. The first addresses the well-lmown inability of DFT to handle strong, many-body electron correlation effects. Our approach is a DFT -based embedding theory, to treat localized features (e.g. impurity, adsorbate, vacancy, etc.) embedded in a periodic, metallic crystal. A description for the embedded region is provided by explicitly correlated, ab initio wave function methods. DFT, as a fo1n1ally ground state theory, does not give a good description of excited states; an additional feature of our approach is the ability to obtain excitations localized in this region. We apply our method to a first-principles study of the adsorption of a single magnetic Co ada tom on non-magnetic Cu( 111 ), a known Kondo system whose behavior is governed by strong electron correlation. The second class of methods that we are developing is an orbital-free density functional theory (OFDFT), which addresses the speed limitations ofKohn-Sham DFT. OFDFT is a powerful, O(N) scaling method for electronic structure calculations. Unlike Kohn-Sham DFT, OFDFT goes back to the original Hohenberg-Kohn idea of directly optimizing an energy functional which is an explicit functional of the density, without invoking an orbital description. This eliminates the need to manipulate orbitals, which leads to O(N{sup 3}) scaling in the Kahn-Sham approach. The speed of OFDFT allows direct electronic structure calculations on large systems on the order of thousands to tens of thousands of atoms, an expensive feat within

  15. Comparison of coupled-cluster methods which include the effects of connected triple excitations

    NASA Technical Reports Server (NTRS)

    Scuseria, Gustavo E.; Lee, Timothy J.

    1990-01-01

    The 'coupled cluster single, double, and triple' (CCSDT) excitation model has been used to ascertain electron correlation energies for 14 different molecules representing a variety of chemical bonds, in conjunction with several methods of this type 'CCSDT-x', which include only an approximate treatment of connected triple excitations; these methods encompass CCSDT-1a, -1b, -2, -3, and -4, as well as the novel CCSD(T). While all methods treat the effects of connected triple excitations iteratively, CCSD(T) approaches then perturbationally. For the 14 molecules considered, the CCSD(T) method's average error relative to CCSDT is substantially lower than any of the CCSDT-x methods.

  16. Electron impact excitation of autoionising states of krypton

    NASA Technical Reports Server (NTRS)

    Srivastava, S. K.; Trajmar, S.

    1978-01-01

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

  17. Spectroscopy of Argon Excited in an Electron Beam Ion Trap

    SciTech Connect

    Trabert, E

    2005-04-18

    Argon is one of the gases best investigated and most widely used in plasma discharge devices for a multitude of applications that range from wavelength reference standards to controlled fusion experiments. Reviewing atomic physics and spectroscopic problems in various ionization stages of Ar, the past use and future options of employing an electron beam ion trap (EBIT) for better and more complete Ar data in the x-ray, EUV and visible spectral ranges are discussed.

  18. Absolute angle-differential vibrational excitation cross sections for electron collisions with diacetylene

    SciTech Connect

    Allan, M.; May, O.; Fedor, J.; Ibanescu, B. C.; Andric, L.

    2011-05-15

    Absolute vibrational excitation cross sections were measured for diacetylene (1,3-butadiyne). The selectivity of vibrational excitation reveals detailed information about the shape resonances. Excitation of the C{identical_to}C stretch and of double quanta of the C-H bend vibrations reveals a {sup 2}{Pi}{sub u} resonance at 1 eV (autodetachment width {approx}30 meV) and a {sup 2}{Pi}{sub g} resonance at 6.2 eV (autodetachment width 1-2 eV). There is a strong preference for excitation of even quanta of the bending vibration. Excitation of the C-H stretch vibration reveals {sigma}* resonances at 4.3, 6.8, and 9.8 eV, with autodetachment widths of {approx}2 eV. Detailed information about resonances permits conclusions about the mechanism of the dissociative electron attachment.

  19. Anisotropic softening of magnetic excitations in lightly electron-doped Sr2IrO4

    DOE PAGESBeta

    Liu, X.; Dean, M. P. M.; Meng, Z. Y.; Upton, M. H.; Qi, T.; Gog, T.; Cao, Y.; Lin, J. Q.; Meyers, D.; Ding, H.; et al

    2016-06-10

    The magnetic excitations in electron doped (Sr1-xLax)2IrO4 with x = 0:03 were measured using resonant inelastic X-ray scattering at the Ir L3-edge. Although much broadened, well defined dispersive magnetic excitations were observed. Comparing with the magnetic dispersion from the undoped compound, the evolution of the magnetic excitations upon doping is highly anisotropic. Along the anti-nodal direction, the dispersion is almost intact. On the other hand, the magnetic excitations along the nodal direction show significant softening. These results establish the presence of strong magnetic correlations in electron doped (Sr1-xLax)2IrO4 with close analogies to the hole doped cuprates, further motivating the searchmore » for high temperature superconductivity in this system.« less

  20. Theoretical evaluation of electron-beam-excited vacuum-ultraviolet F2 lasers

    NASA Astrophysics Data System (ADS)

    Kim, Y.-P.; Obara, M.; Suzuki, T.

    1986-03-01

    A theoretical kinetic model for an electron-beam-excited F2 laser (157 nm) was successfully developed to evaluate the performance characteristics in terms of electron-beam excitation rate, pumping pulse width, and total operating pressure. As a result, it is made clear that a high excitation rate (above 0.2 MW/cu cm atm) is essential to obtain efficient laser operation. An intrinsic laser efficiency of 4.3 percent is obtainable when a 6.5-atm mixture of He-F2 = 1000/1 is pumped at an excitation rate of 0.5 MW/cu cm atm, giving a laser output of over 4 J/l. It is also found that a higher laser output is obtainable with increasing total operating pressure, while the intrinsic laser efficiency slowly decreases.

  1. Avoiding entanglement loss when two-qubit quantum gates are controlled by electronic excitation

    NASA Astrophysics Data System (ADS)

    Rodriquez, R.; Fisher, A. J.; Greenland, P. T.; Stoneham, A. M.

    2004-04-01

    A solid-state two-qubit quantum gate was recently proposed that might be made in a silicon fabrication plant in the near future. In this class of device, entanglement between two quantum bits is controlled by a change from a largely unentangled ground electronic state to an excited state in which useful entanglement can be produced. Such gates have potential advantages, both because they exploit known solid-state behaviour and they separate the storage and manipulation of quantum information. It is important that the excitation step does not create decoherence. We analyse a type of gate proposed before, in which the excitation involves a control electron that interacts with the qubit spins in the excited state. The dynamics of an idealized (but fairly general) gate of this type show that it can be operated to produce a standard two-qubit entangling state.

  2. Anisotropic softening of magnetic excitations in lightly electron-doped Sr2IrO4

    NASA Astrophysics Data System (ADS)

    Liu, X.; Dean, M. P. M.; Meng, Z. Y.; Upton, M. H.; Qi, T.; Gog, T.; Cao, Y.; Lin, J. Q.; Meyers, D.; Ding, H.; Cao, G.; Hill, J. P.

    2016-06-01

    The magnetic excitations in electron-doped (Sr1 -xLax )2IrO4 with x =0.03 were measured using resonant inelastic x-ray scattering at the Ir L3 edge. Although much broadened, well defined dispersive magnetic excitations were observed. Comparing with the magnetic dispersion from the undoped compound, the evolution of the magnetic excitations upon doping is highly anisotropic. Along the antinodal direction, the dispersion is almost intact. On the other hand, the magnetic excitations along the nodal direction show significant softening. These results establish the presence of strong magnetic correlations in electron-doped (Sr1 -xLax )2IrO4 with close analogies to the hole-doped cuprates, further motivating the search for high temperature superconductivity in this system.

  3. Fragment transition density method to calculate electronic coupling for excitation energy transfer

    SciTech Connect

    Voityuk, Alexander A.

    2014-06-28

    A general approach, the Fragment Transition Density (FTD) scheme, is introduced to estimate electronic coupling for excitation energy transfer in a molecular system. Within this method, the excitation energies and transition densities of the system are used to derive the coupling matrix element. The scheme allows one to treat systems where exciton donor and acceptor are close together and their exchange interaction and orbital overlap are significant. The FTD method can be applied in combination with any quantum mechanical approach to treat excited states of general nature including single-, double-, and higher excitations. Using FTD approach, we derive excitonic couplings for several systems computed with the CIS, TD DFT and MS-CASPT2 methods. In particular, it is shown that the estimated coupling values in DNA π-stacks are strongly affected by the short-range electronic interaction of adjacent nucleobases.

  4. The 5p autoionization spectra of Ba atoms excited by electron impact: identification of lines

    NASA Astrophysics Data System (ADS)

    Hrytsko, V.; Kerevičius, G.; Kupliauskienė, A.; Borovik, A.

    2016-07-01

    The ejected-electron spectra corresponding to the radiationless decay of 5p5 {n}1{l}1{n}2{l}2{n}3{l}3 states in Ba atoms have been measured precisely for different incident electron energies ranging from the appearance of the first autoionizing line at 15.68 eV up to 140 eV. The spectra have been obtained at an observation angle of 54.7° and with incident-electron and ejected-electron energy resolutions of 0.2 eV and 0.07 eV, respectively. In total, 63 lines with excitation thresholds below 22 eV have been observed between 9.8 and 16.6 eV ejected-electron kinetic energy. Based on measured excitation energies, intensity behavior of lines, calculated excitation energies, cross sections and decay rates of states in 5p56s{}2{nl}, 5p55d{}2{nl} and 5p55d6snl configurations, assignments for all 63 lines are proposed. The excitation and decay processes for classified autoionizing states have been examined and compared with existing data. The excitation threshold of the 5{{{p}}}6 subshell has been established at 15.61 ± 0.05 eV.

  5. Characterizing the Locality of Diabatic States for Electronic Excitation Transfer by Decomposing the Diabatic Coupling

    SciTech Connect

    Vura-Weis, Josh; Newton, M. D.; Wasielewski, Michael R; Subotnik, J.E.

    2010-12-09

    A common strategy to calculate electronic coupling matrix elements for charge or energy transfer is to take the adiabatic states generated by electronic structure computations and rotate them to form localized diabatic states. In this paper, we show that, for intermolecular transfer of singlet electronic excitation, usually we cannot fully localize the electronic excitations in this way. Instead, we calculate putative initial and final states with small excitation tails caused by weak interactions with high energy excited states in the electronic manifold. These tails do not lead to substantial changes in the total diabatic coupling between states, but they do lead to a different partitioning of the total coupling between Coulomb (Förster), exchange (Dexter), and one-electron components. The tails may be reduced by using a multistate diabatic model or eliminated entirely by truncation (denoted as “chopping”). Without more information, we are unable to conclude with certainty whether the observed diabatic tails are a physical reality or a computational artifact. This research suggests that decomposition of the diabatic coupling between chromophores into Coulomb, exchange, and one-electron components may depend strongly on the number of states considered, and such results should be treated with caution.

  6. Inelastic mean free path, surface excitation parameter, and differential surface excitation parameter in Au for 300-3000 eV electrons

    NASA Astrophysics Data System (ADS)

    Nagatomi, T.; Goto, K.

    2009-11-01

    An analytical approach for simultaneously determining an inelastic mean free path (IMFP), a surface excitation parameter (SEP) and a differential SEP (DSEP) with absolute units was applied for the analysis of absolutely measured reflection electron energy loss spectra for Au. The IMFP, SEP and DSEP in Au for 300-3000 eV electrons are successfully obtained. The obtained DSEPs show a reasonable agreement with those theoretically calculated. The present SEPs were compared with those calculated by several empirical equations, revealing that the present SEPs are close to those calculated using the Oswald's equation. The IMFPs for Au determined by the present analysis were compared with those calculated by the TPP-2M predictive equation, revealing that the present IMFPs are in fairly good agreement with those calculated by the TPP-2M equation. The results confirmed that the present approach is effective for experimentally determining the SEP, DSEP, and IMFP for electrons in solids.

  7. Melting curves of metals with excited electrons in the quasiharmonic approximation

    NASA Astrophysics Data System (ADS)

    Minakov, D. V.; Levashov, P. R.

    2015-12-01

    We present melting curves of aluminum, copper, and nickel calculated on the basis of a quasiharmonic approximation. The dependence of a phonon density of states on electron temperature is taken into account for both thermodynamic properties and a mean square displacement of atoms. Linear expansion coefficients are strongly dependent on an approximation of the exchange-correlation functional; the generalized gradient approximation gives better results at normal conditions. Using the Lindemann criterion we obtain good agreement with experimental pressure dependences of the melting temperature for Al and Cu. In the case of Ni we consider a spin polarization effect to reproduce a recent first-principle simulation and shock-wave data. However, our melting curve is located significantly higher than static experimental points. We also consider a thermal excitation of electrons in a crystal and investigate the dependence of the melting temperature on the electronic one at normal and elevated densities. Hardening of the crystal structure for all the metals is obtained in our simulation; this effect might be confirmed experimentally owing to a relatively long lifetime of the two-temperature state.

  8. Study of intermediates from transition metal excited-state electron-transfer reactions. Final report, August 4, 1986--August 31, 1997

    SciTech Connect

    Hoffman, M.Z.

    1997-12-31

    The techniques of continuous photolysis and pulsed laser flash photolysis, continuous and pulse radiolysis, fast-scan cyclic voltammetry, and time-resolved fluorimetry have been used to examine intramolecular electron transfer within the solvent quenching cage, photodynamics of quenching of the excited states of transition-metal photosensitizers, the properties of excites states and one-electron reduced forms, ground- and excited-state interactions with solutes, and photoinduced oxidations of organic solutes in aqueous solution. The following specific areas were examined: (1) the parameters that govern the yields of redox products from excited-state electron-transfer quenching reactions; (2) the mediation of the properties of excited states and one-electron reduced forms by the ligands and the solution medium; (3) the effect of the interactions between the ground state of the complex and the solution components on the behavior of the excited state; (4) the yields of singlet oxygen from excited-state energy-transfer quenching by O{sub 2}; and (5) the oxidations of solutes by singlet oxygen, excited-state electron-transfer quenching, and free radicals. This report contains the abstracts of 50 publications describing the studies.

  9. Method and apparatus for secondary laser pumping by electron beam excitation

    DOEpatents

    George, E. Victor; Krupke, William F.; Murray, John R.; Powell, Howard T.; Swingle, James C.; Turner, Jr., Charles E.; Rhodes, Charles K.

    1978-01-01

    An electron beam of energy typically 100 keV excites a fluorescer gas which emits ultraviolet radiation. This radiation excites and drives an adjacent laser gas by optical pumping or photolytic dissociation to produce high efficiency pulses. The invention described herein was made in the course of, or under, United States Energy Research and Development Administration Contract No. W-7405-Eng-48 with the University of California.

  10. Measurement of the lifetime of excited-state electron bubbles in superfluid helium

    SciTech Connect

    Ghosh, Ambarish; Maris, Humphrey J.

    2005-08-01

    We report on the measurement of the lifetime of bubbles in superfluid helium that contain an electron in the 1P state. The 1P bubbles are produced by laser excitation of ground-state bubbles, and are detected by ultrasonic cavitation. Our measurements show that the lifetime of these excited bubbles is much less than the calculated lifetime for radiative decay and, hence, is determined by a nonradiative mechanism.

  11. Matrix photochemistry of small molecules: Influencing reaction dynamics on electronically excited hypersurfaces

    SciTech Connect

    Laursen, S.L.

    1990-01-01

    Investigations of chemical reactions on electronically excited reaction surfaces are presented. The role of excited-surface multiplicity is of particular interest, as are chemical reactivity and energy transfer in systems in which photochemistry is initiated through a metal atom sensitizer.'' Two approaches are employed: A heavy-atom matrix affords access to forbidden triplet reaction surfaces, eliminating the need for a potentially reactive sensitizer. Later, the role of the metal atom in the photosensitization process is examined directly.

  12. Tuning of superfine electron-nuclear interaction in structure of the ground states and the characteristics of the full systems electronic excited states for formation of effective phothophysics and spectral-energy of properties in the series of multinuclear compounds

    NASA Astrophysics Data System (ADS)

    Obukhov, A. E.

    2012-06-01

    The help of the measurements (the methods are the NMR 1H and 13C, infrared (IR) and the UV-absorption, Raman scattering of light, the fluorescence and the phosphorescence, the pumping of the lasers and lamps, the low-temperature of the spectroscopy in the solutions (77 K) and the Jet-spectroscopy of vapor (2,6 K) and others) and the calculations with application of the developed new complex of the computer of the programs realizing of the quantum-chemical LCAO-MO SCF extended-CI INDO / S of methods are investigated of the photophysical properties of some news and also some known the organic compounds for variations of the electronic and the spatial structures in the series is the mono-, bi-, three, penta- and quincli-cyclic and the bi- and the bis- phenyl, furyl- and tienyl- oxazoles and - oxadiazoles have been studied of the spectroscopy properties in the wavelength range max λ max abs,osc = 208 ÷ 760 nm.

  13. Reactions of ground-state and electronically excited sodium atoms with methyl bromide and molecular chlorine

    SciTech Connect

    Weiss, P.S.; Mestdagh, J.M.; Schmidt, H.; Covinsky, M.H.; Lee, Y.T. )

    1991-04-18

    The reactions of ground- and excited-state Na atoms with methyl bromide (CH{sub 3}Br) and chlorine (Cl{sub 2}) have been studied by using the crossed molecular beams method. For both reactions, the cross sections increase with increasing electronic energy. The product recoil energies change little with increasing Na electronic energy, implying that the product internal energies increase substantially. For Na + CH{sub 3}Br, the steric angle of acceptance opens with increasing electronic energy.

  14. Laser excitation of clusters: observables from electron emission

    NASA Astrophysics Data System (ADS)

    Wopperer, P.; Dinh, P. M.; Reinhard, P. G.; Suraud, E.

    2012-11-01

    We give a brief review of the theoretical description of photo-electron spectra (PES) and photo-angular distributions (PAD) and discuss a few selected, typical results. The description is based on time-dependent density-functional theory at the level of the local-density approximation augmented by a self-interaction correction which is crucial for a quantitative assessment of emission processes. Coordinate-space grids are used together with absorbing boundary conditions. We discuss the basic features and trends of PES and PAD for two typical test cases, the clusters Na8 and C60.

  15. Relaxation and interaction of electronic excitations induced by intense ultra short light pulses in BaF2 scintillator

    NASA Astrophysics Data System (ADS)

    Kirm, M.; Nagirnyi, V.; Vielhauer, S.; Feldbach, E.

    2011-06-01

    Excitation density effects have a pronounced influence on relaxation processes in solids. They come into play in scintillating and dosimetric materials exposed to ionizing radiation or in laser materials operating in intense ultraviolet light fields. The scientific understanding of the underlying process is poor, mainly because most of the studies of light emitting materials under short wavelength excitation have been performed at weak and moderate excitation intensities due to limited availability of powerful light sources. Disembodied data on excitation density effects have been reported for wide-gap dielectrics studied by luminescence spectroscopy, by using such excitation sources as powerful ion beams,1,2pulsed electron beams,2,3 and wide-band hard X-ray synchrotron radiation.4 It is obvious that such non-selective excitation is a good tool for revealing density-related phenomena in these materials in general, but for investigating specific features of relaxation processes in insulators, light sources with well defined parameters are necessary. Since the shortwavelength free electron laser (FEL) technology has been devised by an international consortium at HASYLAB of DESY, resulting in the development of TESLA Test facility (TTF)5 and later in the construction of a dedicated FEL source FLASH in Hamburg,6 more advanced studies became possible. The range of interests towards this light source covers the fields from material science and various other branches of physics to structural biology. The pioneering luminescence study revealed excitation density effects in the decay of Ce3+ 5d-4f luminescence in Y3Al5O12 crystals and luminescence of BaF2 crystals in UV-visible range.7 These results motivated systematic investigations of excitation density effects in wide gap crystals using FEL8,9 and high-harmonic-generated VUV radiation,10 and, at lower energies, femtosecond laser pulses in the UV.11,12 The main goal of the present work is to analyze the same phenomenon

  16. Seed electron production from O{sup -} ions under high-power microwave excitation

    SciTech Connect

    Edmiston, G. F.; Neuber, A. A.; Krompholz, H. G.; Krile, J. T.

