Coulomb Excitation of the N = 50 nucleus 80Zn

NASA Astrophysics Data System (ADS)

van de Walle, J.; Aksouh, F.; Ames, F.; Behrens, T.; Bildstein, V.; Blazhev, A.; Cederkäll, J.; Clément, E.; Cocolios, T. E.; Davinson, T.; Delahaye, P.; Eberth, J.; Ekström, A.; Fedorov, D. V.; Fedosseev, V. N.; Fraile, L. M.; Franchoo, S.; Gernhauser, R.; Georgiev, G.; Habs, D.; Heyde, K.; Huber, G.; Huyse, M.; Ibrahim, F.; Ivanov, O.; Iwanicki, J.; Jolie, J.; Kester, O.; Köster, U.; Kröll, T.; Krücken, R.; Lauer, M.; Lisetskiy, A. F.; Lutter, R.; Marsh, B. A.; Mayet, P.; Niedermaier, O.; Nilsson, T.; Pantea, M.; Perru, O.; Raabe, R.; Reiter, P.; Sawicka, M.; Scheit, H.; Schrieder, G.; Schwalm, D.; Seliverstov, M. D.; Sieber, T.; Sletten, G.; Smirnova, N.; Stanoiu, M.; Stefanescu, I.; Thomas, J.-C.; Valiente-Dobón, J. J.; van Duppen, P.; Verney, D.; Voulot, D.; Warr, N.; Weisshaar, D.; Wenander, F.; Wolf, B. H.; Zielińska, M.

2008-05-01

Neutron rich Zinc isotopes, including the N = 50 nucleus 80Zn, were produced and post-accelerated at the Radioactive Ion Beam (RIB) facility REX-ISOLDE (CERN). Low-energy Coulomb excitation was induced on these isotopes after post-acceleration, yielding B(E2) strengths to the first excited 2+ states. For the first time, an excited state in 80Zn was observed and the 21+ state in 78Zn was established. The measured B(E2,21+-->01+) values are compared to two sets of large scale shell model calculations. Both calculations reproduce the observed B(E2) systematics for the full Zinc isotopic chain. The results for N = 50 isotones indicate a good N = 50 shell closure and a strong Z = 28 proton core polarization. The new results serve as benchmarks to establish theoretical models, predicting the nuclear properties of the doubly magic nucleus 78Ni.

Low-energy Coulomb excitation of neutron-rich zinc isotopes

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

Walle, J. van de; ISOLDE, CERN, Geneva; Aksouh, F.

2009-01-15

At the radioactive ion beam facility REX-ISOLDE, neutron-rich zinc isotopes were investigated using low-energy Coulomb excitation. These experiments have resulted in B(E2,2{sub 1}{sup +}{yields}0{sub 1}{sup +}) values in {sup 74-80}Zn, B(E2,4{sub 1}{sup +}{yields}2{sub 1}{sup +}) values in {sup 74,76}Zn and the determination of the energy of the first excited 2{sub 1}{sup +} states in {sup 78,80}Zn. The zinc isotopes were produced by high-energy proton- (A=74,76,80) and neutron- (A=78) induced fission of {sup 238}U, combined with selective laser ionization and mass separation. The isobaric beam was postaccelerated by the REX linear accelerator and Coulomb excitation was induced on a thin secondarymore » target, which was surrounded by the MINIBALL germanium detector array. In this work, it is shown how the selective laser ionization can be used to deal with the considerable isobaric beam contamination and how a reliable normalization of the experiment can be achieved. The results for zinc isotopes and the N=50 isotones are compared to collective model predictions and state-of-the-art large-scale shell-model calculations, including a recent empirical residual interaction constructed to describe the present experimental data up to 2004 in this region of the nuclear chart.« less

Magnetic moment and lifetime measurements of Coulomb-excited states in Cd 106

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

Benczer-Koller, N.; Kumbartzki, G. J.; Speidel, K. -H.

2016-09-06

The Cd isotopes are well studied, but experimental data for the rare isotopes are sparse. At energies above the Coulomb barrier, higher states become accessible. Remeasure and supplement existing lifetimes and magnetic moments of low-lying states in 106Cd. Methods: In an inverse kinematics reaction, a 106Cd beam impinging on a 12C target was used to Coulomb excite the projectiles. The high recoil velocities provide a unique opportunity to measure g factors with the transient-field technique and to determine lifetimes from lineshapes by using the Doppler-shift-attenuation method. Large-scale shell-model calculations were carried out for 106Cd. As a result, the g factorsmore » of the 2 + 1 and 4 + 1 states in 106Cd were measured to be g(2 + 1) = +0.398(22) and g(4 + 1) = +0.23(5). A lineshape analysis yielded lifetimes in disagreement with published values. The new results are τ( 106Cd; 2 + 1) = 7.0(3) ps and τ( 106Cd; 4 + 1) = 2.5(2) ps. The mean life τ( 106Cd; 2 + 2) = 0.28(2) ps was determined from the fully-Doppler-shifted γ line. Mean lives of τ( 106Cd; 4 + 3) = 1.1(1) ps and τ( 106Cd; 3 – 1) = 0.16(1) ps were determined for the first time. In conclusion, the newly measured g(4 + 1) of 106Cd is found to be only 59% of the g(2 + 1). This difference cannot be explained by either shell-model or collective-model calculations.« less

Coulomb Correlations Intertwined with Spin and Orbital Excitations in LaCoO_{3}.

PubMed

Tomiyasu, K; Okamoto, J; Huang, H Y; Chen, Z Y; Sinaga, E P; Wu, W B; Chu, Y Y; Singh, A; Wang, R-P; de Groot, F M F; Chainani, A; Ishihara, S; Chen, C T; Huang, D J

2017-11-10

We carried out temperature-dependent (20-550 K) measurements of resonant inelastic x-ray scattering on LaCoO_{3} to investigate the evolution of its electronic structure across the spin-state crossover. In combination with charge-transfer multiplet calculations, we accurately quantified the renomalized crystal-field excitation energies and spin-state populations. We show that the screening of the effective on-site Coulomb interaction of 3d electrons is orbital selective and coupled to the spin-state crossover in LaCoO_{3}. The results establish that the gradual spin-state crossover is associated with a relative change of Coulomb energy versus bandwidth, leading to a Mott-type insulator-to-metal transition.

Coulomb excitation of radioactive Na21 and its stable mirror Ne21

NASA Astrophysics Data System (ADS)

Schumaker, M. A.; Cline, D.; Hackman, G.; Morton, A. C.; Pearson, C. J.; Svensson, C. E.; Wu, C. Y.; Andreyev, A.; Austin, R. A. E.; Ball, G. C.; Bandyopadhyay, D.; Becker, J. A.; Boston, A. J.; Boston, H. C.; Buchmann, L.; Churchman, R.; Cifarelli, F.; Cooper, R. J.; Cross, D. S.; Dashdorj, D.; Demand, G. A.; Dimmock, M. R.; Drake, T. E.; Finlay, P.; Gallant, A. T.; Garrett, P. E.; Green, K. L.; Grint, A. N.; Grinyer, G. F.; Harkness, L. J.; Hayes, A. B.; Kanungo, R.; Leach, K. G.; Lee, G.; Maharaj, R.; Martin, J.-P.; Moisan, F.; Mythili, S.; Nelson, L.; Newman, O.; Nolan, P. J.; Orce, J. N.; Padilla-Rodal, E.; Phillips, A. A.; Porter-Peden, M.; Ressler, J. J.; Roy, R.; Ruiz, C.; Sarazin, F.; Scraggs, D. P.; Waddington, J. C.; Wan, J. M.; Whitbeck, A.; Williams, S. J.; Wong, J.

2008-10-01

The low-energy structures of the mirror nuclei Ne21 and radioactive Na21 have been examined by using Coulomb excitation at the TRIUMF-ISAC radioactive ion beam facility. Beams of ~5×106 ions/s were accelerated to 1.7 MeV/A and Coulomb excited in a 0.5 mg/cm2 natTi target. Scattered beam and target particles were detected by the segmented Si detector BAMBINO, while γ rays were observed by using two TIGRESS HPGe clover detectors perpendicular to the beam axis. For each isobar, Coulomb excitation from the (3)/(2)+ ground state to the first excited (5)/(2)+ state was observed and B(E2) values were determined by using the 2+→0+ de-excitation in Ti48 as a reference. The ϕ segmentation of BAMBINO was used to deduce tentative assignments for the signs of the mixing ratios between the E2 and M1 components of the transitions. The resulting B(E2)↑ values are 131±9e2 fm4 (25.4±1.7 W.u.) for Ne21 and 205±14e2 fm4 (39.7±2.7 W.u.) for Na21. The fit to the present data and the known lifetimes determined E2/M1 mixing ratios and B(M1)↓ values of δ=(-)0.0767±0.0027 and 0.1274±0.0025μN2 and δ=(+)0.0832±0.0028 and 0.1513±0.0017μN2 for Ne21 and Na21, respectively (with Krane and Steffen sign convention). By using the effective charges ep=1.5e and en=0.5e, the B(E2) values produced by the p-sd shell model are 30.7 and 36.4 W.u. for Ne21 and Na21, respectively. This analysis resolves a significant discrepancy between a previous experimental result for Na21 and shell-model calculations.

Coulomb Excitation of Exotic Nuclei

NASA Astrophysics Data System (ADS)

Macchiavelli, Augusto O.

2017-09-01

The structure of nuclei far from the stability line is a central theme of research in nuclear physics. Key to this program has been the worldwide development of radioactive beam facilities and novel detector systems, which provide the tools needed to produce and study these exotic nuclei. Coulomb Excitation provides a unique probe to characterize the interplay of collective and single-particle degrees of freedom of the atomic nucleus. In particular, the combination of state-of-the-art charged particle detectors and gamma-ray spectroscopy plays a vital and ubiquitous role in these studies. As an introduction to this Mini-Symposium, I will present a short overview of this powerful technique and selected examples of recent experiments. Future opportunities with a 4 π gamma-ray tracking array like GRETA will be discussed. This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Nuclear Physics under Contract No. DE-AC02-05CH11231 (LBNL).

Coulomb and nuclear excitations of narrow resonances in 17Ne

DOE PAGES

Marganiec, J.; Wamers, F.; Aksouh, F.; ...

2016-05-25

New experimental data for dissociation of relativistic 17Ne projectiles incident on targets of lead, carbon, and polyethylene targets at GSI are presented. Special attention is paid to the excitation and decay of narrow resonant states in 17Ne. Distributions of internal energy in the 15O+p +p three-body system have been determined together with angular and partial-energy correlations between the decay products in different energy regions. The analysis was done using existing experimental data on 17Ne and its mirror nucleus 17N. The isobaric multiplet mass equation is used for assignment of observed resonances and their spins and parities. A combination of datamore » from the heavy and light targets yielded cross sections and transition probabilities for the Coulomb excitations of the narrow resonant states. Finally, the resulting transition probabilities provide information relevant for a better understanding of the 17Ne structure.« less

/B(E2) values from low-energy Coulomb excitation at an ISOL facility: the /N=80,82 Te isotopes

NASA Astrophysics Data System (ADS)

Barton, C. J.; Caprio, M. A.; Shapira, D.; Zamfir, N. V.; Brenner, D. S.; Gill, R. L.; Lewis, T. A.; Cooper, J. R.; Casten, R. F.; Beausang, C. W.; Krücken, R.; Novak, J. R.

2003-01-01

B(E2;0+1→2+1) values for the unstable, neutron-rich nuclei 132,134Te were determined through Coulomb excitation, in inverse kinematics, of accelerated beams of these nuclei. The systematics of measured B(E2) values from the ground state to the first excited state have been extended to the N=82 shell closure in the Te nuclei and have been compared with the predictions of different theories. The measurements were performed at the Holifield Radioactive Ion Beam Facility (HRIBF) using the GRAFIK detector. The success of this approach, which couples a 5.7% efficient through-well NaI(Tl) γ-ray detector with thin foil microchannel plate beam detectors, also demonstrates the feasibility for Coulomb excitation studies of neutron-rich nuclei even further from the valley of beta stability, both at present-generation ISOL facilities and at the proposed Rare Isotope Accelerator.

Quadrupole collectivity in 42Ca from low-energy Coulomb excitation with AGATA

NASA Astrophysics Data System (ADS)

Hadyńska-Klęk, K.; Napiorkowski, P. J.; Zielińska, M.; Srebrny, J.; Maj, A.; Azaiez, F.; Valiente Dobón, J. J.; Kicińska-Habior, M.; Nowacki, F.; Naïdja, H.; Bounthong, B.; Rodríguez, T. R.; de Angelis, G.; Abraham, T.; Anil Kumar, G.; Bazzacco, D.; Bellato, M.; Bortolato, D.; Bednarczyk, P.; Benzoni, G.; Berti, L.; Birkenbach, B.; Bruyneel, B.; Brambilla, S.; Camera, F.; Chavas, J.; Cederwall, B.; Charles, L.; Ciemała, M.; Cocconi, P.; Coleman-Smith, P.; Colombo, A.; Corsi, A.; Crespi, F. C. L.; Cullen, D. M.; Czermak, A.; Désesquelles, P.; Doherty, D. T.; Dulny, B.; Eberth, J.; Farnea, E.; Fornal, B.; Franchoo, S.; Gadea, A.; Giaz, A.; Gottardo, A.; Grave, X.; Grębosz, J.; Görgen, A.; Gulmini, M.; Habermann, T.; Hess, H.; Isocrate, R.; Iwanicki, J.; Jaworski, G.; Judson, D. S.; Jungclaus, A.; Karkour, N.; Kmiecik, M.; Karpiński, D.; Kisieliński, M.; Kondratyev, N.; Korichi, A.; Komorowska, M.; Kowalczyk, M.; Korten, W.; Krzysiek, M.; Lehaut, G.; Leoni, S.; Ljungvall, J.; Lopez-Martens, A.; Lunardi, S.; Maron, G.; Mazurek, K.; Menegazzo, R.; Mengoni, D.; Merchán, E.; Męczyński, W.; Michelagnoli, C.; Million, B.; Myalski, S.; Napoli, D. R.; Niikura, M.; Obertelli, A.; Özmen, S. F.; Palacz, M.; Próchniak, L.; Pullia, A.; Quintana, B.; Rampazzo, G.; Recchia, F.; Redon, N.; Reiter, P.; Rosso, D.; Rusek, K.; Sahin, E.; Salsac, M.-D.; Söderström, P.-A.; Stefan, I.; Stézowski, O.; Styczeń, J.; Theisen, Ch.; Toniolo, N.; Ur, C. A.; Wadsworth, R.; Wasilewska, B.; Wiens, A.; Wood, J. L.; Wrzosek-Lipska, K.; Ziębliński, M.

2018-02-01

A Coulomb-excitation experiment to study electromagnetic properties of 42Ca was performed using a 170-MeV calcium beam from the TANDEM XPU facility at INFN Laboratori Nazionali di Legnaro. γ rays from excited states in 42Ca were measured with the AGATA spectrometer. The magnitudes and relative signs of ten E 2 matrix elements coupling six low-lying states in 42Ca, including the diagonal E 2 matrix elements of 21+ and 22+ states, were determined using the least-squares code gosia. The obtained set of reduced E 2 matrix elements was analyzed using the quadrupole sum rule method and yielded overall quadrupole deformation for 01,2 + and 21,2 + states, as well as triaxiality for 01,2 + states, establishing the coexistence of a weakly deformed ground-state band and highly deformed slightly triaxial sideband in 42Ca. The experimental results were compared with the state-of-the-art large-scale shell-model and beyond-mean-field calculations, which reproduce well the general picture of shape coexistence in 42Ca.

Collectivity in the light radon nuclei measured directly via Coulomb excitation

NASA Astrophysics Data System (ADS)

Gaffney, L. P.; Robinson, A. P.; Jenkins, D. G.; Andreyev, A. N.; Bender, M.; Blazhev, A.; Bree, N.; Bruyneel, B.; Butler, P. A.; Cocolios, T. E.; Davinson, T.; Deacon, A. N.; De Witte, H.; DiJulio, D.; Diriken, J.; Ekström, A.; Fransen, Ch.; Freeman, S. J.; Geibel, K.; Grahn, T.; Hadinia, B.; Hass, M.; Heenen, P.-H.; Hess, H.; Huyse, M.; Jakobsson, U.; Kesteloot, N.; Konki, J.; Kröll, Th.; Kumar, V.; Ivanov, O.; Martin-Haugh, S.; Mücher, D.; Orlandi, R.; Pakarinen, J.; Petts, A.; Peura, P.; Rahkila, P.; Reiter, P.; Scheck, M.; Seidlitz, M.; Singh, K.; Smith, J. F.; Van de Walle, J.; Van Duppen, P.; Voulot, D.; Wadsworth, R.; Warr, N.; Wenander, F.; Wimmer, K.; Wrzosek-Lipska, K.; Zielińska, M.

2015-06-01

Background: Shape coexistence in heavy nuclei poses a strong challenge to state-of-the-art nuclear models, where several competing shape minima are found close to the ground state. A classic region for investigating this phenomenon is in the region around Z =82 and the neutron midshell at N =104 . Purpose: Evidence for shape coexistence has been inferred from α -decay measurements, laser spectroscopy, and in-beam measurements. While the latter allow the pattern of excited states and rotational band structures to be mapped out, a detailed understanding of shape coexistence can only come from measurements of electromagnetic matrix elements. Method: Secondary, radioactive ion beams of 202Rn and 204Rn were studied by means of low-energy Coulomb excitation at the REX-ISOLDE in CERN. Results: The electric-quadrupole (E 2 ) matrix element connecting the ground state and first excited 21+ state was extracted for both 202Rn and 204Rn, corresponding to B (E 2 ;21+→01+) =29-8+8 and 43-12+17 W.u., respectively. Additionally, E 2 matrix elements connecting the 21+ state with the 41+ and 22+ states were determined in 202Rn. No excited 0+ states were observed in the current data set, possibly owing to a limited population of second-order processes at the currently available beam energies. Conclusions: The results are discussed in terms of collectivity and the deformation of both nuclei studied is deduced to be weak, as expected from the low-lying level-energy schemes. Comparisons are also made to state-of-the-art beyond-mean-field model calculations and the magnitude of the transitional quadrupole moments are well reproduced.

18Ne Excited States Two-Proton Decay

NASA Astrophysics Data System (ADS)

de Napoli, M.; Rapisarda, E.; Raciti, G.; Cardella, G.; Amorini, F.; Giacoppo, F.; Sfienti, C.

2008-04-01

Two-proton radioactivity studies have been performed on excited states of 18Ne produced by 20Ne fragmentation at the FRS of the Laboratori Nazionali del Sud and excited via Coulomb excitation on a 209Pb target. The 18Ne levels decay has been studied by complete kinematical reconstruction. In spite of the low statistic, the energy and angular correlations of the emitted proton pairs indicate the presence of 2He emission toghether with the democratic decay.

Coulomb Excitation of the 64Ni Nucleus and Application of Inverse Kinematics

NASA Astrophysics Data System (ADS)

Greaves, Beau; Muecher, Dennis; Ali, Fuad A.; Drake, Tom; Bildstein, Vinzenz; Berner, Christian; Gernhaeuser, Roman; Nowak, K.; Hellgartner, S.; Lutter, R.; Reichert, S.

2017-09-01

In this contribution, we present new data on the semi-magic 64Ni nucleus, close to the N =40 harmonic oscillator shell gap. Recent studies suggest a complicated existence of shape coexistence in 68Ni, likely caused by type-II shell evolutions. The region studied here thus might define the ``shore'' of the region of more deformed nuclei in the Island of Inversion below 68Ni. At the Maier-Leibnitz-Laboratory (MLL) in Munich, a beam of 64Ni was excited using Coulomb excitation. The high-granularity MINIBALL HPGe array and a segmented silicon strip detector were used to identify gamma decays in 64Ni. Doppler-shifted attenuation method (DSAM) analysis was applied to the experimental data acquired to resolve the low-lying excited states and acquire a lifetime measurement based on Geant4 simulations of the first excited 2 + state, clarifying the previously conflicting results. Furthermore, we show DSAM data following transfer reactions in inverse kinematics. This new method has the potential to provide insight into tests of ab-initio shell model calculations in the sd-pf shell and for the study of nuclear reaction rates. Supported under NSERC SAPIN-2016-00030.

Coulomb excitation of 206Hg at relativistic energies

NASA Astrophysics Data System (ADS)

Alexander, Tom

The region of the nuclear chart surrounding the doubly-magic nucleus 208Pb provides a key area to constrain and develop contemporary nuclear structure models. One aspect of particular interest is the transition strength of the first excited 2+ state in even-even nuclei; this work describes the measurement of this value for the case of 206Hg, where the Z=80 line meets the N=126 shell closure. The nuclei of interest were synthesized using relativistic-energy projectile fragmentation at the GSI facility in Germany. They were produced in the fragmentation of a primary 208Pb beam at an energy of 1 GeV per nucleon, and separated and identifed using the Fragment Separator. The secondary beams with an energy of 140 MeV per nucleon were Coulomb excited on a secondary target of 400 mg/cm. 2 gold. Gamma-rays were detected with the Advanced GAmma Tracking Array (AGATA). The precise scattering angle for Doppler-correction was determined with position information from the Lund-York-Cologne-CAlorimeter(LYCCA). Using the sophisticated tracking algorithm native to AGATA in conjunction with pulse-shape analysis, a precise Doppler-correction is performed on the gamma spectra, and using a complex n-dimensional analysis, the B(E2) value for 206Hg is extracted relative to the known value also measured in 206Pb. A total of 409 million 206Hg particles were measured, and a cross-section of 50 mb was determined for the 2+ state at 1068 keV. The measurement of the B(E2) transition strength was found to be 1.109 W.u. This result is compared to a number of theoretical calculations, including two Gogny forces, and a modified shell model parametrization and is found to be smaller than all calculated estimations, implying that the first excited 2. + state in . {206}Hg is uncollective in nature.

Photoionization of furan from the ground and excited electronic states.

PubMed

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

2016-02-28

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.

Coulomb excitations for a short linear chain of metallic shells

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

Zhemchuzhna, Liubov, E-mail: lzhemchuzhna@unm.edu; Center for High Technology Materials, University of New Mexico, Albuquerque, New Mexico 87106; Gumbs, Godfrey

2015-03-15

A self-consistent-field theory is given for the electronic collective modes of a chain containing a finite number, N, of Coulomb-coupled spherical two-dimensional electron gases arranged with their centers along a straight line, for simulating electromagnetic response of a narrow-ribbon of metallic shells. The separation between nearest-neighbor shells is arbitrary and because of the quantization of the electron energy levels due to their confinement to the spherical surface, all angular momenta L of the Coulomb excitations, as well as their projections M on the quantization axis, are coupled. However, for incoming light with a given polarization, only one angular momentum quantummore » number is usually required. Therefore, the electromagnetic response of the narrow-ribbon of metallic shells is expected to be controlled externally by selecting different polarizations for incident light. We show that, when N = 3, the next-nearest-neighbor Coulomb coupling is larger than its value if they are located at opposite ends of a right-angle triangle forming the triad. Additionally, the frequencies of the plasma excitations are found to depend on the orientation of the line joining them with respect to the axis of quantization since the magnetic field generated from the induced oscillating electric dipole moment on one sphere can couple to the induced magnetic dipole moment on another. Although the transverse inter-shell electromagnetic coupling can be modeled by an effective dynamic medium, the longitudinal inter-shell Coulomb coupling, on the other hand, can still significantly modify the electromagnetic property of this effective medium between shells.« less

Reply to "Comment on 'Calculations for the one-dimensional soft Coulomb problem and the hard Coulomb limit' ".

PubMed

Gebremedhin, Daniel H; Weatherford, Charles A

2015-02-01

This is a response to the comment we received on our recent paper "Calculations for the one-dimensional soft Coulomb problem and the hard Coulomb limit." In that paper, we introduced a computational algorithm that is appropriate for solving stiff initial value problems, and which we applied to the one-dimensional time-independent Schrödinger equation with a soft Coulomb potential. We solved for the eigenpairs using a shooting method and hence turned it into an initial value problem. In particular, we examined the behavior of the eigenpairs as the softening parameter approached zero (hard Coulomb limit). The commenters question the existence of the ground state of the hard Coulomb potential, which we inferred by extrapolation of the softening parameter to zero. A key distinction between the commenters' approach and ours is that they consider only the half-line while we considered the entire x axis. Based on mathematical considerations, the commenters consider only a vanishing solution function at the origin, and they question our conclusion that the ground state of the hard Coulomb potential exists. The ground state we inferred resembles a δ(x), and hence it cannot even be addressed based on their argument. For the excited states, there is agreement with the fact that the particle is always excluded from the origin. Our discussion with regard to the symmetry of the excited states is an extrapolation of the soft Coulomb case and is further explained herein.

Coulomb Excitation of Neutron-Rich Zn Isotopes: First Observation of the 21+ State in Zn80

NASA Astrophysics Data System (ADS)

van de Walle, J.; Aksouh, F.; Ames, F.; Behrens, T.; Bildstein, V.; Blazhev, A.; Cederkäll, J.; Clément, E.; Cocolios, T. E.; Davinson, T.; Delahaye, P.; Eberth, J.; Ekström, A.; Fedorov, D. V.; Fedosseev, V. N.; Fraile, L. M.; Franchoo, S.; Gernhauser, R.; Georgiev, G.; Habs, D.; Heyde, K.; Huber, G.; Huyse, M.; Ibrahim, F.; Ivanov, O.; Iwanicki, J.; Jolie, J.; Kester, O.; Köster, U.; Kröll, T.; Krücken, R.; Lauer, M.; Lisetskiy, A. F.; Lutter, R.; Marsh, B. A.; Mayet, P.; Niedermaier, O.; Nilsson, T.; Pantea, M.; Perru, O.; Raabe, R.; Reiter, P.; Sawicka, M.; Scheit, H.; Schrieder, G.; Schwalm, D.; Seliverstov, M. D.; Sieber, T.; Sletten, G.; Smirnova, N.; Stanoiu, M.; Stefanescu, I.; Thomas, J.-C.; Valiente-Dobón, J. J.; van Duppen, P.; Verney, D.; Voulot, D.; Warr, N.; Weisshaar, D.; Wenander, F.; Wolf, B. H.; Zielińska, M.

2007-10-01

Neutron-rich, radioactive Zn isotopes were investigated at the Radioactive Ion Beam facility REX-ISOLDE (CERN) using low-energy Coulomb excitation. The energy of the 21+ state in Zn78 could be firmly established and for the first time the 2+→01+ transition in Zn80 was observed at 1492(1) keV. B(E2,21+→01+) values were extracted for Zn74,76,78,80 and compared to large scale shell model calculations. With only two protons outside the Z=28 proton core, Zn80 is the lightest N=50 isotone for which spectroscopic information has been obtained to date. Two sets of advanced shell model calculations reproduce the observed B(E2) systematics. The results for N=50 isotones indicate a good N=50 shell closure and a strong Z=28 proton core polarization. The new results serve as benchmarks to establish theoretical models, predicting the nuclear properties of the doubly magic nucleus Ni78.

Deuteron Coulomb Excitation in Peripheral Collisions with a Heavy Ion

NASA Astrophysics Data System (ADS)

Du, Weijie; Yin, Peng; Li, Yang; Chen, Guangyao; Zuo, Wei; Zhao, Xingbo; Vary, James P.

2017-09-01

We develop an ab initio time-dependent Basis Function (tBF) method to solve non-perturbative and time-dependent problems in non-relativistic quantum mechanics. As a test problem, we apply this method to the Coulomb excitation of a deuteron by an impinging heavy ion. We employ wave functions for the bound and excited states of the deuterium system based on a realistic nucleon-nucleon interaction and study the evolution of the transition probability, the r.m.s. radius and the r.m.s. momentum of the system during the scattering process. The dependencies of these quantities on the external field strength and the bombarding energy are also analyzed and compared to corresponding results obtained from first-order perturbation theory. The time evolution of both the charge and the momentum distributions is shown. This work was supported in part by the U. S. Department of Energy (DOE) under Grants No. DESC0008485 (SciDAC/NUCLEI) and DE-FG02-87ER40371. W. Zuo and P. Yin are supported by the National Natural Science Foundation of China (11435014).

Influences of temperature and impurity on excited state of bound polaron in the parabolic quantum dots

NASA Astrophysics Data System (ADS)

Xiao, Jing-Lin

2014-06-01

On the condition of strong electron-LO phonon coupling in parabolic quantum dot (QD), the first excited state energy, the excitation energy and the transition frequency between the first excited and the ground states of the bound polaron are calculated by using the linear combination operator and the unitary transformation methods. The variation of the above quantities with the temperature, the Coulombic impurity potential and the QD confinement strength are studied in detail. We find that (1) These physical quantities will increase with increasing temperature. (2) They are increasing functions of the confinement strength due to the existence of the Coulombic impurity potential between the electron and the hydrogen-like impurity. (3) We obtain three ways of tuning them via controlling the temperature, the Coulombic impurity potential and the confinement strength.

Spin-isospin excitations from the ground-state of 64Ni

NASA Astrophysics Data System (ADS)

Popescu, L.; Adachi, T.; Bäumer, C.; Berg, G. P. A.; van den Berg, A. M.; von Brentano, P.; Frekers, D.; de Frenne, D.; Fujita, K.; Fujita, Y.; Grewe, E. W.; Haefner, P.; Hatanaka, K.; Hunyadi, M.; de Huu, M.; Jacobs, E.; Johansson, H.; Korff, A.; Negret, A.; Nakanishi, K.; von Neumann-Cosel, P.; Rakers, S.; Ryezayeva, N.; Sakemi, Y.; Shevchenko, A.; Shimbara, Y.; Shimizu, Y.; Simon, H.; Tameshige, Y.; Tamii, A.; Uchida, M.; Wörtche, H. J.; Yosoi, M.

2006-03-01

Spin-isospin (Gamow-Teller) excitations in 64Cu and 64Co have been studied using (3He,t) and (d,2He) charge-exchange reactions on 64Ni. As the isospin of the 64Ni ground-state is T0=4, states with T=3, 4 and 5 in 64Cu are excited via the (3He,t) reaction and states with T=5 in 64Co via (d,2He). If we assume that the nuclear interaction is charge symmetric, the T=5 states in 64Cu should appear at corresponding excitation energies (if corrected for the Coulomb displacement) and with similar strengths as the T=5 states in 64Co. As in the 64Cu spectrum the T=5 states are very weakly excited, only by combining the results of the two complementary experiments one can estimate the Gamow-Teller strength starting from 64Ni in a consistent way.

On rate-state and Coulomb failure models

USGS Publications Warehouse

Gomberg, J.; Beeler, N.; Blanpied, M.

2000-01-01

We examine the predictions of Coulomb failure stress and rate-state frictional models. We study the change in failure time (clock advance) Δt due to stress step perturbations (i.e., coseismic static stress increases) added to "background" stressing at a constant rate (i.e., tectonic loading) at time t0. The predictability of Δt implies a predictable change in seismicity rate r(t)/r0, testable using earthquake catalogs, where r0 is the constant rate resulting from tectonic stressing. Models of r(t)/r0, consistent with general properties of aftershock sequences, must predict an Omori law seismicity decay rate, a sequence duration that is less than a few percent of the mainshock cycle time and a return directly to the background rate. A Coulomb model requires that a fault remains locked during loading, that failure occur instantaneously, and that Δt is independent of t0. These characteristics imply an instantaneous infinite seismicity rate increase of zero duration. Numerical calculations of r(t)/r0 for different state evolution laws show that aftershocks occur on faults extremely close to failure at the mainshock origin time, that these faults must be "Coulomb-like," and that the slip evolution law can be precluded. Real aftershock population characteristics also may constrain rate-state constitutive parameters; a may be lower than laboratory values, the stiffness may be high, and/or normal stress may be lower than lithostatic. We also compare Coulomb and rate-state models theoretically. Rate-state model fault behavior becomes more Coulomb-like as constitutive parameter a decreases relative to parameter b. This is because the slip initially decelerates, representing an initial healing of fault contacts. The deceleration is more pronounced for smaller a, more closely simulating a locked fault. Even when the rate-state Δt has Coulomb characteristics, its magnitude may differ by some constant dependent on b. In this case, a rate-state model behaves like a modified

Coulomb bound states of strongly interacting photons

DOE PAGES

Maghrebi, M. F.; Gullans, Michael J.; Bienias, P.; ...

2015-09-16

We show that two photons coupled to Rydberg states via electromagnetically induced transparency (EIT) can interact via an effective Coulomb potential. The interaction then gives rise to a continuum of two-body bound states. Within the continuum, metastable bound states are distinguished in analogy with quasi-bound states tunneling through a potential barrier. We find multiple branches of metastable bound states whose energy spectrum is governed by the Coulomb problem, thus obtaining a photonic analogue of the hydrogen atom. These states propagate with a negative group velocity in the medium, which allows for a simple preparation and detection scheme, before they slowlymore » decay to pairs of bound Rydberg atoms. As a result, we verify the metastability and backward propagation of these Coulomb bound states with exact numerical simulations.« less

Spin-isospin excitations from the ground-state of 64Ni

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

Popescu, L.; Frenne, D. de; Jacobs, E.

2006-03-13

Spin-isospin (Gamow-Teller) excitations in 64Cu and 64Co have been studied using (3He,t) and (d,2He) charge-exchange reactions on 64Ni. As the isospin of the 64Ni ground-state is T0=4, states with T=3, 4 and 5 in 64Cu are excited via the (3He,t) reaction and states with T=5 in 64Co via (d,2He). If we assume that the nuclear interaction is charge symmetric, the T=5 states in 64Cu should appear at corresponding excitation energies (if corrected for the Coulomb displacement) and with similar strengths as the T=5 states in 64Co. As in the 64Cu spectrum the T=5 states are very weakly excited, only bymore » combining the results of the two complementary experiments one can estimate the Gamow-Teller strength starting from 64Ni in a consistent way.« less

Dynamical coupling of pygmy and giant resonances in relativistic Coulomb excitation

DOE PAGES

Brady, N. S.; Aumann, T.; Bertulani, C. A.; ...

2016-04-20

We study the Coulomb excitation of pygmy dipole resonances (PDR) in heavy ion reactions at 100 MeV/nucleon and above. The reactions Ni-68 + Au-197 and Ni-68 + Pb-208 are taken as practical examples. Our goal is to address the question of the influence of giant resonances on the PDR as the dynamics of the collision evolves. We show that the coupling to the giant resonances affects considerably the excitation probabilities of the PDR, a result that indicates the need of an improved theoretical treatment of the reaction dynamics at these bombarding energies. (C) 2016 The Authors. Published by Elsevier B.V.

First measurement with a new setup for low-energy Coulomb excitation studies at INFN LNL

NASA Astrophysics Data System (ADS)

Rocchini, M.; Hadyńska-Klȩk, K.; Nannini, A.; Valiente-Dobón, J. J.; Goasduff, A.; Testov, D.; John, P. R.; Mengoni, D.; Zielińska, M.; Bazzacco, D.; Benzoni, G.; Boso, A.; Cocconi, P.; Chiari, M.; Doherty, D. T.; Galtarossa, F.; Jaworski, G.; Komorowska, M.; Matejska-Minda, M.; Melon, B.; Menegazzo, R.; Napiorkowski, P.; Napoli, D. R.; Ottanelli, M.; Perego, A.; Ramina, L.; Rampazzo, M.; Recchia, F.; Riccetto, S.; Rosso, D.; Siciliano, M.; Sona, P.

2017-07-01

A new segmented particle detector, SPIDER, has been designed to be used as an ancillary device with the GALILEO γ-ray spectrometer, as well as with other multi-detector γ-ray arrays that will be available at LNL in the future (e.g. AGATA). To commission the SPIDER-GALILEO experimental setup, a multi-step Coulomb excitation experiment was carried out with a 240 MeV beam of 66Zn produced by the Tandem-XTU accelerator at INFN Laboratori Nazionali di Legnaro. The measured particle and γ-ray spectra are compared with the results of detailed GEANT4 simulations which used the Coulomb excitation cross sections, estimated with the computer code GOSIA, as an input. The preliminary results indicate that precise transition probabilities will be obtained which are essential for solving discrepancies reported in the literature for this nucleus.

Relativistic Coulomb Excitation within the Time Dependent Superfluid Local Density Approximation

NASA Astrophysics Data System (ADS)

Stetcu, I.; Bertulani, C. A.; Bulgac, A.; Magierski, P.; Roche, K. J.

2015-01-01

Within the framework of the unrestricted time-dependent density functional theory, we present for the first time an analysis of the relativistic Coulomb excitation of the heavy deformed open shell nucleus 238U. The approach is based on the superfluid local density approximation formulated on a spatial lattice that can take into account coupling to the continuum, enabling self-consistent studies of superfluid dynamics of any nuclear shape. We compute the energy deposited in the target nucleus as a function of the impact parameter, finding it to be significantly larger than the estimate using the Goldhaber-Teller model. The isovector giant dipole resonance, the dipole pygmy resonance, and giant quadrupole modes are excited during the process. The one-body dissipation of collective dipole modes is shown to lead a damping width Γ↓≈0.4 MeV and the number of preequilibrium neutrons emitted has been quantified.

First Results with TIGRESS and Accelerated Radioactive Ion Beams from ISAC: Coulomb Excitation of 20,21,29Na

NASA Astrophysics Data System (ADS)

Schumaker, M. A.; Hurst, A. M.; Svensson, C. E.; Wu, C. Y.; Becker, J. A.; Cline, D.; Hackman, G.; Pearson, C. J.; Stoyer, M. A.; Andreyev, A.; Austin, R. A. E.; Ball, G. C.; Bandyopadhyay, D.; Barton, C. J.; Boston, A. J.; Boston, H. C.; Buchmann, L.; Churchman, R.; Cifarelli, F.; Colosimo, S. J.; Cooper, R. J.; Cross, D. S.; Dashdorj, D.; Demand, G. A.; Dimmock, M. R.; Djongolov, M.; Drake, T. E.; Finlay, P.; Gallant, A. T.; Garrett, P. E.; Gray-Jones, C.; Green, K. L.; Grint, A. N.; Grinyer, G. F.; Harkness, L. J.; Hayes, A. B.; Kanungo, R.; Leach, K. G.; Kulp, W. D.; Lisetskiy, A. F.; Lee, G.; Lloyd, S.; Maharaj, R.; Martin, J.-P.; Millar, B. A.; Moisan, F.; Morton, A. C.; Mythili, S.; Nelson, L.; Newman, O.; Nolan, P. J.; Orce, J. N.; Oxley, D. C.; Padilla-Rodal, E.; Phillips, A. A.; Porter-Peden, M.; Ressler, J. J.; Rigby, S. V.; Roy, R.; Ruiz, C.; Sarazin, F.; Scraggs, D. P.; Sumithrarachchi, C. S.; Triambak, S.; Waddington, J. C.; Walker, P. M.; Wan, J.; Whitbeck, A.; Williams, S. J.; Wong, J.; Wood, J. L.

2009-03-01

The TRIUMF-ISAC Gamma-Ray Escape Suppressed Spectrometer (TIGRESS) is a state-of-the-art γ-ray spectrometer being constructed at the ISAC-II radioactive ion beam facility at TRIUMF. TIGRESS will be comprised of twelve 32-fold segmented high-purity germanium (HPGe) clover-type γ-ray detectors, with BGO/CsI(Tl) Compton-suppression shields, and is currently operational at ISAC-II in an early-implementation configuration of six detectors. Results have been obtained for the first experiments performed using TIGRESS, which examined the A = 20, 21, and 29 isotopes of Na by Coulomb excitation.

Relativistic Coulomb excitation within the time dependent superfluid local density approximation

DOE PAGES

Stetcu, I.; Bertulani, C. A.; Bulgac, A.; ...

2015-01-06

Within the framework of the unrestricted time-dependent density functional theory, we present for the first time an analysis of the relativistic Coulomb excitation of the heavy deformed open shell nucleus 238U. The approach is based on the superfluid local density approximation formulated on a spatial lattice that can take into account coupling to the continuum, enabling self-consistent studies of superfluid dynamics of any nuclear shape. We compute the energy deposited in the target nucleus as a function of the impact parameter, finding it to be significantly larger than the estimate using the Goldhaber-Teller model. The isovector giant dipole resonance, themore » dipole pygmy resonance, and giant quadrupole modes are excited during the process. As a result, the one-body dissipation of collective dipole modes is shown to lead a damping width Γ↓≈0.4 MeV and the number of preequilibrium neutrons emitted has been quantified.« less

Coulomb energy differences in isobaric multiplets

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

Lenzi, S. M.; Farnea, E.; Bazzacco, D.

2007-02-12

By comparing the excitation energies of analogue states in isobaric multiplets, several nuclear structure properties can be studied as a function of the angular momentum up to high spin states. In particular, the mirror nuclei 35Ar and 35Cl show large differences between the excitation energies of analogue negative-parity states at high spin, confirming the important contribution of the relativistic electromagnetic spin-orbit interaction to the Coulomb energy. The single-particle character of the configuration of these states is reproduced with very good accuracy by shell model calculations in the sd and pf shells valence space. In addition, evidence of isospin mixing ismore » deduced from the El transitions linking positive and negative parity states.« less

Optical spectroscopy of excited exciton states in MoS2 monolayers in van der Waals heterostructures

NASA Astrophysics Data System (ADS)

Robert, C.; Semina, M. A.; Cadiz, F.; Manca, M.; Courtade, E.; Taniguchi, T.; Watanabe, K.; Cai, H.; Tongay, S.; Lassagne, B.; Renucci, P.; Amand, T.; Marie, X.; Glazov, M. M.; Urbaszek, B.

2018-01-01

The optical properties of MoS2 monolayers are dominated by excitons, but for spectrally broad optical transitions in monolayers exfoliated directly onto SiO2 substrates detailed information on excited exciton states is inaccessible. Encapsulation in hexagonal boron nitride (hBN) allows approaching the homogenous exciton linewidth, but interferences in the van der Waals heterostructures make direct comparison between transitions in optical spectra with different oscillator strength more challenging. Here we reveal in reflectivity and in photoluminescence excitation spectroscopy the presence of excited states of the A exciton in MoS2 monolayers encapsulated in hBN layers of calibrated thickness, allowing us to extrapolate an exciton binding energy of ≈220 meV. We theoretically reproduce the energy separations and oscillator strengths measured in reflectivity by combining the exciton resonances calculated for a screened two-dimensional Coulomb potential with transfer matrix calculations of the reflectivity for the van der Waals structure. Our analysis shows a very different evolution of the exciton oscillator strength with principal quantum number for the screened Coulomb potential as compared to the ideal two-dimensional hydrogen model.

Influences of temperature on asymmetric quantum dot qubit in Coulombic impunity potential

NASA Astrophysics Data System (ADS)

Chen, Y.-J.; Song, H.-T.; Xiao, J.-L.

2018-05-01

Using the variational method of the Pekar-type, we study the influences of the temperature on the asymmetric quantum dot (QD) qubit in the Coulombic impunity potential. Then we derive the numerical results and formulate the derivative relationships of the electron probability density and the electron oscillation period in the superposition state of the ground state and the first-excited state with the electron-phonon coupling constant, the Coulombic impurity potential, the transverse and longitudinal confinement strengths at different temperatures, respectively.

Is the ground state of Yang-Mills theory Coulombic?

NASA Astrophysics Data System (ADS)

Heinzl, T.; Ilderton, A.; Langfeld, K.; Lavelle, M.; Lutz, W.; McMullan, D.

2008-08-01

We study trial states modelling the heavy quark-antiquark ground state in SU(2) Yang-Mills theory. A state describing the flux tube between quarks as a thin string of glue is found to be a poor description of the continuum ground state; the infinitesimal thickness of the string leads to UV artifacts which suppress the overlap with the ground state. Contrastingly, a state which surrounds the quarks with non-Abelian Coulomb fields is found to have a good overlap with the ground state for all charge separations. In fact, the overlap increases as the lattice regulator is removed. This opens up the possibility that the Coulomb state is the true ground state in the continuum limit.

Coulomb Excitation of n-rich nuclei along the N = 50 shell closure

NASA Astrophysics Data System (ADS)

Padilla-Rodal, E.; Galindo-Uribarri, A.; Batchelder, J. C.; Beene, J. R.; Bingham, C.; Brown, B. A.; Lagergren, K. B.; Mueller, P. E.; Radford, D. C.; Stracener, D. W.; Urrego-Blanco, J. P.; Varner, R. L.; Yu, C.-H.

2008-04-01

Recently, we have been investigating characteristics of nuclear states around the neutron-rich mass A=80 region [1]. Using the Radioactive Ion Beams (RIBs) produced at HRIBF, we have successfully measured the B(E2) values for ^78,80,82Ge , using Coulomb excitation in inverse kinematics. For the germanium isotopes, these data allow a study of the systematic trend between the subshell N= 40 and the N=50 shell. Using the same technique, we have measured the B(E2) value of various nuclei along the N=50 shell including the radioactive nucleus ^84Se. This value together with our previously measured ^82Ge, and the recent result on ^80Zn from ISOLDE [2] are providing basic experimental information needed for a better understanding of the neutron-rich nuclei around A˜80. We report the new results and compare with shell model calculations. [1] E. Padilla-Rodal et al., Phys. Rev. Lett. 94 (2005) 122501. [2] J. Van de Walle et al., Phys. Rev. Lett. 99 (2007) 142501.

Testing microscopically derived descriptions of nuclear collectivity: Coulomb excitation of 22Mg

NASA Astrophysics Data System (ADS)

Henderson, J.; Hackman, G.; Ruotsalainen, P.; Stroberg, S. R.; Launey, K. D.; Holt, J. D.; Ali, F. A.; Bernier, N.; Bentley, M. A.; Bowry, M.; Caballero-Folch, R.; Evitts, L. J.; Frederick, R.; Garnsworthy, A. B.; Garrett, P. E.; Jigmeddorj, B.; Kilic, A. I.; Lassen, J.; Measures, J.; Muecher, D.; Olaizola, B.; O'Sullivan, E.; Paetkau, O.; Park, J.; Smallcombe, J.; Svensson, C. E.; Wadsworth, R.; Wu, C. Y.

2018-07-01

Many-body nuclear theory utilizing microscopic or chiral potentials has developed to the point that collectivity might be studied within a microscopic or ab initio framework without the use of effective charges; for example with the proper evolution of the E2 operator, or alternatively, through the use of an appropriate and manageable subset of particle-hole excitations. We present a precise determination of E2 strength in 22Mg and its mirror 22Ne by Coulomb excitation, allowing for rigorous comparisons with theory. No-core symplectic shell-model calculations were performed and agree with the new B (E 2) values while in-medium similarity-renormalization-group calculations consistently underpredict the absolute strength, with the missing strength found to have both isoscalar and isovector components. The discrepancy between two microscopic models demonstrates the sensitivity of E2 strength to the choice of many-body approximation employed.

Numerical calculations of energy, nucleus size and coulomb decay rate for ddμ* resonance states in the variational approach using new wavefunctions

NASA Astrophysics Data System (ADS)

Eskandari, M. R.; Gheisari, R.; Kashian, S.

2006-02-01

This paper provides a theoretical complement to the experimental measurement of the population of excited dμ(2s) and dμ(1s) atoms in a deuterium. The population of these atoms plays an important role in a muon catalyzed fusion cycle. Symmetric and non-symmetric muonic molecular ions have been predicted to form in excited states in collisions between excited muonic atoms and hydrogen molecules. One example is the ddμ*, which is a muonic deuterium-deuterium symmetric ion in excited state and is initially produced in the interaction of dμ(2s) atoms with deuterium nuclei. Our calculations interpret the experimental findings in terms of the so-called side-path model. This model essentially deals with the interaction mentioned above in which the ddμ* ion undergoes Coulomb de-excitation where the excitation energy is shared between a dμ(1s) atom and one deuterium. The structure of ddμ* is studied here using the numerical, variational method and the given wavefunctions. Few resonance energies for ddμ* molecular states are calculated below the 2s threshold. For more precise assessment of the reliability of the given wavefunctions, the nucleus sizes and Coulomb decay rates for the zeroth, first and second vibrational meta-stable states of the mentioned ion are also calculated. The obtained results are close to those previously reported. The advantage of the given method over previous methods is that the used wavefunction has only two terms, which simplifies the calculations with the same results as those from the complicated coupled rearrangement channel method with a Gaussian basis set. These energies are the base data required for size, formation and decay rate calculations of the ddμ* ion.

Ab initio study on electronically excited states of lithium isocyanide, LiNC

NASA Astrophysics Data System (ADS)

Yasumatsu, Hisato; Jeung, Gwang-Hi

2014-01-01

The electronically excited states of the lithium isocyanide molecule, LiNC, were studied by means of ab initio calculations. The bonding nature of LiNC up to ∼10 eV is discussed on the basis of the potential energy surfaces according to the interaction between the ion-pair and covalent states. The ion-pair states are described by Coulomb attractive interaction in the long distance range, while the covalent ones are almost repulsive or bound with a very shallow potential dent. These two states interact each other to form adiabatic potential energy surfaces with non-monotonic change in the potential energy with the internuclear distance.

Computational assignment of redox states to Coulomb blockade diamonds.

PubMed

Olsen, Stine T; Arcisauskaite, Vaida; Hansen, Thorsten; Kongsted, Jacob; Mikkelsen, Kurt V

2014-09-07

With the advent of molecular transistors, electrochemistry can now be studied at the single-molecule level. Experimentally, the redox chemistry of the molecule manifests itself as features in the observed Coulomb blockade diamonds. We present a simple theoretical method for explicit construction of the Coulomb blockade diamonds of a molecule. A combined quantum mechanical/molecular mechanical method is invoked to calculate redox energies and polarizabilities of the molecules, including the screening effect of the metal leads. This direct approach circumvents the need for explicit modelling of the gate electrode. From the calculated parameters the Coulomb blockade diamonds are constructed using simple theory. We offer a theoretical tool for assignment of Coulomb blockade diamonds to specific redox states in particular, and a study of chemical details in the diamonds in general. With the ongoing experimental developments in molecular transistor experiments, our tool could find use in molecular electronics, electrochemistry, and electrocatalysis.

