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
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
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
Lim, Edward C
2013-01-01
Excited States, Volume 4 is a collection of papers that deals with the excited states of molecular activity. One paper investigates the resonance Raman spectroscopy as the key to vibrational-electronic coupling. This paper reviews the basic theory of Raman scattering; it also explains the derivation of the Raman spectra, excitation profiles, and depolarization ratios for simple resonance systems. Another paper reviews the magnetic properties of triplet states, including the zero-field resonance techniques, the high-field experiments, and the spin Hamiltonian. This paper focuses on the magnetic
Institute of Scientific and Technical Information of China (English)
罗万居; 郭应祥; 周小红; 张玉虎; 雷相国; 刘忠; 郑勇; 柳敏良; 何建军; 竺礼华; 温书贤
2003-01-01
Excited states in 207Rn are investigated via the 196Pt(16O,Sn)207Rn reaction at beam energies from 85 to 95 MeV using techniques of in-beam γ-ray spectroscopy. Measurements ofγ-ray excitation function, x - γ and γ - γ- t coincidences are performed with ten BGO(AC)HPGe detectors. Based on these measurements, a level scheme of207Rn, including 17 γ-rays and 18 levels, is established. Spins for most of the levels are proposed according to the measured DCO ratios. The level structure is compared with a weak-coupling calculation using the interaction energies extracted from neighbouring nuclei.
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......, associated with an excited-state intramolecular proton transfer process....
Excited states rotational effects on the behavior of excited molecules
Lim, Edward C
2013-01-01
Excited States, Volume 7 is a collection of papers that discusses the excited states of molecules. The first paper reviews the rotational involvement in intra-molecular in vibrational redistribution. This paper analyzes the vibrational Hamiltonian as to its efficacy in detecting the manifestations of intra-molecular state-mixing in time-resolved and time-averaged spectroscopic measurements. The next paper examines the temporal behavior of intra-molecular vibration-rotation energy transfer (IVRET) and the effects of IVRET on collision, reaction, and the decomposition processes. This paper also
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....
Energy Technology Data Exchange (ETDEWEB)
Cappuzzello, F.; Orrigo, S.E.A.; Cunsolo, A.; Allia, M.C.; Lazzaro, A.; Nociforo, C.; Winfield, J.S. [Istituto Nazionale di Fisica Nucleare, Lab. Nazionali del Sud, Catania (Italy); Lazzaro, A. [Catania Univ., Dipt. Fisica (Italy); Lenske, H. [Giessen Univ. (Germany). Inst. fuer Theoretische Physik; Beaumel, D.; Fortier, S. [Institut de Physique Nucleaire, (IN2P3/CNRS) 91 - Orsay (France); Foti, A. [Istituto Nazionale di Fisica Nucleare, Catania (Italy)
2004-03-01
The N{sup 15}(Li{sup 7},Be{sup 7})C{sup 15} reaction at 55 MeV incident energy was studied at forward angles in order to explore the C{sup 15} excitation energy spectrum. The C{sup 15} ground state and the states at E{sub x} = 0.77, 6.77, 7.30, 8.50 MeV excitation energies were populated. The energy resolution ({approx} 250 keV) allowed the identification of these transitions each for Be{sup 7} ground and first-excited state at E{sub x} = 0.429 MeV. Quasi-particle random phase approximation (QRPA) calculations reproduce the C{sup 15} level structure below 1.5 MeV excitation energy. The strength observed at higher excitation energies probably arises from core-excited components of C{sup 15}. (authors)
Institute of Scientific and Technical Information of China (English)
林承键; 刘祖华; 张焕乔; 吴岳伟; 杨峰; 阮明
2001-01-01
Angular distributions for the 11 B(d,p)12 B transfer reactions have been measured at E1ab = 11.8 Me V. The asymp-totic normalization coefficients (ANC) of the ground state, the second and third excitation states for 12B ( 11 B+n) are extracted from the differential cross sections at three forward angles. With these ANCs, the root-mean-square radii are calculated for these three states. The results show that the second and third excitation states of 12B are neutron halo states.
Rearrangements in ground and excited states
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;
Electron excitation from ground state to first excited state: Bohmian mechanics method
Yang, Song; Shuang, Zhao; Fu-Ming, Guo; Yu-Jun, Yang; Su-Yu, Li
2016-03-01
The excitation process of electrons from the ground state to the first excited state via the resonant laser pulse is investigated by the Bohmian mechanics method. It is found that the Bohmian particles far away from the nucleus are easier to be excited and are excited firstly, while the Bohmian particles in the ground state is subject to a strong quantum force at a certain moment, being excited to the first excited state instantaneously. A detailed analysis for one of the trajectories is made, and finally we present the space and energy distribution of 2000 Bohmian particles at several typical instants and analyze their dynamical process at these moments. Project supported by the Doctoral Research Start-up Funding of Northeast Dianli University, China (Grant No. BSJXM-201332), the National Natural Science Foundation of China (Grant Nos. 11547114, 11534004, 11474129, 11274141, 11447192, and 11304116), and the Graduate Innovation Fund of Jilin University, China (Grant No. 2015091).
Nodal Variational Principle for Excited States
Zahariev, Federico; Levy, Mel
2016-01-01
It is proven that the exact excited-state wavefunction and energy may be obtained by minimizing the energy expectation value of a trial wave function that is constrained only to have the correct nodes of the state of interest. This excited-state nodal minimum principle has the advantage that it requires neither minimization with the con- straint of wavefunction orthogonality to all lower eigenstates nor the antisymmetry of the trial wavefunctions. It is also found that the minimization over the entire space can be partitioned into several in- terconnected minimizations within the individual nodal regions, and the exact excited-state energy may be obtained by a minimization in just one or several of these nodal regions. For the proofs of the the- orem, it is observed that the many-electron eigenfunction, restricted to a nodal region, is equivalent to a ground state wavefunction of one electron in a higher dimensional space; and an explicit excited-state energy variational expression is obtained by generalizing...
Computing Correct Truncated Excited State Wavefunctions
Bacalis, N C; Zang, J; Karaoulanis, D
2016-01-01
We demonstrate that, if a truncated expansion of a wave function is small, then the standard excited states computational method, of optimizing one root of a secular equation, may lead to an incorrect wave function - despite the correct energy according to the theorem of Hylleraas, Undheim and McDonald - whereas our proposed method [J. Comput. Meth. Sci. Eng. 8, 277 (2008)] (independent of orthogonality to lower lying approximants) leads to correct reliable small truncated wave functions. The demonstration is done in He excited states, using truncated series expansions in Hylleraas coordinates, as well as standard configuration-interaction truncated expansions.
Rearrangements in ground and excited states
de Mayo, Paul
1980-01-01
Rearrangements in Ground and Excited States, Volume 2 covers essays on the theoretical approach of rearrangements; the rearrangements involving boron; and the molecular rearrangements of organosilicon compounds. The book also includes essays on the polytopal rearrangement at phosphorus; the rearrangement in coordination complexes; and the reversible thermal intramolecular rearrangements of metal carbonyls. Chemists and people involved in the study of rearrangements will find the book invaluable.
Energy Technology Data Exchange (ETDEWEB)
Filatov, Michael, E-mail: mike.filatov@gmail.com [Department of Chemistry, Southern Methodist University, 3215 Daniel Avenue, Dallas, Texas 75275-0314 (United States); Huix-Rotllant, Miquel; Burghardt, Irene [Institute of Physical and Theoretical Chemistry, Goethe University Frankfurt, Max-von-Laue-Str. 7, D-60438 Frankfurt am Main (Germany)
2015-05-14
State-averaged (SA) variants of the spin-restricted ensemble-referenced Kohn-Sham (REKS) method, SA-REKS and state-interaction (SI)-SA-REKS, implement ensemble density functional theory for variationally obtaining excitation energies of molecular systems. In this work, the currently existing version of the SA-REKS method, which included only one excited state into the ensemble averaging, is extended by adding more excited states to the averaged energy functional. A general strategy for extension of the REKS-type methods to larger ensembles of ground and excited states is outlined and implemented in extended versions of the SA-REKS and SI-SA-REKS methods. The newly developed methods are tested in the calculation of several excited states of ground-state multi-reference systems, such as dissociating hydrogen molecule, and excited states of donor–acceptor molecular systems. For hydrogen molecule, the new method correctly reproduces the distance dependence of the lowest excited state energies and describes an avoided crossing between the doubly excited and singly excited states. For bithiophene–perylenediimide stacked complex, the SI-SA-REKS method correctly describes crossing between the locally excited state and the charge transfer excited state and yields vertical excitation energies in good agreement with the ab initio wavefunction methods.
Excited States in Solution through Polarizable Embedding
DEFF Research Database (Denmark)
Olsen, Jógvan Magnus; Aidas, Kestutis; Kongsted, Jacob
2010-01-01
mechanical calculation. The polarizable embedding potential is described by an atomistic representation including terms up to localized octupoles and anisotropic polarizabilities. It is generally applicable to any quantum chemical description but is here implemented for the case of Kohn−Sham density......We present theory and implementation of an advanced quantum mechanics/molecular mechanics (QM/MM) approach using a fully self-consistent polarizable embedding (PE) scheme. It is a polarizable layered model designed for effective yet accurate inclusion of an anisotropic medium in a quantum...... functional theory which we denote the PE-DFT method. It has been implemented in combination with time-dependent quantum mechanical linear and nonlinear response techniques, thus allowing for assessment of electronic excitation processes and dynamic ground- and excited-state molecular properties using...
Identification of excited states in conjugated polymers
Hartwell, L J
2003-01-01
This thesis reports quasi steady state photoinduced absorption measurements from three conjugated polymers: polypyridine (PPy), polyfluorene (PFO) and the emeraldine base (EB) form of polyaniline. The aim of these experiments was to determine the nature of the photoexcited states existing in these materials in the millisecond time domain, as this has important consequences for the operation of real devices manufactured using these materials. The results from the photoinduced absorption experiments are closely compared with published results from pulse radiolysis experiments. In all cases there is very good correspondence between the two data sets, which has enabled the photoexcited states to be assigned with a high degree of confidence. Quasi steady-state photoinduced absorption involves the measurement of the change in absorption of a material in response to optical excitation with a laser beam. The changes in absorption are small, so a instrument was developed and optimised for each different sample. Lock-i...
Holographic Construction of Excited CFT States
Christodoulou, Ariana
2016-01-01
We present a systematic construction of bulk solutions that are dual to CFT excited states. The bulk solution is constructed perturbatively in bulk fields. The linearised solution is universal and depends only on the conformal dimension of the primary operator that is associated with the state via the operator-state correspondence, while higher order terms depend on detailed properties of the operator, such as its OPE with itself and generally involve many bulk fields. We illustrate the discussion with the holographic construction of the universal part of the solution for states of two dimensional CFTs, either on $R \\times S^1$ or on $R^{1,1}$. We compute the 1-point function both in the CFT and in the bulk, finding exact agreement. We comment on the relation with other reconstruction approaches.
Ultrafast excited-state dynamics of isocytosine.
Szabla, Rafał; Góra, Robert W; Šponer, Jiří
2016-07-27
The alternative nucleobase isocytosine has long been considered as a plausible component of hypothetical primordial informational polymers. To examine this hypothesis we investigated the excited-state dynamics of the two most abundant forms of isocytosine in the gas phase (keto and enol). Our surface-hopping nonadiabatic molecular dynamics simulations employing the algebraic diagrammatic construction to the second order [ADC(2)] method for the electronic structure calculations suggest that both tautomers undergo efficient radiationless deactivation to the electronic ground state with time constants which amount to τketo = 182 fs and τenol = 533 fs. The dominant photorelaxation pathways correspond to ring-puckering (ππ* surface) and C[double bond, length as m-dash]O stretching/N-H tilting (nπ* surface) for the enol and keto forms respectively. Based on these findings, we infer that isocytosine is a relatively photostable compound in the gas phase and in these terms resembles biologically relevant nucleobases. The estimated S1 [radiolysis arrow - arrow with voltage kink] T1 intersystem crossing rate constant of 8.02 × 10(10) s(-1) suggests that triplet states might also play an important role in the overall excited-state dynamics of the keto tautomer. The reliability of ADC(2)-based surface-hopping molecular dynamics simulations was tested against multireference quantum-chemical calculations and the potential limitations of the employed ADC(2) approach are briefly discussed. PMID:27346684
Excited states of muonium in atomic hydrogen
Indian Academy of Sciences (India)
V S Kulhar
2006-06-01
Muonium formation in excited states in muon-hydrogen charge-exchange collision is investigated using a method developed in a previous paper. Differential cross-section results are found to resemble positronium formation cross-section results of positron-hydrogen charge-exchange problem. Forward differential and integrated cross-sections are computed for muon energy of 2 keV and higher. Total muonium formation cross-sections are computed using Jackson and Schiff scaling rules. Muonium formation cross-section results obtained from proton-hydrogen charge-exchange cross-section results, using velocity scaling are compared with the results of the present calculation.
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...... of the excited state dynamics, the presence of this state required the development of a numerical three-excited-state kinetic model to replace the commonly used two-excited-state model. The experimental results shows that the reaction rates are strongly influenced both by substituents and solvent, illustrating...... the importance of including all relevant states in the kinetic modeling. Ultimately it is established that the excited state dynamics can conveniently be followed by optical methods, and the applicability of the system as a model system in time-resolved X-ray scattering experiments is discussed....
Lifetimes of excited states in 164Hf
International Nuclear Information System (INIS)
Lifetimes of excited states in 164Hf were measured using the Doppler-shift recoil-distance method. Gamma-gamma coincidences at eleven target-stopper distances were measured using the twelve Compton-suppressed Ge-detectors of the OSIRIS spectrometer. From the coincidence spectra the intensities of the Doppler-shifted and unshifted γ-lines were determined. The quadrupole moments Qt of transitions within the rotational bands derived from the lifetimes are constant within the experimental uncertainties up to the 18+ state. The Qt value for the transition between the ground- and the neutron i213/2 band (s-band) which is strongly reduced compared to the values of the in-band transitions is used to deduce a band interaction energy of 34 keV≤V≤57 keV. (orig.)
The polaron: Ground state, excited states, and far from equilibrium
Energy Technology Data Exchange (ETDEWEB)
Trugman, S.A. [Los Alamos National Lab., NM (United States). Theory Div.; Bonca, J. [Univ. of Ljubljana (Slovenia)]|[Jozef Stefan Inst., Ljubljana (Slovenia)
1998-12-01
The authors describe a variational approach for solving the Holstein polaron model with dynamical quantum phonons on an infinite lattice. The method is simple, fast, extremely accurate, and gives ground and excited state energies and wavefunctions at any momentum k. The method can also be used to calculate coherent quantum dynamics for inelastic tunneling and for strongly driven polarons far from equilibrium.
The sex-linked fidget mutation abolishes Brn4/Pou3f4 gene expression in the embryonic inner ear.
Phippard, D; Boyd, Y; Reed, V; Fisher, G; Masson, W K; Evans, E P; Saunders, J C; Crenshaw, E B
2000-01-01
We have demonstrated that the phenotype of the mouse mutant sex-linked fidget ( slf ) is caused by developmental malformations of the inner ear that result in hearing loss and vestibular dysfunction. Recently, pilot mapping experiments suggested that the mouse Brn4 / Pou3f4 gene co-segregated with the slf locus on the mouse X chromosome. These mapping data, in conjunction with the observation that the vertical head-shaking phenotype of slf mutants is identical to that observed in mice with a targeted deletion of the Brn4 gene, suggested that slf is a mutant allele of the Brn4 gene. In this paper, we have identified the nature of the slf mutation, and demonstrated that it is an X chromosomal inversion with one breakpoint close to Brn4. This inversion selectively eliminates the expression of the Brn4 gene in the developing inner ear, but not the neural tube. Finally, these results demonstrate that the slf mutation is a good mouse model for the most prevalent form of X-linked congenital deafness in man, which is associated with mutations in the human Brn4 ortholog, POU3F4.
Excited-State Spectroscopy Using Single Spin Manipulation in Diamond
Fuchs, G.D.; Dobrovitski, V.V.; Hanson, R.; Batra, A.; Weis, C.D.; Schenkel, T.; Awschalom, D.D.
2008-01-01
We use single-spin resonant spectroscopy to study the spin structure in the orbital excited state of a diamond nitrogen-vacancy (N-V) center at room temperature. The data show that the excited-state spin levels have a zero-field splitting that is approximately half of the value of the ground state l
Excited states in DNA strands investigated by ultrafast laser spectroscopy.
Chen, Jinquan; Zhang, Yuyuan; Kohler, Bern
2015-01-01
Ultrafast laser experiments on carefully selected DNA model compounds probe the effects of base stacking, base pairing, and structural disorder on excited electronic states formed by UV absorption in single and double DNA strands. Direct π-orbital overlap between two stacked bases in a dinucleotide or in a longer single strand creates new excited states that decay orders of magnitude more slowly than the generally subpicosecond excited states of monomeric bases. Half or more of all excited states in single strands decay in this manner. Ultrafast mid-IR transient absorption experiments reveal that the long-lived excited states in a number of model compounds are charge transfer states formed by interbase electron transfer, which subsequently decay by charge recombination. The lifetimes of the charge transfer states are surprisingly independent of how the stacked bases are oriented, but disruption of π-stacking, either by elevating temperature or by adding a denaturing co-solvent, completely eliminates this decay channel. Time-resolved emission measurements support the conclusion that these states are populated very rapidly from initial excitons. These experiments also reveal the existence of populations of emissive excited states that decay on the nanosecond time scale. The quantum yield of these states is very small for UVB/UVC excitation, but increases at UVA wavelengths. In double strands, hydrogen bonding between bases perturbs, but does not quench, the long-lived excited states. Kinetic isotope effects on the excited-state dynamics suggest that intrastrand electron transfer may couple to interstrand proton transfer. By revealing how structure and non-covalent interactions affect excited-state dynamics, on-going experimental and theoretical studies of excited states in DNA strands can advance understanding of fundamental photophysics in other nanoscale systems.
Excited-State Effective Masses in Lattice QCD
Energy Technology Data Exchange (ETDEWEB)
George Fleming, Saul Cohen, Huey-Wen Lin
2009-10-01
We apply black-box methods, i.e. where the performance of the method does not depend upon initial guesses, to extract excited-state energies from Euclidean-time hadron correlation functions. In particular, we extend the widely used effective-mass method to incorporate multiple correlation functions and produce effective mass estimates for multiple excited states. In general, these excited-state effective masses will be determined by finding the roots of some polynomial. We demonstrate the method using sample lattice data to determine excited-state energies of the nucleon and compare the results to other energy-level finding techniques.
Systematics of α -decay transitions to excited states
Delion, D. S.; Dumitrescu, A.
2015-08-01
We systematize the available experimental material concerning α -decay transitions to low-lying excited states in even-even and odd-mass emitters. We generalize our previous theoretical prediction concerning the linear dependence between hindrance factors and the excitation energy for transitions in even-even α emitters. Thus, we show that α intensities for transitions to excited states depend linearly upon the excitation energy for all known even-even and odd-mass α emitters. It turns out that the well-known Viola-Seaborg law for α -decay transitions between ground states can be generalized for transitions to excited states. This rule can be used to predict any α -decay half-life to a low-lying excited state.
A novel mutation in POU3F4 in a Chinese family with X-linked non-syndromic hearing loss
Institute of Scientific and Technical Information of China (English)
Bang-qing Huang; Jia-ling Zeng; Yong-yi Yuan; Pu Dai
2015-01-01
Objective:Based on the clinical manifestations of a hearing loss patient, the POU3F4 gene was tested for diagnosis of etiology. Methods:A comprehensive physical examination was performed on the proband to exclude abnormalities of other organs, and detailed audi-ological testing and temporal bone CT scan were also performed. Genomic DNA was extracted using the proband's peripheral blood leukocytes. Polymerase chain reactions (PCR) were performed in the coding sequence of the POU3F4 gene. Direct DNA sequencing was subsequently applied to screen the entire coding region of the POU3F4 gene. Results:The proband had severe sensorineural hearing loss. Temporal CT showed bilateral cochlear incomplete partition, vestibule dysplasia, internal auditory canal fundus expansion, and cochlear interlink with the internal auditory canal fundus. A novel mutation (c.530C > A (p.S177X)) in the POU3F4 gene was found in this patient, creating an new stop codon and was predicted to result in a truncated protein lacking normal POU3F4 transcription factor function. Conclusion: Through analysis of the POU3F4 gene and clinical manifestations in the patient, we conclude that a novel mutation may have resulted in a premature stop codon, contributing to the mutation of POU3F4 gene.
Radially Excited States of 1P Charmonium and X(3872)
Chen, Y; Liu, Y; Ma, J; Zhang, J; Chen, Ying; Liu, Chuan; Liu, Yubin; Ma, Jianping; Zhang, Jianbo
2007-01-01
The first excited states of charmonium in $0^{++}$, $1^{++}$, $1^{+-}$ channels are numerically investigated with lattice QCD of improved gauge and Wilson fermion actions, formulated on anisotropic lattices. Having determined the mass of ground states, the masses of excited states can be extracted by a constrained curve fitting algorithm which gives the masses 3.825(88) GeV, 3.853(57) GeV, and 3.858(70) Gev for the first excited states in $0^{++}$, $1^{++}$, $1^{+-}$ channels, respectively. A node structure is also observed in the Bethe-Salpeter wave-function of the $1^{++}$ state. The mass of the radically excited $1^{++}$ state is close to the mass of the newly observed X(3872). It indicates that X(3872) can be the first excited state of $\\chi_{c1}$.
Azuma, T.; Nakano, Y.; Metoki, K.; Hatakeyama, A.; Nakai, Y.; Komaki, K.; Yamazaki, Y.; Takada, E.; Murakami, T.
2009-11-01
Convoy electrons emitted from 416 MeV/u heliumlike Ar16+ ions excited by three-dimensional resonant coherent excitation (3D-RCE) have been explored. The 1s electron in the ground state was excited to the 2p state by a periodic crystal field during the passage through a Si crystal and released into the continuum by collisions with target atoms to form a cusp-shaped peak in the energy distribution, referred to as convoy electron. Under the resonance condition, we found not only enhancement of the convoy electron yield but also significant narrowing in the energy distribution, reflecting the initial bound state momentum distribution of the excited ions. This suggests that RCE is well-suited to study fast ion collisions involving the specific excited state.
Exact ensemble density-functional theory for excited states
Yang, Zeng-hui; Pribram-Jones, Aurora; Burke, Kieron; Needs, Richard J; Ullrich, Carsten A
2014-01-01
We construct exact Kohn-Sham potentials for the ensemble density-functional theory (EDFT) of excited states from the ground and excited states of helium. The exchange-correlation potential is compared with current approximations, which miss prominent features. The ensemble derivative discontinuity is tested, and the virial theorem is proven and illustrated.
Experimental Investigation of Excited-State Lifetimes in Atomic Ytterbium
Energy Technology Data Exchange (ETDEWEB)
Bowers, C.J.; Budker, D.; Commins, E.D.; DeMille, D.; Freedman, S.J.; Nguyen, A.-T.; Shang, S.-Q.; /UC, Berkeley; Zolotorev, M.; /SLAC
2011-11-15
Lifetimes of 21 excited states in atomic Yb were measured using time-resolved fluorescence detection following pulsed laser excitation. The lifetime of the 4f{sup 14}5d6s {sup 3}D{sub 1} state, which is of particular importance for a proposed study of parity nonconservation in atoms, was measured to be 380(30) ns.
Charge-displacement analysis for excited states
Energy Technology Data Exchange (ETDEWEB)
Ronca, Enrico, E-mail: enrico@thch.unipg.it; Tarantelli, Francesco, E-mail: francesco.tarantelli@unipg.it [Istituto CNR di Scienze e Tecnologie Molecolari, via Elce di Sotto 8, I-06123 Perugia (Italy); Dipartimento di Chimica, Biologia e Biotecnologie, Università degli Studi di Perugia, via Elce di Sotto 8, I-06123 Perugia (Italy); Pastore, Mariachiara, E-mail: chiara@thch.unipg.it; Belpassi, Leonardo; De Angelis, Filippo [Istituto CNR di Scienze e Tecnologie Molecolari, via Elce di Sotto 8, I-06123 Perugia (Italy); Angeli, Celestino; Cimiraglia, Renzo [Dipartimento di Scienze Chimiche e Farmaceutiche, Università degli Studi di Ferrara, via Borsari 46, I-44100 Ferrara (Italy)
2014-02-07
We extend the Charge-Displacement (CD) analysis, already successfully employed to describe the nature of intermolecular interactions [L. Belpassi et al., J. Am. Chem. Soc. 132, 13046 (2010)] and various types of controversial chemical bonds [L. Belpassi et al., J. Am. Chem. Soc. 130, 1048 (2008); N. Salvi et al., Chem. Eur. J. 16, 7231 (2010)], to study the charge fluxes accompanying electron excitations, and in particular the all-important charge-transfer (CT) phenomena. We demonstrate the usefulness of the new approach through applications to exemplary excitations in a series of molecules, encompassing various typical situations from valence, to Rydberg, to CT excitations. The CD functions defined along various spatial directions provide a detailed and insightful quantitative picture of the electron displacements taking place.
Bogoliubov Excited States and the Lyth Bound
Aravind, Aditya; Paban, Sonia
2014-01-01
We show that Bogoliubov excited scalar and tensor modes do not alleviate Planckian evolution during inflation if one assumes that $r$ and the Bogoliubov coefficients are approximately scale invariant. We constrain the excitation parameter for the scalar fluctuations, $\\beta$, and tensor perturbations, $\\tilde{\\beta}$, by requiring that there be at least three decades of scale invariance in the scalar and tensor power spectrum. For the scalar fluctuations this is motivated by the observed nearly scale invariant scalar power spectrum. For the tensor fluctuations this assumption may be shown to be valid or invalid by future experiments.
Density functional theory generalized to degenerate excited states
International Nuclear Information System (INIS)
In this paper it is shown that the density functional theory can be generalized to systems with degenerate excited states. There is a one-to-one map between the subspace, spanned by the ground state and any one of the first degenerate excited states, and the sum of their densities. But only a one way correspondence exists between external potential and subspace, as well as between external potential and the sum of densities. The extension of the Hohenberg-Kohn-Sham theory for degenerate excited states has also been developed. (author)
18Ne Excited States Two-Proton Decay
de Napoli, M.; Rapisarda, E.; Raciti, G.; Cardella, G.; Amorini, F.; Giacoppo, F.; Sfienti, C.
2008-04-01
Two-proton radioactivity studies have been performed on excited states of 18Ne produced by 20Ne fragmentation at the FRS of the Laboratori Nazionali del Sud and excited via Coulomb excitation on a 209Pb target. The 18Ne levels decay has been studied by complete kinematical reconstruction. In spite of the low statistic, the energy and angular correlations of the emitted proton pairs indicate the presence of 2He emission toghether with the democratic decay.
Origin of ultrafast excited state dynamics of 1-nitropyrene.
Murudkar, Sushant; Mora, Aruna K; Singh, Prabhat K; Nath, Sukhendu
2011-10-01
Time-resolved emission measurements in subpicosecond time domain have been carried out for 1-nitropyrene in different solvents to understand the mechanism for the observed ultrafast decay of its first excited singlet state. Excited-state dynamics of 1-nitropyrene is found to be independent of the solvent viscosity. This result contradicts the proposition in the literature (J. Phys. Chem. A 2007, 111, 552) that the ultrafast decay in 1-nitropyrene is due to the large amplitude torsional motion of the nitro group around the pyrene moiety. Excited-state dynamics of 1-nitropyrene in solvents with different dielectric constants shows that excited-state lifetime suddenly increases after a certain value of the dielectric constant. Detailed quantum chemical calculations have been carried out to understand the process that is responsible for the observed effect of the dielectric constant on the excited-state dynamics of 1-nitropyrene. It is seen that the excited-state lifetime and the singlet-triplet energy gap follow similar variation with the dielectric constant of the medium. Such a correlation between the excited-state lifetime and the singlet-triplet energy gap supports the fact that the observed ultrafast decay for 1-nitropyrene is due to an efficient intersystem crossing rather than to the torsional motion of the nitro group as proposed in the literature.
Photoionization of excited states of neon-like Mg III
Indian Academy of Sciences (India)
Narendra Singh; Man Mohan
2002-04-01
The close coupling -matrix method is used to calculate cross-sections for photoionization of Mg III from its ﬁrst three excited states. Conﬁguration interaction wave functions are used to represent two target states of Mg III retained in the -matrix expansion. The positions and effective quantum numbers for the Rydberg series converging to the excited state 2226 \\ 2 of the residual ion, are predicted.
Quantum entanglement of localized excited states at finite temperature
Caputa, Pawel; Simón, Joan; Štikonas, Andrius(School of Mathematics and Maxwell Institute for Mathematical Sciences, University of Edinburgh, King’s Buildings, Edinburgh, EH9 3FD, U.K.); Takayanagi, Tadashi
2015-01-01
In this work we study the time evolutions of (Renyi) entanglement entropy of locally excited states in two dimensional conformal field theories (CFTs) at finite temperature.We consider excited states created by acting with local operators on thermal states and give both field theoretic and holographic calculations. In free field CFTs, we find that the growth of Renyi entanglement entropy at finite temperature is reduced compared to the zero temperature result by a small quantity proportional ...
Closser, Kristina D; Ge, Qinghui; Mao, Yuezhi; Shao, Yihan; Head-Gordon, Martin
2015-12-01
We develop a local excited-state method, based on the configuration interaction singles (CIS) wave function, for large atomic and molecular clusters. This method exploits the properties of absolutely localized molecular orbitals (ALMOs), which strictly limits the total number of excitations, and results in formal scaling with the third power of the system size for computing the full spectrum of ALMO-CIS excited states. The derivation of the equations and design of the algorithm are discussed in detail, with particular emphasis on the computational scaling. Clusters containing ∼500 atoms were used in evaluating the scaling, which agrees with the theoretical predictions, and the accuracy of the method is evaluated with respect to standard CIS. A pioneering application to the size dependence of the helium cluster spectrum is also presented for clusters of 25-231 atoms, the largest of which results in the computation of 2310 excited states per sampled cluster geometry. PMID:26609558
Excited state systematics in extracting nucleon electromagnetic form factors
Capitani, Stefano; von Hippel, Georg; Jäger, Benjamin; Knippschild, Bastian; Meyer, Harvey B; Rae, Thomas D; Wittig, Hartmut
2012-01-01
We present updated preliminary results for the nucleon electromagnetic form factors for non-perturbatively $\\mathcal{O}(a)$ improved Wilson fermions in $N_f=2$ QCD measured on the CLS ensembles. The use of the summed operator insertion method allows us to suppress the influence of excited states in our measurements. A study of the effect that excited state contaminations have on the $Q^2$ dependence of the extracted nucleon form factors may then be made through comparisons of the summation method to standard plateau fits, as well as to excited state fits.
Anisotropy of electronic states excited in ion-atom collisions
International Nuclear Information System (INIS)
The author reports coincidence measurements made on the He+ + Ne and He+ + He systems. The complex population amplitudes for the magnetic sublevels of the investigated excited states, Ne(2p43s2)1D and He(2p2)1D, were completely determined and possible excitation mechanisms are described. (Auth.)
Study of excited nucleon states at EBAC: status and plans
Energy Technology Data Exchange (ETDEWEB)
Hiroyuki Kamano
2009-12-01
We present an overview of a research program for the excited nucleon states in Excited Baryon Analysis Center (EBAC) at Jefferson Lab. Current status of our analysis of the meson production reactions based on the unitary dynamical coupled-channels model is summarized, and the N* pole positions extracted from the constructed scattering amplitudes are presented. Our plans for future developments are also discussed.
Excited-State Dynamics in Folic Acid and 6-CARBOXYPTERIN upon Uva Excitation
Huang, Huijuan; Vogt, R. Aaron; Crespo-Hernandez, Carlos E.
2013-06-01
The excited-state dynamics of folic acid (FA) and 6-carboxypterin (6CP) are poorly understood and work is needed to uncover the relaxation pathways that ultimately lead to their oxidative damage of DNA. In our approach, broad-band transient absorption spectroscopy was used to monitor the evolution of the excited states in FA and 6CP in basic aqueous solution upon excitation at 350 nm. In addition, quantum-chemical calculations were performed to assist in the interpretation of the experimental results and in the postulation of kinetic mechanisms. The combined experimental and computational results support a kinetic model where excitation of FA results in ultrafast charge separation (τ = 0.6 ps), which decays back to the ground state primarily by charge recombination with a lifetime of 2.2 ps. A small fraction of the charge transfer state undergoes intersystem crossing to populate the lowest-energy triplet state with a lifetime of 200 ps. On the other hand, a large fraction of the initially excited singlet state in 6CP decays by fluorescence emission with a lifetime of 100 ps, while intersystem crossing to the triplet state occurs with a lifetime of 4.4 ns. The potential implications of these results to the oxidative damage of DNA by FA and 6CP will be discussed. Funding from the National Science Foundation is gratefully acknowledged (CHE-1255084).
Vibronic coupling in the excited-states of carotenoids.
Miki, Takeshi; Buckup, Tiago; Krause, Marie S; Southall, June; Cogdell, Richard J; Motzkus, Marcus
2016-04-28
The ultrafast femtochemistry of carotenoids is governed by the interaction between electronic excited states, which has been explained by the relaxation dynamics within a few hundred femtoseconds from the lowest optically allowed excited state S2 to the optically dark state S1. Extending this picture, some additional dark states (3A(g)(-) and 1B(u)(-)) and their interaction with the S2 state have also been suggested to play a major role in the ultrafast deactivation of carotenoids and their properties. Here, we investigate the interaction between such dark and bright electronic excited states of open chain carotenoids, particularly its dependence on the number of conjugated double bonds (N). We focus on the ultrafast wave packet motion on the excited potential surface, which is modified by the interaction between bright and dark electronic states. Such a coupling between electronic states leads to a shift of the vibrational frequency during the excited-state evolution. In this regard, pump-degenerate four-wave mixing (pump-DFWM) is applied to a series of carotenoids with different numbers of conjugated double bonds N = 9, 10, 11 and 13 (neurosporene, spheroidene, lycopene and spirilloxanthin, respectively). Moreover, we demonstrate in a closed-chain carotenoid (lutein) that the coupling strength and therefore the vibrational shift can be tailored by changing the energy degeneracy between the 1B(u)(+) and 1B(u)(-) states via solvent interaction.
Ultrafast Excited-State Dynamics in Biological Environments
Fürstenberg, Alexandre; Vauthey, Eric
2007-01-01
We discuss and illustrate by several examples how the ultrafast excited-state dynamics of a chromophore can be altered when changing its environment from a homogenous solution to a biological molecule such as proteins or nucleic acids.
The examination of berberine excited state by laser flash photolysis
Cheng, Lingli; Wang, Mei; Zhao, Ping; Zhu, Hui; Zhu, Rongrong; Sun, Xiaoyu; Yao, Side; Wang, Shilong
2009-07-01
The property of the excited triplet state of berberine (BBR) was investigated by using time-resolved laser flash photolysis of 355 nm in acetonitrile. The transient absorption spectra of the excited triplet BBR were obtained in acetonitrile, which have an absorption maximum at 420 nm. And the ratio of excitation to ionization of BBR in acetonitrile solvent was calculated. The self-decay and self-quenching rate constants, and the absorption coefficient of 3BBR* were investigated and the excited state quantum yield was determined. Furthermore utilizing the benzophenone (BEN) as a triplet sensitizer, and the β-carotene (Car) as an excited energy transfer acceptor, the assignment of 3BBR* was further confirmed and the related energy transfer rate constants were also determined.
Controlling Chimera States - The influence of excitable units
Isele, Thomas; Hizanidis, Johanne; Provata, Astero; Hövel, Philipp
2015-01-01
We explore the influence of a block of excitable units on the existence and behavior of chimera states in a nonlocally coupled ring-network of FitzHugh-Nagumo elements. The FitzHugh-Nagumo system, a paradigmatic model in many fields from neuroscience to chemical pattern formation and nonlinear electronics, exhibits oscillatory or excitable behavior depending on the values of its parameters. Until now, chimera states have been studied in networks of coupled oscillatory FitzHugh-Nagumo elements...
Metastable states of highly excited heavy ions
Pegg, D. J.; Griffin, P. M.; Sellin, I. A.; Smith, W. W.; Donnally, B.
1973-01-01
Description of the method used and results obtained in an experimental study of the metastable states of highly stripped heavy ions, aimed at determining the lifetimes of such states by the rates of autoionization and radiation. The significance and limitations of the results presented are discussed.
Institute of Scientific and Technical Information of China (English)
2002-01-01
Neutron capture processes on carbon isotope play an important role in astrophysics ranging fromnucleosynthesis in the stellar helium and carbon burning stages to possibly inhomogeneous big bangmodels. The capture rate in astrophysical environments strongly depends on the structure of these carbonnuclei. For example, the first 1/2+ state in 13C is a neutron halo state, and these results in an enormous
Characterizing RNA Excited States using NMR Relaxation Dispersion
Xue, Yi; Kellogg, Dawn; Kimsey, Isaac J; Sathyamoorthy, Bharathwaj; Stein, Zachary W; McBrairty, Mitchell; Al-Hashimi, Hashim M.
2016-01-01
Changes in RNA secondary structure play fundamental roles in the cellular functions of a growing number of non-coding RNAs. This chapter describes NMR-based approaches for characterizing microsecond-to-millisecond changes in RNA secondary structure that are directed toward short-lived and low-populated species often referred to as “excited states”. Compared to larger-scale changes in RNA secondary structure, transitions towards excited states do not require assistance from chaperones, are often orders of magnitude faster, and are localized to a small number of nearby base pairs in and around non-canonical motifs. Here we describe a procedure for characterizing RNA excited states using off-resonance R1ρ NMR relaxation dispersion utilizing low-to-high spin-lock fields (25–3000 Hz). R1ρ NMR relaxation dispersion experiments are used to measure carbon and nitrogen chemical shifts in base and sugar moieties of the excited state. The chemical shift data is then interpreted with the aid of secondary structure prediction to infer potential excited states that feature alternative secondary structures. Candidate structures are then tested by using mutations, single-atom substitutions, or by changing physiochemical conditions, such as pH and temperature, to either stabilize or destabilize the candidate excited state. The resulting chemical shifts of the mutants or under different physiochemical conditions are then compared to those of the ground and excited state. Application is illustrated with a focus on the transactivation response element (TAR) from the human immune deficiency virus type 1 (HIV-1), which exists in dynamic equilibrium with at least two distinct excited states. PMID:26068737
Excited States of the divacancy in SiC
Bockstedte, Michel; Garratt, Thomas; Ivady, Viktor; Gali, Adam
2014-03-01
The divacancy in SiC - a technologically mature material that fulfills the necessary requirements for hosting defect based quantum computing - is a good candidate for implementing a solid state quantum bit. Its ground state is isovalent to the NV center in diamond as demonstrated by density functional theory (DFT). Furthermore, coherent manipulation of divacancy spins in SiC has been demonstrated. The similarities to NV might indicate that the same inter system crossing (ICS) from the high to the low spin state is responsible for its spin-dependent fluorescent signal. By DFT and a DFT-based multi-reference hamiltonian we analyze the excited state spectrum of the defects. In contrast to the current picture of the spin dynamics of the NV center, we predict that a static Jahn-Teller effect in the first excited triplet states governs an ICS both with the excited and ground state of the divacancy.
Microwave spectroscopy of furfural in vibrationally excited states
Motiyenko, R. A.; Alekseev, E. A.; Dyubko, S. F.
2007-07-01
The results of microwave spectrum investigation of the excited vibrational states of furfural in the frequency range between 49 and 149 GHz are reported. In total 15 excited vibrational states (9 for trans-furfural and 6 for cis-furfural) were assigned and analyzed. Six of the 15 investigated states were assigned for the first time. Accurate values of rigid rotor and quartic centrifugal distortion constants of asymmetric top Hamiltonian have been determined for 13 excited states. Also for some states several sextic and octic level constants were needed in order to fit the data within experimental accuracy. The vt = 3 and vs = 1, va = 1 states of trans-furfural were found to be strongly perturbed and only rotational transitions with low Ka values can be reliably identified in this study.
Neutral Excitations in the Gaffnian state
Kang, Byungmin; Moore, Joel E.
The Fractional Quantum Hall Effect (FQHE) is one of the most well-studied systems having topological order. Starting with the pioneering work by Laughlin, the model wave function approach has been shown to provide essential information for understanding topological order in gapped incompressible states. We study a model wave function called the Gaffnian state which is believed to represent a gapless, strongly correlated state that is very different from conventional metals. To understand this exotic gapless state better, we provide a representation in which the pairing structure of the Gaffnian state becomes more explicit. We employ the single-mode approximation of the Girvin-MacDonald-Platzman (GMP) mode, which is a neutral collective exitation mode, in order to have a physical picture of the gaplessness of the Gaffnian state. In particular, we discuss how to extract systematically the relevant physics in the long-distance, large electron number limit of the FQH states using a numerical calculation with relatively few electrons.
The excited state antiaromatic benzene ring: a molecular Mr Hyde?
Papadakis, Raffaello; Ottosson, Henrik
2015-09-21
The antiaromatic character of benzene in its first ππ* excited triplet state (T1) was deduced more than four decades ago by Baird using perturbation molecular orbital (PMO) theory [J. Am. Chem. Soc. 1972, 94, 4941], and since then it has been confirmed through a range of high-level quantum chemical calculations. With focus on benzene we now first review theoretical and computational studies that examine and confirm Baird's rule on reversal in the electron count for aromaticity and antiaromaticity of annulenes in their lowest triplet states as compared to Hückel's rule for the ground state (S0). We also note that the rule according to quantum chemical calculations can be extended to the lowest singlet excited state (S1) of benzene. Importantly, Baird, as well as Aihara [Bull. Chem. Soc. Jpn. 1978, 51, 1788], early put forth that the destabilization and excited state antiaromaticity of the benzene ring should be reflected in its photochemical reactivity, yet, today these conclusions are often overlooked. Thus, in the second part of the article we review photochemical reactions of a series of benzene derivatives that to various extents should stem from the excited state antiaromatic character of the benzene ring. We argue that benzene can be viewed as a molecular "Dr Jekyll and Mr Hyde" with its largely unknown excited state antiaromaticity representing its "Mr Hyde" character. The recognition of the "Jekyll and Hyde" split personality feature of the benzene ring can likely be useful in a range of different areas. PMID:25960203
Direct observation of photoinduced bent nitrosyl excited-state complexes
Energy Technology Data Exchange (ETDEWEB)
Sawyer, Karma R.; Steele, Ryan P.; Glascoe, Elizabeth A.; Cahoon, James F.; Schlegel, Jacob P.; Head-Gordon, Martin; Harris, Charles B.
2008-06-28
Ground state structures with side-on nitrosyl ({eta}{sup 2}-NO) and isonitrosyl (ON) ligands have been observed in a variety of transition-metal complexes. In contrast, excited state structures with bent-NO ligands have been proposed for years but never directly observed. Here we use picosecond time-resolved infrared spectroscopy and density functional theory (DFT) modeling to study the photochemistry of Co(CO){sub 3}(NO), a model transition-metal-NO compound. Surprisingly, we have observed no evidence for ON and {eta}{sup 2}-NO structural isomers, but have observed two bent-NO complexes. DFT modeling of the ground and excited state potentials indicates that the bent-NO complexes correspond to triplet excited states. Photolysis of Co(CO){sub 3}(NO) with a 400-nm pump pulse leads to population of a manifold of excited states which decay to form an excited state triplet bent-NO complex within 1 ps. This structure relaxes to the ground triplet state in ca. 350 ps to form a second bent-NO structure.
Controlling chimera states: The influence of excitable units
Isele, Thomas; Hizanidis, Johanne; Provata, Astero; Hövel, Philipp
2016-02-01
We explore the influence of a block of excitable units on the existence and behavior of chimera states in a nonlocally coupled ring-network of FitzHugh-Nagumo elements. The FitzHugh-Nagumo system, a paradigmatic model in many fields from neuroscience to chemical pattern formation and nonlinear electronics, exhibits oscillatory or excitable behavior depending on the values of its parameters. Until now, chimera states have been studied in networks of coupled oscillatory FitzHugh-Nagumo elements. In the present work, we find that introducing a block of excitable units into the network may lead to several interesting effects. It allows for controlling the position of a chimera state as well as for generating a chimera state directly from the synchronous state.
Shape vibrations and quasiparticle excitations in the lowest 0+ excited state of the Erbium isotopes
Chen, Fang-Qi
2016-01-01
The ground and first excited 0+ states of the {156-172}Er isotopes are analyzed in the framework of the generator coordinate method. The shape parameter beta is used to generate wave functions with different deformations which together with the two-quasiparticle states built on them provide a set of states. An angular momentum and particle number projection of the latter spawn the basis states of the generator coordinate method. With this ansatz and using the separable pairing plus quadrupole interaction we obtain a good agreement with the experimental spectra and E2 transition rates up to moderate spin values. The structure of the wave functions suggests that the first excited 0+ states in the soft Er isotopes are dominated by shape fluctuations, while in the well deformed Er isotopes the two-quasiparticle states are more relevant. In between both degrees of freedom are necessary .
Shape vibration and quasiparticle excitations in the lowest 0+ excited state in erbium isotopes
Chen, Fang-Qi; Egido, J. Luis
2016-06-01
The ground and first excited 0+ states of the -172Er156 isotopes are analyzed in the framework of the generator coordinate method. The shape parameter β is used to generate wave functions with different deformations which together with the two-quasiparticle states built on them provide a set of states. An angular momentum and particle number projection of the latter spawn the basis states of the generator coordinate method. With this ansatz and using the separable pairing plus quadrupole interaction we obtain a good agreement with the experimental spectra and E 2 transition rates up to moderate spin values. The structure of the wave functions suggests that the first excited 0+ states in the soft Er isotopes are dominated by shape fluctuations, while in the well deformed Er isotopes the two-quasiparticle states are more relevant. In between, both degrees of freedom are necessary.
Nature of ground and electronic excited states of higher acenes.
Yang, Yang; Davidson, Ernest R; Yang, Weitao
2016-08-30
Higher acenes have drawn much attention as promising organic semiconductors with versatile electronic properties. However, the nature of their ground state and electronic excited states is still not fully clear. Their unusual chemical reactivity and instability are the main obstacles for experimental studies, and the potentially prominent diradical character, which might require a multireference description in such large systems, hinders theoretical investigations. Here, we provide a detailed answer with the particle-particle random-phase approximation calculation. The (1)Ag ground states of acenes up to decacene are on the closed-shell side of the diradical continuum, whereas the ground state of undecacene and dodecacene tilts more to the open-shell side with a growing polyradical character. The ground state of all acenes has covalent nature with respect to both short and long axes. The lowest triplet state (3)B2u is always above the singlet ground state even though the energy gap could be vanishingly small in the polyacene limit. The bright singlet excited state (1)B2u is a zwitterionic state to the short axis. The excited (1)Ag state gradually switches from a double-excitation state to another zwitterionic state to the short axis, but always keeps its covalent nature to the long axis. An energy crossing between the (1)B2u and excited (1)Ag states happens between hexacene and heptacene. Further energetic consideration suggests that higher acenes are likely to undergo singlet fission with a low photovoltaic efficiency; however, the efficiency might be improved if a singlet fission into multiple triplets could be achieved. PMID:27528690
Cluster structure in highly-excited states of light nuclei
International Nuclear Information System (INIS)
The cluster structure in the highly-excited states of light nuclei are investigated using the multi-cluster model. For this purpose, we propose a developed treatment method of the multi-cluster model. The method consists of two parts: One is a systematic construction method of the multi-cluster Pauli-allowed states. Another is a truncation method of the large model space of the multi-cluster system. We show that we can easily solve the equation of the orthogonality condition model (OCM) for complex multi-cluster systems by the use of the method. We apply the multi-cluster models 3α, 4α, 12C + 2α and 16O + 2α to 12C, 16O, 20Ne and 24Mg, respectively. As shown in the Ikeda diagram, these models open a very interesting problem not only of the cluster structure in the highly-excited states of those nuclei but also of the structure change between different cluster structures. We show a typical example of the 16O + 2α model for 24Mg ; 1) many excited states with the 20Ne-α cluster structure are obtained at excitation energies above 10 MeV, 2) the 16O-8Be cluster states are obtained at the energy region higher than 20 MeV, and 3) the very interesting states with the α-16O-α linear-chain-like structure are predicted at about 20 MeV excitation energy. (author)
Charge transfer excitations from excited state Hartree-Fock subsequent minimization scheme
Energy Technology Data Exchange (ETDEWEB)
Theophilou, Iris, E-mail: i.theophilou@fz-juelich.de [Peter Grunberg Institut (PGI) Forschungszentrum Jülich, D-52425 Jülich (Germany); Tassi, M.; Thanos, S. [Institute for Advanced Materials, Physicochemical Processes, Nanotechnology and Microsystems, ‘Demokritos’ National Center for Scientific Research, 15310 Athens (Greece)
2014-04-28
Photoinduced charge-transfer processes play a key role for novel photovoltaic phenomena and devices. Thus, the development of ab initio methods that allow for an accurate and computationally inexpensive treatment of charge-transfer excitations is a topic that nowadays attracts a lot of scientific attention. In this paper we extend an approach recently introduced for the description of single and double excitations [M. Tassi, I. Theophilou, and S. Thanos, Int. J. Quantum Chem. 113, 690 (2013); M. Tassi, I. Theophilou, and S. Thanos, J. Chem. Phys. 138, 124107 (2013)] to allow for the description of intermolecular charge-transfer excitations. We describe an excitation where an electron is transferred from a donor system to an acceptor one, keeping the excited state orthogonal to the ground state and avoiding variational collapse. These conditions are achieved by decomposing the space spanned by the Hartree-Fock (HF) ground state orbitals into four subspaces: The subspace spanned by the occupied orbitals that are localized in the region of the donor molecule, the corresponding for the acceptor ones and two more subspaces containing the virtual orbitals that are localized in the neighborhood of the donor and the acceptor, respectively. Next, we create a Slater determinant with a hole in the subspace of occupied orbitals of the donor and a particle in the virtual subspace of the acceptor. Subsequently we optimize both the hole and the particle by minimizing the HF energy functional in the corresponding subspaces. Finally, we test our approach by calculating the lowest charge-transfer excitation energies for a set of tetracyanoethylene-hydrocarbon complexes that have been used earlier as a test set for such kind of excitations.
