Energies of the ground state and first excited 0 sup + state in an exactly solvable pairing model

CERN Document Server

Dinh Dang, N

2003-01-01

Several approximations are tested by calculating the ground-state energy and the energy of the first excited 0 sup + state using an exactly solvable model with two symmetric levels interacting via a pairing force. They are the BCS approximation (BCS), Lipkin-Nogami (LN) method, random-phase approximation (RPA), quasiparticle RPA (QRPA), the renormalized RPA (RRPA), and renormalized QRPA (RQRPA). It is shown that, in the strong-coupling regime, the QRPA which neglects the scattering term of the model Hamiltonian offers the best fit to the exact solutions. A recipe is proposed using the RRPA and RQRPA in combination with the pairing gap given by the LN method. Applying this recipe, it is shown that the superfluid-normal phase transition is avoided, and a reasonably good description for both of the ground-state energy and the energy of the first excited 0 sup + state is achieved. (orig.)

Application of an excited state LDA exchange energy functional for the calculation of transition energy of atoms within time-independent density functional theory

Energy Technology Data Exchange (ETDEWEB)

Shamim, Md; Harbola, Manoj K, E-mail: sami@iitk.ac.i, E-mail: mkh@iitk.ac.i [Department of Physics, Indian Institute of Technology, Kanpur 208 016 (India)

2010-11-14

Transition energies of a new class of excited states (two-gap systems) of various atoms are calculated in time-independent density functional formalism by using a recently proposed local density approximation exchange energy functional for excited states. It is shown that the excitation energies calculated with this functional compare well with those calculated with exact exchange theories.

Application of an excited state LDA exchange energy functional for the calculation of transition energy of atoms within time-independent density functional theory

International Nuclear Information System (INIS)

Shamim, Md; Harbola, Manoj K

2010-01-01

Transition energies of a new class of excited states (two-gap systems) of various atoms are calculated in time-independent density functional formalism by using a recently proposed local density approximation exchange energy functional for excited states. It is shown that the excitation energies calculated with this functional compare well with those calculated with exact exchange theories.

Collective and single-particle states at high excitation energy

International Nuclear Information System (INIS)

Van den Berg, A.M.; Van der Molen, H.K.T.; Harakeh, M.N.; Akimune, H.; Daito, I.; Fujimura, H.; Fujiwara, M.; Ihara, F.; Inomata, T.

2000-01-01

Complete text of publication follows. Damping of high-lying single-particle states was investigated by the study of proton decay from high-lying states in 91 Nb, populated by the 90 Zr(α,t) reaction with E α = 180 MeV. In addition to decay to the ground state of 90 Zr, semi-direct decay was observed to the low-lying (2 + and 3 - ) phonon states, confirming the conclusion from other experiments that these phonon states play an important role in the damping process of the single-particle states. Furthermore, the population and decay of Isobaric Analogue States of 91 Zr, which are located at an excitation energy of about 10 - 12 MeV in 91 Nb, has been studied in the same reaction. (author)

Molecular approaches to solar energy conversion: the energetic cost of charge separation from molecular-excited states.

Science.gov (United States)

Durrant, James R

2013-08-13

This review starts with a brief overview of the technological potential of molecular-based solar cell technologies. It then goes on to focus on the core scientific challenge associated with using molecular light-absorbing materials for solar energy conversion, namely the separation of short-lived, molecular-excited states into sufficiently long-lived, energetic, separated charges capable of generating an external photocurrent. Comparisons are made between different molecular-based solar cell technologies, with particular focus on the function of dye-sensitized photoelectrochemical solar cells as well as parallels with the function of photosynthetic reaction centres. The core theme of this review is that generating charge carriers with sufficient lifetime and a high quantum yield from molecular-excited states comes at a significant energetic cost-such that the energy stored in these charge-separated states is typically substantially less than the energy of the initially generated excited state. The role of this energetic loss in limiting the efficiency of solar energy conversion by such devices is emphasized, and strategies to minimize this energy loss are compared and contrasted.

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

Science.gov (United States)

Li, Chen; Lu, Jianfeng; Yang, Weitao

2015-12-14

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

How Parallel Are Excited State Potential Energy Surfaces from Time-Independent and Time-Dependent DFT? A BODIPY Dye Case Study.

Science.gov (United States)

Komoto, Keenan T; Kowalczyk, Tim

2016-10-06

To support the development and characterization of chromophores with targeted photophysical properties, excited-state electronic structure calculations should rapidly and accurately predict how derivatization of a chromophore will affect its excitation and emission energies. This paper examines whether a time-independent excited-state density functional theory (DFT) approach meets this need through a case study of BODIPY chromophore photophysics. A restricted open-shell Kohn-Sham (ROKS) treatment of the S 1 excited state of BODIPY dyes is contrasted with linear-response time-dependent density functional theory (TDDFT). Vertical excitation energies predicted by the two approaches are remarkably different due to overestimation by TDDFT and underestimation by ROKS relative to experiment. Overall, ROKS with a standard hybrid functional provides the more accurate description of the S 1 excited state of BODIPY dyes, but excitation energies computed by the two methods are strongly correlated. The two approaches also make similar predictions of shifts in the excitation energy upon functionalization of the chromophore. TDDFT and ROKS models of the S 1 potential energy surface are then examined in detail for a representative BODIPY dye through molecular dynamics sampling on both model surfaces. We identify the most significant differences in the sampled surfaces and analyze these differences along selected normal modes. Differences between ROKS and TDDFT descriptions of the S 1 potential energy surface for this BODIPY derivative highlight the continuing need for validation of widely used approximations in excited state DFT through experimental benchmarking and comparison to ab initio reference data.

Excitation of lowest electronic states of thymine by slow electrons

Science.gov (United States)

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

2013-11-01

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

Unveiling the excited state energy transfer pathways in peridinin-chlorophyll a-protein by ultrafast multi-pulse transient absorption spectroscopy.

Science.gov (United States)

Redeckas, Kipras; Voiciuk, Vladislava; Zigmantas, Donatas; Hiller, Roger G; Vengris, Mikas

2017-04-01

Time-resolved multi-pulse methods were applied to investigate the excited state dynamics, the interstate couplings, and the excited state energy transfer pathways between the light-harvesting pigments in peridinin-chlorophyll a-protein (PCP). The utilized pump-dump-probe techniques are based on perturbation of the regular PCP energy transfer pathway. The PCP complexes were initially excited with an ultrashort pulse, resonant to the S 0 →S 2 transition of the carotenoid peridinin. A portion of the peridinin-based emissive intramolecular charge transfer (ICT) state was then depopulated by applying an ultrashort NIR pulse that perturbed the interaction between S 1 and ICT states and the energy flow from the carotenoids to the chlorophylls. The presented data indicate that the peridinin S 1 and ICT states are spectrally distinct and coexist in an excited state equilibrium in the PCP complex. Moreover, numeric analysis of the experimental data asserts ICT→Chl-a as the main energy transfer pathway in the photoexcited PCP systems. Copyright © 2017 Elsevier B.V. All rights reserved.

Hardness and excitation energy

Indian Academy of Sciences (India)

It is shown that the first excitation energy can be given by the Kohn-Sham hardness (i.e. the energy difference of the ground-state lowest unoccupied and highest occupied levels) plus an extra term coming from the partial derivative of the ensemble exchange-correlation energy with respect to the weighting factor in the ...

Accurate adiabatic energy surfaces for the ground and first excited states of He2+

International Nuclear Information System (INIS)

Lee, E.P.F.

1993-01-01

Different factors affecting the accuracy of the computed energy surfaces of the ground and first excited state of He 2 + have been examined, including the choice of the one-and many-particle bases, the configurational space in the MRCI (multi-reference configuration interaction) calculations and other corrections such as the Davidson and the full counterpoise (CP) correction. From basis-variation studies, it was concluded that multi-reference direct-CI calculations (MRDCI) using CASSCF MOs and/or natural orbitals (NOs) from a smaller CISD calculation, gave results close to full CI. The computed dissociation energies, D e , for the ground and first excited state of He 2 + were 2.4670 (2.4659) eV and 17.2 (17.1) cm -1 , respectively, at the highest level [without and with CP correction for basis-set superposition errors (BSSE)] of calculation with an [11s8p3d1f] GTO contraction, in reasonably good agreement with previous calculations, and estimated correct values, where available. It is believed that the computed D e , and the energy surface for the first excited state should be reasonably accurate. However, for the ground state, the effects of multiple f functions and/or functions of higher angular momentum have not been investigated owing to limitation of the available computing resources. This is probably the only weakness is the present study. (Author)

Excitation of higher lying energy states in a rubidium DPAL

Science.gov (United States)

Wallerstein, A. J.; Perram, Glen; Rice, Christopher A.

2018-02-01

The spontaneous emission in a cw rubidium diode dumped alkali laser (DPAL) system was analyzed. The fluorescence from higher lying states decreases with additional buffer gas. The intermediate states (7S, 6P, 5D) decay more slowly with buffer gas and scale super-linearly with alkali density. A detailed kinetic model has been constructed, where the dominant mechanisms are energy pooling and single photon ionization. It also includes pumping into the non-Lorentzian wings of absorption profiles, fine structure mixing, collisional de-excitation, and Penning ionization. Effects of ionization in a high powered CW rubidium DPAL were assessed.

Kinetics studies following state-selective laser excitation

International Nuclear Information System (INIS)

Keto, J.W.

1994-04-01

The objective of this contract was the study of state-to-state, electronic energy transfer reactions relevant to the excited state chemistry observed in discharges. We studied deactivation reactions and excitation transfer in collisions of excited states of xenon and krypton atoms with Ar, Kr, Xe and chlorine. The reactant states were excited selectively in two-photon transitions using tunable u.v. and v.u.v. lasers. Excited states produced by the collision were observed by their fluorescence. Reaction rates were measured by observing the time dependent decay of signals from reactant and product channels. In addition we measured interaction potentials of the reactants by laser spectroscopy where the laser induced fluorescence or ionization is measured as a function of laser wavelength (excitation spectra) or by measuring fluorescence spectra at fixed laser frequencies with monochromators. The spectra were obtained in the form of either lineshapes or individual lines from rovibrational transitions of bound states. Our research then required several categories of experiments in order to fully understand a reaction process: 1. High resolution laser spectroscopy of bound molecules or lineshapes of colliding pairs is used to determine potential curves for reactants. 2. Direct measurements of state-to-state reaction rates were measured by studying the time dependent loss of excited reactants and the time dependent formation of products. 3. The energy selectivity of a laser can be used to excite reactants on an excited surface with controlled internuclear configurations. For free states of reactants (as exist in a gas cell) this has been termed laser assisted reactions, while for initially bound states (as chemically bound reactants or dimers formed in supersonic beams) the experiments have been termed photo-fragmentation spectroscopy

Excited states rotational effects on the behavior of excited molecules

CERN Document Server

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

Construction of Vibronic Diabatic Hamiltonian for Excited-State Electron and Energy Transfer Processes.

Science.gov (United States)

Xie, Yu; Jiang, Shengshi; Zheng, Jie; Lan, Zhenggang

2017-12-21

Photoinduced excited-state electron and energy transfer processes are crucial in biological photoharvesting systems and organic photovoltaic devices. We discuss the construction of a diabatic vibronic Hamiltonian for the proper treatment of these processes involving the projection approach acting on both electronic wave functions and vibrational modes. In the electronic part, the wave function projection approach is used to construct the diabatic Hamiltonian in which both local excited states and charge-transfer states are included on the same footing. For the vibrational degrees of freedom, the vibronic couplings in the diabatic Hamiltonian are obtained in the basis of the pseudonormal modes localized on each monomer site by applying delocalized-to-localized mode projection. This systematic approach allows us to construct the vibronic diabatic Hamiltonian in molecular aggregates.

Optical studies of multiply excited states

International Nuclear Information System (INIS)

Mannervik, S.

1989-01-01

Optical studies of multiply-excited states are reviewed with emphasis on emission spectroscopy. From optical measurements, properties such as excitation energies, lifetimes and autoionization widths can be determined with high accuracy, which constitutes a challenge for modern computational methods. This article mainly covers work on two-, three- and four-electron systems, but also sodium-like quartet systems. Furthermore, some comments are given on bound multiply-excited states in negative ions. Fine structure effects on transition wavelengths and lifetimes (autoionization) are discussed. In particular, the most recent experimental and theoretical studies of multiply-excited states are covered. Some remaining problems, which require further attention, are discussed in more detail. (orig.) With 228 refs

Extended Lagrangian Excited State Molecular Dynamics.

Science.gov (United States)

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

2018-02-13

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

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

Science.gov (United States)

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.

Electronically excited negative ion resonant states in chloroethylenes

Energy Technology Data Exchange (ETDEWEB)

Khvostenko, O.G., E-mail: khv@mail.ru; Lukin, V.G.; Tuimedov, G.M.; Khatymova, L.Z.; Kinzyabulatov, R.R.; Tseplin, E.E.

2015-02-15

Highlights: • Several novel dissociative negative ion channels were revealed in chloroethylenes. • The electronically excited resonant states were recorded in all chloroethylenes under study. • The states were assigned to the inter-shell types, but not to the core-excited Feshbach one. - Abstract: The negative ion mass spectra of the resonant electron capture by molecules of 1,1-dichloroethylene, 1,2-dichloroethylene-cis, 1,2-dichloroethylene-trans, trichloroethylene and tetrachloroethylene have been recorded in the 0–12 eV range of the captured electron energy using static magnetic sector mass spectrometer modified for operation in the resonant electron capture regime. As a result, several novel low-intensive dissociation channels were revealed in the compounds under study. Additionally, the negative ion resonant states were recorded at approximately 3–12 eV, mostly for the first time. These resonant states were assigned to the electronically excited resonances of the inter-shell type by comparing their energies with those of the parent neutral molecules triplet and singlet electronically excited states known from the energy-loss spectra obtained by previous studies.

The energy structure and decay channels of the 4p6-shell excited states in Sr

Science.gov (United States)

Kupliauskienė, A.; Kerevičius, G.; Borovik, V.; Shafranyosh, I.; Borovik, A.

2017-11-01

The ejected-electron spectra arising from the decay of the 4p{}5{{nln}}{\\prime }{l}{\\prime }{n}{\\prime\\prime }{l}{\\prime\\prime } autoionizing states in Sr atoms have been studied precisely at the incident-electron energies close to excitation and ionization thresholds of the 4{{{p}}}6 subshell. The excitation behaviors for 58 lines observed between 12 and 21 eV ejected-electron kinetic energy have been investigated. Also, the ab initio calculations of excitation energies, autoionization probabilities and electron-impact excitation cross sections of the states 4p{}5{{nln}}{\\prime }{l}{\\prime }{n}{\\prime\\prime }{l}{\\prime\\prime } (nl = 4d, 5s, 5p; {n}{\\prime }{l}{\\prime } = 4d, 5s, 5p; {n}{\\prime\\prime }{l}{\\prime\\prime } = 5s, 6s, 7s, 8s, 9s, 5p, 6p, 5d, 6d, 7d, 8d, 4f, 5g) have been performed by employing the large-scale configuration-interaction method in the basis of the solutions of Dirac-Fock-Slater equations. The obtained experimental and theoretical data have been used for the accurate identification of the 60 lines in ejected-electron spectra and the 68 lines observed earlier in photoabsorption spectra. The excitation and decay processes for 105 classified states in the 4p55s{}2{nl}, 4p54d{}2{nl} and 4p55s{{nln}}{\\prime }{l}{\\prime } configurations have been considered in detail. In particular, most of the states lying below the ionization threshold of the 4p6 subshell at 26.92 eV possess up to four decay channels with formation of Sr+ in 5s{}1/2, 4d{}3/{2,5/2} and 5p{}1/{2,3/2} states. Two-step autoionization and two-electron Auger transitions with formation of Sr2+ in the 4p6 {}1{{{S}}}0 ground state are the main decay paths for high-lying autoionizing states. The excitation threshold of the 4{{{p}}}6 subshell in Sr has been established at 20.98 ± 0.05 eV.

Nonadiabatic excited-state molecular dynamics: On-the-fly limiting of essential excited states

Energy Technology Data Exchange (ETDEWEB)

Nelson, Tammie [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Naumov, Artem [Skolkovo Institute of Science and Technology, Moscow 143026 (Russian Federation); Fernandez-Alberti, Sebastian [Universidad Nacional de Quilmes, Roque Saenz Pea 352, B1876BXD Bernal (Argentina); Tretiak, Sergei, E-mail: serg@lanl.gov [Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)

2016-12-20

The simulation of nonadiabatic dynamics in extended molecular systems involving hundreds of atoms and large densities of states is particularly challenging. Nonadiabatic coupling terms (NACTs) represent a significant numerical bottleneck in surface hopping approaches. Rather than using unreliable NACT cutting schemes, here we develop “on-the-fly” state limiting methods to eliminate states that are no longer essential for the non-radiative relaxation dynamics as a trajectory proceeds. We propose a state number criteria and an energy-based state limit. The latter is more physically relevant by requiring a user-imposed energy threshold. For this purpose, we introduce a local kinetic energy gauge by summing contributions from atoms within the spatial localization of the electronic wavefunction to define the energy available for upward hops. The proposed state limiting schemes are implemented within the nonadiabatic excited-state molecular dynamics framework to simulate photoinduced relaxation in poly-phenylene vinylene (PPV) and branched poly-phenylene ethynylene (PPE) oligomers for benchmark evaluation.

Systematics in Rydberg state excitations for ion-atom collisions

International Nuclear Information System (INIS)

Andresen, B.; Jensen, K.; Petersen, N.B.; Veje, E.

1976-01-01

Rydberg state excitations in the Ne + , Mg + -He collisions have been studied in the projectile energy range 10-75 keV by means of optical spectrometry in a search for systematic trends. The relative excitation cross sections for levels of a Rydberg term series are found to follow a general (nsup(x))sup(P) behaviour with P < approximately -3 varying with collision energy and particles, regardless of whether the excited state population results from direct excitation, single electron transfer, or double electron transfer. At higher collision energies P is approximately -3 as predicted by theory. Polarization of the emitted line radiation indicates that there is no general rule for the relative excitation of the different magnetic substates of the same level. A statistical distribution of excitation is found for levels within the same term when the fine structure splitting is small. (Auth.)

Method of producing excited states of atomic nuclei

International Nuclear Information System (INIS)

Morita, M.; Morita, R.

1976-01-01

A method is claimed of producing excited states of atomic nuclei which comprises bombarding atoms with x rays or electrons, characterized in that (1) in the atoms selected to be produced in the excited state of their nuclei, (a) the difference between the nuclear excitation energy and the difference between the binding energies of adequately selected two electron orbits is small enough to introduce the nuclear excitation by electron transition, and (b) the system of the nucleus and the electrons in the case of ionizing an orbital electron in said atoms should satisfy the spin and parity conservation laws; and (2) the energy of the bombarding x rays or electrons should be larger than the binding energy of one of the said two electron orbits which is located at shorter distance from the atomic nucleus. According to the present invention, atomic nuclei can be excited in a relatively simple manner without requiring the use of large scale apparatus, equipment and production facilities, e.g., factories. It is also possible to produce radioactive substances or separate a particular isotope with an extremely high purity from a mixture of isotopes by utilizing nuclear excitation

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

OpenAIRE

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.

Low-lying excited states by constrained DFT

Science.gov (United States)

Ramos, Pablo; Pavanello, Michele

2018-04-01

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

Ergodicity, configurational entropy and free energy in pigment solutions and plant photosystems: influence of excited state lifetime.

Science.gov (United States)

Jennings, Robert C; Zucchelli, Giuseppe

2014-01-01

We examine ergodicity and configurational entropy for a dilute pigment solution and for a suspension of plant photosystem particles in which both ground and excited state pigments are present. It is concluded that the pigment solution, due to the extreme brevity of the excited state lifetime, is non-ergodic and the configurational entropy approaches zero. Conversely, due to the rapid energy transfer among pigments, each photosystem is ergodic and the configurational entropy is positive. This decreases the free energy of the single photosystem pigment array by a small amount. On the other hand, the suspension of photosystems is non-ergodic and the configurational entropy approaches zero. The overall configurational entropy which, in principle, includes contributions from both the single excited photosystems and the suspension which contains excited photosystems, also approaches zero. Thus the configurational entropy upon photon absorption by either a pigment solution or a suspension of photosystem particles is approximately zero. Copyright © 2014 Elsevier B.V. All rights reserved.

Field-dependent molecular ionization and excitation energies: Implications for electrically insulating liquids

Directory of Open Access Journals (Sweden)

N. Davari

2014-03-01

Full Text Available The molecular ionization potential has a relatively strong electric-field dependence as compared to the excitation energies which has implications for electrical insulation since the excited states work as an energy sink emitting light in the UV/VIS region. At some threshold field, all the excited states of the molecule have vanished and the molecule is a two-state system with the ground state and the ionized state, which has been hypothesized as a possible origin of different streamer propagation modes. Constrained density-functional theory is used to calculate the field-dependent ionization potential of different types of molecules relevant for electrically insulating liquids. The low singlet-singlet excitation energies of each molecule have also been calculated using time-dependent density functional theory. It is shown that low-energy singlet-singlet excitation of the type n → π* (lone pair to unoccupied π* orbital has the ability to survive at higher fields. This type of excitation can for example be found in esters, diketones and many color dyes. For alkanes (as for example n-tridecane and cyclohexane on the other hand, all the excited states, in particular the σ → σ* excitations vanish in electric fields higher than 10 MV/cm. Further implications for the design of electrically insulating dielectric liquids based on the molecular ionization potential and excitation energies are discussed.

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

International Nuclear Information System (INIS)

Theophilou, Iris; Tassi, M.; 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 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

Impurity binding energy of lowest-excited state in (In,Ga)N–GaN spherical QD under electric field effect

International Nuclear Information System (INIS)

Ghazi, Haddou El; Jorio, Anouar; Zorkani, Izeddine

2013-01-01

External electric field effect on the lowest-excited state in wurtzite (In,Ga)N–GaN spherical quantum dot is considered. By means of a traditional Ritz variational method within the effective-mass approximation and finite potential barrier, the lowest-excited state energy with and without the presence of the impurity is investigated. The normalized binding energy under electric field effect is also performed. Our numerical results are compared with the previous theoretical findings and show a good agreement with those concerning especially the ground-state for different semiconductors materials and different QDs-shapes

Impurity binding energy of lowest-excited state in (In,Ga)N–GaN spherical QD under electric field effect

Energy Technology Data Exchange (ETDEWEB)

Ghazi, Haddou El, E-mail: hadghazi@gmail.com [LPS, Faculty of Sciences, Dhar EL Mehrez, B.P 1796 Atlas, Fez (Morocco); Special Mathematics, CPGE Kénitra (Morocco); Jorio, Anouar; Zorkani, Izeddine [LPS, Faculty of Sciences, Dhar EL Mehrez, B.P 1796 Atlas, Fez (Morocco)

2013-10-01

External electric field effect on the lowest-excited state in wurtzite (In,Ga)N–GaN spherical quantum dot is considered. By means of a traditional Ritz variational method within the effective-mass approximation and finite potential barrier, the lowest-excited state energy with and without the presence of the impurity is investigated. The normalized binding energy under electric field effect is also performed. Our numerical results are compared with the previous theoretical findings and show a good agreement with those concerning especially the ground-state for different semiconductors materials and different QDs-shapes.

Excited states 2

CERN Document Server

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

Ultrafast excited state relaxation in long-chain polyenes

International Nuclear Information System (INIS)

Antognazza, Maria Rosa; Lueer, Larry; Polli, Dario; Christensen, Ronald L.; Schrock, Richard R.; Lanzani, Guglielmo; Cerullo, Giulio

2010-01-01

Graphical abstract: Excited state dynamics of a long-chain polyene studied by femtosecond pump-probe spectroscopy. - Abstract: We present a comprehensive study, by femtosecond pump-probe spectroscopy, of excited state dynamics in a polyene that approaches the infinite chain limit. By excitation with sub-10-fs pulses resonant with the 0-0 S 0 → S 2 transition, we observe rapid loss of stimulated emission from the bright excited state S 2 , followed by population of the hot S 1 state within 150 fs. Vibrational cooling of S 1 takes place within 500 fs and is followed by decay back to S 0 with 1 ps time constant. By excitation with excess vibrational energy we also observe the ultrafast formation of a long-living absorption, that is assigned to the triplet state generated by singlet fission.

On mechanism of Ar(3p54p) states excitation in low-energy Ar-Ar collisions

International Nuclear Information System (INIS)

Kurskov, S Y; Kashuba, A S

2009-01-01

The present work is devoted to study of Ar(3p 5 4p) states excitation in binary low-energy Ar-Ar collisions. The results of the experimental investigation of excitation cross sections of Ar I 4p'[l/2] 1 , 4p'[3/2] 1 , 4p'[3/2] 2 and 4p[3/2] 2 levels in the collision energy range from threshold up to 500 eV (cm) and degree of polarization for 4s[3/2] 2 0 -4p'[l/2] 1 and 4s[3/2] 2 0 -4p[3/2] 2 transitions in this energy range are represented.

Excitation and photon decay of giant resonances excited by intermediate energy heavy ions

International Nuclear Information System (INIS)

Bertrand, F.E.; Beene, J.R.

1987-01-01

Inelastic scattering of medium energy heavy ions provides very large cross sections and peak-to-continuum ratios for excitation of giant resonances. For energies above about 50 MeV/nucleon, giant resonances are excited primarily through Coulomb excitation, which is indifferent to isospin, thus providing a good probe for the study of isovector giant resonances. The extremely large cross sections available from heavy ion excitation permit the study of rare decay modes of the giant resonances. In particular, recent measurements have been made of the photon decay of giant resonances following excitation by 22 and 84 MeV/nucleon 17 O projectiles. The singles results at 84 MeV/nucleon yield peak cross sections for the isoscalar giant quadrupole resonance and the isovector giant dipole resonance of approximately 0.8 and 3 barns/sr, respectively. Data on the ground state decay of the isoscalar giant quadrupole and isovector giant dipole resonances are presented and compared with calculations. Decays to low-lying excited states are also discussed. Preliminary results from an experiment to isolate the 208 Pb isovector quadrupole resonance using its gamma decay are presented. 22 refs., 19 figs., 1 tab

Analytical Energy Gradients for Excited-State Coupled-Cluster Methods

Science.gov (United States)

Wladyslawski, Mark; Nooijen, Marcel

The equation-of-motion coupled-cluster (EOM-CC) and similarity transformed equation-of-motion coupled-cluster (STEOM-CC) methods have been firmly established as accurate and routinely applicable extensions of single-reference coupled-cluster theory to describe electronically excited states. An overview of these methods is provided, with emphasis on the many-body similarity transform concept that is the key to a rationalization of their accuracy. The main topic of the paper is the derivation of analytical energy gradients for such non-variational electronic structure approaches, with an ultimate focus on obtaining their detailed algebraic working equations. A general theoretical framework using Lagrange's method of undetermined multipliers is presented, and the method is applied to formulate the EOM-CC and STEOM-CC gradients in abstract operator terms, following the previous work in [P.G. Szalay, Int. J. Quantum Chem. 55 (1995) 151] and [S.R. Gwaltney, R.J. Bartlett, M. Nooijen, J. Chem. Phys. 111 (1999) 58]. Moreover, the systematics of the Lagrange multiplier approach is suitable for automation by computer, enabling the derivation of the detailed derivative equations through a standardized and direct procedure. To this end, we have developed the SMART (Symbolic Manipulation and Regrouping of Tensors) package of automated symbolic algebra routines, written in the Mathematica programming language. The SMART toolkit provides the means to expand, differentiate, and simplify equations by manipulation of the detailed algebraic tensor expressions directly. The Lagrangian multiplier formulation establishes a uniform strategy to perform the automated derivation in a standardized manner: A Lagrange multiplier functional is constructed from the explicit algebraic equations that define the energy in the electronic method; the energy functional is then made fully variational with respect to all of its parameters, and the symbolic differentiations directly yield the explicit

Testing an excited-state energy density functional and the associated potential with the ionization potential theorem

International Nuclear Information System (INIS)

Hemanadhan, M; Shamim, Md; Harbola, Manoj K

2014-01-01

The modified local spin density (MLSD) functional and the related local potential for excited states is tested by employing the ionization potential theorem. The exchange functional for an excited state is constructed by splitting k-space. Since its functional derivative cannot be obtained easily, the corresponding exchange potential is given by an analogy to its ground-state counterpart. Further, to calculate the highest occupied orbital energy ϵ max accurately, the potential is corrected for its asymptotic behaviour by employing the van Leeuwen and Baerends (LB) correction to it. ϵ max so obtained is then compared with the ΔSCF ionization energy calculated using the MLSD functional with self-interaction correction for the orbitals involved in the transition. It is shown that the two match quite accurately. The match becomes even better by tuning the LB correction with respect to a parameter in it. (paper)

Embedding potentials for excited states of embedded species

International Nuclear Information System (INIS)

Wesolowski, Tomasz A.

2014-01-01

Frozen-Density-Embedding Theory (FDET) is a formalism to obtain the upper bound of the ground-state energy of the total system and the corresponding embedded wavefunction by means of Euler-Lagrange equations [T. A. Wesolowski, Phys. Rev. A 77(1), 012504 (2008)]. FDET provides the expression for the embedding potential as a functional of the electron density of the embedded species, electron density of the environment, and the field generated by other charges in the environment. Under certain conditions, FDET leads to the exact ground-state energy and density of the whole system. Following Perdew-Levy theorem on stationary states of the ground-state energy functional, the other-than-ground-state stationary states of the FDET energy functional correspond to excited states. In the present work, we analyze such use of other-than-ground-state embedded wavefunctions obtained in practical calculations, i.e., when the FDET embedding potential is approximated. Three computational approaches based on FDET, that assure self-consistent excitation energy and embedded wavefunction dealing with the issue of orthogonality of embedded wavefunctions for different states in a different manner, are proposed and discussed

Energy cascades, excited state dynamics, and photochemistry in cob(III)alamins and ferric porphyrins.

Science.gov (United States)

Rury, Aaron S; Wiley, Theodore E; Sension, Roseanne J

2015-03-17

Porphyrins and the related chlorins and corrins contain a cyclic tetrapyrrole with the ability to coordinate an active metal center and to perform a variety of functions exploiting the oxidation state, reactivity, and axial ligation of the metal center. These compounds are used in optically activated applications ranging from light harvesting and energy conversion to medical therapeutics and photodynamic therapy to molecular electronics, spintronics, optoelectronic thin films, and optomagnetics. Cobalt containing corrin rings extend the range of applications through photolytic cleavage of a unique axial carbon-cobalt bond, permitting spatiotemporal control of drug delivery. The photochemistry and photophysics of cyclic tetrapyrroles are controlled by electronic relaxation dynamics including internal conversion and intersystem crossing. Typically the electronic excitation cascades through ring centered ππ* states, ligand to metal charge transfer (LMCT) states, metal to ligand charge transfer (MLCT) states, and metal centered states. Ultrafast transient absorption spectroscopy provides a powerful tool for the investigation of the electronic state dynamics in metal containing tetrapyrroles. The UV-visible spectrum is sensitive to the oxidation state, electronic configuration, spin state, and axial ligation of the central metal atom. Ultrashort broadband white light probes spanning the range from 270 to 800 nm, combined with tunable excitation pulses, permit the detailed unravelling of the time scales involved in the electronic energy cascade. State-of-the-art theoretical calculations provide additional insight required for precise assignment of the states. In this Account, we focus on recent ultrafast transient absorption studies of ferric porphyrins and corrin containing cob(III)alamins elucidating the electronic states responsible for ultrafast energy cascades, excited state dynamics, and the resulting photoreactivity or photostability of these compounds. Iron

Exploring the vibrational fingerprint of the electronic excitation energy via molecular dynamics

International Nuclear Information System (INIS)

Deyne, Andy Van Yperen-De; Pauwels, Ewald; Ghysels, An; Waroquier, Michel; Van Speybroeck, Veronique; Hemelsoet, Karen; De Meyer, Thierry; De Clerck, Karen

2014-01-01

A Fourier-based method is presented to relate changes of the molecular structure during a molecular dynamics simulation with fluctuations in the electronic excitation energy. The method implies sampling of the ground state potential energy surface. Subsequently, the power spectrum of the velocities is compared with the power spectrum of the excitation energy computed using time-dependent density functional theory. Peaks in both spectra are compared, and motions exhibiting a linear or quadratic behavior can be distinguished. The quadratically active motions are mainly responsible for the changes in the excitation energy and hence cause shifts between the dynamic and static values of the spectral property. Moreover, information about the potential energy surface of various excited states can be obtained. The procedure is illustrated with three case studies. The first electronic excitation is explored in detail and dominant vibrational motions responsible for changes in the excitation energy are identified for ethylene, biphenyl, and hexamethylbenzene. The proposed method is also extended to other low-energy excitations. Finally, the vibrational fingerprint of the excitation energy of a more complex molecule, in particular the azo dye ethyl orange in a water environment, is analyzed

Excited states v.6

CERN Document Server

Lim, Edward C

1982-01-01

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

Excited states

CERN Document Server

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

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

KAUST Repository

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.

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

KAUST Repository

Filatov, Mikhail A.; Etzold, Fabian; Gehrig, Dominik; Laquai, Fré dé ric; Busko, Dmitri; Landfester, Katharina; Baluschev, Stanislav

2015-01-01

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.

Computing correct truncated excited state wavefunctions

Science.gov (United States)

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

2016-12-01

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

Excited-State N2 Dissociation Pathway on Fe-Functionalized Au.

Science.gov (United States)

Martirez, John Mark P; Carter, Emily A

2017-03-29

Localized surface plasmon resonances (LSPRs) offer the possibility of light-activated chemical catalysis on surfaces of strongly plasmonic metal nanoparticles. This technology relies on lower-barrier bond formation and/or dissociation routes made available through energy transfer following the eventual decay of LSPRs. The coupling between these decay processes and a chemical trajectory (nuclear motion, charge-transfer, intersystem crossing, etc.) dictates the availability of these alternative (possibly lower barrier) excited-state channels. The Haber-Bosch method of NH 3 synthesis from N 2 and H 2 is notoriously energy intensive. This is due to the difficulty of N 2 dissociation despite the overall reaction being thermodynamically favorable at ambient temperatures and pressures. LSPRs may provide means to improve the kinetics of N 2 dissociation via induced resonance electronic excitation. In this work, we calculate, via embedded n-electron valence second-order perturbation theory within the density functional embedding theory, the excited-state potential energy surfaces for dissociation of N 2 on an Fe-doped Au(111) surface. This metal alloy may take advantage simultaneously of the strong LSPR of Au and the catalytic activity of Fe toward N 2 dissociation. We find the ground-state dissociation activation energy to be 4.74 eV/N 2 , with Fe as the active site on the surface. Consecutive resonance energy transfers (RETs) may be accessed due to the availability of many electronically excited states with intermediate energies arising from the metal surface that may couple to states induced by the Fe-dopant and the adsorbate molecule, and crossing between excited states may effectively lower the dissociation barrier to 1.33 eV. Our work illustrates that large energetic barriers, prohibitive toward chemical reaction, may be overcome through multiple RETs facilitating an otherwise difficult chemical process.

Excitation of nuclear states by synchrotron radiation

International Nuclear Information System (INIS)

Olariu, Albert

2003-01-01

We study the excitation of nuclear states by gamma ray beams of energy up to 200 keV produced as synchrotron radiation. We consider the possibility to populate an excited state |i> in two steps, from the ground state |g> to an intermediary state |n> which decays by gamma emission or internal conversion to a lower state |i>. The aim of this study is to establish that the probability P 2 of the two-step transition |g> → |n> → |i> should be greater than the probability P 1 of the direct transition |g> → |i>. The probabilities P 1 and P 2 correspond to a radiation pulse of duration equal to the half-time of the state |i>. We have written a computer program in C++ which computes the probability P 2 , the ratio P 2 /P 1 and the rate C 2 of the two-step transitions for any nuclei and different configurations of states. The program uses a database which contains information on the energy levels, half-lives, spins and parities of nuclear states and on the relative intensities of the nuclear transitions. If the half-lives or the relative intensities are not known the program uses the Weisskopf estimates for the transition half-lives. An interpolation program of internal conversion coefficients has also been used. We listed the values obtained for P 2 , P 2 /P 1 and C 2 in a number of cases in which P 2 is significant from the 2900 considered cases. The states |i> and |n> have the energies E i and E n , the corresponding half-lives being t i and t n . The spectral density of the synchrotron radiation has been considered to be 10 12 photons cm -2 s -1 eV -1 . We listed only the cases for which the relative intensities of the transitions from levels |n> and |i> to lower states are known. The calculations carried out in this study allowed us to identify nuclei for which P 2 has relatively great values. In the listed cases P 2 /P 1 >>1, so that the two-step excitation by synchrotron radiation is more efficient than the direct excitation |g> → |i>. For a sample having 10

Lifetime measurements of excited states in 196Pt

International Nuclear Information System (INIS)

Bolotin, H.H.; Katayama, Ichiro; Sakai, Hideyuki; Fujita, Yoshitaka; Fujiwara, Mamoru

1979-01-01

The lifetimes of six excited states in 196 Pt up to an excitation energy of 1525 keV were measured by the recoil-distance method (RDM). These levels were populated by Coulomb excitation using both 90 MeV 20 Ne and 220 MeV 58 Ni ion beams. The measured lifetimes of the 2 1 + , 4 1 + , 6 1 + , 2 2 + , 4 2 + and 0 2 + states and the B(E2) values inferred for the depopulating transitions from these levels are presented. With the exception of the 2 1 + state, the meanlives of all other levels are the first such direct experimental determinations to be reported. (author)

Excited state electron affinity calculations for aluminum

Science.gov (United States)

Hussein, Adnan Yousif

2017-08-01

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

Cathodoluminescence imaging and spectroscopy of excited states in InAs self-assembled quantum dots

International Nuclear Information System (INIS)

Khatsevich, S.; Rich, D.H.; Kim, Eui-Tae; Madhukar, A.