Three-body Coulomb systems using generalized angular-momentum S states

NASA Technical Reports Server (NTRS)

Whitten, R. C.; Sims, J. S.

1974-01-01

An expansion of the three-body Coulomb potential in generalized angular-momentum eigenfunctions developed earlier by one of the authors is used to compute energy eigenvalues and eigenfunctions of bound S states of three-body Coulomb systems. The results for He, H(-), e(-)e(+)e(-), and pmu(-)p are compared with the results of other computational approaches.

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

PubMed

Bircher, Martin P; Rothlisberger, Ursula

2018-06-12

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

Correlated wave functions for three-particle systems with Coulomb interaction - The muonic helium atom

NASA Technical Reports Server (NTRS)

Huang, K.-N.

1977-01-01

A computational procedure for calculating correlated wave functions is proposed for three-particle systems interacting through Coulomb forces. Calculations are carried out for the muonic helium atom. Variational wave functions which explicitly contain interparticle coordinates are presented for the ground and excited states. General Hylleraas-type trial functions are used as the basis for the correlated wave functions. Excited-state energies of the muonic helium atom computed from 1- and 35-term wave functions are listed for four states.

Quasi-stationary states and fermion pair creation from a vacuum in supercritical Coulomb field

NASA Astrophysics Data System (ADS)

Khalilov, V. R.

2017-12-01

Creation of charged fermion pair from a vacuum in so-called supercritical Coulomb potential is examined for the case when fermions can move only in the same (one) plane. In which case, quantum dynamics of charged massive or massless fermions can be described by the two-dimensional Dirac Hamiltonians with an usual (-a/r) Coulomb potential. These Hamiltonians are singular and require the additional definition in order for them to be treated as self-adjoint quantum-mechanical operators. We construct the self-adjoint two-dimensional Dirac Hamiltonians with a Coulomb potential and determine the quantum-mechanical states for such Hamiltonians in the corresponding Hilbert spaces of square-integrable functions. We determine the scattering amplitude in which the self-adjoint extension parameter is incorporated and then obtain equations implicitly defining possible discrete energy spectra of the self-adjoint Dirac Hamiltonians with a Coulomb potential. It is shown that this quantum system becomes unstable in the presence of a supercritical Coulomb potential which manifests in the appearance of quasi-stationary states in the lower (negative) energy continuum. The energy spectrum of those states is quasi-discrete, consists of broadened levels with widths related to the inverse lifetimes of the quasi-stationary states as well as the probability of creation of charged fermion pair by a supercritical Coulomb field. Explicit analytical expressions for the creation probabilities of charged (massive or massless) fermion pair are obtained in a supercritical Coulomb field.

Excited-state relaxation in PbSe quantum dots

NASA Astrophysics Data System (ADS)

An, Joonhee M.; Califano, Marco; Franceschetti, Alberto; Zunger, Alex

2008-04-01

In solids the phonon-assisted, nonradiative decay from high-energy electronic excited states to low-energy electronic excited states is picosecond fast. It was hoped that electron and hole relaxation could be slowed down in quantum dots, due to the unavailability of phonons energy matched to the large energy-level spacings ("phonon-bottleneck"). However, excited-state relaxation was observed to be rather fast (⩽1ps) in InP, CdSe, and ZnO dots, and explained by an efficient Auger mechanism, whereby the excess energy of electrons is nonradiatively transferred to holes, which can then rapidly decay by phonon emission, by virtue of the densely spaced valence-band levels. The recent emergence of PbSe as a novel quantum-dot material has rekindled the hope for a slow down of excited-state relaxation because hole relaxation was deemed to be ineffective on account of the widely spaced hole levels. The assumption of sparse hole energy levels in PbSe was based on an effective-mass argument based on the light effective mass of the hole. Surprisingly, fast intraband relaxation times of 1-7ps were observed in PbSe quantum dots and have been considered contradictory with the Auger cooling mechanism because of the assumed sparsity of the hole energy levels. Our pseudopotential calculations, however, do not support the scenario of sparse hole levels in PbSe: Because of the existence of three valence-band maxima in the bulk PbSe band structure, hole energy levels are densely spaced, in contradiction with simple effective-mass models. The remaining question is whether the Auger decay channel is sufficiently fast to account for the fast intraband relaxation. Using the atomistic pseudopotential wave functions of Pb2046Se2117 and Pb260Se249 quantum dots, we explicitly calculated the electron-hole Coulomb integrals and the P →S electron Auger relaxation rate. We find that the Auger mechanism can explain the experimentally observed P →S intraband decay time scale without the need to

First-principles investigation of quantum transport through an endohedral N@C60 in the Coulomb blockade regime.

PubMed

Yu, Zhizhou; Chen, Jian; Zhang, Lei; Wang, Jian

2013-12-11

We report an investigation of Coulomb blockade transport through an endohedral N@C60 weakly coupled with aluminum leads, employing the first-principles method combined with the Keldysh non-equilibrium Green's function derived from the equation of motion beyond the Hartree-Fock approximation. The differential conductance characteristics of the molecular device are calculated within the Coulomb blockade regime, which shows the Coulomb diamond as observed experimentally. When the gate voltage is less than that of the degeneracy point, there are two peaks in the differential conductance with an excited state induced by the change of the exchange interaction between the spin of C60 and the encapsulated nitrogen atom due to the transition from N@C(1-)(60) to N@C(2-)(60), while for a gate voltage larger than that of the degeneracy point, no excited state is available due to the quenching of exchange energy. As a result, there is only one Coulomb blockade peak in the differential conductance from the electron tunneling through the highest energy level below the Fermi level. Our first-principles results are in good agreement with experimental data obtained by an endohedral N@C60 molecular device.

Coulombic charge ice

NASA Astrophysics Data System (ADS)

McClarty, P. A.; O'Brien, A.; Pollmann, F.

2014-05-01

We consider a classical model of charges ±q on a pyrochlore lattice in the presence of long-range Coulomb interactions. This model first appeared in the early literature on charge order in magnetite [P. W. Anderson, Phys. Rev. 102, 1008 (1956), 10.1103/PhysRev.102.1008]. In the limit where the interactions become short ranged, the model has a ground state with an extensive entropy and dipolar charge-charge correlations. When long-range interactions are introduced, the exact degeneracy is broken. We study the thermodynamics of the model and show the presence of a correlated charge liquid within a temperature window in which the physics is well described as a liquid of screened charged defects. The structure factor in this phase, which has smeared pinch points at the reciprocal lattice points, may be used to detect charge ice experimentally. In addition, the model exhibits fractionally charged excitations ±q/2 which are shown to interact via a 1/r potential. At lower temperatures, the model exhibits a transition to a long-range ordered phase. We are able to treat the Coulombic charge ice model and the dipolar spin ice model on an equal footing by mapping both to a constrained charge model on the diamond lattice. We find that states of the two ice models are related by a staggering field which is reflected in the energetics of these two models. From this perspective, we can understand the origin of the spin ice and charge ice ground states as coming from a dipolar model on a diamond lattice. We study the properties of charge ice in an external electric field, finding that the correlated liquid is robust to the presence of a field in contrast to the case of spin ice in a magnetic field. Finally, we comment on the transport properties of Coulombic charge ice in the correlated liquid phase.

Magnetic Coulomb phase in the spin ice Ho2Ti2O7.

PubMed

Fennell, T; Deen, P P; Wildes, A R; Schmalzl, K; Prabhakaran, D; Boothroyd, A T; Aldus, R J; McMorrow, D F; Bramwell, S T

2009-10-16

Spin-ice materials are magnetic substances in which the spin directions map onto hydrogen positions in water ice. Their low-temperature magnetic state has been predicted to be a phase that obeys a Gauss' law and supports magnetic monopole excitations: in short, a Coulomb phase. We used polarized neutron scattering to show that the spin-ice material Ho2Ti2O7 exhibits an almost perfect Coulomb phase. Our result proves the existence of such phases in magnetic materials and strongly supports the magnetic monopole theory of spin ice.

11Li Breakup on 208 at energies around the Coulomb barrier.

PubMed

Fernández-García, J P; Cubero, M; Rodríguez-Gallardo, M; Acosta, L; Alcorta, M; Alvarez, M A G; Borge, M J G; Buchmann, L; Diget, C A; Falou, H A; Fulton, B R; Fynbo, H O U; Galaviz, D; Gómez-Camacho, J; Kanungo, R; Lay, J A; Madurga, M; Martel, I; Moro, A M; Mukha, I; Nilsson, T; Sánchez-Benítez, A M; Shotter, A; Tengblad, O; Walden, P

2013-04-05

The inclusive breakup for the (11)Li + (208)Pb reaction at energies around the Coulomb barrier has been measured for the first time. A sizable yield of (9)Li following the (11)Li dissociation has been observed, even at energies well below the Coulomb barrier. Using the first-order semiclassical perturbation theory of Coulomb excitation it is shown that the breakup probability data measured at small angles can be used to extract effective breakup energy as well as the slope of B(E1) distribution close to the threshold. Four-body continuum-discretized coupled-channels calculations, including both nuclear and Coulomb couplings between the target and projectile to all orders, reproduce the measured inclusive breakup cross sections and support the presence of a dipole resonance in the (11)Li continuum at low excitation energy.

Laser-modified Coulomb scattering states of an electron in the parabolic quasi-Sturmian-Floquet approach

NASA Astrophysics Data System (ADS)

Zaytsev, A. S.; Zaytsev, S. A.; Ancarani, L. U.; Kouzakov, K. A.

2018-04-01

Electron scattering states in combined Coulomb and laser fields are investigated with a nonperturbative approach based on the Hermitian Floquet theory. Taking into account the Coulomb-specific asymptotic behavior of the electron wave functions at large distances, a Lippmann-Schwinger-Floquet equation is derived in the Kramers-Henneberger frame. Such a scattering-state equation is solved numerically employing a set of parabolic quasi-Sturmian functions which have the great advantage of possessing, by construction, adequately chosen incoming or outgoing Coulomb asymptotic behaviors. Our quasi-Sturmian-Floquet approach is tested with a calculation of triple differential cross sections for a laser-assisted (e ,2 e ) process on atomic hydrogen within a first-order Born treatment of the projectile-atom interaction. Convergence with respect to the number of Floquet-Fourier expansion terms is numerically demonstrated. The illustration shows that the developed method is very efficient for the computation of light-dressed states of an electron moving in a Coulomb potential in the presence of laser radiation.

Coulomb dissociation of {sup 19}C

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

Nakamura, T.; Fukuda, N.; Iwasaki, H.

1998-12-21

We present the results on the Coulomb dissociation of the neutron-halo-nucleus candidate {sup 19}C, which was studied by a kinematically complete measurement of the breakup of {sup 19}C on a Pb target into {sup 18}C and neutron at 67{center_dot}AMeV. A large E1 strength has been observed at the low excitation energy of around 1 MeV to follow the distribution characteristic of the direct Coulomb breakup for the 2s{sub 1/2}-dominant configuration of {sup 19}C halo wave function. The angular distribution of {sup 18}C+n center of mass system has led to the indirect determination of {sup 19}C one-neutron separation energy, with whichmore » the excitation energy spectrum is well reproduced.« less

A cautionary tale: The Coulomb modified ANC for the 1/2+ 2 state in 17O

NASA Astrophysics Data System (ADS)

Keeley, N.; Kemper, K. W.; Rusek, K.

2018-05-01

We discuss the impact of the uncertainty (± 8 keV) in the excitation energy of the astrophysically important 6.356 MeV 1/2+2 state of 17O on the precision with which the Coulomb reduced ANC (\\widetilde{C}) for the < ^{17}O (1/2^+_2) | {}^{13}C + α> overlap can be extracted from direct reaction data. We find a linear dependence of \\widetilde{C}2 on the binding energy, the value extracted varying by a factor of 4 over the range E_{ex} = 6.356-6.348 MeV. This represents an intrinsic limit on the precision with which \\widetilde{C}2 can be determined which cannot be improved unless or until the uncertainty in E_{ex} is reduced.

Effect of compound nuclear reaction mechanism in 12C(6Li,d) reaction at sub-Coulomb energy

NASA Astrophysics Data System (ADS)

Mondal, Ashok; Adhikari, S.; Basu, C.

2017-09-01

The angular distribution of the 12C(6Li,d) reaction populating the 6.92 and 7.12 MeV states of 16O at sub-Coulomb energy (Ecm=3 MeV) are analysed in the framework of the Distorted Wave Born Approximation (DWBA). Recent results on excitation function measurements and backward angle angular distributions derive ANC for both the states on the basis of an alpha transfer mechanism. In the present work, we show that considering both forward and backward angle data in the analysis, the 7.12 MeV state at sub-Coulomb energy is populated from Compound nuclear process rather than transfer process. The 6.92 MeV state is however produced from direct reaction mechanism.

Rayleigh approximation to ground state of the Bose and Coulomb glasses

DOE PAGES

Ryan, S. D.; Mityushev, V.; Vinokur, V. M.; ...

2015-01-16

Glasses are rigid systems in which competing interactions prevent simultaneous minimization of local energies. This leads to frustration and highly degenerate ground states the nature and properties of which are still far from being thoroughly understood. We report an analytical approach based on the method of functional equations that allows us to construct the Rayleigh approximation to the ground state of a two-dimensional (2D) random Coulomb system with logarithmic interactions. We realize a model for 2D Coulomb glass as a cylindrical type II superconductor containing randomly located columnar defects (CD) which trap superconducting vortices induced by applied magnetic field. Ourmore » findings break ground for analytical studies of glassy systems, marking an important step towards understanding their properties.« less

Rayleigh approximation to ground state of the Bose and Coulomb glasses

PubMed Central

Ryan, S. D.; Mityushev, V.; Vinokur, V. M.; Berlyand, L.

2015-01-01

Glasses are rigid systems in which competing interactions prevent simultaneous minimization of local energies. This leads to frustration and highly degenerate ground states the nature and properties of which are still far from being thoroughly understood. We report an analytical approach based on the method of functional equations that allows us to construct the Rayleigh approximation to the ground state of a two-dimensional (2D) random Coulomb system with logarithmic interactions. We realize a model for 2D Coulomb glass as a cylindrical type II superconductor containing randomly located columnar defects (CD) which trap superconducting vortices induced by applied magnetic field. Our findings break ground for analytical studies of glassy systems, marking an important step towards understanding their properties. PMID:25592417

Relativistic Coulomb excitation of the giant dipole resonance in nuclei: How to calculate transition probabilities without invoking the Lienard-Wiechert relativistic scalar and vector potentials

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

Dasso, C.H.; Gallardo, M.

2006-01-15

The conclusions extracted from a recent study of the excitation of giant dipole resonances in nuclei at relativistic bombarding energies open the way for a further simplification of the problem. It consists in the elimination of the relativistic scalar and vector electromagnetic potentials and the familiar numerical difficulties associated with their presence in the calculation scheme. The inherent advantage of a reformulation of the problem of relativistic Coulomb excitation of giant dipole resonances along these lines is discussed.

Spectral representation of the three-body Coulomb problem. I. Nonautoionizing doubly excited states of high angular momentum in helium

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

Eiglsperger, Johannes; Piraux, Bernard; Madronero, Javier

2010-04-15

We investigate high-lying doubly excited nonautoionizing states of helium with total angular momentum L=1,2,...,9 with the help of a configuration interaction approach. We provide highly precise nonrelativistic energies of these states and discuss the properties of the wave functions with respect to the particle exchange operator.

Multiconfiguration pair-density functional theory for doublet excitation energies and excited state geometries: the excited states of CN.

PubMed

Bao, Jie J; Gagliardi, Laura; Truhlar, Donald G

2017-11-15

Multiconfiguration pair-density functional theory (MC-PDFT) is a post multiconfiguration self-consistent field (MCSCF) method with similar performance to complete active space second-order perturbation theory (CASPT2) but with greater computational efficiency. Cyano radical (CN) is a molecule whose spectrum is well established from experiments and whose excitation energies have been used as a testing ground for theoretical methods to treat excited states of open-shell systems, which are harder and much less studied than excitation energies of closed-shell singlets. In the present work, we studied the adiabatic excitation energies of CN with MC-PDFT. Then we compared this multireference (MR) method to some single-reference (SR) methods, including time-dependent density functional theory (TDDFT) and completely renormalized equation-of-motion coupled-cluster theory with singles, doubles and noniterative triples [CR-EOM-CCSD(T)]; we also compared to some other MR methods, including configuration interaction singles and doubles (MR-CISD) and multistate CASPT2 (MS-CASPT2). Through a comparison between SR and MR methods, we achieved a better appreciation of the need to use MR methods to accurately describe higher excited states, and we found that among the MR methods, MC-PDFT stands out for its accuracy for the first four states out of the five doublet states studied this paper; this shows its efficiency for calculating doublet excited states.

In-gap corner states in core-shell polygonal quantum rings

PubMed Central

Sitek, Anna; Ţolea, Mugurel; Niţă, Marian; Serra, Llorenç; Gudmundsson, Vidar; Manolescu, Andrei

2017-01-01

We study Coulomb interacting electrons confined in polygonal quantum rings. We focus on the interplay of localization at the polygon corners and Coulomb repulsion. Remarkably, the Coulomb repulsion allows the formation of in-gap states, i.e., corner-localized states of electron pairs or clusters shifted to energies that were forbidden for non-interacting electrons, but below the energies of corner-side-localized states. We specify conditions allowing optical excitation to those states. PMID:28071750

In-gap corner states in core-shell polygonal quantum rings.

PubMed

Sitek, Anna; Ţolea, Mugurel; Niţă, Marian; Serra, Llorenç; Gudmundsson, Vidar; Manolescu, Andrei

2017-01-10

We study Coulomb interacting electrons confined in polygonal quantum rings. We focus on the interplay of localization at the polygon corners and Coulomb repulsion. Remarkably, the Coulomb repulsion allows the formation of in-gap states, i.e., corner-localized states of electron pairs or clusters shifted to energies that were forbidden for non-interacting electrons, but below the energies of corner-side-localized states. We specify conditions allowing optical excitation to those states.

In-gap corner states in core-shell polygonal quantum rings

NASA Astrophysics Data System (ADS)

Sitek, Anna; Ţolea, Mugurel; Niţă, Marian; Serra, Llorenç; Gudmundsson, Vidar; Manolescu, Andrei

2017-01-01

We study Coulomb interacting electrons confined in polygonal quantum rings. We focus on the interplay of localization at the polygon corners and Coulomb repulsion. Remarkably, the Coulomb repulsion allows the formation of in-gap states, i.e., corner-localized states of electron pairs or clusters shifted to energies that were forbidden for non-interacting electrons, but below the energies of corner-side-localized states. We specify conditions allowing optical excitation to those states.

Solution of two-body relativistic bound state equations with confining plus Coulomb interactions

NASA Technical Reports Server (NTRS)

Maung, Khin Maung; Kahana, David E.; Norbury, John W.

1992-01-01

Studies of meson spectroscopy have often employed a nonrelativistic Coulomb plus Linear Confining potential in position space. However, because the quarks in mesons move at an appreciable fraction of the speed of light, it is necessary to use a relativistic treatment of the bound state problem. Such a treatment is most easily carried out in momentum space. However, the position space Linear and Coulomb potentials lead to singular kernels in momentum space. Using a subtraction procedure we show how to remove these singularities exactly and thereby solve the Schroedinger equation in momentum space for all partial waves. Furthermore, we generalize the Linear and Coulomb potentials to relativistic kernels in four dimensional momentum space. Again we use a subtraction procedure to remove the relativistic singularities exactly for all partial waves. This enables us to solve three dimensional reductions of the Bethe-Salpeter equation. We solve six such equations for Coulomb plus Confining interactions for all partial waves.

Theoretical studies of electronically excited states

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

Besley, Nicholas A.

2014-10-06

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

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

NASA Technical Reports Server (NTRS)

Green, T. J.

1973-01-01

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

Targeting excited states in all-trans polyenes with electron-pair states.

PubMed

Boguslawski, Katharina

2016-12-21

Wavefunctions restricted to electron pair states are promising models for strongly correlated systems. Specifically, the pair Coupled Cluster Doubles (pCCD) ansatz allows us to accurately describe bond dissociation processes and heavy-element containing compounds with multiple quasi-degenerate single-particle states. Here, we extend the pCCD method to model excited states using the equation of motion (EOM) formalism. As the cluster operator of pCCD is restricted to electron-pair excitations, EOM-pCCD allows us to target excited electron-pair states only. To model singly excited states within EOM-pCCD, we modify the configuration interaction ansatz of EOM-pCCD to contain also single excitations. Our proposed model represents a simple and cost-effective alternative to conventional EOM-CC methods to study singly excited electronic states. The performance of the excited state models is assessed against the lowest-lying excited states of the uranyl cation and the two lowest-lying excited states of all-trans polyenes. Our numerical results suggest that EOM-pCCD including single excitations is a good starting point to target singly excited states.

Effective temperature in relaxation of Coulomb glasses.

PubMed

Somoza, A M; Ortuño, M; Caravaca, M; Pollak, M

2008-08-01

We study relaxation in two-dimensional Coulomb glasses up to macroscopic times. We use a kinetic Monte Carlo algorithm especially designed to escape efficiently from deep valleys around metastable states. We find that, during the relaxation process, the site occupancy follows a Fermi-Dirac distribution with an effective temperature much higher than the real temperature T. Long electron-hole excitations are characterized by T(eff), while short ones are thermalized at T. We argue that the density of states at the Fermi level is proportional to T(eff) and is a good thermometer to measure it. T(eff) decreases extremely slowly, roughly as the inverse of the logarithm of time, and it should affect hopping conductance in many experimental circumstances.

Lifetimes of excited states in 196, 198Pt; Application of interacting boson approximation model to even Pt isotopes systematics

NASA Astrophysics Data System (ADS)

Bolotin, H. H.; Stuchbery, A. E.; Morrison, I.; Kennedy, D. L.; Ryan, C. G.; Sie, S. H.

1981-11-01

The lifetimes and lifetime limits of the low-lying excited states up to and including the 6 1+ levels in 196, 198Pt were determined by the recoil-distance method (RDM). Gamma-ray angular distributions in 198Pt were also measured. These states were populated by multiple Coulomb excitation using 220 MeV 58Ni ion beams and the measurements were carried out in coincidence with back-scattered projectiles. The measured mean lives of the states and B(E2) values inferred for the transitions between levels are presented. These specific findings, and the observed structure systematics obtained from the combination of the present results and those of prior workers for the even 194-198Pt isotopes, are critically compared with our structure calculations employing the interacting boson approximation (IBA) model incorporating a symmetry-breaking quadrupole force; evaluative comparisons are also made with boson expansion theory (BET) calculations.

Electronic correlation effects and the Coulomb gap at finite temperature.

PubMed

Sandow, B; Gloos, K; Rentzsch, R; Ionov, A N; Schirmacher, W

2001-02-26

We have investigated the effect of the long-range Coulomb interaction on the one-particle excitation spectrum of n-type germanium, using tunneling spectroscopy on mechanically controllable break junctions. At low temperatures, the tunnel conductance shows a minimum at zero bias voltage due to the Coulomb gap. Above 1 K, the gap is filled by thermal excitations. This behavior is reflected in the variable-range hopping resistivity measured on the same samples: up to a few degrees Kelvin the Efros-Shklovskii lnR infinity T(-1/2) law is obeyed, whereas at higher temperatures deviations from this law occur. The type of crossover differs from that considered previously in the literature.

Applications of the Coulomb-modified Glauber approximation to n = 2 and n = 3 excitation of hydrogenlike ions by incident electrons. II

NASA Technical Reports Server (NTRS)

Thomas, B. K.

1978-01-01

The Coulomb-modified form of the Glauber approximation is applied to the n = 2 and n = 3 excitation of hydrogenlike ions by incident electrons for various values of the target-ion nuclear charge Z sub n. The properly computed e(-)-He(+) 1s - 2s,2p Glauber predictions, including appropriate cascade effects, are compared with available experiment. The Z sub n dependence of the scaled integrated (over scattering angles) cross section is discussed, including the limit as Z sub n approaches infinity.

Nitric oxide excited under auroral conditions: Excited state densities and band emissions

NASA Astrophysics Data System (ADS)

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

2000-09-01

Electron impact excitation of vibrational levels in the ground electronic state and nine excited electronic states in NO has been simulated for an IBC II aurora (i.e., ˜10 kR in 3914 Å radiation) in order to predict NO excited state number densities and band emission intensities. New integral electron impact excitation cross sections for NO were combined with a measured IBC II auroral secondary electron distribution, and the vibrational populations of 10 NO electronic states were determined under conditions of statistical equilibrium. This model predicts an extended vibrational distribution in the NO ground electronic state produced by radiative cascade from the seven higher-lying doublet excited electronic states populated by electron impact. In addition to significant energy storage in vibrational excitation of the ground electronic state, both the a 4Π and L2 Φ excited electronic states are predicted to have relatively high number densities because they are only weakly connected to lower electronic states by radiative decay. Fundamental mode radiative transitions involving the lowest nine excited vibrational levels in the ground electronic state are predicted to produce infrared (IR) radiation from 5.33 to 6.05 μm with greater intensity than any single NO electronic emission band. Fundamental mode radiative transitions within the a 4Π electronic state, in the 10.08-11.37 μm region, are predicted to have IR intensities comparable to individual electronic emission bands in the Heath and ɛ band systems. Results from this model quantitatively predict the vibrational quantum number dependence of the NO IR measurements of Espy et al. [1988].

Orbitally excited spectra and decay of cc¯ meson

NASA Astrophysics Data System (ADS)

Chaturvedi, Raghav; Rai, A. K.

2018-05-01

We use the hydrogen like trial wave function for computation of the mass spectra and decay properties of charmonia within the framework of phenomenological quark anti-quark Coulomb plus power potential with varying potential index from 0.5 to 2.0. The spin-spin hyperfine interaction is considered to incorporate splitting of the ground and radially excited states energy levels, further spin-orbit and tensor interactions are employed to calculate the masses of orbitally excited states. We construct the Regge trajectories from the mass spectra in (J, M2) and (nr, M2) planes. We also compute γγ decay width of P wave states of cc¯.

Negative differential photoconductance in gold nanoparticle arrays in the Coulomb blockade regime.

PubMed

Mangold, Markus A; Calame, Michel; Mayor, Marcel; Holleitner, Alexander W

2012-05-22

We investigate the photoconductance of gold nanoparticle arrays in the Coulomb blockade regime. Two-dimensional, hexagonal crystals of nanoparticles are produced by self-assembly. The nanoparticles are weakly coupled to their neighbors by a tunneling conductance. At low temperatures, the single electron charging energy of the nanoparticles dominates the conductance properties of the array. The Coulomb blockade of the nanoparticles can be lifted by optical excitation with a laser beam. The optical excitation leads to a localized heating of the arrays, which in turn gives rise to a local change in conductance and a redistribution of the overall electrical potential in the arrays. We introduce a dual-beam optical excitation technique to probe the distribution of the electrical potential in the nanoparticle array. A negative differential photoconductance is the direct consequence of the redistribution of the electrical potential upon lifting of the Coulomb blockade. On the basis of our model, we calculate the optically induced current from the dark current-voltage characteristics of the nanoparticle array. The calculations closely reproduce the experimental observations.

Coulomb Impurity Potential RbCl Quantum Pseudodot Qubit

NASA Astrophysics Data System (ADS)

Ma, Xin-Jun; Qi, Bin; Xiao, Jing-Lin

2015-08-01

By employing a variational method of Pekar type, we study the eigenenergies and the corresponding eigenfunctions of the ground and the first-excited states of an electron strongly coupled to electron-LO in a RbCl quantum pseudodot (QPD) with a hydrogen-like impurity at the center. This QPD system may be used as a two-level quantum qubit. The expressions of electron's probability density versus time and the coordinates, and the oscillating period versus the Coulombic impurity potential and the polaron radius have been derived. The investigated results indicate ① that the probability density of the electron oscillates in the QPD with a certain oscillating period of , ② that due to the presence of the asymmetrical potential in the z direction of the RbCl QPD, the electron probability density shows double-peak configuration, whereas there is only one peak if the confinement is a two-dimensional symmetric structure in the xy plane of the QPD, ③ that the oscillation period is a decreasing function of the Coulombic impurity potential, whereas it is an increasing one of the polaron radius.

Higgs transition from a magnetic Coulomb liquid to a ferromagnet in Yb₂Ti₂O₇.

PubMed

Chang, Lieh-Jeng; Onoda, Shigeki; Su, Yixi; Kao, Ying-Jer; Tsuei, Ku-Ding; Yasui, Yukio; Kakurai, Kazuhisa; Lees, Martin Richard

2012-01-01

In a class of frustrated magnets known as spin ice, magnetic monopoles emerge as classical defects and interact via the magnetic Coulomb law. With quantum-mechanical interactions, these magnetic charges are carried by fractionalized bosonic quasi-particles, spinons, which can undergo Bose-Einstein condensation through a first-order transition via the Higgs mechanism. Here, we report evidence of a Higgs transition from a magnetic Coulomb liquid to a ferromagnet in single-crystal Yb(2)Ti(2)O(7). Polarized neutron scattering experiments show that the diffuse [111]-rod scattering and pinch-point features, which develop on cooling are suddenly suppressed below T(C)~0.21 K, where magnetic Bragg peaks and a full depolarization of the neutron spins are observed with thermal hysteresis, indicating a first-order ferromagnetic transition. Our results are explained on the basis of a quantum spin-ice model, whose high-temperature phase is effectively described as a magnetic Coulomb liquid, whereas the ground state shows a nearly collinear ferromagnetism with gapped spin excitations.

Spurious Excitations in Semiclassical Scattering Theory.

ERIC Educational Resources Information Center

Gross, D. H. E.; And Others

1980-01-01

Shows how through proper handling of the nonuniform motion of semiclassical coordinates spurious excitation terms are eliminated. An application to the problem of nuclear Coulomb excitation is presented as an example. (HM)

Long-range Coulomb interaction effects on the topological phase transitions between semimetals and insulators

NASA Astrophysics Data System (ADS)

Han, SangEun; Moon, Eun-Gook

2018-06-01

Topological states may be protected by a lattice symmetry in a class of topological semimetals. In three spatial dimensions, the Berry flux around gapless excitations in momentum space concretely defines a chirality, so a protecting symmetry may be referred to as a chiral symmetry. Prime examples include a Dirac semimetal (DSM) in a distorted spinel, BiZnSiO4, protected by a mirror symmetry, and a DSM in Na3Bi , protected by a rotational symmetry. In these states, topology and chiral symmetry are intrinsically tied. In this Rapid Communication, the characteristic interplay between a chiral symmetry order parameter and an instantaneous long-range Coulomb interaction is investigated with the standard renormalization group method. We show that a topological transition associated with chiral symmetry is stable under the presence of a Coulomb interaction and the electron velocity always becomes faster than the one of a chiral symmetry order parameter. Thus, the transition must not be relativistic, which implies that supersymmetry is intrinsically forbidden by the long-range Coulomb interaction. Asymptotically exact universal ratios of physical quantities such as the energy gap ratio are obtained, and connections with experiments and recent theoretical proposals are also discussed.

Extended Lagrangian Excited State Molecular Dynamics.

PubMed

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

2018-02-13

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

Reorientation-effect measurement of the first 2+ state in 12C: Confirmation of oblate deformation

NASA Astrophysics Data System (ADS)

Kumar Raju, M.; Orce, J. N.; Navrátil, P.; Ball, G. C.; Drake, T. E.; Triambak, S.; Hackman, G.; Pearson, C. J.; Abrahams, K. J.; Akakpo, E. H.; Al Falou, H.; Churchman, R.; Cross, D. S.; Djongolov, M. K.; Erasmus, N.; Finlay, P.; Garnsworthy, A. B.; Garrett, P. E.; Jenkins, D. G.; Kshetri, R.; Leach, K. G.; Masango, S.; Mavela, D. L.; Mehl, C. V.; Mokgolobotho, M. J.; Ngwetsheni, C.; O'Neill, G. G.; Rand, E. T.; Sjue, S. K. L.; Sumithrarachchi, C. S.; Svensson, C. E.; Tardiff, E. R.; Williams, S. J.; Wong, J.

2018-02-01

A Coulomb-excitation reorientation-effect measurement using the TIGRESS γ-ray spectrometer at the TRIUMF/ISAC II facility has permitted the determination of the 〈 21+ ‖ E 2 ˆ ‖21+ 〉 diagonal matrix element in 12C from particle-γ coincidence data and state-of-the-art no-core shell model calculations of the nuclear polarizability. The nuclear polarizability for the ground and first-excited (21+) states in 12C have been calculated using chiral NN N4LO500 and NN+3NF350 interactions, which show convergence and agreement with photo-absorption cross-section data. Predictions show a change in the nuclear polarizability with a substantial increase between the ground state and first excited 21+ state at 4.439 MeV. The polarizability of the 21+ state is introduced into the current and previous Coulomb-excitation reorientation-effect analyses of 12C. Spectroscopic quadrupole moments of QS (21+) = + 0.053 (44) eb and QS (21+) = + 0.08 (3) eb are determined, respectively, yielding a weighted average of QS (21+) = + 0.071 (25) eb, in agreement with recent ab initio calculations. The present measurement confirms that the 21+ state of 12C is oblate and emphasizes the important role played by the nuclear polarizability in Coulomb-excitation studies of light nuclei.

Superdeformed and Triaxial States in 42Ca

NASA Astrophysics Data System (ADS)

Hadyńska-KlÈ©k, K.; Napiorkowski, P. J.; Zielińska, M.; Srebrny, J.; Maj, A.; Azaiez, F.; Valiente Dobón, J. J.; Kicińska-Habior, M.; Nowacki, F.; Naïdja, H.; Bounthong, B.; Rodríguez, T. R.; de Angelis, G.; Abraham, T.; Anil Kumar, G.; Bazzacco, D.; Bellato, M.; Bortolato, D.; Bednarczyk, P.; Benzoni, G.; Berti, L.; Birkenbach, B.; Bruyneel, B.; Brambilla, S.; Camera, F.; Chavas, J.; Cederwall, B.; Charles, L.; Ciemała, M.; Cocconi, P.; Coleman-Smith, P.; Colombo, A.; Corsi, A.; Crespi, F. C. L.; Cullen, D. M.; Czermak, A.; Désesquelles, P.; Doherty, D. T.; Dulny, B.; Eberth, J.; Farnea, E.; Fornal, B.; Franchoo, S.; Gadea, A.; Giaz, A.; Gottardo, A.; Grave, X.; GrÈ©bosz, J.; Görgen, A.; Gulmini, M.; Habermann, T.; Hess, H.; Isocrate, R.; Iwanicki, J.; Jaworski, G.; Judson, D. S.; Jungclaus, A.; Karkour, N.; Kmiecik, M.; Karpiński, D.; Kisieliński, M.; Kondratyev, N.; Korichi, A.; Komorowska, M.; Kowalczyk, M.; Korten, W.; Krzysiek, M.; Lehaut, G.; Leoni, S.; Ljungvall, J.; Lopez-Martens, A.; Lunardi, S.; Maron, G.; Mazurek, K.; Menegazzo, R.; Mengoni, D.; Merchán, E.; MÈ©czyński, W.; Michelagnoli, C.; Mierzejewski, J.; Million, B.; Myalski, S.; Napoli, D. R.; Nicolini, R.; Niikura, M.; Obertelli, A.; Özmen, S. F.; Palacz, M.; Próchniak, L.; Pullia, A.; Quintana, B.; Rampazzo, G.; Recchia, F.; Redon, N.; Reiter, P.; Rosso, D.; Rusek, K.; Sahin, E.; Salsac, M.-D.; Söderström, P.-A.; Stefan, I.; Stézowski, O.; Styczeń, J.; Theisen, Ch.; Toniolo, N.; Ur, C. A.; Vandone, V.; Wadsworth, R.; Wasilewska, B.; Wiens, A.; Wood, J. L.; Wrzosek-Lipska, K.; ZiÈ©bliński, M.

2016-08-01

Shape parameters of a weakly deformed ground-state band and highly deformed slightly triaxial sideband in 42Ca were determined from E 2 matrix elements measured in the first low-energy Coulomb excitation experiment performed with AGATA. The picture of two coexisting structures is well reproduced by new state-of-the-art large-scale shell model and beyond-mean-field calculations. Experimental evidence for superdeformation of the band built on 02+ has been obtained and the role of triaxiality in the A ˜40 mass region is discussed. Furthermore, the potential of Coulomb excitation as a tool to study superdeformation has been demonstrated for the first time.

Excited-State Deactivation of Branched Phthalocyanine Compounds.

PubMed

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

2015-12-21

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

Statistics of excitations in the electron glass model

NASA Astrophysics Data System (ADS)

Palassini, Matteo

2011-03-01

We study the statistics of elementary excitations in the classical electron glass model of localized electrons interacting via the unscreened Coulomb interaction in the presence of disorder. We reconsider the long-standing puzzle of the exponential suppression of the single-particle density of states near the Fermi level, by measuring accurately the density of states of charged and electron-hole pair excitations via finite temperature Monte Carlo simulation and zero-temperature relaxation. We also investigate the statistics of large charge rearrangements after a perturbation of the system, which may shed some light on the slow relaxation and glassy phenomena recently observed in a variety of Anderson insulators. In collaboration with Martin Goethe.

Extended Lagrangian Excited State Molecular Dynamics

DOE PAGES

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

2018-01-09

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

Extended Lagrangian Excited State Molecular Dynamics

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

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

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

Excited-State Effective Masses in Lattice QCD

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

George Fleming, Saul Cohen, Huey-Wen Lin

2009-10-01

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

Charge transfer excitations from exact and approximate ensemble Kohn-Sham theory

NASA Astrophysics Data System (ADS)

Gould, Tim; Kronik, Leeor; Pittalis, Stefano

2018-05-01

By studying the lowest excitations of an exactly solvable one-dimensional soft-Coulomb molecular model, we show that components of Kohn-Sham ensembles can be used to describe charge transfer processes. Furthermore, we compute the approximate excitation energies obtained by using the exact ensemble densities in the recently formulated ensemble Hartree-exchange theory [T. Gould and S. Pittalis, Phys. Rev. Lett. 119, 243001 (2017)]. Remarkably, our results show that triplet excitations are accurately reproduced across a dissociation curve in all cases tested, even in systems where ground state energies are poor due to strong static correlations. Singlet excitations exhibit larger deviations from exact results but are still reproduced semi-quantitatively.

Resource Paper: Molecular Excited State Relaxation Processes.

ERIC Educational Resources Information Center

Rhodes, William

1979-01-01

Develops the concept of oscillatory v dissipative limits as it applies to electronic excited state processes in molecular systems. Main emphasis is placed on the radiative and nonradiative dynamics of the excited state of a molecule prepared by interaction with light or some other excitation source. (BT)

Three-body Coulomb bound states

NASA Technical Reports Server (NTRS)

Bhatia, A. K.; Drachman, Richard J.

1987-01-01

The binding energies of three-particle systems containing two electrons and one positive particle of mass M are reexamined in an attempt to understand the approximate proportionality of the 1Se ground-state binding energies of the reduced masses, as pointed out by Botero and Green (1986). The contribution to the energy of the mass-polarization term is evaluated. No fundamental principle is involved, since the mass polarization merely decreases somewhat as the mass of the positive particle is reduced below the proton mass. In the case of the excited 3Pe state, this reduction is not sufficient to allow binding when M approaches the electron mass. Some properties of the recently observed negative muonium ion (e/-/ mu/+/ e/-/) are also computed.

Coulomb-nuclear interference with {sup 6}Li: Isospin character of the 2{sub 1}{sup +} excitation in {sup 70,72,74}Ge

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

Barbosa, M.D.L.; Borello-Lewin, T.; Horodynski-Matsushigue, L.B.

2005-02-01

Ratios of B(E2) to B(IS2), that is, of the reduced quadrupole transition probabilities related, respectively, to charge and mass were extracted through Coulomb-nuclear interference (CNI) for the excitation of the 2{sub 1}{sup +} states in {sup 70,72,74}Ge, with a relative accuracy of less than 4%. For this purpose, the CNI angular distributions associated with the inelastic scattering of 28-MeV incident {sup 6}Li ions accelerated by the Sao Paulo Pelletron, and momentum analyzed by the Enge magnetic spectrograph were interpreted within the DWBA-DOMP approach (distorted wave approximation for the scattering process and deformed optical model for the structure representation) with globalmore » {sup 6}Li optical parameters. The present CNI results demonstrate an abrupt change in the B(E2)/B(IS2) ratio for {sup 74}Ge: although for {sup 70,72}Ge, values of the order of 1.0 or slightly higher were obtained, this ratio is 0.66 (7) for {sup 74}Ge. The heavier Ge isotope is thus one of the few nuclei that, so far, have been shown to present clear mixed symmetry components in their ground-state band.« less

Search for excited states in 25O

NASA Astrophysics Data System (ADS)

Jones, M. D.; Fossez, K.; Baumann, T.; DeYoung, P. A.; Finck, J. E.; Frank, N.; Kuchera, A. N.; Michel, N.; Nazarewicz, W.; Rotureau, J.; Smith, J. K.; Stephenson, S. L.; Stiefel, K.; Thoennessen, M.; Zegers, R. G. T.

2017-11-01

Background: Theoretical calculations suggest the presence of low-lying excited states in 25O. Previous experimental searches by means of proton knockout on 26F produced no evidence for such excitations. Purpose: We search for excited states in 25O using the 24O(d ,p ) 25O reaction. The theoretical analysis of excited states in unbound O,2725 is based on the configuration interaction approach that accounts for couplings to the scattering continuum. Method: We use invariant-mass spectroscopy to measure neutron-unbound states in 25O. For the theoretical approach, we use the complex-energy Gamow Shell Model and Density Matrix Renormalization Group method with a finite-range two-body interaction optimized to the bound states and resonances of O-2623, assuming a core of 22O. We predict energies, decay widths, and asymptotic normalization coefficients. Results: Our calculations in a large s p d f space predict several low-lying excited states in 25O of positive and negative parity, and we obtain an experimental limit on the relative cross section of a possible Jπ=1/2 + state with respect to the ground state of 25O at σ1 /2 +/σg .s .=0 .25-0.25+1.0 . We also discuss how the observation of negative parity states in 25O could guide the search for the low-lying negative parity states in 27O. Conclusion: Previous experiments based on the proton knockout of 26F suffered from the low cross sections for the population of excited states in 25O because of low spectroscopic factors. In this respect, neutron transfer reactions carry more promise.

Comment on "Calculations for the one-dimensional soft Coulomb problem and the hard Coulomb limit".

PubMed

Carrillo-Bernal, M A; Núñez-Yépez, H N; Salas-Brito, A L; Solis, Didier A

2015-02-01

In the referred paper, the authors use a numerical method for solving ordinary differential equations and a softened Coulomb potential -1/√[x(2)+β(2)] to study the one-dimensional Coulomb problem by approaching the parameter β to zero. We note that even though their numerical findings in the soft potential scenario are correct, their conclusions do not extend to the one-dimensional Coulomb problem (β=0). Their claims regarding the possible existence of an even ground state with energy -∞ with a Dirac-δ eigenfunction and of well-defined parity eigenfunctions in the one-dimensional hydrogen atom are questioned.

State-selective optimization of local excited electronic states in extended systems

NASA Astrophysics Data System (ADS)

Kovyrshin, Arseny; Neugebauer, Johannes

2010-11-01

Standard implementations of time-dependent density-functional theory (TDDFT) for the calculation of excitation energies give access to a number of the lowest-lying electronic excitations of a molecule under study. For extended systems, this can become cumbersome if a particular excited state is sought-after because many electronic transitions may be present. This often means that even for systems of moderate size, a multitude of excited states needs to be calculated to cover a certain energy range. Here, we present an algorithm for the selective determination of predefined excited electronic states in an extended system. A guess transition density in terms of orbital transitions has to be provided for the excitation that shall be optimized. The approach employs root-homing techniques together with iterative subspace diagonalization methods to optimize the electronic transition. We illustrate the advantages of this method for solvated molecules, core-excitations of metal complexes, and adsorbates at cluster surfaces. In particular, we study the local π →π∗ excitation of a pyridine molecule adsorbed at a silver cluster. It is shown that the method works very efficiently even for high-lying excited states. We demonstrate that the assumption of a single, well-defined local excitation is, in general, not justified for extended systems, which can lead to root-switching during optimization. In those cases, the method can give important information about the spectral distribution of the orbital transition employed as a guess.

Coulomb thermal properties and stability of the Io plasma torus

NASA Technical Reports Server (NTRS)

Barbosa, D. D.; Coroniti, F. V.; Eviatar, A.

1983-01-01

Coulomb collisional energy exchange rates are computed for a model of the Io plasma torus consisting of newly created pickup ions, a background of thermally degraded intermediary ions, and a population of cooler electrons. The electrons are collisionally heated by both the pickup ions and background ions and are cooled by electron impact excitation of plasma ions which radiate in the EUV. It is found that a relative concentration of S III pickup ions forbidden S III/electrons = 0.1 with a temperature of 340 eV can deliver energy to the electrons at a rate of 3 x 10 to the -13th erg/cu cm per sec, sufficient to power the EUV emissions in the Io torus. The model predicts a background ion temperature Ti of about 53 eV and an electron temperature Te of about 5.5 eV on the basis of steady-state energy balance relations at Coulomb rates. The model also predicts electron temperature fluctuations at the 30 percent level on a time scale of less than 11 hours, consistent with recent observations of this phenomenon.

Microwave-optical two-photon excitation of Rydberg states

NASA Astrophysics Data System (ADS)

Tate, D. A.; Gallagher, T. F.

2018-03-01

We report efficient microwave-optical two photon excitation of Rb Rydberg atoms in a magneto-optical trap. This approach allows the excitation of normally inaccessible states and provides a path toward excitation of high-angular-momentum states. The efficiency stems from the elimination of the Doppler width, the use of a narrow-band pulsed laser, and the enormous electric-dipole matrix element connecting the intermediate and final states of the transition. The excitation is efficient in spite of the low optical and microwave powers, of order 1 kW and 1 mW, respectively. This is an application of the large dipole coupling strengths between Rydberg states to achieve two-photon excitation of Rydberg atoms.

Laser-induced transitions between triply excited hollow states

NASA Astrophysics Data System (ADS)

Madsen, L. B.; Schlagheck, P.; Lambropoulos, P.

2000-12-01

Using complex scaling and a correlated basis constructed in terms of B splines, we calculate the Li+ photoion yield in the presence of a laser-induced coupling between the triply excited 2s22p(2Po) and 2s2p2(2De) resonances in lithium, the first of which is assumed to be excited by synchrotron radiation from the ground state. The laser coupling between the triply excited states is shown to lead to a significant and readily measurable modification of the line profile which provides a unique probe of the dipole strength between highly correlated triply excited states. We also present results for some higher-lying triply excited states of 2Po symmetry.

Lifetimes of low-lying excited states in Kr 50 36 86

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

Henderson, J.; Chester, A.; Ball, G. C.

b>Bmore » The evolution of nuclear magic numbers at extremes of isospin is a topic at the forefront of contemporary nuclear physics. N = 50 is a prime example, with increasing experimental data coming to light on potentially doubly magic Sn 100 and Ni 78 at the proton-rich and proton-deficient extremes, respectively; however, experimental discrepancies exist in the data for less exotic systems. Purpose: In Kr 86 the B ( E 2 ; 2 1 + → 0 1 + ) value—a key indicator of shell evolution—has been experimentally determined by two different methodologies, with the results deviating by 3 σ . Here, we report on a new high-precision measurement of this value, as well as the first measured lifetimes and hence transition strengths for the 2 2 + and 3 ( 2 ) - states in the nucleus. Methods: The Doppler-shift attenuation method was implemented using the TRIUMF-ISAC γ -ray escape-suppressed spectrometer (TIGRESS) γ -ray spectrometer and the TIGRESS integrated plunger device. High-statistics Monte Carlo simulations were utilized to extract lifetimes in accordance with state-of-the-art methodologies. Results: Lifetimes of τ ( 2 1 + ) = 336 ± 4 (stat.) ± 20 (sys.) fs, τ ( 2 2 + ) = 263 ± 9 (stat.) ± 19 (sys.) fs, and τ ( 3 ( 2 ) - ) = 73 ± 6 (stat.) ± 32 (sys.) fs were extracted. This yields a transition strength for the first-excited state of B ( E 2 ; 2 1 + → 0 1 + ) = 259 ± 3 (stat.) ± 16 (sys.) e 2 fm 4 . Conclusions: Finally, the measured lifetime disagrees with the previous Doppler-shift attenuation method measurement by more than 3 σ , while agreeing well with a previous value extracted from Coulomb excitation. The newly extracted B ( E 2 ; 2 1 + → 0 1 + ) value indicates a more significant reduction in the N = 50 isotones approaching Z = 40 .« less

Lifetimes of low-lying excited states in Kr 50 36 86

DOE PAGES

Henderson, J.; Chester, A.; Ball, G. C.; ...