Neutron halos in the excited states for N=127 isotones
Institute of Scientific and Technical Information of China (English)
SUN Qin; GUO Jian-You
2009-01-01
Properties of the ground states and the excited states of N=127 isotones are investigated by using the nonlinear relativistic mean field theory with the interactions PK1. By analyzing the rms of proton and neutron, the single particle energies of valence nucleon and the density distributions of neutron, proton and the last neutron, it can be found that there exists a neutron halo in the excited states of 3d5/2, 4s1/2 and 3d3/2 in 209Pb. It is also predicted that there exists a neutron halo in the excited states of 3d5/2, 4s1/2 and 3d3/2 in 207Hg, 208Tl, 210Bi and 211Po.
Super-atom molecular orbital excited states of fullerenes.
Johansson, J Olof; Bohl, Elvira; Campbell, Eleanor E B
2016-09-13
Super-atom molecular orbitals are orbitals that form diffuse hydrogenic excited electronic states of fullerenes with their electron density centred at the centre of the hollow carbon cage and a significant electron density inside the cage. This is a consequence of the high symmetry and hollow structure of the molecules and distinguishes them from typical low-lying molecular Rydberg states. This review summarizes the current experimental and theoretical studies related to these exotic excited electronic states with emphasis on femtosecond photoelectron spectroscopy experiments on gas-phase fullerenes.This article is part of the themed issue 'Fullerenes: past, present and future, celebrating the 30th anniversary of Buckminster Fullerene'.
Simulations of Sisyphus cooling including multiple excited states
Svensson, F; Dion, C M
2008-01-01
We extend the theory for laser cooling in a near-resonant optical lattice to include multiple excited hyperfine states. Simulations are performed treating the external degrees of freedom of the atom, i.e., position and momentum, classically, while the internal atomic states are treated quantum mechanically, allowing for arbitrary superpositions. Whereas theoretical treatments including only a single excited hyperfine state predict that the temperature should be a function of lattice depth only, except close to resonance, experiments have shown that the minimum temperature achieved depends also on the detuning from resonance of the lattice light. Our results resolve this discrepancy.
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
A combination of steady-state and dynamic spectral measurements are used to provide new insights into the nature of the excited-state processes of all-trans-1,4-diphenyl-1,3-butadiene and several analogs: 1,4-diphenyl- 1,3-cyclopentadiene, 1,1,4,4-tetraphenylbutadiene, 1,2,3,4-tetraphenyl-1...
Electronic excited states and relaxation dynamics in polymer heterojunction systems
Ramon, John Glenn Santos
The potential for using conducting polymers as the active material in optoelectronic devices has come to fruition in the past few years. Understanding the fundamental photophysics behind their operations points to the significant role played by the polymer interface in their performance. Current device architectures involve the use of bulk heterojunctions which intimately blend the donor and acceptor polymers to significantly increase not only their interfacial surface area but also the probability of exciton formation within the vicinity of the interface. In this dissertation, we detail the role played by the interface on the behavior and performance of bulk heterojunction systems. First, we explore the relation between the exciton binding energy to the band offset in determining device characteristics. As a general rule, when the exciton binding energy is greater than the band offset, the exciton remains the lowest energy excited state leading to efficient light-emitting properties. On the other hand, if the offset is greater than the binding energy, charge separation becomes favorable leading to better photovoltaic behavior. Here, we use a Wannier function, configuration interaction based approach to examine the essential excited states and predict the vibronic absorption and emission spectra of the PPV/BBL, TFB/F8BT and PFB/F8BT heterojunctions. Our results underscore the role of vibrational relaxation in the formation of charge-transfer states following photoexcitation. In addition, we look at the relaxation dynamics that occur upon photoexcitation. For this, we adopt the Marcus-Hush semiclassical method to account for lattice reorganization in the calculation of the interconversion rates in TFB/F8BT and PFB/F8BT. We find that, while a tightly bound charge-transfer state (exciplex) remains the lowest excited state, a regeneration pathway to the optically active lowest excitonic state in TFB/F8BT is possible via thermal repopulation from the exciplex. Finally
Quantum Entanglement of Localized Excited States at Finite Temperature
Caputa, Pawel; Stikonas, Andrius; Takayanagi, Tadashi
2014-01-01
In this work we study the time evolutions of (Renyi) entanglement entropy of locally excited states in two dimensional conformal field theories (CFTs) at finite temperature. We consider excited states created by acting with local operators on thermal states and give both field theoretic and holographic calculations. In free field CFTs, we find that the growth of Renyi entanglement entropy at finite temperature is reduced compared to the zero temperature result by a small quantity proportional to the width of the localized excitations. On the other hand, in finite temperature CFTs with classical gravity duals, we find that the entanglement entropy approaches a characteristic value at late time. This behaviour does not occur at zero temperature. We also study the mutual information between the two CFTs in the thermofield double (TFD) formulation and give physical interpretations of our results.
Quantum entanglement of localized excited states at finite temperature
Caputa, Pawel; Simón, Joan; Štikonas, Andrius; Takayanagi, Tadashi
2015-01-01
In this work we study the time evolutions of (Renyi) entanglement entropy of locally excited states in two dimensional conformal field theories (CFTs) at finite temperature. We consider excited states created by acting with local operators on thermal states and give both field theoretic and holographic calculations. In free field CFTs, we find that the growth of Renyi entanglement entropy at finite temperature is reduced compared to the zero temperature result by a small quantity proportional to the width of the localized excitations. On the other hand, in finite temperature CFTs with classical gravity duals, we find that the entanglement entropy approaches a characteristic value at late time. This behaviour does not occur at zero temperature. We also study the mutual information between the two CFTs in the thermofield double (TFD) formulation and give physical interpretations of our results.
State-Selective Excitation of Quantum Systems via Geometrical Optimization.
Chang, Bo Y; Shin, Seokmin; Sola, Ignacio R
2015-09-01
We lay out the foundations of a general method of quantum control via geometrical optimization. We apply the method to state-selective population transfer using ultrashort transform-limited pulses between manifolds of levels that may represent, e.g., state-selective transitions in molecules. Assuming that certain states can be prepared, we develop three implementations: (i) preoptimization, which implies engineering the initial state within the ground manifold or electronic state before the pulse is applied; (ii) postoptimization, which implies engineering the final state within the excited manifold or target electronic state, after the pulse; and (iii) double-time optimization, which uses both types of time-ordered manipulations. We apply the schemes to two important dynamical problems: To prepare arbitrary vibrational superposition states on the target electronic state and to select weakly coupled vibrational states. Whereas full population inversion between the electronic states only requires control at initial time in all of the ground vibrational levels, only very specific superposition states can be prepared with high fidelity by either pre- or postoptimization mechanisms. Full state-selective population inversion requires manipulating the vibrational coherences in the ground electronic state before the optical pulse is applied and in the excited electronic state afterward, but not during all times. PMID:26575896
First-principles Calculation of Excited State Spectra in QCD
Energy Technology Data Exchange (ETDEWEB)
Jozef Dudek,Robert Edwards,Michael Peardon,David Richards,Christopher Thomas
2011-05-01
Recent progress at understanding the excited state spectra of mesons and baryons is described. I begin by outlining the application of the variational method to compute the spectrum of QCD, and then present results for the excited meson spectrum, with continuum quantum numbers of the states clearly delineated. I emphasise the need to extend the calculation to encompass multi-hadron contributions, and describe a recent calculation of the I=2 pion-pion energy-dependent phase shifts as a precursor to the study of channels with resonant behavior. I conclude with recent results for the low lying baryon spectrum, and the prospects for future calculations.
Kinetic studies following state-selective laser excitation
International Nuclear Information System (INIS)
The objective of this contract is the study of state-to-state, electronic energy transfer reactions following two-photon laser excitation. We have chosen to study reactions of Xe 5p5np because of their relevance to the XeCl excimer laser. We are studying deactivation reactions in collisions with heavy atoms such as Ar, Kr, and Xe and reactive collisions with chlorides. The reactants are excited by multiphoton laser absorption. Product channels are observed by their fluorescence, or by laser induced fluorescence using a second color laser. 36 refs., 16 figs., 5 tabs
Coherent excitation of a single atom to a Rydberg state
DEFF Research Database (Denmark)
Miroshnychenko, Yevhen; Gaëtan, Alpha; Evellin, Charles;
2010-01-01
We present the coherent excitation of a single Rubidium atom to the Rydberg state 58d3/2 using a two-photon transition. The experimental setup is described in detail, as are experimental techniques and procedures. The coherence of the excitation is revealed by observing Rabi oscillations between...... ground and Rydberg states of the atom. We analyze the observed oscillations in detail and compare them to numerical simulations which include imperfections of our experimental system. Strategies for future improvements on the coherent manipulation of a single atom in our settings are given....
Equations of state for self-excited MHD generator studies
Energy Technology Data Exchange (ETDEWEB)
Rogers, F.J.; Ross, M.; Haggin, G.L.; Wong, L.K.
1980-02-26
We have constructed a state-of-the-art equation of state (EOS) for argon covering the temperature density range attainable by currently proposed self-excited MHD generators. The EOS for conditions in the flow channel was obtained primarily by a non-ideal plasma code (ACTEX) that is based on a many body activity expansion. For conditions in the driver chamber the EOS was primarily obtained from a fluid code (HDFP) that calculates the fluid properties from perturbation theory based on the insulator interatomic pair potential but including electronic excitations. The results are in agreement with several sets of experimental data in the 0.6 - 91 GPa pressure range.
Vibrational relaxation pathways in the electronic excited state of carotenoid
International Nuclear Information System (INIS)
The intra- and inter-molecular vibrational relaxation in the electronic excited state (1Bu+) of spheroidene derivative (the number of conjugated double bonds, n=8) has been investigated at room temperature by means of femtosecond time-resolved fluorescence spectroscopy based on an optical-Kerr-gate technique. Depending on the photo-excitation either to the 1Bu+(v=1) or 1Bu+(v=2) vibronic level, remarkable differences were observed in hot luminescence spectra related to the vibrational relaxation process of high- and low-frequency modes. Under the excitation to the 1Bu+(v=2) state hot luminescence from the 1Bu+(v=1) state was observed as a dominant feature of the time-resolved spectra while the dynamic Stokes shift originating from the low-frequency-modes dynamics was clearly observed under the excitation to the 1Bu+(v=1). These observations of the excitation energy dependence of time-resolved fluorescence spectra were discussed by analyzing the Franck-Condon factors of transitions from v=0,1, and 2 levels of high-frequency modes
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.
Excited State Structural Dynamics of Carotenoids and Charge Transfer Systems
International Nuclear Information System (INIS)
This dissertation describes the development and implementation of a visible/near infrared pump/mid-infrared probe apparatus. Chapter 1 describes the background and motivation of investigating optically induced structural dynamics, paying specific attention to solvation and the excitation selection rules of highly symmetric molecules such as carotenoids. Chapter 2 describes the development and construction of the experimental apparatus used throughout the remainder of this dissertation. Chapter 3 will discuss the investigation of DCM, a laser dye with a fluorescence signal resulting from a charge transfer state. By studying the dynamics of DCM and of its methyl deuterated isotopomer (an otherwise identical molecule), we are able to investigate the origins of the charge transfer state and provide evidence that it is of the controversial twisted intramolecular (TICT) type. Chapter 4 introduces the use of two-photon excitation to the S1 state, combined with one-photon excitation to the S2 state of the carotenoid beta-apo-8'-carotenal. These 2 investigations show evidence for the formation of solitons, previously unobserved in molecular systems and found only in conducting polymers Chapter 5 presents an investigation of the excited state dynamics of peridinin, the carotenoid responsible for the light harvesting of dinoflagellates. This investigation allows for a more detailed understanding of the importance of structural dynamics of carotenoids in light harvesting
Wave packet dynamics in molecular excited electronic states
International Nuclear Information System (INIS)
We theoretically explore the use of UV pump – UV probe schemes to resolve in time the dynamics of nuclear wave packets in excited electronic states of the hydrogen molecule. The pump pulse ignites the dynamics in singly excited states, that will be probed after a given time delay by a second identical pulse that will ionize the molecule. The field-free molecular dynamics is first explored by analyizing the autocorrelation function for the pumped wave packet and the excitation probabilities. We investigate both energy and angle differential ionization probabilities and demonstrate that the asymmetry induced in the electron angular distributions gives a direct map of the time evolution of the pumped wave packet
Excited charmonium states from Bethe-Salpeter equation
Sauli, Vladimir
2011-01-01
We solve the Bethe-Salpeter equation for a system of a heavy quark-antiquark pair interacting with a screened linear confining potential. First we show the spinless QFT model is inadequate and fail to describe even gross feature of the quarkonia spectrum. In order to get reliable description the spine degrees of freedom has to be considered. Within the approximation employed we reasonably reproduce known radial excitation of vector charmonium. The BSE favors relatively large string breaking scale $\\mu\\simeq 350MeV$ . Using free charm quark propagators we observe that $J/\\Psi$ is the only charmonium left bellow naive quark-antiquark threshold $2m_c$, while the all excited states are situated above this threshold. Within the numerical method we overcome obstacles related with threshold singularity and discuss the consequences of the use of free propagators for calculation of excited states above the threshold.
Size dependent deactivation of the excited state of DHICA
DEFF Research Database (Denmark)
Gauden, Magdalena; Pezzella, Alessandro; Panzella, Lucia;
2008-01-01
Melanin is a natural pigment mainly responsible for the protection of skin and eyes from UV damage. 5,6- dihydroxyindole- 2 carboxylic acid (DHICA) is a key melanin building block. We have investigated the excited state dynamics of DHICA as well as its derivatives and oligomeric units using ultra...
Calculation of neutral beam deposition accounting for excited states
Energy Technology Data Exchange (ETDEWEB)
Gianakon, T.A.
1992-09-01
Large-scale neutral-beam auxillary heating of plasmas has led to new plasma operational regimes which are often dominated by fast ions injected via the absorption of an energetic beam of hydrogen neutrals. An accurate simulation of the slowing down and transport of these fast ions requires an intimate knowledge of the hydrogenic neutral deposition on each flux surface of the plasma. As a refinement to the present generation of transport codes, which base their beam deposition on ground-state reaction rates, a new set of routines, based on the excited states of hydrogen, is presented as mechanism for computing the attenuation and deposition of a beam of energetic neutrals. Additionally, the numerical formulations for the underlying atomic physics for hydrogen impacting on the constiuent plasma species is developed and compiled as a numerical database. Sample results based on this excited state model are compared with the ground-state model for simple plasma configurations.
Excited-state quantum phase transition in the Rabi model
Puebla, Ricardo; Hwang, Myung-Joong; Plenio, Martin B.
2016-08-01
The Rabi model, a two-level atom coupled to a harmonic oscillator, can undergo a second-order quantum phase transition (QPT) [M.-J. Hwang et al., Phys. Rev. Lett. 115, 180404 (2015), 10.1103/PhysRevLett.115.180404]. Here we show that the Rabi QPT accompanies critical behavior in the higher-energy excited states, i.e., the excited-state QPT (ESQPT). We derive analytic expressions for the semiclassical density of states, which show a logarithmic divergence at a critical energy eigenvalue in the broken symmetry (superradiant) phase. Moreover, we find that the logarithmic singularities in the density of states lead to singularities in the relevant observables in the system such as photon number and atomic polarization. We corroborate our analytical semiclassical prediction of the ESQPT in the Rabi model with its numerically exact quantum mechanical solution.
Direct excitation of butterfly states in Rydberg molecules
Lippe, Carsten; Niederpruem, Thomas; Thomas, Oliver; Eichert, Tanita; Ott, Herwig
2016-05-01
Since their first theoretical prediction Rydberg molecules have become an increasing field of research. These exotic states originate from the binding of a ground state atom in the electronic wave function of a highly-excited Rydberg atom mediated by a Fermi contact type interaction. A special class of long-range molecular states, the butterfly states, were first proposed by Greene et al.. These states arise from a shape resonance in the p-wave scattering channel of a ground state atom and a Rydberg electron and are characterized by an electron wavefunction whose density distribution resembles the shape of a butterfly. We report on the direct observation of deeply bound butterfly states of Rydberg molecules of 87 Rb. The butterfly states are studied by high resolution spectroscopy of UV-excited Rydberg molecules. We find states bound up to - 50 GHz from the 25 P1/2 , F = 1 state, corresponding to binding lengths of 50a0 to 500a0 and with permanent electric dipole moments of up to 500 Debye. This distinguishes the observed butterfly states from the previously observed long range Rydberg molecules in rubidium.
Optimized resonating valence bond state in square lattice: correlations & excitations
Directory of Open Access Journals (Sweden)
Z Nourbakhsh
2009-09-01
Full Text Available We consider RVB state as a variational estimate for the ground state of Heisenberg antiferromagnet in square lattice. We present numerical calculation of energy, spin-spin correlation function and spin excitation spectrum. We show, that the quantum flactuations reduce of magnetization respect to Neel order. Our results are in good agreement with other methods such as spin-wave calculation and series expansions.
Excited States of the Diatomic Molecule CrHe
Pototschnig, Johann V.; Ratschek, Martin; Hauser, Andreas W.; Ernst, Wolfgang E.
2013-06-01
Chromium (Cr) atoms embedded in superfluid helium nanodroplets (He_N) have been investigated by laser induced fluorescence, beam depletion and resonant two-photon ionization spectroscopy in current experiments at our institute. Cr is found to reside inside the He_N in the a^7S ground state. Two electronically excited states, z^7P and y^7P, are involved in a photoinduced ejection process which allowed us to study Fano resonances in the photoionisation spectra The need for a better understanding of the experimental observations triggered a theoretical approach towards the computation of electronically excited states via high-level methods of computational chemistry. Two well-established, wave function-based methods, CASSCF and MRCI, are combined to calculate the potential energy curves for the three states involved. The character of the two excited states z^7P and y^7P turns out to be significantly different. Theory predicts the ejection of the Cr atom in the case of an y^7P excitation as was observed experimentally. The quasi-inert helium environment is expected to weaken spin selection rules, allowing a coupling between different spin states especially during the ejection process. We therefore extend our theoretical analysis to the lowest state in the triplet- and quintet- manifold. Most of these alternative states show very weak bonding of only a few wn. A. Kautsch, M. Hasewend, M. Koch and W. E. Ernst, Phys. Rev. A 86, 033428 (2012). A. Kautsch, M. Koch and W. E. Ernst, J. Phys. Chem. A, accepted, doi:10.1021/jp312336m}.
Solid-State Excitation Laser for Laser-Ultrasonics
Schnars, U.; Platz, W.; Mahnke, P.; A. Fix; Frede, M; Neumann, J.; Peuser, P.
2010-01-01
The inspection speed of laser-ultrasonics compared with conventional ultrasonic testing is limited by the pulse repetition rate of the excitation laser. The maximum pulse repetition rate reported up to now for CO2-lasers, which are presently used for nearly all systems, is in the range of 400 Hz. In this paper a new approach based on a diode-pumped solid-state laser is discussed, which is currently being developed. This new excitation laser is designed for a repetition rate of 1 kHz and will ...
Photodissociation of N2O: excitation of 1A" states.
Schinke, Reinhard; Schmidt, Johan A
2012-11-26
We investigate the contributions of the lowest two (1)A" states in the UV photodissociation of N(2)O employing three-dimensional potential energy surfaces and transition dipole moment functions. Because the transition dipole moments are much smaller than for the 2 (1)A' state, we conclude that excitation of the (1)A" states has a marginal effect. The dense vibrational spectrum of the quasi-bound 2(1)A" state possibly explains some of the tiny, noise-like structures of the measured absorption spectrum. PMID:22536943
MULTIPLY CHARGED IONS COLLISIONS WITH ATOMS INTO EXCITED STATES
Institute of Scientific and Technical Information of China (English)
PanGuangyan
1990-01-01
The emission spectra in collisions between Ions and Atoms have been measured by an Optical Multichannel Analysis System (OMA).The experimental results demonstrate that there are two channels of excitation in collision between single charged ions and atoms and three channels of excitation in collision between double charged ions and atoms.Emission cross cestions and excitation cross sections have been obtained.K.Kadota et al and R.Shingal et al suggested that,under the appropriate conditions,the H42+-Li and He2++Na collision systems can be used efficiently to produce a laser of Lyman-α(30,4nm) and Lyman-β(25.6nm)lines via cascade to He+(2P)state.
Clustered chimera states in systems of type-I excitability
International Nuclear Information System (INIS)
The chimera state is a fascinating phenomenon of coexisting synchronized and desynchronized behaviour that was discovered in networks of nonlocally coupled identical phase oscillators over ten years ago. Since then, chimeras have been found in numerous theoretical and experimental studies and more recently in models of neuronal dynamics as well. In this work, we consider a generic model for a saddle-node bifurcation on a limit cycle representative of neural excitability type I. We obtain chimera states with multiple coherent regions (clustered chimeras/multi-chimeras) depending on the distance from the excitability threshold, the range of nonlocal coupling and the coupling strength. A detailed stability diagram for these chimera states and other interesting coexisting patterns (like traveling waves) is presented. (paper)
Super-atom molecular orbital excited states of fullerenes.
Johansson, J Olof; Bohl, Elvira; Campbell, Eleanor E B
2016-09-13
Super-atom molecular orbitals are orbitals that form diffuse hydrogenic excited electronic states of fullerenes with their electron density centred at the centre of the hollow carbon cage and a significant electron density inside the cage. This is a consequence of the high symmetry and hollow structure of the molecules and distinguishes them from typical low-lying molecular Rydberg states. This review summarizes the current experimental and theoretical studies related to these exotic excited electronic states with emphasis on femtosecond photoelectron spectroscopy experiments on gas-phase fullerenes.This article is part of the themed issue 'Fullerenes: past, present and future, celebrating the 30th anniversary of Buckminster Fullerene'. PMID:27501970
Controlling Excited-State Contamination in Nucleon Matrix Elements
Yoon, Boram; Bhattacharya, Tanmoy; Engelhardt, Michael; Green, Jeremy; Joó, Bálint; Lin, Huey-Wen; Negele, John; Orginos, Kostas; Pochinsky, Andrew; Richards, David; Syritsyn, Sergey; Winter, Frank
2016-01-01
We present a detailed analysis of methods to reduce statistical errors and excited-state contamination in the calculation of matrix elements of quark bilinear operators in nucleon states. All the calculations were done on a 2+1 flavor ensemble with lattices of size $32^3 \\times 64$ generated using the rational hybrid Monte Carlo algorithm at $a=0.081$~fm and with $M_\\pi=312$~MeV. The statistical precision of the data is improved using the all-mode-averaging method. We compare two methods for reducing excited-state contamination: a variational analysis and a two-state fit to data at multiple values of the source-sink separation $t_{\\rm sep}$. We show that both methods can be tuned to significantly reduce excited-state contamination and discuss their relative advantages and cost-effectiveness. A detailed analysis of the size of source smearing used in the calculation of quark propagators and the range of values of $t_{\\rm sep}$ needed to demonstrate convergence of the isovector charges of the nucleon to the $t_...
Controlling excited-state contamination in nucleon matrix elements
Energy Technology Data Exchange (ETDEWEB)
Yoon, Boram; Gupta, Rajan; Bhattacharya, Tanmoy; Engelhardt, Michael; Green, Jeremy; Joó, Bálint; Lin, Huey-Wen; Negele, John; Orginos, Kostas; Pochinsky, Andrew; Richards, David; Syritsyn, Sergey; Winter, Frank
2016-06-01
We present a detailed analysis of methods to reduce statistical errors and excited-state contamination in the calculation of matrix elements of quark bilinear operators in nucleon states. All the calculations were done on a 2+1 flavor ensemble with lattices of size $32^3 \\times 64$ generated using the rational hybrid Monte Carlo algorithm at $a=0.081$~fm and with $M_\\pi=312$~MeV. The statistical precision of the data is improved using the all-mode-averaging method. We compare two methods for reducing excited-state contamination: a variational analysis and a two-state fit to data at multiple values of the source-sink separation $t_{\\rm sep}$. We show that both methods can be tuned to significantly reduce excited-state contamination and discuss their relative advantages and cost-effectiveness. A detailed analysis of the size of source smearing used in the calculation of quark propagators and the range of values of $t_{\\rm sep}$ needed to demonstrate convergence of the isovector charges of the nucleon to the $t_{\\rm sep} \\to \\infty $ estimates is presented.
Controlling excited-state contamination in nucleon matrix elements
Yoon, Boram; Gupta, Rajan; Bhattacharya, Tanmoy; Engelhardt, Michael; Green, Jeremy; Joó, Bálint; Lin, Huey-Wen; Negele, John; Orginos, Kostas; Pochinsky, Andrew; Richards, David; Syritsyn, Sergey; Winter, Frank; Nucleon Matrix Elements NME Collaboration
2016-06-01
We present a detailed analysis of methods to reduce statistical errors and excited-state contamination in the calculation of matrix elements of quark bilinear operators in nucleon states. All the calculations were done on a 2 +1 -flavor ensemble with lattices of size 323×64 generated using the rational hybrid Monte Carlo algorithm at a =0.081 fm and with Mπ=312 MeV . The statistical precision of the data is improved using the all-mode-averaging method. We compare two methods for reducing excited-state contamination: a variational analysis and a 2-state fit to data at multiple values of the source-sink separation tsep. We show that both methods can be tuned to significantly reduce excited-state contamination and discuss their relative advantages and cost effectiveness. A detailed analysis of the size of source smearing used in the calculation of quark propagators and the range of values of tsep needed to demonstrate convergence of the isovector charges of the nucleon to the tsep→∞ estimates is presented.
Reexamination of the excited states of C12
Freer, M.; Boztosun, I.; Bremner, C. A.; Chappell, S. P. G.; Cowin, R. L.; Dillon, G. K.; Fulton, B. R.; Greenhalgh, B. J.; Munoz-Britton, T.; Nicoli, M. P.; Rae, W. D. M.; Singer, S. M.; Sparks, N.; Watson, D. L.; Weisser, D. C.
2007-09-01
An analysis of the C12(C12,3α)C12 reaction was made at beam energies between 82 and 106 MeV. Decays to both the ground state and the excited states of Be8 were isolated, allowing states of different characters to be identified. In particular, evidence was found for a previously observed state at 11.16 MeV. An analysis of the angular distributions of the unnatural parity states at 11.83 and 13.35 MeV, previously assigned Jπ=2-, calls into question the validity of these assignments, suggesting that at least one of the states may correspond to Jπ=4-. Evidence is also found for 1- and 3- strengths associated with broad states between 11 and 14 MeV.
Grozema, FC; van Duijnen, PT; Siebbeles, LDA; Goossens, A
2004-01-01
This paper describes a quantum chemical study of the electronic structure of thienylene vinylene oligomers ranging in size from two thienylene rings (2TV) to 12TV. The geometries of the TV oligomers in the ground state, the lowest triplet state, and the singly and doubly oxidized states were optimiz
Excited-state quantum phase transitions in Dicke superradiance models.
Brandes, Tobias
2013-09-01
We derive analytical results for various quantities related to the excited-state quantum phase transitions in a class of Dicke superradiance models in the semiclassical limit. Based on a calculation of a partition sum restricted to Dicke states, we discuss the singular behavior of the derivative of the density of states and find observables such as the mean (atomic) inversion and the boson (photon) number and its fluctuations at arbitrary energies. Criticality depends on energy and a parameter that quantifies the relative weight of rotating versus counterrotating terms, and we find a close analogy to the logarithmic and jump-type nonanalyticities known from the Lipkin-Meshkov-Glick model. PMID:24125239
Strong-Field Photoionization as Excited-State Tunneling.
Serebryannikov, E E; Zheltikov, A M
2016-03-25
We show that, in an intense laser field, ultrafast photoionization can occur through quantum pathways that cannot be categorized as multiphoton ionization or ground-state tunneling. In this regime, the subcycle electron-wave-packet dynamics leading to photoionization occurs via electron excited states, from where the electrons tunnel to the continuum within a tiny fraction of the field cycle. For high field intensities, this ionization pathway is shown to drastically enhance the dynamic leakage of the electron wave packet into the continuum, opening an ionization channel that dominates over ground-state electron tunneling. PMID:27058079
Negative-parity nucleon excited state in nuclear matter
Ohtani, Keisuke; Oka, Makoto
2016-01-01
Spectral functions of the nucleon and its negative parity excited state in nuclear matter are studied using QCD sum rules and the maximum entropy method (MEM). It is found that in-medium modifications of the spectral functions are attributed mainly to density dependencies of the $\\langle \\bar{q}q \\rangle $ and $\\langle q^{\\dagger}q \\rangle $ condensates. The MEM reproduces the lowest-energy peaks of both the positive and negative parity nucleon states at finite density up to $\\rho \\sim \\rho_N$ (normal nuclear matter density). As the density grows, the residue of the nucleon ground state decreases gradually while the residue of the lowest negative parity excited state increases slightly. On the other hand, the positions of the peaks, which correspond to the total energies of these states, are almost density independent for both parity states. The density dependencies of the effective masses and vector self-energies are also extracted by assuming the mean-field green functions for the peak states. We find that,...
Excited states in large molecular systems through polarizable embedding.
List, Nanna Holmgaard; Olsen, Jógvan Magnus Haugaard; Kongsted, Jacob
2016-07-27
In this perspective, we provide an overview of recent work within the polarizable embedding scheme to describe properties of molecules in realistic environments of increasing complexity. After an outline of the theoretical basis for the polarizable embedding model, we discuss the importance of using an accurate embedding potential, and how this may be used to significantly reduce the size of the part of the system treated using quantum mechanics without compromising the accuracy of the final results. Furthermore, we discuss the calculation of local electronic excited states based on response theory. We finally discuss aspects related to two recent extensions of the model (i) effective external field and (ii) polarizable density embedding emphasizing their importance for efficient yet accurate description of excited-state properties in complex environments. PMID:27416749
Precision study of excited state effects in nucleon matrix elements
Energy Technology Data Exchange (ETDEWEB)
Dinter, Simon; Drach, Vincent; Jansen, Karl; Renner, Dru B. [Deutsches Elektronen-Synchrotron (DESY), Zeuthen (Germany). John von Neumann-Inst. fuer Computing NIC; Alexandrou, Constantia [Cyprus Univ., Nicosia (Cyprus). Dept. of Physics; The Cyprus Insitute, Nicosia (Cyprus). Computation-Based Science and Technology Research Center; Constantinou, Martha [Cyprus Univ., Nicosia (Cyprus). Dept. of Physics
2011-08-15
We present a dedicated analysis of the influence of excited states on the calculation of nucleon matrix elements. This calculation is performed at a fixed value of the lattice spacing, volume and pion mass that are typical of contemporary lattice computations. We focus on the nucleon axial charge, g{sub A}, for which we use about 7,500 measurements, and on the average momentum of the unpolarized isovector parton distribution, left angle x right angle {sub u-d}, for which we use about 23,000 measurements. All computations are done employing N{sub f}=2+1+1 maximally-twisted-mass Wilson fermions and using nonperturbatively calculated renormalization factors. Excited state e ects are shown to be negligible for g{sub A}, whereas they lead to an O(10%) downward shift for left angle x right angle {sub u-d}. (orig.)
The effects of doubly excited states on ionization balance
Institute of Scientific and Technical Information of China (English)
无
2006-01-01
The effects of highly doubly excited states on ionization balance are investigated. In the calculation, A Collisional-Radiative model in Detailed-Configuration-Accounting (DCA) is applied to population calculations for NLTE plasmas. Configuration-averaged rate coefficients that needed in the rate equations are obtained based on the first order perturbation theory. The Hatree-Fock-Slater self-consistent-field method is used to calculate the electron wave functions. The mean ionization stage of high-Z plasma Lu is presented. The comparison shows that the mean ionization stage increases more than 3 stages when doubly excited states 5l6l' and 5l5l' are not included in the population calculations.
On the nature of highly vibrationally excited states of thiophosgene
Indian Academy of Sciences (India)
Srihari Keshavamurthy
2012-01-01
In this work an analysis of the highly vibrationally excited states of thiophosgene (SCCl2) is made in order to gain insights into some of the experimental observations and spectral features. The states analysed here lie in a spectrally complex region where strong mode mixings are expected due to the overlap of several strong anharmonic Fermi resonances. Two recent techniques, a semiclassical angle space representation of the eigenstates and the parametric variation of the eigenvalues (level-velocities) are used to identify eigenstate sequences exhibiting common localization characteristics. Preliminary results on the influence of highly excited out-of-plane bending modes on the nature of the eigenstates suggest a possible bifurcation in the system.
On the nature of highly vibrationally excited states of Thiophosgene
Keshavamurthy, Srihari
2011-01-01
In this work an analysis of the highly vibrationally excited states of thiophosgene (SCCl$_{2}$) is made in order to gain insights into some of the experimental observations and spectral features. The states analyzed herein lie in a spectrally complex region where strong mode mixings are expected due to the overlap of several strong anharmonic Fermi resonances. Two recent techniques, a semiclassical angle space representation of the eigenstates and the parametric variation of the eigenvalues (level-velocities) are used to identify eigenstate sequences exhibiting common localization characteristics. Preliminary results on the influence of highly excited out-of-plane bending modes on the nature of the eigenstates suggest a possible bifurcation in the system.
Wenzel, Jan; Dreuw, Andreas
2016-03-01
The theoretical simulation of X-ray absorption spectra is in general a challenging task. However, for small and medium-sized organic molecules, the algebraic diagrammatic construction scheme (ADC) for the polarization operator in combination with the core-valence separation approximation (CVS) has proven to yield core-excitation energies and transition moments with almost quantitative accuracy allowing for reliable construction of X-ray absorption spectra. Still, to understand core-excitation processes in detail, it is not sufficient to only compute energies, but also properties like static dipole moments and state densities are important as they provide deeper insight into the nature of core-excited states. Here, we present for the first time an implementation of the intermediate state representation (ISR) approach in combination with the CVS approximation (CVS-ISR), which gives, in combination with the CVS-ADC method, direct access to core-excited state properties. The performance of the CVS-ADC/CVS-ISR approach is demonstrated by means of small- and medium-sized organic molecules. Besides the calculation of core-excited state dipole moments, advanced analyses of core-excited state densities are performed using descriptors like exciton sizes and distances. Plotting electron and hole densities helps to determine the character of the state, and in particular, the investigation of detachment/attachment densities provides information about orbital relaxation effects that are crucial for understanding core excitations. PMID:26845396
Clustered Chimera States in Systems of Type-I Excitability
Vüllings, Andrea; Hizanidis, Johanne; Omelchenko, Iryna; Hövel, Philipp
2014-01-01
Chimera is a fascinating phenomenon of coexisting synchronized and desynchronized behaviour that was discovered in networks of nonlocally coupled identical phase oscillators over ten years ago. Since then, chimeras were found in numerous theoretical and experimental studies and more recently in models of neuronal dynamics as well. In this work, we consider a generic model for a saddle-node bifurcation on a limit cycle representative for neural excitability type I. We obtain chimera states wit...
First observation of excited states in 173Hg93
O'Donnell, D; Scholey, C; Bianco, L; Capponi, L; Carroll, R J; Darby, I G; Donosa, L; Drummond, M; Ertugral, F; Greenlees, P T; Grahn, T; Hauschild, K; Herzan, A; Jakobsson, U; Jones, P; Joss, D T; Julin, R; Juutinen, S; Ketelhut, S; Labiche, M; Leino, M; Lopez-Martens, A; Mullholland, K; Nieminen, P; Peura, P; Rahkila, P; Rinta-Antila, S; Ruotsalainen, P; Sandzelius, M; Saren, J; Saygi, B; Simpson, J; Sorri, J; Thornthwaite, A; Uusitalo, J
2012-01-01
The neutron-deficient nucleus 173Hg has been studied following fusion-evaporation reactions. The observation of gamma rays decaying from excited states are reported for the first time and a tentative level scheme is proposed. The proposed level scheme is discussed within the context of the systematics of neighbouring neutron-deficient Hg nuclei. In addition to the gamma-ray spectroscopy, the alpha decay of this nucleus has been measured yielding superior precision to earlier measurements.
Nonlinear Optical Spectroscopy of Excited States in Polyfluorene
Tong, M; Vardeny, Z V
2006-01-01
We used a variety of nonlinear optical (NLO) spectroscopies to study the singlet excited states order, and primary photoexcitations in polyfluorene; an important blue emitting p-conjugated polymer. The polarized NLO spectroscopies include ultrafast pump-probe photomodulation, two-photon absorption, and electroabsorption. For completeness we also measured the linear absorption and photoluminescence spectra. We found that the primary photoexcitations in polyfluorene are singlet excitons.
Doubly excited triplet states of highly stripped ions
International Nuclear Information System (INIS)
Transition energies, Coulomb repulsions and effective quantum numbers have been calculated for the doubly excited Nsnp: 3P0 (for N=2, n=N,..,5); Nsnd: 3De (for N=2, n=N+1,..,5) and Npnd: 3F0 (for N=2, n=N+1,..,5) states for the highly stripped ions Na9+,Mg10+,Al11+,Si12+,P13+ and S14+. Time-dependent perturbation theory has been applied to calculate such transitions properties. A time-dependent harmonic perturbation causes simultaneous excitation of both the electrons with a change of spin state. The doubly excited energy levels and the analytic representation of their wave functions are obtained by identifying the poles of an appropriately constructed linearized variational functional with respect to driving frequency. Most of the results are new. The transition energies and effective quantum numbers of 2s2p: 3P0 states of all the ions agree well with the only available experimental data. (orig.)
Spin radical enhanced magnetocapacitance effect in intermolecular excited states.
Zang, Huidong; Wang, Jianguo; Li, Mingxing; He, Lei; Liu, Zitong; Zhang, Deqing; Hu, Bin
2013-11-14
This article reports the magnetocapacitance effect (MFC) based on both pristine polymer MEH-PPV and its composite system doped with spin radicals (6R-BDTSCSB). We observed that a photoexcitation leads to a significant positive MFC in the pristine MEH-PPV. Moreover, we found that a low doping of spin radicals in polymer MEH-PPV causes a significant change on the MFC signal: an amplitude increase and a line-shape narrowing under light illumination at room temperature. However, no MFC signal was observed under dark conditions in either the pristine MEH-PPV or the radical-doped MEH-PPV. Furthermore, the magnitude increase and line-shape narrowing caused by the doped spin radicals are very similar to the phenomena induced by increasing the photoexcitation intensity. Our studies suggest that the MFC is essentially originated from the intermolecular excited states, namely, intermolecular electron-hole pairs, generated by a photoexcitation in the MEH-PPV. More importantly, by comparing the effects of spin radicals and electrically polar molecules on the MFC magnitude and line shape, we concluded that the doped spin radicals can have the spin interaction with intermolecular excited states and consequently affect the internal spin-exchange interaction within intermolecular excited states in the development of MFC. Clearly, our experimental results indicate that dispersing spin radicals forms a convenient method to enhance the magnetocapacitance effect in organic semiconducting materials. PMID:24144347
Féraud, Géraldine; Broquier, Michel; Dedonder, Claude; Jouvet, Christophe; Grégoire, Gilles; Soorkia, Satchin
2015-06-11
The electronic spectroscopy and the electronic excited state properties of cold protonated phenylalanine and protonated tyrosine have been revisited on a large spectral domain and interpreted by comparison with ab initio calculations. The protonated species are stored in a cryogenically cooled Paul trap, maintained at ∼10 K, and the parent and all the photofragment ions are mass-analyzed in a time-of-flight mass spectrometer, which allows detecting the ionic species with an improved mass resolution compared to what is routinely achieved with a quadrupole mass spectrometer. These new results emphasize the competition around the band origin between two proton transfer reactions from the ammonium group toward either the aromatic chromophore or the carboxylic acid group. These reactions are initiated by the coupling of the locally excited ππ* state with higher charge transfer states, the positions and coupling of which depend on the conformation of the protonated molecules. Each of these reaction processes gives rise to specific fragmentation channels that supports the conformer selectivity observed in the photofragmentation spectra of protonated tyrosine and phenylalanine.
Modular Hamiltonian for Excited States in Conformal Field Theory.
Lashkari, Nima
2016-07-22
We present a novel replica trick that computes the relative entropy of two arbitrary states in conformal field theory. Our replica trick is based on the analytic continuation of partition functions that break the Z_{n} replica symmetry. It provides a method for computing arbitrary matrix elements of the modular Hamiltonian corresponding to excited states in terms of correlation functions. We show that the quantum Fisher information in vacuum can be expressed in terms of two-point functions on the replica geometry. We perform sample calculations in two-dimensional conformal field theories. PMID:27494465
Modular Hamiltonian for Excited States in Conformal Field Theory
Lashkari, Nima
2016-07-01
We present a novel replica trick that computes the relative entropy of two arbitrary states in conformal field theory. Our replica trick is based on the analytic continuation of partition functions that break the Zn replica symmetry. It provides a method for computing arbitrary matrix elements of the modular Hamiltonian corresponding to excited states in terms of correlation functions. We show that the quantum Fisher information in vacuum can be expressed in terms of two-point functions on the replica geometry. We perform sample calculations in two-dimensional conformal field theories.
Modular Hamiltonian for Excited States in Conformal Field Theory.
Lashkari, Nima
2016-07-22
We present a novel replica trick that computes the relative entropy of two arbitrary states in conformal field theory. Our replica trick is based on the analytic continuation of partition functions that break the Z_{n} replica symmetry. It provides a method for computing arbitrary matrix elements of the modular Hamiltonian corresponding to excited states in terms of correlation functions. We show that the quantum Fisher information in vacuum can be expressed in terms of two-point functions on the replica geometry. We perform sample calculations in two-dimensional conformal field theories.
Excited states in 146Sm and 147Sm
Kownacki, J.; Sujkowski, Z.; Hammarén, E.; Liukkonen, E.; Piiparinen, M.; Lindblad, Th.; Ryde, H.; Paar, V.
1980-03-01
The 144, 146Nd(α, χn) and 146,148Nd( 3He, χn) reactions with Eα = 20-43 MeV and E3He , = 19-27 MeV are used to investigate excited states in the isotopes 146Sm and 147Sm. The experiments involve measurements of singles γ-ray spectra and conversion electron spectra, γ-ray angular distributions and three-parameter ( Eγ- Eγ-time) coincidences. From these experiments information is obtained for states with spin up to I = 13 +and I = {27}/{2}-, respectively. These states are interpreted within the framework of the cluster-vibration model (CVM) as well as the shell model. In the latter approach, the energies of several well established states, in both isotopes, are calculated using empirical singleparticle energies, empirical two-particle interaction matrix elements and angular momentum algebra. The average deviation between the calculated and the experimental energies is less than 100 keV. The CVM calculations involve the coupling of a three-particle neutron cluster to the quadrupole vibration of the core. For 147Sm, these calculations reproduce the observed sequence of states based on the I π = {7}/{2}- ground state, as well as the sequence of states based on the I π = {13}/{2}+ excited state. The CVM calculations also reproduce the ground band in 146Sm, while for the negative parity states based on the cluster (f {7}/{2}i {13}/{2}) 3 --10 - an additional shift in energy is expected due to the mixing with octupole phonons.
Self-Scattering for Dark Matter with an Excited State
Schutz, Katelin
2014-01-01
Self-interacting dark matter scenarios have recently attracted much attention, as a possible means to alleviate the tension between N-body simulations and observations of the dark matter distribution on galactic and sub-galactic scales. The presence of internal structure for the dark matter --- for example, a nearly-degenerate state in the spectrum that could decay, or be collisionally excited or de-excited --- has also been proposed as a possible means to address these discrepancies. Such internal structure can be a source of interesting signatures in direct and indirect dark matter searches, for example providing a novel explanation for the 3.5 keV line recently observed in galaxies and galaxy clusters. We analyze a simple model of dark matter self-scattering including a nearly-degenerate excited state, and develop an accurate analytic approximation for the elastic and inelastic $s$-wave cross sections, which is valid outside the perturbative regime provided the particle velocity is sufficiently low (this c...
The investigation of interactions in the excited state of flavins using time-resolved spectroscopy
Visser, A.J.W.G.
1975-01-01
In paper I the results obtained with a very short (3 nsec) intense laser pulse as excitation source are described. This pulse excites such a large amount of flavin molecules into higher excited singlet and triplet states that changes in absorption of these higher excited states can be analyzed with
Excited-State Properties of Molecular Solids from First Principles
Kronik, Leeor; Neaton, Jeffrey B.
2016-05-01
Molecular solids have attracted attention recently in the context of organic (opto)electronics. These materials exhibit unique charge carrier generation and transport phenomena that are distinct from those of conventional semiconductors. Understanding these phenomena is fundamental to optoelectronics and requires a detailed description of the excited-state properties of molecular solids. Recent advances in many-body perturbation theory (MBPT) and density functional theory (DFT) have made such description possible and have revealed many surprising electronic and optical properties of molecular crystals. Here, we review this progress. We summarize the salient aspects of MBPT and DFT as well as various properties that can be described by these methods. These properties include the fundamental gap and its renormalization, hybridization and band dispersion, singlet and triplet excitations, optical spectra, and excitonic properties. For each, we present concrete examples, a comparison to experiments, and a critical discussion.
Three-step laser excitation of the odd-parity 5s5d 3D → 5s nf 3F states of cadmium
Nadeem, Ali; Shah, M.; Haq, S. U.; Shahzada, S.; Mumtaz, M.; Waheed, A.; Nawaz, M.; Ahmed, M.; Baig, M. A.
2014-07-01
We report new experimental data on the term energies and effective quantum numbers of the highly excited odd parity states of cadmium in the 71 773-72 500 cm-1 energy range. The experiment was performed using three dye lasers simultaneously pumped by the second harmonic (532 nm) of the Nd;YAG laser. The vapor containment and detection system was a thermionic diode ion detector working in a space charge limited mode. The new observations include the 5snf3F3 (12 ⩽ n ⩽ 52), 5snf3F4 (13 ⩽ n ⩽ 33) and 5snf3F2 (12 ⩽ n ⩽ 22) Rydberg series excited from the 5s5d3D multiplet. A two parameter fit to the transitions energies of the 5snf3F3 series yields the binding energy of the 5snd 2D2 level as 13 042.178 ± 0.02 cm-1 and consequently the first ionization of cadmium is determined as 72 540.05 ± 0.13 cm-1, which is in good agreement with the previously reported value.
Self-scattering for Dark Matter with an excited state
International Nuclear Information System (INIS)
Self-interacting dark matter scenarios have recently attracted much attention, as a possible means to alleviate the tension between N-body simulations and observations of the dark matter distribution on galactic and sub-galactic scales. The presence of internal structure for the dark matter—for example, a nearly-degenerate state in the spectrum that could decay, or be collisionally excited or de-excited—has also been proposed as a possible means to address these discrepancies. Such internal structure can be a source of interesting signatures in direct and indirect dark matter searches, for example providing a novel explanation for the 3.5 keV line recently observed in galaxies and galaxy clusters. We analyze a simple model of dark matter self-scattering including a nearly-degenerate excited state, and develop an accurate analytic approximation for the elastic and inelastic s-wave cross sections, which is valid outside the perturbative regime provided the particle velocity is sufficiently low (this condition is also required for the s-wave to dominate over higher partial waves). We anticipate our results will be useful in incorporating inelastic self-scattering into N-body simulations, in order to study the quantitative impact of nearly-degenerate states in the dark matter spectrum on galactic structure and dynamics, and in computing the indirect signatures of multi-state dark matter
Theoretical aspects of multiphoton ionization with many resonant excited states
International Nuclear Information System (INIS)
The variety of the parameters involved in multi-color multi-step ionization makes it a formidable job to obtain a theoretically comprehensible overview of the process. We examine these parameters of such processes as well as commonly used assumptions in theoretical investigations of multiphoton ionization with many resonantly excited levels. The density matrix formalism is adequate to treat resonant multiphoton ionization when the number of the resonant levels involved is not too large, solving the resonantly coupled states separately beyond the lowest order perturbation theory, while the rest of the states are treated perturbatively. An example of such formalism is given for a four-level system ionized with three lasers each of which resonantly couples the adjacent pairs of the atomic states.
