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Sample records for 3f4 excited states

  1. On the steady-state population of the Tm 3F4 and Ho 5I7 manifolds in a co-doped crystalline host

    The population of the Tm 3F4 and Ho 5I7 manifolds in a co-doped crystalline host has been calculated under local thermodynamic equilibrium conditions for an arbitrary excitation density. As a result, the normalized population of Ho ions vs. that of Tm ions proves to depend on the temperature and Stark sublevels but not the dopant composition. The equation for the fractional population of Tm, and Ho ions has been experimentally supported by mutilating the emission spectrum of 1%Ho:7%Tm:KYW crystal at higher pumping rates. - Highlights: • The fractional population of Tm, and Ho ions was calculated in the frame LTE approach for an arbitrary excitation density. • The equation for the fractional population of Tm, Ho ions has been supported experimentally. • The model seems to be widely applicable to optimizing the dopant composition in co-doped Ho,Tm gain crystals

  2. Excited states

    Lim, Edward C

    1974-01-01

    Excited States, Volume I reviews radiationless transitions, phosphorescence microwave double resonance through optical spectra in molecular solids, dipole moments in excited states, luminescence of polar molecules, and the problem of interstate interaction in aromatic carbonyl compounds. The book discusses the molecular electronic radiationless transitions; the double resonance techniques and the relaxation mechanisms involving the lowest triplet state of aromatic compounds; as well as the optical spectra and relaxation in molecular solids. The text also describes dipole moments and polarizab

  3. Excited states v.6

    Lim, Edward C

    2013-01-01

    Excited States, Volume 6 is a collection of papers that discusses the excited states of molecules. The first paper discusses the linear polyene electronic structure and potential surfaces, considering both the theoretical and experimental approaches in such electronic states. This paper also reviews the theory of electronic structure and cites some experimental techniques on polyene excitations, polyene spectroscopic phenomenology, and those involving higher states of polyenes and their triplet states. Examples of these experimental studies of excited states involve the high-resolution one-pho

  4. Excited states 2

    Lim, Edward C

    2013-01-01

    Excited States, Volume 2 is a collection of papers that deals with molecules in the excited states. The book describes the geometries of molecules in the excited electronic states. One paper describes the geometries of a diatomic molecule and of polyatomic molecules; it also discusses the determination of the many excited state geometries of molecules with two, three, or four atoms by techniques similar to diatomic spectroscopy. Another paper introduces an ordered theory related to excitons in pure and mixed molecular crystals. This paper also presents some experimental data such as those invo

  5. Excited states 4

    Lim, Edward C

    2013-01-01

    Excited States, Volume 4 is a collection of papers that deals with the excited states of molecular activity. One paper investigates the resonance Raman spectroscopy as the key to vibrational-electronic coupling. This paper reviews the basic theory of Raman scattering; it also explains the derivation of the Raman spectra, excitation profiles, and depolarization ratios for simple resonance systems. Another paper reviews the magnetic properties of triplet states, including the zero-field resonance techniques, the high-field experiments, and the spin Hamiltonian. This paper focuses on the magnetic

  6. Excited Charm States

    Characteristics of mass spectra and decays of orbitally excited charm mesons and baryons, expected on the basis of quark models and Heavy Quark Symmetry, are briefly described. The difficulties associated with measurements on these excited states are discussed. The accuracy and reliability of currently available experimental information is examined. The reasons, for the widely accepted spin-parity assignments to the observed excited mesons and baryons, are stated. Finally, the experimental data, with the accepted spin-parity assignments, is compared with expectations based on quark models and Heavy Quark Symmetry

  7. Excited States in 207Rn

    罗万居; 郭应祥; 周小红; 张玉虎; 雷相国; 刘忠; 郑勇; 柳敏良; 何建军; 竺礼华; 温书贤

    2003-01-01

    Excited states in 207Rn are investigated via the 196Pt(16O,Sn)207Rn reaction at beam energies from 85 to 95 MeV using techniques of in-beam γ-ray spectroscopy. Measurements ofγ-ray excitation function, x - γ and γ - γ- t coincidences are performed with ten BGO(AC)HPGe detectors. Based on these measurements, a level scheme of207Rn, including 17 γ-rays and 18 levels, is established. Spins for most of the levels are proposed according to the measured DCO ratios. The level structure is compared with a weak-coupling calculation using the interaction energies extracted from neighbouring nuclei.

  8. Excited state Intramolecular Proton Transfer in Anthralin

    Møller, Søren; Andersen, Kristine B.; Spanget-Larsen, Jens;

    1998-01-01

    Quantum chemical calculations performed on anthralin (1,8-dihydroxy-9(10H)-anthracenone) predict the possibility of an excited-state intramolecular proton transfer process. Fluorescence excitation and emission spectra of the compound dissolved in n-hexane at ambient temperature results in an......, associated with an excited-state intramolecular proton transfer process....

  9. Excited states in Pd99

    Sihotra, S.; Naik, Z.; Kumar, S.; Singh, K.; Goswamy, J.; Singh, N.; Kumar, R.; Singh, R. P.; Muralithar, S.; Bhowmik, R. K.; Palit, R.; Mehta, D.

    2011-02-01

    Excited states in the Pd99 nucleus populated in the As75(Si28, p3n) fusion-evaporation reaction at Elab=120 MeV have been investigated through in-beam γ-ray spectroscopic techniques using an array of Compton-suppressed clover detectors. The level scheme is established up to excitation energy ~11.5 MeV and spin ~25ℏ with the addition of about 60 new transitions. The level structures observed in Pd99 have been interpreted in the framework of a microscopic theory based on the deformed Hartree-Fock and angular momentum projection techniques. Band structures at lower spins are based on the low-Ω νg7/2 and νd5/2 orbitals, and those at higher spins are reproduced for the π(g9/2)5⊗π(g7/2)⊗ν(g7/2)2⊗ν(h11/2)2⊗ν(g9/2)-1 and π(g9/2)6⊗ν(g9/2)10⊗ν(g7/2)2⊗ν(h11/2) configurations. The octupole correlations in Pd99 have been inferred from new interband E1 transitions linking the ΔI=1 states of the bands based on the νh11/2 and νd5/2 orbitals (Δl=3, Δj=3, and Δπ=-1) with the deduced B(E1) values ~10-6 W.u.

  10. The mechanisms of Excited states in enzymes

    Petersen, Frederic Nicolas Rønne; Bohr, Henrik

    2010-01-01

    Enzyme catalysis is studied on the basis of excited state processes, which are of electronic, vibrational and thermal nature. The ways of achieving the excited state, such as photo-absorption and ligand binding, are discussed and exemplified by various cases of enzymes.......Enzyme catalysis is studied on the basis of excited state processes, which are of electronic, vibrational and thermal nature. The ways of achieving the excited state, such as photo-absorption and ligand binding, are discussed and exemplified by various cases of enzymes....

  11. Excited states rotational effects on the behavior of excited molecules

    Lim, Edward C

    2013-01-01

    Excited States, Volume 7 is a collection of papers that discusses the excited states of molecules. The first paper reviews the rotational involvement in intra-molecular in vibrational redistribution. This paper analyzes the vibrational Hamiltonian as to its efficacy in detecting the manifestations of intra-molecular state-mixing in time-resolved and time-averaged spectroscopic measurements. The next paper examines the temporal behavior of intra-molecular vibration-rotation energy transfer (IVRET) and the effects of IVRET on collision, reaction, and the decomposition processes. This paper also

  12. Excited states of {sup 15}C

    Cappuzzello, F.; Orrigo, S.E.A.; Cunsolo, A.; Allia, M.C.; Lazzaro, A.; Nociforo, C.; Winfield, J.S. [Istituto Nazionale di Fisica Nucleare, Lab. Nazionali del Sud, Catania (Italy); Lazzaro, A. [Catania Univ., Dipt. Fisica (Italy); Lenske, H. [Giessen Univ. (Germany). Inst. fuer Theoretische Physik; Beaumel, D.; Fortier, S. [Institut de Physique Nucleaire, (IN2P3/CNRS) 91 - Orsay (France); Foti, A. [Istituto Nazionale di Fisica Nucleare, Catania (Italy)

    2004-03-01

    The N{sup 15}(Li{sup 7},Be{sup 7})C{sup 15} reaction at 55 MeV incident energy was studied at forward angles in order to explore the C{sup 15} excitation energy spectrum. The C{sup 15} ground state and the states at E{sub x} = 0.77, 6.77, 7.30, 8.50 MeV excitation energies were populated. The energy resolution ({approx} 250 keV) allowed the identification of these transitions each for Be{sup 7} ground and first-excited state at E{sub x} = 0.429 MeV. Quasi-particle random phase approximation (QRPA) calculations reproduce the C{sup 15} level structure below 1.5 MeV excitation energy. The strength observed at higher excitation energies probably arises from core-excited components of C{sup 15}. (authors)

  13. Excited-state dynamics of astaxanthin aggregates

    Fuciman, M.; Durchan, Milan; Šlouf, V.; Kesan, G.; Polívka, Tomáš

    2013-01-01

    Roč. 568, č. 1 (2013), s. 21-25. ISSN 0009-2614 Institutional support: RVO:60077344 Keywords : astaxanthin * aggregates * excited states Subject RIV: BO - Biophysics Impact factor: 1.991, year: 2013

  14. Excited state g factors in Te125

    Chamoli, S. K.; Stuchbery, A. E.; East, M. C.

    2009-11-01

    The transient-field technique has been used to measure, with considerably improved precision, the g factors of the 3/2+ and 5/2+ states in Te125 at 444 and 463 keV, respectively, relative to the g factor of the first excited state in Te126. Together with shell model and weak-coupling core-excitation model calculations, the g-factor measurements provide insight into the orbital occupation of the odd neutron for the low-excitation states in Te125. A new 9/2+ level at 1029 keV, together with a firm 7/2+ spin assignment for the level at 1018 keV, identifies candidate states for the coupling of the s1/2 neutron to the 4+ core excitation.

  15. Excited-state properties of hydrophilic carotenoids

    Fuciman, M.; Chábera, P.; Naqvi, K.R.; Melo, T.B.; Sliwka, H.R.; Partali, V.; Lockwood, S.; Jackson, H.L.; Polívka, Tomáš

    - : -, 2009. s. 408. ISBN N. [International Conference on Photochemistry /24./. 19.07.2009-24.07.2009, Toledo] Institutional research plan: CEZ:AV0Z50510513 Keywords : carotenoids * excited-state dynamics * femtosecond spectroscopy Subject RIV: BO - Biophysics

  16. Excitation Halo States of 12B

    林承键; 刘祖华; 张焕乔; 吴岳伟; 杨峰; 阮明

    2001-01-01

    Angular distributions for the 11 B(d,p)12 B transfer reactions have been measured at E1ab = 11.8 Me V. The asymp-totic normalization coefficients (ANC) of the ground state, the second and third excitation states for 12B ( 11 B+n) are extracted from the differential cross sections at three forward angles. With these ANCs, the root-mean-square radii are calculated for these three states. The results show that the second and third excitation states of 12B are neutron halo states.

  17. Rearrangements in ground and excited states

    de Mayo, Paul

    2013-01-01

    Rearrangements in Ground and Excited States, Volume 3 presents essays on the chemical generation of excited states; the cis-trans isomerization of olefins; and the photochemical rearrangements in trienes. The book also includes essays on the zimmerman rearrangements; the photochemical rearrangements of enones; the photochemical rearrangements of conjugated cyclic dienones; and the rearrangements of the benzene ring. Essays on the photo rearrangements via biradicals of simple carbonyl compounds; the photochemical rearrangements involving three-membered rings or five-membered ring heterocycles;

  18. Excited states of 129Xe

    Here investigation of the observed yrast and excited bands in 129Xe populated by the heavy-ion fusion reaction 124Sn(11B, p5n)129Xe has been presented. An isotopically enriched (99.9%) self-supporting 124Sn target of thickness 2.2 mg/cm2 was utilized. The experiment was performed at the Linac accelerator facility at the Tata Institute of Fundamental Research (TIFR), Mumbai, India. The experimental set-up, called the Indian National Gamma Array (INGA), consisted of 21 Compton suppressed clover HPGe detectors. Two of these detectors were placed at 23°, three at 40°, three at 65°, four at 90°, three at 140°, three at 115° and three at 157° with respect to the beam direction. The triple gamma coincidence data were collected in the event-by-event mode

  19. Photoionization of excited molecular states using multiphoton excitation techniques

    Photoelectron spectra are reported for three photon resonant, four photon ionization of H2 via the B 1Σ/sub u/+, v = 7 (J = 2,4) and C 1π/sub u'/, v = 0-4 (J = 1) levels and of N2 via the o31π/sub u'/, v = 1,2, b 1π/sub u'/, v = 3-5, and c 1π/sub u'/, v = 0 levels. The results reflect both the spectroscopy and the dynamics of photoionization of excited molecular states and are discussed in terms of the selection rules for photoionization and the relative probabilities of photoionization from Rydberg and valence states. In some cases, in accordance with the Franck-Condon principle, the results demonstrate that resonant multiphoton ionization through Rydberg states may be a powerful technique for the production of electronic, vibrational, and rotational state selected ions. However, in other cases, systematic departures from Franck-Condon factors are observed, which reflect the more subtle dynamics of excited state photoionization. 23 references, 6 figures, 2 tables

  20. Photoionization of excited molecular states using multiphoton excitation techniques

    Dehmer, Patricia M. [Argonne National Laboratory (ANL), Argonne, IL (United States); Pratt, Stephen T. [Argonne National Laboratory (ANL), Argonne, IL (United States); Dehmer, Joseph L. [Argonne National Laboratory (ANL), Argonne, IL (United States)

    1984-01-01

    Photoelectron spectra are reported for three photon resonant, four photon ionization of H₂ via the B ¹Σu⁺, v = 7 (J = 2,4) and C ¹Πu v = 0-4 (J = 1) levels and of N₂ via the o₃ ¹Πu, v = 1,2, b ¹Πu, v = 3-5, and c ¹Πu, v = 0 levels. The results reflect both the spectroscopy and the dynamics of photoionization of excited molecular states and are discussed in terms of the selection rules for photoionization and the relative probabilities of photoionization from Rydberg and valence states. In some cases, in accordance with the Franck-Condon principle, the results demonstrate that resonant multiphoton ionization through Rydberg states may be a powerful technique for the production of electronic, vibrational, and rotational state selected ions. However, in other cases, systematic departures from Franck-Condon factors are observed, which reflect the more subtle dynamics of excited state photoionization.

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

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

    2016-03-01

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

  2. Application of the coherent state formalism to multiply excited states

    A general expression is obtained for the matrix element of an m-body operator between coherent states constructed from multiple orthogonal coherent boson species. This allows the coherent state formalism to be applied to states possessing an arbitrarily large number of intrinsic excitation quanta. For illustration, the formalism is applied to the two-dimensional vibron model (U(3) model), to calculate the energies of all excited states in the large-N limit

  3. Nodal Variational Principle for Excited States

    Zahariev, Federico; Levy, Mel

    2016-01-01

    It is proven that the exact excited-state wavefunction and energy may be obtained by minimizing the energy expectation value of a trial wave function that is constrained only to have the correct nodes of the state of interest. This excited-state nodal minimum principle has the advantage that it requires neither minimization with the con- straint of wavefunction orthogonality to all lower eigenstates nor the antisymmetry of the trial wavefunctions. It is also found that the minimization over the entire space can be partitioned into several in- terconnected minimizations within the individual nodal regions, and the exact excited-state energy may be obtained by a minimization in just one or several of these nodal regions. For the proofs of the the- orem, it is observed that the many-electron eigenfunction, restricted to a nodal region, is equivalent to a ground state wavefunction of one electron in a higher dimensional space; and an explicit excited-state energy variational expression is obtained by generalizing...

  4. Computing Correct Truncated Excited State Wavefunctions

    Bacalis, N C; Zang, J; Karaoulanis, D

    2016-01-01

    We demonstrate that, if a truncated expansion of a wave function 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.

  5. Impact of ground- and excited-state aromaticity on cyclopentadiene and silole excitation energies and excited-state polarities.

    Jorner, Kjell; Emanuelsson, Rikard; Dahlstrand, Christian; Tong, Hui; Denisova, Aleksandra V; Ottosson, Henrik

    2014-07-21

    A new qualitative model for estimating the properties of substituted cyclopentadienes and siloles in their lowest ππ* excited states is introduced and confirmed through quantum chemical calculations, and then applied to explain earlier reported experimental excitation energies. According to our model, which is based on excited-state aromaticity and antiaromaticity, siloles and cyclopentadienes are cross-hyperconjugated "aromatic chameleons" that adapt their electronic structures to conform to the various aromaticity rules in different electronic states (Hückel's rule in the π(2) electronic ground state (S0) and Baird's rule in the lowest ππ* excited singlet and triplet states (S1 and T1)). By using pen-and-paper arguments, one can explain polarity changes upon excitation of substituted cyclopentadienes and siloles, and one can tune their lowest excitation energies by combined considerations of ground- and excited-state aromaticity/antiaromaticity effects. Finally, the "aromatic chameleon" model can be extended to other monocyclic compound classes of potential use in organic electronics, thereby providing a unified view of the S0, T1, and S1 states of a range of different cyclic cross-π-conjugated and cross-hyperconjugated compound classes. PMID:25043523

  6. Excited state properties of aryl carotenoids

    Fuciman, M.; Chábera, P.; Župčanová, Anita; Hříbek, P.; Arellano, J.B.; Vácha, František; Pšenčík, J.; Polívka, Tomáš

    2010-01-01

    Roč. 12, č. 13 (2010), s. 3112-3120. ISSN 1463-9076 R&D Projects: GA AV ČR IAA608170604 Institutional research plan: CEZ:AV0Z50510513 Keywords : carotenoids * excited-states * femtosecond spectroscopy Subject RIV: BO - Biophysics Impact factor: 3.454, year: 2010

  7. Excited-state properties of hydrophilic carotenoids

    Chábera, P.; Naqvi, K.R.; Melo, T.B.; Sliwka, H.R.; Partali, V.; Lockwood, S.; Nodolski, G.; Polívka, Tomáš

    Nové Hrady : Academic and University Center, 2008. s. 40. [ESF Workshop on Novel Methods in Exploring Carotenoid Excited State Dynamics. 21.09.2008-25.09.2008, Nové Hrady] Institutional research plan: CEZ:AV0Z50510513 Keywords : carotenoids * biophysics Subject RIV: BO - Biophysics

  8. Femtosecond spectroscopy of reacting excited states

    Thanks to recent advance of ultra short pulse lasers, we are now able to observe ultra fast phenomena taking place in a time scale as short as 10 fs. This time scale is the time scale of the nuclear motion of molecules, and the observation of coherent nuclear wavepacket motion is a central issue of femtosecond spectroscopy. One of the dreams of chemists is to see chemical reactions, i.e., the change of chemical bonds, in real time. In a sense, observation of the wavepacket motion of reacting molecules is realization of this dream. However, the significance of the coherent nuclear motion in chemical reactions is still unclear for polyatomic molecules where the reaction coordinate does not simply correspond to the change of a particular chemical bond. To discuss the relation between the initial coherent wavepacket motion and the reaction coordinate, we studied several fundamental photochemical reactions in solution, i.e., photoisomerization of cis-stilbene, photodissociation of diphenylcyclopropenone and excited-state intramolecular proton transfer of 10-hydorxybenzoquinoline, using two-color pump-probe spectroscopy with time resolution of 30-70 fs. The photoisomerization of cis-stilbene proceeds in the S1 state in a time scale of ∼1 ps. Time-resolved absorption of cis-stilbene in cyclohexane (pump 315 nm; probe 660 nm) clearly showed an oscillatory feature, which was attributed to the ∼220 cm-1 wavepacket motion in the S1 state. The dephasing time of the wavepacket motion was 0.21±0.04 ps, which was much shorter than the isomerization time of S1 cis-stilbene (1.25 ps). This indicates that a fast dephasing of the vibrational coherence takes place before isomerization. The result of the experiments on the solvent dependence demonstrated that the dephasing rate and isomerization rate do not correlate with each other, indicating that the observed wavepacket motion is not directly coupled with the isomerization coordinate. Photoexcitation to the S2 state of

  9. Extension of LCAO to excited states

    Koval, Peter; Foerster, Dietrich

    2009-01-01

    We extend the LCAO (Linear Combination of Atomic Orbitals) method to excited states by constructing a particularly simple basis in the space of orbital products. The residual error of our procedure vanishes exponentially with the number of products and our procedure avoids auxiliary sets of fitting functions and their intrinsic ambiguities. As an application of our technique, we compute the Kohn--Sham density response function $\\chi_{0}$ for a molecule consisting of $N$ atoms in $O(N^{2}N_{\\o...

  10. Rearrangements in ground and excited states

    de Mayo, Paul

    2013-01-01

    Rearrangements in Ground and Excited States, Volume 2 covers essays on the theoretical approach of rearrangements; the rearrangements involving boron; and the molecular rearrangements of organosilicon compounds. The book also includes essays on the polytopal rearrangement at phosphorus; the rearrangement in coordination complexes; and the reversible thermal intramolecular rearrangements of metal carbonyls. Chemists and people involved in the study of rearrangements will find the book invaluable.

  11. Excited States in Solution through Polarizable Embedding

    Olsen, Jógvan Magnus; Aidas, Kestutis; Kongsted, Jacob

    2010-01-01

    We present theory and implementation of an advanced quantum mechanics/molecular mechanics (QM/MM) approach using a fully self-consistent polarizable embedding (PE) scheme. It is a polarizable layered model designed for effective yet accurate inclusion of an anisotropic medium in a quantum mechani......, nanoparticles and solute−solvent systems. Here, we present numerical examples of solvent shifts and excited-state properties related to a set of organic molecules in aqueous solution....

  12. Identification of excited states in conjugated polymers

    Hartwell, L J

    2003-01-01

    This thesis reports quasi steady state photoinduced absorption measurements from three conjugated polymers: polypyridine (PPy), polyfluorene (PFO) and the emeraldine base (EB) form of polyaniline. The aim of these experiments was to determine the nature of the photoexcited states existing in these materials in the millisecond time domain, as this has important consequences for the operation of real devices manufactured using these materials. The results from the photoinduced absorption experiments are closely compared with published results from pulse radiolysis experiments. In all cases there is very good correspondence between the two data sets, which has enabled the photoexcited states to be assigned with a high degree of confidence. Quasi steady-state photoinduced absorption involves the measurement of the change in absorption of a material in response to optical excitation with a laser beam. The changes in absorption are small, so a instrument was developed and optimised for each different sample. Lock-i...

  13. Holographic Construction of Excited CFT States

    Christodoulou, Ariana

    2016-01-01

    We present a systematic construction of bulk solutions that are dual to CFT excited states. The bulk solution is constructed perturbatively in bulk fields. The linearised solution is universal and depends only on the conformal dimension of the primary operator that is associated with the state via the operator-state correspondence, while higher order terms depend on detailed properties of the operator, such as its OPE with itself and generally involve many bulk fields. We illustrate the discussion with the holographic construction of the universal part of the solution for states of two dimensional CFTs, either on $R \\times S^1$ or on $R^{1,1}$. We compute the 1-point function both in the CFT and in the bulk, finding exact agreement. We comment on the relation with other reconstruction approaches.