2018-04-16

b>Bmore » The evolution of nuclear magic numbers at extremes of isospin is a topic at the forefront of contemporary nuclear physics. N = 50 is a prime example, with increasing experimental data coming to light on potentially doubly magic Sn 100 and Ni 78 at the proton-rich and proton-deficient extremes, respectively; however, experimental discrepancies exist in the data for less exotic systems. Purpose: In Kr 86 the B ( E 2 ; 2 1 + → 0 1 + ) value—a key indicator of shell evolution—has been experimentally determined by two different methodologies, with the results deviating by 3 σ . Here, we report on a new high-precision measurement of this value, as well as the first measured lifetimes and hence transition strengths for the 2 2 + and 3 ( 2 ) - states in the nucleus. Methods: The Doppler-shift attenuation method was implemented using the TRIUMF-ISAC γ -ray escape-suppressed spectrometer (TIGRESS) γ -ray spectrometer and the TIGRESS integrated plunger device. High-statistics Monte Carlo simulations were utilized to extract lifetimes in accordance with state-of-the-art methodologies. Results: Lifetimes of τ ( 2 1 + ) = 336 ± 4 (stat.) ± 20 (sys.) fs, τ ( 2 2 + ) = 263 ± 9 (stat.) ± 19 (sys.) fs, and τ ( 3 ( 2 ) - ) = 73 ± 6 (stat.) ± 32 (sys.) fs were extracted. This yields a transition strength for the first-excited state of B ( E 2 ; 2 1 + → 0 1 + ) = 259 ± 3 (stat.) ± 16 (sys.) e 2 fm 4 . Conclusions: Finally, the measured lifetime disagrees with the previous Doppler-shift attenuation method measurement by more than 3 σ , while agreeing well with a previous value extracted from Coulomb excitation. The newly extracted B ( E 2 ; 2 1 + → 0 1 + ) value indicates a more significant reduction in the N = 50 isotones approaching Z = 40 .« less

Lifetimes of low-lying excited states in 50 36 86Kr

NASA Astrophysics Data System (ADS)

Henderson, J.; Chester, A.; Ball, G. C.; Caballero-Folch, R.; Domingo, T.; Drake, T. E.; Evitts, L. J.; Garnsworthy, A. B.; Hackman, G.; Hallam, S.; Moukaddam, M.; Ruotsalainen, P.; Smallcombe, J.; Smith, J. K.; Starosta, K.; Svensson, C. E.; Williams, J.

2018-04-01

Background: The evolution of nuclear magic numbers at extremes of isospin is a topic at the forefront of contemporary nuclear physics. N =50 is a prime example, with increasing experimental data coming to light on potentially doubly magic 100Sn and 78Ni at the proton-rich and proton-deficient extremes, respectively; however, experimental discrepancies exist in the data for less exotic systems. Purpose: In 86Kr the B (E 2 ;21+→01+) value—a key indicator of shell evolution—has been experimentally determined by two different methodologies, with the results deviating by 3 σ . Here, we report on a new high-precision measurement of this value, as well as the first measured lifetimes and hence transition strengths for the 22+ and 3(2) - states in the nucleus. Methods: The Doppler-shift attenuation method was implemented using the TRIUMF-ISAC γ -ray escape-suppressed spectrometer (TIGRESS) γ -ray spectrometer and the TIGRESS integrated plunger device. High-statistics Monte Carlo simulations were utilized to extract lifetimes in accordance with state-of-the-art methodologies. Results: Lifetimes of τ (21+)=336 ±4 (stat.)±20 (sys.) fs, τ (22+)=263 ±9 (stat.)±19 (sys.) fs, and τ (3(2) -)=73 ±6 (stat.)±32 (sys.) fs were extracted. This yields a transition strength for the first-excited state of B (E 2 ;21+→01+)=259 ±3 (stat.)±16 (sys.) e2 fm4. Conclusions: The measured lifetime disagrees with the previous Doppler-shift attenuation method measurement by more than 3 σ , while agreeing well with a previous value extracted from Coulomb excitation. The newly extracted B (E 2 ;21+→01+) value indicates a more significant reduction in the N =50 isotones approaching Z =40 .

Cluster structure and Coulomb shift in two-center mirror systems

NASA Astrophysics Data System (ADS)

Nakao, M.; Umehara, H.; Sonoda, S.; Ebata, S.; Ito, M.

2017-11-01

The α + 14C elastic scattering and the nuclear structure of its compound systems, 18O = α + 14C, are analyzed on the basis of the semi-microscopic model. The α + 14C interaction potential is constructed from the double folding (DF) model with the effective nucleon-nucleon interaction of the density-dependent Michigan 3-range Yukawa. The DF potential is applied to the α+14C elastic scattering in the energy range of Eα/Aα = 5.5 8.8 MeV, and the observed differential cross sections are reasonably reproduced. The energy spectra of 18O are calculated by employing the orthogonality condition model (OCM) plus the absorbing boundary condition (ABC). The OCM + ABC calculation predicts the formation of the 0+ resonance around E = 3MeV with respect to the α threshold, which seems to correspond to the resonance identified in the recent experiment. We also apply the OCM + ABC calculation to the mirror system, such as 18Ne = α+14O, and the Coulomb shift of 18O - 18Ne is evaluated. We have found that the Coulomb shift is clearly reduced in the excited 0+ state due to the development of the α cluster structure. This result strongly supports that the Coulomb shift is a candidate of new probe to identify the clustering phenomena.

Coulomb crystals in neutron star crust

NASA Astrophysics Data System (ADS)

Baiko, D. A.

2014-03-01

It is well known that neutron star crust in a wide range of mass densities and temperatures is in a crystal state. At a given density, the crystal is made of fully ionized atomic nuclei of a single species immersed in a nearly incompressible (i.e., constant and uniform) charge compensating background of electrons. This model is known as the Coulomb crystal model. In this talk we analyze thermodynamic and elastic properties of the Coulomb crystals and discuss various deviations from the ideal model. In particular, we study the Coulomb crystal behavior in the presence of a strong magnetic field, consider the effect of the electron gas polarizability, outline the main properties of binary Coulomb crystals, and touch the subject of quasi-free neutrons permeating the Coulomb crystal of ions in deeper layers of neutron star crust.

Coulomb gap triptych in a periodic array of metal nanocrystals.

PubMed

Chen, Tianran; Skinner, Brian; Shklovskii, B I

2012-09-21

The Coulomb gap in the single-particle density of states (DOS) is a universal consequence of electron-electron interaction in disordered systems with localized electron states. Here we show that in arrays of monodisperse metallic nanocrystals, there is not one but three identical adjacent Coulomb gaps, which together form a structure that we call a "Coulomb gap triptych." We calculate the DOS and the conductivity in two- and three-dimensional arrays using a computer simulation. Unlike in the conventional Coulomb glass models, in nanocrystal arrays the DOS has a fixed width in the limit of large disorder. The Coulomb gap triptych can be studied via tunneling experiments.

Transition-density-fragment interaction combined with transfer integral approach for excitation-energy transfer via charge-transfer states

NASA Astrophysics Data System (ADS)

Fujimoto, Kazuhiro J.

2012-07-01

A transition-density-fragment interaction (TDFI) combined with a transfer integral (TI) method is proposed. The TDFI method was previously developed for describing electronic Coulomb interaction, which was applied to excitation-energy transfer (EET) [K. J. Fujimoto and S. Hayashi, J. Am. Chem. Soc. 131, 14152 (2009)] and exciton-coupled circular dichroism spectra [K. J. Fujimoto, J. Chem. Phys. 133, 124101 (2010)]. In the present study, the TDFI method is extended to the exchange interaction, and hence it is combined with the TI method for applying to the EET via charge-transfer (CT) states. In this scheme, the overlap correction is also taken into account. To check the TDFI-TI accuracy, several test calculations are performed to an ethylene dimer. As a result, the TDFI-TI method gives a much improved description of the electronic coupling, compared with the previous TDFI method. Based on the successful description of the electronic coupling, the decomposition analysis is also performed with the TDFI-TI method. The present analysis clearly shows a large contribution from the Coulomb interaction in most of the cases, and a significant influence of the CT states at the small separation. In addition, the exchange interaction is found to be small in this system. The present approach is useful for analyzing and understanding the mechanism of EET.

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

NASA Astrophysics Data System (ADS)

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

2017-04-01

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

Evaluating excited state atomic polarizabilities of chromophores.

PubMed

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

2018-03-28

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

Production of low kinetic energy electrons and energetic ion pairs by Intermolecular Coulombic Decay.

PubMed

Hergenhahn, Uwe

2012-12-01

The paper gives an introduction into Interatomic and Intermolecular Coulombic Decay (ICD). ICD is an autoionization process, which contrary to Auger decay involves neighbouring sites of the initial vacancy as an integral part of the decay transition. As a result of ICD, slow electrons are produced which generally are known to be active in radiation damage. The author summarizes the properties of ICD and reviews a number of important experiments performed in recent years. Intermolecular Coulombic Decay can generally take place in weakly bonded aggregates in the presence of ionizing particles or ionizing radiation. Examples collected here mostly use soft X-rays produced by synchrotron radiation to ionize, and use rare-gas clusters, water clusters or solutes in a liquid jet to observe ICD after irradiation. Intermolecular Coulombic Decay is initiated by single ionization into an excited state. The subsequent relaxation proceeds via an ultra-fast energy transfer to a neighbouring site, where a second ionization occurs. Secondary electrons from ICD have clearly been identified in numerous systems. ICD can take place after primary ionization, as the second step of a decay cascade which also involves Auger decay, or after resonant excitation with an energy which exceeds the ionization potential of the system. ICD is expected to play a role whenever particles or radiation with photon energies above the ionization energies for inner valence electrons are present in weakly bonded matter, e.g., biological tissue. The process produces at the same time a slow electron and two charged atomic or molecular fragments, which will lead to structural changes around the ionized site.

Multimode optical fibers: steady state mode exciter.

PubMed

Ikeda, M; Sugimura, A; Ikegami, T

1976-09-01

The steady state mode power distribution of the multimode graded index fiber was measured. A simple and effective steady state mode exciter was fabricated by an etching technique. Its insertion loss was 0.5 dB for an injection laser. Deviation in transmission characteristics of multimode graded index fibers can be avoided by using the steady state mode exciter.

Excited states of protonated DNA/RNA bases.

PubMed

Berdakin, Matias; Féraud, Géraldine; Dedonder-Lardeux, Claude; Jouvet, Christophe; Pino, Gustavo A

2014-06-14

The very fast relaxation of the excited states to the ground state in DNA/RNA bases is a necessary process to ensure the photostability of DNA and its rate is highly sensitive to the tautomeric form of the bases. Protonation of the bases plays a crucial role in many biochemical and mutagenic processes and it can result in alternative tautomeric structures, thus making important the knowledge of the properties of protonated DNA/RNA bases. We report here the photofragmentation spectra of the five protonated DNA/RNA bases. In most of the cases, the spectra exhibit well resolved vibrational structures, with broad bands associated with very short excited state lifetimes. The similarity between the electronic properties, e.g. excitation energy and very short excited state lifetimes for the canonical tautomers of protonated and neutral DNA bases, suggests that the former could also play an important role in the photostability mechanism of DNA.

Excitation energies from particle-particle random phase approximation with accurate optimized effective potentials

NASA Astrophysics Data System (ADS)

Jin, Ye; Yang, Yang; Zhang, Du; Peng, Degao; Yang, Weitao

2017-10-01

The optimized effective potential (OEP) that gives accurate Kohn-Sham (KS) orbitals and orbital energies can be obtained from a given reference electron density. These OEP-KS orbitals and orbital energies are used here for calculating electronic excited states with the particle-particle random phase approximation (pp-RPA). Our calculations allow the examination of pp-RPA excitation energies with the exact KS density functional theory (DFT). Various input densities are investigated. Specifically, the excitation energies using the OEP with the electron densities from the coupled-cluster singles and doubles method display the lowest mean absolute error from the reference data for the low-lying excited states. This study probes into the theoretical limit of the pp-RPA excitation energies with the exact KS-DFT orbitals and orbital energies. We believe that higher-order correlation contributions beyond the pp-RPA bare Coulomb kernel are needed in order to achieve even higher accuracy in excitation energy calculations.

Measurement of the Spectroscopic Quadrupole Moment for the 2+1 State in 10Be:. Testing AB Initio Calculations

NASA Astrophysics Data System (ADS)

Orce, J. N.; Djongolov, M.; Navratil, P.; Ball, G.; Garnsworthy, A. B.; Hackman, G.; Lassen, J.; Meissner, J.; Pearson, C. J.; Li, R.; Milovanovic, L.; Sjue, S. K. L.; Teigelhoefer, A.; Triambak, S.; Williams, S. J.; Falou, H. Al; Drake, T. E.; Andreoiu, C.; Cross, D.; Kshetri, R.; Finlay, P.; Garrett, P. E.; Leach, K. G.; Rand, E. T.; Sumithrarachchi, C. S.; Svensson, C. E.; Tardiff, E. R.; Wong, J.; Forssen, C.; Hayes, A. B.; Sarazin, F.; Stoyer, M. A.; Wu, C. Y.

2013-03-01

The highly efficient and segmented TIGRESS HPGe γ-ray array at TRIUMF has been used to perform a reorientation effect Coulomb excitation study of the 2+1 state at 3.368 MeV in 10Be. This is the first Coulomb excitation measurement that provides information on diagonal matrix elements for such a high lying first excited state from μ-ray data. With the availability of accurate lifetime data, a restriction on the diagonal < 2+1|M({E}2)|2+1> matrix element is determined. This result is compared to a no core shell model calculation with the CD-Bonn 2000 two nucleon potential.

Relativistic Coulomb Problem for Z Larger than 137

NASA Astrophysics Data System (ADS)

Alhaidari, A. D.

We propose a relativistic one-parameter Hermitian theory for the Coulomb problem with an electric charge greater than 137. In the nonrelativistic limit, the theory becomes identical to the Schrödinger-Coulomb problem for all Z. Moreover, it agrees with the Dirac-Coulomb problem to order (αZ)2, where α is the fine structure constant. The vacuum in the theory is stable and does not suffer from the "charged vacuum" problem for all Z. Moreover, transition between positive and negative energy states could be eliminated. The relativistic bound states energy spectrum and corresponding spinor wave functions are obtained.

Low-lying excited states by constrained DFT

NASA Astrophysics Data System (ADS)

Ramos, Pablo; Pavanello, Michele

2018-04-01

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

Low-lying excited states by constrained DFT.

PubMed

Ramos, Pablo; Pavanello, Michele

2018-04-14

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

Vibronic coupling in the excited-states of carotenoids

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

Miki, Takeshi; Buckup, Tiago; Krause, Marie S.

2016-01-01

The ultrafast femtochemistry of carotenoids is governed by the interaction between electronic excited states, which has been explained by the relaxation dynamics within a few hundred femtoseconds from the lowest optically allowed excited state S 2to the optically dark state S 1.

Vibronic coupling in the excited-states of carotenoids

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

Miki, Takeshi; Buckup, Tiago; Krause, Marie S.

The ultrafast femtochemistry of carotenoids is governed by the interaction between electronic excited states, which has been explained by the relaxation dynamics within a few hundred femtoseconds from the lowest optically allowed excited state S 2to the optically dark state S 1.

Excited State Properties of Hybrid Perovskites.

PubMed

Saba, Michele; Quochi, Francesco; Mura, Andrea; Bongiovanni, Giovanni

2016-01-19

Metal halide perovskites have come to the attention of the scientific community for the progress achieved in solar light conversion. Energy sustainability is one of the priorities of our society, and materials advancements resulting in low-cost but efficient solar cells and large-area lighting devices represent a major goal for applied research. From a basic point of view, perovskites are an exotic class of hybrid materials combining some merits of organic and inorganic semiconductors: large optical absorption, large mobilities, and tunable band gap together with the possibility to be processed in solution. When a novel class of promising semiconductors comes into the limelight, lively discussions ensue on the photophysics of band-edge excitations, because just the states close to the band edge are entailed in energy/charge transport and light emission. This was the case several decades ago for III-V semiconductors, it has been up to 10 years ago for organics, and it is currently the case for perovskites. Our aim in this Account is to rationalize the body of experimental evidence on perovskite photophysics in a coherent theoretical framework, borrowing from the knowledge acquired over the years in materials optoelectronics. A crucial question is whether photon absorption leads to a population of unbound, conductive free charges or instead excitons, neutral and insulating bound states created by Coulomb interaction just below the energy of the band gap. We first focus on the experimental estimates of the exciton binding energy (Eb): at room temperature, Eb is comparable to the thermal energy kBT in MAPbI3 and increases up to values 2-3kBT in wide band gap MAPbBr3 and MAPbCl3. Statistical considerations predict that these values, even though comparable to or larger than thermal energy, let free carriers prevail over bound excitons for all levels of excitation densities relevant for devices. The analysis of photophysics evidence confirms that all hybrid halide

Time-resolved photoelectron spectroscopy of a dinuclear Pt(II) complex: Tunneling autodetachment from both singlet and triplet excited states of a molecular dianion

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

Winghart, Marc-Oliver, E-mail: marc-oliver.winghart@kit.edu; Unterreiner, Andreas-Neil; Yang, Ji-Ping

2016-02-07

Time-resolved pump-probe photoelectron spectroscopy has been used to study the relaxation dynamics of gaseous [Pt{sub 2}(μ-P{sub 2}O{sub 5}H{sub 2}){sub 4} + 2H]{sup 2−} after population of its first singlet excited state by 388 nm femtosecond laser irradiation. In contrast to the fluorescence and phosphorescence observed in condensed phase, a significant fraction of the photoexcited isolated dianions decays by electron loss to form the corresponding monoanions. Our transient photoelectron data reveal an ultrafast decay of the initially excited singlet {sup 1}A{sub 2u} state and concomitant rise in population of the triplet {sup 3}A{sub 2u} state, via sub-picosecond intersystem crossing (ISC). Wemore » find that both of the electronically excited states are metastably bound behind a repulsive Coulomb barrier and can decay via delayed autodetachment to yield electrons with characteristic kinetic energies. While excited state tunneling detachment (ESETD) from the singlet {sup 1}A{sub 2u} state takes only a few picoseconds, ESETD from the triplet {sup 3}A{sub 2u} state is much slower and proceeds on a time scale of hundreds of nanoseconds. The ISC rate in the gas phase is significantly higher than in solution, which can be rationalized in terms of changes to the energy dissipation mechanism in the absence of solvent molecules. [Pt{sub 2}(μ-P{sub 2}O{sub 5}H{sub 2}){sub 4} + 2H]{sup 2−} is the first example of a photoexcited multianion for which ESETD has been observed following ISC.« less

DNA bubble dynamics as a quantum Coulomb problem.

PubMed

Fogedby, Hans C; Metzler, Ralf

2007-02-16

We study the dynamics of denaturation bubbles in double-stranded DNA. Demonstrating that the associated Fokker-Planck equation is equivalent to a Coulomb problem, we derive expressions for the bubble survival distribution W(t). Below Tm, W(t) is associated with the continuum of scattering states of the repulsive Coulomb potential. At Tm, the Coulomb potential vanishes and W(t) assumes a power-law tail with nontrivial dynamic exponents: the critical exponent of the entropy loss factor may cause a finite mean lifetime. Above Tm (attractive potential), the long-time dynamics is controlled by the lowest bound state. Correlations and finite size effects are discussed.

Higgs transition from a magnetic Coulomb liquid to a ferromagnet in Yb2Ti2O7

PubMed Central

Chang, Lieh-Jeng; Onoda, Shigeki; Su, Yixi; Kao, Ying-Jer; Tsuei, Ku-Ding; Yasui, Yukio; Kakurai, Kazuhisa; Lees, Martin Richard

2012-01-01

In a class of frustrated magnets known as spin ice, magnetic monopoles emerge as classical defects and interact via the magnetic Coulomb law. With quantum-mechanical interactions, these magnetic charges are carried by fractionalized bosonic quasi-particles, spinons, which can undergo Bose–Einstein condensation through a first-order transition via the Higgs mechanism. Here, we report evidence of a Higgs transition from a magnetic Coulomb liquid to a ferromagnet in single-crystal Yb2Ti2O7. Polarized neutron scattering experiments show that the diffuse [111]-rod scattering and pinch-point features, which develop on cooling are suddenly suppressed below TC~0.21 K, where magnetic Bragg peaks and a full depolarization of the neutron spins are observed with thermal hysteresis, indicating a first-order ferromagnetic transition. Our results are explained on the basis of a quantum spin-ice model, whose high-temperature phase is effectively described as a magnetic Coulomb liquid, whereas the ground state shows a nearly collinear ferromagnetism with gapped spin excitations. PMID:22871811

Three-photon Gaussian-Gaussian-Laguerre-Gaussian excitation of a localized atom to a highly excited Rydberg state

NASA Astrophysics Data System (ADS)

Mashhadi, L.

2017-12-01

Optical vortices are currently one of the most intensively studied topics in light-matter interaction. In this work, a three-step axial Doppler- and recoil-free Gaussian-Gaussian-Laguerre-Gaussian (GGLG) excitation of a localized atom to the highly excited Rydberg state is presented. By assuming a large detuning for intermediate states, an effective quadrupole excitation related to the Laguerre-Gaussian (LG) excitation to the highly excited Rydberg state is obtained. This special excitation system radially confines the single highly excited Rydberg atom independently of the trapping system into a sharp potential landscape into the so-called ‘far-off-resonance optical dipole-quadrupole trap’ (FORDQT). The key parameters of the Rydberg excitation to the highly excited state, namely the effective Rabi frequency and the effective detuning including a position-dependent AC Stark shift, are calculated in terms of the basic parameters of the LG beam and of the polarization of the excitation lasers. It is shown that the obtained parameters can be tuned to have a precise excitation of a single atom to the desired Rydberg state as well. The features of transferring the optical orbital and spin angular momentum of the polarized LG beam to the atom via quadrupole Rydberg excitation offer a long-lived and controllable qudit quantum memory. In addition, in contrast to the Gaussian laser beam, the doughnut-shaped LG beam makes it possible to use a high intensity laser beam to increase the signal-to-noise ratio in quadrupole excitation with minimized perturbations coming from stray light broadening in the last Rydberg excitation process.

The triplet excited state of Bodipy: formation, modulation and application.

PubMed

Zhao, Jianzhang; Xu, Kejing; Yang, Wenbo; Wang, Zhijia; Zhong, Fangfang

2015-12-21

Boron dipyrromethene (Bodipy) is one of the most extensively investigated organic chromophores. Most of the investigations are focused on the singlet excited state of Bodipy, such as fluorescence. In stark contrast, the study of the triplet excited state of Bodipy is limited, but it is an emerging area, since the triplet state of Bodipy is tremendously important for several areas, such as the fundamental photochemistry study, photodynamic therapy (PDT), photocatalysis and triplet-triplet annihilation (TTA) upconversion. The recent developments in the study of the production, modulation and application of the triplet excited state of Bodipy are discussed in this review article. The formation of the triplet state of Bodipy upon photoexcitation, via the well known approach such as the heavy atom effect (including I, Br, Ru, Ir, etc.), and the new methods, such as using a spin converter (e.g. C60), charge recombination, exciton coupling and the doubly substituted excited state, are summarized. All the Bodipy-based triplet photosensitizers show strong absorption of visible or near IR light and the long-lived triplet excited state, which are important for the application of the triplet excited state in PDT or photocatalysis. Moreover, the methods for switching (or modulation) of the triplet excited state of Bodipy were discussed, such as those based on the photo-induced electron transfer (PET), by controlling the competing Förster-resonance-energy-transfer (FRET), or the intermolecular charge transfer (ICT). Controlling the triplet excited state will give functional molecules such as activatable PDT reagents or molecular devices. It is worth noting that switching of the singlet excited state and the triplet state of Bodipy may follow different principles. Application of the triplet excited state of Bodipy in PDT, hydrogen (H2) production, photoredox catalytic organic reactions and TTA upconversion were discussed. The challenges and the opportunities in these areas were

Excitation of lowest electronic states of thymine by slow electrons

NASA Astrophysics Data System (ADS)

Chernyshova, I. V.; Kontros, E. J.; Markush, P. P.; Shpenik, O. B.

2013-11-01

Excitation of lowest electronic states of the thymine molecules in the gas phase is studied by elec- tron energy loss spectroscopy. In addition to dipole-allowed transitions to singlet states, transitions to the lowest triplet states were observed. The low-energy features of the spectrum at 3.66 and 4.61 eV are identified with the excitation of the first triplet states 13 A' (π → π*) and 13 A″ ( n → π*). The higher-lying features at 4.96, 5.75, 6.17, and 7.35 eV are assigned mainly to the excitation of the π → π* transitions to the singlet states of the molecule. The excitation dynamics of the lowest states is studied. It is found that the first triplet state 13 A'(π → π*) is most efficiently excited at a residual energy close to zero, while the singlet 21 A'(π → π*) state is excited with almost identical efficiency at different residual energies.

Singlet-triplet splittings from the virial theorem and single-particle excitation energies

NASA Astrophysics Data System (ADS)

Becke, Axel D.

2018-01-01

The zeroth-order (uncorrelated) singlet-triplet energy difference in single-particle excited configurations is 2Kif, where Kif is the Coulomb self-energy of the product of the transition orbitals. Here we present a non-empirical, virial-theorem argument that the correlated singlet-triplet energy difference should be half of this, namely, Kif. This incredibly simple result gives vertical HOMO-LUMO excitation energies in small-molecule benchmarks as good as the popular TD-B3LYP time-dependent approach to excited states. For linear acenes and nonlinear polycyclic aromatic hydrocarbons, the performance is significantly better than TD-B3LYP. In addition to the virial theorem, the derivation borrows intuitive pair-density concepts from density-functional theory.

Coulomb Mediated Hybridization of Excitons in Coupled Quantum Dots.

PubMed

Ardelt, P-L; Gawarecki, K; Müller, K; Waeber, A M; Bechtold, A; Oberhofer, K; Daniels, J M; Klotz, F; Bichler, M; Kuhn, T; Krenner, H J; Machnikowski, P; Finley, J J

2016-02-19

We report Coulomb mediated hybridization of excitonic states in optically active InGaAs quantum dot molecules. By probing the optical response of an individual quantum dot molecule as a function of the static electric field applied along the molecular axis, we observe unexpected avoided level crossings that do not arise from the dominant single-particle tunnel coupling. We identify a new few-particle coupling mechanism stemming from Coulomb interactions between different neutral exciton states. Such Coulomb resonances hybridize the exciton wave function over four different electron and hole single-particle orbitals. Comparisons of experimental observations with microscopic eight-band k·p calculations taking into account a realistic quantum dot geometry show good agreement and reveal that the Coulomb resonances arise from broken symmetry in the artificial semiconductor molecule.

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

PubMed

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

2017-08-08

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

Extensive degeneracy, Coulomb phase and magnetic monopoles in artificial square ice.

PubMed

Perrin, Yann; Canals, Benjamin; Rougemaille, Nicolas

2016-12-15

Artificial spin-ice systems are lithographically patterned arrangements of interacting magnetic nanostructures that were introduced as way of investigating the effects of geometric frustration in a controlled manner. This approach has enabled unconventional states of matter to be visualized directly in real space, and has triggered research at the frontier between nanomagnetism, statistical thermodynamics and condensed matter physics. Despite efforts to create an artificial realization of the square-ice model-a two-dimensional geometrically frustrated spin-ice system defined on a square lattice-no simple geometry based on arrays of nanomagnets has successfully captured the macroscopically degenerate ground-state manifold of the model. Instead, square lattices of nanomagnets are characterized by a magnetically ordered ground state that consists of local loop configurations with alternating chirality. Here we show that all of the characteristics of the square-ice model are observed in an artificial square-ice system that consists of two sublattices of nanomagnets that are vertically separated by a small distance. The spin configurations we image after demagnetizing our arrays reveal unambiguous signatures of a Coulomb phase and algebraic spin-spin correlations, which are characterized by the presence of 'pinch' points in the associated magnetic structure factor. Local excitations-the classical analogues of magnetic monopoles-are free to evolve in an extensively degenerate, divergence-free vacuum. We thus provide a protocol that could be used to investigate collective magnetic phenomena, including Coulomb phases and the physics of ice-like materials.

An Ab Initio Exciton Model Including Charge-Transfer Excited States

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

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

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

An Ab Initio Exciton Model Including Charge-Transfer Excited States

DOE PAGES

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

2017-06-15

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

Ultrafast excited-state dynamics of 2,5-dimethylpyrrole.

PubMed

Yang, Dongyuan; Min, Yanjun; Chen, Zhichao; He, Zhigang; Yuan, Kaijun; Dai, Dongxu; Yang, Xueming; Wu, Guorong

2018-04-17

The ultrafast excited-state dynamics of 2,5-dimethylpyrrole following excitation at wavelengths in the range of 265.7-216.7 nm is studied using the time-resolved photoelectron imaging method. It is found that excitation at longer wavelengths (265.7-250.2 nm) results in the population of the S1(1πσ*) state, which decays out of the photoionization window in about 90 fs. At shorter pump wavelengths (242.1-216.7 nm), the assignments are less clear-cut. We tentatively assign the initially photoexcited state(s) to the 1π3p Rydberg state(s) which has lifetimes of 159 ± 20, 125 ± 15, 102 ± 10 and 88 ± 10 fs for the pump wavelengths of 242.1, 238.1, 232.6 and 216.7 nm, respectively. Internal conversion to the S1(1πσ*) state represents at most a minor decay channel. The methyl substitution effects on the decay dynamics of the excited states of pyrrole are also discussed. Methyl substitution on the pyrrole ring seems to enhance the direct internal conversion from the 1π3p Rydberg state to the ground state, while methyl substitution on the N atom has less influence and the internal conversion to the S1(πσ*) state represents a main channel.

Shell- and subshell-resolved projectile excitation of hydrogenlike Au{sup 78+} ions in relativistic ion-atom collisions

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

Gumberidze, A.; Frankfurt Institute for Advanced Studies FIAS, D-60438 Frankfurt am Main; Fritzsche, S.

2010-11-15

The projectile excitation of high-Z ions has been investigated in relativistic ion-atoms collisions by observing the subsequent x-ray emission. The x-ray spectra from the projectile excitation have been separated from the x-ray emission following electron capture into the excited states using a novel anticoincidence technique. For the particular case of hydrogenlike Au{sup 78+} ions colliding with Ar atoms, Coulomb excitation from the ground state into the fine-structure-resolved n=2 levels as well as into levels with principal quantum number n{>=}3 has been measured with excellent statistics. The observed spectra agree well with simulated spectra that are based on Dirac's relativistic equationmore » and the proper inclusion of the magnetic interaction into the amplitudes for projectile excitation. It is shown that a coherent inclusion of the magnetic part of the Lienard-Wiechert potential leads to the lowering of the excitation cross section by up to 35%. This effect is more pronounced for excitation into states with high angular momentum and is confirmed by our experimental data.« less

Coulomb couplings in solubilised light harvesting complex II (LHCII): challenging the ideal dipole approximation from TDDFT calculations.

PubMed

López-Tarifa, P; Liguori, Nicoletta; van den Heuvel, Naudin; Croce, Roberta; Visscher, Lucas

2017-07-19

The light harvesting complex II (LHCII), is a pigment-protein complex responsible for most of the light harvesting in plants. LHCII harvests sunlight and transfers excitation energy to the reaction centre of the photo-system, where the water oxidation process takes place. The energetics of LHCII can be modulated by means of conformational changes allowing a switch from a harvesting to a quenched state. In this state, the excitation energy is no longer transferred but converted into thermal energy to prevent photooxidation. Based on molecular dynamics simulations at the microsecond time scale, we have recently proposed that the switch between different fluorescent states can be probed by correlating shifts in the chromophore-chromophore Coulomb interactions to particular protein movements. However, these findings are based upon calculations in the ideal point dipole approximation (IDA) where the Coulomb couplings are simplified as first order dipole-dipole interactions, also assuming that the chromophore transition dipole moments lay in particular directions of space with constant moduli (FIX-IDA). In this work, we challenge this approximation using the time-dependent density functional theory (TDDFT) combined with the frozen density embedding (FDE) approach. Our aim is to establish up to which limit FIX-IDA can be applied and which chromophore types are better described under this approximation. For that purpose, we use the classical trajectories of solubilised light harvesting complex II (LHCII) we have recently reported [Liguori et al., Sci. Rep., 2015, 5, 15661] and selected three pairs of chromophores containing chlorophyll and carotenoids (Chl and Car): Chla611-Chla612, Chlb606-Chlb607 and Chla612-Lut620. Using the FDE in the Tamm-Dancoff approximation (FDEc-TDA), we show that IDA is accurate enough for predicting Chl-Chl Coulomb couplings. However, the FIX-IDA largely overestimates Chl-Car interactions mainly because the transition dipole for the Cars is not

Excited state correlations of the finite Heisenberg chain

NASA Astrophysics Data System (ADS)

Pozsgay, Balázs

2017-02-01

We consider short range correlations in excited states of the finite XXZ and XXX Heisenberg spin chains. We conjecture that the known results for the factorized ground state correlations can be applied to the excited states too, if the so-called physical part of the construction is changed appropriately. For the ground state we derive simple algebraic expressions for the physical part; the formulas only use the ground state Bethe roots as an input. We conjecture that the same formulas can be applied to the excited states as well, if the exact Bethe roots of the excited states are used instead. In the XXZ chain the results are expected to be valid for all states (except certain singular cases where regularization is needed), whereas in the XXX case they only apply to singlet states or group invariant operators. Our conjectures are tested against numerical data from exact diagonalization and coordinate Bethe Ansatz calculations, and perfect agreement is found in all cases. In the XXX case we also derive a new result for the nearest-neighbour correlator < σ 1zσ 2z> , which is valid for non-singlet states as well. Our results build a bridge between the known theory of factorized correlations, and the recently conjectured TBA-like description for the building blocks of the construction.

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.

Computing correct truncated excited state wavefunctions

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Excited States of the divacancy in SiC

NASA Astrophysics Data System (ADS)

Bockstedte, Michel; Garratt, Thomas; Ivady, Viktor; Gali, Adam

2014-03-01

The divacancy in SiC - a technologically mature material that fulfills the necessary requirements for hosting defect based quantum computing - is a good candidate for implementing a solid state quantum bit. Its ground state is isovalent to the NV center in diamond as demonstrated by density functional theory (DFT). Furthermore, coherent manipulation of divacancy spins in SiC has been demonstrated. The similarities to NV might indicate that the same inter system crossing (ICS) from the high to the low spin state is responsible for its spin-dependent fluorescent signal. By DFT and a DFT-based multi-reference hamiltonian we analyze the excited state spectrum of the defects. In contrast to the current picture of the spin dynamics of the NV center, we predict that a static Jahn-Teller effect in the first excited triplet states governs an ICS both with the excited and ground state of the divacancy.

Excited-state dynamics of pentacene derivatives with stable radical substituents.

PubMed

Ito, Akitaka; Shimizu, Akihiro; Kishida, Noriaki; Kawanaka, Yusuke; Kosumi, Daisuke; Hashimoto, Hideki; Teki, Yoshio

2014-06-23

The excited-state dynamics of pentacene derivatives with stable radical substituents were evaluated in detail through transient absorption measurements. The derivatives showed ultrafast formation of triplet excited state(s) in the pentacene moiety from a photoexcited singlet state through the contributions of enhanced intersystem crossing and singlet fission. Detailed kinetic analyses for the transient absorption data were conducted to quantify the excited-state characteristics of the derivatives. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Electron-Impact Excitation of Ions Effects of Presence of Another Ion

NASA Astrophysics Data System (ADS)

Ohsaki, Akihiko; Nagasaki, Satoshi; Uramoto, Sei-iti; Takayanagi, Kazuo

2000-02-01

Present work gives for the first time the formulation of the two-center Coulomb-Born approximation (TCCBA) and presents some calculations for the electron-impact excitations in electron-ion-ion systems.The effect of the third body was relatively small in the cases studied so far. However, if the third body is a bare ion with a charge larger than the target ion, there will be a marked influence of the three-body collisions.Utilizing TCCBA we present the total and partial cross sections of hydrogen-like ions He+(Z=2), and C5+(Z=6) in the hydrogen plasma from the ground states 1s to the excited states 2s and 2p0, 2p± for the collision energies from 0.4Z2 to 2Z2 a.u.; for the excited states of the target ions, Stark effect is also studied.It is found that the presence of another ion have little effect on the 1s-2s transition and the 2s-2p Stark mixing has a prominent effect.

The low-lying electronic excitations in long polyenes: A PPP-MRD-CI study

NASA Astrophysics Data System (ADS)

Tavan, Paul; Schulten, Klaus

1986-12-01

A correct description of the electronic excitations in polyenes demands that electron correlation is accounted for correctly. Very large expansions are necessary including many-electron configurations with at least one, two, three, and four electrons promoted from the Hartree-Fock ground state. The enormous size of such expansions had prohibited accurate computations of the spectra for polyenes with more than ten π electrons. We present a multireference double excitation configuration interaction method (MRD-CI) which allows such computations for polyenes with up to 16 π electrons. We employ a Pariser-Parr-Pople (PPP) model Hamiltonian. For short polyenes with up to ten π electrons our calculations reproduce the excitation energies resulting from full-CI calculations. We extend our calculations to study the low-lying electronic excitations of the longer polyenes, in particular, the gap between the first optically forbidden and the first optically allowed excited singlet state. The size of this gap is shown to depend strongly on the degree of bond alternation and on the dielectric shielding of the Coulomb repulsion between the π electrons.

Role of electronic excited N2 in vibrational excitation of the N2 ground state at high latitudes

NASA Astrophysics Data System (ADS)

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

2006-09-01

Vibrationally excited N2 is important in determining the ionospheric electron density and has also been proposed to play a role in the production of NO in disturbed atmospheres. We report here predictions of the absolute vibrational distributions in the ground electronic state of N2 produced by electron impact excitation, at noon and midnight under quiet geomagnetic conditions and disturbed conditions corresponding to the aurora IBCII+ and IBCIII+ at 60°N latitude and 0° longitude, at altitudes between 130 and 350 km. These predictions were obtained from a model which includes thermal excitation and direct electron impact excitation of the vibrational levels of the N2 ground state and its excited electronic states; radiative cascade from all excited electronic states to all vibrational levels of the ground electronic state; quenching by O, O2, and N2; molecular and ambipolar diffusion; and the dominant chemical reactions. Results from this study show that for both aurora and daytime electron environments: (1) cascade from the higher electronic states of N2 determines the population of the higher vibrational levels in the N2 ground state and (2) the effective ground state vibrational temperature for levels greater than 4 in N2 is predicted to be in the range 4000-13000 K for altitudes greater than 200 km. Correspondingly, the associated enhancement factor for the O+ reaction with vibrationally excited N2 to produce NO+ is predicted to increase with increasing altitude (up to a maximum at a height which increases with auroral strength) for both aurora and daytime environments and to increase with increasing auroral strength. The contribution of the cascade from the excited electronic states was evaluated and found to be relatively minor compared to the direct excitation process.

Charmonium excited state spectrum in lattice QCD

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

Jozef Dudek; Robert Edwards; Nilmani Mathur

2008-02-01

Working with a large basis of covariant derivative-based meson interpolating fields we demonstrate the feasibility of reliably extracting multiple excited states using a variational method. The study is performed on quenched anisotropic lattices with clover quarks at the charm mass. We demonstrate how a knowledge of the continuum limit of a lattice interpolating field can give additional spin-assignment information, even at a single lattice spacing, via the overlap factors of interpolating field and state. Excited state masses are systematically high with respect to quark potential model predictions and, where they exist, experimental states. We conclude that this is most likelymore » a result of the quenched approximation.« less

Excited state properties of the astaxanthin radical cation: A quantum chemical study

NASA Astrophysics Data System (ADS)

Dreuw, Andreas; Starcke, Jan Hendrik; Wachtveitl, Josef

2010-07-01

Using time-dependent density functional theory, the excited electronic states of the astaxanthin radical cation (AXT rad + ) are investigated. While the optically allowed excited D 1 and D 3 states are typical ππ∗ excited states, the D 2 and D 4 states are nπ∗ states. Special emphasis is put onto the influence of the carbonyl groups onto the excited states. For this objective, the excited states of four hypothetical carotenoids and zeaxanthin have been computed. Addition of a carbonyl group to a conjugated carbon double bond system does essentially not change the vertical excitation energies of the optically allowed ππ∗ states due to two counter-acting effects: the excitation energy should increase due to the -M-effect of the carbonyl group and at the same time decrease owing to the elongation of the conjugated double bond system by the carbonyl group itself.

Electron capture and excitation processes in H+-H collisions in dense quantum plasmas

NASA Astrophysics Data System (ADS)

Jakimovski, D.; Markovska, N.; Janev, R. K.

2016-10-01

Electron capture and excitation processes in proton-hydrogen atom collisions taking place in dense quantum plasmas are studied by employing the two-centre atomic orbital close-coupling (TC-AOCC) method. The Debye-Hückel cosine (DHC) potential is used to describe the plasma screening effects on the Coulomb interaction between charged particles. The properties of a hydrogen atom with DHC potential are investigated as a function of the screening strength of the potential. It is found that the decrease in binding energy of nl levels with increasing screening strength is considerably faster than in the case of the Debye-Hückel (DH) screening potential, appropriate for description of charged particle interactions in weakly coupled classical plasmas. This results in a reduction in the number of bound states in the DHC potential with respect to that in the DH potential for the same plasma screening strength, and is reflected in the dynamics of excitation and electron capture processes for the two screened potentials. The TC-AOCC cross sections for total and state-selective electron capture and excitation cross sections with the DHC potential are calculated for a number of representative screening strengths in the 1-300 keV energy range and compared with those for the DH and pure Coulomb potential. The total capture cross sections for a selected number of screening strengths are compared with the available results from classical trajectory Monte Carlo calculations.

Excited states of neutral donor bound excitons in GaN

NASA Astrophysics Data System (ADS)

Callsen, G.; Kure, T.; Wagner, M. R.; Butté, R.; Grandjean, N.

2018-06-01

We investigate the excited states of a neutral donor bound exciton (D0X) in bulk GaN by means of high-resolution, polychromatic photoluminescence excitation (PLE) spectroscopy. The optically most prominent donor in our sample is silicon accompanied by only a minor contribution of oxygen—the key for an unambiguous assignment of excited states. Consequently, we can observe a multitude of Si0X-related excitation channels with linewidths down to 200 μeV. Two groups of excitation channels are identified, belonging either to rotational-vibrational or electronic excited states of the hole in the Si0X complex. Such identification is achieved by modeling the excited states based on the equations of motion for a Kratzer potential, taking into account the particularly large anisotropy of effective hole masses in GaN. Furthermore, several ground- and excited states of the exciton-polaritons and the dominant bound exciton are observed in the photoluminescence (PL) and PLE spectra, facilitating an estimate of the associated complex binding energies. Our data clearly show that great care must be taken if only PL spectra of D0X centers in GaN are analyzed. Every PL feature we observe at higher emission energies with regard to the Si0X ground state corresponds to an excited state. Hence, any unambiguous peak identification renders PLE spectra highly valuable, as important spectral features are obscured in common PL spectra. Here, GaN represents a particular case among the wide-bandgap, wurtzite semiconductors, as comparably low localization energies for common D0X centers are usually paired with large emission linewidths and the prominent optical signature of exciton-polaritons, making the sole analysis of PL spectra a challenging task.

Sub-50 fs excited state dynamics of 6-chloroguanine upon deep ultraviolet excitation.

PubMed

Mondal, Sayan; Puranik, Mrinalini

2016-05-18

The photophysical properties of natural nucleobases and their respective nucleotides are ascribed to the sub-picosecond lifetime of their first singlet states in the UV-B region (260-350 nm). Electronic transitions of the ππ* type, which are stronger than those in the UV-B region, lie at the red edge of the UV-C range (100-260 nm) in all isolated nucleobases. The lowest energetic excited states in the UV-B region of nucleobases have been investigated using a plethora of experimental and theoretical methods in gas and solution phases. The sub-picosecond lifetime of these molecules is not a general attribute of all nucleobases but specific to the five primary nucleobases and a few xanthine and methylated derivatives. To determine the overall UV photostability, we aim to understand the effect of more energetic photons lying in the UV-C region on nucleobases. To determine the UV-C initiated photophysics of a nucleobase system, we chose a halogen substituted purine, 6-chloroguanine (6-ClG), that we had investigated previously using resonance Raman spectroscopy. We have performed quantitative measurements of the resonance Raman cross-section across the Bb absorption band (210-230 nm) and constructed the Raman excitation profiles. We modeled the excitation profiles using Lee and Heller's time-dependent theory of resonance Raman intensities to extract the initial excited state dynamics of 6-ClG within 30-50 fs after photoexcitation. We found that imidazole and pyrimidine rings of 6-ClG undergo expansion and contraction, respectively, following photoexcitation to the Bb state. The amount of distortions of the excited state structure from that of the ground state structure is reflected by the total internal reorganization energy that is determined at 112 cm(-1). The contribution of the inertial component of the solvent response towards the total reorganization energy was obtained at 1220 cm(-1). In addition, our simulation also yields an instantaneous response of the first

Bound state and localization of excitation in many-body open systems

NASA Astrophysics Data System (ADS)

Cui, H. T.; Shen, H. Z.; Hou, S. C.; Yi, X. X.

2018-04-01

We study the exact bound state and time evolution for single excitations in one-dimensional X X Z spin chains within a non-Markovian reservoir. For the bound state, a common feature is the localization of single excitations, which means the spontaneous emission of excitations into the reservoir is prohibited. Exceptionally, the pseudo-bound state can be found, for which the single excitation has a finite probability of emission into the reservoir. In addition, a critical energy scale for bound states is also identified, below which only one bound state exists, and it is also the pseudo-bound state. The effect of quasirandom disorder in the spin chain is also discussed; such disorder induces the single excitation to locate at some spin sites. Furthermore, to display the effect of bound state and disorder on the preservation of quantum information, the time evolution of single excitations in spin chains is studied exactly. An interesting observation is that the excitation can stay at its initial location with high probability only when the bound state and disorder coexist. In contrast, when either one of them is absent, the information of the initial state can be erased completely or becomes mixed. This finding shows that the combination of bound state and disorder can provide an ideal mechanism for quantum memory.

Vibronic relaxation dynamics of o-dichlorobenzene in its lowest excited singlet state

NASA Astrophysics Data System (ADS)

Liu, Benkang; Zhao, Haiyan; Lin, Xiang; Li, Xinxin; Gao, Mengmeng; Wang, Li; Wang, Wei

2018-01-01

Vibronic dynamics of o-dichlorobenzene in its lowest excited singlet state, S1, is investigated in real time by using femtosecond pump-probe method, combined with time-of-flight mass spectroscopy and photoelectron velocity mapping technique. Relaxation processes for the excitation in the range of 276-252 nm can be fitted by single exponential decay model, while in the case of wavelength shorter than 252 nm two-exponential decay model must be adopted for simulating transient profiles. Lifetime constants of the vibrationally excited S1 states change from 651 ± 10 ps for 276 nm excitation to 61 ± 1 ps for 242 nm excitation. Both the internal conversion from the S1 to the highly vibrationally excited ground state S0 and the intersystem crossing from the S1 to the triplet state are supposed to play important roles in de-excitation processes. Exponential fitting of the de-excitation rates on the excitation energy implies such de-excitation process starts from the highly vibrationally excited S0 state, which is validated, by probing the relaxation following photoexcitation at 281 nm, below the S1 origin. Time-dependent photoelectron kinetic energy distributions have been obtained experimentally. As the excitation wavelength changes from 276 nm to 242 nm, different cationic vibronic vibrations can be populated, determined by the Franck-Condon factors between the large geometry distorted excited singlet states and final cationic states.

Investigation into chromophore excited-state coupling in allophycocyanin

NASA Astrophysics Data System (ADS)

Zheng, Xiguang; Zhao, Fuli; Wang, He Z.; Gao, Zhaolan; Yu, Zhenxin; Zhu, Jinchang; Xia, Andong; Jiang, Lijin

1994-08-01

Both theoretical and experimental studies are presented on chromophore excited-state coupling in linker-free allophycocyanin (APC), one of the antenna phycobiliproteins in algal photosynthesis. A three-site-coupling model has been introduced to describe the exciton interaction mechanism amoung the excited (beta) chromophore in APC, and the exciton energy splitting is estimated. Picosecond polarized fluorescence experiments both on monomeric and trimeric APC isolated from alga Spirulina platensis have been performed. The experimental results show that APC monomer and trimer exhibit remarkedly different spectropic characteristics, and satisfy the suggestion of strong excited- state coupling among chromophores in APC.

Effect of nuclear-reaction mechanisms on the population of excited nuclear states and isomeric ratios

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

Skobelev, N. K., E-mail: skobelev@jinr.ru

2016-07-15

Experimental data on the cross sections for channels of fusion and transfer reactions induced by beams of radioactive halo nuclei and clustered and stable loosely bound nuclei were analyzed, and the results of this analysis were summarized. The interplay of the excitation of single-particle states in reaction-product nuclei and direct reaction channels was established for transfer reactions. Respective experiments were performed in stable ({sup 6}Li) and radioactive ({sup 6}He) beams of the DRIBs accelerator complex at the Flerov Laboratory of Nuclear Reactions, Joint Institute for Nuclear Research, and in deuteron and {sup 3}He beams of the U-120M cyclotron at themore » Nuclear Physics Institute, Academy Sciences of Czech Republic (Řež and Prague, Czech Republic). Data on subbarrier and near-barrier fusion reactions involving clustered and loosely bound light nuclei ({sup 6}Li and {sup 3}He) can be described quite reliably within simple evaporation models with allowance for different reaction Q-values and couple channels. In reactions involving halo nuclei, their structure manifests itself most strongly in the region of energies below the Coulomb barrier. Neutron transfer occurs with a high probability in the interactions of all loosely bound nuclei with light and heavy stable nuclei at positive Q-values. The cross sections for such reactions and the respective isomeric ratios differ drastically for nucleon stripping and nucleon pickup mechanisms. This is due to the difference in the population probabilities for excited single-particle states.« less

Enhanced Bulk-Edge Coulomb Coupling in Fractional Fabry-Perot Interferometers.

PubMed

von Keyserlingk, C W; Simon, S H; Rosenow, Bernd

2015-09-18

Recent experiments use Fabry-Perot (FP) interferometry to claim that the ν=5/2 quantum Hall state exhibits non-Abelian topological order. We note that the experiments appear inconsistent with a model neglecting bulk-edge Coulomb coupling and Majorana tunneling, so we reexamine the theory of FP devices. Even a moderate Coulomb coupling may strongly affect some fractional plateaus, but very weakly affect others, allowing us to model the data over a wide range of plateaus. While experiments are consistent with the ν=5/2 state harboring Moore-Read topological order, they may have measured Coulomb effects rather than an "even-odd effect" due to non-Abelian braiding.

Non-perturbative RPA-method implemented in the Coulomb gauge QCD Hamiltonian: From quarks and gluons to baryons and mesons

NASA Astrophysics Data System (ADS)

Yepez-Martinez, Tochtli; Civitarese, Osvaldo; Hess, Peter O.