Excited states in 146Sm and 147Sm
International Nuclear Information System (INIS)
The sup(144,146)Nd(α,xn) and sup(146,148)Nd(3He,xn) reactions with Esub(α) = 20 - 43 MeV and E3sub(He) = 19 - 27 MeV are used to investigate excited states in the isotopes 146Sm and 147Sm. The experiments involve measurements of singles γ-ray spectra and conversion electron spectra, γ-ray angular distributions and three parameter (E sub(γ)E sub(γ) time) coincidences. From these experiments information is obtained for states with spin up to I = 13+ and I = 27/2-, respectively, These states are interpeted within the framework of the cluster-vibration model (CVM) as well as the shell model. (author)
Unusual behavior in the first excited state lifetime of catechol
Weiler, Martin; Féraud, Géraldine; Ishiuchi, Shun-Ichi; Dedonder, Claude; Jouvet, Christophe; Fujii, Masaaki
2014-01-01
We are presenting vibrationally selective pump-probe measurements of the first electronic excited-state (pp*) lifetime of jet-cooled neutral catechol (1,2-dihydroxybenzene). The lifetime of the 0-0 transition is very short (7 ps) as rationalized by the small pp*/psigma* gap calculated. However the lifetimes implying higher out-of-plane vibrational levels are longer (~11 ps). This emphasizes the role of the out-of-plane vibration in the pp*/psigma* coupling not only in its nature but also in the number of quanta
Normalized Excited Squeezed Vacuum State and Its Applications
Institute of Scientific and Technical Information of China (English)
MENG Xiang-Guo; WANG Ji-Suo; LIANG Bao-Long
2007-01-01
By using the intermediate coordinate-momentum representation in quantum optics and generating function for the normalization of the excited squeezed vacuum state (ESVS), the normalized ESVS is obtained. We find that its normalization constants obtained via two new methods are uniform and a new form which is different from the result obtained by Zhang and Fan [Phys. Lett. A 165 (1992) 14]. By virtue of the normalization constant of the ESVS and the intermediate coordinate-momentum representation, the tomogram of the normalized ESVS and some useful formulae are derived.
DEFF Research Database (Denmark)
Bohr, Henrik; Malik, F. Bary
2013-01-01
The observed multiple de-excitation pathways of photo-absorbed electronic excited state in the peridinin–chlorophyll complex, involving both energy and charge transfers among its constituents, are analyzed using the bio-Auger (B-A) theory. It is also shown that the usually used F¨orster–Dexter th...
Excited-state relaxation in π-conjugated polymers
Frolov, S. V.; Bao, Z.; Wohlgenannt, M.; Vardeny, Z. V.
2002-05-01
We study ultrafast relaxation processes of odd- (Bu) and even-parity (Ag) exciton states in poly(p-phenylene vinylene) derivatives. The Bu states are studied using a regular two-beam pump-and-probe spectroscopy, which can monitor vibronic relaxation and exciton diffusion. In order to observe the Ag states, a three-beam femtosecond transient spectroscopy is developed, in which two different excitation pulses successively generate odd-parity (1Bu) excitons at 2.2 eV and then reexcite them to higher Ag states. We are able to distinguish two different classes of Ag states: one class (mAg) experiences ultrafast internal conversion back to the lowest singlet exciton, whereas the other class (kAg) in violation of the Vavilov-Kasha's rule undergoes a different relaxation pathway. The excitons subsequently dissociate into long-lived polaron pairs, which results in emission quenching with the action spectrum similar to that of the intrinsic photoconductivity. We conclude that the Ag states above 3.3 eV (kAg) are charge-transfer states, that mediate carrier photogeneration.
Optical Generation of Single- or Two-Mode Excited Entangled Coherent States
Institute of Scientific and Technical Information of China (English)
REN Zhen-Zhong; JING Hui; ZHANG Xian-Zhou
2008-01-01
With nonlinear Mach-Zehnder interferometer (NLMZI) and a type-Ⅰ beta-barium borate (BBO) crystal, we optically generate single-mode excited entangled coherent states. This scheme can be easily generalized to generate two-mode excited entangled coherent states. We simply analyse different influences of single- and two-mode photon excitations on entangled coherent states.
Institute of Scientific and Technical Information of China (English)
Jianzhong Li; Dongyi Han; Huijun Yuan; Jing Cheng; Yanping Lu; Yu Lu; Aiting Chen; Yi Sun; Dongyang Kang; Xin Zhang; Pu Dai
2010-01-01
We present the clinical and genetic findings for a Chinese family with X-linked non-syndromic hearing loss in which the affected males showed congenital profound sensorineural hearing impairment. In two affected brothers, the computer tomography of temporal bone showed bilateral dilation of the internal auditory canal with fistulous communication between the lateral canal and the basal cochlear turn, which is consistent with the typical DFNX2 phenotype. A missense mutation (c.647G→A) in the POU3F4 gene caused a substitution from glycine to glutamic acid at position 216 (p.G216E), and this mutation was found to consistently cosegregate with the deafness phenotype in the family. The mutation resulted in the loss of function of the POU3F4 by decreasing the affinity between the protein and DNA, as shown in silico by the structural analysis. Prenatal diagnosis of pregnant proband of this family revealed the C.647G→A mutation in DNA extracted from the amniotic fluid surrounding the fetus. The appropriate use of genetic testing and prenatal diagnosis plays a key role in reducing the recurrence of genetic defects in high-risk families.
Probing the Locality of Excited States with Linear Algebra.
Etienne, Thibaud
2015-04-14
This article reports a novel theoretical approach related to the analysis of molecular excited states. The strategy introduced here involves gathering two pieces of physical information, coming from Hilbert and direct space operations, into a general, unique quantum mechanical descriptor of electronic transitions' locality. Moreover, the projection of Hilbert and direct space-derived indices in an Argand plane delivers a straightforward way to visually probe the ability of a dye to undergo a long- or short-range charge-transfer. This information can be applied, for instance, to the analysis of the electronic response of families of dyes to light absorption by unveiling the trend of a given push-pull chromophore to increase the electronic cloud polarization magnitude of its main transition with respect to the size extension of its conjugated spacer. We finally demonstrate that all the quantities reported in this article can be reliably approximated by a linear algebraic derivation, based on the contraction of detachment/attachment density matrices from canonical to atomic space. This alternative derivation has the remarkable advantage of a very low computational cost with respect to the previously used numerical integrations, making fast and accurate characterization of large molecular systems' excited states easily affordable.
Probing the Locality of Excited States with Linear Algebra.
Etienne, Thibaud
2015-04-14
This article reports a novel theoretical approach related to the analysis of molecular excited states. The strategy introduced here involves gathering two pieces of physical information, coming from Hilbert and direct space operations, into a general, unique quantum mechanical descriptor of electronic transitions' locality. Moreover, the projection of Hilbert and direct space-derived indices in an Argand plane delivers a straightforward way to visually probe the ability of a dye to undergo a long- or short-range charge-transfer. This information can be applied, for instance, to the analysis of the electronic response of families of dyes to light absorption by unveiling the trend of a given push-pull chromophore to increase the electronic cloud polarization magnitude of its main transition with respect to the size extension of its conjugated spacer. We finally demonstrate that all the quantities reported in this article can be reliably approximated by a linear algebraic derivation, based on the contraction of detachment/attachment density matrices from canonical to atomic space. This alternative derivation has the remarkable advantage of a very low computational cost with respect to the previously used numerical integrations, making fast and accurate characterization of large molecular systems' excited states easily affordable. PMID:26574379
Excitation gap of fractal quantum hall states in graphene
Luo, Wenchen; Chakraborty, Tapash
2016-01-01
In the presence of a magnetic field and an external periodic potential the Landau level spectrum of a two-dimensional electron gas exhibits a fractal pattern in the energy spectrum which is described as the Hofstadter’s butterfly. In this work, we develop a Hartree-Fock theory to deal with the electron-electron interaction in the Hofstadter’s butterfly state in a finite-size graphene with periodic boundary conditions, where we include both spin and valley degrees of freedom. We then treat the butterfly state as an electron crystal so that we could obtain the order parameters of the crystal in the momentum space and also in an infinite sample. A phase transition between the liquid phase and the fractal crystal phase can be observed. The excitation gaps obtained in the infinite sample is comparable to those in the finite-size study, and agree with a recent experimental observation.
Kondo, Jorge M; Guttridge, Alex; Wade, Christopher G; De Melo, Natalia R; Adams, Charles S; Weatherill, Kevin J
2015-01-01
We report on the observation of Electromagnetically Induced Transparency (EIT) and Absorption (EIA) of highly-excited Rydberg states in thermal Cs vapor using a 4-step excitation scheme. The advantage of this 4-step scheme is that the final transition to the Rydberg state has a large dipole moment and one can achieve similar Rabi frequencies to 2 or 3 step excitation schemes using two orders of magnitude less laser power. Consequently each step is driven by a relatively low power infra-red diode laser opening up the prospect for new applications. The observed lineshapes are in good agreement with simulations based on multilevel optical Bloch equations.
Kinetic studies following state-selective laser excitation
International Nuclear Information System (INIS)
We have made measurements of state-to-state deactivation cross sections and radiative lifetimes for Xe*(6p,6p',7p) and Kr*(5p) states in xenon and krypton buffer gases. These results are relevant to kinetic models and both excimer lasers and the infrared xenon laser; and they are a significant improvement in the precision of the known radiative lifetimes. This type of experiment can now be compared with recent calculations of state-to-state collisional relaxation in rare-gases by Hickman, Huestis, and Saxon. We have also made significant progress in the study of the electronic spectra of small molecules of the rare gases. Spectra have been obtained for Xe2, Xe3, Xe4, and larger clusters. As guidance for the larger clusters of the rare gases we have obtained the first multiphoton spectra for excitons in condensed xenon. In collaboration with research on the multiphoton spectra of the rare gases, we have continued experiments using synchrotron radiation in collaboration with the University of Hamburg. In experiments there we have observed excitation and fluorescence spectra for single xenon atoms at the surface, within the second layer, and within the bulk of large argon clusters
Marks, M.; Sachs, S.; Schwalb, C. H.; Schöll, A.; Höfer, U.
2013-09-01
We present an investigation of the electronic structure and excited state dynamics of optically excited 3,4,9,10-perylene-tetracarboxylic acid dianhydride (PTCDA) thin films adsorbed on Ag(111) using two-photon photoemission spectroscopy (2PPE). 2PPE allows us to study both occupied and unoccupied electronic states, and we are able to identify signals from the highest occupied and the two lowest unoccupied electronic states of the PTCDA thin film in the 2PPE spectra. The energies for occupied states are identical to values from ultraviolet photoelectron spectroscopy. Compared to results from inverse photoelectron spectroscopy (IPES), the 2PPE signals from the two lowest unoccupied electronic states, LUMO and LUMO+1, are found at 0.8 eV and 1.0 eV lower energies, respectively. We attribute this deviation to the different final states probed in 2PPE and IPES and the attractive interaction of the photoexcited electron and the remaining hole. Furthermore, we present a time-resolved investigation of the excited state dynamics of the PTCDA film in the femtosecond time regime. We observe a significantly shorter inelastic excited state lifetime compared to findings from time-resolved photoluminescence spectroscopy of PTCDA single crystals which could originate from excitation quenching by the metal substrate.
Breathing-like excited state of the Hoyle state in ${^{12}{\\rm C}}$
Zhou, Bo; Horiuchi, Hisashi; Ren, Zhongzhou
2016-01-01
The existence of the $0_3^+$ and $0_4^+$ states around 10 MeV excitation energy in ${^{12}{\\rm C}}$ is confirmed by a fully microscopic 3$\\alpha$ cluster model. Firstly, a GCM (generator coordinate method) calculation is performed by superposing optimized 2$\\alpha$+$\\alpha$ THSR (Tohsaki-Horiuchi-Schuck-R\\"{o}pke) wave functions with the radius-constraint method. The obtained two excited $0^+$ states above the Hoyle state are consistent with the recently observed states by experiment. Secondly, a variational calculation using the single 2$\\alpha$+$\\alpha$ THSR wave function orthogonalized to the ground and Hoyle states is made and it also supports the existence of the $0_3^+$ state obtained by the GCM calculation. The analysis of the obtained $0_3^+$ state is made by studying its 2$\\alpha$-$\\alpha$ reduced width amplitude, its 2$\\alpha$ correlation function, and the large monopole matrix element between this state and the Hoyle state, which shows that this $0_3^+$ state is a breathing-like excited state of th...
Chimera states and excitation waves in networks with complex topologies
Schöll, Eckehard
2016-06-01
Chimera patterns, which consist of coexisting spatial domains of coherent (synchronized) and incoherent (desyn- chronized) dynamics are studied in networks of FitzHugh-Nagumo systems with complex topologies. To test the robustness of chimera patterns with respect to changes in the structure of the network, we study the following network topologies: Regular ring topology with R nearest neigbors coupled to each side, small-world topology with additional long-range random links, and a hierarchical geometry in the connectivity matrix. We find that chimera states are generally robust with respect to these perturbations, but qualitative changes of the chimera patterns in form of nested coherent and incoherent regions can be induced by a hierarchical topology. The suppression of propagating excitation waves by a small-world topology is also reviewed.
Alpha-particle decays from excited states in 24Mg
Institute of Scientific and Technical Information of China (English)
LIOTTA; R; J
2011-01-01
Using a cluster model based on the Woods-Saxon potential, alpha-particle decays from excited states in 24Mg have been system atically investigated. Calculations can in general reproduce experimental data, noticing the fact that the preformation factor P of alpha particle in alpha-decaying nuclei is of order from 100 to 10?2. This can be the evidence for the α+20Ne structure in 24Mg. Meanwhile, the results also show the existence of other configurations, such as 16O+2α. Since the calculated decay widths are very sensitive to the angular momentum carried by the outgoing cluster (α particle), our results could serve as a guide to experimental spin assignments.
Suppression of Excited-State Contributions to Stellar Reaction Rates
Rauscher, T
2013-01-01
It has been shown in previous work [Phys. Rev. Lett. 101, 191101 (2008); Phys. Rev. C 80, 035801 (2009)] that a suppression of the stellar enhancement factor (SEF) occurs in some endothermic reactions at and far from stability. This effect is re-evaluated using the ground-state contributions to the stellar reaction rates, which were shown to be better suited to judge the importance of excited state contributions than the previously applied SEFs. An update of the tables shown in Phys. Rev. C 80, 035801 (2009) is given. The new evalution finds 2350 cases (out of a full set of 57513 reactions) for which the ground-state contribution is larger in the reaction direction with negative reaction Q-value than in the exothermic direction, thus providing exceptions to the commonly applied Q-value rule. The results confirm the Coulomb suppression effect but lead to a larger number of exceptions than previously found. This is due to the fact that often a large variation in the g.s. contribution does not lead to a sizeable...
Excited-State Wigner Crystals in One Dimension
Rogers, Fergus J M
2016-01-01
Wigner crystals (WC) are electronic phases peculiar to low-density systems, particularly in the uniform electron gas. Since its introduction in the early twentieth century, this model has remained essential to many aspects of electronic structure theory and condensed-matter physics. Although the (lowest-energy) ground-state WC (GSWC) has been thoroughly studied, the properties of excited-state WCs (ESWCs) are basically unknown. To bridge this gap, we present a well-defined procedure to obtain an entire family of ESWCs in a one-dimensional electron gas using a symmetry-broken mean-field approach. While the GSWC is a commensurate crystal (i.e.~the number of density maxima equals the number of electrons), these ESWCs are incommensurate crystals exhibiting more or less maxima. Interestingly, they are lower in energy than the (uniform) Fermi fluid state. For some of these ESWCs we have found asymmetrical band gaps, which would lead to anisotropic conductivity. These properties are associated to unusual characteris...
Transfer matrices and excitations with matrix product states
Zauner, V.; Draxler, D.; Vanderstraeten, L.; Degroote, M.; Haegeman, J.; Rams, M. M.; Stojevic, V.; Schuch, N.; Verstraete, F.
2015-05-01
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.
Foil dissociation of fast molecular ions into atomic excited states
International Nuclear Information System (INIS)
The intensity and polarizations of light emitted from atomic excited states of dissociated molecular ions were measured. The dissociations are induced when fast molecular ions (50 to 500 keV/amu) are transmitted through thin carbon foils. A calculation of multiple scattering and the Coulomb explosion gives the average internuclear separation of the projectile at the foil surface. Experimentally, the foil thickness is varied to give varying internuclear separations at the foil surface and observe the consequent variation in light yield and optical polarization. Using HeH+ projectiles, factors of 1 to 5 enhancements of the light yields from n = 3, 13P,D states of He I and some He II and H I emissions were observed. The results can be explained in terms of molecular level crossings which provide mixings of the various final states during dissociation of the molecular ions at the exit surface. They suggest a short range surface interaction of the electron pick-up followed by a slow molecular dissociation. Alignment measurements confirm the essential features of the model. Observations of Lyman α emission after dissociation of H2+ amd H3+ show rapid variations in light yield for small internuclear separations at the foil surface
Excited-State Dynamics in Colloidal Semiconductor Nanocrystals.
Rabouw, Freddy T; de Mello Donega, Celso
2016-10-01
Colloidal semiconductor nanocrystals have attracted continuous worldwide interest over the last three decades owing to their remarkable and unique size- and shape-, dependent properties. The colloidal nature of these nanomaterials allows one to take full advantage of nanoscale effects to tailor their optoelectronic and physical-chemical properties, yielding materials that combine size-, shape-, and composition-dependent properties with easy surface manipulation and solution processing. These features have turned the study of colloidal semiconductor nanocrystals into a dynamic and multidisciplinary research field, with fascinating fundamental challenges and dazzling application prospects. This review focuses on the excited-state dynamics in these intriguing nanomaterials, covering a range of different relaxation mechanisms that span over 15 orders of magnitude, from a few femtoseconds to a few seconds after photoexcitation. In addition to reviewing the state of the art and highlighting the essential concepts in the field, we also discuss the relevance of the different relaxation processes to a number of potential applications, such as photovoltaics and LEDs. The fundamental physical and chemical principles needed to control and understand the properties of colloidal semiconductor nanocrystals are also addressed. PMID:27573500
Ground States and Excited States in a Tunable Graphene Quantum Dot
Institute of Scientific and Technical Information of China (English)
WANG Lin-Jun; CAO Gang; TU Tao; LI Hai-Ou; ZHOU Cheng; HAO Xiao-Jie; GUO Guang-Can; GUO Guo-Ping
2011-01-01
We prepare an etched gate tunable quantum dot in single-layer graphene and present transport measurement in this system. We extract the information of the ground states and excited states of the graphene quantum dot, as denoted by the presence of characteristic Coulomb blockade diamond diagrams. The results demonstrate that the quantum dot in single-layer graphene bodes well in future quantum transport study and quantum computing applications.%@@ We prepare an etched gate tunable quantum dot in single-layer graphene and present transport measurement in this system.We extract the information of the ground states and excited states of the graphene quantum dot, as denoted by the presence of characteristic Coulomb blockade diamond diagrams.The results demonstrate that the quantum dot in single-layer graphene bodes well in future quantum transport study and quantum computing applications.
Ground States and Excited States in a Tunable Graphene Quantum Dot
International Nuclear Information System (INIS)
We prepare an etched gate tunable quantum dot in single-layer graphene and present transport measurement in this system. We extract the information of the ground states and excited states of the graphene quantum dot, as denoted by the presence of characteristic Coulomb blockade diamond diagrams. The results demonstrate that the quantum dot in single-layer graphene bodes well for future quantum transport study and quantum computing applications. (condensed matter: electronic structure, electrical, magnetic, and optical properties)
Prabhumirashi, L. S.; Satpute, R. S.
The dipole moments of isomeric o-, m- and p-chloroanilines and chlorophenols in electronically excited L a and L b states are estimated from solvent induced polarization shifts in electronic absorption spectra. It is observed that μ e( L a) > μ e( L b) > μ g, which is consistent with the general theory of polarization red shift. The μ es are found to be approximately co-linear with the corresponding μ gs. The concept of group moments is extended to aromatic molecules in excited states. This approach is found to be useful in understanding correlations among the excited states of mono- and disubstituted benzenes.
Gamiz-Hernandez, Ana P; Magomedov, Artiom; Hummer, Gerhard; Kaila, Ville R I
2015-02-12
Proton-coupled electron transfer (PCET) processes are elementary chemical reactions involved in a broad range of radical and redox reactions. Elucidating fundamental PCET reaction mechanisms are thus of central importance for chemical and biochemical research. Here we use quantum chemical density functional theory (DFT), time-dependent density functional theory (TDDFT), and the algebraic diagrammatic-construction through second-order (ADC(2)) to study the mechanism, thermodynamic driving force effects, and reaction barriers of both ground state proton transfer (pT) and photoinduced proton-coupled electron transfer (PCET) between nitrosylated phenyl-phenol compounds and hydrogen-bonded t-butylamine as an external base. We show that the obtained reaction barriers for the ground state pT reactions depend linearly on the thermodynamic driving force, with a Brønsted slope of 1 or 0. Photoexcitation leads to a PCET reaction, for which we find that the excited state reaction barrier depends on the thermodynamic driving force with a Brønsted slope of 1/2. To support the mechanistic picture arising from the static potential energy surfaces, we perform additional molecular dynamics simulations on the excited state energy surface, in which we observe a spontaneous PCET between the donor and the acceptor groups. Our findings suggest that a Brønsted analysis may distinguish the ground state pT and excited state PCET processes.
q-NONLINEAR CAVITY FIELD STATES GENERATED BY THE EXCITATIONS ON A q-COHERENT STATE
Institute of Scientific and Technical Information of China (English)
Wei Lian-fu; Xi Ding-ping
2000-01-01
It is shown that photon-excitation state defined by|α,k)q=α+kq|q(k=1,2,3...) up to a normalization constant can be produced innonlinear processes in q-nonlinear cavities. The mathematical andquantum statistical properties of this state are studied indetail. We show that this state, along with the numberstates absented in it, forms a complete set. We also show bynumerical method that this state exhibits quantum-squeezing forsome values of |α| and always reveals quantum-antibunchingeffect.
International Nuclear Information System (INIS)
The presence of weakly bound rotationally excited initial states of HD2+ lying just below the lowest dissociation limit has been observed as well as quasi-bound, predissociative final states above the dissociation limit resulting from one-photon excitation of those weakly bound states. The excitation of the initial weakly bound and possibly only few quasi-bound states took place with 1064 nm laser radiation. The possibility of one-photon excitation of the vibrationally excited initial HD2+ ions is considered. The centre-of-mass kinetic energy distributions of the D+ and H+ fragment were used to identify the possible initial and final states involved in the transitions leading to these fragments. The fragment ratio D+/H+ is shown to be critically dependent on the ion source pressure. A strong preference is observed for the D++HD dissociation channel over the H++D2 channel at high source gas pressures. The centre-of-mass energy of the resulting H+ and D+ fragments was found to agree with predicted theoretical values, and suggest that among initially excited HD2+ ions, only a few of these lie initially above the lowest dissociation limit. (author)
Energy Technology Data Exchange (ETDEWEB)
Yousif, F.B. [Centro de Ciencias Fisicas, UNAM, Cuernavaca, Morelos (Mexico)]. E-mail: fbyousif@fis.unam.mx; Cisneros, C.; Urquijo, J. de; Alvarez, I. [Centro de Ciencias Fisicas, UNAM, Cuernavaca, Morelos (Mexico)
2001-03-14
The presence of weakly bound rotationally excited initial states of HD{sub 2}{sup +} lying just below the lowest dissociation limit has been observed as well as quasi-bound, predissociative final states above the dissociation limit resulting from one-photon excitation of those weakly bound states. The excitation of the initial weakly bound and possibly only few quasi-bound states took place with 1064 nm laser radiation. The possibility of one-photon excitation of the vibrationally excited initial HD{sub 2}{sup +} ions is considered. The centre-of-mass kinetic energy distributions of the D{sup +} and H{sup +} fragment were used to identify the possible initial and final states involved in the transitions leading to these fragments. The fragment ratio D{sup +}/H{sup +} is shown to be critically dependent on the ion source pressure. A strong preference is observed for the D{sup +}+HD dissociation channel over the H{sup +}+D{sub 2} channel at high source gas pressures. The centre-of-mass energy of the resulting H{sup +} and D{sup +} fragments was found to agree with predicted theoretical values, and suggest that among initially excited HD{sub 2}{sup +} ions, only a few of these lie initially above the lowest dissociation limit. (author)
International Nuclear Information System (INIS)
Using pulsed optically detected magnetic resonance techniques, we directly probe electron-spin resonance transitions in the excited-state of single nitrogen-vacancy (NV) color centers in diamond. Unambiguous assignment of excited state fine structure is made, based on changes of NV defect photoluminescence lifetime. This study provides significant insight into the structure of the emitting 3E excited state, which is invaluable for the development of diamond-based quantum information processing.
The Need, Benefits, and Demonstration of a Minimization Principle for Excited States
Bacalis, Naoum C
2015-01-01
It is shown that the standard methods of computing excited states in truncated spaces must yield wave functions that, beyond truncation, are in principle veered away from the exact, and a remedy is demonstrated via a presented functional, F$_n$, obeying a minimization principle for excited states. It is further demonstrated that near avoided crossings, between two MCSCF 'flipped roots' the wave function that leads to the excited state has the lowest F$_n$.
Excitation and ionization of atomic hydrogen from various states
Vriens, L.
1965-01-01
For large energies E1 of the impinging electrons, the cross sections Q for optically allowed excitation and ionization of atoms are given by Q = A/E1 ln cE1, where A and c are constants for one transition. For excitation A is proportional to the optical oscillator strength for the transition. For io
Hertzian spectroscopy application to excited states in accelerated ion beams
International Nuclear Information System (INIS)
It is shown that accelerated ion beams enables the application of optical hertzian spectrometry methods to be extended to research on the excited states of free ionic systems. The photon beat method has proved especially simple to apply in beam foil geometry because of the unidirectional beam velocity while the beam gas device is suitable for experiments of the energy level crossing type. Only the resonance technique involving direct application of high-frequency magnetic fields poses serious problems because of the high HF powers necessary. So far structure intervals have been measured in ions carrying up to three charges (seven in the special case of Lamb shift measurements) with a precision of a few percent. The interest of these structure studies in free ions is emphasized particularly. The study of hydrogen-like or helium-like ions of high Z allows the fundamental calculations of quantum electrodynamics to be checked with regard to the Lamb shift or the spontaneous emission theory. In more complex electronic systems, optical spectroscopy of accelerated ion beams gives wavelengths with a resolution reaching 10-5, lifetimes with an accuracy better than 10% when the cascade effects are properly studied, and Lande factors with a precision of several % under present technical conditions. The photon beat method concerns hyperfine nuclear effects in light atoms of Z<=20. Another line of research study the hyperfine structure of a given configuration in an isoelectronic sequence
A Simple Hubbard Model for the Excited States of $\\pi$ Conjugated -acene Molecules
Sadeq, Z S
2015-01-01
In this paper we present a model that elucidates in a simple way the electronic excited states of $\\pi$ conjugated -acene molecules such as tetracene, pentacene, and hexacene. We use a tight-binding and truncated Hubbard model written in the electron-hole basis to describe the low lying excitations with reasonable quantitative accuracy. We are able to produce semi-analytic wavefunctions for the electronic states of the system, which allows us to compute the density correlation functions for various states such as the ground state, the first two singly excited states, and the lowest lying doubly excited state. We show that in this lowest lying doubly excited state, a state which has been speculated as to being involved in the singlet fission process, the electrons and holes behave in a triplet like manner.
Probing an Excited-State Atomic Transition Using Hyperfine Quantum Beat Spectroscopy
Wade, Christopher G; Keaveney, James; Adams, Charles S; Weatherill, Kevin J
2014-01-01
We describe a method to observe the dynamics of an excited-state transition in a room temperature atomic vapor using hyperfine quantum beats. Our experiment using cesium atoms consists of a pulsed excitation of the D2 transition, and continuous-wave driving of an excited-state transition from the 6P$_{3/2}$ state to the 7S$_{1/2}$ state. We observe quantum beats in the fluorescence from the 6P$_{3/2}$ state which are modified by the driving of the excited-state transition. The Fourier spectrum of the beat signal yields evidence of Autler-Townes splitting of the 6P$_{3/2}$, F = 5 hyperfine level and Rabi oscillations on the excited-state transition. A detailed model provides qualitative agreement with the data, giving insight to the physical processes involved.
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.
Excited state lifetime during photostimulated desorption of no from a Pt surface
Magkoev, T. T.
1998-07-01
We analyze the rotational energy distribution N(J) for NO molecules desorbed from a Pt (111) surface, taking into account the valence electron excitations, using a simple impulse model. We find a linear dependence between ln N(J) and (Er)1/2, where Er is the rotational energy of the desorbed molecules. The excited state lifetime and the critical residence time in the excited state, evaluated from the given dependences, are close to each other, and in order of magnitude are 10-15 s. We also estimate the frequency and amplitude of the tilting vibrations of the adsorbed molecules in the excited state.
A Dark Excited State of Fluorescent Protein Chromophores, Considered as Brooker Dyes
Olsen, Seth
2010-01-01
The green fluorescent protein (GFP) chromophore is an asymmetric monomethine dye system. In the resonance color theory of dyes, a strong optical excitation arises from interactions of two valence-bond structures with a third, higher structure. We use correlated quantum chemistry to show that the anionic chromophore is a resonant Brooker dye, and that the third structure corresponds to a higher stationary electronic state of this species. The excitation energy of this state should be just below the first excitation energy of the neutral form. This has implications for excited state mechanism in GFPs, which we discuss.
Excited-state lifetime of adenine near the first electronic band origin.
Kang, Hyuk; Chang, Jinyoung; Lee, Sang Hak; Ahn, Tae Kyu; Kim, Nam Joon; Kim, Seong Keun
2010-10-21
The excited-state lifetime of supersonically cooled adenine was measured in the gas phase by femtosecond pump-probe transient ionization as a function of excitation energy between 36 100 and 37 500cm(-1). The excited-state lifetime of adenine is ∼2ps around the 0-0 band of the (1)L(b) ππ(∗) state (36 105cm(-1)). The lifetime drops to ∼1ps when adenine is excited to the (1)L(a) ππ(∗) state with the pump energy at 36 800cm(-1) and above. The excited-state lifetimes of (1)L(a) and (1)L(b) ππ(∗) states are differentiated in accordance with previous frequency-resolved and computational studies.
Two-mode excited entangled coherent states and their entanglement properties
Institute of Scientific and Technical Information of China (English)
Zhou Dong-Lin; Kuang Le-Man
2009-01-01
This paper introduces two types of two-mode excited entangled coherent states(TMEECSs)|Ψ±(α,m,n)>,studies their entanglement characteristics,and investigates the influence of photon excitations on quantum entanglement.It shows that for the state|Ψ+(α,m,m)>the two-mode photon excitations affect seriously entanglement character while the state |Ψ-(α,m,m)>is always a maximally entangled state,and shows how such states can be produced by using cavity quantum electrodynamics and quantum measurements.It finds that the entanglement amount of the TMEECSs is larger than that of the single-mode excited entangled coherent states with the same photon excitation number.
State-averaged Monte Carlo configuration interaction applied to electronically excited states
Coe, J P
2014-01-01
We introduce state-averaging into the method of Monte Carlo configuration interaction (SA-MCCI) to allow the stable and efficient calculation of excited states. We show that excited potential curves for H$_{3}$, including a crossing with the ground state, can be accurately reproduced using a small fraction of the FCI space. A recently introduced error measure for potential curves [J. P. Coe and M. J. Paterson, J. Chem. Phys., 137, 204108 (2012)] is shown to also be a fair approach when considering potential curves for multiple states. We demonstrate that potential curves for LiF using SA-MCCI agree well with the FCI results and the avoided crossing occurs correctly. The seam of conical intersections for CH$_{2}$ found by Yarkony [J. Chem. Phys., 104, 2932 (1996)] is used as a test for SA-MCCI and we compare potential curves from SA-MCCI with FCI results for this system for the first three triplet states. We then demonstrate the improvement from using SA-MCCI on the dipole of the $2$ $^{1}A_{1}$ state of carbo...
Head-Gordon, Martin; Rico, Rudolph J.; Lee, Timothy J.; Oumi, Manabu
1994-01-01
A perturbative correction to the method of configuration interaction with single substitutions (CIS) is presented. This CIS(D) correction approximately introduces the effect of double substitutions which are absent in CIS excited states. CIS(D) is a second-order perturbation expansion of the coupled-cluster excited state method, restricted to single and double substitutions, in a series in which CIS is zeroth order, and the first-order correction vanishes. CIS (D) excitation energies are size consistent and the calculational complexity scales with the fifth power of molecular size, akin to second-order Moller-Plesset theory for the ground state. Calculations on singlet excited states of ethylene, formaldehyde, acetaldehyde, butadiene and benzene show that CIS (D) is a uniform improvement over CIS. CIS(D) appears to be a promising method for examining excited states of large molecules, where more accurate methods are not feasible.
Dereka, Bogdan; Rosspeintner, Arnulf; Li, Zhiquan; Liska, Robert; Vauthey, Eric
2016-04-01
Most symmetric quadrupolar molecules designed for two-photon absorption behave as dipolar molecules in the S1 electronic excited state. This is usually explained by a breakup of the symmetry in the excited state. However, the origin of this process and its dynamics are still not fully understood. Here, excited-state symmetry breaking in a quadrupolar molecule with a D-π-A-π-D motif, where D and A are electron donating and accepting units, is observed in real time using ultrafast transient infrared absorption spectroscopy. The nature of the relaxed S1 state was found to strongly depend on the solvent polarity: (1) in nonpolar solvents, it is symmetric and quadrupolar; (2) in weakly polar media, the quadrupolar state observed directly after excitation transforms to a symmetry broken S1 state with one arm bearing more excitation than the other; and (3) in highly polar solvents, the excited state evolves further to a purely dipolar S1 state with the excitation localized entirely on one arm. The time scales associated with the transitions between these states coincide with those of solvation dynamics, indicating that symmetry breaking is governed by solvent fluctuations.
Betowski, Leon D; Enlow, Mark; Riddick, Lee
2002-06-01
Investigators using models to determine the phototoxic effects of sunlight on polycyclic aromatic hydrocarbons (PAHs) have invoked the excited states of the molecule as important in elucidating the mechanism of these reactions. Energies of actual excited states were calculated for ten PAHs by several ab initio methods. The main method used for these calculations was the Configuration Interaction approach, modeling excited states as combinations of single substitutions out of the Hartree-Fock ground state. These calculations correlate well with both experimentally measured singlet and triplet state energies and also previous HOMO-LUMO gap energies that approximate the singlet state energies. The excited state calculations then correlate well with general models of photo-induced toxicity based for the PAHs.
Ground and Excited States of Bipolarons in Two and Three Dimensions
Institute of Scientific and Technical Information of China (English)
RUAN Yong-Hong; CHEN Qing-Hu
2007-01-01
The properties of large bipolarons in two and three dimensions are investigated by averaging over the relative wavefunction of the two electrons and using the Lee-Low-Pines-Huybrechts variational method. The groundstate (GS) and excited-state energies of the Fr(o)hlich bipolaron for the whole range of electron-phonon coupling constants can be obtained. The energies of the first relaxed excited state (RES) and Franck-Condon (FC) excited state of the bipolaron are also calculated. It is found that the first RES energy is lower than the FC state energy. The comparison of our GS and RES energies with those in literature is also given.
Szczepanik, Beata
2015-11-01
The excited state proton transfer (ESPT) has been extensively studied for hydroxyarenes, phenols, naphthols, hydroxystilbenes, etc., which undergo large enhancement of acidity upon electronic excitation, thus classified as photoacids. The changes of acidic character in the excited state of cyano-substituted derivatives of phenol, hydroxybiphenyl and naphthol are reviewed in this paper. The acidity constants pKa in the ground state (S0), pKa∗ in the first singlet excited state (S1) and the change of the acidity constant in the excited state ΔpKa for the discussed compounds are summarized and compared. The results of the acidity studies show, that the "electro-withdrawing" CN group in the molecules of naphthol, hydroxybiphenyl and phenol causes dramatic increase of their acidity in the excited state in comparison to the ground state. This effect is greatest for the cyanonaphthols (the doubly substituted CN derivatives are almost as strong as a mineral acid in the excited state), comparable for cyanobiphenyls, and smaller for phenol derivatives. The increase of acidity enables proton transfer to various organic solvents, and the investigation of ESPT can be extended to a variety of solvents besides water. The results of theoretical investigations were also presented and used for understanding the protolytic equilibria of cyano derivatives of naphthol, hydroxybiphenyl and phenol.
Femtosecond Excited State Dynamics of Size Selected Neutral Molecular Clusters.
Montero, Raúl; León, Iker; Fernández, José A; Longarte, Asier
2016-07-21
The work describes a novel experimental approach to track the relaxation dynamics of an electronically excited distribution of neutral molecular clusters formed in a supersonic expansion, by pump-probe femtosecond ionization. The introduced method overcomes fragmentation issues and makes possible to retrieve the dynamical signature of a particular cluster from each mass channel, by associating it to an IR transition of the targeted structure. We have applied the technique to study the nonadiabatic relaxation of pyrrole homoclusters. The results obtained exciting at 243 nm, near the origin of the bare pyrrole electronic absorption, allow us to identify the dynamical signature of the dimer (Py)2, which exhibits a distinctive lifetime of τ1 ∼ 270 fs, considerably longer than the decays recorded for the monomer and bigger size clusters (Py)n>2. A possible relationship between the measured lifetime and the clusters geometries is tentatively discussed.
Excited triplet states as photooxidants in surface waters
Canonica, S.
2012-12-01
The chromophoric components of dissolved organic matter (DOM) are generally the main absorbers of sunlight in surface waters and therefore a source of transient reactants under irradiation. Such short-lived species can be relevant for the fate of various classes of chemical contaminants in the aquatic environment. The present contribution focuses on the role of excited triplet states of chromophoric DOM, 3CDOM*, as transient photooxidants initiating the transformation and degradation of organic chemical contaminants. An early study [1] indicated that 3CDOM* may play a dominant role in the photo-induced transformation of electron-rich phenols, a conclusion which was later fortified by the results of transient absorption investigations using aromatic ketones as model photosensitizers [2] and by a recent careful analysis of the effect of oxygen concentration on transformation rates [3]. The variety of aquatic contaminants shown to be affected by triplet-induced oxidation has kept increasing, phenylurea herbicides [4], sulfonamide antibiotics [5] and some phytoestrogens [6] being prominent examples. Recent research has shown that the triplet-induced transformation of specific contaminants, especially aromatic nitrogen compounds, could be inhibited by the presence of DOM, very probably due to its antioxidant moieties [7]. While such moieties are not relevant for the quenching of 3CDOM*, they are expected to react with it in a similar way as the studied contaminants. Analogous reactions can be postulated to occur in liquid or solid phases of the atmospheric environment, as demonstrated in the case of HONO formation [8]. References 1. Canonica, S.; Jans, U.; Stemmler, K.; Hoigné, J. Transformation kinetics of phenols in water: Photosensitization by dissolved natural organic material and aromatic ketones. Environ. Sci. Technol. 1995, 29 (7), 1822-1831. 2. Canonica, S.; Hellrung, B.; Wirz, J. Oxidation of phenols by triplet aromatic ketones in aqueous solution. J. Phys
Efficient 800nm upconversion luminescence emission in 1.319μm excited thulium-doped fluorogermanate
Gouveia-Neto, A. S.; Vermelho, M. V. D.; Jacinto, C.; Gouveia, E. A.; Bueno, L. A.
2016-02-01
Generation of near-infrared light within the first biological optical window via frequency upconversion in Tm3+-doped PbGeO3-PbF2-CdF2 glass excited within the second biological window at 1.319 μm is reported. The upconversion emission at 800 nm is the sole light signal observed in the entire UV-VIS-NIR spectral region making possible obtaining high contrast imaging. The dependence of the 800 nm signal upon the sample temperature was investigated and results showed an increase by a factor of x2.5 in the 30°C - 280°C range. Generation of detectable 690 nm for temperatures above 100°C in addition to the intense 800 nm main signal was also observed. The proposed excitation mechanism for the 800 nm thulium emitting level is assigned to a multiphonon-assisted excitation from the ground-state 3H6 to the 3H5 excited-state level, a rapid relaxation to the 3F4 level and followed by an excited-state absorption of the pump photons mediated by multiphonons connecting the 3F4 level to the 3H4 emitting level.
1.319 μm excited intense 800 nm frequency upconversion emission in Tm3+-doped fluorogermanate glass
Gouveia-Neto, A. S.; Vermelho, M. V. D.; Gouveia, E. A.; Bueno, L. A.; Jacinto, C.
2015-11-01
Generation of near-infrared light within the first biological optical window via frequency upconversion in Tm3+-doped PbGeO3-PbF2-CdF2 glass excited within the second biological window at 1.319 μm is reported. The upconversion emission at 800 nm is the sole light signal observed in the entire ultraviolet-visible-near-infrared spectral region making it possible obtaining high contrast imaging. The dependence of the 800 nm signal upon the sample temperature was investigated and results showed an increase by a factor of ×2.5 in the 30-280 °C range. Generation of detectable 690 nm for temperatures above 100 °C in addition to the intense 800 nm main signal was also observed. The proposed excitation mechanism for the 800 nm thulium emitting level is assigned to a multiphonon-assisted excitation from the ground-state 3H6 to the 3H5 excited-state level, a rapid relaxation to the 3F4 level and followed by an excited-state absorption of the pump photons mediated by multiphonons connecting the 3F4 level to the 3H4 emitting level.
High-energy excited states in 98Cd
Blazhev, A.; Braun, N.; Grawe, H.; Boutachkov, P.; Nara Singh, B. S.; Brock, T.; Liu, Zh; Wadsworth, R.; Górska, M.; Jolie, J.; Nowacki, F.; Pietri, S.; Domingo-Pardo, C.; Kojouharov, I.; Caceres, L.; Engert, T.; Farinon, F.; Gerl, J.; Goel, N.; Grȩbosz, J.; Hoischen, R.; Kurz, N.; Nociforo, C.; Prochazka, A.; Schaffner, H.; Steer, S.; Weick, H.; Wollersheim, H.-J.; Ataç, A.; Bettermann, L.; Eppinger, K.; Faestermann, T.; Finke, F.; Geibel, K.; Hinke, C.; Gottardo, A.; Ilie, G.; Iwasaki, H.; Krücken, R.; Merchan, E.; Nyberg, J.; Pfützner, M.; Podolyák, Zs; Regan, P.; Reiter, P.; Rinta-Antila, S.; Rudolph, D.; Scholl, C.; Söderström, P.-A.; Warr, N.; Woods, P.
2010-01-01
In 98Cd a new high-energy isomeric γ-ray transition was identified, which confirms previous spin-parity assignments and enables for the first time the measurement of the E2 and E4 strength for the two decay branches of the isomer. Preliminary results on the 98Cd high-excitation level scheme are presented. A comparison to shell-model calculations as well as implications for the nuclear structure around 100Sn are discussed.
Dual channel nitrogen laser useful for nanosecond excited state studies
International Nuclear Information System (INIS)
Shipman (1967) adapted the Blumlein discharge circuit to lasers and this method has proved highly useful in producing high peak pulses. The authors describe a double Blumlein producing two 250 kW pulses separated by 15 nanosecs. The dual channel nitrogen laser is designed for use in atomic spectroscopy, the first pulse excites the target atoms while the second pumps another laser whose output is used to study the levels. (U.S.)
von Hippel, G M; Djukanovic, D; Hua, J; Jäger, B; Junnarkar, P; Meyer, H B; Rae, T D; Wittig, H
2014-01-01
We study the ability of a variety of fitting techniques to extract the ground state matrix elements of the vector current from ratios of nucleon three- and two-point functions that contain contaminations from excited states. Extending our high-statistics study of nucleon form factors, we are able to demonstrate that the treatment of excited-state contributions in conjunction with approaching the physical pion mass has a significant impact on the $Q^2$-dependence of the form factors.
Heme photolysis occurs by ultrafast excited state metal-to-ring charge transfer.
Franzen, S.; Kiger, L.; Poyart, C; Martin, J.L.
2001-01-01
Ultrafast time-resolved resonance Raman spectra of carbonmonoxy hemoglobin (Hb), nitroxy Hb, and deoxy Hb are compared to determine excited state decay mechanisms for both ligated and unligated hemes. Transient absorption and Raman data provide evidence for a sequential photophysical relaxation pathway common to both ligated and unligated forms of Hb* (photolyzed heme), in which the excited state 1Q decays sequentially: 1Q-->Hb*I-->Hb*II-->Hb ground state. Consistent with the observed kinetic...
Quantum number dimensional scaling analysis for excited states of multielectron atoms
Murawski, R K; Murawski, Robert K.; Svidzinsky, Anatoly A.
2006-01-01
A new dimensional scaling method for the calculation of excited states of multielectron atoms is introduced. By including the principle and orbital quantum numbers in the dimension parameter, we obtain an energy expression for excited states including high angular momentum states. The method is tested on He, Li, and Be. We obtain good agreement with more orthodox quantum mechanical treatments even in the zeroth order.
Carbazole-containing light- emitting polymers: Properties of excited states
Institute of Scientific and Technical Information of China (English)
无
2003-01-01
A series of light-emitting conjugated polymers alternatively involving carbazole and bivinylene arylene moieties in the main chain were synthesized via Wittig-Horner type copolymerization. The photoinduced charge transfer process relating to these polymers was investigated by using the technique of fluorescence spectroscopy. The interaction between excited copolymers and C60 in benzene solution was studied. The fluorescence quenching can be well described by the "sphere-of-action" mechanism. It is believed that two basic steps are involved in the quenching process, i.e. the diffusion of excitation within the conjugated polymers and the dissociation of the exctions trapped by fullerene. The radius of the sphere-of-action can be related to the excitation diffusion length, which depends on the lifetime of the exciton. The dynamic fluorescence quenching of the copolymers by another quencher, 1,4-dicyanobenzene (DCB) was also surveyed. Copolymers with different chain conformations show different temperature effects in the dynamic quenching. A planar conformation is beneficial for the quenching via bimolecular collision.
Cheng, Yan; Chini, Michael; Wang, Xiaowei; González-Castrillo, Alberto; Palacios, Alicia; Argenti, Luca; Martín, Fernando; Chang, Zenghu
2016-08-01
Attosecond science promises to allow new forms of quantum control in which a broadband isolated attosecond pulse excites a molecular wave packet consisting of a coherent superposition of multiple excited electronic states. This electronic excitation triggers nuclear motion on the molecular manifold of potential energy surfaces and can result in permanent rearrangement of the constituent atoms. Here, we demonstrate attosecond transient absorption spectroscopy (ATAS) as a viable probe of the electronic and nuclear dynamics initiated in excited states of a neutral molecule by a broadband vacuum ultraviolet pulse. Owing to the high spectral and temporal resolution of ATAS, we are able to reconstruct the time evolution of a vibrational wave packet within the excited B'Σ1u+ electronic state of H2 via the laser-perturbed transient absorption spectrum.
Institute of Scientific and Technical Information of China (English)
Fang Chao; Sun Li-Feng
2011-01-01
An algorithm has been introduced to calculate molecular bond polarizabilities of thiourea, which supply essential electronic information about the nonresonant Raman excited virtual states.The main dynamical behaviour of the excited virtual states of thiourea is that the Raman excited electrons tend to flow to the N-H bonds and C-N bonds from the S-C bonds because of the electronic repulsion effect. The difference in Raman excited electron relaxation time of thiourea under 514.5-nm and 325-nm excitations has been observed, which quantitatively shows that the Raman scattering process is dependent on the wavelength of the pumping laser. Finally, the distribution of the electrons at the final stage of relaxation is given out through the comparison between the bond electronic densities of the ground states and the bond polarizabilities after deexcitation.
Joshi, Sunita; Pant, Debi D.
2012-06-01
Ground and excited state dipole moments of probe quinine sulphate (QS) was obtained using Solvatochromic shift method. Higher dipole moment is observed for excited state as compared to the ground state which is attributed to the higher polarity of excited state.
Characterization of ground state entanglement by single-qubit operations and excitation energies
Giampaolo, S M; Illuminati, F; Verrucchi, P; Giampaolo, Salvatore M.; Illuminati, Fabrizio; Siena, Silvio De; Verrucchi, Paola
2006-01-01
We consider single-qubit unitary operations and study the associated excitation energies above the ground state of interacting quantum spins. We prove that there exists a unique operation such that the vanishing of the corresponding excitation energy determines a necessary and sufficient condition for the separability of the ground state. We show that the energy difference associated to factorization exhibits a monotonic behavior with the one-tangle and the entropy of entanglement, including non analiticity at quantum critical points. The single-qubit excitation energy thus provides an independent, directly observable characterization of ground state entanglement, and a simple relation connecting two universal physical resources, energy and nonlocal quantum correlations.
