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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

    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.

  6. 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.

  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. 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.

  1. 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.

  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. "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…

  14. 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

  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. 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.

  12. 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.

  13. 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.

  14. 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.

  15. 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.

  16. 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.

  17. 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.

  18. 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.

  19. 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.

  20. 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.

  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. 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

  9. 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.

  10. 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.

  11. 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.

  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. 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

  5. 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.

  6. 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.

  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. 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.

  9. 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.

  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. 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.

  16. 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

  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.

    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

  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

    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.

  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. 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

  13. 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.

  14. 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.

  15. 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

  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. 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.

  6. 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.

  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