2018-02-01

Starting from an algebraic model based on the QCD-Hamiltonian and previously applied to study meson states, we have developed an extension of it in order to explore the structure of baryon states. In developing our approach we have adapted concepts taken from group theory and non-perturbative many-body methods to describe states built from effective quarks and anti-quarks degrees of freedom. As a Hamiltonian we have used the QCD Hamiltonian written in the Coulomb Gauge, and expressed it in terms of effective quark-antiquark, di-quarks and di-antiquark excitations. To gain some insights about the relevant interactions of quarks in hadronic states, the Hamiltonian was approximately diagonalized by mapping quark-antiquark pairs and di-quarks (di-antiquarks) onto phonon states. In dealing with the structure of the vacuum of the theory, color-scalar and color-vector states are introduced to account for ground-state correlations. While the use of a purely color-scalar ground state is an obvious choice, so that colorless hadrons contain at least three quarks, the presence of coupled color-vector pairs in the ground state allows for colorless excitations resulting from the action of color objects upon it.

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

PubMed

Kowalczyk, Tim; Le, Khoa; Irle, Stephan

2016-01-12

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

Two-dimensional Fano lineshapes: Excited-state absorption contributions

NASA Astrophysics Data System (ADS)

Finkelstein-Shapiro, Daniel; Pullerits, Tõnu; Hansen, Thorsten

2018-05-01

Fano interferences in nanostructures are influenced by dissipation effects as well as many-body interactions. Two-dimensional coherent spectroscopies have just begun to be applied to these systems where the spectroscopic signatures of a discrete-continuum structure are not known. In this article, we calculate the excited-state absorption contribution for different models of higher lying excited states. We find that the characteristic asymmetry of one-dimensional spectroscopies is recovered from the many-body contributions and that the higher lying excited manifolds have distorted lineshapes that are not anticipated from discrete-level Hamiltonians. We show that the Stimulated Emission cannot have contributions from a flat continuum of states. This work completes the Ground-State Bleach and Stimulated Emission signals that were calculated previously [D. Finkelstein-Shapiro et al., Phys. Rev. B 94, 205137 (2016)]. The model reproduces the observations reported for molecules on surfaces probed by 2DIR.

Two-dimensional Fano lineshapes: Excited-state absorption contributions.

PubMed

Finkelstein-Shapiro, Daniel; Pullerits, Tõnu; Hansen, Thorsten

2018-05-14

Fano interferences in nanostructures are influenced by dissipation effects as well as many-body interactions. Two-dimensional coherent spectroscopies have just begun to be applied to these systems where the spectroscopic signatures of a discrete-continuum structure are not known. In this article, we calculate the excited-state absorption contribution for different models of higher lying excited states. We find that the characteristic asymmetry of one-dimensional spectroscopies is recovered from the many-body contributions and that the higher lying excited manifolds have distorted lineshapes that are not anticipated from discrete-level Hamiltonians. We show that the Stimulated Emission cannot have contributions from a flat continuum of states. This work completes the Ground-State Bleach and Stimulated Emission signals that were calculated previously [D. Finkelstein-Shapiro et al., Phys. Rev. B 94, 205137 (2016)]. The model reproduces the observations reported for molecules on surfaces probed by 2DIR.

σ-SCF: A direct energy-targeting method to mean-field excited states.

PubMed

Ye, Hong-Zhou; Welborn, Matthew; Ricke, Nathan D; Van Voorhis, Troy

2017-12-07

The mean-field solutions of electronic excited states are much less accessible than ground state (e.g., Hartree-Fock) solutions. Energy-based optimization methods for excited states, like Δ-SCF (self-consistent field), tend to fall into the lowest solution consistent with a given symmetry-a problem known as "variational collapse." In this work, we combine the ideas of direct energy-targeting and variance-based optimization in order to describe excited states at the mean-field level. The resulting method, σ-SCF, has several advantages. First, it allows one to target any desired excited state by specifying a single parameter: a guess of the energy of that state. It can therefore, in principle, find all excited states. Second, it avoids variational collapse by using a variance-based, unconstrained local minimization. As a consequence, all states-ground or excited-are treated on an equal footing. Third, it provides an alternate approach to locate Δ-SCF solutions that are otherwise hardly accessible by the usual non-aufbau configuration initial guess. We present results for this new method for small atoms (He, Be) and molecules (H 2 , HF). We find that σ-SCF is very effective at locating excited states, including individual, high energy excitations within a dense manifold of excited states. Like all single determinant methods, σ-SCF shows prominent spin-symmetry breaking for open shell states and our results suggest that this method could be further improved with spin projection.

Excited state conformational dynamics in carotenoids: dark intermediates and excitation energy transfer.

PubMed

Beck, Warren F; Bishop, Michael M; Roscioli, Jerome D; Ghosh, Soumen; Frank, Harry A

2015-04-15

A consideration of the excited state potential energy surfaces of carotenoids develops a new hypothesis for the nature of the conformational motions that follow optical preparation of the S2 (1(1)Bu(+)) state. After an initial displacement from the Franck-Condon geometry along bond length alternation coordinates, it is suggested that carotenoids pass over a transition-state barrier leading to twisted conformations. This hypothesis leads to assignments for several dark intermediate states encountered in femtosecond spectroscopic studies. The Sx state is assigned to the structure reached upon the onset of torsional motions near the transition state barrier that divides planar and twisted structures on the S2 state potential energy surface. The X state, detected recently in two-dimensional electronic spectra, corresponds to a twisted structure well past the barrier and approaching the S2 state torsional minimum. Lastly, the S(∗) state is assigned to a low lying S1 state structure with intramolecular charge transfer character (ICT) and a pyramidal conformation. It follows that the bent and twisted structures of carotenoids that are found in photosynthetic light-harvesting proteins yield excited-state structures that favor the development of an ICT character and optimized energy transfer yields to (bacterio)chlorophyll acceptors. Copyright © 2015 Elsevier Inc. All rights reserved.

Photocyclization Reactions of Diarylethenes via the Excited Triplet State.

PubMed

Murata, Ryutaro; Yago, Tomoaki; Wakasa, Masanobu

2015-11-12

Cyclization reactions of three diarylethene derivatives, 1,2-bis(2-methyl-3-benzothienyl)perfluorocyclopentene (BT), 1,2-bis(2-hexyl-3-benzothienyl)perfluorocyclopentene (BTHex), and 1,2-bis(2-isopropyl-3-benzothienyl)perfluorocyclopentene (BTiPr), via their excited triplet states were studied by means of steady-state and nanosecond transient absorption spectroscopy. The excited triplet states of BT, BTHex, and BTiPr were generated by energy transfer from the photoexcited triplet states of sensitizers such as xanthone, phenanthrene, and pyrene. The single-step quantum yields of the cyclization reactions from the excited triplet states of BT, BTHex, and BTiPr were determined to be 0.34, 0.53, and 0.65, respectively. The triplet energies of these three BTs were estimated to be 190-200 kJ mol(-1).

Tunnel ionization of highly excited atoms in a noncoherent laser radiation field

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

Krainov, V.P.; Todirashku, S.S.

1982-10-01

A theory is developed of the ionization of highly excited atomic states by a low-frequency field of noncoherent laser radiation with a large number of modes. Analytic formulas are obtained for the probability of the tunnel ionization in such a field. An analysis is made of the case of the hydrogen atom when the parabolic quantum numbers are sufficiently good in the low-frequency limit, as well as of the case of highly excited states of complex atoms when these states are characterized by a definite orbital momentum and parity. It is concluded that the statistical factor representing the ratio ofmore » the probability in a stochastic field to the probability in a monochromatic field decreases, compared with the case of a short-range potential, if the ''Coulomb tail'' is included. It is shown that at a given field intensity the statistical factor decreases on increase in the principal quantum number of the state being ionized.« less

Excited State Atom-Ion Charge-Exchange

NASA Astrophysics Data System (ADS)

Li, Ming; Makrides, Constantinos; Petrov, Alexander; Kotochigova, Svetlana

2017-04-01

We theoretically investigate the exothermic charge-exchange reaction between an excited atom and a ground-state positive ion. In particular, we focus on MOT-excited Ca*(4s4p 1P) atoms colliding with ground-state Yb+ ions, which are under active study by the experimental group of E. Hudson at UCLA. Collisions between an excited atom and an ion are guided by two major contributions to the long-range interaction potentials, the induction C4 /R4 and charge-quadrupole C3 /R3 potentials, and their coupling by the electron-exchange interaction. Our model of these forces leads to close-coupling equations for multiple reaction channels. We find several avoided crossings between the potentials that couple to the nearby asymptotic limits of Yb*+Ca+, some of which can possibly provide large charge exchange rate coefficients above 10-10 cm3 / s. We acknowledge support from the US Army Research Office, MURI Grants W911NF-14-1-0378 and the US National Science Foundation, Grant PHY-1619788.

Rate/state Coulomb stress transfer model for the CSEP Japan seismicity forecast

NASA Astrophysics Data System (ADS)

Toda, Shinji; Enescu, Bogdan

2011-03-01

Numerous studies retrospectively found that seismicity rate jumps (drops) by coseismic Coulomb stress increase (decrease). The Collaboratory for the Study of Earthquake Prediction (CSEP) instead provides us an opportunity for prospective testing of the Coulomb hypothesis. Here we adapt our stress transfer model incorporating rate and state dependent friction law to the CSEP Japan seismicity forecast. We demonstrate how to compute the forecast rates of large shocks in 2009 using the large earthquakes during the past 120 years. The time dependent impact of the coseismic stress perturbations explains qualitatively well the occurrence of the recent moderate size shocks. Such ability is partly similar to that of statistical earthquake clustering models. However, our model differs from them as follows: the off-fault aftershock zones can be simulated using finite fault sources; the regional areal patterns of triggered seismicity are modified by the dominant mechanisms of the potential sources; the imparted stresses due to large earthquakes produce stress shadows that lead to a reduction of the forecasted number of earthquakes. Although the model relies on several unknown parameters, it is the first physics based model submitted to the CSEP Japan test center and has the potential to be tuned for short-term earthquake forecasts.

Phase-dependent above-barrier ionization of excited-state electrons.

PubMed

Yang, Weifeng; Song, Xiaohong; Chen, Zhangjin

2012-05-21

The carrier-envelope phase (CEP)-dependent above-barrier ionization (ABI) has been investigated in order to probe the bound-state electron dynamics. It is found that when the system is initially prepared in the excited state, the ionization yield asymmetry between left and right sides can occur both in low-energy and high-energy parts of the photoelectron spectra. Moreover, in electron momentum map, a new interference effect along the direction perpendicular to the laser polarization is found. We show that this interference is related to the competition among different excited states. The interference effect is dependent on CEPs of few-cycle probe pulses, which can be used to trace the superposition information and control the electron wave packet of low excited states.

Coulomb matrix elements in multi-orbital Hubbard models.

PubMed

Bünemann, Jörg; Gebhard, Florian

2017-04-26

Coulomb matrix elements are needed in all studies in solid-state theory that are based on Hubbard-type multi-orbital models. Due to symmetries, the matrix elements are not independent. We determine a set of independent Coulomb parameters for a d-shell and an f-shell and all point groups with up to 16 elements (O h , O, T d , T h , D 6h , and D 4h ). Furthermore, we express all other matrix elements as a function of the independent Coulomb parameters. Apart from the solution of the general point-group problem we investigate in detail the spherical approximation and first-order corrections to the spherical approximation.

Excited state dynamics of the astaxanthin radical cation

NASA Astrophysics Data System (ADS)

Amarie, Sergiu; Förster, Ute; Gildenhoff, Nina; Dreuw, Andreas; Wachtveitl, Josef

2010-07-01

Femtosecond transient absorption spectroscopy in the visible and NIR and ultrafast fluorescence spectroscopy were used to examine the excited state dynamics of astaxanthin and its radical cation. For neutral astaxanthin, two kinetic components corresponding to time constants of 130 fs (decay of the S 2 excited state) and 5.2 ps (nonradiative decay of the S 1 excited state) were sufficient to describe the data. The dynamics of the radical cation proved to be more complex. The main absorption band was shifted to 880 nm (D 0 → D 3 transition), showing a weak additional band at 1320 nm (D 0 → D 1 transition). We found, that D 3 decays to the lower-lying D 2 within 100 fs, followed by a decay to D 1 with a time constant of 0.9 ps. The D 1 state itself exhibited a dual behavior, the majority of the population is transferred to the ground state in 4.9 ps, while a small population decays on a longer timescale of 40 ps. Both transitions from D 1 were found to be fluorescent.

Excited state characteristics of acridine dyes: acriflavine and acridine orange.

PubMed

Sharma, Vijay K; Sahare, P D; Rastogi, Ramesh C; Ghoshal, S K; Mohan, D

2003-06-01

The magnitude of the Stokes shift (frequency shifts in absorption and fluorescence spectra) is observed on changing the solvents and further has been used to calculate experimentally the dipole moments (ground state and excited state) of acriflavine and acridine orange dye molecules. Theoretically, dipole moments are calculated using PM 3 Model. The dipole moments of excited states, for both molecules investigated here, are higher than the corresponding values in the ground states. The increase in the dipole moment has been explained in terms of the nature of the excited state. Acriflavine dye overcomes the non-lasing behaviour of acridine orange due to quaternization of the central nitrogen atom.

A comparison of Coulomb and pseudo-Coulomb friction implementations: Application to the table contact phase of gymnastics vaulting.

PubMed

Jackson, M I; Hiley, M J; Yeadon, M R

2011-10-13

In the table contact phase of gymnastics vaulting both dynamic and static friction act. The purpose of this study was to develop a method of simulating Coulomb friction that incorporated both dynamic and static phases and to compare the results with those obtained using a pseudo-Coulomb implementation of friction when applied to the table contact phase of gymnastics vaulting. Kinematic data were obtained from an elite level gymnast performing handspring straight somersault vaults using a Vicon optoelectronic motion capture system. An angle-driven computer model of vaulting that simulated the interaction between a seven segment gymnast and a single segment vaulting table during the table contact phase of the vault was developed. Both dynamic and static friction were incorporated within the model by switching between two implementations of the tangential frictional force. Two vaulting trials were used to determine the model parameters using a genetic algorithm to match simulations to recorded performances. A third independent trial was used to evaluate the model and close agreement was found between the simulation and the recorded performance with an overall difference of 13.5%. The two-state simulation model was found to be capable of replicating performance at take-off and also of replicating key contact phase features such as the normal and tangential motion of the hands. The results of the two-state model were compared to those using a pseudo-Coulomb friction implementation within the simulation model. The two-state model achieved similar overall results to those of the pseudo-Coulomb model but obtained solutions more rapidly. Copyright © 2011 Elsevier Ltd. All rights reserved.

Nature of ground and electronic excited states of higher acenes

PubMed Central

Yang, Yang; Yang, Weitao

2016-01-01

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 1Ag 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 3B2u 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 1B2u is a zwitterionic state to the short axis. The excited 1Ag 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 1B2u and excited 1Ag 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

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

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

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

1998-02-01

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

Excited state X-ray absorption spectroscopy: Probing both electronic and structural dynamics

NASA Astrophysics Data System (ADS)

Neville, Simon P.; Averbukh, Vitali; Ruberti, Marco; Yun, Renjie; Patchkovskii, Serguei; Chergui, Majed; Stolow, Albert; Schuurman, Michael S.

2016-10-01

We investigate the sensitivity of X-ray absorption spectra, simulated using a general method, to properties of molecular excited states. Recently, Averbukh and co-workers [M. Ruberti et al., J. Chem. Phys. 140, 184107 (2014)] introduced an efficient and accurate L 2 method for the calculation of excited state valence photoionization cross-sections based on the application of Stieltjes imaging to the Lanczos pseudo-spectrum of the algebraic diagrammatic construction (ADC) representation of the electronic Hamiltonian. In this paper, we report an extension of this method to the calculation of excited state core photoionization cross-sections. We demonstrate that, at the ADC(2)x level of theory, ground state X-ray absorption spectra may be accurately reproduced, validating the method. Significantly, the calculated X-ray absorption spectra of the excited states are found to be sensitive to both geometric distortions (structural dynamics) and the electronic character (electronic dynamics) of the initial state, suggesting that core excitation spectroscopies will be useful probes of excited state non-adiabatic dynamics. We anticipate that the method presented here can be combined with ab initio molecular dynamics calculations to simulate the time-resolved X-ray spectroscopy of excited state molecular wavepacket dynamics.

One-dimensional Coulomb problem in Dirac materials

NASA Astrophysics Data System (ADS)

Downing, C. A.; Portnoi, M. E.

2014-11-01

We investigate the one-dimensional Coulomb potential with application to a class of quasirelativistic systems, so-called Dirac-Weyl materials, described by matrix Hamiltonians. We obtain the exact solution of the shifted and truncated Coulomb problems, with the wave functions expressed in terms of special functions (namely, Whittaker functions), while the energy spectrum must be determined via solutions to transcendental equations. Most notably, there are critical band gaps below which certain low-lying quantum states are missing in a manifestation of atomic collapse.

σ-SCF: A direct energy-targeting method to mean-field excited states

NASA Astrophysics Data System (ADS)

Ye, Hong-Zhou; Welborn, Matthew; Ricke, Nathan D.; Van Voorhis, Troy

2017-12-01

The mean-field solutions of electronic excited states are much less accessible than ground state (e.g., Hartree-Fock) solutions. Energy-based optimization methods for excited states, like Δ-SCF (self-consistent field), tend to fall into the lowest solution consistent with a given symmetry—a problem known as "variational collapse." In this work, we combine the ideas of direct energy-targeting and variance-based optimization in order to describe excited states at the mean-field level. The resulting method, σ-SCF, has several advantages. First, it allows one to target any desired excited state by specifying a single parameter: a guess of the energy of that state. It can therefore, in principle, find all excited states. Second, it avoids variational collapse by using a variance-based, unconstrained local minimization. As a consequence, all states—ground or excited—are treated on an equal footing. Third, it provides an alternate approach to locate Δ-SCF solutions that are otherwise hardly accessible by the usual non-aufbau configuration initial guess. We present results for this new method for small atoms (He, Be) and molecules (H2, HF). We find that σ-SCF is very effective at locating excited states, including individual, high energy excitations within a dense manifold of excited states. Like all single determinant methods, σ-SCF shows prominent spin-symmetry breaking for open shell states and our results suggest that this method could be further improved with spin projection.

Excitation of lowest electronic states of the uracil molecule by slow electrons

NASA Astrophysics Data System (ADS)

Chernyshova, I. V.; Kontros, J. E.; Markush, P. P.; Shpenik, O. B.

2012-07-01

The excitation of lowest electronic states of the uracil molecule in the gas phase has been studied by electron energy loss spectroscopy. Along with excitation of lowest singlet states, excitation of two lowest triplet states at 3.75 and 4.76 eV (±0.05 eV) and vibrational excitation of the molecule in two resonant ranges (1-2 and 3-4 eV) have been observed for the first time. The peak of the excitation band related to the lowest singlet state (5.50 eV) is found to be blueshifted by 0.4 eV in comparison with the optical absorption spectroscopy data. The threshold excitation spectra have been measured for the first time, with detection of electrons inelastically scattered by an angle of 180°. These spectra exhibit clear separation of the 5.50-eV-wide band into two bands, which are due to the excitation of the triplet 13 A″ and singlet 11 A' states.

Vibrational spectroscopy of the electronically excited state. 4. Nanosecond and picosecond time-resolved resonance Raman spectroscopy of carotenoid excited states

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

Dallinger, R.F.; Farquharson, S.; Woodruff, W.H.

Resonance Raman and electronic absorption spectra are reported for the S/sub 0/ and T/sub 1/ states of the carotenoids ..beta..-carotene, zeaxanthin, echinenone, canthaxanthin, dihydroxylycopene, astaxanthin, decapreno(C/sub 50/)-..beta..-carotene, ..beta..-apo-8'-carotenal, and ethyl ..beta..-apo-8'-carotenoate. The results reveal qualitatively similar ground-state spectra and similar frequency shifts in all observed resonance Raman modes between S/sub 0/ and T/sub 1/, regardless of carotenoid structure. Examinations of the relationship of the putative C--C and C==C frequencies in S/sub 0/ and T/sub 1/ reveals anomalous shifts to lower frequency in the ''single-bond'' mode upon electronic excitation. These shifts may be due to molecular distortions in the excited statemore » which force changes in molecular motions comprising the observed modes. However, another possibility requiring no distortion is that the interaction (off-diagonal) force constants connecting the C--C and C==C modes change sign upon electronic excitation. This latter phenomenon may provide a unitary explanation for the ''anomalous'' frequency shifts in the C--C and C==C modes, both in the T/sub 1/ states of carotenoids and in the S/sub 1/ states of simpler polyenes, without postulating large, unpredicted structural changes upon excitation or general errors in existing vibrational or theoretical analyses. Resonance Raman and absorbance studies with 35-ps time resolution suggest that S/sub 1/ lifetime (of the /sup 1/B/sub u/ and/or the /sup 1/A/sub g/* states) of ..beta..-carotene in benzene is less than 1 ps.« less

Ultrafast Dynamics of 1,3-Cyclohexadiene in Highly Excited States

DOE PAGES

Bühler, Christine C.; Minitti, Michael P.; Deb, Sanghamitra; ...

2011-01-01

The ultrafast dynamics of 1,3-cyclohexadiene has been investigated via structurally sensitive Rydberg electron binding energies and shown to differ upon excitation to the 1B state and the 3p Rydberg state. Excitation of the molecule with 4.63 eV photons into the ultrashort-lived 1B state yields the well-known ring opening to 1,3,5-hexatriene, while a 5.99 eV photon lifts the molecule directly into the 3p-Rydberg state. Excitation to 3p does not induce ring opening. In both experiments, time-dependent shifts of the Rydberg electron binding energy reflect the structural dynamics of the molecular core. Structural distortions associated with 3p-excitation cause a dynamical shift in the -more » and -binding energies by 10 and 26 meV/ps, respectively, whereas after excitation into 1B, more severe structural transformations along the ring-opening coordinate produce shifts at a rate of 40 to 60 meV/ps. The experiment validates photoionization-photoelectron spectroscopy via Rydberg states as a powerful technique to observe structural dynamics of polyatomic molecules.« less

Fluorescence excitation and excited state intramolecular relaxation dynamics of jet-cooled methyl-2-hydroxy-3-naphthoate

NASA Astrophysics Data System (ADS)

McCarthy, Annemarie; Ruth, Albert A.

2013-11-01

Two distinct S0 → S1 fluorescence excitation spectra of methyl-2-hydroxy-3-napthoate (MHN23) have been obtained by monitoring fluorescence separately in the short (˜410 nm) and long (˜650 nm) wavelength emission bands. The short wavelength fluorescence is assigned to two MHN23 conformers which do not undergo excited state intramolecular proton transfer (ESIPT). Analysis of the 'long wavelength' fluorescence excitation spectrum, which arises from the proton transfer tautomer of MHN23 indicates an average lifetime of τ ⩾ 18 ± 2 fs for the initially excited states. Invoking the results of Catalan et al. [J. Phys. Chem. A, 1999, 103, 10921], who determined the N tautomer to decay predominantly via a fast non-radiative process, the limit of the rate of intramolecular excited proton transfer in MHN23 is calculated as, kpt ⩽ 1 × 1012 s-1.

Excited state electron affinity calculations for aluminum

NASA Astrophysics Data System (ADS)

Hussein, Adnan Yousif

2017-08-01

Excited states of negative aluminum ion are reviewed, and calculations of electron affinities of the states (3s^23p^2)^1D and (3s3p^3){^5}{S}° relative to the (3s^23p)^2P° and (3s3p^2)^4P respectively of the neutral aluminum atom are reported in the framework of nonrelativistic configuration interaction (CI) method. A priori selected CI (SCI) with truncation energy error (Bunge in J Chem Phys 125:014107, 2006) and CI by parts (Bunge and Carbó-Dorca in J Chem Phys 125:014108, 2006) are used to approximate the valence nonrelativistic energy. Systematic studies of convergence of electron affinity with respect to the CI excitation level are reported. The calculated value of the electron affinity for ^1D state is 78.675(3) meV. Detailed Calculations on the ^5S°c state reveals that is 1216.8166(3) meV below the ^4P state.

Nested variant of the method of moments of coupled cluster equations for vertical excitation energies and excited-state potential energy surfaces.

PubMed

Kowalski, Karol

2009-05-21

In this article we discuss the problem of proper balancing of the noniterative corrections to the ground- and excited-state energies obtained with approximate coupled cluster (CC) and equation-of-motion CC (EOMCC) approaches. It is demonstrated that for a class of excited states dominated by single excitations and for states with medium doubly excited component, the newly introduced nested variant of the method of moments of CC equations provides mathematically rigorous way of balancing the ground- and excited-state correlation effects. The resulting noniterative methodology accounting for the effect of triples is tested using its parallel implementation on the systems, for which iterative CC/EOMCC calculations with full inclusion of triply excited configurations or their most important subset are numerically feasible.

Controlling excited-state contamination in nucleon matrix elements

DOE PAGES

Yoon, Boram; Gupta, Rajan; Bhattacharya, Tanmoy; ...

2016-06-08

We present a detailed analysis of methods to reduce statistical errors and excited-state contamination in the calculation of matrix elements of quark bilinear operators in nucleon states. All the calculations were done on a 2+1-flavor ensemble with lattices of size 32 3 × 64 generated using the rational hybrid Monte Carlo algorithm at a = 0.081 fm and with M π = 312 MeV. The statistical precision of the data is improved using the all-mode-averaging method. We compare two methods for reducing excited-state contamination: a variational analysis and a 2-state fit to data at multiple values of the source-sink separationmore » t sep. We show that both methods can be tuned to significantly reduce excited-state contamination and discuss their relative advantages and cost effectiveness. As a result, a detailed analysis of the size of source smearing used in the calculation of quark propagators and the range of values of t sep needed to demonstrate convergence of the isovector charges of the nucleon to the t sep → ∞ estimates is presented.« less

Circular polarization of X-ray radiation emitted by longitudinally polarized electron impact excitation: Under a screened Coulomb interaction

NASA Astrophysics Data System (ADS)

Chen, Zhan-Bin

2017-12-01

Longitudinally polarized electron impact excitation from the ground state 1s2 to the excited state 1s2l (l =s,p) levels of highly charged He-like Fe24+ ions in weakly coupled hot-dense plasmas is investigated using a fully relativistic distorted-wave method. The Debye-Hückel potential is used to describe the plasma screening. Benchmark results such as the total cross sections, the magnetic sublevels cross sections, and the circular polarizations of corresponding X-ray radiations are presented. For the excitation process, results show that the plasma screening has an effect in reducing both the total and magnetic sublevels cross sections. For the de-excitation process, it is found that while the plasma screening as a slightly effect on the circular polarizations of radiations for the 1 s 2 s 3S1 → 1 s21S0,1 s 2 p 3P2 → 1 s21S0 , and 1 s 2 p 1P1 → 1 s21S0 transition lines, it gives a substantial contribution for the same properties of the 1 s 2 p 3P1 → 1 s21S0 line.

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

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

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

1999-10-14

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

σ -SCF: A Direct Energy-targeting Method To Mean-field Excited States

NASA Astrophysics Data System (ADS)

Ye, Hongzhou; Welborn, Matthew; Ricke, Nathan; van Voorhis, Troy

The mean-field solutions of electronic excited states are much less accessible than ground state (e.g. Hartree-Fock) solutions. Energy-based optimization methods for excited states, like Δ-SCF, tend to fall into the lowest solution consistent with a given symmetry - a problem known as ``variational collapse''. In this work, we combine the ideas of direct energy-targeting and variance-based optimization in order to describe excited states at the mean-field level. The resulting method, σ-SCF, has several advantages. First, it allows one to target any desired excited state by specifying a single parameter: a guess of the energy of that state. It can therefore, in principle, find all excited states. Second, it avoids variational collapse by using a variance-based, unconstrained local minimization. As a consequence, all states - ground or excited - are treated on an equal footing. Third, it provides an alternate approach to locate Δ-SCF solutions that are otherwise hardly accessible by the usual non-aufbau configuration initial guess. We present results for this new method for small atoms (He, Be) and molecules (H2, HF). This work was funded by a Grant from NSF (CHE-1464804).

Gyromagnetic ratios of excited states in 198Pt; measurements and interacting boson approximation model calculations

NASA Astrophysics Data System (ADS)

Stuchbery, A. E.; Ryan, C. G.; Bolotin, H. H.; Morrison, I.; Sie, S. H.

1981-07-01

The enhanced transient hyperfine field manifest at the nuclei of swiftly recoiling ions traversing magnetized ferromagnetic materials was utilized to measure the gyromagnetic ratios of the 2 +1, 2 +2 and 4 +1 states in 198Pt by the thin-foil technique. The states of interest were populated by Coulomb excitation using a beam of 220 MeV 58Ni ions. The results obtained were: g(2 +1) = 0.324 ± 0.026; g(2 +2) = 0.34 ± 0.06; g(4 +1) = 0.34 ± 0.06. In addition, these measurements served to discriminate between the otherwise essentially equally probable values previously reported for the E2/M1 ratio of the 2 +2 → 2 +1 transition in 198Pt. We also performed interacting boson approximation (IBA) model-based calculations in the O(6) limit symmetry, with and without inclusion of a small degree of symmetry breaking, and employed the M1 operator in both first- and second-order to obtain M1 selection rules and to calculate gyromagnetic ratios of levels. When O(6) symmetry is broken, there is a predicted departure from constancy of the g-factors which provides a good test of the nuclear wave function. Evaluative comparisons are made between these experimental and predicted g-factors.

The examination of berberine excited state by laser flash photolysis

NASA Astrophysics Data System (ADS)

Cheng, Lingli; Wang, Mei; Zhao, Ping; Zhu, Hui; Zhu, Rongrong; Sun, Xiaoyu; Yao, Side; Wang, Shilong

2009-07-01

The property of the excited triplet state of berberine (BBR) was investigated by using time-resolved laser flash photolysis of 355 nm in acetonitrile. The transient absorption spectra of the excited triplet BBR were obtained in acetonitrile, which have an absorption maximum at 420 nm. And the ratio of excitation to ionization of BBR in acetonitrile solvent was calculated. The self-decay and self-quenching rate constants, and the absorption coefficient of 3BBR* were investigated and the excited state quantum yield was determined. Furthermore utilizing the benzophenone (BEN) as a triplet sensitizer, and the β-carotene (Car) as an excited energy transfer acceptor, the assignment of 3BBR* was further confirmed and the related energy transfer rate constants were also determined.

Coulomb interactions in charged fluids.

PubMed

Vernizzi, Graziano; Guerrero-García, Guillermo Iván; de la Cruz, Monica Olvera

2011-07-01

The use of Ewald summation schemes for calculating long-range Coulomb interactions, originally applied to ionic crystalline solids, is a very common practice in molecular simulations of charged fluids at present. Such a choice imposes an artificial periodicity which is generally absent in the liquid state. In this paper we propose a simple analytical O(N(2)) method which is based on Gauss's law for computing exactly the Coulomb interaction between charged particles in a simulation box, when it is averaged over all possible orientations of a surrounding infinite lattice. This method mitigates the periodicity typical of crystalline systems and it is suitable for numerical studies of ionic liquids, charged molecular fluids, and colloidal systems with Monte Carlo and molecular dynamics simulations.

Polymethine and squarylium molecules with large excited-state absorption

NASA Astrophysics Data System (ADS)

Lim, Jin Hong; Przhonska, Olga V.; Khodja, Salah; Yang, Sidney; Ross, T. S.; Hagan, David J.; Van Stryland, Eric W.; Bondar, Mikhail V.; Slominsky, Yuriy L.

1999-07-01

We study nonlinear absorption in a series of ten polymethine dyes and two squarylium dyes using Z-scan, pump-probe and optical limiting experiments. Both picosecond and nanosecond characterization were performed at 532 nm, while picosecond measurements were performed using an optical parametric oscillator (OPO) from 440 to 650 nm. The photophysical parameters of these dyes including cross sections and excited-state lifetimes are presented both in solution in ethanol and in an elastopolymeric material, polyurethane acrylate (PUA). We determine that the dominant nonlinearity in all these dyes is large excited-state absorption (ESA), i.e. reverse saturable absorption. For several of the dyes we measure a relatively large ground-state absorption cross section, σ01, which effectively populates an excited state that possesses an extremely large ESA cross section, σ12. The ratios of σ12/ σ01 are the largest we know of, up to 200 at 532 nm, and lead to very low thresholds for optical limiting. However, the lifetimes of the excited state are of the order of 1 ns in ethanol, which is increased to up to 3 ns in PUA. This lifetime is less than optimum for sensor protection applications for Q-switched inputs, and intersystem crossing times for these molecules are extremely long, so that triplet states are not populated. These parameters show a significant improvement over those of the first set of this class of dyes studied and indicate that further improvement of the photophysical parameters may be possible. From these measurements, correlations between molecular structure and nonlinear properties are made. We propose a five-level, all-singlet state model, which includes reorientation processes in the first excited state. This includes a trans- cis conformational change that leads to the formation of a new state with a new molecular configuration which is also absorbing but can undergo a light-induced degradation at high inputs.

Nonadiabatic excited-state molecular dynamics: modeling photophysics in organic conjugated materials.

PubMed

Nelson, Tammie; Fernandez-Alberti, Sebastian; Roitberg, Adrian E; Tretiak, Sergei

2014-04-15

To design functional photoactive materials for a variety of technological applications, researchers need to understand their electronic properties in detail and have ways to control their photoinduced pathways. When excited by photons of light, organic conjugated materials (OCMs) show dynamics that are often characterized by large nonadiabatic (NA) couplings between multiple excited states through a breakdown of the Born-Oppenheimer (BO) approximation. Following photoexcitation, various nonradiative intraband relaxation pathways can lead to a number of complex processes. Therefore, computational simulation of nonadiabatic molecular dynamics is an indispensable tool for understanding complex photoinduced processes such as internal conversion, energy transfer, charge separation, and spatial localization of excitons. Over the years, we have developed a nonadiabatic excited-state molecular dynamics (NA-ESMD) framework that efficiently and accurately describes photoinduced phenomena in extended conjugated molecular systems. We use the fewest-switches surface hopping (FSSH) algorithm to treat quantum transitions among multiple adiabatic excited state potential energy surfaces (PESs). Extended molecular systems often contain hundreds of atoms and involve large densities of excited states that participate in the photoinduced dynamics. We can achieve an accurate description of the multiple excited states using the configuration interaction single (CIS) formalism with a semiempirical model Hamiltonian. Analytical techniques allow the trajectory to be propagated "on the fly" using the complete set of NA coupling terms and remove computational bottlenecks in the evaluation of excited-state gradients and NA couplings. Furthermore, the use of state-specific gradients for propagation of nuclei on the native excited-state PES eliminates the need for simplifications such as the classical path approximation (CPA), which only uses ground-state gradients. Thus, the NA-ESMD methodology

Uncertainties of α-particle optical potential assessment around and below the Coulomb barrier

NASA Astrophysics Data System (ADS)

Avrigeanu, V.; Avrigeanu, M.; Mǎnǎilescu, C.

2017-06-01

A competition of the low-energy Coulomb excitation (CE) with the compound nucleus (CN) formation in α-induced reactions below the Coulomb barrier has recently been assumed in order to make possible the description of the latter as well as the α-particle emission by the same optical model (OM) potential. However, we show in the present work that the corresponding partial waves and integration radii provide evidence for the distinct account of the CE cross section and OM total-reaction cross section σR. Thus the largest contribution to CE cross section comes by far from partial waves larger than the ones contributing to the σR values. Finally, effects of statistical model parameters are comparatively discussed.

Thermality and excited state Rényi entropy in two-dimensional CFT

NASA Astrophysics Data System (ADS)

Lin, Feng-Li; Wang, Huajia; Zhang, Jia-ju

2016-11-01

We evaluate one-interval Rényi entropy and entanglement entropy for the excited states of two-dimensional conformal field theory (CFT) on a cylinder, and examine their differences from the ones for the thermal state. We assume the interval to be short so that we can use operator product expansion (OPE) of twist operators to calculate Rényi entropy in terms of sum of one-point functions of OPE blocks. We find that the entanglement entropy for highly excited state and thermal state behave the same way after appropriate identification of the conformal weight of the state with the temperature. However, there exists no such universal identification for the Rényi entropy in the short-interval expansion. Therefore, the highly excited state does not look thermal when comparing its Rényi entropy to the thermal state one. As the Rényi entropy captures the higher moments of the reduced density matrix but the entanglement entropy only the average, our results imply that the emergence of thermality depends on how refined we look into the entanglement structure of the underlying pure excited state.

Electronic excited states and relaxation dynamics in polymer heterojunction systems

NASA Astrophysics Data System (ADS)

Ramon, John Glenn Santos

The potential for using conducting polymers as the active material in optoelectronic devices has come to fruition in the past few years. Understanding the fundamental photophysics behind their operations points to the significant role played by the polymer interface in their performance. Current device architectures involve the use of bulk heterojunctions which intimately blend the donor and acceptor polymers to significantly increase not only their interfacial surface area but also the probability of exciton formation within the vicinity of the interface. In this dissertation, we detail the role played by the interface on the behavior and performance of bulk heterojunction systems. First, we explore the relation between the exciton binding energy to the band offset in determining device characteristics. As a general rule, when the exciton binding energy is greater than the band offset, the exciton remains the lowest energy excited state leading to efficient light-emitting properties. On the other hand, if the offset is greater than the binding energy, charge separation becomes favorable leading to better photovoltaic behavior. Here, we use a Wannier function, configuration interaction based approach to examine the essential excited states and predict the vibronic absorption and emission spectra of the PPV/BBL, TFB/F8BT and PFB/F8BT heterojunctions. Our results underscore the role of vibrational relaxation in the formation of charge-transfer states following photoexcitation. In addition, we look at the relaxation dynamics that occur upon photoexcitation. For this, we adopt the Marcus-Hush semiclassical method to account for lattice reorganization in the calculation of the interconversion rates in TFB/F8BT and PFB/F8BT. We find that, while a tightly bound charge-transfer state (exciplex) remains the lowest excited state, a regeneration pathway to the optically active lowest excitonic state in TFB/F8BT is possible via thermal repopulation from the exciplex. Finally

Exploring Photoinduced Excited State Evolution in Heterobimetallic Ru(II)-Co(III) Complexes.

PubMed

Kuhar, Korina; Fredin, Lisa A; Persson, Petter

2015-06-18

Quantum chemical calculations provide detailed theoretical information concerning key aspects of photoinduced electron and excitation transfer processes in supramolecular donor-acceptor systems, which are particularly relevant to fundamental charge separation in emerging molecular approaches for solar energy conversion. Here we use density functional theory (DFT) calculations to explore the excited state landscape of heterobimetallic Ru-Co systems with varying degrees of interaction between the two metal centers, unbound, weakly bound, and tightly bound systems. The interplay between structural and electronic factors involved in various excited state relaxation processes is examined through full optimizations of multiple charge/spin states of each of the investigated systems. Low-energy relaxed heterobimetallic states of energy transfer and excitation transfer character are characterized in terms of energy, structure, and electronic properties. These findings support the notion of efficient photoinduced charge separation from a Ru(II)-Co(III) ground state, via initial optical excitation of the Ru-center, to low-energy Ru(III)-Co(II) states. The strongly coupled system has significant involvement of the conjugated bridge, qualitatively distinguishing it from the other two weakly coupled systems. Finally, by constructing potential energy surfaces for the three systems where all charge/spin state combinations are projected onto relevant reaction coordinates, excited state decay pathways are explored.

Ground and excited states of CaSH through electron propagator calculations

NASA Astrophysics Data System (ADS)

Ortiz, J. V.

1990-05-01

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

Signature of nonadiabatic coupling in excited-state vibrational modes.

PubMed

Soler, Miguel A; Nelson, Tammie; Roitberg, Adrian E; Tretiak, Sergei; Fernandez-Alberti, Sebastian

2014-11-13

Using analytical excited-state gradients, vibrational normal modes have been calculated at the minimum of the electronic excited-state potential energy surfaces for a set of extended conjugated molecules with different coupling between them. Molecular model systems composed of units of polyphenylene ethynylene (PPE), polyphenylenevinylene (PPV), and naphthacene/pentacene (NP) have been considered. In all cases except the NP model, the influence of the nonadiabatic coupling on the excited-state equilibrium normal modes is revealed as a unique highest frequency adiabatic vibrational mode that overlaps with the coupling vector. This feature is removed by using a locally diabatic representation in which the effect of NA interaction is removed. Comparison of the original adiabatic modes with a set of vibrational modes computed in the locally diabatic representation demonstrates that the effect of nonadiabaticity is confined to only a few modes. This suggests that the nonadiabatic character of a molecular system may be detected spectroscopically by identifying these unique state-specific high frequency vibrational modes.

Thermodynamic Theory of Spherically Trapped Coulomb Clusters

NASA Astrophysics Data System (ADS)

Wrighton, Jeffrey; Dufty, James; Bonitz, Michael; K"{A}Hlert, Hanno

2009-11-01

The radial density profile of a finite number of identical charged particles confined in a harmonic trap is computed over a wide ranges of temperatures (Coulomb coupling) and particle numbers. At low temperatures these systems form a Coulomb crystal with spherical shell structure which has been observed in ultracold trapped ions and in dusty plasmas. The shell structure is readily reproduced in simulations. However, analytical theories which used a mean field approachfootnotetext[1]C. Henning et al., Phys. Rev. E 74, 056403 (2006) or a local density approximationfootnotetext[2]C. Henning et al., Phys. Rev. E 76, 036404 (2007) have, so far, only been able to reproduce the average density profile. Here we present an approach to Coulomb correlations based on the hypernetted chain approximation with additional bridge diagrams. It is demonstrated that this model reproduces the correct shell structure within a few percent and provides the basis for a thermodynamic theory of Coulomb clusters in the strongly coupled fluid state.footnotetext[3]J. Wrighton, J.W. Dufty, H. K"ahlert and M. Bonitz, J. Phys. A 42, 214052 (2009) and Phys. Rev. E (2009) (to be submitted)

Excited electronic states of the methyl radical. Ab initio molecular orbital study of geometries, excitation energies and vibronic spectra

NASA Astrophysics Data System (ADS)

Mebel, Alexander M.; Lin, Sheng-Hsien

1997-03-01

The geometries, vibrational frequencies and vertical and adiabatic excitation energies of the excited valence and Rydberg 3s, 3p, 3d, and 4s electronic states of CH 3 have been studied using ab initio molecular orbital multiconfigurational SCF (CASSCF), internally contracted multireference configuration interaction (MRCI) and equation-of-motion coupled cluster (EOM-CCSD) methods. The vibronic spectra are determined through the calculation of Franck-Condon factors. Close agreement between theory and experiment has been found for the excitation energies, vibrational frequencies and vibronic spectra. The adiabatic excitation energies of the Rydberg 3s B˜ 2A' 1 and 3p 2 2A″ 2 states are calculated to be 46435 and 60065 cm -1 compared to the experimental values of 46300 and 59972 cm -1, respectively. The valence 2A″ excited state of CH 3 has been found to have a pyramidal geometry within C s symmetry and to be adiabatically by 97 kcal/mol higher in energy than the ground state. The 2A″ state is predicted to be stable by 9 and 13 kcal/mol with respect to H 2 and H elimination.

On the Klein–Gordon oscillator subject to a Coulomb-type potential

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

Bakke, K., E-mail: kbakke@fisica.ufpb.br; Furtado, C., E-mail: furtado@fisica.ufpb.br

2015-04-15

By introducing the scalar potential as modification in the mass term of the Klein–Gordon equation, the influence of a Coulomb-type potential on the Klein–Gordon oscillator is investigated. Relativistic bound states solutions are achieved to both attractive and repulsive Coulomb-type potentials and the arising of a quantum effect characterized by the dependence of angular frequency of the Klein–Gordon oscillator on the quantum numbers of the system is shown. - Highlights: • Interaction between the Klein–Gordon oscillator and a modified mass term. • Relativistic bound states for both attractive and repulsive Coulomb-type potentials. • Dependence of the Klein–Gordon oscillator frequency on themore » quantum numbers. • Relativistic analogue of a position-dependent mass system.« less

Excited-state dynamics of acetylene excited to individual rotational level of the V04K01 subband

NASA Astrophysics Data System (ADS)

Makarov, Vladimir I.; Kochubei, Sergei A.; Khmelinskii, Igor V.

2006-01-01

Dynamics of the IR emission induced by excitation of the acetylene molecule using the (32Ka0,1,2,ÃAu1←41la1,X˜Σg+1) transition was investigated. The observed IR emission was assigned to transitions between the ground-state vibrational levels. Acetylene fluorescence quenching induced by external electric and magnetic fields acting upon the system prepared using the (34Ka1,ÃAu1←00la0,X˜Σg+1) excitation was also studied. External electric field creates an additional radiationless pathway to the ground-state levels, coupling levels of the ÃAu1 excited state to the quasiresonant levels of the X˜Σg+1 ground state. The level density of the ground state in the vicinity of the excited state is very high, thus the electric-field-induced transition is irreversible, with the rate constant described by the Fermi rule. Magnetic field alters the decay profile without changing the fluorescence quantum yield in collisionless conditions. IR emission from the CCH transient was detected, and was also affected by the external electric and magnetic fields. Acetylene predissociation was demonstrated to proceed by the direct S1→S0 mechanism. The results were explained using the previously developed theoretical approach, yielding values of the relevant model parameters.

Spectroscopic properties of the S1 state of linear carotenoids after excess energy excitation

NASA Astrophysics Data System (ADS)

Kuznetsova, Valentyna; Southall, June; Cogdell, Richard J.; Fuciman, Marcel; Polívka, Tomáš

2017-09-01

Properties of the S1 state of neurosporene, spheroidene and lycopene were studied after excess energy excitation in the S2 state. Excitation of carotenoids into higher vibronic levels of the S2 state generates excess vibrational energy in the S1 state. The vibrationally hot S1 state relaxes faster when carotenoid is excited into the S2 state with excess energy, but the S1 lifetime remains constant regardless of which vibronic level of the S2 state is excited. The S∗ signal depends on excitation energy only for spheroidene, which is likely due to asymmetry of the molecule, facilitating conformations responsible for the S∗ signal.

Population trapping in the excited states using vacuum-induced coherence and adiabatic process

NASA Astrophysics Data System (ADS)

Lal Kumawat, Babu; Kumar, Pardeep; Dasgupta, Shubhrangshu

2018-02-01

We theoretically investigate how population can be trapped in the closely spaced excited levels in presence of vacuum-induced coherence (VIC). We employ delayed pulses to transfer population from a meta-stable state to the excited states. Subsequently, spontaneous emission from these excited states builds coherence between them. This coherence can be probed by using chirping, which leads to the decoupling of the excited states from the ground state thereby ensuring population transfer via delayed pulses. Our results indicate that the existence of VIC leads to the generation of a mixed state in the excited state manifold, where trapping of the population occurs even in the presence of large decay. This trapping may be realized in molecular systems and can be interpreted as a sensitive probe of VIC. We present suitable numerical analysis to support our results.

Minimal excitation states for heat transport in driven quantum Hall systems

NASA Astrophysics Data System (ADS)

Vannucci, Luca; Ronetti, Flavio; Rech, Jérôme; Ferraro, Dario; Jonckheere, Thibaut; Martin, Thierry; Sassetti, Maura

2017-06-01

We investigate minimal excitation states for heat transport into a fractional quantum Hall system driven out of equilibrium by means of time-periodic voltage pulses. A quantum point contact allows for tunneling of fractional quasiparticles between opposite edge states, thus acting as a beam splitter in the framework of the electron quantum optics. Excitations are then studied through heat and mixed noise generated by the random partitioning at the barrier. It is shown that levitons, the single-particle excitations of a filled Fermi sea recently observed in experiments, represent the cleanest states for heat transport since excess heat and mixed shot noise both vanish only when Lorentzian voltage pulses carrying integer electric charge are applied to the conductor. This happens in the integer quantum Hall regime and for Laughlin fractional states as well, with no influence of fractional physics on the conditions for clean energy pulses. In addition, we demonstrate the robustness of such excitations to the overlap of Lorentzian wave packets. Even though mixed and heat noise have nonlinear dependence on the voltage bias, and despite the noninteger power-law behavior arising from the fractional quantum Hall physics, an arbitrary superposition of levitons always generates minimal excitation states.

Electron-driven excitation of O 2 under night-time auroral conditions: Excited state densities and band emissions

NASA Astrophysics Data System (ADS)

Jones, D. B.; Campbell, L.; Bottema, M. J.; Teubner, P. J. O.; Cartwright, D. C.; Newell, W. R.; Brunger, M. J.

2006-01-01

Electron impact excitation of vibrational levels in the ground electronic state and seven excited electronic states in O 2 have been simulated for an International Brightness Coefficient-Category 2+ (IBC II+) night-time aurora, in order to predict O 2 excited state number densities and volume emission rates (VERs). These number densities and VERs are determined as a function of altitude (in the range 80-350 km) in the present study. Recent electron impact excitation cross-sections for O 2 were combined with appropriate altitude dependent IBC II+ auroral secondary electron distributions and the vibrational populations of the eight O 2 electronic states were determined under conditions of statistical equilibrium. Pre-dissociation, atmospheric chemistry involving atomic and molecular oxygen, radiative decay and quenching of excited states were included in this study. This model predicts relatively high number densities for the X3Σg-(v'⩽4),a1Δandb1Σg+ metastable electronic states and could represent a significant source of stored energy in O 2* for subsequent thermospheric chemical reactions. Particular attention is directed towards the emission intensities of the infrared (IR) atmospheric (1.27 μm), Atmospheric (0.76 μm) and the atomic oxygen 1S→ 1D transition (5577 Å) lines and the role of electron-driven processes in their origin. Aircraft, rocket and satellite observations have shown both the IR atmospheric and Atmospheric lines are dramatically enhanced under auroral conditions and, where possible, we compare our results to these measurements. Our calculated 5577 Å intensity is found to be in good agreement with values independently measured for a medium strength IBC II+ aurora.