Iterative solutions for low lying excited states of a class of Schr(o)dinger equation
Institute of Scientific and Technical Information of China (English)
R.Friedberga; T.D.Lee; Zhao Wei-Qin
2006-01-01
The convergent iterative procedure for solving the groundstate Schr(o)dinger equation is extended to derive the excitation energy and the wavefunction of the low-lying excited states. The method is applied to the one-dimensional quartic potential problem. The results show that the iterative solution converges rapidly when the coupling g is not too small.
Spin-state transition in LaCoO3: direct neutron spectroscopic evidence of excited magnetic states.
Podlesnyak, A; Streule, S; Mesot, J; Medarde, M; Pomjakushina, E; Conder, K; Tanaka, A; Haverkort, M W; Khomskii, D I
2006-12-15
A gradual spin-state transition occurs in LaCoO3 around T approximately 80-120 K, whose detailed nature remains controversial. We studied this transition by means of inelastic neutron scattering and found that with increasing temperature an excitation at approximately 0.6 meV appears, whose intensity increases with temperature, following the bulk magnetization. Within a model including crystal-field interaction and spin-orbit coupling, we interpret this excitation as originating from a transition between thermally excited states located about 120 K above the ground state. We further discuss the nature of the magnetic excited state in terms of intermediate-spin (t(2g)(5)e(g)(1), S=1) versus high-spin (t(2g)(4)e(g)(2), S=2) states. Since the g factor obtained from the field dependence of the inelastic neutron scattering is g approximately 3, the second interpretation is definitely favored.
Shelby, Megan L; Lestrange, Patrick J; Jackson, Nicholas E; Haldrup, Kristoffer; Mara, Michael W; Stickrath, Andrew B; Zhu, Diling; Lemke, Henrik T; Chollet, Matthieu; Hoffman, Brian M; Li, Xiaosong; Chen, Lin X
2016-07-20
Photoexcited Nickel(II) tetramesitylporphyrin (NiTMP), like many open-shell metalloporphyrins, relaxes rapidly through multiple electronic states following an initial porphyrin-based excitation, some involving metal centered electronic configuration changes that could be harnessed catalytically before excited state relaxation. While a NiTMP excited state present at 100 ps was previously identified by X-ray transient absorption (XTA) spectroscopy at a synchrotron source as a relaxed (d,d) state, the lowest energy excited state (J. Am. Chem. Soc., 2007, 129, 9616 and Chem. Sci., 2010, 1, 642), structural dynamics before thermalization were not resolved due to the ∼100 ps duration of the available X-ray probe pulse. Using the femtosecond (fs) X-ray pulses of the Linac Coherent Light Source (LCLS), the Ni center electronic configuration from the initial excited state to the relaxed (d,d) state has been obtained via ultrafast Ni K-edge XANES (X-ray absorption near edge structure) on a time scale from hundreds of femtoseconds to 100 ps. This enabled the identification of a short-lived Ni(I) species aided by time-dependent density functional theory (TDDFT) methods. Computed electronic and nuclear structure for critical excited electronic states in the relaxation pathway characterize the dependence of the complex's geometry on the electron occupation of the 3d orbitals. Calculated XANES transitions for these excited states assign a short-lived transient signal to the spectroscopic signature of the Ni(I) species, resulting from intramolecular charge transfer on a time scale that has eluded previous synchrotron studies. These combined results enable us to examine the excited state structural dynamics of NiTMP prior to thermal relaxation and to capture intermediates of potential photocatalytic significance. PMID:27286410
$\\sigma$-SCF: A Direct Energy-targeting Method To Mean-field Excited States
Ye, Hong-Zhou; Ricke, Nathan D; Van Voorhis, Troy
2016-01-01
The mean-field solutions of electronic excited states are much less accessible than ground state (e.g.\\ Hartree-Fock) solutions. Energy-based optimization methods for excited states, like $\\Delta$-scf, tend to fall into the lowest solution consistent with a given symmetry -- a problem known as "variational collapse". In this work, we combine the ideas of direct energy-targeting and variance-based optimization in order to describe excited states at the mean-field level. The resulting method, $\\sigma$-scf, has several advantages. First, it allows one to target any desired excited state by specifying a single parameter: a guess of the energy of that state. It can therefore, in principle, find \\emph{all} excited states. Second, it avoids variational collapse by using a variance-based, unconstrained local minimization. As a consequence, all states -- ground or excited -- are treated on an equal footing. Third, it provides an alternate approach to locate $\\Delta$-scf solutions that are otherwise inaccessible by the...
International Nuclear Information System (INIS)
Photodissociation dynamics of pyruvic acid experimentally differs from that of commonly known ketones. We have employed the complete active space self-consistent field and its multi-state second-order perturbation methods to study its photodissociation mechanism in the S0, T1, and S1 states. We have uncovered four nonadiabatic photodecarboxylation paths. (i) The S1 system relaxes via an excited-state intramolecular proton transfer (ESIPT) to a hydrogen-transferred tautomer, near which an S1/S0 conical intersection funnels the S1 to S0 state. Then, some trajectories continue completing the decarboxylation reaction in the S0 state; the remaining trajectories via a reverse hydrogen transfer return to the S0 minimum, from which a thermal decarboxylation reaction occurs. (ii) Due to a small S1 −T1 energy gap and a large S1/T1 spin-orbit coupling, an efficient S1 → T1 intersystem crossing process happens again near this S1/S0 conical intersection. When decaying to T1 state, a direct photodecarboxylation proceeds. (iii) Prior to ESIPT, the S1 system first decays to the T1 state via an S1 → T1 intersystem crossing; then, the T1 system evolves to a hydrogen-transferred tautomer. Therefrom, an adiabatic T1 decarboxylation takes place due to a small barrier of 7.7 kcal/mol. (iv) Besides the aforementioned T1 ESIPT process, there also exists a comparable Norrish type I reaction in the T1 state, which forms the ground-state products of CH3CO and COOH. Finally, we have found that ESIPT plays an important role. It closes the S1-T1 and S1-S0 energy gaps, effecting an S1/T1/S0 three-state intersection region, and mediating nonadiabatic photodecarboxylation reactions of pyruvic acid
Semiclassical hyperspherical matrix elements for helium doubly excited states
International Nuclear Information System (INIS)
A classical description of the two-electron atom, analogous to the quantum adiabatic hyperspherical channel approach, is presented. The classical problems, analogue to the quantum eigenvalue problem for the great angular momentum operator, and the separated dynamical systems defined by each of the other constants of the motion of the non-interacting system are solved, using the Hamiltonian-Jacobi method. Some matrix elements of the Coulomb interaction terms of the Hamilton for doubly excited helium atom using the Heisenberg correspondence principle are calculated. (author). 26 refs, 4 tabs
Thermodynamical property of entanglement entropy for excited states.
Bhattacharya, Jyotirmoy; Nozaki, Masahiro; Takayanagi, Tadashi; Ugajin, Tomonori
2013-03-01
We argue that the entanglement entropy for a very small subsystem obeys a property which is analogous to the first law of thermodynamics when we excite the system. In relativistic setups, its effective temperature is proportional to the inverse of the subsystem size. This provides a universal relationship between the energy and the amount of quantum information. We derive the results using holography and confirm them in two-dimensional field theories. We will also comment on an example with negative specific heat and suggest a connection between the second law of thermodynamics and the strong subadditivity of entanglement entropy. PMID:23496702
Neutral Fermion Excitations in the Moore-Read state at \
Moller, Gunnar; Wojs, Arkadiusz; Cooper, Nigel R.
2010-01-01
We present evidence supporting the weakly paired Moore-Read phase in the half-filled second Landau level, focusing on some of the qualitative features of its excitations. Based on numerical studies, we show that systems with odd particle number at the flux $N_\\phi=2N-3$ can be interpreted as a neutral fermion mode of one unpaired fermion, which is gapped. The mode is found to have two distinct minima, providing a signature that could be observed by photoluminescence. In the presence of two qu...
Structural and excited-state properties of oligoacene crystals from first principles
Rangel, Tonatiuh; Berland, Kristian; Sharifzadeh, Sahar; Brown-Altvater, Florian; Lee, Kyuho; Hyldgaard, Per; Kronik, Leeor; Neaton, Jeffrey B.
2016-03-01
Molecular crystals are a prototypical class of van der Waals (vdW) bound organic materials with excited-state properties relevant for optoelectronics applications. Predicting the structure and excited-state properties of molecular crystals presents a challenge for electronic structure theory, as standard approximations to density functional theory (DFT) do not capture long-range vdW dispersion interactions and do not yield excited-state properties. In this work, we use a combination of DFT including vdW forces, using both nonlocal correlation functionals and pairwise correction methods, together with many-body perturbation theory (MBPT) to study the geometry and excited states, respectively, of the entire series of oligoacene crystals, from benzene to hexacene. We find that vdW methods can predict lattice constants within 1% of the experimental measurements, on par with the previously reported accuracy of pairwise approximations for the same systems. We further find that excitation energies are sensitive to geometry, but if optimized geometries are used MBPT can yield excited-state properties within a few tenths of an eV from experiment. We elucidate trends in MBPT-computed charged and neutral excitation energies across the acene series and discuss the role of common approximations used in MBPT.
Permanent Magnet Synchronous Condenser with Solid State Excitation
Energy Technology Data Exchange (ETDEWEB)
Hsu, Ping; Muljadi, Eduard; Wu, Ziping; Gao, Wenzhong
2015-10-05
A synchronous condenser consists of a free-spinning wound-field synchronous generator and a field excitation controller. In this paper, we propose a synchronous generator that employs a permanent magnet synchronous generator (PMSG) instead of a wound-field machine. PMSGs have the advantages of higher efficiency and reliability. In the proposed configuration, the reactive power control is achieved by a voltage source converter connected in series with the PMSG and the grid. The converter varies the phase voltage of the PMSG so as to create the same effect of over or under excitation in a wound-field machine. The converter output voltage level controls the amount and the direction of the produced reactive power and the voltage's phase is kept in-phase with the grid voltage except a slight phase can be introduced so that some power can be drawn from the grid for maintaining the DC bus voltage level of the converter. Since the output voltage of the converter is only a fraction of the line voltage, its VA rating is only a fraction of the rating of the PMSG. The proposed scheme is shown to be effective by computer simulation.
Notes on entanglement entropy for excites holographic states in 2d
Rashkov, Radoslav C
2016-01-01
In this work we revisit the problem of contributions of excited holographic states to the entanglement entropy in two-dimensional conformal field theories. Using the results of replica trick method we find three expressions for these contributions. First, we express the contribution of the excited states in terms of Aharonov invariants. It is shown that beside the Schwarzian, the one-point functions of descendants of energy-momentum also contribute. Given Schwarz-Christoffel map, the contributions to any order can be easily computed. The second expression relates the entanglement entropy of excited states to Faber polynomials and Grunsky coefficients. Based on the relation of Grunsky coefficiens to tau-funcion of dispersionless Toda hierarchy, we find the third expression for contributions of excited holographic states to the entanglement entropy.
Inelastic WIMP-nucleus scattering to the first excited state in $^{125}$Te
Vergados, J D; Kortelainen, M; Pirinen, P; Srivastava, P C; Suhonen, J; Thomas, A W
2016-01-01
The direct detection of dark matter constituents, in particular the weakly interacting massive particles (WIMPs), is considered central to particle physics and cosmology. In this paper we study transitions to the excited states, possible in some nuclei, which have sufficiently low lying excited states. Examples considered previously were the first excited states of $^{127}$I and $^{129}$Xe and $^{83}$Kr. Here we examine $^{125}$Te, which offers some advantages and is currently being considered as a target.In all these cases the extra signature of the gamma rays following the de-excitation of these states has definite advantages over the purely nuclear recoil and, in principle, such a signature can be exploited experimentally. A brief discussion of the experimental feasibility is given in the context of the CUORE experiment.
Ultrafast excited state dynamics of S2 and S1 states of triphenylmethane dyes.
Singhal, Pallavi; Ghosh, Hirendra N
2014-08-21
Excited state dynamics of S2 and S1 states for a series of TPM dyes, pyrogallol red (PGR), bromopyrogallol red (Br-PGR) and aurin tricarboxylic acid (ATC), have been monitored by using ultrafast transient absorption and fluorescence up-conversion techniques. Optical absorption studies indicate that all the TPM dyes exist as keto-enol tautomers depending upon the pH of the solution. Interestingly, all the TPM dyes give S2 emission (major emitting state) in addition to weak S1 emission. S2 emission lifetimes as fast as ∼150-300 fs and S1 emission lifetimes of 2-5 ns were observed depending upon the molecular structure of the dyes. Femtosecond transient absorption studies suggest the presence of an ultrafast non-radiative decay channel from the S2 state in addition to S2 luminescence. The vibrational relaxation time from hot S1 state is found to be 2-6 ps. The heavy atom effect has been observed in ultrafast relaxation dynamics of Br-PGR.
Directory of Open Access Journals (Sweden)
Sakai S.
2013-03-01
Full Text Available Vibrational dynamics of dark excited states in carotenoids have been investigated using tunable Raman pump pulses. The S1 state has same vibrational dynamics in light-harvesting complex (LH1 and solution. The S* state in LH1 has similar vibrational modes with the triplet state of carotenoid. However, the so-called S* state in solution does not have the modes and is concluded to be different from the S* state in LH1.
Mixed symmetry states and isospin excitation in N = Z nucleus 52Fe
Institute of Scientific and Technical Information of China (English)
2008-01-01
The interacting boson model with isospin (IBM-3) was applied to study the band structure and electromagnetic transition properties of the low-lying states in the even-even N = Z nucleus 52Fe. The isospin excitation states with T = 0, 1 and 2 were identified, and compared with the available data. The study shows that the 2+3 state is the lowest mixed symmetry state in 52Fe. The excitation energy of the second 0+2 state with T = 0 in nucleus 52Fe was identified. The model calculations with the data show a reasonably good agreement.
Zheng, Greg Y.; Rillema, D. Paul; DePriest, Jeff; Woods, Clifton
1998-07-13
Direct access to the triplet emitting state from the ground state is observed for Pt(II) complexes containing heterocyclic (CwedgeC', CwedgeN, NwedgeN') and bis(diphenylphosphino)alkane (PwedgeP') ligands. Extinction coefficients for such transitions are in the range 4-25 M(-)(1) cm(-)(1). Emission quantum yields resulting from singlet-to-triplet excitation are as high as 61-77 times the emission quantum yields resulting from singlet-to-singlet excitation at 296 K. The intersystem crossing quantum yield from the singlet excited state to triplet emitting state is lower than 2% at 296 K but is greatly enhanced at 77 K. The forbidden electronic transition observed for Pt(II) complexes is attributed to result from spin-orbit coupling due to the presence of Pt(II) in the skeleton structure. The importance of excitation spectra on the computation of emission quantum yields is discussed.
Counting the number of excited states in organic semiconductor systems using topology
Energy Technology Data Exchange (ETDEWEB)
Catanzaro, Michael J. [Department of Mathematics, Wayne State University, 656 W. Kirby, Detroit, Michigan 48202 (United States); Shi, Tian [Department of Chemistry, Wayne State University, 5101 Cass Ave., Detroit, Michigan 48202 (United States); Tretiak, Sergei, E-mail: serg@lanl.gov [Theoretical Division, Center for Nonlinear Studies, and Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, New Mexico 87545 (United States); Chernyak, Vladimir Y., E-mail: chernyak@chem.wayne.edu [Department of Mathematics, Wayne State University, 656 W. Kirby, Detroit, Michigan 48202 (United States); Department of Chemistry, Wayne State University, 5101 Cass Ave., Detroit, Michigan 48202 (United States)
2015-02-28
Exciton scattering theory attributes excited electronic states to standing waves in quasi-one-dimensional molecular materials by assuming a quasi-particle picture of optical excitations. The quasi-particle properties at branching centers are described by the corresponding scattering matrices. Here, we identify the topological invariant of a scattering center, referred to as its winding number, and apply topological intersection theory to count the number of quantum states in a quasi-one-dimensional system.
Distribution of populations in excited states of electrodeless discharge lamp of Rb atoms
Institute of Scientific and Technical Information of China (English)
TAO ZhiMing; WANG YanFei; HONG YeLong; WANG DongYing; ZHANG ShengNan; ZHUANG Wei; CHEN JingBiao
2013-01-01
The intensity of fluorescence spectral lines of Rb atoms in the region of 350-1110 nm is measured in eletrodeless discharge lamp.The population ratio between the excited states is calculated according to the spontaneous transition probabilities with rate equations.At the same time,the population density of energy level is also obtained.The results provide the potential applications of electrodeless discharge lamp in atomic filter and optical frequency reference at higher excited states without a pumping laser.
Steady-state photoluminescent excitation characterization of semiconductor carrier recombination
Bhosale, J. S.; Moore, J. E.; Wang, X.; Bermel, P.; Lundstrom, M. S.
2016-01-01
Photoluminescence excitation spectroscopy is a contactless characterization technique that can provide valuable information about the surface and bulk recombination parameters of a semiconductor device, distinct from other sorts of photoluminescent measurements. For this technique, a temperature-tuned light emitting diode (LED) has several advantages over other light sources. The large radiation density offered by LEDs from near-infrared to ultraviolet region at a low cost enables efficient and fast photoluminescence measurements. A simple and inexpensive LED-based setup facilitates measurement of surface recombination velocity and bulk Shockley-Read-Hall lifetime, which are key parameters to assess device performance. Under the right conditions, this technique can also provide a contactless way to measure the external quantum efficiency of a solar cell.
High-energy excited states in {sup 98}Cd
Energy Technology Data Exchange (ETDEWEB)
Braun, Norbert; Blazhev, Andrey; Jolie, Jan [Institut fuer Kernphysik, Universitaet Koeln (Germany); Boutachkov, Plamen; Gorska, Magda; Grawe, Hubert; Pietri, Stephane [GSI, Darmstadt (Germany); Brock, Tim; Nara Singh, B.S.; Wadsworth, Robert [Department of Physics, University of York, York (United Kingdom); Liu, Zhong [University of Edinburgh, Edinburgh (United Kingdom)
2009-07-01
Studies of isomerism in the proton-rich N {approx_equal}Z nuclei around {sup 100}Sn give important insights into the role of proton-neutron pairing and also serve as testing grounds for nuclear models. In summer 2008, an experiment on {sup 96,97,98}Cd was performed using the FRS fragment separator and the RISING germanium array at GSI. These exotic nuclei of interest were produced using fragmentation of a 850 MeV/u {sup 124}Xe beam on a 4 g/cm{sup 2} {sup 9}Be target and finally implanted into an active stopper consisting of 9 double-sided silicon strip detectors. In {sup 98}Cd, a new high-energy isomeric transition was identified. Preliminary results on {sup 98}Cd are presented and their implications for the high-excitation level scheme are discussed.
Steady-state photoluminescent excitation characterization of semiconductor carrier recombination
Energy Technology Data Exchange (ETDEWEB)
Bhosale, J. S. [Intel Corporation, Hillsboro, Oregon 97124 (United States); Department of Electrical and Computer Engineering, Purdue University, West Lafayette, Indiana 47907 (United States); Moore, J. E.; Wang, X.; Bermel, P.; Lundstrom, M. S. [Department of Electrical and Computer Engineering, Purdue University, West Lafayette, Indiana 47907 (United States)
2016-01-15
Photoluminescence excitation spectroscopy is a contactless characterization technique that can provide valuable information about the surface and bulk recombination parameters of a semiconductor device, distinct from other sorts of photoluminescent measurements. For this technique, a temperature-tuned light emitting diode (LED) has several advantages over other light sources. The large radiation density offered by LEDs from near-infrared to ultraviolet region at a low cost enables efficient and fast photoluminescence measurements. A simple and inexpensive LED-based setup facilitates measurement of surface recombination velocity and bulk Shockley-Read-Hall lifetime, which are key parameters to assess device performance. Under the right conditions, this technique can also provide a contactless way to measure the external quantum efficiency of a solar cell.
Steady-state photoluminescent excitation characterization of semiconductor carrier recombination
International Nuclear Information System (INIS)
Photoluminescence excitation spectroscopy is a contactless characterization technique that can provide valuable information about the surface and bulk recombination parameters of a semiconductor device, distinct from other sorts of photoluminescent measurements. For this technique, a temperature-tuned light emitting diode (LED) has several advantages over other light sources. The large radiation density offered by LEDs from near-infrared to ultraviolet region at a low cost enables efficient and fast photoluminescence measurements. A simple and inexpensive LED-based setup facilitates measurement of surface recombination velocity and bulk Shockley-Read-Hall lifetime, which are key parameters to assess device performance. Under the right conditions, this technique can also provide a contactless way to measure the external quantum efficiency of a solar cell
Institute of Scientific and Technical Information of China (English)
无
2006-01-01
The electronic singlet vertical excited states of photosynthetic reaction center (PSRC) in Rhodopseudomonas (Rps.) viridis were investigated by ZINDO and INDO/S methods. The effects of the interactions of pigment-pigment and pigment-protein on the electronic excitations were examined. The calculation results showed that the interactions of pigment-pigment and pigment-protein play an important role in reasonably assigning the experimental absorption and circular dichroism (CD) spectra of PSRC in Rps. virids. By comparing the theoretically computed excited states with the experimental absorption and CD spectra, satisfactory assignments of the experimental spectroscopic peaks were achieved.
Non-orthogonal configuration interaction for the calculation of multielectron excited states
Energy Technology Data Exchange (ETDEWEB)
Sundstrom, Eric J., E-mail: eric.jon.sundstrom@berkeley.edu; Head-Gordon, Martin [Department of Chemistry, University of California Berkeley, Berkeley, California 94720, USA and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)
2014-03-21
We apply Non-orthogonal Configuration Interaction (NOCI) to molecular systems where multielectron excitations, in this case double excitations, play a substantial role: the linear polyenes and β-carotene. We demonstrate that NOCI when applied to systems with extended conjugation, provides a qualitatively correct wavefunction at a fraction of the cost of many other multireference treatments. We also present a new extension to this method allowing for purification of higher-order spin states by utilizing Generalized Hartree-Fock Slater determinants and the details for computing 〈S{sup 2}〉 for the ground and excited states.
Study on even-parity highly excited states of the Sm atom
Energy Technology Data Exchange (ETDEWEB)
Zhao Yanhong; Dai Changjian; Ye Shiwei, E-mail: daicj@126.com [School of Science, Tianjin University of Technology, Tianjin 300384 (China)
2011-10-14
Spectra of even-parity highly excited states of the Sm atom have been systematically studied using the two-color three-step excitation and photoionization detection method. With three different excitation paths distinguished by three different intermediate states with the 4f{sup 6}6s6p configuration, the atom is resonantly excited to given highly excited states in the energy region between 30 040 and 38 065 cm{sup -1}, where it is detected by photoionization. The wavelength of the second laser is scanned from 440 to 700 nm, while that of the first laser is fixed at 638.96, 636.92 or 627.50 nm. Based on precise calibration of the wavelength, the energy levels of 198 even-parity states are determined with the relative line intensities of the related transitions. A unique value of J, the total angular momentum, is assigned to all detected states by comparing the three spectra obtained with the different excitation paths. Except that the energy levels of 113 states are confirmed in this work, the rest of the information mentioned above has not been previously reported.
One Neutron Halo in a 12B Excited State
Institute of Scientific and Technical Information of China (English)
陈宝秋; 马中玉
2001-01-01
The nonlinear relativistic mean field (RMF) theory with a new effective interaction NL3 has been used to inves tigate the bulk properties of the 12B nucleus. The results obtained in the RMF predict one neutron halo in a 12Bexcited state. 12B does not show the neutron halo structure if it is in its ground state.
Energy Technology Data Exchange (ETDEWEB)
Niedzwiedzki, Dariusz; Kobayashi, Masayuki; Blankenship, R. E.
2011-01-13
Light-harvesting complex 2 from the anoxygenic phototrophic purple bacterium Thermochromatium tepidum was purified and studied by steady-state absorption, fluorescence and flash photolysis spectroscopy. Steady-state absorption and fluorescence measurements show that carotenoids play a negligible role as supportive energy donors and transfer excitation to bacteriochlorophyll-a with low energy transfer efficiency of ~30%. HPLC analysis determined that the dominant carotenoids in the complex are rhodopin and spirilloxanthin. Carotenoid excited triplet state formation upon direct (carotenoid) or indirect (bacteriochlorophyll-a Q{sub x} band) excitation shows that carotenoid triplets are mostly localized on spirilloxanthin. In addition, no triplet excitation transfer between carotenoids was observed. Such specific carotenoid composition and spectroscopic results strongly suggest that this organism optimized carotenoid composition in the light-harvesting complex 2 in order to maximize photoprotective capabilities of carotenoids but subsequently drastically suppressed their supporting role in light-harvesting process.
Study of the giant dipole resonance built on highly excited states in Sn and Dy nuclei
International Nuclear Information System (INIS)
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 114Sn 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 152-156Dy nuclei is presented. A theoretical model developed to describe fusion-evaporation reactions is presented. 149 refs.; 63 figs.; 13 tabs
Excited-State Dynamics of Carotenoids Studied by Femtosecond Transient Absorption Spectroscopy
Energy Technology Data Exchange (ETDEWEB)
Lee, Ingu; Pang, Yoonsoo [Department of Physics and Photon Science, Gwangju (Korea, Republic of); Lee, Sebok [Gwangju Institute of Science and Technology, Gwangju (Korea, Republic of)
2014-03-15
Carotenoids, natural antenna pigments in photosynthesis share a symmetric backbone of conjugated polyenes. Contrary to the symmetric and almost planar geometries of carotenoids, excited state structure and dynamics of carotenoids are exceedingly complex. In this paper, recent infrared and visible transient absorption measurements and excitation dependent dynamics of 8'-apo-β-caroten-8'-al and 7',7'-dicyano-7'-apo-β-carotene will be reviewed. The recent visible transient absorption measurements of 8'-apo-β-caroten-8'-al in polar and nonpolar solvents will also be introduced to emphasize the complex excited-state dynamics and unsolved problems in the S{sub 2} and S{sub 1} excited states.
Emergence of nontrivial magnetic excitations in a spin-liquid state of kagomé volborthite.
Watanabe, Daiki; Sugii, Kaori; Shimozawa, Masaaki; Suzuki, Yoshitaka; Yajima, Takeshi; Ishikawa, Hajime; Hiroi, Zenji; Shibauchi, Takasada; Matsuda, Yuji; Yamashita, Minoru
2016-08-01
When quantum fluctuations destroy underlying long-range ordered states, novel quantum states emerge. Spin-liquid (SL) states of frustrated quantum antiferromagnets, in which highly correlated spins fluctuate down to very low temperatures, are prominent examples of such quantum states. SL states often exhibit exotic physical properties, but the precise nature of the elementary excitations behind such phenomena remains entirely elusive. Here, we use thermal Hall measurements that can capture the unexplored property of the elementary excitations in SL states, and report the observation of anomalous excitations that may unveil the unique features of the SL state. Our principal finding is a negative thermal Hall conductivity [Formula: see text] which the charge-neutral spin excitations in a gapless SL state of the 2D kagomé insulator volborthite Cu3V2O7(OH)2[Formula: see text]2H2O exhibit, in much the same way in which charged electrons show the conventional electric Hall effect. We find that [Formula: see text] is absent in the high-temperature paramagnetic state and develops upon entering the SL state in accordance with the growth of the short-range spin correlations, demonstrating that [Formula: see text] is a key signature of the elementary excitation formed in the SL state. These results suggest the emergence of nontrivial elementary excitations in the gapless SL state which feel the presence of fictitious magnetic flux, whose effective Lorentz force is found to be less than 1/100 of the force experienced by free electrons. PMID:27439874
Control of multiple excited image states around segmented carbon nanotubes
Energy Technology Data Exchange (ETDEWEB)
Knörzer, J., E-mail: johannes.knoerzer@physnet.uni-hamburg.de; Fey, C., E-mail: christian.fey@physnet.uni-hamburg.de [Zentrum für Optische Quantentechnologien, Universität Hamburg, Luruper Chaussee 149, Hamburg 22761 (Germany); Sadeghpour, H. R. [ITAMP, Harvard-Smithsonian Center for Astrophysics, 60 Garden Street, Cambridge, Massachusetts 02138 (United States); Schmelcher, P. [Zentrum für Optische Quantentechnologien, Universität Hamburg, Luruper Chaussee 149, Hamburg 22761 (Germany); The Hamburg Centre for Ultrafast Imaging, Luruper Chaussee 149, Hamburg 22761 (Germany)
2015-11-28
Electronic image states around segmented carbon nanotubes can be confined and shaped along the nanotube axis by engineering the image potential. We show how several such image states can be prepared simultaneously along the same nanotube. The inter-electronic distance can be controlled a priori by engineering tubes of specific geometries. High sensitivity to external electric and magnetic fields can be exploited to manipulate these states and their mutual long-range interactions. These building blocks provide access to a new kind of tailored interacting quantum systems.
Control of multiple excited Rydberg states around segmented carbon nanotubes
Schmelcher, Peter; Sadeghpour, Hossein; Knoerzer, Johannes; Fey, Christian
2016-05-01
Electronic image Rydberg states around segmented carbon nanotubes can be confined and shaped along the nanotube axis by engineering the image potential. We show how several such image states can be prepared simultaneously along the same nanotube. The inter-electronic distance can be controlled a priori by engineering tubes of specific geometries. High sensitivity to external electric and magnetic fields can be exploited to manipulate these states and their mutual long-range interactions. These building blocks provide access to a new kind of tailored long-range interacting quantum systems.
Wurstbauer, U.; Levy, A. L.; Pinczuk, A.; West, K. W.; Pfeiffer, L. N.; Manfra, M. J.; Gardner, G. C.; Watson, J. D.
2015-12-01
We report the observation of low-lying collective charge and spin excitations in the second Landau level at ν =2 +1 /3 and also for the very fragile states at ν =2 +2 /5 and 2 +3 /8 in inelastic light scattering experiments. These modes exhibit a clear dependence on filling factor and temperature substantiating the unique access to the characteristic neutral excitation spectra of the incompressible fractional quantum Hall effect (FQHE) states. A detailed mode analysis reveals low-energy modes at around 70 μ eV and a sharp mode slightly below the Zeeman energy interpreted as gap and spin-wave excitation, respectively. The lowest-energy collective charge excitation spectrum at ν =2 +1 /3 exhibits significant qualitative similarities with its cousin state in the lowest Landau level at ν =1 /3 suggesting similar magnetoroton minima in the neutral excitations. The mode energies differ by a scaling of 0.15 indicating different interaction physics in the N =0 and N =1 Landau levels. The striking polarization dependence in elastic and inelastic light scattering is discussed in the framework of anisotropic electron phases that allow for the stabilization of nematic FQHE states. The observed excitation spectra provide new insights by accessing quantum phases in the bulk of electron systems and facilitate comparison with different theoretical descriptions of those enigmatic FQHE states.
Accounting for highly excited states in detailed opacity calculations
Pain, Jean-Christophe
2015-01-01
In multiply-charged ion plasmas, a significant number of electrons may occupy high-energy orbitals. These "Rydberg" electrons, when they act as spectators, are responsible for a number of satellites of X-ray absorption or emission lines, yielding a broadening of the red wing of the resonance lines. The contribution of such satellite lines may be important, because of the high degeneracy of the relevant excited configurations which give these large Boltzmann weights. However, it is in general difficult to take these configurations into account since they are likely to give rise to a large number of lines. We propose to model the perturbation induced by the spectators in a way similar to the Partially-Resolved-Transition-Array approach recently published by C. Iglesias. It consists in a partial detailed-line-accounting calculation in which the effect of the Rydberg spectators is included through a shift and width, expressed in terms of the canonical partition functions, which are key-ingredients of the Super-Tr...
Permanent Magnet Synchronous Condenser with Solid State Excitation: Preprint
Energy Technology Data Exchange (ETDEWEB)
Hsu, P.; Muljadi, E.; Wu, Z.; Gao, W.
2015-04-07
A typical synchronous condenser (SC) consists of a free-spinning, wound-field synchronous generator and a field excitation controller. In this paper, we propose an SC that employs a permanent magnet synchronous generator (PMSG) instead of a wound-field machine. PMSGs have the advantages of higher efficiency and reliability. In the proposed configuration, the reactive power control is achieved by a voltage converter controller connected in series to the PMSG. The controller varies the phase voltage of the PMSG and creates the same effect on the reactive power flow as that of an over- or underexcited wound-field machine. The controller’s output voltage magnitude controls the amount of the reactive power produced by the SC. The phase of the controller’s output is kept within a small variation from the grid voltage phase. This small phase variation is introduced so that a small amount of power can be drawn from the grid into the controller to maintain its DC bus voltage. Because the output voltage of the controller is only a fraction of the line voltage, its VA rating is only a fraction of the rating of the PMSG. The proposed scheme is shown to be effective by computer simulations.
Dynamic quenching as a simple test for the mechanism of excited-state reaction
International Nuclear Information System (INIS)
We report on comparative studies of dynamic fluorescence quenching of 3-hydroxyflavone (3HF) and of its novel analogs by nitric oxide spin compound TEMPO. These dyes exhibit the excited-state intramolecular proton transfer (ESIPT) reaction that allows observation of two separate bands in fluorescence emission - of initially excited form and of the product of ESIPT reaction. In the frame of two-state excited-state reaction formalism, we develop the theory predicting different dependence of intensities at two bands in steady-state spectra in the cases of thermodynamic and kinetic control of ESIPT. In line with these predictions, the quenching changes strongly the distribution of intensities between these bands for 3HF but does not change it for the novel compounds whose excited states exhibit strong charge transfer character. Based on these findings, we suggest that the quenching of fluorescence by an efficient collisional quencher can be a simple and convenient method using only the steady-state experiment for distinguishing the excited-state reactions occurring under thermodynamic or under kinetic controls. This method can be used for large-scale screening of a series of compounds - potential candidates for application in fluorescence sensor and biosensor technologies
Xie, Hongqiang; Li, Guihua; Yao, Jinping; Chu, Wei; Li, Ziting; Zeng, Bin; Wang, Zhanshan; Cheng, Ya
2015-01-01
We report on generation of third harmonic from nitrogen molecules on the excited state with a weak driver laser pulse at a mid-infrared wavelength. The excited nitrogen molecules are generated using a circularly polarized intense femtosecond pulse which produces energetic electrons by photoionization to realize collisional excitation of nitrogen molecules. Furthermore, since the third harmonic is generated using a pump-probe scheme, it enables investigation of the excited-state dynamics of nitrogen molecules produced under different conditions. We also perform a comparative investigation in excited argon atoms, revealing different decay dynamics of the molecules and atoms from the excited states in femtosecond laser induced filaments. PMID:26522886
The excited spin-triplet state of a charged exciton in quantum dots
Molas, M. R.; Nicolet, A. A. L.; Piętka, B.; Babiński, A.; Potemski, M.
2016-09-01
We report on spectroscopic studies of resonances related to ladder of states of a charged exciton in single GaAlAs/AlAs quantum dot structures. Polarization-resolved photoluminescence, photoluminescence excitation and photon-correlation measurements were performed at low (T = 4.2 K) temperature also in magnetic field applied in Faraday configuration. The investigated resonances are assigned to three different configurations of a positively charged exciton. Together with a singlet ground state and a conventional triplet state (involving an electron from the ground state electronic s-shell), an excited triplet state, which involved an electron from the excited electronic p-shell was identified in single dots. The appearance of an emission line related to the latter complex is due to a partially suppressed electron relaxation in the investigated dots. An analysis of this emission line allows us to scrupulously determine properties of the excited triplet state and compare them with those of the conventional triplet state. Both triplets exhibit similar patterns of anisotropic fine structure and Zeeman splitting, however their amplitudes significantly differ for those two states. Presented results emphasize the role of the symmetry of the electronic state on the properties of the triplet states of two holes + electron excitonic complex.
The excited spin-triplet state of a charged exciton in quantum dots.
Molas, M R; Nicolet, A A L; Piętka, B; Babiński, A; Potemski, M
2016-09-14
We report on spectroscopic studies of resonances related to ladder of states of a charged exciton in single GaAlAs/AlAs quantum dot structures. Polarization-resolved photoluminescence, photoluminescence excitation and photon-correlation measurements were performed at low (T = 4.2 K) temperature also in magnetic field applied in Faraday configuration. The investigated resonances are assigned to three different configurations of a positively charged exciton. Together with a singlet ground state and a conventional triplet state (involving an electron from the ground state electronic s-shell), an excited triplet state, which involved an electron from the excited electronic p-shell was identified in single dots. The appearance of an emission line related to the latter complex is due to a partially suppressed electron relaxation in the investigated dots. An analysis of this emission line allows us to scrupulously determine properties of the excited triplet state and compare them with those of the conventional triplet state. Both triplets exhibit similar patterns of anisotropic fine structure and Zeeman splitting, however their amplitudes significantly differ for those two states. Presented results emphasize the role of the symmetry of the electronic state on the properties of the triplet states of two holes + electron excitonic complex. PMID:27391126
Potential-energy surfaces of local excited states from subsystem- and selective Kohn–Sham-TDDFT
International Nuclear Information System (INIS)
Research highlights: ► Application of selective TDDFT for potential-energy surfaces. ► Improved eigenvector guesses for convergence speed-up. ► Intuitive single-orbital transition picture breaks down in adsorbate–surface model. ► Comparison of frozen-density embedding with classical point-charge models. ► Frozen-density embedding yields smooth potential-energy surfaces for adsorbate states. - Abstract: Calculating excited-state potential-energy surfaces for systems with a large number of close-lying excited states requires the identification of the relevant electronic transitions for several geometric structures. Time-dependent density functional theory (TDDFT) is very efficient in such calculations, but the assignment of local excited states of the active molecule can be difficult. We compare the results of the frozen-density embedding (FDE) method with those of standard Kohn–Sham density-functional theory (KS-DFT) and simpler QM/MM-type methods. The FDE results are found to be more accurate for the geometry dependence of excitation energies than classical models. We also discuss how selective iterative diagonalization schemes can be exploited to directly target specific excitations for different structures. Problems due to strongly interacting orbital transitions and possible solutions are discussed. Finally, we apply FDE and the selective KS-TDDFT to investigate the potential energy surface of a high-lying π → π∗ excitation in a pyridine molecule approaching a silver cluster.
Energy Technology Data Exchange (ETDEWEB)
Nelson, Tammie [Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Nonlinear Studies (CNLS) and Center for Integrated Nanotechnologies (CINT), Theoretical Division; Fernandez-Alberti, Sebastian [Univ. Nacional de Quilmes, Buenos Aires (Argentina); Chernyak, Vladimir [Wayne State Univ., Detroit, MI (United States). Dept. of Chemistry; Roitberg, Adrian E. [Univ. of Florida, Gainesville, FL (United States). Depts. of Physics and Chemistry. Quantum Theory Project; Tretiak, Sergei [Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Nonlinear Studies (CNLS) and Center for Integrated Nanotechnologies (CINT), Theoretical Division
2011-01-10
Nonadiabatic dynamics generally defines the entire evolution of electronic excitations in optically active molecular materials. It is commonly associated with a number of fundamental and complex processes such as intraband relaxation, energy transfer, and light harvesting influenced by the spatial evolution of excitations and transformation of photoexcitation energy into electrical energy via charge separation (e.g., charge injection at interfaces). To treat ultrafast excited-state dynamics and exciton/charge transport we have developed a nonadiabatic excited-state molecular dynamics (NA-ESMD) framework incorporating quantum transitions. Our calculations rely on the use of the Collective Electronic Oscillator (CEO) package accounting for many-body effects and actual potential energy surfaces of the excited states combined with Tully’s fewest switches algorithm for surface hopping for probing nonadiabatic processes. This method is applied to model the photoinduced dynamics of distyrylbenzene (a small oligomer of polyphenylene vinylene, PPV). Our analysis shows intricate details of photoinduced vibronic relaxation and identifies specific slow and fast nuclear motions that are strongly coupled to the electronic degrees of freedom, namely, torsion and bond length alternation, respectively. Nonadiabatic relaxation of the highly excited mA{sub g} state is predicted to occur on a femtosecond time scale at room temperature and on a picosecond time scale at low temperature.
Excited state proton transfer in the Cinchona alkaloid cupreidine
J. Qian; A.M. Brouwer
2010-01-01
Photophysical properties of the organocatalyst cupreidine (CPD) and its chromophoric building block 6-hydroxyquinoline (6HQ) in protic and nonprotic polar solvents (methanol and acetonitrile) were investigated by means of UV-vis absorption, and steady state and time resolved fluorescence spectroscop
Indirect predissociation of highly excited singlet states of N2
Directory of Open Access Journals (Sweden)
Heays A.N.
2015-01-01
Full Text Available Indirect predissociation of the b′ 1Σu+(v = 20 level of N2 is studied experimentally by vacuum-ultraviolet photoabsorption employing synchrotron radiation and a Fourier-transform spectrometer, and interpreted with the aid of a quantitative model of interacting 1Πu and 1Σu+, bound and unbound states which solves the coupled Schrödinger equation. An observed rotationally-localised peak in the b′(20 predissociation linewidths is identified by the model as arising from an interaction with a strongly predissociated and unobserved bound level of the mixed c3 1Πu and o3 1Πu Rydberg states. This leads to the dissociation of b′(20 into the continuum of the b 1Πu valence state. The residual observed predissociation of b′ 1Σu+(v = 20 apart from the rotationally-localised peak cannot be explained by a mechanism of 1Πu and 1Σu+ interaction, and must involve states of higher multiplicity.
Stretching of hydrogen-bonded OH in the lowest singlet excited electronic state of water dimer.
Chipman, Daniel M
2006-01-28
The lowest singlet excited electronic state of water monomer in the gas phase is strictly dissociative along a OH stretch coordinate but changes its nature when the stretched OH moiety is hydrogen bonded to a neighboring water molecule. This work extends previous exploration of the water dimer excited singlet potential-energy surface, using computational methods that are reliable even at geometries well removed from the ground-state equilibrium. First, the hydrogen-bonded OH moiety is stretched far enough to establish the existence of a barrier that is sufficient to support a quasibound vibrational state of the OH oscillator near the Franck-Condon region. Second, the constraint of an icelike structure is relaxed, and it is found that a substantial fraction of liquidlike structures also supports a quasibound vibrational state. These potential-energy explorations on stretching of the hydrogen-bonded OH moiety in a water dimer are discussed as a model for understanding the initial dynamics upon excitation into the lowest excited singlet state of condensed water. The possibility is raised that the excited-state lifetime may be long enough to allow for exciton migration, which would provide a mechanism for energy transport in condensed water phases. PMID:16460160
Valkunas, L; Trinkunas, G; Müller, M G; Holzwarth, A R
1999-01-01
The excited state mixing effect is taken into account considering the difference spectra of dimers. Both the degenerate (homo) dimer as well as the nondegenerate (hetero) dimer are considered. Due to the higher excited state mixing with the two-exciton states in the homodimer, the excited state absorption (or the difference spectrum) can be strongly affected in comparison with the results obtained in the Heitler-London approximation. The difference spectrum of the heterodimer is influenced by two resonance effects (i) mixing of the ground state optical transitions of both monomers in the dimer and (ii) mixing of the excited state absorption of the excited monomer with the ground state optical transition in the nonexcited monomer. These effects have been tested by simulating the difference absorption spectra of the light-harvesting complex of photosystem II (LHC II) experimentally obtained with the 60 fs excitation pulses at zero delay times and various excitation wavelengths. The pairs of coupled chlorophylls...
Lifetime measurement of excited low-spin states via the $(p,p^{\\prime}\\gamma$) reaction
Hennig, A; Mineva, M N; Petkov, P; Pickstone, S G; Spieker, M; Zilges, A
2015-01-01
In this article a method for lifetime measurements in the sub-picosecond regime via the Doppler-shift attenuation method (DSAM) following the inelastic proton scattering reaction is presented. In a pioneering experiment we extracted the lifetimes of 30 excited low-spin states of $^{96}$Ru, taking advantage of the coincident detection of scattered protons and de-exciting $\\gamma$-rays as well as the large number of particle and $\\gamma$-ray detectors provided by the SONIC@HORUS setup at the University of Cologne. The large amount of new experimental data shows that this technique is suited for the measurement of lifetimes of excited low-spin states, especially for isotopes with a low isotopic abundance, where $(n,n^{\\prime}\\gamma$) or - in case of investigating dipole excitations - ($\\gamma,\\gamma^{\\prime}$) experiments are not feasible due to the lack of sufficient isotopically enriched target material.
Coupled state analysis of electron excitations in asymmetric collision systems
Energy Technology Data Exchange (ETDEWEB)
Mehler, G.; Reus, T. de; Mueller, U.; Reinhardt, J.; Mueller, B.; Greiner, W.; Soff, G.
1985-11-01
A coupled channel formalism is presented, using relativistic basis states of the target atom. Screening effects are incorporated by means of an effective potential of the Hartree-Fock-Slater type. Relativistic wave packets are employed for the description of the continuum. The impact parameter dependence of the K-hole production in p-Ag collisions is calculated, including quadrupole contributions of the projectile Coulomb potential. The results are compared with experimental data. (orig.).
Coupled state analysis of electron excitations in asymmetric collision systems
International Nuclear Information System (INIS)
A coupled channel formalism is presented, using relativistic basis states of the target atom. Screening effects are incorporated by means of an effective potential of Hartree-Fock-Slater type. Relativistic wave packets are employed for the description of the continuum. The impact parameter dependence of the K-hole production in p-Ag collisions is calculated, including quadrupole contributions of the projectile Coulomb potential. The results are compared with experimental data. (orig.)
Separable interactions and excited states in open-shell nuclei
International Nuclear Information System (INIS)
The relevant matrix elements of the Hamiltonian for a RPA description of collective states in open-shell nuclei are determined. For separable interactions it is found necessary to include the particle-particle and particle-hole interactions simultaneously. The energy-weighted sum rule for the electromagnetic operator (with angular momentum I) is greatly reduced by the use of the pairing interaction with the same angular momentum. (author)
Quantum-chemical study of electronically excited states ofprotolytic forms of vanillic acid
Vusovich, O. V.; Tchaikovskaya, O. N.; I. V. Sokolova; Vasileva, N. Y.
2015-01-01
The paper describes an analysis of possible ways of deactivation of electronically excited states of 4-hydroxy- 3-methoxy-benzoic acid (vanillic acid) and its protolytic forms with the use of quantum-chemical methods INDO/S (intermediate neglect of differential overlap with a spectroscopic parameterization) and MEP (molecular electrostatic potential). The ratio of radiative and non-radiative deactivation channels of the electronic excitation energy is established. The rate constants of photop...
Jiménez-Hoyos, Carlos A; Scuseria, Gustavo E
2013-01-01
Recent work from our research group has demonstrated that symmetry-projected Hartree--Fock (HF) methods provide a compact representation of molecular ground state wavefunctions based on a superposition of non-orthogonal Slater determinants. The symmetry-projected ansatz can account for static correlations in a computationally efficient way. Here we present a variational extension of this methodology applicable to excited states of the same symmetry as the ground state. Benchmark calculations on the C$_2$ dimer with a modest basis set, which allows comparison with full configuration interaction results, indicate that this extension provides a high quality description of the low-lying spectrum for the entire dissociation profile. We apply the same methodology to obtain the full low-lying vertical excitation spectrum of formaldehyde, in good agreement with available theoretical and experimental data, as well as to a challenging model $C_{2v}$ insertion pathway for BeH$_2$. The variational excited state methodolo...
Vibronic resonances sustain excited state coherence in light harvesting proteins at room temperature
Novelli, Fabio; Roozbeh, Ashkan; Wilk, Krystyna E; Curmi, Paul M G; Davis, Jeffrey A
2015-01-01
Until recently it was believed that photosynthesis, a fundamental process for life on earth, could be fully understood with semi-classical models. However, puzzling quantum phenomena have been observed in several photosynthetic pigment-protein complexes, prompting questions regarding the nature and role of these effects. Recent attention has focused on discrete vibrational modes that are resonant or quasi-resonant with excitonic energy splittings and strongly coupled to these excitonic states. Here we report a series of experiments that unambiguously identify excited state coherent superpositions that dephase on the timescale of the excited state lifetime. Low energy (56 cm-1) oscillations on the signal intensity provide direct experimental evidence for the role of vibrational modes resonant with excitonic splittings in sustaining coherences involving different excited excitonic states at physiological temperature.
Photoemission from excited states in rare gas solids by combining synchrotronradiation with a laser
International Nuclear Information System (INIS)
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 hwSR=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 (hwL=1.9 - 3.7 eV). This experimental technique was applied to solid Xe, Kr, Ar and Ne. (orig./GSCH)
Negative-continuum dielectronic recombination into excited states of highly-charged ions
Artemyev, A. N.; Shabaev, V. M.; Stöhlker, Th; Surzhykov, A. S.
2009-01-01
The recombination of a free electron into a bound state of bare, heavy nucleus under simultaneous production of bound-electron--free-positron pair is studied within the framework of relativistic first--order perturbation theory. This process, denoted as "negative-continuum dielectronic recombination" leads to a formation of not only the ground but also the singly- and doubly-excited states of the residual helium-like ion. The contributions from such an excited--state capture to the total as w...
Autoionizing doubly-excited states of 3Σg− symmetry of H2
Directory of Open Access Journals (Sweden)
Argoubi F.