  14. Ultrafast excited-state dynamics of isocytosine.

    Szabla, Rafał; Góra, Robert W; Šponer, Jiří

    2016-07-27

    The alternative nucleobase isocytosine has long been considered as a plausible component of hypothetical primordial informational polymers. To examine this hypothesis we investigated the excited-state dynamics of the two most abundant forms of isocytosine in the gas phase (keto and enol). Our surface-hopping nonadiabatic molecular dynamics simulations employing the algebraic diagrammatic construction to the second order [ADC(2)] method for the electronic structure calculations suggest that both tautomers undergo efficient radiationless deactivation to the electronic ground state with time constants which amount to τketo = 182 fs and τenol = 533 fs. The dominant photorelaxation pathways correspond to ring-puckering (ππ* surface) and C[double bond, length as m-dash]O stretching/N-H tilting (nπ* surface) for the enol and keto forms respectively. Based on these findings, we infer that isocytosine is a relatively photostable compound in the gas phase and in these terms resembles biologically relevant nucleobases. The estimated S1 [radiolysis arrow - arrow with voltage kink] T1 intersystem crossing rate constant of 8.02 × 10(10) s(-1) suggests that triplet states might also play an important role in the overall excited-state dynamics of the keto tautomer. The reliability of ADC(2)-based surface-hopping molecular dynamics simulations was tested against multireference quantum-chemical calculations and the potential limitations of the employed ADC(2) approach are briefly discussed. PMID:27346684

  15. Dynamic hyperpolarizabilities of excited states of hydrogen

    On the basis of the generalized Sturm expansion of the radial part of the Coulomb Green function, a computational method is proposed and numerical results are presented for the dynamic hyperpolarizability γ and the corrections E(4) (quadratic in the light intensity) to the quasi-energy of the ground and excited states of hydrogen with principal quantum numbers n ≤ 5 in a monochromatic light field. In this approach, the problem is reduced to the summation of well-convergent double series of the hypergeometric kind, which ensures reliable numerical results both for states with a large n, and in a wide range of field frequencies ω, including the above-threshold frequency range of (ℎ/2π)ω >> vertical bar En vertical bar (vertical bar En vertical bar is the ionization potential of the state |nlm> under investigation). We consider the frequency dependence of γ and E(4), their differences for the cases of linear and circular polarizations of the field, and the relation between their real and imaginary parts, which determine the laser field-induced corrections to the position and width of energy levels. For n = 5, the significant role of mixing the vertical bar nlm> states with different values of l by a laser field in the region of resonances on intermediate bound states is demonstrated. The linear (in intensity) corrections to the photoionization cross section for excited states are analyzed and the threshold intensity corresponding to the onset of atomic level stabilization is estimated for a number of states with n = 3 and n = 5

  16. Excited state dynamics of DNA bases

    Kleinermanns, K.; Nachtigallová, Dana; de Vries, M. S.

    2013-01-01

    Roč. 32, č. 2 (2013), s. 308-342. ISSN 0144-235X R&D Projects: GA ČR GAP208/12/1318 Grant ostatní: National Science Foundation(US) CHE-0911564; NASA(US) NNX12AG77G; Deutsche Forschungsgemeinschaft(DE) SFB 663; Deutsche Forschungsgemeinschaft(DE) KI 531-29 Institutional support: RVO:61388963 Keywords : DNA bases * nucleobases * excited state * dynamics * computations * gas phase * conical intersections Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 4.920, year: 2013

  17. Excited states of muonium in atomic hydrogen

    V S Kulhar

    2006-06-01

    Muonium formation in excited states in muon-hydrogen charge-exchange collision is investigated using a method developed in a previous paper. Differential cross-section results are found to resemble positronium formation cross-section results of positron-hydrogen charge-exchange problem. Forward differential and integrated cross-sections are computed for muon energy of 2 keV and higher. Total muonium formation cross-sections are computed using Jackson and Schiff scaling rules. Muonium formation cross-section results obtained from proton-hydrogen charge-exchange cross-section results, using velocity scaling are compared with the results of the present calculation.

  18. Excited state halos in 10Be

    The structure of certain bound excited states in 10Be have been shown to have exotic features because of their weak binding and cluster-like configurations. In this article, we investigate E1 and E2 transitions between these states and compare the findings with recent experimental results. We compare the predictions of two types of structure calculations: a microscopic multicluster model and an ab initio no-core shell model. Both predict very similar transition strengths. By considering the relative contributions from the various matrix elements contributing to the transitions arising from the coupling of different 9Bexn configurations in the wave functions making up the states, we conclude that the very weak B(E1;2-→21+) can only be understood if the 2- state (with a separation energy of its predominantly 1s1/2 neutron of just 0.548 MeV) is a clear halo state. Other nearby states, such as the 22+, do not exhibit a clear halo signature because of the less than clean decoupling into the well-defined 9Be core plus halo neutron

  19. Excited-state relaxation of some aminoquinolines

    B. M. Uzhinov

    2006-04-01

    Full Text Available The absorption and fluorescence spectra, fluorescence quantum yields and lifetimes, and fluorescence rate constants (kf of 2-amino-3-(2′-benzoxazolylquinoline (I, 2-amino-3-(2′-benzothiazolylquinoline (II, 2-amino-3-(2′-methoxybenzothiazolyl-quinoline (III, 2-amino-3-(2′-benzothiazolylbenzoquinoline (IV at different temperatures have been measured. The shortwavelength shift of fluorescence spectra of compounds studied (23–49 nm in ethanol as the temperature decreases (the solvent viscosity increases points out that the excited-state relaxation process takes place. The rate of this process depends essentially on the solvent viscosity, but not the solvent polarity. The essential increasing of fluorescence rate constant kf (up to about 7 times as the solvent viscosity increases proves the existence of excited-state structural relaxation consisting in the mutual internal rotation of molecular fragments of aminoquinolines studied, followed by the solvent orientational relaxation.

  20. Lifetimes of excited states in 164Hf

    Lifetimes of excited states in 164Hf were measured using the Doppler-shift recoil-distance method. Gamma-gamma coincidences at eleven target-stopper distances were measured using the twelve Compton-suppressed Ge-detectors of the OSIRIS spectrometer. From the coincidence spectra the intensities of the Doppler-shifted and unshifted γ-lines were determined. The quadrupole moments Qt of transitions within the rotational bands derived from the lifetimes are constant within the experimental uncertainties up to the 18+ state. The Qt value for the transition between the ground- and the neutron i213/2 band (s-band) which is strongly reduced compared to the values of the in-band transitions is used to deduce a band interaction energy of 34 keV≤V≤57 keV. (orig.)

  1. Lifetimes of 167Yb excited states

    Lifetimes of 167Yb excited states arising at the decay of 167Lu → 167Yb monoisotope have been determined using eγ and γγ delayed coincidence methods. The time spectrometers mounted on the base of a magnetic lens β-spectrometer and a scintillation detector, a scintillation and a Ge(Li) detectors, a scintillation and Si(Li)-detectors are used. 167Yb level fifetimes are measured with energies of 29 keV (Tsub(1/2)=13.5(7) ns), 78 keV (Tsub(1/2=0.84(4) ns), 178 keV (Tsub(1/2)167Yb investigated levels are analysed. On the basis of intrarotational transitions internal quadrupole momenta of 5/2-/523/, 3/2-/512/ and 1/2-/521/ bands have been determined

  2. Excited state quantum phase transitions in many-body systems

    Phenomena analogous to ground state quantum phase transitions have recently been noted to occur among states throughout the excitation spectra of certain many-body models. These excited state phase transitions are manifested as simultaneous singularities in the eigenvalue spectrum (including the gap or level density), order parameters, and wave function properties. In this article, the characteristics of excited state quantum phase transitions are investigated. The finite-size scaling behavior is determined at the mean-field level. It is found that excited state quantum phase transitions are universal to two-level bosonic and fermionic models with pairing interactions

  3. Representation of electronic excited states by conditional wavefunction

    Koichiro, Yamaguchi; Yoshiaki, Ito; Takeshi, Mukoyama

    2000-03-01

    Hartree-Fock scheme is an ordinary method to calculate the zeroth order approximation for non-relativistic electronic excited states of atoms and molecules. The accuracy of zeroth order hamiltonian affects the efficiency of higher order estimation of the Hamiltonian and the Green's function. To improve the preciseness of zeroth order Hamiltonian, we try to include the relaxation of electronic excited states into zeroth order approximation by using conditional wavefunction representation instead of Hartree-Fock method. Our method is illustrated by the calculation of electronic double-excited states of Helium and single-excited states of Neon. Further extention of our formulation for multiple-exfcited states are also discussed.

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

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

  5. Excited states in DNA strands investigated by ultrafast laser spectroscopy.

    Chen, Jinquan; Zhang, Yuyuan; Kohler, Bern

    2015-01-01

    Ultrafast laser experiments on carefully selected DNA model compounds probe the effects of base stacking, base pairing, and structural disorder on excited electronic states formed by UV absorption in single and double DNA strands. Direct π-orbital overlap between two stacked bases in a dinucleotide or in a longer single strand creates new excited states that decay orders of magnitude more slowly than the generally subpicosecond excited states of monomeric bases. Half or more of all excited states in single strands decay in this manner. Ultrafast mid-IR transient absorption experiments reveal that the long-lived excited states in a number of model compounds are charge transfer states formed by interbase electron transfer, which subsequently decay by charge recombination. The lifetimes of the charge transfer states are surprisingly independent of how the stacked bases are oriented, but disruption of π-stacking, either by elevating temperature or by adding a denaturing co-solvent, completely eliminates this decay channel. Time-resolved emission measurements support the conclusion that these states are populated very rapidly from initial excitons. These experiments also reveal the existence of populations of emissive excited states that decay on the nanosecond time scale. The quantum yield of these states is very small for UVB/UVC excitation, but increases at UVA wavelengths. In double strands, hydrogen bonding between bases perturbs, but does not quench, the long-lived excited states. Kinetic isotope effects on the excited-state dynamics suggest that intrastrand electron transfer may couple to interstrand proton transfer. By revealing how structure and non-covalent interactions affect excited-state dynamics, on-going experimental and theoretical studies of excited states in DNA strands can advance understanding of fundamental photophysics in other nanoscale systems. PMID:25326834

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

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

    2009-11-01

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

  7. Exact ensemble density-functional theory for excited states

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

    2014-01-01

    We construct exact Kohn-Sham potentials for the ensemble density-functional theory (EDFT) of excited states from the ground and excited states of helium. The exchange-correlation potential is compared with current approximations, which miss prominent features. The ensemble derivative discontinuity is tested, and the virial theorem is proven and illustrated.

  8. Charge-displacement analysis for excited states

    Ronca, Enrico, E-mail: enrico@thch.unipg.it; Tarantelli, Francesco, E-mail: francesco.tarantelli@unipg.it [Istituto CNR di Scienze e Tecnologie Molecolari, via Elce di Sotto 8, I-06123 Perugia (Italy); Dipartimento di Chimica, Biologia e Biotecnologie, Università degli Studi di Perugia, via Elce di Sotto 8, I-06123 Perugia (Italy); Pastore, Mariachiara, E-mail: chiara@thch.unipg.it; Belpassi, Leonardo; De Angelis, Filippo [Istituto CNR di Scienze e Tecnologie Molecolari, via Elce di Sotto 8, I-06123 Perugia (Italy); Angeli, Celestino; Cimiraglia, Renzo [Dipartimento di Scienze Chimiche e Farmaceutiche, Università degli Studi di Ferrara, via Borsari 46, I-44100 Ferrara (Italy)

    2014-02-07

    We extend the Charge-Displacement (CD) analysis, already successfully employed to describe the nature of intermolecular interactions [L. Belpassi et al., J. Am. Chem. Soc. 132, 13046 (2010)] and various types of controversial chemical bonds [L. Belpassi et al., J. Am. Chem. Soc. 130, 1048 (2008); N. Salvi et al., Chem. Eur. J. 16, 7231 (2010)], to study the charge fluxes accompanying electron excitations, and in particular the all-important charge-transfer (CT) phenomena. We demonstrate the usefulness of the new approach through applications to exemplary excitations in a series of molecules, encompassing various typical situations from valence, to Rydberg, to CT excitations. The CD functions defined along various spatial directions provide a detailed and insightful quantitative picture of the electron displacements taking place.

  9. Bogoliubov Excited States and the Lyth Bound

    Aravind, Aditya; Paban, Sonia

    2014-01-01

    We show that Bogoliubov excited scalar and tensor modes do not alleviate Planckian evolution during inflation if one assumes that $r$ and the Bogoliubov coefficients are approximately scale invariant. We constrain the excitation parameter for the scalar fluctuations, $\\beta$, and tensor perturbations, $\\tilde{\\beta}$, by requiring that there be at least three decades of scale invariance in the scalar and tensor power spectrum. For the scalar fluctuations this is motivated by the observed nearly scale invariant scalar power spectrum. For the tensor fluctuations this assumption may be shown to be valid or invalid by future experiments.

  10. Inelastic scattering of 9Li and excitation mechanism of its first excited state

    The first measurement of inelastic scattering of 9Li from deuterons at the ISAC facility is reported. The measured angular distribution for the first excited state confirms the nature of excitation to be an E2 transition. The quadrupole deformation parameter is extracted from an analysis of the angular distribution

  11. Density functional theory generalized to degenerate excited states

    In this paper it is shown that the density functional theory can be generalized to systems with degenerate excited states. There is a one-to-one map between the subspace, spanned by the ground state and any one of the first degenerate excited states, and the sum of their densities. But only a one way correspondence exists between external potential and subspace, as well as between external potential and the sum of densities. The extension of the Hohenberg-Kohn-Sham theory for degenerate excited states has also been developed. (author)

  12. Charge transfer excitations from excited state Hartree-Fock subsequent minimization scheme

    Theophilou, Iris; Thanos, S

    2014-01-01

    Photoinduced charge transfer processes play a key role for novel photovoltaic phenomena and devices. Thus, the development of ab initio methods that allow for accurate and computationally inexpensive treatment of charge transfer excitations is a topic that attracts nowadays a lot of scientific attention. In this paper we extend an approach recently introduced for the description of single and double excitations (M. Tassi, I. Theophilou and S. Thanos, Int. J. Quantum Chem., {113}, 690 (2013), M. Tassi, I. Theophilou and S. Thanos, J. Chem. Phys. {138}, 124107 (2013)) to allow for the description of intermolecular charge transfer excitations. For the description of an excitation where an electron is transferred from a donor system to an acceptor one, it is necessary to keep the excited state orthogonal to the ground sate in order to avoid variational collapse. These conditions are achieved by decomposing the subspace spanned by the Hartree-Fock (HF) ground state orbitals to four subspaces: The subspace spanned ...

  13. 18Ne Excited States Two-Proton Decay

    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.

  14. Photoionization of excited states of neon-like Mg III

    Narendra Singh; Man Mohan

    2002-04-01

    The close coupling -matrix method is used to calculate cross-sections for photoionization of Mg III from its first three excited states. Configuration interaction wave functions are used to represent two target states of Mg III retained in the -matrix expansion. The positions and effective quantum numbers for the Rydberg series converging to the excited state 2226 \\ 2 of the residual ion, are predicted.

  15. Quantum entanglement of localized excited states at finite temperature

    Caputa, Pawel; Simón, Joan; Štikonas, Andrius(School of Mathematics and Maxwell Institute for Mathematical Sciences, University of Edinburgh, King’s Buildings, Edinburgh, EH9 3FD, U.K.); Takayanagi, Tadashi

    2015-01-01

    In this work we study the time evolutions of (Renyi) entanglement entropy of locally excited states in two dimensional conformal field theories (CFTs) at finite temperature.We consider excited states created by acting with local operators on thermal states and give both field theoretic and holographic calculations. In free field CFTs, we find that the growth of Renyi entanglement entropy at finite temperature is reduced compared to the zero temperature result by a small quantity proportional ...

  16. Energy levels of Sm2+ excited state

    The energy levels of excited configurations 4f5u'l' of Sm2+ calculated in detail by using unitary group approach are covered. The energy expressions with slater integral as parameters are given and the spin-orbit coupling is considered according to the Russell-Saunders approximation. The coupling parameters λ of the main energy levels are also calculated in the paper

  17. Increased radiative lifetime of Tm3+:3F4 → 3H6 transition in oxyfluoride tellurite glasses

    Highlights: • We prepare Tm3+-doped tellurite-zinc glasses with F− substitution. • Thermal stability becomes better with increasing F− in present glasses. • Tm3+ 1.8 μm radiative lifetime increases with F− concentration. • The origin of the increased lifetime has been discussed. - Abstract: The 1.8 μm emission properties of Tm3+-doped zinc tellurite glasses modified by the substitution of ZnF2 are investigated in this paper. The thermal stability, Raman and phonon sideband spectra, transmission and absorption spectra, emission spectra and decay curves are discussed. It is found that substitution of fluoride ions into the zinc tellurite matrix produces dramatic increase in the emission lifetime of Tm3+ 1.8 μm emission. Absorption, Raman and phonon sideband spectra are used to estimate the local structure of Tm3+ ions. These analyses indicate structural change around Tm3+ ions caused by substitution of fluoride ions monitors the increased intrinsic radiative lifetimes. An increase in the measured radiative lifetimes of the Tm3+:3F4 → 3H6 transition is observed. The origin has been discussed and the reduction of OH− absorption, decrease of maximum phonon energy and phonon density are considered to be dominant in all of the nonradiative relaxations

  18. Excited state systematics in extracting nucleon electromagnetic form factors

    Capitani, Stefano; von Hippel, Georg; Jäger, Benjamin; Knippschild, Bastian; Meyer, Harvey B; Rae, Thomas D; Wittig, Hartmut

    2012-01-01

    We present updated preliminary results for the nucleon electromagnetic form factors for non-perturbatively $\\mathcal{O}(a)$ improved Wilson fermions in $N_f=2$ QCD measured on the CLS ensembles. The use of the summed operator insertion method allows us to suppress the influence of excited states in our measurements. A study of the effect that excited state contaminations have on the $Q^2$ dependence of the extracted nucleon form factors may then be made through comparisons of the summation method to standard plateau fits, as well as to excited state fits.

  19. Coherent excitation of a single atom to a Rydberg state

    Miroshnychenko, Yevhen; Gaëtan, Alpha; Evellin, Charles;

    2010-01-01

    We present the coherent excitation of a single Rubidium atom to the Rydberg state 58d3/2 using a two-photon transition. The experimental setup is described in detail, as are experimental techniques and procedures. The coherence of the excitation is revealed by observing Rabi oscillations between...

  20. Anisotropy of electronic states excited in ion-atom collisions

    The author reports coincidence measurements made on the He+ + Ne and He+ + He systems. The complex population amplitudes for the magnetic sublevels of the investigated excited states, Ne(2p43s2)1D and He(2p2)1D, were completely determined and possible excitation mechanisms are described. (Auth.)

  1. Superposition of Fragment Excitations for Excited States of Large Clusters with Application to Helium Clusters.

    Closser, Kristina D; Ge, Qinghui; Mao, Yuezhi; Shao, Yihan; Head-Gordon, Martin

    2015-12-01

    We develop a local excited-state method, based on the configuration interaction singles (CIS) wave function, for large atomic and molecular clusters. This method exploits the properties of absolutely localized molecular orbitals (ALMOs), which strictly limits the total number of excitations, and results in formal scaling with the third power of the system size for computing the full spectrum of ALMO-CIS excited states. The derivation of the equations and design of the algorithm are discussed in detail, with particular emphasis on the computational scaling. Clusters containing ∼500 atoms were used in evaluating the scaling, which agrees with the theoretical predictions, and the accuracy of the method is evaluated with respect to standard CIS. A pioneering application to the size dependence of the helium cluster spectrum is also presented for clusters of 25-231 atoms, the largest of which results in the computation of 2310 excited states per sampled cluster geometry. PMID:26609558

  2. Vibronic coupling in the excited-states of carotenoids.

    Miki, Takeshi; Buckup, Tiago; Krause, Marie S; Southall, June; Cogdell, Richard J; Motzkus, Marcus

    2016-04-20

    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 S2 to the optically dark state S1. Extending this picture, some additional dark states (3A and 1B) and their interaction with the S2 state have also been suggested to play a major role in the ultrafast deactivation of carotenoids and their properties. Here, we investigate the interaction between such dark and bright electronic excited states of open chain carotenoids, particularly its dependence on the number of conjugated double bonds (N). We focus on the ultrafast wave packet motion on the excited potential surface, which is modified by the interaction between bright and dark electronic states. Such a coupling between electronic states leads to a shift of the vibrational frequency during the excited-state evolution. In this regard, pump-degenerate four-wave mixing (pump-DFWM) is applied to a series of carotenoids with different numbers of conjugated double bonds N = 9, 10, 11 and 13 (neurosporene, spheroidene, lycopene and spirilloxanthin, respectively). Moreover, we demonstrate in a closed-chain carotenoid (lutein) that the coupling strength and therefore the vibrational shift can be tailored by changing the energy degeneracy between the 1B and 1B states via solvent interaction. PMID:27055720

  3. Quantification of Entanglement Entropies for Doubly Excited States in Helium

    In this work, we study the quantum entanglement for doubly excited resonance states in helium by using highly correlated Hylleraas type functions to represent such states of the two-electron system. The doubly-excited resonance states are determined by calculation of density of resonance states under the framework of the stabilization method. The spatial (electron–electron orbital) entanglement measures for the low-lying doubly excited 2s2, 2s3s, and 2p21 Se states are carried out. Once a resonance state wave function is obtained, the linear entropy and von Neumann entropy for such a state are quantified using the Schmidt-Slater decomposition method. To check the consistence, linear entropy is also determined by solving analytically the needed four-electron (12-dimensional) integrals. (author)

  4. Ultrafast Excited-State Dynamics in Biological Environments

    Fürstenberg, Alexandre; Vauthey, Eric

    2007-01-01

    We discuss and illustrate by several examples how the ultrafast excited-state dynamics of a chromophore can be altered when changing its environment from a homogenous solution to a biological molecule such as proteins or nucleic acids.

  5. Optimal control of peridinin excited-state dynamics

    Chábera, P.; Dietzek, B.; Yartsev, A.; Polívka, Tomáš

    Nové Hrady: Academic and University Center, 2008. s. 15. [ESF Workshop on Novel Methods in Exploring Carotenoid Excited State Dynamics. 21.09.2008-25.09.2008, Nové Hrady] Keywords : peridinin * biophysics Subject RIV: BO - Biophysics

  6. Boson analysis of the excited O+ state in Ge isotopes

    Motivated by attemp to explain the strong variation in energy of the excited O+ state in even Ge isotopes in terms of a simple collective configuration, a boson mapping is introduced for proton, neutron and proton-neutron pairing

  7. The examination of berberine excited state by laser flash photolysis

    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.

  8. Controlling Chimera States - The influence of excitable units

    Isele, Thomas; Hizanidis, Johanne; Provata, Astero; Hövel, Philipp

    2015-01-01

    We explore the influence of a block of excitable units on the existence and behavior of chimera states in a nonlocally coupled ring-network of FitzHugh-Nagumo elements. The FitzHugh-Nagumo system, a paradigmatic model in many fields from neuroscience to chemical pattern formation and nonlinear electronics, exhibits oscillatory or excitable behavior depending on the values of its parameters. Until now, chimera states have been studied in networks of coupled oscillatory FitzHugh-Nagumo elements...

  9. Investigation into chromophore excited-state coupling in allophycocyanin

    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.

  10. Photoacoustic imaging of the excited state lifetime of fluorophores

    Märk, Julia; Schmitt, Franz-Josef; Laufer, Jan

    2016-05-01

    Photoacoustic (PA) imaging using pump-probe excitation has been shown to allow the detection and visualization of fluorescent contrast agents. The technique relies upon inducing stimulated emission using pump and probe pulses at excitation wavelengths that correspond to the absorption and fluorescence spectra. By changing the time delay between the pulses, the excited state lifetime of the fluorophore is modulated to vary the amount of thermalized energy, and hence PA signal amplitude, to provide fluorophore-specific PA contrast. In this study, this approach was extended to the detection of differences in the excited state lifetime of fluorophores. PA waveforms were measured in solutions of a near-infrared fluorophore using simultaneous and time-delayed pump-probe excitation. The lifetime of the fluorophore solutions was varied by using different solvents and quencher concentrations. By calculating difference signals and by plotting their amplitude as a function of pump-probe time delay, a correlation with the excited state lifetime of the fluorophore was observed. The results agreed with the output of a forward model of the PA signal generation in fluorophores. The application of this method to tomographic PA imaging of differences in the excited state lifetime was demonstrated in tissue phantom experiments.