Identification of Excited States in the N=Z Nucleus 82Nb

NASA Astrophysics Data System (ADS)

Caceres, L. S.; Gorska, M.; Jungclaus, A.; Regan, P. H.; Garnsworthy, A. B.; Pietri, S.; Podolyak, Zs.; Rudolph, D.; Steer, S. J.; Grawe, H.; Balabanski, D. L.; Becker, F.; Bednarczyk, P.; Benzoni, G.; Blank, B.; Brandau, C.; Bruce, A. M.; Camera, F.; Catford, W. N.; Cullen, I. J.; Dombradi, Zs.; Doornenbal, P.; Estevez, E.; Geissel, H.; Gelletly, W.; Gerl, J.; Grebosz, J.; Heinz, A.; Hoischen, R.; Ilie, G.; Jolie, J.; Jones, G. A.; Kmiecik, M.; Kojouharov, I.; Kondev, F. G.; Kurtukian-Nieto, T.; Kurz, N.; Lalkowski, S.; Liu, L.; Maj, A.; Myalski, S.; Montes, F.; Pfuetzner, M.; Prokopowicz, W.; Saito, T.; Schaffner, H.; Schwertel, S.; Shizuma, T.; Simons, A. J.; Tashenov, S.; Walker, P. M.; Werner-Malento, E.; Wieland, O.; Wollersheim, H. J.

2007-04-01

Information on the first excited states in the N=Z=41 nucleus 82Nb sheds light on the competition of isospin T=0 and T=1 states in the A sim 80 region. The measurement was performed at the GSI laboratory using fragmentation of a 107Ag primary beam at 750 MeV/u on a 4 g/cm2 9Be target. The fragments were separated and identified unambiguously in the FRagment Separator. Three excited states were observed and the half-life estimate for the isomeric state was extracted. A tentative spin assignment based on the isobaric analogue states systematics in the Tz=1 nucleus 82Zr, and transition probabilities indicate T=1 character of the first two excited states, and T=0 for the isomeric state.

Dynamics and Steady States in Excitable Mobile Agent Systems

NASA Astrophysics Data System (ADS)

Peruani, Fernando; Sibona, Gustavo J.

2008-04-01

We study the spreading of excitations in 2D systems of mobile agents where the excitation is transmitted when a quiescent agent keeps contact with an excited one during a nonvanishing time. We show that the steady states strongly depend on the spatial agent dynamics. Moreover, the coupling between exposition time (ω) and agent-agent contact rate (CR) becomes crucial to understand the excitation dynamics, which exhibits three regimes with CR: no excitation for low CR, an excited regime in which the number of quiescent agents (S) is inversely proportional to CR, and, for high CR, a novel third regime, model dependent, where S scales with an exponent ξ-1, with ξ being the scaling exponent of ω with CR.

Sideband cooling of small ion Coulomb crystals in a Penning trap

NASA Astrophysics Data System (ADS)

Stutter, G.; Hrmo, P.; Jarlaud, V.; Joshi, M. K.; Goodwin, J. F.; Thompson, R. C.

2018-03-01

We have recently demonstrated the laser cooling of a single ? ion to the motional ground state in a Penning trap using the resolved-sideband cooling technique on the electric quadrupole transition S? D?. Here we report on the extension of this technique to small ion Coulomb crystals made of two or three ? ions. Efficient cooling of the axial motion is achieved outside the Lamb-Dicke regime on a two-ion string along the magnetic field axis as well as on two- and three-ion planar crystals. Complex sideband cooling sequences are required in order to cool both axial degrees of freedom simultaneously. We measure a mean excitation after cooling of ? for the centre of mass (COM) mode and ? for the breathing mode of the two-ion string with corresponding heating rates of 11(2) ? and ? at a trap frequency of 162 kHz. The occupation of the ground state of the axial modes (?) is above 75% for the two-ion planar crystal and the associated heating rates 0.8(5) ? at a trap frequency of 355 kHz.

Investigating Coulomb's Law.

ERIC Educational Resources Information Center

Noll, Ellis; Koehlinger, Mervin; Kowalski, Ludwik; Swackhamer, Gregg

1998-01-01

Describes the use of a computer-linked camera to demonstrate Coulomb's law. Suggests a way of reducing the difficulties in presenting Coulomb's law by teaching the inverse square law of gravity and the inverse square law of electricity in the same unit. (AIM)

Coulomb-coupled quantum-dot thermal transistors

NASA Astrophysics Data System (ADS)

Zhang, Yanchao; Yang, Zhimin; Zhang, Xin; Lin, Bihong; Lin, Guoxing; Chen, Jincan

2018-04-01

A quantum-dot thermal transistor consisting of three Coulomb-coupled quantum dots coupled to the respective electronic reservoirs by tunnel contacts is established. The heat flows through the collector and emitter can be controlled by the temperature of the base. It is found that a small change in the base heat flow can induce a large heat flow change in the collector and emitter. The huge amplification factor can be obtained by optimizing the Coulomb interaction between the collector and the emitter or by decreasing the tunneling rate at the base. The proposed quantum-dot thermal transistor may open up potential applications in low-temperature solid-state thermal circuits at the nanoscale.

Coulomb energy of uniformly charged spheroidal shell systems.

PubMed

Jadhao, Vikram; Yao, Zhenwei; Thomas, Creighton K; de la Cruz, Monica Olvera

2015-03-01

We provide exact expressions for the electrostatic energy of uniformly charged prolate and oblate spheroidal shells. We find that uniformly charged prolate spheroids of eccentricity greater than 0.9 have lower Coulomb energy than a sphere of the same area. For the volume-constrained case, we find that a sphere has the highest Coulomb energy among all spheroidal shells. Further, we derive the change in the Coulomb energy of a uniformly charged shell due to small, area-conserving perturbations on the spherical shape. Our perturbation calculations show that buckling-type deformations on a sphere can lower the Coulomb energy. Finally, we consider the possibility of counterion condensation on the spheroidal shell surface. We employ a Manning-Oosawa two-state model approximation to evaluate the renormalized charge and analyze the behavior of the equilibrium free energy as a function of the shell's aspect ratio for both area-constrained and volume-constrained cases. Counterion condensation is seen to favor the formation of spheroidal structures over a sphere of equal area for high values of shell volume fractions.

Efficient evaluation of the Coulomb force in the Gaussian and finite-element Coulomb method.

PubMed

Kurashige, Yuki; Nakajima, Takahito; Sato, Takeshi; Hirao, Kimihiko

2010-06-28

We propose an efficient method for evaluating the Coulomb force in the Gaussian and finite-element Coulomb (GFC) method, which is a linear-scaling approach for evaluating the Coulomb matrix and energy in large molecular systems. The efficient evaluation of the analytical gradient in the GFC is not straightforward as well as the evaluation of the energy because the SCF procedure with the Coulomb matrix does not give a variational solution for the Coulomb energy. Thus, an efficient approximate method is alternatively proposed, in which the Coulomb potential is expanded in the Gaussian and finite-element auxiliary functions as done in the GFC. To minimize the error in the gradient not just in the energy, the derived functions of the original auxiliary functions of the GFC are used additionally for the evaluation of the Coulomb gradient. In fact, the use of the derived functions significantly improves the accuracy of this approach. Although these additional auxiliary functions enlarge the size of the discretized Poisson equation and thereby increase the computational cost, it maintains the near linear scaling as the GFC and does not affects the overall efficiency of the GFC approach.

Diffusion in Coulomb crystals.

PubMed

Hughto, J; Schneider, A S; Horowitz, C J; Berry, D K

2011-07-01

Diffusion in Coulomb crystals can be important for the structure of neutron star crusts. We determine diffusion constants D from molecular dynamics simulations. We find that D for Coulomb crystals with relatively soft-core 1/r interactions may be larger than D for Lennard-Jones or other solids with harder-core interactions. Diffusion, for simulations of nearly perfect body-centered-cubic lattices, involves the exchange of ions in ringlike configurations. Here ions "hop" in unison without the formation of long lived vacancies. Diffusion, for imperfect crystals, involves the motion of defects. Finally, we find that diffusion, for an amorphous system rapidly quenched from Coulomb parameter Γ=175 to Coulomb parameters up to Γ=1750, is fast enough that the system starts to crystalize during long simulation runs. These results strongly suggest that Coulomb solids in cold white dwarf stars, and the crust of neutron stars, will be crystalline and not amorphous.

Correlated scattering states of N-body Coulomb systems

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

Berakdar, J.

1997-03-01

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

Non-extensive entropy and properties of polaron in RbCl delta quantum dot under an applied electric field and Coulombic impurity

NASA Astrophysics Data System (ADS)

Tiotsop, M.; Fotue, A. J.; Fotsin, H. B.; Fai, L. C.

2017-08-01

Bound polaron in RbCl delta quantum dot under electric field and Coulombic impurity were considered. The ground and first excited state energy were derived by employing Pekar variational and unitary transformation methods. Applying Fermi golden rule, the expression of temperature and polaron lifetime were derived. The decoherence was studied trough the Tsallis entropy. Results shows that decreasing (or increasing) the lifetime increases (or decreases) the temperature and delta parameter (electric field strength and hydrogenic impurity). This suggests that to accelerate quantum transition in nanostructure, temperature and delta have to be enhanced. The improvement of electric field and coulomb parameter, increases the lifetime of the delta quantum dot qubit. Energy spectrum of polaron increases with increase in temperature, electric field strength, Coulomb parameter, delta parameter, and polaronic radius. The control of the delta quantum dot energies can be done via the electric field, coulomb impurity, and delta parameter. Results also show that the non-extensive entropy is an oscillatory function of time. With the enhancement of delta parameter, non-extensive parameter, Coulombic parameter, and electric field strength, the entropy has a sinusoidal increase behavior with time. With the study of decoherence through the Tsallis entropy, it may be advised that to have a quantum system with efficient transmission of information, the non-extensive and delta parameters need to be significant. The study of the probability density showed an increase from the boundary to the center of the dot where it has its maximum value and oscillates with period T0 = ℏ / ΔE with the tunneling of the delta parameter, electric field strength, and Coulombic parameter. The results may be very helpful in the transmission of information in nanostructures and control of decoherence

Mobile bound states of Rydberg excitations in a lattice

NASA Astrophysics Data System (ADS)

Letscher, Fabian; Petrosyan, David

2018-04-01

Spin-lattice models play a central role in the studies of quantum magnetism and nonequilibrium dynamics of spin excitations—-magnons. We show that a spin lattice with strong nearest-neighbor interactions and tunable long-range hopping of excitations can be realized by a regular array of laser-driven atoms, with an excited Rydberg state representing the spin-up state and a Rydberg-dressed ground state corresponding to the spin-down state. We find exotic interaction-bound states of magnons that propagate in the lattice via the combination of resonant two-site hopping and nonresonant second-order hopping processes. Arrays of trapped Rydberg-dressed atoms can thus serve as a flexible platform to simulate and study fundamental few-body dynamics in spin lattices.

Electronic and Structural Properties of ABO3: Role of the B-O Coulomb Repulsions for Ferroelectricity

PubMed Central

Miura, Kaoru; Azuma, Masaki; Funakubo, Hiroshi

2011-01-01

We have investigated the role of the Ti–O Coulomb repulsions in the appearance of the ferroelectric state in BaTiO3 as well as the role of the Zn–O Coulomb repulsions in BiZn0.5Ti0.5O3, using a first-principles calculation with optimized structures. In tetragonal BaTiO3, it is found that the Coulomb repulsions between Ti 3s and 3p states and O 2s and 2p states have an important role for the appearance of Ti ion displacement. In BiZn0.5Ti0.5O3, on the other hand, the stronger Zn–O Coulomb repulsions, which are due to the 3s, 3p, and 3d (d10) states of the Zn ion, have more important role than the Ti–O Coulomb repulsions for the appearance of the tetragonal structure. Our suggestion is consistent with the other ferroelectric perovskite oxides ABO3 in the appearance of tetragonal structures as well as rhombohedral structures. PMID:28879987

Electronic and Structural Properties of ABO3: Role of the B-O Coulomb Repulsions for Ferroelectricity.

PubMed

Miura, Kaoru; Azuma, Masaki; Funakubo, Hiroshi

2011-01-17

We have investigated the role of the Ti-O Coulomb repulsions in the appearance of the ferroelectric state in BaTiO3 as well as the role of the Zn-O Coulomb repulsions in BiZn0.5Ti0.5O3, using a first-principles calculation with optimized structures. In tetragonal BaTiO3, it is found that the Coulomb repulsions between Ti 3s and 3p states and O 2s and 2p states have an important role for the appearance of Ti ion displacement. In BiZn0.5Ti0.5O3, on the other hand, the stronger Zn-O Coulomb repulsions, which are due to the 3s, 3p, and 3d (d10) states of the Zn ion, have more important role than the Ti-O Coulomb repulsions for the appearance of the tetragonal structure. Our suggestion is consistent with the other ferroelectric perovskite oxides ABO3 in the appearance of tetragonal structures as well as rhombohedral structures.

Universal monopole scaling near transitions from the Coulomb phase.

PubMed

Powell, Stephen

2012-08-10

Certain frustrated systems, including spin ice and dimer models, exhibit a Coulomb phase at low temperatures, with power-law correlations and fractionalized monopole excitations. Transitions out of this phase, at which the effective gauge theory becomes confining, provide examples of unconventional criticality. This Letter studies the behavior at nonzero monopole density near such transitions, using scaling theory to arrive at universal expressions for the crossover phenomena. For a particular transition in spin ice, quantitative predictions are made by mapping to the XY model and confirmed using Monte Carlo simulations.

Ultrafast Excited-State Dynamics of Cytosine Aza-Derivative and Analogues.

PubMed

Zhou, Zhongneng; Zhou, Xueyao; Wang, Xueli; Jiang, Bin; Li, Yongle; Chen, Jinquan; Xu, Jianhua

2017-04-13

Excited state dynamics of 5-azacytosine (5-AC), 2,4-diamino-1,3,5-triazine (2,4-DT), and 2-amino-1,3,5-triazine (2-AT) were comprehensively investigated by steady state absorption, fluorescence, and femtosecond transient absorption measurements. Time-dependent density functional theory (TDDFT) calculations were performed to help assign the absorption bands and understand the excited state decay mechanisms. The experimental results of excited singlet state dynamics for 5-AC, 2,4-DT, and 2-AT with femtosecond time resolution were reported for the first time. Two distinct decay pathways, with ∼1 ps and tens of picosecond lifetimes, were observed in 5-AC. Only one decay pathway with 17 ps lifetime was observed in 2,4-DT while an emissive state was found in 2-AT. TDDFT calculations suggest that 5-AC has a dark nπ* (S 1 ) state below the first allowed ππ* (S 2 ) state, which leads to the ultrafast decay of the ππ* state. In 2,4-DT, there is no dark nπ* state below the bright ππ* (S 1 ) state and the 17 ps lifetime is assigned to the relaxation from the ππ* (S 1 ) state to ground state. Two dark nπ* states (S 1 and S 2 ) were found in 2-AT, which exhibits much more complex excited state dynamics compared with the other two. Photoluminescence in 2-AT has been confirmed to be fluorescence emission from its bright ππ* (S 3 ) state. Our results strongly suggest that electronic structures are very sensitive to the substitution on the triazine ring and that the photophysical properties of nucleic acid analogues depend highly on their molecular structures.

The Coulomb based magneto-electric coupling in multiferroic tunnel junctions and granular multiferroics

NASA Astrophysics Data System (ADS)

Udalov, O. G.; Beloborodov, I. S.

2018-05-01

We study magneto-electric effect in two systems: i) multiferroic tunnel junction (MFTJ) - magnetic tunnel junction with ferroelectric barrier and ii) granular multiferroic (GMF) in which ferromagnetic (FM) metallic grains embedded into ferroelectric matrix. We show that the Coulomb interaction influences the magnetic state of the system in several ways: i) through the spin-dependent part of the Coulomb interaction; ii) due to the Coulomb blockade effect suppressing electron hopping and therefore reducing magnetic coupling; and iii) through image forces and polarization screening that modify the barrier for electrons in MFTJ and GMF. We show that in the absence of spin-orbit or strain-mediated coupling magneto-electric effect appears in GMF and MFTJ. The Coulomb interaction depends on the dielectric properties of the system. For GMF it depends on the dielectric constant of FE matrix and for MFTJ on the dielectric constant of the FE barrier. Applying external electric field one can tune the dielectric constant and the Coulomb interaction. Thus, one can control magnetic state with electric field.

Ultrafast excited-state dynamics of RNA and DNA C tracts

NASA Astrophysics Data System (ADS)

Cohen, Boiko; Larson, Matthew H.; Kohler, Bern

2008-06-01

The excited-state dynamics of the RNA homopolymer of cytosine and of the 18-mer (dC) 18 were studied by steady-state and time-resolved absorption and emission spectroscopy. At pH 6.8, excitation of poly(rC) by a femtosecond UV pump pulse produces excited states that decay up to one order of magnitude more slowly than the excited states formed in the mononucleotide cytidine 5'-monophosphate under the same conditions. Even slower relaxation is observed for the hemiprotonated, self-associated form of poly(rC), which is stable at acidic pH. Transient absorption and time-resolved fluorescence signals for (dC) 18 at pH 6.8 are similar to ones observed for poly(rC) near pH 4, indicating that hemiprotonated structures are found in DNA C tracts at neutral pH. In both systems, there is evidence for two kinds of emitting states with lifetimes of ˜100 ps and slightly more than 1 ns. The former states are responsible for the bulk of emission from the hemiprotonated structures. Evidence suggests that slow electronic relaxation in these self-complexes is the result of vertical base stacking. The similar signals from RNA and DNA C tracts suggest a common base-stacked structure, which may be identical with that of i-motif DNA.

Multiparticle configurations of excited states in 155Lu

NASA Astrophysics Data System (ADS)

Carroll, R. J.; Hadinia, B.; Qi, C.; Joss, D. T.; Page, R. D.; Uusitalo, J.; Andgren, K.; Cederwall, B.; Darby, I. G.; Eeckhaudt, S.; Grahn, T.; Gray-Jones, C.; Greenlees, P. T.; Jones, P. M.; Julin, R.; Juutinen, S.; Leino, M.; Leppänen, A.-P.; Nyman, M.; Pakarinen, J.; Rahkila, P.; Sandzelius, M.; Sarén, J.; Scholey, C.; Seweryniak, D.; Simpson, J.

2016-12-01

Excited states in the neutron-deficient N =84 nuclide 155Lu have been populated by using the 102Pd(58Ni,α p ) reaction. The 155Lu nuclei were separated by using the gas-filled recoil ion transport unit (RITU) separator and implanted into the Si detectors of the gamma recoil electron alpha tagging (GREAT) spectrometer. Prompt γ -ray emissions measured at the target position using the JUROGAM Ge detector array were assigned to 155Lu through correlations with α decays measured in GREAT. Structures feeding the (11 /2-) and (25 /2-)α -decaying states have been revised and extended. Shell-model calculations have been performed and are found to reproduce the excitation energies of several of the low-lying states observed to within an average of 71 keV. In particular, the seniority inversion of the 25 /2- and 27 /2- states is reproduced.

Excited State Trends in Bidirectionally Expanded Closed-Shell PAH and PANH Anions

PubMed Central

Moore, Megan M.; Lee, Timothy J.

2018-01-01

Some anions are known to exhibit excited states independent of external forces such as dipole moments and induced polarizabilities. Such states exist simply as a result of the stabilization of valence accepting orbitals whereby the binding energy of the extra electron is greater than the valence excitation energy. Closed-shell anions are interesting candidates for such transitions since their ground-state, spin-paired nature makes the anions more stable from the beginning. Consequently, this work shows the point beyond which deprotonated, closed-shell polycyclic aromatic hydrocarbons (PAHs) and those PAHs containing nitrogen heteroatoms (PANHs) will exhibit valence excited states. This behavior has already been demonstrated in some PANHs and for anistropically-extended PAHs. This work establishes a general trend for PAHs/PANHs of arbitrary size and directional extension, whether in one dimension or two. Once seven six-membered rings make up a PAH/PANH, valence excited states are present. For most classes of PAHs/PANHs, this number is closer to four. Even though most of these excited states are weak absorbers, the sheer number of PAHs present in various astronomical environments should make them significant contributors to astronomical spectra. PMID:27585793

Rotational excitation of the Hoyle state in 12C

NASA Astrophysics Data System (ADS)

Garg, R.; Barton, C.; Diget, C. Aa; Courtin, S.; Fruet, G.; Fynbo, H. O. U.; Howard, A.; Illana, A.; Jenkins, D. G.; Marroquin, I.; Kirsebom, O. S.; Lund, M. V.; Moore, I.; Perea, A.; Refsgaard, J.; Riley, J. E.; Rinta-Antila, S.; Sinclair, L.; Tengblad, O.; IGISOL Collaboration

2018-01-01

12C is synthesised in stars by fusion of three α particles. This process occurs through a resonance in the 12C nucleus, famously known as the Hoyle state. In this state, the 12C nucleus exists as a cluster of α particles. The state is the band-head for a rotational band with the 2+ rotational excitation predicted in the energy region 9 - 11 MeV. This rotational excitation can affect the triple-α process reaction rate by more than an order of magnitude at high temperatures (109 K). Depending on the energy of the resonance, the knowledge of the state can also help determine the structure of the Hoyle state. In the work presented here, the state of interest is populated by beta decay of radioactive 12N ion beam delivered by the IGISOL facility at JYFL, Jyväskylä.

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.

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

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

Egidi, Franco, E-mail: franco.egidi@sns.it; Segado, Mireia; Barone, Vincenzo, E-mail: vincenzo.barone@sns.it

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.

Excitation on the Coherent States of Pseudoharmonic Oscillator

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

Popov, Dusan; Pop, Nicolina; Sajfert, Vjekoslav

In the last decades, much attention has been paid to the excitation on coherent states, especially for coherent states of the harmonic oscillator ([1] and references therein). But an interesting anharmonic oscillator with many potential applications is also the pseudoharmonic oscillator (PHO). So, in the present paper we have defined the excitation on the Klauder-Perelomov coherent states (E-KP-CSs) for the PHO. These states are obtained by repeatedly operating the raising operator K{sub +} on a usual Klauder-Perelomov coherent state (KP-CS) of the PHO [2]. We have verified that really, the E-KP-CSs fulfill all the properties of the coherent states, asmore » stated by Klauder [3]. We have examined the nonclassical properties of the E-KP-CSs, by using the density matrix formalism and examining the dependence of the Mandel parameter Q{sub z,k;m}(|z|{sup 2}) on the |z|{sup 2} and on the m. It seems that these states can be used in optical communication field and in the physics of quantum information, as signal beams, due to the fact that in these fields the nonclassicality plays an important role.« less

The properties of 4'-N,N-dimethylaminoflavonol in the ground and excited states

NASA Astrophysics Data System (ADS)

Moroz, V. V.; Chalyi, A. G.; Roshal, A. D.

2008-09-01

The mechanism of protonation of 4-N,N-dimethylaminoflavonol and the structure of its protolytic forms in the ground and excited states were studied by electron absorption and fluorescence (steady-state and time-resolved) spectroscopy and with the use of the RM1 quantum-chemical method. A comparison of equilibrium constants and the theoretical enthalpies of formation showed that excitation should be accompanied by the inversion of the basicity of the electron acceptor groups of this compound and, as a consequence, changes in the structure of its monocationic form. An analysis of the spectral parameters of the protolytic 4-N,N-dimethylaminoflavonol forms, however, showed that their structure and the sequence of protonation in the excited state were the same as in the ground state. Changes in the structure of the monocation in the excited state were not observed because of the fast radiationless deactivation of this form and the occurrence of excited state intramolecular proton transfer in aprotic solvents.

Elastic Coulomb breakup of 34Na

NASA Astrophysics Data System (ADS)

Singh, G.; Shubhchintak, Chatterjee, R.

2016-08-01

Background: 34Na is conjectured to play an important role in the production of seed nuclei in the alternate r -process paths involving light neutron rich nuclei very near the β -stability line, and as such, it is important to know its ground state properties and structure to calculate rates of the reactions it might be involved in, in the stellar plasma. Found in the region of `island of inversion', its ground state might not be in agreement with normal shell model predictions. Purpose: The aim of this paper is to study the elastic Coulomb breakup of 34Na on 208Pb to give us a core of 33Na with a neutron and in the process we try and investigate the one neutron separation energy and the ground state configuration of 34Na. Method: A fully quantum mechanical Coulomb breakup theory within the architecture of post-form finite range distorted wave Born approximation extended to include the effects of deformation is used to research the elastic Coulomb breakup of 34Na on 208Pb at 100 MeV/u. The triple differential cross section calculated for the breakup is integrated over the desired components to find the total cross-section, momentum, and angular distributions as well as the average momenta, along with the energy-angular distributions. Results: The total one neutron removal cross section is calculated to test the possible ground state configurations of 34Na. The average momentum results along with energy-angular calculations indicate 34Na to have a halo structure. The parallel momentum distributions with narrow full widths at half-maxima signify the same. Conclusion: We have attempted to analyze the possible ground state configurations of 34Na and in congruity with the patterns in the `island of inversion' conclude that even without deformation, 34Na should be a neutron halo with a predominant contribution to its ground state most probably coming from 33Na(3 /2+)⊗ 2 p3 /2ν configuration. We also surmise that it would certainly be useful and rewarding to test our

Theory of superconductivity and spin excitations in cuprates

NASA Astrophysics Data System (ADS)

Plakida, Nikolay M.

2018-06-01

A microscopic theory of high-temperature superconductivity in strongly correlated systems as cuprates is presented. The two-subband extended Hubbard model is considered where the intersite Coulomb repulsion and electron-phonon interaction are taken into account. The low-energy spin excitations are considered within the t-J model.

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

PubMed

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

2009-02-07

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

Stability of quantum-dot excited-state laser emission under simultaneous ground-state perturbation

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

Kaptan, Y., E-mail: yuecel.kaptan@physik.tu-berlin.de; Herzog, B.; Schöps, O.

2014-11-10

The impact of ground state amplification on the laser emission of In(Ga)As quantum dot excited state lasers is studied in time-resolved experiments. We find that a depopulation of the quantum dot ground state is followed by a drop in excited state lasing intensity. The magnitude of the drop is strongly dependent on the wavelength of the depletion pulse and the applied injection current. Numerical simulations based on laser rate equations reproduce the experimental results and explain the wavelength dependence by the different dynamics in lasing and non-lasing sub-ensembles within the inhomogeneously broadened quantum dots. At high injection levels, the observedmore » response even upon perturbation of the lasing sub-ensemble is small and followed by a fast recovery, thus supporting the capacity of fast modulation in dual-state devices.« less

Spectroscopic Diagnosis of Excited-State Aromaticity: Capturing Electronic Structures and Conformations upon Aromaticity Reversal.

PubMed

Oh, Juwon; Sung, Young Mo; Hong, Yongseok; Kim, Dongho

2018-03-06

Aromaticity, the special energetic stability derived from cyclic [4 n + 2]π-conjugated electronic structures, has been the topic of intense interest in chemistry because it plays a critical role in rationalizing molecular stability, reactivity, and physical/chemical properties. Recently, the pioneering work by Colin Baird on aromaticity reversal, postulating that aromatic (antiaromatic) character in the ground state reverses to antiaromatic (aromatic) character in the lowest excited triplet state, has attracted much scientific attention. The completely reversed aromaticity in the excited state provides direct insight into understanding the photophysical/chemical properties of photoactive materials. In turn, the application of aromatic molecules to photoactive materials has led to numerous studies revealing this aromaticity reversal. However, most studies of excited-state aromaticity have been based on the theoretical point of view. The experimental evaluation of aromaticity in the excited state is still challenging and strenuous because the assessment of (anti)aromaticity with conventional magnetic, energetic, and geometric indices is difficult in the excited state, which practically restricts the extension and application of the concept of excited-state aromaticity. Time-resolved optical spectroscopies can provide a new and alternative avenue to evaluate excited-state aromaticity experimentally while observing changes in the molecular features in the excited states. Time-resolved optical spectroscopies take advantage of ultrafast laser pulses to achieve high time resolution, making them suitable for monitoring ultrafast changes in the excited states of molecular systems. This can provide valuable information for understanding the aromaticity reversal. This Account presents recent breakthroughs in the experimental assessment of excited-state aromaticity and the verification of aromaticity reversal with time-resolved optical spectroscopic measurements. To

Deciphering excited state evolution in halorhodopsin with stimulated emission pumping.

PubMed

Bismuth, Oshrat; Komm, Pavel; Friedman, Noga; Eliash, Tamar; Sheves, Mordechai; Ruhman, Sanford

2010-03-04

The primary photochemical dynamics of Hb. pharaonis Halorhodopsin (pHR) are investigated by femtosecond visible pump-near IR dump-hyperspectral probe spectroscopy. The efficiency of excited state depletion is deduced from transient changes in absorption, recorded with and without stimulated emission pumping (SEP), as a function of the dump delay. The concomitant reduction of photocycle population is assessed by probing the "K" intermediate difference spectrum. Results show that the cross section for stimulating emission is nearly constant throughout the fluorescent state lifetime. Probing "K" demonstrates that dumping produces a proportionate reduction in photocycle yields. We conclude that, despite its nonexponential internal conversion (IC) kinetics, the fluorescent state in pHR constitutes a single intermediate in the photocycle. This contrasts with conclusions drawn from the study of primary events in the related chloride pump from Hb. salinarum (sHR), believed to produce the "K" intermediate from a distinct short-lived subpopulation in the excited state. Our discoveries concerning internal conversion dynamics in pHR are discussed in light of recent expectations for similar excited state dynamics in both proteins.

Energy Dispersive XAFS: Characterization of Electronically Excited States of Copper(I) Complexes

PubMed Central

2013-01-01

Energy dispersive X-ray absorption spectroscopy (ED-XAS), in which the whole XAS spectrum is acquired simultaneously, has been applied to reduce the real-time for acquisition of spectra of photoinduced excited states by using a germanium microstrip detector gated around one X-ray bunch of the ESRF (100 ps). Cu K-edge XAS was used to investigate the MLCT states of [Cu(dmp)2]+ (dmp =2,9-dimethyl-1,10-phenanthroline) and [Cu(dbtmp)2]+ (dbtmp =2,9-di-n-butyl-3,4,7,8-tetramethyl-1,10-phenanthroline) with the excited states created by excitation at 450 nm (10 Hz). The decay of the longer lived complex with bulky ligands, was monitored for up to 100 ns. DFT calculations of the longer lived MLCT excited state of [Cu(dbp)2]+ (dbp =2,9-di-n-butyl-1,10-phenanthroline) with the bulkier diimine ligands, indicated that the excited state behaves as a Jahn–Teller distorted Cu(II) site, with the interligand dihedral angle changing from 83 to 60° as the tetrahedral coordination geometry flattens and a reduction in the Cu–N distance of 0.03 Å. PMID:23718738

Energy-Looping Nanoparticles: Harnessing Excited-State Absorption for Deep-Tissue Imaging.

PubMed

Levy, Elizabeth S; Tajon, Cheryl A; Bischof, Thomas S; Iafrati, Jillian; Fernandez-Bravo, Angel; Garfield, David J; Chamanzar, Maysamreza; Maharbiz, Michel M; Sohal, Vikaas S; Schuck, P James; Cohen, Bruce E; Chan, Emory M

2016-09-27

Near infrared (NIR) microscopy enables noninvasive imaging in tissue, particularly in the NIR-II spectral range (1000-1400 nm) where attenuation due to tissue scattering and absorption is minimized. Lanthanide-doped upconverting nanocrystals are promising deep-tissue imaging probes due to their photostable emission in the visible and NIR, but these materials are not efficiently excited at NIR-II wavelengths due to the dearth of lanthanide ground-state absorption transitions in this window. Here, we develop a class of lanthanide-doped imaging probes that harness an energy-looping mechanism that facilitates excitation at NIR-II wavelengths, such as 1064 nm, that are resonant with excited-state absorption transitions but not ground-state absorption. Using computational methods and combinatorial screening, we have identified Tm(3+)-doped NaYF4 nanoparticles as efficient looping systems that emit at 800 nm under continuous-wave excitation at 1064 nm. Using this benign excitation with standard confocal microscopy, energy-looping nanoparticles (ELNPs) are imaged in cultured mammalian cells and through brain tissue without autofluorescence. The 1 mm imaging depths and 2 μm feature sizes are comparable to those demonstrated by state-of-the-art multiphoton techniques, illustrating that ELNPs are a promising class of NIR probes for high-fidelity visualization in cells and tissue.

Excited State Structural Dynamics of Carotenoids and ChargeTransfer Systems

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

Van Tassle, Aaron Justin

This dissertation describes the development andimplementation of a visible/near infrared pump/mid-infrared probeapparatus. Chapter 1 describes the background and motivation ofinvestigating optically induced structural dynamics, paying specificattention to solvation and the excitation selection rules of highlysymmetric molecules such as carotenoids. Chapter 2 describes thedevelopment and construction of the experimental apparatus usedthroughout the remainder of this dissertation. Chapter 3 will discuss theinvestigation of DCM, a laser dye with a fluorescence signal resultingfrom a charge transfer state. By studying the dynamics of DCM and of itsmethyl deuterated isotopomer (an otherwise identical molecule), we areable to investigate the origins of the charge transfer statemore » and provideevidence that it is of the controversial twisted intramolecular (TICT)type. Chapter 4 introduces the use of two-photon excitation to the S1state, combined with one-photon excitation to the S2 state of thecarotenoid beta-apo-8'-carotenal. These 2 investigations show evidencefor the formation of solitons, previously unobserved in molecular systemsand found only in conducting polymers Chapter 5 presents an investigationof the excited state dynamics of peridinin, the carotenoid responsiblefor the light harvesting of dinoflagellates. This investigation allowsfor a more detailed understanding of the importance of structuraldynamics of carotenoids in light harvesting.« less

A general ansatz for constructing quasi-diabatic states in electronically excited aggregated systems

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

Liu, Wenlan; Köhn, Andreas; InnovationLab GmbH, Speyerer St. 4, D-69115 Heidelberg

2015-08-28

We present a general method for analyzing the character of singly excited states in terms of charge transfer (CT) and locally excited (LE) configurations. The analysis is formulated for configuration interaction singles (CIS) singly excited wave functions of aggregate systems. It also approximately works for the second-order approximate coupled cluster singles and doubles and the second-order algebraic-diagrammatic construction methods [CC2 and ADC(2)]. The analysis method not only generates a weight of each character for an excited state, but also allows to define the related quasi-diabatic states and corresponding coupling matrix elements. In the character analysis approach, we divide the targetmore » system into domains and use a modified Pipek-Mezey algorithm to localize the canonical MOs on each domain, respectively. The CIS wavefunction is then transformed into the localized basis, which allows us to partition the wavefunction into LE configurations within domains and CT configuration between pairs of different domains. Quasi-diabatic states are then obtained by mixing excited states subject to the condition of maximizing the weight of one single LE or CT configuration (localization in configuration space). Different aims of such a procedure are discussed, either the construction of pure LE and CT states for analysis purposes (by including a large number of excited states) or the construction of effective models for dynamics calculations (by including a restricted number of excited states). Applications are given to LE/CT mixing in π-stacked systems, charge-recombination matrix elements in a hetero-dimer, and excitonic couplings in multi-chromophoric systems.« less

Interstate vibronic coupling constants between electronic excited states for complex molecules

NASA Astrophysics Data System (ADS)

Fumanal, Maria; Plasser, Felix; Mai, Sebastian; Daniel, Chantal; Gindensperger, Etienne

2018-03-01

In the construction of diabatic vibronic Hamiltonians for quantum dynamics in the excited-state manifold of molecules, the coupling constants are often extracted solely from information on the excited-state energies. Here, a new protocol is applied to get access to the interstate vibronic coupling constants at the time-dependent density functional theory level through the overlap integrals between excited-state adiabatic auxiliary wavefunctions. We discuss the advantages of such method and its potential for future applications to address complex systems, in particular, those where multiple electronic states are energetically closely lying and interact. We apply the protocol to the study of prototype rhenium carbonyl complexes [Re(CO)3(N,N)(L)]n+ for which non-adiabatic quantum dynamics within the linear vibronic coupling model and including spin-orbit coupling have been reported recently.

Resonant interatomic Coulombic decay in HeNe: Electron angular emission distributions

NASA Astrophysics Data System (ADS)

Mhamdi, A.; Trinter, F.; Rauch, C.; Weller, M.; Rist, J.; Waitz, M.; Siebert, J.; Metz, D.; Janke, C.; Kastirke, G.; Wiegandt, F.; Bauer, T.; Tia, M.; Cunha de Miranda, B.; Pitzer, M.; Sann, H.; Schiwietz, G.; Schöffler, M.; Simon, M.; Gokhberg, K.; Dörner, R.; Jahnke, T.; Demekhin, Ph. Â. V.

2018-05-01

We present a joint experimental and theoretical study of resonant interatomic Coulombic decay (RICD) in HeNe employing high resolution cold target recoil ion momentum spectroscopy and ab initio electronic structure and nuclear dynamics calculations. In particular, laboratory- and molecular-frame angular emission distributions of RICD electrons are examined in detail. The exciting-photon energy-dependent anisotropy parameter β (ω ) , measured for decay events that populate bound HeNe+ ions, is in agreement with the calculations performed for the ground ionic state X2Σ1/2 + . A contribution from the a2Π3 /2 final ionic state is found to be negligible. For the He +Ne+ fragmentation channel, the observed laboratory-frame angular distribution of RICD electrons is explained by a slow homogeneous dissociation of bound vibrational levels of the final ionic state A2Π1 /2 into vibrational continua of the lower lying states X2Σ1/2 + and a2Π3 /2 . Our calculations predict that the angular distributions of RICD electrons in the body-fixed dipole plane provide direct access to the electronic character (i.e., symmetry) of intermediate vibronic resonances. However, because of the very slow dissociation of the A2Π1 /2 state, the molecular-frame angular distributions of RICD electrons in the He +Ne+ fragmentation channel are inaccessible to our coincidence experiment.

Di-lepton yield from the decay of excited 28Si states

NASA Astrophysics Data System (ADS)

Bacelar, J. C.; Buda, A.; Bałanda, A.; Krasznahorkay, A.; van der Ploeg, H.; Sujkowski, Z.; van der Woude, A.

1994-03-01

The first dilepton yield measurements from excited nuclear states obtained with a new Positron-Electron Pair Spectroscopic Instrument (PEPSI) are reported. Nuclear states in 28Si, with an initial excitation energy E∗ = 50 MeV, were populated via the isospin T = 0 reaction 4He + 24Mg and the mixed-isospin 3He + 25Mg reaction. In both reactions the dilepton (e +e -) and photon decay yields were measured concurrently. An excess of counts in the e +e - spectrum, over the converted photon yield, is observed in the energy region above 15 MeV. An analyses is discussed whereby the observed excess counts are assumed to represent the isoscalar E0 strength in excited nuclear states.

Excited-state Raman spectroscopy with and without actinic excitation: S{sub 1} Raman spectra of trans-azobenzene

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

Dobryakov, A. L.; Quick, M.; Ioffe, I. N.

We show that femtosecond stimulated Raman spectroscopy can record excited-state spectra in the absence of actinic excitation, if the Raman pump is in resonance with an electronic transition. The approach is illustrated by recording S{sub 1} and S{sub 0} spectra of trans-azobenzene in n-hexane. The S{sub 1} spectra were also measured conventionally, upon nπ* (S{sub 0} → S{sub 1}) actinic excitation. The results are discussed and compared to earlier reports.

The excited spin-triplet state of a charged exciton in quantum dots.

PubMed

Molas, M R; Nicolet, A A L; Piętka, B; Babiński, A; Potemski, M

2016-09-14

We report on spectroscopic studies of resonances related to ladder of states of a charged exciton in single GaAlAs/AlAs quantum dot structures. Polarization-resolved photoluminescence, photoluminescence excitation and photon-correlation measurements were performed at low (T  =  4.2 K) temperature also in magnetic field applied in Faraday configuration. The investigated resonances are assigned to three different configurations of a positively charged exciton. Together with a singlet ground state and a conventional triplet state (involving an electron from the ground state electronic s-shell), an excited triplet state, which involved an electron from the excited electronic p-shell was identified in single dots. The appearance of an emission line related to the latter complex is due to a partially suppressed electron relaxation in the investigated dots. An analysis of this emission line allows us to scrupulously determine properties of the excited triplet state and compare them with those of the conventional triplet state. Both triplets exhibit similar patterns of anisotropic fine structure and Zeeman splitting, however their amplitudes significantly differ for those two states. Presented results emphasize the role of the symmetry of the electronic state on the properties of the triplet states of two holes  +  electron excitonic complex.

Coulomb disorder in three-dimensional Dirac materials

NASA Astrophysics Data System (ADS)

Skinner, Brian

2015-03-01

In three-dimensional materials with a Dirac spectrum, weak short-ranged disorder is essentially irrelevant near the Dirac point. This is manifestly not the case for Coulomb disorder, where the long-ranged nature of the potential produced by charged impurities implies large fluctuations of the disorder potential even when impurities are sparse, and these fluctuations are screened by the formation of electron/hole puddles. Here I outline a theory of such nonlinear screening of Coulomb disorder in three-dimensional Dirac systems, and present results for the typical magnitude of the disorder potential, the corresponding density of states, and the size and density of electron/hole puddles. The resulting conductivity is also discussed.

Nonadiabatic excited-state molecular dynamics modeling of photoinduced dynamics in conjugated molecules.

PubMed

Nelson, Tammie; Fernandez-Alberti, Sebastian; Chernyak, Vladimir; Roitberg, Adrian E; Tretiak, Sergei

2011-05-12

Nonadiabatic dynamics generally defines the entire evolution of electronic excitations in optically active molecular materials. It is commonly associated with a number of fundamental and complex processes such as intraband relaxation, energy transfer, and light harvesting influenced by the spatial evolution of excitations and transformation of photoexcitation energy into electrical energy via charge separation (e.g., charge injection at interfaces). To treat ultrafast excited-state dynamics and exciton/charge transport we have developed a nonadiabatic excited-state molecular dynamics (NA-ESMD) framework incorporating quantum transitions. Our calculations rely on the use of the Collective Electronic Oscillator (CEO) package accounting for many-body effects and actual potential energy surfaces of the excited states combined with Tully's fewest switches algorithm for surface hopping for probing nonadiabatic processes. This method is applied to model the photoinduced dynamics of distyrylbenzene (a small oligomer of polyphenylene vinylene, PPV). Our analysis shows intricate details of photoinduced vibronic relaxation and identifies specific slow and fast nuclear motions that are strongly coupled to the electronic degrees of freedom, namely, torsion and bond length alternation, respectively. Nonadiabatic relaxation of the highly excited mA(g) state is predicted to occur on a femtosecond time scale at room temperature and on a picosecond time scale at low temperature.

A Coulomb-Like Off-Shell T-Matrix with the Correct Coulomb Phase Shift

NASA Astrophysics Data System (ADS)

Oryu, Shinsho; Watanabe, Takashi; Hiratsuka, Yasuhisa; Togawa, Yoshio

2017-03-01

We confirm the reliability of the well-known Coulomb renormalization method (CRM). It is found that the CRM is only available for a very-long-range screened Coulomb potential (SCP). However, such an SCP calculation in momentum space is considerably difficult because of the cancelation of significant digits. In contrast to the CRM, we propose a new method by using an on-shell equivalent SCP and the rest term. The two-potential theory with r-space is introduced, which defines fully the off-shell Coulomb amplitude.

Real-time ab initio simulations of excited-state dynamics in nanostructures

NASA Astrophysics Data System (ADS)

Tomanek, David

2007-03-01

Combining time-dependent ab initio density functional calculations for electrons with molecular dynamics simulations for ions, we investigate the effect of excited-state dynamics in nanostructures. In carbon nanotubes, we find electronic excitations to last for a large fraction of a picosecond. The de-excitation process is dominated by coupling to other electronic degrees of freedom during the first few hundred femtoseconds. Later, the de-excitation process becomes dominated by coupling to ionic motion. The onset point and damping rate in that regime change with initial ion velocities, a manifestation of temperature dependent electron-phonon coupling. Considering the fact that the force field in the electronically excited state differs significantly from the ground state, as reflected in the Franck-Condon effect, atomic bonds can easily be broken or restored during the relatively long lifetime of electronic excitations. This effect can be utilized in a ``photo-surgery" of nanotubes, causing structural self-healing at vacancy sites or selective de-oxidation processes induced by photo-absorption. Also, electronic excitations are a key ingredient for the understanding of sputtering processes in nanostructures, induced by energetic collisions with ions. Yoshiyuki Miyamoto, Angel Rubio, and David Tomanek, Phys. Rev. Lett. 97, 126104 (2006). Yoshiyuki Miyamoto, Savas Berber, Mina Yoon, Angel Rubio, and David Tomanek, Chem. Phys. Lett. 392, 209 (2004). Yoshiyuki Miyamoto, Noboru Jinbo, Hisashi Nakamura, Angel Rubio, and David Tomanek, Phys. Rev. B 70, 233408 (2004). Yoshiyuki Miyamoto, Arkady Krasheninnikov, and David Tomanek (in preparation).

Refinements in the description of excited VRT states of the water dimer

NASA Astrophysics Data System (ADS)

Harker, H. A.; Keutsch, F. N.; Leforestier, C.; Scribano, Y.; Han, J.-X.; Saykally, R. J.

2007-03-01

Extensive new spectroscopic measurements are combined with a global analysis of the ground state data in order to re-examine and to refine the description of the excited vibration rotation tunneling (VRT) states of the water dimer. Notably, six new 'donor torsion' subbands are analytically identified, current vibrational assignments of the Ka = 1 stacks are reassessed, the previously reported (H2O)2 donor torsion overtone (DT)2 and hydrogen bond stretch (S) data sets are augmented, and four new (S) subbands have been measured. Unusually large Coriolis effects are predicted, excited state E2 ↔ E1 assignments are reinforced, and possibilities of experimentally determining ground state AS splitting in (H2O)2 from excited state data are discussed.

Observation of excited state charge transfer with fs/ps-CARS

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

Blom, Alex Jason

2009-01-01

Excited state charge transfer processes are studied using the fs/ps-CARS probe technique. This probe allows for multiplexed detection of Raman active vibrational modes. Systems studied include Michler's Ketone, Coumarin 120, 4-dimethylamino-4'-nitrostilbene, and several others. The vibrational spectrum of the para di-substituted benzophenone Michler's Ketone in the first excited singlet state is studied for the first time. It is found that there are several vibrational modes indicative of structural changes of the excited molecule. A combined experimental and theoretical approach is used to study the simplest 7-amino-4-methylcoumarin, Coumarin 120. Vibrations observed in FTIR and spontaneous Raman spectra are assigned using densitymore » functional calculations and a continuum solvation model is used to predict how observed modes are affected upon inclusion of a solvent. The low frequency modes of the excited state charge transfer species 4-dimethylamino-4{prime}-nitrostilbene are studied in acetonitrile. Results are compared to previous work on this molecule in the fingerprint region. Finally, several partially completed projects and their implications are discussed. These include the two photon absorption of Coumarin 120, nanoconfinement in cyclodextrin cavities and sensitization of titania nanoparticles.« less

Watson-Crick base pairing controls excited-state decay in natural DNA.

PubMed

Bucher, Dominik B; Schlueter, Alexander; Carell, Thomas; Zinth, Wolfgang

2014-10-13

Excited-state dynamics are essential to understanding the formation of DNA lesions induced by UV light. By using femtosecond IR spectroscopy, it was possible to determine the lifetimes of the excited states of all four bases in the double-stranded environment of natural DNA. After UV excitation of the DNA duplex, we detected a concerted decay of base pairs connected by Watson-Crick hydrogen bonds. A comparison of single- and double-stranded DNA showed that the reactive charge-transfer states formed in the single strands are suppressed by base pairing in the duplex. The strong influence of the Watson-Crick hydrogen bonds indicates that proton transfer opens an efficient decay path in the duplex that prohibits the formation or reduces the lifetime of reactive charge-transfer states. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Stability of Dirac Liquids with Strong Coulomb Interaction.

PubMed

Tupitsyn, Igor S; Prokof'ev, Nikolay V

2017-01-13

We develop and apply the diagrammatic Monte Carlo technique to address the problem of the stability of the Dirac liquid state (in a graphene-type system) against the strong long-range part of the Coulomb interaction. So far, all attempts to deal with this problem in the field-theoretical framework were limited either to perturbative or random phase approximation and functional renormalization group treatments, with diametrically opposite conclusions. Our calculations aim at the approximation-free solution with controlled accuracy by computing vertex corrections from higher-order skeleton diagrams and establishing the renormalization group flow of the effective Coulomb coupling constant. We unambiguously show that with increasing the system size L (up to ln(L)∼40), the coupling constant always flows towards zero; i.e., the two-dimensional Dirac liquid is an asymptotically free T=0 state with divergent Fermi velocity.

The Millimeter-Wave Spectrum of Methacrolein. Torsion-Rotation Effects in the Excited States

NASA Astrophysics Data System (ADS)

Zakharenko, Olena; Motiyenko, R. A.; Aviles Moreno, Juan-Ramon; Huet, T. R.

2015-06-01

Last year we reported the analysis of the rotational spectrum of s-trans conformer of methacrolein CH2=C(CH3)CHO in the ground vibrational state. In this talk we report the study of its low lying excited vibrational states. The study is based on room-temperature absorption spectra of methacrolein recorded in the frequency range 150 - 465 GHz using the spectrometer in Lille. The new results include assignment of the first excited torsional state (131 cm-1), and the joint analysis of the vt = 0 and vt = 1 states, that allowed us to improve the model in the frame of Rho-Axis-Method (RAM) Hamiltonian and to remove some strong correlations between parameters. Also we assigned the first excited vibrational state of the skeletal torsion mode (170 cm-1). The inverse sequence of A and E tunneling substates as well as anomalous A-E splittings observed for the rotational lines of vsk = 1 state clearly indicate a coupling between methyl torsion and skeletal torsion. However we were able to fit within experimental accuracy the rotational lines of vsk = 1 state using the RAM Hamiltonian. Because of the inversion of the A and E tunneling substates the rotational lines of the vsk = 1 states were assumed to belong to a virtual first excited torsional state. Finally, we assigned several low-Ka rotational transitions of the excited vibrational states above 200 cm-1 but their analysis is complicated by different rotation-vibration interactions. In particular there is an evidence of the Fermi-type resonance between the second excited torsional state and the first excited state of the in-plane skeletal bending mode (265 cm-1). Support from the French Laboratoire d'Excellence CaPPA (Chemical and Physical Properties of the Atmosphere) through contract ANR-10-LABX-0005 of the Programme d'Investissements d'Avenir is acknowledged. Zakharenko O. et al., 69th ISMS, 2014, TI01

Inelastic light scattering from plasmons tunneling between Wannier-Stark states

NASA Astrophysics Data System (ADS)

Fluegel, B.; Pfeiffer, L. N.; West, K.; Mascarenhas, A.