2015-01-01
Full Text Available We report R-matrix calculations of doubly-excited 3Σg− states of molecular hydrogen corresponding to 3d̃πnℓ̃π configurations. These states form Rydberg series converging to the 3d̃π series limit. They lie in the continuum of the doubly-excited states of 3Σg− symmetry built on the 2p̃π ion core, and therefore they are autoionized. Calculations of resonance positions and widths are presented.
Signature of triply excited Li-like V states in ion-solid collisions
Sharma, Gaurav; Haris, K.; Singh, G.; Kumar, B.; Karmakar, S.; Puri, N. K.; Mishra, Adya P.; Kumar, Pravin; Nandi, T.
2016-10-01
The transitions originating from triply excited, doubly autoionizing states of Li-like V formed in beam-foil experiments detected within a set of blended spectroscopic profiles have been assigned tentatively by the Hartree-Fock calculations including relativistic corrections and multi-configuration interactions as perturbations. The x-ray decay channels from the triply excited states such as 3p34S, 2p2 np4S (n ∼ 12) through radiative transitions to the ground state via two or more steps have been observed.
Directory of Open Access Journals (Sweden)
Chien-Hao Lin
2015-09-01
Full Text Available In the present work, we report an investigation on quantum entanglement in the doubly excited 2s2 1Se resonance state of the positronium negative ion by using highly correlated Hylleraas type wave functions, determined by calculation of the density of resonance states with the stabilization method. Once the resonance wave function is obtained, the spatial (electron-electron orbital entanglement entropies (von Neumann and linear can be quantified using the Schmidt decomposition method. Furthermore, Shannon entropy in position space, a measure for localization (or delocalization for such a doubly excited state, is also calculated.
Energy Technology Data Exchange (ETDEWEB)
Shin, Hee Won; Ocola, Esther J.; Laane, Jaan, E-mail: laane@mail.chem.tamu.edu [Department of Chemistry, Texas A and M University, College Station, Texas 77843-3255 (United States); Kim, Sunghwan [National Center for Biotechnology Information, National Library of Medicine, National Institutes of Health, Department of Health and Human Services, 8600 Rockville Pike, Bethesda, Maryland 20894 (United States)
2014-01-21
The fluorescence excitation spectra of jet-cooled benzocyclobutane have been recorded and together with its ultraviolet absorption spectra have been used to assign the vibrational frequencies for this molecule in its S{sub 1}(π,π{sup *}) electronic excited state. Theoretical calculations at the CASSCF(6,6)/aug-cc-pVTZ level of theory were carried out to compute the structure of the molecule in its excited state. The calculated structure was compared to that of the molecule in its electronic ground state as well as to the structures of related molecules in their S{sub 0} and S{sub 1}(π,π{sup *}) electronic states. In each case the decreased π bonding in the electronic excited states results in longer carbon-carbon bonds in the benzene ring. The skeletal vibrational frequencies in the electronic excited state were readily assigned and these were compared to the ground state and to the frequencies of five similar molecules. The vibrational levels in both S{sub 0} and S{sub 1}(π,π{sup *}) states were remarkably harmonic in contrast to the other bicyclic molecules. The decreases in the frequencies of the out-of-plane skeletal modes reflect the increased floppiness of these bicyclic molecules in their S{sub 1}(π,π{sup *}) excited state.
Zhu, Xi-Ming; Cheng, Zhi-Wen; Carbone, Emile; Pu, Yi-Kang; Czarnetzki, Uwe
2016-08-01
Electron-impact excitation processes play an important role in low-temperature plasma physics. Cross section and rate coefficient data for electron-impact processes from the ground state to excited states or between two excited states are required for both diagnostics and modeling works. However, the collisional processes between excited states are much less investigated than the ones involving the ground state due to various experimental challenges. Recently, a method for determining electron excitation rate coefficients between Ar excited states in afterglow plasmas was successfully implemented and further developed to obtain large sets of collisional data. This method combines diagnostics for electron temperature, electron density, and excited species densities and kinetic modeling of excited species, from which the electron excitation rate coefficients from one of the 1s states to the other 1s states or to one of 2p or 3p states are determined (states are in Paschen’s notation). This paper reviews the above method—namely the combined diagnostics and modeling in afterglow plasmas. The results from other important approaches, including electron-beam measurement of cross sections, laser pump-probe technique for measuring rate coefficients, and theoretical calculations by R-matrix and distorted-wave models are also discussed. From a comparative study of these results, a fitted mathematical expression of excitation rate coefficients is obtained for the electron temperature range of 1-5 eV, which can be used for the collisional-radiative modeling of low-temperature Ar plasmas. At last, we report the limitations in the present dataset and give some suggestions for future work in this area.
EXCITATION OF LOW-LYING STATES IN ND-144 BY MEANS OF (E,E') SCATTERING
PERRINO, R; BLASI, N; DELEO, R; HARAKEH, MN; DEJAGER, CW; MICHELETTI, S; MIEREMET, J; PIGNANELLI, M; PONOMAREV, VY; SANDOR, RKJ; DEVRIES, H
1993-01-01
The low-lying states of Nd-144 have been investigated up to an excitation energy of 3.1 MeV by means of high-resolution inelastic electron scattering. Transition charge densities have been extracted for natural-parity states. The experimental data have been compared with the predictions of the quasi
Determination of Leu Side-Chain Conformations in Excited Protein States by NMR Relaxation Dispersion
Hansen, D. Flemming; Neudecker, Philipp; Vallurupalli, Pramodh; Mulder, Frans A. A.; Kay, Lewis E.
2010-01-01
Fits of Carr-Purcell-Meiboom-Gill (CPMG) relaxation dispersion profiles allow extraction of the kinetics and thermodynamics of exchange reactions that interconvert highly populated, ground state and low Populated, excited state conformers. Structural information is also available in the form of chem
Excitation of exciton states on a curved surface
Silotia, Poonam; Prasad, Vinod
2016-05-01
Excitonic transitions on the surface of a sphere have been studied in he presence of external static electric and laser fields. The spectrum and the various coupling matrix elements, (for n = 1 , 2 , 3), between few states of exciton have been evaluated in the absence and presence of excitonic Coulombic interaction with different values of dielectric constant. Variation of various physical quantities: energy eigenvalues, transition probability, orientational and alignment parameter, has been shown to have strong dependence on the laser field and static electric field.
Polarization and dissociation of a high energy photon-excited state in conjugated polymers
Energy Technology Data Exchange (ETDEWEB)
Li, Xiao-xue, E-mail: sps_lixx@ujn.edu.cn
2015-02-20
We use the tight-binding Su–Schrieffer–Heeger model for the one-dimensional conjugated polymers to explore the static polarization behavior of a high energy photon-excited state under the electric field. An obvious reverse polarization is obtained although the electric field is weak. With the increase of field strength, the degree of polarization increases first and then decreases. When the electric field is strong enough, the excited state is dissociated into the polaron pair. In addition, the effects of electron–electron interaction and interchain coupling are also discussed. The results indicate that the electron–electron interaction could weaken the reverse polarization of the high energy photon-excited state, which tends to be dissociated into a high-energy exciton and a pair of solitons with the including of interchain coupling. - Highlights: • We explore the polarization of a high energy photon-excited state in polymers. • An obvious reverse polarization under the moderate electric field is obtained. • High energy photon-excited state is dissociated into polaron pair at strong field. • Increasing electron–electron interaction will weaken the reverse polarization. • Interchain coupling induces dissociation into high-energy exciton and solitons.
Production of excited beauty states in Z decays
Buskulic, Damir; De Bonis, I; Décamp, D; Ghez, P; Goy, C; Lees, J P; Lucotte, A; Minard, M N; Odier, P; Pietrzyk, B; Ariztizabal, F; Chmeissani, M; Crespo, J M; Efthymiopoulos, I; Fernández, E; Fernández-Bosman, M; Gaitan, V; Garrido, L; Martínez, M; Orteu, S; Pacheco, A; Padilla, C; Palla, Fabrizio; Pascual, A; Perlas, J A; Sánchez, F; Teubert, F; Colaleo, A; Creanza, D; De Palma, M; Farilla, A; Gelao, G; Girone, M; Iaselli, Giuseppe; Maggi, G; Maggi, M; Marinelli, N; Natali, S; Nuzzo, S; Ranieri, A; Raso, G; Romano, F; Ruggieri, F; Selvaggi, G; Silvestris, L; Tempesta, P; Zito, G; Huang, X; Lin, J; Ouyang, Q; Wang, T; Xie, Y; Xu, R; Xue, S; Zhang, J; Zhang, L; Zhao, W; Bonvicini, G; Cattaneo, M; Comas, P; Coyle, P; Drevermann, H; Engelhardt, A; Forty, Roger W; Frank, M; Hagelberg, R; Harvey, J; Jacobsen, R; Janot, P; Jost, B; Knobloch, J; Lehraus, Ivan; Markou, C; Martin, E B; Mato, P; Meinhard, H; Minten, Adolf G; Miquel, R; Oest, T; Palazzi, P; Pater, J R; Pusztaszeri, J F; Ranjard, F; Rensing, P E; Rolandi, Luigi; Schlatter, W D; Schmelling, M; Schneider, O; Tejessy, W; Tomalin, I R; Venturi, A; Wachsmuth, H W; Wiedenmann, W; Wildish, T; Witzeling, W; Wotschack, J; Ajaltouni, Ziad J; Bardadin-Otwinowska, Maria; Barrès, A; Boyer, C; Falvard, A; Gay, P; Guicheney, C; Henrard, P; Jousset, J; Michel, B; Monteil, S; Montret, J C; Pallin, D; Perret, P; Podlyski, F; Proriol, J; Rossignol, J M; Saadi, F; Fearnley, Tom; Hansen, J B; Hansen, J D; Hansen, J R; Hansen, P H; Nilsson, B S; Kyriakis, A; Simopoulou, Errietta; Siotis, I; Vayaki, Anna; Zachariadou, K; Blondel, A; Bonneaud, G R; Brient, J C; Bourdon, P; Passalacqua, L; Rougé, A; Rumpf, M; Tanaka, R; Valassi, Andrea; Verderi, M; Videau, H L; Candlin, D J; Parsons, M I; Focardi, E; Parrini, G; Corden, M; Delfino, M C; Georgiopoulos, C H; Jaffe, D E; Antonelli, A; Bencivenni, G; Bologna, G; Bossi, F; Campana, P; Capon, G; Chiarella, V; Felici, G; Laurelli, P; Mannocchi, G; Murtas, F; Murtas, G P; Pepé-Altarelli, M; Dorris, S J; Halley, A W; ten Have, I; Knowles, I G; Lynch, J G; Morton, W T; O'Shea, V; Raine, C; Reeves, P; Scarr, J M; Smith, K; Smith, M G; Thompson, A S; Thomson, F; Thorn, S; Turnbull, R M; Becker, U; Braun, O; Geweniger, C; Graefe, G; Hanke, P; Hepp, V; Kluge, E E; Putzer, A; Rensch, B; Schmidt, M; Sommer, J; Stenzel, H; Tittel, K; Werner, S; Wunsch, M; Beuselinck, R; Binnie, David M; Cameron, W; Colling, D J; Dornan, Peter J; Konstantinidis, N P; Moneta, L; Moutoussi, A; Nash, J; San Martin, G; Sedgbeer, J K; Stacey, A M; Dissertori, G; Girtler, P; Kneringer, E; Kuhn, D; Rudolph, G; Bowdery, C K; Brodbeck, T J; Colrain, P; Crawford, G; Finch, A J; Foster, F; Hughes, G; Sloan, Terence; Whelan, E P; Williams, M I; Galla, A; Greene, A M; Kleinknecht, K; Quast, G; Raab, J; Renk, B; Sander, H G; Wanke, R; Zeitnitz, C; Aubert, Jean-Jacques; Bencheikh, A M; Benchouk, C; Bonissent, A; Bujosa, G; Calvet, D; Carr, J; Diaconu, C A; Etienne, F; Thulasidas, M; Nicod, D; Payre, P; Rousseau, D; Talby, M; Abt, I; Assmann, R W; Bauer, C; Blum, Walter; Brown, D; Dietl, H; Dydak, Friedrich; Ganis, G; Gotzhein, C; Jakobs, K; Kroha, H; Lütjens, G; Lutz, Gerhard; Männer, W; Moser, H G; Richter, R H; Rosado-Schlosser, A; Schael, S; Settles, Ronald; Seywerd, H C J; Stierlin, U; Saint-Denis, R; Wolf, G; Alemany, R; Boucrot, J; Callot, O; Cordier, A; Courault, F; Davier, M; Duflot, L; Grivaz, J F; Heusse, P; Jacquet, M; Kim, D W; Le Diberder, F R; Lefrançois, J; Lutz, A M; Musolino, G; Nikolic, I A; Park, H J; Park, I C; Schune, M H; Simion, S; Veillet, J J; Videau, I; Abbaneo, D; Azzurri, P; Bagliesi, G; Batignani, G; Bettarini, S; Bozzi, C; Calderini, G; Carpinelli, M; Ciocci, M A; Ciulli, V; Dell'Orso, R; Fantechi, R; Ferrante, I; Foà, L; Forti, F; Giassi, A; Giorgi, M A; Gregorio, A; Ligabue, F; Lusiani, A; Marrocchesi, P S; Messineo, A; Rizzo, G; Sanguinetti, G; Sciabà, A; Spagnolo, P; Steinberger, Jack; Tenchini, Roberto; Tonelli, G; Triggiani, G; Vannini, C; Verdini, P G; Walsh, J; Betteridge, A P; Blair, G A; Bryant, L M; Cerutti, F; Gao, Y; Green, M G; Johnson, D L; Medcalf, T; Mir, L M; Perrodo, P; Strong, J A; Bertin, V; Botterill, David R; Clifft, R W; Edgecock, T R; Haywood, S; Edwards, M; Maley, P; Norton, P R; Thompson, J C; Bloch-Devaux, B; Colas, P; Duarte, H; Emery, S; Kozanecki, Witold; Lançon, E; Lemaire, M C; Locci, E; Marx, B; Pérez, P; Rander, J; Renardy, J F; Rossowsky, A; Roussarie, A; Schuller, J P; Schwindling, J; Si Mohand, D; Trabelsi, A; Vallage, B; Johnson, R P; Kim, H Y; Litke, A M; McNeil, M A; Taylor, G; Beddall, A; Booth, C N; Boswell, R; Cartwright, S L; Combley, F; Dawson, I; Köksal, A; Letho, M; Newton, W M; Rankin, C; Thompson, L F; Böhrer, A; Brandt, S; Cowan, G D; Feigl, E; Grupen, Claus; Lutters, G; Minguet-Rodríguez, J A; Rivera, F; Saraiva, P; Smolik, L; Van Gemmeren, P; Apollonio, M; Bosisio, L; Della Marina, R; Giannini, G; Gobbo, B; Ragusa, F; Rothberg, J E; Wasserbaech, S R; Armstrong, S R; Bellantoni, L; Elmer, P; Feng, Z; Ferguson, D P S; Gao, Y S; González, S; Grahl, J; Harton, J L; Hayes, O J; Hu, H; McNamara, P A; Nachtman, J M; Orejudos, W; Pan, Y B; Saadi, Y; Schmitt, M; Scott, I J; Sharma, V; Turk, J; Walsh, A M; Wu Sau Lan; Wu, X; Yamartino, J M; Zheng, M; Zobernig, G
1996-01-01
A data sample of about 3.0 million hadronic Z decays collected by the ALEPH experiment at LEP in the years 1991 through 1994, is used to make an inclusive selection of B~hadron events. In this event sample 4227 \\pm 140 \\pm 252 B^* mesons in the decay B^* \\to B \\gamma and 1944 \\pm 108 \\pm 161 B^{**} mesons decaying into a B~meson and a charged pion are reconstructed. For the well established B^* meson the following quantities areobtained: \\Delta M = M_{B^*} - M_{B} = (45.30\\pm 0.35\\pm 0.87)~\\mathrm{MeV}/c^2 and N_{B^*}/(N_B+N_{B^*}) = (77.1 \\pm 2.6 \\pm 7.0)\\%. The angular distribution of the photons in the B^* rest frame is used to measure the relative contribution of longitudinal B^* polarization states to be \\sigma_L/(\\sigma_L + \\sigma_T)= (33 \\pm 6 \\pm 5)\\%. \\\\ Resonance structure in the M(B\\pi)-M(B) mass difference is observed at (424 \\pm 4 \\pm 10)~\\mathrm{MeV}/c^2. Its shape and position is in agreement with the expectation for B^{**}_{u,d} states decaying into B_{u,d}^{(*)} \\pi^\\pm. The signal is therefo...
Bandyopadhyay, Subhajit; Roy, Saswata
2014-01-01
This paper describes an inexpensive experiment to determine the carbonyl stretching frequency of an organic keto compound in its ground state and first electronic excited state. The experiment is simple to execute, clarifies some of the fundamental concepts of spectroscopy, and is appropriate for a basic spectroscopy laboratory course. The…
Investigations into photo-excited state dynamics in colloidal quantum dots
Singh, Gaurav
Colloidal Quantum dots (QDs) have garnered considerable scientific and technological interest as a promising material for next generation solar cells, photo-detectors, lasers, bright light-emitting diodes (LEDs), and reliable biomarkers. However, for practical realization of these applications, it is crucial to understand the complex photo-physics of QDs that are very sensitive to surface chemistry and chemical surroundings. Depending on the excitation density, QDs can support single or multiple excitations. The first part of this talk addresses evolution of QD excited state dynamics in the regime of low excitation intensity. We use temperature-resolved time-resolved fluorescence spectroscopy to study exciton dynamics from picoseconds to microseconds and use kinetic modeling based on classical electron transfer to show the effect of surface trap states on dynamics of ground-state exciton manifold in core-shell CdSe/CdS QDs. We show that the thickness of CdS shell plays an important role in interaction of CdSe core exciton states with nanocrystal environment, and find that a thicker shell can minimize the mixing of QD exciton states with surface trap states. I will then present an investigation into the dynamics of multiply-excited states in QDs. One of the key challenges in QD spectroscopy is to reliably distinguish multi- from single-excited states that have similar lifetime components and spectroscopic signatures. I will describe the development of a novel multi-pulse fluorescence technique to selectively probe multi-excited states in ensemble QD samples and determine the nature of the multi-excited state contributing to the total fluorescence even in the limit of low fluorescent yields. We find that in our sample of CdSe/CdS core/shell QDs the multi-excited emission is dominated by emissive trion states rather than biexcitons. Next, I will discuss the application of this technique to probe exciton-plasmon coupling in layered hybrid films of QD/gold nanoparticles
Coherent secondary emission from resonantly excited two-exciton states
DEFF Research Database (Denmark)
Birkedal, Dan
2000-01-01
theories as e.g. the semiconductor Bloch equations, recent experimental and theoretical developments have demonstrated contributions to the third order nonlinear susceptibility from exciton-exciton correlations beyond the mean field approximation. Ultrafast transient four-wave mixing (TFWM)has been......The coherent interaction of light and the electronic states of semiconductors near the fundamental bandgap has been a very active topic of research since the advent of ultrafast lasers. While many of the ultrafast nonlinear properties of semiconductors have been well explained within mean field...... the experimental technique of choice to investigate these effects, and comparison of experiment and theory have so far been based on calculated TFWM line shapes. In this presentation a new experimental approach has been used to investigate directly the contribution from exciton-exciton correlations...
International Nuclear Information System (INIS)
Photo- or electro-excited states in polyatomic molecules, aggregates, and conjugated polymers are at the center of organic light-emitting diodes (OLEDs). These can decay radiatively or non-radiatively, determining the luminescence quantum efficiency of molecular materials. According to Kasha’s rule, light-emission is dictated by the lowest-lying excited state. For conjugated polymers, the electron correlation effect can lead the lowest-lying excited state to the even-parity 2Ag state which is non-emissive. To understand the nature of the low-lying excited state structure, we developed the density matrix renormalization group (DMRG) theory and its symmetrization scheme for quantum chemistry applied to calculate the excited states structure. We found there are three types of 1Bu/2Ag crossover behaviors: with electron correlation strength U, with bond length alternation, and with conjugation length. These directly influence the light-emitting property. For the electro-excitation, carriers (electron and hole) are injected independently, forming both singlet and triplet excited bound states with statistically 25% and 75% portions, respectively. We found that the exciton formation rate can depend on spin manifold, and for conjugated polymers, the singlet exciton can have larger formation rate leading to the internal electroluminescence quantum efficiency larger than the 25% spin statistical limit. It is originated from the interchain electron correlation as well as intrachain lattice relaxation. For the dipole allowed emissive state, the radiative decay process via either spontaneous emission or stimulated emission can be computed from electronic structure plus vibronic couplings. The challenging issue lies in the non-radiative decay via non-adiabatic coupling and/or spin–orbit coupling. We developed a unified correlation function formalism for the excited state radiative and non-radiative decay rates. We emphasized the low-frequency mode mixing (Duschinsky rotation
Hongqiang Xie; Guihua Li; Jinping Yao; Wei Chu; Ziting Li; Bin Zeng; Zhanshan Wang; Ya Cheng
2015-01-01
We report on generation of third harmonic from nitrogen molecules on the excited state with a weak driver laser pulse at a mid-infrared wavelength. The excited nitrogen molecules are generated using a circularly polarized intense femtosecond pulse which produces energetic electrons by photoionization to realize collisional excitation of nitrogen molecules. Furthermore, since the third harmonic is generated using a pump-probe scheme, it enables investigation of the excited-state dynamics of ni...
Institute of Scientific and Technical Information of China (English)
Yu-ling Chu; Zhong Yang; Zhe-feng Pan; Jing Liu; Yue-yi Han; Yong Ding; Peng Song
2012-01-01
Density functional theory and time-dependent density-functional theory have been used to investigate the photophysical properties and relaxation dynamics of dimethylaminobenzophenone (DMABP) and its hydrogen-bonded DMABP-MeOH dimer.It is found that,in nonpolar aprotic solvent,the transitions from S0 to S1 and S2 states of DMABP have both n→π* and π→π* characters,with the locally excited feature mainly located on the C=O group and the partial CT one characterized by electron transfer mainly from the dimethylaminophenyl group to the C=O group.But when the intermolecular hydrogen bond C=O…H-O is formed,the highly polar intramolecular charge transfer character switches over to the first excited state of DMABP-MeOH dimer and the energy difference between the two lowlying electronically excited states increases.To gain insight into the relaxation dynamics of DMABP and DMABP-MeOH dimer in the excited state,the potential energy curves for conformational relaxation are calculated.The formation of twisted intramolecular charge transfer state via diffusive twisting motion of the dimethylamino/dimethylaminophenyl groups is found to be the major relaxation process.In addition,the decay of the S1 state of DMABP-MeOH dimer to the ground state,through nonradiative intermolecular hydrogen bond stretching vibrations,is facilitated by the formation of the hydrogen bond between DMABP and alcohols.
International Nuclear Information System (INIS)
An experimental and theoretical study is performed of the angular photoelectron distribution for three-photon ionization of Ba atoms through the 2ω-excited intermediate state 6p2(1S0) and the auto-ionized state 6p8s(3P1). Rotation of the polarization plane of dye-laser radiation allowed us to investigate the photoelectron angular distribution. Electrons were counted with the help of a time-of-flight electron spectrometer. The density-matrix formalism is used to obtain expressions for the angular dependence of the differential ionization probability. Possible experiments are discussed
Avison, A; Fuller, G A; Caswell, J L; Green, J A; Breen, S L; Ellingsen, S P; Gray, M D; Pestalozzi, M; Thompson, M A; Voronkov, M A
2016-01-01
We present the results of the first complete unbaised survey of the Galactic Plane for 6035-MHz excited-state hydroxyl masers undertaken as part of the Methanol Multibeam Survey. These observations cover the Galactic longitude ranges $186^{\\circ}< l < 60^{\\circ}$ including the Galactic Centre. We report the detection of 127 excited-state hydroxyl masers within the survey region, 47 being new sources. The positions of new detections were determined from interferometric observations with the Australia Telescope Compact Array. We discuss the association of 6035-MHz masers in our survey with the 6668-MHz masers from the MMB Survey, finding 37 likely methanol-excited-state hydroxyl masers maser pairs with physical separations of <=0.03pc and 55 pairings separated by <=0.1pc. Using these we calculate for the first time an excited-state hydroxyl maser life time of between 3.3x10^3 and 8.3x10^3 years. We also discuss the variability of the 6035-MHz masers and detection rates of counterpart 6030-MHz excite...
Energy Technology Data Exchange (ETDEWEB)
Wilke, Josefin; Wilke, Martin; Schmitt, Michael, E-mail: mschmitt@uni-duesseldorf.de [Institut für Physikalische Chemie, Heinrich-Heine-Universität, D-40225 Düsseldorf (Germany); Meerts, W. Leo, E-mail: leo.meerts@science.ru.nl [Institute for Molecules and Materials, Radboud University, NL-6525 AS Nijmegen (Netherlands)
2016-01-28
The dipole moments of the ground and lowest electronically excited singlet state of 5-methoxyindole have been determined by means of optical Stark spectroscopy in a molecular beam. The resulting spectra arise from a superposition of different field configurations, one with the static electric field almost parallel to the polarization of the exciting laser radiation, the other nearly perpendicular. Each field configuration leads to different intensities in the rovibronic spectrum. With an automated evolutionary algorithm approach, the spectra can be fit and the ratio of both field configurations can be determined. A simultaneous fit of two spectra with both field configurations improved the precision of the dipole moment determination by a factor of two. We find a reduction of the absolute dipole moment from 1.59(3) D to 1.14(6) D upon electronic excitation to the lowest electronically excited singlet state. At the same time, the dipole moment orientation rotates by 54{sup ∘} showing the importance of the determination of the dipole moment components. The dipole moment in the electronic ground state can approximately be obtained from a vector addition of the indole and the methoxy group dipole moments. However, in the electronically excited state, vector addition completely fails to describe the observed dipole moment. Several reasons for this behavior are discussed.
Zhang, Wei; Zhao, Yong Sheng
2016-07-12
Nanophotonics have recently captured broad attention because of their great potential in information processing and communication, which may allow rates and bandwidth beyond what is feasible in the realm of electronics. Organic materials could be well suitable for such applications due to their ability to generate, transmit, modulate and detect light in their lightweight and flexible nanoarchitectures. Their distinct nanophotonic properties strongly depend on their extrinsic morphologies and intrinsic molecular excited-state processes. In this feature article, we mainly focus on a comprehensive understanding of the relationship between molecular excited-state processes and the advanced photonic functionalities of organic micro/nano-crystals in recent organic nanophotonic research, and then expect to provide enlightenment for the design and development of tiny photonic devices with broadband tunable properties by tailoring the excited-state processes of organic microcrystals. PMID:26883812
Li, Changwei; Yang, Kun; Feng, Yan; Su, Xinyan; Yang, Junyi; Jin, Xiao; Shui, Min; Wang, Yuxiao; Zhang, Xueru; Song, Yinglin; Xu, Hongyao
2009-12-01
Two-photon absorption induced excited state absorption in the solution of a new fluorenyl-based chromophore is investigated by a time-resolved pump-probe technique using femtosecond pulses. With the help of an additional femtosecond open-aperture Z-scan technique, numerical simulations based on a three-energy level model are used to interpret the experimental results, and we determine the nonlinear optical parameters of this new chromophore uniquely. Large two-photon absorption cross section and excited state absorption cross section for singlet excited state are obtained, indicating a good candidate for optical limiting devices. Moreover, the influence of two-beam coupling induced energy transfer in neat N,N'-dimethylformamide solvent is also considered, although this effect is strongly restrained by the instantaneous two-photon absorption. PMID:19894682
Institute of Scientific and Technical Information of China (English)
HONG Fang-Yu; XIONG Shi-Jie; FU Jing-Li; ZHU Zhi-Yan
2013-01-01
In the famous quantum communication scheme developed by Duan et al.[L.M.Duan,M.D.Lukin,J.L.Cirac,and P.Zoller,Nature (London) 414 (2001) 413],the probability of successful generating a symmetric collective atomic state with a single-photon emitted have to be far smaller than 1 to obtain an acceptable entangled state.Based on strong dipole-dipole interaction between two Rydberg atoms,two simultaneous excitations in an atomic ensemble are greatly suppressed,which makes it possible to excite a mesoscopic cold atomic ensemble into a near-ideal singly-excited symmetric collective state accompanied by a signal-photon with near unity success probability.
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
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...... that these capabilities will make our method a valuable tool for mapping in unprecedented detail the fundamental electronic excited-state dynamics that underpin many useful light-triggered molecular phenomena involving 3d transition metal complexes....
Excited state coherent dynamics in light-harvesting complexes from photosynthetic marine algae
Richards, G. H.; Wilk, K. E.; Curmi, P. M. G.; Quiney, H. M.; Davis, J. A.
2012-08-01
We explore coherence dynamics in light-harvesting complexes and their interactions with other electronic states and vibrational modes. This is achieved by utilizing a two-colour four-wave mixing spectroscopy to excite and analyse a specific coherence pathway in the phycocyanin-645 (PC645) light-harvesting complex. We observe the dephasing rate increase as a function of temperature and oscillations in the signal intensity as a function of waiting time which reveals coherent excitation of pathways not directly resonant with the laser pulses. This coherent excitation of non-resonant electronic states implies strong coupling to phonon modes, which is necessary if coherent energy transfer between non-resonant states is to play any role in photosynthetic energy transfer.
Excited state coherent dynamics in light-harvesting complexes from photosynthetic marine algae
International Nuclear Information System (INIS)
We explore coherence dynamics in light-harvesting complexes and their interactions with other electronic states and vibrational modes. This is achieved by utilizing a two-colour four-wave mixing spectroscopy to excite and analyse a specific coherence pathway in the phycocyanin-645 (PC645) light-harvesting complex. We observe the dephasing rate increase as a function of temperature and oscillations in the signal intensity as a function of waiting time which reveals coherent excitation of pathways not directly resonant with the laser pulses. This coherent excitation of non-resonant electronic states implies strong coupling to phonon modes, which is necessary if coherent energy transfer between non-resonant states is to play any role in photosynthetic energy transfer. (paper)
Precision Excited State Lifetime Measurements for Atomic Parity Violation and Atomic Clocks
Sell, Jerry; Patterson, Brian; Gearba, Alina; Snell, Jeremy; Knize, Randy
2016-05-01
Measurements of excited state atomic lifetimes provide a valuable test of atomic theory, allowing comparisons between experimental and theoretical transition dipole matrix elements. Such tests are important in Rb and Cs, where atomic parity violating experiments have been performed or proposed, and where atomic structure calculations are required to properly interpret the parity violating effect. In optical lattice clocks, precision lifetime measurements can aid in reducing the uncertainty of frequency shifts due to the surrounding blackbody radiation field. We will present our technique for precisely measuring excited state lifetimes which employs mode-locked ultrafast lasers interacting with two counter-propagating atomic beams. This method allows the timing in the experiment to be based on the inherent timing stability of mode-locked lasers, while counter-propagating atomic beams provides cancellation of systematic errors due to atomic motion to first order. Our current progress measuring Rb excited state lifetimes will be presented along with future planned measurements in Yb.
Zhang, Wei; Zhao, Yong Sheng
2016-07-12
Nanophotonics have recently captured broad attention because of their great potential in information processing and communication, which may allow rates and bandwidth beyond what is feasible in the realm of electronics. Organic materials could be well suitable for such applications due to their ability to generate, transmit, modulate and detect light in their lightweight and flexible nanoarchitectures. Their distinct nanophotonic properties strongly depend on their extrinsic morphologies and intrinsic molecular excited-state processes. In this feature article, we mainly focus on a comprehensive understanding of the relationship between molecular excited-state processes and the advanced photonic functionalities of organic micro/nano-crystals in recent organic nanophotonic research, and then expect to provide enlightenment for the design and development of tiny photonic devices with broadband tunable properties by tailoring the excited-state processes of organic microcrystals.
Electron energy-loss spectroscopy of excited states of the pyridine molecules
Linert, Ireneusz; Zubek, Mariusz
2016-04-01
Electron energy-loss spectra of the pyridine, C5H5N, molecules in the gas phase have been measured to investigate electronic excitation in the energy range 3.5-10 eV. The applied wide range of residual electron energy and the scattering angle range from 10° to 180° enabled to differentiate between optically-allowed and -forbidden transitions. These measurements have allowed vertical excitation energies of the triplet excited states of pyridine to be determined and tentative assignments of these states to be proposed. Some of these states have not been identified in the previous works. Contribution to the Topical Issue "Advances in Positron and Electron Scattering", edited by Paulo Limao-Vieira, Gustavo Garcia, E. Krishnakumar, James Sullivan, Hajime Tanuma and Zoran Petrovic.
Excited states in the doubly closed shell nucleus $^{132}_{50}Sn_{82}$
Bjørnstad, T; Ewan, G T; Jonson, B; Kawade, K; Kérek, A; Mattsson, S; Sistemich, K
1982-01-01
New excited states in the nucleus /sup 1/ /sup 32/Sn have been identified from gamma gamma coincidence measurements. Strong beta feeding to a state at 7.210 keV was established. This level is interpreted as a 6^{-} state formed after a\\pig/sup -1//sub 9/2/ to nu g/sup -1//sub 7/2/GT beta ^{-} transition from the 7^{-} ground state of /sup 132/In. The deexcitation of the 7210 keV state passes through a 4351 keV state, providing support for a 3^{-} assignment of this level.
Even-parity states of the Sm atom with stepwise excitation
Institute of Scientific and Technical Information of China (English)
Li Ming; Dai Chang-Jian; Xie Jun
2011-01-01
Two-colour stepwise excitation and photoionization schemes are adopted to study the spectra of high-lying states of the Sm atom. These bound even-parity states are excited with three different excitation paths from the 4f66s6p7DJ (J = 1, 2, 3) intermediate states, respectively. They are probed by photoionization process with an extra photon driving them to the continuum states. In this experiment, 270 states are detected in an energy range from 36160 cm-1 to 42250 cm-1, 109 of which are newly discovered, while the rest of them are confirmed to be the energy levels reported previously. Furthermore, based on the J-momentum selection rules of three excitation paths, a unique assignment of J-momentum for all observed states is determined, eliminating all remaining ambiguities in the literature. Finally, 53 single-colour transitions originating from the scanning laser are also identified. For all the relevant transitions, the information about their relative intensities is also given in the paper.
Energy Technology Data Exchange (ETDEWEB)
Dupuy, Nicolas, E-mail: nicolas.dupuy@impmc.upmc.fr [Institut de Minéralogie, de Physique des Matériaux et de Cosmochimie, Université Pierre et Marie Curie, case 115, 4 place Jussieu, 75252 Paris Cedex 05 (France); Bouaouli, Samira, E-mail: samira.bouaouli@lct.jussieu.fr [Laboratoire de Chimie Théorique, Université Pierre et Marie Curie, case 115, 4 place Jussieu, 75252 Paris Cedex 05 (France); Mauri, Francesco, E-mail: francesco.mauri@impmc.upmc.fr; Casula, Michele, E-mail: michele.casula@impmc.upmc.fr [CNRS and Institut de Minéralogie, de Physique des Matériaux et de Cosmochimie, Université Pierre et Marie Curie, case 115, 4 place Jussieu, 75252 Paris Cedex 05 (France); Sorella, Sandro, E-mail: sorella@sissa.it [International School for Advanced Studies (SISSA), Via Beirut 2-4, 34014 Trieste, Italy and INFM Democritos National Simulation Center, Trieste (Italy)
2015-06-07
We study the ionization energy, electron affinity, and the π → π{sup ∗} ({sup 1}L{sub a}) excitation energy of the anthracene molecule, by means of variational quantum Monte Carlo (QMC) methods based on a Jastrow correlated antisymmetrized geminal power (JAGP) wave function, developed on molecular orbitals (MOs). The MO-based JAGP ansatz allows one to rigorously treat electron transitions, such as the HOMO → LUMO one, which underlies the {sup 1}L{sub a} excited state. We present a QMC optimization scheme able to preserve the rank of the antisymmetrized geminal power matrix, thanks to a constrained minimization with projectors built upon symmetry selected MOs. We show that this approach leads to stable energy minimization and geometry relaxation of both ground and excited states, performed consistently within the correlated QMC framework. Geometry optimization of excited states is needed to make a reliable and direct comparison with experimental adiabatic excitation energies. This is particularly important in π-conjugated and polycyclic aromatic hydrocarbons, where there is a strong interplay between low-lying energy excitations and structural modifications, playing a functional role in many photochemical processes. Anthracene is an ideal benchmark to test these effects. Its geometry relaxation energies upon electron excitation are of up to 0.3 eV in the neutral {sup 1}L{sub a} excited state, while they are of the order of 0.1 eV in electron addition and removal processes. Significant modifications of the ground state bond length alternation are revealed in the QMC excited state geometry optimizations. Our QMC study yields benchmark results for both geometries and energies, with values below chemical accuracy if compared to experiments, once zero point energy effects are taken into account.
Dupuy, Nicolas; Bouaouli, Samira; Mauri, Francesco; Sorella, Sandro; Casula, Michele
2015-06-01
We study the ionization energy, electron affinity, and the π → π∗ (1La) excitation energy of the anthracene molecule, by means of variational quantum Monte Carlo (QMC) methods based on a Jastrow correlated antisymmetrized geminal power (JAGP) wave function, developed on molecular orbitals (MOs). The MO-based JAGP ansatz allows one to rigorously treat electron transitions, such as the HOMO → LUMO one, which underlies the 1La excited state. We present a QMC optimization scheme able to preserve the rank of the antisymmetrized geminal power matrix, thanks to a constrained minimization with projectors built upon symmetry selected MOs. We show that this approach leads to stable energy minimization and geometry relaxation of both ground and excited states, performed consistently within the correlated QMC framework. Geometry optimization of excited states is needed to make a reliable and direct comparison with experimental adiabatic excitation energies. This is particularly important in π-conjugated and polycyclic aromatic hydrocarbons, where there is a strong interplay between low-lying energy excitations and structural modifications, playing a functional role in many photochemical processes. Anthracene is an ideal benchmark to test these effects. Its geometry relaxation energies upon electron excitation are of up to 0.3 eV in the neutral 1La excited state, while they are of the order of 0.1 eV in electron addition and removal processes. Significant modifications of the ground state bond length alternation are revealed in the QMC excited state geometry optimizations. Our QMC study yields benchmark results for both geometries and energies, with values below chemical accuracy if compared to experiments, once zero point energy effects are taken into account.
Higashi, Yoichi; Nagai, Yuki; Yoshida, Tomohiro; Kato, Masaru; Yanase, Youichi
2016-01-01
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 exceed the critical value.
Hot-electron-mediated desorption rates calculated from excited-state potential energy surfaces
DEFF Research Database (Denmark)
Olsen, Thomas; Gavnholt, Jeppe; Schiøtz, Jakob
2009-01-01
We present a model for desorption induced by (multiple) electronic transitions [DIET (DIMET)] based on potential energy surfaces calculated with the delta self-consistent field extension of density-functional theory. We calculate potential energy surfaces of CO and NO molecules adsorbed on various...... transition-metal surfaces and show that classical nuclear dynamics does not suffice for propagation in the excited state. We present a simple Hamiltonian describing the system with parameters obtained from the excited-state potential energy surface and show that this model can describe desorption dynamics...
Charge sensing of excited states in an isolated double quantum dot
DEFF Research Database (Denmark)
C. Johnson, A.; M. Marcus, C.; P. Hanson, M.;
2005-01-01
Pulsed electrostatic gating combined with capacitive charge sensing is used to perform excited state spectroscopy of an electrically isolated double-quantum-dot system. The tunneling rate of a single charge moving between the two dots is affected by the alignment of quantized energy levels......; measured tunneling probabilities thereby reveal spectral features. Two pulse sequences are investigated, one of which, termed latched detection, allows measurement of a single tunneling event without repetition. Both provide excited-state spectroscopy without electrical contact to the double-dot system....
Electronic properties of excited states in single InAs quantum dots
International Nuclear Information System (INIS)
The application of quantum-mechanical effects in semiconductor nanostructures enables the realization of novel opto-electronic devices. Examples are given by single-photon emitters and emitters of entangled photon pairs, both being essential for quantum cryptography, or for qubit systems as needed for quantum computing. InAs/GaAs quantum dots are one of the most promising candidates for such applications. A detailed knowledge of the electronic properties of quantum dots is a prerequisite for this development. The aim of this work is an experimental access to the detailed electronic structure of the excited states in single InAs/GaAs quantum dots including few-particle effects and in particular exchange interaction. The experimental approach is micro photoluminescence excitation spectroscopy (μPLE). One of the main difficulties using μPLE to probe single QDs is the unambiguous assignment of the observed resonances in the spectrum to specific transitions. By comparing micro photoluminescence (μPL) and μPLE spectra, the identification of the main resonances becomes possible. The key is given by the fine structure of the hot trion. Excitation spectroscopy on single charged QDs enables for the first time the complete observation of a non-trivial fine structure of an excitonic complex in a QD, the hot trion. Modelling based on eight-band k.p theory in combination with a configuration interaction scheme is in excellent agreement. Therewith the simulation also enables realistic predictions on the fine structure of the ground-state exciton which is of large importance for single quantum dot devices. Theory concludes from the observed transitions that the structural symmetry of the QDs is broken. Micro photoluminescence excitation spectroscopy combined with resonantly excited micro photoluminescence enables an optical access to the single particle states of the hole without the influence of few-particle coulomb interactions. Based on this knowledge the exciton binding
Quantum entanglement for two electrons in the excited states of helium-like systems
Lin, Yen-Chang; Ho, Yew Kam
2013-01-01
The quantum entanglement for the two electrons in the excited states of the helium-like atom/ions is investigated using the two-electron wave functions constructed by the B-spline basis. As a measure of the spatial (electron-electron orbital) entanglement, the von Neumann entropy and linear entropy of the reduced density matrix are calculated for the 1s2s 1,3S excited states for systems with some selected Z values from Z=2 to Z=100. Results for the helium atom are compared with other availabl...
Ou, Qi; Fatehi, Shervin; Alguire, Ethan; Shao, Yihan; Subotnik, Joseph E.
2014-07-01
Working within the Tamm-Dancoff approximation, we calculate the derivative couplings between time-dependent density-functional theory excited states by assuming that the Kohn-Sham superposition of singly excited determinants represents a true electronic wavefunction. All Pulay terms are included in our derivative coupling expression. The reasonability of our approach can be established by noting that, for closely separated electronic states in the infinite basis limit, our final expression agrees exactly with the Chernyak-Mukamel expression (with transition densities from response theory). Finally, we also validate our approach empirically by analyzing the behavior of the derivative couplings around the {T}1/{T}2 conical intersection of benzaldehyde.
Effects of Heavy Elements and Excited States in the Equation of State of the Solar Interior
Gong, Zhigang; Däppen, Werner; Nayfonov, Alan
2001-12-01
Although 98% of the solar material consists of hydrogen and helium, the remaining chemical elements contribute in a discernible way to the thermodynamic quantities. An adequate treatment of the heavy elements and their excited states is important for solar models that are subject to the stringent requirements of helioseismology. The contribution of various heavy elements in a set of thermodynamic quantities has been examined. Characteristic features that can trace individual heavy elements in the adiabatic exponent γ1=(∂lnp/∂lnϱ)s (s being specific entropy), and hence in the adiabatic sound speed, were searched. It has emerged that prominent signatures of individual elements exist and that these effects are greatest in the ionization zones, typically located near the bottom of the convection zone. The main result is that part of the features found here depend strongly on both the given species (atom or ion) and its detailed internal partition function, whereas other features only depend on the presence of the species itself, not on details such as the internal partition function. The latter features are obviously well suited for a helioseismic abundance determination, while the former features present a unique opportunity to use the Sun as a laboratory to test the validity of physical theories of partial ionization in a relatively dense and hot plasma. This domain of plasma physics has so far no competition from terrestrial laboratories. Another, quite general, finding of this work is that the inclusion of a relatively large number of heavy elements has a tendency to smear out individual features. This affects both the features that determine the abundance of elements and the ones that identify physical effects. This property alleviates the task of solar modelers because it helps to construct a good working equation of state that is relatively free of the uncertainties from basic physics. By the same token, it makes more difficult the reverse task, which is
Variation of Excited-State Dynamics in Trifluoromethyl Functionalized C60 Fullerenes
Energy Technology Data Exchange (ETDEWEB)
Park, Jaehong; Ramirez, Jessica J.; Clikeman, Tyler T.; Larson, Bryon W.; Boltalina, Olga V.; Strauss, Steven H.; Rumbles, Garry
2016-09-07
We report on electronically excited-state dynamics of three different trifluoromethyl C60 fullerenes (TMFs, C60(CF3)n: C60/4-1, C60/6-2, and C60/10-1, featuring four, six, and ten trifluoromethyl groups, respectively) using steady-state and time-resolved optical spectroscopy as well as ultrafast pump/probe transient absorption spectroscopy. C60/4-1 and C60/6-2 dissolved in toluene solvent show near-unity S1--T1 intersystem crossing quantum yield (..phi..ISC), ca. 1 ns S1-state lifetimes, and microsecond-timescale T1-state lifetimes, which are typical of the fullerene class. On the other hand, C60/10-1 exhibits a dominant sub-nanosecond nonradiative S1--S0 relaxation mechanism and negligible ..phi..ISC, therefore decreasing the average excited-state lifetime (..tau..avg) by about 5 orders of magnitude compared to that of C60/4-1 and C60/6-2 (..tau..avg approx. 17 us and 54 us for C60/4-1 and C60/6-2, respectively, whereas ..tau..avg approx. 100 ps for C60/10-1). These excited-state characteristics of C60/4-1 and C60/6-2 are preserved in polymer matrix, suggesting that fullerene/polymer interactions do not modulate intrinsic photophysics of trifluoromethyl-substituted fullerenes. The contrasting excited- state study results of C60/4-1 and C60/6-2 to that of C60/10-1 infer that intrinsic optical properties and excited-state dynamics can be affected by the substitution on the fullerene.
Variation of excited-state dynamics in trifluoromethyl functionalized C60 fullerenes.
Park, Jaehong; Ramirez, Jessica J; Clikeman, Tyler T; Larson, Bryon W; Boltalina, Olga V; Strauss, Steven H; Rumbles, Garry
2016-08-17
We report on electronically excited-state dynamics of three different trifluoromethyl C60 fullerenes (TMFs, C60(CF3)n: C60/4-1, C60/6-2, and C60/10-1, featuring four, six, and ten trifluoromethyl groups, respectively) using steady-state and time-resolved optical spectroscopy as well as ultrafast pump/probe transient absorption spectroscopy. C60/4-1 and C60/6-2 dissolved in toluene solvent show near-unity S1 → T1 intersystem crossing quantum yield (ΦISC), ca. 1 ns S1-state lifetimes, and microsecond-timescale T1-state lifetimes, which are typical of the fullerene class. On the other hand, C60/10-1 exhibits a dominant sub-nanosecond nonradiative S1 → S0 relaxation mechanism and negligible ΦISC, therefore decreasing the average excited-state lifetime (τavg) by about 5 orders of magnitude compared to that of C60/4-1 and C60/6-2 (τavg ≈ 17 μs and 54 μs for C60/4-1 and C60/6-2, respectively, whereas τavg ≈ 100 ps for C60/10-1). These excited-state characteristics of C60/4-1 and C60/6-2 are preserved in polymer matrix, suggesting that fullerene/polymer interactions do not modulate intrinsic photophysics of trifluoromethyl-substituted fullerenes. The contrasting excited-state study results of C60/4-1 and C60/6-2 to that of C60/10-1 infer that intrinsic optical properties and excited-state dynamics can be affected by the substitution on the fullerene. PMID:27485768
DEFF Research Database (Denmark)
Wallace-Williams, Stacie E.; Møller, Søren; Goldbeck, Robert A.;
1993-01-01
with the wavelength independence observed for the excited singlet-state absorption and fluorescence emission spectra of 1,5-diphenyl-2,3,4,6,7,8- hexahydronaphthalene and for the fluorescence emission spectra of 1,4diphenyl-1,3-cyclopentadiene, s-trans and s-cis structural analogs of DPB, respectively. The spectral...... changes in DPB can be explained in terms of an excitation wavelength-dependent production of s-cis and s-trans rotamer populations in the excited state. The DPB fluorescence emission spectrum was resolved into s-cis and s-trans components. The vibronic structure of the s-cis fluorescence spectrum...
Bacalis, Naoum C
2016-01-01
The computation of small concise and comprehensible excited state wave functions is needed because many electronic processes occur in excited states. But since the excited energies are saddle points in the Hilbert space of wave functions, the standard computational methods, based on orthogonality to lower lying approximants, resort to huge and incomprehensible wave functions, otherwise, the truncated wave function is veered away from the exact. The presented variational principle for excited states, Fn, is demonstrated to lead to the correct excited eigenfunction in necessarily small truncated spaces. Using Hylleraas coordinates for He 1S 1s2s, the standard method based on the theorem of Hylleraas - Unheim, and MacDonald, yields misleading main orbitals 1s1s' and needs a series expansion of 27 terms to be corrected, whereas minimizing Fn goes directly to the corect main orbitals, 1s2s, and can be adequately improved by 8 terms. Fn uses crude, rather inaccurate, lower lying approximants and does not need ortho...