2005-01-01

We have examined state filling and thermal activation of carriers in buried InAs self-assembled quantum dots (SAQDs) with excitation-dependent cathodoluminescence (CL) imaging and spectroscopy. The InAs SAQDs were formed during molecular-beam epitaxial growth of InAs on undoped planar GaAs (001). The intensities of the ground- and excited-state transitions were analyzed as a function of temperature and excitation density to study the thermal activation and reemission of carriers. The thermal activation energies associated with the thermal quenching of the luminescence were measured for ground- and excited-state transitions of the SAQDs, as a function of excitation density. By comparing these activation energies with the ground- and excited-state transition energies, we have considered various processes that describe the reemission of carriers. Thermal quenching of the intensity of the QD ground- and first excited-state transitions at low excitations in the ∼230-300-K temperature range is attributed to dissociation of excitons from the QD states into the InAs wetting layer. At high excitations, much lower activation energies of the ground and excited states are obtained, suggesting that thermal reemission of single holes from QD states into the GaAs matrix is responsible for the observed temperature dependence of the QD luminescence in the ∼230-300-K temperature range. The dependence of the CL intensity of the ground-and first excited-state transition on excitation density was shown to be linear at all temperatures at low-excitation density. This result can be understood by considering that carriers escape and are recaptured as excitons or correlated electron-hole pairs. At sufficiently high excitations, state-filling and spatial smearing effects are observed together with a sublinear dependence of the CL intensity on excitation. Successive filling of the ground and excited states in adjacent groups of QDs that possess different size distributions is assumed to

Effect of high lying states on the ground and few low lying excited O+ energy levels of some closed-shell nuclei

International Nuclear Information System (INIS)

Ayoub, N.Y.

1980-02-01

The ground and some excited O + (J=O, T=O positive parity) energy levels of closed-shell nuclei are examined, in an oscillator basis, using matrix techniques. The effect of states outside the mixed (O+2(h/2π)ω). model space in 4 He (namely configurations at 4(h/2π)ω excitation) are taken into account by renormalization using the generalized Rayleigh-Schroedinger perturbation expressions for a mixed multi-configurational model space, where the resultant non-symmetric energy matrices are diagonalized. It is shown that the second-order renormalized O + energy spectrum is close to the corresponding energy spectrum obtained by diagonalizing the O+2+4(h/2π)ω 4 He energy matrix. The effect, on the ground state and the first few low-lying excited O + energy levels, of renormalizing certain parts of the model space energy matrix up to second order in various approximations is also studied in 4 He and 16 O. It is found that the low-lying O + energy levels in these various approximations behave similarly in both 4 He and 16 O. (author)

Lowest excited-state impurity binding energy in InGaN/GaN parabolic QWW: magnetic field effect

International Nuclear Information System (INIS)

Haddou El Ghazi; Anouar Jorio; Izeddine Zorkani

2013-01-01

In this paper, we have investigated the magnetic field effect on the lowest excited-state binding energy of hydrogenic shallow-donor impurity in wurtzite (In,Ga)N/GaN parabolic transversal-section quantum-well wire (PQWW) using the finite-difference method within the quasi-one-dimensional effective potential model. The calculations are performed within the framework of the effective mass approximation. A cylindrical QWW effective radius is taken into account to describe the lateral confinement strength. The numerical results show that: (i) the probability density is the largest on a circularity whose radius is the effective radius and (ii) the lowest excited-state binding energy is the largest when an impurity is located on this circularity while it starts to decrease as the impurity is away from the circularity. (author)

Electronic excited states and relaxation dynamics in polymer heterojunction systems

Science.gov (United States)

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

The formation and decay of triply excited He- states in e-He scattering

International Nuclear Information System (INIS)

Heideman, H.G.M.

1988-01-01

A description is given of doubly and triply excited negative-ion states and their effects on the electron impact excitation of atomic states. Mechanisms for indirect excitation of singly excited states are discussed with respect to:- negative-ion resonance, autoionisation and post-collision interaction, and excitation of an autoionising state via a negative ion resonance. A classification of doubly excited states is considered. Experimental results on the excitation of the n'S states of helium as a function of the incident electron energy are presented, along with theoretical PCI (post collision interaction) profiles in excitation functions, and an interpretation of the results. (UK)

Giant resonances on excited states

International Nuclear Information System (INIS)

Besold, W.; Reinhard, P.G.; Toepffer, C.

1984-01-01

We derive modified RPA equations for small vibrations about excited states. The temperature dependence of collective excitations is examined. The formalism is applied to the ground state and the first excited state of 90 Zr in order to confirm a hypothesis which states that not only the ground state but every excited state of a nucleus has a giant resonance built upon it. (orig.)

Excitation energies from Görling-Levy perturbation theory along the range-separated adiabatic connection

Science.gov (United States)

Rebolini, Elisa; Teale, Andrew M.; Helgaker, Trygve; Savin, Andreas; Toulouse, Julien

2018-06-01

A Görling-Levy (GL)-based perturbation theory along the range-separated adiabatic connection is assessed for the calculation of electronic excitation energies. In comparison with the Rayleigh-Schrödinger (RS)-based perturbation theory this GL-based perturbation theory keeps the ground-state density constant at each order and thus gives the correct ionisation energy at each order. Excitation energies up to first order in the perturbation have been calculated numerically for the helium and beryllium atoms and the hydrogen molecule without introducing any density-functional approximations. In comparison with the RS-based perturbation theory, the present GL-based perturbation theory gives much more accurate excitation energies for Rydberg states but similar excitation energies for valence states.

Electron impact excitation of the lowest doublet and quartet core-excited autoionizing states in Rb atoms

International Nuclear Information System (INIS)

Borovik, A; Roman, V; Zatsarinny, O; Bartschat, K

2013-01-01

Electron impact excitation of the (4p 5 5s 2 ) 2 P 3/2,1/2 and (4p 5 4d5s) 4 P 1/2,3/2,5/2 autoionizing states in rubidium atoms was studied experimentally by measuring the ejected-electron excitation functions and theoretically by employing a fully relativistic Dirac B-spline R-matrix (close-coupling) model. The experimental data were collected in an impact energy range from the respective excitation thresholds up to 50 eV with an incident electron energy resolution of 0.2 eV and an observation angle of 54.7°. Absolute values of the excitation cross sections were obtained by normalizing to the theoretical predictions. The observed near-threshold resonance structures were also analysed by comparison with theory. For the 2 P 3/2,1/2 doublet states, a detailed analysis of the R-matrix results reveals that the most intense resonances are related to odd-parity negative-ion states with dominant configurations 4p 5 5s5p 2 and 4p 5 4d5s6s. The measured excitation functions for the 2 P 1/2 and 4 P J states indicate a noticeable cascade population due to the radiative decay from high-lying autoionizing states. A comparative analysis with similar data for other alkali atoms is also presented.

DILEPTON YIELD FROM THE DECAY OF EXCITED SI-28 STATES

NARCIS (Netherlands)

BACELAR, JC; BUDA, A; BALANDA, A; KRASZNAHORKAY, A; VANDERPLOEG, H; SUJKOWSKI, Z; VANDERWOUDE, A

1994-01-01

The first dilepton yield measurements from excited nuclear states obtained with a new Positron-Electron Pair Spectroscopic Instrument (PEPSI) are reported. Nuclear states in Si-28, with an initial excitation energy E* = 50 MeV, were populated via the isospin T = 0 reaction He-4 + Mg-24 and the

Excited states of open strings from N=4 SYM

International Nuclear Information System (INIS)

Dzienkowski, Eric

2015-01-01

We continue the analysis of building open strings stretched between giant gravitons from N=4 SYM by going to second order in perturbation theory using the three-loop dilatation generator from the field theory. In the process we build a Fock-like space of states using Cuntz oscillators which can be used to access the excited open string states. We find a remarkable cancellation among the excited states that shows the ground state energy is consistent with a fully relativistic dispersion relation.

Local CC2 response method for triplet states based on Laplace transform: excitation energies and first-order properties.

Science.gov (United States)

Freundorfer, Katrin; Kats, Daniel; Korona, Tatiana; Schütz, Martin

2010-12-28

A new multistate local CC2 response method for calculating excitation energies and first-order properties of excited triplet states in extended molecular systems is presented. The Laplace transform technique is employed to partition the left/right local CC2 eigenvalue problems as well as the linear equations determining the Lagrange multipliers needed for the properties. The doubles part in the equations can then be inverted on-the-fly and only effective equations for the singles part must be solved iteratively. The local approximation presented here is adaptive and state-specific. The density-fitting method is utilized to approximate the electron-repulsion integrals. The accuracy of the new method is tested by comparison to canonical reference values for a set of 12 test molecules and 62 excited triplet states. As an illustrative application example, the lowest four triplet states of 3-(5-(5-(4-(bis(4-(hexyloxy)phenyl)amino)phenyl)thiophene-2-yl)thiophene-2-yl)-2-cyanoacrylic acid, an organic sensitizer for solar-cell applications, are computed in the present work. No triplet charge-transfer states are detected among these states. This situation contrasts with the singlet states of this molecule, where the lowest singlet state has been recently found to correspond to an excited state with a pronounced charge-transfer character having a large transition strength.

Dependence of the giant dipole strength function on excitation energy

International Nuclear Information System (INIS)

Draper, J.E.; Newton, J.O.; Sobotka, L.G.; Lindenberger, H.; Wozniak, G.J.; Moretto, L.G.; Stephens, F.S.; Diamond, R.M.; McDonald, R.J.

1982-01-01

Spectra of γ rays associated with deep-inelastic products from the 1150-MeV 136 Xe+ 181 Ta reaction have been measured. The yield of 10--20-MeV γ rays initially increases rapidly with the excitation energy of the products and then more slowly for excitation energies in excess of 120 MeV. Statistical-model calculations with ground-state values of the giant dipole strength function fail to reproduce the shape of the measured γ-ray spectra. This suggests a dependence of the giant dipole strength function on excitation energy

Investigation of the Impact of Different Terms in the Second Order Hamiltonian on Excitation Energies of Valence and Rydberg States.

Science.gov (United States)

Tajti, Attila; Szalay, Péter G

2016-11-08

Describing electronically excited states of molecules accurately poses a challenging problem for theoretical methods. Popular second order techniques like Linear Response CC2 (CC2-LR), Partitioned Equation-of-Motion MBPT(2) (P-EOM-MBPT(2)), or Equation-of-Motion CCSD(2) (EOM-CCSD(2)) often produce results that are controversial and are ill-balanced with their accuracy on valence and Rydberg type states. In this study, we connect the theory of these methods and, to investigate the origin of their different behavior, establish a series of intermediate variants. The accuracy of these on excitation energies of singlet valence and Rydberg electronic states is benchmarked on a large sample against high-accuracy Linear Response CC3 references. The results reveal the role of individual terms of the second order similarity transformed Hamiltonian, and the reason for the bad performance of CC2-LR in the description of Rydberg states. We also clarify the importance of the T̂ 1 transformation employed in the CC2 procedure, which is found to be very small for vertical excitation energies.

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

Science.gov (United States)

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

Examination of excited state populations in sputtering using Multiphoton Resonance Ionization

International Nuclear Information System (INIS)

Kimock, F.M.; Baxter, J.P.; Pappas, D.L.; Kobrin, P.H.; Winograd, N.

1984-01-01

Multiphoton Resonance Ionization has been employed to study the populations of excited state atoms ejected from ion bombarded metal surfaces. Preliminary investigations have focused on three model systems: aluminum, indium and cobalt. In this paper the authors examine the effect of primary ion energy (2 to 12 keV Ar + ) on excited state yields for these three systems. The influence of the sample matrix on excited state populations of sputtered atoms is also discussed

Hybrid lead halide perovskites for light energy conversion: Excited state properties and photovoltaic applications

Science.gov (United States)

Manser, Joseph S.

travel 220 nm over the course of 2 ns after photoexcitation, with an extrapolated diffusion length greater than one micrometer over the full excited state lifetime. The solution-processability of metal halide perovskites necessarily raises questions as to the properties of the solvated precursors and their connection to the final solid-state perovskite phase. Through structural and steady-state and time-resolved absorption studies, the important link between the excited state properties of the precursor components, composed of solvated and solid-state halometallate complexes, and CH3NH3PbI3 is evinced. This connection provides insight into optical nonlinearities and electronic properties of the perovskite phase. Fundamental studies of CH 3NH3PbI3 ultimately serve as a foundation for application of this and other related materials in high-performance devices. In the final chapter, the operation of CH3NH3PbI 3 solar cells in a tandem architecture is presented. The quest for economic, large scale hydrogen production has motivated the search for new materials and device designs capable of splitting water using only energy from the sun. In light of this, we introduce an all solution-processed tandem water splitting assembly composed of a BiVO4 photoanode and a single-junction CH3NH3PbI3 hybrid perovskite solar cell. This unique configuration allows efficient solar photon management, with the metal oxide photoanode selectively harvesting high energy visible photons and the underlying perovskite solar cell capturing lower energy visible-near IR wavelengths in a single-pass excitation. Operating without external bias under standard terrestrial one sun illumination, the photoanode-photovoltaic architecture, in conjunction with an earthabundant cobalt phosphate catalyst, exhibits a solar-to-hydrogen conversion efficiency of 2.5% at neutral pH. The design of low-cost tandem water splitting assemblies employing single-junction hybrid perovskite materials establishes a potentially

Photoinduced Ultrafast Intramolecular Excited-State Energy Transfer in the Silylene-Bridged Biphenyl and Stilbene (SBS) System: A Nonadiabatic Dynamics Point of View.

Science.gov (United States)

Wang, Jun; Huang, Jing; Du, Likai; Lan, Zhenggang

2015-07-09

The photoinduced intramolecular excited-state energy-transfer (EET) process in conjugated polymers has received a great deal of research interest because of its important role in the light harvesting and energy transport of organic photovoltaic materials in photoelectric devices. In this work, the silylene-bridged biphenyl and stilbene (SBS) system was chosen as a simplified model system to obtain physical insight into the photoinduced intramolecular energy transfer between the different building units of the SBS copolymer. In the SBS system, the vinylbiphenyl and vinylstilbene moieties serve as the donor (D) unit and the acceptor (A) unit, respectively. The ultrafast excited-state dynamics of the SBS system was investigated from the point of view of nonadiabatic dynamics with the surface-hopping method at the TDDFT level. The first two excited states (S1 and S2) are characterized by local excitations at the acceptor (vinylstilbene) and donor (vinylbiphenyl) units, respectively. Ultrafast S2-S1 decay is responsible for the intramolecular D-A excitonic energy transfer. The geometric distortion of the D moiety play an essential role in this EET process, whereas the A moiety remains unchanged during the nonadiabatic dynamics simulation. The present work provides a direct dynamical approach to understand the ultrafast intramolecular energy-transfer dynamics in SBS copolymers and other similar organic photovoltaic copolymers.

Charge transfer in low-energy collisions of H with He+ and H+ with He in excited states

Science.gov (United States)

Loreau, J.; Ryabchenko, S.; Muñoz Burgos, J. M.; Vaeck, N.

2018-04-01

The charge transfer process in collisions of excited (n = 2, 3) hydrogen atoms with He+ and in collisions of excited helium atoms with H+ is studied theoretically. A combination of a fully quantum-mechanical method and a semi-classical approach is employed to calculate the charge-exchange cross sections at collision energies from 0.1 eV u‑1 up to 1 keV u‑1. These methods are based on accurate ab initio potential energy curves and non-adiabatic couplings for the molecular ion HeH+. Charge transfer can occur either in singlet or in triplet states, and the differences between the singlet and triplet spin manifolds are discussed. The dependence of the cross section on the quantum numbers n and l of the initial state is demonstrated. The isotope effect on the charge transfer cross sections, arising at low collision energy when H is substituted by D or T, is investigated. Rate coefficients are calculated for all isotopes up to 106 K. Finally, the impact of the present calculations on models of laboratory plasmas is discussed.

Optogalvanic monitoring of collisional transfer of laser excitation energy in a neon RF plasma

International Nuclear Information System (INIS)

Armstrong, T.D.

1994-01-01

The optogalvanic signals produced by pulsed laser excitation of 1s5--2p8 and 1s5-2p9 (Paschen notation) transition by a ∼29 MHz radiofrequency (rf) discharge at ∼5 torr have been investigated. The optogalvanic signal produced by 1s5-2p9 excitations indicates that there is transfer of energy from the 2p9 state to some other state. The state to which this energy is transferred is believed to be mainly the 2p8 state because of the very small energy gap between the 2p9 and 2p8 states. To verify this transfer, the 1s5-2p8 transition was investigated. The similarity of the temporal profiles of the optogalvanic signals in both excitations confirms the collisional transfer of laser excitation energy from 2p9 to 2p8

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

International Nuclear Information System (INIS)

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

1994-01-01

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

JANUS - A setup for low-energy Coulomb excitation at ReA3

Science.gov (United States)

Lunderberg, E.; Belarge, J.; Bender, P. C.; Bucher, B.; Cline, D.; Elman, B.; Gade, A.; Liddick, S. N.; Longfellow, B.; Prokop, C.; Weisshaar, D.; Wu, C. Y.

2018-03-01

A new experimental setup for low-energy Coulomb excitation experiments was constructed in a collaboration between the National Superconducting Cyclotron Laboratory (NSCL), Lawrence Livermore National Laboratory (LLNL), and the University of Rochester and was commissioned at the general purpose beam line of NSCL's ReA3 reaccelerator facility. The so-called JANUS setup combines γ-ray detection with the Segmented Ge Array (SeGA) and scattered particle detection using a pair of segmented double-sided Si detectors (Bambino 2). The low-energy Coulomb excitation program that JANUS enables will complement intermediate-energy Coulomb excitation studies that have long been performed at NSCL by providing access to observables that quantify collectivity beyond the first excited state, including the sign and magnitude of excited-state quadrupole moments. In this work, the setup and its performance will be described based on the commissioning run that used stable 78Kr impinging onto a 1.09 mg/cm2208Pb target at a beam energy of 3.9 MeV/u.

Examination of excited state populations in sputtering using multiphoton resonance ionization

International Nuclear Information System (INIS)

Kimock, F.M.; Baxter, J.P.; Pappas, D.L.; Kobrin, P.H.; Winograd, N.

1984-01-01

Multiphoton Resonance Ionization has been employed to study the populations of excited state atoms ejected from ion bombarded metal surfaces. Preliminary investigations have focused on three model systems: aluminum, indium and cobalt. In this paper we examine the effect of primary ion energy (2 to 12 keV Ar + ) on excited state yields for these three systems. The influence of the sample matrix on excited state populations of sputtered atoms is also discussed. 8 refs., 4 figs

Trapping Dynamics in Photosystem I-Light Harvesting Complex I of Higher Plants Is Governed by the Competition Between Excited State Diffusion from Low Energy States and Photochemical Charge Separation.

Science.gov (United States)

Molotokaite, Egle; Remelli, William; Casazza, Anna Paola; Zucchelli, Giuseppe; Polli, Dario; Cerullo, Giulio; Santabarbara, Stefano

2017-10-26

The dynamics of excited state equilibration and primary photochemical trapping have been investigated in the photosystem I-light harvesting complex I isolated from spinach, by the complementary time-resolved fluorescence and transient absorption approaches. The combined analysis of the experimental data indicates that the excited state decay is described by lifetimes in the ranges of 12-16 ps, 32-36 ps, and 64-77 ps, for both detection methods, whereas faster components, having lifetimes of 550-780 fs and 4.2-5.2 ps, are resolved only by transient absorption. A unified model capable of describing both the fluorescence and the absorption dynamics has been developed. From this model it appears that the majority of excited state equilibration between the bulk of the antenna pigments and the reaction center occurs in less than 2 ps, that the primary charge separated state is populated in ∼4 ps, and that the charge stabilization by electron transfer is completed in ∼70 ps. Energy equilibration dynamics associated with the long wavelength absorbing/emitting forms harbored by the PSI external antenna are also characterized by a time mean lifetime of ∼75 ps, thus overlapping with radical pair charge stabilization reactions. Even in the presence of a kinetic bottleneck for energy equilibration, the excited state dynamics are shown to be principally trap-limited. However, direct excitation of the low energy chlorophyll forms is predicted to lengthen significantly (∼2-folds) the average trapping time.

Multi-step intramolecular excitation energy transfer in dendritic pyrene-phosphorus(V)porphyrin heptads

Energy Technology Data Exchange (ETDEWEB)

Hirakawa, Kazutaka, E-mail: hirakawa.kazutaka@shizuoka.ac.jp [Applied Chemistry and Biochemical Engineering Course, Department of Engineering, Graduate School of Integrated Science and Technology, Shizuoka University, Johoku 3-5-1, Naka-ku, Hamamatsu, Shizuoka 432-8561 (Japan); Department of Optoelectronics and Nanostructure Science, Graduate School of Science and Technology, Shizuoka University, Johoku 3-5-1, Naka-ku, Hamamatsu, Shizuoka 432-8561 (Japan); Segawa, Hiroshi [Department of Multi-Disciplinary Science - General Systems Studies, Graduate School of Arts and Sciences, The University of Tokyo, Komaba 3-8-1, Meguro-ku, Tokyo 153-8904 (Japan); Research Center for Advanced Science and Technology, The University of Tokyo, Komaba 4-6-1, Meguro-ku, Tokyo 153-8904 (Japan)

2016-11-15

Dendritic heptad molecules in which four pyrenyl groups are connected at the central phosphorus atom of the edge-porphyrins of the center-to-edge type porphyrin trimers were synthesized to investigate a multi-step excitation energy transfer. As the central energy acceptor, two types porphyrins which one was phosphorus(V)tetraphenylporphyrin (H2) and another was its derivative substituted by butoxy groups at four para-position of meso-phenyl groups (H1) were used. In the photoexcited state of the pyrene units, the excitation energy transfer to the central-porphyrin unit was observed in toluene. The excitation energy transfer is considered to be through two pathways; one is a stepwise pathway through the edge-porphyrin unit and another is a direct excitation energy transfer to the central porphyrin. The direct excitation energy transfer from pyrenes to the edge-porphyrin and central-porphyrin were observed in the case for H1. From the excited state of the edge-porphyrins, the excitation energy transfer to the central-porphyrin occurs in the H1 case. In the H2 case, the excitation energy of central-porphyrin is higher than that of H1, and the electron transfer from edge-porphyrin to the central-porphyrin become predominant process. - Highlights: • Dendritic pyrene-porphyrin heptads were synthesized. • Excitation energy transfer occurs from the pyrenyl moiety to the phosphorus(V)porphyrin. • The stepwise and direct energy transfer pathways were observed. • The quantum yields of these energy transfer pathways could be determined.

Multi-step intramolecular excitation energy transfer in dendritic pyrene-phosphorus(V)porphyrin heptads

International Nuclear Information System (INIS)

Hirakawa, Kazutaka; Segawa, Hiroshi

2016-01-01

Dendritic heptad molecules in which four pyrenyl groups are connected at the central phosphorus atom of the edge-porphyrins of the center-to-edge type porphyrin trimers were synthesized to investigate a multi-step excitation energy transfer. As the central energy acceptor, two types porphyrins which one was phosphorus(V)tetraphenylporphyrin (H2) and another was its derivative substituted by butoxy groups at four para-position of meso-phenyl groups (H1) were used. In the photoexcited state of the pyrene units, the excitation energy transfer to the central-porphyrin unit was observed in toluene. The excitation energy transfer is considered to be through two pathways; one is a stepwise pathway through the edge-porphyrin unit and another is a direct excitation energy transfer to the central porphyrin. The direct excitation energy transfer from pyrenes to the edge-porphyrin and central-porphyrin were observed in the case for H1. From the excited state of the edge-porphyrins, the excitation energy transfer to the central-porphyrin occurs in the H1 case. In the H2 case, the excitation energy of central-porphyrin is higher than that of H1, and the electron transfer from edge-porphyrin to the central-porphyrin become predominant process. - Highlights: • Dendritic pyrene-porphyrin heptads were synthesized. • Excitation energy transfer occurs from the pyrenyl moiety to the phosphorus(V)porphyrin. • The stepwise and direct energy transfer pathways were observed. • The quantum yields of these energy transfer pathways could be determined.

State-to-State Mode Specificity: Energy Sequestration and Flow Gated by Transition State.

Science.gov (United States)

Zhao, Bin; Sun, Zhigang; Guo, Hua

2015-12-23

Energy flow and sequestration at the state-to-state level are investigated for a prototypical four-atom reaction, H2 + OH → H + H2O, using a transition-state wave packet (TSWP) method. The product state distribution is found to depend strongly on the reactant vibrational excitation, indicating mode specificity at the state-to-state level. From a local-mode perspective, it is shown that the vibrational excitation of the H2O product derives from two different sources, one attributable to the energy flow along the reaction coordinate into the newly formed OH bond and the other due to the sequestration of the vibrational energy in the OH spectator moiety during the reaction. The analysis provided a unified interpretation of some seemingly contradicting experimental observations. It is further shown that the transfer of vibrational energy from the OH reactant to H2O product is gated by the transition state, accomplished coherently by multiple TSWPs with the corresponding OH vibrational excitation.

Direct conversion of graphite into diamond through electronic excited states

CERN Document Server

Nakayama, H

2003-01-01

An ab initio total energy calculation has been performed for electronic excited states in diamond and rhombohedral graphite by the full-potential linearized augmented plane wave method within the framework of the local density approximation (LDA). First, calculations for the core-excited state in diamond have been performed to show that the ab initio calculations based on the LDA describe the wavefunctions in the electronic excited states as well as in the ground state quite well. Fairly good coincidence with both experimental data and theoretical prediction has been obtained for the lattice relaxation of the core exciton state. The results of the core exciton state are compared with nitrogen-doped diamond. Next, the structural stability of rhombohedral graphite has been investigated to examine the possibility of the transition into the diamond structure through electronic excited states. While maintaining the rhombohedral symmetry, rhombohedral graphite can be spontaneously transformed to cubic diamond. Tota...

Coherent excitation-energy transfer and quantum entanglement in a dimer

International Nuclear Information System (INIS)

Liao Jieqiao; Sun, C. P.; Huang Jinfeng; Kuang Leman

2010-01-01

We study coherent energy transfer of a single excitation and quantum entanglement in a dimer, which consists of a donor and an acceptor modeled by two two-level systems. Between the donor and the acceptor, there exists a dipole-dipole interaction, which provides the physical mechanism for coherent energy transfer and entanglement generation. The donor and the acceptor couple to two independent heat baths with diagonal couplings that do not dissipate the energy of the noncoupling dimer. Special attention is paid to the effect on single-excitation energy transfer and entanglement generation of the energy detuning between the donor and the acceptor and the temperatures of the two heat baths. It is found that, the probability for single-excitation energy transfer largely depends on the energy detuning in the low temperature limit. Concretely, the positive and negative energy detunings can increase and decrease the probability at steady state, respectively. In the high temperature limit, however, the effect of the energy detuning on the probability is negligibly small. We also find that the probability is negligibly dependent on the bath temperature difference of the two heat baths. In addition, it is found that quantum entanglement can be generated in the process of coherent energy transfer. As the bath temperature increases, the generated steady-state entanglement decreases. For a given bath temperature, the steady-state entanglement decreases with the increase of the absolute value of the energy detuning.

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

Science.gov (United States)

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

2015-12-21

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

Excited-state formation as H+ and He+ ions scatter from metal surfaces

International Nuclear Information System (INIS)

Baird, W.E.; Zivitz, M.; Thomas, E.W.

1975-01-01

Impact of 10-to30KeV H + or He + ions on polycrystalline metal surfaces causes some projectiles to be backscattered in a neutral excited state. These projectiles subsequently radiatively decay, emitting Doppler-broadened spectral lines. By analysis of the spectral shape of these lines, we are able to determine the probability of radiationless deexcitation of the excited backscattered atoms. Quantitative measurements of spectral intensity indicate that less than 1% of all projectiles are backscattered in an excited state. The relative variation of total spectral line intensity with angle of projectile incidence and with projectile primary energy has been successfully predicted using a model which assumes that the probability for excited-state formation is independent of the scattered projectile's energy and direction. The variation in total spectral line intensity with target atomic number is predicted, and the sputtering and excitation of Al under He + impact is briefly examined

Cluster decay of Ba isotopes from ground state and as an excited ...

Indian Academy of Sciences (India)

otherwise, inclusion of excitation energy decreases the T1/2 values. ... penetrates the nuclear barrier and reaches scission configuration after running .... between the ground-state energy levels of the parent nuclei and the ground-state energy.

Two-electron excitation in slow ion-atom collisions: Excitation mechanisms and interferences among autoionizing states

International Nuclear Information System (INIS)

Kimura, M.; Rice Univ., Houston, TX

1990-01-01

The two-electron capture or excitation process resulting from collisions of H + and O 6+ ions with He atoms in the energy range from 0.5 keV/amu to 5 keV/amu is studied within a molecular representation. The collision dynamics for formation of doubly excited O 4+ ions and He** atoms and their (n ell, n'ell ') populations are analyzed in conjunction with electron correlations. Autoionizing states thus formed decay through the Auger process. An experimental study of an ejected electron energy spectrum shows ample structures in addition to two characteristic peaks that are identified by atomic and molecular autoionizations. These structures are attributable to various interferences among electronic states and trajectories. We examine the dominant sources of the interferences. 12 refs., 5 figs

Low-energy Coulomb excitation of neutron-rich zinc isotopes

CERN Document Server

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

2009-01-01

At the radioactive ion beam facility REX-ISOLDE, neutron-rich zinc isotopes were investigated using low-energy Coulomb excitation. These experiments have resulted in B(E2,20) values in 74-80Zn, B(E2,42) values in 74,76Zn and the determination of the energy of the first excited 2 states in 78,80Zn. The zinc isotopes were produced by high-energy proton- (A=74,76,80) and neutron- (A=78) induced fission of 238U, combined with selective laser ionization and mass separation. The isobaric beam was postaccelerated by the REX linear accelerator and Coulomb excitation was induced on a thin secondary target, which was surrounded by the MINIBALL germanium detector array. In this work, it is shown how the selective laser ionization can be used to deal with the considerable isobaric beam contamination and how a reliable normalization of the experiment can be achieved. The results for zinc isotopes and the N=50 isotones are compared to collective model predictions and state-of-the-art large-scale shell-model calculations, i...

Variational predictions of transition energies and electron affinities: He and Li ground states and Li, Be, and Mg core-excited states

International Nuclear Information System (INIS)

Fischer, C.F.

1990-01-01

Variational procedures for predicting energy differences of many-electron systems are investigated. Several different calculations for few-electron systems are considered that illustrate the problems encountered when a many-electron system is modeled as a core plus outer electrons. It is shown that sequences of increasingly more accurate calculations for outer correlation may converge yielding wrong transition energies. At the same time, accurate core-polarization calculations overestimate the binding energy, requiring a core-valence correction. For the high-spin, core-excited states of Li, it was found that outer correlation only predicted electron affinities as accurately as full-correlation studies. This observation suggested a prediction of the core-excited 4 P endash 4 S transition in Be - , based on observed 3 P 0 endash 3 P transition energies of the neutral species, predicted electron affinities including only outer correlation, and a core-valence correction, that is shown to be in good agreement with experiment. A similar calculation for Mg - predicts a wavelength of 2895.1 A for this transition

Formation and role of excited states in radiolysis - a foreword

International Nuclear Information System (INIS)

Singh, A.

1976-01-01

It is stated that the choice of contributions to the special issue of this Journal has been limited to those which bear on the details of the mechanisms of excited state formation and are likely to be useful to radiation chemists. Since more than half the energy deposited in radiolysis goes into excitation, studies on the fate of the excited species formed are very important. A brief reference is made to the subject matter of each of the fifteen contributions, and its significance to the development of the technique of radiolysis is outlined. (U.K.)

Particle hole excitations coupled to complex states in heavy-ion collisions

International Nuclear Information System (INIS)

Jolos, R.V.; Schmidt, R.

1982-01-01

The excitation of uncorrelated 1p-1h states in one nucleus due to the action of the time-dependent mean field of the other nucleus was studied earlier. No statistical assumptions or average procedures were made. Such a mechanism can be responsible for an appreciable excitation of the two nuclei during the short approach phase of the reaction (E* approximately> 100 MeV). The reversibility of the equations of motion leads to a deexcitation of the initially stored excitation energy into that of the relative motion for later times. This feedback behaviour of the internal excitation energy which results in particular to the deexcitation of high energetic 1p-1h pairs is probably not realistic due to the coupling of this states to more complex states with high density. It is studied the influence of this coupling due to the residual interaction between the nucleons on the dynamics of two colliding heavy ions

Calculation of 0-0 excitation energies of organic molecules by CIS(D) quantum chemical methods

International Nuclear Information System (INIS)

Grimme, Stefan; Izgorodina, Ekaterina I.

2004-01-01

The accuracy and reliability of the CIS(D) quantum chemical method and a spin-component scaled variant (SCS-CIS(D)) are tested for calculating 0-0 excitation energies of organic molecules. The ground and excited state geometries and the vibrational zero-point corrections are taken from (TD)DFT-B3LYP calculations. In total 32 valence excited states of different character are studied: π → π* states of polycyclic aromatic compounds/polyenes and n → π* states of carbonyl, thiocarbonyl and aza(azo)-aromatic compounds. This set is augmented by two systems of special interest, i.e., indole and the TICT state of dimethylaminbenzonitrile (DMABN). Both methods predict excitation energies that are on average higher than experiment by about 0.2 eV. The errors are found to be quite systematic (with a standard deviation of about 0.15 eV) and especially SCS-CIS(D) provides a more balanced treatment of π → π* vs. n → π* states. For the test suite of states, both methods clearly outperform the (TD)DFT-B3LYP approach. Opposed to previous conclusions about the performance of CIS(D), these methods can be recommended as reliable and efficient tools for computational studies of excited state problems in organic chemistry. In order to obtain conclusive results, however, the use of optimized excited state geometries and comparison with observables (0-0 excitation energies) are necessary

The influence of autoionizing states on the excitation of helium by electrons

International Nuclear Information System (INIS)

Ittersum, T. van

1976-01-01

The work described in this thesis deals with resonance effects in the scattering of electrons by helium at energies near the threshold of the autoionizing states (50-70 eV). The investigation is performed by studying light emission following the excitation of singly excited states. In some cases, the polarization of the radiation was also investigated. The purpose of the research was (i) to enlarge our knowledge of triply excited negative ion states, i.e. resonance states which are formed by temporary binding of the incident electron to a doubly excited (autoionizing) state of neutral helium, and (ii) to clear up the nature of some resonance structures which could not be explained in terms of negative ion resonances

Electronic properties of excited states in single InAs quantum dots

International Nuclear Information System (INIS)

Warming, Till

2009-01-01

energy of excited exciton states is accessible. From the shift of the exciton binding energy, when the hole is not in the ground state, but in the first or second excited states, conclusions on the shape of the wavefunctions can be drawn. Energy selective storage of charge carriers enables the access to few-particle binding energies of excited states also in quantum dot ensemble. The storage of charge carriers is refined to storage of defined spin states in the quantum dots. A technique for the deterministic preparation and readout is presented, what is of utmost importance for the realization of qubits for quantum computation. (orig.)

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

Science.gov (United States)

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

2018-04-01

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

First 3- excited state of 56Fe

International Nuclear Information System (INIS)

Fotiades, N.; Nelson, R. O.; Devlin, M.

2010-01-01

There is no reliable evidence for the existence of the 3.076 MeV (3 - ) level adopted in the ENSDF evaluation for 56 Fe although it has been reported in a few experiments. Previous reports of the observation of this level appear to be based on an incorrect assignment in early (e,e ' ) work. Recent neutron inelastic scattering measurements by Demidov et al. [Phys. At. Nucl. 67, 1884, (2004)] show that the assigned γ-ray decay of this state does not occur at a level consistent with known properties of inelastic scattering. In the present work the 56 Fe(n,n ' γ) reaction was used to populate excited states in 56 Fe. Neutrons in the energy range from 1 to 250 MeV were provided by the pulsed neutron source of the Los Alamos Neutron Science Center's WNR facility. Deexciting γ rays were detected with the GEANIE spectrometer, a Compton suppressed array of 26 Ge detectors. The γ-γ data obtained with GEANIE were used to establish coincidence relations between transitions. All previously reported levels up to E x =3.6 MeV excitation energy were observed except for the 3.076 MeV (3 - ) level. The 991- and 2229-keV transitions, previously reported to deexcite this level, were not observed in the γ-γ coincidence data obtained in the present experiment. The present work supports the assignment of the 4509.6 keV level as the first 3 - excited state in 56 Fe by observation of two previously known transitions deexciting this state.

Low-energy d-d excitations in MnO studied by resonant x-ray fluorescence spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Butorin, S.M.; Guo, J.; Magnuson, M. [Uppsala Univ. (Sweden)] [and others

1997-04-01

Resonant soft X-ray emission spectroscopy has been demonstrated to possess interesting abilities for studies of electronic structure in various systems, such as symmetry probing, alignment and polarization dependence, sensitivity to channel interference, etc. In the present abstract the authors focus on the feasibility of resonant soft X-ray emission to probe low energy excitations by means of resonant electronic X-ray Raman scattering. Resonant X-ray emission can be regarded as an inelastic scattering process where a system in the ground state is transferred to a low excited state via a virtual core excitation. The energy closeness to a core excitation of the exciting radiation enhances the (generally) low probability for inelastic scattering at these wavelengths. Therefore soft X-ray emission spectroscopy (in resonant electronic Raman mode) can be used to study low energy d-d excitations in transition metal systems. The involvement of the intermediate core state allows one to use the selection rules of X-ray emission, and the appearance of the elastically scattered line in the spectra provides the reference to the ground state.

Low-energy d-d excitations in MnO studied by resonant x-ray fluorescence spectroscopy

International Nuclear Information System (INIS)

Butorin, S.M.; Guo, J.; Magnuson, M.