    2008-03-15

    Surface and volume breakdown formation during pulsed high-power microwave (HPM) excitation can severely limit the power densities which can be transmitted into an atmospheric medium. Recent studies in this area have focused on developing models which accurately predict flashover formation at either dielectric/air interfaces or in the gas volume directly adjacent to these interfaces. These models are typically validated through comparison with experimentally gathered data. With respect to HPM surface flashover, experiments in the S-band at 5 MW power levels have reported on the contributing factors to flashover development including the effects of gas type, pressure, and relative humidity. A Monte Carlo-type electron motion simulation code, MC, has been developed to calculate the increasing electron density during flashover formation in this case. Results from the MC code have exhibited a quantitative agreement with experimental data over a wide range of atmospheric conditions. A critical parameter to flashover development is the stochastic process involving the appearance of initiatory or ''seed'' electrons, as seen by the reduction in flashover delay time by approximately 10-20% in the presence of external ultraviolet illumination. While the current version of the MC code seeds the flashover location with electron densities on the order of background ion densities produced by cosmic radiation, it fails to incorporate the field-assisted collisional detachment processes which are often assumed to be the primary origin of these electrons on the time scales of interest. Investigation of these processes and development of more accurate seeding in the MC code is a key step toward predicting HPM flashover over a wide range of parameters, particularly in the presence of highly electronegative gases such as SF{sub 6} or O{sub 2}, in which there is an absence of free electrons with zero applied field.

  17. A QM/MM Approach Using the AMOEBA Polarizable Embedding: From Ground State Energies to Electronic Excitations.

    PubMed

    Loco, Daniele; Polack, Étienne; Caprasecca, Stefano; Lagardère, Louis; Lipparini, Filippo; Piquemal, Jean-Philip; Mennucci, Benedetta

    2016-08-01

    A fully polarizable implementation of the hybrid quantum mechanics/molecular mechanics approach is presented, where the classical environment is described through the AMOEBA polarizable force field. A variational formalism, offering a self-consistent relaxation of both the MM induced dipoles and the QM electronic density, is used for ground state energies and extended to electronic excitations in the framework of time-dependent density functional theory combined with a state specific response of the classical part. An application to the calculation of the solvatochromism of the pyridinium N-phenolate betaine dye used to define the solvent ET(30) scale is presented. The results show that the QM/AMOEBA model not only properly describes specific and bulk effects in the ground state but it also correctly responds to the large change in the solute electronic charge distribution upon excitation. PMID:27340904

  18. Core excitation effects in the breakup of halo nuclei

    SciTech Connect

    Moro, A. M.; Diego, R. de; Lay, J. A.; Crespo, R.; Johnson, R. C.; Arias, J. M.; Gomez-Camacho, J.

    2012-10-20

    The role of core excitation in the structure and dynamics of two-body halo nuclei is investigated. We present calculations for the resonant breakup of {sup 11}Be on protons at an incident energy of 63.7 MeV/nucleon, where core excitation effects were shown to be important. To describe the reaction, we use a recently developed extension of the DWBA formalism which incorporates these core excitation effects within the no-recoil approximation. The validity of the no-recoil approximation is also examined by comparing with DWBA calculations which take into account core recoil. In addition, calculations with two different continuum representations are presented and compared.

  19. Electron impact excitation of the Ne II and Ne III fine structure levels

    NASA Astrophysics Data System (ADS)

    Wang, Q.; Loch, S. D.; Pindzola, M. S.; Cumbee, R.; Stancil, P. C.; Ballance, C. P.; McLaughlin, B. M.

    2016-05-01

    Electron impact excitation cross sections and rate coefficients of the low lying levels of the Ne II and Ne III ions are of great interest in cool molecular environments including young stellar objects, photodissociation regions, active galactic nuclei, and X-ray dominated regions. We have carried out details computations for cross sections and rate coefficients using the Dirac R-matrix codes (DARC), the Breit-Pauli R-matrix codes (BP) and the Intermediate Coupling Frame Transformation (ICFT) codes, for both Ne II and Ne III. We also compare our results with previous calculations. We are primarily interested in rate coefficients in the temperature range below 1000 K, and the focus is on obtaining the most accurate rate coefficients for those temperatures. We present both a recommended set of effective collision strengths and an indication of the uncertainties on these values. Work at Auburn University and UGA partly supported by NASA Grant NNX15AE47G.

  20. Hedgehog excitations in double-exchange magnetism: Energetics and electronic structure

    NASA Astrophysics Data System (ADS)

    Pekker, David; Goldbart, Paul; Salamon, Myron; Abanov, Alexander

    2004-03-01

    Topological hedgehog excitations of the magnetic state are believed to play an important role in the three-dimensional ferromagnet-to-paramagnet phase transition. This is true not only in Heisenberg magnets but also in double-exchange magnets, for which the transition is accompanied by a metal-insulator transition. The energetics and electronic structure of hedgehog excitations in double-exchange systems are investigated using a model in which the electrons move through a lattice of classical spins, to which they are coupled via Hund's Rule interactions. The core energy of hedgehog excitations is determined, as is the extent to which charge is expelled from the hedgehog cores. In settings involving pairs of hedgehogs, the manner in which the electronic energetics determines the magnetic structure is explored variationally, especially in the region between the hedgehogs.

  1. Modeling Electronic-Nuclear Interactions for Excitation Energy Transfer Processes in Light-Harvesting Complexes.

    PubMed

    Lee, Mi Kyung; Coker, David F

    2016-08-18

    An accurate approach for computing intermolecular and intrachromophore contributions to spectral densities to describe the electronic-nuclear interactions relevant for modeling excitation energy transfer processes in light harvesting systems is presented. The approach is based on molecular dynamics (MD) calculations of classical correlation functions of long-range contributions to excitation energy fluctuations and a separate harmonic analysis and single-point gradient quantum calculations for electron-intrachromophore vibrational couplings. A simple model is also presented that enables detailed analysis of the shortcomings of standard MD-based excitation energy fluctuation correlation function approaches. The method introduced here avoids these problems, and its reliability is demonstrated in accurate predictions for bacteriochlorophyll molecules in the Fenna-Matthews-Olson pigment-protein complex, where excellent agreement with experimental spectral densities is found. This efficient approach can provide instantaneous spectral densities for treating the influence of fluctuations in environmental dissipation on fast electronic relaxation. PMID:27472379

  2. Density gradient free electron collisionally excited x-ray laser

    DOEpatents

    Campbell, E.M.; Rosen, M.D.

    1984-11-29

    An operational x-ray laser is provided that amplifies 3p-3s transition x-ray radiation along an approximately linear path. The x-ray laser is driven by a high power optical laser. The driving line focused optical laser beam illuminates a free-standing thin foil that may be associated with a substrate for improved structural integrity. This illumination produces a generally cylindrically shaped plasma having an essentially uniform electron density and temperature, that exists over a long period of time, and provides the x-ray laser gain medium. The x-ray laser may be driven by more than one optical laser beam. The x-ray laser has been successfully demonstrated to function in a series of experimental tests.

  3. Density gradient free electron collisionally excited X-ray laser

    DOEpatents

    Campbell, Edward M.; Rosen, Mordecai D.

    1989-01-01

    An operational X-ray laser (30) is provided that amplifies 3p-3s transition X-ray radiation along an approximately linear path. The X-ray laser (30) is driven by a high power optical laser. The driving line focused optical laser beam (32) illuminates a free-standing thin foil (34) that may be associated with a substrate (36) for improved structural integrity. This illumination produces a generally cylindrically shaped plasma having an essentially uniform electron density and temperature, that exists over a long period of time, and provides the X-ray laser gain medium. The X-ray laser (30) may be driven by more than one optical laser beam (32, 44). The X-ray laser (30) has been successfully demonstrated to function in a series of experimental tests.

  4. Electronic density fluctuation associated to coherent plasmon excitations

    NASA Astrophysics Data System (ADS)

    Gervasoni, Juana; Segui, Silvina; Arista, Nestor

    2011-10-01

    In this work we analyze, in the frame of the coherent states, the fluctuation of the electronic collective modes associated with the wake potential generated by an external particle of charge Ze. This perturbation is described as coherent states of plasmons spatially localized in an average distance of the order of the velocity of the projectile divided by the plasmon frequency of the material. One of the most important features is that in all the cases, for different trajectories of the external particle, and for different structures of the material, the fluctuations are not negligible. In particular, we observe that due to the importance of the surface in nanostructured materials, the fluctuation of density is very sensitive to their geometry and composition, fact that must have taken into account for the nanodevices designs. In this work we analyze, in the frame of the coherent states, the fluctuation of the electronic collective modes associated with the wake potential generated by an external particle of charge Ze. This perturbation is described as coherent states of plasmons spatially localized in an average distance of the order of the velocity of the projectile divided by the plasmon frequency of the material. One of the most important features is that in all the cases, for different trajectories of the external particle, and for different structures of the material, the fluctuations are not negligible. In particular, we observe that due to the importance of the surface in nanostructured materials, the fluctuation of density is very sensitive to their geometry and composition, fact that must have taken into account for the nanodevices designs. Acknowledgements to CNEA and CONICET, Argentina.

  5. Low energy electronic excitations and fano resonance in K doped C 60 from Raman scattering excited at 1.16 eV

    NASA Astrophysics Data System (ADS)

    Danieli, R.; Denisov, V. N.; Ruani, G.; Zamboni, R.; Taliani, C.; Zakhidov, A. A.; Ugawa, A.; Imaeda, K.; Yakushi, K.; Inokuchi, H.; Kikuchi, K.; Ikemoto, I.; Suzuki, S.; Achiba, Y.

    1992-01-01

    We present a Raman scattering study of pristine and K doped C 60 at various doping levels by exciting in the near-IR at 1.16 eV. The normal metallic state of K 3C 60 is characterized by a broad scattering background and by the resonance of low energy phonons in the range of 250-500 cm -1. We assign the broad background to an electronic Raman scattering due to low energy electronic excitations. This spectral feature is indicative of an anomalous normal state behaviour and is similar to the case of high temperature ceramic superconductors. In the overdoped K 6C 60 the squashing mode at 278 cm -1 shows a Fano resonance with the electronic scattering associated with localized electronic excitations which are characteristic of isolated regions of K 3C 60 into the matrix of K 6C 60 as a result of inhomogeneous doping. The Fano resonance indicates a specific electron-phonon coupling of this Jahn-Teller mode with low energy excitations and suggests that the symmetry of this electronic excitation is h g (i.e. the same of the coupled phonon mode). We discuss the nature of the anomalous electronic Raman scattering in terms of scattering from low energy excitations involving a low lying singlet band resulting from electron correlation and/or dynamical J-T distortion caused by the squashing mode.

  6. Excitation of surface and volume plasmons in a metal nanosphere by fast electrons

    NASA Astrophysics Data System (ADS)

    Gildenburg, V. B.; Kostin, V. A.; Pavlichenko, I. A.

    2016-03-01

    Collective multipole oscillations (surface and volume plasmons) excited in a metal nanosphere by moving electron and corresponding inelastic scattering spectra are studied based on the hydrodynamic approach. Along with the bulk (dielectric) losses traditionally taken into account, the surface and radiative ones are also considered as the physical mechanisms responsible for the plasmon damping. The second and third mechanisms are found to be essential for the surface plasmons (at small or large cluster radii, respectively) and depend very differently on the multipole mode order. The differential equations are obtained which describe the temporal evolution of every particular mode as that one of a linear oscillator excited by the given external force, and the electron energy loss spectra are calculated. The changes in spectrum shape with the impact parameter and with the electron passage time are analyzed; the first of them is found to be in good enough agreement with the data of scanning transmission electron microscopy experiments. It is shown that, in the general case, a pronounced contribution to the formation of the loss spectrum is given by the both surface and volume plasmons with low and high multipole indices. In particular, at long electron passage time, the integral (averaged over the impact parameter) loss spectrum which is calculated for the free-electron cluster model contains two main peaks: a broad peak from merging of many high-order multipole resonances of the surface plasmons and a narrower peak of nearly the same height from merged volume plasmons excited by the electrons that travel through the central region of the cluster. Comparatively complex dependences of the calculated excitation coefficients and damping constants of various plasmons on the order of the excited multipole result in wide diversity of possible types of the loss spectrum even for the same cluster material and should be taken into account in interpretation of corresponding

  7. Controlling electronic access to the spin excitations of a single molecule in a tunnel junction

    NASA Astrophysics Data System (ADS)

    Hirjibehedin, Cyrus F.; Warner, Ben; El Hallak, Fadi; Prueser, Henning; Ajibade, Afolabi; Gill, Tobias G.; Fisher, Andrew J.; Persson, Mats

    Spintronic phenomena can be utilized to create new devices with applications in data storage and sensing. Scaling these down to the single molecule level requires controlling the properties of the current-carrying orbitals to enable access to spin states through phenomena such as inelastic electron tunneling. Here we show that the spintronic properties of a tunnel junction containing a single molecule can be controlled by their coupling to the local environment. For tunneling through iron phthalocyanine (FePc) on an insulating copper nitride (Cu2N) monolayer above Cu(001), we find that spin transitions may be strongly excited depending on the binding site of the central Fe atom. Different interactions between the Fe and the underlying Cu or N atoms shift the Fe d-orbitals with respect to the Fermi energy, and control the relative strength of the spin excitations, an effect that can described in a simple co-tunneling model. This work demonstrates the importance of the atomic-scale environment in the development of single molecule spintronic devices.

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

    NASA Astrophysics Data System (ADS)

    Zdyb, Agata; Krawczyk, Stanisław

    2016-03-01

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

  9. Electron emission from photo-excited testosterone in water-ethanol solution.

    PubMed

    Getoff, Nikola; Schittl, Heike; Hartmann, Johannes; Quint, Ruth Maria

    2009-03-01

    Testosterone (TES; 4-androstene-17beta-ol-3-on) is found for the first time to eject electrons from its singlet excited state in water-ethanol solvent mixture. This ability was very recently also observed for 17beta-estradiol (17betaE2) and progesterone (PRG)/1/. With increasing TES-concentration, the yield of solvated electrons (e(s)(-)) is decreasing, because of "associate" formation. At higher absorbed UV-doses (lambda=254 nm) the e(s)(-) yield is passing a sharp maximum by formation of TES-ethanol adducts, which are able likewise to emit electrons when excited. At prolonged irradiation the resulting photolytic products of TES-ethanol adducts are also able to emit electrons. The capability of the hormones: 17betaE2, PRG and TES to eject electrons and the resulting metabolites, some of which can induce cancer, is discussed. PMID:19124256

  10. Electron-impact excitation collision strengths and theoretical line intensities for transitions in S III

    SciTech Connect

    Grieve, M. F. R.; Ramsbottom, C. A.; Hudson, C. E.; Keenan, F. P.

    2014-01-01

    We present Maxwellian-averaged effective collision strengths for the electron-impact excitation of S III over a wide range of electron temperatures of astrophysical importance, log T{sub e} (K) = 3.0-6.0. The calculation incorporates 53 fine-structure levels arising from the six configurations—3s {sup 2}3p {sup 2}, 3s3p {sup 3}, 3s {sup 2}3p3d, 3s {sup 2}3p4s, 3s {sup 2}3p4p, and 3s {sup 2}3p4d—giving rise to 1378 individual lines and is undertaken using the recently developed RMATRX II plus FINE95 suite of codes. A detailed comparison is made with a previous R-matrix calculation and significant differences are found for some transitions. The atomic data are subsequently incorporated into the modeling code CLOUDY to generate line intensities for a range of plasma parameters, with emphasis on allowed ultraviolet extreme-ultraviolet emission lines detected from the Io plasma torus. Electron density-sensitive line ratios are calculated with the present atomic data and compared with those from CHIANTI v7.1, as well as with Io plasma torus spectra obtained by Far-Ultraviolet Spectroscopic Explorer and Extreme-Ultraviolet Explorer. The present line intensities are found to agree well with the observational results and provide a noticeable improvement on the values predicted by CHIANTI.

  11. Surface excitations in electron spectroscopy. Part I: dielectric formalism and Monte Carlo algorithm

    PubMed Central

    Salvat-Pujol, F; Werner, W S M

    2013-01-01

    The theory describing energy losses of charged non-relativistic projectiles crossing a planar interface is derived on the basis of the Maxwell equations, outlining the physical assumptions of the model in great detail. The employed approach is very general in that various common models for surface excitations (such as the specular reflection model) can be obtained by an appropriate choice of parameter values. The dynamics of charged projectiles near surfaces is examined by calculations of the induced surface charge and the depth- and direction-dependent differential inelastic inverse mean free path (DIIMFP) and stopping power. The effect of several simplifications frequently encountered in the literature is investigated: differences of up to 100% are found in heights, widths, and positions of peaks in the DIIMFP. The presented model is implemented in a Monte Carlo algorithm for the simulation of the electron transport relevant for surface electron spectroscopy. Simulated reflection electron energy loss spectra are in good agreement with experiment on an absolute scale. Copyright © 2012 John Wiley & Sons, Ltd. PMID:23794766

  12. Envelope excitations in electronegative plasmas with electrons featuring the Tsallis distribution

    SciTech Connect

    Bains, A. S.; Li, Bo; Tribeche, Mouloud

    2013-09-15

    We examine the modulational instability (MI) of ion-acoustic waves (IAWs) in an electronegative plasma containing positive and negative ions as well as electrons that follow the nonextensive statistics proposed by Tsallis [J. Stat. Phys. 52, 479 (1988)]. Using the reductive perturbation method, the nonlinear Schrödinger equation that governs the modulational instability of the IAWs is obtained. Inspired by the experimental work of Ichiki et al.[Phys. Plasmas 8, 4275 (2001)], three types of electronegative plasmas are investigated. The effects of various parameters on the propagation of IAWs are discussed in detail numerically. We find that the plasma supports both bright and dark solutions. The presence of the non-extensively distributed electrons is found to play a crucial role in the formation of envelope excitations. The region in the parameter space where the MI exists depends sensitively on the positive to negative ion mass ratio (M) and negative to positive ion density ratio (ν). An extensive range of the nonextensive q-parameters (−1electrons.

  13. Surface excitations in electron spectroscopy. Part I: dielectric formalism and Monte Carlo algorithm.

    PubMed

    Salvat-Pujol, F; Werner, W S M

    2013-05-01

    The theory describing energy losses of charged non-relativistic projectiles crossing a planar interface is derived on the basis of the Maxwell equations, outlining the physical assumptions of the model in great detail. The employed approach is very general in that various common models for surface excitations (such as the specular reflection model) can be obtained by an appropriate choice of parameter values. The dynamics of charged projectiles near surfaces is examined by calculations of the induced surface charge and the depth- and direction-dependent differential inelastic inverse mean free path (DIIMFP) and stopping power. The effect of several simplifications frequently encountered in the literature is investigated: differences of up to 100% are found in heights, widths, and positions of peaks in the DIIMFP. The presented model is implemented in a Monte Carlo algorithm for the simulation of the electron transport relevant for surface electron spectroscopy. Simulated reflection electron energy loss spectra are in good agreement with experiment on an absolute scale. Copyright © 2012 John Wiley & Sons, Ltd. PMID:23794766

  14. Dynamical effects in electron spectroscopy

    NASA Astrophysics Data System (ADS)

    Zhou, Jianqiang Sky; Kas, J. J.; Sponza, Lorenzo; Reshetnyak, Igor; Guzzo, Matteo; Giorgetti, Christine; Gatti, Matteo; Sottile, Francesco; Rehr, J. J.; Reining, Lucia

    2015-11-01

    One of the big challenges of theoretical condensed-matter physics is the description, understanding, and prediction of the effects of the Coulomb interaction on materials properties. In electronic spectra, the Coulomb interaction causes a renormalization of energies and change of spectral weight. Most importantly, it can lead to new structures, often called satellites. These can be linked to the coupling of excitations, also termed dynamical effects. State-of-the-art methods in the framework of many-body perturbation theory, in particular, the widely used GW approximation, often fail to describe satellite spectra. Instead, approaches based on a picture of electron-boson coupling such as the cumulant expansion are promising for the description of plasmon satellites. In this work, we give a unified derivation of the GW approximation and the cumulant expansion for the one-body Green's function. Using the example of bulk sodium, we compare the resulting spectral functions both in the valence and in the core region, and we discuss the dispersion of quasi-particles and satellites. We show that self-consistency is crucial to obtain meaningful results, in particular, at large binding energies. Very good agreement with experiment is obtained when the intrinsic spectral function is corrected for extrinsic and interference effects. Finally, we sketch how one can approach the problem in the case of the two-body Green's function, and we discuss the cancellation of various dynamical effects that occur in that case.