Ramsey interferometry for resonant Auger decay through core-excited states
Chatterjee, Souvik; Nakajima, Takashi
2016-08-01
We theoretically investigate the electron dynamics in Ne atoms involving core-excited states through the Ramsey scheme with a pair of time-delayed x-ray pulses. Irradiation of Ne atoms by the ˜1 femtosecond x-ray pulse simultaneously populates two core-excited states, and an identical but time-delayed x-ray pulse probes the dynamics of the core-excited electron wave packet which is subject to the resonant Auger decay. The energy-integrated total Auger electron yield and energy-resolved Auger electron spectra in the time domain show periodic structures due to the temporal evolution of the wave packet, from which we can obtain the counterpart in the frequency domain through the Fourier transformation. The Auger electron energy spectra in the time as well as frequency domains show the interference patterns between the two Auger electron wave packets released into the continuum from the superposition of two core-excited states at different times. These spectra are important to clarify the individual contribution of the different Auger decay channels upon core excitation by the x-ray pulse.
Kreitner, Christoph; Heinze, Katja
2016-09-21
Deactivation pathways of the triplet metal-to-ligand charge transfer ((3)MLCT) excited state of cyclometalated polypyridine ruthenium complexes with [RuN5C](+) coordination are discussed on the basis of the available experimental data and a series of density functional theory calculations. Three different complex classes are considered, namely with [Ru(N^N)2(N^C)](+), [Ru(N^N^N)(N^C^N)](+) and [Ru(N^N^N)(N^N^C)](+) coordination modes. Excited state deactivation in these complex types proceeds via five distinct decay channels. Vibronic coupling of the (3)MLCT state to high-energy oscillators of the singlet ground state ((1)GS) allows tunneling to the ground state followed by vibrational relaxation (path A). A ligand field excited state ((3)MC) is thermally accessible via a (3)MLCT →(3)MC transition state with the (3)MC state being strongly coupled to the (1)GS surface via a low-energy minimum energy crossing point (path B). Furthermore, a (3)MLCT →(1)GS surface crossing point directly couples the triplet and singlet potential energy surfaces (path C). Charge transfer states either with higher singlet character or with different orbital parentage and intrinsic symmetry restrictions are thermally populated which promote non-radiative decay via tunneling to the (1)GS state (path D). Finally, the excited state can decay via phosphorescence (path E). The dominant deactivation pathways differ for the three individual complex classes. The implications of these findings for isoelectronic iridium(iii) or iron(ii) complexes are discussed. Ultimately, strategies for optimizing the emission efficiencies of cyclometalated polypyridine complexes of d(6)-metal ions, especially Ru(II), are suggested.
Extended Eckart Theorem and New Variation Method for Excited States of Atoms
Xiong, Zhuang; Bacalis, N C; Zhou, Qin
2016-01-01
We extend the Eckart theorem, from the ground state to excited statew, which introduces an energy augmentation to the variation criterion for excited states. It is shown that the energy of a very good excited state trial function can be slightly lower than the exact eigenvalue. Further, the energy calculated by the trial excited state wave function, which is the closest to the exact eigenstate through Gram-Schmidt orthonormalization to a ground state approximant, is lower than the exact eigenvalue as well. In order to avoid the variation restrictions inherent in the upper bound variation theory based on Hylleraas, Undheim, and McDonald [HUM] and Eckart Theorem, we have proposed a new variation functional Omega-n and proved that it has a local minimum at the eigenstates, which allows approaching the eigenstate unlimitedly by variation of the trial wave function. As an example, we calculated the energy and the radial expectation values of Triplet-S(even) Helium atom by the new variation functional, and by HUM a...
Carbon nanorings with inserted acenes: breaking symmetry in excited state dynamics.
Franklin-Mergarejo, R; Alvarez, D Ondarse; Tretiak, S; Fernandez-Alberti, S
2016-01-01
Conjugated cycloparaphenylene rings have unique electronic properties being the smallest segments of carbon nanotubes. Their conjugated backbones support delocalized electronic excitations, which dynamics is strongly influenced by cyclic geometry. Here we present a comparative theoretical study of the electronic and vibrational energy relaxation and redistribution in photoexcited cycloparaphenylene carbon nanorings with inserted naphthalene, anthracene, and tetracene units using non-adiabatic excited-state molecular dynamics simulations. Calculated excited state structures reflect modifications of optical selection rules and appearance of low-energy electronic states localized on the acenes due to gradual departure from a perfect circular symmetry. After photoexcitation, an ultrafast electronic energy relaxation to the lowest excited state is observed on the time scale of hundreds of femtoseconds in all molecules studied. Concomitantly, the efficiency of the exciton trapping in the acene raises when moving from naphthalene to anthracene and to tetracene, being negligible in naphthalene, and ~60% and 70% in anthracene and tetracene within the first 500 fs after photoexcitation. Observed photoinduced dynamics is further analyzed in details using induced molecular distortions, delocatization properties of participating electronic states and non-adiabatic coupling strengths. Our results provide a number of insights into design of cyclic molecular systems for electronic and light-harvesting applications. PMID:27507429
Excited State Structural Dynamics of Carotenoids and ChargeTransfer Systems
Energy Technology Data Exchange (ETDEWEB)
Van Tassle, Aaron Justin [Univ. of California, Berkeley, CA (United States)
2006-01-01
This dissertation describes the development andimplementation of a visible/near infrared pump/mid-infrared probeapparatus. Chapter 1 describes the background and motivation ofinvestigating optically induced structural dynamics, paying specificattention to solvation and the excitation selection rules of highlysymmetric molecules such as carotenoids. Chapter 2 describes thedevelopment and construction of the experimental apparatus usedthroughout the remainder of this dissertation. Chapter 3 will discuss theinvestigation of DCM, a laser dye with a fluorescence signal resultingfrom a charge transfer state. By studying the dynamics of DCM and of itsmethyl deuterated isotopomer (an otherwise identical molecule), we areable to investigate the origins of the charge transfer state and provideevidence that it is of the controversial twisted intramolecular (TICT)type. Chapter 4 introduces the use of two-photon excitation to the S1state, combined with one-photon excitation to the S2 state of thecarotenoid beta-apo-8'-carotenal. These 2 investigations show evidencefor the formation of solitons, previously unobserved in molecular systemsand found only in conducting polymers Chapter 5 presents an investigationof the excited state dynamics of peridinin, the carotenoid responsiblefor the light harvesting of dinoflagellates. This investigation allowsfor a more detailed understanding of the importance of structuraldynamics of carotenoids in light harvesting.
Directory of Open Access Journals (Sweden)
Marco Lamperti
2014-08-01
Full Text Available Cyclovalone is a synthetic curcumin derivative in which the keto-enolic system is replaced by a cyclohexanone ring. This modification of the chemical structure might in principle result in an excited state that is more stable than that of curcumin, which in turn should produce an enhanced phototoxicity. Indeed, although curcumin exhibits photosensitized antibacterial activity, this compound is characterized by very fast excited-state dynamics which limit its efficacy as a photosensitizer. In previous works we showed that the main non-radiative decay pathway of keto-enolic curcuminoids is through excited-state transfer of the enolic proton to the keto-oxygen. Another effective deactivation pathway involves an intermolecular charge transfer mechanism occurring at the phenyl rings, made possible by intramolecular H-bonding between the methoxy and the hydroxyl substituent. In this paper we present UV-Vis and IR absorption spectra data with the aim of elucidating the intramolecular charge distribution of this compound and its solvation patterns in different environments, with particular focus on solute-solvent H-bonding features. Moreover, we discuss steady state and time-resolved fluorescence data that aim at characterizing the excited-state dynamics of cyclovalone, and we compare its decay photophysics to that of curcumin. Finally, because during the characterization procedures we found evidence of very fast photodegradation of cyclovalone, its photostability in four organic solvents was studied by HPLC and the corresponding relative degradation rates were calculated.
The structure of low-lying states in ${}^{140}$Sm studied by Coulomb excitation
Klintefjord, M; Görgen, A; Bauer, C; Garrote, F L Bello; 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
2016-01-01
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...
Excited State Structural Dynamics of Carotenoids and ChargeTransfer Systems
Energy Technology Data Exchange (ETDEWEB)
Van Tassle, Aaron Justin
2006-09-01
This dissertation describes the development andimplementation of a visible/near infrared pump/mid-infrared probeapparatus. Chapter 1 describes the background and motivation ofinvestigating optically induced structural dynamics, paying specificattention to solvation and the excitation selection rules of highlysymmetric molecules such as carotenoids. Chapter 2 describes thedevelopment and construction of the experimental apparatus usedthroughout the remainder of this dissertation. Chapter 3 will discuss theinvestigation of DCM, a laser dye with a fluorescence signal resultingfrom a charge transfer state. By studying the dynamics of DCM and of itsmethyl deuterated isotopomer (an otherwise identical molecule), we areable to investigate the origins of the charge transfer state and provideevidence that it is of the controversial twisted intramolecular (TICT)type. Chapter 4 introduces the use of two-photon excitation to the S1state, combined with one-photon excitation to the S2 state of thecarotenoid beta-apo-8'-carotenal. These 2 investigations show evidencefor the formation of solitons, previously unobserved in molecular systemsand found only in conducting polymers Chapter 5 presents an investigationof the excited state dynamics of peridinin, the carotenoid responsiblefor the light harvesting of dinoflagellates. This investigation allowsfor a more detailed understanding of the importance of structuraldynamics of carotenoids in light harvesting.
Structure of low-lying states in 140Sm studied by Coulomb excitation
Klintefjord, M.; Hadyńska-KlÈ©k, K.; 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.
2016-05-01
The electromagnetic structure of 140Sm 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 multistep 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 21+ 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 140Sm shows considerable γ 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 collectivity in this mass region.
Analytical derivative techniques for TDDFT excited-state properties：Theory and application
Institute of Scientific and Technical Information of China (English)
CHEN DanPing; LIU Jie; MA HuiLi; ZENG Qiao; LIANG WanZhen
2014-01-01
We review our recent work on the methodology development of the excited-state properties for the molecules in vacuum and liquid solution.The general algorithms of analytical energy derivatives for the specific properties such as the first and second geometrical derivatives and IR/Raman intensities are demonstrated in the framework of the time-dependent density functional theory（TDDFT）.The performance of the analytical approaches on the calculation of excited-state energy Hessian has also been shown.It is found that the analytical approaches are superior to the finite-difference method on the computational accuracy and efficiency.The computational cost for a TDDFT excited-state Hessian calculation is only 2–3 times as that for the DFT ground-state Hessian calculation.With the low computational complexity of the developed analytical approaches,it becomes feasible to realize the large-scale numerical calculations on the excited-state vibrational frequencies,vibrational spectroscopies and the electronic-structure parameters which enter the spectrum calculations of electronic absorption and emission,and resonance Raman spectroscopies for medium-to large-sized systems.
Carbon nanorings with inserted acenes: breaking symmetry in excited state dynamics
Franklin-Mergarejo, R.; Alvarez, D. Ondarse; Tretiak, S.; Fernandez-Alberti, S.
2016-08-01
Conjugated cycloparaphenylene rings have unique electronic properties being the smallest segments of carbon nanotubes. Their conjugated backbones support delocalized electronic excitations, which dynamics is strongly influenced by cyclic geometry. Here we present a comparative theoretical study of the electronic and vibrational energy relaxation and redistribution in photoexcited cycloparaphenylene carbon nanorings with inserted naphthalene, anthracene, and tetracene units using non-adiabatic excited-state molecular dynamics simulations. Calculated excited state structures reflect modifications of optical selection rules and appearance of low-energy electronic states localized on the acenes due to gradual departure from a perfect circular symmetry. After photoexcitation, an ultrafast electronic energy relaxation to the lowest excited state is observed on the time scale of hundreds of femtoseconds in all molecules studied. Concomitantly, the efficiency of the exciton trapping in the acene raises when moving from naphthalene to anthracene and to tetracene, being negligible in naphthalene, and ~60% and 70% in anthracene and tetracene within the first 500 fs after photoexcitation. Observed photoinduced dynamics is further analyzed in details using induced molecular distortions, delocatization properties of participating electronic states and non-adiabatic coupling strengths. Our results provide a number of insights into design of cyclic molecular systems for electronic and light-harvesting applications.
Excited-state dynamics in light-harvesting complex of Rhodobacter sphaeroides
Institute of Scientific and Technical Information of China (English)
LIU KangJun; LIU WeiMin; YAN YongLi; DONG ZhiWei; XU ChunHe; QIAN ShiXiong
2008-01-01
Photodynamics of peripheral antenna complexes, light-harvesting complex (LH2) of Rhodobacter (Rb) Sphaeroides 601, was studied using femtosecond pump-probe technique at different laser wavelengths. The obtained results reveal dramatic dynamical evolutions within B800 and B850 absorption bands of antenna complexes LH2. At excitation wavelength around 835 nm, a sharp photobleaching signal was observed which was assigned to the contribution of the two-exciton state, which was further confirmed by the power dependence measurement. Rate equations with eight-level scheme were used to calculate the population evolution in LH2 and the transient dynamics under femtosecond pulse excitation. The research results prove that not only the transition from ground state to one-exciton state but also that from one-exciton state to two-exciton state contribute to the photodynamics of B850.
Scaling of collision strengths for highly-excited states of ions of the H- and He-like sequences
Fernandez-Menchero, L; Badnell, N R
2016-01-01
Emission lines from highly-excited states (n >= 5) of H- and He-like ions have been detected in astrophysical sources and fusion plasmas. For such excited states, R-matrix or distorted wave calculations for electron-impact excitation are very limited, due to the large size of the atomic basis set needed to describe them. Calculations for n >= 6 are also not generally available. We study the behaviour of the electron-impact excitation collision strengths and effective collision strengths for the most important transitions used to model electron collision dominated astrophysical plasmas, solar, for example. We investigate the dependence on the relevant parameters: the principal quantum number n or the nuclear charge Z. We also estimate the importance of coupling to highly-excited states and the continuum by comparing the results of different sized calculations. We provide analytic formulae to calculate the electron-impact excitation collision strengths and effective collision strengths to highly-excited states ...
Energy Technology Data Exchange (ETDEWEB)
Kullie, Ossama, E-mail: kullie@uni-kassel.de [Institute de Chimie de Strasbourg, CNRS et Université de Strasbourg, Laboratoire de Chimie Quantique, 4 rue Blaise Pascal, 67070 Strasbourg (France); Theoretical Physics, Institute for Physics, Department of Mathematics and Natural Science, University of Kassel (Germany)
2013-03-29
Highlights: ► The achievement of CAMB3LYP functional for excited states in framework of TD-DFT. ► Relativistic 4-components calculations for the excited states of the Cd{sub 2} dimer. ► Relativistic Spin-Free calculations for the excited states of Cd{sub 2} dimer. ► A comparison of the achievements of different types of DFT approximations upon Cd{sub 2}. - Abstract: In this paper we present a time-dependent density functional study for the ground-state as well the 20-lowest laying excited states of the cadmium dimer Cd{sub 2}, we analyze its spectrum obtained from all electrons calculations performed with time-depended density functional for the relativistic Dirac-Coulomb- and relativistic spin-free-Hamiltonian as implemented in DIRAC-PACKAGE. The calculations were obtained with different density functional approximations, and a comparison with the literature is given as far as available. Our result is very encouraging, especially for the lowest excited states of this dimer, and is expected to be enlightened for similar systems. The result shows that only long-range corrected functionals such as CAMB3LYP, gives the correct asymptotic behavior for the higher states. A comparable but less satisfactory results were obtained with B3LYP and PBE0 functionals. Spin-free-Hamiltonian is shown to be very efficient for systems containing heavy elements such as Cd{sub 2} in frameworks of (time-dependent) density functional without introducing large errors.
Lifetimes of ultralong-range Rydberg molecules in vibrational ground and excited states
Energy Technology Data Exchange (ETDEWEB)
Butscher, Bjoern; Bendkowsky, Vera; Nipper, Johannes; Balewski, Jonathan B; Kukota, Ludmila; Loew, Robert; Pfau, Tilman [5. Physikalisches Institut, Universitaet Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart (Germany); Li, Weibin; Pohl, Thomas; Rost, Jan Michael, E-mail: b.butscher@physik.uni-stuttgart.de [Max-Planck-Institut fuer Physik komplexer Systeme, Noethnitzer Str. 38, 01187 Dresden (Germany)
2011-09-28
Since their first experimental observation, ultralong-range Rydberg molecules consisting of a highly excited Rydberg atom and a ground state atom [1, 2] have attracted the interest in the field of ultracold chemistry [3, 4]. Especially the intriguing properties such as size, polarizability and type of binding they inherit from the Rydberg atom are of interest. An open question in the field is the reduced lifetime of the molecules compared to the corresponding atomic Rydberg states [2]. In this paper we present an experimental study on the lifetimes of the {sup 3}{Sigma}(5s - 35s) molecule in its vibrational ground state and in an excited state. We show that the lifetimes depend on the density of ground state atoms and that this can be described in the frame of a classical scattering between the molecules and ground state atoms. We also find that the excited molecular state has an even more reduced lifetime compared to the ground state which can be attributed to an inward penetration of the bound atomic pair due to imperfect quantum reflection that takes place in the special shape of the molecular potential [5].
First experimental evidence of 2He decay from 18Ne excited states
Rapisarda, E; Cardella, G; De Napoli, M; Raciti, G; Sfienti, C
2010-01-01
Two-proton decay from 18Ne excited states has been studied by complete kinematical detection of the decay products. The 18Ne nucleus has been produced as a radioactive beam by 20Ne projectile fragmentation at 45 AMeV on a 9Be target, using the FRIBs in-flight facility of the LNS. The 18Ne at 33 AMeV incident energy has been excited via Coulomb excitation on a natPb target. The correlated 2p emission has been disentangled from the uncorrelated 2p emission using a high granularity particle detector setup allowing the reconstruction of momentum and angle correlations of the two emitted protons. The obtained results unambiguously show that the 6.15 MeV 18Ne state two-proton decay proceeds through 2He emission (31%) and democratic or virtual sequential decay (69%).
Experimental Evidence of He2 Decay from Ne18 Excited States
Raciti, G.; Cardella, G.; de Napoli, M.; Rapisarda, E.; Amorini, F.; Sfienti, C.
2008-05-01
Two-proton decay from Ne18 excited states has been studied by complete kinematical reconstruction of the decay products. The Ne18 nucleus has been produced as a radioactive beam by Ne20 primary projectile fragmentation at 45AMeV incident energy on a Be target. The Ne18 at 33AMeV incident energy has been excited via Coulomb excitation on a Pbnat target. The obtained results unambiguously show that the 6.15 MeV Ne18 state two-proton decay proceeds through a He2 diproton resonance (31%) and democratic or virtual sequential decay (69%). The quoted branching ratio has been deduced from relative angle and momentum correlations of the emitted proton pairs.
Institute of Scientific and Technical Information of China (English)
无
2009-01-01
Kr atoms were produced in their metastable states 4p55s [3/2]2 and 4p55s’ [1/2]0 in a pulsed DC dis-charge in a beam,and subsequently excited to the even-parity autoionizing Rydberg states 4p5np’ [3/2]1,2,[1/2]1 and 4p5nf’ [5/2]3 using single photon excitation.The excitation spectra of the even-parity autoionizing resonance series from the metastable Kr were obtained by recording the autoionized Kr+ ions with time-of-flight ion detection in the photon energy range of 29000-40000 cm1.A wealth of autoionizing resonances were newly observed,from which more precise and more systematic spec-troscopic data of the level energy and quantum defects were derived.
Electron impact excitation of 2p and 3p states of hydrogen at intermediate energies
International Nuclear Information System (INIS)
A coupled-channel-optical (CCO) calculation with 9 and 12 atomic states supplemented with the continuum optical potentials for the stronger coupling channels has been performed for the electron impact excitation of hydrogen. The calculated n = 2 and n = 3 differential cross sections and the reduced Stokes parameters are comparable with the state-of-the art calculations. There is closer agreement between the present calculations and the experimental measurements for the reduced Stokes parameters P-bar1 and P-bar3 in the n = 2p excitation at 54.4 eV. The present CCO calculations also display good accord with the limited experimental data for the reduced Stokes parameters in the n = 3p excitation. (authors)
Institute of Scientific and Technical Information of China (English)
LI ChunYan; WANG TingTing; ZHEN JunFeng; ZHANG Qun; CHEN Yang
2009-01-01
Kr atoms were produced in their metastable states 4p55s [3/2]2 and 4p55s' [1/2]0 in a pulsed DC discharge in a beam, and subsequently excited to the even-parity autoionizing Rydberg states 4p5np' [3/2]1,2, [1/2]1 and 4p5nf' [5/2]3 using single photon excitation. The excitation spectra of the even-parity autoionizing resonance series from the metastable Kr were obtained by recording the autoionized Kr+ ions with time-of-flight ion detection in the photon energy range of 29000-40000 cm-1. A wealth of autoionizing resonances were newly observed, from which more precise and more systematic spec-troscopic data of the level energy and quantum defects were derived.
Institute of Scientific and Technical Information of China (English)
Chun-yan Li; Ting-ting Wang; Jun-feng Zhen; Qun Zhang; Yang Chen
2008-01-01
Xenon atoms were produced in their metastable states 5p56s[3/2]2 and 5p56s'[1/2]0 in a pulsed DC discharge in a beam, and subsequently excited to the even-parity autoionizing Rydberg states 5p5np' [3/2] 1 ,[1/2]1, t, and 5p5 nf'[5/2]3 using single photon excitation. The excitation spectra of the even-parity autoionizing resonance series from the metastable 129Xe were obtained by recording the autoionized Xe+ with time-of-flight ion detection in the photon energy range of 28000-42000 cm-1. A wealth of autoionizing resonances were newly observed, from which more precise and systematic spectroscopic data of the level energies and quantum defects were derived.
Reichardt, Christian; Sainuddin, Tariq; Wächtler, Maria; Monro, Susan; Kupfer, Stephan; Guthmuller, Julien; Gräfe, Stefanie; McFarland, Sherri; Dietzek, Benjamin
2016-08-18
The influence of ligand protonation on the photophysics of a ruthenium (Ru) dyad bearing the 2-(1-pyrenyl)-1H-imidazo[4,5-f][1,10]-phenanthroline (ippy) ligand was investigated by time-resolved transient absorption spectroscopy. It was found that changes in the protonation state of the imidazole group led to changes in the electronic configuration of the lowest lying excited state. Formation of the fully deprotonated imidazole anion resulted in excited state signatures that were consistent with a low-lying intraligand (IL) triplet state. This assignment was supported by time-dependent density functional theory (TDDFT) calculations. IL triplet states have been suggested to be potent mediators of photodynamic effects. Thus, these results are of interest in the design of Ru metal complexes as photosensitizers (PSs) for photodynamic therapy (PDT). PMID:27459188
Perun, Serhiy; Tatchen, Jörg; Marian, Christel M
2008-02-01
Extensive time-dependent DFT (TDDFT) and DFT/multireference configuration interaction (MRCI) calculations are performed on the singlet and triplet excited states of free-base porphyrin, with emphasis on intersystem crossing processes. The equilibrium geometries, as well as the vertical and adiabatic excitation energies of the lowest singlet and triplet excited states are determined. Single and double proton-transfer reactions in the first excited singlet state are explored. Harmonic vibrational frequencies are calculated at the equilibrium geometries of the ground state and of the lowest singlet and triplet excited states. Furthermore, spin-orbit coupling matrix elements of the lowest singlet and triplet states and their numerical derivatives with respect to nuclear displacements are computed. It is shown that opening of an unprotonated pyrrole ring as well as excited-state single and double proton transfer inside the porphyrin cavity lead to crossings of the potential energy curves of the lowest singlet and triplet excited states. It is also found that displacements along out-of-plane normal modes of the first excited singlet state cause a significant increase of the , , and spin-orbit coupling matrix elements. These phenomena lead to efficient radiationless deactivation of the lowest excited states of free-base porphyrin via intercombination conversion. In particular, the S1-->T1 population transfer is found to proceed at a rate of approximately 10(7) s(-1) in the isolated molecule. PMID:18189251
Kimoto, Yoshio; Okano, Makoto; Kanemitsu, Yoshihiko
2013-01-01
The higher Rydberg states of the E11 exciton in undoped and hole-doped single-walled carbon nanotubes (SWCNTs) were studied using one- and two-photon photoluminescence excitation spectroscopy. Increasing the hole-dopant concentration resulted in a redshift of the first excited state (2g) and a blueshift of the ground state (1u) of the E11 exciton. From the redshift of higher Rydberg states, we found that a reduction of the band-gap energy occurs in hole-doped SWCNTs. These findings show that ...
DEFF Research Database (Denmark)
Kuhlman, Thomas Scheby; Mikkelsen, Kurt V.; Møller, Klaus Braagaard;
2009-01-01
We present a study on the excited states of an ethylene dimer as to investigate the presence of and perturbation from low-lying charge-resonance states calculated by linear response density functional theory (DFT) using the B3LYP and CAM-B3LYP functionals. The calculations are compared to a refer......We present a study on the excited states of an ethylene dimer as to investigate the presence of and perturbation from low-lying charge-resonance states calculated by linear response density functional theory (DFT) using the B3LYP and CAM-B3LYP functionals. The calculations are compared...
Measurement of double beta decay of 100Mo to excited states in the NEMO 3 experiment
International Nuclear Information System (INIS)
The double beta decay of 100Mo to the 01+ and 21+ excited states of 100Ru is studied using the NEMO 3 data. After the analysis of 8024 h of data the half-life for the two-neutrino double beta decay of 100Mo to the excited 01+ state is measured to be T1/2(2ν)=[5.7-0.9+1.3(stat.)+/-0.8(syst.)]x1020 y. The signal-to-background ratio is equal to 3. Information about energy and angular distributions of emitted electrons is also obtained. No evidence for neutrinoless double beta decay to the excited 01+ state has been found. The corresponding half-life limit is T1/2(0ν)(0+->01+)>8.9x1022 y (at 90% C.L.). The search for the double beta decay to the 21+ excited state has allowed the determination of limits on the half-life for the two neutrino mode T1/2(2ν)(0+->21+)>1.1x1021 y (at 90% C.L.) and for the neutrinoless mode T1/2(0ν)(0+->21+)>1.6x1023 y (at 90% C.L.)
Excited State Mass spectra and Regge trajectories of Bottom Baryons in Hypercentral quark Model
Thakkar, Kaushal; Rai, Ajay Kumar; Vinodkumar, P C
2016-01-01
We present the mass spectra of excited states of singly heavy baryons consist of a bottom quark and light quarks (u, d and s). The QCD motivated hypercentral quark model is employed for the three body description of baryons. The form of confinement potential is hyper coloumb plus power potential with potential index $\
Ab Initio Excited States from the In-Medium Similarity Renormalization Group
Parzuchowski, N M; Bogner, S K
2016-01-01
We present two new methods for performing \\emph{ab initio} calculations of excited states for closed-shell systems within the in-medium similarity renormalization group (IMSRG) framework. Both are based on combining the IMSRG with simple many-body methods commonly used to target excited states, such as the Tamm-Dancoff approximation (TDA) and equations-of-motion (EOM) techniques. In the first approach, a two-step sequential IMSRG transformation is used to drive the Hamiltonian to a form where a simple TDA calculation (i.e., diagonalization in the space of $1$p$1$h excitations) becomes exact for a subset of eigenvalues. In the second approach, equations-of-motion (EOM) techniques are applied to the ground-state-decoupled IMSRG Hamiltonian to access excited states. We perform proof-of-principle calculations for parabolic quantum dots in two-dimensions and the closed shell nuclei $^{16}$O and $^{22}$O. We find that the TDA-IMSRG approach gives better accuracy than the EOM-IMSRG when calculations converge, but is...
Ponderomotive dressing of doubly-excited states with intensity-controlled laser light
Directory of Open Access Journals (Sweden)
Ding Thomas
2013-03-01
Full Text Available We laser-dress several doubly-excited states in helium. Tuning the coupling-laser intensity from perturbative to the strong-coupling regime, we are able to measure phases imprinted on the two-electron wavefunctions, and observe a new continuum coupling mechanism.
Double Beta Decays into Excited States in $^{110}$Pd and $^{102}$Pd
Lehnert, B; Degering, D; Hult, M; Laubenstein, M; Wester, T; Zuber, K
2016-01-01
A search for double beta decays of $^{110}$Pd and $^{102}$Pd into excited states of the daughter nuclides has been performed using three ultra-low background gamma-spectrometry measurements in the Felsenkeller laboratory, Germany, the HADES laboratory, Belgium and at the LNGS, Italy. The combined Bayesian analysis of the three measurements sets improved half-life limits for the $2\
DILEPTON DECAY OF GIANT-RESONANCES BUILT ON EXCITED-STATES OF SI-28
BUDA, A; BACELAR, JC; BALANDA, A; SUJKOWSKI, Z; VANDERWOUDE, A; BERSCH, R; CHING, H; DIOSZEGI, [No Value; HOFMAN, DJ; PAUL, P; SCHADMAND, S; VARMA, R
1995-01-01
Nuclear states in Si-28 were populated at an initial excitation energy E* = 50 MeV via the isospin T = 0 reaction O-16 + C-12. The dilepton- and photon-decay yields were measured simultaneously for the first time up to transition energies of 30 MeV. Statistical decay calculations describe well both
Generation of motional Fock states of a trappedion in the mediate-excitation regime
Institute of Scientific and Technical Information of China (English)
Zheng Shi-Biao
2004-01-01
We propose a scheme to prepare Fock states for the vibrational motion of a trapped ion. Unlike previous schemes,the present scheme works in the mediate-excitation regime, in which the corresponding Rabi frequency is equal to the trap frequency. Thus, the required time is greatly shortened, which is important in view of decoherence.
THE ACQM THEORETICAL CALCULATION OF LOW—LYING EXCITED STATES FOR HeH
Institute of Scientific and Technical Information of China (English)
Q.Q.GOU; Z.Y.Huang; 等
1990-01-01
The Low-lying excited states of HeH have been calculated by arrangement channel quantum mechanics(ACQM),The calculated potential curves,equilibrium geometry,Rc.dissociation energy Dc.harmonic vibration frequency ω0 and quadratic force coustant F2 are comparable with Ci calculations.
Stark effect of interfering electronic states: Localization of the nπ* excitations in toluquinone
Galaup, J. P.; Trommsdorff, H. P.
1984-04-01
High-precision Stark measurements on oriented single crystals of toluquinone at low temperatures have been performed and lead to an assessment of the electronic parenthood of the levels giving rise to the complex spectral region of interference between the two nearby nπ* excited states. The origin bands of the lowest excited singlet and triplet states are characterized by a measure of their factor-group splittings and an evaluation of the change in dipole moment and in polarizability upon excitation. The value of the change in dipole moment is shown to vary strongly between different vibrational levels of the lower state and an evaluation of the degree of localization of the electronic excitation on one CO group is made. The previous assignment of the second nπ* state is confirmed by the sign of the corresponding Stark shift. From measurements on crystals having been oriented in an electric field the absolute orientation of the polar crystal as well as the sign of the pyroelectric coefficient are proposed.
A Theoretical Study of Super-Excited States of F2
Institute of Scientific and Technical Information of China (English)
ZHANG Wei-Hua; HE Chun-long; HAO Yu-Song; MO Yu-Xiang; Li Jia-Ming
2007-01-01
In the framework of quantum defect theory, we study super-excited states of F2 molecules which can dissociate into F+(3P2,1,0) and F-(1So) ion-pair. Based on our calculation, we present a vibrational resolved assignment of the high precision photofragment yield spectra for F- from the F2 ion-pair production.
Symmetry-breaking intramolecular charge transfer in the excited state of meso-linked BODIPY dyads
Whited, Matthew T.
2012-01-01
We report the synthesis and characterization of symmetric BODIPY dyads where the chromophores are attached at the meso position, using either a phenylene bridge or direct linkage. Both molecules undergo symmetry-breaking intramolecular charge transfer in the excited state, and the directly linked dyad serves as a visible-light-absorbing analogue of 9,9′-bianthryl.
Time-resolved spectroscopy of doubly-excited states in helium
Directory of Open Access Journals (Sweden)
Ding Thomas
2013-03-01
Full Text Available A two-electron wave packet among the lowest-lying doubly-excited states in helium is experimentally observed. It creates a 1-femtosecond modulation in the transient-absorption signal modified by a time-delayed coupling laser.
Non-Monotonicity of Excited State Populations Observed in a Cu-He Hollow Cathode Discharge
Institute of Scientific and Technical Information of China (English)
ZHENG Xu-Tao
2005-01-01
@@ An interesting non-monotonic structure in the distribution of excited state populations is observed in a Cu-He hollow cathode discharge, and this is explained by l-changing collisions of the excited states with background gas atoms. At helium pressure of 0.1 Torr and cathode current of 200-300mA, relative populations of He I 1snp 1p (n = 2-16) states are measured with the corresponding VUV radiation intensities, and are plotted against excitation energies. As energy levels increase, populations of high-n (n ＞ 10) states are found to decrease much more quickly than low-n (n ＜ 7) populations. For intermediate states (n = 7-10), the declining tendency is interfered by population transfers from 1sns 1 S states due to l-changing collisions, and an obvious non-monotonic structure is formed at relatively low electric current. Measurements have also been carried out for He Ⅱ np 2 p (n = 2-14) series, in which the l-changing collisions are overwhelmed by Stark quenching of the n2S states and thus population interference does not occur.
Thermality and excited state R\\'enyi entropy in two-dimensional CFT
Lin, Feng-Li; Zhang, Jia-ju
2016-01-01
We evaluate one-interval R\\'enyi entropy and entanglement entropy for the excited states of two-dimensional conformal field theory (CFT) on a cylinder, and examine their differences from the ones for the thermal state. We assume the interval to be short so that we can use operator product expansion (OPE) of twist operators to calculate R\\'enyi entropy in terms of sum of one-point functions of OPE blocks. We find that the entanglement entropy for highly excited state and thermal state behave the same way after appropriate identification of the conformal weight of the state with the temperature. However, there exists no such universal identification for the R\\'enyi entropy in the short-interval expansion. Therefore, the highly excited state does not look thermal when comparing its R\\'enyi entropy to the thermal state one. As the R\\'enyi entropy captures the higher moments of the reduced density matrix but the entanglement entropy only the average, our results imply that the emergence of thermality depends on ho...
Wilkinson, Iain; Boguslavskiy, Andrey E; Mikosch, Jochen; Bertrand, Julien B; Wörner, Hans Jakob; Villeneuve, David M; Spanner, Michael; Patchkovskii, Serguei; Stolow, Albert
2014-05-28
The excited state dynamics of isolated sulfur dioxide molecules have been investigated using the time-resolved photoelectron spectroscopy and time-resolved photoelectron-photoion coincidence techniques. Excited state wavepackets were prepared in the spectroscopically complex, electronically mixed (B̃)(1)B1/(Ã)(1)A2, Clements manifold following broadband excitation at a range of photon energies between 4.03 eV and 4.28 eV (308 nm and 290 nm, respectively). The resulting wavepacket dynamics were monitored using a multiphoton ionisation probe. The extensive literature associated with the Clements bands has been summarised and a detailed time domain description of the ultrafast relaxation pathways occurring from the optically bright (B̃)(1)B1 diabatic state is presented. Signatures of the oscillatory motion on the (B̃)(1)B1/(Ã)(1)A2 lower adiabatic surface responsible for the Clements band structure were observed. The recorded spectra also indicate that a component of the excited state wavepacket undergoes intersystem crossing from the Clements manifold to the underlying triplet states on a sub-picosecond time scale. Photoelectron signal growth time constants have been predominantly associated with intersystem crossing to the (c̃)(3)B2 state and were measured to vary between 750 and 150 fs over the implemented pump photon energy range. Additionally, pump beam intensity studies were performed. These experiments highlighted parallel relaxation processes that occurred at the one- and two-pump-photon levels of excitation on similar time scales, obscuring the Clements band dynamics when high pump beam intensities were implemented. Hence, the Clements band dynamics may be difficult to disentangle from higher order processes when ultrashort laser pulses and less-differential probe techniques are implemented.
Booth, George H; Chan, Garnet Kin-Lic
2012-11-21
In this communication, we propose a method for obtaining isolated excited states within the full configuration interaction quantum Monte Carlo framework. This method allows for stable sampling with respect to collapse to lower energy states and requires no uncontrolled approximations. In contrast with most previous methods to extract excited state information from quantum Monte Carlo methods, this results from a modification to the underlying propagator, and does not require explicit orthogonalization, analytic continuation, transient estimators, or restriction of the Hilbert space via a trial wavefunction. Furthermore, we show that the propagator can directly yield frequency-domain correlation functions and spectral functions such as the density of states which are difficult to obtain within a traditional quantum Monte Carlo framework. We demonstrate this approach with pilot applications to the neon atom and beryllium dimer.
Influence of axial coordination on the photophysical property of excited state of zinc porphyrin
Institute of Scientific and Technical Information of China (English)
FENG; Juan; (冯娟); ZHANG; Huijuan; (张慧娟); XIANG; Junfeng; (向俊峰); AI; Xicheng; (艾希成); ZHANG; Xingkang; (张兴康); XU; Guangzhi; (徐广智); ZHANG; Jianping; (张建平)
2003-01-01
The effect of axial ligand 4-N,N-dimethyl aminopyridine (DMAP) on the fluorescence property of the second singlet excited state (S2) and first singlet excited state (S1) of 5,10,15, 20-tetra(p-methoxyl)phenyl zinc porphyrin has been investigated using steady-state absorption, fluorescence spectroscopy and picosecond time-resolved fluorescence spectroscopy. Hot fluorescence is clearly observed and is then reasonably assigned to the higher vibronic level from S1 state. A further analysis of fluorescence kinetics results shows that the coordination of DMAP to the zinc ion results in a decrease of hot fluorescence lifetime and an increase of the relative content of hot fluorescence. Similar phenomenon was observed with respects to S1 fluorescence upon the addition of DMAP in toluene. For a complete understanding of such an effect, a possible mechanism has been put forward and discussed in detail.
Institute of Scientific and Technical Information of China (English)
XU Xing-Lei
2007-01-01
Mesoscopic damped mutual capacitance coupled double resonance circuit is quantized by the method of damped harmonic oscillator quantization. Hamiltonian is diagonalized by the method of unitary transformation. The energy spectra of this circuit are given. The quantum fluctuations of the charge and current of each loop are investigated by the method of thermofield dynamics (TFD) in thermal excitation state,thermal squeezed vacuum state,thermal vacuum state and vacuum state. It is shown that the quantum fluctuations of the charge and current are related to not only circuit inherent parameter and coupled magnitude,but also quantum number of excitation,squeezed coefficients,squeezed angle and environmental temperature. And the quantum fluctuations increase with the increase of temperature and decay with time.
Impact of Electric Fields on Highly Excited Rovibrational States of Polar Dimers
Gonzalez-Ferez, Rosario
2008-01-01
We study the effect of a strong static homogeneous electric field on the highly excited rovibrational levels of the LiCs dimer in its electronic ground state. Our full rovibrational investigation of the system includes the interaction with the field due to the permanent electric dipole moment and the polarizability of the molecule. We explore the evolution of the states next to the dissociation threshold as the field strength is increased. The rotational and vibrational dynamics are influenced by the field; effects such as orientation, angular motion hybridization and squeezing of the vibrational motion are demonstrated and analyzed. The field also induces avoided crossings causing a strong mixing of the electrically dressed rovibrational states. Importantly, we show how some of these highly excited levels can be shifted to the continuum as the field strength is increased, and reversely how two atoms in the continuum can be brought into a bound state by lowering the electric field strength.
Mayer, G. V.; Plotnikov, V. G.; Artyukhov, V. Ya.
2016-08-01
Models of quantum-chemical calculation of rate constants for internal processes and intersystem crossing in polyatomic molecules are considered. The influence of the nature of electronically excited states in organic compounds is investigated. It is shown that the explicit allowance for the nature of wave functions of electronic states for estimation of electronic matrix elements of nonadiabaticity operators and spin-orbit interaction allows photophysical processes in organic compounds to be considered in detail.
Excited-state proton transfer from pyranine to acetate in methanol
Indian Academy of Sciences (India)
Sudip Kumar Mondal; Subhadip Ghosh; Kalyanasis Sahu; Pratik Sen; Kankan Bhattacharyya
2007-03-01
Excited-state proton transfer (ESPT) of pyranine (8-hydroxypyrene-1,3,6-trisulphonate, HPTS) to acetate in methanol has been studied by steady-state and time-resolved fluorescence spectroscopy. The rate constant of direct proton transfer from pyranine to acetate (1) is calculated to be ∼ 1 × 109 M-1 s-1. This is slower by about two orders of magnitude than that in bulk water (8 × 1010 M-1 s-1) at 4 M acetate.
International Nuclear Information System (INIS)
Detection of single atoms Yb has been achieved using the method of electric-field ionization from the high-lying Rydberg states. Atoms of Yb in a beam were excited in three steps to a 17-p state by radiation of three pulsed dye lasers. The statistics of an atom's appearance in the interaction volume have been studied in the single-ion counting regime at low beam density
The excited states of the neutral and ionized carbon in the regenerative sooting discharges
International Nuclear Information System (INIS)
We report the mechanisms of production and the state of excitation of the neutral and singly charged monatomic carbon in the regenerative soot as a function of the discharge parameters in graphite hollow cathode (HC) sources. Two distinctly different source configurations have been investigated. Comparisons of the level densities of various charged states of C1 have identified the regenerative properties of the C radicals in graphite HC soot
Triplet excited state properties in variable gap π-conjugated donor–acceptor–donor chromophores
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.
Picosecond spectral relaxation of curcumin excited state in toluene–alcohol mixtures
International Nuclear Information System (INIS)
Excited state photophysics of Curcumin in a binary solvent mixture of toluene and five different alcohols (Methanol, Ethanol, 1-Propanol, 1-Butanol and 1-Octanol) are compared with an instrument time resolution of ∼40 ps. As the alcohol mole-fraction is varied from zero to unity, the observed trends in the fluorescence quantum yield and lifetime of the pigment in toluene–alcohol mixtures changes significantly in going from Methanol to 1-Octanol. This is attributed to the different degree of modulation of the non-radiative rates associated with the excited state intermolecular H bonding between the pigment and the alcohol. Fluorescence decays taken at the red edge of the emission spectrum started to show measurable rise times (200–30 ps) the magnitude of which decreased gradually with increasing alcohol mole-fraction. As a consequence the solvation times in the binary mixture were observed to slow down considerably at certain solvent compositions compared to that in neat alcohol. However, in toluene-1-Octanol mixture, the rise times and corresponding solvation times did not show a dependence on the 1-Octanol mole-fraction. The observed results suggest that viscosity, polarity and hydrogen bonding property of the alcohol solvent plays an important role in the excited state processes of the pigment in toluene–alcohol mixture. -- Highlights: • Excited state photophysics of Curcumin in a binary solvent mixture of toluene and five different alcohols were studied. • The observed trends in the fluorescence properties are attributed to intermolecular H bonding between the pigment and the alcohol. • Except 1-Octanol, the average solvation times of the pigment were observed to depend upon alcohol mole-fraction. • Viscosity, polarity and hydrogen bonding play an important role in the excited state processes of the pigment
Picosecond spectral relaxation of curcumin excited state in toluene–alcohol mixtures
Energy Technology Data Exchange (ETDEWEB)
Saini, R.K.; Das, K., E-mail: kaustuv@rrcat.gov.in
2013-12-15
Excited state photophysics of Curcumin in a binary solvent mixture of toluene and five different alcohols (Methanol, Ethanol, 1-Propanol, 1-Butanol and 1-Octanol) are compared with an instrument time resolution of ∼40 ps. As the alcohol mole-fraction is varied from zero to unity, the observed trends in the fluorescence quantum yield and lifetime of the pigment in toluene–alcohol mixtures changes significantly in going from Methanol to 1-Octanol. This is attributed to the different degree of modulation of the non-radiative rates associated with the excited state intermolecular H bonding between the pigment and the alcohol. Fluorescence decays taken at the red edge of the emission spectrum started to show measurable rise times (200–30 ps) the magnitude of which decreased gradually with increasing alcohol mole-fraction. As a consequence the solvation times in the binary mixture were observed to slow down considerably at certain solvent compositions compared to that in neat alcohol. However, in toluene-1-Octanol mixture, the rise times and corresponding solvation times did not show a dependence on the 1-Octanol mole-fraction. The observed results suggest that viscosity, polarity and hydrogen bonding property of the alcohol solvent plays an important role in the excited state processes of the pigment in toluene–alcohol mixture. -- Highlights: • Excited state photophysics of Curcumin in a binary solvent mixture of toluene and five different alcohols were studied. • The observed trends in the fluorescence properties are attributed to intermolecular H bonding between the pigment and the alcohol. • Except 1-Octanol, the average solvation times of the pigment were observed to depend upon alcohol mole-fraction. • Viscosity, polarity and hydrogen bonding play an important role in the excited state processes of the pigment.
Sugawara, Kenichi; Tanabe, Shigeo; Suzuki, Tomotaka; Higashi, Toshio
2013-09-01
We aimed to investigate whether motor learning induces different excitability changes in the human motor cortex (M1) between two different muscle contraction states (before voluntary contraction [static] or during voluntary contraction [dynamic]). For the same, using motor evoked potentials (MEPs) obtained by transcranial magnetic stimulation (TMS), we compared excitability changes during these two states after pinch-grip motor skill learning. The participants performed a force output tracking task by pinch grip on a computer screen. TMS was applied prior to the pinch grip (static) and after initiation of voluntary contraction (dynamic). MEPs of the following muscles were recorded: first dorsal interosseous (FDI), thenar muscle (Thenar), flexor carpi radialis (FCR), and extensor carpi radialis (ECR) muscles. During both the states, motor skill training led to significant improvement of motor performance. During the static state, MEPs of the FDI muscle were significantly facilitated after motor learning; however, during the dynamic state, MEPs of the FDI, Thenar, and FCR muscles were significantly decreased. Based on the results of this study, we concluded that excitability changes in the human M1 are differentially influenced during different voluntary contraction states (static and dynamic) after motor learning.
The finite volume spectrum of excited states from lattice QCD simulations
Bulava, John; Jhang, You-Cyuan; Lenkner, David; Morningstar, Colin J; Foley, Justin; Juge, Keisuke J; Wong, Chik Him
2014-01-01
We present results for the spectrum of excited mesons obtained from temporal correlations of spatially-extended single-hadron and multi-hadron operators computed in lattice QCD. The stochastic LapH algorithm is implemented on anisotropic, dynamical lattices for isovectors for pions of mass $390$ MeV. A large correlation matrix with single-particle and two-particle probe operators is diagonalized to identify resonances. The masses of excited states in the $I=1, S=0, T_{1u}^+$ channel as well as the mixing of single and multi-particle probe operators are presented.
N. Andres; Catara, F.; Lanza, E. G.; Chomaz, Ph.; FALLOT M.; Scarpaci, J.A.
2001-01-01
We calculate the inelastic scattering cross sections to populate one- and two-phonon states in heavy ion collisions with both Coulomb and nuclear excitations. Starting from a microscopic approach based on RPA, we go beyond it in order to treat anharmonicities and non-linear terms in the exciting field. These anharmonicities and non-linearities are shown to have important effects on the cross sections both in the low energy part of the spectrum and in the energy region of the Double Giant Quad...
Excitation into high-lying states in Li3+–H collisions
Ibaaz, Aicha; Esteban Hernandez, Rosa; Dubois, Alain; Sisourat, Nicolas
2016-04-01
We have studied the excitation of atomic hydrogen by fully-stripped lithium ion impact in the intermediate energy range using a new and efficient implementation of the two-center atomic orbital approach with Gaussian-type orbitals. Partial and state-selective cross sections have been obtained for excitation up to H(6 h). A careful investigation of the convergence of the results with respect to the basis set has been performed which allows us to estimate the accuracy of the cross sections. Furthermore, our calculations provide an explanation for the discrepancies between previous calculations on this collision system.
Assessing Accuracy of Exchange-Correlation Functionals for the Description of Atomic Excited States
Makowski, Marcin; Hanas, Martyna
2016-09-01
The performance of exchange-correlation functionals for the description of atomic excitations is investigated. A benchmark set of excited states is constructed and experimental data is compared to Time-Dependent Density Functional Theory (TDDFT) calculations. The benchmark results show that for the selected group of functionals good accuracy may be achieved and the quality of predictions provided is competitive to computationally more demanding coupled-cluster approaches. Apart from testing the standard TDDFT approaches, also the role of self-interaction error plaguing DFT calculations and the adiabatic approximation to the exchange-correlation kernels is given some insight.
Quantum-chemical study of electronically excited states of protolytic forms of vanillic acid
Vusovich, O. V.; Tchaikovskaya, O. N.; Sokolova, I. V.; Vasil'eva, N. Y.