1997-01-01

Resonant soft X-ray emission spectroscopy has been demonstrated to possess interesting abilities for studies of electronic structure in various systems, such as symmetry probing, alignment and polarization dependence, sensitivity to channel interference, etc. In the present abstract the authors focus on the feasibility of resonant soft X-ray emission to probe low energy excitations by means of resonant electronic X-ray Raman scattering. Resonant X-ray emission can be regarded as an inelastic scattering process where a system in the ground state is transferred to a low excited state via a virtual core excitation. The energy closeness to a core excitation of the exciting radiation enhances the (generally) low probability for inelastic scattering at these wavelengths. Therefore soft X-ray emission spectroscopy (in resonant electronic Raman mode) can be used to study low energy d-d excitations in transition metal systems. The involvement of the intermediate core state allows one to use the selection rules of X-ray emission, and the appearance of the elastically scattered line in the spectra provides the reference to the ground state

The Sommerfeld enhancement for dark matter with an excited state

International Nuclear Information System (INIS)

Slatyer, Tracy R.

2010-01-01

We present an analysis of the Sommerfeld enhancement to dark matter annihilation in the presence of an excited state, where the interaction inducing the enhancement is purely off-diagonal, such as in models of exciting or inelastic dark matter. We derive a simple and accurate semi-analytic approximation for the s-wave enhancement, which is valid provided the mass splitting between the ground and excited states is not too large, and discuss the cutoff of the enhancement for large mass splittings. We reproduce previously derived results in the appropriate limits, and demonstrate excellent agreement with numerical calculations of the enhancement. We show that the presence of an excited state leads to generically larger values of the Sommerfeld enhancement, larger resonances, and shifting of the resonances to lower mediator masses. Furthermore, in the presence of a mass splitting the enhancement is no longer a monotonic function of velocity: the enhancement where the kinetic energy is close to that required to excite the higher state can be up to twice as large as the enhancement at zero velocity

Sensitivity of (α,α') cross sections to excited-state quadrupole moments

International Nuclear Information System (INIS)

Baker, F.T.; Scott, A.; Ronningen, R.M.; Hamilton, J.H.; Kruse, T.H.; Suchannek, R.; Savin, W.

1977-01-01

Inelastic α particle scattering at 21 and 24 MeV has been used to estimate the electric quadrupole moment of the second 2 + state in 180 Hf. Sensitivity to the assumed quadrupole moment is due almost entirely to reorientation via the nuclear force. Results suggest that the technique may be a useful method of estimating excited state quadrupole moments, particularly for states with high excitation energies or with J greater than 2

The structure of low-lying states in ${}^{140}$Sm studied by Coulomb excitation

CERN Document Server

Klintefjord, M.; Görgen, A.; Bauer, C.; Bello Garrote, F.L.; Bönig, S.; Bounthong, B.; Damyanova, A.; Delaroche, J.P.; Fedosseev, V.; Fink, D.A.; Giacoppo, F.; Girod, M.; Hoff, P.; Imai, N.; Korten, W.; Larsen, A.C.; Libert, J.; Lutter, R.; Marsh, B.A.; Molkanov, P.L.; Naïdja, H.; Napiorkowski, P.; Nowacki, F.; Pakarinen, J.; Rapisarda, E.; Reiter, P.; Renstrøm, T.; Rothe, S.; Seliverstov, M.D.; Siebeck, B.; Siem, S.; Srebrny, J.; Stora, T.; Thöle, P.; Tornyi, T.G.; Tveten, G.M.; Van Duppen, P.; Vermeulen, M.J.; Voulot, D.; Warr, N.; Wenander, F.; De Witte, H.; Zielińska, M.

2016-05-02

The electromagnetic structure of $^{140}$Sm was studied in a low-energy Coulomb excitation experiment with a radioactive ion beam from the REX-ISOLDE facility at CERN. The $2^+$ and $4^+$ states of the ground-state band and a second $2^+$ state were populated by multi-step excitation. The analysis of the differential Coulomb excitation cross sections yielded reduced transition probabilities between all observed states and the spectroscopic quadrupole moment for the $2_1^+$ state. The experimental results are compared to large-scale shell model calculations and beyond-mean-field calculations based on the Gogny D1S interaction with a five-dimensional collective Hamiltonian formalism. Simpler geometric and algebraic models are also employed to interpret the experimental data. The results indicate that $^{140}$Sm shows considerable $\\gamma$ softness, but in contrast to earlier speculation no signs of shape coexistence at low excitation energy. This work sheds more light on the onset of deformation and collectivit...

An excited-state approach within full configuration interaction quantum Monte Carlo

International Nuclear Information System (INIS)

Blunt, N. S.; Smart, Simon D.; Booth, George H.; Alavi, Ali

2015-01-01

We present a new approach to calculate excited states with the full configuration interaction quantum Monte Carlo (FCIQMC) method. The approach uses a Gram-Schmidt procedure, instantaneously applied to the stochastically evolving distributions of walkers, to orthogonalize higher energy states against lower energy ones. It can thus be used to study several of the lowest-energy states of a system within the same symmetry. This additional step is particularly simple and computationally inexpensive, requiring only a small change to the underlying FCIQMC algorithm. No trial wave functions or partitioning of the space is needed. The approach should allow excited states to be studied for systems similar to those accessible to the ground-state method due to a comparable computational cost. As a first application, we consider the carbon dimer in basis sets up to quadruple-zeta quality and compare to existing results where available

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

Science.gov (United States)

Closser, Kristina Danielle

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

On some aspects of Coulomb excitation of nuclear rotational states

International Nuclear Information System (INIS)

Massmann, H.; Robotham, H.

1979-01-01

The Coulomb excitation of nuclear rotational states is studied with a semiclassical method using classical trajectories and the classical action in order to construct the excitation probabilities. This method allows one to consider the effect on the excitation probabilities of a weak nuclear potential. An explicit expression for the 'safe bombarding energy' that is the largest bombarding energy for which the nuclear force can be neglected, is found. Also the transfer of angular momentum to the projectile's orbit is considered. One finds that the dynamical distortion of the orbit has a measurable effect on the excitation probabilities for the case of very heavy ions. Furthermore, new dimensionless parameters measuring the dynamical distortion and the effect of the adiabaticity of the collision are introduced and discussed. (author)

Excited-state molecular photoionization dynamics

International Nuclear Information System (INIS)

Pratt, S.T.

1995-01-01

This review presents a survey of work using resonance-enhanced multiphoton ionization and double-resonance techniques to study excited-state photoionization dynamics in molecules. These techniques routinely provide detail and precision that are difficult to achieve in single-photon ionization from the ground state. The review not only emphasizes new aspects of photoionization revealed in the excited-state experiments but also shows how the excited-state techniques can provide textbook illustrations of some fundamental mechanisms in molecular photoionization dynamics. Most of the examples are confined to diatomic molecules. (author)

Excited states in biological systems

International Nuclear Information System (INIS)

Cilento, G.; Zinner, K.; Bechara, E.J.H.; Duran, N.; Baptista, R.C. de; Shimizu, Y.; Augusto, O.; Faljoni-Alario, A.; Vidigal, C.C.C.; Oliveira, O.M.M.F.; Haun, M.

1979-01-01

Some aspects of bioluminescence related to bioenergetics are discussed: 1. chemical generation of excited species, by means of two general processes: electron transference and cyclic - and linear peroxide cleavage; 2. biological systems capable of generating excited states and 3. biological functions of these states, specially the non-emissive ones (tripletes). The production and the role of non-emissive excited states in biological systems are analysed, the main purpose of the study being the search for non-emissive states. Experiences carried out in biological systems are described; results and conclusions are given. (M.A.) [pt

Differential cross sections for intermediate-energy electron scattering from α-tetrahydrofurfuryl alcohol: Excitation of electronic-states

Energy Technology Data Exchange (ETDEWEB)

Chiari, L.; Jones, D. B.; Thorn, P. A.; Pettifer, Z. [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, SA 5001 (Australia); Duque, H. V. [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, SA 5001 (Australia); Departamento de Física, Universidade Federal de Juiz de Fora, Juiz de Fora, MG (Brazil); Silva, G. B. da [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, SA 5001 (Australia); Universidade Federal de Mato Grosso, Barra do Garças, Mato Grosso (Brazil); Limão-Vieira, P. [Laboratório de Colisões Atómicas e Moleculares, CEFITEC, Departamento de Física, Faculdade de Ciências e Tecnologia, Universidade Nova de Lisboa, 2829-516 Caparica (Portugal); Duflot, D. [Laboratoire de Physique des Lasers, Atomes et Molécules, UMR CNRS 8523, Université Lille, F-59655 Villeneuve d’Ascq Cedex (France); Hubin-Franskin, M.-J.; Delwiche, J. [Départment de Chimie, Université de Liège, Institut de Chimie-Bât. B6C, B-4000 Liège 1 (Belgium); Blanco, F. [Departamento de Física Atómica, Molecular y Nuclear, Universidad Complutense de Madrid, Madrid E-28040 (Spain); García, G. [Instituto de Física Fundamental, CSIC, Madrid E-28006 (Spain); and others

2014-07-14

We report on measurements of differential cross sections (DCSs) for electron impact excitation of a series of Rydberg electronic-states in α-tetrahydrofurfuryl alcohol (THFA). The energy range of these experiments was 20–50 eV, while the scattered electron was detected in the 10°–90° angular range. There are currently no other experimental data or theoretical computations against which we can directly compare the present measured results. Nonetheless, we are able to compare our THFA DCSs with earlier cross section measurements for Rydberg-state electronic excitation for tetrahydrofuran, a similar cyclic ether, from Do et al. [J. Chem. Phys. 134, 144302 (2011)]. In addition, “rotationally averaged” elastic DCSs, calculated using our independent atom model with screened additivity rule correction approach are also reported. Those latter results give integral cross sections consistent with the optical theorem, and supercede those from the only previous study of Milosavljević et al. [Eur. Phys. J. D 40, 107 (2006)].

Photochemistry of ethylene: A multireference configuration interaction investigation of the excited-state energy surfaces

International Nuclear Information System (INIS)

Barbatti, M.; Paier, J.; Lischka, H.

2004-01-01

Multireference configuration interaction with singles and doubles (MR-CISD) calculations have been performed for the optimization of conical intersections and stationary points on the ethylene excited-state energy surfaces using recently developed methods for the computation of analytic gradients and nonadiabatic coupling terms. Basis set dependence and the effect of various choices of reference spaces for the MR-CISD calculations have been investigated. The crossing seam between the S 0 and S 1 states has been explored in detail. This seam connects all conical intersections presently known for ethylene. Major emphasis has been laid on the hydrogen-migration path. Starting in the V state of twisted-orthogonal ethylene, a barrierless path to ethylidene was found. The feasibility of ethylidene formation will be important for the explanation of the relative yield of cis and trans H 2 elimination

Excitation energy of /sup 3/B/sub 1/ state of H/sub 2/O calculated from generalized oscillator strengths

Energy Technology Data Exchange (ETDEWEB)

Klump, K N; Lassettre, E N

1975-01-01

Generalized oscillator strengths have been determined for the 7.4 eV excitation in H/sub 2/O at initial electron kinetic energies from 300 to 600 eV and squared momentum changes (of the colliding electron) to 4.5 a.u. These data are employed, in an approximate formula developed by Lassettre and Dillon, to calculate the excitation energy of the lowest /sup 3/B/sub 1/ state of H/sub 2/O. The value obtained, 7.0 eV, is in good agreement with accurate quantum chemical calculations and with experiment. The estimated uncertainty, based on errors found for CO and He, is 0.1 eV. This is a plausible estimate, not an upper bound.

Reparameterization invariance of NRQED self-energy corrections and improved theory for excited D states in hydrogenlike systems

International Nuclear Information System (INIS)

Wundt, Benedikt J.; Jentschura, Ulrich D.

2008-01-01

Canonically, the quantum electrodynamic radiative corrections in bound systems have been evaluated in photon energy regularization, i.e., using a noncovariant overlapping parameter that separates the high-energy relativistic scales of the virtual quanta from the nonrelativistic domain. Here, we calculate the higher-order corrections to the one-photon self-energy calculation with three different overlapping parameters (photon energy, photon mass and dimensional regularization) and demonstrate the reparameterization invariance of nonrelativistic quantum electrodynamics (NRQED) using this particular example. We also present new techniques for the calculation of the low-energy part of this correction, which lead to results for the Lamb shift of highly excited states that are important for high-precision spectroscopy

Reparameterization invariance of NRQED self-energy corrections and improved theory for excited D states in hydrogenlike systems

Energy Technology Data Exchange (ETDEWEB)

Wundt, Benedikt J. [Max-Planck-Institut fuer Kernphysik, Postfach 103980, 69029 Heidelberg (Germany); Jentschura, Ulrich D. [Max-Planck-Institut fuer Kernphysik, Postfach 103980, 69029 Heidelberg (Germany); Institut fuer Theoretische Physik, Philosophenweg 16, 69120 Heidelberg (Germany)], E-mail: ulrich.jentschura@mpi-hd.mpg.de

2008-01-24

Canonically, the quantum electrodynamic radiative corrections in bound systems have been evaluated in photon energy regularization, i.e., using a noncovariant overlapping parameter that separates the high-energy relativistic scales of the virtual quanta from the nonrelativistic domain. Here, we calculate the higher-order corrections to the one-photon self-energy calculation with three different overlapping parameters (photon energy, photon mass and dimensional regularization) and demonstrate the reparameterization invariance of nonrelativistic quantum electrodynamics (NRQED) using this particular example. We also present new techniques for the calculation of the low-energy part of this correction, which lead to results for the Lamb shift of highly excited states that are important for high-precision spectroscopy.

Excited state potential energy surfaces and their interactions in FeIV[double bond, length as m-dash]O active sites

Czech Academy of Sciences Publication Activity Database

Srnec, Martin; Wong, S. D.; Solomon, E. I.

2014-01-01

Roč. 43, č. 47 (2014), s. 17567-17577 ISSN 1477-9226 Institutional support: RVO:61388955 Keywords : excited state potential energy * chemical analysis * Frontier molecular orbitals Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 4.197, year: 2014

Excitation of spin-1 states in 166168170Er using bremsstrahlung

International Nuclear Information System (INIS)

Metzger, F.R.

1976-01-01

Some 40 states in 166 , 168 , 170 Er, most of them previously unknown, have been excited using bremsstrahlung with < or =4.2 MeV endpoint energy. For all but three of these levels, the angular distribution of the resonantly scattered radiation favors the assignment of spin 1. For some of the strongly excited levels, linear polarization measurements have been performed. They indicate that these levels have positive parity. The branching ratios further characterize them as K=1 excitations

Excitation spectra and wave functions of quasiparticle bound states in bilayer Rashba superconductors

Energy Technology Data Exchange (ETDEWEB)

Higashi, Yoichi, E-mail: higashiyoichi@ms.osakafu-u.ac.jp [Department of Mathematical Sciences, Osaka Prefecture University, 1-1 Gakuen-cho, Naka-ku, Sakai 599-8531 (Japan); Nagai, Yuki [CCSE, Japan Atomic Energy Agency, 178-4-4, Wakashiba, Kashiwa, Chiba 277-0871 (Japan); Yoshida, Tomohiro [Graduate School of Science and Technology, Niigata University, Niigata 950-2181 (Japan); Kato, Masaru [Department of Mathematical Sciences, Osaka Prefecture University, 1-1 Gakuen-cho, Naka-ku, Sakai 599-8531 (Japan); Yanase, Youichi [Department of Physics, Niigata University, Niigata 950-2181 (Japan)

2015-11-15

Highlights: • We focus on the pair-density wave state in bilayer Rashba superconductors. • The zero energy Bogoliubov wave functions are localized at the edge and vortex core. • We investigate the excitation spectra of edge and vortex bound states. - Abstract: We study the excitation spectra and the wave functions of quasiparticle bound states at a vortex and an edge in bilayer Rashba superconductors under a magnetic field. In particular, we focus on the quasiparticle states at the zero energy in the pair-density wave state in a topologically non-trivial phase. We numerically demonstrate that the quasiparticle wave functions with zero energy are localized at both the edge and the vortex core if the magnetic field exceeds the critical value.

Lifetime measurements of excited states in 73As

International Nuclear Information System (INIS)

Singh, K.P.; Kavakand, T.; Hajivaliei, M.

2004-01-01

The excited states of 73 As have been investigated via the 73 Ge(p, nγ) 73 As reaction with proton beam energies from 2.5–4.3 MeV. The lifetimes of the levels at 769.6, 860.5, 1177.8, 1188.7, 1274.9, 1344.1, 1557.1 and 1975.2 keV excitation energies have been measured for the first time using the Doppler shift attenuation method. The angular distributions have been used to assign the spins and the multipole mixing ratios using statistical theory for compound nuclear reactions. The ambiguity in the spin values for the various levels has been removed. The multipole mixing ratios for eight γ-transitions have been newly measured. (author)

Radiative proton capture to the first excited state of sup 29 P nucleus at subbarrier energies

Energy Technology Data Exchange (ETDEWEB)

Matulewicz, T; Dabrowska, M; Decowski, P; Kicinska-Habior, M; Sikora, B [Warsaw Univ. (Poland). Inst. Fizyki Doswiadczalnej; Toke, J [Rochester Univ., NY (USA). Nuclear Structure Research Lab.; Somorjai, E [Magyar Tudomanyos Akademia, Debrecen (Hungary). Atommag Kutato Intezete

1985-08-01

Differential cross sections at 0 deg and 90 deg measured for {sup 28}Si(p,{gamma}{sub 1}){sup 29}P reaction at proton energy range 2.3-2.9 MeV have been analyzed in terms of the direct-semidirect capture model extended by the effective potential approach. Spectroscopic factor of the first excited states of {sup 29}P nucleus was found to be 0.10+-0.05. 9 refs., 1 fig. (author).

High energy nuclear excitations

International Nuclear Information System (INIS)

Gogny, D.; Decharge, J.

1983-09-01

The main purpose of this talk is to see whether a simple description of the nuclear excitations permits one to characterize some of the high energy structures recently observed. The discussion is based on the linear response to different external fields calculated using the Random Phase Approximation. For those structure in heavy ion collisions at excitation energies above 50 MeV which cannot be explained with such a simple approach, we discuss a possible mechanism for this heavy ion scattering

Excitation of non-normal parity states by inelastic proton scattering

Energy Technology Data Exchange (ETDEWEB)

Emery, G. T. [Indiana Univ. (USA). Cyclotron Facility; Ikegami, Hidetsugu; Muraoka, Mitsuo [eds.; Osaka Univ., Suita (Japan). Research Center for Nuclear Physics

1980-01-01

This is a review of the works done at the Indiana University Cyclotron Facility. The purposes of works are to find excitations that should have especially simple particle-hole structure in proton inelastic scattering, to use the data on these excitations to try to understand the mechanism and the effective interaction for the (p, p') reaction in this energy range, and to go on to study the nuclear structure involved in less simple excitation. As an example, the single-nucleon level diagram for the region of Si-28 is presented. A high spin state was made, and its spin-parity was 6/sup -/. It was tried to interpret the data in terms of a on-step distorted-wave impulse approximation. The optical model parameters derived from the extensive and precise elastic scattering results were used. The cross sections for the excitation of the 6/sup -/ states found in various reactions were not large. The T = 1 state is mainly excited by the direct tensor interaction, while the T = 0 state gets its strength mainly from the knock-on exchange contribution of both the tensor and spin-orbit interactions. Experiments on Pb-208 and Fe-54 are being performed.

Mean excitation energies for molecular ions

DEFF Research Database (Denmark)

Jensen, Phillip W.K.; Sauer, Stephan P.A.; Oddershede, Jens

2017-01-01

The essential material constant that determines the bulk of the stopping power of high energy projectiles, the mean excitation energy, is calculated for a range of smaller molecular ions using the RPA method. It is demonstrated that the mean excitation energy of both molecules and atoms increase...

Study of the giant dipole resonance built on highly excited states in Sn and Dy nuclei

International Nuclear Information System (INIS)

Stolk, A.

1988-01-01

A study is presented of the giant dipole resonance built on highly excited states. The aim is to get more detailed information on the properties of the GDR and to use it as a tool for the investigation of nuclear structure at high excitation energy. The high energy γ-rays seen from the decay of excited state GDRs in heavy ion fusion reactions reflect the average properties of the states populated by the γ-emission. The measurements at different initial excitation energies of 114 Sn provide information on the nuclear level density near the particle separation energy at an average angular momentum of 10ℎ. The study of shape changes at very high spin in 152-156 Dy nuclei is presented. A theoretical model developed to describe fusion-evaporation reactions is presented. 149 refs.; 63 figs.; 13 tabs

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

Science.gov (United States)

Becke, Axel D.

2018-01-01

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

Statistical density of nuclear excited states

Directory of Open Access Journals (Sweden)

V. M. Kolomietz

2015-10-01

Full Text Available A semi-classical approximation is applied to the calculations of single-particle and statistical level densities in excited nuclei. Landau's conception of quasi-particles with the nucleon effective mass m* < m is used. The approach provides the correct description of the continuum contribution to the level density for realistic finite-depth potentials. It is shown that the continuum states does not affect significantly the thermodynamic calculations for sufficiently small temperatures T ≤ 1 MeV but reduce strongly the results for the excitation energy at high temperatures. By use of standard Woods - Saxon potential and nucleon effective mass m* = 0.7m the A-dependency of the statistical level density parameter K was evaluated in a good qualitative agreement with experimental data.

New ab initio adiabatic potential energy surfaces and bound state calculations for the singlet ground X˜ 1A1 and excited C˜ 1B2(21A') states of SO2

Science.gov (United States)

Kłos, Jacek; Alexander, Millard H.; Kumar, Praveen; Poirier, Bill; Jiang, Bin; Guo, Hua

2016-05-01

We report new and more accurate adiabatic potential energy surfaces (PESs) for the ground X˜ 1A1 and electronically excited C˜ 1B2(21A') states of the SO2 molecule. Ab initio points are calculated using the explicitly correlated internally contracted multi-reference configuration interaction (icMRCI-F12) method. A second less accurate PES for the ground X ˜ state is also calculated using an explicitly correlated single-reference coupled-cluster method with single, double, and non-iterative triple excitations [CCSD(T)-F12]. With these new three-dimensional PESs, we determine energies of the vibrational bound states and compare these values to existing literature data and experiment.

Probing shape coexistence in neutron-deficient $^{72}$Se via low-energy Coulomb excitation

CERN Multimedia

We propose to study the evolution of nuclear structure in neutron-­deficient $^{72}$Se by performing a low-­energy Coulomb excitation measurement. Matrix elements will be determined for low-­lying excited states allowing for a full comparison with theoretical predictions. Furthermore, the intrinsic shape of the ground state, and the second 0$^{+}$ state, will be investigated using the quadrupole sum rules method.

Investigation of transversal nuclear excitation in 208Pb at excitation energies between 6 MeV and 8 MeV using inelastic electron scattering

International Nuclear Information System (INIS)

Frey, R.W.

1978-01-01

Using high resolution inelastic electron scattering magnitic dipole and quadrupole excitations in 208 Pb were investigated in the energy range between 6 MeV and 8 MeV. The electron energy was 50 MeV and 63.5 MeV. With a mean absolute energy resolution of 33 kev. 44 excited states were found in the above energy range. The measured angular distributions were compared with DWBA-calculations using random phase approximated wave functions. (FKS)

Ultrafast excitation energy transfer from encapsulated quaterrylene to single-walled carbon nanotube

Energy Technology Data Exchange (ETDEWEB)

Koyama, Takeshi, E-mail: koyama@nuap.nagoya-u.ac.jp [Department of Applied Physics, Nagoya University, Chikusa, Nagoya 464-8603 (Japan); Tsunekawa, Takuya [Department of Applied Physics, Nagoya University, Chikusa, Nagoya 464-8603 (Japan); Saito, Takeshi [Research Center for Advanced Carbon Materials, AIST, Tsukuba, Ibaraki 305-8565 (Japan); Asaka, Koji; Saito, Yahachi [Department of Quantum Engineering, Nagoya University, Chikusa, Nagoya 464-8603 (Japan); Kishida, Hideo [Department of Applied Physics, Nagoya University, Chikusa, Nagoya 464-8603 (Japan); Nakamura, Arao [Department of Applied Physics, Nagoya University, Chikusa, Nagoya 464-8603 (Japan); Toyota Physical and Chemical Research Institute, Nagakute, Aichi 480-1192 (Japan)

2016-01-15

We investigate excitation energy transfer from an encapsulated quaterrylene molecule to a single-walled carbon nanotube by means of femtosecond pump-probe spectroscopy. The time constant of energy transfer becomes shorter with increasing average diameter of nanotube: 1.4±0.2 ps for 1.0 nm, 1.1±0.2 ps for 1.4 nm, and 0.4±0.1 ps for 1.8 nm. The observed behavior is discussed considering the distance of less than 1 nm between the molecule and the nanotube wall. - Highlights: • Dynamical properties of excited states in quaterrylene/SWNT composites were studied. • Excitation energy transfer occurs in the time range of 0.4-1.4 ps. • The transfer rate depends on the nanotube diameter, i.e. molecule-nanotube wall distance. • This dependence indicates the feature of excitation energy transfer on the nanoscale.

Excitation methods for energy dispersive analysis

International Nuclear Information System (INIS)

Jaklevic, J.M.

1976-01-01

The rapid development in recent years of energy dispersive x-ray fluorescence analysis has been based primarily on improvements in semiconductor detector x-ray spectrometers. However, the whole analysis system performance is critically dependent on the availability of optimum methods of excitation for the characteristic x rays in specimens. A number of analysis facilities based on various methods of excitation have been developed over the past few years. A discussion is given of the features of various excitation methods including charged particles, monochromatic photons, and broad-energy band photons. The effects of the excitation method on background and sensitivity are discussed from both theoretical and experimental viewpoints. Recent developments such as pulsed excitation and polarized photons are also discussed

Molecular excited states from the SCAN functional

Science.gov (United States)

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

2018-06-01

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

Energy levels of the single excited states in NaI and Na-like ions

International Nuclear Information System (INIS)

El-Sherbini, T.M.; Wahby, A.S.

1987-08-01

Energy levels of the single excited 1s 2 2s 2 2p 6 ns( 2 S), 1s 2 2s 2 2p 6 mp( 2 P), 1s 2 2s 2 2p 6 md( 2 D) and 1s 2 2s 2 2p 6 nf( 2 F); n=4-7, m=3-6 states for NaI and Na-like ions are calculated using the one configuration Hartree-Fock method. Good agreement is obtained between our results for the higher members of the NaI sequence and previous data from photo-absorption and beam foil experiments. (author). 11 refs, 3 figs, 9 tabs

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

Science.gov (United States)

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

2013-12-01

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

Triplet excited state properties in variable gap π-conjugated donor–acceptor–donor chromophores

KAUST Repository

Cekli, Seda; Winkel, Russell W.; Alarousu, Erkki; Mohammed, Omar F.; Schanze, Kirk S.

2016-01-01

A series of variable band-gap donor–acceptor–donor (DAD) chromophores capped with platinum(II) acetylide units has been synthesized and fully characterized by electrochemical and photophysical methods, with particular emphasis placed on probing triplet excited state properties. A counter-intuitive trend of increasing fluorescence quantum efficiency and lifetime with decreasing excited state energy (optical gap) is observed across the series of DAD chromophores. Careful study of the excited state dynamics, including triplet yields (as inferred from singlet oxygen sensitization), reveals that the underlying origin of the unusual trend in the fluorescence parameters is that the singlet–triplet intersystem crossing rate and yield decrease with decreasing optical gap. It is concluded that the rate of intersystem crossing decreases as the LUMO is increasingly localized on the acceptor unit in the DAD chromophore, and this result is interpreted as arising because the extent of spin–orbit coupling induced by the platinum heavy metal centers decreases as the LUMO is more localized on the acceptor. In addition to the trend in intersystem crossing, the results show that the triplet decay rates follow the Energy Gap Law correlation over a 1.8 eV range of triplet energy and 1000-fold range of triplet decay rates. Finally, femtosecond transient absorption studies for the DAD chromophores reveals a strong absorption in the near-infrared region which is attributed to the singlet excited state. This spectral band appears to be general for DAD chromophores, and may be a signature of the charge transfer (CT) singlet excited state.

Triplet excited state properties in variable gap π-conjugated donor–acceptor–donor chromophores

KAUST Repository

Cekli, Seda

2016-02-12

A series of variable band-gap donor–acceptor–donor (DAD) chromophores capped with platinum(II) acetylide units has been synthesized and fully characterized by electrochemical and photophysical methods, with particular emphasis placed on probing triplet excited state properties. A counter-intuitive trend of increasing fluorescence quantum efficiency and lifetime with decreasing excited state energy (optical gap) is observed across the series of DAD chromophores. Careful study of the excited state dynamics, including triplet yields (as inferred from singlet oxygen sensitization), reveals that the underlying origin of the unusual trend in the fluorescence parameters is that the singlet–triplet intersystem crossing rate and yield decrease with decreasing optical gap. It is concluded that the rate of intersystem crossing decreases as the LUMO is increasingly localized on the acceptor unit in the DAD chromophore, and this result is interpreted as arising because the extent of spin–orbit coupling induced by the platinum heavy metal centers decreases as the LUMO is more localized on the acceptor. In addition to the trend in intersystem crossing, the results show that the triplet decay rates follow the Energy Gap Law correlation over a 1.8 eV range of triplet energy and 1000-fold range of triplet decay rates. Finally, femtosecond transient absorption studies for the DAD chromophores reveals a strong absorption in the near-infrared region which is attributed to the singlet excited state. This spectral band appears to be general for DAD chromophores, and may be a signature of the charge transfer (CT) singlet excited state.

Spectroscopic probes of vibrationally excited molecules at chemically significant energies

Energy Technology Data Exchange (ETDEWEB)

Rizzo, T.R. [Univ. of Rochester, NY (United States)

1993-12-01

This project involves the application of multiple-resonance spectroscopic techniques for investigating energy transfer and dissociation dynamics of highly vibrationally excited molecules. Two major goals of this work are: (1) to provide information on potential energy surfaces of combustion related molecules at chemically significant energies, and (2) to test theoretical modes of unimolecular dissociation rates critically via quantum-state resolved measurements.

Proton capture to the ground and excited states in light nuclei

International Nuclear Information System (INIS)

Anghinolfi, M.; Corvisiero, P.; Guarnone, M.; Ricco, G.; Sanzone, M.; Taiuti, M.; Zucchiatti, A.

1984-01-01

Proton capture experiments, when performed with good resolution, generally provide two different kinds of physical information; the ground-state pγ/sub o/ cross section, which is related, through the detailed balance, to the inverse photonuclear γp/sub o/ reaction; the advantage of capture experiments is the definite kinematics, corresponding to monochromatic photons in γp reactions, and a more precise beam monitoring. The pγ/sub x/ cross section to the various excited states of the final nucleus; this information is typical of capture experiments, since excited nuclear targets are not available. Many laboratories performed extensive capture experiments at excitation energies up to the GDR region, but only recently few groups (Ohio, Triangle and Genova Universities) extended the investigation to energies above the GDR. In fact more severe experimental problems arise at higher energies: since the pγ differential cross sections range in this energy region between 0.1 and 1Γb/sr, while competitive reactions have two or three order of magnitude higher cross sections, the signal-to-background ratio is very low. The data analysis strongly depends on the detector line shape, scarsely known at photon energies above 20 MeV; a very accurate knowledge of the detector response function is therefore necessary

Electronic-excitation energy transfer in heterogeneous dye solutions under laser excitation

International Nuclear Information System (INIS)

Levshin, L.V.; Mukushev, B.T.; Saletskii, A.M.

1995-01-01

An experimental study has been made of electronic-excitation energy transfer (EEET) among dye molecules of different types for different exciting-fight wavelengths and temperatures. Upon selective laser excitation of the donor, the inhomogeneous broadening of molecular levels increases the probability of EEET from the donor to acceptor molecules. The efficiency of this process is directly proportional to the acceptor molecule concentration and is temperature dependent. The EEET is accompanied by the spectral migration of energy among donor molecules, which reduces the fluorescence quantum efficiency of the donor. Increasing the frequency of the exciting light decreases in the donor fluorescence quantum efficiency. An increase in the acceptor molecule concentration results in a decrease of the spectral migration of excitation in the donor molecule system. 5 refs., 5 figs

Study of ionizing collisions involving excited states in a potassium-rubidium mixture at thermal energy

International Nuclear Information System (INIS)

Djerad, M.T.

1987-01-01

This study concerns mainly ionising collisions involving excited states in a saturated mixture of K-Rb vapours, at thermal energy. The experimental method consists into continuous resonant two steps laser excitation of the atoms (n ≤ 10) and mass spectrometry of ion currents. Radiative and collisional relaxation of the atoms create a complex medium. The most efficient collisional processes are Penning ionisation and Hornbeck-Molnar ionisation. In the heteronuclear system Rb(n1) + K(4P), the following exit channels may be operative: Rb(n1) + K(4P) → Rb + + e - + K Rb(n1) + K(4p) → K + + e - + Rb Rb(n1) + K(4P) → KRb + + e - . The measurements show that the first channel has an average cross section ∼ 10 -13 cm 2 . Those of the other channels are at least three orders of magnitude smaller and thus comparatively negligible. The data obtained from 5D to 10S allow to conclude that the flux in the entrance channel ionises at large separation between Rb(n1) and K(4P). The process of ionisation is dominated by polarisation forces, exchange forces being negligible. In the present mixture, Hornbeck-Molnar ionisation leads to homonuclear molecular ions K 2 + , Rb 2 + as well as the heteronuclear one KRb + . We have measured the rate coefficients for the systems: K(n1) + Rb → KRb + + e - Rb(n1) + K → KRb + + e - . The rate coefficients increase with the excitation energy of the level n1; they do not exhibit fundamental differences with those measured in pure alkali vapours [fr

Photoionization dynamics of excited molecular states

International Nuclear Information System (INIS)

Dehmer, J.L.; O'Halloran, M.A.; Tomkins, F.S.; Dehmer, P.M.; Pratt, S.T.

1987-01-01

Resonance Enhanced Multiphoton Ionization (REMPI) utilizes tunable dye lasers to ionize an atom or molecule by first preparing an excited state by multiphoton absorption and then ionizing that state before it can decay. This process is highly selective with respect to both the initial and resonant intermediate states of the target, and it can be extremely sensitive. In addition, the products of the REMPI process can be detected as needed by analyzing the resulting electrons, ions, fluorescence, or by additional REMPI. This points to a number of opportunities for exploring excited state physics and chemistry at the quantum-state-specific level. Here we will first give a brief overview of the large variety of experimental approaches to excited state phenomena made possible by REMPI. Then we will examine in more detail, recent studies of the three photon resonant, four photon (3 + 1) ionization of H 2 via the C 'PI/sup u/ state. Strong non-Franck-Condon behavior in the photoelectron spectra of this nominally simple Rydberg state has led to the examination of a variety of dynamical mechanisms. Of these, the role of doubly excited autoionizing states now seems decisive. Progress on photoelectron studies of autoionizing states in H 2 , excited in a (2 + 1) REMPI process via the E, F 1 Σ/sub g/ + will also be briefly discussed. 26 refs., 7 figs

The triplet excited state of bilirubin

International Nuclear Information System (INIS)

Land, E.J.

1976-01-01

Pulse radiolysis of benzene solutions of 40 μM bilirubin alone or with 0.1 M biphenyl has yielded evidence for the formation of the triplet excited state of bilirubin. Measurements were made of a number of properties, including the absorption spectrum (lambdasub(max)500nm), lifetime 9μs), extinction coefficient (8800 M -1 cm -1 ), energy level (approximately 150 kJ mol -1 ) and the rate of quenching by oxygen (rate constant, 8.2 x 10 8 M -1 s -1 ). An upper limit of 0.1 has also been obtained for the singlet to triplet crossover efficiency of bilirubin following excitation by 353 nm radiation. Consideration is given to the relevance of these data to the mechanism of bilirubin photo-destruction, both in vivo and in vitro. (U.K.)

The mechanisms of Excited states in enzymes

DEFF Research Database (Denmark)

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....

Excited state Intramolecular Proton Transfer in Anthralin

DEFF Research Database (Denmark)

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 unus......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......, associated with an excited-state intramolecular proton transfer process....

Coulomb excitation of 206Hg at relativistic energies

Science.gov (United States)

Alexander, Tom

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

Electronically excited states of chloroethylenes: Experiment and DFT calculations in comparison

International Nuclear Information System (INIS)

Khvostenko, O.G.

2014-01-01

Highlights: • B3LYP/6-311 + G(d,p) calculations of chloroethylenes molecules were performed. • Calculations were correlated with experiment on the molecules ground and excited states. • The general pattern of electron structure of chloroethylenes was obtained. • Necessity of this data for chloroethylenes negative ions study was noted. - Abstract: B3LYP/6-311 + G(d,p) calculations of ground and electronically excited states of ethylene, chloroethylene, 1,1-dichloroethylene, 1,2-dichloroethylene-cis, 1,2-dichloroethylene-trans trichloroethylene and tetrachloroethylene molecules have been performed. Molecular orbitals images and orbital correlation diagram are given. The calculation results for chloroethylenes electronically excited states were compared with experimental data from the energy-loss spectra obtained and generally considered previously by C.F. Koerting, K.N. Walzl and A. Kupperman. Several new additional triplet and singlet transitions were pointed out in these spectra considering the calculation results. The finding of the additional transitions was supported by the UV absorption spectrum of trichloroethylene recorded in big cuvette (10 cm), where the first three triplet and two low-intensive forbidden singlet transitions were registered. The first triplet of this compound was recorded to be at the same energy as was found with the energy-loss spectroscopy

Electronically excited states of chloroethylenes: Experiment and DFT calculations in comparison

Energy Technology Data Exchange (ETDEWEB)

Khvostenko, O.G., E-mail: khv@mail.ru

2014-08-15

Highlights: • B3LYP/6-311 + G(d,p) calculations of chloroethylenes molecules were performed. • Calculations were correlated with experiment on the molecules ground and excited states. • The general pattern of electron structure of chloroethylenes was obtained. • Necessity of this data for chloroethylenes negative ions study was noted. - Abstract: B3LYP/6-311 + G(d,p) calculations of ground and electronically excited states of ethylene, chloroethylene, 1,1-dichloroethylene, 1,2-dichloroethylene-cis, 1,2-dichloroethylene-trans trichloroethylene and tetrachloroethylene molecules have been performed. Molecular orbitals images and orbital correlation diagram are given. The calculation results for chloroethylenes electronically excited states were compared with experimental data from the energy-loss spectra obtained and generally considered previously by C.F. Koerting, K.N. Walzl and A. Kupperman. Several new additional triplet and singlet transitions were pointed out in these spectra considering the calculation results. The finding of the additional transitions was supported by the UV absorption spectrum of trichloroethylene recorded in big cuvette (10 cm), where the first three triplet and two low-intensive forbidden singlet transitions were registered. The first triplet of this compound was recorded to be at the same energy as was found with the energy-loss spectroscopy.