  15. Dynamical effects in electron spectroscopy

    SciTech Connect

    Zhou, Jianqiang Sky Reshetnyak, Igor; Giorgetti, Christine; Sottile, Francesco; Reining, Lucia; Kas, J. J.; Rehr, J. J.; Sponza, Lorenzo; Guzzo, Matteo; Gatti, Matteo

    2015-11-14

    One of the big challenges of theoretical condensed-matter physics is the description, understanding, and prediction of the effects of the Coulomb interaction on materials properties. In electronic spectra, the Coulomb interaction causes a renormalization of energies and change of spectral weight. Most importantly, it can lead to new structures, often called satellites. These can be linked to the coupling of excitations, also termed dynamical effects. State-of-the-art methods in the framework of many-body perturbation theory, in particular, the widely used GW approximation, often fail to describe satellite spectra. Instead, approaches based on a picture of electron-boson coupling such as the cumulant expansion are promising for the description of plasmon satellites. In this work, we give a unified derivation of the GW approximation and the cumulant expansion for the one-body Green’s function. Using the example of bulk sodium, we compare the resulting spectral functions both in the valence and in the core region, and we discuss the dispersion of quasi-particles and satellites. We show that self-consistency is crucial to obtain meaningful results, in particular, at large binding energies. Very good agreement with experiment is obtained when the intrinsic spectral function is corrected for extrinsic and interference effects. Finally, we sketch how one can approach the problem in the case of the two-body Green’s function, and we discuss the cancellation of various dynamical effects that occur in that case.

  16. Dynamical effects in electron spectroscopy.

    PubMed

    Zhou, Jianqiang Sky; Kas, J J; Sponza, Lorenzo; Reshetnyak, Igor; Guzzo, Matteo; Giorgetti, Christine; Gatti, Matteo; Sottile, Francesco; Rehr, J J; Reining, Lucia

    2015-11-14

    One of the big challenges of theoretical condensed-matter physics is the description, understanding, and prediction of the effects of the Coulomb interaction on materials properties. In electronic spectra, the Coulomb interaction causes a renormalization of energies and change of spectral weight. Most importantly, it can lead to new structures, often called satellites. These can be linked to the coupling of excitations, also termed dynamical effects. State-of-the-art methods in the framework of many-body perturbation theory, in particular, the widely used GW approximation, often fail to describe satellite spectra. Instead, approaches based on a picture of electron-boson coupling such as the cumulant expansion are promising for the description of plasmon satellites. In this work, we give a unified derivation of the GW approximation and the cumulant expansion for the one-body Green's function. Using the example of bulk sodium, we compare the resulting spectral functions both in the valence and in the core region, and we discuss the dispersion of quasi-particles and satellites. We show that self-consistency is crucial to obtain meaningful results, in particular, at large binding energies. Very good agreement with experiment is obtained when the intrinsic spectral function is corrected for extrinsic and interference effects. Finally, we sketch how one can approach the problem in the case of the two-body Green's function, and we discuss the cancellation of various dynamical effects that occur in that case. PMID:26567648

  17. Synthesis of metal silicide at metal/silicon oxide interface by electronic excitation

    SciTech Connect

    Lee, J.-G.; Nagase, T.; Yasuda, H.; Mori, H.

    2015-05-21

    The synthesis of metal silicide at the metal/silicon oxide interface by electronic excitation was investigated using transmission electron microscopy. A platinum silicide, α-Pt{sub 2}Si, was successfully formed at the platinum/silicon oxide interface under 25–200 keV electron irradiation. This is of interest since any platinum silicide was not formed at the platinum/silicon oxide interface by simple thermal annealing under no-electron-irradiation conditions. From the electron energy dependence of the cross section for the initiation of the silicide formation, it is clarified that the silicide formation under electron irradiation was not due to a knock-on atom-displacement process, but a process induced by electronic excitation. It is suggested that a mechanism related to the Knotek and Feibelman mechanism may play an important role in silicide formation within the solid. Similar silicide formation was also observed at the palladium/silicon oxide and nickel/silicon oxide interfaces, indicating a wide generality of the silicide formation by electronic excitation.

  18. Nonlinear response of metal nanoparticles: Double plasmon excitation and electron transfer.

    PubMed

    Gao, Shiwu

    2015-06-21

    We investigate the dynamical response of a metal nanoparticle and the electron transfer to a molecule near its surface using time-dependent density functional theory. In addition to the linear response of the Mie resonance, double plasmon excitations and a low-frequency charge transfer band emerge and become prominent at high laser intensities. Both modes are nonlinear processes, which are derived from the re-excitation and decay of the primary plasmon mode, respectively. Our results shed light on the localised characters of the plasmon-molecule coupling and hot electron distributions. These findings have general implications to photoinduced phenomena in nanosystems. PMID:26093567

  19. Nonlinear response of metal nanoparticles: Double plasmon excitation and electron transfer

    NASA Astrophysics Data System (ADS)

    Gao, Shiwu

    2015-06-01

    We investigate the dynamical response of a metal nanoparticle and the electron transfer to a molecule near its surface using time-dependent density functional theory. In addition to the linear response of the Mie resonance, double plasmon excitations and a low-frequency charge transfer band emerge and become prominent at high laser intensities. Both modes are nonlinear processes, which are derived from the re-excitation and decay of the primary plasmon mode, respectively. Our results shed light on the localised characters of the plasmon-molecule coupling and hot electron distributions. These findings have general implications to photoinduced phenomena in nanosystems.

  20. Validity of Eucken formula and Stokes’ viscosity relation in high-temperature electronically excited gases

    SciTech Connect

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

    2014-12-09

    In the present work we evaluate the accuracy of the Eucken formula and Stokes’ viscosity relation in high temperature non-equilibrium air species with electronic excitation. The thermal conductivity coefficient calculated using the exact kinetic theory methods is compared with that obtained applying approximate formulas in the temperature range 200–20000 K. A modification of the Eucken formula providing a good agreement with exact calculations is proposed. It is shown that the Stokes viscosity relation is not valid in electronically excited monoatomic gases at temperatures higher than 2000 K.

  1. Nonlinear response of metal nanoparticles: Double plasmon excitation and electron transfer

    SciTech Connect

    Gao, Shiwu

    2015-06-21

    We investigate the dynamical response of a metal nanoparticle and the electron transfer to a molecule near its surface using time-dependent density functional theory. In addition to the linear response of the Mie resonance, double plasmon excitations and a low-frequency charge transfer band emerge and become prominent at high laser intensities. Both modes are nonlinear processes, which are derived from the re-excitation and decay of the primary plasmon mode, respectively. Our results shed light on the localised characters of the plasmon-molecule coupling and hot electron distributions. These findings have general implications to photoinduced phenomena in nanosystems.

  2. Quantum-chemical study of electronically excited states of protolytic forms of vanillic acid

    NASA Astrophysics Data System (ADS)

    Vusovich, O. V.; Tchaikovskaya, O. N.; Sokolova, I. V.; Vasil'eva, N. Y.

    2015-12-01

    The paper describes an analysis of possible ways of deactivation of electronically excited states of 4-hydroxy- 3-methoxy-benzoic acid (vanillic acid) and its protolytic forms with the use of quantum-chemical methods INDO/S (intermediate neglect of differential overlap with a spectroscopic parameterization) and MEP (molecular electrostatic potential). The ratio of radiative and non-radiative deactivation channels of the electronic excitation energy is established. The rate constants of photophysical processes (internal and intercombination conversions) occurring after the absorption of light in these forms are evaluated.

  3. Exciting: a full-potential all-electron package implementing density-functional theory and many-body perturbation theory.

    PubMed

    Gulans, Andris; Kontur, Stefan; Meisenbichler, Christian; Nabok, Dmitrii; Pavone, Pasquale; Rigamonti, Santiago; Sagmeister, Stephan; Werner, Ute; Draxl, Claudia

    2014-09-10

    Linearized augmented planewave methods are known as the most precise numerical schemes for solving the Kohn-Sham equations of density-functional theory (DFT). In this review, we describe how this method is realized in the all-electron full-potential computer package, exciting. We emphasize the variety of different related basis sets, subsumed as (linearized) augmented planewave plus local orbital methods, discussing their pros and cons and we show that extremely high accuracy (microhartrees) can be achieved if the basis is chosen carefully. As the name of the code suggests, exciting is not restricted to ground-state calculations, but has a major focus on excited-state properties. It includes time-dependent DFT in the linear-response regime with various static and dynamical exchange-correlation kernels. These are preferably used to compute optical and electron-loss spectra for metals, molecules and semiconductors with weak electron-hole interactions. exciting makes use of many-body perturbation theory for charged and neutral excitations. To obtain the quasi-particle band structure, the GW approach is implemented in the single-shot approximation, known as G(0)W(0). Optical absorption spectra for valence and core excitations are handled by the solution of the Bethe-Salpeter equation, which allows for the description of strongly bound excitons. Besides these aspects concerning methodology, we demonstrate the broad range of possible applications by prototypical examples, comprising elastic properties, phonons, thermal-expansion coefficients, dielectric tensors and loss functions, magneto-optical Kerr effect, core-level spectra and more. PMID:25135665

  4. Excited-State Electronic Structure in Polypyridyl Complexes Containing Unsymmetrical Ligands.

    PubMed

    Omberg, Kristin M.; Smith, Gregory D.; Kavaliunas, Darius A.; Chen, Pingyun; Treadway, Joseph A.; Schoonover, Jon R.; Palmer, Richard A.; Meyer, Thomas J.

    1999-03-01

    Step-scan Fourier transform infrared absorption difference time-resolved (S(2)FTIR DeltaA TRS) and time-resolved resonance Raman (TR(3)) spectroscopies have been applied to a series of questions related to excited-state structure in the metal-to-ligand charge transfer (MLCT) excited states of [Ru(bpy)(2)(4,4'-(CO(2)Et)(2)bpy)](2+), [Ru(bpy)(2)(4-CO(2)Et-4'-CH(3)bpy)](2+), [Ru(bpy)(4,4'-(CO(2)Et)(2)bpy)(2)](2+), [Ru(4,4'-(CO(2)Et)(2)bpy)(3)](2+), [Ru(bpy)(2)(4,4'-(CONEt(2))(2)bpy)](2+), [Ru(bpy)(2)(4-CONEt(2)-4'-CH(3)bpy)](2+), and [Ru(4-CONEt(2)-4'-CH(3)bpy)(3)](2+) (bpy is 2,2'-bipyridine). These complexes contain bpy ligands which are either symmetrically or unsymmetrically derivatized with electron-withdrawing ester or amide substituents. Analysis of the vibrational data, largely based on the magnitudes of the nu(CO) shifts of the amide and ester substituents (Deltanu(CO)), reveals that the ester- or amide-derivatized ligands are the ultimate acceptors and that the excited electron is localized on one acceptor ligand on the nanosecond time scale. In the unsymmetrically substituted acceptor ligands, the excited electron is largely polarized toward the ester- or amide-derivatized pyridine rings. In the MLCT excited states of [Ru(bpy)(2)(4,4'-(CO(2)Et)(2)bpy)](2+) and [Ru(bpy)(2)(4,4'-(CONEt(2))(2)bpy)](2+), Deltanu(CO) is only 60-70% of that observed upon complete ligand reduction due to a strong polarization interaction in the excited state between the dpi(5) Ru(III) core and the excited electron. PMID:11670867

  5. Concerted electron-proton transfer in the optical excitation of hydrogen-bonded dyes

    SciTech Connect

    Westlake, Brittany C.; Brennaman, Kyle M.; Concepcion, Javier J.; Paul, Jared J.; Bettis, Stephanie E.; Hampton, Shaun D.; Miller, Stephen A.; Lebedeva, Natalia V.; Forbes, Malcolm D. E.; Moran, Andrew M.; Meyer, Thomas J.; Papanikolas, John M.

    2011-05-24

    The simultaneous, concerted transfer of electrons and protons—electron-proton transfer (EPT)—is an important mechanism utilized in chemistry and biology to avoid high energy intermediates. There are many examples of thermally activated EPT in ground-state reactions and in excited states following photoexcitation and thermal relaxation. Here we report application of ultrafast excitation with absorption and Raman monitoring to detect a photochemically driven EPT process (photo-EPT). In this process, both electrons and protons are transferred during the absorption of a photon. Photo-EPT is induced by intramolecular charge-transfer (ICT) excitation of hydrogen-bonded-base adducts with either a coumarin dye or 4-nitro-4'-biphenylphenol. Femtosecond transient absorption spectral measurements following ICT excitation reveal the appearance of two spectroscopically distinct states having different dynamical signatures. One of these states corresponds to a conventional ICT excited state in which the transferring H⁺ is initially associated with the proton donor. Proton transfer to the base (B) then occurs on the picosecond time scale. The other state is an ICT-EPT photoproduct. Upon excitation it forms initially in the nuclear configuration of the ground state by application of the Franck–Condon principle. However, due to the change in electronic configuration induced by the transition, excitation is accompanied by proton transfer with the protonated base formed with a highly elongated ⁺H–B bond. Coherent Raman spectroscopy confirms the presence of a vibrational mode corresponding to the protonated base in the optically prepared state.

  6. [Effective control of excitable waves in 2D cardiac excitable media].

    PubMed

    Li, Li; Liu, Li; Zhang, Guangcai; Wang, Guangrui; Qu, Zhi

    2005-12-01

    We propose a method for effective control of patter on dissipative system by use of little perturbation analysis, and apply this nonuniform feed back method to control the polarization wave of heart represented by FHN equation. In the numerical experiment, we successfully alter the propagating direction of planar waves and drift the spiral waves to boundary without resonant repulsion. The effective control of the excited system will be used to study the mechanism of defibrillation and that is our interesting work. PMID:16422076

  7. The possible role of anisotropy in kinetic electronic excitation of solids by particle bombardment

    NASA Astrophysics Data System (ADS)

    Heuser, C.; Marpe, M.; Diesing, D.; Wucher, A.

    2011-06-01

    The kinetic excitation of a solid surface by impact of energetic particles is investigated by means of internal electron emission across a buried metal-insulator-metal (MIM) tunnel junction. By bombarding the top metal surface of such a device with keV noble gas ions, internal emission yields were determined as a function of projectile impact energy and angle of incidence with respect to the surface normal. In order to understand the observed impact angle dependence, we apply a modified formalism originally published to describe external electron emission. As a result, we find that the measured data can be explained by assuming the spatial distribution of excited electrons propagating towards the buried oxide interface to be strongly influenced by the projectile impact angle. A simple ballistic model assuming excited electrons generated by direct collisions with the projectile to preferably propagate along the direction of the original projectile motion, while electrons excited by scattering from moving recoils propagate isotropically, appears to describe the observed experimental data quite well.

  8. Convergent-close-coupling calculations for excitation and ionization processes of electron-hydrogen collisions in Debye plasmas

    SciTech Connect

    Zammit, Mark C.; Fursa, Dmitry V.; Bray, Igor

    2010-11-15

    Electron-hydrogen scattering in weakly coupled hot-dense plasmas has been investigated using the convergent-close-coupling method. The Yukawa-type Debye-Hueckel potential has been used to describe the plasma screening effects. The target structure, excitation dynamics, and ionization process change dramatically as the screening is increased. Excitation cross sections for the 1s{yields}2s,2p,3s,3p,3d and 2s{yields}2p,3s,3p,3d transitions and total and total ionization cross sections for the scattering from the 1s and 2s states are presented. Calculations cover the energy range from thresholds to high energies (250 eV) for various Debye lengths. We find that as the screening increases, the excitation and total cross sections decrease, while the total ionization cross sections increase.

  9. Excitation threshold of Stimulated Electromagnetic Emissions SEEs generated at pump frequency near the third electron gyroharmonic

    NASA Astrophysics Data System (ADS)

    Mahmoudian, A.; Bernhardt, P. A.; Scales, W.

    2012-12-01

    The High-Frequency Active Auroral Research Program (HAARP) in Gakona, Alaska provides effective radiated powers in the megawatt range that have allowed researchers to study many non-linear effects of wave-plasma interactions. Stimulated Electromagnetic Emission (SEE) is of interest to the ionospheric community for its diagnostic purposes. In recent HAARP heating experiments, it has been shown that during the Magnetized Stimulated Brillouin Scattering MSBS instability, the pumped electromagnetic wave may decay into an electromagnetic wave and a low frequency electrostatic wave (either ion acoustic IA wave or electrostatic ion cyclotron EIC wave). Using Stimulated Electromagnetic Emission (SEE) spectral features, side bands which extend above and below the pump frequency can yield significant diagnostics for the modified ionosphere. It has been shown that the IA wave frequency offsets can be used to measure electron temperature in the heated ionosphere and EIC wave offsets can be used as a sensitive method to determine the ion species by measuring ion mass using the ion gyro-frequency offset. The threshold of each emission line has been measured by changing the amplitude of pump wave. The experimental results aimed to show the threshold for transmitter power to excite IA wave propagating along the magnetic field lines as well as for EIC wave excited at an oblique angle relative to the background magnetic field. Another parametric decay instability studied is the ion Bernstein decay instability that has been attributed to the simultaneous parametric decay of electron Bernstein waves into multiple electron Bernstein and ion Bernstein waves. The SIB process is thought to involve mode conversion from EM to EB waves followed by parametric decay of the EB wave to multiple EB and IB waves. The parametric decay instability of ion Bernstein modes has been observed simultaneously for the first time at the third electron gyroharmonics during 2011 Summer Student Research

  10. Microwave-Excited Microplasma Thrusters Using Surface Wave and Electron Cyclotron Resonance Discharges

    NASA Astrophysics Data System (ADS)

    Mori, Daisuke; Kawanabe, Tetsuo; Takao, Yoshinori; Eriguchi, Koji; Ono, Kouichi

    2012-10-01

    Downsizing spacecrafts has recently been focused on to decrease mission costs and to increase launch rates, and missions with small satellites would bring a great advantage of reducing their risks. Such a concept supports a new approach to developing precise, reliable, and low-cost micropropulsion systems. We have studied two types of microwave-excited microplasma thrusters, using surface wave-excited and electron cyclotron resonance-excited discharges. Microwaves of S-band (4 GHz) and X-band (11 GHz) were employed to excite the plasma in these experiments, with the feed or propellant gases of Ar and He. A microplasma thruster of electrothermal type consisted of a surface wave-excited microplasma source, and a converging-diverging micronozzle to obtain the thrust. For 11-GHz microwaves at a power of 6 W, a thrust of 1.1 mN and a specific impulse of 90 s were obtained at an Ar gas flow rate of 40 sccm, where the plasma electron density was 1.2x10^20 m-3, and the gas temperature was 1.5x10^3 K; under the same conditions for 4-GHz microwaves, the thrust, specific impulse, electron density, and gas temperature were 0.93 mN, 80 s, 7.0x10^19 m-3, and 8.0x10^2 K, respectively. A microplasma thruster of electromagnetic type had a microplasma source excited by electron cyclotron resonance with external magnetic fields, to obtain the thrust through accelerating ions by ambipolar electric fields. Optical emission spectrum was dominated by Ar^+ ion lines in the microplasma thruster of electromagnetic type, owing to higher electron temperatures at lower feed-gas pressures.