2015-12-01
The paper describes an analysis of possible ways of deactivation of electronically excited states of 4-hydroxy- 3-methoxy-benzoic acid (vanillic acid) and its protolytic forms with the use of quantum-chemical methods INDO/S (intermediate neglect of differential overlap with a spectroscopic parameterization) and MEP (molecular electrostatic potential). The ratio of radiative and non-radiative deactivation channels of the electronic excitation energy is established. The rate constants of photophysical processes (internal and intercombination conversions) occurring after the absorption of light in these forms are evaluated.
Numerical computation of dynamically important excited states of many-body systems
Łącki, Mateusz; Delande, Dominique; Zakrzewski, Jakub
2012-07-01
We present an extension of the time-dependent density matrix renormalization group, also known as the time evolving block decimation algorithm, allowing for the computation of dynamically important excited states of one-dimensional many-body systems. We show its practical use for analyzing the dynamical properties and excitations of the Bose-Hubbard model describing ultracold atoms loaded in an optical lattice from a Bose-Einstein condensate. This allows for a deeper understanding of nonadiabaticity in experimental realizations of insulating phases.
Institute of Scientific and Technical Information of China (English)
HU Li-Yun; FAN Hong-Yi
2008-01-01
We find that the squeezed two-mode number state is just a two-variable Hermite polynomial excitation of the two-mode squeezed vacuum state (THPES). We find that the Wigner function of THPES and its marginal distributions are just related to two-variable Hermite polynomials (or Laguerre polynomials) and that the tomogram of THPES can be expressed by one-mode Hermite polynomial.
Coherent Excitation of Lithium to Rydberg States and Application to Rydberg Atom Optics
Stevens, G.; Widmer, M.; Tudorica, F.; Iu, C.-H.; Metcalf, H.
1996-05-01
We present a theoretical analysis of several schemes for coherently exciting lithium atoms in a thermal beam to Rydberg states in a four level/three laser system, previously discussed by Oreg et al.(J. Oreg et al.), Phys. Rev. A 45, 4888 (1992). The time evolution of the dressed states and their populations are calculated numerically, solving the optical Bloch equations by a fourth order Runge-Kutta integration. Our code closely models actual experimental conditions, including spontaneous decay, beam profiles, intensities and detunings. Large Rydberg populations (50%) around n=15 may be obtained by non-adiabatic excitation, with each laser power on the order of 1 mW. We discuss the effects of an externally controlled time dependent detuning in the Rydberg state, for example as produced by atoms traversing an inhomogeneous electric field. An understanding of this excitation mechanism is important for large angle reflection of coherently excited atoms using field gradients. Some primitive ideas of Stark-Rydberg atom optics are presented.
Observation of excited state charge transfer with fs/ps-CARS
Energy Technology Data Exchange (ETDEWEB)
Blom, Alex Jason [Iowa State Univ., Ames, IA (United States)
2009-01-01
Excited state charge transfer processes are studied using the fs/ps-CARS probe technique. This probe allows for multiplexed detection of Raman active vibrational modes. Systems studied include Michler's Ketone, Coumarin 120, 4-dimethylamino-4'-nitrostilbene, and several others. The vibrational spectrum of the para di-substituted benzophenone Michler's Ketone in the first excited singlet state is studied for the first time. It is found that there are several vibrational modes indicative of structural changes of the excited molecule. A combined experimental and theoretical approach is used to study the simplest 7-amino-4-methylcoumarin, Coumarin 120. Vibrations observed in FTIR and spontaneous Raman spectra are assigned using density functional calculations and a continuum solvation model is used to predict how observed modes are affected upon inclusion of a solvent. The low frequency modes of the excited state charge transfer species 4-dimethylamino-4{prime}-nitrostilbene are studied in acetonitrile. Results are compared to previous work on this molecule in the fingerprint region. Finally, several partially completed projects and their implications are discussed. These include the two photon absorption of Coumarin 120, nanoconfinement in cyclodextrin cavities and sensitization of titania nanoparticles.
Observation of excited state charge transfer with fs/ps-CARS
International Nuclear Information System (INIS)
Excited state charge transfer processes are studied using the fs/ps-CARS probe technique. This probe allows for multiplexed detection of Raman active vibrational modes. Systems studied include Michler's Ketone, Coumarin 120, 4-dimethylamino-4(prime)-nitrostilbene, and several others. The vibrational spectrum of the para di-substituted benzophenone Michler's Ketone in the first excited singlet state is studied for the first time. It is found that there are several vibrational modes indicative of structural changes of the excited molecule. A combined experimental and theoretical approach is used to study the simplest 7-amino-4-methylcoumarin, Coumarin 120. Vibrations observed in FTIR and spontaneous Raman spectra are assigned using density functional calculations and a continuum solvation model is used to predict how observed modes are affected upon inclusion of a solvent. The low frequency modes of the excited state charge transfer species 4-dimethylamino-4(prime)-nitrostilbene are studied in acetonitrile. Results are compared to previous work on this molecule in the fingerprint region. Finally, several partially completed projects and their implications are discussed. These include the two photon absorption of Coumarin 120, nanoconfinement in cyclodextrin cavities and sensitization of titania nanoparticles
Fermionic Basis in Conformal Field Theory and Thermodynamic Bethe Ansatz for Excited States
Directory of Open Access Journals (Sweden)
Hermann Boos
2011-01-01
Full Text Available We generalize the results of [Comm. Math. Phys. 299 (2010, 825-866] (hidden Grassmann structure IV to the case of excited states of the transfer matrix of the six-vertex model acting in the so-called Matsubara direction. We establish an equivalence between a scaling limit of the partition function of the six-vertex model on a cylinder with quasi-local operators inserted and special boundary conditions, corresponding to particle-hole excitations, on the one hand, and certain three-point correlation functions of conformal field theory (CFT on the other hand. As in hidden Grassmann structure IV, the fermionic basis developed in previous papers and its conformal limit are used for a description of the quasi-local operators. In paper IV we claimed that in the conformal limit the fermionic creation operators generate a basis equivalent to the basis of the descendant states in the conformal field theory modulo integrals of motion suggested by A. Zamolodchikov (1987. Here we argue that, in order to completely determine the transformation between the above fermionic basis and the basis of descendants in the CFT, we need to involve excitations. On the side of the lattice model we use the excited-state TBA approach. We consider in detail the case of the descendant at level 8.
Role of excited state solvent fluctuations on time-dependent fluorescence Stokes shift
Energy Technology Data Exchange (ETDEWEB)
Li, Tanping, E-mail: tanping@lsu.edu, E-mail: revatik@lsu.edu; Kumar, Revati, E-mail: tanping@lsu.edu, E-mail: revatik@lsu.edu [Department of Chemistry, Louisiana State University, Baton Rouge, Louisiana 70803 (United States)
2015-11-07
We explore the connection between the solvation dynamics of a chromophore upon photon excitation and equilibrium fluctuations of the solvent. Using molecular dynamics simulations, fluorescence Stokes shift for the tryptophan in Staphylococcus nuclease was examined using both nonequilibrium calculations and linear response theory. When the perturbed and unperturbed surfaces exhibit different solvent equilibrium fluctuations, the linear response approach on the former surface shows agreement with the nonequilibrium process. This agreement is excellent when the perturbed surface exhibits Gaussian statistics and qualitative in the case of an isomerization induced non-Gaussian statistics. However, the linear response theory on the unperturbed surface breaks down even in the presence of Gaussian fluctuations. Experiments also provide evidence of the connection between the excited state solvent fluctuations and the total fluorescence shift. These observations indicate that the equilibrium statistics on the excited state surface characterize the relaxation dynamics of the fluorescence Stokes shift. Our studies specifically analyze the Gaussian fluctuations of the solvent in the complex protein environment and further confirm the role of solvent fluctuations on the excited state surface. The results are consistent with previous investigations, found in the literature, of solutes dissolved in liquids.
Excited state polarizabilities for CC2 using the resolution-of-the-identity approximation.
Graf, Nora K; Friese, Daniel H; Winter, Nina O C; Hättig, Christof
2015-12-28
We report an implementation of static and frequency-dependent excited state polarizabilities for the approximate coupled cluster single and doubles model CC2 as analytic second derivatives of an excited state quasienergy Lagrangian. By including appropriate conditions for the normalization and the phase of the eigenvectors, divergent secular terms are avoided. This leads to response equations in a subspace orthogonal to the unperturbed eigenvectors. It is shown how these projected equations can be solved without storage of the double excitation part of the eigenvectors. By exploiting the resolution-of-the-identity approximation and a numerical Laplace transformation, the quadratic scaling of the main memory demands of RI-CC2 with the system size could be preserved. This enables calculations of excited state polarizabilities for large molecules, e.g., linear polyacenes up to decacene with almost 2500 basis functions on a single compute node within a few days. For a test set of molecules where measurements are available as reference data, we compare the orbital-relaxed and unrelaxed CC2 approaches with experiment to validate its accuracy. The approach can be easily extended to other response methods, in particular CIS(D∞). The latter gives results which, in the orbital-relaxed case, are within a few percent of the CC2 values, while coupled cluster singles results deviate typically by about 20% from orbital-relaxed CC2 and experimental reference data. PMID:26723652
Red and blue shift of liquid water's excited states: A many body perturbation study
Ziaei, Vafa; Bredow, Thomas
2016-08-01
In the present paper, accurate optical absorption spectrum of liquid H2O is calculated in the energy range of 5-20 eV to probe the nature of water's excited states by means of many body perturbation approach. Main features of recent inelastic X-ray measurements are well reproduced, such as a bound excitonic peak at 7.9 eV with a shoulder at 9.4 eV as well as the absorption maximum at 13.9 eV, followed by a broad shoulder at 18.4 eV. The spectrum is dominated by excitonic effects impacting the structures of the spectrum at low and higher energy regimes mixed by single particle effects at high energies. The exciton distribution of the low-energy states, in particular of S1, is highly anisotropic and localized mostly on one water molecule. The S1 state is essentially a HOCO-LUCO (highest occupied crystal orbital - lowest unoccupied crystal orbital) transition and of intra-molecular type, showing a localized valence character. Once the excitation energy is increased, a significant change in the character of the electronically excited states occurs, characterized through emergence of multiple quasi-particle peaks at 7.9 eV in the quasi-particle (QP) transition profile and in the occurring delocalized exciton density distribution, spread over many more water molecules. The exciton delocalization following a change of the character of excited states at around 7.9 eV causes the blue shift of the first absorption band with respect to water monomer S1. However, due to reduction of the electronic band gap from gas to liquid phase, following enhanced screening upon condensation, the localized S1 state of liquid water is red-shifted with respect to S1 state of water monomer. For higher excitations, near vertical ionization energy (11 eV), quasi-free electrons emerge, in agreement with the conduction band electron picture. Furthermore, the occurring red and blue shift of the excited states are independent of the coupling of resonant and anti-resonant contributions to the
Calculations of three-dimensional magnetic excitations in permalloy nanostructures with vortex state
International Nuclear Information System (INIS)
Dynamic susceptibility spectra of the vortex state in nanorings and nanodots are studied using three-dimensional micromagnetic simulations. Spatial maps of the susceptibility have enabled identification of various resonance modes. For an exciting field along the x axis, several resonance peaks appear for a thin dot, including a core mode, whereas only one main resonance peak is detected for a ring corresponding to a volume mode with uniform magnetization perpendicular to the exciting field (x direction). A low-frequency resonance peak related to a surface mode and a high-frequency resonance peak viewed as an edge mode are additionally observed for a thick ring. These three resonance modes (surface, volume and edge modes) which correspond to low, intermediate and high-frequency resonance peaks, respectively, are also captured for an exciting field along the y axis. In addition, a mixed edge and volume mode is revealed at a higher frequency.
Transient spectra of photo-excited states in double exchange model
International Nuclear Information System (INIS)
We investigate photo-induced effect in strongly correlated electron systems where conduction electrons couple with localized spins. In particular, the photo-induced phenomena in a charge-ordered insulator associated with antiferromagnetic order are examined. Transient excitation spectra are calculated by the exact diagonalization method in one-dimensional extended double exchange model. We find that in the photo-excited states, finite spectral weights in the one-particle excitation spectra appear inside the insulating gap and its band width increases with increasing time. This change of the electronic structure is correlated with the time development of the localized spin correlation. These results indicate that a strong coupling between spin and charge governs the photo-induced phenomena in this system.
Transient spectra of photo-excited states in double exchange model
Energy Technology Data Exchange (ETDEWEB)
Kanamori, Yu; Ishihara, Sumio [Department of Physics, Tohoku University, Aramaki-Aoba, Sendai, 980-8578 (Japan); Matsueda, Hiroaki, E-mail: ykanamori@cmpt.phys.tohoku.ac.j [Sendai National College of Technology, Ayashi, Sendai, 989-3128 (Japan)
2009-02-01
We investigate photo-induced effect in strongly correlated electron systems where conduction electrons couple with localized spins. In particular, the photo-induced phenomena in a charge-ordered insulator associated with antiferromagnetic order are examined. Transient excitation spectra are calculated by the exact diagonalization method in one-dimensional extended double exchange model. We find that in the photo-excited states, finite spectral weights in the one-particle excitation spectra appear inside the insulating gap and its band width increases with increasing time. This change of the electronic structure is correlated with the time development of the localized spin correlation. These results indicate that a strong coupling between spin and charge governs the photo-induced phenomena in this system.
Pion inelastic scattering to the first three excited states of lithium-6
International Nuclear Information System (INIS)
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 6Li at incident pion energies of 120 and 180 MeV and laboratory scattering angles between 150 and 470. 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 12C. 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 12C (0.026 less than or equal to β less than or equal to 0.096)
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.
Analytic study of some excited state effects in a slightly bent Renner-Teller molecule
Energy Technology Data Exchange (ETDEWEB)
Vertesi, T [Institute of Nuclear Research of the Hungarian Academy of Sciences, H-4001 Debrecen, PO Box 51 (Hungary); Englman, R [Soreq NRC, Yavne 81800 (Israel)
2008-01-28
The two lowest electronic states (arising from X{sup 2}{pi}{sub u}) are treated analytically with inclusion of excited state effects in a slightly bent Renner-Teller acetylene molecular ion. The aim is to explain the anomalous values of approximately {pi} for the integrated non-adiabatic coupling term (NACT), recently obtained by ab initio calculations, as, e.g., in Halasz et al (2007 J. Chem. Phys. 126 154309). These occur when the molecular path twice coincides with symmetrically placed positions of degeneracies (conical intersections). However, the admixture of excited states into X{sup 2}{pi}{sub u} removes these coincidences, creates two aligned conical intersections in a planar arrangement and perturbationally reduces the integrated NACT from its value of {pi}.
Analytic study of some excited state effects in a slightly bent Renner Teller molecule
Vértesi, T.; Englman, R.
2008-01-01
The two lowest electronic states (arising from X2Πu) are treated analytically with inclusion of excited state effects in a slightly bent Renner-Teller acetylene molecular ion. The aim is to explain the anomalous values of approximately π for the integrated non-adiabatic coupling term (NACT), recently obtained by ab initio calculations, as, e.g., in Halász et al (2007 J. Chem. Phys. 126 154309). These occur when the molecular path twice coincides with symmetrically placed positions of degeneracies (conical intersections). However, the admixture of excited states into X2Πu removes these coincidences, creates two aligned conical intersections in a planar arrangement and perturbationally reduces the integrated NACT from its value of π.
Constraining nuclear photon strength functions by the decay properties of photo-excited states
Energy Technology Data Exchange (ETDEWEB)
Isaak, J., E-mail: j.isaak@gsi.de [ExtreMe Matter Institute EMMI and Research Division, GSI Helmholtzzentrum für Schwerionenforschung GmbH, 64291 Darmstadt (Germany); Frankfurt Institute for Advanced Studies FIAS, 60438 Frankfurt (Germany); Savran, D. [ExtreMe Matter Institute EMMI and Research Division, GSI Helmholtzzentrum für Schwerionenforschung GmbH, 64291 Darmstadt (Germany); Frankfurt Institute for Advanced Studies FIAS, 60438 Frankfurt (Germany); Krtička, M. [Faculty of Mathematics and Physics, Charles University, Prague 8 (Czech Republic); Ahmed, M.W. [Department of Mathematics and Physics, North Carolina Central University, Durham, NC 27707 (United States); Department of Physics, Duke University, Durham, NC 27708 (United States); Triangle Universities Nuclear Laboratory, Durham, NC 27708 (United States); Beller, J. [Institut für Kernphysik, Technische Universität Darmstadt, 64289 Darmstadt (Germany); Fiori, E. [ExtreMe Matter Institute EMMI and Research Division, GSI Helmholtzzentrum für Schwerionenforschung GmbH, 64291 Darmstadt (Germany); Frankfurt Institute for Advanced Studies FIAS, 60438 Frankfurt (Germany); Glorius, J. [Institut für Angewandte Physik, Goethe-Universität Frankfurt, 60438 Frankfurt (Germany); Kelley, J.H. [Department of Physics, North Carolina State University, Raleigh, NC 27695 (United States); Triangle Universities Nuclear Laboratory, Durham, NC 27708 (United States); Löher, B. [ExtreMe Matter Institute EMMI and Research Division, GSI Helmholtzzentrum für Schwerionenforschung GmbH, 64291 Darmstadt (Germany); Frankfurt Institute for Advanced Studies FIAS, 60438 Frankfurt (Germany); and others
2013-12-18
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{sup →}-Ray Source have been performed to investigate the decay properties of {sup 130}Te 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.
Unconventional decay law for excited states in closed many-body systems
Flambaum, V V
2001-01-01
We study the time evolution of an initially excited many-body state in a finite system of interacting Fermi-particles in the situation when the interaction gives rise to the ``chaotic'' structure of compound states. This situation is generic for highly excited many-particle states in quantum systems, such as heavy nuclei, complex atoms, quantum dots, spin systems, and quantum computers. For a strong interaction the leading term for the return probability $W(t)$ has the form $W(t)\\simeq \\exp (-\\Delta_E^2t^2)$ with $\\Delta_E^2$ as the variance of the strength function. The conventional exponential linear dependence $W(t)=C\\exp (-\\Gamma t)$ formally arises for a very large time. However, the prefactor $C$ turns out to be exponentially large, thus resulting in a strong difference from the conventional estimate for $W(t)$.
Highly selective population of two excited states in nonresonant two-photon absorption
Institute of Scientific and Technical Information of China (English)
Zhang Hui; Zhang Shi-An; Sun Zhen-Rong
2011-01-01
A nonresonant two-photon absorption process can be manipulated by tailoring the ultra-short laser pulse.In this paper,we theoretically demonstrate a highly selective population of two excited states in the nonresonant two-photon absorption process by rationally designing a spectral phase distribution.Our results show that one excited state is maximally populated while the other state population is widely tunable from zero to the maximum value.We believe that the theoretical results may play an important role in the selective population of a more complex nonlinear process comprising nonresonant two-photon absorption,such as resonance-mediated(2+1)-three-photon absorption and (2+1)-resonant multiphoton ionization.
On the effect of excited states in lattice calculations of the nucleon axial charge
Hansen, Maxwell T
2016-01-01
Excited-state contamination is one of the dominant uncertainties in lattice calculations of the nucleon axial-charge, $g_A$. Recently published results in leading-order chiral perturbation theory (ChPT) predict the excited-state contamination to be independent of the nucleon interpolator and positive. However, empirical results from numerical lattice calculations show negative contamination (downward curvature), indicating that present-day calculations are not in the regime where the leading-order ChPT predictions apply. In this paper we show that, under plausible assumptions, one can reproduce the behavior of lattice correlators by taking into account final-state $N \\pi$ interactions, in particular the effect of the Roper resonance, and by postulating a sign change in the infinite-volume $N \\to N \\pi$ axial-vector transition amplitude.
Long-Lived Triplet Excited States of Bent-Shaped Pentacene Dimers by Intramolecular Singlet Fission.
Sakuma, Takao; Sakai, Hayato; Araki, Yasuyuki; Mori, Tadashi; Wada, Takehiko; Tkachenko, Nikolai V; Hasobe, Taku
2016-03-24
Intramolecular singlet fission (ISF) is a promising photophysical process to construct more efficient light energy conversion systems as one excited singlet state converts into two excited triplet states. Herein we synthesized and evaluated bent-shaped pentacene dimers as a prototype of ISF to reveal intrinsic characters of triplet states (e.g., lifetimes of triplet excited states). In this study, meta-phenylene-bridged TIPS-pentacene dimer (PcD-3Ph) and 2,2'-bipheynyl bridged TIPS-pentacene dimer (PcD-Biph) were newly synthesized as bent-shaped dimers. In the steady-state spectroscopy, absorption and emission bands of these dimers were fully characterized, suggesting the appropriate degree of electronic coupling between pentacene moieties in these dimers. In addition, the electrochemical measurements were also performed to check the electronic interaction between two pentacene moieties. Whereas the successive two oxidation peaks owing to the delocalization were observed in a directly linked-pentacene dimer (PcD) by a single bond, the cyclic voltammograms in PcD-Biph and PcD-3Ph implied the weaker interaction compared to that of p-phenylene-bridged TIPS-pentacene dimer (PcD-4Ph) and PcD. The femtosecond and nanosecond transient absorption spectra clearly revealed the slower ISF process in bent-shaped pentacene dimers (PcD-Biph and PcD-3Ph), more notably, the slower relaxation of the excited triplet states in PcD-Biph and PcD-3Ph. Namely, the quantum yields of triplet states (ΦT) by ISF approximately remain constant (ca. 180-200%) in all dimer systems, whereas the lifetimes of the triplet excited states became much longer (up to 360 ns) in PcD-Biph as compared to PcD-4Ph (15 ns). Additionally, the lifetimes of the corresponding triplet states in PcD-Biph and PcD-3Ph were sufficiently affected by solvent viscosity. In particular, the lifetimes of PcD-Biph triplet state in THF/paraffin (1.0 μs) increased up to approximately three times as compared to that in THF
Excited state mass spectra of doubly heavy baryons {Ω _{cc}}, {Ω _{bb}}, and {Ω _{bc}}
Shah, Zalak; Thakkar, Kaushal; Rai, Ajay Kumar
2016-10-01
We discuss the mass spectrum of Ω baryon with two heavy quarks and one light quark ( ccs, bbs, and bcs). The main goal of the paper is to calculate the ground state masses and after that, the positive and negative parity excited states masses are also obtained within a hypercentral constituent quark model, using Coulomb plus linear potential framework. We also added a first order correction to the potential. The mass spectra up to 5S for radial excited states and 1P-5P, 1D-4D, and 1F-2F states for orbital excited states are computed for Ω _{cc}, Ω _{bb}, and Ω _{bc} baryons. Our obtained results are compared with other theoretical predictions, which could be a useful complementary tool for the interpretation of experimentally unknown heavy baryon spectra. The Regge trajectory is constructed in both the (n_r, M2) and the ( J, M2) planes for Ω _{cc}, Ω _{bb}, and Ω _{bc} baryons and their slopes and intercepts are also determined. Magnetic moments of doubly heavy Ω 's are also calculated.
A theoretical study on the wavepacket dynamics in the excited states of aromatic biomolecules
International Nuclear Information System (INIS)
The relaxation of the low-lying excited states of 9H-adenine through conical intersections of the dissociative “1πσ”* excited state with the lowest “1ππ”* excited state and the electronic-structure calculations and wave packet dynamics simulation. Adiabatic and quasidiabatic potential-energy surfaces and coupling elements were calculated as a function of the NH stretch coordinate of the azine group and the out-of-plane angle of the hydrogen atom, employing multireference configuration-interaction (MRCI) as well as restricted-active-space self-consistent-field (RASSCF) methods. Characteristic properties of the “1πσ”*-“1ππ”* and “1πσ”*-S0 conical intersections such as the diabatic-to-adiabatic mixing angle, the geometric phase of the adiabatic electronic wave functions, the derivative coupling, as well as adiabatic and diabatic trasition-dipole-moment surfaces were investigated in detail. Time-dependent wave packet simulations reveal an ultrafast relaxations dynamics of the optically-allowed lowest “1ππ”* state driven by vibronic coupling between strongly coupled electronic states that add to our understanding of the origin of the intrinsic photostability of the building blocks of life. (author)
Spectroscopy of ground and excited states of pseudoscalar and vector charmonium and bottomonium
Negash, Hluf; Bhatnagar, Shashank
2016-07-01
In this paper, we calculate the mass spectrum, weak decay constants, two photon decay widths, and two-gluon decay widths of ground (1S) and radially excited (2S, 3S,…) states of pseudoscalar charmoniuum and bottomonium such as ηc and ηb, as well as the mass spectrum and leptonic decay constants of ground state (1S), excited (2S, 1D, 3S, 2D, 4S,…, 5D) states of vector charmonium and bottomonium such as J/ψ, and Υ, using the formulation of Bethe-Salpeter equation under covariant instantaneous ansatz (CIA). Our results are in good agreement with data (where ever available) and other models. In this framework, from the beginning, we employ a 4 × 4 representation for two-body (qq¯) BS amplitude for calculating both the mass spectra as well as the transition amplitudes. However, the price we have to pay is to solve a coupled set of equations for both pseudoscalar and vector quarkonia, which we have explicitly shown get decoupled in the heavy-quark approximation, leading to mass spectral equation with analytical solutions for both masses, as well as eigenfunctions for all the above states, in an approximate harmonic oscillator basis. The analytical forms of eigenfunctions for ground and excited states so obtained are used to evaluate the decay constants and decay widths for different processes.
Phonon-like excitations in the two-state Bose-Hubbard model
Directory of Open Access Journals (Sweden)
I.V. Stasyuk
2015-12-01
Full Text Available The spectrum of phonon-like collective excitations in the system of Bose-atoms in optical lattice (more generally, in the system of quantum particles described by the Bose-Hubbard model is investigated. Such excitations appear due to displacements of particles with respect to their local equilibrium positions. The two-level model taking into account the transitions of bosons between the ground state and the first excited state in potential wells, as well as interaction between them, is used. Calculations are performed within the random phase approximation in the hard-core boson limit. It is shown that excitation spectrum in normal phase consists of the one exciton-like band, while in the phase with BE condensate an additional band appears. The positions, spectral weights and widths of bands strongly depend on chemical potential of bosons and temperature. The conditions of stability of a system with respect to the lowering of symmetry and displacement modulation are discussed.
Evolution of l-photon excited thermo vacuum state in a single-mode damping channel
He, Rui; Fan, Hong-Yi
2016-01-01
In this paper, we investigate how a kind of non-Gaussian states (l-photon excited thermo vacuum state Cla†l|0(β)>) evolves in a single-mode damping channel. We find that it evolves into a Laguerre-polynomial-weighted real-fictitious squeezed thermo vacuum state, which exhibits strong decoherence and its original nonclassicality fades. In particular, when l = 0, in this damping process the thermo squeezing effect decreases while the fictitious-mode vacuum becomes chaotic. In overcoming the difficulty of calculation, we employ the summation method within ordered product of operators, a new generating function formula about two-variable Hermite polynomials is derived.
Probing ground and low-lying excited states for HIO{sub 2} isomers
Energy Technology Data Exchange (ETDEWEB)
Souza, Gabriel L. C. de [Departamento de Química, Universidade Federal de Mato Grosso, Cuiabá, Mato Grosso 78060-900 (Brazil); Instituto de Ciências Exatas e Tecnologia, Universidade Federal do Amazonas, Itacoatiara, Amazonas 69100-000 (Brazil); Department of Chemistry, University of Alberta, Edmonton, Alberta T6G 2G2 (Canada); Brown, Alex, E-mail: alex.brown@ualberta.ca [Department of Chemistry, University of Alberta, Edmonton, Alberta T6G 2G2 (Canada)
2014-12-21
We present a computational study on HIO{sub 2} molecules. Ground state properties such as equilibrium structures, relative energetics, vibrational frequencies, and infrared intensities were obtained for all the isomers at the coupled-cluster with single and double excitations as well as perturbative inclusion of triples (CCSD(T)) level of theory with the aug-cc-pVTZ-PP basis set and ECP-28-PP effective core potential for iodine and the aug-cc-pVTZ basis set for hydrogen and oxygen atoms. The HOIO structure is confirmed as the lowest energy isomer. The relative energies are shown to be HOIO < HOOI < HI(O)O. The HO(O)I isomer is only stable at the density functional theory (DFT) level of theory. The transition states determined show interconversion of the isomers is possible. In order to facilitate future experimental identification, vibrational frequencies are also determined for all corresponding deuterated species. Vertical excitation energies for the three lowest-lying singlet and triplet excited states were determined using the configuration interaction singles, time-dependent density functional theory (TD-DFT)/B3LYP, TD-DFT/G96PW91, and equation of motion-CCSD approaches with the LANL2DZ basis set plus effective core potential for iodine and the aug-cc-pVTZ basis set for hydrogen and oxygen atoms. It is shown that HOIO and HOOI isomers have excited states accessible at solar wavelengths (<4.0 eV) but these states have very small oscillator strengths (<2 × 10{sup −3})
A relativistic time-dependent density functional study of the excited states of the mercury dimer
Energy Technology Data Exchange (ETDEWEB)
Kullie, Ossama, E-mail: kullie@uni-kassel.de, E-mail: ossama.kullie@unistra.fr [Institute de Chimie de Strasbourg, CNRS et Université de Strasbourg, Laboratoire de Chimie Quantique, 4 rue Blaise Pascal, 67070 Strasbourg, France and Theoretical Physics, Institute for Physics, Department of Mathematics and Natural Science, University of Kassel, D-34127 Kassel (Germany)
2014-01-14
In previous works on Zn{sub 2} and Cd{sub 2} dimers we found that the long-range corrected CAMB3LYP gives better results than other density functional approximations for the excited states, especially in the asymptotic region. In this paper, we use it to present a time-dependent density functional (TDDFT) study for the ground-state as well as the excited states corresponding to the (6s{sup 2} + 6s6p), (6s{sup 2} + 6s7s), and (6s{sup 2} + 6s7p) atomic asymptotes for the mercury dimer Hg{sub 2}. We analyze its spectrum obtained from all-electron calculations performed with the relativistic Dirac-Coulomb and relativistic spinfree Hamiltonian as implemented in DIRAC-PACKAGE. A comparison with the literature is given as far as available. Our result is excellent for the most of the lower excited states and very encouraging for the higher excited states, it shows generally good agreements with experimental results and outperforms other theoretical results. This enables us to give a detailed analysis of the spectrum of the Hg{sub 2} including a comparative analysis with the lighter dimers of the group 12, Cd{sub 2}, and Zn{sub 2}, especially for the relativistic effects, the spin-orbit interaction, and the performance of CAMB3LYP and is enlightened for similar systems. The result shows, as expected, that spinfree Hamiltonian is less efficient than Dirac-Coulomb Hamiltonian for systems containing heavy elements such as Hg{sub 2}.
López, A; Kisiel, Z; Daly, A M; Bermúdez, C; Calcutt, H; Marcelino, N; Viti, S; Drouin, B J; Medvedev, I R; Neese, C F; Pszczółkowski, L; Alonso, J L; Cernicharo, J
2014-01-01
New laboratory data of CH$_2$CHCN (vinyl cyanide) in its ground and vibrationally excited states at the microwave to THz domain allow searching for these excited state transitions in the Orion-KL line survey. Frequency-modulated spectrometers combined into a single broadband 50-1900 GHz spectrum provided measurements of CH$_2$CHCN covering a spectral range of 18-1893 GHz, whose assignments was confirmed by Stark modulation spectra in the 18-40 GHz region and by ab-initio anharmonic force field calculations. For analyzing the emission lines of CH$_2$CHCN species detected in Orion-KL we used the excitation and radiative transfer code (MADEX) at LTE conditions. The rotational transitions of the ground state of this molecule emerge from four cloud components of hot core nature which trace the physical and chemical conditions of high mass star forming regions in the Orion-KL Nebula. The total column density of CH$_2$CHCN in the ground state is (3.0$\\pm$0.9)x10$^{15}$ cm$^{-2}$. We report on the first interstellar ...
Pulsed excitation of Rydberg-atom-pair states in an ultracold Cs gas
Saßmannshausen, Heiner; Deiglmayr, Johannes
2015-01-01
Pulsed laser excitation of a dense ultracold Cs vapor has been used to study the pairwise interactions between Cs atoms excited to $n$p$_{3/2}$ Rydberg states of principal quantum numbers in the range $n=22-36$. Molecular resonances were observed that correspond to excitation of Rydberg-atom-pair states correlated not only to the $n$p$_{3/2}+n$p$_{3/2}$ dissociation asymptotes, but also to $n$s$_{1/2}+(n+1)$s$_{1/2}$, $n$s$_{1/2}+n'$f$_{j}$, and $(n-4)$f$_{j}+(n-3)$f$_{j}$ $(j=5/2,7/2)$ dissociation asymptotes. These pair resonances are interpreted as arising from dipole-dipole, and higher long-range-interaction terms between the Rydberg atoms on the basis of i) their spectral positions, ii) their response to static and pulsed electric fields, and iii) millimeter-wave spectra between pair states correlated to different pair-dissociation asymptotes. The Rydberg-atom--pair states were found to spontaneously decay by Penning ionization and the dynamics of the ionization process were investigated during the first...
Excited-state evolution probed by convoy-electron emission in relativistic heavy-ion collisions
Takabayashi, Y.; Ito, T.; Azuma, T.; Komaki, K.; Yamazaki, Y.; Tawara, H.; Takada, E.; Murakami, T.; Seliger, M.; Tökési, K.; O. Reinhold, C.; Burgdörfer, J.
2003-10-01
We present a joint experimental and theoretical study of convoy-electron emission resulting from highly-charged-ion transport through carbon foils at moderately relativistic speeds. Energy spectra of electrons ejected at 0° have been measured for 390 MeV/u hydrogen-like Ar17+ ions and 460 MeV/u (β=v/c=0.74,γ=1.49) Fe25+ (1s), Fe24+ (1s2), and Fe23+ (1s22s) incident on carbon foils with thicknesses from 25 to 8700 μg/cm2. Due to this unprecedented wide range of thicknesses, the sequential excitation and ionization of initially deeply bound electrons to highly excited states and continuum states can be followed in considerable detail. The analysis of the spectra is aided by simulations based on the classical transport theory which has been extended to relativistic energies and to multielectron projectiles. The motion of the projectile electron inside the solid target is calculated taking into account the Coulomb potential of the projectile ion and the multiple stochastic collisions with target cores and target electrons. Different phases of the convoy-electron emissions can be disentangled: direct ejection to the continuum, the transient buildup of an excited-state wave packet followed by ionization, and postionization modification of the continuum spectrum. We find good agreement between experiment and simulation for the evolution of charge states and the emission spectrum.
It is proposed to investigate the structure of excited states in $^{68, 70}$Ni(Z =28, N=40, 42) via the measurement of electromagnetic matrix elements in a Coulomb excitation experiment in order to study the N = 40 harmonic-oscillator shell and the Z = 28 proton shell closures. The measured B(E2) values connecting low-lying 0$^{+}$ and 2$^{+}$ can be compared to shell-model predictions. It is also proposed to perform the one-neutron transfer reaction ${d}$($^{68}$Ni,$^{69}$Ni)${p}$, with the aim of populating excited states in $^{69}$Ni. Comparisons with the states populated in the recently performed ${d}$($^{66}$Ni,$^{67}$Ni)${p}$ reaction will be useful in determining the role of the neutron $d_{5/2}$ orbital in the semi-magic properties of $^{68}$Ni.
Ground state and excitations of a Bose-Einstein condensate of atoms and their diatomic bound states
International Nuclear Information System (INIS)
We study theoretically a many-body system of spinless atoms and their diatomic bound states (or molecules) which form a single Bose-Einstein condensate at zero temperature. The equilibrium states of such a system and its dynamics are analyzed within the Gross-Pitaevskii approach. It is shown that the system exhibits two phases depending on binding energy value: it can be in the states with atomic-molecular condensate or molecular condensate. The basic thermodynamic characteristics of the two phases and their stability conditions are obtained. Both phases are characterized by two branches of collective excitations. The first branch is acoustic mode and the second one is gapfull
Energy Technology Data Exchange (ETDEWEB)
Lamour, E
1997-11-01
In ion-solid collisions, more excited states of projectile ions with high angular momenta l are populated than in ion-atom collisions. The use of 13.6 MeV/u Ar{sup 18+} projectile ions and solid carbon targets allowed us to study Ar{sup 17+} excited states initially populated by electron capture. Using various targets with increasing thickness from 3.5 to 200 {mu}g/cm{sup 2}, the evolution of excited states from the single collision condition to the population equilibrium was investigated. We observed the evolution of the Lyman line intensities as a function of the ion transit time inside the target (sensitive to core state population) and as a function of the ion time of flight behind the target (sensitive to Rydberg state population). To explain the experimental results, a complete theoretical analysis of the transport of excited states inside the medium was performed. We used two different collisional models. The first one is a rate equation model based on a statistical description of binary collisions of the projectile with target atoms. The second one is a classical transport theory based on an equation describing the motion of the projectile electron on a classical orbit perturbed by a stochastic force. A comparison with experiment shows that such a collisional approach allows to interpret the excited l-state population, but fails in describing the core state population. The observed l mixing in these states is much larger than predicted by the models. The polarization of the medium induced by the projectile ion, with both models do not take into account, could be responsible for this mixing by means of the Stark effect. (author)
Herbert, John M; Zhang, Xing; Morrison, Adrian F; Liu, Jie
2016-05-17
Single-excitation methods, namely, configuration interaction singles and time-dependent density functional theory (TDDFT), along with semiempirical versions thereof, represent the most computationally affordable electronic structure methods for describing electronically excited states, scaling as [Formula: see text] absent further approximations. This relatively low cost, combined with a treatment of electron correlation, has made TDDFT the most widely used excited-state quantum chemistry method over the past 20+ years. Nevertheless, certain inherent problems (beyond just the accuracy of this or that exchange-correlation functional) limit the utility of traditional TDDFT. For one, it affords potential energy surfaces whose topology is incorrect in the vicinity of any conical intersection (CI) that involves the ground state. Since CIs are the conduits for transitions between electronic states, the TDDFT description of photochemistry (internal conversion and intersystem crossing) is therefore suspect. Second, the [Formula: see text] cost can become prohibitive in large systems, especially those that involve multiple electronically coupled chromophores, for example, the antennae structures of light-harvesting complexes or the conjugated polymers used in organic photovoltaics. In such cases, the smallest realistic mimics might already be quite large from the standpoint of ab initio quantum chemistry. This Account describes several new computational methods that address these problems. Topology around a CI can be rigorously corrected using a "spin-flip" version of TDDFT, which involves an α → β spin-flipping transition in addition to occupied → virtual excitation of one electron. Within this formalism, singlet states are generated via excitation from a high-spin triplet reference state, doublets from a quartet, etc. This provides a more balanced treatment of electron correlation between ground and excited states. Spin contamination is problematic away from the
Herbert, John M; Zhang, Xing; Morrison, Adrian F; Liu, Jie
2016-05-17
Single-excitation methods, namely, configuration interaction singles and time-dependent density functional theory (TDDFT), along with semiempirical versions thereof, represent the most computationally affordable electronic structure methods for describing electronically excited states, scaling as [Formula: see text] absent further approximations. This relatively low cost, combined with a treatment of electron correlation, has made TDDFT the most widely used excited-state quantum chemistry method over the past 20+ years. Nevertheless, certain inherent problems (beyond just the accuracy of this or that exchange-correlation functional) limit the utility of traditional TDDFT. For one, it affords potential energy surfaces whose topology is incorrect in the vicinity of any conical intersection (CI) that involves the ground state. Since CIs are the conduits for transitions between electronic states, the TDDFT description of photochemistry (internal conversion and intersystem crossing) is therefore suspect. Second, the [Formula: see text] cost can become prohibitive in large systems, especially those that involve multiple electronically coupled chromophores, for example, the antennae structures of light-harvesting complexes or the conjugated polymers used in organic photovoltaics. In such cases, the smallest realistic mimics might already be quite large from the standpoint of ab initio quantum chemistry. This Account describes several new computational methods that address these problems. Topology around a CI can be rigorously corrected using a "spin-flip" version of TDDFT, which involves an α → β spin-flipping transition in addition to occupied → virtual excitation of one electron. Within this formalism, singlet states are generated via excitation from a high-spin triplet reference state, doublets from a quartet, etc. This provides a more balanced treatment of electron correlation between ground and excited states. Spin contamination is problematic away from the
The investigation of excited state proton transfer mechanism in water-bridged 7-azaindole
Zhang, Yong-Jia; Zhao, Jin-Feng; Li, Yong-Qing
2016-01-01
Based on the time-dependent density functional theory (TDDFT), the excited-state intermolecular proton transfer (ESIPT) mechanism of water-bridged 7-azaindole has been investigated theoretically. The calculations of primary bond lengths and the IR vibrational spectra between the S0 state and the S1 state that verified the intramolecular hydrogen bond were strengthened. The fact that reproduced experimental absorbance and fluorescence emission spectra well theoretically demonstrate that the TDDFT theory we adopted is reasonable and effective. In addition, intramolecular charge transfer based on the frontier molecular orbitals demonstrated the indication of the ESIPT reaction. The constructed potential energy curves of ground state and the first excited state based on keeping the H2···O3 and H6···N7 distances fixed at a series of values have been used to illustrate the ESIPT process. A relative lower barrier of 5.94 kcal/mol in the S1 state potential energy curve for type II (lower than that of 9.82 kcal/mol in the S1 state for type I) demonstrates that type II ESIPT process occurs firstly in 7Al-2H2O complex.
Search of the first excited states 0+ of 108Cd and106Cd
International Nuclear Information System (INIS)
108Cd and 106Cd nuclei have been studied from the β+/EC decay of 108In and 106In using the isocele II isotope separator working on-line with the Orsay synchrocyclotron. In order to produce indium nuclei, a molten tin target is irradiated by protons (E = 200 MeV) or 3He (E = 270 MeV). The comparison of saturation activity measured after mass separation with the one measured before mass-separation has allowed us to determine the average delay-time of indium isotopes and the overall efficiency of the separator. Single γ rays, conversion electrons rays, γ-γ-t and γ-e--t coincidence measurements have been performed to build level schemes of 108Cd and 106Cd. In 108Cd, the first excited 0+ state has been established unambiguously. This state preferably decays to the 22+ and not to the 21+ as it does in the even-even neighbouring Cd nuclei. An excited 0+ state is proposed in 106Cd. These states could not be interpreted as headstate of collective band corresponding to a shape different from the ground state one. On the other hand, the model of G. Alaga (vibrator + two proton holes), as well as the IBA2 F. Iachello one seem to be able to describe the low-lying states properties. Finally, the feeding balance and the deduced log ft values have led us to discuss the possible values of the 108In and 106In isomeric state spins
Indian Academy of Sciences (India)
Jahur A Mondal; Sandeep Verma; Hirendra N Ghosh; Dipak K Palit
2008-01-01
Relaxation dynamics of the excited singlet states of 2,5-bis-(N-methyl-N-1,3-propdienylaniline)-cyclopentanone (MPAC), a ketocyanine dye, have been investigated using steady-state absorption and emission as well as femtosecond time-resolved absorption spectroscopic techniques. Following photoexcitation using 400 nm light, the molecule is excited to the S2 state, which is fluorescent in rigid matrices at 77 K. S2 state is nearly non-fluorescent in solution and has a very short lifetime (0.5 ± 0.2 ps). In polar aprotic solvents, the S1 state follows a complex multi-exponential relaxation dynamics consisting of torsional motion of the donor groups, solvent re-organization as well as photoisomerization processes. However, in alcoholic solvents, solvent re-organization via intermolecular hydrogen-bonding interaction is the only relaxation process observed in the S1 state. In trifluoroethanol, a strong hydrogen bonding solvent, conversion of the non-hydrogen-bonded form, which is formed following photoexcitation, to the hydrogen-bonded complex has been clearly evident in the relaxation process of the S1 state.
Comparison of calculation methods for the tunnel splitting at excited states of biaxial spin models
Institute of Scientific and Technical Information of China (English)
Cui Xiao-Bo; Chen Zhi-De
2004-01-01
We present the calculation and comparison of tunnel splitting at excited levels of biaxial spin models by various methods, including the generalized instanton method, the generalized path integral method for coherent spin states,the perturbation method, and the exact method by numerical diagonalization of the Hamiltonian. It is found that,for integer spin with spin number around 10, tunnel splitting predicted by the generalized path integral for coherent spin states is about 10-n times of the exact numerical result for the nth excited level, while the ratio of the results of the perturbation method and the exact numerical method diverges in the large spin limit. We thus conclude that the generalized instanton method is the best approximate way for calculating tunnel splitting in spin models.
Excited State Lifetime Measurements in Rare Earth Nuclei with Fast Electronics
Werner, V.; Cooper, N.; Bonett-Matiz, M.; Williams, E.; Régis, J.-M.; Rudigier, M.; Ahn, T.; Anagnostatou, V.; Berant, Z.; Bunce, M.; Elvers, M.; Heinz, A.; Ilie, G.; Jolie, J.; Radeck, D.; Savran, D.; Smith, M.
2011-09-01
We investigated the collectivity of the lowest excited 2+ states of even-even rare earth nuclei. The B(E2) excitation strengths of these nuclei should directly correlate to the size of the valence space, and maximize at mid-shell. The previously identified saturation of B(E2) strength in well-deformed rotors at mid-shell is put to a high precision test in this series of measurements. Lifetimes of the 2+1 states in 168Hf and 174W have been measured using the newly developed LaBr3 scintillation detectors. The excellent energy resolution in conjunction with superb time properties of the new material allows for reliable handling of background, which is a source of systematic error in such experiments. Preliminary lifetime values are obtained and discussed in the context of previous and ongoing work.
Zdyb, Agata; Krawczyk, Stanisław
2016-03-01
Adsorption of quercetin on colloidal titanium dioxide nanoparticles in ethanol and its excited-state electronic structure were investigated by means of electronic and vibrational spectroscopies. The changes in electronic charge redistribution as reflected by the dipole moment difference, ∆μ, between the ground and excited electronic states were measured with electroabsorption spectroscopy and analyzed using results of TD DFT computations. Adsorption of quercetin causes a red shift of its absorption spectrum. Raman spectra of quercetin analyzed with reference to analogous data for morin indicate binding of quercetin through the hydroxy groups of the catechol moiety. The difference dipole moment, which is 5.5 D in free quercetin, increases to 11.8 D in opposite direction in adsorbed quercetin, and is associated with charge-transfer to the Ti atom. The computed transition energy, intensity, vector Δμ and molecular orbitals involved in the electronic transition at different molecular configurations indicate a bidentate chelating mode of binding of quercetin.
Chong, C; Kim, E; Charalampidis, E G; Kim, H; Li, F; Kevrekidis, P G; Lydon, J; Daraio, C; Yang, J
2016-05-01
This article explores the excitation of different vibrational states in a spatially extended dynamical system through theory and experiment. As a prototypical example, we consider a one-dimensional packing of spherical particles (a so-called granular chain) that is subject to harmonic boundary excitation. The combination of the multimodal nature of the system and the strong coupling between the particles due to the nonlinear Hertzian contact force leads to broad regions in frequency where different vibrational states are possible. In certain parametric regions, we demonstrate that the nonlinear Schrödinger equation predicts the corresponding modes fairly well. The electromechanical model we apply predicts accurately the conversion from the obtained mechanical energy to the electrical energy observed in experiments. PMID:27300876
Hot electron mediated desorption rates calculated from excited state potential energy surfaces
Olsen, Thomas; Schiøtz, Jakob
2008-01-01
We present a model for Desorption Induce by (Multiple) Electronic Transitions (DIET/DIMET) based on potential energy surfaces calculated with the Delta Self-Consistent Field extension of Density Functional Theory. We calculate potential energy surfaces of CO and NO molecules adsorbed on various transition metal surfaces, and show that classical nuclear dynamics does not suffice for propagation in the excited state. We present a simple Hamiltonian describing the system, with parameters obtained from the excited state potential energy surface, and show that this model can describe desorption dynamics in both the DIET and DIMET regime, and reproduce the power law behavior observed experimentally. We observe that the internal stretch degree of freedom in the molecules is crucial for the energy transfer between the hot electrons and the molecule when the coupling to the surface is strong.
Demchenko, Alexander P; Tang, Kuo-Chun; Chou, Pi-Tai
2013-02-01
Charge and proton transfer reactions in the excited states of organic dyes can be coupled in many different ways. Despite the complementarity of charges, they can occur on different time scales and in different directions of the molecular framework. In certain cases, excited-state equilibrium can be established between the charge-transfer and proton-transfer species. The interplay of these reactions can be modulated and even reversed by variations in dye molecular structures and changes of the surrounding media. With knowledge of the mechanisms of these processes, desired rates and directions can be achieved, and thus the multiple emission spectral features can be harnessed. These features have found versatile applications in a number of cutting-edge technological areas, particularly in fluorescence sensing and imaging.