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

Science.gov (United States)

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

2017-06-22

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

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

Science.gov (United States)

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

2017-11-01

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

Neutron scattering investigation of magnetic excitations at high energy transfers

International Nuclear Information System (INIS)

Loong, C.K.

1984-01-01

With the advance of pulsed spallation neutron sources, neutron scattering investigation of elementary excitations in magnetic materials can now be extended to energies up to several hundreds of MeV. We have measured, using chopper spectrometers and time-of-flight techniques, the magnetic response functions of a series of d and f transition metals and compounds over a wide range of energy and momentum transfer. In PrO 2 , UO 2 , BaPrO 3 and CeB 6 we observed crystal-field transitions between the magnetic ground state and the excited levels in the energy range from 40 to 260 MeV. In materials exhibiting spin-fluctuation or mixed-valent character such as Ce 74 Th 26 , on the other hand, no sharp crystal-field lines but a broadened quasielastic magnetic peak was observed. The line width of the quasielastic component is thought to be connected to the spin-fluctuation energy of the 4f electrons. The significance of the neutron scattering results in relation to the ground state level structure of the magnetic ions and the spin-dynamics of the f electrons is discussed. Recently, in a study of the spin-wave excitations in itinerant magnetic systems, we have extended the spin-wave measurements in ferromagnetic iron up to about 160 MeV. Neutron scattering data at high energy transfers are of particular interest because they provide direct comparison with recent theories of itinerant magnetism. 26 references, 7 figures

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

Science.gov (United States)

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

2018-04-05

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

Study on the characteristics of sup(163,165,167)Tm excited states

International Nuclear Information System (INIS)

Adam, I.; Alikov, B.A.; Badalov, Kh.N.

1985-01-01

On the basis of analysis of transition intensities, de-excitation nature and systematics of sup(163,1965, 167)Tm nucleus level energy the interpretation of some excited states of studied isotopes is suggested. Results of calculations within the framework of an independent quasiparticle model and quasiparticle-phonon model confirm the suggested interpretation and show that taking account of quasiparticle-phonon interaction improves agreement of theoretical energy values with experimental as compared with the independent quasiparticle model. The calculation of energy of rotational states within the framework of a non adi batic rotational model shows that it is possible to obtain rather good agreement with experiment. It is noted that taking account of correctly the difference in deformations of one-particle states can result in the improvement of agreement of theory and experiment. When calculating rotational spectra for the description of high-lying states it is desirable to consider dependence of collective parameters, for example, inertia momentum, on spin

Excited-state imaging of cold atoms

NARCIS (Netherlands)

Sheludko, D.V.; Bell, S.C.; Vredenbregt, E.J.D.; Scholten, R.E.; Deshmukh, P.C.; Chakraborty, P.; Williams, J.F.

2007-01-01

We have investigated state-selective diffraction contrast imaging (DCI) of cold 85Rb atoms in the first excited (52P3/2) state. Excited-state DCI requires knowledge of the complex refractive index of the atom cloud, which was calculated numerically using a semi-classical model. The Autler-Townes

Dependence of Excited State Potential Energy Surfaces on the Spatial Overlap of the Kohn-Sham Orbitals and the Amount of Nonlocal Hartree-Fock Exchange in Time-Dependent Density Functional Theory.

Science.gov (United States)

Plötner, Jürgen; Tozer, David J; Dreuw, Andreas

2010-08-10

Time-dependent density functional theory (TDDFT) with standard GGA or hybrid exchange-correlation functionals is not capable of describing the potential energy surface of the S1 state of Pigment Yellow 101 correctly; an additional local minimum is observed at a twisted geometry with substantial charge transfer (CT) character. To investigate the influence of nonlocal exact orbital (Hartree-Fock) exchange on the shape of the potential energy surface of the S1 state in detail, it has been computed along the twisting coordinate employing the standard BP86, B3LYP, and BHLYP xc-functionals as well as the long-range separated (LRS) exchange-correlation (xc)-functionals LC-BOP, ωB97X, ωPBE, and CAM-B3LYP and compared to RI-CC2 benchmark results. Additionally, a recently suggested Λ-parameter has been employed that measures the amount of CT in an excited state by calculating the spatial overlap of the occupied and virtual molecular orbitals involved in the transition. Here, the error in the calculated S1 potential energy curves at BP86, B3LYP, and BHLYP can be clearly related to the Λ-parameter, i.e., to the extent of charge transfer. Additionally, it is demonstrated that the CT problem is largely alleviated when the BHLYP xc-functional is employed, although it still exhibits a weak tendency to underestimate the energy of CT states. The situation improves drastically when LRS-functionals are employed within TDDFT excited state calculations. All tested LRS-functionals give qualitatively the correct potential energy curves of the energetically lowest excited states of P. Y. 101 along the twisting coordinate. While LC-BOP and ωB97X overcorrect the CT problem and now tend to give too large excitation energies compared to other non-CT states, ωPBE and CAM-B3LYP are in excellent agreement with the RI-CC2 results, with respect to both the correct shape of the potential energy curve as well as the absolute values of the calculated excitation energies.

Using a Spreadsheet to Solve the Schro¨dinger Equations for the Energies of the Ground Electronic State and the Two Lowest Excited States of H[subscript2

Science.gov (United States)

Ge, Yingbin; Rittenhouse, Robert C.; Buchanan, Jacob C.; Livingston, Benjamin

2014-01-01

We have designed an exercise suitable for a lab or project in an undergraduate physical chemistry course that creates a Microsoft Excel spreadsheet to calculate the energy of the S[subscript 0] ground electronic state and the S[subscript 1] and T[subscript 1] excited states of H[subscript 2]. The spreadsheet calculations circumvent the…

Entanglement entropy of excited states

International Nuclear Information System (INIS)

Alba, Vincenzo; Fagotti, Maurizio; Calabrese, Pasquale

2009-01-01

We study the entanglement entropy of a block of contiguous spins in excited states of spin chains. We consider the XY model in a transverse field and the XXZ Heisenberg spin chain. For the latter, we developed a numerical application of the algebraic Bethe ansatz. We find two main classes of states with logarithmic and extensive behavior in the dimension of the block, characterized by the properties of excitations of the state. This behavior can be related to the locality properties of the Hamiltonian having a given state as the ground state. We also provide several details of the finite size scaling

Orientation and alignment of the first excited p state in Li+He and Na+He scattering

International Nuclear Information System (INIS)

Archer, B.J.; Lane, N.F.; Kimura, M.

1990-01-01

Orientation and alignment parameters for the first excited p state of Li and Na in collisions with He through direct excitation from the ground state are studied theoretically in the energy region up to E c.m. =100 keV by using a quasi-one-electron theory. Scattering states are expanded in terms of molecular orbitals, which are calculated by using the pseudopotential method and include electron translation factors. The approach appears to work well for Li+He, giving good agreement for the 2p excitation probability and orientation. For alignment, the situation is less clear because of difficulty in experimental measurement. Two-electron effects and cascades from more highly excited states cause our description of Na+He collisions to be less satisfactory. However, agreement with the experimental 3p excitation probability and orientation parameters where all data are available is fairly good at lower energies (E c.m. 1.25 a.u.)

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

Science.gov (United States)

Oka, Hisaki

2011-03-28

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

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

DEFF Research Database (Denmark)

Zhang, Wenkai; Kjær, Kasper Skov; Alonso-Mori, Roberto

2017-01-01

iron complexes with four cyanide (CN-;) ligands and one 2,2′-bipyridine (bpy) ligand. This enables MLCT excited state and metal-centered excited state energies to be manipulated with partial independence and provides a path to suppressing spin crossover. We have combined X-ray Free-Electron Laser (XFEL...... state lifetime of iron based complexes due to spin crossover-the extremely fast intersystem crossing and internal conversion to high spin metal-centered excited states. We revitalize a 30 year old synthetic strategy for extending the MLCT excited state lifetimes of iron complexes by making mixed ligand...

Local CC2 response method based on the Laplace transform: Analytic energy gradients for ground and excited states

Energy Technology Data Exchange (ETDEWEB)

Ledermüller, Katrin; Schütz, Martin, E-mail: martin.schuetz@chemie.uni-regensburg.de [Institute of Physical and Theoretical Chemistry, University of Regensburg, Universitätsstraße 31, D-93040 Regensburg (Germany)

2014-04-28

A multistate local CC2 response method for the calculation of analytic energy gradients with respect to nuclear displacements is presented for ground and electronically excited states. The gradient enables the search for equilibrium geometries of extended molecular systems. Laplace transform is used to partition the eigenvalue problem in order to obtain an effective singles eigenvalue problem and adaptive, state-specific local approximations. This leads to an approximation in the energy Lagrangian, which however is shown (by comparison with the corresponding gradient method without Laplace transform) to be of no concern for geometry optimizations. The accuracy of the local approximation is tested and the efficiency of the new code is demonstrated by application calculations devoted to a photocatalytic decarboxylation process of present interest.

Local CC2 response method based on the Laplace transform: analytic energy gradients for ground and excited states.

Science.gov (United States)

Ledermüller, Katrin; Schütz, Martin

2014-04-28

A multistate local CC2 response method for the calculation of analytic energy gradients with respect to nuclear displacements is presented for ground and electronically excited states. The gradient enables the search for equilibrium geometries of extended molecular systems. Laplace transform is used to partition the eigenvalue problem in order to obtain an effective singles eigenvalue problem and adaptive, state-specific local approximations. This leads to an approximation in the energy Lagrangian, which however is shown (by comparison with the corresponding gradient method without Laplace transform) to be of no concern for geometry optimizations. The accuracy of the local approximation is tested and the efficiency of the new code is demonstrated by application calculations devoted to a photocatalytic decarboxylation process of present interest.

Local CC2 response method based on the Laplace transform: Analytic energy gradients for ground and excited states

International Nuclear Information System (INIS)

Ledermüller, Katrin; Schütz, Martin

2014-01-01

A multistate local CC2 response method for the calculation of analytic energy gradients with respect to nuclear displacements is presented for ground and electronically excited states. The gradient enables the search for equilibrium geometries of extended molecular systems. Laplace transform is used to partition the eigenvalue problem in order to obtain an effective singles eigenvalue problem and adaptive, state-specific local approximations. This leads to an approximation in the energy Lagrangian, which however is shown (by comparison with the corresponding gradient method without Laplace transform) to be of no concern for geometry optimizations. The accuracy of the local approximation is tested and the efficiency of the new code is demonstrated by application calculations devoted to a photocatalytic decarboxylation process of present interest

Low-energy heavy-atom impact as a tool for production and classification of doubly excited states

International Nuclear Information System (INIS)

Andersen, N.

1985-01-01

Low-energy heavy-atom impact may be an efficient way of preferentially populating doubly excited levels. Using neon as an example, this paper discusses why this is so. The similarity of the structure of the energy level diagrams for doubly excited neon and the level scheme for neutral magnesium is pointed out, suggesting that collective quantum numbers may describe the electron pair. (orig.)

Tracking excited-state charge and spin dynamics in iron coordination complexes

DEFF Research Database (Denmark)

Zhang, Wenkai; Alonso-Mori, Roberto; Bergmann, Uwe

2014-01-01

to spin state, can elucidate the spin crossover dynamics of [Fe(2,2'-bipyridine)(3)](2+) on photoinduced metal-to-ligand charge transfer excitation. We are able to track the charge and spin dynamics, and establish the critical role of intermediate spin states in the crossover mechanism. We anticipate......Crucial to many light-driven processes in transition metal complexes is the absorption and dissipation of energy by 3d electrons(1-4). But a detailed understanding of such non-equilibrium excited-state dynamics and their interplay with structural changes is challenging: a multitude of excited...... states and possible transitions result in phenomena too complex to unravel when faced with the indirect sensitivity of optical spectroscopy to spin dynamics(5) and the flux limitations of ultrafast X-ray sources(6,7). Such a situation exists for archetypal poly-pyridyl iron complexes, such as [Fe(2...

Characterization of weakly excited final states by shakedown spectroscopy of laser-excited potassium

International Nuclear Information System (INIS)

Schulz, J.; Heinaesmaeki, S.; Aksela, S.; Aksela, H.; Sankari, R.; Rander, T.; Lindblad, A.; Bergersen, H.; Oehrwall, G.; Svensson, S.; Kukk, E.

2006-01-01

3p shakedown spectra of laser excited potassium atoms as well as direct 3p photoemission of ground state potassium have been studied. These two excitation schemes lead to the same final states and thereby provide a good basis for a detailed study of the 3p 5 (4s3d) 1 configurations of singly ionized potassium and the photoemission processes leading to these configurations. The comparison of direct photoemission from the ground state and conjugate shakedown spectra from 4p 1/2 laser excited potassium made it possible to experimentally determine the character of final states that are only weakly excited in the direct photoemission but have a much higher relative intensity in the shakedown spectrum. Based on considerations of angular momentum and parity conservation the excitation scheme of the final states can be understood

Communication: State-to-state dynamics of the Cl + H2O → HCl + OH reaction: Energy flow into reaction coordinate and transition-state control of product energy disposal.

Science.gov (United States)

Zhao, Bin; Sun, Zhigang; Guo, Hua

2015-06-28

Quantum state-to-state dynamics of a prototypical four-atom reaction, namely, Cl + H2O → HCl + OH, is investigated for the first time in full dimensionality using a transition-state wave packet method. The state-to-state reactivity and its dependence on the reactant internal excitations are analyzed and found to share many similarities both energetically and dynamically with the H + H2O → H2 + OH reaction. The strong enhancement of reactivity by the H2O stretching vibrational excitations in both reactions is attributed to the favorable energy flow into the reaction coordinate near the transition state. On the other hand, the insensitivity of the product state distributions with regard to reactant internal excitation stems apparently from the transition-state control of product energy disposal.

Communication: State-to-state dynamics of the Cl + H2O → HCl + OH reaction: Energy flow into reaction coordinate and transition-state control of product energy disposal

International Nuclear Information System (INIS)

Zhao, Bin; Guo, Hua; Sun, Zhigang

2015-01-01

Quantum state-to-state dynamics of a prototypical four-atom reaction, namely, Cl + H 2 O → HCl + OH, is investigated for the first time in full dimensionality using a transition-state wave packet method. The state-to-state reactivity and its dependence on the reactant internal excitations are analyzed and found to share many similarities both energetically and dynamically with the H + H 2 O → H 2 + OH reaction. The strong enhancement of reactivity by the H 2 O stretching vibrational excitations in both reactions is attributed to the favorable energy flow into the reaction coordinate near the transition state. On the other hand, the insensitivity of the product state distributions with regard to reactant internal excitation stems apparently from the transition-state control of product energy disposal

Excitation-energy-dependent resonances in x-ray emissions under near-threshold electron excitation of the Ce 3d and 4d levels

International Nuclear Information System (INIS)

Chamberlain, M.B.; Baun, W.L.

1975-01-01

Soft x-ray appearance potential spectra of the 3d and 4d levels of polycrystalline cerium metal are reported in this paper. Resonant x-ray emissions are observed when the electron-excitation energy sweeps through the ionization energies of the 3d and 4d levels. The resonant x rays excited at the 3d-level onsets are considerably more intense, and are excited at a lower electron-excitation energy than the 3d-series characteristic x rays. In the neighborhood of the 4d-electron thresholds, four line-like structures extend to approx.8 eV below the 4d-electron binding energies, while two broad and more intense structures occur above the 4d onsets, with the largest one reaching a peak intensity at 12 eV above the 4d thresholds. The resonant emissions apparently arise from the decay of threshold-excited states which are bound to the inner vacancy and have core configurations nd 9 4f 3 , (n=3,4). The exchange interaction between the three 4f electrons and the respective d-orbital vacancy spreads the 4d-threshold structures over a 20 eV range of excitation energies and the 3d-threshold structures over a much smaller range

Excited states configurations of the quantum Toda lattice

International Nuclear Information System (INIS)

Matsuyama, A.

2001-01-01

Excited states configurations of the quantum Toda lattice are studied by the direct diagonalization of the Hamiltonian. The most probable configurations of one-hole and one-particle excitations are shown to be similar to the profiles of classical phonon and soliton excitations, respectively. One-hole excitation states, which are always ground states of definite E m -symmetry of the dihedral group D N , change those structures abruptly with the potential range varied. One-particle excitations, which are buried in complicated excitation spectra, have well-defined configurations similar to the conoidal profile of the classical periodic Toda lattice. The relationship that the hole (particle) excitations in quantum mechanics correspond to the phonon (soliton) excitations in classical mechanics, which has been suggested based on the similarity of dispersion relations, is confirmed in a geometrically understandable way. Based on the study of one-soliton and two-soliton states, the structure of multi-soliton states in quantum mechanics can be conjectured

Excited states of 12C above the alpha-decay threshold

International Nuclear Information System (INIS)

Freer, M; Ashwood, N I; Barr, M; Curtis, N; Malcolm, J D; Wheldon, C; Ziman, V A; Almaraz-Calderon, S; Aprahamian, A; Bucher, B; Couder, M; Fang, X; Jung, F; Lu, W; Roberts, A; Tan, W P; Copp, P; Lesher, S

2011-01-01

The excitation energy spectrum of 12 C is important for both structural and astrophysical reasons; here we present evidence for a new state in 12 C. The two reactions 12 C( 4 He, 4 He+ 4 He+ 4 He) 4 He and 9 Be( 4 He, 4 He+ 4 He+ 4 He)n were measured using an array of four double sided strip detectors. Excited states in 12 C were reconstructed filtered by the condition that the alpha-decay proceeded via the 8 Be ground-state. In both measurements evidence was found for a new state at 13.3(0.2) MeV with a width 1.7(0.2) MeV. Angular correlation measurements from the 12 C( 4 He, 4 He+ 4 He+ 4 He) 4 He reaction indicates that the state may have J π = 4 + .

Effect of magnetic field on the impurity binding energy of the excited ...

Indian Academy of Sciences (India)

The effect of external magnetic field on the excited state energies in a spherical quantum dot was studied. The impurity energy and binding energy were calculated using the variational method within the effective mass approximation and finite barrier potential. The results showed that by increasing the magnetic field, the ...

Effect of magnetic field on the impurity binding energy of the excited ...

Indian Academy of Sciences (India)

Abstract. The effect of external magnetic field on the excited state energies in a spher- ical quantum dot was studied. The impurity energy and binding energy were calculated using the variational method within the effective mass approximation and finite barrier potential. The results showed that by increasing the magnetic ...

Performance of Popular XC-Functionals for the Description of Excitation Energies in GFP-Like Chromophore Models

DEFF Research Database (Denmark)

List, Nanna Holmgaard; Olsen, Jógvan Magnus Haugaard; Rocha-Rinza, Tomás

2012-01-01

this task. We present an evaluation of the performance of commonly used XC-functionals for the prediction of excitation energies of GFP-like chromophores. In particular, we have considered the TD-DFT vertical excitation energies of chromophores displaying different charge states. We compare the quality...

Ultrafast Nonradiative Decay and Excitation Energy Transfer by Carotenoids in Photosynthetic Light-Harvesting Proteins

Science.gov (United States)

Ghosh, Soumen

This dissertation investigates the photophysical and structural dynamics that allow carotenoids to serve as efficient excitation energy transfer donor to chlorophyll acceptors in photosynthetic light harvesting proteins. Femtosecond transient grating spectroscopy with optical heterodyne detection has been employed to follow the nonradiative decay pathways of carotenoids and excitation energy transfer to chlorophylls. It was found that the optically prepared S2 (11Bu+) state of beta-carotene decays in 12 fs fs to populate an intermediate electronic state, Sx, which then decays nonradiatively to the S 1 state. The ultrafast rise of the dispersion component of the heterodyne transient grating signal reports the formation of Sx intermediate since the rise of the dispersion signal is controlled by the loss of stimulated emission from the S2 state. These findings were extended to studies of peridinin, a carbonyl substituted carotenoid that serves as a photosynthetic light-harvesting chromophore in dinoflagellates. Numerical simulations using nonlinear response formalism and the multimode Brownian oscillator model assigned the Sx intermediate to a torsionally distorted structure evolving on the S2 potential surface. The decay of the Sx state is promoted by large amplitude out-of-plane torsional motions and is significantly retarded by solvent friction owing to the development of an intramolecular charge transfer character in peridinin. The slowing of the nonradiative decay allows the Sx state to transfer significant portion of the excitation energy to chlorophyll a acceptors in the peridinin-chlorophyll a protein. The results of heterodyne transient grating study on peridinin-chlorophyll a protein suggests two distinct energy transfer channels from peridinin to chlorophyll a: a 30 fs process involving quantum coherence and delocalized peridinin-Chl states and an incoherent, 2.5 ps process involving the distorted S2 state of peridinin. The torsional evolution on the S2

The role of the excited electronic states in the C++H2O reaction

International Nuclear Information System (INIS)

Flores, Jesus R.; Gonzalez, Adan B.

2008-01-01

The electronic excited states of the [COH 2 ] + system have been studied in order to establish their role in the dynamics of the C + +H 2 O→[COH] + +H reaction, which is a prototypical ion-molecule reaction. The most relevant minima and saddle points of the lowest excited state have been determined and energy profiles for the lowest excited doublet and quartet electronic states have been computed along the fragmentation and isomerization coordinates. Also, nonadiabatic coupling strengths between the ground and the first excited state have been computed where they can be large. Our analysis suggests that the first excited state could play an important role in the generation of the formyl isomer, which has been detected in crossed beam experiments [D. M. Sonnenfroh et al., J. Chem. Phys. 83, 3985 (1985)], but could not be explained in quasiclassical trajectory computations [Y. Ishikawa et al., Chem. Phys. Lett. 370, 490 (2003); J. R. Flores, J. Chem. Phys. 125, 164309 (2006)

Electric quadrupole excitation of the first excited state of 11B

International Nuclear Information System (INIS)

Fewell, M.P.; Spear, R.H.; Zabel, T.H.; Baxter, A.M.

1980-02-01

The Coulomb excitation of backscattered 11 B projectiles has been used to measure the reduced E2 transition probability B(E2; 3/2 - →1/2 - ) between the 3/2 - ground state and the 1/2 - first excited state of 11 B. It is found that B(E2; 3/2 - →1/2 - ) = 2.1 +- 0.4 e 2 fm 4 , which agrees with shell-model predictions but is a factor of 10 larger than the prediction of the core-excitation model

Electric dipole moments of He atoms excited to the 1s5l (l  ⩾ 2) states by He+-ion impact at intermediate energies

International Nuclear Information System (INIS)

Baszanowska, E; Drozdowski, R; Kamiński, P; Von Oppen, G

2014-01-01

The post-collisional 1s5l (l ⩾ 2) states of He atoms after He + -ion impact (10 keV–28 keV) have been investigated using anticrossing spectroscopy. In particular, the intensity of the spectral line λ(1s5l 3 D-1s2p 3 P) = 402.6 nm emitted by the impact-excited He atoms was measured as a function of an axial electric field (which varied from −30 kV cm −1 to +30 kV cm −1 ). By fitting the theoretical intensity functions to the measured ones, the post-collisional states of the atoms and their electric dipole moments were determined. The results indicate that for projectile energies below 20 keV, the electric dipole moments are small; however, for energies above 20 keV, mainly the parabolic Stark states with maximal electric dipole moments are excited. We conclude that in the upper section of the energy range investigated here, the Paul-trap promotion is the dominant excitation mechanism for He + –He collisions. (paper)

Statistical description of massless excitations within a sphere with a linear equation of state and the dark energy case

Science.gov (United States)

Viaggiu, S.

2018-04-01

In this paper, we continue the investigations present in Refs. 1-3. In particular, we extend the theorem proved in Ref. 3 to any massless excitation in a given spherical box. As a first interesting result, we show that it is possible, contrary to the black hole case studied in detail in Refs. 1-3, to build macroscopic configurations with a dark energy equation of state. To this purpose, by requiring a stable configuration, a macroscopic dark fluid is obtained with an internal energy U scaling as the volume V, but with a fundamental correction looking like ˜ 1/R motivated by quantum fluctuations. Thanks to the proposition in Sec. 3 (and in Ref. 3 for gravitons), one can depict the dark energy in terms of massless excitations with a discrete spectrum. This fact opens the possibility to test a possible physical mechanism converting usual radiation into dark energy in a macroscopic configuration, also in a cosmological context. In fact, for example, in a Friedmann flat universe with a cosmological constant, particles are marginally trapped at the Hubble horizon for any given comoving observer.

Spectroscopy of weakly-bound complexes in highly excited electronic states: the He-I2(E3Πg) ion-pair state

International Nuclear Information System (INIS)

Prosmiti, Rita; Valdés, Álvaro; Kalemost, Apostolos

2014-01-01

The study of electronically excited van der Waals (vdW) systems presents a challenge for the theory of intermolecular interactions, and here we show how far ab initio computations can go. We found that the interaction energies for such electronically excited systems can indeed be determined, providing a reliable and accurate description for the E state potential of the HeI 2 , that in combination with the ground X and electronic excited B state of the complex, is useful to model experimental data related with potential minima and also predict higher vibrational vdW states

Lattice Boltzmann simulation for the energy and entropy of excitable systems

Institute of Scientific and Technical Information of China (English)

Deng Min-Yi; Tang Guo-Ning; Kong Ling-Jiang; Liu Mu-Ren

2011-01-01

The internal energy and the spatiotemporal entropy of excitable systems are investigated with the lattice Boltzmann method. The numerical results show that the breakup of spiral wave is attributed to the inadequate supply of energy, i.e., the internal energy of system is smaller than the energy of self-sustained spiral wave. It is observed that the average internal energy of a regular wave state reduces with its spatiotemporal entropy decreasing. Interestingly, although the energy difference between two regular wave states is very small, the different states can be distinguished obviously due to the large difference between their spatiotemporal entropies. In addition, when the unstable spiral wave converts into the spatiotemporal chaos, the internal energy of system decreases, while the spatiotemporal entropy increases, which behaves as the thermodynamic entropy in an isolated system.

Critical Assessment of TD-DFT for Excited States of Open-Shell Systems: I. Doublet-Doublet Transitions.

Science.gov (United States)

Li, Zhendong; Liu, Wenjian

2016-01-12

A benchmark set of 11 small radicals is set up to assess the performance of time-dependent density functional theory (TD-DFT) for the excited states of open-shell systems. Both the unrestricted (U-TD-DFT) and spin-adapted (X-TD-DFT) formulations of TD-DFT are considered. For comparison, the well-established EOM-CCSD (equation-of-motion coupled-cluster with singles and doubles) is also used. In total, 111 low-lying singly excited doublet states are accessed by all the three approaches. Taking the MRCISD+Q (multireference configuration interaction with singles and doubles plus the Davidson correction) results as the benchmark, it is found that both U-TD-DFT and EOM-CCSD perform well for those states dominated by singlet-coupled single excitations (SCSE) from closed-shell to open-shell, open-shell to vacant-shell, or closed-shell to vacant-shell orbitals. However, for those states dominated by triplet-coupled single excitations (TCSE) from closed-shell to vacant-shell orbitals, both U-TD-DFT and EOM-CCSD fail miserably due to severe spin contaminations. In contrast, X-TD-DFT provides balanced descriptions of both SCSE and TCSE. As far as the functional dependence is concerned, it is found that, when the Hartree-Fock ground state does not suffer from the instability problem, both global hybrid (GH) and range-separated hybrid (RSH) functionals perform grossly better than pure density functionals, especially for Rydberg and charge-transfer excitations. However, if the Hartree-Fock ground state is instable or nearly instable, GH and RSH tend to underestimate severely the excitation energies. The SAOP (statistically averaging of model orbital potentials) performs more uniformly than any other density functionals, although it generally overestimates the excitation energies of valence excitations. Not surprisingly, both EOM-CCSD and adiabatic TD-DFT are incapable of describing excited states with substantial double excitation characters.

Benzonitrile: Electron affinity, excited states, and anion solvation

Science.gov (United States)

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

2015-10-01

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

Gamma decays, lifetimes and spins of 47V excited states

International Nuclear Information System (INIS)

Thompson, J.V.; Bell, R.A.I.; Carlson, E.; Najam, M.R.

1974-11-01

The nucleus 47 V has been studied using the 47 Ti(p,nγ) 47 V reaction, with isotopically enriched 47 Ti targets, incident proton energies from 4.7 to 5.4 MeV, and Ge(Li) gamma-ray detectors. The previously unreported gamma decay of the second excited state was observed. Energies of the first seven excited states were deduced to be 87.5 +- 0.1, 145.7 +- 0.2, 259.6 +-0.4, 660.1 +- 0.3, 1138.3 +- 0.4, 1272.2 +- 0.4 and 1295.1 +- 0.4 keV. Their gamma-decay branching ratios were measured. The lifetimes of the last four mentioned states were deduced from attenuated Doppler shifts to be [680-340, 680+1400], [960-440, 960+1700], [390-150, 390+390], and > 750 fs respectively. Angular distribution measurements resulted in the assignment of Jsup(π) = 9/2 - to the 1272 keV level and J = 9/2 or 11/2 to the 1295 keV level. The results are discussed in the light of the Coriolis coupling model. (author)

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

Science.gov (United States)

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

2012-12-01

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

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

International Nuclear Information System (INIS)

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

2010-01-01

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.

Electron scattering by CO2: Elastic scattering, rotational excitation, and excitation of the asymmetric stretch at 10 eV impact energy

International Nuclear Information System (INIS)

Thirumalai, D.; Onda, K.; Truhlar, D.G.

1981-01-01

Coupled-channels calculations based on an effective potential are presented for electron scattering by CO 2 at 10 eV impact energy. The processes studied are pure elastic scattering, rotational excitation, and vibrational excitation of the asymmetric stretch; the vibrational excitation is always accompanied by rotational excitation. The quantities calculated are differential, partial, integral, and momentum transfer cross sections, both state to state and summed over final rotational states for a given final vibrational level. The effective potential is based on the INDOX2/1s method for the static and polarization potentials and the semiclassical exchange approximation for the exchange potential. There are no empirical parameters. The present calculations are compared to experiment and to previous calculations where available, and we also perform calculations with an altered polarization potential to further elucidate the reasons for the differences from one of the previous calculations. The agreement of the present results with the experimental rotationally summed, vibrationally inelastic differential cross section is excellent

A note on calm excited states of inflation

International Nuclear Information System (INIS)

Ashoorioon, Amjad; Shiu, Gary

2011-01-01

We identify a two-parameter family of excited states within slow-roll inflation for which either the corrections to the two-point function or the characteristic signatures of excited states in the three-point function — i.e. the enhancement for the flattened momenta configurations– are absent. These excited states may nonetheless violate the adiabaticity condition maximally. We dub these initial states of inflation calm excited states. We show that these two sets do not intersect, i.e., those that leave the power-spectrum invariant can be distinguished from their bispectra, and vice versa. The same set of calm excited states that leave the two-point function invariant for slow-roll inflation, do the same task for DBI inflation. However, at the level of three-point function, the calm excited states whose flattened configuration signature is absent for slow-roll inflation, will lead to an enhancement for DBI inflation generally, although the signature is smaller than what suggested by earlier analysis. This example also illustrates that imposing the Wronskian condition is important for obtaining a correct estimate of the non-Gaussian signatures

Lifetime measurements of excited states in 17C: Possible interplay between collectivity and halo effects

International Nuclear Information System (INIS)

Suzuki, D.; Iwasaki, H.; Ong, H.J.; Imai, N.; Sakurai, H.; Nakao, T.; Aoi, N.; Baba, H.; Bishop, S.; Ichikawa, Y.; Ishihara, M.; Kondo, Y.; Kubo, T.; Kurita, K.; Motobayashi, T.; Nakamura, T.; Okumura, T.; Onishi, T.K.; Ota, S.; Suzuki, M.K.

2008-01-01

Lifetime measurements were performed on low-lying excited states of the neutron-rich isotope 17 C using the recoil shadow method. The γ-decay mean lifetimes were determined to be 583±21(stat)±35(syst) ps for the first excited state at 212 keV and 18.9±0.6(stat)±4.7(syst) ps for the second excited state at 333 keV. Based on a comparison with the empirical upper limits for the electromagnetic transition strengths, these decays are concluded to be predominantly M1 transitions. The reduced M1 transition probabilities to the ground state were deduced to be (1.0±0.1)x10 -2 μ N 2 and (8.2 -1.8 +3.2 )x10 -2 μ N 2 , respectively, for the first and second excited states. The strongly hindered M1 strength as well as the lowered excitation energy represents unique nature of the 212-keV state

Energy-optimal electrical excitation of nerve fibers.

Science.gov (United States)

Jezernik, Saso; Morari, Manfred

2005-04-01

We derive, based on an analytical nerve membrane model and optimal control theory of dynamical systems, an energy-optimal stimulation current waveform for electrical excitation of nerve fibers. Optimal stimulation waveforms for nonleaky and leaky membranes are calculated. The case with a leaky membrane is a realistic case. Finally, we compare the waveforms and energies necessary for excitation of a leaky membrane in the case where the stimulation waveform is a square-wave current pulse, and in the case of energy-optimal stimulation. The optimal stimulation waveform is an exponentially rising waveform and necessitates considerably less energy to excite the nerve than a square-wave pulse (especially true for larger pulse durations). The described theoretical results can lead to drastically increased battery lifetime and/or decreased energy transmission requirements for implanted biomedical systems.

Impact of nuclear lattice relaxation on the excitation energy transfer along a chain of pi-conjugated molecules

NARCIS (Netherlands)

Schmid, S.A.; Abbel, R.J.; Schenning, A.P.H.J.; Meijer, E.W.; Herz, L.M.

2010-01-01

We have investigated the extent to which delocalization of the ground-state and excited-state wave functions of a p-conjugated molecule affects the excitation energy transfer (EET) between such molecules. Using femtosecond photoluminescence spectroscopy, we experimentally monitored the EET along

Roles of the Excitation in Harvesting Energy from Vibrations.

Directory of Open Access Journals (Sweden)

Hui Zhang

Full Text Available The study investigated the role of excitation in energy harvesting applications. While the energy ultimately comes from the excitation, it was shown that the excitation may not always behave as a source. When the device characteristics do not perfectly match the excitation, the excitation alternately behaves as a source and a sink. The extent to which the excitation behaves as a sink determines the energy harvesting efficiency. Such contradictory roles were shown to be dictated by a generalized phase defined as the instantaneous phase angle between the velocity of the device and the excitation. An inductive prototype device with a diamagnetically levitated seismic mass was proposed to take advantage of the well established phase changing mechanism of vibro-impact to achieve a broader device bandwidth. Results suggest that the vibro-impact can generate an instantaneous, significant phase shift in response velocity that switches the role of the excitation. If introduced properly outside the resonance zone it could dramatically increase the energy harvesting efficiency.

Photoemission from excited states in rare gas solids by combining synchrotronradiation with a laser

International Nuclear Information System (INIS)

Bernstorff, S.

1984-09-01

A new spectroscopic method has been developed to study excited states in rare gas solids: Excitons and conductionband-states are populated by synchrotron radiation (photon energy hw SR =5 - 30 eV). Subsequently electrons from these bound or conduction band-states are excited above the vacuum level of the solid by a pulsed dye laser (hw L =1.9 - 3.7 eV). This experimental technique was applied to solid Xe, Kr, Ar and Ne. (orig./GSCH)

Dielectronic recombination rate coefficients to the excited states of CIII from CIV

Energy Technology Data Exchange (ETDEWEB)

Safronova, U.; Kato, Takako; Ohira, Mituhiko

1996-07-01

Energy levels, radiative transition probabilities and autoionization rates for CIII including 1s{sup 2}2pnl` (n=2/6, l`{<=}(n-1)) and 1s{sup 2}3lnl` (n=3/6, l`{<=}(n-1)) states were calculated by using multi-configurational Hartree-Fock (Cowan code) method. Autoionizing levels above the 1s{sup 2}2s and 1s{sup 2}2p thresholds were considered and their contributions were computed. Branching ratios on the autoionization rate to the first threshold and intensity factor were calculated for satellite lines of CIII ion. The dielectronic recombination rate coefficients to the excited states for n=2-6 were calculated. The values for the excited states higher than n=6 were extrapolated and the total dielectronic recombination rate coefficients were also derived. The rate coefficients to the excited states were fitted to an analytical formula and the fitting parameters are given. (author)

High-Yield Excited Triplet States in Pentacene Self-Assembled Monolayers on Gold Nanoparticles through Singlet Exciton Fission.