  11. Influence of Tm3+ optical centers on spectroscopic properties at the 3F4–3H6 2-μm laser transition

    Individual low temperature (77 K) fluorescence spectra of tetragonal (C4v), clustered, and long-lifetime optical centers of Tm3+ ions at the 3F4–3H6 transition are recorded and the lifetimes of these centers are measured. Analysis of the number and positions of the fluorescence lines of the long-lifetime optical center allows to suggest that it has tetragonal (C4v) local symmetry. - Highlights: • Tm3+ optical centers fluorescence spectra at 77K for 3F4-3H6 transition are obtained. • Tm3+ optical centers lifetimes at 77K for 3F4-3H6 transition are measured. • Tm3+ long-lifetime optical center is suggested to have tetragonal local symmetry

  12. Metastable states of highly excited heavy ions

    Pegg, D. J.; Griffin, P. M.; Sellin, I. A.; Smith, W. W.; Donnally, B.

    1973-01-01

    Description of the method used and results obtained in an experimental study of the metastable states of highly stripped heavy ions, aimed at determining the lifetimes of such states by the rates of autoionization and radiation. The significance and limitations of the results presented are discussed.

  13. Excited-state Halo of 14C

    2002-01-01

    Neutron capture processes on carbon isotope play an important role in astrophysics ranging fromnucleosynthesis in the stellar helium and carbon burning stages to possibly inhomogeneous big bangmodels. The capture rate in astrophysical environments strongly depends on the structure of these carbonnuclei. For example, the first 1/2+ state in 13C is a neutron halo state, and these results in an enormous

  14. Microwave spectroscopy of furfural in vibrationally excited states

    Motiyenko, R. A.; Alekseev, E. A.; Dyubko, S. F.

    2007-07-01

    The results of microwave spectrum investigation of the excited vibrational states of furfural in the frequency range between 49 and 149 GHz are reported. In total 15 excited vibrational states (9 for trans-furfural and 6 for cis-furfural) were assigned and analyzed. Six of the 15 investigated states were assigned for the first time. Accurate values of rigid rotor and quartic centrifugal distortion constants of asymmetric top Hamiltonian have been determined for 13 excited states. Also for some states several sextic and octic level constants were needed in order to fit the data within experimental accuracy. The vt = 3 and vs = 1, va = 1 states of trans-furfural were found to be strongly perturbed and only rotational transitions with low Ka values can be reliably identified in this study.

  15. Neutral Excitations in the Gaffnian state

    Kang, Byungmin; Moore, Joel E.

    The Fractional Quantum Hall Effect (FQHE) is one of the most well-studied systems having topological order. Starting with the pioneering work by Laughlin, the model wave function approach has been shown to provide essential information for understanding topological order in gapped incompressible states. We study a model wave function called the Gaffnian state which is believed to represent a gapless, strongly correlated state that is very different from conventional metals. To understand this exotic gapless state better, we provide a representation in which the pairing structure of the Gaffnian state becomes more explicit. We employ the single-mode approximation of the Girvin-MacDonald-Platzman (GMP) mode, which is a neutral collective exitation mode, in order to have a physical picture of the gaplessness of the Gaffnian state. In particular, we discuss how to extract systematically the relevant physics in the long-distance, large electron number limit of the FQH states using a numerical calculation with relatively few electrons.

  16. The excited state antiaromatic benzene ring: a molecular Mr Hyde?

    Papadakis, Raffaello; Ottosson, Henrik

    2015-09-21

    The antiaromatic character of benzene in its first ππ* excited triplet state (T1) was deduced more than four decades ago by Baird using perturbation molecular orbital (PMO) theory [J. Am. Chem. Soc. 1972, 94, 4941], and since then it has been confirmed through a range of high-level quantum chemical calculations. With focus on benzene we now first review theoretical and computational studies that examine and confirm Baird's rule on reversal in the electron count for aromaticity and antiaromaticity of annulenes in their lowest triplet states as compared to Hückel's rule for the ground state (S0). We also note that the rule according to quantum chemical calculations can be extended to the lowest singlet excited state (S1) of benzene. Importantly, Baird, as well as Aihara [Bull. Chem. Soc. Jpn. 1978, 51, 1788], early put forth that the destabilization and excited state antiaromaticity of the benzene ring should be reflected in its photochemical reactivity, yet, today these conclusions are often overlooked. Thus, in the second part of the article we review photochemical reactions of a series of benzene derivatives that to various extents should stem from the excited state antiaromatic character of the benzene ring. We argue that benzene can be viewed as a molecular "Dr Jekyll and Mr Hyde" with its largely unknown excited state antiaromaticity representing its "Mr Hyde" character. The recognition of the "Jekyll and Hyde" split personality feature of the benzene ring can likely be useful in a range of different areas. PMID:25960203

  17. Controlling chimera states: The influence of excitable units

    Isele, Thomas; Hizanidis, Johanne; Provata, Astero; Hövel, Philipp

    2016-02-01

    We explore the influence of a block of excitable units on the existence and behavior of chimera states in a nonlocally coupled ring-network of FitzHugh-Nagumo elements. The FitzHugh-Nagumo system, a paradigmatic model in many fields from neuroscience to chemical pattern formation and nonlinear electronics, exhibits oscillatory or excitable behavior depending on the values of its parameters. Until now, chimera states have been studied in networks of coupled oscillatory FitzHugh-Nagumo elements. In the present work, we find that introducing a block of excitable units into the network may lead to several interesting effects. It allows for controlling the position of a chimera state as well as for generating a chimera state directly from the synchronous state.

  18. Shape vibration and quasiparticle excitations in the lowest 0+ excited state in erbium isotopes

    Chen, Fang-Qi; Egido, J. Luis

    2016-06-01

    The ground and first excited 0+ states of the -172Er156 isotopes are analyzed in the framework of the generator coordinate method. The shape parameter β is used to generate wave functions with different deformations which together with the two-quasiparticle states built on them provide a set of states. An angular momentum and particle number projection of the latter spawn the basis states of the generator coordinate method. With this ansatz and using the separable pairing plus quadrupole interaction we obtain a good agreement with the experimental spectra and E 2 transition rates up to moderate spin values. The structure of the wave functions suggests that the first excited 0+ states in the soft Er isotopes are dominated by shape fluctuations, while in the well deformed Er isotopes the two-quasiparticle states are more relevant. In between, both degrees of freedom are necessary.

  19. Shape vibrations and quasiparticle excitations in the lowest 0+ excited state of the Erbium isotopes

    Chen, Fang-Qi

    2016-01-01

    The ground and first excited 0+ states of the {156-172}Er isotopes are analyzed in the framework of the generator coordinate method. The shape parameter beta is used to generate wave functions with different deformations which together with the two-quasiparticle states built on them provide a set of states. An angular momentum and particle number projection of the latter spawn the basis states of the generator coordinate method. With this ansatz and using the separable pairing plus quadrupole interaction we obtain a good agreement with the experimental spectra and E2 transition rates up to moderate spin values. The structure of the wave functions suggests that the first excited 0+ states in the soft Er isotopes are dominated by shape fluctuations, while in the well deformed Er isotopes the two-quasiparticle states are more relevant. In between both degrees of freedom are necessary .

  20. Cluster structure in highly-excited states of light nuclei

    The cluster structure in the highly-excited states of light nuclei are investigated using the multi-cluster model. For this purpose, we propose a developed treatment method of the multi-cluster model. The method consists of two parts: One is a systematic construction method of the multi-cluster Pauli-allowed states. Another is a truncation method of the large model space of the multi-cluster system. We show that we can easily solve the equation of the orthogonality condition model (OCM) for complex multi-cluster systems by the use of the method. We apply the multi-cluster models 3α, 4α, 12C + 2α and 16O + 2α to 12C, 16O, 20Ne and 24Mg, respectively. As shown in the Ikeda diagram, these models open a very interesting problem not only of the cluster structure in the highly-excited states of those nuclei but also of the structure change between different cluster structures. We show a typical example of the 16O + 2α model for 24Mg ; 1) many excited states with the 20Ne-α cluster structure are obtained at excitation energies above 10 MeV, 2) the 16O-8Be cluster states are obtained at the energy region higher than 20 MeV, and 3) the very interesting states with the α-16O-α linear-chain-like structure are predicted at about 20 MeV excitation energy. (author)

  1. Doubly excited 3P(e) resonant states in Ps(-)

    Ho, Y. K.; Bhatia, A. K.

    1992-01-01

    Doubly excited 3P(e) resonant states in Ps(-) are calculated using a method of complex-coordinate rotation. Resonance parameters (both resonance positions and widths) for doubly excited states associated with the n = 2, 3, 4, 5, and 6 thresholds of positronium atoms are evaluated using elaborate Hylleraas-type functions. In addition to ten Feshbach-type resonances lying below various Ps thresholds, three shape resonances were identified, one each lying above the n = 2, 4, and 6 Ps thresholds. It is further noted that the energy levels for the present 3P(e) states are nearly degenerate with respect to the previously calculated 1P(0) states. Such a symmetric character suggests that the highly and doubly excited Ps(-), similar to its counterpart in H(-), would exhibit rovibrational behaviors analogous to those of XYX triatomic molecules.

  2. Neutron halos in the excited states for N=127 isotones

    SUN Qin; GUO Jian-You

    2009-01-01

    Properties of the ground states and the excited states of N=127 isotones are investigated by using the nonlinear relativistic mean field theory with the interactions PK1. By analyzing the rms of proton and neutron, the single particle energies of valence nucleon and the density distributions of neutron, proton and the last neutron, it can be found that there exists a neutron halo in the excited states of 3d5/2, 4s1/2 and 3d3/2 in 209Pb. It is also predicted that there exists a neutron halo in the excited states of 3d5/2, 4s1/2 and 3d3/2 in 207Hg, 208Tl, 210Bi and 211Po.

  3. Charge transfer excitations from excited state Hartree-Fock subsequent minimization scheme

    Theophilou, Iris, E-mail: i.theophilou@fz-juelich.de [Peter Grunberg Institut (PGI) Forschungszentrum Jülich, D-52425 Jülich (Germany); Tassi, M.; Thanos, S. [Institute for Advanced Materials, Physicochemical Processes, Nanotechnology and Microsystems, ‘Demokritos’ National Center for Scientific Research, 15310 Athens (Greece)

    2014-04-28

    Photoinduced charge-transfer processes play a key role for novel photovoltaic phenomena and devices. Thus, the development of ab initio methods that allow for an accurate and computationally inexpensive treatment of charge-transfer excitations is a topic that nowadays attracts a lot of scientific attention. In this paper we extend an approach recently introduced for the description of single and double excitations [M. Tassi, I. Theophilou, and S. Thanos, Int. J. Quantum Chem. 113, 690 (2013); M. Tassi, I. Theophilou, and S. Thanos, J. Chem. Phys. 138, 124107 (2013)] to allow for the description of intermolecular charge-transfer excitations. We describe an excitation where an electron is transferred from a donor system to an acceptor one, keeping the excited state orthogonal to the ground state and avoiding variational collapse. These conditions are achieved by decomposing the space spanned by the Hartree-Fock (HF) ground state orbitals into four subspaces: The subspace spanned by the occupied orbitals that are localized in the region of the donor molecule, the corresponding for the acceptor ones and two more subspaces containing the virtual orbitals that are localized in the neighborhood of the donor and the acceptor, respectively. Next, we create a Slater determinant with a hole in the subspace of occupied orbitals of the donor and a particle in the virtual subspace of the acceptor. Subsequently we optimize both the hole and the particle by minimizing the HF energy functional in the corresponding subspaces. Finally, we test our approach by calculating the lowest charge-transfer excitation energies for a set of tetracyanoethylene-hydrocarbon complexes that have been used earlier as a test set for such kind of excitations.

  4. Excited states and transition metal compounds with quantum Monte Carlo

    Bande, Annika

    2007-01-01

    To the most challenging electron structure calculations belong weak interactions, excited state calculations, transition metals and properties. In this work the performance of variational (VMC) and fixed-node diffusion quantum Monte Carlo (FN-DMC) is tested for challenging electron structure problems using the quantum Monte Carlo amolqc code by Lüchow et al. The transition metal compounds under consideration are vanadium oxides. Here excitation, ionization, oxygen atom and molecule abstractio...

  5. Excited State Spectra and Dynamics of Phenyl-Substituted Butadienes

    Wallace-Williams, Stacie E.; Schwartz, Benjamin J.; Møller, Søren;

    1994-01-01

    A combination of steady-state and dynamic spectral measurements are used to provide new insights into the nature of the excited-state processes of all-trans-1,4-diphenyl-1,3-butadiene and several analogs: 1,4-diphenyl- 1,3-cyclopentadiene, 1,1,4,4-tetraphenylbutadiene, 1,2,3,4-tetraphenyl-1...

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

    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

  7. Excited-state dynamics of astaxanthin aggregates

    Fuciman, Marcel; Durchan, Milan; Šlouf, Václav; Keşan, Gürkan; Polívka, Tomáš

    2013-05-01

    Astaxanthin forms three types of aggregates in hydrated dimethyl sulfoxide (DMSO). In DMSO/water ratio of 1:1, a red-shifted J-aggregate with maximum at 570 nm is generated, while a ratio of 1:9 produces blue-shifted H-aggregates with peaks at 386 nm (H1) and 460 nm (H2). Monomeric astaxanthin in DMSO has an S1 lifetime of 5.3 ps, but a long-lived (33 ps) S∗ signal was also identified. Aggregation changes the S1 lifetimes to 17 ps (H1), 30 ps (H2), and 14 ps (J). Triplet state of astaxanthin, most likely generated via singlet homofission, was observed in H1 and H2 aggregates.

  8. Quantum entanglement of localized excited states at finite temperature

    Caputa, Pawel; Simón, Joan; Štikonas, Andrius; Takayanagi, Tadashi

    2015-01-01

    In this work we study the time evolutions of (Renyi) entanglement entropy of locally excited states in two dimensional conformal field theories (CFTs) at finite temperature. We consider excited states created by acting with local operators on thermal states and give both field theoretic and holographic calculations. In free field CFTs, we find that the growth of Renyi entanglement entropy at finite temperature is reduced compared to the zero temperature result by a small quantity proportional to the width of the localized excitations. On the other hand, in finite temperature CFTs with classical gravity duals, we find that the entanglement entropy approaches a characteristic value at late time. This behaviour does not occur at zero temperature. We also study the mutual information between the two CFTs in the thermofield double (TFD) formulation and give physical interpretations of our results.

  9. Quantum Entanglement of Localized Excited States at Finite Temperature

    Caputa, Pawel; Stikonas, Andrius; Takayanagi, Tadashi

    2014-01-01

    In this work we study the time evolutions of (Renyi) entanglement entropy of locally excited states in two dimensional conformal field theories (CFTs) at finite temperature. We consider excited states created by acting with local operators on thermal states and give both field theoretic and holographic calculations. In free field CFTs, we find that the growth of Renyi entanglement entropy at finite temperature is reduced compared to the zero temperature result by a small quantity proportional to the width of the localized excitations. On the other hand, in finite temperature CFTs with classical gravity duals, we find that the entanglement entropy approaches a characteristic value at late time. This behaviour does not occur at zero temperature. We also study the mutual information between the two CFTs in the thermofield double (TFD) formulation and give physical interpretations of our results.

  10. State-Selective Excitation of Quantum Systems via Geometrical Optimization.

    Chang, Bo Y; Shin, Seokmin; Sola, Ignacio R

    2015-09-01

    We lay out the foundations of a general method of quantum control via geometrical optimization. We apply the method to state-selective population transfer using ultrashort transform-limited pulses between manifolds of levels that may represent, e.g., state-selective transitions in molecules. Assuming that certain states can be prepared, we develop three implementations: (i) preoptimization, which implies engineering the initial state within the ground manifold or electronic state before the pulse is applied; (ii) postoptimization, which implies engineering the final state within the excited manifold or target electronic state, after the pulse; and (iii) double-time optimization, which uses both types of time-ordered manipulations. We apply the schemes to two important dynamical problems: To prepare arbitrary vibrational superposition states on the target electronic state and to select weakly coupled vibrational states. Whereas full population inversion between the electronic states only requires control at initial time in all of the ground vibrational levels, only very specific superposition states can be prepared with high fidelity by either pre- or postoptimization mechanisms. Full state-selective population inversion requires manipulating the vibrational coherences in the ground electronic state before the optical pulse is applied and in the excited electronic state afterward, but not during all times. PMID:26575896

  11. Accurate Excited State Geometries within Reduced Subspace TDDFT/TDA.

    Robinson, David

    2014-12-01

    A method for the calculation of TDDFT/TDA excited state geometries within a reduced subspace of Kohn-Sham orbitals has been implemented and tested. Accurate geometries are found for all of the fluorophore-like molecules tested, with at most all valence occupied orbitals and half of the virtual orbitals included but for some molecules even fewer orbitals. Efficiency gains of between 15 and 30% are found for essentially the same level of accuracy as a standard TDDFT/TDA excited state geometry optimization calculation. PMID:26583218

  12. Coupled cluster calculations of ground and excited states of nuclei

    The standard and renormalized coupled cluster methods with singles, doubles, and noniterative triples and their generalizations to excited states, based on the equation of motion coupled cluster approach, are applied to the He4 and O16 nuclei. A comparison of coupled cluster results with the results of the exact diagonalization of the Hamiltonian in the same model space shows that the quantum chemistry inspired coupled cluster approximations provide an excellent description of ground and excited states of nuclei. The bulk of the correlation effects is obtained at the coupled cluster singles and doubles level. Triples, treated noniteratively, provide the virtually exact description

  13. First-principles Calculation of Excited State Spectra in QCD

    Jozef Dudek,Robert Edwards,Michael Peardon,David Richards,Christopher Thomas

    2011-05-01

    Recent progress at understanding the excited state spectra of mesons and baryons is described. I begin by outlining the application of the variational method to compute the spectrum of QCD, and then present results for the excited meson spectrum, with continuum quantum numbers of the states clearly delineated. I emphasise the need to extend the calculation to encompass multi-hadron contributions, and describe a recent calculation of the I=2 pion-pion energy-dependent phase shifts as a precursor to the study of channels with resonant behavior. I conclude with recent results for the low lying baryon spectrum, and the prospects for future calculations.

  14. Kinetic studies following state-selective laser excitation

    The objective of this contract is the study of state-to-state, electronic energy transfer reactions following two-photon laser excitation. We have chosen to study reactions of Xe 5p5np because of their relevance to the XeCl excimer laser. We are studying deactivation reactions in collisions with heavy atoms such as Ar, Kr, and Xe and reactive collisions with chlorides. The reactants are excited by multiphoton laser absorption. Product channels are observed by their fluorescence, or by laser induced fluorescence using a second color laser. 36 refs., 16 figs., 5 tabs

  15. Equations of state for self-excited MHD generator studies

    We have constructed a state-of-the-art equation of state (EOS) for argon covering the temperature density range attainable by currently proposed self-excited MHD generators. The EOS for conditions in the flow channel was obtained primarily by a non-ideal plasma code (ACTEX) that is based on a many body activity expansion. For conditions in the driver chamber the EOS was primarily obtained from a fluid code (HDFP) that calculates the fluid properties from perturbation theory based on the insulator interatomic pair potential but including electronic excitations. The results are in agreement with several sets of experimental data in the 0.6 - 91 GPa pressure range

  16. Equations of state for self-excited MHD generator studies

    Rogers, F.J.; Ross, M.; Haggin, G.L.; Wong, L.K.

    1980-02-26

    We have constructed a state-of-the-art equation of state (EOS) for argon covering the temperature density range attainable by currently proposed self-excited MHD generators. The EOS for conditions in the flow channel was obtained primarily by a non-ideal plasma code (ACTEX) that is based on a many body activity expansion. For conditions in the driver chamber the EOS was primarily obtained from a fluid code (HDFP) that calculates the fluid properties from perturbation theory based on the insulator interatomic pair potential but including electronic excitations. The results are in agreement with several sets of experimental data in the 0.6 - 91 GPa pressure range.

  17. Vibrational relaxation pathways in the electronic excited state of carotenoid

    The intra- and inter-molecular vibrational relaxation in the electronic excited state (1Bu+) of spheroidene derivative (the number of conjugated double bonds, n=8) has been investigated at room temperature by means of femtosecond time-resolved fluorescence spectroscopy based on an optical-Kerr-gate technique. Depending on the photo-excitation either to the 1Bu+(v=1) or 1Bu+(v=2) vibronic level, remarkable differences were observed in hot luminescence spectra related to the vibrational relaxation process of high- and low-frequency modes. Under the excitation to the 1Bu+(v=2) state hot luminescence from the 1Bu+(v=1) state was observed as a dominant feature of the time-resolved spectra while the dynamic Stokes shift originating from the low-frequency-modes dynamics was clearly observed under the excitation to the 1Bu+(v=1). These observations of the excitation energy dependence of time-resolved fluorescence spectra were discussed by analyzing the Franck-Condon factors of transitions from v=0,1, and 2 levels of high-frequency modes

  18. Attosecond dynamics of electron correlation in doubly excited atomic states

    We have solved the time-dependent Schroedinger equation describing the simultaneous interaction of the He 1s2s 1S state with two laser-generated pulses of trapezoidal or Gaussian shape, of duration 86 fs and of frequencies ω1=1.453 au and ω2=1.781 au. The system is excited to the energy region of two strongly correlated doubly excited states, chosen for this study according to specific criteria. It is demonstrated quantitatively that, provided one focuses on the dynamics occurring within the attosecond timescale, the corresponding orbital configurations, 2s2p and 2p3d 1P0, exist as nonstationary states, with occupation probabilities that are oscillating as the states decay exponentially into the 1sεp continuum, during and after the laser-atom interaction. It follows that it is feasible to probe by attosecond pulses the motion of configurations of electrons as they correlate via the total Hamiltonian. For the particular system studied here, the probe pulses could register the oscillating doubly excited configurations by de-exciting to the He 1s3d 1D state, which emits at 6680 A. (author). Letter-to-the-editor

  19. Excited State Structural Dynamics of Carotenoids and Charge Transfer Systems

    This dissertation describes the development and implementation of a visible/near infrared pump/mid-infrared probe apparatus. Chapter 1 describes the background and motivation of investigating optically induced structural dynamics, paying specific attention to solvation and the excitation selection rules of highly symmetric molecules such as carotenoids. Chapter 2 describes the development and construction of the experimental apparatus used throughout the remainder of this dissertation. Chapter 3 will discuss the investigation of DCM, a laser dye with a fluorescence signal resulting from a charge transfer state. By studying the dynamics of DCM and of its methyl deuterated isotopomer (an otherwise identical molecule), we are able to investigate the origins of the charge transfer state and provide evidence that it is of the controversial twisted intramolecular (TICT) type. Chapter 4 introduces the use of two-photon excitation to the S1 state, combined with one-photon excitation to the S2 state of the carotenoid beta-apo-8'-carotenal. These 2 investigations show evidence for the formation of solitons, previously unobserved in molecular systems and found only in conducting polymers Chapter 5 presents an investigation of the excited state dynamics of peridinin, the carotenoid responsible for the light harvesting of dinoflagellates. This investigation allows for a more detailed understanding of the importance of structural dynamics of carotenoids in light harvesting

  20. Wave packet dynamics in molecular excited electronic states

    We theoretically explore the use of UV pump – UV probe schemes to resolve in time the dynamics of nuclear wave packets in excited electronic states of the hydrogen molecule. The pump pulse ignites the dynamics in singly excited states, that will be probed after a given time delay by a second identical pulse that will ionize the molecule. The field-free molecular dynamics is first explored by analyizing the autocorrelation function for the pumped wave packet and the excitation probabilities. We investigate both energy and angle differential ionization probabilities and demonstrate that the asymmetry induced in the electron angular distributions gives a direct map of the time evolution of the pumped wave packet

  1. Excited charmonium states from Bethe-Salpeter equation

    Sauli, Vladimir

    2011-01-01

    We solve the Bethe-Salpeter equation for a system of a heavy quark-antiquark pair interacting with a screened linear confining potential. First we show the spinless QFT model is inadequate and fail to describe even gross feature of the quarkonia spectrum. In order to get reliable description the spine degrees of freedom has to be considered. Within the approximation employed we reasonably reproduce known radial excitation of vector charmonium. The BSE favors relatively large string breaking scale $\\mu\\simeq 350MeV$ . Using free charm quark propagators we observe that $J/\\Psi$ is the only charmonium left bellow naive quark-antiquark threshold $2m_c$, while the all excited states are situated above this threshold. Within the numerical method we overcome obstacles related with threshold singularity and discuss the consequences of the use of free propagators for calculation of excited states above the threshold.