  11. Electron impact excitation rate coefficients for P-like Ni XIV

    SciTech Connect

    Wang, K.; Shanghai EBIT Lab, Institute of Modern Physics, Department of Nuclear Science and Technology, Fudan University, Shanghai 200433 ; Yan, J.; Center for Applied Physics and Technology, Peking University, Beijing 100871 ; Huang, M.; Shanghai EBIT Lab, Institute of Modern Physics, Department of Nuclear Science and Technology, Fudan University, Shanghai 200433 ; Li, C.Y.; Zeng, J.L.; Chen, C.Y.; Wang, Y.S.; Zou, Y.M.; Shanghai EBIT Lab, Institute of Modern Physics, Department of Nuclear Science and Technology, Fudan University, Shanghai 200433

    2012-07-15

    We have calculated the atomic data including electron impact excitations and radiative decays among the lowest 143 fine-structure levels arising from 3s{sup 2}3p{sup 3}, 3s3p{sup 4}, 3s{sup 2}3p{sup 2}3d, 3p{sup 5}, 3s3p{sup 3}3d, and 3s{sup 2}3p3d{sup 2} configurations in P-like Ni XIV. Direct excitation collision strengths are calculated employing the relativistic distorted-wave method. Resonances are included via the isolated resonance approximation using distorted-waves. Resonance contributions from S-like [3s{sup 2}3p{sup 3}, 3s3p{sup 4}, 3s{sup 2}3p{sup 2}3d,3p{sup 5}, 3s3p{sup 3}3d,3s{sup 2}3p3d{sup 2}, 3p{sup 4}3d,3s3p{sup 2}3d{sup 2},3s{sup 2}3d{sup 3}]n{sup Prime }l{sup Prime} complex series are taken into account. Effective collision strengths are reported over an electron temperature range of 1.0 Multiplication-Sign 10{sup 5}-1.0 Multiplication-Sign 10{sup 8} K. -- Highlights: Black-Right-Pointing-Pointer Radiative and collisional atomic data are presented for the lowest 143 fine-structure levels in P-like Ni XIV. Black-Right-Pointing-Pointer Calculations are performed using the FAC package. Black-Right-Pointing-Pointer Resonances enhance significantly a large amount of transitions. Black-Right-Pointing-Pointer Resonances play an important role of level population and line intensity ratios.

  12. Monitoring the Coherent Vibrational Control of Electronic Excitation Transfer Using Ultrafast Pump-Probe Polarization Spectroscopy

    NASA Astrophysics Data System (ADS)

    Biggs, Jason; Cina, Jeffrey

    2010-03-01

    The interplay between nuclear and electronic degrees of freedom in molecular energy-transfer complexes is a subject of current interest. We have proposed a method to use coherent nuclear motion to control the transfer of electronic excitation energy between donor and acceptor moieties in electronically coupled dimers. The underlying electronic and nuclear motion at the level of quantum mechanical amplitudes can be observed using nonlinear wave-packet interferometry(nl-WPI), a form of fluorescence-detected multidimensional electronic spectroscopy. In our control scheme, coherent nuclear motion is induced in the acceptor chromophore prior to direct electronic excitation of the donor. This nuclear motion affects the instantaneous resonance conditions between donor and acceptor moieties and thus affects subsequent energy transfer dynamics. We have developed the framework to simulate four-pulse nl-WPI experiments, and the pump-probe limit thereof, on energy-transfer systems after interaction with a control pulse that induces nuclear motion. We present simulations in the pump-probe limit from model energy-transfer systems subjected to prior impulsive vibrational excitation, and show how pulse polarization can be used to infer electronic dynamics from isotropically oriented dimers.

  13. Sub-nanometre resolution of atomic motion during electronic excitation in phase-change materials

    PubMed Central

    Mitrofanov, Kirill V.; Fons, Paul; Makino, Kotaro; Terashima, Ryo; Shimada, Toru; Kolobov, Alexander V.; Tominaga, Junji; Bragaglia, Valeria; Giussani, Alessandro; Calarco, Raffaella; Riechert, Henning; Sato, Takahiro; Katayama, Tetsuo; Ogawa, Kanade; Togashi, Tadashi; Yabashi, Makina; Wall, Simon; Brewe, Dale; Hase, Muneaki

    2016-01-01

    Phase-change materials based on Ge-Sb-Te alloys are widely used in industrial applications such as nonvolatile memories, but reaction pathways for crystalline-to-amorphous phase-change on picosecond timescales remain unknown. Femtosecond laser excitation and an ultrashort x-ray probe is used to show the temporal separation of electronic and thermal effects in a long-lived (>100 ps) transient metastable state of Ge2Sb2Te5 with muted interatomic interaction induced by a weakening of resonant bonding. Due to a specific electronic state, the lattice undergoes a reversible nondestructive modification over a nanoscale region, remaining cold for 4 ps. An independent time-resolved x-ray absorption fine structure experiment confirms the existence of an intermediate state with disordered bonds. This newly unveiled effect allows the utilization of non-thermal ultra-fast pathways enabling artificial manipulation of the switching process, ultimately leading to a redefined speed limit, and improved energy efficiency and reliability of phase-change memory technologies. PMID:26868451

  14. Sub-nanometre resolution of atomic motion during electronic excitation in phase-change materials

    NASA Astrophysics Data System (ADS)

    Mitrofanov, Kirill V.; Fons, Paul; Makino, Kotaro; Terashima, Ryo; Shimada, Toru; Kolobov, Alexander V.; Tominaga, Junji; Bragaglia, Valeria; Giussani, Alessandro; Calarco, Raffaella; Riechert, Henning; Sato, Takahiro; Katayama, Tetsuo; Ogawa, Kanade; Togashi, Tadashi; Yabashi, Makina; Wall, Simon; Brewe, Dale; Hase, Muneaki

    2016-02-01

    Phase-change materials based on Ge-Sb-Te alloys are widely used in industrial applications such as nonvolatile memories, but reaction pathways for crystalline-to-amorphous phase-change on picosecond timescales remain unknown. Femtosecond laser excitation and an ultrashort x-ray probe is used to show the temporal separation of electronic and thermal effects in a long-lived (>100 ps) transient metastable state of Ge2Sb2Te5 with muted interatomic interaction induced by a weakening of resonant bonding. Due to a specific electronic state, the lattice undergoes a reversible nondestructive modification over a nanoscale region, remaining cold for 4 ps. An independent time-resolved x-ray absorption fine structure experiment confirms the existence of an intermediate state with disordered bonds. This newly unveiled effect allows the utilization of non-thermal ultra-fast pathways enabling artificial manipulation of the switching process, ultimately leading to a redefined speed limit, and improved energy efficiency and reliability of phase-change memory technologies.

  15. Sub-nanometre resolution of atomic motion during electronic excitation in phase-change materials.

    PubMed

    Mitrofanov, Kirill V; Fons, Paul; Makino, Kotaro; Terashima, Ryo; Shimada, Toru; Kolobov, Alexander V; Tominaga, Junji; Bragaglia, Valeria; Giussani, Alessandro; Calarco, Raffaella; Riechert, Henning; Sato, Takahiro; Katayama, Tetsuo; Ogawa, Kanade; Togashi, Tadashi; Yabashi, Makina; Wall, Simon; Brewe, Dale; Hase, Muneaki

    2016-01-01

    Phase-change materials based on Ge-Sb-Te alloys are widely used in industrial applications such as nonvolatile memories, but reaction pathways for crystalline-to-amorphous phase-change on picosecond timescales remain unknown. Femtosecond laser excitation and an ultrashort x-ray probe is used to show the temporal separation of electronic and thermal effects in a long-lived (>100 ps) transient metastable state of Ge2Sb2Te5 with muted interatomic interaction induced by a weakening of resonant bonding. Due to a specific electronic state, the lattice undergoes a reversible nondestructive modification over a nanoscale region, remaining cold for 4 ps. An independent time-resolved x-ray absorption fine structure experiment confirms the existence of an intermediate state with disordered bonds. This newly unveiled effect allows the utilization of non-thermal ultra-fast pathways enabling artificial manipulation of the switching process, ultimately leading to a redefined speed limit, and improved energy efficiency and reliability of phase-change memory technologies. PMID:26868451

  16. Sub-nanometre resolution of atomic motion during electronic excitation in phase-change materials

    DOE PAGESBeta

    Mitrofanov, Kirill V.; Fons, Paul; Makino, Kotaro; Terashima, Ryo; Shimada, Toru; Kolobov, Alexander V.; Tominaga, Junji; Bragaglia, Valeria; Giussani, Alessandro; Calarco, Raffaella; et al

    2016-02-12

    Phase-change materials based on Ge-Sb-Te alloys are widely used in industrial applications such as nonvolatile memories, but reaction pathways for crystalline-to-amorphous phase-change on picosecond timescales remain unknown. Femtosecond laser excitation and an ultrashort x-ray probe is used to show the temporal separation of electronic and thermal effects in a long-lived (>100 ps) transient metastable state of Ge2Sb2Te5 with muted interatomic interaction induced by a weakening of resonant bonding. Due to a specific electronic state, the lattice undergoes a reversible nondestructive modification over a nanoscale region, remaining cold for 4 ps. An independent time-resolved x-ray absorption fine structure experiment confirms themore » existence of an intermediate state with disordered bonds. Furthermore, this newly unveiled effect allows the utilization of non-thermal ultra-fast pathways enabling artificial manipulation of the switching process, ultimately leading to a redefined speed limit, and improved energy efficiency and reliability of phase-change memory technologies.« less

  17. Direct Delta-MBPT(2) method for ionization potentials, electron affinities, and excitation energies using fractional occupation numbers

    SciTech Connect

    Beste, Ariana; Vazquez-Mayagoitia, Alvaro; Ortiz, J. Vincent

    2013-01-01

    A direct method (D-Delta-MBPT(2)) to calculate second-order ionization potentials (IPs), electron affinities (EAs), and excitation energies is developed. The Delta-MBPT(2) method is defined as the correlated extension of the Delta-HF method. Energy differences are obtained by integrating the energy derivative with respect to occupation numbers over the appropriate parameter range. This is made possible by writing the second-order energy as a function of the occupation numbers. Relaxation effects are fully included at the SCF level. This is in contrast to linear response theory, which makes the D-Delta-MBPT(2) applicable not only to single excited but also higher excited states. We show the relationship of the D-Delta-MBPT(2) method for IPs and EAs to a second-order approximation of the effective Fock-space coupled-cluster Hamiltonian and a second-order electron propagator method. We also discuss the connection between the D-Delta-MBPT(2) method for excitation energies and the CIS-MP2 method. Finally, as a proof of principle, we apply our method to calculate ionization potentials and excitation energies of some small molecules. For IPs, the Delta-MBPT(2) results compare well to the second-order solution of the Dyson equation. For excitation energies, the deviation from EOM-CCSD increases when correlation becomes more important. When using the numerical integration technique, we encounter difficulties that prevented us from reaching the Delta-MBPT(2) values. Most importantly, relaxation beyond the Hartree Fock level is significant and needs to be included in future research.

  18. Kinetic studies of Kr2F/asterisk/ in electron-beam excited mixtures

    NASA Astrophysics Data System (ADS)

    Luches, A.; Nassisi, V.; Perrone, A.; Perrone, M. R.

    1982-12-01

    The results of an examination of the formation and quenching processes of excited-state rare gas-halogen laser mixtures are presented. Attention was given to Kr-SF6 and Kr-NF3 mixtures in ArKrNF3, ArKrSF6, and ArKrF2 mixtures. Electron beam pulses in the 100-1000 mbar range were employed at 10 kA, 350 eV, with 15 ns repetition. Reaction kinetics for the formation and quenching of trimers are defined quantitatively in terms of the three-body reaction and an exoenergic reaction. Spectroscopic measurements of the fluorescence produced with excited Kr2F are reported, as are the subsequently determined rate constants. The production of excited Kr2 was found to be the most critical formation channel of excited Kr2F.

  19. Electron-impact excitation rate-coefficients and polarization of subsequent emission for Ar+ ion

    NASA Astrophysics Data System (ADS)

    Dipti; Srivastava, Rajesh

    2016-06-01

    Electron impact excitation in Ar+ ions has been studied by using fully relativistic distorted wave theory. Calculations are performed to obtain the excitation cross-sections and rate-coefficients for the transitions from the ground state 3p5 (J=3/2) to fine-structure levels of excited states 3p44s, 3p44p, 3p45s, 3p45p, 3p43d and 3p44d. Polarization of the radiation following the excitation has been calculated using the obtained magnetic sub-level cross-sections. Comparison of the present rate-coefficients is also done with the previously reported theoretical results for some unresolved fine structure transitions.

  20. Rate-coefficients and polarization results for the electron-impact excitation of Ar+ ion

    NASA Astrophysics Data System (ADS)

    Srivastava, Rajesh; Dipti, Dipti

    2016-05-01

    A fully relativistic distorted wave theory has been employed to study the electron impact excitation in Ar+ ion. Results have been obtained for the excitation cross-sections and rate-coefficients for the transitions from the ground state 3p5 (J = 3/2) to fine-structure levels of excited states 3p4 4 s, 3p4 4 p , 3p4 5 s, 3p4 5 p, 3p4 3 d and 3p4 4 d. Polarization of the radiation following the excitation has been calculated using the obtained magnetic sub-level cross-sections. Comparison of the present rate-coefficients is also done with the previously reported theoretical results for some unresolved fine structure transitions. Work is supported by DAE-BRNS Mumbai and CSIR, New Delhi.

  1. Investigation of plasma excitation. volume i. electron impact studies of selected ground state and excited state rare gas atoms. Final report 7 Jun 77-20 Sep 80

    SciTech Connect

    Lake, M.L.

    1981-08-01

    Experiments were undertaken to determine electron impact cross sections of atoms in metastable states. One or two electron guns were used to first produce atoms in metastable states, then further excite these atoms to other levels. Limits on certain cross sections of helium atoms were obtained, but the detection limits of the apparatus prevented exhaustive study. Excitation functions and cross sections of xenon were obtained in the wavelength range from 3000 A to 9000 A.

  2. Possible interaction between thermal electrons and vibrationally excited N2 in the lower E-region

    NASA Astrophysics Data System (ADS)

    Oyama, K.-I.; Shimoyama, M.; Liu, J. Y.; Cheng, C. Z.

    2011-03-01

    As one of the tasks to find the energy source(s) of thermal electrons, which elevate(s) electron temperature higher than neutral temperature in the lower ionosphere E-region, energy distribution function of thermal electron was measured with a sounding rocket at the heights of 93-131 km by the applying second harmonic method. The energy distribution function showed a clear hump at the energy of ~0.4 eV. In order to find the reason of the hump, we conducted laboratory experiment. We studied difference of the energy distribution functions of electrons in thermal energy range, which were measured with and without EUV radiation to plasma of N2/Ar and N2/O2 gas mixture respectively. For N2/Ar gas mixture plasma, the hump is not clearly identified in the energy distribution of thermal electrons. On the other hand for N2/O2 gas mixture, which contains vibrationally excited N2, a clear hump is found when irradiated by EUV. The laboratory experiment seems to suggest that the hump is produced as a result of interaction between vibrationally excited N2 and thermal electrons, and this interaction is the most probable heating source for the electrons of thermal energy range in the lower E-region. It is also suggested that energy distribution of the electrons in high energy part may not be Maxwellian, and DC probe measures the electrons which are non Maxwellian, and therefore "electron temperature" is calculated higher.

  3. Electronic noise in high electron-mobility transistors under photo-excitation conditions

    SciTech Connect

    Marinchio, H.; Sabatini, G.; Varani, L.; Palermo, C.; Shiktorov, P.; Starikov, E.; Gruzinskis, V.; Ziade, P.; Kallassy, Z.

    2009-04-23

    The hydrodynamic approach based on the carrier concentration and velocity conservation equations is used to investigate the influence of photo-excitation of plasma waves at the beating frequency of two lasers on the intrinsic extra noise in InGaAs HEMTs caused by thermally-induced plasma oscillations. It is found that, by increasing the amplitude of the photo-excitation, a significant supression of the intrinsic excess noise is observed at the beating frequency as well as at all the frequencies where plasma waves can be excited.

  4. Simultaneous ionization and excitation of helium by electron impact

    NASA Astrophysics Data System (ADS)

    Dal Cappello, C.; Roy, A. C.; Ren, X. G.; Dey, R.

    2008-02-01

    We present numerical results for He (1s2) (e, 2e) He+ reaction process for transitions to the n = 1, 2 and 3 states of He+ for noncoplanar symmetric geometry at incident energies of 1000 and 1600 eV. The calculations are performed using the plane wave impulse approximation (PWIA) and the 3C method (also called the Brauner, Briggs and Klar (BBK) model) that includes post collision interaction and multiple scattering effects. In both the methods we have used the highly correlated configuration interaction wave function for the ground state of helium. A comparison of the present theoretical cross sections with the recent measured data of Ren et al. [X.G. Ren, C.G. Ning, J.K. Deng, G.L. Su, S.F. Zhang, Y.R. Huang, G.Q. Li, Phys. Rev. A 72 (2005) 042718] shows reasonably good agreement.

  5. Electron collisional excitation and resonant photoexcitation of solar S XI

    NASA Technical Reports Server (NTRS)

    Kastner, S. O.; Bhatia, A. K.

    1986-01-01

    The line emission of carbon-like S XI is predicted using a comprehensive 46-level model including the configurations 2p2, 2s2p3, 2p3s, 2p4, 2p3p, 2p3d. Relative intensities of allowed, intercombination, and forbidden lines are computed for quiet and active solar conditions. The process of photoexcitation by the Fe XIII 191.26 A line is included to study its effect on EUV lines and the infrared forbidden lines at 1.92 and 1.39 microns. It is concluded that an observation of the 1.92-micron line by Olsen, Anderson, and Stewart (1971) is consistent with quiet solar conditions in the absence of photoexcitation.

  6. Electron-impact excitation of the n 1P levels of helium - Theory and experiment

    NASA Technical Reports Server (NTRS)

    Cartwright, David C.; Csanak, George; Trajmar, Sandor; Register, D. F.

    1992-01-01

    New experimental electron-energy-loss data have been used to extract differential and integral cross sections for excitation of the 2 1P level, and for the overlapping (3 1P, 3 1D, 3 3D) levels of helium, at 30-, 50-, and 100-eV incident electron energies. First-order many-body theory (FOMBT) has been used to calculate the differential and integral cross sections for excitation of the n 1P (n = 2,...,6) levels of helium by electron impact, for incident electron energies from threshold to 500 eV. Detailed comparisons between these two new sets of data are made as well as comparisons with appropriate published experimental and theoretical results. A simple scaling relationship is derived from the FOMBT results for n = 2,...,6 that provides differential and integral cross sections for all symmetry final levels of helium with n = 6 or greater.

  7. Highly charged ion induced nanostructures at surfaces by strong electronic excitations

    NASA Astrophysics Data System (ADS)

    Wilhelm, Richard A.; El-Said, Ayman S.; Krok, Franciszek; Heller, René; Gruber, Elisabeth; Aumayr, Friedrich; Facsko, Stefan

    2015-08-01

    Nanostructure formation by single slow highly charged ion impacts can be associated with high density of electronic excitations at the impact points of the ions. Experimental results show that depending on the target material these electronic excitations may lead to very large desorption yields in the order of a few 1000 atoms per ion or the formation of nanohillocks at the impact site. Even in ultra-thin insulating membranes the formation of nanometer sized pores is observed after ion impact. In this paper, we show recent results on nanostructure formation by highly charged ions and compare them to structures and defects observed after intense electron and light ion irradiation of ionic crystals and graphene. Additional data on energy loss, charge exchange and secondary electron emission of highly charged ions clearly show that the ion charge dominates the defect formation at the surface.

  8. Intermediate energy electron impact excitation of composite vibrational modes in phenol

    SciTech Connect

    Neves, R. F. C.; Jones, D. B.; Lopes, M. C. A.; Nixon, K. L.; Oliveira, E. M. de; Lima, M. A. P.; Costa, R. F. da; Varella, M. T. do N.; Bettega, M. H. F.; Silva, G. B. da; Brunger, M. J.