2018-06-01

Using inelastic light scattering, we measure the zone-center electronic excitation modes in a set of multiple quantum wells. The width of the wavefunction barriers was chosen such that it prevents significant coupling of the electron ground states between wells yet is transparent to electron tunneling under an electric field. Under these conditions, we find charge-density-like and spin-density-like plasmons whose energies do not correspond to the excitations calculated for either a single well or a set of Coulomb-coupled wells. The observed energies are proportional to the electric field strength and the lower energy modes agree with predictions for plasmons tunneling between the Wannier-Stark ladder states.

Carbon nanorings with inserted acenes: Breaking symmetry in excited state dynamics

DOE PAGES

Franklin-Mergarejo, R.; Alvarez, D. Ondarse; Tretiak, S.; ...

2016-08-10

Conjugated cycloparaphenylene rings have unique electronic properties being the smallest segments of carbon nanotubes. Their conjugated backbones support delocalized electronic excitations, which dynamics is strongly influenced by cyclic geometry. Here we present a comparative theoretical study of the electronic and vibrational energy relaxation and redistribution in photoexcited cycloparaphenylene carbon nanorings with inserted naphthalene, anthracene, and tetracene units using non-adiabatic excited-state molecular dynamics simulations. Calculated excited state structures reflect modifications of optical selection rules and appearance of low-energy electronic states localized on the acenes due to gradual departure from a perfect circular symmetry. After photoexcitation, an ultrafast electronic energy relaxation tomore » the lowest excited state is observed on the time scale of hundreds of femtoseconds in all molecules studied. Concomitantly, the efficiency of the exciton trapping in the acene raises when moving from naphthalene to anthracene and to tetracene, being negligible in naphthalene, and ~60% and 70% in anthracene and tetracene within the first 500 fs after photoexcitation. Observed photoinduced dynamics is further analyzed in details using induced molecular distortions, delocatization properties of participating electronic states and non-adiabatic coupling strengths. Lastly, our results provide a number of insights into design of cyclic molecular systems for electronic and light-harvesting applications.« less

Emergence of nontrivial magnetic excitations in a spin-liquid state of kagomé volborthite

PubMed Central

Watanabe, Daiki; Sugii, Kaori; Shimozawa, Masaaki; Suzuki, Yoshitaka; Yajima, Takeshi; Ishikawa, Hajime; Hiroi, Zenji; Shibauchi, Takasada; Matsuda, Yuji; Yamashita, Minoru

2016-01-01

When quantum fluctuations destroy underlying long-range ordered states, novel quantum states emerge. Spin-liquid (SL) states of frustrated quantum antiferromagnets, in which highly correlated spins fluctuate down to very low temperatures, are prominent examples of such quantum states. SL states often exhibit exotic physical properties, but the precise nature of the elementary excitations behind such phenomena remains entirely elusive. Here, we use thermal Hall measurements that can capture the unexplored property of the elementary excitations in SL states, and report the observation of anomalous excitations that may unveil the unique features of the SL state. Our principal finding is a negative thermal Hall conductivity κxy which the charge-neutral spin excitations in a gapless SL state of the 2D kagomé insulator volborthite Cu3V2O7(OH)2⋅2H2O exhibit, in much the same way in which charged electrons show the conventional electric Hall effect. We find that κxy is absent in the high-temperature paramagnetic state and develops upon entering the SL state in accordance with the growth of the short-range spin correlations, demonstrating that κxy is a key signature of the elementary excitation formed in the SL state. These results suggest the emergence of nontrivial elementary excitations in the gapless SL state which feel the presence of fictitious magnetic flux, whose effective Lorentz force is found to be less than 1/100 of the force experienced by free electrons. PMID:27439874

Revealing the Coulomb interaction strength in a cuprate superconductor

DOE PAGES

Yang, S. -L.; Sobota, J. A.; He, Y.; ...

2017-12-08

Here, we study optimally doped Bi 2 Sr 2 Ca 0.92 Y 0.08 Cu 2 O 8 + δ (Bi2212) using angle-resolved two-photon photoemission spectroscopy. Three spectral features are resolved near 1.5, 2.7, and 3.6 eV above the Fermi level. By tuning the photon energy, we determine that the 2.7-eV feature arises predominantly from unoccupied states. The 1.5- and 3.6-eV features reflect unoccupied states whose spectral intensities are strongly modulated by the corresponding occupied states. These unoccupied states are thus consistent with the prediction from a cluster perturbation theory based on the single-band Hubbard model. Through this comparison, amore » Coulomb interaction strength U of 2.7 eV is extracted. Our study complements equilibrium photoemission spectroscopy and provides a direct spectroscopic measurement of the unoccupied states in cuprates. The determined Coulomb U indicates that the charge-transfer gap of optimally doped Bi2212 is 1.1 eV.« less

Manipulating charge transfer excited state relaxation and spin crossover in iron coordination complexes with ligand substitution

DOE PAGES

Zhang, Wenkai; Kjaer, Kasper S.; Alonso-Mori, Roberto; ...

2016-08-25

Developing light-harvesting and photocatalytic molecules made with iron could provide a cost effective, scalable, and environmentally benign path for solar energy conversion. To date these developments have been limited by the sub-picosecond metal-to-ligand charge transfer (MLCT) electronic excited state lifetime of iron based complexes due to spin crossover – the extremely fast intersystem crossing and internal conversion to high spin metal-centered excited states. We revitalize a 30 year old synthetic strategy for extending the MLCT excited state lifetimes of iron complexes by making mixed ligand iron complexes with four cyanide (CN –) ligands and one 2,2'-bipyridine (bpy) ligand. This enablesmore » MLCT excited state and metal-centered excited state energies to be manipulated with partial independence and provides a path to suppressing spin crossover. We have combined X-ray Free-Electron Laser (XFEL) Kβ hard X-ray fluorescence spectroscopy with femtosecond time-resolved UV-visible absorption spectroscopy to characterize the electronic excited state dynamics initiated by MLCT excitation of [Fe(CN) 4(bpy)] 2–. The two experimental techniques are highly complementary; the time-resolved UV-visible measurement probes allowed electronic transitions between valence states making it sensitive to ligand-centered electronic states such as MLCT states, whereas the Kβ fluorescence spectroscopy provides a sensitive measure of changes in the Fe spin state characteristic of metal-centered excited states. Here, we conclude that the MLCT excited state of [Fe(CN) 4(bpy)] 2– decays with roughly a 20 ps lifetime without undergoing spin crossover, exceeding the MLCT excited state lifetime of [Fe(2,2'-bipyridine) 3] 2+ by more than two orders of magnitude.« less

Excited-state dynamics of the medicinal pigment curcumin in a hydrogel.

PubMed

Harada, Takaaki; Lincoln, Stephen F; Kee, Tak W

2016-10-12

Curcumin is a yellow polyphenol with multiple medicinal effects. These effects, however, are limited due to its poor aqueous stability and solubility. A hydrogel of 3% octadecyl randomly substituted polyacrylate (PAAC18) has been shown to provide high aqueous stability for curcumin under physiological conditions, offering a route for photodynamic therapy. In this study, the excited-state photophysics of curcumin in the PAAC18 hydrogel is investigated using a combination of femtosecond transient absorption and fluorescence upconversion spectroscopy. The transient absorption results reveal a multiexponential decay in the excited-state kinetics with fast (1 ps & 15 ps) and slow (110 ps & ≈5 ns) components. The fast decay component exhibits a deuterium isotope effect with D 2 O in the hydrogel, indicating that the 15 ps decay component is attributable to excited-state intramolecular hydrogen atom transfer of curcumin in the PAAC18 hydrogel. In addition, solvent reorganisation of excited-state curcumin is investigated using multiwavelength femtosecond fluorescence upconversion spectroscopy. The results show that the dominant solvation response (τ = 0.08 ps) is a fast inertial motion owing to the presence of bulk-like water in the vicinity of the hydrophobic octadecyl substituents of the PAAC18 hydrogel. The results also show an additional response with longer time constants of 1 and 6 ps, which is attributable to translational diffusion of confined water molecules in the three-dimensional, cross-linking network of the octadecyl substituents of PAAC18. Overall, we show that excited-state intramolecular hydrogen atom transfer and solvent reorganisation are major photophysical events for curcumin in the PAAC18 hydrogel.

Resolving the excited state equilibrium of peridinin in solution.

PubMed

Papagiannakis, Emmanouil; Larsen, Delmar S; van Stokkum, Ivo H M; Vengris, Mikas; Hiller, Roger G; van Grondelle, Rienk

2004-12-14

The carotenoid peridinin is abundant in the biosphere, as it is the main pigment bound by the light-harvesting complexes of dinoflagellates, where it collects blue and green sunlight and transfers energy to chlorophyll a with high efficiency. Its molecular structure is particularly complex, giving rise to an intricate excited state manifold, which includes a state with charge-transfer character. To disentangle the excited states of peridinin and understand their function in vivo, we applied dispersed pump-probe and pump-dump-probe spectroscopy. The preferential depletion of population from the intramolecular charge transfer state by the dump pulse demonstrates that the S(1) and this charge transfer state are distinct entities. The ensuing dump-induced dynamics illustrates the equilibration of the two states which occurs on the time scale of a few picoseconds. Additionally, the dump pulse populates a short-lived ground state intermediate, which is suggestive of a complex relaxation pathway, probably including structural reorientation or solvation of the ground state. These findings indicate that the unique intramolecular charge transfer state of peridinin is an efficient energy donor to chlorophyll a in the peridinin-chlorophyll-protein complex and thus plays a significant role in global light harvesting.

Are there near-threshold Coulomb-like Baryonia?

NASA Astrophysics Data System (ADS)

Geng, Li-Sheng; Lu, Jun-Xu; Valderrama, M. Pavon; Ren, Xiu-Lei

2018-05-01

The Λc(2590 )Σc system can exchange a pion near the mass-shell. Owing to the opposite intrinsic parity of the Λc(2590 ) and Σc, the pion is exchanged in S-wave. This gives rise to a Coulomb-like force that might be able to bind the system. If one takes into account that the pion is not exactly on the mass shell, there is a shallow S-wave state, which we generically call the Yc c(5045 ) and Yc c ¯(5045 ) for the Λc(2590 )Σc and Λc(2590 )Σ¯c systems respectively. For the baryon-antibaryon case this Coulomb-like force is independent of spin: the Yc c ¯(5045 ) baryonia will appear either in the spin S =0 or S =1 configurations with G-parities G =(-1 )L+S +1. For the baryon-baryon case the Coulomb-like force is attractive in the spin S =0 configuration, for which a doubly charmed molecule is expected to form near the threshold. This type of spectrum might be very well realized in other molecular states composed of two opposite parity hadrons with the same spin and a mass difference close to that of a pseudo-Goldstone boson, of which a few examples include the Λ (1405 )N , Λ (1520 )Σ*, Ξ (1690 )Σ , Ds0 *(2317 )D and Ds1 *(2460 )D* molecules.

Heat of formation determination of the ground and excited state of cyanomethylene (HCCN) radical

NASA Technical Reports Server (NTRS)

Francisco, Joseph S.

1994-01-01

Ab initio electronic structure theory has been used to characterize the structure of the ground triplet and lowest singlet excited states of cyanomethylene. The geometries, vibrational frequencies, and heats of formation have been determined using second-order Moller-Plesset perturbation, single and double excitation configuration interaction, and quadratic configuration interaction theory. The heat of formation is predicted with isodesmic reaction and Gaussian-2 theory (G2) for the ground triplet and first excited singlet states of cyanomethylene. For the ground state Delta-H(sub 0)(sup f,0) is 114.8+/-2 kcal/mol while for the excited single state it is 126.5+/-2 kcal/mol.

Using narrowband excitation to confirm that the S∗ state in carotenoids is not a vibrationally-excited ground state species

NASA Astrophysics Data System (ADS)

Jailaubekov, Askat E.; Song, Sang-Hun; Vengris, Mikas; Cogdell, Richard J.; Larsen, Delmar S.

2010-02-01

The hypothesis that S∗ is a vibrationally-excited ground-state population is tested and discarded for two carotenoid samples: β-carotene in solution and rhodopin glucoside embedded in the light harvesting 2 protein from Rhodopseudomonas acidophila. By demonstrating that the transient absorption signals measured in both systems that are induced by broadband (1000 cm -1) and narrowband (50 cm -1) excitation pulses are near identical and hence bandwidth independent, the impulsive stimulated Raman scattering mechanism proposed as the primary source for S∗ generation is discarded. To support this conclusion, previously published multi-pulse pump-dump-probe signals [17] are revisited to discard secondary mechanisms for S∗ formation.

Time-resolved and steady-state fluorescence studies of excited-state proton-transfer reactions of proflavine

NASA Astrophysics Data System (ADS)

De Silvestri, S.; Laporta, P.

1984-01-01

Time-resolved and steady-state fluorescence studies of proflavine in aqueous solution are presented. The observation of a monoexponential fluorescence decay with a time constant decreasing with increasing pH and the presence of an anomalous red-shift in the fluorescence spectrum as a function of pH indicate the existence of a complex proton-transfer mechanism in the excited state. A reaction scheme is proposed and the corresponding proton-transfer rates are evaluated. An excited-state pK value of 12.85 is obtained for the equilibrium between the cationic form of proflavine and the same form dissociated at an amino group.

Unified approach to probing Coulomb effects in tunnel ionization for any ellipticity of laser light.

PubMed

Landsman, A S; Hofmann, C; Pfeiffer, A N; Cirelli, C; Keller, U

2013-12-27

We present experimental data that show significant deviations from theoretical predictions for the location of the center of the electron momenta distribution at low values of ellipticity ε of laser light. We show that these deviations are caused by significant Coulomb focusing along the minor axis of polarization, something that is normally neglected in the analysis of electron dynamics, even in cases where the Coulomb correction is otherwise taken into account. By investigating ellipticity-resolved electron momenta distributions in the plane of polarization, we show that Coulomb focusing predominates at lower values of ellipticity of laser light, while Coulomb asymmetry becomes important at higher values, showing that these two complementary phenomena can be used to probe long-range Coulomb interaction at all polarizations of laser light. Our results suggest that both the breakdown of Coulomb focusing and the onset of Coulomb asymmetry are linked to the disappearance of Rydberg states with increasing ellipticity.

Mechanism for the Excited-State Multiple Proton Transfer Process of Dihydroxyanthraquinone Chromophores.

PubMed

Zhou, Qiao; Du, Can; Yang, Li; Zhao, Meiyu; Dai, Yumei; Song, Peng

2017-06-22

The single and dual cooperated proton transfer dynamic process in the excited state of 1,5-dihydroxyanthraquinone (1,5-DHAQ) was theoretically investigated, taking solvent effects (ethanol) into account. The absorption and fluorescence spectra were simulated, and dual fluorescence exhibited, which is consistent with previous experiments. Analysis of the calculated IR and Raman vibration spectra reveals that the intramolecular hydrogen bonding interactions (O 20 -H 21 ···O 24 and O 22 -H 23 ···O 25 ) are strengthened following the excited proton transfer process. Finally, by constructing the potential energy surfaces of the ground state, first excited singlet state, and triplet state, the mechanism of the intramolecular proton transfer of 1,5-DHAQ can be revealed.

Bottom-up excited state dynamics of two cinnamate-based sunscreen filter molecules.

PubMed

Peperstraete, Yoann; Staniforth, Michael; Baker, Lewis A; Rodrigues, Natércia D N; Cole-Filipiak, Neil C; Quan, Wen-Dong; Stavros, Vasilios G

2016-10-12

Methyl-E-4-methoxycinnamate (E-MMC) is a model chromophore of the commonly used commercial sunscreen agent, 2-ethylhexyl-E-4-methoxycinnamate (E-EHMC). In an effort to garner a molecular-level understanding of the photoprotection mechanisms in operation with E-EHMC, we have used time-resolved pump-probe spectroscopy to explore E-MMC's and E-EHMC's excited state dynamics upon UV-B photoexcitation to the S 1 (1 1 ππ*) state in both the gas- and solution-phase. In the gas-phase, our studies suggest that the excited state dynamics are driven by non-radiative decay from the 1 1 ππ* to the S 3 (1 1 nπ*) state, followed by de-excitation from the 1 1 nπ* to the ground electronic state (S 0 ). Using both a non-polar-aprotic solvent, cyclohexane, and a polar-protic solvent, methanol, we investigated E-MMC and E-EHMC's photochemistry in a more realistic, 'closer-to-shelf' environment. A stark change to the excited state dynamics in the gas-phase is observed in the solution-phase suggesting that the dynamics are now driven by efficient E/Z isomerisation from the initially photoexcited 1 1 ππ* state to S 0 .

Vibronic structure and coupling of higher excited electronic states in carotenoids

NASA Astrophysics Data System (ADS)

Krawczyk, Stanisław; Luchowski, Rafał

2013-03-01

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

Direct probe of the variability of Coulomb correlation in iron pnictide superconductors

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

Vilmercati, P.; Parks Cheney, C.; Bondino, F.

2012-01-01

We use core-valence-valence Auger spectra to probe the Coulomb repulsion between holes in the valence band of Fe pnictide superconductors. By comparing the two-hole final-state spectra to density functional theory calculations of the single-particle density of states, we extract a measure of the electron correlations that exist in these systems. Our results show that the Coulomb repulsion is highly screened and can definitively be considered as weak. We also find that there are differences between the 1111 and 122 families and even a small variation as a function of the doping x in Ba(Fe{sub 1-x}Co{sub x}){sub 2}As{sub 2}. We discussmore » how the values of the hole-hole Coulomb repulsion obtained from our study relate to the onsite Coulomb parameter U used in model and first-principles calculations based on dynamical mean field theory and establish an upper bound for its effective value. Our results impose stringent constraints on model-based phase diagrams that vary with the quantity U or U/W by restricting the latter to a rather small range of values.« less

Electronic Excited States of Tungsten(0) Arylisocyanides.

PubMed

Kvapilová, Hana; Sattler, Wesley; Sattler, Aaron; Sazanovich, Igor V; Clark, Ian P; Towrie, Michael; Gray, Harry B; Záliš, Stanislav; Vlček, Antonín

2015-09-08

W(CNAryl)6 complexes containing 2,6-diisopropylphenyl isocyanide (CNdipp) are powerful photoreductants with strongly emissive long-lived excited states. These properties are enhanced upon appending another aryl ring, e.g., W(CNdippPh(OMe2))6; CNdippPh(OMe2) = 4-(3,5-dimethoxyphenyl)-2,6-diisopropylphenylisocyanide (Sattler et al. J. Am. Chem. Soc. 2015, 137, 1198-1205). Electronic transitions and low-lying excited states of these complexes were investigated by time-dependent density functional theory (TDDFT); the lowest triplet state was characterized by time-resolved infrared spectroscopy (TRIR) supported by density functional theory (DFT). The intense absorption band of W(CNdipp)6 at 460 nm and that of W(CNdippPh(OMe2))6 at 500 nm originate from transitions of mixed ππ*(C≡N-C)/MLCT(W → Aryl) character, whereby W is depopulated by ca. 0.4 e(-) and the electron-density changes are predominantly localized along two equatorial molecular axes. The red shift and intensity rise on going from W(CNdipp)6 to W(CNdippPh(OMe2))6 are attributable to more extensive delocalization of the MLCT component. The complexes also exhibit absorptions in the 300-320 nm region, owing to W → C≡N MLCT transitions. Electronic absorptions in the spectrum of W(CNXy)6 (Xy = 2,6-dimethylphenyl), a complex with orthogonal aryl orientation, have similar characteristics, although shifted to higher energies. The relaxed lowest W(CNAryl)6 triplet state combines ππ* excitation of a trans pair of C≡N-C moieties with MLCT (0.21 e(-)) and ligand-to-ligand charge transfer (LLCT, 0.24-0.27 e(-)) from the other four CNAryl ligands to the axial aryl and, less, to C≡N groups; the spin density is localized along a single Aryl-N≡C-W-C≡N-Aryl axis. Delocalization of excited electron density on outer aryl rings in W(CNdippPh(OMe2))6 likely promotes photoinduced electron-transfer reactions to acceptor molecules. TRIR spectra show an intense broad bleach due to ν(C≡N), a prominent transient

Quantum solution for the one-dimensional Coulomb problem

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

Nunez-Yepez, H. N.; Salas-Brito, A. L.; Solis, Didier A.

2011-06-15

The one-dimensional hydrogen atom has been a much studied system with a wide range of applications. Since the pioneering work of Loudon [R. Loudon, Am. J. Phys. 27, 649 (1959).], a number of different features related to the nature of the eigenfunctions have been found. However, many of the claims made throughout the years in this regard are not correct--such as the existence of only odd eigenstates or of an infinite binding-energy ground state. We explicitly show that the one-dimensional hydrogen atom does not admit a ground state of infinite binding energy and that the one-dimensional Coulomb potential is notmore » its own supersymmetric partner. Furthermore, we argue that at the root of many such false claims lies the omission of a superselection rule that effectively separates the right side from the left side of the singularity of the Coulomb potential.« less

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

PubMed

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

2014-05-14

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

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

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

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

2014-05-14

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

Exotic and excited-state radiative transitions in charmonium from lattice QCD

DOE PAGES

Dudek, Jozef J.; Edwards, Robert G.; Thomas, Christopher E.

2009-05-01

We compute, for the first time using lattice QCD methods, radiative transition rates involving excited charmonium states, states of high spin and exotics. Utilizing a large basis of interpolating fields we are able to project out various excited state contributions to three-point correlators computed on quenched anisotropic lattices. In the first lattice QCD calculation of the exoticmore » $$1^{-+}$$ $$\\eta_{c1}$$ radiative decay, we find a large partial width $$\\Gamma(\\eta_{c1} \\to J/\\psi \\gamma) \\sim 100 \\,\\mathrm{keV}$$. We find clear signals for electric dipole and magnetic quadrupole transition form factors in $$\\chi_{c2} \\to J/\\psi \\gamma$$, calculated for the first time in this framework, and study transitions involving excited $$\\psi$$ and $$\\chi_{c1,2}$$ states. We calculate hindered magnetic dipole transition widths without the sensitivity to assumptions made in model studies and find statistically significant signals, including a non-exotic vector hybrid candidate $Y_{\\mathrm{hyb?}} \\to \\et« less

Ultrafast coherent excitation of a trapped ion qubit for fast gates and photon frequency qubits.

PubMed

Madsen, M J; Moehring, D L; Maunz, P; Kohn, R N; Duan, L-M; Monroe, C

2006-07-28

We demonstrate ultrafast coherent excitation of an atomic qubit stored in the hyperfine levels of a single trapped cadmium ion. Such ultrafast excitation is crucial for entangling networks of remotely located trapped ions through the interference of photon frequency qubits, and is also a key component for realizing ultrafast quantum gates between Coulomb-coupled ions.

Two-magnon excitations in resonant inelastic x-ray scattering studied within spin density wave formalism

NASA Astrophysics Data System (ADS)

Nomura, Takuji

2017-10-01

We study two-magnon excitations in resonant inelastic x-ray scattering (RIXS) at the transition-metal K edge. Instead of working with effective Heisenberg spin models, we work with a Hubbard-type model (d -p model) for a typical insulating cuprate La2CuO4 . For the antiferromagnetic ground state within the spin density wave (SDW) mean-field formalism, we calculate the dynamical correlation function within the random-phase approximation (RPA), and then obtain two-magnon excitation spectra by calculating the convolution of it. Coupling between the K -shell hole and the magnons in the intermediate state is calculated by means of diagrammatic perturbation expansion in the Coulomb interaction. The calculated momentum dependence of RIXS spectra agrees well with that of experiments. A notable difference from previous calculations based on the Heisenberg spin models is that RIXS spectra have a large two-magnon weight near the zone center, which may be confirmed by further careful high-resolution experiments.

Coulomb Impurity Problem of Graphene in Strong Coupling Regime in Magnetic Fields.

PubMed

Kim, S C; Yang, S-R Eric

2015-10-01

We investigate the Coulomb impurity problem of graphene in strong coupling limit in the presence of magnetic fields. When the strength of the Coulomb potential is sufficiently strong the electron of the lowest energy boundstate of the n = 0 Landau level may fall to the center of the potential. To prevent this spurious effect the Coulomb potential must be regularized. The scaling function for the inverse probability density of this state at the center of the impurity potential is computed in the strong coupling regime. The dependence of the computed scaling function on the regularization parameter changes significantly as the strong coupling regime is approached.

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

PubMed

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

2013-11-01

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

Negative Coulomb damping, limit cycles, and self-oscillation of the vocal folds

NASA Astrophysics Data System (ADS)

Fulcher, Lewis P.; Scherer, Ronald C.; Melnykov, Artem; Gateva, Vesela; Limes, Mark E.

2006-05-01

An effective one-mass model of phonation is developed. It borrows the salient features of the classic two-mass model of human speech developed by Ishizaka, Matsudaira, and Flanagan. Their model is based on the idea that the oscillating vocal folds maintain their motion by deriving energy from the flow of air through the glottis. We argue that the essence of the action of the aerodynamic forces on the vocal folds is captured by negative Coulomb damping, which acts on the oscillator to energize it. A viscous force is added to include the effects of tissue damping. The solutions to this single oscillator model show that when it is excited by negative Coulomb damping, it will reach a limit cycle. Displacements, phase portraits, and energy histories are presented for two underdamped linear oscillators. A nonlinear force is added so that the variations of the fundamental frequency and the open quotient with lung pressure are comparable to the behavior of the two-mass model.

Evidence for excited state intramolecular charge transfer in benzazole-based pseudo-stilbenes.

PubMed

Santos, Fabiano da Silveira; Descalzo, Rodrigo Roceti; Gonçalves, Paulo Fernando Bruno; Benvenutti, Edilson Valmir; Rodembusch, Fabiano Severo

2012-08-21

Two azo compounds were obtained through the diazotization reaction of aminobenzazole derivatives and N,N-dimethylaniline using clay montmorillonite KSF as catalyst. The synthesized dyes were characterized using elemental analysis, Fourier transform infrared spectroscopy, and (13)C and (1)H NMR spectroscopy in solution. Their photophysical behavior was studied using UV-vis and steady-state fluorescence in solution. These dyes present intense absorption in the blue region. The spectral features of the azo compounds can be related to the pseudo-stilbene type as well as the E isomer of the dyes. Excitation at the absorption maxima does not produce emissive species in the excited state. However, excitation around 350 nm allowed dual emission of fluorescence, from both a locally excited (LE, short wavelength) and an intramolecular charge transfer (ICT, long wavelength) state, which was corroborated by a linear relation of the fluorescence maximum (ν(max)) versus the solvent polarity function (Δf) from the Lippert-Mataga correlation. Evidence of TICT in these dyes was discussed from the viscosity dependence of the fluorescence intensity in the ICT emission band. Theoretical calculations were also performed in order to study the geometry and charge distribution of the dyes in their ground and excited electronic states. Using DFT methods at the theoretical levels BLYP/Aug-cc-pVDZ, for geometry optimizations and frequency calculations, and B3LYP/6-311+G(2d), for single-point energy evaluations, the calculations revealed that the least energetic and most intense photon absorption leads to a very polar excited state that relaxes non-radioactively, which can be associated with photochemical isomerization.

Hydrogen bond strengthening between o-nitroaniline and formaldehyde in electronic excited states: A theoretical study

NASA Astrophysics Data System (ADS)

Yang, Juan; Li, An Yong

2018-06-01

To study the hydrogen bonds upon photoexcited, the time dependent density function method (TD DFT) was performed to investigate the excited state hydrogen bond properties of between o-nitroaniline (ONA) and formaldehyde (CH2O). The optimized structures of the complex and the monomers both in the ground state and the electronically excited states are calculated using DFT and TD DFT method respectively. Quantum chemical calculations of the electronic and vibrational absorption spectra are also carried out by TD DFT method at the different level. The complex ONA⋯CH2O forms the intramolecular hydrogen bond and intermolecular hydrogen bonds. Since the strength of hydrogen bonds can be measured by studying the vibrational absorption spectra of the characteristic groups on the hydrogen bonding acceptor and donor, it evidently confirms that the hydrogen bonds is strengthened in the S1/S2/T1 excited states upon photoexcitation. As a result, the hydrogen bonds cause that the CH stretch frequency of the proton donor CH2O has a blue shift, and the electron excitations leads to a frequency red shift of Ndbnd O and Nsbnd H stretch modes in the o-nitroaniline(ONA) and a small frequency blue shift of CH stretch mode in the formaldehyde(CH2O) in the S1 and S2 excited states. The excited states S1, S2 and T1 are locally excited states where only the ONA moiety is excited, but the CH2O moiety remains in its ground state.

Self-Consistent Monte Carlo Study of the Coulomb Interaction under Nano-Scale Device Structures

NASA Astrophysics Data System (ADS)

Sano, Nobuyuki

2011-03-01

It has been pointed that the Coulomb interaction between the electrons is expected to be of crucial importance to predict reliable device characteristics. In particular, the device performance is greatly degraded due to the plasmon excitation represented by dynamical potential fluctuations in high-doped source and drain regions by the channel electrons. We employ the self-consistent 3D Monte Carlo (MC) simulations, which could reproduce both the correct mobility under various electron concentrations and the collective plasma waves, to study the physical impact of dynamical potential fluctuations on device performance under the Double-gate MOSFETs. The average force experienced by an electron due to the Coulomb interaction inside the device is evaluated by performing the self-consistent MC simulations and the fixed-potential MC simulations without the Coulomb interaction. Also, the band-tailing associated with the local potential fluctuations in high-doped source region is quantitatively evaluated and it is found that the band-tailing becomes strongly dependent of position in real space even inside the uniform source region. This work was partially supported by Grants-in-Aid for Scientific Research B (No. 2160160) from the Ministry of Education, Culture, Sports, Science and Technology in Japan.

Selective two-photon excitation of a vibronic state by correlated photons.

PubMed

Oka, Hisaki

2011-03-28

We theoretically investigate the two-photon excitation of a molecular vibronic state by correlated photons with energy anticorrelation. A Morse oscillator having three sets of vibronic states is used, as an example, to evaluate the selectivity and efficiency of two-photon excitation. We show that a vibrational mode can be selectively excited with high efficiency by the correlated photons, without phase manipulation or pulse-shaping techniques. This can be achieved by controlling the quantum correlation so that the photon pair concurrently has two pulse widths, namely, a temporally narrow width and a spectrally narrow width. Though this concurrence is seemingly contradictory, we can create such a photon pair by tailoring the quantum correlation between two photons.

Influence of solvent and substituent on excited state characteristics of laser grade coumarin dyes.

PubMed

Sharma, Vijay K; Saharo, P D; Sharma, Neera; Rastogi, Ramesh C; Ghoshal, S K; Mohan, D

2003-04-01

Absorption and fluorescence emission of 4 and 7 substituted coumarins viz. C 440, C 490, C 485 and C 311 have been studied in various polar and non-polar organic solvents. These coumarin dyes are substituted with alkyl, amine and fluorine groups at 4- and 7-positions. They give different absorption and emission spectra in different solvents. The study leads to a possible assignment of energy level scheme for such coumarins including the effect on ground state and excited state dipole moments due to substitutions. Excited state dipole moments of these dyes are calculated by solvetochromic data experimentally and theoretically these are calculated by PM 3 method. The dipole moments in excited state, for all molecules investigated here, are higher than the corresponding values in the ground state. The increase in dipole moment has been explained in terms of the nature of excited state and resonance structure.

Correction of the near threshold behavior of electron collisional excitation cross-sections in the plane-wave Born approximation

NASA Astrophysics Data System (ADS)

Kilcrease, D. P.; Brookes, S.

2013-12-01

The modeling of NLTE plasmas requires the solution of population rate equations to determine the populations of the various atomic levels relevant to a particular problem. The equations require many cross sections for excitation, de-excitation, ionization and recombination. A simple and computational fast way to calculate electron collisional excitation cross-sections for ions is by using the plane-wave Born approximation. This is essentially a high-energy approximation and the cross section suffers from the unphysical problem of going to zero near threshold. Various remedies for this problem have been employed with varying degrees of success. We present a correction procedure for the Born cross-sections that employs the Elwert-Sommerfeld factor to correct for the use of plane waves instead of Coulomb waves in an attempt to produce a cross-section similar to that from using the more time consuming Coulomb Born approximation. We compare this new approximation with other, often employed correction procedures. We also look at some further modifications to our Born Elwert procedure and its combination with Y.K. Kim's correction of the Coulomb Born approximation for singly charged ions that more accurately approximate convergent close coupling calculations.

Dual structure in the charge excitation spectrum of electron-doped cuprates

NASA Astrophysics Data System (ADS)

Bejas, Matías; Yamase, Hiroyuki; Greco, Andrés

2017-12-01

Motivated by the recent resonant x-ray scattering (RXS) and resonant inelastic x-ray scattering (RIXS) experiments for electron-doped cuprates, we study the charge excitation spectrum in a layered t -J model with the long-range Coulomb interaction. We show that the spectrum is not dominated by a specific type of charge excitations, but by different kinds of charge fluctuations, and is characterized by a dual structure in the energy space. Low-energy charge excitations correspond to various types of bond-charge fluctuations driven by the exchange term (J term), whereas high-energy charge excitations are due to usual on-site charge fluctuations and correspond to plasmon excitations above the particle-hole continuum. The interlayer coupling, which is frequently neglected in many theoretical studies, is particularly important to the high-energy charge excitations.

Testing the Predictive Power of Coulomb Stress on Aftershock Sequences

NASA Astrophysics Data System (ADS)

Woessner, J.; Lombardi, A.; Werner, M. J.; Marzocchi, W.

2009-12-01

Empirical and statistical models of clustered seismicity are usually strongly stochastic and perceived to be uninformative in their forecasts, since only marginal distributions are used, such as the Omori-Utsu and Gutenberg-Richter laws. In contrast, so-called physics-based aftershock models, based on seismic rate changes calculated from Coulomb stress changes and rate-and-state friction, make more specific predictions: anisotropic stress shadows and multiplicative rate changes. We test the predictive power of models based on Coulomb stress changes against statistical models, including the popular Short Term Earthquake Probabilities and Epidemic-Type Aftershock Sequences models: We score and compare retrospective forecasts on the aftershock sequences of the 1992 Landers, USA, the 1997 Colfiorito, Italy, and the 2008 Selfoss, Iceland, earthquakes. To quantify predictability, we use likelihood-based metrics that test the consistency of the forecasts with the data, including modified and existing tests used in prospective forecast experiments within the Collaboratory for the Study of Earthquake Predictability (CSEP). Our results indicate that a statistical model performs best. Moreover, two Coulomb model classes seem unable to compete: Models based on deterministic Coulomb stress changes calculated from a given fault-slip model, and those based on fixed receiver faults. One model of Coulomb stress changes does perform well and sometimes outperforms the statistical models, but its predictive information is diluted, because of uncertainties included in the fault-slip model. Our results suggest that models based on Coulomb stress changes need to incorporate stochastic features that represent model and data uncertainty.

Coulomb-free and Coulomb-distorted recolliding quantum orbits in photoelectron holography

NASA Astrophysics Data System (ADS)

Maxwell, A. S.; Figueira de Morisson Faria, C.

2018-06-01

We perform a detailed analysis of the different types of orbits in the Coulomb quantum orbit strong-field approximation (CQSFA), ranging from direct to those undergoing hard collisions. We show that some of them exhibit clear counterparts in the standard formulations of the strong-field approximation for direct and rescattered above-threshold ionization, and show that the standard orbit classification commonly used in Coulomb-corrected models is over-simplified. We identify several types of rescattered orbits, such as those responsible for the low-energy structures reported in the literature, and determine the momentum regions in which they occur. We also find formerly overlooked interference patterns caused by backscattered Coulomb-corrected orbits and assess their effect on photoelectron angular distributions. These orbits improve the agreement of photoelectron angular distributions computed with the CQSFA with the outcome of ab initio methods for high energy phtotoelectrons perpendicular to the field polarization axis.

Sub-Nanosecond Lifetime Measurement Using the Recoil-Distance Method

PubMed Central

Wu, Ching-Yen

2000-01-01

The electromagnetic properties of low-lying nuclear states are a sensitive probe of both collective and single-particle degrees of freedom in nuclear structure. The recoil-distance technique provides a very reliable, direct and precise method for measuring lifetimes of nuclear states with lifetimes ranging from less than one to several hundred picoseconds. This method complements the powerful, but complicated, heavy-ion induced Coulomb excitation technique for measuring electromagnetic properties. The recoil distance technique has been combined with heavy-ion induced Coulomb excitation to study a variety of problems. Examples discussed are: study of the two-phonon triplet in 110Pd, coupling of the β and γ degrees of freedom in 182,184W, highly deformed γ bands in 165Ho, octupole collectivity in 96Zr, and opposite parity states in 153Eu. Consistency between the Coulomb excitation results and the lifetime measurements confirms the reliability of the complex analysis often encountered in heavy-ion induced Coulomb excitation work. PMID:27551588

Itinerant electrons in the Coulomb phase

NASA Astrophysics Data System (ADS)

Jaubert, L. D. C.; Piatecki, Swann; Haque, Masudul; Moessner, R.

2012-02-01

We study the interplay between magnetic frustration and itinerant electrons. For example, how does the coupling to mobile charges modify the properties of a spin liquid, and does the underlying frustration favor insulating or conducting states? Supported by Monte Carlo simulations, our goal is in particular to provide an analytical picture of the mechanisms involved. The models under consideration exhibit Coulomb phases in two and three dimensions, where the itinerant electrons are coupled to the localized spins via double exchange interactions. Because of the Hund coupling, magnetic loops naturally emerge from the Coulomb phase and serve as conducting channels for the mobile electrons, leading to doping-dependent rearrangements of the loop ensemble in order to minimize the electronic kinetic energy. At low electron density ρ, the double exchange coupling mainly tends to segment the very long loops winding around the system into smaller ones while it gradually lifts the extensive degeneracy of the Coulomb phase with increasing ρ. For higher doping, the results are strongly lattice dependent, displaying loop crystals with a given loop length for some specific values of ρ. By varying ρ, they can melt into different mixtures of these loop crystals, recovering extensive degeneracy in the process. Finally, we contrast this to the qualitatively different behavior of analogous models on kagome or triangular lattices.

Dynamic study of excited state hydrogen-bonded complexes of harmane in cyclohexane-toluene mixtures.

PubMed

Carmona, Carmen; Balón, Manuel; Galán, Manuel; Guardado, Pilar; Muñoz, María A

2002-09-01

Photoinduced proton transfer reactions of harmane or 1-methyl-9H-pyrido[3,4-b]indole (HN) in the presence of the proton donor hexafluoroisopropanol (HFIP) in cyclohexane-toluene mixtures (CY-TL; 10% vol/vol of TL) have been studied. Three excited state species have been identified: a 1:2 hydrogen-bonded proton transfer complex (PTC), between the pyridinic nitrogen of the substrate and the proton donor, a hydrogen-bonded cation-like exciplex (CL*) with a stoichiometry of at least 1:3 and a zwitterionic exciplex (Z*). Time-resolved fluorescence measurements evidence that upon excitation of ground state PTC, an excited state equilibrium is established between PTC* and the cationlike exciplex, CL*, lambdaem approximately/= 390 nm. This excited state reaction is assisted by another proton donor molecule. Further reaction of CL* with an additional HFIP molecule produces the zwitterionic species, Z*, lambda(em) approximately/= 500 nm. From the analysis of the multiexponential decays, measured at different emission wavelengths and as a function of HFIP concentration, the mechanism of these excited state reactions has been established. Thus, three rate constants and three reciprocal lifetimes have been determined. The simultaneous study of 1,9-dimethyl-9H-pyrido[3,4-b]indole (MHN) under the same experimental conditions has helped to understand the excited state kinetics of these processes.

Resonant inelastic x-ray scattering study of charge excitations in superconducting and nonsuperconducting PrFeAsO₁₋ y

DOE PAGES

Jarrige, I.; Nomura, T.; Ishii, K.; ...

2012-09-05

We report the first observation by momentum-resolved resonant inelastic x-ray scattering of charge excitations in an iron-based superconductor and its parent compound, PrFeAsO₀.₇ and PrFeAsO, respectively, with two main results. First, using calculations based on a 16-band dp model, we show that the energy of the lowest-lying excitations, identified as dd interband transitions of dominant xz,yz orbital character, exhibits a dramatic dependence on electron correlation. This enables us to estimate the Coulomb repulsion U and Hund's coupling J, and to highlight the role played by J in these peculiar orbital-dependent electron correlation effects. Second, we show that short-range antiferromagnetic correlations,more » which are a prerequisite to the occurrence of these excitations at the Γ point, are still present in the superconducting state.« less

An equation of state for partially ionized plasmas: The Coulomb contribution to the free energy

NASA Astrophysics Data System (ADS)

Kilcrease, D. P.; Colgan, J.; Hakel, P.; Fontes, C. J.; Sherrill, M. E.

2015-09-01

We have previously developed an equation of state (EOS) model called ChemEOS (Hakel and Kilcrease, Atomic Processes in Plasmas, Eds., J. Cohen et al., AIP, 2004) for a plasma of interacting ions, atoms and electrons. It is based on a chemical picture of the plasma and is derived from an expression for the Helmholtz free energy of the interacting species. All other equilibrium thermodynamic quantities are then obtained by minimizing this free energy subject to constraints, thus leading to a thermodynamically consistent EOS. The contribution to this free energy from the Coulomb interactions among the particles is treated using the method of Chabrier and Potekhin (Phys. Rev. E 58, 4941 (1998)) which we have adapted for partially ionized plasmas. This treatment is further examined and is found to give rise to unphysical behavior for various elements at certain values of the density and temperature where the Coulomb coupling begins to become significant and the atoms are partially ionized. We examine the source of this unphysical behavior and suggest corrections that produce acceptable results. The sensitivity of the thermodynamic properties and frequency-dependent opacity of iron is examined with and without these corrections. The corrected EOS is used to determine the fractional ion populations and level populations for a new generation of OPLIB low-Z opacity tables currently being prepared at Los Alamos National Laboratory with the ATOMIC code.

Ab initio study of the ground and excited electronic states of the methyl radical

PubMed Central

Zanchet, A.; Bañares, L.; Senent, M. L.; García-Vela, A.

2016-01-01

The ground and some excited electronic states of the methyl radical have been characterized by means of highly correlated ab intio techniques. The specific excited states investigated are those involved in the dissociation of the radical, namely the 3s and 3pz Rydberg states, and the A1 and B1 valence states crossing them, respectively. The C-H dissociative coordinate and the HCH bending angle were considered in order to generate the first two-dimensional ab initio representation of the potential surfaces of the above electronic states of CH3, along with the nonadiabatic couplings between them. Spectroscopic constants and frequencies calculated for the ground and bound excited states agree well with most of the available experimental data. Implications of the shape of the excited potential surfaces and couplings for the dissociation pathways of CH3 are discussed in the light of recent experimental results for dissociation from low-lying vibrational states of CH3. Based on the ab initio data some predictions are made regarding methyl photodissociation from higher initial vibrational states. PMID:27892569

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.

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

PubMed

Stone, Philip M; Kim, Yong-Ki

2004-01-01

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

Effect of xenon on the excited states of phototropic receptor flavin in corn seedlings

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

Vierstra, R.D.; Poff, K.L.; Walker, E.B.

1981-05-01

The chemically inert, water-soluble heavy atom gas, xenon, at millimolar concentrations specifically quenches the triplet excited state of flavin in solution without quenching the flavin singlet excited state. The preferential quenching of the flavin triplet over the singlet excited state by Xe has been established by showing that the flavin triplet-sensitized photooxidation of NADH is inhibited while the fluorescence intensity and lifetime of flavin are not affected by Xe. No significant inhibition of phototropism and geotropism by Xe was observed, suggesting that a flavin singlet state is more likely involved than the triplet state in the primary photoprocess of phototropismmore » in corn.« less

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

NASA Technical Reports Server (NTRS)

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

2002-01-01

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

Protolytic dissociation of cyano derivatives of naphthol, biphenyl and phenol in the excited state: A review

NASA Astrophysics Data System (ADS)

Szczepanik, Beata

2015-11-01

The excited state proton transfer (ESPT) has been extensively studied for hydroxyarenes, phenols, naphthols, hydroxystilbenes, etc., which undergo large enhancement of acidity upon electronic excitation, thus classified as photoacids. The changes of acidic character in the excited state of cyano-substituted derivatives of phenol, hydroxybiphenyl and naphthol are reviewed in this paper. The acidity constants pKa in the ground state (S0), pKa∗ in the first singlet excited state (S1) and the change of the acidity constant in the excited state ΔpKa for the discussed compounds are summarized and compared. The results of the acidity studies show, that the "electro-withdrawing" CN group in the molecules of naphthol, hydroxybiphenyl and phenol causes dramatic increase of their acidity in the excited state in comparison to the ground state. This effect is greatest for the cyanonaphthols (the doubly substituted CN derivatives are almost as strong as a mineral acid in the excited state), comparable for cyanobiphenyls, and smaller for phenol derivatives. The increase of acidity enables proton transfer to various organic solvents, and the investigation of ESPT can be extended to a variety of solvents besides water. The results of theoretical investigations were also presented and used for understanding the protolytic equilibria of cyano derivatives of naphthol, hydroxybiphenyl and phenol.

Exact finite volume expectation values of local operators in excited states

NASA Astrophysics Data System (ADS)

Pozsgay, B.; Szécsényi, I. M.; Takács, G.

2015-04-01

We present a conjecture for the exact expression of finite volume expectation values in excited states in integrable quantum field theories, which is an extension of an earlier conjecture to the case of general diagonal factorized scattering with bound states and a nontrivial bootstrap structure. The conjectured expression is a spectral expansion which uses the exact form factors and the excited state thermodynamic Bethe Ansatz as building blocks. The conjecture is proven for the case of the trace of the energy-moment tensor. Concerning its validity for more general operators, we provide numerical evidence using the truncated conformal space approach. It is found that the expansion fails to be well-defined for small values of the volume in cases when the singularity structure of the TBA equations undergoes a non-trivial rearrangement under some critical value of the volume. Despite these shortcomings, the conjectured expression is expected to be valid for all volumes for most of the excited states, and as an expansion above the critical volume for the rest.

Energies of Screened Coulomb Potentials.

ERIC Educational Resources Information Center

Lai, C. S.

1979-01-01

This article shows that, by applying the Hellman-Feynman theorem alone to screened Coulomb potentials, the first four coefficients in the energy series in powers of the perturbation parameter can be obtained from the unperturbed Coulomb system. (Author/HM)

Emergent low-energy bound states in the two-orbital Hubbard model

NASA Astrophysics Data System (ADS)

Núñez-Fernández, Y.; Kotliar, G.; Hallberg, K.

2018-03-01

A repulsive Coulomb interaction between electrons in different orbitals in correlated materials can give rise to bound quasiparticle states. We study the nonhybridized two-orbital Hubbard model with intra- (inter)orbital interaction U (U12) and different bandwidths using an improved dynamical mean-field theory numerical technique which leads to reliable spectra on the real energy axis directly at zero temperature. We find that a finite density of states at the Fermi energy in one band is correlated with the emergence of well-defined quasiparticle states at excited energies Δ =U -U12 in the other band. These excitations are interband holon-doublon bound states. At the symmetric point U =U12 , the quasiparticle peaks are located at the Fermi energy, leading to a simultaneous and continuous Mott transition settling a long-standing controversy.

Excited-state dynamics of mononucleotides and DNA strands in a deep eutectic solvent.

PubMed

Zhang, Yuyuan; de La Harpe, Kimberly; Hariharan, Mahesh; Kohler, Bern

2018-04-17

The photophysics of several mono- and oligonucleotides were investigated in a deep eutectic solvent for the first time. The solvent glyceline, prepared as a 1 : 2 mole ratio mixture of choline chloride and glycerol, was used to study excited-state deactivation in a non-aqueous solvent by the use of steady-state and time-resolved spectroscopy. DNA strands in glyceline retain the secondary structures that are present in aqueous solution to some degree, thus enabling a study of the effects of solvent properties on the excited states of stacked bases and stacked base pairs. The excited-state lifetime of the mononucleotide 5'-AMP in glyceline is 630 fs, or twice as long as in aqueous solution. Even slower relaxation is seen for 5'-TMP in glyceline, and a possible triplet state with a lifetime greater than 3 ns is observed. Circular dichroism spectra show that the single strand (dA)18 and the duplex d(AT)9·d(AT)9 adopt similar structures in glyceline and in aqueous solution. Despite having similar conformations in both solvents, femtosecond transient absorption experiments reveal striking changes in the dynamics. Excited-state decay and vibrational cooling generally take place more slowly in glyceline than in water. Additionally, the fraction of long-lived excited states in both oligonucleotide systems is lower in glyceline than in aqueous solution. For a DNA duplex, water is suggested to favor decay pathways involving intrastrand charge separation, while the deep eutectic solvent favors interstrand deactivation channels involving neutral species. Slower solvation dynamics in the viscous deep eutectic solvent may also play a role. These results demonstrate that the dynamics of excitations in stacked bases and stacked base pairs depend not only on conformation, but are also highly sensitive to the solvent.

Experimental and Theoretical Investigations of Doubly-excited Sextet States in

NASA Astrophysics Data System (ADS)

Lin, Bin; Berry, H. Gordon; Livingston, A. Eugene; Garnir, Henri-Pierre; Bastin, Thierry; Désesquelles, J.