  2. Size dependent deactivation of the excited state of DHICA

    Gauden, Magdalena; Pezzella, Alessandro; Panzella, Lucia;

    2008-01-01

    Melanin is a natural pigment mainly responsible for the protection of skin and eyes from UV damage. 5,6- dihydroxyindole- 2 carboxylic acid (DHICA) is a key melanin building block. We have investigated the excited state dynamics of DHICA as well as its derivatives and oligomeric units using...

  3. Optimal control of peridinin excited-state dynamics

    Dietzek, B.; Chábera, P.; Hanf, R.; Tschierlei, S.; Popp, J.; Pascher, T.; Yartsev, A.; Polívka, Tomáš

    2010-01-01

    Roč. 373, 1-2 (2010), s. 129-136. ISSN 0301-0104 Institutional research plan: CEZ:AV0Z50510513 Keywords : peridin * excited-state dynamics * coherent control Subject RIV: BO - Biophysics Impact factor: 2.017, year: 2010

  4. Dark excited states of carotenoids: Consensus and controversy

    Polívka, Tomáš; Sundström, V.

    2009-01-01

    Roč. 477, 1-3 (2009), s. 1-11. ISSN 0009-2614 Institutional research plan: CEZ:AV0Z50510513 Keywords : carotenoids * excited states * relaxation pathways * femtosecond spectroscopy Subject RIV: BO - Biophysics Impact factor: 2.291, year: 2009

  5. Calculation of neutral beam deposition accounting for excited states

    Gianakon, T.A.

    1992-09-01

    Large-scale neutral-beam auxillary heating of plasmas has led to new plasma operational regimes which are often dominated by fast ions injected via the absorption of an energetic beam of hydrogen neutrals. An accurate simulation of the slowing down and transport of these fast ions requires an intimate knowledge of the hydrogenic neutral deposition on each flux surface of the plasma. As a refinement to the present generation of transport codes, which base their beam deposition on ground-state reaction rates, a new set of routines, based on the excited states of hydrogen, is presented as mechanism for computing the attenuation and deposition of a beam of energetic neutrals. Additionally, the numerical formulations for the underlying atomic physics for hydrogen impacting on the constiuent plasma species is developed and compiled as a numerical database. Sample results based on this excited state model are compared with the ground-state model for simple plasma configurations.

  6. Calculation of neutral beam deposition accounting for excited states

    Large-scale neutral-beam auxillary heating of plasmas has led to new plasma operational regimes which are often dominated by fast ions injected via the absorption of an energetic beam of hydrogen neutrals. An accurate simulation of the slowing down and transport of these fast ions requires an intimate knowledge of the hydrogenic neutral deposition on each flux surface of the plasma. As a refinement to the present generation of transport codes, which base their beam deposition on ground-state reaction rates, a new set of routines, based on the excited states of hydrogen, is presented as mechanism for computing the attenuation and deposition of a beam of energetic neutrals. Additionally, the numerical formulations for the underlying atomic physics for hydrogen impacting on the constiuent plasma species is developed and compiled as a numerical database. Sample results based on this excited state model are compared with the ground-state model for simple plasma configurations

  7. Direct excitation of butterfly states in Rydberg molecules

    Lippe, Carsten; Niederpruem, Thomas; Thomas, Oliver; Eichert, Tanita; Ott, Herwig

    2016-05-01

    Since their first theoretical prediction Rydberg molecules have become an increasing field of research. These exotic states originate from the binding of a ground state atom in the electronic wave function of a highly-excited Rydberg atom mediated by a Fermi contact type interaction. A special class of long-range molecular states, the butterfly states, were first proposed by Greene et al.. These states arise from a shape resonance in the p-wave scattering channel of a ground state atom and a Rydberg electron and are characterized by an electron wavefunction whose density distribution resembles the shape of a butterfly. We report on the direct observation of deeply bound butterfly states of Rydberg molecules of 87 Rb. The butterfly states are studied by high resolution spectroscopy of UV-excited Rydberg molecules. We find states bound up to - 50 GHz from the 25 P1/2 , F = 1 state, corresponding to binding lengths of 50a0 to 500a0 and with permanent electric dipole moments of up to 500 Debye. This distinguishes the observed butterfly states from the previously observed long range Rydberg molecules in rubidium.

  8. Optimized resonating valence bond state in square lattice: correlations & excitations

    Z Nourbakhsh

    2009-09-01

    Full Text Available We consider RVB state as a variational estimate for the ground state of Heisenberg antiferromagnet in square lattice. We present numerical calculation of energy, spin-spin correlation function and spin excitation spectrum. We show, that the quantum flactuations reduce of magnetization respect to Neel order. Our results are in good agreement with other methods such as spin-wave calculation and series expansions.

  9. Excited States of the Diatomic Molecule CrHe

    Pototschnig, Johann V.; Ratschek, Martin; Hauser, Andreas W.; Ernst, Wolfgang E.

    2013-06-01

    Chromium (Cr) atoms embedded in superfluid helium nanodroplets (He_N) have been investigated by laser induced fluorescence, beam depletion and resonant two-photon ionization spectroscopy in current experiments at our institute. Cr is found to reside inside the He_N in the a^7S ground state. Two electronically excited states, z^7P and y^7P, are involved in a photoinduced ejection process which allowed us to study Fano resonances in the photoionisation spectra The need for a better understanding of the experimental observations triggered a theoretical approach towards the computation of electronically excited states via high-level methods of computational chemistry. Two well-established, wave function-based methods, CASSCF and MRCI, are combined to calculate the potential energy curves for the three states involved. The character of the two excited states z^7P and y^7P turns out to be significantly different. Theory predicts the ejection of the Cr atom in the case of an y^7P excitation as was observed experimentally. The quasi-inert helium environment is expected to weaken spin selection rules, allowing a coupling between different spin states especially during the ejection process. We therefore extend our theoretical analysis to the lowest state in the triplet- and quintet- manifold. Most of these alternative states show very weak bonding of only a few wn. A. Kautsch, M. Hasewend, M. Koch and W. E. Ernst, Phys. Rev. A 86, 033428 (2012). A. Kautsch, M. Koch and W. E. Ernst, J. Phys. Chem. A, accepted, doi:10.1021/jp312336m}.

  10. Coupling of single-particle states to collective excitations

    We discuss the effects of colletive vibrations of the closed shell core on the fragmentation of single-particle states in the neighbouring odd nuclei. A scheme for calculating microscopically these effects is presented. Starting from a Skyrme-type effective interaction, one can obtain the Hartree-Fock spectrum, the core excited states and giant resonances and then the energy-dependent mass operator which determines the fragmentation. Results for the 207Pb are discussed and compared with the data

  11. Photodissociation of N2O: excitation of 1A" states.

    Schinke, Reinhard; Schmidt, Johan A

    2012-11-26

    We investigate the contributions of the lowest two (1)A" states in the UV photodissociation of N(2)O employing three-dimensional potential energy surfaces and transition dipole moment functions. Because the transition dipole moments are much smaller than for the 2 (1)A' state, we conclude that excitation of the (1)A" states has a marginal effect. The dense vibrational spectrum of the quasi-bound 2(1)A" state possibly explains some of the tiny, noise-like structures of the measured absorption spectrum. PMID:22536943

  12. Temperature measurements from relative populations of excited states with INDRA

    For the first time, INDRA has been used to analyse resonances observed in correlation functions, giving thus the possibility to probe the caloric curve (correlation between the excitation energy and the temperature). First results obtained for the reaction 1836Ar+2858Ni at 95 MeV/nucleon are presented where the projectile-like apparent temperature has been evaluated. Moreover, the measured populations of excited states are compared with the predictions of a statistical model which includes an original hypothesis of excluded volume for species at the freeze-out. (author)

  13. Solid-State Excitation Laser for Laser-Ultrasonics

    Schnars, U.; Platz, W.; Mahnke, P.; A. Fix; Frede, M; Neumann, J.; Peuser, P.

    2010-01-01

    The inspection speed of laser-ultrasonics compared with conventional ultrasonic testing is limited by the pulse repetition rate of the excitation laser. The maximum pulse repetition rate reported up to now for CO2-lasers, which are presently used for nearly all systems, is in the range of 400 Hz. In this paper a new approach based on a diode-pumped solid-state laser is discussed, which is currently being developed. This new excitation laser is designed for a repetition rate of 1 kHz and will ...

  14. HYPERDIRE. HYPERgeometric functions DIfferential REduction. MATHEMATICA based packages for differential reduction of generalized hypergeometric functions pFp-1, F1, F2, F3, F4

    HYPERDIRE is a project devoted to the creation of a set of Mathematica based programs for the differential reduction of hypergeometric functions. The current version includes two parts: one, pfq, is relevant for manipulations of hypergeometric functions p+1Fp, and the second one, AppellF1F4, for manipulations with Appell hypergeometric functions F1, F2, F3, F4 of two variables.

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

    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

  16. MULTIPLY CHARGED IONS COLLISIONS WITH ATOMS INTO EXCITED STATES

    PanGuangyan

    1990-01-01

    The emission spectra in collisions between Ions and Atoms have been measured by an Optical Multichannel Analysis System (OMA).The experimental results demonstrate that there are two channels of excitation in collision between single charged ions and atoms and three channels of excitation in collision between double charged ions and atoms.Emission cross cestions and excitation cross sections have been obtained.K.Kadota et al and R.Shingal et al suggested that,under the appropriate conditions,the H42+-Li and He2++Na collision systems can be used efficiently to produce a laser of Lyman-α(30,4nm) and Lyman-β(25.6nm)lines via cascade to He+(2P)state.

  17. Super-atom molecular orbital excited states of fullerenes.

    Johansson, J Olof; Bohl, Elvira; Campbell, Eleanor E B

    2016-09-13

    Super-atom molecular orbitals are orbitals that form diffuse hydrogenic excited electronic states of fullerenes with their electron density centred at the centre of the hollow carbon cage and a significant electron density inside the cage. This is a consequence of the high symmetry and hollow structure of the molecules and distinguishes them from typical low-lying molecular Rydberg states. This review summarizes the current experimental and theoretical studies related to these exotic excited electronic states with emphasis on femtosecond photoelectron spectroscopy experiments on gas-phase fullerenes.This article is part of the themed issue 'Fullerenes: past, present and future, celebrating the 30th anniversary of Buckminster Fullerene'. PMID:27501970

  18. Clustered chimera states in systems of type-I excitability

    The chimera state is a fascinating phenomenon of coexisting synchronized and desynchronized behaviour that was discovered in networks of nonlocally coupled identical phase oscillators over ten years ago. Since then, chimeras have been found in numerous theoretical and experimental studies and more recently in models of neuronal dynamics as well. In this work, we consider a generic model for a saddle-node bifurcation on a limit cycle representative of neural excitability type I. We obtain chimera states with multiple coherent regions (clustered chimeras/multi-chimeras) depending on the distance from the excitability threshold, the range of nonlocal coupling and the coupling strength. A detailed stability diagram for these chimera states and other interesting coexisting patterns (like traveling waves) is presented. (paper)

  19. Controlling excited-state contamination in nucleon matrix elements

    Yoon, Boram; Gupta, Rajan; Bhattacharya, Tanmoy; Engelhardt, Michael; Green, Jeremy; Joó, Bálint; Lin, Huey-Wen; Negele, John; Orginos, Kostas; Pochinsky, Andrew; Richards, David; Syritsyn, Sergey; Winter, Frank; Nucleon Matrix Elements NME Collaboration

    2016-06-01

    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 323×64 generated using the rational hybrid Monte Carlo algorithm at a =0.081 fm and with Mπ=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 separation tsep. We show that both methods can be tuned to significantly reduce excited-state contamination and discuss their relative advantages and cost effectiveness. A detailed analysis of the size of source smearing used in the calculation of quark propagators and the range of values of tsep needed to demonstrate convergence of the isovector charges of the nucleon to the tsep→∞ estimates is presented.

  20. Excited state dynamics of the astaxanthin radical cation

    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.

  1. Controlling Excited-State Contamination in Nucleon Matrix Elements

    Yoon, Boram; Bhattacharya, Tanmoy; Engelhardt, Michael; Green, Jeremy; Joó, Bálint; Lin, Huey-Wen; Negele, John; Orginos, Kostas; Pochinsky, Andrew; Richards, David; Syritsyn, Sergey; Winter, Frank

    2016-01-01

    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 $32^3 \\times 64$ generated using the rational hybrid Monte Carlo algorithm at $a=0.081$~fm and with $M_\\pi=312$~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 two-state fit to data at multiple values of the source-sink separation $t_{\\rm sep}$. We show that both methods can be tuned to significantly reduce excited-state contamination and discuss their relative advantages and cost-effectiveness. A detailed analysis of the size of source smearing used in the calculation of quark propagators and the range of values of $t_{\\rm sep}$ needed to demonstrate convergence of the isovector charges of the nucleon to the $t_...

  2. Strong-Field Photoionization as Excited-State Tunneling.

    Serebryannikov, E E; Zheltikov, A M

    2016-03-25

    We show that, in an intense laser field, ultrafast photoionization can occur through quantum pathways that cannot be categorized as multiphoton ionization or ground-state tunneling. In this regime, the subcycle electron-wave-packet dynamics leading to photoionization occurs via electron excited states, from where the electrons tunnel to the continuum within a tiny fraction of the field cycle. For high field intensities, this ionization pathway is shown to drastically enhance the dynamic leakage of the electron wave packet into the continuum, opening an ionization channel that dominates over ground-state electron tunneling. PMID:27058079

  3. First observation of excited states in {sup 182}Pb.

    Jenkins, D. G.; Muikku, M.; Greenlees, P. T.; Hauschild, K.; Helarjutta, K.; Jones, P. M.; Julin, R.; Juutinen, S.; Kankaanpaa, H.; Kelsall, N. S.; Kettunen, H.; Kuusiniemi, P.; Leino, M.; Moore, C. J.; Nieminen, P.; O' Leary, C. D.; Page, R. D.; Rakhila, P.; Reviol, W.; Taylor, M. J.; Uusitalo, J.; Wadsworth, R.; Physics; Univ. of York; Univ. of Jyvaskyla; CEA Saclay; Univ. of Liverpool; Univ. of Tennessee

    2000-01-01

    Excited states in the light lead nucleus, {sup 182}Pb, have been observed for the first time, by means of the recoil-decay tagging technique. A rotational band has been observed which has features in common with bands attributed to a prolate configuration in the heavier neutron deficient lead nuclei, {sup 184-188}Pb. A variable moment of inertia fit to the states in this band suggests that the prolate minimum has risen significantly in energy compared to the next even lead nucleus, {sup 184}Pb. This constitutes firm evidence for the minimization of this configuration with respect to the spherical ground state around N=103.

  4. Ultrafast excited state dynamics in 9,9'-bifluorenylidene.

    Conyard, Jamie; Heisler, Ismael A; Browne, Wesley R; Feringa, Ben L; Amirjalayer, Saeed; Buma, Wybren Jan; Woutersen, Sander; Meech, Stephen R

    2014-08-01

    9,9'-Bifluorenylidene has been proposed as an alternative and flexible electron acceptor in organic photovoltaic cells. Here we characterize its excited state properties and photokinetics, combining ultrafast fluorescence and transient IR measurements with quantum chemical calculations. The fluorescence decay is ultrafast (sub-100 fs) and remarkably independent of viscosity. This suggests that large scale structure change is not the primary relaxation mode. The ultrafast decay populates a dark state characterized by distinct vibrational and electronic spectra. This state decays with a 6 ps time constant to a hot ground state that ultimately populates the initial state with a 20 ps time constant; these times are also insensitive to solvent viscosity. No metastable intermediate structures are resolved in the photocycle after population of the dark state. The implications of these results for the operation of 9,9'-bifluorenylidene as an electron acceptor and as a potential molecular switch are discussed. PMID:25025227

  5. Negative-parity nucleon excited state in nuclear matter

    Ohtani, Keisuke; Oka, Makoto

    2016-01-01

    Spectral functions of the nucleon and its negative parity excited state in nuclear matter are studied using QCD sum rules and the maximum entropy method (MEM). It is found that in-medium modifications of the spectral functions are attributed mainly to density dependencies of the $\\langle \\bar{q}q \\rangle $ and $\\langle q^{\\dagger}q \\rangle $ condensates. The MEM reproduces the lowest-energy peaks of both the positive and negative parity nucleon states at finite density up to $\\rho \\sim \\rho_N$ (normal nuclear matter density). As the density grows, the residue of the nucleon ground state decreases gradually while the residue of the lowest negative parity excited state increases slightly. On the other hand, the positions of the peaks, which correspond to the total energies of these states, are almost density independent for both parity states. The density dependencies of the effective masses and vector self-energies are also extracted by assuming the mean-field green functions for the peak states. We find that,...

  6. Physical Properties, Exciton Analysis, and Visualization of Core-Excited States: An Intermediate State Representation Approach.

    Wenzel, Jan; Dreuw, Andreas

    2016-03-01

    The theoretical simulation of X-ray absorption spectra is in general a challenging task. However, for small and medium-sized organic molecules, the algebraic diagrammatic construction scheme (ADC) for the polarization operator in combination with the core-valence separation approximation (CVS) has proven to yield core-excitation energies and transition moments with almost quantitative accuracy allowing for reliable construction of X-ray absorption spectra. Still, to understand core-excitation processes in detail, it is not sufficient to only compute energies, but also properties like static dipole moments and state densities are important as they provide deeper insight into the nature of core-excited states. Here, we present for the first time an implementation of the intermediate state representation (ISR) approach in combination with the CVS approximation (CVS-ISR), which gives, in combination with the CVS-ADC method, direct access to core-excited state properties. The performance of the CVS-ADC/CVS-ISR approach is demonstrated by means of small- and medium-sized organic molecules. Besides the calculation of core-excited state dipole moments, advanced analyses of core-excited state densities are performed using descriptors like exciton sizes and distances. Plotting electron and hole densities helps to determine the character of the state, and in particular, the investigation of detachment/attachment densities provides information about orbital relaxation effects that are crucial for understanding core excitations. PMID:26845396

  7. Excited states in large molecular systems through polarizable embedding.

    List, Nanna Holmgaard; Olsen, Jógvan Magnus Haugaard; Kongsted, Jacob

    2016-07-27

    In this perspective, we provide an overview of recent work within the polarizable embedding scheme to describe properties of molecules in realistic environments of increasing complexity. After an outline of the theoretical basis for the polarizable embedding model, we discuss the importance of using an accurate embedding potential, and how this may be used to significantly reduce the size of the part of the system treated using quantum mechanics without compromising the accuracy of the final results. Furthermore, we discuss the calculation of local electronic excited states based on response theory. We finally discuss aspects related to two recent extensions of the model (i) effective external field and (ii) polarizable density embedding emphasizing their importance for efficient yet accurate description of excited-state properties in complex environments. PMID:27416749

  8. On the nature of highly vibrationally excited states of thiophosgene

    Srihari Keshavamurthy

    2012-01-01

    In this work an analysis of the highly vibrationally excited states of thiophosgene (SCCl2) is made in order to gain insights into some of the experimental observations and spectral features. The states analysed here lie in a spectrally complex region where strong mode mixings are expected due to the overlap of several strong anharmonic Fermi resonances. Two recent techniques, a semiclassical angle space representation of the eigenstates and the parametric variation of the eigenvalues (level-velocities) are used to identify eigenstate sequences exhibiting common localization characteristics. Preliminary results on the influence of highly excited out-of-plane bending modes on the nature of the eigenstates suggest a possible bifurcation in the system.

  9. The effects of doubly excited states on ionization balance

    2006-01-01

    The effects of highly doubly excited states on ionization balance are investigated. In the calculation, A Collisional-Radiative model in Detailed-Configuration-Accounting (DCA) is applied to population calculations for NLTE plasmas. Configuration-averaged rate coefficients that needed in the rate equations are obtained based on the first order perturbation theory. The Hatree-Fock-Slater self-consistent-field method is used to calculate the electron wave functions. The mean ionization stage of high-Z plasma Lu is presented. The comparison shows that the mean ionization stage increases more than 3 stages when doubly excited states 5l6l' and 5l5l' are not included in the population calculations.

  10. Time evolution of vibration-induced excited state decay

    Menšík, Miroslav; Nešpůrek, Stanislav

    2002-01-01

    Roč. 52, č. 8 (2002), s. 945-962. ISSN 0011-4626 R&D Projects: GA AV ČR IAB1050903; GA AV ČR IAA1050901 Institutional research plan: CEZ:AV0Z4050913 Keywords : excited state decay * exciton-phonon interaction Subject RIV: BG - Nuclear, Atomic and Molecular Physics, Colliders Impact factor: 0.311, year: 2002

  11. Algorithm for Computing Excited States in Quantum Theory

    Luo, X. Q.; Jirari, H.; Kroger, H; Moriarty, K.

    2001-01-01

    Monte Carlo techniques have been widely employed in statistical physics as well as in quantum theory in the Lagrangian formulation. However, in the conventional approach, it is extremely difficult to compute the excited states. Here we present a different algorithm: the Monte Carlo Hamiltonian method, designed to overcome the difficulties of the conventional approach. As a new example, application to the Klein-Gordon field theory is shown.

  12. Clustered Chimera States in Systems of Type-I Excitability

    Vüllings, Andrea; Hizanidis, Johanne; Omelchenko, Iryna; Hövel, Philipp

    2014-01-01

    Chimera is a fascinating phenomenon of coexisting synchronized and desynchronized behaviour that was discovered in networks of nonlocally coupled identical phase oscillators over ten years ago. Since then, chimeras were found in numerous theoretical and experimental studies and more recently in models of neuronal dynamics as well. In this work, we consider a generic model for a saddle-node bifurcation on a limit cycle representative for neural excitability type I. We obtain chimera states wit...

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

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

    2013-10-01

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

  14. Doubly excited triplet states of highly stripped ions

    Transition energies, Coulomb repulsions and effective quantum numbers have been calculated for the doubly excited Nsnp: 3P0 (for N=2, n=N,..,5); Nsnd: 3De (for N=2, n=N+1,..,5) and Npnd: 3F0 (for N=2, n=N+1,..,5) states for the highly stripped ions Na9+,Mg10+,Al11+,Si12+,P13+ and S14+. Time-dependent perturbation theory has been applied to calculate such transitions properties. A time-dependent harmonic perturbation causes simultaneous excitation of both the electrons with a change of spin state. The doubly excited energy levels and the analytic representation of their wave functions are obtained by identifying the poles of an appropriately constructed linearized variational functional with respect to driving frequency. Most of the results are new. The transition energies and effective quantum numbers of 2s2p: 3P0 states of all the ions agree well with the only available experimental data. (orig.)