    2015-05-21

    We report differential cross section results from an experimental investigation into the electron impact excitation of a number of the low-lying composite (unresolved) vibrational modes in phenol (C{sub 6}H{sub 5}OH). The measurements were carried out at incident electron energies in the range 15–40 eV and for scattered-electron angles in the range 10–90°. The energy resolution of those measurements was typically ∼80 meV. Calculations, using the GAMESS code, were also undertaken with a B3LYP/aug-cc-pVDZ level model chemistry, in order to enable us to assign vibrational modes to the features observed in our energy loss spectra. To the best of our knowledge, the present cross sections are the first to be reported for vibrational excitation of the C{sub 6}H{sub 5}OH molecule by electron impact.

  9. Injection locking of an electronic maser in the hard excitation mode

    SciTech Connect

    Yakunina, K. A.; Kuznetsov, A. P.; Ryskin, N. M.

    2015-11-15

    The phenomenon of hard excitation is natural for many electronic oscillators. In particular, in a gyrotron, a maximal efficiency is often attained in the hard excitation regime. In this paper, we study the injection-locking phenomena using two models of an electronic maser in the hard excitation mode. First, bifurcation analysis is performed for the quasilinear model described by ordinary differential equations for the slow amplitude and phase. Two main scenarios of transition to the injection-locked mode are described, which are generalizations of the well-known phase-locking and suppression mechanisms. The results obtained for the quasilinear model are confirmed by numerical simulations of a gyrotron with fixed Gaussian structure of the RF field.

  10. An optimized configuration interaction method for calculating electronic excitations in nanostructures

    SciTech Connect

    Troparevsky, M Claudia; Franceschetti, Alberto G

    2008-01-01

    The configuration interaction method has been widely used to calculate electronic excitations in nanostructures, but it suffers from a slow rate of convergence with the number of configurations in the basis set and from the inability to select a priori the most important configurations. The optimized configuration interaction method presented here removes the limitations of the conventional approach by identifying at the outset the configurations that are most relevant for describing electronic excitations. We show that the best configurations are remarkably different from the configurations that one would expect on the basis of the single-particle energy ladder, and that a small, optimized set of configurations predicts excitation energies with accuracy comparable to that for much larger, non-optimized sets of configurations. This approach opens the way to a new generation of configuration interaction methods where the configurations are pre-selected using heuristic search methods.

  11. Injection locking of an electronic maser in the hard excitation mode

    NASA Astrophysics Data System (ADS)

    Yakunina, K. A.; Kuznetsov, A. P.; Ryskin, N. M.

    2015-11-01

    The phenomenon of hard excitation is natural for many electronic oscillators. In particular, in a gyrotron, a maximal efficiency is often attained in the hard excitation regime. In this paper, we study the injection-locking phenomena using two models of an electronic maser in the hard excitation mode. First, bifurcation analysis is performed for the quasilinear model described by ordinary differential equations for the slow amplitude and phase. Two main scenarios of transition to the injection-locked mode are described, which are generalizations of the well-known phase-locking and suppression mechanisms. The results obtained for the quasilinear model are confirmed by numerical simulations of a gyrotron with fixed Gaussian structure of the RF field.

  12. Electronic excitation induced modification in fullerene C70 thin films

    NASA Astrophysics Data System (ADS)

    Sharma, Pooja; Singhal, R.; Banerjee, M. K.; Vishnoi, R.; Kaushik, R.; Singh, F.

    2016-07-01

    Fullerene C70 thin films were deposited by resistive heating on glass substrates and the thickness were approximated to be 150 nm. The effect of energy deposition by 55 MeV Si ions on the optical and structural properties of the prepared thin film samples is investigated. The samples were irradiated with 55 MeV Si ions within fluence range from 1 × 1012 to 3 × 1013 ions/cm2. For optical studies, the pristine and the Si ion irradiated samples are examined by UV-visible absorption spectroscopy and Raman spectroscopy. UV-visible absorption studies reveal that the absorption peaks of irradiated samples decrease with a decrease in the band gap of the thin films. The damage cross-section (σ) and radius of damaged cylindrical zone (r) are determined as ∼0.6 × 10-13 cm2 and ∼1.41 nm, respectively from the Raman spectra. Raman studies also suggest that at higher fluence (up to 3 × 1013 ions/cm2), the damage caused by the SHI results in partial amorphization of fullerene C70 thin film. Modification in the surface properties has been investigated by atomic force microscopy; it has revealed that the roughness decreases and average particle size increases with the increase in fluences.

  13. Electron-ion collisions. [Basic physics of inelastic processes of excitation, ionization, and recombination

    SciTech Connect

    Crandall, D.H.

    1982-01-01

    This discussion concentrates on basic physics aspects of inelastic processes of excitation, ionization, and recombination that occur during electron-ion collisions. Except for cases of illustration along isoelectronic sequences, only multicharged (at least +2) ions will be specifically discussed with some emphasis of unique physics aspects associated with ionic charge. The material presented will be discussed from a primarily experimental viewpoint with most attention to electron-ion interacting beams experiments.

  14. Current status of free radicals and electronically excited metastable species as high energy propellants

    NASA Technical Reports Server (NTRS)

    Rosen, G.

    1973-01-01

    A survey is presented of free radicals and electronically excited metastable species as high energy propellants for rocket engines. Nascent or atomic forms of diatomic gases are considered free radicals as well as the highly reactive diatomic triatomic molecules that posess unpaired electrons. Manufacturing and storage problems are described, and a review of current experimental work related to the manufacture of atomic hydrogen propellants is presented.

  15. Radiative rates and electron impact excitation rate coefficients for Ne-like selenium, Se XXV

    SciTech Connect

    Wang, K.; Chen, C.Y. Huang, M.; Wang, Y.S.; Zou, Y.M.

    2011-07-15

    In this article we report calculations of energy levels, radiative rates, electron impact collision strengths, and effective collision strengths for transitions among the 241 fine-structure levels arising from 2l{sup 8} and 2l{sup 7}n{sup '}l{sup '} (n{sup '{<=}}6 and l{sup '{<=}}n{sup '}-1) configurations of Ne-like Se XXV using the Flexible Atomic Code. Energy levels and radiative rates are calculated within the relativistic configuration-interaction method. Direct excitation collision strengths are calculated using the relativistic distorted-wave approximation and high-energy collision strengths are obtained in the relativistic plane-wave approximation. Resonance contributions through the relevant Na-like doubly-excited configurations 2l{sup 7}n'l'n''l'' (3{<=}n'{<=}7, l'{<=}n'-1, n'{<=}n''{<=}50, and l''{<=}8) are explicitly taken into account via the independent-process and isolated-resonance approximation using distorted waves. Resonant stabilizing transitions and possibly important radiative decays from the resonances toward low-lying autoionizing levels are considered. In addition, the resonance contributions from Na-like 2l{sup 6}3l'3l'''n''' (n'''=3-6) configurations are included and found to be predominant for many transitions among the singly-excited states in Ne-like Se XXV. We present the radiative rates, oscillator strengths, and line strengths for all electric dipole, magnetic dipole, electric quadrupole, magnetic quadrupole, electric octopole, and magnetic octopole transitions among the 241 levels. The effective collision strengths are reported for all 28920 transitions among the 241 levels over a wide temperature range up to 10 keV. To assess the reliability and accuracy of the present collisional data, we have performed a 27-state close-coupling calculation, employing the Dirac R-matrix theory. The results from the close-coupling calculation and the independent-process calculation for the identical target states are found to be in good agreement

  16. Excitation of the a {sup 3{Pi}} state of CO by electron impact

    SciTech Connect

    Ristic, M. M.; Poparic, G. B.; Belic, D. S.

    2011-04-15

    Electron impact excitation of the a {sup 3{Pi}} valence state of the carbon-monoxide molecule has been studied in the energy region from threshold to 10 eV. Excitation functions for spin forbidden transitions from the {nu}=0 level of the ground X {sup 1}{Sigma}{sup +} state of CO to the {nu}{sup '}=0, 1, 2, 3, 4, and 5 levels of the a {sup 3{Pi}} state are measured. A crossed beam double trochoidal electron spectrometer is used. Forward and backward scattered electrons from the {nu}{sup '}=0 excitation channel are separated by electron beam modulation and a time-of-flight detection technique. The present results are normalized to the ground state {sup 2{Pi}} resonance vibrational excitation cross sections and absolute values of the differential cross sections at the border angles of 0 deg. and 180 deg. are determined. In this way the differential cross section measurements are completed in the full angular range from 0 deg. to 180 deg. The present results are compared to the existing literature data.

  17. Electron-impact excitation-autoionization of helium in the S-wave limit

    SciTech Connect

    Horner, Daniel A.; McCurdy, C. William; Rescigno, Thomas N.

    2004-10-01

    Excitation of the autoionizing states of helium by electron impact is shown in calculations in the s-wave limit to leave a clear signature in the singly differential cross section for the (e,2e) process. It is suggested that such behavior should be seen generally in (e,2e) experiments on atoms that measure the single differential cross section.

  18. Relativistic atomic structure calculations and electron impact excitations of Fe23+

    NASA Astrophysics Data System (ADS)

    El-Maaref, A. A.

    2016-02-01

    Relativistic calculations using the multiconfiguration Dirac-Fock method for energy levels, oscillator strengths, and electronic dipole transition probabilities of Li-like iron (Fe23+) are presented. A configuration state list with the quantum numbers nl, where n = 2 - 7 and l = s , p , d , f , g , h , i has been considered. Excitations up to three electrons and correlation contributions from higher orbitals up to 7 l have been included. Contributions from core levels have been taken into account, EOL (extended optimal level) type calculations have been applied, and doubly excited levels are considered. The calculations have been executed by using the fully relativistic atomic structure package GRASP2K. The present calculations have been compared with the available experimental and theoretical sources, the comparisons show a good agreement between the present results of energy levels and oscillator strengths with the literature. In the second part of the present study, the atomic data (energy levels, and radiative parameters) have been used to calculate the excitation and deexcitation rates of allowed transitions by electron impact, as well as the population densities of some excited levels at different electron temperatures.

  19. Excited state dipole moments of chloroanilines and chlorophenols from solvatochromic shifts in electronic absorption spectra: Support for the concept of excited state group moments

    NASA Astrophysics Data System (ADS)

    Prabhumirashi, L. S.; Satpute, R. S.

    The dipole moments of isomeric o-, m- and p-chloroanilines and chlorophenols in electronically excited L a and L b states are estimated from solvent induced polarization shifts in electronic absorption spectra. It is observed that μ e( L a) > μ e( L b) > μ g, which is consistent with the general theory of polarization red shift. The μ es are found to be approximately co-linear with the corresponding μ gs. The concept of group moments is extended to aromatic molecules in excited states. This approach is found to be useful in understanding correlations among the excited states of mono- and disubstituted benzenes.

  20. Computational simulation and interpretation of the low-lying excited electronic states and electronic spectrum of thioanisole.

    PubMed

    Li, Shaohong L; Xu, Xuefei; Truhlar, Donald G

    2015-08-21

    Three singlet states, namely a closed-shell ground state and two excited states with (1)ππ* and (1)nσ* character, have been suggested to be responsible for the radiationless decay or photochemical reaction of photoexcited thioanisole. The correct interpretation of the electronic spectrum is critical for understanding the character of these low-lying excited states, but the experimental spectrum is yet to be fully interpreted. In the work reported here, we investigated the nature of those three states and a fourth singlet state of thioanisole using electronic structure calculations by multireference perturbation theory, by completely-renormalized equation-of-motion coupled cluster theory with single and double excitations and noniterative inclusion of connected triples (CR-EOM-CCSD(T)), and by linear-response time-dependent density functional theory (TDDFT). We clarified the assignment of the electronic spectrum by simulating it using a normal-mode sampling approach combined with TDDFT in the Tamm-Dancoff approximation (TDA). The understanding of the electronic states and of the accuracy of the electronic structure methods lays the foundation of our future work of constructing potential energy surfaces. PMID:26088195

  1. A Doubles Correction to Electronic Excited States from Configuration Interaction in the Space of Single Substitutions

    NASA Technical Reports Server (NTRS)

    Head-Gordon, Martin; Rico, Rudolph J.; Lee, Timothy J.; Oumi, Manabu

    1994-01-01

    A perturbative correction to the method of configuration interaction with single substitutions (CIS) is presented. This CIS(D) correction approximately introduces the effect of double substitutions which are absent in CIS excited states. CIS(D) is a second-order perturbation expansion of the coupled-cluster excited state method, restricted to single and double substitutions, in a series in which CIS is zeroth order, and the first-order correction vanishes. CIS (D) excitation energies are size consistent and the calculational complexity scales with the fifth power of molecular size, akin to second-order Moller-Plesset theory for the ground state. Calculations on singlet excited states of ethylene, formaldehyde, acetaldehyde, butadiene and benzene show that CIS (D) is a uniform improvement over CIS. CIS(D) appears to be a promising method for examining excited states of large molecules, where more accurate methods are not feasible.

  2. Excited-state evolution probed by convoy-electron emission in relativistic heavy-ion collisions

    NASA Astrophysics Data System (ADS)

    Takabayashi, Y.; Ito, T.; Azuma, T.; Komaki, K.; Yamazaki, Y.; Tawara, H.; Takada, E.; Murakami, T.; Seliger, M.; Tökési, K.; O. Reinhold, C.; Burgdörfer, J.

    2003-10-01

    We present a joint experimental and theoretical study of convoy-electron emission resulting from highly-charged-ion transport through carbon foils at moderately relativistic speeds. Energy spectra of electrons ejected at 0° have been measured for 390 MeV/u hydrogen-like Ar17+ ions and 460 MeV/u (β=v/c=0.74,γ=1.49) Fe25+ (1s), Fe24+ (1s2), and Fe23+ (1s22s) incident on carbon foils with thicknesses from 25 to 8700 μg/cm2. Due to this unprecedented wide range of thicknesses, the sequential excitation and ionization of initially deeply bound electrons to highly excited states and continuum states can be followed in considerable detail. The analysis of the spectra is aided by simulations based on the classical transport theory which has been extended to relativistic energies and to multielectron projectiles. The motion of the projectile electron inside the solid target is calculated taking into account the Coulomb potential of the projectile ion and the multiple stochastic collisions with target cores and target electrons. Different phases of the convoy-electron emissions can be disentangled: direct ejection to the continuum, the transient buildup of an excited-state wave packet followed by ionization, and postionization modification of the continuum spectrum. We find good agreement between experiment and simulation for the evolution of charge states and the emission spectrum.

  3. Excitation of kinetic Alfvén waves by fast electron beams

    SciTech Connect

    Chen, L.; Wu, D. J.; Zhao, G. Q.; Tang, J. F.; Huang, J. E-mail: djwu@pmo.ac.cn E-mail: jftang@xao.ac.cn

    2014-09-20

    Energetic electron beams, which are ubiquitous in a large variety of active phenomena in space and astrophysical plasmas, are one of the most important sources that drive plasma instabilities. In this paper, taking account of the return-current effect of fast electron beams, kinetic Alfvén wave (KAW) instability driven by a fast electron beam is investigated in a finite-β plasma of Q < β < 1 (where β is the kinetic-to-magnetic pressure ratio and Q ≡ m{sub e} /m{sub i} is the mass ratio of electrons to ions). The results show that the kinetic resonant interaction of beam electrons is the driving source for KAW instability, unlike the case driven by a fast ion beam, where both the kinetic resonant interaction of beam ions and the return-current are the driving source for the KAW instability. KAW instability has a nonzero growth rate in the range of the perpendicular wave number, 0electron beam v{sub b} , and the most favorable beam velocity occurs between 8v{sub A} < v{sub b} < 10v{sub A} . On the other hand, the excited KAWs are weakly dispersive with k ρ {sub i} < 1 and have the maximum growth rate at relatively low perpendicular wave numbers in the range 0.3electron beams in the terrestrial magnetosphere is briefly discussed.

  4. On the internal rotations in p-cresol in its ground and first electronically excited states

    NASA Astrophysics Data System (ADS)

    Hellweg, Arnim; Hättig, Christof

    2007-07-01

    The overall rotation and internal rotation of p-cresol (4-methyl-phenol) has been studied by comparison of the microwave spectrum with accurate ab initio calculations using the principal axis method in the electronic ground state. Both internal rotations, the torsions of the methyl and the hydroxyl groups relative to the aromatic ring, have been investigated. The internal rotation of the hydroxyl group can be approximately described as the motion of a symmetrical rotor on an asymmetric frame. For the methyl group it has been found that the potential barrier hindering its internal rotation is very small with the first two nonvanishing Fourier coefficients of the potential V3 and V6 in the same order of magnitude. Different splittings of b-type transitions for the A and E species of the methyl torsion indicate a top-top interaction between both internal rotors through the benzene ring. An effective coupling potential for the top-top interaction could be estimated. The hindering barriers of the hydroxyl and methyl rotation have been calculated using second-order Møller-Plesset perturbation theory and the approximate coupled-cluster singles-and-doubles model (CC2) in the ground state and using CC2 and the algebraic diagrammatic construction through second order in the first electronically excited state. The results are in excellent agreement with the experimental values.

  5. Quantum propagation of electronic excitations in macromolecules: A computationally efficient multiscale approach

    NASA Astrophysics Data System (ADS)

    Schneider, E.; a Beccara, S.; Mascherpa, F.; Faccioli, P.

    2016-07-01

    We introduce a theoretical approach to study the quantum-dissipative dynamics of electronic excitations in macromolecules, which enables to perform calculations in large systems and cover long-time intervals. All the parameters of the underlying microscopic Hamiltonian are obtained from ab initio electronic structure calculations, ensuring chemical detail. In the short-time regime, the theory is solvable using a diagrammatic perturbation theory, enabling analytic insight. To compute the time evolution of the density matrix at intermediate times, typically ≲ps , we develop a Monte Carlo algorithm free from any sign or phase problem, hence computationally efficient. Finally, the dynamics in the long-time and large-distance limit can be studied combining the microscopic calculations with renormalization group techniques to define a rigorous low-resolution effective theory. We benchmark our Monte Carlo algorithm against the results obtained in perturbation theory and using a semiclassical nonperturbative scheme. Then, we apply it to compute the intrachain charge mobility in a realistic conjugated polymer.

  6. Electronic Structure and Dynamics of Higher-Lying Excited States in Light Harvesting Complex 1 from Rhodobacter sphaeroides.

    PubMed

    Dahlberg, Peter D; Ting, Po-Chieh; Massey, Sara C; Martin, Elizabeth C; Hunter, C Neil; Engel, Gregory S

    2016-06-23

    Light harvesting in photosynthetic organisms involves efficient transfer of energy from peripheral antenna complexes to core antenna complexes, and ultimately to the reaction center where charge separation drives downstream photosynthetic processes. Antenna complexes contain many strongly coupled chromophores, which complicates analysis of their electronic structure. Two-dimensional electronic spectroscopy (2DES) provides information on energetic coupling and ultrafast energy transfer dynamics, making the technique well suited for the study of photosynthetic antennae. Here, we present 2DES results on excited state properties and dynamics of a core antenna complex, light harvesting complex 1 (LH1), embedded in the photosynthetic membrane of Rhodobacter sphaeroides. The experiment reveals weakly allowed higher-lying excited states in LH1 at 770 nm, which transfer energy to the strongly allowed states at 875 nm with a lifetime of 40 fs. The presence of higher-lying excited states is in agreement with effective Hamiltonians constructed using parameters from crystal structures and atomic force microscopy (AFM) studies. The energy transfer dynamics between the higher- and lower-lying excited states agree with Redfield theory calculations. PMID:27232937

  7. Using wave-packet interferometry to monitor the external vibrational control of electronic excitation transfer

    NASA Astrophysics Data System (ADS)

    Biggs, Jason D.; Cina, Jeffrey A.