Science.gov (United States)

Kato, Daiki; Sakai, Hayato; Tkachenko, Nikolai V; Hasobe, Taku

2016-04-18

One of the major drawbacks of organic-dye-modified self-assembled monolayers on metal nanoparticles when employed for efficient use of light energy is the fact that singlet excited states on dye molecules can be easily deactivated by means of energy transfer to the metal surface. In this study, a series of 6,13-bis(triisopropylsilylethynyl)pentacene-alkanethiolate monolayer protected gold nanoparticles with different particle sizes and alkane chain lengths were successfully synthesized and were employed for the efficient generation of excited triplet states of the pentacene derivatives by singlet fission. Time-resolved transient absorption measurements revealed the formation of excited triplet states in high yield (172±26 %) by suppressing energy transfer to the gold surface. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Radiative and nonradiative lifetimes in excited states of Ar, Kr and Xe atoms in Ne matrix

International Nuclear Information System (INIS)

Hahn, U.; Schwentner, N.

1979-10-01

Synchrotron radiation with its intense continuum and its excellent time structure has been exploited for time resolved luminescence spectroscopy in the solid state. By selective excitation of n = 1, n' = 1 and n = 2 exciton states of Xe, Kr and Ar atoms in Ne matrix we were able to identify the emitting states involved. Lifetimes within the cascade of radiative and radiationless relaxation between excited states as well as the radiative lifetimes for transitions to the ground state have been derived from the decay curves. Energy positions and radiative lifetimes of the emitting states correspond quite well with those of the free atoms. Radiative and radiationless relaxation processes take place within the manifold of excited states of the guest atoms. The rate constants for radiationless decay confirm an energy gap law. The order of the radiationless processes reaches in some cases extremely high values. Selection rules for spin and angular momentum are essential to understand the observed radiationless transition rates. (orig.)

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

Science.gov (United States)

Ziegler, Tom; Krykunov, Mykhaylo; Autschbach, Jochen

2014-09-09

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

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

Science.gov (United States)

Maurer, Reinhard J; Reuter, Karsten

2013-07-07

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

Process to produce excited states of atomic nuclei

International Nuclear Information System (INIS)

Morita, M.; Morita, R.

The claims of a patented process which relates to the production of excited states of atomic nuclei are outlined. Among these are (1) production of nuclear excited states by bombarding the atoms with x rays or electrons under given conditions, (2) production of radioactive substances by nuclear excitation with x rays or electrons, (3) separation of specific isotopes from a mixture of isotopes of the same element by means of nuclear excitation followed by chemical treatment. The invention allows production of excited states of atomic nuclei in a relatively simple manner without the need of large apparatus and equipment

De-excitation gamma-ray technique for improved resolution in intermediate energy photonuclear reactions

International Nuclear Information System (INIS)

Kuzin, A.; Thompson, M.N.; Rassool, R.; Adler, J.O.; Fissum, K.; Issaksson, L.; Ruijter, H.; Schroeder, B.; Annand, J.R.M.; McGeorge, J.C.; Crawford, G.I.; Gregel, J.

1997-01-01

The 12 C (γ,p) reaction was studied. The experiment was done at the MAX Laboratory of Lund University, using tagged photons with energy between 50 and 70 MeV and natural carbon targets. It has been possible to detect γ-ray emitted from the residual nucleus, in coincidence with photoprotons leading to the excited residual state. The 200 KeV gamma-ray resolution permitted the identification of the residual states and allowed off-line cuts to be made in order to identify the excitation region in 11 B from what particular de-excitation gamma-ray were seen. 9 refs., 1 tab., 3 figs

Isoelectronic study of triply excited Li-like states

International Nuclear Information System (INIS)

Benis, E P; Zouros, T J M; Gorczyca, T W; Zamkov, M; Richard, P

2003-01-01

Absolute doubly differential cross sections (DDCSs) for the production and Auger decay of the intra-shell 2s2p 22 D triply excited state formed in collisions of He-like ions (Z = 5-9) with H 2 were determined experimentally, using zero-degree Auger projectile electron spectroscopy. The 2 D e state was directly produced by 180 deg. resonant scattering of the quasi-free H 2 electrons from the 1s2s 3 S metastable state of the ion. Resonant energies and DDCSs calculated using the R-matrix approach within the electron scattering model were found to be in good overall agreement with experiment. (letter to the editor)

Non-degenerated Ground States and Low-degenerated Excited States in the Antiferromagnetic Ising Model on Triangulations

Science.gov (United States)

Jiménez, Andrea

2014-02-01

We study the unexpected asymptotic behavior of the degeneracy of the first few energy levels in the antiferromagnetic Ising model on triangulations of closed Riemann surfaces. There are strong mathematical and physical reasons to expect that the number of ground states (i.e., degeneracy) of the antiferromagnetic Ising model on the triangulations of a fixed closed Riemann surface is exponential in the number of vertices. In the set of plane triangulations, the degeneracy equals the number of perfect matchings of the geometric duals, and thus it is exponential by a recent result of Chudnovsky and Seymour. From the physics point of view, antiferromagnetic triangulations are geometrically frustrated systems, and in such systems exponential degeneracy is predicted. We present results that contradict these predictions. We prove that for each closed Riemann surface S of positive genus, there are sequences of triangulations of S with exactly one ground state. One possible explanation of this phenomenon is that exponential degeneracy would be found in the excited states with energy close to the ground state energy. However, as our second result, we show the existence of a sequence of triangulations of a closed Riemann surface of genus 10 with exactly one ground state such that the degeneracy of each of the 1st, 2nd, 3rd and 4th excited energy levels belongs to O( n), O( n 2), O( n 3) and O( n 4), respectively.

Excited-state kinetics of the carotenoid S//1 state in LHC II and two-photon excitation spectra of lutein and beta-carotene in solution Efficient Car S//1 yields Chl electronic energy transfer via hot S//1 states?

CERN Document Server

Walla, P J; Linden, Patricia A; Ohta, Kaoru

2002-01-01

The excited-state dynamics of the carotenoids (Car) in light- harvesting complex II (LHC II) of Chlamydomonas reinhardtii were studied by transient absorption measurements. The decay of the Car S //1 population ranges from similar to 200 fs to over 7 ps, depending on the excitation and detection wavelengths. In contrast, a 200 fs Car S//1 yields Chlorophyll (Chl) energy transfer component was the dominant time constant for our earlier two-photon fluorescence up- conversion measurements (Walla, P.J. ; et al. J. Phys. Chem. B 2000, 104, 4799-4806). We also present the two-photon excitation (TPE) spectra of lutein and beta-carotene in solution and compare them with the TPE spectrum of LHC II. The TPE-spectrum of LHC II has an onset much further to the blue and a width that is narrower than expected from comparison to the S//1 fluorescence of lutein and beta-carotene in solution. Different environments may affect the shape of the S//1 spectrum significantly. To explain the blue shift of the TPE spectrum and the d...

Exact finite volume expectation values of local operators in excited states

Energy Technology Data Exchange (ETDEWEB)

Pozsgay, B. [MTA-BME “Momentum” Statistical Field Theory Research Group,Budafoki út 8, 1111 Budapest (Hungary); Szécsényi, I.M. [Department of Mathematical Sciences, Durham University, South Road, Durham, DH1 3LE (United Kingdom); Institute of Theoretical Physics, Eötvös Loránd University,Pázmány Péter sétány 1/A, 1117 Budapest (Hungary); Takács, G. [MTA-BME “Momentum” Statistical Field Theory Research Group,Budafoki út 8, 1111 Budapest (Hungary); Department of Theoretical Physics, Budapest University of Technology and Economics,Budafoki út 8, 1111 Budapest (Hungary)

2015-04-07

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

Exact finite volume expectation values of local operators in excited states

International Nuclear Information System (INIS)

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

2015-01-01

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

Photoionization of excited molecular states using multiphoton excitation techniques

International Nuclear Information System (INIS)

Dehmer, P.M.; Pratt, S.T.; Dehmer, J.L.

1984-01-01

Photoelectron spectra are reported for three photon resonant, four photon ionization of H 2 via the B 1 Σ + /sub u/, v = 7 (J = 2,4) and C 1 Pi/sub u/, v = 0-4 (J = 1) levels and of N 2 via the o 3 1 Pi/sub u/, v = 1,2, b 1 Pi/sub u/, v = 3-5, and c 1 Pi/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

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

Science.gov (United States)

Sadybekov, Arman

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

Plasmon assisted control of photo-induced excitation energy transfer in a molecular chain

Science.gov (United States)

Wang, Luxia; May, Volkhard

2017-08-01

The strong and ultrafast laser pulse excitation of a molecular chain in close vicinity to a spherical metal nano-particle (MNP) is studied theoretically. Due to local-field enhancement around the MNP, pronounced excited-state formation has to be expected for the part of the chain which is in proximity to the MNP. Here, the description of this phenomenon will be based on a uniform quantum theory of the MNP-molecule system. It accounts for local-field effects due to direct consideration of the strong excitation energy transfer coupling between the MNP and the various molecules. The molecule-MNP distances are chosen in such a way as to achieve a correct description of the MNP via dipole-plasmon excitations. Short plasmon life-times are incorporated in the framework of a density matrix approach. By extending earlier work the present description allows for multi-exciton formation and multiple dipole-plasmon excitation. The region of less intense and not-too-short optical excitation is identified as being best suited for excitation energy localization in the chain.

Neutron-scattering study of low-energy excitations in triphenyl phosphite

CERN Document Server

Mayer, J; Massalska-Arodz, M; Janik, J A; Natkaniec, I; Steinsvoll, O

2002-01-01

The low-energy excitations in crystalline and glassy triphenyl phosphite were studied by inelastic incoherent neutron scattering with two different instruments. The results - the incoherent dynamic structure factor S(2 theta,omega) and the density of states G(omega) - were obtained using direct and inverted geometry time-of-flight spectrometers, respectively. The probable origin of the excess density of states in the glass (boson peak) is discussed. (orig.)

Neutron-scattering study of low-energy excitations in triphenyl phosphite

International Nuclear Information System (INIS)

Mayer, J.; Krawczyk, J.; Massalska-Arodz, M.; Janik, J.A.; Natkaniec, I.; Steinsvoll, O.

2002-01-01

The low-energy excitations in crystalline and glassy triphenyl phosphite were studied by inelastic incoherent neutron scattering with two different instruments. The results - the incoherent dynamic structure factor S(2θ,ω) and the density of states G(ω) - were obtained using direct and inverted geometry time-of-flight spectrometers, respectively. The probable origin of the excess density of states in the glass (boson peak) is discussed. (orig.)

Excitation Energies of Superdeformed States in 196Pb: Towards a Systematic Study of the Second Well in Pb Isotopes

International Nuclear Information System (INIS)

Wilson, A.N.; Singh, A.K.; Huebel, H.; Rossbach, D.; Schonwasser, G.; Davidson, P.M.; Dracoulis, G.D.; Lane, G.J.; Goergen, A.; Korichi, A.; Hannachi, F.; Lopez-Martens, A.; Astier, A.; Azaiez, F.; Bourgeois, C.; Bazzacco, D.; Kroell, T.; Rossi-Alvarez, C.; Buforn, N.; Redon, N.

2005-01-01

The excitation energy of the lowest-energy superdeformed band in 196 Pb is established using the techniques of time-correlated γ-ray spectroscopy. Together with previous measurements on 192 Pb and 194 Pb, this result allows superdeformed excitation energies, binding energies, and two-proton and two-neutron separation energies to be studied systematically, providing stringent tests for current nuclear models. The results are examined for evidence of a 'superdeformed shell gap'

Pion inelastic scattering to the first three excited states of lithium-6

International Nuclear Information System (INIS)

Kiziah, R.R.

1984-10-01

Using the Energetic Pion Channel and Spectrometer system at the Clinton P. Anderson Meson Physics Facility, differential cross sections were measured for π + inelastic scattering to the 3 + , T=0, 2.185-MeV, 0 + , T=1, 3.563-MeV, and 2 + , T=0, 4.25-MeV states of 6 Li at incident pion energies of 120 and 180 MeV and laboratory scattering angles between 15 0 and 47 0 . Excitation functions were measured at a constant momentum transfer of approximately 109 MeV/c for incident pion energies from 100 to 260 MeV. The constant momentum transfer corresponds to the maxima of the angular distributions for π + inelastic scattering to the 3.563-MeV level. Microscopic calculations using the distorted-wave impulse approximation (DWIA) agree well with the measured angular distributions and excitation functions for the 2.185- and 4.25-MeV levels. However, microscopic DWIA calculations do not adequately reproduce the measured angular distributions for the 3.563-MeV level and fail to reproduce the observed anomalous excitation function. The shape of the 3.563-MeV excitation function is similar to that previously observed for π +- inelastic scattering to the 1 + , T=1, 15.11-MeV state of 12 C. The same mechanism may be responsible for the observed excitation functions of both ΔS=ΔT=1 transitions. A possible mechanism is the direct excitation of Δ particle-nucleon hole (Δ-h) components in the final state wave functions. Within the Δ-h model interpretation, the peak of the 3.563-MeV excitation function is reproduced with an estimated probability amplitude for the Δ-h component of the 3.563-MeV state with respect to the ground state of 0.01 less than or equal to β less than or equal to 0.13, a range of values of β consistent with the range estimated for the 15.11-MeV level of 12 C (0.026 less than or equal to β less than or equal to 0.096)

Electron affinity and excited states of methylglyoxal

Science.gov (United States)

Dauletyarov, Yerbolat; Dixon, Andrew R.; Wallace, Adam A.; Sanov, Andrei

2017-07-01

Using photoelectron imaging spectroscopy, we characterized the anion of methylglyoxal (X2A″ electronic state) and three lowest electronic states of the neutral methylglyoxal molecule: the closed-shell singlet ground state (X1A'), the lowest triplet state (a3A″), and the open-shell singlet state (A1A″). The adiabatic electron affinity (EA) of the ground state, EA(X1A') = 0.87(1) eV, spectroscopically determined for the first time, compares to 1.10(2) eV for unsubstituted glyoxal. The EAs (adiabatic attachment energies) of two excited states of methylglyoxal were also determined: EA(a3A″) = 3.27(2) eV and EA(A1A″) = 3.614(9) eV. The photodetachment of the anion to each of these two states produces the neutral species near the respective structural equilibria; hence, the a3A″ ← X2A″ and A1A″ ← X2A″ photodetachment transitions are dominated by intense peaks at their respective origins. The lowest-energy photodetachment transition, on the other hand, involves significant geometry relaxation in the X1A' state, which corresponds to a 60° internal rotation of the methyl group, compared to the anion structure. Accordingly, the X1A' ← X2A″ transition is characterized as a broad, congested band, whose vertical detachment energy, VDE = 1.20(4) eV, significantly exceeds the adiabatic EA. The experimental results are in excellent agreement with the ab initio predictions using several equation-of-motion methodologies, combined with coupled-cluster theory.

Excited state kinetics of anthracene-bridge-aniline intramolecular exciplexes

DEFF Research Database (Denmark)

Thyrhaug, Erling; Hammershøj, Peter; Kjær, Kasper Skov

2014-01-01

excited anthracene state (LE) and an excited state complex (exciplex, EP) in non-polar solvents. The kinetics of the excited state processes were established in decalin from the time-resolved emission, and was shown to be strongly influenced by an electron-transfer state (ET). For quantitative studies...

Application of spectroscopy and super-resolution microscopy: Excited state

Energy Technology Data Exchange (ETDEWEB)

Bhattacharjee, Ujjal [Iowa State Univ., Ames, IA (United States)

2016-02-19

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

Superconducting qubit in a nonstationary transmission line cavity: Parametric excitation, periodic pumping, and energy dissipation

Energy Technology Data Exchange (ETDEWEB)

Zhukov, A.A. [N.L. Dukhov All-Russia Research Institute of Automatics, 127055 Moscow (Russian Federation); National Research Nuclear University (MEPhI), 115409 Moscow (Russian Federation); Shapiro, D.S., E-mail: shapiro.dima@gmail.com [N.L. Dukhov All-Russia Research Institute of Automatics, 127055 Moscow (Russian Federation); V.A. Kotel' nikov Institute of Radio Engineering and Electronics, Russian Academy of Sciences, 125009 Moscow (Russian Federation); Moscow Institute of Physics and Technology, Dolgoprudny, Moscow Region 141700 (Russian Federation); National University of Science and Technology MISIS, 119049 Moscow (Russian Federation); Remizov, S.V. [N.L. Dukhov All-Russia Research Institute of Automatics, 127055 Moscow (Russian Federation); V.A. Kotel' nikov Institute of Radio Engineering and Electronics, Russian Academy of Sciences, 125009 Moscow (Russian Federation); Pogosov, W.V. [N.L. Dukhov All-Russia Research Institute of Automatics, 127055 Moscow (Russian Federation); Moscow Institute of Physics and Technology, Dolgoprudny, Moscow Region 141700 (Russian Federation); Institute for Theoretical and Applied Electrodynamics, Russian Academy of Sciences, 125412 Moscow (Russian Federation); Lozovik, Yu.E. [N.L. Dukhov All-Russia Research Institute of Automatics, 127055 Moscow (Russian Federation); National Research Nuclear University (MEPhI), 115409 Moscow (Russian Federation); Moscow Institute of Physics and Technology, Dolgoprudny, Moscow Region 141700 (Russian Federation); Institute of Spectroscopy, Russian Academy of Sciences, 142190 Moscow Region, Troitsk (Russian Federation)

2017-02-12

We consider a superconducting qubit coupled to the nonstationary transmission line cavity with modulated frequency taking into account energy dissipation. Previously, it was demonstrated that in the case of a single nonadiabatical modulation of a cavity frequency there are two channels of a two-level system excitation which are due to the absorption of Casimir photons and due to the counterrotating wave processes responsible for the dynamical Lamb effect. We show that the parametric periodical modulation of the resonator frequency can increase dramatically the excitation probability. Remarkably, counterrotating wave processes under such a modulation start to play an important role even in the resonant regime. Our predictions can be used to control qubit-resonator quantum states as well as to study experimentally different channels of a parametric qubit excitation. - Highlights: • Coupled qubit-resonator system under the modulation of a resonator frequency is considered. • Counterrotating terms of the Hamiltonian are of importance even in the resonance. • Qubit excited state population is highest if driving frequency matches dressed-state energy.

The theory and experiment of solute migration caused by excited state absorptions

International Nuclear Information System (INIS)

Xiao, Jin; Ying-Lin, Song; Yu-Xiao, Wang; Min, Shui; Chang-Wei, Li; Jun-Yi, Yang; Xue-Ru, Zhang; Kun, Yang

2010-01-01

Nonsymmetrical transition from reverse-saturable absorption (RSA) to saturable absorption (SA) caused by excited state absorption induced mass transport of the CuPcTs dissolved in dimethyl sulfoxide is observed in an open aperture Z-scan experiment with a 21-ps laser pulse. The nonsymmetrical transition from RSA to SA is ascribed neither to saturation of excited state absorption nor to thermal induced mass transport, the so-called Soret effect. In our consideration, strong nonlinear absorption causes the rapid accumulation of the non-uniform kinetic energy of the solute molecules. The non-uniform kinetic field in turn causes the migration of the solute molecules. Additionally, an energy-gradient-induced mass transport theory is presented to interpret the experimental results, and the theoretical calculations are also taken to fit our experimental results. (classical areas of phenomenology)

Excited State Spectra and Dynamics of Phenyl-Substituted Butadienes

DEFF Research Database (Denmark)

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

1994-01-01

indicate that phenyl torsional motion is not important to the excited-state dynamics and reveal alternative excited-state reaction pathways. The results demonstrate how molecular systems that are structually similar can exhibit different electronic properties and excited-state dynamics....

Calculation of the ground and excited states of the Ne2 molecule by the variational cellular method

International Nuclear Information System (INIS)

Dias, A.M.; Rosato, A.

1981-07-01

The potential curves for the ground state 1 Σ + sub(g) and for the first singlet excited state 1 Σ + sub (u) of the Ne 2 molecule are determined by the Variational Cellular Method. From these curves some spectroscopical constants are obtained. Ionization energies of the excited state 1 Σ + sub (u) are calculated. (Author) [pt

UV excitation of single DNA and RNA strands produces high yields of exciplex states between two stacked bases.

Science.gov (United States)

Takaya, Tomohisa; Su, Charlene; de La Harpe, Kimberly; Crespo-Hernández, Carlos E; Kohler, Bern

2008-07-29

Excited electronic states created by UV excitation of the diribonucleoside monophosphates ApA, ApG, ApC, ApU, and CpG were studied by the femtosecond transient-absorption technique. Bleach recovery signals recorded at 252 nm show that long-lived excited states are formed in all five dinucleosides. The lifetimes of these states exceed those measured in equimolar mixtures of the constituent mononucleotides by one to two orders of magnitude, indicating that electronic coupling between proximal nucleobases dramatically slows the relaxation of excess electronic energy. The decay rates of the long-lived states decrease with increasing energy of the charge-transfer state produced by transferring an electron from one base to another. The charge-transfer character of the long-lived states revealed by this analysis supports their assignment to excimer or exciplex states. Identical bleach recovery signals were seen for ApA, (A)(4), and poly(A) at delay times >10 ps after photoexcitation. This indicates that excited states localized on a stack of just two bases are the common trap states independent of the number of stacked nucleotides. The fraction of initial excitations that decay to long-lived exciplex states is approximately equal to the fraction of stacked bases determined by NMR measurements. This supports a model in which excitations associated with two stacked bases decay to exciplex states, whereas excitations in unstacked bases decay via ultrafast internal conversion. These results establish the importance of charge transfer-quenching pathways for UV-irradiated RNA and DNA in room-temperature solution.

Optimized RVB states of the 2-d antiferromagnet: ground state and excitation spectrum

Science.gov (United States)

Chen, Yong-Cong; Xiu, Kai

1993-10-01

The Gutzwiller projection of the Schwinger-boson mean-field solution of the 2-d spin- {1}/{2} antiferromagnet in a square lattice is shown to produce the optimized, parameter-free RVB ground state. We get -0.6688 J/site and 0.311 for the energy and the staggered magnetization. The spectrum of the excited states is found to be linear and gapless near k≅0. Our calculation suggests, upon breaking of the rotational symmetry, ɛ k≅2JZ r1-γ 2k with Zr≅1.23.

Multimode optical fibers: steady state mode exciter.

Science.gov (United States)

Ikeda, M; Sugimura, A; Ikegami, T

1976-09-01

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

Use of a 3-MV proton accelerator for study of noble gases, including laser ionization of excited states

International Nuclear Information System (INIS)

Hurst, G.S.; Judish, J.P.; Nayfeh, M.H.; Parks, J.E.; Payne, M.G.; Wagner, E.B.

1974-01-01

The use of a pulsed 3-MV accelerator to study energy pathways in the noble gases is described. The objectives of pathways research are to obtain (1) information on the spectrum of excited states produced by a charged particle in a noble gas, (2) the rate of decay of the various states through various channels as a function of gas pressure, and (3) the modification of the decay channels due to the introduction of foreign species. A new energy pathways model is presented for helium as a general illustration. A method for the study of excited states, using a laser ionization technique is reported. Use is made of a laser which is tuned to a resonance transition between the desired excited state and some higher excited state. Photons in the same pulse photoionize the higher excited state; thus the ionization current vs photon wavelength has a resonance structure. Absolute yields of selected excited states can be obtained whenever the photon fluence per pulse is large enough to saturate the ionization current. A general summary is given of experimental facilities which include a 3-MV Van de Graaff accelerator, electronics for measuring radiation lifetimes, vacuum ultraviolet spectrometers, and a pulsed laser facility for direct study of excited states. Finally, the relevance of pathways research to (1) the interaction of radiation with matter, (2) the development of gas lasers, and (3) methods of ultrasensitive elemental analysis is pointed out

Generalization of the variational principle and the Hohenberg and Kohn theorems for excited states of Fermion systems

Energy Technology Data Exchange (ETDEWEB)

Gonis, A., E-mail: gonis@comcast.net

2017-01-05

Through the entanglement of a collection of K non-interacting replicas of a system of N interacting Fermions, and making use of the properties of reduced density matrices the variational principle and the theorems of Hohenberg and Kohn are generalized to excited states. The generalization of the variational principle makes use of the natural orbitals of an N-particle density matrix describing the state of lowest energy of the entangled state. The extension of the theorems of Hohenberg and Kohn is based on the ground-state formulation of density functional theory but with a new interpretation of the concept of a ground state: It is the state of lowest energy of a system of KN Fermions that is described in terms of the excited states of the N-particle interacting system. This straightforward implementation of the line of reasoning of ground-state density functional theory to a new domain leads to a unique and logically valid extension of the theory to excited states that allows the systematic treatment of all states in the spectrum of the Hamiltonian of an interacting system. - Highlights: • Use of entanglement in connection with the properties of density matrices. • An anti-symmetric entangled state of order KN expressed in terms of excited states of an interacting N-particle system.

Energy conservation attenuates the loss of skeletal muscle excitability during intense contractions

DEFF Research Database (Denmark)

Macdonald, W A; Ørtenblad, N; Nielsen, Ole Bækgaard

2007-01-01

High-frequency stimulation of skeletal muscle has long been associated with ionic perturbations, resulting in the loss of membrane excitability, which may prevent action potential propagation and result in skeletal muscle fatigue. Associated with intense skeletal muscle contractions are large...... with control muscles, the resting metabolites ATP, phosphocreatine, creatine, and lactate, as well as the resting muscle excitability as measured by M-waves, were unaffected by treatment with BTS plus dantrolene. Following 20 or 30 s of continuous 60-Hz stimulation, BTS-plus-dantrolene-treated muscles showed...... changes in muscle metabolites. However, the role of metabolites in the loss of muscle excitability is not clear. The metabolic state of isolated rat extensor digitorum longus muscles at 30 degrees C was manipulated by decreasing energy expenditure and thereby allowed investigation of the effects of energy...

Electron energy distribution functions and thermalization times in methane and in argon--methane mixtures: An effect of vibrational excitation processes

International Nuclear Information System (INIS)

Krajcar-Bronic, I.; Kimura, M.

1995-01-01

Electron thermalization in methane and argon--methane mixtures is studied by using the Boltzmann equation. The presence of low-lying vibrational excited states in methane significantly changes electron energy distribution functions and relaxation times. We found that (i) the mean electron energy just below the first vibrational excited state is reached faster by 1000 times when the vibrational states are taken into account, and (ii) electron energy distribution functions have distinct peaks at energy intervals equal to the vibrational threshold energies. Both these effects are due to large vibrational stopping cross section. The thermalization time in mixtures of argon--methane (without vibrational states) smoothly changes as the mixture composition varies, and no significant difference in the electron energy distribution function is observed. When the vibrational excited states are taken into account, thermalization is almost completely defined by CH 4 , even at very low fractional concentrations of CH 4 . The sensitivity of the electron energy distribution functions on the momentum transfer cross sections used in calculation on the thermalization is discussed. copyright 1995 American Institute of Physics

Electron-tunneling observation of localized excited states in superconducting manganese-doped lead

International Nuclear Information System (INIS)

Tsang, J.; Ginsberg, D.M.

1980-01-01

We have made electron-tunneling measurements on a dilute, superconducting lead-manganese alloy. A well-defined structure was observed in the ac-conductance--voltage curves, indicating excited states within the BCS energy gap. These states were partially accounted for by Shiba theory when spin-dependent s-, p-, and d-wave scattering were included. The phase shifts used in doing that were the results of band calculations. The experimental data also show the existence of a broad background density of states in the energy gap, which cannot be accounted for by the theory

High-energy double photoeffect and photoionization with excitation from 2 {sup 1}S and 2 {sup 3}S states of helium-like ions

Energy Technology Data Exchange (ETDEWEB)

Amusia, M.Ya. [The Racah Institute of Physics, Hebrew University, 91904 Jerusalem (Israel); A F Ioffe Physical-Technical Institute, 194921 St Petersburg (Russian Federation); Mikhailov, A.I.; Mikhailov, I.A. [St Petersburg Nuclear Physics Institute, Gatchina, 188350 St Petersburg (Russian Federation)

1999-10-28

Double ionization and ionization with excitation of helium-like ions with Z>>1 from 2 {sup 1}S and 2 {sup 3}S states on the absorption of a high-frequency photon have been considered. The analytical calculation is performed in the non-relativistic photon energy range in the lowest order of perturbation theory in the inter-electron interaction. Coulomb wavefunctions and the Coulomb Green function are used as a zeroth-order approximation. Differential and total cross sections of the processes are expressed via the corresponding values for the single photoionization. The photoelectron energy spectrum is obtained in the marginal energy range (i.e. for p{sub 1}>>p{sub 2}, p{sub 1} and p{sub 2} momenta of photoelectrons) for the double-ionization process. Simple relations between the cross sections of double ionization and ionization with excitation are derived. (author)

The structure of 83Sr excited states

International Nuclear Information System (INIS)

Liptak, J.; Kristiak, J.; Kristiakova, K.

1976-01-01

The β-decay of 83 Y isomers (7.06 min and 2.85 min) have been studied by means of Ge(Li) detectors. The proposed level scheme of the 83 Sr nucleus is based on the coincidence measurement and the analysis of energy sums. The intensity balance requirement leads to αsub(T)(35.5keV)=3.2 which is consistent with M1 multipolarity of this transition. A probable structure of some of the excited states in the 83 Sr nucleus is discussed in the frame work of Alaga's model and Kuriyama's model

Photoionization of excited molecular states using multiphoton excitation techniques

International Nuclear Information System (INIS)

Dehmer, P.M.; Pratt, S.T.; Dehmer, J.L.

1984-01-01

Photoelectron spectra are reported for three photon resonant, four photon ionization of H 2 via the B 1 Σ/sub u/ + , v = 7 (J = 2,4) and C 1 π/sub u'/, v = 0-4 (J = 1) levels and of N 2 via the o 3 1 π/sub u'/, v = 1,2, b 1 π/sub u'/, v = 3-5, and c 1 π/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

Proton-hole and core-excited states in the semi-magic nucleus {sup 131}In{sub 82}

Energy Technology Data Exchange (ETDEWEB)

Taprogge, J. [Instituto de Estructura de la Materia, CSIC, Madrid (Spain); Universidad Autonoma de Madrid, Departamento de Fisica Teorica, Madrid (Spain); RIKEN Nishina Center, RIKEN, Saitama (Japan); Jungclaus, A. [Instituto de Estructura de la Materia, CSIC, Madrid (Spain); Grawe, H. [GSI Helmholtzzentrum fuer Schwerionenforschung GmbH, Darmstadt (Germany); Borzov, I.N. [Kurchatov Institute, Moscow (Russian Federation); Joint Institute for Nuclear Research, Dubna (Russian Federation); Nishimura, S.; Doornenbal, P.; Soederstroem, P.A.; Baba, H.; Fukuda, N.; Inabe, N.; Isobe, T.; Kameda, D.; Kubo, T.; Shimizu, Y.; Suzuki, H.; Takeda, H.; Watanabe, H. [RIKEN Nishina Center, RIKEN, Saitama (Japan); Lorusso, G. [RIKEN Nishina Center, RIKEN, Saitama (Japan); National Physical Laboratory, NPL, Teddington, Middlesex (United Kingdom); University of Surrey, Department of Physics, Guildford (United Kingdom); Simpson, G.S.; Drouet, F. [LPSC, Universite Joseph Fourier Grenoble 1, CNRS/IN2P3, Institut National Polytechnique de Grenoble, Grenoble Cedex (France); Sumikama, T. [Tohoku University, Department of Physics, Sendai, Miyagi (Japan); Xu, Z.Y.; Niikura, M. [University of Tokyo, Department of Physics, Tokyo (Japan); Browne, F. [RIKEN Nishina Center, RIKEN, Saitama (Japan); University of Brighton, School of Computing, Engineering and Mathematics, Brighton (United Kingdom); Gernhaeuser, R.; Steiger, K.; Muecher, D. [Technische Universitaet Muenchen, Physik Department E12, Garching (Germany); Gey, G. [RIKEN Nishina Center, RIKEN, Saitama (Japan); LPSC, Universite Joseph Fourier Grenoble 1, CNRS/IN2P3, Institut National Polytechnique de Grenoble, Grenoble Cedex (France); Institut Laue-Langevin, B.P. 156, Grenoble Cedex 9 (France); Jung, H.S. [Chung-Ang University, Department of Physics, Seoul (Korea, Republic of); Kim, G.D.; Kwon, Y.K. [Institute for Basic Science, Rare Isotope Science Project, Daejeon (Korea, Republic of); Kim, Y.K. [Institute for Basic Science, Rare Isotope Science Project, Daejeon (Korea, Republic of); Hanyang University, Department of Nuclear Engineering, Seoul (Korea, Republic of); Kojouharov, I.; Kurz, N.; Schaffner, H. [Joint Institute for Nuclear Research, Dubna (Russian Federation); Li, Z. [Peking University, School of Physics and State key Laboratory of Nuclear Physics and Technology, Beijing (China); Sakurai, H. [RIKEN Nishina Center, RIKEN, Saitama (Japan); University of Tokyo, Department of Physics, Tokyo (Japan); Vajta, Zs. [RIKEN Nishina Center, RIKEN, Saitama (Japan); MTA Atomki, P.O. Box 51, Debrecen (Hungary); Wu, J. [RIKEN Nishina Center, RIKEN, Saitama (Japan); Peking University, School of Physics and State key Laboratory of Nuclear Physics and Technology, Beijing (China); Yagi, A.; Nishibata, H.; Odahara, A. [Osaka University, Department of Physics, Toyonaka (Japan); Yoshinaga, K. [Tokyo University of Science, Department of Physics, Faculty of Science and Technology, Noda, Chiba (Japan); Benzoni, G. [INFN, Sezione di Milano, Milano (Italy); Boenig, S.; Ilieva, S.; Kroell, T. [Technische Universitaet Darmstadt, Institut fuer Kernphysik, Darmstadt (Germany); Chae, K.Y. [Sungkyunkwan University, Department of Physics, Suwon (Korea, Republic of); Coraggio, L.; Gargano, A. [Complesso Universitario di Monte S. Angelo, Istituto Nazionale di Fisica Nucleare, Napoli (Italy); Daugas, J.M. [CEA, DAM, DIF, Arpajon cedex (France); Gadea, A.; Montaner-Piza, A. [CSIC-Univ. of Valencia, Instituto de Fisica Corpuscular, Paterna (Spain); Itaco, N. [Seconda Universita di Napoli, Dipartimento di Matematica e Fisica, Caserta (Italy); Kondev, F.G. [Argonne National Laboratory, Nuclear Engineering Division, Argonne, IL (United States); Lane, G.J. [Australian National University, Department of Nuclear Physics, Research School of Physical Sciences and Engineering, Canberra (Australia); Moschner, K.; Wendt, A. [University of Cologne, IKP, Cologne (Germany); Naqvi, F. [Yale University, Wright Nuclear Structure Laboratory, New Haven, CT (United States); Orlandi, R. [K.U. Leuven, Instituut voor Kern- en StralingsFysica, Heverlee (Belgium); Japan Atomic Energy Agency, Advanced Science Research Center, Tokai, Ibaraki (Japan); Patel, Z.; Podolyak, Zs. [University of Surrey, Department of Physics, Guildford (United Kingdom)

2016-11-15

The β decay of the N = 83 nucleus {sup 131}Cd has been studied at the RIBF facility at the RIKEN Nishina Center. The main purpose of the study was to identify the position of the 1p{sub 3/2} and 0f{sub 5/2} proton-hole states and the energies of core-excited configurations in the semi-magic nucleus {sup 131}In. From the radiation emitted following the β decay, a level scheme of {sup 131}In was established and the β feeding to each excited state determined. Similarities between the single-particle transitions observed in the β decays of the N = 83 isotones {sup 132}In and {sup 131}Cd are discussed. Finally the excitation energies of several core-excited configurations in {sup 131}In are compared to QRPA and shell-model calculations. (orig.)

Shape resonances and the excitation of helium autoionising states by electrons in the 57-66 eV region

International Nuclear Information System (INIS)

Burgt, P.J.M. van der; Eck, J. van; Heideman, H.G.M.

1986-01-01

Optical excitation functions of singly excited helium states are presented, measured by detecting the yield of emitted photons as a function of the incident electron energy from 56 to 66 eV. Many structures are observed, which are caused by negative-ion resonances and by the decay of autoionising states followed by post-collision interaction. Some of the structures are interpreted as being caused by hitherto unknown shape resonances lying very close to the thresholds of a particular class of autoionising states. As these shape resonances almost exclusively decay to their respective parent (autoionising) states, thereby considerably enhancing the threshold excitation cross sections of these states, they can only be observed via the PCI effect on the excitation functions of (higher lying) singly excited states. Using the recently introduced supermultiplet classification for doubly excited states a selection rule for the near-threshold excitation of doubly excited states by electron impact is deduced from the measurements. Only states with large probabilities in the Wannier region of configuration space (where the two electrons are at nearly equal distances and on opposite sides of the nucleus) are strongly excited. It is pointed out that these states are precisely the states that can support the above mentioned shape resonances at their thresholds. (author)

Resonant states in 13C and 16,17O at high excitation energy

Science.gov (United States)

Rodrigues, M. R. D.; Borello-Lewin, T.; Miyake, H.; Duarte, J. L. M.; Rodrigues, C. L.; Horodynski-Matsushigue, L. B.; Ukita, G. M.; Cappuzzello, F.; Cavallaro, M.; Foti, A.; Agodi, C.; Cunsolo, A.; Carbone, D.; Bondi, M.; De Napoli, M.; Roeder, B. T.; Linares, R.; Lombardo, I.

2014-12-01

The 9Be(6Li,d)13C and 12,13C(6Li,d)16,17O reactions were measured at the São Paulo Pelletron-Enge-Spectrograph facility at 25.5 MeV incident energy. The nuclear emulsion detection technique was applied. Several narrow resonances were populated up to approximately 17 MeV of excitation energy. An excellent energy resolution was obtained: 40 keV for 13C and 15-30 keV for 16O. The upper limit for the resonance widths were determined. Recently, d-a angular correlations were measured at θd = 0° with incident energy of 25 MeV using the LNS Tandem-MAGNEX Spectrometer facility.