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

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

    2013-11-14

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

  16. Entanglement Temperature and Entanglement Entropy of Excited States

    Wong, Gabriel; Zayas, Leopoldo A Pando; Vaman, Diana

    2013-01-01

    We derive a general relation between the ground state entanglement Hamiltonian and the physical stress tensor within the path integral formalism. For spherical entangling surfaces in a CFT, we reproduce the \\emph{local} ground state entanglement Hamiltonian derived by Casini, Huerta and Myers. The resulting reduced density matrix can be interpreted as a state of local thermal equilibrium with a spatially varying "entanglement temperature." Using the entanglement Hamiltonian, we calculate the first order change in the entanglement entropy due to changes in conserved charges of the ground state, and find a generalized, local first law-like relation for the entanglement entropy. Our approach provides a field theory derivation and generalization of recent results obtained by holographic techniques. However, we note a discrepancy between our field theoretically derived results for the entanglement entropy of excited states with a non-uniform energy density and current holographic results in the literature. Finally...

  17. Three-step laser excitation of the odd-parity 5s5d 3D → 5s nf 3F states of cadmium

    Nadeem, Ali; Shah, M.; Haq, S. U.; Shahzada, S.; Mumtaz, M.; Waheed, A.; Nawaz, M.; Ahmed, M.; Baig, M. A.

    2014-07-01

    We report new experimental data on the term energies and effective quantum numbers of the highly excited odd parity states of cadmium in the 71 773-72 500 cm-1 energy range. The experiment was performed using three dye lasers simultaneously pumped by the second harmonic (532 nm) of the Nd;YAG laser. The vapor containment and detection system was a thermionic diode ion detector working in a space charge limited mode. The new observations include the 5snf3F3 (12 ⩽ n ⩽ 52), 5snf3F4 (13 ⩽ n ⩽ 33) and 5snf3F2 (12 ⩽ n ⩽ 22) Rydberg series excited from the 5s5d3D multiplet. A two parameter fit to the transitions energies of the 5snf3F3 series yields the binding energy of the 5snd 2D2 level as 13 042.178 ± 0.02 cm-1 and consequently the first ionization of cadmium is determined as 72 540.05 ± 0.13 cm-1, which is in good agreement with the previously reported value.

  18. Internal-nuclear conversion of energy of nucleus excited state

    In the work an effect of penetration electrons of internal conversion showing in hindered M1-transitions was studied. At the moment of a nucleus transition from excited state in low state, electron of atomic shell can appear inside a nucleus and the internal conversion of electrons occur. For such transitions nuclear parameter do not equal zero. The analytical method of definition of nuclear parameter is offered from the relation of intensities L1/L2, L1/L3, L2/L3 of internal conversion of electrons. (authors)

  19. Modular Hamiltonian for Excited States in Conformal Field Theory

    Lashkari, Nima

    2016-07-01

    We present a novel replica trick that computes the relative entropy of two arbitrary states in conformal field theory. Our replica trick is based on the analytic continuation of partition functions that break the Zn replica symmetry. It provides a method for computing arbitrary matrix elements of the modular Hamiltonian corresponding to excited states in terms of correlation functions. We show that the quantum Fisher information in vacuum can be expressed in terms of two-point functions on the replica geometry. We perform sample calculations in two-dimensional conformal field theories.

  20. Is the Z+(4430) a radially excited state of Ds?

    We present the interpretation that the recently discovered Z+(4430) by the Belle Collaboration can be a radial excitation of the cs-bar state, being consistent with an observed value of the product of branching ratios, B(B0→K±Z±(4430))xB(Z±(4430)→π±ψ')∼10-5. We give an explicit cs-bar candidate for this state by calculating the mass value in our semirelativistic quark potential model and also give a natural understanding for the facts that the decay mode Z→J/ψπ+ has not yet been seen while Z→ψ'π can be seen

  1. Self-Scattering for Dark Matter with an Excited State

    Schutz, Katelin

    2014-01-01

    Self-interacting dark matter scenarios have recently attracted much attention, as a possible means to alleviate the tension between N-body simulations and observations of the dark matter distribution on galactic and sub-galactic scales. The presence of internal structure for the dark matter --- for example, a nearly-degenerate state in the spectrum that could decay, or be collisionally excited or de-excited --- has also been proposed as a possible means to address these discrepancies. Such internal structure can be a source of interesting signatures in direct and indirect dark matter searches, for example providing a novel explanation for the 3.5 keV line recently observed in galaxies and galaxy clusters. We analyze a simple model of dark matter self-scattering including a nearly-degenerate excited state, and develop an accurate analytic approximation for the elastic and inelastic $s$-wave cross sections, which is valid outside the perturbative regime provided the particle velocity is sufficiently low (this c...

  2. Quantum Entanglement of Locally Excited States in Maxwell Theory

    Nozaki, Masahiro

    2016-01-01

    In 4 dimensional Maxwell gauge theory, we study the changes of (Renyi) entangle-ment entropy which are defined by subtracting the entropy for the ground state from the one for the locally excited states generated by acting with the gauge invariant local operators on the state. The changes for the operators which we consider in this paper reflect the electric-magnetic duality. The late-time value of changes can be interpreted in terms of electromagnetic quasi-particles. When the operator constructed of both electric and magnetic fields acts on the ground state, it shows that the operator acts on the late-time structure of quantum entanglement differently from free scalar fields.

  3. Excited-State Properties of Molecular Solids from First Principles.

    Kronik, Leeor; Neaton, Jeffrey B

    2016-05-27

    Molecular solids have attracted attention recently in the context of organic (opto)electronics. These materials exhibit unique charge carrier generation and transport phenomena that are distinct from those of conventional semiconductors. Understanding these phenomena is fundamental to optoelectronics and requires a detailed description of the excited-state properties of molecular solids. Recent advances in many-body perturbation theory (MBPT) and density functional theory (DFT) have made such description possible and have revealed many surprising electronic and optical properties of molecular crystals. Here, we review this progress. We summarize the salient aspects of MBPT and DFT as well as various properties that can be described by these methods. These properties include the fundamental gap and its renormalization, hybridization and band dispersion, singlet and triplet excitations, optical spectra, and excitonic properties. For each, we present concrete examples, a comparison to experiments, and a critical discussion. PMID:27090844

  4. Excited-State Properties of Molecular Solids from First Principles

    Kronik, Leeor; Neaton, Jeffrey B.

    2016-05-01

    Molecular solids have attracted attention recently in the context of organic (opto)electronics. These materials exhibit unique charge carrier generation and transport phenomena that are distinct from those of conventional semiconductors. Understanding these phenomena is fundamental to optoelectronics and requires a detailed description of the excited-state properties of molecular solids. Recent advances in many-body perturbation theory (MBPT) and density functional theory (DFT) have made such description possible and have revealed many surprising electronic and optical properties of molecular crystals. Here, we review this progress. We summarize the salient aspects of MBPT and DFT as well as various properties that can be described by these methods. These properties include the fundamental gap and its renormalization, hybridization and band dispersion, singlet and triplet excitations, optical spectra, and excitonic properties. For each, we present concrete examples, a comparison to experiments, and a critical discussion.

  5. Self-scattering for Dark Matter with an excited state

    Self-interacting dark matter scenarios have recently attracted much attention, as a possible means to alleviate the tension between N-body simulations and observations of the dark matter distribution on galactic and sub-galactic scales. The presence of internal structure for the dark matter—for example, a nearly-degenerate state in the spectrum that could decay, or be collisionally excited or de-excited—has also been proposed as a possible means to address these discrepancies. Such internal structure can be a source of interesting signatures in direct and indirect dark matter searches, for example providing a novel explanation for the 3.5 keV line recently observed in galaxies and galaxy clusters. We analyze a simple model of dark matter self-scattering including a nearly-degenerate excited state, and develop an accurate analytic approximation for the elastic and inelastic s-wave cross sections, which is valid outside the perturbative regime provided the particle velocity is sufficiently low (this condition is also required for the s-wave to dominate over higher partial waves). We anticipate our results will be useful in incorporating inelastic self-scattering into N-body simulations, in order to study the quantitative impact of nearly-degenerate states in the dark matter spectrum on galactic structure and dynamics, and in computing the indirect signatures of multi-state dark matter

  6. Systematic study of double beta decay to excited final states

    A systematic study of two-neutrino double beta (2νββ) decay to the final ground state and excited states is performed within a microscopic quasiparticle random phase approximation (QRPA) model. The excited states are assumed to have the structure of one or two QRPA phonons. This study of the 2νββ decay rates is complemented with the study of single-beta-decay feeding of the relevant nuclei taking part in the double beta process. The Woods-Saxon single-particle energies have been corrected near the Fermi surface by comparing the BCS quasi-particle energies with spectroscopic data of the relevant odd-mass nuclei. Pairing gaps, energy systematics of the Gamow-Teller-States and the available beta-decay data have been used to obtain effective, model-space adapted, two-body matrix elements starting from the G-matrix elements of the Bonn one-boson-exchange potential. This enables a parameter-free calculation of the double Gamow-Teller matrix elements and theoretical prediction of double-beta half lives. The harmonic two-phonon approximation has been used in the beta-decay analysis and the subsequent 2νββ calculations. (authors)

  7. Output power of a quantum dot laser: Effects of excited states

    A theory of operating characteristics of quantum dot (QD) lasers is discussed in the presence of excited states in QDs. We consider three possible situations for lasing: (i) ground-state lasing only; (ii) ground-state lasing at first and then the onset of also excited-state lasing with increasing injection current; (iii) excited-state lasing only. The following characteristics are studied: occupancies of the ground-state and excited-state in QDs, free carrier density in the optical confinement layer, threshold currents for ground- and excited-state lasing, densities of photons emitted via ground- and excited-state stimulated transitions, output power, internal and external differential quantum efficiencies. Under the conditions of ground-state lasing only, the output power saturates with injection current. Under the conditions of both ground- and excited-state lasing, the output power of ground-state lasing remains pinned above the excited-state lasing threshold while the power of excited-state lasing increases. There is a kink in the light-current curve at the excited-state lasing threshold. The case of excited-state lasing only is qualitatively similar to that for single-state QDs—the role of ground-state transitions is simply reduced to increasing the threshold current

  8. Excited state dynamics and isomerization in ruthenium sulfoxide complexes.

    King, Albert W; Wang, Lei; Rack, Jeffrey J

    2015-04-21

    Molecular photochromic compounds are those that interconvert between two isomeric forms with light. The two isomeric forms display distinct electronic and molecular structures and must not be in equilibrium with one another. These light-activated molecular switch compounds have found wide application in areas of study ranging from chemical biology to materials science, where conversion from one isomeric form to another by light prompts a response in the environment (e.g., protein or polymeric material). Certain ruthenium and osmium polypyridine sulfoxide complexes are photochromic. The mode of action is a phototriggered isomerization of the sulfoxide from S- to O-bonded. The change in ligation drastically alters both the spectroscopic and electrochemical properties of the metal complex. Our laboratory has pioneered the preparation and study of these complexes. In particular, we have applied femtosecond pump-probe spectroscopy to reveal excited state details of the isomerization mechanism. The data from numerous complexes allowed us to predict that the isomerization was nonadiabatic in nature, defined as occurring from a S-bonded triplet excited state (primarily metal-to-ligand charge transfer in character) to an O-bonded singlet ground state potential energy surface. This prediction was corroborated by high-level density functional theory calculations. An intriguing aspect of this reactivity is the coupling of nuclear motion to the electronic wave function and how this coupling affects motions productive for isomerization. In an effort to learn more about this coupling, we designed a project to examine phototriggered isomerization in bis-sulfoxide complexes. The goal of these studies was to determine whether certain complexes could be designed in which a single photon excitation event would prompt two sulfoxide isomerizations. We employed chelating sulfoxides in this study and found that both the nature of the chelate ring and the R group on the sulfoxide affect

  9. Theoretical aspects of multiphoton ionization with many resonant excited states

    The variety of the parameters involved in multi-color multi-step ionization makes it a formidable job to obtain a theoretically comprehensible overview of the process. We examine these parameters of such processes as well as commonly used assumptions in theoretical investigations of multiphoton ionization with many resonantly excited levels. The density matrix formalism is adequate to treat resonant multiphoton ionization when the number of the resonant levels involved is not too large, solving the resonantly coupled states separately beyond the lowest order perturbation theory, while the rest of the states are treated perturbatively. An example of such formalism is given for a four-level system ionized with three lasers each of which resonantly couples the adjacent pairs of the atomic states.

  10. Excited states in 146Sm and 147Sm

    The sup(144,146)Nd(α,xn) and sup(146,148)Nd(3He,xn) reactions with Esub(α) = 20 - 43 MeV and E3sub(He) = 19 - 27 MeV are used to investigate excited states in the isotopes 146Sm and 147Sm. The experiments involve measurements of singles γ-ray spectra and conversion electron spectra, γ-ray angular distributions and three parameter (E sub(γ)E sub(γ) time) coincidences. From these experiments information is obtained for states with spin up to I = 13+ and I = 27/2-, respectively, These states are interpeted within the framework of the cluster-vibration model (CVM) as well as the shell model. (author)

  11. Excited states above the proton threshold in {sup 26}Si

    Komatsubara, T. [Institute for Basic Science (IBS), Rare Isotope Science Project, Yuseong-gu Daejeon (Korea, Republic of); Kubono, S.; Ito, Y. [RIKEN, Saitama (Japan); Hayakawa, T.; Shizuma, T. [Japan Atomic Energy Agency, Tokai, Ibaraki (Japan); Ozawa, A.; Ishibashi, Y. [University of Tsukuba, Institute of Physics, Tsukuba, Ibaraki (Japan); Moriguchi, T. [National Cerebral and Cardiovascular Center Research Institute, Suita, Osaka (Japan); Yamaguchi, H.; Kahl, D. [University of Tokyo, Wako Branch, Center for Nuclear Study (CNS), Wako, Saitama (Japan); Hayakawa, S. [Laboratori Nazionali del Sud-INFN, Catania (Italy); Nguyen Binh, Dam [Vietnamese Academy for Science and Technology, Institute of Physics, Hanoi (Viet Nam); Chen, A.A.; Chen, J. [McMaster University, Hamilton, Ontario (Canada); Setoodehnia, K. [University of Notre Dame, Department of Physics, Notre Dame, Indiana (United States); Kajino, T. [National Astronomical Observatory, Tokyo (Japan); University of Tokyo, Department of Astronomy, Graduate School of Science, Tokyo (Japan)

    2014-09-15

    The level scheme above the proton threshold in {sup 26}Si is crucial for evaluating the {sup 25}Al(p, γ){sup 26}Si stellar reaction, which is important for understanding the astrophysical origin of the long-lived cosmic radioactivity {sup 26}Al(T{sub 1/2} = 7.17 x 10{sup 5} y) in the Galaxy. The excited states in {sup 26}Si have been studied using an in-beam γ-ray spectroscopy technique with the {sup 24}Mg({sup 3}He, nγ){sup 26}Si reaction. γ-rays with energies up to 4.6 MeV emitted from excited states in {sup 26}Si have been measured using large volume HPGe detectors. The spin-parity of one of the most important states reported recently at 5890.0keV has been assigned as 0{sup +} by γ-γ angular correlation measurements in this work. (orig.)

  12. Weighing excited nuclear states with a Penning trap mass spectrometer

    We report on high-accuracy mass measurements and isomer identification of 187Pb. In this nuclide, two close-lying isomeric states are known from α-decay studies. With the combined use of the ISOLDE resonance ionization laser ion source and the Penning trap mass spectrometer ISOLTRAP the energy difference of 187Pb and 187mPb was determined to be E = 33(13) keV. This is the lowest isomeric excitation energy ever determined by weighing nuclei. (orig.)

  13. Coherence, energy and charge transfers in de-excitation pathways of electronic excited state of biomolecules in photosynthesis

    Bohr, Henrik; Malik, F. Bary

    2013-01-01

    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 F¨orster–Dexter...

  14. Probing the Locality of Excited States with Linear Algebra.

    Etienne, Thibaud

    2015-04-14

    This article reports a novel theoretical approach related to the analysis of molecular excited states. The strategy introduced here involves gathering two pieces of physical information, coming from Hilbert and direct space operations, into a general, unique quantum mechanical descriptor of electronic transitions' locality. Moreover, the projection of Hilbert and direct space-derived indices in an Argand plane delivers a straightforward way to visually probe the ability of a dye to undergo a long- or short-range charge-transfer. This information can be applied, for instance, to the analysis of the electronic response of families of dyes to light absorption by unveiling the trend of a given push-pull chromophore to increase the electronic cloud polarization magnitude of its main transition with respect to the size extension of its conjugated spacer. We finally demonstrate that all the quantities reported in this article can be reliably approximated by a linear algebraic derivation, based on the contraction of detachment/attachment density matrices from canonical to atomic space. This alternative derivation has the remarkable advantage of a very low computational cost with respect to the previously used numerical integrations, making fast and accurate characterization of large molecular systems' excited states easily affordable. PMID:26574379

  15. Excitation gap of fractal quantum hall states in graphene

    Luo, Wenchen; Chakraborty, Tapash

    2016-01-01

    In the presence of a magnetic field and an external periodic potential the Landau level spectrum of a two-dimensional electron gas exhibits a fractal pattern in the energy spectrum which is described as the Hofstadter’s butterfly. In this work, we develop a Hartree-Fock theory to deal with the electron-electron interaction in the Hofstadter’s butterfly state in a finite-size graphene with periodic boundary conditions, where we include both spin and valley degrees of freedom. We then treat the butterfly state as an electron crystal so that we could obtain the order parameters of the crystal in the momentum space and also in an infinite sample. A phase transition between the liquid phase and the fractal crystal phase can be observed. The excitation gaps obtained in the infinite sample is comparable to those in the finite-size study, and agree with a recent experimental observation.

  16. 3alpha clustering in the excited states of 16C

    Baba, T; Kimura, M

    2014-01-01

    The alpha cluster states of 16C are investigated by using the antisymmetrized molecular dynamics. It is shown that two different types of alpha cluster states exist: triangular and linear-chain states. The former has an approximate isosceles triangular configuration of alpha particles surrounded by four valence neutrons occupying sd-shell, while the latter has the linearly aligned alpha particles with two sd-shell neutrons and two pf-shell neutrons. It is found that the structure of the linear-chain state is qualitatively understood in terms of the 3/2 pi- and 1/2 sigma- molecular orbit as predicted by molecular-orbital model, but there exists non-negligible Be+alpha+2n correlation. The band-head energies of the triangular and linear-chain rotational bands are 8.0 and 15.5 MeV, and the latter is close to the He+Be threshold energy. It is also shown that the linear-chain state becomes the yrast sstate at J=10 with excitation energy 27.8 MeV owing to its very large moment-of-inertia comparable with hyperdeforma...

  17. Kinetic studies following state-selective laser excitation

    We have made measurements of state-to-state deactivation cross sections and radiative lifetimes for Xe*(6p,6p',7p) and Kr*(5p) states in xenon and krypton buffer gases. These results are relevant to kinetic models and both excimer lasers and the infrared xenon laser; and they are a significant improvement in the precision of the known radiative lifetimes. This type of experiment can now be compared with recent calculations of state-to-state collisional relaxation in rare-gases by Hickman, Huestis, and Saxon. We have also made significant progress in the study of the electronic spectra of small molecules of the rare gases. Spectra have been obtained for Xe2, Xe3, Xe4, and larger clusters. As guidance for the larger clusters of the rare gases we have obtained the first multiphoton spectra for excitons in condensed xenon. In collaboration with research on the multiphoton spectra of the rare gases, we have continued experiments using synchrotron radiation in collaboration with the University of Hamburg. In experiments there we have observed excitation and fluorescence spectra for single xenon atoms at the surface, within the second layer, and within the bulk of large argon clusters

  18. Observation of interference effects via four photon excitation of highly excited Rydberg states in thermal cesium vapor

    Kondo, Jorge M; Guttridge, Alex; Wade, Christopher G; De Melo, Natalia R; Adams, Charles S; Weatherill, Kevin J

    2015-01-01

    We report on the observation of Electromagnetically Induced Transparency (EIT) and Absorption (EIA) of highly-excited Rydberg states in thermal Cs vapor using a 4-step excitation scheme. The advantage of this 4-step scheme is that the final transition to the Rydberg state has a large dipole moment and one can achieve similar Rabi frequencies to 2 or 3 step excitation schemes using two orders of magnitude less laser power. Consequently each step is driven by a relatively low power infra-red diode laser opening up the prospect for new applications. The observed lineshapes are in good agreement with simulations based on multilevel optical Bloch equations.

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

    Egidi, Franco, E-mail: franco.egidi@sns.it; Segado, Mireia; Barone, Vincenzo, E-mail: vincenzo.barone@sns.it [Scuola Normale Superiore, Piazza dei Cavalieri, 7 I-56126 Pisa (Italy); Koch, Henrik [Department of Chemistry, Norwegian University of Science and Technology, 7491 Trondheim (Norway); Cappelli, Chiara [Dipartimento di Chimica e Chimica Industriale, Università di Pisa, via G. Moruzzi, 3 I-56124 Pisa (Italy)

    2014-12-14

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

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

    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

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

    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.

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

    Dreuw, Andreas, E-mail: andreas.dreuw@theochem.uni-frankfurt.de [Institute of Physical and Theoretical Chemistry, Goethe-University Frankfurt, Max von Laue-Str. 7, 60438 Frankfurt am Main (Germany); Starcke, Jan Hendrik; Wachtveitl, Josef [Institute of Physical and Theoretical Chemistry, Goethe-University Frankfurt, Max von Laue-Str. 7, 60438 Frankfurt am Main (Germany)

    2010-07-19

    Using time-dependent density functional theory, the excited electronic states of the astaxanthin radical cation (AXT{sup {center_dot}+}) are investigated. While the optically allowed excited D{sub 1} and D{sub 3} states are typical {pi}{pi}* excited states, the D{sub 2} and D{sub 4} states are n{pi}* 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 {pi}{pi}* 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.

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

    Using time-dependent density functional theory, the excited electronic states of the astaxanthin radical cation (AXT·+) are investigated. While the optically allowed excited D1 and D3 states are typical ππ* excited states, the D2 and D4 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.

  4. Ultrafast electronic relaxation of excited state vitamin B12 in the gas phase

    The time evolution of electronically excited vitamin B12 (cyanocobalamin) has been observed for the first time in the gas phase. It reveals an ultrafast decay to a state corresponding to metal excitation. This decay is interpreted as resulting from a ring to metal electron transfer. This opens the observation of the excited state of other complex biomimetic systems in the gas phase, the key to the characterisation of their complex evolution through excited electronic states

  5. Breathing-like excited state of the Hoyle state in ${^{12}{\\rm C}}$

    Zhou, Bo; Horiuchi, Hisashi; Ren, Zhongzhou

    2016-01-01

    The existence of the $0_3^+$ and $0_4^+$ states around 10 MeV excitation energy in ${^{12}{\\rm C}}$ is confirmed by a fully microscopic 3$\\alpha$ cluster model. Firstly, a GCM (generator coordinate method) calculation is performed by superposing optimized 2$\\alpha$+$\\alpha$ THSR (Tohsaki-Horiuchi-Schuck-R\\"{o}pke) wave functions with the radius-constraint method. The obtained two excited $0^+$ states above the Hoyle state are consistent with the recently observed states by experiment. Secondly, a variational calculation using the single 2$\\alpha$+$\\alpha$ THSR wave function orthogonalized to the ground and Hoyle states is made and it also supports the existence of the $0_3^+$ state obtained by the GCM calculation. The analysis of the obtained $0_3^+$ state is made by studying its 2$\\alpha$-$\\alpha$ reduced width amplitude, its 2$\\alpha$ correlation function, and the large monopole matrix element between this state and the Hoyle state, which shows that this $0_3^+$ state is a breathing-like excited state of th...