    2009-12-01

    We investigate the control of electronic energy transfer in molecular dimers through the preparation of specific vibrational coherences prior to electronic excitation, and its observation by nonlinear wave-packet interferometry (nl-WPI). Laser-driven coherent nuclear motion can affect the instantaneous resonance between site-excited electronic states and thereby influence short-time electronic excitation transfer (EET). We first illustrate this control mechanism with calculations on a dimer whose constituent monomers undergo harmonic vibrations. We then consider the use of nl-WPI experiments to monitor the nuclear dynamics accompanying EET in general dimer complexes following impulsive vibrational excitation by a subresonant control pulse (or control pulse sequence). In measurements of this kind, two pairs of polarized phase-related femtosecond pulses following the control pulse generate superpositions of coherent nuclear wave packets in optically accessible electronic states. Interference contributions to the time- and frequency-integrated fluorescence signals due to overlaps among the superposed wave packets provide amplitude-level information on the nuclear and electronic dynamics. We derive the basic expression for a control-pulse-dependent nl-WPI signal. The electronic transition moments of the constituent monomers are assumed to have a fixed relative orientation, while the overall orientation of the complex is distributed isotropically. We include the limiting case of coincident arrival by pulses within each phase-related pair in which control-influenced nl-WPI reduces to a fluorescence-detected pump-probe difference experiment. Numerical calculations of pump-probe signals based on these theoretical expressions are presented in the following paper [J. D. Biggs and J. A. Cina, J. Chem. Phys. 131, 224302 (2009)].

  8. Gapped excitations of unconventional fractional quantum Hall effect states in the second Landau level

    NASA Astrophysics Data System (ADS)

    Wurstbauer, U.; Levy, A. L.; Pinczuk, A.; West, K. W.; Pfeiffer, L. N.; Manfra, M. J.; Gardner, G. C.; Watson, J. D.

    2015-12-01

    We report the observation of low-lying collective charge and spin excitations in the second Landau level at ν =2 +1 /3 and also for the very fragile states at ν =2 +2 /5 and 2 +3 /8 in inelastic light scattering experiments. These modes exhibit a clear dependence on filling factor and temperature substantiating the unique access to the characteristic neutral excitation spectra of the incompressible fractional quantum Hall effect (FQHE) states. A detailed mode analysis reveals low-energy modes at around 70 μ eV and a sharp mode slightly below the Zeeman energy interpreted as gap and spin-wave excitation, respectively. The lowest-energy collective charge excitation spectrum at ν =2 +1 /3 exhibits significant qualitative similarities with its cousin state in the lowest Landau level at ν =1 /3 suggesting similar magnetoroton minima in the neutral excitations. The mode energies differ by a scaling of 0.15 indicating different interaction physics in the N =0 and N =1 Landau levels. The striking polarization dependence in elastic and inelastic light scattering is discussed in the framework of anisotropic electron phases that allow for the stabilization of nematic FQHE states. The observed excitation spectra provide new insights by accessing quantum phases in the bulk of electron systems and facilitate comparison with different theoretical descriptions of those enigmatic FQHE states.

  9. Ground- and excited-state electronic structure of an iron-containing molecular spin photoswitch

    NASA Astrophysics Data System (ADS)

    Rodriguez, Jorge H.

    2005-09-01

    The electronic structure of the cation of [Fe(ptz)6](BF4)2, a prototype of a class of complexes that display light-induced excited-state spin trapping (LIESST), has been investigated by time-independent and time-dependent density-functional theories. The density of states of the singlet ground state reveals that the highest occupied orbitals are metal centered and give rise to a low spin configuration Fe2+(3dxy↑↓3dxz↑↓3dyz↑↓) in agreement with experiment. Upon excitation with light in the 2.3-3.3eV range, metal-centered spin-allowed but parity-forbidden ligand field (LF) antibonding states are populated which, in conjunction with electron-phonon coupling, explain the experimental absorption intensities. The computed excitation energies are in excellent agreement with experiment. Contrary to simpler models we show that the LF absorption bands, which are important for LIESST, do not originate in transitions from the ground to a single excited state but from transitions to manifolds of nearly degenerate excited singlets. Consistent with crystallography, population of the LF states promotes a drastic dilation of the ligand cage surrounding the iron.

  10. Fluorescence excitation and ultraviolet absorption spectra and theoretical calculations for benzocyclobutane: Vibrations and structure of its excited S{sub 1}(π,π{sup *}) electronic state

    SciTech Connect

    Shin, Hee Won; Ocola, Esther J.; Laane, Jaan; Kim, Sunghwan

    2014-01-21

    The fluorescence excitation spectra of jet-cooled benzocyclobutane have been recorded and together with its ultraviolet absorption spectra have been used to assign the vibrational frequencies for this molecule in its S{sub 1}(π,π{sup *}) electronic excited state. Theoretical calculations at the CASSCF(6,6)/aug-cc-pVTZ level of theory were carried out to compute the structure of the molecule in its excited state. The calculated structure was compared to that of the molecule in its electronic ground state as well as to the structures of related molecules in their S{sub 0} and S{sub 1}(π,π{sup *}) electronic states. In each case the decreased π bonding in the electronic excited states results in longer carbon-carbon bonds in the benzene ring. The skeletal vibrational frequencies in the electronic excited state were readily assigned and these were compared to the ground state and to the frequencies of five similar molecules. The vibrational levels in both S{sub 0} and S{sub 1}(π,π{sup *}) states were remarkably harmonic in contrast to the other bicyclic molecules. The decreases in the frequencies of the out-of-plane skeletal modes reflect the increased floppiness of these bicyclic molecules in their S{sub 1}(π,π{sup *}) excited state.

  11. Angular momentum and orientation effects in excitation-ionization collisions

    NASA Astrophysics Data System (ADS)

    Harris, A. L.; Esposito, T. P.

    2016-08-01

    We present theoretical fully differential cross sections (FDCS) for electron-impact excitation-ionization of helium in which the final state He+ ion is oriented in a particular direction. Specifically, we study the process for He+ ions in the 2p0 state. Using our 4-body distorted wave model, we show a strong dependence of the FDCS on the ion’s orientation and trace some unexpected structures in the FDCS to the L = 2 term in the partial wave expansion for the ionized electron. A comparison is drawn to the ionization of oriented Mg (3p0) atoms, and unlike that process, we find that for excitation-ionization angular momentum must be transferred from either the projectile or the target atom.

  12. X-ray scattering study of pyrochlore iridates: Crystal structure, electronic, and magnetic excitations

    NASA Astrophysics Data System (ADS)

    Clancy, J. P.; Gretarsson, H.; Lee, E. K. H.; Tian, Di; Kim, J.; Upton, M. H.; Casa, D.; Gog, T.; Islam, Z.; Jeon, Byung-Gu; Kim, Kee Hoon; Desgreniers, S.; Kim, Yong Baek; Julian, S. J.; Kim, Young-June

    2016-07-01

    We have investigated the structural, electronic, and magnetic properties of the pyrochlore iridates Eu2Ir2O7 and Pr2Ir2O7 using a combination of resonant elastic x-ray scattering, x-ray powder diffraction, and resonant inelastic x-ray scattering (RIXS). The structural parameters of Eu2Ir2O7 have been examined as a function of temperature and applied pressure, with a particular emphasis on regions of the phase diagram where electronic and magnetic phase transitions have been reported. We find no evidence of crystal symmetry change over the range of temperatures (˜6 to 300 K) and pressures (˜0.1 to 17 GPa) studied. We have also investigated the electronic and magnetic excitations in single-crystal samples of Eu2Ir2O7 and Pr2Ir2O7 using high-resolution Ir L3-edge RIXS. In spite of very different ground state properties, we find that these materials exhibit qualitatively similar excitation spectra, with crystal field excitations at ˜3 -5 eV, spin-orbit excitations at ˜0.5 -1 eV, and broad low-lying excitations below ˜0.15 eV. In single-crystal samples of "Eu-rich" Eu2Ir2O7 (found to possess an actual stoichiometry of Eu2.18Ir1.82O7.06 ) we observe highly damped magnetic excitations at ˜45 meV, which display significant momentum dependence. We compare these results with recent dynamical structure factor calculations.

  13. Influence of environment induced correlated fluctuations in electronic coupling on coherent excitation energy transfer dynamics in model photosynthetic systems

    NASA Astrophysics Data System (ADS)

    Huo, Pengfei; Coker, David F.

    2012-03-01

    Two-dimensional photon-echo experiments indicate that excitation energy transfer between chromophores near the reaction center of the photosynthetic purple bacterium Rhodobacter sphaeroides occurs coherently with decoherence times of hundreds of femtoseconds, comparable to the energy transfer time scale in these systems. The original explanation of this observation suggested that correlated fluctuations in chromophore excitation energies, driven by large scale protein motions could result in long lived coherent energy transfer dynamics. However, no significant site energy correlation has been found in recent molecular dynamics simulations of several model light harvesting systems. Instead, there is evidence of correlated fluctuations in site energy-electronic coupling and electronic coupling-electronic coupling. The roles of these different types of correlations in excitation energy transfer dynamics are not yet thoroughly understood, though the effects of site energy correlations have been well studied. In this paper, we introduce several general models that can realistically describe the effects of various types of correlated fluctuations in chromophore properties and systematically study the behavior of these models using general methods for treating dissipative quantum dynamics in complex multi-chromophore systems. The effects of correlation between site energy and inter-site electronic couplings are explored in a two state model of excitation energy transfer between the accessory bacteriochlorophyll and bacteriopheophytin in a reaction center system and we find that these types of correlated fluctuations can enhance or suppress coherence and transfer rate simultaneously. In contrast, models for correlated fluctuations in chromophore excitation energies show enhanced coherent dynamics but necessarily show decrease in excitation energy transfer rate accompanying such coherence enhancement. Finally, for a three state model of the Fenna-Matthews-Olsen light

  14. Influence of environment induced correlated fluctuations in electronic coupling on coherent excitation energy transfer dynamics in model photosynthetic systems.

    PubMed

    Huo, Pengfei; Coker, David F

    2012-03-21

    Two-dimensional photon-echo experiments indicate that excitation energy transfer between chromophores near the reaction center of the photosynthetic purple bacterium Rhodobacter sphaeroides occurs coherently with decoherence times of hundreds of femtoseconds, comparable to the energy transfer time scale in these systems. The original explanation of this observation suggested that correlated fluctuations in chromophore excitation energies, driven by large scale protein motions could result in long lived coherent energy transfer dynamics. However, no significant site energy correlation has been found in recent molecular dynamics simulations of several model light harvesting systems. Instead, there is evidence of correlated fluctuations in site energy-electronic coupling and electronic coupling-electronic coupling. The roles of these different types of correlations in excitation energy transfer dynamics are not yet thoroughly understood, though the effects of site energy correlations have been well studied. In this paper, we introduce several general models that can realistically describe the effects of various types of correlated fluctuations in chromophore properties and systematically study the behavior of these models using general methods for treating dissipative quantum dynamics in complex multi-chromophore systems. The effects of correlation between site energy and inter-site electronic couplings are explored in a two state model of excitation energy transfer between the accessory bacteriochlorophyll and bacteriopheophytin in a reaction center system and we find that these types of correlated fluctuations can enhance or suppress coherence and transfer rate simultaneously. In contrast, models for correlated fluctuations in chromophore excitation energies show enhanced coherent dynamics but necessarily show decrease in excitation energy transfer rate accompanying such coherence enhancement. Finally, for a three state model of the Fenna-Matthews-Olsen light

  15. Analysis and simulation for a model of electron impact excitation/deexcitation and ionization/recombination

    SciTech Connect

    Yan, Bokai; Caflisch, Russel E.; Barekat, Farzin; Cambier, Jean-Luc

    2015-10-15

    This paper describes a kinetic model and a corresponding Monte Carlo simulation method for excitation/deexcitation and ionization/recombination by electron impact in a plasma free of external fields. The atoms and ions in the plasma are represented by continuum densities and the electrons by a particle distribution. A Boltzmann-type equation is formulated and a corresponding H-theorem is formally derived. An efficient Monte Carlo method is developed for an idealized analytic model of the excitation and ionization collision cross sections. To accelerate the simulation, the reduced rejection method and binary search method are used to overcome the singular rate in the recombination process. Numerical results are presented to demonstrate the efficiency of the method on spatially homogeneous problems. The evolution of the electron distribution function and atomic states is studied, revealing the possibility under certain circumstances of system relaxation towards stationary states that are not the equilibrium states, a potential non-ergodic behavior.

  16. Electronic excitations of bulk LiCl from many-body perturbation theory

    SciTech Connect

    Jiang, Yun-Feng; Wang, Neng-Ping; Rohlfing, Michael

    2013-12-07

    We present the quasiparticle band structure and the optical excitation spectrum of bulk LiCl, using many-body perturbation theory. Density-functional theory is used to calculate the ground-state geometry of the system. The quasiparticle band structure is calculated within the GW approximation. Taking the electron-hole interaction into consideration, electron-hole pair states and optical excitations are obtained by solving the Bethe-Salpeter equation for the electron-hole two-particle Green function. The calculated band gap is 9.5 eV, which is in good agreement with the experimental result of 9.4 eV. And the calculated optical absorption spectrum, which contains an exciton peak at 8.8 eV and a resonant-exciton peak at 9.8 eV, is also in good agreement with experimental data.

  17. Excitation of vibrational quanta in furfural by intermediate-energy electrons.

    PubMed

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

    2015-12-14

    We report cross sections for electron-impact excitation of vibrational quanta in furfural, at intermediate incident electron energies (20, 30, and 40 eV). The present differential cross sections are measured over the scattered electron angular range 10°-90°, with corresponding integral cross sections subsequently being determined. Furfural is a viable plant-derived alternative to petrochemicals, being produced via low-temperature plasma treatment of biomass. Current yields, however, need to be significantly improved, possibly through modelling, with the present cross sections being an important component of such simulations. To the best of our knowledge, there are no other cross sections for vibrational excitation of furfural available in the literature, so the present data are valuable for this important molecule. PMID:26671372

  18. Study of intermediates from transition metal excited-state electron-transfer reactions

    SciTech Connect

    Hoffman, M.Z.

    1991-12-31

    During this period, conventional and fast-kinetics techniques of photochemistry, photophysics, radiation chemistry, and electrochemistry were used for the characterization of the intermediates that are involved in transition metal excited-state electron-transfer reactions. The intermediates of interest were the excited states of Ru(II) and Cr(III) photosensitizers, their reduced forms, and the species formed in the reactions of redox quenchers and electron-transfer agents. Of particular concern has been the back electron-transfer reaction between the geminate pair formed in the redox quenching of the photosensitizers, and the dependence of its rate on solution medium and temperature in competition with transformation and cage escape processes.

  19. Excitation of vibrational quanta in furfural by intermediate-energy electrons

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

    We report cross sections for electron-impact excitation of vibrational quanta in furfural, at intermediate incident electron energies (20, 30, and 40 eV). The present differential cross sections are measured over the scattered electron angular range 10°-90°, with corresponding integral cross sections subsequently being determined. Furfural is a viable plant-derived alternative to petrochemicals, being produced via low-temperature plasma treatment of biomass. Current yields, however, need to be significantly improved, possibly through modelling, with the present cross sections being an important component of such simulations. To the best of our knowledge, there are no other cross sections for vibrational excitation of furfural available in the literature, so the present data are valuable for this important molecule.

  20. Excitation of vibrational quanta in furfural by intermediate-energy electrons

    SciTech Connect

    Jones, D. B.; Neves, R. F. C.; Lopes, M. C. A.; Costa, R. F. da; Varella, M. T. do N.; Bettega, M. H. F.; Lima, M. A. P.; García, G.; and others

    2015-12-14

    We report cross sections for electron-impact excitation of vibrational quanta in furfural, at intermediate incident electron energies (20, 30, and 40 eV). The present differential cross sections are measured over the scattered electron angular range 10°–90°, with corresponding integral cross sections subsequently being determined. Furfural is a viable plant-derived alternative to petrochemicals, being produced via low-temperature plasma treatment of biomass. Current yields, however, need to be significantly improved, possibly through modelling, with the present cross sections being an important component of such simulations. To the best of our knowledge, there are no other cross sections for vibrational excitation of furfural available in the literature, so the present data are valuable for this important molecule.

  1. The repopulation of electronic states upon vibrational excitation of niobium carbide clusters.

    PubMed

    Chernyy, V; Logemann, R; Bakker, J M; Kirilyuk, A

    2016-07-14

    We study the infrared (IR) resonant heating of neutral niobium carbide clusters probed through ultraviolet photoionization spectroscopy. The IR excitation not only changes the photoionization spectra for the photon energies above the ionization threshold, but also modulates ion yield for energies significantly below it. An attempt to describe the experimental spectra using either Fowler's theory or thermally populated vibrational states was not successful. However, the data can be fully modeled by vibrationally and rotationally broadened discrete electronic levels obtained from Density Functional Theory (DFT) calculations. The application of this method to spectra with different IR pulse energies not only yields information about the excited electronic states in the vicinity of the HOMO level, populated by manipulation of the vibrational coordinates of a cluster, but also can serve as an extra indicator for the cluster isomeric structure and corresponding DFT-calculated electronic levels. PMID:27421411

  2. Electron impact excitation of the 3s3p 1P1 state in magnesium

    NASA Astrophysics Data System (ADS)

    Predojević, Branko

    2006-12-01

    Differential cross sections (DCSs) for electron-impact excitation of the 3s3p 1P1 resonance state of magnesium have been measured at 10, 15, 20, 40, 60, 80 and 100 eV incident electron energies (Eo). Scattered-electron intensities were measured over wide range of scattering angles from 2° to 150°. The absolute DCS scale for the 1P1 state was determined through normalizations of its relative DCSs to optical oscillator strength using forward scattering function method, except at Eo ⩽ 15 eV where the excitation function of the 3s3p 1P1 state experimentally obtained by Leep and Gallagher (1976 Phys. Rev. A 13 148) was utilized for normalization. These absolute DCSs were extrapolated to 0° and 180° and numerically integrated to yield integral, momentum transfer and viscosity cross sections. Our results are compared with available experimental and theoretical data.

  3. The repopulation of electronic states upon vibrational excitation of niobium carbide clusters

    NASA Astrophysics Data System (ADS)

    Chernyy, V.; Logemann, R.; Bakker, J. M.; Kirilyuk, A.

    2016-07-01

    We study the infrared (IR) resonant heating of neutral niobium carbide clusters probed through ultraviolet photoionization spectroscopy. The IR excitation not only changes the photoionization spectra for the photon energies above the ionization threshold, but also modulates ion yield for energies significantly below it. An attempt to describe the experimental spectra using either Fowler's theory or thermally populated vibrational states was not successful. However, the data can be fully modeled by vibrationally and rotationally broadened discrete electronic levels obtained from Density Functional Theory (DFT) calculations. The application of this method to spectra with different IR pulse energies not only yields information about the excited electronic states in the vicinity of the HOMO level, populated by manipulation of the vibrational coordinates of a cluster, but also can serve as an extra indicator for the cluster isomeric structure and corresponding DFT-calculated electronic levels.

  4. Influence of the excited states on the electron-energy distribution function in low-pressure microwave argon plasmas

    SciTech Connect

    Yanguas-Gil, A.; Cotrino, J.; Gonzalez-Elipe, A.R.

    2005-07-01

    In this work the influence of the excited states on the electron-energy distribution function has been determined for an argon microwave discharge at low pressure. A collisional-radiative model of argon has been developed taking into account the most recent experimental and theoretical values of argon-electron-impact excitation cross sections. The model has been solved along with the electron Boltzmann equation in order to study the influence of the inelastic collisions from the argon excited states on the electron-energy distribution function. Results show that under certain conditions the excited states can play an important role in determining the shape of the distribution function and the mean kinetic energy of the electrons, deplecting the high-energy tail due to inelastic processes from the excited states, especially from the 4s excited configuration. It has been found that from the populations of the excited states an excitation temperature can be defined. This excitation temperature, which can be experimentally determined by optical emission spectroscopy, is lower than the electron kinetic temperature obtained from the electron-energy distribution function.