2002-05-01

The energies and wave functions of the highly doubly-excited sextet states of boron-like O IV, F V and Ne VI are calculated with the Multi-Configuration Hartree-Fock (MCHF) plus the hydrogen-like QED effects and higher-order corrections method. The highly doubly-excited sextet states of boron-like O IV, F V and Ne VI are well above several ionization levels and metastable, and possible candidates for XUV- and soft x-ray laser and energy storage. Three doubly-excited sextet configurations (1s2s2p3 6So, 1s2s2p23s 6P and 1s2p33s 6So) are studied. The wavelengths of electric dipole transitions from the inner-shell excited terms 1s2s2p23s 6P-1s2p33s 6So are investigated by the beam-foil spectroscopy in the XUV spectral region. The predicted transition wavelengths agree with the experiment to 0.08Å. The higher-order corrections and fine structures are found to be critically important in these comparisons.

Charge transfer excitons and image potential states on organic semiconductor surfaces

NASA Astrophysics Data System (ADS)

Yang, Qingxin; Muntwiler, Matthias; Zhu, X.-Y.

2009-09-01

We report two types of excited electronic states on organic semiconductor surfaces: image potential states (IPS) and charge transfer excitons (CTE). In the former, an excited electron is localized in the surface-normal direction by the image potential and delocalized in the surface plane. In the latter, the electron is localized in all directions by both the image potential and the Coulomb potential from a photogenerated hole on an organic molecule. We use crystalline pentacene and tetracene surfaces as model systems, and time- and angle-resolved two-photon photoemission spectroscopy to probe the energetics and dynamics of both the IPS and the CTE states. On either pentacene or tetracene surfaces, we observe delocalized image bands and a series of CT excitons with binding energies <0.5eV below the image-band minimum. The binding energies of these CT excitons agree well with solutions to the atomic-H-like Schrödinger equation based on the image potential and the electron-hole Coulomb potential. We hypothesize that the formation of CT excitons should be general to the surfaces of organic semiconductors where the relatively narrow valance-band width facilitates the localization of the hole and the low dielectric constant ensures strong electron-hole attraction.

Application of spectroscopy and super-resolution microscopy: Excited state

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

Bhattacharjee, Ujjal

Photophysics of inorganic materials and organic molecules in complex systems have been extensively studied with absorption and emission spectroscopy.1-4 Steady-state and time-resolved fluorescence studies are commonly carried out to characterize excited-state properties of fluorophores. Although steady-state fluorescence measurements are widely used for analytical applications, time-resolved fluorescence measurements provide more detailed information about excited-state properties and the environment in the vicinity of the fluorophore. Many photophysical processes, such as photoinduced electron transfer (PET), rotational reorientation, solvent relaxation, and energy transfer, occur on a nanosecond (10 -9 s) timescale, thus affecting the lifetime of the fluorophores. Moreover, time-resolved microscopy methods, such asmore » lifetimeimaging, combine the benefits of the microscopic measurement and information-rich, timeresolved data. Thus, time-resolved fluorescence spectroscopy combined with microscopy can be used to quantify these processes and to obtain a deeper understanding of the chemical surroundings of the fluorophore in a small area under investigation. This thesis discusses various photophysical and super-resolution microscopic studies of organic and inorganic materials, which have been outlined below.« less

New Theoretical Developments in Exploring Electronically Excited States: Including Localized Configuration Interaction Singles and Application to Large Helium Clusters

NASA Astrophysics Data System (ADS)

Closser, Kristina Danielle

This thesis presents new developments in excited state electronic structure theory. Contrasted with the ground state, the electronically excited states of atoms and molecules often are unstable and have short lifetimes, exhibit a greater diversity of character and are generally less well understood. The very unusual excited states of helium clusters motivated much of this work. These clusters consist of large numbers of atoms (experimentally 103--109 atoms) and bands of nearly degenerate excited states. For an isolated atom the lowest energy excitation energies are from 1s → 2s and 1s → 2 p transitions, and in clusters describing the lowest energy band minimally requires four states per atom. In the ground state the clusters are weakly bound by van der Waals interactions, however in the excited state they can form well-defined covalent bonds. The computational cost of quantum chemical calculations rapidly becomes prohibitive as the size of the systems increase. Standard excited-state methods such as configuration interaction singles (CIS) and time-dependent density functional theory (TD-DFT) can be used with ≈100 atoms, and are optimized to treat only a few states. Thus, one of our primary aims is to develop a method which can treat these large systems with large numbers of nearly degenerate excited states. Additionally, excited states are generally formed far from their equilibrium structures. Vertical excitations from the ground state induce dynamics in the excited states. Thus, another focus of this work is to explore the results of these forces and the fate of the excited states. Very little was known about helium cluster excited states when this work began, thus we first investigated the excitations in small helium clusters consisting of 7 or 25 atoms using CIS. The character of these excited states was determined using attachment/detachment density analysis and we found that in the n = 2 manifold the excitations could generally be interpreted as

Coulomb Blockade Plasmonic Switch.

PubMed

Xiang, Dao; Wu, Jian; Gordon, Reuven

2017-04-12

Tunnel resistance can be modulated with bias via the Coulomb blockade effect, which gives a highly nonlinear response current. Here we investigate the optical response of a metal-insulator-nanoparticle-insulator-metal structure and show switching of a plasmonic gap from insulator to conductor via Coulomb blockade. By introducing a sufficiently large charging energy in the tunnelling gap, the Coulomb blockade allows for a conductor (tunneling) to insulator (capacitor) transition. The tunnelling electrons can be delocalized over the nanocapacitor again when a high energy penalty is added with bias. We demonstrate that this has a huge impact on the plasmonic resonance of a 0.51 nm tunneling gap with ∼70% change in normalized optical loss. Because this structure has a tiny capacitance, there is potential to harness the effect for high-speed switching.

Structures and Binding Energies of the Naphthalene Dimer in Its Ground and Excited States.

PubMed

Dubinets, N O; Safonov, A A; Bagaturyants, A A

2016-05-05

Possible structures of the naphthalene dimer corresponding to local energy minima in the ground and excited (excimer) electronic states are comprehensively investigated using DFT-D and TDDFT-D methods with a special accent on the excimer structures. The corresponding binding and electronic transition energies are calculated, and the nature of the electronic states in different structures is analyzed. Several parallel (stacked) and T-shaped structures were found in both the ground and excited (excimer) states in a rather narrow energy range. The T-shaped structure with the lowest energy in the excited state exhibits a marked charge transfer from the upright molecule to the base one.

Excitation energy dependence of excited states dynamics in all- trans-carotenes determined by femtosecond absorption and fluorescence spectroscopy

NASA Astrophysics Data System (ADS)

Kosumi, Daisuke; Yanagi, Kazuhiro; Nishio, Tomohiro; Hashimoto, Hideki; Yoshizawa, Masayuki

2005-06-01

Ultrafast relaxation kinetics in β-carotene and lycopene has been investigated by femtosecond absorption and fluorescence spectroscopies using tunable excitation pulses. The transient signals induced by the photoexcitation with larger excess energy have broader bands and longer lifetimes both in the 11Bu+and21Ag- excited states. The excess vibrational energy remains longer than several picoseconds and slows the relaxation kinetics in carotenoids.

Driven similarity renormalization group for excited states: A state-averaged perturbation theory

NASA Astrophysics Data System (ADS)

Li, Chenyang; Evangelista, Francesco A.

2018-03-01

The multireference driven similarity renormalization group (MRDSRG) approach [C. Li and F. A. Evangelista, J. Chem. Theory Comput. 11, 2097 (2015)] is generalized to treat quasi-degenerate electronic excited states. The new scheme, termed state-averaged (SA) MRDSRG, is a state-universal approach that considers an ensemble of quasi-degenerate states on an equal footing. Using the SA-MRDSRG framework, we implement second- (SA-DSRG-PT2) and third-order (SA-DSRG-PT3) perturbation theories. These perturbation theories can treat a manifold of near-degenerate states at the cost of a single state-specific computation. At the same time, they have several desirable properties: (1) they are intruder-free and size-extensive, (2) their energy expressions can be evaluated non-iteratively and require at most the three-body density cumulant of the reference states, and (3) the reference states are allowed to relax in the presence of dynamical correlation effects. Numerical benchmarks on the potential energy surfaces of lithium fluoride, ammonia, and the penta-2,4-dieniminium cation reveal that the SA-DSRG-PT2 method yields results with accuracy similar to that of other second-order quasi-degenerate perturbation theories. The SA-DSRG-PT3 results are instead consistent with those from multireference configuration interaction with singles and doubles (MRCISD). Finally, we compute the vertical excitation energies of (E,E)-1,3,5,7-octatetraene. The ordering of the lowest three states is predicted to be 2 1Ag-<1 1Bu+<1 1Bu- by both SA-DSRG-PT2 and SA-DSRG-PT3, in accordance with MRCISD plus Davidson correction.

Two-photon excitation of 2,5-diphenyloxazole using a low power green solid state laser

NASA Astrophysics Data System (ADS)

Luchowski, Rafal

2011-01-01

This Letter concerns two-photon excitation of 2,5-diphenyloxazole (PPO) upon illumination from a pulsed 532 nm solid state laser, with an average power of 30 mW, and a repetition rate of 20 MHz. A very agreeable emission spectrum position and shape has been achieved for PPO receiving one- and two-photon excitation, which suggests that the same excited state is involved for both excitation modes. Also, a perfect quadratic dependence of laser power in the emission intensity function has been recorded. We tested the application of a small solid state green laser to two-photon induced time-resolved fluorescence, revealing the emission anisotropy of PPO to be considerably higher for two-photon than for one-photon excitation.

Electron molecular ion recombination: product excitation and fragmentation.

PubMed

Adams, Nigel G; Poterya, Viktoriya; Babcock, Lucia M

2006-01-01

Electron-ion dissociative recombination is an important ionization loss process in any ionized gas containing molecular ions. This includes the interstellar medium, circumstellar shells, cometary comae, planetary ionospheres, fusion plasma boundaries, combustion flames, laser plasmas and chemical deposition and etching plasmas. In addition to controlling the ionization density, the process generates many radical species, which can contribute to a parallel neutral chemistry. Techniques used to obtain rate data and product information (flowing afterglows and storage rings) are discussed and recent data are reviewed including diatomic to polyatomic ions and cluster ions. The data are divided into rate coefficients and cross sections, including their temperature/energy dependencies, and quantitative identification of neutral reaction products. The latter involve both ground and electronically excited states and including vibrational excitation. The data from the different techniques are compared and trends in the data are examined. The reactions are considered in terms of the basic mechanisms (direct and indirect processes including tunneling) and recent theoretical developments are discussed. Finally, new techniques are mentioned (for product identification; electrostatic storage rings, including single and double rings; Coulomb explosion) and new ways forward are suggested.

Ab initio excited states from the in-medium similarity renormalization group

NASA Astrophysics Data System (ADS)

Parzuchowski, N. M.; Morris, T. D.; Bogner, S. K.

2017-04-01

We present two new methods for performing ab initio calculations of excited states for closed-shell systems within the in-medium similarity renormalization group (IMSRG) framework. Both are based on combining the IMSRG with simple many-body methods commonly used to target excited states, such as the Tamm-Dancoff approximation (TDA) and equations-of-motion (EOM) techniques. In the first approach, a two-step sequential IMSRG transformation is used to drive the Hamiltonian to a form where a simple TDA calculation (i.e., diagonalization in the space of 1 p 1 h excitations) becomes exact for a subset of eigenvalues. In the second approach, EOM techniques are applied to the IMSRG ground-state-decoupled Hamiltonian to access excited states. We perform proof-of-principle calculations for parabolic quantum dots in two dimensions and the closed-shell nuclei 16O and 22O. We find that the TDA-IMSRG approach gives better accuracy than the EOM-IMSRG when calculations converge, but it is otherwise lacking the versatility and numerical stability of the latter. Our calculated spectra are in reasonable agreement with analogous EOM-coupled-cluster calculations. This work paves the way for more interesting applications of the EOM-IMSRG approach to calculations of consistently evolved observables such as electromagnetic strength functions and nuclear matrix elements, and extensions to nuclei within one or two nucleons of a closed shell by generalizing the EOM ladder operator to include particle-number nonconserving terms.

Coupling between graphene and intersubband collective excitations in quantum wells

NASA Astrophysics Data System (ADS)

Gonzalez de la Cruz, G.

2017-08-01

Recently, strong light-matter coupling between the electromagnetic modes in plasmonic metasurfaces with quantum-engineering electronic intersubband transitions in quantum wells has been demonstrated experimentally (Benz et al., [14], Lee et al., [15]). These novel materials combining different two-dimensional electronic systems offer new opportunities for tunable optical devices and fundamental studies of collective excitations driven by interlayer Coulomb interactions. In this work, our aim is to study the plasmon spectra of a hybrid structure consisting of conventional two-dimensional electron gas (2DEG) in a semiconductor quantum well and a graphene sheet with an interlayer separation of a. This electronic bilayer structure is immersed in a nonhomgeneous dielectric background of the system. We use a simple model in which the graphene surface plasmons and both; the intrasubband and intersubband collective electron excitations in the quantum well are coupled via screened Coulomb interaction. Here we calculate the dispersion of these relativistic/nonrelativistic new plasmon modes taking into account the thickness of the quantum well providing analytical expressions in the long-wavelength limit.

Routes to formation of highly excited neutral atoms in the break-up of strongly driven hydrogen molecule

NASA Astrophysics Data System (ADS)

Emmanouilidou, Agapi

2012-06-01

We present a theoretical quasiclassical treatment of the formation, during Coulomb explosion, of highly excited neutral H atoms for strongly-driven hydrogen molecule. This process, where after the laser field is turned off, one electron escapes to the continuum while the other occupies a Rydberg state, was recently reported in an experimental study in Phys. Rev. Lett 102, 113002 (2009). We find that two-electron effects are important in order to correctly account for all pathways leading to highly excited neutral hydrogen formation [1]. We identify two pathways where the electron that escapes to the continuum does so either very quickly or after remaining bound for a few periods of the laser field. These two pathways of highly excited neutral H formation have distinct traces in the probability distribution of the escaping electron momentum components. [4pt] [1] A. Emmanouilidou, C. Lazarou, A. Staudte and U. Eichmann, Phys. Rev. A (Rapid) 85 011402 (2012).

The laser versus the lamp: Reactivity of the diphenyl ketyl radical in the ground and excited states

NASA Astrophysics Data System (ADS)

Baumann, H.; Merckel, C.; Timpe, H.-J.; Graness, A.; Kleinschmidt, J.; Gould, I. R.; Turro, N. J.

1984-01-01

The diphenyl ketyl radical which is formed upon photolysis of α-phenyl benzoin is produced in its excited state upon intense pulsed laser irradiation. Using the techniques of time-resolved absorption and emission spectroscopy, reaction rate constants for the ground and excited states of this radical were obtained. For the radical quenchers employed, the excited state reactivity is found to be typically several orders of magnitude greater than that of the ground state. It is concluded that the excited state of diphenyl ketyl radical reacts predominantly by electron transfer processes.

Quantum mechanical identification of quadrupolar plasmonic excited states in silver nanorods

DOE PAGES

Gieseking, Rebecca L.; Ratner, Mark A.; Schatz, George C.

2016-10-27

Quadrupolar plasmonic modes in noble metal nanoparticles have gained interest in recent years for various sensing applications. Although quantum mechanical studies have shown that dipolar plasmons can be modeled in terms of excited states where several to many excitations contribute coherently to the transition dipole moment, new approaches are needed to identify the quadrupolar plasmonic states. We show that quadrupolar states in Ag nanorods can be identified using the semiempirical INDO/SCI approach by examining the quadrupole moment of the transition density. The main longitudinal quadrupolar states occur at higher energies than the longitudinal dipolar states, in agreement with previous classicalmore » electrodynamics results, and have collective plasmonic character when the nanorods are sufficiently long. In conclusion, the ability to identify these states will make it possible to evaluate the differences between dipolar and quadrupolar plasmons that are relevant for sensing applications.« less

Spin texture and magnetoroton excitations at nu=1/3.

PubMed

Groshaus, Javier G; Dujovne, Irene; Gallais, Yann; Hirjibehedin, Cyrus F; Pinczuk, Aron; Tan, Yan-Wen; Stormer, Horst; Dennis, Brian S; Pfeiffer, Loren N; West, Ken W

2008-02-01

Neutral spin texture (ST) excitations at nu=1/3 are directly observed for the first time by resonant inelastic light scattering. They are determined to involve two simultaneous spin flips. At low magnetic fields, the ST energy is below that of the magnetoroton minimum. With increasing in-plane magnetic field these mode energies cross at a critical ratio of the Zeeman and Coulomb energies of eta(c)=0.020+/-0.001. Surprisingly, the intensity of the ST mode grows with temperature in the range in which the magnetoroton modes collapse. The temperature dependence is interpreted in terms of a competition between coexisting phases supporting different excitations. We consider the role of the ST excitations in activated transport at nu=1/3.

Observation of Excited Quadrupole-Bound States in Cold Anions

NASA Astrophysics Data System (ADS)

Zhu, Guo-Zhu; Liu, Yuan; Wang, Lai-Sheng

2017-07-01

We report the first observation of an excited quadrupole-bound state (QBS) in an anion. High-resolution photoelectron imaging of cryogenically cooled 4-cyanophenoxide (4 CP- ) anions yields an electron detachment threshold of 24 927 cm-1 . The photodetachment spectrum reveals a resonant transition 20 cm-1 below the detachment threshold, which is attributed to an excited QBS of 4 CP- because neutral 4CP has a large quadrupole moment with a negligible dipole moment. The QBS is confirmed by observation of seventeen above-threshold resonances due to autodetachment from vibrational levels of the QBS.

Effect of Coulomb stress on the Gutenberg-Richter law

NASA Astrophysics Data System (ADS)

Navas-Portella, V.; Corral, A.; Jimenez, A.

2017-12-01

Coulomb stress theory has been used for years in seismology to understand how earthquakes trigger each other. Whenever an earthquake occurs, the stress field changes in its neighbourhood, with places with positive values brought closer to failure, whereas negative values distance away that location from failure. Earthquake models that relate rate changes and Coulomb stress after a main event, such as the rate-and-state model, assume negative and positive stress values affect rate changes according to the same functional form. As a first order approximation, under uniform background seismicity before the main event, different values of the b-exponent in the Gutenberg-Richter law would indicate different behaviour for positive and negative stress. In this work, we study the Gutenberg-Richter law in the aftershock sequence of the Landers earthquake (California, 1992, MW=7.3). By using a statistically based fitting method, we discuss whether the sign of Coulomb stresses and the distance to the fault have a significant effect on the value of the b-exponent.

Correction of the near threshold behavior of electron collisional excitation cross-sections in the plane-wave Born approximation

DOE PAGES

Kilcrease, D. P.; Brookes, S.

2013-08-19

The modeling of NLTE plasmas requires the solution of population rate equations to determine the populations of the various atomic levels relevant to a particular problem. The equations require many cross sections for excitation, de-excitation, ionization and recombination. Additionally, a simple and computational fast way to calculate electron collisional excitation cross-sections for ions is by using the plane-wave Born approximation. This is essentially a high-energy approximation and the cross section suffers from the unphysical problem of going to zero near threshold. Various remedies for this problem have been employed with varying degrees of success. We present a correction procedure formore » the Born cross-sections that employs the Elwert–Sommerfeld factor to correct for the use of plane waves instead of Coulomb waves in an attempt to produce a cross-section similar to that from using the more time consuming Coulomb Born approximation. We compare this new approximation with other, often employed correction procedures. Furthermore, we also look at some further modifications to our Born Elwert procedure and its combination with Y.K. Kim's correction of the Coulomb Born approximation for singly charged ions that more accurately approximate convergent close coupling calculations.« less

Ab Initio Calculations of Singlet and Triplet Excited States of Chlorine Nitrate and Nitric Acid

NASA Technical Reports Server (NTRS)

Grana, Ana M.; Lee, Timothy J.; Head-Gordon, Martin; Langhoff, Stephen R. (Technical Monitor)

1994-01-01

Ab initio calculations of vertical excitations to singlet and triplet excited states of chlorine nitrate and nitric acid are reported. The nature of the electronic transitions are examined by decomposing the difference density into the sum of detachment and attachment densities. Counterparts for the three lowest singlet excited states of nitric acid survive relatively unperturbed in chlorine nitrate, while other low-lying singlet states of chlorine nitrate appear to be directly dissociative in the ClO chromophore. These results suggest an assignment of the two main peaks in the experimental chlorine nitrate absorption spectrum. In addition, triplet vertical excitations and the lowest optimized triplet geometries of both molecules are studied.

An equation of state for partially ionized plasmas: The Coulomb contribution to the free energy

DOE PAGES

Kilcrease, D. P.; Colgan, J.; Hakel, P.; ...

2015-06-20

We have previously developed an equation of state (EOS) model called ChemEOS (Hakel and Kilcrease, Atomic Processes in Plasmas, Eds., J. Cohen et al., AIP, 2004) for a plasma of interacting ions, atoms and electrons. It is based on a chemical picture of the plasma and is derived from an expression for the Helmholtz free energy of the interacting species. All other equilibrium thermodynamic quantities are then obtained by minimizing this free energy subject to constraints, thus leading to a thermodynamically consistent EOS. The contribution to this free energy from the Coulomb interactions among the particles is treated using themore » method of Chabrier and Potekhin (Phys. Rev. E 58, 4941 (1998)) which we have adapted for partially ionized plasmas. This treatment is further examined and is found to give rise to unphysical behavior for various elements at certain values of the density and temperature where the Coulomb coupling begins to become significant and the atoms are partially ionized. We examine the source of this unphysical behavior and suggest corrections that produce acceptable results. The sensitivity of the thermodynamic properties and frequency-dependent opacity of iron is examined with and without these corrections. Lastly, the corrected EOS is used to determine the fractional ion populations and level populations for a new generation of OPLIB low-Z opacity tables currently being prepared at Los Alamos National Laboratory with the ATOMIC code.« less

Dynamics of DNA breathing: weak noise analysis, finite time singularity, and mapping onto the quantum Coulomb problem.

PubMed

Fogedby, Hans C; Metzler, Ralf

2007-12-01

We study the dynamics of denaturation bubbles in double-stranded DNA on the basis of the Poland-Scheraga model. We show that long time distributions for the survival of DNA bubbles and the size autocorrelation function can be derived from an asymptotic weak noise approach. In particular, below the melting temperature the bubble closure corresponds to a noisy finite time singularity. We demonstrate that the associated Fokker-Planck equation is equivalent to a quantum Coulomb problem. Below the melting temperature, the bubble lifetime is associated with the continuum of scattering states of the repulsive Coulomb potential; at the melting temperature, the Coulomb potential vanishes and the underlying first exit dynamics exhibits a long time power law tail; above the melting temperature, corresponding to an attractive Coulomb potential, the long time dynamics is controlled by the lowest bound state. Correlations and finite size effects are discussed.

Excited-state decay processes of binuclear rhodium(I) isocyanide complexes

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

Miskowski, V.M.; Rice, S.F.; Gray, H.B.

1993-04-29

Emission lifetimes, quantum yields, and polarized excitation spectra of Rh[sub 2]b[sub 4][sup 2+] and Rh[sub 2](TMB)[sub 4][sup 2+] (b = 1,3-diisocyanopropane; TMB = 2,5-diisocyano-2,5-dimethylhexane) have been determined. The singlet and triplet d[sigma]* [yields] p[sigma]([sup 1,3]A[sub 2u]) excited states are luminescent with radiative rates of ca. 10[sup 8] and 10[sup 4] s[sup [minus

Excited states and electrochromism of radical cation of the carotenoid astaxanthin

NASA Astrophysics Data System (ADS)

Krawczyk, Stanisław

1998-09-01

Radical cations of the carotenoid astaxanthin were generated by chemical oxidation with Fe(Cl) 3, and their absorption and electroabsorption (Stark) spectra at temperatures about 150 K were recorded in the spectral range from 5900 to 26000 cm -1 (380 to 1700 nm), covering two absorptive electronic transitions from D 0 (ground) to D 1 and D 2 excited states. The changes in static polarizability are negative and equal -40±10 A 3 for D 0→D 1 and -105±15 A 3 for D 0→D 2, pointing that dominant contribution to polarizabilities results from the coupling of D 1 and D 2 with the ground state. An approximate localization of the next excited state with ground-state parity is estimated based on arguments from perturbation theory.

Electronically excited and ionized states in condensed phase: Theory and applications

NASA Astrophysics Data System (ADS)

Sadybekov, Arman

Predictive modeling of chemical processes in silico is a goal of XXI century. While robust and accurate methods exist for ground-state properties, reliable methods for excited states are still lacking and require further development. Electronically exited states are formed by interactions of matter with light and are responsible for key processes in solar energy harvesting, vision, artificial sensors, and photovoltaic applications. The greatest challenge to overcome on our way to a quantitative description of light-induced processes is accurate inclusion of the effect of the environment on excited states. All above mentioned processes occur in solution or solid state. Yet, there are few methodologies to study excited states in condensed phase. Application of highly accurate and robust methods, such as equation-of-motion coupled-cluster theory EOM-CC, is limited by a high computational cost and scaling precluding full quantum mechanical treatment of the entire system. In this thesis we present successful application of the EOM-CC family of methods to studies of excited states in liquid phase and build hierarchy of models for inclusion of the solvent effects. In the first part of the thesis we show that a simple gasphase model is sufficient to quantitatively analyze excited states in liquid benzene, while the latter part emphasizes the importance of explicit treatment of the solvent molecules in the case of glycine in water solution. In chapter 2, we use a simple dimer model to describe exciton formation in liquid and solid benzene. We show that sampling of dimer structures extracted from the liquid benzene is sufficient to correctly predict exited-state properties of the liquid. Our calculations explain experimentally observed features, which helped to understand the mechanism of the excimer formation in liquid benzene. Furthermore, we shed light on the difference between dimer configurations in the first solvation shell of liquid benzene and in unit cell of solid

Excited state baryon spectroscopy from lattice QCD

DOE PAGES

Robert G. Edwards; Dudek, Jozef J.; Richards, David G.; ...

2011-10-31

Here, we present a calculation of the Nucleon and Delta excited state spectrum on dynamical anisotropic clover lattices. A method for operator construction is introduced that allows for the reliable identification of the continuum spins of baryon states, overcoming the reduced symmetry of the cubic lattice. Using this method, we are able to determine a spectrum of single-particle states for spins up to and including $J = 7/2$, of both parities, the first time this has been achieved in a lattice calculation. We find a spectrum of states identifiable as admixtures of $SU(6) Ⓧ O(3)$ representations and a counting ofmore » levels that is consistent with the non-relativistic $qqq$ constituent quark model. This dense spectrum is incompatible with quark-diquark model solutions to the "missing resonance problem" and shows no signs of parity doubling of states.« less

Solvent control of charge transfer excited state relaxation pathways in [Fe(2,2'-bipyridine)(CN) 4] 2-

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

Kjær, Kasper S.; Kunnus, Kristjan; Harlang, Tobias C. B.

The excited state dynamics of solvated [Fe(bpy)(CN) 4] 2-, where bpy = 2,2'-bipyridine, show significant sensitivity to the solvent Lewis acidity. Using a combination of optical absorption and X-ray emission transient spectroscopies, we have previously shown that the metal to ligand charge transfer (MLCT) excited state of [Fe(bpy)(CN) 4] 2- has a 19 picosecond lifetime and no discernable contribution from metal centered (MC) states in weak Lewis acid solvents, such as dimethyl sulfoxide and acetonitrile. Here, in the present work, we use the same combination of spectroscopic techniques to measure the MLCT excited state relaxation dynamics of [Fe(bpy)(CN) 4] 2-more » in water, a strong Lewis acid solvent. The charge-transfer excited state is now found to decay in less than 100 femtoseconds, forming a quasi-stable metal centered excited state with a 13 picosecond lifetime. We find that this MC excited state has triplet ( 3MC) character, unlike other reported six-coordinate Fe(II)-centered coordination compounds, which form MC quintet ( 5MC) states. The solvent dependent changes in excited state non-radiative relaxation for [Fe(bpy)(CN) 4] 2- allows us to infer the influence of the solvent on the electronic structure of the complex. Lastly, the robust characterization of the dynamics and optical spectral signatures of the isolated 3MC intermediate provides a strong foundation for identifying 3MC intermediates in the electronic excited state relaxation mechanisms of similar Fe-centered systems being developed for solar applications.« less

Solvent control of charge transfer excited state relaxation pathways in [Fe(2,2'-bipyridine)(CN) 4] 2-

DOE PAGES

Kjær, Kasper S.; Kunnus, Kristjan; Harlang, Tobias C. B.; ...

2018-01-19

The excited state dynamics of solvated [Fe(bpy)(CN) 4] 2-, where bpy = 2,2'-bipyridine, show significant sensitivity to the solvent Lewis acidity. Using a combination of optical absorption and X-ray emission transient spectroscopies, we have previously shown that the metal to ligand charge transfer (MLCT) excited state of [Fe(bpy)(CN) 4] 2- has a 19 picosecond lifetime and no discernable contribution from metal centered (MC) states in weak Lewis acid solvents, such as dimethyl sulfoxide and acetonitrile. Here, in the present work, we use the same combination of spectroscopic techniques to measure the MLCT excited state relaxation dynamics of [Fe(bpy)(CN) 4] 2-more » in water, a strong Lewis acid solvent. The charge-transfer excited state is now found to decay in less than 100 femtoseconds, forming a quasi-stable metal centered excited state with a 13 picosecond lifetime. We find that this MC excited state has triplet ( 3MC) character, unlike other reported six-coordinate Fe(II)-centered coordination compounds, which form MC quintet ( 5MC) states. The solvent dependent changes in excited state non-radiative relaxation for [Fe(bpy)(CN) 4] 2- allows us to infer the influence of the solvent on the electronic structure of the complex. Lastly, the robust characterization of the dynamics and optical spectral signatures of the isolated 3MC intermediate provides a strong foundation for identifying 3MC intermediates in the electronic excited state relaxation mechanisms of similar Fe-centered systems being developed for solar applications.« less

Emergent low-energy bound states in the two-orbital Hubbard model

DOE PAGES

Nunez-Fernandez, Y.; Kotliar, G.; Hallberg, K.

2018-03-30

A repulsive Coulomb interaction between electrons in different orbitals in correlated materials can give rise to bound quasiparticle states. We study the nonhybridized two-orbital Hubbard model with intra- (inter)orbital interaction U (U 12) and different bandwidths using an improved dynamical mean-field theory numerical technique which leads to reliable spectra on the real energy axis directly at zero temperature. We find that a finite density of states at the Fermi energy in one band is correlated with the emergence of well-defined quasiparticle states at excited energies Δ = U - U 12 in the other band. These excitations are interband holon-doublonmore » bound states. At the symmetric point U = U 12, the quasiparticle peaks are located at the Fermi energy, leading to a simultaneous and continuous Mott transition settling a long-standing controversy.« less

"Bright" and "dark" excited states of an alternating at oligomer characterized by femtosecond broadband spectroscopy.

PubMed

Kwok, Wai-Ming; Ma, Chensheng; Phillips, David Lee

2009-08-20

The nature and dynamics of DNA excited states is of pivotal importance in determining both DNA ultraviolet photostability and its vulnerability toward photodamage. The complexity regarding the involvement of "bright" and "dark" excited states, their molecular origin, and the roles played by these states in the course of electronic energy relaxation constitute an active and contentious area in current research of DNA excited states. As a case study, we report here a combined broadband femtosecond time-resolved fluorescence (TRF) and transient absorption (TA) study on a self-complementary d(AT)(10) oligomer and a reference system of an equal molar mixture of the constituent bases represented by adenosine and thymidine (A+T). Comparison of the spectral character and temporal evolution of the TRF and TA data for 267 nm excited d(AT)(10) and A+T provides evidence for a base-localized excitation feature for an early (< approximately 50 fs) "bright" S(LE) state and its ensuing evolution within approximately 3 ps into a approximately 72 ps "dark" S(E) exciplex in d(AT)(10). Combined analysis of the d(AT)(10) TRF and TA results suggests the presence of a weakly fluorescent transient S(G) state that acts as a gateway to mediate the excitation transfer and energy elimination. A distinct base conformation-dependent model involving an ultrafast approximately 0.3 ps conversion of the S(LE) to S(G) that then evolves by approximately 3 ps into the S(E) has been proposed to account for the collective deactivation character of d(AT)(10). This presents a novel excited-state picture that can unify the seemingly conflicting time-resolved results reported previously for related AT DNAs. The direct spectral and dynamical data provided here contributes important photophysical parameters for the description of the excited states of AT oligomers. The possible connection between the energy transfer giving the S(E) and the photostability vs photodamage of A/T DNAs is briefly discussed.

Optimised effective potential for ground states, excited states, and time-dependent phenomena

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

Gross, E.K.U.

1996-12-31

(1) The optimized effective potential method is a variant of the traditional Kohn-Sham scheme. In this variant, the exchange-correlation energy E{sub xc} is an explicit functional of single-particle orbitals. The exchange-correlation potential, given as usual by the functional derivative v{sub xc} = {delta}E{sub xc}/{delta}{rho}, then satisfies as integral equation involving the single-particle orbitals. This integral equation in solved semi-analytically using a scheme recently proposed by Krieger, Li and Iafrate. If the exact (Fock) exchange-energy functional is employed together with the Colle-Salvetti orbital functional for the correlation energy, the mean absolute deviation of the resulting ground-state energies from the exact nonrelativisticmore » values is CT mH for the first-row atoms, as compared to 4.5 mH in a state-of-the-art CI calculation. The proposed scheme is thus significantly more accurate than the conventional Kohn-Sham method while the numerical effort involved is about the same as for an ordinary Hanree-Fock calculation. (2) A time-dependent generalization of the optimized-potential method is presented and applied to the linear-response regime. Since time-dependent density functional theory leads to a formally exact representation of the frequency-dependent linear density response and since the latter, as a function of frequency, has poles at the excitation energies of the fully interacting system, the formalism is suitable for the calculation of excitation energies. A simple additive correction to the Kohn-Sham single-particle excitation energies will be deduced and first results for atomic and molecular singlet and triplet excitation energies will be presented. (3) Beyond the regime of linear response, the time-dependent optimized-potential method is employed to describe atoms in strong emtosecond laser pulses. Ionization yields and harmonic spectra will be presented and compared with experimental data.« less

Role of excited state solvent fluctuations on time-dependent fluorescence Stokes shift

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

Li, Tanping, E-mail: tanping@lsu.edu, E-mail: revatik@lsu.edu; Kumar, Revati, E-mail: tanping@lsu.edu, E-mail: revatik@lsu.edu

2015-11-07

We explore the connection between the solvation dynamics of a chromophore upon photon excitation and equilibrium fluctuations of the solvent. Using molecular dynamics simulations, fluorescence Stokes shift for the tryptophan in Staphylococcus nuclease was examined using both nonequilibrium calculations and linear response theory. When the perturbed and unperturbed surfaces exhibit different solvent equilibrium fluctuations, the linear response approach on the former surface shows agreement with the nonequilibrium process. This agreement is excellent when the perturbed surface exhibits Gaussian statistics and qualitative in the case of an isomerization induced non-Gaussian statistics. However, the linear response theory on the unperturbed surface breaksmore » down even in the presence of Gaussian fluctuations. Experiments also provide evidence of the connection between the excited state solvent fluctuations and the total fluorescence shift. These observations indicate that the equilibrium statistics on the excited state surface characterize the relaxation dynamics of the fluorescence Stokes shift. Our studies specifically analyze the Gaussian fluctuations of the solvent in the complex protein environment and further confirm the role of solvent fluctuations on the excited state surface. The results are consistent with previous investigations, found in the literature, of solutes dissolved in liquids.« less

Inhibition of Radiolytic Molecular Hydrogen Formation by Quenching of Excited State Water

DOE PAGES

Horne, Gregory P.; Pimblott, Simon M.; LaVerne, Jay A.

2017-05-11

Comparison of experimental measurements of the yield of molecular hydrogen produced in the gamma radiolysis of water and aqueous nitrate solutions with predictions of a Monte Carlo track chemistry model shows that the nitrate anion scavenging of the hydrated electron, its precursor, and hydrogen atom cannot account for the observed decrease in the yield at high nitrate anion concentrations. Inclusion of the quenching of excited states of water (formed by either direct excitation or reaction of the water radical cation with the precursor to the hydrated electron) by the nitrate anion into the reaction scheme provides excellent agreement between themore » stochastic calculations and experiment demonstrating the existence of this short-lived species and its importance in water radiolysis. Energy transfer from the excited states of water to the nitrate anion producing an excited state provides an additional pathway for the production of nitrogen containing products not accounted for in traditional radiation chemistry scenarios. Such reactions are of central importance in predicting the behavior of liquors common in the reprocessing of spent nuclear fuel and the storage of highly radioactive liquid waste prior to vitrification.« less

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

NASA Astrophysics Data System (ADS)

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

2012-12-01

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

Level Anticrossing of Impurity States in Semiconductor Nanocrystals

PubMed Central

Baimuratov, Anvar S.; Rukhlenko, Ivan D.; Turkov, Vadim K.; Ponomareva, Irina O.; Leonov, Mikhail Yu.; Perova, Tatiana S.; Berwick, Kevin; Baranov, Alexander V.; Fedorov, Anatoly V.

2014-01-01

The size dependence of the quantized energies of elementary excitations is an essential feature of quantum nanostructures, underlying most of their applications in science and technology. Here we report on a fundamental property of impurity states in semiconductor nanocrystals that appears to have been overlooked—the anticrossing of energy levels exhibiting different size dependencies. We show that this property is inherent to the energy spectra of charge carriers whose spatial motion is simultaneously affected by the Coulomb potential of the impurity ion and the confining potential of the nanocrystal. The coupling of impurity states, which leads to the anticrossing, can be induced by interactions with elementary excitations residing inside the nanocrystal or an external electromagnetic field. We formulate physical conditions that allow a straightforward interpretation of level anticrossings in the nanocrystal energy spectrum and an accurate estimation of the states' coupling strength. PMID:25369911

Describing excited state relaxation and localization in TiO 2 nanoparticles using TD-DFT

DOE PAGES

Berardo, Enrico; Hu, Han -Shi; van Dam, Hubertus J. J.; ...

2014-02-26

We have investigated the description of excited state relaxation in naked and hydrated TiO 2 nanoparticles using Time-Dependent Density Functional Theory (TD-DFT) with three common hybrid exchange-correlation (XC) potentials; B3LYP, CAM-B3LYP and BHLYP. Use of TD-CAM-B3LYP and TD-BHLYP yields qualitatively similar results for all structures, which are also consistent with predictions of coupled cluster theory for small particles. TD-B3LYP, in contrast, is found to make rather different predictions; including apparent conical intersections for certain particles that are not observed with TD-CAM-B3LYP nor with TD-BHLYP. In line with our previous observations for vertical excitations, the issue with TD-B3LYP appears to bemore » the inherent tendency of TD-B3LYP, and other XC potentials with no or a low percentage of Hartree-Fock Like Exchange, to spuriously stabilize the energy of charge-transfer (CT) states. Even in the case of hydrated particles, for which vertical excitations are generally well described with all XC potentials, the use of TD-B3LYP appears to result in CT-problems for certain particles. We hypothesize that the spurious stabilization of CT-states by TD-B3LYP even may drive the excited state optimizations to different excited state geometries than those obtained using TD-CAM-B3LYP or TD-BHLYP. In conclusion, focusing on the TD-CAM-B3LYP and TD-BHLYP results, excited state relaxation in naked and hydrated TiO 2 nanoparticles is predicted to be associated with a large Stokes’ shift.« less

Describing excited state relaxation and localization in TiO 2 nanoparticles using TD-DFT

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

Berardo, Enrico; Hu, Han -Shi; van Dam, Hubertus J. J.

We have investigated the description of excited state relaxation in naked and hydrated TiO 2 nanoparticles using Time-Dependent Density Functional Theory (TD-DFT) with three common hybrid exchange-correlation (XC) potentials; B3LYP, CAM-B3LYP and BHLYP. Use of TD-CAM-B3LYP and TD-BHLYP yields qualitatively similar results for all structures, which are also consistent with predictions of coupled cluster theory for small particles. TD-B3LYP, in contrast, is found to make rather different predictions; including apparent conical intersections for certain particles that are not observed with TD-CAM-B3LYP nor with TD-BHLYP. In line with our previous observations for vertical excitations, the issue with TD-B3LYP appears to bemore » the inherent tendency of TD-B3LYP, and other XC potentials with no or a low percentage of Hartree-Fock Like Exchange, to spuriously stabilize the energy of charge-transfer (CT) states. Even in the case of hydrated particles, for which vertical excitations are generally well described with all XC potentials, the use of TD-B3LYP appears to result in CT-problems for certain particles. We hypothesize that the spurious stabilization of CT-states by TD-B3LYP even may drive the excited state optimizations to different excited state geometries than those obtained using TD-CAM-B3LYP or TD-BHLYP. In conclusion, focusing on the TD-CAM-B3LYP and TD-BHLYP results, excited state relaxation in naked and hydrated TiO 2 nanoparticles is predicted to be associated with a large Stokes’ shift.« less

Early-Time Excited-State Relaxation Dynamics of Iridium Compounds: Distinct Roles of Electron and Hole Transfer.

PubMed

Liu, Xiang-Yang; Zhang, Ya-Hui; Fang, Wei-Hai; Cui, Ganglong

2018-06-28

Excited-state and photophysical properties of Ir-containing complexes have been extensively studied because of their potential applications as organic light-emitting diode emitting materials. However, their early time excited-state relaxation dynamics are less explored computationally. Herein we have employed our recently implemented TDDFT-based generalized surface-hopping dynamics method to simulate excited-state relaxation dynamics of three Ir(III) compounds having distinct ligands. According to our multistate dynamics simulations including five excited singlet states i.e., S n ( n = 1-5) and ten excited triplet states, i.e., T n ( n = 1-10), we have found that the intersystem crossing (ISC) processes from the S n to T n are very efficient and ultrafast in these three Ir(III) compounds. The corresponding ISC rates are estimated to be 65, 81, and 140 fs, which are reasonably close to the experimentally measured ca. 80, 80, and 110 fs. In addition, the internal conversion (IC) processes within respective singlet and triplet manifolds are also ultrafast. These ultrafast IC and ISC processes are caused by large nonadiabatic and spin-orbit couplings, respectively, as well as small energy gaps. Importantly, although these Ir(III) complexes share similar macroscopic phenomena, i.e., ultrafast IC and ISC, their microscopic excited-state relaxation mechanism and dynamics are qualitatively distinct. Specifically, the dynamical behaviors of electron and hole and their roles are variational in modulating the excited-state relaxation dynamics of these Ir(III) compounds. In other words, the electronic properties of the ligands that are coordinated with the central Ir(III) atom play important roles in regulating the microscopic excited-state relaxation dynamics. These gained insights could be useful for rationally designing Ir(III) compounds with excellent photoluminescence.

Excited states in polydiacetylene chains: A density matrix renormalization group study

NASA Astrophysics Data System (ADS)

Barcza, Gergely; Barford, William; Gebhard, Florian; Legeza, Örs

2013-06-01

We study theoretically polydiacetylene chains diluted in their monomer matrix. We employ the density matrix renormalization group method on finite chains to calculate the ground state and low-lying excitations of the corresponding Peierls-Hubbard-Ohno Hamiltonian which is characterized by the electron transfer amplitude t0 between nearest neighbors, by the electron-phonon coupling constant α, by the Hubbard interaction U, and by the long-range interaction V. We treat the lattice relaxation in the adiabatic limit, i.e., we calculate the polaronic lattice distortions for each excited state. Using chains with up to 102 lattice sites, we can safely perform the extrapolation to the thermodynamic limit for the ground-state energy and conformation, the single-particle gap, and the energies of the singlet exciton, the triplet ground state, and the optical excitation of the triplet ground state. The corresponding gaps are known with high precision from experiments. We determine a coherent parameter set (t0*=2.4eV,α*=3.4eV/Å,U*=6eV,V*=3eV) from a fit of the experimental gap energies to the theoretical values which we obtain for 81 parameter points in the four-dimensional search space (t0,α,U,V). We identify dark in-gap states in the singlet and triplet sectors as seen in experiments. Using a fairly stiff spring constant, the length of our unit cell is about 1% larger than its experimental value.

Chemical modulation of electronic structure at the excited state

NASA Astrophysics Data System (ADS)

Li, F.; Song, C.; Gu, Y. D.; Saleem, M. S.; Pan, F.

2017-12-01

Spin-polarized electronic structures are the cornerstone of spintronics, and have thus attracted a significant amount of interest; in particular, researchers are looking into how to modulate the electronic structure to enable multifunctional spintronics applications, especially in half-metallic systems. However, the control of the spin polarization has only been predicted in limited two-dimensional systems with spin-polarized Dirac structures and is difficult to achieve experimentally. Here, we report the modulation of the electronic structure in the light-induced excited state in a typical half-metal, L a1 /2S r1 /2Mn O3 -δ . According to the spin-transport measurements, there appears a light-induced increase in magnetoresistance due to the enhanced spin scattering, which is closely associated with the excited spin polarization. Strikingly, the light-induced variation can be enhanced via alcohol processing and reduced by oxygen annealing. X-ray photoelectron spectroscopy measurements show that in the chemical process, a redox reaction occurs with a change in the valence of Mn. Furthermore, first-principles calculations reveal that the change in the valence of Mn alters the electronic structure and consequently modulates the spin polarization in the excited state. Our findings thus report a chemically tunable electronic structure, demonstrating interesting physics and the potential for multifunctional applications and ultrafast spintronics.

Evidence for carrier localization in the pseudogap state of cuprate superconductors from coherent quench experiments

PubMed Central

Madan, I.; Kurosawa, T.; Toda, Y.; Oda, M.; Mertelj, T.; Mihailovic, D.

2015-01-01

A ‘pseudogap' was introduced by Mott to describe a state of matter that has a minimum in the density of states at the Fermi level, deep enough for states to become localized. It can arise either from Coulomb repulsion between electrons, and/or incipient charge or spin order. Here we employ ultrafast spectroscopy to study dynamical properties of the normal to pseudogap state transition in the prototype high-temperature superconductor Bi2Sr2CaCu2O8+δ. We perform a systematic temperature and doping dependence study of the pseudogap photodestruction and recovery in coherent quench experiments, revealing marked absence of critical behaviour of the elementary excitations, which implies an absence of collective electronic ordering beyond a few coherence lengths on short timescales. The data imply ultrafast carrier localization into a textured polaronic state arising from a competing Coulomb interaction and lattice strain, enhanced by a Fermi surface instability. PMID:25891310

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

Tetracarboxy-phthalocyanines: From excited state dynamics to photodynamic inactivation against Bovine herpesvirus type 1.

PubMed

Cocca, Leandro H Z; Oliveira, Taise M A; Gotardo, Fernando; Teles, Amanda V; Menegatti, Ricardo; Siqueira, Jonathas P; Mendonça, Cleber R; Bataus, Luiz A M; Ribeiro, Anderson O; Souza, Thalita F M; Souza, Guilherme R L; Gonçalves, Pablo J; De Boni, Leonardo

2017-10-01

Herein we present the excited state dynamic of zinc and aluminum tetracarboxy-phthalocyanines (ZnPc and AlPc) and its application in the photodynamic inactivation (PDI) of Bovine herpesvirus type 1 (BoHV-1) in vitro. The excited state dynamic provides valuable data to describe the excited state properties of potential optical limiters and/or photosensitizers (PSs), such as: the excited state cross-sections, fluorescence lifetime and triplet state quantum yield. The excited state characterization was performed using three different Z-scan techniques: Single Pulse, White Light Continuum and Pulse Train. Considering the photodynamic inactivation of BoHV-1, an initial viral suspension containing 10 5.75 TCID 50 /mL was incubated with the PSs for 1h at 37°C under agitation and protected from light. The samples were placed in microtiter plates and irradiated (180mW/cm 2 ). During irradiation, a sample was taken every 15min and the viability of the virus was evaluated. The results show that both phthalocyanines were efficient against viruses. However, a higher photodynamic efficiency was observed by ZnPc, which can be attributed to its higher triplet and singlet quantum yields. The results presented here are important for animal health (treatment of BoHV-1) and also open up a field of studies to use AlPc and ZnPc as potential agents against a wide range of microorganisms of veterinary interest. Copyright © 2017 Elsevier B.V. All rights reserved.

Coulomb-Driven Relativistic Electron Beam Compression

NASA Astrophysics Data System (ADS)

Lu, Chao; Jiang, Tao; Liu, Shengguang; Wang, Rui; Zhao, Lingrong; Zhu, Pengfei; Xiang, Dao; Zhang, Jie

2018-01-01

Coulomb interaction between charged particles is a well-known phenomenon in many areas of research. In general, the Coulomb repulsion force broadens the pulse width of an electron bunch and limits the temporal resolution of many scientific facilities such as ultrafast electron diffraction and x-ray free-electron lasers. Here we demonstrate a scheme that actually makes use of the Coulomb force to compress a relativistic electron beam. Furthermore, we show that the Coulomb-driven bunch compression process does not introduce additional timing jitter, which is in sharp contrast to the conventional radio-frequency buncher technique. Our work not only leads to enhanced temporal resolution in electron-beam-based ultrafast instruments that may provide new opportunities in probing material systems far from equilibrium, but also opens a promising direction for advanced beam manipulation through self-field interactions.

Coulomb-Driven Relativistic Electron Beam Compression.

PubMed

Lu, Chao; Jiang, Tao; Liu, Shengguang; Wang, Rui; Zhao, Lingrong; Zhu, Pengfei; Xiang, Dao; Zhang, Jie

2018-01-26

Coulomb interaction between charged particles is a well-known phenomenon in many areas of research. In general, the Coulomb repulsion force broadens the pulse width of an electron bunch and limits the temporal resolution of many scientific facilities such as ultrafast electron diffraction and x-ray free-electron lasers. Here we demonstrate a scheme that actually makes use of the Coulomb force to compress a relativistic electron beam. Furthermore, we show that the Coulomb-driven bunch compression process does not introduce additional timing jitter, which is in sharp contrast to the conventional radio-frequency buncher technique. Our work not only leads to enhanced temporal resolution in electron-beam-based ultrafast instruments that may provide new opportunities in probing material systems far from equilibrium, but also opens a promising direction for advanced beam manipulation through self-field interactions.