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

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

    2013-09-01

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

  7. Hemispherical Asymmetry from Parity-Violating Excited Initial States

    Ashoorioon, Amjad

    2015-01-01

    We investigate if the hemispherical asymmetry in the CMB is produced from parity-violating excited initial condition. We show that in the limit where the deviations from the Bunch-Davies vacuum is large and the scale of new physics is maximally separated from the inflationary Hubble parameter, the primordial power spectrum is modulated only by dipole and quadrupole terms. Requiring the dipole contribution in the power spectrum accounts for the observed power asymmetry, $A=0.07\\pm0.022$, we show that the amount of quadrupole terms is roughly equal to $A^2$, which is still consistent with the bounds from the CMB. The mean local bispectrum which gets enhanced for the excited initial states is within the $1\\sigma$ bound of Planck 2015 results, $f_{\\rm NL}\\simeq 4.17$, but reachable by future CMB experiments. The amplitude of the local non-gaussianity modulates around this mean value, approximately depending on the angle that the short wavelength mode makes with the preferred direction. The amount of variation max...

  8. Excited states of quantum many-body interacting systems: A variational coupled-cluster description

    Xian, Y.

    2007-01-01

    We extend recently proposed variational coupled-cluster method to describe excitation states of quantum many-body interacting systems. We discuss, in general terms, both quasiparticle excitations and quasiparticle-density-wave excitations (collective modes). In application to quantum antiferromagnets, we reproduce the well-known spin-wave excitations, i.e. quasiparticle magnons of spin $\\pm 1$. In addition, we obtain new, spin-zero magnon-density-wave excitations which has been missing in Ans...

  9. Masses of ground and excited-state hadrons

    Roberts, H L L; Cloet, I C; Roberts, C D

    2011-01-01

    We present the first Dyson-Schwinger equation calculation of the light hadron spectrum that simultaneously correlates the masses of meson and baryon ground- and excited-states within a single framework. At the core of our analysis is a symmetry-preserving treatment of a vector-vector contact interaction. In comparison with relevant quantities the root-mean-square-relative-error/degree-of freedom is 13%. Notable amongst our results is agreement between the computed baryon masses and the bare masses employed in modern dynamical coupled-channels models of pion-nucleon reactions. Our analysis provides insight into numerous aspects of baryon structure; e.g., relationships between the nucleon and Delta masses and those of the dressed-quark and diquark correlations they contain.

  10. Masses of Ground- and Excited-State Hadrons

    Roberts, Hannes L. L.; Chang, Lei; Cloët, Ian C.; Roberts, Craig D.

    2011-07-01

    We present the first Dyson-Schwinger equation calculation of the light hadron spectrum that simultaneously correlates the masses of meson and baryon ground- and excited-states within a single framework. At the core of our analysis is a symmetry-preserving treatment of a vector-vector contact interaction. In comparison with relevant quantities the root-mean-square-relative-error/degree-of freedom is 13%. Notable amongst our results is agreement between the computed baryon masses and the bare masses employed in modern dynamical coupled-channels models of pion-nucleon reactions. Our analysis provides insight into numerous aspects of baryon structure; e.g., relationships between the nucleon and Δ masses and those of the dressed-quark and diquark correlations they contain.

  11. Chimera states and excitation waves in networks with complex topologies

    Schöll, Eckehard

    2016-06-01

    Chimera patterns, which consist of coexisting spatial domains of coherent (synchronized) and incoherent (desyn- chronized) dynamics are studied in networks of FitzHugh-Nagumo systems with complex topologies. To test the robustness of chimera patterns with respect to changes in the structure of the network, we study the following network topologies: Regular ring topology with R nearest neigbors coupled to each side, small-world topology with additional long-range random links, and a hierarchical geometry in the connectivity matrix. We find that chimera states are generally robust with respect to these perturbations, but qualitative changes of the chimera patterns in form of nested coherent and incoherent regions can be induced by a hierarchical topology. The suppression of propagating excitation waves by a small-world topology is also reviewed.

  12. Ultrafast Spectroscopy of Delocalized Excited States of the Hydrated Electron

    Research under support of this grant has been focused on the understanding of highly delocalized ''conduction-band-like'' excited states of solvated electrons in bulk water, in water trapped in the core of reverse micelles, and in alkane solvents. We have strived in this work to probe conduction-band-like states by a variety of ultrafast spectroscopy techniques. (Most of which were developed under DOE support in a previous funding cycle.) We have recorded the optical spectrum of the hydrated electron for the first time. This was accomplished by applying a photo-detrapping technique that we had developed in a previous funding cycle, but had not yet been applied to characterize the actual spectrum. In the cases of reverse micelles, we have been investigating the potential role of conduction bands in the electron attachment process and the photoinduced detrapping, and have published two papers on this topic. Finally, we have been exploring solvated electrons in isooctane from various perspectives. All of these results strongly support the conclusion that optically accessible, highly delocalized electronic states exist in these various media

  13. Suppression of Excited-State Contributions to Stellar Reaction Rates

    Rauscher, T

    2013-01-01

    It has been shown in previous work [Phys. Rev. Lett. 101, 191101 (2008); Phys. Rev. C 80, 035801 (2009)] that a suppression of the stellar enhancement factor (SEF) occurs in some endothermic reactions at and far from stability. This effect is re-evaluated using the ground-state contributions to the stellar reaction rates, which were shown to be better suited to judge the importance of excited state contributions than the previously applied SEFs. An update of the tables shown in Phys. Rev. C 80, 035801 (2009) is given. The new evalution finds 2350 cases (out of a full set of 57513 reactions) for which the ground-state contribution is larger in the reaction direction with negative reaction Q-value than in the exothermic direction, thus providing exceptions to the commonly applied Q-value rule. The results confirm the Coulomb suppression effect but lead to a larger number of exceptions than previously found. This is due to the fact that often a large variation in the g.s. contribution does not lead to a sizeable...

  14. Foil dissociation of fast molecular ions into atomic excited states

    The intensity and polarizations of light emitted from atomic excited states of dissociated molecular ions were measured. The dissociations are induced when fast molecular ions (50 to 500 keV/amu) are transmitted through thin carbon foils. A calculation of multiple scattering and the Coulomb explosion gives the average internuclear separation of the projectile at the foil surface. Experimentally, the foil thickness is varied to give varying internuclear separations at the foil surface and observe the consequent variation in light yield and optical polarization. Using HeH+ projectiles, factors of 1 to 5 enhancements of the light yields from n = 3, 13P,D states of He I and some He II and H I emissions were observed. The results can be explained in terms of molecular level crossings which provide mixings of the various final states during dissociation of the molecular ions at the exit surface. They suggest a short range surface interaction of the electron pick-up followed by a slow molecular dissociation. Alignment measurements confirm the essential features of the model. Observations of Lyman α emission after dissociation of H2+ amd H3+ show rapid variations in light yield for small internuclear separations at the foil surface

  15. Dynamics of the excited state intramolecular charge transfer

    The 6-dodecanoyl-2-dimethylaminonaphtalene (laurdan), a derivative of 6-propanoyl- 2-dimethylaminonaphthalene (prodan), has been used as a fluorescent probe in cell imaging, especially in visualizing the lipid rafts by the generalized polarization (GP) images, where GP=(I440-I490)/(I440+I490) with I being the fluorescence intensity. The fluorescence spectrum of laurdan is sensitive to its dipolar environment due to the intramolecular charge transfer (ICT) process in S1 state, which results in a dual emission from the locally excited (LE) and the ICT states. The ICT process and the solvation of the ICT state are very sensitive to the dipolar nature of the environment. In this work, the ICT of laurdan in ethanol has been studied by femtosecond time resolved fluorescence (TRF), especially TRF spectra measurement without the conventional spectral reconstruction method. TRF probes the excited states exclusively, a unique advantage over the pump/probe transient absorption technique, although time resolution of the TRF is generally lower than transient absorption and the TRF spectra measurement was possible only though the spectral reconstruction. Over the years, critical advances in TRF technique have been made in our group to achieve <50 fs time resolution with direct full spectra measurement capability. Detailed ICT and the subsequent solvation processes can be visualized unambiguously from the TRF spectra. Fig. 1 shows the TRF spectra of laurdan in ethanol at several time delays. Surprisingly, two bands at 433 and 476 nm are clearly visible in the TRF spectra of laurdan even at T = 0 fs. As time increases, the band at 476 nm shifts to the red while its intensity increases. The band at 433 nm also shifts slightly to the red, but loses intensity as time increases. The intensity of the 476 nm band reaches maximum at around 5 ps, where it is roughly twice as intense as that at 0 fs, and stays constant until lifetime decay is noticeable. The spectra were fit by two log

  16. Carotenoid excited states: Mystery of the dark states and their roles in relaxation pathways

    Polívka, Tomáš

    Messina : Universitá di Messina, 2008. s. 36. [ESF Workshop on Ultrafast Excited-State Processes in Condensed Phases. 18.06.2008-21.06.2008, Santa Tecla] Institutional research plan: CEZ:AV0Z50510513 Keywords : carotenoids Subject RIV: BO - Biophysics

  17. Study of excited states of mass=4 hypernuclei

    The excited states, J=1+, of the mirror hypernuclei sub(Λ)sup(4)H and sub(Λsup(4)He were observed by γ-spectroscopy. These hypernuclei were producted by K- absorption in 6Li and 7Li targets. Their identification was given by the detection and the energy measurement of the mesonic decay products: 53 MeV π- for sub(Λ)sup(4)H and 57 MeV π0 for sub(Λ)sup(4)He. A γ line at (1.04+-0.04) MeV has been observed in coincidence with charged pions in the energy range of 40 to 60 MeV then ascribed to a γ-transition in sub(Λ)sup(4)H. Whereas a second γ-line at (1.15+-0.04) MeV, in coincidence with neutral pions of 45 MeV to 75 MeV, has been ascribed to a γ transition in sub(Λ)sup(4)He. With these new experimental data, the phenomenological Λ-N potential for the S-state interaction was recalculated. It may be concluded that the CSB component of this Λ-N potential is spin-independant and that potentials with intrinsic range of 1.5 fm give the bast fit of the total low energy Λ - p elastic scattering cross-sections and to the experimental Bsub(Λ) value for sub(Λ)sup(3)H

  18. Ground States and Excited States in a Tunable Graphene Quantum Dot

    WANG Lin-Jun; CAO Gang; TU Tao; LI Hai-Ou; ZHOU Cheng; HAO Xiao-Jie; GUO Guang-Can; GUO Guo-Ping

    2011-01-01

    We prepare an etched gate tunable quantum dot in single-layer graphene and present transport measurement in this system. We extract the information of the ground states and excited states of the graphene quantum dot, as denoted by the presence of characteristic Coulomb blockade diamond diagrams. The results demonstrate that the quantum dot in single-layer graphene bodes well in future quantum transport study and quantum computing applications.%@@ We prepare an etched gate tunable quantum dot in single-layer graphene and present transport measurement in this system.We extract the information of the ground states and excited states of the graphene quantum dot, as denoted by the presence of characteristic Coulomb blockade diamond diagrams.The results demonstrate that the quantum dot in single-layer graphene bodes well in future quantum transport study and quantum computing applications.

  19. Ground States and Excited States in a Tunable Graphene Quantum Dot

    We prepare an etched gate tunable quantum dot in single-layer graphene and present transport measurement in this system. We extract the information of the ground states and excited states of the graphene quantum dot, as denoted by the presence of characteristic Coulomb blockade diamond diagrams. The results demonstrate that the quantum dot in single-layer graphene bodes well for future quantum transport study and quantum computing applications. (condensed matter: electronic structure, electrical, magnetic, and optical properties)

  20. Excited state dipole moments of chloroanilines and chlorophenols from solvatochromic shifts in electronic absorption spectra: Support for the concept of excited state group moments

    Prabhumirashi, L. S.; Satpute, R. S.

    The dipole moments of isomeric o-, m- and p-chloroanilines and chlorophenols in electronically excited L a and L b states are estimated from solvent induced polarization shifts in electronic absorption spectra. It is observed that μ e( L a) > μ e( L b) > μ g, which is consistent with the general theory of polarization red shift. The μ es are found to be approximately co-linear with the corresponding μ gs. The concept of group moments is extended to aromatic molecules in excited states. This approach is found to be useful in understanding correlations among the excited states of mono- and disubstituted benzenes.

  1. One-photon excitation and dissociation of both weakly bound rotational excited states and vibrational excited states of HD2+ and photofragment branching ratio D+/H+ of the final predissociative states

    The presence of weakly bound rotationally excited initial states of HD2+ lying just below the lowest dissociation limit has been observed as well as quasi-bound, predissociative final states above the dissociation limit resulting from one-photon excitation of those weakly bound states. The excitation of the initial weakly bound and possibly only few quasi-bound states took place with 1064 nm laser radiation. The possibility of one-photon excitation of the vibrationally excited initial HD2+ ions is considered. The centre-of-mass kinetic energy distributions of the D+ and H+ fragment were used to identify the possible initial and final states involved in the transitions leading to these fragments. The fragment ratio D+/H+ is shown to be critically dependent on the ion source pressure. A strong preference is observed for the D++HD dissociation channel over the H++D2 channel at high source gas pressures. The centre-of-mass energy of the resulting H+ and D+ fragments was found to agree with predicted theoretical values, and suggest that among initially excited HD2+ ions, only a few of these lie initially above the lowest dissociation limit. (author)

  2. One-photon excitation and dissociation of both weakly bound rotational excited states and vibrational excited states of HD{sub 2}{sup +} and photofragment branching ratio D{sup +}/H{sup +} of the final predissociative states

    Yousif, F.B. [Centro de Ciencias Fisicas, UNAM, Cuernavaca, Morelos (Mexico)]. E-mail: fbyousif@fis.unam.mx; Cisneros, C.; Urquijo, J. de; Alvarez, I. [Centro de Ciencias Fisicas, UNAM, Cuernavaca, Morelos (Mexico)

    2001-03-14

    The presence of weakly bound rotationally excited initial states of HD{sub 2}{sup +} lying just below the lowest dissociation limit has been observed as well as quasi-bound, predissociative final states above the dissociation limit resulting from one-photon excitation of those weakly bound states. The excitation of the initial weakly bound and possibly only few quasi-bound states took place with 1064 nm laser radiation. The possibility of one-photon excitation of the vibrationally excited initial HD{sub 2}{sup +} ions is considered. The centre-of-mass kinetic energy distributions of the D{sup +} and H{sup +} fragment were used to identify the possible initial and final states involved in the transitions leading to these fragments. The fragment ratio D{sup +}/H{sup +} is shown to be critically dependent on the ion source pressure. A strong preference is observed for the D{sup +}+HD dissociation channel over the H{sup +}+D{sub 2} channel at high source gas pressures. The centre-of-mass energy of the resulting H{sup +} and D{sup +} fragments was found to agree with predicted theoretical values, and suggest that among initially excited HD{sub 2}{sup +} ions, only a few of these lie initially above the lowest dissociation limit. (author)

  3. TDDFT study on the excited-state proton transfer of 8-hydroxyquinoline: Key role of the excited-state hydrogen-bond strengthening

    Lan, Sheng-Cheng; Liu, Yu-Hui

    2015-03-01

    Density functional theory (DFT) and time-dependent density functional theory (TDDFT) calculations have been employed to study the excited-state intramolecular proton transfer (ESIPT) reaction of 8-hydroxyquinoline (8HQ). Infrared spectra of 8HQ in both the ground and the lowest singlet excited states have been calculated, revealing a red-shift of the hydroxyl group (-OH) stretching band in the excited state. Hence, the intramolecular hydrogen bond (O-H···N) in 8HQ would be significantly strengthened upon photo-excitation to the S1 state. As the intramolecular proton-transfer reaction occurs through hydrogen bonding, the ESIPT reaction of 8HQ is effectively facilitated by strengthening of the electronic excited-state hydrogen bond (O-H···N). As a result, the intramolecular proton-transfer reaction would occur on an ultrafast timescale with a negligible barrier in the calculated potential energy curve for the ESIPT reaction. Therefore, although the intramolecular proton-transfer reaction is not favorable in the ground state, the ESIPT process is feasible in the excited state. Finally, we have identified that radiationless deactivation via internal conversion (IC) becomes the main dissipative channel for 8HQ by analyzing the energy gaps between the S1 and S0 states for the enol and keto forms.

  4. The Need, Benefits, and Demonstration of a Minimization Principle for Excited States

    Bacalis, Naoum C

    2015-01-01

    It is shown that the standard methods of computing excited states in truncated spaces must yield wave functions that, beyond truncation, are in principle veered away from the exact, and a remedy is demonstrated via a presented functional, F$_n$, obeying a minimization principle for excited states. It is further demonstrated that near avoided crossings, between two MCSCF 'flipped roots' the wave function that leads to the excited state has the lowest F$_n$.

  5. Structural and excited-state properties of oligoacene crystals from first principles

    Rangel, Tonatiuh; Berland, Kristian; Sharifzadeh, Sahar; Brown-Altvater, Florian; Lee, Kyuho; Hyldgaard, Per; Kronik, Leeor; Neaton, Jeffrey B.

    2016-01-01

    Molecular crystals are a prototypical class of van der Waals (vdW) bound organic materials with excited state properties relevant for optoelectronics applications. Predicting the structure and excited state properties of molecular crystals presents a challenge for electronic structure theory, as standard approximations to density functional theory (DFT) do not capture long range vdW dispersion interactions and do not yield excited state properties. In this work, we use a combination of DFT in...

  6. Excited-state spectroscopy of single NV defects in diamond using optically detected magnetic resonance

    Using pulsed optically detected magnetic resonance techniques, we directly probe electron-spin resonance transitions in the excited-state of single nitrogen-vacancy (NV) color centers in diamond. Unambiguous assignment of excited state fine structure is made, based on changes of NV defect photoluminescence lifetime. This study provides significant insight into the structure of the emitting 3E excited state, which is invaluable for the development of diamond-based quantum information processing.

  7. Excited states in doubly-odd 98Rh

    Excited states in the 98Rh nucleus were populated in the 75As(28Si, 2p3n) fusion-evaporation reaction using the 120 MeV 28Si beam. The experiment was carried out at Inter University Accelerator Centre (IUAC), New Delhi. The 28Si projectiles were provided by the 15UD Pelletron accelerator. The target ∼ 3 mg/cm2 thick (ΔE ∼ 20 MeV) was prepared by vacuum evaporation of natural 75As on to ∼ 10 mg/cm2 natural Pb backing followed by rolling. The 103Ag compound nucleus produced in the present reaction is found to decay via several reaction channels associated with 5-particle emission, viz., p4n (98Pd), 2p3n (98Rh), and αp3n (95Ru) with relative population of ∼ 4%, 13%, and 2%, respectively, 4-particle emission, viz., p3n (99Pd), 2p2n (99Rh), and αp2n (96Ru) with relative population of ∼ 12%, 26%, and 20%, respectively, and 3-particle emission, viz., p2n (100Pd), α2n (97Rh), and 2αn (94Tc) with relative population of ∼ 9%, 6%, and 2%, respectively

  8. Hertzian spectroscopy application to excited states in accelerated ion beams

    It is shown that accelerated ion beams enables the application of optical hertzian spectrometry methods to be extended to research on the excited states of free ionic systems. The photon beat method has proved especially simple to apply in beam foil geometry because of the unidirectional beam velocity while the beam gas device is suitable for experiments of the energy level crossing type. Only the resonance technique involving direct application of high-frequency magnetic fields poses serious problems because of the high HF powers necessary. So far structure intervals have been measured in ions carrying up to three charges (seven in the special case of Lamb shift measurements) with a precision of a few percent. The interest of these structure studies in free ions is emphasized particularly. The study of hydrogen-like or helium-like ions of high Z allows the fundamental calculations of quantum electrodynamics to be checked with regard to the Lamb shift or the spontaneous emission theory. In more complex electronic systems, optical spectroscopy of accelerated ion beams gives wavelengths with a resolution reaching 10-5, lifetimes with an accuracy better than 10% when the cascade effects are properly studied, and Lande factors with a precision of several % under present technical conditions. The photon beat method concerns hyperfine nuclear effects in light atoms of Z<=20. Another line of research study the hyperfine structure of a given configuration in an isoelectronic sequence

  9. A Simple Hubbard Model for the Excited States of $\\pi$ Conjugated -acene Molecules

    Sadeq, Z S

    2015-01-01

    In this paper we present a model that elucidates in a simple way the electronic excited states of $\\pi$ conjugated -acene molecules such as tetracene, pentacene, and hexacene. We use a tight-binding and truncated Hubbard model written in the electron-hole basis to describe the low lying excitations with reasonable quantitative accuracy. We are able to produce semi-analytic wavefunctions for the electronic states of the system, which allows us to compute the density correlation functions for various states such as the ground state, the first two singly excited states, and the lowest lying doubly excited state. We show that in this lowest lying doubly excited state, a state which has been speculated as to being involved in the singlet fission process, the electrons and holes behave in a triplet like manner.

  10. The Structure of the Nucleon and its Excited States

    The past year has been an exciting and productive one for particle physics research at Abilene Christian University. The thrust of our experimental investigations is the study of the nucleon and its excited states. Laboratories where these investigations are presently being conducted are the AGS at Brookhaven, Fermilab and LAMPF. Some analysis of the data for experiments at the Petersburg Nuclear Physics Institute (Gatchina, Russia) is still in progress. Scheduling of activities at different laboratories inevitably leads to occasional conflicts. This likelihood is increased by the present budget uncertainties at the laboratories that make long-term scheduling difficult. For the most part, the investigators have been able to avoid such conflicts. Only one experiment received beam time in 1994 (E890 at the AGS). The situation for 1995-1996 also appears manageable at this point. E890 and another AGS experiment (E909) will run through May, 1995. El 178 at LAMPF is presently scheduled for August/September 1995. E866 at Fermilab is scheduled to start in Spring/Summer 1996. Undergraduate student involvement has been a key element in this research contract since its inception. Summer students participated at all of the above laboratories in 1994 and the same is planned in 1995. A transition to greater involvement by graduate students will provide cohesiveness to ACU involvement at a given laboratory and full-time on-site involvement in the longer running experiments at FNAL and BNL. Funds to support a full-time graduate student are requested this year. Finally, collaboration by Russian, Croatian and Bosnian scientists has proven to be mutually beneficial to these experimental programs and to the overall programs at the institutions involved. Past support has been augmented by other grants from government agencies and from the Research Council at Abilene Christian University. Additional funds are requested in this renewal to enable more programmatic support for these

  11. Photodissociation path in H2 + induced by nonuniform optical near fields: Two-step excitation via vibrationally excited states

    Yamaguchi, Maiku; Nobusada, Katsuyuki

    2016-02-01

    In this paper, effects of the spatial nonuniformity of an optical near field (ONF) on the molecular photodissociation process are presented. The dissociation dynamics of H2 + was theoretically investigated by solving a non-Born-Oppenheimer Schrödinger equation. It was found that in addition to two dissociation mechanisms, which are one-photon and three-photon processes induced by uniform laser light excitation, the nonuniform ONF opens another dissociation path: two-step excitation mediated by vibrationally excited states. The nonuniformity of the ONF causes a transition between vibrational states that is forbidden according to conventional selection rules, leading to the dissociation path. The dependences of photodissociation on the intensity and nonuniformity of the ONF were calculated and the results validated the two-step dissociation mechanism.

  12. Interplay between singlet and triplet excited states in a conformationally locked donor–acceptor dyad

    Filatov, Mikhail A.

    2015-10-13

    The synthesis and photophysical characterization of a palladium(II) porphyrin – anthracene dyad bridged via short and conformationally rigid bicyclo[2.2.2]octadiene spacer were achieved. A spectroscopic investigation of the prepared molecule in solution has been undertaken to study electronic energy transfer in excited singlet and triplet states between the anthracene and porphyrin units. By using steady-state and time-resolved photoluminescence spectroscopy it was shown that excitation of the singlet excited state of the anthracene leads to energy transfer to the lower-lying singlet state of porphyrin. Alternatively, excitation of the porphyrin followed by intersystem crossing to the triplet state leads to very fast energy transfer to the triplet state of anthracene. The rate of this energy transfer has been determined by transient absorption spectroscopy. Comparative studies of the dynamics of triplet excited states of the dyad and reference palladium octaethylporphyrin (PdOEP) have been performed.