Resonant states in 13C and 16,17O at high excitation energy

International Nuclear Information System (INIS)

Rodrigues, M R D; Borello-Lewin, T; Miyake, H; Duarte, J L M; Rodrigues, C L; Horodynski-Matsushigue, L B; Ukita, G M; Cappuzzello, F; Foti, A; Cavallaro, M; Agodi, C; Cunsolo, A; Carbone, D; Bondi, M; Napoli, M De; Roeder, B T; Linares, R; Lombardo, I

2014-01-01

The 9 Be( 6 Li,d) 13 C and 12,13 C( 6 Li,d) 16,17 O reactions were measured at the São Paulo Pelletron-Enge-Spectrograph facility at 25.5 MeV incident energy. The nuclear emulsion detection technique was applied. Several narrow resonances were populated up to approximately 17 MeV of excitation energy. An excellent energy resolution was obtained: 40 keV for 13 C and 15-30 keV for 16 O. The upper limit for the resonance widths were determined. Recently, d-a angular correlations were measured at θ d = 0° with incident energy of 25 MeV using the LNS Tandem-MAGNEX Spectrometer facility

Excitation-energy influence at the scission configuration

Directory of Open Access Journals (Sweden)

Ramos D.

2017-01-01

Full Text Available Transfer- and fusion-induced fission in inverse kinematics was proven to be a powerful tool to investigate nuclear fission, widening the information of the fission fragments and the access to unstable fissioning systems with respect to other experimental approaches. An experimental campaign for fission investigation has being carried out at GANIL with this technique since 2008. In these experiments, a beam of 238U, accelerated to 6.1 MeV/u, impinges on a 12C target. Fissioning systems from U to Cf are populated through transfer and fusion reactions, with excitation energies that range from few MeV up to 46 MeV. The use of inverse kinematics, the SPIDER telescope, and the VAMOS spectrometer permitted the characterization of the fissioning system in terms of mass, nuclear charge, and excitation energy, and the isotopic identification of the full fragment distribution. The neutron excess, the total neutron multiplicity, and the even-odd staggering in the nuclear charge of fission fragments are presented as a function of the excitation energy of the fissioning system. Structure effects are observed at Z∼50 and Z∼55, where their impact evolves with the excitation energy.

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

Energy Technology Data Exchange (ETDEWEB)

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.)

Relative excitation functions for singly-excited and core-excited levels of S V--S IX populated by the beam-foil interaction

International Nuclear Information System (INIS)

Moenke, D.; Bengtsson, P.; Engstroem, L.; Hutton, R.; Jupen, C.; Kirm, M.; Westerlind, M.

1994-01-01

We have investigated the relative excitation functions for low-lying singly excited and low-lying core-excited levels in S V (S 4+ ) to S IX (S 8+ ) after beam-foil excitation using ions in the energy range 2--10 MeV. The spectral line intensities have been normalized to the same number of particles at each ion energy and corrections for the level lifetimes have been made. The overall accuracy of the measured relative excitation function at each energy and charge state is estimated to be better than 2%. A comparison of the relative excitation functions for singly excited and core-excited lines shows a difference in S VII, but not in S VI

Observation of an excited Bc+/- meson state with the ATLAS detector

Czech Academy of Sciences Publication Activity Database

Aad, G.; Abbott, B.; Abdallah, J.; Böhm, Jan; Chudoba, Jiří; Havránek, Miroslav; Hejbal, Jiří; Jakoubek, Tomáš; Kepka, Oldřich; Kupčo, Alexander; Kůs, Vlastimil; Lokajíček, Miloš; Lysák, Roman; Marčišovský, Michal; Mikeštíková, Marcela; Němeček, Stanislav; Šícho, Petr; Staroba, Pavel; Svatoš, Michal; Taševský, Marek; Vrba, Václav

2014-01-01

Roč. 113, č. 21 (2014), "2120041"-"212004-5" ISSN 0031-9007 R&D Projects: GA MŠk(CZ) LG13009 Institutional support: RVO:68378271 Keywords : error * statistical * p p * scattering * B/c+ * ATLAS * meson * mass difference * CERN LHC Coll * excited state * ground state * J/psi(3100) * pi+ pi- Subject RIV: BF - Elementary Particles and High Energy Physics Impact factor: 7.512, year: 2014

Luminescence and excited state dynamics in Bi3+-doped LiLaP4O12 phosphates

International Nuclear Information System (INIS)

Babin, V.; Chernenko, K.; Demchenko, P.; Mihokova, E.; Nikl, M.; Pashuk, I.; Shalapska, T.; Voloshinovskii, A.; Zazubovich, S.

2016-01-01

Photo- and X-ray-excited luminescence characteristics of Bi-doped LiLaP 4 O 12 phosphates with different bismuth contents (from 1 to 25 at% in the melt) are investigated in the 4.2–300 K temperature range and compared with the characteristics of the undoped LiLaP 4 O 12 phosphate. The broad 2.95 eV emission band of LiLaP 4 O 12 :Bi excited around 5.4 eV is found to arise from the bismuth dopant. Relatively large FWHM and Stokes shift of the emission band and especially the data on the low-temperature decay kinetics of the 2.95 eV emission and its temperature dependence, indicating a very small spin-orbit splitting energy of the corresponding excited state, allow the conclusion that this emission arises from the radiative decay of the triplet state of an exciton localized around a Bi 3+ ion. No spectral bands are observed, arising from the electron transitions between the energy levels of Bi 3+ ions. Phenomenological model is proposed for the description of the excited state dynamics of the Bi 3+ -related localized exciton in LiLaP 4 O 12 :Bi and the parameters of the triplet localized exciton state are determined. Keywords: Photoluminescence; Time-resolved spectroscopy; Excited states; Bi 3+ centers; LiLaP 4 O 12 :Bi powders

Integrated light in direct excitation and energy transfer luminescence

OpenAIRE

Chimczak, Eugeniusz

2007-01-01

Integrated light in direct excitation and energy transfer luminescence has been investigated. In the investigations reported here, monomolecular centers were taken into account. It was found that the integrated light is equal to the product of generation rate and time of duration of excitation pulse for both direct excitation and energy transfer luminescence.

Electron impact excitation of helium: A ploarization correlation study of the 31P state at 40 eV incident energy

International Nuclear Information System (INIS)

Harris, C.L.; Dorio, L.A.; Neill, P.A.

1996-01-01

Recently the Convergent Close-Coupling calculations, (CCC), of Fursa and Bray have been very successful predicting the behavior of the electron impact coherence parameters (EICP) for electron impact excitation of helium. In the present experimental study the linear Stokes parameters P 1 and P 2 have been measured for He(3 1 P) excitation using the polarization correlation technique. Data will be presented for electron impact energies of 40eV and 50eV. At present no other experimental data is available at 40eV. At 50eV angular correlation data measured using the VUV 3 1 P-1 1 S photons are available only out to a maximum electron scattering angle of 85 degrees. Due to the disadvantageous differential cross section and 40:1 branching ratio in favor of the VUV decay, the uncertainties in the present data are large. However, at selected electron scattering angles they are sufficient to distinguish the lack of convergence of the CCC predictions for the 69 state calculations (CCC69) in comparison with the 75 state model (CCC75). In particular at 50 eV incident electron energy and 120 degrees scattering angle the charge cloud alignment angles predicted by the two calculations differ by 90 degrees

Visible-Light-Mediated Excited State Relaxation in Semi-Synthetic Genetic Alphabet: d5SICS and dNaM.

Science.gov (United States)

Bhattacharyya, Kalishankar; Datta, Ayan

2017-08-25

The excited state dynamics of an unnatural base pair (UBP) d5SICS/dNaM were investigated by accurate ab-initio calculations. Time-dependent density functional and high-level multireference calculations (MS-CASPT2) were performed to elucidate the excitation of this UBP and its excited state relaxation mechanism. After excitation to the bright state S 2 (ππ*), it decays to the S 1 state and then undergoes efficient intersystem crossing to the triplet manifold. The presence of sulfur atom in d5SICS leads to strong spin-orbit coupling (SOC) and a small energy gap that facilitates intersystem crossing from S 1 (n s π*) to T 2 (ππ*) followed by internal conversion to T 1 state. Similarly in dNaM, the deactivation pathway follows analogous trends. CASPT2 calculations suggest that the S 1 (ππ*) state is a dark state below the accessible S 2 (ππ*) bright state. During the ultrafast deactivation, it exhibits bond length inversion. From S 1 state, significant SOC leads the population transfer to T 3 due to a smaller energy gap. Henceforth, fast internal conversion occurs from T 3 to T 2 followed by T 1 . From time-dependent trajectory surface hopping dynamics, it is found that excited state relaxation occurs on a sub-picosecond timescale in d5SICS and dNaM. Our findings strongly suggest that there is enough energy available in triplet state of UBP to generate reactive oxygen species and induce phototoxicity with respect to cellular DNA. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Performance of SOPPA-based methods in the calculation of vertical excitation energies and oscillator strengths

DEFF Research Database (Denmark)

Sauer, Stephan P. A.; Pitzner-Frydendahl, Henrik Frank; Buse, Mogens

2015-01-01

methods, the original SOPPA method as well as SOPPA(CCSD) and RPA(D) in the calculation of vertical electronic excitation energies and oscillator strengths is investigated for a large benchmark set of 28 medium-size molecules with 139 singlet and 71 triplet excited states. The results are compared...

Energy dependence of the ionization of highly excited atoms by collisions with excited atoms

International Nuclear Information System (INIS)

Shirai, T.; Nakai, Y.; Nakamura, H.

1979-01-01

Approximate analytical expressions are derived for the ionization cross sections in the high- and low-collision-energy limits using the improved impulse approximation based on the assumption that the electron-atom inelastic-scattering amplitude is a function only of the momentum transfer. Both cases of simultaneous excitation and de-excitation of one of the atoms are discussed. The formulas are applied to the collisions between two excited hydrogen atoms and are found very useful for estimating the cross sections in the wide range of collisions energies

Pressure dependence of excited-state charge-carrier dynamics in organolead tribromide perovskites

Science.gov (United States)

Liu, X. C.; Han, J. H.; Zhao, H. F.; Yan, H. C.; Shi, Y.; Jin, M. X.; Liu, C. L.; Ding, D. J.

2018-05-01

Excited-state charge-carrier dynamics governs the performance of organometal trihalide perovskites (OTPs) and is strongly influenced by the crystal structure. Characterizing the excited-state charge-carrier dynamics in OTPs under high pressure is imperative for providing crucial insights into structure-property relations. Here, we conduct in situ high-pressure femtosecond transient absorption spectroscopy experiments to study the excited-state carrier dynamics of CH3NH3PbBr3 (MAPbBr3) under hydrostatic pressure. The results indicate that compression is an effective approach to modulate the carrier dynamics of MAPbBr3. Across each pressure-induced phase, carrier relaxation, phonon scattering, and Auger recombination present different pressure-dependent properties under compression. Responsiveness is attributed to the pressure-induced variation in the lattice structure, which also changes the electronic band structure. Specifically, simultaneous prolongation of carrier relaxation and Auger recombination is achieved in the ambient phase, which is very valuable for excess energy harvesting. Our discussion provides clues for optimizing the photovoltaic performance of OTPs.

Simulations of the dissociation of small helium clusters with ab initio molecular dynamics in electronically excited states

International Nuclear Information System (INIS)

Closser, Kristina D.; Head-Gordon, Martin; Gessner, Oliver

2014-01-01

The dynamics resulting from electronic excitations of helium clusters were explored using ab initio molecular dynamics. The simulations were performed with configuration interaction singles and adiabatic classical dynamics coupled to a state-following algorithm. 100 different configurations of He 7 were excited into the 2s and 2p manifold for a total of 2800 trajectories. While the most common outcome (90%) was complete fragmentation to 6 ground state atoms and 1 excited state atom, 3% of trajectories yielded bound, He 2 * , and <0.5% yielded an excited helium trimer. The nature of the dynamics, kinetic energy release, and connections to experiments are discussed

Localized excitations and the geometry of the 1nπ* excited states of pyrazine

International Nuclear Information System (INIS)

Kleier, D.A.; Martin, R.L.; Wadt, W.R.; Moomaw, W.R.

1982-01-01

Previous theoretical work has shown that the lowest excited singlet state of pyrazine, the π* 1 B 3 u state, is best described in terms of interacting excitations localized on each nitrogen. The present work refines the localized excitation model and considers its implications for the geometry of the 1 B 3 u state. Hartree-Fock calculations show that the best single configuration description of the nπ* state has broken ( 1 B 1 ) symmetry with the excitation strongly localized at one end of the molcule. If the symmetry-restricted hf result is used for reference, this localization describes an important correlation effect. The excited-state geometry was probed using configuration interaction wave functions based on the symmetry-restricted orbitals, as well as properly symmetrized ''valance-bond'' wave functions based on the broken symmetry solutions. Both descriptions lead to a very flat potential for a b/sub 1u/ vibrational mode. This mode reduces the molecular geometry from D/sub 2h/ to C/sub 2v/. We present spectroscopic evidence of our own and of other workers which is consistent with such a flat potential

Multiconfiguration Pair-Density Functional Theory Outperforms Kohn-Sham Density Functional Theory and Multireference Perturbation Theory for Ground-State and Excited-State Charge Transfer.

Science.gov (United States)

Ghosh, Soumen; Sonnenberger, Andrew L; Hoyer, Chad E; Truhlar, Donald G; Gagliardi, Laura

2015-08-11

The correct description of charge transfer in ground and excited states is very important for molecular interactions, photochemistry, electrochemistry, and charge transport, but it is very challenging for Kohn-Sham (KS) density functional theory (DFT). KS-DFT exchange-correlation functionals without nonlocal exchange fail to describe both ground- and excited-state charge transfer properly. We have recently proposed a theory called multiconfiguration pair-density functional theory (MC-PDFT), which is based on a combination of multiconfiguration wave function theory with a new type of density functional called an on-top density functional. Here we have used MC-PDFT to study challenging ground- and excited-state charge-transfer processes by using on-top density functionals obtained by translating KS exchange-correlation functionals. For ground-state charge transfer, MC-PDFT performs better than either the PBE exchange-correlation functional or CASPT2 wave function theory. For excited-state charge transfer, MC-PDFT (unlike KS-DFT) shows qualitatively correct behavior at long-range with great improvement in predicted excitation energies.

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

Science.gov (United States)

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

2012-08-21

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

Atomic excitation and molecular dissociation by low energy electron collisions

International Nuclear Information System (INIS)

Weyland, Marvin

2016-01-01

In this work, momentum imaging experiments have been conducted for the electron impact excitation of metastable states in noble gases and for dissociative electron attachment (DEA) in polyatomic molecules. For the electron impact excitation study a new experimental technique has been developed which is able to measure the scattering angle distribution of the electrons by detection of the momentum transfer to the atoms. Momentum transfer images have been recorded for helium and neon at fixed electron impact energy close to the excitation threshold and good agreement with current R-matrix theory calculations was found. A new momentum imaging apparatus for negative ions has been built for the purpose of studying DEA in biologically relevant molecules. During this work, DEA was investigated in the molecules ammonia, water, formic acid, furan, pyridine and in two chlorofluorocarbons. Furthermore, the change of DEA resonance energies when molecules form clusters compared to monomers was investigated in ammonia and formic acid. The experimental results of most studied molecules could be compared to recent theoretical calculations and they support further development in the theoretical description of DEA. The new apparatus built in this work also delivered a superior momentum resolution compared to existing setups. This allows the momentum imaging of heavier fragments and fragments with lower kinetic energy.

Atomic excitation and molecular dissociation by low energy electron collisions

Energy Technology Data Exchange (ETDEWEB)

Weyland, Marvin

2016-11-16

In this work, momentum imaging experiments have been conducted for the electron impact excitation of metastable states in noble gases and for dissociative electron attachment (DEA) in polyatomic molecules. For the electron impact excitation study a new experimental technique has been developed which is able to measure the scattering angle distribution of the electrons by detection of the momentum transfer to the atoms. Momentum transfer images have been recorded for helium and neon at fixed electron impact energy close to the excitation threshold and good agreement with current R-matrix theory calculations was found. A new momentum imaging apparatus for negative ions has been built for the purpose of studying DEA in biologically relevant molecules. During this work, DEA was investigated in the molecules ammonia, water, formic acid, furan, pyridine and in two chlorofluorocarbons. Furthermore, the change of DEA resonance energies when molecules form clusters compared to monomers was investigated in ammonia and formic acid. The experimental results of most studied molecules could be compared to recent theoretical calculations and they support further development in the theoretical description of DEA. The new apparatus built in this work also delivered a superior momentum resolution compared to existing setups. This allows the momentum imaging of heavier fragments and fragments with lower kinetic energy.

Calculation of the ground and excited states of the Ne2 molecule by the Variational Cellular Method

International Nuclear Information System (INIS)

Dias, A.M.; Rosato, A.

1982-01-01

The potential curves for the ground 1 μ + sub(g) and for the first singlet excited state 1 μ + sub(u) of the Ne 2 molecule are determined by the Variational Cellular Method. From these curves some spectroscopical constants are obtained. Ionization energies of the excited state 1 μ + sub(u) are calculated. (Author) [pt

Energy dependence phase shift analysis of PI4He elastic scattering and the possibility of the (PI4He) excited states existence

International Nuclear Information System (INIS)

Nichitiu, F.; Falomkin, I.V.; Sapozhnikov, M.G.; Shcherbakov, Yu.A.; Piragino, G.

1981-06-01

In the 24 MeV-260 MeV kinetic energy interval, the energy dependent phase shift analysis of π 4 He elastic scattering is done. The eneray dependence is given by the rational fraction approximants of the partial S matrix. The search for the stable S matrix zero-pole pairs in the k and √s complex plane give some proofs for the existence of the (π 4 He) excited states in the S, P and probably D partial waves. (authors)

A pair natural orbital based implementation of CCSD excitation energies within the framework of linear response theory

Science.gov (United States)

Frank, Marius S.; Hättig, Christof

2018-04-01

We present a pair natural orbital (PNO)-based implementation of coupled cluster singles and doubles (CCSD) excitation energies that builds upon the previously proposed state-specific PNO approach to the excited state eigenvalue problem. We construct the excited state PNOs for each state separately in a truncated orbital specific virtual basis and use a local density-fitting approximation to achieve an at most quadratic scaling of the computational costs for the PNO construction. The earlier reported excited state PNO construction is generalized such that a smooth convergence of the results for charge transfer states is ensured for general coupled cluster methods. We investigate the accuracy of our implementation by applying it to a large and diverse test set comprising 153 singlet excitations in organic molecules. Already moderate PNO thresholds yield mean absolute errors below 0.01 eV. The performance of the implementation is investigated through the calculations on alkene chains and reveals an at most cubic cost-scaling for the CCSD iterations with the system size.

Eff icient energy back transfer from Ce{sup 3+} 5d state to Pr{sup 3+} {sup 1}D{sub 2} level in Lu{sub 3}Al{sub 5}O{sub 12} upon Pr{sup 3+} 4f5d excitation

Energy Technology Data Exchange (ETDEWEB)

Dan Wu [State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun 130033, Jilin (China); University of Chinese Academy of Sciences, Beijing 100049 (China); Hao, Zhendong; Zhang, Xia; Pan, Guo-Hui; Luo, Yongshi; Zhang, Ligong; Zhao, Haifeng [State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun 130033, Jilin (China); Zhang, Jiahua, E-mail: zhangjh@ciomp.ac.cn [State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun 130033, Jilin (China)

2017-06-15

The step energy transfers from Pr{sup 3+} 4f5d state to Ce{sup 3+} 5d state followed by energy back transfer from Ce{sup 3+} 5d state to Pr{sup 3+} {sup 1}D{sub 2} level are studied. The Ce{sup 3+}→Pr{sup 3+} energy back transfer upon Pr{sup 3+} 4f5d excitation is found to be more efficient than the normal Ce{sup 3+}→Pr{sup 3+} energy transfer upon Ce{sup 3+} 5d excitation. The efficient energy back transfer is attributed to preferential excitation of the Ce{sup 3+} ion with an adjacent Pr{sup 3+} surrounding in Pr{sup 3+}→Ce{sup 3+} energy transfer of the first step, whereas Ce{sup 3+} is excited randomly in the normal energy transfer. The efficiencies of Ce{sup 3+}→Pr{sup 3+} energy back transfer as a function of Ce{sup 3+} and Pr{sup 3+} concentration are evaluated, respectively.

Branching ratios of α-decay to ground and excited states of Fm, Cf, Cm and Pu

Science.gov (United States)

Hassanabadi, H.; Hosseini, S. S.

2018-06-01

We use the well-known Wentzel-Kramers-Brillouin (WKB) barrier penetration probability to calculate α-decay branching ratios for ground and excited states of heavy even-even nuclei of Fermium (248-254Fm), Californium (244-252Cf), Curium (238-248Cm) and Plutonium (234-244Pu) with 94 ≤Zp ≤100. We obtained the branching ratios for the excited states of daughter nucleus by the α-decay energy (Qα), the angular momentum of α-particle (ℓα), and the excitation probability of the daughter nucleus with the excitation energy of state ℓ in the daughter nucleus (i.e. Eℓ*). α-Decay half-lives have been evaluated by using the proximity potential model for the heavy even-even nuclei. We have reported the half-lives and compared the results with the experimental data. The theoretical branching ratios of α-transitions in our calculation are found to agree with the available experimental data well for 0+→ 0+, 0+→ 2+, 0+→ 4+, 0+→ 6+ and 0+ → 8+α-transitions.

Development and Application of Single-Referenced Perturbation and Coupled-Cluster Theories for Excited Electronic States

Science.gov (United States)

Lee, Timothy J.; Langhoff, Stephen R. (Technical Monitor)

1997-01-01

Recent work on the development of single-reference perturbation theories for the study of excited electronic states will be discussed. The utility of these methods will be demonstrated by comparison to linear-response coupled-cluster excitation energies. Results for some halogen molecules of interest in stratospheric chemistry will be presented.

Spectroscopy at the two-proton drip line: Excited states in 158W

Directory of Open Access Journals (Sweden)

D.T. Joss

2017-09-01

Full Text Available Excited states have been identified in the heaviest known even-Z N=84 isotone 158W, which lies in a region of one-proton emitters and the two-proton drip line. The observation of γ-ray transitions feeding the ground state establishes the excitation energy of the yrast 6+ state confirming the spin-gap nature of the α-decaying 8+ isomer. The 8+ isomer is also expected to be unbound to two-proton emission but no evidence for this decay mode was observed. An upper limit for the two-proton decay branch has been deduced as b2p≤ 0.17% at the 90% confidence level. The possibility of observing two-proton emission from multiparticle isomers in nearby nuclides is considered.

Spectroscopy at the two-proton drip line: Excited states in 158W

Science.gov (United States)

Joss, D. T.; Page, R. D.; Herzán, A.; Donosa, L.; Uusitalo, J.; Carroll, R. J.; Darby, I. G.; Andgren, K.; Cederwall, B.; Eeckhaudt, S.; Grahn, T.; Greenlees, P. T.; Hadinia, B.; Jakobsson, U.; Jones, P. M.; Julin, R.; Juutinen, S.; Leino, M.; Leppanen, A.-P.; Nyman, M.; O'Donnell, D.; Pakarinen, J.; Rahkila, P.; Sandzelius, M.; Sarén, J.; Scholey, C.; Seweryniak, D.; Simpson, J.; Sorri, J.

2017-09-01

Excited states have been identified in the heaviest known even-Z N = 84 isotone 158W, which lies in a region of one-proton emitters and the two-proton drip line. The observation of γ-ray transitions feeding the ground state establishes the excitation energy of the yrast 6+ state confirming the spin-gap nature of the α-decaying 8+ isomer. The 8+ isomer is also expected to be unbound to two-proton emission but no evidence for this decay mode was observed. An upper limit for the two-proton decay branch has been deduced as b2p ≤ 0.17% at the 90% confidence level. The possibility of observing two-proton emission from multiparticle isomers in nearby nuclides is considered.

Resonant excitation and the decay of autoionization states in a strong electromagnetic field

International Nuclear Information System (INIS)

Andryushin, A.I.; Kazakov, A.E.; Fedorov, M.V.

1985-01-01

Photoionization of atoms involving resonant excitation of the auto-ionization state is studied. The evolution of the total ionization probability, its dependence on the frequency of the resonance radiation and also the photoelectron energy spectrum are investigated. It is shown that the energy of the final state of the system may be localized either in the vicinity of E approximately Esub(α), where Esub(α) is the auto-ionization energy, or in the vicinity of E approximately Esub(α)+h/2πω where h/2πω is the quantum energy of the resonance radiation. The photoelectron specturum in the region E approximately Esub(α)+h/2πω as a whole is similar to the electron spectrum on photoionization of atoms involving resonance excitation of the bound state. A strong effect on the photoelectron spectrum in the region E approximately Esub(α) is exerted by interference of various decay channels of the ground state in the resonance field which leads to the appearance in the spectrum of a characteristic structure of the Fano type. Interence also affects the widths of the two spectral curves, the relatve amount of electrons in the two energy ranges and also other characteristics of the ionization process. It is shown that the presence of a noninterfering photoionization channel of the autoionization state ensures the finiteness of the swidths and heights of the spectral curves and the absence of complete ''coherency merging''

Vibronic coupling in the excited-states of carotenoids

Energy Technology Data Exchange (ETDEWEB)

Miki, Takeshi [Physikalisch-Chemisches Institut; Ruprecht-Karls-Universität Heidelberg; D-69120 Heidelberg; Germany; Buckup, Tiago [Physikalisch-Chemisches Institut; Ruprecht-Karls-Universität Heidelberg; D-69120 Heidelberg; Germany; Krause, Marie S. [Physikalisch-Chemisches Institut; Ruprecht-Karls-Universität Heidelberg; D-69120 Heidelberg; Germany; Southall, June [College of Medical; Veterinary, and Life Science; University of Glasgow; G12 8QQ Glasgow; UK; Cogdell, Richard J. [College of Medical; Veterinary, and Life Science; University of Glasgow; G12 8QQ Glasgow; UK; Motzkus, Marcus [Physikalisch-Chemisches Institut; Ruprecht-Karls-Universität Heidelberg; D-69120 Heidelberg; Germany

2016-01-01

The ultrafast femtochemistry of carotenoids is governed by the interaction between electronic excited states, which has been explained by the relaxation dynamics within a few hundred femtoseconds from the lowest optically allowed excited state S₂to the optically dark state S₁.

Excitation and charge transfer in low-energy hydrogen atom collisions with neutral iron

Science.gov (United States)

Barklem, P. S.

2018-05-01

Data for inelastic processes due to hydrogen atom collisions with iron are needed for accurate modelling of the iron spectrum in late-type stars. Excitation and charge transfer in low-energy Fe+H collisions is studied theoretically using a previously presented method based on an asymptotic two-electron linear combination of atomic orbitals model of ionic-covalent interactions in the neutral atom-hydrogen-atom system, together with the multi-channel Landau-Zener model. An extensive calculation including 166 covalent states and 25 ionic states is presented and rate coefficients are calculated for temperatures in the range 1000-20 000 K. The largest rates are found for charge transfer processes to and from two clusters of states around 6.3 and 6.6 eV excitation, corresponding in both cases to active 4d and 5p electrons undergoing transfer. Excitation and de-excitation processes among these two sets of states are also significant. Full Tables and rate coefficient data are only available at the CDS via anonymous ftp to cdsarc.u-strasbg.fr (130.79.128.5) or via http://cdsarc.u-strasbg.fr/viz-bin/qcat?J/A+A/612/A90

Restricted second random phase approximations and Tamm-Dancoff approximations for electronic excitation energy calculations

International Nuclear Information System (INIS)

Peng, Degao; Yang, Yang; Zhang, Peng; Yang, Weitao

2014-01-01

In this article, we develop systematically second random phase approximations (RPA) and Tamm-Dancoff approximations (TDA) of particle-hole and particle-particle channels for calculating molecular excitation energies. The second particle-hole RPA/TDA can capture double excitations missed by the particle-hole RPA/TDA and time-dependent density-functional theory (TDDFT), while the second particle-particle RPA/TDA recovers non-highest-occupied-molecular-orbital excitations missed by the particle-particle RPA/TDA. With proper orbital restrictions, these restricted second RPAs and TDAs have a formal scaling of only O(N 4 ). The restricted versions of second RPAs and TDAs are tested with various small molecules to show some positive results. Data suggest that the restricted second particle-hole TDA (r2ph-TDA) has the best overall performance with a correlation coefficient similar to TDDFT, but with a larger negative bias. The negative bias of the r2ph-TDA may be induced by the unaccounted ground state correlation energy to be investigated further. Overall, the r2ph-TDA is recommended to study systems with both single and some low-lying double excitations with a moderate accuracy. Some expressions on excited state property evaluations, such as 〈S ^2 〉 are also developed and tested

Restricted second random phase approximations and Tamm-Dancoff approximations for electronic excitation energy calculations

Energy Technology Data Exchange (ETDEWEB)

Peng, Degao; Yang, Yang; Zhang, Peng [Department of Chemistry, Duke University, Durham, North Carolina 27708 (United States); Yang, Weitao, E-mail: weitao.yang@duke.edu [Department of Chemistry and Department of Physics, Duke University, Durham, North Carolina 27708 (United States)

2014-12-07

In this article, we develop systematically second random phase approximations (RPA) and Tamm-Dancoff approximations (TDA) of particle-hole and particle-particle channels for calculating molecular excitation energies. The second particle-hole RPA/TDA can capture double excitations missed by the particle-hole RPA/TDA and time-dependent density-functional theory (TDDFT), while the second particle-particle RPA/TDA recovers non-highest-occupied-molecular-orbital excitations missed by the particle-particle RPA/TDA. With proper orbital restrictions, these restricted second RPAs and TDAs have a formal scaling of only O(N{sup 4}). The restricted versions of second RPAs and TDAs are tested with various small molecules to show some positive results. Data suggest that the restricted second particle-hole TDA (r2ph-TDA) has the best overall performance with a correlation coefficient similar to TDDFT, but with a larger negative bias. The negative bias of the r2ph-TDA may be induced by the unaccounted ground state correlation energy to be investigated further. Overall, the r2ph-TDA is recommended to study systems with both single and some low-lying double excitations with a moderate accuracy. Some expressions on excited state property evaluations, such as 〈S{sup ^2}〉 are also developed and tested.

Application of the Broad Energy Germanium detector: A technique for elucidating β-decay schemes which involve daughter nuclei with very low energy excited states

Energy Technology Data Exchange (ETDEWEB)

Venhart, M., E-mail: martin.venhart@savba.sk [Institute of Physics, Slovak Academy of Sciences, SK-84511 Bratislava (Slovakia); Wood, J.L. [Department of Physics, Georgia Institute of Technology, Atlanta GA 30332 (United States); Boston, A.J. [Institute of Physics, Slovak Academy of Sciences, SK-84511 Bratislava (Slovakia); Cocolios, T.E. [School of Physics and Astronomy, The University of Manchester, Manchester M13 9PL (United Kingdom); KU Leuven, Instituut voor Kern, en Stralingsfysica, B-3001 Leuven (Belgium); Harkness-Brennan, L.J.; Herzberg, R.-D.; Joss, D.T.; Judson, D.S. [Oliver Lodge Laboratory, University of Liverpool, Liverpool L69 7ZE (United Kingdom); Kliman, J.; Matoušek, V. [Institute of Physics, Slovak Academy of Sciences, SK-84511 Bratislava (Slovakia); Motyčák, Š. [Faculty of Electrical Engineering and Information Technology, Slovak University of Technology, SK-812 19 Bratislava (Slovakia); Page, R.D.; Patel, A. [Oliver Lodge Laboratory, University of Liverpool, Liverpool L69 7ZE (United Kingdom); Petrík, K.; Sedlák, M.; Veselský, M. [Institute of Physics, Slovak Academy of Sciences, SK-84511 Bratislava (Slovakia)

2017-03-21

A technique for elucidating β-decay schemes of isotopes with a large density of states at low excitation energy has been developed, in which a Broad Energy Germanium (BEGe) detector is used in conjunction with coaxial hyper-pure germanium detectors. The power of this technique is demonstrated using the example of {sup 183}Hg decay. Mass-separated samples of {sup 183}Hg were produced by a deposition of the low-energy radioactive-ion beam delivered by the ISOLDE facility at CERN. The excellent energy resolution of the BEGe detector allowed γ-ray energies to be determined with a precision of a few tens of eV, which was sufficient for the analysis of the Rydberg-Ritz combinations (in conjunction with γ-γ coincidences) in the level scheme. The timestamped structure of the data was used for unambiguous separation of γ rays arising from the decay of {sup 183}Hg from those due to the daughter decays.

Non-adiabatic Excited State Molecule Dynamics Modeling of Photochemistry and Photophysics of Materials

Energy Technology Data Exchange (ETDEWEB)

Nelson, Tammie Renee [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Tretiak, Sergei [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

2017-01-06

Understanding and controlling excited state dynamics lies at the heart of all our efforts to design photoactive materials with desired functionality. This tailor-design approach has become the standard for many technological applications (e.g., solar energy harvesting) including the design of organic conjugated electronic materials with applications in photovoltaic and light-emitting devices. Over the years, our team has developed efficient LANL-based codes to model the relevant photophysical processes following photoexcitation (spatial energy transfer, excitation localization/delocalization, and/or charge separation). The developed approach allows the non-radiative relaxation to be followed on up to ~10 ps timescales for large realistic molecules (hundreds of atoms in size) in the realistic solvent dielectric environment. The Collective Electronic Oscillator (CEO) code is used to compute electronic excited states, and the Non-adiabatic Excited State Molecular Dynamics (NA-ESMD) code is used to follow the non-adiabatic dynamics on multiple coupled Born-Oppenheimer potential energy surfaces. Our preliminary NA-ESMD simulations have revealed key photoinduced mechanisms controlling competing interactions and relaxation pathways in complex materials, including organic conjugated polymer materials, and have provided a detailed understanding of photochemical products and intermediates and the internal conversion process during the initiation of energetic materials. This project will be using LANL-based CEO and NA-ESMD codes to model nonradiative relaxation in organic and energetic materials. The NA-ESMD and CEO codes belong to a class of electronic structure/quantum chemistry codes that require large memory, “long-queue-few-core” distribution of resources in order to make useful progress. The NA-ESMD simulations are trivially parallelizable requiring ~300 processors for up to one week runtime to reach a meaningful restart point.

Rearrangements in ground and excited states

CERN Document Server

de Mayo, Paul

1980-01-01

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;

Even-parity resonances with synchrotron radiation from Laser Excited Lithium at 1s^22p State

Science.gov (United States)

Huang, Ming-Tie; Wehlitz, Ralf

2010-03-01

Correlated many-body dynamics is still one of the unsolved fundamental problems in physics. Such correlation effects can be most clearly studied in processes involving single atoms for their simplicity.Lithium, being the simplest open shell atom, has been under a lot of study. Most of the studies focused on ground state lithium. However, only odd parity resonances can be populated through single photon (synchrotron radiation) absorption from ground state lithium (1s^22s). Lithium atoms, after being laser excited to the 1s^22p state, allow the study of even parity resonances. We have measured some of the even parity resonances of lithium for resonant energies below 64 eV. A single-mode diode laser is used to excite lithium from 1s^22s ground state to 1s^22p (^2P3/2) state. Photoions resulting from the interaction between the excited lithium and synchrotron radiation were analyzed and collected by an ion time-of-flight (TOF) spectrometer with a Z- stack channel plate detector. The Li^+ ion yield was recorded while scanning the undulator along with the monochromator. The energy scans have been analyzed regarding resonance energies and parameters of the Fano profiles. Our results for the observed resonances will be presented.

Partial radiative recombination cross sections for excited states of hydrogen

International Nuclear Information System (INIS)

Fazio, P.M.

1984-01-01

In calculating the radiative recombination cross sections for interstellar H II regions, usually only the electric dipole term in the expansion of the interaction Hamiltonian is kept. The dipole and quadrupole transition strengths in closed analytical form are calculated here using the Coulomb wave functions because results for any electron energy and for recombination into any angular momentum state of hydrogen are needed. Several interesting effects are found. First, the transition probabilities are maximum for recombination into specific intermediate angular momentum states at low energies (w < 2eV) and where the free state angular momentum is greater than that of the bound state. Further, that specific intermediate angular momentum state depends on the kinetic energy of the free electron. This behavior is in contrast to the normal behavior of the transition strengths where recombination into s states is greatest and decreases with increasing angular momentum. Second, the quadrupole matrix elements vanish for certain velocities of the free electron. This leads to minima in the corresponding quadrupole cross sections when plotted as a function of the free electron's kinetic energy. Finally, the partial cross sections for highly excited states are greater than previously calculated because of the additional effects of the quadrupole transitions

Product state resolved excitation spectroscopy of He-, Ne-, and Ar-Br2 linear isomers: experiment and theory.

Science.gov (United States)

Pio, Jordan M; van der Veer, Wytze E; Bieler, Craig R; Janda, Kenneth C

2008-04-07

Valence excitation spectra for the linear isomers of He-, Ne-, and Ar-Br2 are reported and compared to a two-dimensional simulation using the currently available potential energy surfaces. Excitation spectra from the ground electronic state to the region of the inner turning point of the Rg-Br2 (B,nu') stretching coordinate are recorded while probing the asymptotic Br2 (B,nu') state. Each spectrum is a broad continuum extending over hundreds of wavenumbers, becoming broader and more blueshifted as the rare gas atom is changed from He to Ne to Ar. In the case of Ne-Br2, the threshold for producing the asymptotic product state reveals the X-state linear isomer bond energy to be 71+/-3 cm(-1). The qualitative agreement between experiment and theory shows that the spectra can be correctly regarded as revealing the one-atom solvent shifts and also provides new insight into the one-atom cage effect on the halogen vibrational relaxation. The measured spectra provide data to test future ab initio potential energy surfaces in the interaction of rare gas atoms with the halogen valence excited state.