  5. Wakefield Excitation by a Sequence of Electron Bunches in a Rectangular Waveguide Lined with Dielectric Slabs

    SciTech Connect

    Kiselev, V. A.; Linnik, A. F.; Onishchenko, I. N.; Onishchenko, N. I.; Sotnikov, G. V.; Uskov, V. V.; Marshall, T. C.

    2006-11-27

    A rectangular dielectric-lined metallic structure was studied that has an advantage over a cylindrical structure from the possibility of exciting by a sequence of bunches many equally-spaced modes, thereby building up a larger mode-locked wakefield. A rectangular vacuum copper waveguide was lined with two dielectric slabs, the size of which was calculated to provide resonant excitation of the fundamental LSM mode by a sequence of bunches with repetition frequency f0=2805 MHz, produced by linear resonant electron accelerator (4.5 MeV, number of bunches 6.103, diameter 1cm, duration 60 ps each, distance between bunches 300 ps, number of electrons in each bunch 109). The waveguide has cross section 85 mm x 180 mm, and Teflon ({epsilon} 2.1) plates were placed along the smaller sides of the waveguide, their thickness from the calculation being 22 mm. In experiments, the length of the resonator was 535mm. We found that the total wakefield is three times larger than the fundamental mode; thus a greater number of excited modes was excited compared with the cylindrical case, for which this ratio was only 1.5. We found considerably more energy loss of electron bunches for the resonator case compared with the waveguide case.

  6. A proposal for fs-electron microscopy experiments on high-energy excitations in solids.

    PubMed

    Piazza, L; Musumeci, P; Luiten, O J; Carbone, Fabrizio

    2014-08-01

    Recent advances in ultrafast technology enable both the study and the control of materials properties thanks to the ability to record high temporal resolution movies of their transformations, or the ability to generate new states of matter by selecting ad hoc an excitation to drive the system out of equilibrium. The holy grail of this type of experiments is to combine a high tuneability of the excitation with a wide observation window. For example, this is achieved in multidimensional optical spectroscopy where the response to several excitation energies is monitored in a broad energy range by a large bandwidth optical pulse. In this article, the possibility to combine the chemical sensitivity of intense tuneable X-rays pulses from a free electron laser, with the wide range of observables available in an ultrafast transmission electron microscope is discussed. The requirements for such experiments are quantified via estimates based on state of the art experiments and simulations, and it is proposed that ultrafast electron imaging, diffraction and spectroscopy experiments can be performed in combination with a chemically selective X-ray excitation of materials. PMID:24631423

  7. Double-electron excitation of H- by fast proton and antiproton impact

    NASA Astrophysics Data System (ADS)

    Hino, Ken-Ichi; Nagase, Mamoru; Okamoto, Hiroyuki; Morishita, Toru; Matsuzawa, Michio; Kimura, Mineo

    1994-05-01

    A theoretical investigation is carried out for double-electron excitation processes of H- induced by proton and antiproton impact at the enegy of 1.5 MeV. Excitation cross sections to the 2s2 1Se, 2s2p 1Po, and 2p2 1De states are calculated by using the plane-wave Born approximation, the distorted-wave Born approximation, and the close-coupling method. Wave functions of H- are generated employing the hyperspherical coordinate method. It is shown that the low-lying continuum 1skp 1Po is identified as an important intermediate state in the double-electron excitation process to the 2p2 1De state. We have also evaluated the ejected-electron spectra from the 2s2p 1Po shape-resonance state. It is found that its spectral shape is close to the observed line profile of the photodetachment of H- since the excitation mechanism to this state is mostly dominated by the optically allowed transition at the projectile energy concerned here.

  8. Infrared/ultraviolet quadruple resonance spectroscopy to investigate structures of electronically excited states

    SciTech Connect

    Weiler, M.; Bartl, K.; Gerhards, M.

    2012-03-21

    Molecular beam investigations in combination with IR/UV spectroscopy offer the possibility to obtain structural information on isolated molecules and clusters. One of the demanding tasks is the discrimination of different isomers, e.g., by the use of isomer specific UV excitations. If this discrimination fails due to overlaying UV spectra of different isomers, IR/IR methods offer another possibility. Here, we present a new IR/UV/IR/UV quadruple resonance technique to distinguish between different isomers especially in the electronically excited state. Due to the IR spectra, structural changes and photochemical pathways in excited states can be assigned and identified. The method is applied to the dihydrated cluster of 3-hydroxyflavone which has been investigated as photochemically relevant system and proton wire model in the S{sub 1} state. By applying the new IR/UV/IR/UV technique, we are able to show experimentally that both in the electronic ground (S{sub 0}) and the electronically excited state (S{sub 1}) two isomers have to be assigned.

  9. Effect of Turbulence Modeling on an Excited Jet

    NASA Technical Reports Server (NTRS)

    Brown, Clifford A.; Hixon, Ray

    2010-01-01

    The flow dynamics in a high-speed jet are dominated by unsteady turbulent flow structures in the plume. Jet excitation seeks to control these flow structures through the natural instabilities present in the initial shear layer of the jet. Understanding and optimizing the excitation input, for jet noise reduction or plume mixing enhancement, requires many trials that may be done experimentally or computationally at a significant cost savings. Numerical simulations, which model various parts of the unsteady dynamics to reduce the computational expense of the simulation, must adequately capture the unsteady flow dynamics in the excited jet for the results are to be used. Four CFD methods are considered for use in an excited jet problem, including two turbulence models with an Unsteady Reynolds Averaged Navier-Stokes (URANS) solver, one Large Eddy Simulation (LES) solver, and one URANS/LES hybrid method. Each method is used to simulate a simplified excited jet and the results are evaluated based on the flow data, computation time, and numerical stability. The knowledge gained about the effect of turbulence modeling and CFD methods from these basic simulations will guide and assist future three-dimensional (3-D) simulations that will be used to understand and optimize a realistic excited jet for a particular application.

  10. The electronic origin and vibrational levels of the first excited singlet state of isocyanic acid (HNCO)

    SciTech Connect

    Berghout, H. Laine; Crim, F. Fleming; Zyrianov, Mikhail; Reisler, Hanna

    2000-04-15

    The combination of vibrationally mediated photofragment yield spectroscopy, which excites molecules prepared in single vibrational states, and multiphoton fluorescence spectroscopy, which excites molecules cooled in a supersonic expansion, provides detailed information on the energetics and vibrational structure of the first excited singlet state (S{sub 1}) of isocyanic acid (HNCO). Dissociation of molecules prepared in individual vibrational states by stimulated Raman excitation probes vibrational levels near the origin of the electronically excited state. Detection of fluorescence from dissociation products formed by multiphoton excitation through S{sub 1} of molecules cooled in a supersonic expansion reveals the vibrational structure at higher energies. Both types of spectra show long, prominent progressions in the N-C-O bending vibration built on states with different amounts of N-C stretching excitation and H-N-C bending excitation. Analyzing the spectra locates the origin of the S{sub 1} state at 32 449{+-}20 cm{sup -1} and determines the harmonic vibrational frequencies of the N-C stretch ({omega}{sub 3}=1034{+-}20 cm{sup -1}), the H-N-C bend ({omega}{sub 4}=1192{+-}19 cm{sup -1}), and the N-C-O bend ({omega}{sub 5}=599{+-}7 cm{sup -1}), values that are consistent with several ab initio calculations. The assigned spectra strongly suggest that the N-C stretching vibration is a promoting mode for internal conversion from S{sub 1} to S{sub 0}. (c) 2000 American Institute of Physics.

  11. Rate coefficients for dissociative attachment and resonant electron-impact dissociation involving vibrationally excited O{sub 2} molecules

    SciTech Connect

    Laporta, V.; Celiberto, R.; Tennyson, J.

    2014-12-09

    Rate coefficients for dissociative electron attachment and electron-impact dissociation processes, involving vibrationally excited molecular oxygen, are presented. Analytical fits of the calculated numerical data, useful in the applications, are also provided.

  12. Internal Stark effect mediates intramolecular excited-state proton transfer in 3-hydroxyflavone derivatives

    NASA Astrophysics Data System (ADS)

    Klymchenko, Andriy S.; Demchenko, Alexander P.

    2002-12-01

    Internal Stark effect in electronic spectra is the effect that is observed when the electronic bands shift udner the influence of promixal charges. In order to study the possible involvement of this effect in modulating the intramolecular proton transfer reactions in the excited state, we designed and studied several derivatives of 3-hydroxyflavone. They include the species containing neutral and positively charged substituents in 6 position of chromone ring. These compounds were studied in solvents of different polarities. In these experiments the shifts of both normal and tautomer flurosence bands are clearly observed in a manner predicted by Stark effect theory. In addition, a dramatic effect of suppression by introduced charge of intramolecular excited-state proton transfer was observed.

  13. Threshold vibrational excitation of CO{sub 2} by slow electrons

    SciTech Connect

    Vanroose, Wim; Zhang, Zhiyong; McCurdy, C.W.; Rescigno, T.N.

    2003-07-08

    Threshold structures, reminiscent of those seen in the polar hydrogen halides, have recently been observed in the cross sections for electron impact excitation of certain vibrational levels of the non-polar CO2 molecule. These structures occur at energies outside the range where shape resonances dominate the dynamics. We propose a virtual state model that describes the multi-dimensional nuclear dynamics during the collision and explains quantitatively the selectivity observed in the excitation of the Fermi dyad, as well as the pattern of threshold peaks and oscillations seen in the upper levels of the higher polyads.

  14. Novel relativistic plasma excitations in a gated two-dimensional electron system.

    PubMed

    Muravev, V M; Gusikhin, P A; Andreev, I V; Kukushkin, I V

    2015-03-13

    The microwave response of a two-dimensional electron system (2DES) covered by a conducting top gate is investigated in the relativistic regime for which the 2D conductivity σ_{2D}>c/2π. Weakly damped plasma waves are excited in the gated region of the 2DES. The frequency and amplitude of the resulting plasma excitations show a very unusual dependence on the magnetic field, conductivity, gate geometry, and separation from the 2DES. We show that such relativistic plasmons survive for temperatures up to 300 K, allowing for new room-temperature microwave and terahertz applications. PMID:25815956

  15. The quantified NTO analysis for the electronic excitations of molecular many-body systems

    NASA Astrophysics Data System (ADS)

    Li, Jian-Hao; Chai, Jeng-Da; Guo, Guang-Yu; Hayashi, Michitoshi

    2011-10-01

    We show that the origin of electronic transitions of molecular many-body systems can be investigated by a quantified natural transition orbitals (QNTO) analysis and the electronic excitations of the total system can be mapped onto a standard orbitals set of a reference system. We further illustrate QNTO on molecular systems by studying the origin of electronic transitions of DNA moiety, thymine and thymidine. This QNTO analysis also allows us to assess the performance of various functionals used in time-dependent density functional response theory.

  16. Excitation density distribution in electron-beam-pumped ZnSe semiconductor lasers

    SciTech Connect

    Donskoi, E N; Zalyalov, A N; Petrushin, O N; Savel'ev, Yu A; Tarasov, M D; Shigaev, Yu S; Zhdanova, E V; Zverev, M M; Peregudov, D V; Ivanov, S V; Sedova, I V; Sorokin, S V

    2008-12-31

    The spatial density distribution of the absorbed energy in ZnSe semiconductor lasers excited by electrons with energies from 2 keV to 1 MeV is calculated by the Monte-Carlo method. Approximate analytic expressions determining the absorbed energy of electrons in ZnSe are presented. The pump power threshold in a semiconductor quantum-well ZnSe structure is experimentally determined. The lasing threshold in such structures is estimated as a function of the electron energy. (active media)

  17. Scalable Methods for Electronic Excitations and Optical Responses in Nanostructures: Mathematics to Algorithms to Observables

    SciTech Connect

    James R. Chelikowsky

    2009-03-31

    The work reported here took place at the University of Minnesota from September 15, 2003 to November 14, 2005. This funding resulted in 10 invited articles or book chapters, 37 articles in refereed journals and 13 invited talks. The funding helped train 5 PhD students. The research supported by this grant focused on developing theoretical methods for predicting and understanding the properties of matter at the nanoscale. Within this regime, new phenomena occur that are characteristic of neither the atomic limit, nor the crystalline limit. Moreover, this regime is crucial for understanding the emergence of macroscopic properties such as ferromagnetism. For example, elemental Fe clusters possess magnetic moments that reside between the atomic and crystalline limits, but the transition from the atomic to the crystalline limit is not a simple interpolation between the two size regimes. To capitalize properly on predicting such phenomena in this transition regime, a deeper understanding of the electronic, magnetic and structural properties of matter is required, e.g., electron correlation effects are enhanced within this size regime and the surface of a confined system must be explicitly included. A key element of our research involved the construction of new algorithms to address problems peculiar to the nanoscale. Typically, one would like to consider systems with thousands of atoms or more, e.g., a silicon nanocrystal that is 7 nm in diameter would contain over 10,000 atoms. Previous ab initio methods could address systems with hundreds of atoms whereas empirical methods can routinely handle hundreds of thousands of atoms (or more). However, these empirical methods often rely on ad hoc assumptions and lack incorporation of structural and electronic degrees of freedom. The key theoretical ingredients in our work involved the use of ab initio pseudopotentials and density functional approaches. The key numerical ingredients involved the implementation of algorithms for

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

    NASA Astrophysics Data System (ADS)

    Yonehara, Takehiro; Takatsuka, Kazuo

    2016-04-01

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

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

    PubMed

    Yonehara, Takehiro; Takatsuka, Kazuo

    2016-04-28

    Following the previous study on nonadiabatic reaction dynamics including boron clusters [T. Yonehara and K. Takatsuka, J. Chem. Phys. 137, 22A520 (2012)], we explore deep into highly excited electronic states of the singlet boron cluster (B12) to find the characteristic features of the densely quasi-degenerate electronic state manifold, which undergo very frequent nonadiabatic transitions and thereby intensive electronic state mixing among very many of the relevant states. So much so, isolating the individual adiabatic states and tracking the expected potential energy surfaces both lose the physical sense. This domain of molecular situation is far beyond the realm of the Born-Oppenheimer approximation. To survey such a violent electronic state-mixing, we apply a method of nonadiabatic electron wavepacket dynamics, the semiclassical Ehrenfest method. We have tracked those electron wavepackets and found the electronic state mixing looks like an ultrafast diffusion in the Hilbert space, which results in huge fluctuation. Furthermore, due to such a violent mixing, the quantum phases associated with the electronic states are swiftly randomized, and consequently the coherence among the electronic states are lost quickly. Besides, these highly excited states are mostly of highly poly-radical nature, even in the spin singlet manifold and the number of radicals amounts up to 10 electrons in the sense of unpaired electrons. Thus the electronic states are summarized to be poly-radical and decoherent with huge fluctuation in shorter time scales of vibrational motions. The present numerical study sets a theoretical foundation for unknown molecular properties and chemical reactivity of such densely quasi-degenerate chemical species. PMID:27131547

  20. Electron Attachment in Low-Energy Electron Elastic Collisions with Au and Pt Atoms: Identification of Excited Anions

    NASA Astrophysics Data System (ADS)

    Msezane, A. Z.; Eure, A.; Felfli, Z.; Sokolovski, D.

    2009-11-01

    The recent Regge-pole methodology has been benchmarked [1] on the accurately measured binding energies of the excited Ge= and Sn= anions [2] through the binding energies (BEs) extracted from the Regge-pole calculated elastic total cross sections (TCSs). Here the methodology is applied together with a Thomas-Fermi type potential that incorporates the vital core polarization interaction to investigate the possibility of forming excited Au= and Pt= anions in low-energy electron elastic collisions with Au and Pt atoms. From the positions of the characteristic extremely narrow resonances in the total cross sections, we extract the binding energies of the excited Au= and Pt= anions formed as Regge resonances during the collisions. The angular life of the complexes thus formed is used to differentiate the stable excited bound states of the anions from the shape resonances [3]. The BEs for the excited Au= and Pt= anions are found to be 0.475eVand 0.543eV, respectively, challenging both theory and experiment to verify. [1] A. Msezane et al, Phys. Rev. A, Submitted (2009) [2] M. Scheer et al, Phys. Rev. A 58, 2844 (1998) [3] Z. Felfli et al, Phys. Rev. A 79, 012714 (2009)

  1. Multidirectional Angular Electronic Flux during Adiabatic Attosecond Charge Migration in Excited Benzene.

    PubMed

    Hermann, Gunter; Liu, ChunMei; Manz, Jörn; Paulus, Beate; Pérez-Torres, Jhon Fredy; Pohl, Vincent; Tremblay, Jean Christophe

    2016-07-14

    Recently, adiabatic attosecond charge migration (AACM) has been monitored and simulated for the first time, with application to the oriented iodoacetylene cation where AACM starts from the initial superposition of the ground state (φ0) and an electronic excited state (φ1). Here, we develop the theory for electronic fluxes during AACM in ring-shaped molecules, with application to oriented benzene prepared in the superposition of the ground and first excited singlet states. The initial state and its time evolution are analogous to coherent tunneling where φ0 and φ1 have different meanings; however, they denote the wave functions of the lowest tunneling doublet. This analogy suggests to transfer the theory of electronic fluxes during coherent tunneling to AACM, with suitable modifications which account for (i) the different time scales and (ii) the different electronic states, and which make use of (iii) the preparation of the initial state for AACM by a linearly polarized laser pulse. Application to benzene yields the multidirectional angular electronic flux with a pincer-motion type pattern during AACM: this unequivocal result confirms a previous working hypothesis. Moreover, the theory of AACM allows quantification of the electronic flux; that is, the maximum number of electrons (out of 42) which flow concertedly during AACM in benzene is 6 × 0.08 = 0.48. PMID:27046151

  2. Electron-impact ionization cross sections out of the ground and excited states of cesium

    SciTech Connect

    Lukomski, M.; Sutton, S.; Kedzierski, W.; Reddish, T. J.; Bartschat, K.; Bartlett, P. L.; Bray, I.; Stelbovics, A. T.; McConkey, J. W.

    2006-09-15

    An atom trapping technique for determining absolute, total ionization cross sections (TICS) out of an excited atom is presented. The unique feature of our method is in utilizing Doppler cooling of neutral atoms to determine ionization cross sections. This fluorescence-monitoring experiment, which is a variant of the 'trap loss' technique, has enabled us to obtain the experimental electron impact ionization cross sections out of the Cs state between 7 eV and 400 eV. CCC, RMPS, and Born theoretical results are also presented for both the ground and excited states of cesium and rubidium. In the low energy region (<11 eV) where best agreement between these excited state measurements and theory might be expected, a discrepancy of approximately a factor of five is observed. Above this energy there are significant contributions to the TICS from both autoionization and multiple ionization.

  3. Electron impact excitation of atomic oxygen - Revised cross sections. [in thermosphere and auroral substorms

    NASA Technical Reports Server (NTRS)

    Zipf, E. C.; Erdman, P. W.

    1985-01-01

    Revised cross-section values for the excitation of three O I resonance transitions at 1304, 1027, and 989 A, by electron impact on atomic oxygen are presented from threshold to 300 eV. These results are smaller than the excitation cross sections used in some airglow models by a factor of about 2.8. The revised values are in good agreement with recent quantum-scattering calculations. The downward revision is required by new laboratory studies in which the direct and dissociative cross sections for 1304 A excitation were normalized with small probable error to the O and O2 ionization cross sections. The results also reflect new advances in VUV optical calibration techniques. A number of outstanding airglow problems are simplified by these revisions.

  4. Low-Energy Electron Impact Excitation of the (010) Bending Mode of CO2

    NASA Technical Reports Server (NTRS)

    Huo, Winifred M.; Langhoff, Stephen R. (Technical Monitor)

    1996-01-01

    Low-energy electron impact excitation of the fundamental modes of CO2 has been extensively studied, both experimentally and theoretically. Much attention has been paid to the virtual state feature in the the (100) mode excitation and the (sup 2)II(sub upsilon) resonance feature around 3.8 eV, which is observable in all three fundamental modes. For the excitation of the (010) mode away from the resonance region, the Born dipole approximation was generally considered adequate. The present study employs the Born dipole approximation to treat the long range interaction and the Schwinger multichannel method for the short range interaction. The roles of the two interaction potentials will be compared.