  13. Probing an Excited-State Atomic Transition Using Hyperfine Quantum Beat Spectroscopy

    Wade, Christopher G; Keaveney, James; Adams, Charles S; Weatherill, Kevin J

    2014-01-01

    We describe a method to observe the dynamics of an excited-state transition in a room temperature atomic vapor using hyperfine quantum beats. Our experiment using cesium atoms consists of a pulsed excitation of the D2 transition, and continuous-wave driving of an excited-state transition from the 6P$_{3/2}$ state to the 7S$_{1/2}$ state. We observe quantum beats in the fluorescence from the 6P$_{3/2}$ state which are modified by the driving of the excited-state transition. The Fourier spectrum of the beat signal yields evidence of Autler-Townes splitting of the 6P$_{3/2}$, F = 5 hyperfine level and Rabi oscillations on the excited-state transition. A detailed model provides qualitative agreement with the data, giving insight to the physical processes involved.

  14. Excited state lifetime during photostimulated desorption of no from a Pt surface

    Magkoev, T. T.

    1998-07-01

    We analyze the rotational energy distribution N(J) for NO molecules desorbed from a Pt (111) surface, taking into account the valence electron excitations, using a simple impulse model. We find a linear dependence between ln N(J) and (Er)1/2, where Er is the rotational energy of the desorbed molecules. The excited state lifetime and the critical residence time in the excited state, evaluated from the given dependences, are close to each other, and in order of magnitude are 10-15 s. We also estimate the frequency and amplitude of the tilting vibrations of the adsorbed molecules in the excited state.

  15. A Dark Excited State of Fluorescent Protein Chromophores, Considered as Brooker Dyes

    Olsen, Seth

    2010-01-01

    The green fluorescent protein (GFP) chromophore is an asymmetric monomethine dye system. In the resonance color theory of dyes, a strong optical excitation arises from interactions of two valence-bond structures with a third, higher structure. We use correlated quantum chemistry to show that the anionic chromophore is a resonant Brooker dye, and that the third structure corresponds to a higher stationary electronic state of this species. The excitation energy of this state should be just below the first excitation energy of the neutral form. This has implications for excited state mechanism in GFPs, which we discuss.

  16. Two-mode excited entangled coherent states and their entanglement properties

    Zhou Dong-Lin; Kuang Le-Man

    2009-01-01

    This paper introduces two types of two-mode excited entangled coherent states(TMEECSs)|Ψ±(α,m,n)>,studies their entanglement characteristics,and investigates the influence of photon excitations on quantum entanglement.It shows that for the state|Ψ+(α,m,m)>the two-mode photon excitations affect seriously entanglement character while the state |Ψ-(α,m,m)>is always a maximally entangled state,and shows how such states can be produced by using cavity quantum electrodynamics and quantum measurements.It finds that the entanglement amount of the TMEECSs is larger than that of the single-mode excited entangled coherent states with the same photon excitation number.

  17. State-averaged Monte Carlo configuration interaction applied to electronically excited states

    Coe, J P

    2014-01-01

    We introduce state-averaging into the method of Monte Carlo configuration interaction (SA-MCCI) to allow the stable and efficient calculation of excited states. We show that excited potential curves for H$_{3}$, including a crossing with the ground state, can be accurately reproduced using a small fraction of the FCI space. A recently introduced error measure for potential curves [J. P. Coe and M. J. Paterson, J. Chem. Phys., 137, 204108 (2012)] is shown to also be a fair approach when considering potential curves for multiple states. We demonstrate that potential curves for LiF using SA-MCCI agree well with the FCI results and the avoided crossing occurs correctly. The seam of conical intersections for CH$_{2}$ found by Yarkony [J. Chem. Phys., 104, 2932 (1996)] is used as a test for SA-MCCI and we compare potential curves from SA-MCCI with FCI results for this system for the first three triplet states. We then demonstrate the improvement from using SA-MCCI on the dipole of the $2$ $^{1}A_{1}$ state of carbo...

  18. Optimization of Ground- and Excited-State Wave Functions and van der Waals Clusters

    A quantum Monte Carlo method is introduced to optimize excited-state trial wave functions. The method is applied in a correlation function Monte Carlo calculation to compute ground- and excited-state energies of bosonic van der Waals clusters of up to seven particles. The calculations are performed using trial wave functions with general three-body correlations

  19. Local density approximation for exchange in excited-state density functional theory

    Harbola, Manoj K.; Samal, Prasanjit

    2004-01-01

    Local density approximation for the exchange energy is made for treatment of excited-states in density-functional theory. It is shown that taking care of the state-dependence of the LDA exchange energy functional leads to accurate excitation energies.

  20. Ultrafast dynamics and excited state deactivation of [Ru(bpy)2Sq]+ (Ru-Sq)

    Excited state dynamics of Ru-Sq has been studied using time resolved transient absorption spectroscopy with a time resolution of about 100fs. [Ru(bpy)2Sq]+, where bpy is the bipyridyl and Sq is the semi quinone is known to have two ground state absorption bands corresponding to two different metal to ligand charge transfer (MLCT) states. The absorption band centered on 460 nm is assigned to Ru(d) to bpy (π*) and the one on 890 nm is assigned to Ru(d) to Sq(π*). Significantly different excited state relaxation dynamics for both the MLCT states have been observed exciting both the bands separately. (author)

  1. Influence of multiple excitation of low lying states and giant resonances on heavy ion inelastic spectra

    The inelastic excitation probabilities of 40Ca, 90Zr and 208Pb impinged by 40Ca projectiles at bombarding energies between 10 and 100 MeV/nucleon are calculated in a model where the excitation amplitudes are evaluated along classical trajectories. The excited states are calculated in the random phase approximation and the nuclear and Coulomb excitations of both low lying states and giant resonances of the target and projectile are taken into account. A general feature of the calculated spectra for near grazing impact parameters and bombarding energies above 20 MeV/nucleon is the presence of broad regularly-spaced structures mainly due to the excitation of multiphonon states built with giant resonances. Cross section estimates for the inelastic excitations are given

  2. A Doubles Correction to Electronic Excited States from Configuration Interaction in the Space of Single Substitutions

    Head-Gordon, Martin; Rico, Rudolph J.; Lee, Timothy J.; Oumi, Manabu

    1994-01-01

    A perturbative correction to the method of configuration interaction with single substitutions (CIS) is presented. This CIS(D) correction approximately introduces the effect of double substitutions which are absent in CIS excited states. CIS(D) is a second-order perturbation expansion of the coupled-cluster excited state method, restricted to single and double substitutions, in a series in which CIS is zeroth order, and the first-order correction vanishes. CIS (D) excitation energies are size consistent and the calculational complexity scales with the fifth power of molecular size, akin to second-order Moller-Plesset theory for the ground state. Calculations on singlet excited states of ethylene, formaldehyde, acetaldehyde, butadiene and benzene show that CIS (D) is a uniform improvement over CIS. CIS(D) appears to be a promising method for examining excited states of large molecules, where more accurate methods are not feasible.

  3. Efficient 800nm upconversion luminescence emission in 1.319μm excited thulium-doped fluorogermanate

    Gouveia-Neto, A. S.; Vermelho, M. V. D.; Jacinto, C.; Gouveia, E. A.; Bueno, L. A.

    2016-02-01

    Generation of near-infrared light within the first biological optical window via frequency upconversion in Tm3+-doped PbGeO3-PbF2-CdF2 glass excited within the second biological window at 1.319 μm is reported. The upconversion emission at 800 nm is the sole light signal observed in the entire UV-VIS-NIR spectral region making possible obtaining high contrast imaging. The dependence of the 800 nm signal upon the sample temperature was investigated and results showed an increase by a factor of x2.5 in the 30°C - 280°C range. Generation of detectable 690 nm for temperatures above 100°C in addition to the intense 800 nm main signal was also observed. The proposed excitation mechanism for the 800 nm thulium emitting level is assigned to a multiphonon-assisted excitation from the ground-state 3H6 to the 3H5 excited-state level, a rapid relaxation to the 3F4 level and followed by an excited-state absorption of the pump photons mediated by multiphonons connecting the 3F4 level to the 3H4 emitting level.

  4. 1.319 μm excited intense 800 nm frequency upconversion emission in Tm3+-doped fluorogermanate glass

    Gouveia-Neto, A. S.; Vermelho, M. V. D.; Gouveia, E. A.; Bueno, L. A.; Jacinto, C.

    2015-11-01

    Generation of near-infrared light within the first biological optical window via frequency upconversion in Tm3+-doped PbGeO3-PbF2-CdF2 glass excited within the second biological window at 1.319 μm is reported. The upconversion emission at 800 nm is the sole light signal observed in the entire ultraviolet-visible-near-infrared spectral region making it possible obtaining high contrast imaging. The dependence of the 800 nm signal upon the sample temperature was investigated and results showed an increase by a factor of ×2.5 in the 30-280 °C range. Generation of detectable 690 nm for temperatures above 100 °C in addition to the intense 800 nm main signal was also observed. The proposed excitation mechanism for the 800 nm thulium emitting level is assigned to a multiphonon-assisted excitation from the ground-state 3H6 to the 3H5 excited-state level, a rapid relaxation to the 3F4 level and followed by an excited-state absorption of the pump photons mediated by multiphonons connecting the 3F4 level to the 3H4 emitting level.

  5. Exotic and excited-state meson spectroscopy and radiative transitions from lattice QCD

    Christopher Thomas

    2010-09-01

    We discuss recent progress in extracting the excited meson spectrum and radiative transition form factors using lattice QCD. We mention results in the charmonium sector, including the first lattice QCD calculation of radiative transition rates involving excited charmonium states, highlighting results for high spin and exotic states. We present recent results on a highly excited isovector meson spectrum from dynamical anisotropic lattices. Using carefully constructed operators we show how the continuum spin of extracted states can be reliably identified and confidently extract excited states, states with exotic quantum numbers and states of high spin. This spectrum includes the first spin-four state extracted from lattice QCD. We conclude with some comments on future prospects.

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

    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. PMID:26587877

  7. Ground and Excited States of Bipolarons in Two and Three Dimensions

    RUAN Yong-Hong; CHEN Qing-Hu

    2007-01-01

    The properties of large bipolarons in two and three dimensions are investigated by averaging over the relative wavefunction of the two electrons and using the Lee-Low-Pines-Huybrechts variational method. The groundstate (GS) and excited-state energies of the Fr(o)hlich bipolaron for the whole range of electron-phonon coupling constants can be obtained. The energies of the first relaxed excited state (RES) and Franck-Condon (FC) excited state of the bipolaron are also calculated. It is found that the first RES energy is lower than the FC state energy. The comparison of our GS and RES energies with those in literature is also given.

  8. Continuum excitations of $^{26}$O in a three-body model: $0^+$ and $2^+$ states

    Grigorenko, L V

    2015-01-01

    The structure and decay dynamics for $0^+$ and $2^+$ continuum excitations of $^{26}$O are investigated in a three-body $^{24}$O+$n$+$n$ model. Validity of a simple approximation for the cross section profile for long-lived $2n$ emission is demonstrated. Sequence of three $0^+$ monopole ("breathing mode" type) excited states is predicted. These states could probably be interpreted as analogues of Efimov states pushed into continuum by insufficient binding. The possible energies of the $2^+$ states are related to excitation spectrum of $^{25}$O. We discuss possible connection of predicted $^{26}$O spectrum with observations.

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

    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.

  10. Excited triplet states as photooxidants in surface waters

    Canonica, S.

    2012-12-01

    The chromophoric components of dissolved organic matter (DOM) are generally the main absorbers of sunlight in surface waters and therefore a source of transient reactants under irradiation. Such short-lived species can be relevant for the fate of various classes of chemical contaminants in the aquatic environment. The present contribution focuses on the role of excited triplet states of chromophoric DOM, 3CDOM*, as transient photooxidants initiating the transformation and degradation of organic chemical contaminants. An early study [1] indicated that 3CDOM* may play a dominant role in the photo-induced transformation of electron-rich phenols, a conclusion which was later fortified by the results of transient absorption investigations using aromatic ketones as model photosensitizers [2] and by a recent careful analysis of the effect of oxygen concentration on transformation rates [3]. The variety of aquatic contaminants shown to be affected by triplet-induced oxidation has kept increasing, phenylurea herbicides [4], sulfonamide antibiotics [5] and some phytoestrogens [6] being prominent examples. Recent research has shown that the triplet-induced transformation of specific contaminants, especially aromatic nitrogen compounds, could be inhibited by the presence of DOM, very probably due to its antioxidant moieties [7]. While such moieties are not relevant for the quenching of 3CDOM*, they are expected to react with it in a similar way as the studied contaminants. Analogous reactions can be postulated to occur in liquid or solid phases of the atmospheric environment, as demonstrated in the case of HONO formation [8]. References 1. Canonica, S.; Jans, U.; Stemmler, K.; Hoigné, J. Transformation kinetics of phenols in water: Photosensitization by dissolved natural organic material and aromatic ketones. Environ. Sci. Technol. 1995, 29 (7), 1822-1831. 2. Canonica, S.; Hellrung, B.; Wirz, J. Oxidation of phenols by triplet aromatic ketones in aqueous solution. J. Phys

  11. Heme photolysis occurs by ultrafast excited state metal-to-ring charge transfer.

    Franzen, S.; Kiger, L.; Poyart, C; Martin, J.L.

    2001-01-01

    Ultrafast time-resolved resonance Raman spectra of carbonmonoxy hemoglobin (Hb), nitroxy Hb, and deoxy Hb are compared to determine excited state decay mechanisms for both ligated and unligated hemes. Transient absorption and Raman data provide evidence for a sequential photophysical relaxation pathway common to both ligated and unligated forms of Hb* (photolyzed heme), in which the excited state 1Q decays sequentially: 1Q-->Hb*I-->Hb*II-->Hb ground state. Consistent with the observed kinetic...

  12. Suppression of excited-state effects in lattice determination of nucleon electromagnetic form factors

    von Hippel, G M; Djukanovic, D; Hua, J; Jäger, B; Junnarkar, P; Meyer, H B; Rae, T D; Wittig, H

    2014-01-01

    We study the ability of a variety of fitting techniques to extract the ground state matrix elements of the vector current from ratios of nucleon three- and two-point functions that contain contaminations from excited states. Extending our high-statistics study of nucleon form factors, we are able to demonstrate that the treatment of excited-state contributions in conjunction with approaching the physical pion mass has a significant impact on the $Q^2$-dependence of the form factors.

  13. Dual channel nitrogen laser useful for nanosecond excited state studies

    Shipman (1967) adapted the Blumlein discharge circuit to lasers and this method has proved highly useful in producing high peak pulses. The authors describe a double Blumlein producing two 250 kW pulses separated by 15 nanosecs. The dual channel nitrogen laser is designed for use in atomic spectroscopy, the first pulse excites the target atoms while the second pumps another laser whose output is used to study the levels. (U.S.)

  14. Carbazole-containing light- emitting polymers: Properties of excited states

    2003-01-01

    A series of light-emitting conjugated polymers alternatively involving carbazole and bivinylene arylene moieties in the main chain were synthesized via Wittig-Horner type copolymerization. The photoinduced charge transfer process relating to these polymers was investigated by using the technique of fluorescence spectroscopy. The interaction between excited copolymers and C60 in benzene solution was studied. The fluorescence quenching can be well described by the "sphere-of-action" mechanism. It is believed that two basic steps are involved in the quenching process, i.e. the diffusion of excitation within the conjugated polymers and the dissociation of the exctions trapped by fullerene. The radius of the sphere-of-action can be related to the excitation diffusion length, which depends on the lifetime of the exciton. The dynamic fluorescence quenching of the copolymers by another quencher, 1,4-dicyanobenzene (DCB) was also surveyed. Copolymers with different chain conformations show different temperature effects in the dynamic quenching. A planar conformation is beneficial for the quenching via bimolecular collision.

  15. Reconstruction of an excited-state molecular wave packet with attosecond transient absorption spectroscopy

    Cheng, Yan; Chini, Michael; Wang, Xiaowei; González-Castrillo, Alberto; Palacios, Alicia; Argenti, Luca; Martín, Fernando; Chang, Zenghu

    2016-08-01

    Attosecond science promises to allow new forms of quantum control in which a broadband isolated attosecond pulse excites a molecular wave packet consisting of a coherent superposition of multiple excited electronic states. This electronic excitation triggers nuclear motion on the molecular manifold of potential energy surfaces and can result in permanent rearrangement of the constituent atoms. Here, we demonstrate attosecond transient absorption spectroscopy (ATAS) as a viable probe of the electronic and nuclear dynamics initiated in excited states of a neutral molecule by a broadband vacuum ultraviolet pulse. Owing to the high spectral and temporal resolution of ATAS, we are able to reconstruct the time evolution of a vibrational wave packet within the excited B'Σ1u+ electronic state of H2 via the laser-perturbed transient absorption spectrum.

  16. Characterization of ground state entanglement by single-qubit operations and excitation energies

    Giampaolo, S M; Illuminati, F; Verrucchi, P; Giampaolo, Salvatore M.; Illuminati, Fabrizio; Siena, Silvio De; Verrucchi, Paola

    2006-01-01

    We consider single-qubit unitary operations and study the associated excitation energies above the ground state of interacting quantum spins. We prove that there exists a unique operation such that the vanishing of the corresponding excitation energy determines a necessary and sufficient condition for the separability of the ground state. We show that the energy difference associated to factorization exhibits a monotonic behavior with the one-tangle and the entropy of entanglement, including non analiticity at quantum critical points. The single-qubit excitation energy thus provides an independent, directly observable characterization of ground state entanglement, and a simple relation connecting two universal physical resources, energy and nonlocal quantum correlations.

  17. Mechanistic photodecarboxylation of pyruvic acid: Excited-state proton transfer and three-state intersection

    Photodissociation dynamics of pyruvic acid experimentally differs from that of commonly known ketones. We have employed the complete active space self-consistent field and its multi-state second-order perturbation methods to study its photodissociation mechanism in the S0, T1, and S1 states. We have uncovered four nonadiabatic photodecarboxylation paths. (i) The S1 system relaxes via an excited-state intramolecular proton transfer (ESIPT) to a hydrogen-transferred tautomer, near which an S1/S0 conical intersection funnels the S1 to S0 state. Then, some trajectories continue completing the decarboxylation reaction in the S0 state; the remaining trajectories via a reverse hydrogen transfer return to the S0 minimum, from which a thermal decarboxylation reaction occurs. (ii) Due to a small S1 −T1 energy gap and a large S1/T1 spin-orbit coupling, an efficient S1 → T1 intersystem crossing process happens again near this S1/S0 conical intersection. When decaying to T1 state, a direct photodecarboxylation proceeds. (iii) Prior to ESIPT, the S1 system first decays to the T1 state via an S1 → T1 intersystem crossing; then, the T1 system evolves to a hydrogen-transferred tautomer. Therefrom, an adiabatic T1 decarboxylation takes place due to a small barrier of 7.7 kcal/mol. (iv) Besides the aforementioned T1 ESIPT process, there also exists a comparable Norrish type I reaction in the T1 state, which forms the ground-state products of CH3CO and COOH. Finally, we have found that ESIPT plays an important role. It closes the S1-T1 and S1-S0 energy gaps, effecting an S1/T1/S0 three-state intersection region, and mediating nonadiabatic photodecarboxylation reactions of pyruvic acid

  18. Bound states and entanglement in the excited states of quantum spin chains

    We investigate the entanglement properties of the excited states of the spin- (1/2) Heisenberg (XXX) chain with isotropic antiferromagnetic interactions, by exploiting the Bethe ansatz solution of the model. We consider eigenstates obtained from both real and complex solutions (‘strings’) of the Bethe equations. Physically, the former are states of interacting magnons, whereas the latter contain bound states of groups of particles. We first focus on the situation with few particles in the chain. Using exact results and semiclassical arguments, we derive an upper bound SMAX for the entanglement entropy. This exhibits an intermediate behaviour between logarithmic and extensive, and it is saturated for highly-entangled states. As a function of the eigenstate energy, the entanglement entropy is organized in bands. Their number depends on the number of blocks of contiguous Bethe–Takahashi quantum numbers. In the presence of bound states a significant reduction in the entanglement entropy occurs, reflecting that a group of bound particles behaves effectively as a single particle. Interestingly, the associated entanglement spectrum shows edge-related levels. At a finite particle density, the semiclassical bound SMAX becomes inaccurate. For highly-entangled states SA∝ Lc, with Lc the chord length, signalling the crossover to extensive entanglement. Finally, we consider eigenstates containing a single pair of bound particles. No significant entanglement reduction occurs, in contrast with the few-particle case. (paper)

  19. Effects of crossed states on photoluminescence excitation spectroscopy of InAs quantum dots

    Lin Chien-Hung

    2011-01-01

    Full Text Available Abstract In this report, the influence of the intrinsic transitions between bound-to-delocalized states (crossed states or quasicontinuous density of electron-hole states on photoluminescence excitation (PLE spectra of InAs quantum dots (QDs was investigated. The InAs QDs were different in size, shape, and number of bound states. Results from the PLE spectroscopy at low temperature and under a high magnetic field (up to 14 T were compared. Our findings show that the profile of the PLE resonances associated with the bound transitions disintegrated and broadened. This was attributed to the coupling of the localized QD excited states to the crossed states and scattering of longitudinal acoustical (LA phonons. The degree of spectral linewidth broadening was larger for the excited state in smaller QDs because of the higher crossed joint density of states and scattering rate.

  20. Effect of xanthophyll composition on the chlorophyll excited state lifetime in plant leaves and isolated LHCII

    Johnson, Matthew P.; Zia, Ahmad; Horton, Peter; Ruban, Alexander V.

    2010-07-01

    Xanthophyll excited states have been implicated by transient absorption and two-photon excitation studies in playing a key role in the regulation of photosynthetic light harvesting via photoprotective energy dissipation. For any proposed quenching mechanism to be effective it must reduce the chlorophyll excited state lifetime from 2 ns to ˜0.5-0.4 ns. In the presented study the effect of xanthophyll composition on the chlorophyll excited state lifetime in Arabidopsis leaves in the light harvesting ( F m) and photoprotective (NPQ) states was determined. The data was compared to the chlorophyll excited state lifetime of native isolated LHCII and CP26 in detergent micelles with varying xanthophyll composition. It was found that although the differences in xanthophyll composition between LHC complexes from various Arabidopsis mutants were sufficient to explain the varying F m lifetime (and varying PSII efficiency), they were not of a sufficient scale to fully explain the observed differences in the NPQ lifetimes. Only when the LHC complexes were exposed to a low detergent/low pH media, a condition known to mimic the conformational state of LHCII associated with NPQ in vivo, were variations in excited state lifetime large enough to explain the differences observed in leaves. Furthermore, the data reveal that the replacement of lutein by either zeaxanthin or violaxanthin in the internal xanthophyll binding sites of LHCII and CP26 reduces the efficiency of energy dissipation in the photoprotective state in leaves and isolated complexes.

  1. $\\sigma$-SCF: A Direct Energy-targeting Method To Mean-field Excited States

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

    2016-01-01

    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 $\\Delta$-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, $\\sigma$-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 \\emph{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 $\\Delta$-scf solutions that are otherwise inaccessible by the...