Obtaining Hartree-Fock and density functional theory doubly excited states with Car-Parrinello density matrix search

Science.gov (United States)

Liang, Wenkel; Isborn, Christine M.; Li, Xiaosong

2009-11-01

The calculation of doubly excited states is one of the major problems plaguing the modern day excited state workhorse methodology of linear response time dependent Hartree-Fock (TDHF) and density function theory (TDDFT). We have previously shown that the use of a resonantly tuned field within real-time TDHF and TDDFT is able to simultaneously excite both the α and β electrons to achieve the two-electron excited states of minimal basis H2 and HeH+ [C. M. Isborn and X. Li, J. Chem. Phys. 129, 204107 (2008)]. We now extend this method to many electron systems with the use of our Car-Parrinello density matrix search (CP-DMS) with a first-principles fictitious mass method for wave function optimization [X. Li, C. L. Moss, W. Liang, and Y. Feng, J. Chem. Phys. 130, 234115 (2009)]. Real-time TDHF/TDDFT is used during the application of the laser field perturbation, driving the electron density toward the doubly excited state. The CP-DMS method then converges the density to the nearest stationary state. We present these stationary state doubly excited state energies and properties at the HF and DFT levels for H2, HeH+, lithium hydride, ethylene, and butadiene.

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

International Nuclear Information System (INIS)

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

2008-01-01

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

Theory and computation of triply excited resonances: Application to states of He-

International Nuclear Information System (INIS)

Nicolaides, C.A.; Piangos, N.A.; Komninos, Y.

1993-01-01

Autoionizing multiply excited states offer unusual challenges to the theory of electronic structure and spectra because of the presence of strong electron correlations, of their occasional weak binding, of their proximity to more than one threshold, and of their degeneracy with many continua. Here we discuss a theory that addresses these difficulties in conjunction with the computation of their wave functions and intrinsic properties. Emphasis is given on the justification of the possible presence of self-consistently obtained open-channel-like (OCL) correlating configurations in the square-integrable representation of such states and on their effect on the energy E and the width Γ. Application of the theory has allowed the prediction of two hitherto unknown He - triply excited resonances, the 2s2p 2 2 P (E=59.71 eV, above the He ground state, Γ=79 meV) and the 2p 3 2 Do (E=59.46 eV, Γ=282 meV) (1 a.u.=27.2116 eV). These resonances are above the singly excited states of He and are embedded in its doubly excited spectrum. The relatively broad 2p 3 2 Do state interacts strongly with the He 2s2p 3 Po εd continuum. The effect of this interaction has been studied in terms of the coupling with fixed core scattering states as well as with a self-consistently computed OCL bound configuration

Optical energy transport and interactions between the excitations in a coumarin-perylene bisimide dendrimer

NARCIS (Netherlands)

Augulis, Ramunas; Pugzlys, Audrius; Hurenkamp, Johannes; Feringa, Ben L.; van Esch, Jan H.; van Loosdrecht, Paul H. M.

2007-01-01

Energy transfer properties of novel coumarin-perylene bisimide dendrimer are studied by means of steady state and time-resolved UV/vis spectroscopy. At low donor excitation density fast (transfer rate similar to 10 ps(-1)) and efficient (quantum yield similar to 99.5%) donor-acceptor energy transfer

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

Energy Technology Data Exchange (ETDEWEB)

Neves, R. F. C. [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide SA 5001 (Australia); Instituto Federal do Sul de Minas Gerais, Campus Poços de Caldas, Minas Gerais (Brazil); Departamento de Física, Universidade Federal de Juiz de Fora, 36036-330 Juiz de Fora, Minas Gerais (Brazil); Jones, D. B. [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide SA 5001 (Australia); Lopes, M. C. A. [Departamento de Física, Universidade Federal de Juiz de Fora, 36036-330 Juiz de Fora, Minas Gerais (Brazil); Blanco, F. [Departamento de Física Atómica, Molecular y Nuclear, Universidad Complutense de Madrid, 28040 Madrid (Spain); García, G. [Instituto de Física Fundamental, CSIC, Serrano 113-bis, 28006 Madrid (Spain); Ratnavelu, K. [Institute of Mathematical Sciences, University of Malaya, 50603 Kuala Lumpur (Malaysia); Brunger, M. J., E-mail: Michael.Brunger@flinders.edu.au [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide SA 5001 (Australia); Institute of Mathematical Sciences, University of Malaya, 50603 Kuala Lumpur (Malaysia)

2015-05-21

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

An experimental and theoretical investigation into the excited electronic states of phenol

Energy Technology Data Exchange (ETDEWEB)

Jones, D. B.; Chiari, L. [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, SA 5001 (Australia); Silva, G. B. da [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, SA 5001 (Australia); Universidade Federal de Mato Grosso, Barra do Garças, Mato Grosso (Brazil); Neves, R. F. C. [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, SA 5001 (Australia); Departamento de Física, UFJF, Juiz de Fora, MG (Brazil); Instituto Federal do Sul de Minas Gerais, Campus Poços de Caldas, Minas Gerais (Brazil); Duque, H. V. [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, SA 5001 (Australia); Departamento de Física, UFJF, Juiz de Fora, MG (Brazil); Oliveira, E. M. de; Lima, M. A. P. [Instituto de Física “Gleb Wataghin,” Universidade Estadual de Campinas, 13083-859 Campinas, São Paulo (Brazil); Lopes, M. C. A. [Departamento de Física, UFJF, Juiz de Fora, MG (Brazil); Costa, R. F. da [Centro de Ciências Naturais e Humanas, Universidade Federal do ABC, 09210-580 Santo André, São Paulo (Brazil); Varella, M. T. do N. [Instituto de Física, Universidade de São Paulo, CP 66318, 05315-970 São Paulo (Brazil); Bettega, M. H. F. [Departamento de Física, Universidade Federal do Paraná, CP 19044, 81531-990 Curitiba, Paraná (Brazil); and others

2014-08-21

We present experimental electron-energy loss spectra (EELS) that were measured at impact energies of 20 and 30 eV and at angles of 90° and 10°, respectively, with energy resolution ∼70 meV. EELS for 250 eV incident electron energy over a range of angles between 3° and 50° have also been measured at a moderate energy resolution (∼0.9 eV). The latter spectra were used to derive differential cross sections and generalised oscillator strengths (GOS) for the dipole-allowed electronic transitions, through normalization to data for elastic electron scattering from benzene. Theoretical calculations were performed using time-dependent density functional theory and single-excitation configuration interaction methods. These calculations were used to assign the experimentally measured spectra. Calculated optical oscillator strengths were also compared to those derived from the GOS data. This provides the first investigation of all singlet and triplet excited electronic states of phenol up to the first ionization potential.

Ab Initio Potential Energy Surfaces for Both the Ground (X̃1A′ and Excited (A∼1A′′ Electronic States of HSiBr and the Absorption and Emission Spectra of HSiBr/DSiBr

Directory of Open Access Journals (Sweden)

Anyang Li

2012-01-01

Full Text Available Ab initio potential energy surfaces for the ground (X̃1A′ and excited (A˜A′′1 electronic states of HSiBr were obtained by using the single and double excitation coupled-cluster theory with a noniterative perturbation treatment of triple excitations and the multireference configuration interaction with Davidson correction, respectively, employing an augmented correlation-consistent polarized valence quadruple zeta basis set. The calculated vibrational energy levels of HSiBr and DSiBr of the ground and excited electronic states are in excellent agreement with the available experimental band origins. In addition, the absorption and emission spectra of HSiBr and DSiBr were calculated using an efficient single Lanczos propagation method and are in good agreement with the available experimental observations.

Study of a Quantum Dot in an Excited State

Science.gov (United States)

Slamet, Marlina; Sahni, Viraht

We have studied the first excited singlet state of a quantum dot via quantal density functional theory (QDFT). The quantum dot is represented by a 2D Hooke's atom in an external magnetostatic field. The QDFT mapping is from an excited singlet state of this interacting system to one of noninteracting fermions in a singlet ground state. The results of the study will be compared to (a) the corresponding mapping from a ground state of the quantum dot and (b) to the similar mapping from an excited singlet state of the 3D Hooke's atom.

Excited-state absorption and fluorescence dynamics of Er3+:KY3F10

Science.gov (United States)

Labbé, C.; Doualan, J. L.; Moncorgé, R.; Braud, A.; Camy, P.

2018-05-01

We report here on a complete investigation of the excited-state absorption and fluorescence dynamics of Er3+ doped KY3F10 single crystals versus dopant concentrations and optical excitation conditions. Radiative and effective (including non-radiative relaxations) emission lifetimes and branching ratios are determined from a Judd-Ofelt analysis of the absorption spectra and via specific fluorescence experiments using wavelength selective laser excitations. Excited-state absorption and emission spectra are registered within seven spectral domains, i.e. 560 nm, 650 nm, 710 nm, 810 nm, 970 nm, 1550 nm and 2750 nm. A maximum gain cross-section of 0.93 × 10-21 cm2 is determined at the potential laser wavelength of 2.801 μm for a population ratio of 0.48. Saturation of fluorescence intensities and variations of population ratios versus pumping rates are registered and confronted with a rate equation model to derive the rates of the most important up-conversion and cross-relaxation energy transfers occurring at high dopant concentrations.

Multireference excitation energies for bacteriochlorophylls A within light harvesting system 2

DEFF Research Database (Denmark)

Anda, Andre; Hansen, Thorsten; De Vico, Luca

2016-01-01

Light-harvesting system 2 (LH2) of purple bacteria is one of the most popular antenna complexes used to study Nature's way of collecting and channeling solar energy. The dynamics of the absorbed energy is probed by ultrafast spectroscopy. Simulation of these experiments relies on fitting a range...... bacteriochlorophylls in LH2. We find that the excitation energies vary among the bacteriochlorophyll monomers and that they are regulated by the curvature of the macrocycle ring and the dihedral angle of an acetyl moiety. Increasing the curvature lifts the ground state energy, which causes a red shift...

State-selective charge transfer and excitation in ion-ion interactions at intermediate and high energies

International Nuclear Information System (INIS)

Samanta, R; Purkait, M

2012-01-01

Boundary Corrected Continuum Intermediate State (BCCIS) approximation and Classical Trajectory Monte Carlo (CTMC) methods are applied to calculate the charge transfer and excitation cross sections for ion-ion collisions.

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

Science.gov (United States)

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

2017-08-01

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

Singlet versus Triplet Excited State Mediated Photoinduced Dehalogenation Reactions of Itraconazole in Acetonitrile and Aqueous Solutions.

Science.gov (United States)

Zhu, Ruixue; Li, Ming-de; Du, Lili; Phillips, David Lee

2017-04-06

Photoinduced dehalogenation of the antifungal drug itraconazole (ITR) in acetonitrile (ACN) and ACN/water mixed solutions was investigated using femtosecond and nanosecond time-resolved transient absorption (fs-TA and ns-TA, respectively) and nanosecond time-resolved resonance Raman spectroscopy (ns-TR 3 ) experiments. An excited resonance energy transfer is found to take place from the 4-phenyl-4,5-dihydro-3H-1,2,4-triazol-3-one part of the molecule to the 1,3-dichlorobenzene part of the molecule when ITR is excited by ultraviolet light. This photoexcitation is followed by a fast carbon-halogen bond cleavage that leads to the generation of radical intermediates via either triplet and/or singlet excited states. It is found that the singlet excited state-mediated carbon-halogen cleavage is the predominant dehalogenation process in ACN solvent, whereas a triplet state-mediated carbon-halogen cleavage prefers to occur in the ACN/water mixed solutions. The singlet-to-triplet energy gap is decreased in the ACN/water mixed solvents and this helps facilitate an intersystem crossing process, and thus, the carbon-halogen bond cleavage happens mostly through an excited triplet state in the aqueous solutions examined. The ns-TA and ns-TR 3 results also provide some evidence that radical intermediates are generated through a homolytic carbon-halogen bond cleavage via predominantly the singlet excited state pathway in ACN but via mainly the triplet state pathway in the aqueous solutions. In strong acidic solutions, protonation at the oxygen and/or nitrogen atoms of the 1,2,4-triazole-3-one group appears to hinder the dehalogenation reactions. This may offer the possibility that the phototoxicity of ITR due to the generation of aryl or halogen radicals can be reduced by protonation of certain moieties in suitably designed ITR halogen-containing derivatives.

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

Science.gov (United States)

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

2018-04-17

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

Vibrational excitation of D2 by low energy electrons

International Nuclear Information System (INIS)

Buckman, S.J.; Phelps, A.V.

1985-01-01

Excitation coefficients for the production of vibrationally exicted D 2 by low energy electrons have been determined from measurements of the intensity of infrared emission from mixtures of D 2 and small concentrations of CO 2 or CO. The measurements were made using the electron drift tube technique and covered electric field to gas density ratios (E/n) from (5 to 80) x 10 -21 V m 2 , corresponding to mean electron energies between 0.45 and 4.5 eV. The CO 2 and CO concentrations were chosen to allow efficient excitation transfer from the D 2 to the carbon containing molecule, but to minimize direct excitation of the CO 2 or CO. The measured infrared intensities were normalized to predicted values for N 2 --CO 2 and N 2 --CO mixtures at E/n where the efficiency of vibrational excitation is known to be very close to 100%. The experimental excitation coefficients are in satisfactory agreement with predictions based on electron--D 2 cross sections at mean electron energies below 1 eV, but are about 50% too high at mean energies above about 2 eV. Application of the technique to H 2 did not yield useful vibrational excitation coefficients. The effective coefficients in H 2 --CO 2 mixtures were a factor of about 3 times the predicted values. For our H 2 --CO mixtures the excitation of CO via excitation transfer from H 2 is small compared to direct electron excitation of CO molecules. Published experiments and theories on electron--H 2 and electron--D 2 collisions are reviewed to obtain the cross sections used in the predictions

Mean excitation energies for use in Bethe's stopping-power formula

International Nuclear Information System (INIS)

Berger, M.J.; Seltzer, S.M.

1983-01-01

A review has been made of the mean excitation energies that can be derived from the analysis of stopping-power and range measurements, and from semi-empirical dipole oscillator-strength distributions for gases and dielectric-response functions for solids. On the basis of this review, mean excitation energies have been selected for 43 elemental substances and 54 compounds. Additivity rules have also been considered which allow one to estimate the mean excitation energies for compounds for which no direct data are available. These additivity rules are based on the use of mean excitation energies for atomic constituents which, to a certain extent, take into account the effects of chemical binding and physical aggregation

Deconvolution of overlapping features in electron energy-loss spectra: the determination of absolute differential cross sections for electron-impact excitation of electronic states of molecules

International Nuclear Information System (INIS)

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

1996-06-01

A set of three computer programs is reported which allow for the deconvolution of overlapping molecular electronic state structure in electron energy-loss spectra, even in highly perturbed systems. This procedure enables extraction of absolute differential cross sections for electron-impact excitation of electronic states of diatomic molecules from electron energy-loss spectra. The first code in the sequence uses the Rydberg-Klein-Rees procedure to generate potential energy curves from spectroscopic constants, while the second calculates Franck-Condon factors by numerical solution of the Schroedinger equation, given the potential energy curves. The third, given these Franck-Condon factors, the previously calculated relevant energies for the vibrational levels of the respective electronic states and the experimental energy-loss spectra, extracts the differential cross sections for each state. Each program can be run independently, or the three can run in sequence to determine these cross sections from the spectroscopic constants and the experimental energy-loss spectra. The application of these programs to the specific case of electron scattering from nitric oxide (NO) is demonstrated. 25 refs., 2 tabs., 2 figs

Intermolecular Modes between LH2 Bacteriochlorophylls and Protein Residues: The Effect on the Excitation Energies.

Science.gov (United States)

Anda, André; De Vico, Luca; Hansen, Thorsten

2017-06-08

Light-harvesting system 2 (LH2) executes the primary processes of photosynthesis in purple bacteria; photon absorption, and energy transportation to the reaction center. A detailed mechanistic insight into these operations is obscured by the complexity of the light-harvesting systems, particularly by the chromophore-environment interaction. In this work, we focus on the effects of the protein residues that are ligated to the bacteriochlorophylls (BChls) and construct potential energy surfaces of the ground and first optically excited state for the various BChl-residue systems where we in each case consider two degrees of freedom in the intermolecular region. We find that the excitation energies are only slightly affected by the considered modes. In addition, we see that axial ligands and hydrogen-bonded residues have opposite effects on both excitation energies and oscillator strengths by comparing to the isolated BChls. Our results indicate that only a small part of the chromophore-environment interaction can be associated with the intermolecular region between a BChl and an adjacent residue, but that it may be possible to selectively raise or lower the excitation energy at the axial and planar residue positions, respectively.

An experimentally validated bimorph cantilever model for piezoelectric energy harvesting from base excitations

International Nuclear Information System (INIS)

Erturk, A; Inman, D J

2009-01-01

Piezoelectric transduction has received great attention for vibration-to-electric energy conversion over the last five years. A typical piezoelectric energy harvester is a unimorph or a bimorph cantilever located on a vibrating host structure, to generate electrical energy from base excitations. Several authors have investigated modeling of cantilevered piezoelectric energy harvesters under base excitation. The existing mathematical modeling approaches range from elementary single-degree-of-freedom models to approximate distributed parameter solutions in the sense of Rayleigh–Ritz discretization as well as analytical solution attempts with certain simplifications. Recently, the authors have presented the closed-form analytical solution for a unimorph cantilever under base excitation based on the Euler–Bernoulli beam assumptions. In this paper, the analytical solution is applied to bimorph cantilever configurations with series and parallel connections of piezoceramic layers. The base excitation is assumed to be translation in the transverse direction with a superimposed small rotation. The closed-form steady state response expressions are obtained for harmonic excitations at arbitrary frequencies, which are then reduced to simple but accurate single-mode expressions for modal excitations. The electromechanical frequency response functions (FRFs) that relate the voltage output and vibration response to translational and rotational base accelerations are identified from the multi-mode and single-mode solutions. Experimental validation of the single-mode coupled voltage output and vibration response expressions is presented for a bimorph cantilever with a tip mass. It is observed that the closed-form single-mode FRFs obtained from the analytical solution can successfully predict the coupled system dynamics for a wide range of electrical load resistance. The performance of the bimorph device is analyzed extensively for the short circuit and open circuit resonance

Rotational Spectra in 29 Vibrationally Excited States of Interstellar Aminoacetonitrile

Energy Technology Data Exchange (ETDEWEB)

Kolesniková, L.; Alonso, E. R.; Mata, S.; Alonso, J. L. [Grupo de Espectroscopia Molecular (GEM), Edificio Quifima, Área de Química-Física, Laboratorios de Espectroscopia y Bioespectroscopia, Parque Científico UVa, Unidad Asociada CSIC, Universidad de Valladolid, E-47011 Valladolid (Spain)

2017-04-01

We report a detailed spectroscopic investigation of the interstellar aminoacetonitrile, a possible precursor molecule of glycine. Using a combination of Stark and frequency-modulation microwave and millimeter wave spectroscopies, we observed and analyzed the room-temperature rotational spectra of 29 excited states with energies up to 1000 cm{sup −1}. We also observed the {sup 13}C isotopologues in the ground vibrational state in natural abundance (1.1%). The extensive data set of more than 2000 new rotational transitions will support further identifications of aminoacetonitrile in the interstellar medium.

Electron-impact excitation of Zn II

International Nuclear Information System (INIS)

Msezane, A.Z.; Henry, R.J.W.

1982-01-01

Collision strengths are calculated for excitation of Zn II from the 4s ground state to excited states 4p, 3d 9 4s 2 , 5s, and 4d in a five-state close-coupling approximation for the electron-impact energy range 15 5 3d 10 4s 2 in a two-state close-coupling approximation for the same energy range. Accurate target functions are used in the expansion. Very good agreement with measurements of absolute emission cross sections of Rogers et al. is obtained for energy region 15< E<100 eV, when cascade contributions are included. Poorer agreement is obtained with experiment for excitation of the 5s state, owing to sensitivities in the close-coupling approximation

Measured lifetimes of states in 197Au and a critical comparison with the weak-coupling core-excitation model

International Nuclear Information System (INIS)

Bolotin, H.H.; Kennedy, D.L.; Linard, B.J.; Stuchbery, A.E.

1979-01-01

The lifetimes of five excited states in 197 Au up to an excitation energy of 885 keV were measured by the recoil-distance method (RDM). These levels were populated by Coulomb excitation using both 90 MeV 20 Ne and 120 MeV 35 Cl ion beams. The experimentally determined spectroscopy of the low-lying levels 3/2 + (ground state) and 1/2 + , (3/2) + 2 , 5/2 + and 7/2 + at 77.3, 268.8, 278.9, and 547.5 keV excitation energy, respectively, has been critically compared with the detailed predictions of the de-Shalit weak-coupling core-excitation model. When the model is taken to represent the case of a dsub(3/2) proton hole coupled to a 198 Hg core, the model parameters obtained are in accord with the criteria implicit for weak core coupling and, at the same time, are in remarkably good agreement with virtually all measured E2 and M1 transition rates. (Auth.)

Transfer matrices and excitations with matrix product states

International Nuclear Information System (INIS)

Zauner, V; Rams, M M; Verstraete, F; Draxler, D; Vanderstraeten, L; Degroote, M; Haegeman, J; Stojevic, V; Schuch, N

2015-01-01

We use the formalism of tensor network states to investigate the relation between static correlation functions in the ground state of local quantum many-body Hamiltonians and the dispersion relations of the corresponding low-energy excitations. In particular, we show that the matrix product state transfer matrix (MPS-TM)—a central object in the computation of static correlation functions—provides important information about the location and magnitude of the minima of the low-energy dispersion relation(s), and we present supporting numerical data for one-dimensional lattice and continuum models as well as two-dimensional lattice models on a cylinder. We elaborate on the peculiar structure of the MPS-TM’s eigenspectrum and give several arguments for the close relation between the structure of the low-energy spectrum of the system and the form of the static correlation functions. Finally, we discuss how the MPS-TM connects to the exact quantum transfer matrix of the model at zero temperature. We present a renormalization group argument for obtaining finite bond dimension approximations of the MPS, which allows one to reinterpret variational MPS techniques (such as the density matrix renormalization group) as an application of Wilson’s numerical renormalization group along the virtual (imaginary time) dimension of the system. (paper)

Populations of excited states and reaction mechanisms in the emission of complex fragments

International Nuclear Information System (INIS)

Gomez del Campo, J.

1990-01-01

Cross sections for emission of complex fragments (Z>2) in their ground and excited states are presented for several heavy-ion reactions at bombarding energies above 10 MeV/nucleon. Data presented are mostly on the cross sections extracted by γ-ray techniques. It is shown that a simple statistical approach to associate the ratio, of cross sections for excited states and ground states, to the temperature of the emitter fails to give the expected temperatures. However, it is shown that this is mostly due to the fact that the fragments that γ decay are secondary fragments, produced by the particle decay of the primary emitted complex fragments. A Hauser-Feshbach analysis accounts well for the cross sections and extracted temperatures. 22 refs., 6 figs

Neutron correlations in the decay of the first excited state of {sup 11}Li

Energy Technology Data Exchange (ETDEWEB)

Smith, J.K., E-mail: jsmith@triumf.ca [National Superconducting Cyclotron Laboratory, East Lansing, MI 48824 (United States); Department of Physics, Michigan State University, East Lansing, MI 48824 (United States); Baumann, T.; Bazin, D. [National Superconducting Cyclotron Laboratory, East Lansing, MI 48824 (United States); Brown, J. [Department of Physics, Wabash College, Crawfordsville, IN 47933 (United States); DeYoung, P.A. [Department of Physics, Hope College, Holland, MI 49422 (United States); Frank, N. [Department of Physics and Astronomy, Augustana College, Rock Island, IL 61201 (United States); Jones, M.D. [National Superconducting Cyclotron Laboratory, East Lansing, MI 48824 (United States); Department of Physics, Michigan State University, East Lansing, MI 48824 (United States); Kohley, Z. [National Superconducting Cyclotron Laboratory, East Lansing, MI 48824 (United States); Department of Chemistry, Michigan State University, East Lansing, MI 48824 (United States); Luther, B. [Department of Physics, Concordia College, Moorhead, MN 56562 (United States); Marks, B. [Department of Physics, Hope College, Holland, MI 49422 (United States); Spyrou, A. [National Superconducting Cyclotron Laboratory, East Lansing, MI 48824 (United States); Department of Physics, Michigan State University, East Lansing, MI 48824 (United States); Stephenson, S.L. [Department of Physics, Gettysburg College, Gettysburg, PA 17325 (United States); Thoennessen, M. [National Superconducting Cyclotron Laboratory, East Lansing, MI 48824 (United States); Department of Physics, Michigan State University, East Lansing, MI 48824 (United States); Volya, A. [Department of Physics, Florida State University, Tallahassee, FL 32306 (United States)

2016-11-15

The decay of unbound excited {sup 11}Li was measured after being populated by a two-proton removal from a {sup 13}B beam at 71 MeV/nucleon. Decay energy spectra and Jacobi plots were obtained from measurements of the momentum vectors of the {sup 9}Li fragment and neutrons. A resonance at an excitation energy of ∼1.2 MeV was observed. The kinematics of the decay are equally well fit by a simple dineutron-like model or a phase-space model that includes final state interactions. A sequential decay model can be excluded.

Neutron correlations in the decay of the first excited state of "1"1Li

International Nuclear Information System (INIS)

Smith, J.K.; Baumann, T.; Bazin, D.; Brown, J.; DeYoung, P.A.; Frank, N.; Jones, M.D.; Kohley, Z.; Luther, B.; Marks, B.; Spyrou, A.; Stephenson, S.L.; Thoennessen, M.; Volya, A.

2016-01-01

The decay of unbound excited "1"1Li was measured after being populated by a two-proton removal from a "1"3B beam at 71 MeV/nucleon. Decay energy spectra and Jacobi plots were obtained from measurements of the momentum vectors of the "9Li fragment and neutrons. A resonance at an excitation energy of ∼1.2 MeV was observed. The kinematics of the decay are equally well fit by a simple dineutron-like model or a phase-space model that includes final state interactions. A sequential decay model can be excluded.

Lifetime measurements of the excited states in {sup 145} Sm

Energy Technology Data Exchange (ETDEWEB)

El-Badry, A M; Abdel Samie, Sh; Ahmad, A A [Depatment of Physics, Faculty of Science, ElMinia University, ElMinia, (Egypt); Kuroyanagi, T; Odahara, A; Gono, Y; Morinobu, S [Tandem Accelerator Laboratory, Department of Physics, Kyushu University, (Japan)

1997-12-31

Lifetime of the excited levels in {sup 145} Sm has been measured through the {sup 139} La ({sup 10} B, 4 n){sup 145} Sm nuclear reaction. The optimal beam energy of 49 MeV was determined from the measurements of the excitation function and Cascade program. With the possibility of studying lifetime of this nucleus a conventional plunger system have been designed and constructed at kyushu University tandem accelerator laboratory. A La target of 0.22 mg/cm{sup 2} thickness which was evaporated onto a Au foil of 2 mg/cm{sup 2} thickness was used. Since the recoil velocity was estimated to be 1.76 mm/ns (beta 0.00585), the measurable time range resulted in the range from 5 Ps to 5 ns. The single spectra measurements were performed at the 20 plunger positions in the range from 10 {mu} to 10 mm. Analyses of the data were carried using hypermet and/or GF2 program to obtain the lifetimes. A new list of lifetimes for 12 excited states up to 3.922 MeV excitations for {sup 145} Sm were determined for the first time. Decay curves of the these transitions are discussed. The new lifetimes of excited states in {sup 145} Sm enabled us to understand the electromagnetic properties. The deduced transition probabilities were established and compared with that of N = 83 isotones and the closed shell nucleus {sup 144} Sm. In addition, a nuclear structure of {sup 145} Sm have been discussed and proposed in framework of the shell model. 4 figs., 1 tab.

General theory for environmental effects on (vertical) electronic excitation energies.

Science.gov (United States)

Schwabe, Tobias

2016-10-21

Almost 70 years ago, the first theoretical model for environmental effects on electronic excitation energies has been derived. Since then, several different interpretations and refined models have been proposed for the perichromic shift of a chromophore due to its surrounding medium. Some of these models are contradictory. Here, the contributing terms are derived within the framework of long-range perturbation theory with the least approximations so far. The derivation is based on a state-specific interpretation of the interaction energies and all terms can be identified with individual properties of either the chromophore or the surroundings, respectively. Further, the much debated contribution due to transition moments coupled to the environment can be verified in the form of a non-resonant excitonic coupling to the dynamic polarizabilities in the environment. These general insights should clarify discussions and interpretations of environmental effects on electronic excitations and should foster the development of new models for the computation of these effects.

Benchmarks for electronically excited states: Time-dependent density functional theory and density functional theory based multireference configuration interaction

DEFF Research Database (Denmark)

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

2008-01-01

Time-dependent density functional theory (TD-DFT) and DFT-based multireference configuration interaction (DFT/MRCI) calculations are reported for a recently proposed benchmark set of 28 medium-sized organic molecules. Vertical excitation energies, oscillator strengths, and excited-state dipole...

Probability of collective excited state decay

International Nuclear Information System (INIS)

Manykin, Eh.A.; Ozhovan, M.I.; Poluehktov, P.P.

1987-01-01

Decay mechanisms of condensed excited state formed of highly excited (Rydberg) atoms are considered, i.e. stability of so-called Rydberg substance is analyzed. It is shown that Auger recombination and radiation transitions are the basic processes. The corresponding probabilities are calculated and compared. It is ascertained that the ''Rydberg substance'' possesses macroscopic lifetime (several seconds) and in a sense it is metastable

Efficient Predictions of Excited State for Nanomaterials Using Aces 3 and 4

Science.gov (United States)

2017-12-20

energetics of the various isomers of the materials, obtained from computed heats of reactions that provide the enthalpy and free energy for the species... modeling , excited states, optical properties, structure, stability, activation barriers first principle methods, parallel computing 16. SECURITY...6 Figure 7. Charge- transfer from ethylene to tetrafluro ethylene

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

Science.gov (United States)

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

2018-03-01

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

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

Science.gov (United States)

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

2014-06-23

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

Photoluminescence and excited state structure in Bi3+-doped Y2SiO5 single crystalline films

International Nuclear Information System (INIS)

Babin, V.; Gorbenko, V.; Krasnikov, A.; Mihokova, E.; Nikl, M.; Zazubovich, S.; Zorenko, Yu.

2013-01-01

Single crystalline films of Bi-doped Y 2 SiO 5 are studied at 4.2–350 K by the time-resolved luminescence methods under excitation in the 3.8–6.2 eV energy range. Ultraviolet luminescence of Y 2 SiO 5 :Bi (≈3.6 eV) is shown to arise from the radiative decay of the metastable and radiative minima of the triplet relaxed excited state (RES) of Bi 3+ centers which are related to the 3 P 0 and 3 P 1 levels of a free Bi 3+ ion, respectively. The lowest-energy excitation band of this emission, located at ≈4.5 eV, is assigned to the 1 S 0 → 3 P 1 transitions of a free Bi 3+ ion. The phenomenological model is proposed to describe the excited-state dynamics of Bi 3+ centers in Y 2 SiO 5 :Bi, and parameters of the triplet RES are determined. -- Highlights: •Luminescence of Y 2 SiO 5 :Bi is investigated for the first time. •Ultraviolet emission arises from Bi 3+ ions located in Y lattice sites. •The triplet relaxed excited states parameters of Bi 3+ centers are determined

Estimation of excitation forces for wave energy converters control using pressure measurements

Science.gov (United States)

Abdelkhalik, O.; Zou, S.; Robinett, R.; Bacelli, G.; Wilson, D.

2017-08-01

Most control algorithms of wave energy converters require prediction of wave elevation or excitation force for a short future horizon, to compute the control in an optimal sense. This paper presents an approach that requires the estimation of the excitation force and its derivatives at present time with no need for prediction. An extended Kalman filter is implemented to estimate the excitation force. The measurements in this approach are selected to be the pressures at discrete points on the buoy surface, in addition to the buoy heave position. The pressures on the buoy surface are more directly related to the excitation force on the buoy as opposed to wave elevation in front of the buoy. These pressure measurements are also more accurate and easier to obtain. A singular arc control is implemented to compute the steady-state control using the estimated excitation force. The estimated excitation force is expressed in the Laplace domain and substituted in the control, before the latter is transformed to the time domain. Numerical simulations are presented for a Bretschneider wave case study.

Describing excited state relaxation and localization in TiO2 nanoparticles using TD-DFT

International Nuclear Information System (INIS)

Berardo, Enrico; Hu, Han-Shi; Van Dam, Hubertus J. J.; Shevlin, Stephen A.; Woodley, Scott M.; Kowalski, Karol; Zwijnenburg, Martijn A.

2014-01-01

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

On the determination of the mean excitation energy of water

DEFF Research Database (Denmark)

Sabin, John R.; Oddershede, Jens; Sauer, Stephan P. A.

2013-01-01

Water is a ubiquitous substance in nature, and thus the mean excitation energy of water is an important quantity for understanding and prediction of the details of many fast ion/molecule collision processes such as those involved in external beam radiotherapy of tumors. There are several methods...... for determining numerical values for a mean excitation energy for water, both theoretical and experimental. Here the factors affecting the determination of the value of the mean excitation energy of water, especially from experiment, are discussed....

Targeted energy transfers and passive acoustic wave redirection in a two-dimensional granular network under periodic excitation

Energy Technology Data Exchange (ETDEWEB)

Zhang, Yijing, E-mail: yzhng123@illinois.edu; Moore, Keegan J.; Vakakis, Alexander F. [Department of Mechanical Science and Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801 (United States); McFarland, D. Michael [Department of Aerospace Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801 (United States)

2015-12-21

We study passive pulse redirection and nonlinear targeted energy transfer in a granular network composed of two semi-infinite, ordered homogeneous granular chains mounted on linear elastic foundations and coupled by weak linear stiffnesses. Periodic excitation in the form of repetitive half-sine pulses is applied to one of the chains, designated as the “excited chain,” whereas the other chain is initially at rest and is regarded as the “absorbing chain.” We show that passive pulse redirection and targeted energy transfer from the excited to the absorbing chain can be achieved by macro-scale realization of the spatial analog of the Landau-Zener quantum tunneling effect. This is realized by finite stratification of the elastic foundation of the excited chain and depends on the system parameters (e.g., the percentage of stratification) and on the parameters of the periodic excitation. Utilizing empirical mode decomposition and numerical Hilbert transforms, we detect the existence of two distinct nonlinear phenomena in the periodically forced network; namely, (i) energy localization in the absorbing chain due to sustained 1:1 resonance capture leading to irreversible pulse redirection from the excited chain, and (ii) continuous energy exchanges in the form of nonlinear beats between the two chains in the absence of resonance capture. Our results extend previous findings of transient passive energy redirection in impulsively excited granular networks and demonstrate that steady state passive pulse redirection in these networks can be robustly achieved under periodic excitation.

High energy excitations in itinerant ferromagnets

International Nuclear Information System (INIS)

Prange, R.E.

1984-01-01

Itinerant magnets, those whose electrons move throughout the crystal, are described by band theory. Single particle excitations offer confirmation of band theory, but their description requires important corrections. The energetics of magnetism in iron and nickel is also described in band theory but requires complex bands. Magnetism above the critical temperature and the location of the critical temperature offer discriminants between the two major models of magnetism at high temperature and can be addressed by high energy excitations

A scalable piezoelectric impulse-excited energy harvester for human body excitation

International Nuclear Information System (INIS)

Pillatsch, P; Yeatman, E M; Holmes, A S

2012-01-01

Harvesting energy from low-frequency and non-harmonic excitations typical of human motion presents specific challenges. While resonant devices do have an advantage in environments where the excitation frequency is constant, and while they can make use of the entire proof mass travel range in the case of excitation amplitudes that are smaller than the internal displacement limit, they are not suitable for body applications since the frequencies are random and the amplitudes tend to be larger than the device size. In this paper a piezoelectric, impulse-excited approach is presented. A cylindrical proof mass actuates an array of piezoelectric bi-morph beams through magnetic attraction. After the initial excitation these transducers are left to vibrate at their natural frequency. This increases the operational frequency range as well as the electromechanical coupling. The principle of impulse excitation is discussed and a centimetre-scale functional model is introduced as a proof of concept. The obtained data show the influence of varying the frequency, acceleration and proof mass. Finally, a commercially available integrated circuit for voltage regulation is tested. At a frequency of 2 Hz and an acceleration of 2.7 m s −2 a maximal power output of 2.1 mW was achieved. (paper)

Role of methylene spacer in the excitation energy transfer in europium 1- and 2- naphthylcarboxylates

Energy Technology Data Exchange (ETDEWEB)

Zhuravlev, K. [V.A. Kotelnikov Institute of Radioengineering and Electronics of RAS, 1 Vvedenskii sq., Fryazino Moscow reg. 141190 (Russian Federation); Tsaryuk, V., E-mail: vit225@ire216.msk.s [V.A. Kotelnikov Institute of Radioengineering and Electronics of RAS, 1 Vvedenskii sq., Fryazino Moscow reg. 141190 (Russian Federation); Kudryashova, V.; Pekareva, I. [V.A. Kotelnikov Institute of Radioengineering and Electronics of RAS, 1 Vvedenskii sq., Fryazino Moscow reg. 141190 (Russian Federation); Sokolnicki, J. [Faculty of Chemistry, University of WrocLaw, 14 F. Joliot-Curie str., WrocLaw 50-383 (Poland); Yakovlev, Yu. [V.A. Kotelnikov Institute of Radioengineering and Electronics of RAS, 1 Vvedenskii sq., Fryazino Moscow reg. 141190 (Russian Federation)

2010-08-15

A series of compounds Ln(RCOO){sub 3}.Phen (Ln=Eu, Gd, Tb; RCOO{sup -}-1- and 2-naphthoate, 1- and 2-naphthylacetate, 1- and 2-naphthoxyacetate anions, Phen-1,10-phenanthroline) was investigated by methods of optical spectroscopy. Compounds of composition Ln(RCOO){sub 3}.nH{sub 2}O with the same carboxylate ligands are also considered. Results of studies of the effects of methylene spacer decoupling the {pi}-{pi}- or p-{pi}-conjugation in the naphthylcarboxylate ligand on the structure of Eu{sup 3+} coordination centre, on the lifetime of {sup 5}D{sub 0} (Eu{sup 3+}) state, and on processes of the excitation energy transfer to Eu{sup 3+} or Tb{sup 3+} ions are presented. Introduction of the methylene bridge in the ligand weakens the influence of the steric hindrances in forming of a crystal lattice and results in lowering the distortion of the Eu{sup 3+} luminescence centre, and in elongation of the observed {sup 5}D{sub 0} lifetime {tau}{sub obs}. The latter is caused by decrease in contribution of the radiative processes rate 1/{tau}{sub r}. This is confirmed by the correlation between the lifetimes {tau}{sub obs} and the quantities '{tau}{sub r}.const' inversely proportional to the total integral intensities of Eu(RCOO){sub 3}.Phen luminescence spectra. The methylene spacer performs a role of regulator of sensitization of the Ln{sup 3+} luminescence efficiency by means of an influence on mutual location of lowest triplet states of the ligands, the ligand-metal charge transfer (LMCT) states, and the emitting states of Ln{sup 3+} ions. The lowest triplet state in lanthanide naphthylcarboxylate adducts with Phen is related to carboxylate anion. A presence of the methylene spacer in naphthylcarboxylate ligand increases the triplet state energy. At the same time, the energy of 'carboxylic group-Eu{sup 3+} ion' charge transfer states falls, which can promote the degradation of excitation energy. In naphthylcarboxylates investigated a range of the

Power density and temperature dependent multi-excited states in InAs/GaAs quantum dots

International Nuclear Information System (INIS)

Bouzaïene, L.; Sfaxi, L.; Baira, M.; Maaref, H.; Bru-Chevallier, C.