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

NASA Astrophysics Data System (ADS)

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

2018-05-01

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

Multiconfiguration Pair-Density Functional Theory Outperforms Kohn-Sham Density Functional Theory and Multireference Perturbation Theory for Ground-State and Excited-State Charge Transfer.

PubMed

Ghosh, Soumen; Sonnenberger, Andrew L; Hoyer, Chad E; Truhlar, Donald G; Gagliardi, Laura

2015-08-11

The correct description of charge transfer in ground and excited states is very important for molecular interactions, photochemistry, electrochemistry, and charge transport, but it is very challenging for Kohn-Sham (KS) density functional theory (DFT). KS-DFT exchange-correlation functionals without nonlocal exchange fail to describe both ground- and excited-state charge transfer properly. We have recently proposed a theory called multiconfiguration pair-density functional theory (MC-PDFT), which is based on a combination of multiconfiguration wave function theory with a new type of density functional called an on-top density functional. Here we have used MC-PDFT to study challenging ground- and excited-state charge-transfer processes by using on-top density functionals obtained by translating KS exchange-correlation functionals. For ground-state charge transfer, MC-PDFT performs better than either the PBE exchange-correlation functional or CASPT2 wave function theory. For excited-state charge transfer, MC-PDFT (unlike KS-DFT) shows qualitatively correct behavior at long-range with great improvement in predicted excitation energies.

Structure Effect of Squarylium Cyanine Dyes on Third-Order Optical Nonlinearities in Ground and Excited States

NASA Astrophysics Data System (ADS)

Liu, Xu-chun; Xu, Gang; Si, Jin-hai; Ye, Pei-xian; Lin, Tong; Peng, Bi-xian

1999-08-01

A series of squarylium cyanine dyes with different substituents were synthesized and the third-order optical nonlinearities of their ground and excited states were investigated by backward degenerate four-wave-mixing. For the ground state, the molecular hyperpolarizability γg increases with the red-shift of the absorption peak λmaxab of the squaraine with different substituents, whereas for the excited-state molecular hyperpolarizability γe, the nonlinear enhancement γe/γg decreases, which may indicate that in the excited state the electron accepting-donating ability of different substituents changes in the reverse order compared with the order in the ground state.

Uncovering Highly-Excited State Mixing in Acetone Using Ultrafast VUV Pulses and Coincidence Imaging Techniques

DOE PAGES

Couch, David E.; Kapteyn, Henry C.; Murnane, Margaret M.; ...

2017-03-17

Here, understanding the ultrafast dynamics of highly-excited electronic states of small molecules is critical for a better understanding of atmospheric and astrophysical processes, as well as for designing coherent control strategies for manipulating chemical dynamics. In highly excited states, nonadiabatic coupling, electron-electron interactions, and the high density of states govern dynamics. However, these states are computationally and experimentally challenging to access. Fortunately, new sources of ultrafast vacuum ultraviolet pulses, in combination with electron-ion coincidence spectroscopies, provide new tools to unravel the complex electronic landscape. Here we report time-resolved photoelectron-photoion coincidence experiments using 8 eV pump photons to study the highlymore » excited states of acetone. We uncover for the first time direct evidence that the resulting excited state consists of a mixture of both n y → 3p and π → π* character, which decays with a time constant of 330 fs. In the future, this approach can inform models of VUV photochemistry and aid in designing coherent control strategies for manipulating chemical reactions.« less

Uncovering Highly-Excited State Mixing in Acetone Using Ultrafast VUV Pulses and Coincidence Imaging Techniques

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

Couch, David E.; Kapteyn, Henry C.; Murnane, Margaret M.

Here, understanding the ultrafast dynamics of highly-excited electronic states of small molecules is critical for a better understanding of atmospheric and astrophysical processes, as well as for designing coherent control strategies for manipulating chemical dynamics. In highly excited states, nonadiabatic coupling, electron-electron interactions, and the high density of states govern dynamics. However, these states are computationally and experimentally challenging to access. Fortunately, new sources of ultrafast vacuum ultraviolet pulses, in combination with electron-ion coincidence spectroscopies, provide new tools to unravel the complex electronic landscape. Here we report time-resolved photoelectron-photoion coincidence experiments using 8 eV pump photons to study the highlymore » excited states of acetone. We uncover for the first time direct evidence that the resulting excited state consists of a mixture of both n y → 3p and π → π* character, which decays with a time constant of 330 fs. In the future, this approach can inform models of VUV photochemistry and aid in designing coherent control strategies for manipulating chemical reactions.« less

Red and blue shift of liquid water's excited states: A many body perturbation study

NASA Astrophysics Data System (ADS)

Ziaei, Vafa; Bredow, Thomas

2016-08-01

In the present paper, accurate optical absorption spectrum of liquid H2O is calculated in the energy range of 5-20 eV to probe the nature of water's excited states by means of many body perturbation approach. Main features of recent inelastic X-ray measurements are well reproduced, such as a bound excitonic peak at 7.9 eV with a shoulder at 9.4 eV as well as the absorption maximum at 13.9 eV, followed by a broad shoulder at 18.4 eV. The spectrum is dominated by excitonic effects impacting the structures of the spectrum at low and higher energy regimes mixed by single particle effects at high energies. The exciton distribution of the low-energy states, in particular of S1, is highly anisotropic and localized mostly on one water molecule. The S1 state is essentially a HOCO-LUCO (highest occupied crystal orbital - lowest unoccupied crystal orbital) transition and of intra-molecular type, showing a localized valence character. Once the excitation energy is increased, a significant change in the character of the electronically excited states occurs, characterized through emergence of multiple quasi-particle peaks at 7.9 eV in the quasi-particle (QP) transition profile and in the occurring delocalized exciton density distribution, spread over many more water molecules. The exciton delocalization following a change of the character of excited states at around 7.9 eV causes the blue shift of the first absorption band with respect to water monomer S1. However, due to reduction of the electronic band gap from gas to liquid phase, following enhanced screening upon condensation, the localized S1 state of liquid water is red-shifted with respect to S1 state of water monomer. For higher excitations, near vertical ionization energy (11 eV), quasi-free electrons emerge, in agreement with the conduction band electron picture. Furthermore, the occurring red and blue shift of the excited states are independent of the coupling of resonant and anti-resonant contributions to the

Excitation wavelength dependence of excited state intramolecular proton transfer reaction of 4'-N,N-diethylamino-3-hydroxyflavone in room temperature ionic liquids studied by optical Kerr gate fluorescence measurement.

PubMed

Suda, Kayo; Terazima, Masahide; Sato, Hirofumi; Kimura, Yoshifumi

2013-10-17

Excited state intramolecular proton transfer reactions (ESIPT) of 4'-N,N-diethylamino-3-hydroxyflavone (DEAHF) in ionic liquids have been studied by steady-state and time-resolved fluorescence measurements at different excitation wavelengths. Steady-state measurements show the relative yield of the tautomeric form to the normal form of DEAHF decreases as excitation wavelength is increased from 380 to 450 nm. The decrease in yield is significant in ionic liquids that have cations with long alkyl chains. The extent of the decrease is correlated with the number of carbon atoms in the alkyl chains. Time-resolved fluorescence measurements using optical Kerr gate spectroscopy show that ESIPT rate has a strong excitation wavelength dependence. There is a large difference between the spectra at a 200 ps delay from different excitation wavelengths in each ionic liquid. The difference is pronounced in ionic liquids having a long alkyl chain. The equilibrium constant in the electronic excited state obtained at a 200 ps delay and the average reaction rate are also correlated with the alkyl chain length. Considering the results of the steady-state fluorescence and time-resolved measurements, the excitation wavelength dependence of ESIPT is explained by state selective excitation due to the difference of the solvation, and the number of alkyl chain carbon atoms is found to be a good indicator of the effect of inhomogeneity for this reaction.

Coulomb branches with complex singularities

NASA Astrophysics Data System (ADS)

Argyres, Philip C.; Martone, Mario

2018-06-01

We construct 4d superconformal field theories (SCFTs) whose Coulomb branches have singular complex structures. This implies, in particular, that their Coulomb branch coordinate rings are not freely generated. Our construction also gives examples of distinct SCFTs which have identical moduli space (Coulomb, Higgs, and mixed branch) geometries. These SCFTs thus provide an interesting arena in which to test the relationship between moduli space geometries and conformal field theory data. We construct these SCFTs by gauging certain discrete global symmetries of N = 4 superYang-Mills (sYM) theories. In the simplest cases, these discrete symmetries are outer automorphisms of the sYM gauge group, and so these theories have lagrangian descriptions as N = 4 sYM theories with disconnected gauge groups.

Pushing the limits of excited-state g-factor measurements

NASA Astrophysics Data System (ADS)

Stuchbery, Andrew E.; McCormick, Brendan P.; Gray, Timothy J.; Coombes, Ben J.

2018-05-01

Current developments in excited-state g-factor measurements are discussed with an emphasis on cases where the experimental methodology is being extended into new regimes. The transient-field technique, the recoil in vacuum method, and moment measurements with LaBr3 detectors are discussed.

Cotunneling Drag Effect in Coulomb-Coupled Quantum Dots.

PubMed

Keller, A J; Lim, J S; Sánchez, David; López, Rosa; Amasha, S; Katine, J A; Shtrikman, Hadas; Goldhaber-Gordon, D

2016-08-05

In Coulomb drag, a current flowing in one conductor can induce a voltage across an adjacent conductor via the Coulomb interaction. The mechanisms yielding drag effects are not always understood, even though drag effects are sufficiently general to be seen in many low-dimensional systems. In this Letter, we observe Coulomb drag in a Coulomb-coupled double quantum dot and, through both experimental and theoretical arguments, identify cotunneling as essential to obtaining a correct qualitative understanding of the drag behavior.

Hot excited state management for long-lived blue phosphorescent organic light-emitting diodes

DOE PAGES

Lee, Jaesang; Jeong, Changyeong; Batagoda, Thilini; ...

2017-05-31

Since their introduction over 15 years ago, the operational lifetime of blue phosphorescent organic light-emitting diodes (PHOLEDs) has remained insufficient for their practical use in displays and lighting. Their short lifetime results from annihilation between high-energy excited states, producing energetically hot states (46.0 eV) that lead to molecular dissociation. We introduce a strategy to avoid dissociative reactions by including a molecular hot excited state manager within the device emission layer. Hot excited states transfer to the manager and rapidly thermalize before damage is induced on the dopant or host. As a consequence, the managed blue PHOLED attains T80=334±5 h (timemore » to 80% of the 1,000 cd m -2 initial luminance) with a chromaticity coordinate of (0.16, 0.31), corresponding to 3.6±0.1 times improvement in a lifetime compared to conventional, unmanaged devices. We believe that, this significant improvement results in the longest lifetime for such a blue PHOLED.« less

Hot excited state management for long-lived blue phosphorescent organic light-emitting diodes

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

Lee, Jaesang; Jeong, Changyeong; Batagoda, Thilini

Since their introduction over 15 years ago, the operational lifetime of blue phosphorescent organic light-emitting diodes (PHOLEDs) has remained insufficient for their practical use in displays and lighting. Their short lifetime results from annihilation between high-energy excited states, producing energetically hot states (46.0 eV) that lead to molecular dissociation. We introduce a strategy to avoid dissociative reactions by including a molecular hot excited state manager within the device emission layer. Hot excited states transfer to the manager and rapidly thermalize before damage is induced on the dopant or host. As a consequence, the managed blue PHOLED attains T80=334±5 h (timemore » to 80% of the 1,000 cd m -2 initial luminance) with a chromaticity coordinate of (0.16, 0.31), corresponding to 3.6±0.1 times improvement in a lifetime compared to conventional, unmanaged devices. We believe that, this significant improvement results in the longest lifetime for such a blue PHOLED.« less

Collective charge excitations and the metal-insulator transition in the square lattice Hubbard-Coulomb model

DOE PAGES

Ulybyshev, Maksim; Winterowd, Christopher; Zafeiropoulos, Savvas

2017-11-09

Here in this article, we discuss the nontrivial collective charge excitations (plasmons) of the extended square lattice Hubbard model. Using a fully nonperturbative approach, we employ the hybrid Monte Carlo algorithm to simulate the system at half-filling. A modified Backus-Gilbert method is introduced to obtain the spectral functions via numerical analytic continuation. We directly compute the single-particle density of states which demonstrates the formation of Hubbard bands in the strongly correlated phase. The momentum-resolved charge susceptibility also is computed on the basis of the Euclidean charge-density-density correlator. In agreement with previous extended dynamical mean-field theory studies, we find that, atmore » high strength of the electron-electron interaction, the plasmon dispersion develops two branches.« less

Collective charge excitations and the metal-insulator transition in the square lattice Hubbard-Coulomb model

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

Ulybyshev, Maksim; Winterowd, Christopher; Zafeiropoulos, Savvas

Here in this article, we discuss the nontrivial collective charge excitations (plasmons) of the extended square lattice Hubbard model. Using a fully nonperturbative approach, we employ the hybrid Monte Carlo algorithm to simulate the system at half-filling. A modified Backus-Gilbert method is introduced to obtain the spectral functions via numerical analytic continuation. We directly compute the single-particle density of states which demonstrates the formation of Hubbard bands in the strongly correlated phase. The momentum-resolved charge susceptibility also is computed on the basis of the Euclidean charge-density-density correlator. In agreement with previous extended dynamical mean-field theory studies, we find that, atmore » high strength of the electron-electron interaction, the plasmon dispersion develops two branches.« less

Photodissociation Efficiency Spectroscopy Study of the Rydberg Excited Ion-Pair States of Carbon Dioxide

NASA Astrophysics Data System (ADS)

Feng, Qiang; Xu, Yun-Feng; Sun, Jin-Da; Tian, Shan-Xi; Shan, Xiao-Bin; Liu, Fu-Yi; Sheng, Liu-Si

2009-10-01

Photodissociation efficiency spectrum of anionic oxygen atom produced via ion-pair dissociations of carbon dioxide is recorded by means of the synchrotron radiation excitation (XUV photon energy 17.40-20.00 eV). The present spectrum is assigned as the Rydberg-like excited ion-pair states, i.e., Tanaka-Ogawa and Henning series, tilde C2Σg+ (CO+2) vibrational ground-state and excitation series. Three Rydberg series, npσu, npπu, and nfu, converging to tilde C2Σg+ (0, 0, 0), show the higher cross sections.

Calculation of Vibrational and Electronic Excited-State Absorption Spectra of Arsenic-Water Complexes Using Density Functional Theory

DTIC Science & Technology

2016-06-03

Naval Research Laboratory Washington, DC 20375-5320 NRL/MR/6390--16-9681 Calculation of Vibrational and Electronic Excited-State Absorption Spectra...NUMBER OF PAGES 17. LIMITATION OF ABSTRACT Calculation of Vibrational and Electronic Excited-State Absorption Spectra of Arsenic-Water Complexes Using...Unclassified Unlimited Unclassified Unlimited 59 Samuel G. Lambrakos (202) 767-2601 Calculations are presented of vibrational and electronic excited-state

An excited state underlies gene regulation of a transcriptional riboswitch

PubMed Central

Zhao, Bo; Guffy, Sharon L.; Williams, Benfeard; Zhang, Qi

2017-01-01

Riboswitches control gene expression through ligand-dependent structural rearrangements of the sensing aptamer domain. However, we found that the Bacillus cereus fluoride riboswitch aptamer adopts identical tertiary structures in solution with and without ligand. Using chemical exchange saturation transfer (CEST) NMR spectroscopy, we revealed that the structured ligand-free aptamer transiently accesses a low-populated (~1%) and short-lived (~3 ms) excited conformational state that unravels a conserved ‘linchpin’ base pair to signal transcription termination. Upon fluoride binding, this highly localized fleeting process is allosterically suppressed to activate transcription. We demonstrated that this mechanism confers effective fluoride-dependent gene activation over a wide range of transcription rates, which is essential for robust toxicity response across diverse cellular conditions. These results unveil a novel switching mechanism that employs ligand-dependent suppression of an aptamer excited state to coordinate regulatory conformational transitions rather than adopting distinct aptamer ground-state tertiary architectures, exemplifying a new mode of ligand-dependent RNA regulation. PMID:28719589

Interatomic Coulombic Decay Effects in Theoretical DNA Recombination Systems Involving Protein Interaction Sites

NASA Astrophysics Data System (ADS)

Vargas, E. L.; Rivas, D. A.; Duot, A. C.; Hovey, R. T.; Andrianarijaona, V. M.

2015-03-01

DNA replication is the basis for all biological reproduction. A strand of DNA will ``unzip'' and bind with a complimentary strand, creating two identical strands. In this study, we are considering how this process is affected by Interatomic Coulombic Decay (ICD), specifically how ICD affects the individual coding proteins' ability to hold together. ICD mainly deals with how the electron returns to its original state after excitation and how this affects its immediate atomic environment, sometimes affecting the connectivity between interaction sites on proteins involved in the DNA coding process. Biological heredity is fundamentally controlled by DNA and its replication therefore it affects every living thing. The small nature of the proteins (within the range of nanometers) makes it a good candidate for research of this scale. Understanding how ICD affects DNA molecules can give us invaluable insight into the human genetic code and the processes behind cell mutations that can lead to cancer. Authors wish to give special thanks to Pacific Union College Student Senate in Angwin, California, for their financial support.

Search for two-neutrino double-β decay of 96Zr to excited states of 96Mo

NASA Astrophysics Data System (ADS)

Finch, S. W.; Tornow, W.

2015-10-01

Background: Double-β decay is a rare second-order nuclear decay. The importance of this decay stems from the possibility of neutrinoless double-β decay and its applications to neutrino physics. Purpose: A search was conducted for the 2 ν β β decay of 96Zr to excited final states of the daughter nucleus, 96Mo. Measurements of this decay are important to test nuclear matrix element calculations, which are necessary to extract the neutrino mass from a measurement of the neutrinoless double-β decay half-life. Method: Two coaxial high-purity germanium detectors were used in coincidence to detect γ rays produced by the daughter nucleus as it de-excited to the ground state. The experiment was carried out at the Kimballton Underground Research Facility and produced 685.7 d of data with a 17.91 g enriched sample. Results: No counts were seen above background. For the decay to the first excited 0+ state, a limit of T1 /2>3.1 ×1020 yr was produced. Limits to higher excited states are also reported. Conclusion: The new limits on double-β decay are an improvement over previous experiments by a factor of 2 to 5 for the various excited states. The nuclear matrix element for the double-β decay to the first excited 0+ state is found to be <0.13 .

Search for excited B c + states

NASA Astrophysics Data System (ADS)

Aaij, R.; Adeva, B.; Adinolfi, M.; Ajaltouni, Z.; Akar, S.; Albrecht, J.; Alessio, F.; Alexander, M.; Alfonso Albero, A.; Ali, S.; Alkhazov, G.; Alvarez Cartelle, P.; Alves, A. A.; Amato, S.; Amerio, S.; Amhis, Y.; An, L.; Anderlini, L.; Andreassi, G.; Andreotti, M.; Andrews, J. E.; Appleby, R. B.; Archilli, F.; d'Argent, P.; Arnau Romeu, J.; Artamonov, A.; Artuso, M.; Aslanides, E.; Atzeni, M.; Auriemma, G.; Baalouch, M.; Babuschkin, I.; Bachmann, S.; Back, J. J.; Badalov, A.; Baesso, C.; Baker, S.; Balagura, V.; Baldini, W.; Baranov, A.; Barlow, R. J.; Barschel, C.; Barsuk, S.; Barter, W.; Baryshnikov, F.; Batozskaya, V.; Battista, V.; Bay, A.; Beaucourt, L.; Beddow, J.; Bedeschi, F.; Bediaga, I.; Beiter, A.; Bel, L. J.; Beliy, N.; Bellee, V.; Belloli, N.; Belous, K.; Belyaev, I.; Ben-Haim, E.; Bencivenni, G.; Benson, S.; Beranek, S.; Berezhnoy, A.; Bernet, R.; Berninghoff, D.; Bertholet, E.; Bertolin, A.; Betancourt, C.; Betti, F.; Bettler, M. O.; van Beuzekom, M.; Bezshyiko, Ia.; Bifani, S.; Billoir, P.; Birnkraut, A.; Bizzeti, A.; Bjørn, M.; Blake, T.; Blanc, F.; Blusk, S.; Bocci, V.; Boettcher, T.; Bondar, A.; Bondar, N.; Bordyuzhin, I.; Borghi, S.; Borisyak, M.; Borsato, M.; Bossu, F.; Boubdir, M.; Bowcock, T. J. V.; Bowen, E.; Bozzi, C.; Braun, S.; Brodzicka, J.; Brundu, D.; Buchanan, E.; Burr, C.; Bursche, A.; Buytaert, J.; Byczynski, W.; Cadeddu, S.; Cai, H.; Calabrese, R.; Calladine, R.; Calvi, M.; Calvo Gomez, M.; Camboni, A.; Campana, P.; Campora Perez, D. H.; Capriotti, L.; Carbone, A.; Carboni, G.; Cardinale, R.; Cardini, A.; Carniti, P.; Carson, L.; Carvalho Akiba, K.; Casse, G.; Cassina, L.; Cattaneo, M.; Cavallero, G.; Cenci, R.; Chamont, D.; Chapman, M. G.; Charles, M.; Charpentier, Ph.; Chatzikonstantinidis, G.; Chefdeville, M.; Chen, S.; Cheung, S. F.; Chitic, S.-G.; Chobanova, V.; Chrzaszcz, M.; Chubykin, A.; Ciambrone, P.; Cid Vidal, X.; Ciezarek, G.; Clarke, P. E. L.; Clemencic, M.; Cliff, H. V.; Closier, J.; Coco, V.; Cogan, J.; Cogneras, E.; Cogoni, V.; Cojocariu, L.; Collins, P.; Colombo, T.; Comerma-Montells, A.; Contu, A.; Coombs, G.; Coquereau, S.; Corti, G.; Corvo, M.; Costa Sobral, C. M.; Couturier, B.; Cowan, G. A.; Craik, D. C.; Crocombe, A.; Cruz Torres, M.; Currie, R.; D'Ambrosio, C.; Da Cunha Marinho, F.; Da Silva, C. L.; Dall'Occo, E.; Dalseno, J.; Davis, A.; De Aguiar Francisco, O.; De Bruyn, K.; De Capua, S.; De Cian, M.; De Miranda, J. M.; De Paula, L.; De Serio, M.; De Simone, P.; Dean, C. T.; Decamp, D.; Del Buono, L.; Dembinski, H.-P.; Demmer, M.; Dendek, A.; Derkach, D.; Deschamps, O.; Dettori, F.; Dey, B.; Di Canto, A.; Di Nezza, P.; Dijkstra, H.; Dordei, F.; Dorigo, M.; Dosil Suárez, A.; Douglas, L.; Dovbnya, A.; Dreimanis, K.; Dufour, L.; Dujany, G.; Durante, P.; Durham, J. M.; Dutta, D.; Dzhelyadin, R.; Dziewiecki, M.; Dziurda, A.; Dzyuba, A.; Easo, S.; Ebert, M.; Egede, U.; Egorychev, V.; Eidelman, S.; Eisenhardt, S.; Eitschberger, U.; Ekelhof, R.; Eklund, L.; Ely, S.; Esen, S.; Evans, H. M.; Evans, T.; Falabella, A.; Farley, N.; Farry, S.; Fazzini, D.; Federici, L.; Ferguson, D.; Fernandez, G.; Fernandez Declara, P.; Fernandez Prieto, A.; Ferrari, F.; Ferreira Lopes, L.; Ferreira Rodrigues, F.; Ferro-Luzzi, M.; Filippov, S.; Fini, R. A.; Fiorini, M.; Firlej, M.; Fitzpatrick, C.; Fiutowski, T.; Fleuret, F.; Fontana, M.; Fontanelli, F.; Forty, R.; Franco Lima, V.; Frank, M.; Frei, C.; Fu, J.; Funk, W.; Furfaro, E.; Färber, C.; Gabriel, E.; Gallas Torreira, A.; Galli, D.; Gallorini, S.; Gambetta, S.; Gandelman, M.; Gandini, P.; Gao, Y.; Garcia Martin, L. M.; García Pardiñas, J.; Garra Tico, J.; Garrido, L.; Garsed, P. J.; Gascon, D.; Gaspar, C.; Gavardi, L.; Gazzoni, G.; Gerick, D.; Gersabeck, E.; Gersabeck, M.; Gershon, T.; Ghez, Ph.; Gianì, S.; Gibson, V.; Girard, O. G.; Giubega, L.; Gizdov, K.; Gligorov, V. V.; Golubkov, D.; Golutvin, A.; Gomes, A.; Gorelov, I. V.; Gotti, C.; Govorkova, E.; Grabowski, J. P.; Graciani Diaz, R.; Granado Cardoso, L. A.; Graugés, E.; Graverini, E.; Graziani, G.; Grecu, A.; Greim, R.; Griffith, P.; Grillo, L.; Gruber, L.; Gruberg Cazon, B. R.; Grünberg, O.; Gushchin, E.; Guz, Yu.; Gys, T.; Göbel, C.; Hadavizadeh, T.; Hadjivasiliou, C.; Haefeli, G.; Haen, C.; Haines, S. C.; Hamilton, B.; Han, X.; Hancock, T. H.; Hansmann-Menzemer, S.; Harnew, N.; Harnew, S. T.; Hasse, C.; Hatch, M.; He, J.; Hecker, M.; Heinicke, K.; Heister, A.; Hennessy, K.; Henrard, P.; Henry, L.; van Herwijnen, E.; Heß, M.; Hicheur, A.; Hill, D.; Hopchev, P. H.; Hu, W.; Huang, W.; Huard, Z. C.; Hulsbergen, W.; Humair, T.; Hushchyn, M.; Hutchcroft, D.; Ibis, P.; Idzik, M.; Ilten, P.; Jacobsson, R.; Jalocha, J.; Jans, E.; Jawahery, A.; Jiang, F.; John, M.; Johnson, D.; Jones, C. R.; Joram, C.; Jost, B.; Jurik, N.; Kandybei, S.; Karacson, M.; Kariuki, J. M.; Karodia, S.; Kazeev, N.; Kecke, M.; Keizer, F.; Kelsey, M.; Kenzie, M.; Ketel, T.; Khairullin, E.; Khanji, B.; Khurewathanakul, C.; Kirn, T.; Klaver, S.; Klimaszewski, K.; Klimkovich, T.; Koliiev, S.; Kolpin, M.; Kopecna, R.; Koppenburg, P.; Kosmyntseva, A.; Kotriakhova, S.; Kozeiha, M.; Kravchuk, L.; Kreps, M.; Kress, F.; Krokovny, P.; Krzemien, W.; Kucewicz, W.; Kucharczyk, M.; Kudryavtsev, V.; Kuonen, A. K.; Kvaratskheliya, T.; Lacarrere, D.; Lafferty, G.; Lai, A.; Lanfranchi, G.; Langenbruch, C.; Latham, T.; Lazzeroni, C.; Le Gac, R.; Leflat, A.; Lefrançois, J.; Lefèvre, R.; Lemaitre, F.; Lemos Cid, E.; Leroy, O.; Lesiak, T.; Leverington, B.; Li, P.-R.; Li, T.; Li, Y.; Li, Z.; Liang, X.; Likhomanenko, T.; Lindner, R.; Lionetto, F.; Lisovskyi, V.; Liu, X.; Loh, D.; Loi, A.; Longstaff, I.; Lopes, J. H.; Lucchesi, D.; Lucio Martinez, M.; Luo, H.; Lupato, A.; Luppi, E.; Lupton, O.; Lusiani, A.; Lyu, X.; Machefert, F.; Maciuc, F.; Macko, V.; Mackowiak, P.; Maddrell-Mander, S.; Maev, O.; Maguire, K.; Maisuzenko, D.; Majewski, M. W.; Malde, S.; Malecki, B.; Malinin, A.; Maltsev, T.; Manca, G.; Mancinelli, G.; Marangotto, D.; Maratas, J.; Marchand, J. F.; Marconi, U.; Marin Benito, C.; Marinangeli, M.; Marino, P.; Marks, J.; Martellotti, G.; Martin, M.; Martinelli, M.; Martinez Santos, D.; Martinez Vidal, F.; Massafferri, A.; Matev, R.; Mathad, A.; Mathe, Z.; Matteuzzi, C.; Mauri, A.; Maurice, E.; Maurin, B.; Mazurov, A.; McCann, M.; McNab, A.; McNulty, R.; Mead, J. V.; Meadows, B.; Meaux, C.; Meier, F.; Meinert, N.; Melnychuk, D.; Merk, M.; Merli, A.; Michielin, E.; Milanes, D. A.; Millard, E.; Minard, M.-N.; Minzoni, L.; Mitzel, D. S.; Mogini, A.; Molina Rodriguez, J.; Mombächer, T.; Monroy, I. A.; Monteil, S.; Morandin, M.; Morello, M. J.; Morgunova, O.; Moron, J.; Morris, A. B.; Mountain, R.; Muheim, F.; Mulder, M.; Müller, D.; Müller, J.; Müller, K.; Müller, V.; Naik, P.; Nakada, T.; Nandakumar, R.; Nandi, A.; Nasteva, I.; Needham, M.; Neri, N.; Neubert, S.; Neufeld, N.; Neuner, M.; Nguyen, T. D.; Nguyen-Mau, C.; Nieswand, S.; Niet, R.; Nikitin, N.; Nikodem, T.; Nogay, A.; O'Hanlon, D. P.; Oblakowska-Mucha, A.; Obraztsov, V.; Ogilvy, S.; Oldeman, R.; Onderwater, C. J. G.; Ossowska, A.; Otalora Goicochea, J. M.; Owen, P.; Oyanguren, A.; Pais, P. R.; Palano, A.; Palutan, M.; Papanestis, A.; Pappagallo, M.; Pappalardo, L. L.; Parker, W.; Parkes, C.; Passaleva, G.; Pastore, A.; Patel, M.; Patrignani, C.; Pearce, A.; Pellegrino, A.; Penso, G.; Pepe Altarelli, M.; Perazzini, S.; Pereima, D.; Perret, P.; Pescatore, L.; Petridis, K.; Petrolini, A.; Petrov, A.; Petruzzo, M.; Picatoste Olloqui, E.; Pietrzyk, B.; Pietrzyk, G.; Pikies, M.; Pinci, D.; Pisani, F.; Pistone, A.; Piucci, A.; Placinta, V.; Playfer, S.; Plo Casasus, M.; Polci, F.; Poli Lener, M.; Poluektov, A.; Polyakov, I.; Polycarpo, E.; Pomery, G. J.; Ponce, S.; Popov, A.; Popov, D.; Poslavskii, S.; Potterat, C.; Price, E.; Prisciandaro, J.; Prouve, C.; Pugatch, V.; Puig Navarro, A.; Pullen, H.; Punzi, G.; Qian, W.; Qin, J.; Quagliani, R.; Quintana, B.; Rachwal, B.; Rademacker, J. H.; Rama, M.; Ramos Pernas, M.; Rangel, M. S.; Raniuk, I.; Ratnikov, F.; Raven, G.; Ravonel Salzgeber, M.; Reboud, M.; Redi, F.; Reichert, S.; dos Reis, A. C.; Remon Alepuz, C.; Renaudin, V.; Ricciardi, S.; Richards, S.; Rihl, M.; Rinnert, K.; Robbe, P.; Robert, A.; Rodrigues, A. B.; Rodrigues, E.; Rodriguez Lopez, J. A.; Rogozhnikov, A.; Roiser, S.; Rollings, A.; Romanovskiy, V.; Romero Vidal, A.; Rotondo, M.; Rudolph, M. S.; Ruf, T.; Ruiz Valls, P.; Ruiz Vidal, J.; Saborido Silva, J. J.; Sadykhov, E.; Sagidova, N.; Saitta, B.; Salustino Guimaraes, V.; Sanchez Mayordomo, C.; Sanmartin Sedes, B.; Santacesaria, R.; Santamarina Rios, C.; Santimaria, M.; Santovetti, E.; Sarpis, G.; Sarti, A.; Satriano, C.; Satta, A.; Saunders, D. M.; Savrina, D.; Schael, S.; Schellenberg, M.; Schiller, M.; Schindler, H.; Schmelling, M.; Schmelzer, T.; Schmidt, B.; Schneider, O.; Schopper, A.; Schreiner, H. F.; Schubiger, M.; Schune, M. H.; Schwemmer, R.; Sciascia, B.; Sciubba, A.; Semennikov, A.; Sepulveda, E. S.; Sergi, A.; Serra, N.; Serrano, J.; Sestini, L.; Seyfert, P.; Shapkin, M.; Shapoval, I.; Shcheglov, Y.; Shears, T.; Shekhtman, L.; Shevchenko, V.; Siddi, B. G.; Silva Coutinho, R.; Silva de Oliveira, L.; Simi, G.; Simone, S.; Sirendi, M.; Skidmore, N.; Skwarnicki, T.; Smith, I. T.; Smith, J.; Smith, M.; Soares Lavra, l.; Sokoloff, M. D.; Soler, F. J. P.; Souza De Paula, B.; Spaan, B.; Spradlin, P.; Sridharan, S.; Stagni, F.; Stahl, M.; Stahl, S.; Stefko, P.; Stefkova, S.; Steinkamp, O.; Stemmle, S.; Stenyakin, O.; Stepanova, M.; Stevens, H.; Stone, S.; Storaci, B.; Stracka, S.; Stramaglia, M. E.; Straticiuc, M.; Straumann, U.; Sun, J.; Sun, L.; Swientek, K.; Syropoulos, V.; Szumlak, T.; Szymanski, M.; T'Jampens, S.; Tayduganov, A.; Tekampe, T.; Tellarini, G.; Teubert, F.; Thomas, E.; van Tilburg, J.; Tilley, M. J.; Tisserand, V.; Tobin, M.; Tolk, S.; Tomassetti, L.; Tonelli, D.; Tourinho Jadallah Aoude, R.; Tournefier, E.; Traill, M.; Tran, M. T.; Tresch, M.; Trisovic, A.; Tsaregorodtsev, A.; Tsopelas, P.; Tully, A.; Tuning, N.; Ukleja, A.; Usachov, A.; Ustyuzhanin, A.; Uwer, U.; Vacca, C.; Vagner, A.; Vagnoni, V.; Valassi, A.; Valat, S.; Valenti, G.; Vazquez Gomez, R.; Vazquez Regueiro, P.; Vecchi, S.; van Veghel, M.; Velthuis, J. J.; Veltri, M.; Veneziano, G.; Venkateswaran, A.; Verlage, T. A.; Vernet, M.; Vesterinen, M.; Viana Barbosa, J. V.; Vieira, D.; Vieites Diaz, M.; Viemann, H.; Vilasis-Cardona, X.; Vitti, M.; Volkov, V.; Vollhardt, A.; Voneki, B.; Vorobyev, A.; Vorobyev, V.; Voß, C.; de Vries, J. A.; Vázquez Sierra, C.; Waldi, R.; Walsh, J.; Wang, J.; Wang, Y.; Ward, D. R.; Wark, H. M.; Watson, N. K.; Websdale, D.; Weiden, A.; Weisser, C.; Whitehead, M.; Wicht, J.; Wilkinson, G.; Wilkinson, M.; Williams, M.; Williams, M.; Williams, T.; Wilson, F. F.; Wimberley, J.; Winn, M.; Wishahi, J.; Wislicki, W.; Witek, M.; Wormser, G.; Wotton, S. A.; Wyllie, K.; Xie, Y.; Xu, M.; Xu, Q.; Xu, Z.; Xu, Z.; Yang, Z.; Yang, Z.; Yao, Y.; Yin, H.; Yu, J.; Yuan, X.; Yushchenko, O.; Zarebski, K. A.; Zavertyaev, M.; Zhang, L.; Zhang, Y.; Zhelezov, A.; Zheng, Y.; Zhu, X.; Zhukov, V.; Zonneveld, J. B.; Zucchelli, S.

2018-01-01

A search is performed in the invariant mass spectrum of the B c + π+π- system for the excited B c + states B c (21 S 0)+ and B c (23 S 1)+ using a data sample of pp collisions collected by the LHCb experiment at the centre-of-mass energy of √{s}=8 TeV, corresponding to an integrated luminosity of 2 fb-1. No evidence is seen for either state. Upper limits on the ratios of the production cross-sections of the B c (21 S 0)+ and B c (23 S 1)+ states times the branching fractions of B c (21 S 0)+ → B c + π+π- and B c (23 S 1)+ → B c * +π+π- over the production cross-section of the B c + state are given as a function of their masses. They are found to be between 0.02 and 0.14 at 95% confidence level for B c (21 S 0)+ and B c (23 S 1)+ in the mass ranges [6830 , 6890] MeV /c 2 and [6795 , 6890] MeV /c 2, respectively. [Figure not available: see fulltext.

Defect States in Copper Indium Gallium Selenide Solar Cells from Two-Wavelength Excitation Photoluminescence Spectroscopy

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

Jensen, Soren A.; Dippo, Patricia; Mansfield, Lorelle M.

2016-11-21

We use two-wavelength excitation photoluminescence spectroscopy to probe defect states in CIGS thin films. Above-Eg excitation is combined with a tunable IR bias light that modulates the population of the defect states. We find that IR illumination in the range of 1400-2000 nm (0.62-0.89 eV) causes a reduction of the PL intensity, the magnitude of which scales linearly with IR power. Further, KF post deposition treatment has only a modest influence on the effect of the IR excitation. Initial data suggest that we have developed an optical characterization tool for band-gap defect states.

Coulomb string tension, asymptotic string tension, and the gluon chain

DOE PAGES

Greensite, Jeff; Szczepaniak, Adam P.

2015-02-01

We compute, via numerical simulations, the non-perturbative Coulomb potential and position-space ghost propagator in pure SU(3) gauge theory in Coulomb gauge. We find that that the Coulomb potential scales nicely in accordance with asymptotic freedom, that the Coulomb potential is linear in the infrared, and that the Coulomb string tension is about four times larger than the asymptotic string tension. We explain how it is possible that the asymptotic string tension can be lower than the Coulomb string tension by a factor of four.

Determination of differential cross sections for electron-impact excitation of electronic states of molecular oxygen

NASA Astrophysics Data System (ADS)

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

2000-02-01

The development and initial results of a method for the determination of differential cross sections for electron scattering by molecular oxygen are described. The method has been incorporated into an existing package of computer programs which, given spectroscopic factors, dissociation energies and an energy-loss spectrum for electron-impact excitation, determine the differential cross sections for each electronic state relative to that of the elastic peak. Enhancements of the original code were made to deal with particular aspects of electron scattering from O2, such as the overlap of vibrational levels of the ground state with transitions to excited states, and transitions to levels close to and above the dissocation energy in the Herzberg and Schumann-Runge continua. The utility of the code is specifically demonstrated for the ``6-eV states'' of O2, where we report absolute differential cross sections for their excitation by 15-eV electrons. In addition an integral cross section, derived from the differential cross section measurements, is also reported for this excitation process and compared against available theoretical results. The present differential and integral cross sections for excitation of the ``6-eV states'' of O2 are the first to be reported in the literature for electron-impact energies below 20 eV.

Compilation of giant electric dipole resonances built on excited states

NASA Astrophysics Data System (ADS)

Schiller, A.; Thoennessen, M.

2007-07-01

Giant Electric Dipole Resonance (GDR) parameters for γ decay to excited states with finite spin and temperature are compiled. Over 100 original works have been reviewed and from some 70 of them, about 350 sets of hot GDR parameters for different isotopes, excitation energies, and spin regions have been extracted. All parameter sets have been brought onto a common footing by calculating the equivalent Lorentzian parameters. The current compilation is complementary to an earlier compilation by Samuel S. Dietrich and Barry L. Berman (At. Data Nucl. Data Tables 38 (1988) 199-338) on ground-state photo-neutron and photo-absorption cross sections and their Lorentzian parameters. A comparison of the two may help shed light on the evolution of GDR parameters with temperature and spin. The present compilation is current as of July 2006.

Photoelectron wave function in photoionization: Plane wave or Coulomb wave? [Does photoionization of neutral targets produce Coulomb or plane waves?

DOE PAGES

Gozem, Samer; Gunina, Anastasia O.; Ichino, Takatoshi; ...

2015-10-28

The calculation of absolute total cross sections requires accurate wave functions of the photoelectron and of the initial and final states of the system. The essential information contained in the latter two can be condensed into a Dyson orbital. We employ correlated Dyson orbitals and test approximate treatments of the photoelectron wave function, that is, plane and Coulomb waves, by comparing computed and experimental photoionization and photodetachment spectra. We find that in anions, a plane wave treatment of the photoelectron provides a good description of photodetachment spectra. For photoionization of neutral atoms or molecules with one heavy atom, the photoelectronmore » wave function must be treated as a Coulomb wave to account for the interaction of the photoelectron with the +1 charge of the ionized core. For larger molecules, the best agreement with experiment is often achieved by using a Coulomb wave with a partial (effective) charge smaller than unity. This likely derives from the fact that the effective charge at the centroid of the Dyson orbital, which serves as the origin of the spherical wave expansion, is smaller than the total charge of a polyatomic cation. Finally, the results suggest that accurate molecular photoionization cross sections can be computed with a modified central potential model that accounts for the nonspherical charge distribution of the core by adjusting the charge in the center of the expansion.« less

Ultrafast 25-fs relaxation in highly excited states of methyl azide mediated by strong nonadiabatic coupling.

PubMed

Peters, William K; Couch, David E; Mignolet, Benoit; Shi, Xuetao; Nguyen, Quynh L; Fortenberry, Ryan C; Schlegel, H Bernhard; Remacle, Françoise; Kapteyn, Henry C; Murnane, Margaret M; Li, Wen

2017-12-26

Highly excited electronic states are challenging to explore experimentally and theoretically-due to the large density of states and the fact that small structural changes lead to large changes in electronic character with associated strong nonadiabatic dynamics. They can play a key role in astrophysical and ionospheric chemistry, as well as the detonation chemistry of high-energy density materials. Here, we implement ultrafast vacuum-UV (VUV)-driven electron-ion coincidence imaging spectroscopy to directly probe the reaction pathways of highly excited states of energetic molecules-in this case, methyl azide. Our data, combined with advanced theoretical simulations, show that photoexcitation of methyl azide by a 10-fs UV pulse at 8 eV drives fast structural changes and strong nonadiabatic coupling that leads to relaxation to other excited states on a surprisingly fast timescale of 25 fs. This ultrafast relaxation differs from dynamics occurring on lower excited states, where the timescale required for the wavepacket to reach a region of strong nonadiabatic coupling is typically much longer. Moreover, our theoretical calculations show that ultrafast relaxation of the wavepacket to a lower excited state occurs along one of the conical intersection seams before reaching the minimum energy conical intersection. These findings are important for understanding the unique strongly coupled non-Born-Oppenheimer molecular dynamics of VUV-excited energetic molecules. Although such observations have been predicted for many years, this study represents one of the few where such strongly coupled non-Born-Oppenheimer molecular dynamics of VUV-excited energetic molecules have been conclusively observed directly, making it possible to identify the ultrafast reaction pathways.

Proton-hole and core-excited states in the semi-magic nucleus 131In82

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

Taprogge, J.; Jungclaus, A.; Grawe, H.

2016-11-01

The decay of the N = 83 nucleus Cd-131 has been studied at the RIBF facility at the RIKEN Nishina Center. The main purpose of the study was to identify the position of the and proton-hole states and the energies of core-excited configurations in the semi-magic nucleus In-131. From the radiation emitted following the decay, a level scheme of In-131 was established and the feeding to each excited state determined. Similarities between the single-particle transitions observed in the decays of the N = 83 isotones In-132 and Cd-131 are discussed. Finally the excitation energies of several core-excited configurations in In-131more » are compared to QRPA and shell-model calculations.« less

Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy.

PubMed

Hayes, Dugan; Kohler, Lars; Hadt, Ryan G; Zhang, Xiaoyi; Liu, Cunming; Mulfort, Karen L; Chen, Lin X

2018-01-28

The kinetics of photoinduced electron and energy transfer in a family of tetrapyridophenazine-bridged heteroleptic homo- and heterodinuclear copper(i) bis(phenanthroline)/ruthenium(ii) polypyridyl complexes were studied using ultrafast optical and multi-edge X-ray transient absorption spectroscopies. This work combines the synthesis of heterodinuclear Cu(i)-Ru(ii) analogs of the homodinuclear Cu(i)-Cu(i) targets with spectroscopic analysis and electronic structure calculations to first disentangle the dynamics at individual metal sites by taking advantage of the element and site specificity of X-ray absorption and theoretical methods. The excited state dynamical models developed for the heterodinuclear complexes are then applied to model the more challenging homodinuclear complexes. These results suggest that both intermetallic charge and energy transfer can be observed in an asymmetric dinuclear copper complex in which the ground state redox potentials of the copper sites are offset by only 310 meV. We also demonstrate the ability of several of these complexes to effectively and unidirectionally shuttle energy between different metal centers, a property that could be of great use in the design of broadly absorbing and multifunctional multimetallic photocatalysts. This work provides an important step toward developing both a fundamental conceptual picture and a practical experimental handle with which synthetic chemists, spectroscopists, and theoreticians may collaborate to engineer cheap and efficient photocatalytic materials capable of performing coulombically demanding chemical transformations.

Electronic cooling via interlayer Coulomb coupling in multilayer epitaxial graphene

PubMed Central

Mihnev, Momchil T.; Tolsma, John R.; Divin, Charles J.; Sun, Dong; Asgari, Reza; Polini, Marco; Berger, Claire; de Heer, Walt A.; MacDonald, Allan H.; Norris, Theodore B.

2015-01-01

In van der Waals bonded or rotationally disordered multilayer stacks of two-dimensional (2D) materials, the electronic states remain tightly confined within individual 2D layers. As a result, electron–phonon interactions occur primarily within layers and interlayer electrical conductivities are low. In addition, strong covalent in-plane intralayer bonding combined with weak van der Waals interlayer bonding results in weak phonon-mediated thermal coupling between the layers. We demonstrate here, however, that Coulomb interactions between electrons in different layers of multilayer epitaxial graphene provide an important mechanism for interlayer thermal transport, even though all electronic states are strongly confined within individual 2D layers. This effect is manifested in the relaxation dynamics of hot carriers in ultrafast time-resolved terahertz spectroscopy. We develop a theory of interlayer Coulomb coupling containing no free parameters that accounts for the experimentally observed trends in hot-carrier dynamics as temperature and the number of layers is varied. PMID:26399955

Mapping the Coulomb Environment in Interference-Quenched Ballistic Nanowires.

PubMed

Gutstein, D; Lynall, D; Nair, S V; Savelyev, I; Blumin, M; Ercolani, D; Ruda, H E

2018-01-10

The conductance of semiconductor nanowires is strongly dependent on their electrostatic history because of the overwhelming influence of charged surface and interface states on electron confinement and scattering. We show that InAs nanowire field-effect transistor devices can be conditioned to suppress resonances that obscure quantized conduction thereby revealing as many as six sub-bands in the conductance spectra as the Fermi-level is swept across the sub-band energies. The energy level spectra extracted from conductance, coupled with detailed modeling shows the significance of the interface state charge distribution revealing the Coulomb landscape of the nanowire device. Inclusion of self-consistent Coulomb potentials, the measured geometrical shape of the nanowire, the gate geometry and nonparabolicity of the conduction band provide a quantitative and accurate description of the confinement potential and resulting energy level structure. Surfaces of the nanowire terminated by HfO 2 are shown to have their interface donor density reduced by a factor of 30 signifying the passivating role played by HfO 2 .

Vibrational frequencies and dephasing times in excited electronic states by femtosecond time-resolved four-wave mixing

NASA Astrophysics Data System (ADS)

Joo, Taiha; Albrecht, A. C.

1993-06-01

Time-resolved degenerate four-wave mixing (TRDFWM) for an electronically resonant system in a phase-matching configuration that measures population decay is reported. Because the spectral width of input light exceeds the vibrational Bohr frequency of a strong Raman active mode, the vibrational coherence produces strong oscillations in the TRDFWM signal together with the usual population decay from the excited electronic state. The data are analyzed in terms of a four-level system: ground and excited electronic states each split by a vibrational quantum of a Raman active mode. Absolute frequencies and their dephasing times of the vibrational modes at ≈590 cm -1 are obtained for the excited as well as the ground electronic state. The vibrational dephasing rate in the excited electronic state is about an order of magnitude faster than that in the ground state, the origin of which is speculated upon.

Excited states from quantum Monte Carlo in the basis of Slater determinants

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

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

2014-11-21

Building on the full configuration interaction quantum Monte Carlo (FCIQMC) algorithm introduced recently by Booth et al. [J. Chem. Phys. 131, 054106 (2009)] to compute the ground state of correlated many-electron systems, an extension to the computation of excited states (exFCIQMC) is presented. The Hilbert space is divided into a large part consisting of pure Slater determinants and a much smaller orthogonal part (the size of which is controlled by a cut-off threshold), from which the lowest eigenstates can be removed efficiently. In this way, the quantum Monte Carlo algorithm is restricted to the orthogonal complement of the lower excitedmore » states and projects out the next highest excited state. Starting from the ground state, higher excited states can be found one after the other. The Schrödinger equation in imaginary time is solved by the same population dynamics as in the ground state algorithm with modified probabilities and matrix elements, for which working formulae are provided. As a proof of principle, the method is applied to lithium hydride in the 3-21G basis set and to the helium dimer in the aug-cc-pVDZ basis set. It is shown to give the correct electronic structure for all bond lengths. Much more testing will be required before the applicability of this method to electron correlation problems of interesting size can be assessed.« less

Determination of ground and excited state dipole moments via electronic Stark spectroscopy: 5-methoxyindole

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