  2. Ultrafast Excited State Relaxation of a Metalloporphyrin Revealed by Femtosecond X-ray Absorption Spectroscopy.

    Shelby, Megan L; Lestrange, Patrick J; Jackson, Nicholas E; Haldrup, Kristoffer; Mara, Michael W; Stickrath, Andrew B; Zhu, Diling; Lemke, Henrik T; Chollet, Matthieu; Hoffman, Brian M; Li, Xiaosong; Chen, Lin X

    2016-07-20

    Photoexcited Nickel(II) tetramesitylporphyrin (NiTMP), like many open-shell metalloporphyrins, relaxes rapidly through multiple electronic states following an initial porphyrin-based excitation, some involving metal centered electronic configuration changes that could be harnessed catalytically before excited state relaxation. While a NiTMP excited state present at 100 ps was previously identified by X-ray transient absorption (XTA) spectroscopy at a synchrotron source as a relaxed (d,d) state, the lowest energy excited state (J. Am. Chem. Soc., 2007, 129, 9616 and Chem. Sci., 2010, 1, 642), structural dynamics before thermalization were not resolved due to the ∼100 ps duration of the available X-ray probe pulse. Using the femtosecond (fs) X-ray pulses of the Linac Coherent Light Source (LCLS), the Ni center electronic configuration from the initial excited state to the relaxed (d,d) state has been obtained via ultrafast Ni K-edge XANES (X-ray absorption near edge structure) on a time scale from hundreds of femtoseconds to 100 ps. This enabled the identification of a short-lived Ni(I) species aided by time-dependent density functional theory (TDDFT) methods. Computed electronic and nuclear structure for critical excited electronic states in the relaxation pathway characterize the dependence of the complex's geometry on the electron occupation of the 3d orbitals. Calculated XANES transitions for these excited states assign a short-lived transient signal to the spectroscopic signature of the Ni(I) species, resulting from intramolecular charge transfer on a time scale that has eluded previous synchrotron studies. These combined results enable us to examine the excited state structural dynamics of NiTMP prior to thermal relaxation and to capture intermediates of potential photocatalytic significance. PMID:27286410

  3. Semiclassical hyperspherical matrix elements for helium doubly excited states

    A classical description of the two-electron atom, analogous to the quantum adiabatic hyperspherical channel approach, is presented. The classical problems, analogue to the quantum eigenvalue problem for the great angular momentum operator, and the separated dynamical systems defined by each of the other constants of the motion of the non-interacting system are solved, using the Hamiltonian-Jacobi method. Some matrix elements of the Coulomb interaction terms of the Hamilton for doubly excited helium atom using the Heisenberg correspondence principle are calculated. (author). 26 refs, 4 tabs

  4. Neutral Fermion Excitations in the Moore-Read state at \

    Moller, Gunnar; Wojs, Arkadiusz; Cooper, Nigel R.

    2010-01-01

    We present evidence supporting the weakly paired Moore-Read phase in the half-filled second Landau level, focusing on some of the qualitative features of its excitations. Based on numerical studies, we show that systems with odd particle number at the flux $N_\\phi=2N-3$ can be interpreted as a neutral fermion mode of one unpaired fermion, which is gapped. The mode is found to have two distinct minima, providing a signature that could be observed by photoluminescence. In the presence of two qu...

  5. Thermodynamical property of entanglement entropy for excited states.

    Bhattacharya, Jyotirmoy; Nozaki, Masahiro; Takayanagi, Tadashi; Ugajin, Tomonori

    2013-03-01

    We argue that the entanglement entropy for a very small subsystem obeys a property which is analogous to the first law of thermodynamics when we excite the system. In relativistic setups, its effective temperature is proportional to the inverse of the subsystem size. This provides a universal relationship between the energy and the amount of quantum information. We derive the results using holography and confirm them in two-dimensional field theories. We will also comment on an example with negative specific heat and suggest a connection between the second law of thermodynamics and the strong subadditivity of entanglement entropy. PMID:23496702

  6. Direct excitation of high-orbital-angular-momentum states of rare-gas atoms by electron impact

    Tarr, S.M.; Schiavone, J.A.; Freund, R.S.

    1980-12-01

    Narrow threshold peaks are observed in the excitation functions for high-Rydberg states of the rare-gas atoms. They are considered to be evidence for the direct excitation of high-orbital-angular-momentum (l) states.

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

    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

  8. Structural and excited-state properties of oligoacene crystals from first principles

    Rangel, Tonatiuh; Berland, Kristian; Sharifzadeh, Sahar; Brown-Altvater, Florian; Lee, Kyuho; Hyldgaard, Per; Kronik, Leeor; Neaton, Jeffrey B.

    2016-03-01

    Molecular crystals are a prototypical class of van der Waals (vdW) bound organic materials with excited-state properties relevant for optoelectronics applications. Predicting the structure and excited-state properties of molecular crystals presents a challenge for electronic structure theory, as standard approximations to density functional theory (DFT) do not capture long-range vdW dispersion interactions and do not yield excited-state properties. In this work, we use a combination of DFT including vdW forces, using both nonlocal correlation functionals and pairwise correction methods, together with many-body perturbation theory (MBPT) to study the geometry and excited states, respectively, of the entire series of oligoacene crystals, from benzene to hexacene. We find that vdW methods can predict lattice constants within 1% of the experimental measurements, on par with the previously reported accuracy of pairwise approximations for the same systems. We further find that excitation energies are sensitive to geometry, but if optimized geometries are used MBPT can yield excited-state properties within a few tenths of an eV from experiment. We elucidate trends in MBPT-computed charged and neutral excitation energies across the acene series and discuss the role of common approximations used in MBPT.

  9. Inelastic WIMP-nucleus scattering to the first excited state in $^{125}$Te

    Vergados, J D; Kortelainen, M; Pirinen, P; Srivastava, P C; Suhonen, J; Thomas, A W

    2016-01-01

    The direct detection of dark matter constituents, in particular the weakly interacting massive particles (WIMPs), is considered central to particle physics and cosmology. In this paper we study transitions to the excited states, possible in some nuclei, which have sufficiently low lying excited states. Examples considered previously were the first excited states of $^{127}$I and $^{129}$Xe and $^{83}$Kr. Here we examine $^{125}$Te, which offers some advantages and is currently being considered as a target.In all these cases the extra signature of the gamma rays following the de-excitation of these states has definite advantages over the purely nuclear recoil and, in principle, such a signature can be exploited experimentally. A brief discussion of the experimental feasibility is given in the context of the CUORE experiment.

  10. Hyperon and charmed baryon masses and nucleon excited states from lattice QCD

    Alexandrou, Constantia

    2014-01-01

    We discuss the status of current dynamical lattice QCD simulations in connection to the emerging results on the strange and charmed baryon spectrum, excited states of the nucleon and the investigation of the structure of scalar mesons.

  11. Notes on entanglement entropy for excites holographic states in 2d

    Rashkov, Radoslav C

    2016-01-01

    In this work we revisit the problem of contributions of excited holographic states to the entanglement entropy in two-dimensional conformal field theories. Using the results of replica trick method we find three expressions for these contributions. First, we express the contribution of the excited states in terms of Aharonov invariants. It is shown that beside the Schwarzian, the one-point functions of descendants of energy-momentum also contribute. Given Schwarz-Christoffel map, the contributions to any order can be easily computed. The second expression relates the entanglement entropy of excited states to Faber polynomials and Grunsky coefficients. Based on the relation of Grunsky coefficiens to tau-funcion of dispersionless Toda hierarchy, we find the third expression for contributions of excited holographic states to the entanglement entropy.

  12. Theoretical direct WIMP detection rates for inelastic scattering to excited states

    The recent WMAP and Planck data have confirmed that exotic dark matter together with the vacuum energy (cosmological constant) dominate in the flat Universe. Many extensions of the standard model provide dark matter candidates, in particular Weakly Interacting Massive Particles (WIMPs). Thus the direct dark matter detection is central to particle physics and cosmology. Most of the research on this issue has hitherto focused on the detection of the recoiling nucleus. In this paper we study transitions to the excited states, possible in some nuclei, which have sufficiently low lying excited states. Good examples are the first excited states of 127I and 129Xe. We find appreciable branching ratios for the inelastic scattering mediated by the spin cross sections. So, in principle, the extra signature of the gamma ray following the de-excitation of these states can, in principle, be exploited experimentally

  13. Dark excited states of carotenoid in light harvesting complex probing with femtosecond stimulated Raman spectroscopy

    Sakai S.

    2013-03-01

    Full Text Available Vibrational dynamics of dark excited states in carotenoids have been investigated using tunable Raman pump pulses. The S1 state has same vibrational dynamics in light-harvesting complex (LH1 and solution. The S* state in LH1 has similar vibrational modes with the triplet state of carotenoid. However, the so-called S* state in solution does not have the modes and is concluded to be different from the S* state in LH1.

  14. Excited-state absorption and radiative up-conversion in porphyrin-doped gels

    Wang, X.; Yates, L. M., III; Knobbe, Edward T.

    1994-10-01

    Optical absorption and emission behavior have been investigated in aluminosilicate sol-gel materials containing the sodium salt of tetra-4-sulfonatophenylporphyrinatocopper(II). Concentration-dependent nonlinear absorption was observed in the porphyrin-doped specimens. Up-converted optical emission from the second excited doublet band was studied, and a saturated behavior was observed as a function of incoming excitation energies. These phenomena have been attributed to excited state absorption from both doublet and quartet manifolds. Intersystem crossing and quartet-quartet absorption effects are believed to dominate the nonlinear processes, especially in the case of strong excitation. Rate equation analysis also suggests that the quartet manifold is extensively involved for intersystem relaxation and excited state absorption. Good agreement was obtained between experimental observations and the presented rate equations.

  15. Mixed symmetry states and isospin excitation in N = Z nucleus 52Fe

    2008-01-01

    The interacting boson model with isospin (IBM-3) was applied to study the band structure and electromagnetic transition properties of the low-lying states in the even-even N = Z nucleus 52Fe. The isospin excitation states with T = 0, 1 and 2 were identified, and compared with the available data. The study shows that the 2+3 state is the lowest mixed symmetry state in 52Fe. The excitation energy of the second 0+2 state with T = 0 in nucleus 52Fe was identified. The model calculations with the data show a reasonably good agreement.

  16. Multiple-Resonance Local Wave Functions for Accurate Excited States in Quantum Monte Carlo.

    Zulfikri, Habiburrahman; Amovilli, Claudio; Filippi, Claudia

    2016-03-01

    We introduce a novel class of local multideterminant Jastrow-Slater wave functions for the efficient and accurate treatment of excited states in quantum Monte Carlo. The wave function is expanded as a linear combination of excitations built from multiple sets of localized orbitals that correspond to the bonding patterns of the different Lewis resonance structures of the molecule. We capitalize on the concept of orbital domains of local coupled-cluster methods, which is here applied to the active space to select the orbitals to correlate and construct the important transitions. The excitations are further grouped into classes, which are ordered in importance and can be systematically included in the Jastrow-Slater wave function to ensure a balanced description of all states of interest. We assess the performance of the proposed wave function in the calculation of vertical excitation energies and excited-state geometry optimization of retinal models whose π → π* state has a strong intramolecular charge-transfer character. We find that our multiresonance wave functions recover the reference values of the total energies of the ground and excited states with only a small number of excitations and that the same expansion can be flexibly used at very different geometries. Furthermore, significant computational saving can also be gained in the orbital optimization step by selectively mixing occupied and virtual orbitals based on spatial considerations without loss of accuracy on the excitation energy. Our multiresonance wave functions are therefore compact, accurate, and very promising for the calculation of multiple excited states of different character in large molecules. PMID:26761421

  17. Counting the number of excited states in organic semiconductor systems using topology

    Catanzaro, Michael J. [Department of Mathematics, Wayne State University, 656 W. Kirby, Detroit, Michigan 48202 (United States); Shi, Tian [Department of Chemistry, Wayne State University, 5101 Cass Ave., Detroit, Michigan 48202 (United States); Tretiak, Sergei, E-mail: serg@lanl.gov [Theoretical Division, Center for Nonlinear Studies, and Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, New Mexico 87545 (United States); Chernyak, Vladimir Y., E-mail: chernyak@chem.wayne.edu [Department of Mathematics, Wayne State University, 656 W. Kirby, Detroit, Michigan 48202 (United States); Department of Chemistry, Wayne State University, 5101 Cass Ave., Detroit, Michigan 48202 (United States)

    2015-02-28

    Exciton scattering theory attributes excited electronic states to standing waves in quasi-one-dimensional molecular materials by assuming a quasi-particle picture of optical excitations. The quasi-particle properties at branching centers are described by the corresponding scattering matrices. Here, we identify the topological invariant of a scattering center, referred to as its winding number, and apply topological intersection theory to count the number of quantum states in a quasi-one-dimensional system.

  18. Distribution of populations in excited states of electrodeless discharge lamp of Rb atoms

    TAO ZhiMing; WANG YanFei; HONG YeLong; WANG DongYing; ZHANG ShengNan; ZHUANG Wei; CHEN JingBiao

    2013-01-01

    The intensity of fluorescence spectral lines of Rb atoms in the region of 350-1110 nm is measured in eletrodeless discharge lamp.The population ratio between the excited states is calculated according to the spontaneous transition probabilities with rate equations.At the same time,the population density of energy level is also obtained.The results provide the potential applications of electrodeless discharge lamp in atomic filter and optical frequency reference at higher excited states without a pumping laser.

  19. Sum rule analysis of vector and axial-vector spectral functions with excited states in vacuum

    Hohler, Paul M.; Rapp, Ralf

    2012-01-01

    We simultaneously analyze vector and axial-vector spectral functions in vacuum using hadronic models constrained by experimental data and the requirement that Weinberg-type sum rules are satisfied. Upon explicit inclusion of an excited vector state, viz. rho', and the requirement that the perturbative continua are degenerate in vector and axial-vector channels, we deduce the existence of an excited axial-vector resonance state, a1', in order that the Weinberg sum rules are satisfied. The resu...

  20. Relativistic Hartree-Fock-Bogoliubov theory: ground states and excitations

    Long, Wen Hui; Meng, Jie; Giai, Nguyen Van

    The covariant density functional (CDF) theory with the Fock diagrams, the indivisible part of the effective nuclear interaction, is introduced, including both the relativistic Hartree-Fock and its extension -- the relativistic Hartree-Fock-Bogoliubov methods. The specific roles played by Fock diagrams, particularly for the new degrees of freedom associated with the π and ρ-tensor fields and the non-local mean fields, are discussed in determining the nuclear energy functional, the shell structure and the evolution, and nuclear isospin excitations. The existing problems and limits of the CDF theory with Fock terms are also discussed, and the perspective on a new algorithm of dealing with the non-local Fock terms is given.

  1. First observation of excited states in 108Sb

    A spectroscopic study of 108Sb has been carried out as a part of a larger experiment where in total twenty-nine different residual nuclei were identified. This study gives the first information on excited levels in this nucleus. A low-lying two-quasi-particle multiplet together with some of the higher lying levels are discussed within the framework of the nuclear shell model. A rotational, strongly coupled, band is identified as, most likely, being built on the deformed πg9/2-1xνh11/2 configuration in accordance with total routhian surface calculations. Tentative spins and parities are presented as well as B(M1)/B(E2) ratios for some of the transitions in the strongly coupled band. ((orig.))

  2. Steady-state photoluminescent excitation characterization of semiconductor carrier recombination

    Photoluminescence excitation spectroscopy is a contactless characterization technique that can provide valuable information about the surface and bulk recombination parameters of a semiconductor device, distinct from other sorts of photoluminescent measurements. For this technique, a temperature-tuned light emitting diode (LED) has several advantages over other light sources. The large radiation density offered by LEDs from near-infrared to ultraviolet region at a low cost enables efficient and fast photoluminescence measurements. A simple and inexpensive LED-based setup facilitates measurement of surface recombination velocity and bulk Shockley-Read-Hall lifetime, which are key parameters to assess device performance. Under the right conditions, this technique can also provide a contactless way to measure the external quantum efficiency of a solar cell

  3. High-energy excited states in {sup 98}Cd

    Braun, Norbert; Blazhev, Andrey; Jolie, Jan [Institut fuer Kernphysik, Universitaet Koeln (Germany); Boutachkov, Plamen; Gorska, Magda; Grawe, Hubert; Pietri, Stephane [GSI, Darmstadt (Germany); Brock, Tim; Nara Singh, B.S.; Wadsworth, Robert [Department of Physics, University of York, York (United Kingdom); Liu, Zhong [University of Edinburgh, Edinburgh (United Kingdom)

    2009-07-01

    Studies of isomerism in the proton-rich N {approx_equal}Z nuclei around {sup 100}Sn give important insights into the role of proton-neutron pairing and also serve as testing grounds for nuclear models. In summer 2008, an experiment on {sup 96,97,98}Cd was performed using the FRS fragment separator and the RISING germanium array at GSI. These exotic nuclei of interest were produced using fragmentation of a 850 MeV/u {sup 124}Xe beam on a 4 g/cm{sup 2} {sup 9}Be target and finally implanted into an active stopper consisting of 9 double-sided silicon strip detectors. In {sup 98}Cd, a new high-energy isomeric transition was identified. Preliminary results on {sup 98}Cd are presented and their implications for the high-excitation level scheme are discussed.

  4. Steady-state photoluminescent excitation characterization of semiconductor carrier recombination

    Bhosale, J. S.; Moore, J. E.; Wang, X.; Bermel, P.; Lundstrom, M. S.

    2016-01-01

    Photoluminescence excitation spectroscopy is a contactless characterization technique that can provide valuable information about the surface and bulk recombination parameters of a semiconductor device, distinct from other sorts of photoluminescent measurements. For this technique, a temperature-tuned light emitting diode (LED) has several advantages over other light sources. The large radiation density offered by LEDs from near-infrared to ultraviolet region at a low cost enables efficient and fast photoluminescence measurements. A simple and inexpensive LED-based setup facilitates measurement of surface recombination velocity and bulk Shockley-Read-Hall lifetime, which are key parameters to assess device performance. Under the right conditions, this technique can also provide a contactless way to measure the external quantum efficiency of a solar cell.

  5. A theoretical study of electronic excited states of photosynthetic reaction center in Rhodopseudomonas viridis

    2006-01-01

    The electronic singlet vertical excited states of photosynthetic reaction center (PSRC) in Rhodopseudomonas (Rps.) viridis were investigated by ZINDO and INDO/S methods. The effects of the interactions of pigment-pigment and pigment-protein on the electronic excitations were examined. The calculation results showed that the interactions of pigment-pigment and pigment-protein play an important role in reasonably assigning the experimental absorption and circular dichroism (CD) spectra of PSRC in Rps. virids. By comparing the theoretically computed excited states with the experimental absorption and CD spectra, satisfactory assignments of the experimental spectroscopic peaks were achieved.

  6. Non-orthogonal configuration interaction for the calculation of multielectron excited states

    Sundstrom, Eric J., E-mail: eric.jon.sundstrom@berkeley.edu; Head-Gordon, Martin [Department of Chemistry, University of California Berkeley, Berkeley, California 94720, USA and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)

    2014-03-21

    We apply Non-orthogonal Configuration Interaction (NOCI) to molecular systems where multielectron excitations, in this case double excitations, play a substantial role: the linear polyenes and β-carotene. We demonstrate that NOCI when applied to systems with extended conjugation, provides a qualitatively correct wavefunction at a fraction of the cost of many other multireference treatments. We also present a new extension to this method allowing for purification of higher-order spin states by utilizing Generalized Hartree-Fock Slater determinants and the details for computing 〈S{sup 2}〉 for the ground and excited states.

  7. Excited state evolution towards ligand loss and ligand chelation at group 6 metal carbonyl centres.

    Manton, Jennifer C; Amirjalayer, Saeed; Coleman, Anthony C; McMahon, Suzanne; Harvey, Emma C; Greetham, Gregory M; Clark, Ian P; Buma, Wybren Jan; Woutersen, Sander; Pryce, Mary T; Long, Conor

    2014-12-21

    The photochemistry and photophysics of three model "half-sandwich" complexes (η(6)-benzophenone)Cr(CO)3, (η(6)-styrene)Cr(CO)3, and (η(6)-allylbenzene)Cr(CO)3 were investigated using pico-second time-resolved infrared spectroscopy and time-dependent density functional theory methods. The (η(6)-benzophenone)Cr(CO)3 complex was studied using two excitation wavelengths (470 and 320 nm) while the remaining complexes were irradiated using 400 nm light. Two independent excited states were detected spectroscopically for each complex, one an unreactive excited state of metal-to-arene charge-transfer character and the other with metal-to-carbonyl charge transfer character. This second excited state leads to an arrested release of CO on the pico-second time-scale. Low-energy excitation (470 nm) of (η(6)-benzophenone)Cr(CO)3 populated only the unreactive excited state which simply relaxes to the parent complex. Higher energy irradiation (320 nm) induced CO-loss. Irradiation of (η(6)-styrene)Cr(CO)3, or (η(6)-allylbenzene)Cr(CO)3 at 400 nm provided evidence for the simultaneous population of both the reactive and unreactive excited states. The efficiency at which the unreactive excited state is populated depends on the degree of conjugation of the substituent with the arene π-system and this affects the efficiency of the CO-loss process. The quantum yield of CO-loss is 0.50 for (η(6)-allylbenzene)Cr(CO)3 and 0.43 for (η(6)-styrene)Cr(CO)3. These studies provide evidence for the existence of two photophysical routes to CO loss, a minor ultrafast route and an arrested mechanism involving the intermediate population of a reactive excited state. This reactive excited state either relaxes to reform the parent species or eject CO. Thus the quantum yield of the CO-loss is strongly dependent on the excitation wavelength. Time-dependent density functional theory calculations confirm that the state responsible for ultrafast CO-loss has significant metal-centred character while

  8. Study on even-parity highly excited states of the Sm atom

    Zhao Yanhong; Dai Changjian; Ye Shiwei, E-mail: daicj@126.com [School of Science, Tianjin University of Technology, Tianjin 300384 (China)

    2011-10-14

    Spectra of even-parity highly excited states of the Sm atom have been systematically studied using the two-color three-step excitation and photoionization detection method. With three different excitation paths distinguished by three different intermediate states with the 4f{sup 6}6s6p configuration, the atom is resonantly excited to given highly excited states in the energy region between 30 040 and 38 065 cm{sup -1}, where it is detected by photoionization. The wavelength of the second laser is scanned from 440 to 700 nm, while that of the first laser is fixed at 638.96, 636.92 or 627.50 nm. Based on precise calibration of the wavelength, the energy levels of 198 even-parity states are determined with the relative line intensities of the related transitions. A unique value of J, the total angular momentum, is assigned to all detected states by comparing the three spectra obtained with the different excitation paths. Except that the energy levels of 113 states are confirmed in this work, the rest of the information mentioned above has not been previously reported.

  9. The structure of the ground state and low excited states of quantum fluids

    The structure of the ground state of a quantum fluid is described in terms of the pair correlation function and pair-pair correlation function, which are the response functions to first and second order scattering respectively. Results are presented for the pair-pair correlation function of liquid 4He obtained using two methods; a Monte Carlo simulation and a hypernetted chain approximation. These results are used to obtain the solution of the Euler-Lagrange equation for the optimum Jastrow function for the ground state of liquid 4He. The Monte Carlo calculation is in good agreement with the augmented HNC approximation. General properties of the pair correlation function are discussed in terms of its Fourier transform, the liquid structure function. A critical review is given of the present status of the Jastrow theory ( and its generalizations) of the ground state of boson and fermion quantum fluids. The recent extension of the Jastrow theory to include three-body factors by Pandharipande is compared to the earlier theory of Campbell along with a parallel discussion of the theories of the low excited states of the boson fluid by Feynman and Cohen and by Jackson and Feenberg. The importance fo the three-body factors to the quantitative agreement between the theoretical and experimental phonon-roton spectrum of liquid 4He is discussed. (Auth.)

  10. One Neutron Halo in a 12B Excited State

    陈宝秋; 马中玉

    2001-01-01

    The nonlinear relativistic mean field (RMF) theory with a new effective interaction NL3 has been used to inves tigate the bulk properties of the 12B nucleus. The results obtained in the RMF predict one neutron halo in a 12Bexcited state. 12B does not show the neutron halo structure if it is in its ground state.