2011-01-01

Self-assembled InAs/GaAs (001) quantum dots (QDs) were grown by molecular beam epitaxy using ultra low-growth rate. A typical dot diameter of around 28 ± 2 nm and a typical height of 5 ± 1 nm are observed based on atomic force microscopy image. The photoluminescence (PL) spectra, their power and temperature dependences have been studied for ground (GS) and three excited states (1–3ES) in InAs QDs. By changing the excitation power density, we can significantly influence the distribution of excitons within the QD ensemble. The PL peak energy positions of GS and ES emissions bands depend on an excitation light power. With increasing excitation power, the GS emission energy was red-shifted, while the 1–3ES emission energies were blue-shifted. It is found that the full width at half maximum of the PL spectra has unusual relationship with increasing temperature from 9 to 300 K. The temperature dependence of QD PL spectra shown the existence of two stages of PL thermal quenching and two distinct activation energies corresponding to the temperature ranges I (9–100 K) and II (100–300 K).

Excited-state lifetime measurements: Linearization of the Foerster equation by the phase-plane method

International Nuclear Information System (INIS)

Love, J.C.; Demas, J.N.

1983-01-01

The Foerster equation describes excited-state decay curves involving resonance intermolecular energy transfer. A linearized solution based on the phase-plane method has been developed. The new method is quick, insensitive to the fitting region, accurate, and precise

The use of dendrimers as high-performance shells for round-trip energy transfer: efficient trans-cis photoisomerization from an excited triplet state produced within a dendrimer shell.

Science.gov (United States)

Miura, Yousuke; Momotake, Atsuya; Takeuchi, Keiichirou; Arai, Tatsuo

2011-01-01

A series of stilbene-cored poly(benzyl ether) dendrimers with benzophenone peripheries were synthesized and their photophysical and photochemical properties were studied. Fluorescence studies revealed that singlet-singlet energy transfer (SSET) from the stilbene core to the benzophenone units took place efficiently in dendrimers of all generations. Similarly, phosphorescence and time-resolved spectroscopic measurements indicated efficient triplet-triplet energy transfer (TTET) from the benzophenone periphery to the stilbene core. Upon excitation at 310 nm, the stilbene core isomerizes via an energy round trip within the dendrimer shell. The quantum yields for the energy round trip (Φ(ERT)), defined as the product of the quantum yields of SSET, intersystem crossing, and TTET (Φ(ERT) = Φ(SS)Φ(isc)Φ(TT)), were extremely high for all generations--99%, 95% and 94% for G1, G2, and G3, respectively--which means that the excitation energy of the dendrimer core was transferred to the dendrimer periphery and back to the core almost quantitatively. The quantum yield for photoisomerization of G1-G3 via an energy round trip was higher than for other stilbene-cored dendrimers, which mainly isomerize from the excited singlet state. Photostability in the dendrimers was also demonstrated and discussed.

YIELDS OF IONS AND EXCITED STATES IN NONPOLAR LIQUIDS EXPOSED TO X-RAYS OF 1 TO 30 KEV ENERGY

International Nuclear Information System (INIS)

HOLROYD, R.A.

1999-01-01

When x-rays from a synchrotron source are absorbed in a liquid, the x-ray energy (E x ) is converted by the photoelectric effect into the kinetic energy of the electrons released. For hydrocarbons, absorption by the K-electrons of carbon dominates. Thus the energy of the photoelectron (E pe ) is E x -E b , where E b is the K-shell binding energy of carbon. Additional electrons with energy equal to E b is released in the Auger process that fills the hole in the K-shell. These energetic electrons will produce many ionizations, excitations and products. The consequences of the high density of ionizations and excitations along the track of the photoelectron and special effects near the K-edge are examined here

Fine structures of atomic excited states: precision atomic spectroscopy and electron-ion collision process

International Nuclear Information System (INIS)

Gao Xiang; Cheng Cheng; Li Jiaming

2011-01-01

Scientific research fields for future energies such as inertial confinement fusion researches and astrophysics studies especially with satellite observatories advance into stages of precision physics. The relevant atomic data are not only enormous but also of accuracy according to requirements, especially for both energy levels and the collision data. The fine structure of high excited states of atoms and ions can be measured by precision spectroscopy. Such precision measurements can provide not only knowledge about detailed dynamics of electron-ion interactions but also a bench mark examination of the accuracy of electron-ion collision data, especially incorporating theoretical computations. We illustrate that by using theoretical calculation methods which can treat the bound states and the adjacent continua on equal footing. The precision spectroscopic measurements of excited fine structures can be served as stringent tests of electron-ion collision data. (authors)

Excitation and decay of correlated atomic states

International Nuclear Information System (INIS)

Rau, A.R.P.

1992-01-01

Doubly excited states of atoms and ions in which two electrons are excited from the ground configuration display strong radial and angular electron correlations. They are prototypical examples of quantum-mechanical systems with strong coupling. Two distinguishing characteristics of these states are: (1) their organization into successive families, with only weak coupling between families, and (2) a hierarchical nature of this coupling, with states from one family decaying primarily to those in the next lower family. A view of the pair of electrons as a single entity, with the electron-electron repulsion between them divided into a adiabatic and nonadiabatic piece, accounts for many of the dominant features. The stronger, adiabatic part determines the family structure and the weaker, nonadiabatic part the excitation and decay between successive families. Similar considerations extend to three-electron atomic states, which group into five different classes. They are suggestive of composite models for quarks in elementary particle physics, which exhibit analogous groupings into families with a hierarchical arrangement of masses and electroweak decays. 49 refs., 6 figs., 2 tabs

Electron impact excitation and ionization of laser-excited sodium atoms Na*(7d)

International Nuclear Information System (INIS)

Nienhaus, J.; Dorn, A.; Mehlhorn, W.; Zatsarinny, O.I.

1997-01-01

We have investigated the ejected-electron spectrum following impact excitation and ionization of laser-excited Na * (nl) atoms by 1.5 keV electrons. By means of two-laser excitation 3s → 3p 3/2 → 7d and subsequent cascading transitions about 8% (4%) of the target atoms were in excited states with n > 3 (7d). The experimental ejected-electron spectrum due to the decay of Auger and autoionization states of laser-excited atoms Na * (nl) with n = 4-7 has been fully interpreted by comprehensive calculations of the energies, cross sections and decay probabilities of the corresponding states. The various processes contributing to the ejected-electron spectrum are with decreasing magnitude: 2s ionization leading to 2s2p 6 nl Auger states, 2p → 3s excitation leading to 2p 5 3s( 1 P)nl autoionization states and 2s → 3l' excitation leading to 2s2p 6 3l'( 1 L)nl autoionization states. (Author)

New excited states in sd-shell nucleus {sup 33}P

Energy Technology Data Exchange (ETDEWEB)

Fu, B.; Reiter, P.; Arnswald, K.; Hess, H.; Hirsch, R.; Lewandowski, L.; Schneiders, D.; Seidlitz, M.; Siebeck, B.; Steinbach, T.; Vogt, A.; Wendt, A.; Wolf, K. [Institut fuer Kernphysik, Universitaet zu Koeln (Germany)

2015-07-01

Isospin-symmetry breaking in nuclear physics is mainly described by Mirror-Energy Differences (MED) for mirror nuclei or Triplet-Energy Differences (TED) for isobaric triplets. Modified USD-calculations successfully reproduce MED for T=1,3/2,2 sd-shell nuclei. Refined tests of theory are given by lifetime measurements in order to deduce transition-strength values. In order to study the mirror pair {sup 33}Ar and {sup 33}P, the fusion-evaporation reaction {sup 13}C+{sup 26}Mg at 46 MeV was measured at the Cologne tandem accelerator and the HORUS spectrometer employing the Doppler-Shift-Attenuation-Method (DSAM). First results yielded new γ-ray transitions in {sup 33}P and {sup 33}S. The level scheme of {sup 33}P was extended up to excitation energies of 10 MeV. Spins and parities of the new levels were determined exploiting γγ-angular correlations. Together with values from the proton-rich T{sub z} = - 3/2 partner, the levels are compared to shell model calculations, describing excitation energies of sd -shell mirror pairs. The understanding of isospin symmetry and isospin-symmetry breaking is a fundamental question in nuclear physics. Isospin-symmetry breaking is mainly described by Mirror-Energy Differences (MED) for mirror nuclei or Triplet-Energy Differences (TED) for isobaric triplets. Modified USD{sup m}{sub 1,2,3}-calculations successfully reproduced MED for the mirror nuclei {sup 33}Ar and {sup 33}P. Both {sup 33}P and {sup 33}S were produced at the Cologne FN tandem accelerator employing the fusion-evaporation reaction {sup 13}C+{sup 26}Mg at 46 MeV and spectroscopically investigated using 14 HPGe detectors. Several new energy states (in {sup 33}P) and γ-ray transitions (in {sup 33}P and {sup 33}S) were detected. Spins and parities of the new levels in {sup 33}P were determined exploiting γγ-angular correlations. The level scheme of {sup 33}P was extended up to excitation energies of 10 MeV.

Implications of electron attachment to highly-excited states in pulsed-power discharges

International Nuclear Information System (INIS)

Pinnaduwage, L.A.; Univ. of Tennessee, Knoxville, TN

1997-01-01

The author points out the possible implications of electron attachment to highly-excited states of molecules in two pulsed power technologies. One involves the pulsed H 2 discharges used for the generation of H ion beams for magnetic fusion energy and particle accelerators. The other is the power modulated plasma discharges used for material processing

Electronic properties of excited states in single InAs quantum dots; Elektronische Struktur angeregter Zustaende einzelner InAs-Quantenpunkte

Energy Technology Data Exchange (ETDEWEB)

Warming, Till

2009-02-20

binding energy of excited exciton states is accessible. From the shift of the exciton binding energy, when the hole is not in the ground state, but in the first or second excited states, conclusions on the shape of the wavefunctions can be drawn. Energy selective storage of charge carriers enables the access to few-particle binding energies of excited states also in quantum dot ensemble. The storage of charge carriers is refined to storage of defined spin states in the quantum dots. A technique for the deterministic preparation and readout is presented, what is of utmost importance for the realization of qubits for quantum computation. (orig.)

Range-separated density-functional theory for molecular excitation energies

International Nuclear Information System (INIS)

Rebolini, E.

2014-01-01

Linear-response time-dependent density-functional theory (TDDFT) is nowadays a method of choice to compute molecular excitation energies. However, within the usual adiabatic semi-local approximations, it is not able to describe properly Rydberg, charge-transfer or multiple excitations. Range separation of the electronic interaction allows one to mix rigorously density-functional methods at short range and wave function or Green's function methods at long range. When applied to the exchange functional, it already corrects most of these deficiencies but multiple excitations remain absent as they need a frequency-dependent kernel. In this thesis, the effects of range separation are first assessed on the excitation energies of a partially-interacting system in an analytic and numerical study in order to provide guidelines for future developments of range-separated methods for excitation energy calculations. It is then applied on the exchange and correlation TDDFT kernels in a single-determinant approximation in which the long-range part of the correlation kernel vanishes. A long-range frequency-dependent second-order correlation kernel is then derived from the Bethe-Salpeter equation and added perturbatively to the range-separated TDDFT kernel in order to take into account the effects of double excitations. (author)

Excitation dynamics and relaxation in a molecular heterodimer

International Nuclear Information System (INIS)

Balevičius, V.; Gelzinis, A.; Abramavicius, D.; Mančal, T.; Valkunas, L.

2012-01-01

Highlights: ► Dynamics of excitation within a heterogenous molecular dimer. ► Excited states can be swapped due to different reorganization energies of monomers. ► Conventional excitonic basis becomes renormalized due to interaction with the bath. ► Relaxation is independent of mutual positioning of monomeric excited states. -- Abstract: The exciton dynamics in a molecular heterodimer is studied as a function of differences in excitation and reorganization energies, asymmetry in transition dipole moments and excited state lifetimes. The heterodimer is composed of two molecules modeled as two-level systems coupled by the resonance interaction. The system-bath coupling is taken into account as a modulating factor of the molecular excitation energy gap, while the relaxation to the ground state is treated phenomenologically. Comparison of the description of the excitation dynamics modeled using either the Redfield equations (secular and full forms) or the Hierarchical quantum master equation (HQME) is demonstrated and discussed. Possible role of the dimer as an excitation quenching center in photosynthesis self-regulation is discussed. It is concluded that the system-bath interaction rather than the excitonic effect determines the excitation quenching ability of such a dimer.

Time-resolved stimulated emission depletion and energy transfer dynamics in two-photon excited EGFP

Science.gov (United States)

Masters, T. A.; Robinson, N. A.; Marsh, R. J.; Blacker, T. S.; Armoogum, D. A.; Larijani, B.; Bain, A. J.

2018-04-01

Time and polarization-resolved stimulated emission depletion (STED) measurements are used to investigate excited state evolution following the two-photon excitation of enhanced green fluorescent protein (EGFP). We employ a new approach for the accurate STED measurement of the hitherto unmeasured degree of hexadecapolar transition dipole moment alignment ⟨α40 ⟩ present at a given excitation-depletion (pump-dump) pulse separation. Time-resolved polarized fluorescence measurements as a function of pump-dump delay reveal the time evolution of ⟨α40 ⟩ to be considerably more rapid than predicted for isotropic rotational diffusion in EGFP. Additional depolarization by homo-Förster resonance energy transfer is investigated for both ⟨α20 ⟩ (quadrupolar) and ⟨α40 ⟩ transition dipole alignments. These results point to the utility of higher order dipole correlation measurements in the investigation of resonance energy transfer processes.

Study of excitation energy dependence of nuclear level density parameter

International Nuclear Information System (INIS)

Mohanto, G.; Nayak, B.K.; Saxena, A.

2016-01-01

In the present study, we have populated CN by fusion reaction and excitation energy of the intermediate nuclei is determined after first chance α-emission to investigate excitation energy dependence of the NLD parameter. Evaporated neutron spectra were measured following alpha evaporation for obtaining NLD parameter for the reaction 11 B + 197 Au, populating CN 208 Po. This CN after evaporating an α-particle populates intermediate nucleus 204 Pb. The 204 Pb has magic number of Z=82. Our aim is to study the excitation energy dependence of NLD parameter for closed shell nuclei

Effect of charged and excited states on the decomposition of 1,1-diamino-2,2-dinitroethylene molecules

International Nuclear Information System (INIS)

Kimmel, Anna V.; Sushko, Peter V.; Shluger, Alexander L.; Kuklja, Maija M.

2007-01-01

The authors have calculated the electronic structure of individual 1,1-diamino-2,2-dinitroethylene molecules (FOX-7) in the gas phase by means of density functional theory with the hybrid B3LYP functional and 6-31+G(d,p) basis set and considered their dissociation pathways. Positively and negatively charged states as well as the lowest excited states of the molecule were simulated. They found that charging and excitation can not only reduce the activation barriers for decomposition reactions but also change the dominating chemistry from endo- to exothermic type. In particular, they found that there are two competing primary initiation mechanisms of FOX-7 decomposition: C-NO 2 bond fission and C-NO 2 to CONO isomerization. Electronic excitation or charging of FOX-7 disfavors CONO formation and, thus, terminates this channel of decomposition. However, if CONO is formed from the neutral FOX-7 molecule, charge trapping and/or excitation results in spontaneous splitting of an NO group accompanied by the energy release. Intramolecular hydrogen transfer is found to be a rare event in FOX-7 unless free electrons are available in the vicinity of the molecule, in which case HONO formation is a feasible exothermic reaction with a relatively low energy barrier. The effect of charged and excited states on other possible reactions is also studied. Implications of the obtained results to FOX-7 decomposition in condensed state are discussed

Mapping the Excited State Potential Energy Surface of a Retinal Chromophore Model with Multireference and Equation-of-Motion Coupled-Cluster Methods.

Science.gov (United States)

Gozem, Samer; Melaccio, Federico; Lindh, Roland; Krylov, Anna I; Granovsky, Alexander A; Angeli, Celestino; Olivucci, Massimo

2013-10-08

The photoisomerization of the retinal chromophore of visual pigments proceeds along a complex reaction coordinate on a multidimensional surface that comprises a hydrogen-out-of-plane (HOOP) coordinate, a bond length alternation (BLA) coordinate, a single bond torsion and, finally, the reactive double bond torsion. These degrees of freedom are coupled with changes in the electronic structure of the chromophore and, therefore, the computational investigation of the photochemistry of such systems requires the use of a methodology capable of describing electronic structure changes along all those coordinates. Here, we employ the penta-2,4-dieniminium (PSB3) cation as a minimal model of the retinal chromophore of visual pigments and compare its excited state isomerization paths at the CASSCF and CASPT2 levels of theory. These paths connect the cis isomer and the trans isomer of PSB3 with two structurally and energetically distinct conical intersections (CIs) that belong to the same intersection space. MRCISD+Q energy profiles along these paths provide benchmark values against which other ab initio methods are validated. Accordingly, we compare the energy profiles of MRPT2 methods (CASPT2, QD-NEVPT2, and XMCQDPT2) and EOM-SF-CC methods (EOM-SF-CCSD and EOM-SF-CCSD(dT)) to the MRCISD+Q reference profiles. We find that the paths produced with CASSCF and CASPT2 are topologically and energetically different, partially due to the existence of a "locally excited" region on the CASPT2 excited state near the Franck-Condon point that is absent in CASSCF and that involves a single bond, rather than double bond, torsion. We also find that MRPT2 methods as well as EOM-SF-CCSD(dT) are capable of quantitatively describing the processes involved in the photoisomerization of systems like PSB3.

Excitation of autoionizing states of helium by 100 keV proton impact: II. Excitation cross sections and mechanisms of excitation

Energy Technology Data Exchange (ETDEWEB)

Godunov, A.L. [Department of Physics, Tulane University, New Orleans, LA 70118-5698 (United States); Ivanov, P.B.; Schipakov, V.A. [Troitsk Institute of Innovation and Fusion Research Troitsk, Moscow region, 142092 (Russian Federation); Moretto-Capelle, P.; Bordenave-Montesquieu, D.; Bordenave-Montesquieu, A. [Laboratoire Collisions, Agregats, Reactivite, IRSAMC, UMR 5589, CNRS-Universite Paul Sabatier, 31062 Toulouse Cedex (France)

2000-03-14

Mechanisms of two-electron excitation of the (2s{sup 2}){sup 1} S, (2p{sup 2} ){sup 1} D and (2s2p){sup 1} P autoionizing states of helium are studied both experimentally and theoretically. It is shown that an explicit introduction of a kinematic factor, with a process-specific phase leads to a productive parametrization of experimental cross sections of ionization, allowing one to extract cross sections of excitation of autoionizing states. Using a new fitting procedure together with the proposed parametrization made it possible to obtain the excitation cross sections and magnetic sublevel population from electron spectra as well as, for the first time, to resolve the contribution of resonance and interference components to resonance profiles. Interference with direct ionization is shown to contribute significantly into resonance formation even for backward ejection angles. We demonstrate theoretically that the excitation cross sections thus extracted from experimental electron spectra hold information about the interaction of autoionizing states with an adjacent continuum. (author)

Excited-state intramolecular proton transfer and photoswitching in hydroxyphenyl-imidazopyridine derivatives: A theoretical study

Science.gov (United States)

Omidyan, Reza; Iravani, Maryam

2016-11-01

The MP2/CC2 and CASSCF theoretical approaches have been employed to determine the excited state proton transfer and photophysical nature of the four organic compounds, having the main frame of hydroxyphenyl-imidzaopyridine (HPIP). The nitrogen insertion effect, in addition to amine (-NH2) substitution has been investigated extensively by following the transition energies and deactivation pathways of resulted HPIP derivatives. It has been predicted that the excited state intramolecular proton transfer with or without small barrier is the most important feature of these compounds. Also, for all of the considered HPIP derivatives, a conical intersection (CI) between ground and the S1 excited state has been predicted. The strong non-adiabatic coupling in the CI (S1/S0), drives the system back to the ground state in which the proton may either return to the phenoxy unit and thus close the photocycle, or the system can continue the twisting motion that results in formation of a γ-photochromic species. This latter species can be responsible for photochromism of HPIP derivative systems.

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

International Nuclear Information System (INIS)

Dallinger, R.F.; Farquharson, S.; Woodruff, W.H.; Rodgers, M.A.J.

1981-01-01

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

Molecular and excited state properties of isomeric scarlet disperse dyes

Science.gov (United States)

Lim, Jihye; Szymczyk, Malgorzata; Mehraban, Nahid; Ding, Yi; Parrillo-Chapman, Lisa; El-Shafei, Ahmed; Freeman, Harold S.

2018-06-01

This work was part of an investigation aimed at characterizing the molecular and excited state properties of currently available disperse dyes developed to provide stability to extensive sunlight exposures when adsorbed on poly(ethylene terephthalate) (PET) fibers. Having completed the characterization of yellow, magenta, and cyan disperse dyes for PET-based fabrics used outdoors, our attention turned to the colors designed to enhance the color gamut of a standard 4-member (cyan/yellow/magenta/black) color set. The present study pertained specifically to the characterization of commercially available scarlet dyes. In this regard, HPLC analysis showed that a scarlet product used for PET coloration was mainly a 70/30 mixture of dyes, and the use of HRMS and single crystal X-ray diffraction analyses indicated that these two dyes were azo compounds derived from isomeric pyridine-based couplers which differed in the location of the primary amino (sbnd NH2) and anilino (sbnd NHPh) groups attached to the pyridine ring. One dye structure has the sbnd NHPh group para to the azo group (Sc2), while the other has that group in the ortho position (Sc3). The presence of either ortho substituent provides photostabilization through intramolecular H-bonding with the azo moiety. Further, results from molecular modeling studies showed that the lower excited state oxidation potential of Sc3 relative to that of Sc2 allows Sc3 to function as an energy quencher for the excited state of Sc2 - through thermodynamically favorable electron transfer.

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

International Nuclear Information System (INIS)

Al Falou, H.; Kanungo, R.; Andreoiu, C.; Cross, D.S.; Davids, B.; Djongolov, M.; Gallant, A.T.; Galinski, N.; Howell, D.; Kshetri, R.; Niamir, D.; Orce, J.N.; Shotter, A.C.; Sjue, S.; Tanihata, I.; Thompson, I.J.; Triambak, S.; Uchida, M.; Walden, P.; Wiringa, R.B.

2013-01-01

The first measurement of inelastic scattering of 9 Li 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

Glass-like, low-energy excitations in neutron-irradiated quartz

International Nuclear Information System (INIS)

Gardner, J.W.

1980-01-01

The specific heat and thermal conductivity of neutron-irradiated crystalline quartz have been measured for temperatures approx. = 0.1 to 5 K. Four types of low-energy excitations are observed in the irradiated samples, two of which can be removed selectively by heat treatment. One set of remaining excitations gives rise to low-temperature thermal behavior characteristic of glassy (amorphous) solids. The density of these glass-like excitations can be 50% the density observed in vitreous silica, yet the sample still retains long-range atomic order. In a less-irradiated sample, glass-like excitations may be present with a density only approx. = 2.5% that observed in vitreous silica and possess a similar broad energy spectrum over 0.1 to 1 K

Excitation energy transfer between Light-harvesting complex II and Photosystem I in reconstituted membranes.

Science.gov (United States)

Akhtar, Parveen; Lingvay, Mónika; Kiss, Teréz; Deák, Róbert; Bóta, Attila; Ughy, Bettina; Garab, Győző; Lambrev, Petar H

2016-04-01

Light-harvesting complex II (LHCII), the major peripheral antenna of Photosystem II in plants, participates in several concerted mechanisms for regulation of the excitation energy and electron fluxes in thylakoid membranes. In part, these include interaction of LHCII with Photosystem I (PSI) enhancing the latter's absorption cross-section - for example in the well-known state 1 - state 2 transitions or as a long-term acclimation to high light. In this work we examined the capability of LHCII to deliver excitations to PSI in reconstituted membranes in vitro. Proteoliposomes with native plant thylakoid membrane lipids and different stoichiometric ratios of LHCII:PSI were reconstituted and studied by steady-state and time-resolved fluorescence spectroscopy. Fluorescence emission from LHCII was strongly decreased in PSI-LHCII membranes due to trapping of excitations by PSI. Kinetic modelling of the time-resolved fluorescence data revealed the existence of separate pools of LHCII distinguished by the time scale of energy transfer. A strongly coupled pool, equivalent to one LHCII trimer per PSI, transferred excitations to PSI with near-unity efficiency on a time scale of less than 10ps but extra LHCIIs also contributed significantly to the effective antenna size of PSI, which could be increased by up to 47% in membranes containing 3 LHCII trimers per PSI. The results demonstrate a remarkable competence of LHCII to increase the absorption cross-section of PSI, given the opportunity that the two types of complexes interact in the membrane. Copyright © 2016 Elsevier B.V. All rights reserved.

Free electrons and ionic liquids: study of excited states by means of electron-energy loss spectroscopy and the density functional theory multireference configuration interaction method.

Science.gov (United States)

Regeta, Khrystyna; Bannwarth, Christoph; Grimme, Stefan; Allan, Michael

2015-06-28

The technique of low energy (0-30 eV) electron impact spectroscopy, originally developed for gas phase molecules, is applied to room temperature ionic liquids (IL). Electron energy loss (EEL) spectra recorded near threshold, by collecting 0-2 eV electrons, are largely continuous, assigned to excitation of a quasi-continuum of high overtones and combination vibrations of low-frequency modes. EEL spectra recorded by collecting 10 eV electrons show predominantly discrete vibrational and electronic bands. The vibrational energy-loss spectra correspond well to IR spectra except for a broadening (∼0.04 eV) caused by the liquid surroundings, and enhanced overtone activity indicating a contribution from resonant excitation mechanism. The spectra of four representative ILs were recorded in the energy range of electronic excitations and compared to density functional theory multireference configuration interaction (DFT/MRCI) calculations, with good agreement. The spectra up to about 8 eV are dominated by π-π* transitions of the aromatic cations. The lowest bands were identified as triplet states. The spectral region 2-8 eV was empty in the case of a cation without π orbitals. The EEL spectrum of a saturated solution of methylene green in an IL band showed the methylene green EEL band at 2 eV, indicating that ILs may be used as a host to study nonvolatile compounds by this technique in the future.

Design and development of a parametrically excited nonlinear energy harvester

International Nuclear Information System (INIS)

Yildirim, Tanju; Ghayesh, Mergen H.; Li, Weihua; Alici, Gursel

2016-01-01

Highlights: • A parametrically broadband energy harvester was fabricated. • Strong softening-type nonlinear behaviour was observed. • Experiments were conducted showing the large bandwidth of the device. - Abstract: An energy harvester has been designed, fabricated and tested based on the nonlinear dynamical response of a parametrically excited clamped-clamped beam with a central point-mass; magnets have been used as the central point-mass which pass through a coil when parametrically excited. Experiments have been conducted for the energy harvester when the system is excited (i) harmonically near the primary resonance; (ii) harmonically near the principal parametric resonance; (iii) by means of a non-smooth periodic excitation. An electrodynamic shaker was used to parametrically excite the system and the corresponding displacement of the magnet and output voltages of the coil were measured. It has been shown that the system displays linear behaviour at the primary resonance; however, at the principal parametric resonance, the motion characteristic of the magnet substantially changed displaying a strong softening-type nonlinearity. Theoretical simulations have also been conducted in order to verify the experimental results; the comparison between theory and experiment were within very good agreement of each other. The energy harvester developed in this paper is capable of harvesting energy close to the primary resonance as well as the principal parametric resonance; the frequency-band has been broadened significantly mainly due to the nonlinear effects as well as the parametric excitation.

On excited states in real-time AdS/CFT

Energy Technology Data Exchange (ETDEWEB)

Botta-Cantcheff, Marcelo; Martínez, Pedro J.; Silva, Guillermo A. [Instituto de Física de La Plata - CONICET & Departamento de Física - UNLP,C.C. 67, 1900 La Plata (Argentina)

2016-02-25

The Skenderis-van Rees prescription, which allows the calculation of time-ordered correlation functions of local operators in CFT’s using holographic methods is studied and applied for excited states. Calculation of correlators and matrix elements of local CFT operators between generic in/out states are carried out in global Lorentzian AdS. We find the precise form of such states, obtain an holographic formula to compute the inner product between them, and using the consistency with other known prescriptions, we argue that the in/out excited states built according to the Skenderis-Van Rees prescription correspond to coherent states in the (large-N) AdS-Hilbert space. This is confirmed by explicit holographic computations. The outcome of this study has remarkable implications on generalizing the Hartle-Hawking construction for wave functionals of excited states in AdS quantum gravity.

From fusion hierarchy to excited state TBA

International Nuclear Information System (INIS)

Juettner, G.; Kluemper, A.

1998-01-01

Functional relations among the fusion hierarchy of quantum transfer matrices give a novel derivation of the TBA equations, namely without string hypothesis. This is demonstrated for two important models of 1D highly correlated electron systems, the supersymmetric t-J model and the supersymmetric extended Hubbard model. As a consequence, ''the excited state TBA'' equations, which characterize correlation lengths, are explicitly derived for the t-J model. To the authors' knowledge, this is the first explicit derivation of excited state TBA equations for 1D lattice electron systems. (orig.)

Energy-dependent collisional deactivation of vibrationally excited azulene

International Nuclear Information System (INIS)

Shi, J.; Barker, J.R.

1988-01-01

Collisional energy transfer parameters for highly vibrationally excited azulene have been deduced from new infrared fluorescence (IRF) emission lifetime data with an improved calibration relating IRF intensity to vibrational energy [J. Shi, D. Bernfeld, and J. R. Barker, J. Chem. Phys. 88, XXXX (1988), preceding paper]. In addition, data from previous experiments [M. J. Rossi, J. R. Pladziewicz, and J. R. Barker, J. Chem. Phys. 78, 6695 (1983)] have been reanalyzed based on the improved calibration. Inversion of the IRF decay curves produced plots of energy decay, which were analyzed to determine , the average energy transferred per collision. Master equation simulations reproduced both the original IRF decays and the deduced energy decays. A third (simple) method of determination agrees well with the other two. The results show to be nearly directly proportional to the vibrational energy of the excited azulene from ∼8000 to 33 000 cm -1 . At high energies, there are indications that the energy dependence may be slightly reduced

Review of high excitation energy structures in heavy ion collisions: target excitations and three body processes

International Nuclear Information System (INIS)

Frascaria, N.

1987-09-01

A review of experimental results on high excitation energy structures in heavy ion inelastic scattering is presented. The contribution to the spectra of the pick-up break-up mechanism is discussed in the light of the data obtained with light heavy ion projectiles. Recent results obtained with 40 Ar beams at various energies will show that target excitations contribute strongly to the measured cross section

Manipulating the Electronic Excited State Energies of Pyrimidine-Based Thermally Activated Delayed Fluorescence Emitters To Realize Efficient Deep-Blue Emission.

Science.gov (United States)

Komatsu, Ryutaro; Ohsawa, Tatsuya; Sasabe, Hisahiro; Nakao, Kohei; Hayasaka, Yuya; Kido, Junji

2017-02-08

The development of efficient and robust deep-blue emitters is one of the key issues in organic light-emitting devices (OLEDs) for environmentally friendly, large-area displays or general lighting. As a promising technology that realizes 100% conversion from electrons to photons, thermally activated delayed fluorescence (TADF) emitters have attracted considerable attention. However, only a handful of examples of deep-blue TADF emitters have been reported to date, and the emitters generally show large efficiency roll-off at practical luminance over several hundreds to thousands of cd m -2 , most likely because of the long delayed fluorescent lifetime (τ d ). To overcome this problem, we molecularly manipulated the electronic excited state energies of pyrimidine-based TADF emitters to realize deep-blue emission and reduced τ d . We then systematically investigated the relationships among the chemical structure, properties, and device performances. The resultant novel pyrimidine emitters, called Ac-XMHPMs (X = 1, 2, and 3), contain different numbers of bulky methyl substituents at acceptor moieties, increasing the excited singlet (E S ) and triplet state (E T ) energies. Among them, Ac-3MHPM, with a high E T of 2.95 eV, exhibited a high external quantum efficiency (η ext,max ) of 18% and an η ext of 10% at 100 cd m -2 with Commission Internationale de l'Eclairage chromaticity coordinates of (0.16, 0.15). These efficiencies are among the highest values to date for deep-blue TADF OLEDs. Our molecular design strategy provides fundamental guidance to design novel deep-blue TADF emitters.

Monte Carlo wave-packet approach to trace nuclear dynamics in molecular excited states by XUV-pump-IR-probe spectroscopy

Science.gov (United States)

Jing, Qingli; Bello, Roger Y.; Martín, Fernando; Palacios, Alicia; Madsen, Lars Bojer

2018-04-01

Recent research interests have been raised in uncovering and controlling ultrafast dynamics in excited neutral molecules. In this work we generalize the Monte Carlo wave packet (MCWP) approach to XUV-pump-IR-probe schemes to simulate the process of dissociative double ionization of H2 where singly excited states in H2 are involved. The XUV pulse is chosen to resonantly excite the initial ground state of H2 to the lowest excited electronic state of 1Σu + symmetry in H2 within the Franck-Condon region. The delayed intense IR pulse couples the excited states of 1Σu + symmetry with the nearby excited states of 1Σg + symmetry. It also induces the first ionization from H2 to H2 + and the second ionization from H2 + to H++H+. To reduce the computational costs in the MCWP approach, a sampling method is proposed to determine in time the dominant ionization events from H2 to H2+. By conducting a trajectory analysis, which is a unique possibility within the MCWP approach, the origins of the characteristic features in the nuclear kinetic energy release spectra are identified for delays ranging from 0 to 140 fs and the nuclear dynamics in the singly excited states in H2 is mapped out.

Dielectronic recombination rate coefficients to the excited states of CII from CIII

International Nuclear Information System (INIS)

Kato, Takako; Safronova, U.; Ohira, Mituhiko.

1996-02-01

Energy levels, radiative transition probabilities and autoionization rates for CII including 1s 2 2l2l'nl'' (n=2-6, l'≤(n-1)) states were calculated by using multi-configurational Hartree-Fock (Cowan code) method. Autoionizing levels above three thresholds: 1s 2 2s 2 ( 1 S), 1s 2 2s2p( 3 P), 1s 2 2s2p( 1 P) were considered. Branching ratios related to the first threshold and the intensity factor were calculated for satellite lines of CII ion. The dielectronic recombination rate coefficients to the excited states for n=2-6 are calculated with these atomic data. The rate coefficients are fitted to an analytical formula and the fit parameters are given. The values for higher excited states than n=6 are extrapolated and the total dielectronic recombination rate coefficients are derived. The effective recombination rate coefficient for different electron densities are also derived. (author)

Relativistic configuration interaction calculation on the ground and excited states of iridium monoxide

International Nuclear Information System (INIS)

Suo, Bingbing; Yu, Yan-Mei; Han, Huixian

2015-01-01

We present the fully relativistic multi-reference configuration interaction calculations of the ground and low-lying excited electronic states of IrO for individual spin-orbit component. The lowest-lying state is calculated for Ω = 1/2, 3/2, 5/2, and 7/2 in order to clarify the ground state of IrO. Our calculation suggests that the ground state is of Ω = 1/2, which is highly mixed with 4 Σ − and 2 Π states in Λ − S notation. The two low-lying states 5/2 and 7/2 are nearly degenerate with the ground state and locate only 234 and 260 cm −1 above, respectively. The equilibrium bond length 1.712 Å and the harmonic vibrational frequency 903 cm −1 of the 5/2 state are close to the experimental measurement of 1.724 Å and 909 cm −1 , which suggests that the 5/2 state should be the low-lying state that contributes to the experimental spectra. Moreover, the electronic states that give rise to the observed transition bands are assigned for Ω = 5/2 and 7/2 in terms of the obtained excited energies and oscillator strengths

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

Science.gov (United States)

Heßelmann, Andreas

2015-04-14

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

The Mean Excitation Energy of Atomic Ions

DEFF Research Database (Denmark)