  5. Comparison endpoint study of process plasma and secondary electron beam exciter optical emission spectroscopy

    SciTech Connect

    Stephan Thamban, P. L.; Yun, Stuart; Padron-Wells, Gabriel; Hosch, Jimmy W.; Goeckner, Matthew J.

    2012-11-15

    Traditionally process plasmas are often studied and monitored by optical emission spectroscopy. Here, the authors compare experimental measurements from a secondary electron beam excitation and direct process plasma excitation to discuss and illustrate its distinctiveness in the study of process plasmas. They present results that show excitations of etch process effluents in a SF{sub 6} discharge and endpoint detection capabilities in dark plasma process conditions. In SF{sub 6} discharges, a band around 300 nm, not visible in process emission, is observed and it can serve as a good indicator of etch product emission during polysilicon etches. Based on prior work reported in literature the authors believe this band is due to SiF{sub 4} gas phase species.

  6. Excited electronic state calculations by the transcorrelated variational Monte Carlo method: application to a helium atom.

    PubMed

    Umezawa, Naoto; Tsuneyuki, Shinji

    2004-10-15

    We have implemented the excited electronic state calculations for a helium atom by the transcorrelated variational Monte Carlo (TC-VMC) method. In this method, Jastrow-Slater-type wave function is efficiently optimized not only for the Jastrow factor but also for the Slater determinant. Since the formalism for the TC-VMC method is based on the variance minimization, excited states as well as the ground state calculations are feasible. It is found that both the first and the second excitation energies given by TC-VMC are much closer to the experimental data than those given by the variational Monte Carlo method with using the Hartree-Fock orbitals. The successful results in the TC-VMC method are considered to be due to the nodal optimization of the wave functions. PMID:15473772

  7. Inelastic electron and Raman scattering from the collective excitations in quantum wires: Zero magnetic field

    NASA Astrophysics Data System (ADS)

    Kushwaha, Manvir S.

    2013-04-01

    The nanofabrication technology has taught us that an m-dimensional confining potential imposed upon an n-dimensional electron gas paves the way to a quasi-(n-m)-dimensional electron gas, with m ⩽ n and 1 ⩽ n, m ⩽ 3. This is the road to the (semiconducting) quasi-n dimensional electron gas systems we have been happily traversing on now for almost two decades. Achieving quasi-one dimensional electron gas (Q-1DEG) [or quantum wire(s) for more practical purposes] led us to some mixed moments in this journey: while the reduced phase space for the scattering led us believe in the route to the faster electron devices, the proximity to the 1D systems left us in the dilemma of describing it as a Fermi liquid or as a Luttinger liquid. No one had ever suspected the potential of the former, but it took quite a while for some to convince the others on the latter. A realistic Q-1DEG system at the low temperatures is best describable as a Fermi liquid rather than as a Luttinger liquid. In the language of condensed matter physics, a critical scrutiny of Q-1DEG systems has provided us with a host of exotic (electronic, optical, and transport) phenomena unseen in their higher- or lower-dimensional counterparts. This has motivated us to undertake a systematic investigation of the inelastic electron scattering (IES) and the inelastic light scattering (ILS) from the elementary electronic excitations in quantum wires. We begin with the Kubo's correlation functions to derive the generalized dielectric function, the inverse dielectric function, and the Dyson equation for the dynamic screened potential in the framework of Bohm-Pines' random-phase approximation. These fundamental tools then lead us to develop methodically the theory of IES and ILS for the Q-1DEG systems. As an application of the general formal results, which know no bounds regarding the subband occupancy, we compute the density of states, the Fermi energy, the full excitation spectrum [comprised of intrasubband and

  8. Fluorescence in air excited by electrons from a 90Sr source

    NASA Astrophysics Data System (ADS)

    Sakaki, N.; Watanabe, Y.; Nagano, M.; Kobayakawa, K.

    2008-11-01

    The air fluorescence technique is used to observe ultra-high energy cosmic rays (UHECRs). In this technique, fluorescence from air excited by electrons within an extensive air shower (EAS) under various pressure and temperature conditions is detected by a telescope. The primary energy of the UHECR is estimated from the amount of fluorescence. Since ground-based experiments, such as Fly's Eye, HiRes, Auger, Telescope Array, are carried out at high altitudes, the effects of water vapor may be negligible and the photon yields in dry air, which we have measured and reported so far, will be applicable. However, in case of space-based experiments such as JEM-EUSO, most events will be observed above the sea. Photon yields in moist air are measured with a 90Sr β source and compared to those in dry air at wavelengths of 337, 358 and 391 nm. The presence of water vapor considerably reduces the photon yield. The decrease in the photon yield in moist air should be taken into account to interpret the longitudinal development of EASs near the sea surface, although the effects around the shower maximum for most showers might be small.

  9. Surface modification of monocrystalline zinc oxide induced by high-density electronic excitation

    NASA Astrophysics Data System (ADS)

    Museur, Luc; Manousaki, Alexandra; Anglos, Demetrios; Kanaev, Andrei V.

    2011-12-01

    Strong modifications of semiconductors can be provoked by high-density electronic excitation. We report on surface structuring of monocrystalline wurtzite O-face (0001) ZnO excited by UV femtosecond laser pulses (248 nm) below the ablation threshold. At fluences above 11 mJ/cm2, nanoholes of D=10 nm diameter appear quasi-periodically separated by a distance ˜30 nm (=3 D). Dual-pulse (pump-pump) experiments permit estimation of the electronic excitation lifetime responsible for this nanostructuring, which is in agreement with the electron-hole plasma lifetime 220 ps. The nanostructuring results in a smaller monocrystalline domain of ˜0.1 μm size and increases the crystalline interplane c-distance by 0.11%. The excitonic luminescence of the irradiated sample is found to increase by about 10 times. The nanostructuring remains stable in a limited range of laser fluences: above 40 mJ/cm2 the surface melts, which accelerates the photoinduced bonds breaking leading to surface erosion. We tentatively ascribe the related mechanism to the nucleation-growth of cluster vacancies at crystal dislocations accelerated by the non-thermal (electronic) melting of the surface layer. At fluences lower than 11 mJ/cm2, larger volcano-like features of 60-nm diameter were observed. The characteristic crater shape and irregular surface repartition permit their assignment to thermal explosion of impurities due to multiple exciton condensation.

  10. Coherent and Tunable Terahertz Radiation from Graphene Surface Plasmon Polarirons Excited by Cyclotron Electron Beam.

    PubMed

    Zhao, Tao; Gong, Sen; Hu, Min; Zhong, Renbin; Liu, Diwei; Chen, Xiaoxing; Zhang, Ping; Wang, Xinran; Zhang, Chao; Wu, Peiheng; Liu, Shenggang

    2015-01-01

    Terahertz (THz) radiation can revolutionize modern science and technology. To this date, it remains big challenges to develop intense, coherent and tunable THz radiation sources that can cover the whole THz frequency region either by means of only electronics (both vacuum electronics and semiconductor electronics) or of only photonics (lasers, for example, quantum cascade laser). Here we present a mechanism which can overcome these difficulties in THz radiation generation. Due to the natural periodicity of 2π of both the circular cylindrical graphene structure and cyclotron electron beam (CEB), the surface plasmon polaritions (SPPs) dispersion can cross the light line of dielectric, making transformation of SPPs into radiation immediately possible. The dual natural periodicity also brings significant excellences to the excitation and the transformation. The fundamental and hybrid SPPs modes can be excited and transformed into radiation. The excited SPPs propagate along the cyclotron trajectory together with the beam and gain energy from the beam continuously. The radiation density is enhanced over 300 times, up to 10(5) W/cm(2). The radiation frequency can be widely tuned by adjusting the beam energy or chemical potential. This mechanism opens a way for developing desired THz radiation sources to cover the whole THz frequency regime. PMID:26525516

  11. Coherent and Tunable Terahertz Radiation from Graphene Surface Plasmon Polarirons Excited by Cyclotron Electron Beam

    NASA Astrophysics Data System (ADS)

    Zhao, Tao; Gong, Sen; Hu, Min; Zhong, Renbin; Liu, Diwei; Chen, Xiaoxing; Zhang, Ping; Wang, Xinran; Zhang, Chao; Wu, Peiheng; Liu, Shenggang

    2015-11-01

    Terahertz (THz) radiation can revolutionize modern science and technology. To this date, it remains big challenges to develop intense, coherent and tunable THz radiation sources that can cover the whole THz frequency region either by means of only electronics (both vacuum electronics and semiconductor electronics) or of only photonics (lasers, for example, quantum cascade laser). Here we present a mechanism which can overcome these difficulties in THz radiation generation. Due to the natural periodicity of 2π of both the circular cylindrical graphene structure and cyclotron electron beam (CEB), the surface plasmon polaritions (SPPs) dispersion can cross the light line of dielectric, making transformation of SPPs into radiation immediately possible. The dual natural periodicity also brings significant excellences to the excitation and the transformation. The fundamental and hybrid SPPs modes can be excited and transformed into radiation. The excited SPPs propagate along the cyclotron trajectory together with the beam and gain energy from the beam continuously. The radiation density is enhanced over 300 times, up to 105 W/cm2. The radiation frequency can be widely tuned by adjusting the beam energy or chemical potential. This mechanism opens a way for developing desired THz radiation sources to cover the whole THz frequency regime.

  12. Coherent and Tunable Terahertz Radiation from Graphene Surface Plasmon Polarirons Excited by Cyclotron Electron Beam

    PubMed Central

    Zhao, Tao; Gong, Sen; Hu, Min; Zhong, Renbin; Liu, Diwei; Chen, Xiaoxing; Zhang, Ping; Wang, Xinran; Zhang, Chao; Wu, Peiheng; Liu, Shenggang

    2015-01-01

    Terahertz (THz) radiation can revolutionize modern science and technology. To this date, it remains big challenges to develop intense, coherent and tunable THz radiation sources that can cover the whole THz frequency region either by means of only electronics (both vacuum electronics and semiconductor electronics) or of only photonics (lasers, for example, quantum cascade laser). Here we present a mechanism which can overcome these difficulties in THz radiation generation. Due to the natural periodicity of 2π of both the circular cylindrical graphene structure and cyclotron electron beam (CEB), the surface plasmon polaritions (SPPs) dispersion can cross the light line of dielectric, making transformation of SPPs into radiation immediately possible. The dual natural periodicity also brings significant excellences to the excitation and the transformation. The fundamental and hybrid SPPs modes can be excited and transformed into radiation. The excited SPPs propagate along the cyclotron trajectory together with the beam and gain energy from the beam continuously. The radiation density is enhanced over 300 times, up to 105 W/cm2. The radiation frequency can be widely tuned by adjusting the beam energy or chemical potential. This mechanism opens a way for developing desired THz radiation sources to cover the whole THz frequency regime. PMID:26525516

  13. Explicitly correlated equation-of-motion coupled-cluster methods for excited and electron-attached states.

    PubMed

    Bokhan, Denis; Ten-No, Seiichiro

    2010-11-28

    Based on the linearly approximated F12 coupled cluster singles and doubles [CCSD(F12)] model, equation-of-motion [EOM-CCSD(F12)] methods for electron affinities (EAs) and excitation energies (EEs) have been formulated and implemented. Extended electron-attachment and excitation operators are introduced for balanced descriptions of both neutral and electron-attached (or excited) states. In our implementation the cusp conditions are used for the definition of extended electron-attachment (excitation) operators. It is shown that EA-EOM-CCSD(F12) provides vertical electron affinities accurate to 0.1 eV compared to those in the complete basis set limit. Numerical tests conducted on a selection of small molecules have also shown notable improvement in Rydberg excitation energies compared to valence ones by the use of correlation factors. PMID:21133437

  14. Electronic excitation of molecules in solution calculated using the symmetry-adapted cluster–configuration interaction method in the polarizable continuum model

    SciTech Connect

    Fukuda, Ryoichi Ehara, Masahiro

    2015-12-31

    The effects from solvent environment are specific to the electronic states; therefore, a computational scheme for solvent effects consistent with the electronic states is necessary to discuss electronic excitation of molecules in solution. The PCM (polarizable continuum model) SAC (symmetry-adapted cluster) and SAC-CI (configuration interaction) methods are developed for such purposes. The PCM SAC-CI adopts the state-specific (SS) solvation scheme where solvent effects are self-consistently considered for every ground and excited states. For efficient computations of many excited states, we develop a perturbative approximation for the PCM SAC-CI method, which is called corrected linear response (cLR) scheme. Our test calculations show that the cLR PCM SAC-CI is a very good approximation of the SS PCM SAC-CI method for polar and nonpolar solvents.

  15. Tracking the charge and spin dynamics of electronic excited states in inorganic complexes

    NASA Astrophysics Data System (ADS)

    Gaffney, Kelly

    2015-03-01

    Inorganic complexes have many advantageous properties for solar energy applications, including strong visible absorption and photocatalytic activity. Whether used as a photocatalyst or a photosensitizer, the lifetime of electronic excited states and the earth abundance of the molecular components represent a key property for solar energy applications. These dual needs have undermined the usefulness of many coordination compounds. Isoelectronic iron and ruthenium based complexes represent a clear example. Ru-polypyridal based molecules have been the workhorse of solar energy related research and dye sensitized solar cells for decades, but the replacement of low abundance Ru with Fe leads to million-fold reductions in metal to ligand charge transfer (MLCT) excited state lifetimes. Understanding the origin of this million-fold reduction in lifetime and how to control excited state relaxation in 3d-metal complexes motivates the work I will discuss. We have used the spin sensitivity of hard x-ray fluorescence spectroscopy and the intense femtosecond duration pulses generated by the LCLS x-ray laser to probe the spin dynamics in a series of electronically excited [Fe(CN)6-2N(2,2'-bipyridine)N]2 N - 4 complexes, with N = 1-3. These femtosecond resolution measurements demonstrate that modification of the solvent and ligand environment can lengthen the MLCT excited state lifetime by more than two orders of magnitude. They also verify the role of triplet ligand field excited states in the spin crossover dynamics from singlet to quintet spin configurations. Work supported by the AMOS program within the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy.

  16. Effect of valence holes kinetics on material excitation in tracks of swift heavy ions

    NASA Astrophysics Data System (ADS)

    Rymzhanov, R. A.; Medvedev, N. A.; Volkov, A. E.

    2015-12-01

    A considerable part of the excess energy of the electronic subsystem of a solid penetrated by a swift heavy ion (SHI) is accumulated in valence holes. Spatial redistribution of these holes can affect subsequent relaxation, resulting in ionizations of new electrons by hole impacts as well as energy transfer to the target lattice. A new version of the Monte Carlo code TREKIS is applied to study this effect in Al2O3 for SHI tracks. The complex dielectric function (CDF) formalism is used to calculate the cross sections of interaction of involved charged particles (an ion, electrons, holes) with the target giving us ability to take into account collective response of a target to excitations. We compare the radial distributions of the densities and energies of excited electrons and valence holes at different times to those obtained under the assumption of immobile holes used in earlier works. The comparison shows a significant difference between these distributions within the track core, where the majority of slow electrons and valence holes are located at femtosecond timescales after the ion impact. The study demonstrates that the energy deposited by valence holes into the lattice in nanometric tracks is comparable to the energy transferred by excited electrons. Radii of structure transformations in tracks produced by these energy exchange channels are in a good agreement with experiments.

  17. Electronically Excited States of Anisotropically Extended Singly-Deprotonated PAH Anions.

    PubMed

    Theis, Mallory L; Candian, Alessandra; Tielens, Alexander G G M; Lee, Timothy J; Fortenberry, Ryan C

    2015-12-31

    Polycyclic aromatic hydrocarbons (PAHs) play a significant role in the chemistry of the interstellar medium (ISM) as well as in hydrocarbon combustion. These molecules can have high levels of diversity with the inclusion of heteroatoms and the addition or removal of hydrogens to form charged or radical species. There is an abundance of data on the cationic forms of these molecules, but there have been many fewer studies on the anionic species. The present study focuses on the anionic forms of deprotonated PAHs. It has been shown in previous work that PAHs containing nitrogen heteroatoms (PANHs) have the ability to form valence excited states giving anions electronic absorption features. This work analyzes how the isoelectronic pure PAHs behave under similar structural constructions. Singly deprotonated forms of benzene, naphthalene, anthracene, and tetracene classes are examined. None of the neutral-radicals possess dipole moments large enough to support dipole-bound excited states in their corresponding closed-shell anions. Even though the PANH anion derivatives support valence excited states for three-ringed structures, it is not until four-ringed structures of the pure PAH anion derivatives that valence excited states are exhibited. However, anisotropically extended PAHs larger than tetracene will likely exhibit valence excited states. The relative energies for the anion isomers are very small for all of the systems in this study. PMID:26645382

  18. Stretching of hydrogen-bonded OH in the lowest singlet excited electronic state of water dimer.

    PubMed

    Chipman, Daniel M

    2006-01-28

    The lowest singlet excited electronic state of water monomer in the gas phase is strictly dissociative along a OH stretch coordinate but changes its nature when the stretched OH moiety is hydrogen bonded to a neighboring water molecule. This work extends previous exploration of the water dimer excited singlet potential-energy surface, using computational methods that are reliable even at geometries well removed from the ground-state equilibrium. First, the hydrogen-bonded OH moiety is stretched far enough to establish the existence of a barrier that is sufficient to support a quasibound vibrational state of the OH oscillator near the Franck-Condon region. Second, the constraint of an icelike structure is relaxed, and it is found that a substantial fraction of liquidlike structures also supports a quasibound vibrational state. These potential-energy explorations on stretching of the hydrogen-bonded OH moiety in a water dimer are discussed as a model for understanding the initial dynamics upon excitation into the lowest excited singlet state of condensed water. The possibility is raised that the excited-state lifetime may be long enough to allow for exciton migration, which would provide a mechanism for energy transport in condensed water phases. PMID:16460160

  19. Influence of peculiarities of electronic excitation relaxation on luminescent properties of MgWO4

    NASA Astrophysics Data System (ADS)

    Krutyak, N. R.; Spassky, D. A.; Tupitsyna, I. A.; Dubovik, A. M.

    2016-07-01

    Luminescent properties of magnesium tungstate monocrystals grown by two different methods are studied. Only the exciton luminescence of these crystals themselves is observed. Temperature dependence of the low-energy range in the luminescence excitation spectra is described by the Urbach rule. Slope coefficient σ0 = 0.74 obtained from this dependence implies autolocalization of the excitons in MgWO4. The processes of electronic excitations relaxation are considered depending on the structure of valence band in MgWO4 and in other wolframites, ZnWO4 and CdWO4. In contrast to ZnWO4 and CdWO4, the d-states of the cation do not participate in formation of the MgWO4 valence band. Using the excitation spectra measured in the range of the fundamental absorption (4-20 eV), it is shown that this difference manifests itself in relaxation of electronic excitations and may be the cause of the relatively low light yield of MgWO4.

  20. Excitation cross-sections by electron impact for O V and O VI levels

    NASA Astrophysics Data System (ADS)

    Elabidi, H.; Sahal-Bréchot, S.

    2013-12-01

    Radiative atomic and electron impact excitation data for O V and O VI ions have been calculated. The radiative atomic data have been calculated with the AUTOSTRUCTURE code. Besides the one-body and the two-body fine structure interactions, the two-body non-fine structure operators of the Breit-Pauli Hamiltonian, namely contact spin-spin, two-body Darwin and orbit-orbit are incorporated in AUTOSTRUCTURE. The scattering problem has been treated in the Breit-Pauli distorted wave approximation using the same code AUTOSTRUCTURE. The O V atomic calculations have been extended from 46 to 92 levels. We have calculated excitation cross-sections for the O V 2s2-2s2p and the O VI 2s-2p transitions at energies near the corresponding excitation threshold regions. We have also calculated collision strengths for transitions from the most important levels for collisional excitation at electron energies up to 120 Ry for O V and up to 140 Ry for O VI. Our results have been compared with the available theoretical/experimental ones and a satisfactory agreement has been found between them.