Excitation of high orbital angular momentum Rydberg states with Laguerre-Gauss beams
Rodrigues, J D; Mendonça, J T
2015-01-01
We consider the excitation of Rydberg states through photons carrying an intrinsic orbital angular momentum degree of freedom. Laguerre-Gauss modes, with a helical wave-front structure, correspond to such a set of laser beams, which carry some units of orbital angular momentum in their propagation direction. We demonstrate that, in a proper geometrical setting, this orbital angular momentum can be transferred to the internal degrees of freedom of the atoms, thus violating the standard dipolar selection rules. Higher orbital angular momentum states become accessible through a single photon excitation process. We investigate how the spacial structure of the Laguerre-Gauss beam affects the radial coupling strength, assuming the simplest case of hydrogen-like wavefunctions. Finally we discuss a generalization of the angular momentum coupling, in order to include the effects of the fine and hyperfine splitting, in the context of the Wigner-Eckart theorem.
Excited states in {sup 31}S studied via beta decay of {sup 31}Cl
Energy Technology Data Exchange (ETDEWEB)
Kankainen, A.; Eronen, T.; Hager, U.; Hakala, J.; Huikari, J.; Jokinen, A.; Kopecky, S.; Moore, I.; Nieminen, A.; Penttilae, H.; Rinta-Antila, S.; Wang, Y.; Aeystoe, J. [University of Jyvaeskylae, Department of Physics (Finland); Fox, S.P.; Jenkins, D.G. [University of York, Department of Physics, Heslington, York (United Kingdom); Fynbo, H.O.U. [University of Aarhus, Department of Physics and Astronomy, Aarhus (Denmark); Tengblad, O. [CSIC, Instituto de Estructura de la Materia, Madrid (Spain)
2006-01-15
The beta decay of {sup 31}Cl has been studied with a silicon detector array and a HPGe detector at the IGISOL facility. Previously controversial proton peaks have been confirmed to belong to {sup 31}Cl and a new proton group with an energy of 762(14) keV has been found. Proton captures to this state at 6921(15) keV in {sup 31}S can have an effect on the reaction rate of {sup 30}P(p,{gamma}) in ONe novae. Gamma rays of 1249.1(14) keV and 2234.5(8) keV corresponding to the de-excitations of the first two excited states in {sup 31}S have been measured. No beta-delayed protons from the IAS have been observed. (orig.)
Excitation of high orbital angular momentum Rydberg states with Laguerre-Gauss beams
Rodrigues, J. D.; Marcassa, L. G.; Mendonça, J. T.
2016-04-01
We consider the excitation of Rydberg states through photons carrying an intrinsic orbital angular momentum degree of freedom. Laguerre-Gauss modes, with a helical wave-front structure, correspond to such a set of laser beams, which carry {{\\ell }}0 units of orbital angular momentum in their propagation direction, with ℓ 0 the winding number. We demonstrate that, in a proper geometry setting, this orbital angular momentum can be transferred to the internal degrees of freedom of the atoms, thus violating the standard dipole selection rules. Higher orbital angular momentum states become accessible through a single photon excitation process. We investigate how the spacial structure of the Laguerre-Gauss beam affects the radial coupling strength, assuming the simplest case of hydrogen-like wavefunctions. Finally we discuss a generalization of the angular momentum coupling, in order to include the effects of the fine and hyperfine splitting, in the context of the Wigner-Eckart theorem.
Proteolytic Equilibria of Vanillic Acid in the Ground and Excited States
Vusovich, O. V.; Tchaikovskaya, O. N.; Sokolova, I. V.; Vasil‧eva, N. Yu.
2016-03-01
Proteolytic equilibria of vanillic acid in aqueous solutions were studied using electronic spectroscopy. The pH ranges for anionic, dianionic, cationic, and neutral forms of vanillic acid in the ground and excited states were determined. The electron density distribution on atoms in the proteolytic forms was determined using quantum-chemistry methods. The anion formed as a result of dissociation of the carboxylic acid. The dianion formed in the presence of two and more equivalents of alkali as a result of proton loss from the phenol and carboxylic acid. The vanillic acid cation formed via protonation of the carbonyl oxygen. Differences in spectral features of the proteolytic forms in the ground and excited states were observed.
Importance of local exact exchange potential in hybrid functionals for accurate excited states
Kim, Jaewook; Hwang, Sang-Yeon; Ryu, Seongok; Choi, Sunghwan; Kim, Woo Youn
2016-01-01
Density functional theory has been an essential analysis tool for both theoretical and experimental chemists since accurate hybrid functionals were developed. Here we propose a local hybrid method derived from the optimized effective potential (OEP) method and compare its distinct features with conventional nonlocal ones from the Hartree-Fock (HF) exchange operator. Both are formally exact for ground states and thus show similar accuracy for atomization energies and reaction barrier heights. For excited states, the local version yields virtual orbitals with N-electron character, while those of the nonlocal version have mixed characters between N- and (N+1)-electron orbitals. As a result, the orbital energy gaps from the former well approximate excitation energies with a small mean absolute error (MAE = 0.40 eV) for the Caricato benchmark set. The correction from time-dependent density functional theory with a simple local density approximation kernel further improves its accuracy by incorporating multi-config...
The repopulation of electronic states upon vibrational excitation of niobium carbide clusters.
Chernyy, V; Logemann, R; Bakker, J M; Kirilyuk, A
2016-07-14
We study the infrared (IR) resonant heating of neutral niobium carbide clusters probed through ultraviolet photoionization spectroscopy. The IR excitation not only changes the photoionization spectra for the photon energies above the ionization threshold, but also modulates ion yield for energies significantly below it. An attempt to describe the experimental spectra using either Fowler's theory or thermally populated vibrational states was not successful. However, the data can be fully modeled by vibrationally and rotationally broadened discrete electronic levels obtained from Density Functional Theory (DFT) calculations. The application of this method to spectra with different IR pulse energies not only yields information about the excited electronic states in the vicinity of the HOMO level, populated by manipulation of the vibrational coordinates of a cluster, but also can serve as an extra indicator for the cluster isomeric structure and corresponding DFT-calculated electronic levels. PMID:27421411
The repopulation of electronic states upon vibrational excitation of niobium carbide clusters.
Chernyy, V; Logemann, R; Bakker, J M; Kirilyuk, A
2016-07-14
We study the infrared (IR) resonant heating of neutral niobium carbide clusters probed through ultraviolet photoionization spectroscopy. The IR excitation not only changes the photoionization spectra for the photon energies above the ionization threshold, but also modulates ion yield for energies significantly below it. An attempt to describe the experimental spectra using either Fowler's theory or thermally populated vibrational states was not successful. However, the data can be fully modeled by vibrationally and rotationally broadened discrete electronic levels obtained from Density Functional Theory (DFT) calculations. The application of this method to spectra with different IR pulse energies not only yields information about the excited electronic states in the vicinity of the HOMO level, populated by manipulation of the vibrational coordinates of a cluster, but also can serve as an extra indicator for the cluster isomeric structure and corresponding DFT-calculated electronic levels.
Institute of Scientific and Technical Information of China (English)
LI Yuan-Zuo; SUN Yu; LI Yong-Qing; MA Feng-Cai
2006-01-01
The first fluorine-substituted hexabenzocoronene has been synthesized and its electronic structure and optical properties have been reported [Q. Zhang, et al., Org. Lett.7 (2005) 5019]. In this letter, the electronic structure and excited state properties of the fluorine-substituted hexabenzocoronene are studied with quantum chemistry method as well as the transition and the charge difference densities. The transition densities show the orientations and strength of the dipole moments and the charge difference densities reveal the orientation and results of the intramolecular charge transfer. The calculated transition energies and oscillator strengths are consistent with the experimental data, and the theoretical results of transition and charge difference densities are valuable to understanding the excited state properties of the fluorine-substituted hexabenzocoronene.
Energy Technology Data Exchange (ETDEWEB)
Ou, Qi; Fatehi, Shervin; Alguire, Ethan; Subotnik, Joseph E., E-mail: subotnik@sas.upenn.edu [Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104 (United States); Shao, Yihan [Q-Chem, Inc., 6601 Owens Drive, Suite 105, Pleasanton, California 94588 (United States)
2014-07-14
Working within the Tamm-Dancoff approximation, we calculate the derivative couplings between time-dependent density-functional theory excited states by assuming that the Kohn-Sham superposition of singly excited determinants represents a true electronic wavefunction. All Pulay terms are included in our derivative coupling expression. The reasonability of our approach can be established by noting that, for closely separated electronic states in the infinite basis limit, our final expression agrees exactly with the Chernyak-Mukamel expression (with transition densities from response theory). Finally, we also validate our approach empirically by analyzing the behavior of the derivative couplings around the T{sub 1}/T{sub 2} conical intersection of benzaldehyde.
Quenching of the excited state of hydrated Europium(III) ions by electron transfer
Energy Technology Data Exchange (ETDEWEB)
Christensen, K.
1993-08-01
This thesis explores the oxidation-reduction chemistry of the excited state of Eu(III) ions, *Eu{sub aq}{sup 3+}, in aqueous solutions. Evidence is presented for the quenching of *Eu{sup 3+} by reductive electron transfer. It is concluded that *Eu{sup 3+} is not a strong energy transfer reagent. The reactivity of *Eu{sub aq}{sup 3+} is compared with that of *UO{sub 2}{sup 2+}.
On the excited electronic state dissociation of nitramine energetic materials and model systems
Guo, Y. Q.; Greenfield, M.; Bhattacharya, A.; Bernstein, E. R.
2007-10-01
In order to elucidate the difference between nitramine energetic materials, such as RDX (1,3,5-trinitro-1,3,5-triazacyclohexane), HMX (1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane), and CL-20 (2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane), and their nonenergetic model systems, including 1,4-dinitropiperazine, nitropiperidine, nitropyrrolidine, and dimethylnitramine, both nanosecond mass resolved excitation spectroscopy and femtosecond pump-probe spectroscopy in the UV spectral region have been employed to investigate the mechanisms and dynamics of the excited electronic state photodissociation of these materials. The NO molecule is an initial decomposition product of all systems. The NO molecule from the decomposition of energetic materials displays cold rotational and hot vibrational spectral structures. Conversely, the NO molecule from the decomposition of model systems shows relatively hot rotational and cold vibrational spectra. In addition, the intensity of the NO ion signal from energetic materials is proportional to the number of nitramine functional groups in the molecule. Based upon experimental observations and theoretical calculations of the potential energy surface for these systems, we suggest that energetic materials dissociate from ground electronic states after internal conversion from their first excited states, and model systems dissociate from their first excited states. In both cases a nitro-nitrite isomerization is suggested to be part of the decomposition mechanism. Parent ions of dimethylnitramine and nitropyrrolidine are observed in femtosecond experiments. All the other molecules generate NO as a decomposition product even in the femtosecond time regime. The dynamics of the formation of the NO product is faster than 180fs, which is equivalent to the time duration of our laser pulse.
Coherent excitation transferring via dark state in light-harvesting process
Dong, H.; Xu, D. Z.; Sun, C. P.
2011-01-01
We study the light absorption and energy transferring in a donor-acceptor system with a bionic structure. In the optimal case with uniform couplings, it is found that the quantum dynamics of this seemingly complicated system is reduced as a three-level system of $\\Lambda$-type. With this observation, we show that the dark state based electromagnetically-induced transparency (EIT) effect could enhance the energy transfer efficiency, through a quantum interference effect suppressing the excited...
Energetics of Excited States in the Conjugated Polymer Poly(3-hexylthiophene)
Deibel, Carsten; Mack, Daniel; Gorenflot, Julien; Schoell, Achim; Krause, Stefan; Reinert, Friedrich; Rauh, Daniel; Dyakonov, Vladimir
2010-01-01
There is an enormous potential in applying conjugated polymers in novel organic opto-electronic devices such as light emitting diodes and solar cells. Although prototypes and first products exist, a comprehensive understanding of the fundamental processes and energetics involved during photoexcitation is still lacking and limits further device optimisations. Here we report on a unique analysis of the excited states involved in charge generation by photoexcitation. On the model system poly(3-h...
Electron-phonon interaction and excited states relaxation in carbon nanotubes
Perebeinos, Vasili
2008-03-01
We will discuss the role of electron-phonon interaction on excited states relaxation and phonon spectra in carbon nanotubes (CNTs). The electron-phonon interaction leads to the polaronic effects of the charge carriers, but it also renormalizes the energy and the lifetime of phonons. We present a theoretical model that predicts the changes induced in the phonon modes of CNTs as a function of the charge carrier doping, i.e. position of the Fermi level. In agreement with the predictions, our experiments show sharpening and blue shifts of the G-phonons of metallic CNTs, but only blue shifts for semiconducting CNTs, making the Raman scattering a useful probe of local doping of CNTs [1]. The non-equilibrium dynamics of charge carriers under external electric field is determined by the electron-phonon scattering. The hot carriers under unipolar transport conditions can be produced, leading to the strong impact excitation and light emission, which intensity is determined by electric field, phonon scattering, and impact excitation cross section [2, 3]. In the reverse process of photoconductivity, light is absorbed creating excited states. We will discuss electronic relaxation of high energy excited states leading to the free carriers, contributing to the photoconductivity, and phonon relaxation, leading to the bound excitons [4]. The later can contribute to the photocurrent only after ionization by the external field [5]. Finally, we will discuss the role of phonons in the long puzzling question regarding the nature of the dominant decay channel of the low energy excited states and the potential of optoelectronic applications of CNTs. [1] J.C. Tsang, M. Freitag, V. Perebeinos, J. Liu, and Ph. Avouris, Nature Nanotechnology 2, 725 (2007); [2] J. Chen, V. Perebeinos, M. Freitag, J. Tsang, Q. Fu, J. Liu, Ph. Avouris, Science 310, 1171 (2005); [3] V. Perebeinos and Ph. Avouris, Phys. Rev. B. 74, 121410(R), (2006); [4] T. Hertel, V. Perebeinos, J. Crochet, K. Arnold, M. Kappes
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.
International Nuclear Information System (INIS)
The objective of this contract is the study of state-to-state, electronic energy transfer reactions following two-photon laser excitation. We have chosen to study reactions of Xe 5p5np because of their relevance to the XeCl excimer laser. We are studying deactivation reactions in collisions with heavy atoms such as Ar, Kr, and Xe and reactive collisions with chlorides. The reactants are excited by multiphoton laser absorption. Product channels are observed by their fluorescence, or by laser induced fluorescence using a second color laser. Reaction rates are measured by observing the time dependent decay of signals from reactant and product channels. In addition we measure 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 are obtained in the form of either lineshapes or individual lines from rovibrational transitions of bound states. 11 refs. 4 figs., 3 tabs
Excited states from range-separated density-functional perturbation theory
Rebolini, Elisa; Teale, Andrew M; Helgaker, Trygve; Savin, Andreas
2014-01-01
We explore the possibility of calculating electronic excited states by using perturbation theory along a range-separated adiabatic connection. Starting from the energies of a partially interacting Hamiltonian, a first-order correction is defined with two variants of perturbation theory: a straight-forward perturbation theory, and an extension of the G{\\"o}rling--Levy one that has the advantage of keeping the ground-state density constant at each order in the perturbation. Only the first, simpler, variant is tested here on the helium and beryllium atoms and on the dihydrogene molecule. The first-order correction within this perturbation theory improves significantly the total ground-and excited-state energies of the different systems. However, the excitation energies are mostly deterio-rated with respect to the zeroth-order ones, which may be explained by the fact that the ionization energy is no longer correct for all interaction strengths. The second variant of the perturbation theory should improve these re...
Highlighting short-lived excited electronic states with pump-degenerate-four-wave-mixing.
Marek, Marie S; Buckup, Tiago; Southall, June; Cogdell, Richard J; Motzkus, Marcus
2013-08-21
Detection of short-lived transient species is a major challenge in femtosecond spectroscopy, especially when third-order techniques like transient absorption are used. Higher order methods employ additional interactions between light and matter to highlight such transient species. In this work we address numerically and experimentally the detection of ultrafast species with pump-Degenerate Four Wave Mixing (pump-DFWM). In this respect, conclusive identification of ultrafast species requires the proper determination of time-zero between all four laser pulses (pump pulse and the DFWM sequence). This is addressed here under the light of experimental parameters as well as molecular properties: The role of pulse durations, amount of pulse chirp as well as excited state life time is investigated by measuring a row of natural pigments differing mainly in the number of conjugated double bonds (N = 9 to 13). A comparison of the different signals reveals a strikingly unusual behavior of spheroidene (N = 10). Complete analysis of the pump-DFWM signal illustrates the power of the method and clearly assigns the uniqueness of spheroidene to a mixing of the initially excited state with a dark excited electronic state.
Theoretical direct WIMP detection rates for transitions to nuclear excited states
Vergados, J D; Pirinen, P; Srivastava, P C; Kortelainen, M; Suhonen, J
2015-01-01
The recent WMAP and Planck data have confirmed that exotic dark matter together with the vacuum energy (cosmological constant) dominate in the flat Universe. Many extensions of the standard model provide dark matter candidates, in particular Weakly Interacting Massive Particles (WIMPs). Thus the direct dark matter detection is central to particle physics and cosmology. Most of the research on this issue has hitherto focused on the detection of the recoiling nucleus. In this paper we study transitions to the excited states, possible in some nuclei, which have sufficiently low lying excited states. Examples considered previously were the first excited states of $^{127}$I and $^{129}$Xe. We examine here $^{83}$Kr, which offers some kinematical advantages and is currently considered as a possible target. We find appreciable branching ratios for the inelastic scattering mediated by the spin cross sections, with an inelastic event rate of $4.4\\times 10^{-4}$kg$^{-1}$d$^{-1}$. So, the extra signature of the gamma ra...
Nonadiabtic electron dynamics in densely quasidegenerate states in highly excited boron cluster.
Yonehara, Takehiro; Takatsuka, Kazuo
2016-04-28
Following the previous study on nonadiabatic reaction dynamics including boron clusters [T. Yonehara and K. Takatsuka, J. Chem. Phys. 137, 22A520 (2012)], we explore deep into highly excited electronic states of the singlet boron cluster (B12) to find the characteristic features of the densely quasi-degenerate electronic state manifold, which undergo very frequent nonadiabatic transitions and thereby intensive electronic state mixing among very many of the relevant states. So much so, isolating the individual adiabatic states and tracking the expected potential energy surfaces both lose the physical sense. This domain of molecular situation is far beyond the realm of the Born-Oppenheimer approximation. To survey such a violent electronic state-mixing, we apply a method of nonadiabatic electron wavepacket dynamics, the semiclassical Ehrenfest method. We have tracked those electron wavepackets and found the electronic state mixing looks like an ultrafast diffusion in the Hilbert space, which results in huge fluctuation. Furthermore, due to such a violent mixing, the quantum phases associated with the electronic states are swiftly randomized, and consequently the coherence among the electronic states are lost quickly. Besides, these highly excited states are mostly of highly poly-radical nature, even in the spin singlet manifold and the number of radicals amounts up to 10 electrons in the sense of unpaired electrons. Thus the electronic states are summarized to be poly-radical and decoherent with huge fluctuation in shorter time scales of vibrational motions. The present numerical study sets a theoretical foundation for unknown molecular properties and chemical reactivity of such densely quasi-degenerate chemical species. PMID:27131547
Ab Initio Investigations of the Excited Electronic States of CaOCa
Fawzy, Wafaa M.; Heaven, Michael
2016-06-01
Chemical bonding in alkaline earth hypermetalic oxides is of fundamental interest. Previous Ab initio studies of CaOCa predicted a centrosymmetric linear geometry for both the 1Σg^+ ground state and the low lying triplet 3Σu^+ state. However, there have been no reports concerning the higher energy singlet and triplet states. The present work is focused on characterization of the potential energy surface (PES) of the excited 1Σu^+ state (assuming a centrosymmetric linear geometry) and obtaining predictions for the 1Σu^+←1Σg^+ vibronic transitions. We employed the multireference configuration interaction (MRCISD) method with state-averaged, full-valence complete active space self-consistent field (SA-FV-CASSCF) wavefunctions. In these calculations, the active space consisted of ten valence electrons in twelve orbitals, where all the valence electrons were correlated. Contributions of higher excitation and relativistic effects were taken into account using the Davidson correction and the Douglas-Kroll (DK) Hamiltonian, respectively. The correlation-consistent polarized weighed core-valence quadruple zeta basis set (cc-pwCVQZ-DK) was used for all three atoms. The full level of theory is abbreviated as SA-FV-CASSCF (10,12)-MRCISD-Q/cc-pwCVQZ-DK. The calculations were carried out using the MOLPRO2012 suite of programs. For the centrosymmetric linear geometry in all states, initial investigations of one-dimensional radial cuts provided equilibrium bond distances of 2.034 {Å}, 2.034 {Å}, and 1.999 {Å} for the 1Σg^+ , 3Σu^+ , and 1Σu^+ states, respectively. The vertical excitation frequency of the 1Σu^+←1Σg^+ optical transition was calculated to occur at 14801 wn. These predictions were followed by spectroscopic searches by Heaven et al. Indeed, rotationally resolved vibronic progressions were recorded in the vicinity of the predicted electronic band origin. Calculation of the three-dimensional PES showed that the potential minimum in the 1Σu^+ corresponds
Recent results related to excited states of 6Be and 10He
Directory of Open Access Journals (Sweden)
Wolski R.
2012-12-01
Full Text Available The 1H(6Li, 6Ben charge-exchange reaction and the 3H(8He,p10He two-neutron transfer reaction were recently carried out at the ACCULINNA fragment separator (FLNR, Dubna to populate the ground and excited states of 6Be and 10He nuclei, respectively. The 6Be ET spectrum (ET is the 6Be energy above its 4He+p+p decay threshold was obtained with high statistics and described by the well-known 0+ ground state of 6Be at ET = 1.37 MeV, the 2+ state at ET = 3.05 MeV and a broad structure extending from 4 to 16 MeV which could be interpreted as the isovector soft dipole mode associated with the 6Li ground state. In the 10He case the 0+ ground state was found at about 2.1(2 MeV (Γ ~ 2 MeV above the 8He+n+n breakup threshold. Angular correlations observed for 10He decay products show prominent interference patterns allowing to draw conclusions about the structure of low-energy excited states: 1-(ET ~ 5 MeV and 2+ (ET ~ 6 MeV.
Hybrid CIS-DFT method to study electric field effects on electronic excited states of ethylene
Institute of Scientific and Technical Information of China (English)
Ma Mei-Zhong; Zhu Zheng-He; Chen Xiao-Jun; Xu Guo-Liang; Zhang Yong-Bin; Mao Hua-Ping; Shen Xiao-Hong
2005-01-01
The present work is devoted to the study of the effects of external dipole electric field on the molecular structure of ethylene using a hybrid method which combines the single-excitation configuration interactions (CIS) with density functional theory (DFT), i.e. CIS-DFT(B3LYP). It is found that the effects of electric dipole field on the molecular geometry (D2h, D2d and C2v), dipole moment, transition dipole moment, polarizability and, particularly, excitation energy of ethylene are remarkable. The advantages of the hybrid CIS-DFT method are that it can determine the symmetry of molecule and the correct order of excitation as well as the Molecular Orbital (MO) electron configuration;thereby the electronic excitation states of ethylene are easily derived, and most of them are in agreement with those obtained in experiments or references. It may be the first time the effects of external electric field on ethylene molecule have been considered. Compared with other ab initio methods, the CIS-DFT method is relatively accurate and low cost in computation. We expect that it can be used to study other closed-shell molecules.
Photoluminescence and excited states dynamics in PbWO4:Pr3+ crystals
Auffray, E; Shalapska, T; Zazubovich, S
2014-01-01
Luminescence and photo-thermally stimulated defects creation processes are studied for a Pr3+-doped PbWO4 crystal at 4.2-400 K under excitation in the band-to-band, exciton, and charge-transfer transitions regions, as well as in the Pr3+-related absorption bands. Emission spectra of Pr3+ centers depend on the excitation energy, indicating the presence of Pr3+ centers of two types. The origin of these centers is discussed. The 2.03-2.06 eV emission, arising from the D-1(2) -> H-3(4) transitions of Pr3+ ions, is found to be effectively excited in a broad intense absorption band peaking at 4.2 K at 3.92 eV. By analogy with some other Pe(3+)-doped compounds, this band is suggested to arise from an electron transfer from an impurity Pr3+ ion to the crystal lattice W6+ or Pb2+ ions. The dynamics of the Pr3+-related excited states is clarified. In the PbWO4:Pr crystal studied, the concentration of single oxygen and lead vacancies as traps for electrons and holes is found to be negligible.
Energy Technology Data Exchange (ETDEWEB)
Rozet, J.P.; Politis, M.F.; Blumenfeld, L.; Vernhet, D.; Wohrer, K.; Touati, A.; Stephan, C.; Chetioui, A.; Roncin, P.; Laurent, H.
1987-12-01
Autoionization branching ratios of O/sup 6+/ doubly excited states are shown to depend sensitively on the K, T and L quantum numbers of these states. A measurement of the decay probabilities to 2s and 2p sublevels has been performed for the (3, 3) and (3, 4) doubly excited states populated in the 1.3 keV/u O/sup 8+/ -> He collision. A new technique of X-ray, energy gain coincidence has been used. Results are discussed in terms of possible distributions K, L for the doubly excited states.
Decoherence of quantum excitation of even/odd coherent states in thermal environment
Indian Academy of Sciences (India)
Mohammadbeigi A; Tavassoly M K
2016-04-01
In this paper, we study the decoherence of quantum excitation (photon-added)even/odd coherent states, $((\\^{a})^m|\\alpha_{\\pm}\\rangle)$, in a thermal environment by investigating the variation of negative part of the Wigner quasidistribution function vs. the rescaled time. For this purpose, at first we obtain the time-dependent Wigner function corresponding to the mentioned states in the framework of standard master equation. Then, the time evolution of the Wigner function associated with photon-added even/odd coherent states, as well as the number of added photons $m$ are analysed. It is shown that, in both states, the negative part of the Wigner function decreases with time. By deriving the threshold value of the rescaled time for single photon-added even/odd coherent states, it is also found that, if the rescaled time exceeds the threshold value, the associated Wigner function becomes positive, i.e., the decoherence occurs completely.
Keane, Páraic M; Baptista, Frederico R; Gurung, Sarah P; Devereux, Stephen J; Sazanovich, Igor V; Towrie, Michael; Brazier, John A; Cardin, Christine J; Kelly, John M; Quinn, Susan J
2016-05-01
UV-generated excited states of cytosine (C) nucleobases are precursors to mutagenic photoproduct formation. The i-motif formed from C-rich sequences is known to exhibit high yields of long-lived excited states following UV absorption. Here the excited states of several i-motif structures have been characterized following 267 nm laser excitation using time-resolved infrared spectroscopy (TRIR). All structures possess a long-lived excited state of ∼300 ps and notably in some cases decays greater than 1 ns are observed. These unusually long-lived lifetimes are attributed to the interdigitated DNA structure which prevents direct base stacking overlap.
International Nuclear Information System (INIS)
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
Ab Initio Inverstagation of the Excited States of Nucleobases and Nucleosides
Szalay, Péter G.; Fogarasi, Géza; Watson, Thomas; Perera, Ajith; Lotrich, Victor; Bartlett, Rod J.
2011-06-01
Most living bodies are exposed to sunlight, essential life sustaining processes are using this natural radiation. Sunlight has, however, several components (has a broad "spectrum") and in particular the invisible component (UV, ultraviolet) is harmful for living organisms. Scientists around the word are busy to understand what happens in the cell when it is exposed to light: it seems that the building blocks of cells and in particular those carrying the genetic information (DNA and RNA) are highly protected against this exposition. Our research focuses on the spectral properties of the building blocks of DNA and RNA, the so called nucleobases and nucleosides, in order to understand this mechanism. Due to improvement in computer technology both at hardware and software side we are now able to use the most accurate methods of ab initio quantum chemistry to investigate the spectroscopic properties of these building blocks. These calculations provide direct information on the properties of these molecules but also provide important benchmarks for cheaper methods which can be used for even larger systems. We have calculated the excited state properties for the nucleobases (cytosine, guanine and adenine), their complexes with water and with each other (Watson-Crick base pairs and stacks) as well as corresponding nucleosides at the EOM-CCSD(T)/aug-cc-pVDZ level of theory and try to answer the following questions: (1) how the order of excited states varies in different nucleobases; (2) how hydration influences the excitation energy and order of excited states; (3) is there any effect of the sugar substituent; (4) how do close lying other bases change the spectrum. The calculations involve over hundred correlated electrons and up to thousand basis functions. Such calculations are now routinely available with the recently developed ACESIII code and can make use of hundreds or even several thousand of processors. V. Lotrich, N. Flocke, M. Ponton, A. Yau, A. Perera, E. Deumens
Steady-state responses of a belt-drive dynamical system under dual excitations
Ding, Hu
2016-02-01
The stable steady-state periodic responses of a belt-drive system with a one-way clutch are studied. For the first time, the dynamical system is investigated under dual excitations. The system is simultaneously excited by the firing pulsations of the engine and the harmonic motion of the foundation. Nonlinear discrete-continuous equations are derived for coupling the transverse vibration of the belt spans and the rotations of the driving and driven pulleys and the accessory pulley. The nonlinear dynamics is studied under equal and multiple relations between the frequency of the firing pulsations and the frequency of the foundation motion. Furthermore, translating belt spans are modeled as axially moving strings. A set of nonlinear piecewise ordinary differential equations is achieved by using the Galerkin truncation. Under various relations between the excitation frequencies, the time histories of the dynamical system are numerically simulated based on the time discretization method. Furthermore, the stable steady-state periodic response curves are calculated based on the frequency sweep. Moreover, the convergence of the Galerkin truncation is examined. Numerical results demonstrate that the one-way clutch reduces the resonance amplitude of the rotations of the driven pulley and the accessory pulley. On the other hand, numerical examples prove that the resonance areas of the belt spans are decreased by eliminating the torque-transmitting in the opposite direction. With the increasing amplitude of the foundation excitation, the damping effect of the one-way clutch will be reduced. Furthermore, as the amplitude of the firing pulsations of the engine increases, the jumping phenomena in steady-state response curves of the belt-drive system with or without a one-way clutch both occur.
Electron impact excitation of the states of Mg, Ca and Sr atoms: Complete experiment results
Indian Academy of Sciences (India)
Sachin Saxena; Kshamata Muktavat; Rajesh Srivastava
2004-11-01
We have used non-relativistic and relativistic distorted wave approximation methods to study the excitation of the 1 states of magnesium ( = 3), calcium ( = 4) and strontium ( = 5) from the ground 1 state. Calculations have been performed for the complete set of parameters $(, \\tilde{L}_{\\bot}^{+}, \\tilde{L}_{\\bot}^{-}, \\tilde{}^{+}, \\tilde{}^{-})$. The results are presented for electron impact energies of 20 and 40 eV. We compare our results obtained from both the non-relativistic and relativistic methods with each other. Good agreement is found on comparison and the importance of relativistic effects is also explored.
Low-lying states and isospin excitation in the Ge isotopes
Institute of Scientific and Technical Information of China (English)
Falih H. Al-Khudair
2009-01-01
The level structure of 64-70Ge isotopes has been studied within the framework of the interacting boson model-3 (IBM-3). The symmetry character in the proton and neutron degrees of freedom of the energy levels has been investigated. The isospin excitation states (T>Tz) have been assigned for the 64Ge (N=Z) nucleus. Some intruder states in these nuclei have been suggested. The calculated energy levels and transition probabilities are in good agreement with recent experimental data. The study indicates that the Ge isotopes are in transition from γ-unstable to vibrational.
Doubly excited 3Pe resonance states of two-electron positive ions in Debye plasmas
International Nuclear Information System (INIS)
We investigate the doubly excited 3Pe resonance states of two-electron positive ions Li+, Be2+, B3+, and C4+ by employing correlated exponential wave functions. In the framework of the stabilization method, we calculate two series (3pnp and 3dnd) of 3Pe resonances below the N = 3 threshold. The 3Pe resonance parameters (resonance energies and widths) are reported for the first time as a function of the screening parameter. For free-atomic cases, comparisons are made with the reported results and few resonance states are reported for the first time
Excited state Faraday anomalous dispersion optical filters based on indirect laser pumping.
Yin, Longfei; Luo, Bin; Chen, Zhongjie; Zhong, Lei; Guo, Hong
2014-02-15
The direct pump method now used in excited state Faraday anomalous dispersion optical filters (ES-FADOFs) requires that the transition between the target and the ground state is an electric dipole allowed transition and that a laser that operates at the exact pump wavelength is available. This is not always satisfied in practice. An indirect laser pump method for ES-FADOF is proposed and experimentally realized. Compared with the commonly used direct pump method, this indirect pump method can reach the same performance using lasers at very different wavelengths. This method can greatly extend the wavelength range of FADOF and provide a novel scheme for ES-FADOF design. PMID:24562221
Excited hadrons and the analytical structure of bound-state interaction kernels
El-Bennich, Bruno; Rojas, Eduardo; Serna, Fernando E
2016-01-01
We highlight Hermiticity issues in bound-state equations whose kernels are subject to a highly asymmetric mass and momentum distribution and whose eigenvalue spectrum becomes complex for radially excited states. We trace back the presence of imaginary components in the eigenvalues and wave functions to truncation artifacts and suggest how they can be eliminated in the case of charmed mesons. The solutions of the gap equation in the complex plane, which play a crucial role in the analytic structure of the Bethe-Salpeter kernel, are discussed for several interaction models and qualitatively and quantitatively compared to analytic continuations by means of complex-conjugate pole models fitted to real solutions.
Zhao, Luning; Neuscamman, Eric
2016-08-01
An equation of motion formalism for excited states in variational Monte Carlo is derived, and a pilot implementation for the Jastrow-modified antisymmetric geminal power is tested. In single excitations across a range of small molecules, this combination is shown to be intermediate in accuracy between configuration interaction singles and equation of motion coupled cluster with singles and doubles. For double excitations, energy errors are found to be similar to those for coupled cluster. PMID:27398808
Zhao, Luning
2016-01-01
An equation of motion formalism for excited states in variational Monte Carlo is derived and a pilot implementation for the Jastrow-modified antisymmetric geminal power is tested. In single excitations across a range of small molecules, this combination is shown to be intermediate in accuracy between configuration interaction singles and equation of motion coupled cluster with singles and doubles. For double excitations, energy errors are found to be similar to those for coupled cluster.
Excited state absorption of Cr/sup 3+/ in low field crystalline hosts
International Nuclear Information System (INIS)
A simple single configuration coordinate crystal field model has been developed to predict the excited state absorption (ESA) spectra of Cr/sup +3/ in hosts where the /sup 4/T/sub 2g/ is the lowest excited state. Two spin allowed transitions are predicted to lie near 19,000 and 7,000 cm/sup -1/ for Cr/sup 3+/ in a typical fluoride host. On the other hand, ESA from a /sup 2/E lowest excited state is more complex having a number of near infrared and visible transitions to a rich manifold of high energy doublets. To corroborate the model, ESA measurements have been made on GSGG:Cr, GSAG:Cr and K/sub 2/NaScF/sub 6/:Cr over the range 250 nm to 1,750 nm. The higher energy ESA transition was located near 19,000 cm/sup -1/ and is accompanied by bleaching of the strong ground state transitions at 15,500 and 22,000 cm/sup -1/. The lower energy transition was found centered at 8,000 cm/sup -1/ and to be far broader than predicted by a single configuration coordinate model. In addition to these crystal field transitions, intense charge transfer bands were found at 31,000 and 32,000 cm/sup -1/ for GSGG:Cr and GSAG:Cr, respectively, but they are not present in this region for the elpasolite. The peculiar band shape of these charge-transfer transitions suggest that the terminal state of the transition is the host conduction band. Finally, saturation experiments were made at 632.8 nm in order to determine ESA cross sections. Threshold for damage and thermal lensing was found to be near 10 Mwatt/cm/sup 2/ for GSGG, consequently only partial saturation could be achieved. ESA cross sections were extracted from these data with a coupled three level kinetic model
2νββ decay of 76Ge into excited states with GERDA phase I
GERDA Collaboration; Agostini, M.; Allardt, M.; Bakalyarov, A. M.; Balata, M.; Barabanov, I.; Barros, N.; Baudis, L.; Bauer, C.; Becerici-Schmidt, N.; Bellotti, E.; Belogurov, S.; Belyaev, S. T.; Benato, G.; Bettini, A.; Bezrukov, L.; Bode, T.; Borowicz, D.; Brudanin, V.; Brugnera, R.; Budjáš, D.; Caldwell, A.; Cattadori, C.; Chernogorov, A.; D'Andrea, V.; Demidova, E. V.; di Vacri, A.; Domula, A.; Doroshkevich, E.; Egorov, V.; Falkenstein, R.; Fedorova, O.; Freund, K.; Frodyma, N.; Gangapshev, A.; Garfagnini, A.; Gooch, C.; Grabmayr, P.; Gurentsov, V.; Gusev, K.; Hegai, A.; Heisel, M.; Hemmer, S.; Heusser, G.; Hofmann, W.; Hult, M.; Inzhechik, L. V.; Janicskó Csáthy, J.; Jochum, J.; Junker, M.; Kazalov, V.; Kihm, T.; Kirpichnikov, I. V.; Kirsch, A.; Klimenko, A.; Knöpfle, K. T.; Kochetov, O.; Kornoukhov, V. N.; Kuzminov, V. V.; Laubenstein, M.; Lazzaro, A.; Lebedev, V. I.; Lehnert, B.; Liao, H. Y.; Lindner, M.; Lippi, I.; Lubashevskiy, A.; Lubsandorzhiev, B.; Lutter, G.; Macolino, C.; Majorovits, B.; Maneschg, W.; Medinaceli, E.; Mi, Y.; Misiaszek, M.; Moseev, P.; Nemchenok, I.; Palioselitis, D.; Panas, K.; Pandola, L.; Pelczar, K.; Pullia, A.; Riboldi, S.; Rumyantseva, N.; Sada, C.; Salathe, M.; Schmitt, C.; Schneider, B.; Schreiner, J.; Schulz, O.; Schwingenheuer, B.; Schönert, S.; Schütz, A.-K.; Selivanenko, O.; Shirchenko, M.; Simgen, H.; Smolnikov, A.; Stanco, L.; Stepaniuk, M.; Ur, C. A.; Vanhoefer, L.; Vasenko, A. A.; Veresnikova, A.; von Sturm, K.; Wagner, V.; Walter, M.; Wegmann, A.; Wester, T.; Wilsenach, H.; Wojcik, M.; Yanovich, E.; Zavarise, P.; Zhitnikov, I.; Zhukov, S. V.; Zinatulina, D.; Zuber, K.; Zuzel, G.
2015-11-01
Two neutrino double beta decay of {}76{Ge} to excited states of {}76{Se} has been studied using data from Phase I of the GERDA experiment. An array composed of up to 14 germanium detectors including detectors that have been isotopically enriched in {}76{Ge} was deployed in liquid argon. The analysis of various possible transitions to excited final states is based on coincidence events between pairs of detectors where a de-excitation γ ray is detected in one detector and the two electrons in the other. No signal has been observed and an event counting profile likelihood analysis has been used to determine Frequentist 90% C.L. bounds for three transitions: {0}{{g}.{{s}}.}+-{2}1+: {T}1/22ν \\gt 1.6× {10}23 yr, {0}{{g}.{{s}}.}+-{0}1+: {T}1/22ν \\gt 3.7× {10}23 yr and {0}{{g}.{{s}}.}+-{2}2+: {T}1/22ν \\gt 2.3× {10}23 yr. These bounds are more than two orders of magnitude larger than those reported previously. Bayesian 90% credibility bounds were extracted and used to exclude several models for the {0}{{g}.{{s}}.}+-{0}1+ transition.
Excited states of hypernuclei (populated by low energetic separated K- beam)
Bamberger, A; Haddock, R; Lynen, U; Moszkowski, S; Piekarz, H; Piekarz, J; Pniewski, J; Povh, B; Ritter, H G; Soergel, Volker; Van Oers, W T H
1972-01-01
The experimental investigation of hypernuclei up to now has been done using emulsions and bubble chambers and therefore, with only 2 exemptions, all existing knowledge concerns hypernuclear ground states. The investigation of excited states in general is only possible using counter techniques, but these experiments could not be performed due to the low intensity of available K/sup -/-beams. At CERN a low energetic separated K-beam has been built, at which 1000 K /sup -/-mesons per burst can be stopped in a target of 6g/cm/sup 2/ thickness. At this beam an experiment looking for gamma -transitions in excited hypernuclei has been performed. In order to eliminate background gamma -radiation arising from kappa /sup -/ annihilation and de-excitation of residual nuclei, only light targets were used, namely /sup 6/Li, /sup 7/Li, /sup 9/Be, /sup 12/C and /sup 16/O. Hypernuclear transitions were found in /sup 4//sub Lambda /H and /sup 4//sub Lambda /He and possible transitions in /sup 6/Li and /sup 7/Li. The scatterin...
Long-range states in excited ultracold 3He*-4He* dimers
Cocks, Daniel G; Whittingham, Ian B
2014-01-01
Long-range bound states of the excited heteronuclear 3He*--4He* system that dissociate to either 3He(1s2s 3S_1) + 4He(1s2p 3P_j) or 3He(1s2p 3P_j) + 4He(1s2s 3S_1), where j=0, 1, 2, are investigated using both single-channel and multichannel calculations in order to analyse the effects of Coriolis and non-adiabatic couplings. The multichannel calculations predict two groups of resonances above the lowest asymptotic energy. One of these groups dissociates to an atomic pair with the 2p excitation on the fermionic atom and the other dissociates to two asymptotes which correspond to the 2p excitation on either atom. Many of these resonances could be identified with levels in the single-channel calculation although the differences in energies were large. The total parity was found to have a significant influence on the ability to make these identifications. No purely bound states were found, although several resonances with line widths smaller than 1 MHz were obtained.
Selective excitation in a three-state system using a hybrid adiabatic-nonadiabatic interaction
Song, Yunheung; Lee, Han-gyeol; Jo, Hanlae; Ahn, Jaewook
2016-08-01
The chirped-pulse interaction in the adiabatic coupling regime induces cyclic permutations of the energy states of a three-level system in the V -type configuration, which process is known as the three-level chirped rapid adiabatic passage (RAP). Here we show that a spectral hole in a chirped pulse can turn on or off the level mixing at adiabatic crossing points of this process, reducing the system to an effective two-level system. The given hybrid adiabatic-nonadiabatic transition enables selective excitation of the three-level system, controlled by the laser intensity and spectral position of the hole, as well as the sign of the chirp parameter. Experiments performed with shaped femtosecond laser pulses and the three lowest energy levels (5 S1 /2 , 5 P1 /2 , and 5 P3 /2 ) of atomic rubidium (Rb) show good agreement with the theoretically analyzed dynamics. The result indicates that our method, when being combined with the ordinary chirped RAP, implements an adiabatic transition between the Raman-coupled excited states. Furthermore, our laser intensity-dependent control may have applications including selective excitations of atoms or ions arranged in space when being used in conjunction with laser beam profile programming.
Suo, Bingbing; Han, Huixian
2014-01-01
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 states for four spin-orbit components 1/2, 3/2, 5/2, and 7/2 are calculated intensively to clarify the ground state of IrO. Our calculation suggests that the ground state is of 1/2 spin-orbit component, which is highly mixed with $^4\\Sigma^-$ and $^2\\Pi$ states in $\\Lambda-S$ notation. The two low-lying states of the 5/2 and 7/2 spin-orbit components are nearly degenerate with the ground state and locate only 234 and 260 cm$^{-1}$ above, respectively. The equilibrium bond length 1.712 \\AA \\ and harmonic vibrational frequency 903 cm$^{-1}$ of the 5/2 spin-orbit component are close to the experimental measurement of 1.724 \\AA \\ and 909 cm$^{-1}$, which suggests the 5/2 state should be the low-lying state contributed to spectra in experimental study. Moreover, the electronic states that give rise to the observed trans...
Characterization of excited-state reactions with instant spectra of fluorescence kinetics
International Nuclear Information System (INIS)
Comprehensible knowledge of the excited-state proton transfer processes in organic compounds is overwhelmingly important not only for physics, but also chemistry and Life Sciences, since they play a key role in main processes of photosynthesis and functioning of biological organisms. Moreover compounds with Excited-State Intramolecular Proton Transfer (ESIPT) are in the focus of the interest of scientists throughout the world, because dual fluorescence spectra of such objects corresponding to two forms of molecular structure (normal and photoproduct) are very sensitive to characteristics of molecular microenvironment. This property allows to use such substances as fluorescent probes for diverse applications in chemistry and Life Sciences. But at the same time studying of proton transfer processes is not simple, because this process is characterized by extremely fast times (on picoseconds time scale and less order) and very often contribution of reverse reactions is essentially complicates an interpretation of observed properties of dual fluorescence. Hence, understanding of a role of reversible reactions is crucial for a comprehensive description of all processes accompanying excited state reactions. We discuss new approach for treatment ESIPT reaction on the basis of experimentally measured instant spectra of dual fluorescence and temporal behavior of ratiometric signal of normal to tautomer form intensities. Simple analytical expressions show in transparent way how to distinguish a degree of reverse reaction contribution to ratiometric signal. A validation of the approach under consideration is fulfilled with two different flavonols – 3-hydroxyflavone and 4′-(Dimethylamino)-3-hydroxyflavone – representing two extreme cases in affecting reversible reaction on dual emission. A comparing of new approach and traditional method when we analyze kinetics of separate the N* and T* fluorescence bands decays, has been carried out. - Highlights: • The excited-state
Characterization of excited-state reactions with instant spectra of fluorescence kinetics
Energy Technology Data Exchange (ETDEWEB)
Tomin, Vladimir I., E-mail: tomin@apsl.edu.pl; Ushakou, Dzmitryi V.
2015-10-15
Comprehensible knowledge of the excited-state proton transfer processes in organic compounds is overwhelmingly important not only for physics, but also chemistry and Life Sciences, since they play a key role in main processes of photosynthesis and functioning of biological organisms. Moreover compounds with Excited-State Intramolecular Proton Transfer (ESIPT) are in the focus of the interest of scientists throughout the world, because dual fluorescence spectra of such objects corresponding to two forms of molecular structure (normal and photoproduct) are very sensitive to characteristics of molecular microenvironment. This property allows to use such substances as fluorescent probes for diverse applications in chemistry and Life Sciences. But at the same time studying of proton transfer processes is not simple, because this process is characterized by extremely fast times (on picoseconds time scale and less order) and very often contribution of reverse reactions is essentially complicates an interpretation of observed properties of dual fluorescence. Hence, understanding of a role of reversible reactions is crucial for a comprehensive description of all processes accompanying excited state reactions. We discuss new approach for treatment ESIPT reaction on the basis of experimentally measured instant spectra of dual fluorescence and temporal behavior of ratiometric signal of normal to tautomer form intensities. Simple analytical expressions show in transparent way how to distinguish a degree of reverse reaction contribution to ratiometric signal. A validation of the approach under consideration is fulfilled with two different flavonols – 3-hydroxyflavone and 4′-(Dimethylamino)-3-hydroxyflavone – representing two extreme cases in affecting reversible reaction on dual emission. A comparing of new approach and traditional method when we analyze kinetics of separate the N* and T* fluorescence bands decays, has been carried out. - Highlights: • The excited-state
Parkin, E R
2012-01-01
Global three dimensional magnetohydrodynamic (MHD) simulations of turbulent accretion disks are presented which start from fully equilibrium initial conditions in which the magnetic forces are accounted for and the induction equation is satisfied. The local linear theory of the magnetorotational instability (MRI) is used as a predictor of the growth of magnetic field perturbations in the global simulations. The linear growth estimates and global simulations diverge when non-linear motions - perhaps triggered by the onset of turbulence - upset the velocity perturbations used to excite the MRI. The saturated state is found to be independent of the initially excited MRI mode, showing that once the disk has expelled the initially net flux field and settled into quasi-periodic oscillations in the toroidal magnetic flux, the dynamo cycle regulates the global saturation stress level. Furthermore, time-averaged measures of converged turbulence, such as the ratio of magnetic energies, are found to be in agreement with...
Vibrational dynamics of aniline (N2)1 clusters in their first excited singlet state
Hineman, M. F.; Kim, S. K.; Bernstein, E. R.; Kelley, D. F.
1992-04-01
The first excited singlet state S1 vibrational dynamics of aniline(N2)1 clusters are studied and compared to previous results on aniline(CH4)1 and aniline(Ar)1. Intramolecular vibrational energy redistribution (IVR) and vibrational predissociation (VP) rates fall between the two extremes of the CH4 (fast IVR, slow VP) and Ar (slow IVR, fast VP) cluster results as is predicted by a serial IVR/VP model using Fermi's golden rule to describe IVR processes and a restricted Rice-Ramsperger-Kassel-Marcus (RRKM) theory to describe unimolecular VP rates. The density of states is the most important factor determining the rates. Two product states, 00 and 10b1, of bare aniline and one intermediate state ˜(00) in the overall IVR/VP process are observed and time resolved measurements are obtained for the 000 and ˜(000) transitions. The results are modeled with the serial mechanism described above.
Cao, Jun; Xie, Zhi-Zhong; Yu, Xiaodong
2016-08-01
In the present work, the combined electronic structure calculations and surface hopping simulations have been performed to investigate the excited-state decay of the parent oxazole in the gas phase. Our calculations show that the S2 state decay of oxazole is an ultrafast process characterized by the ring-opening and ring-closure of the five-membered oxazole ring, in which the triplet contribution is minor. The ring-opening involves the Osbnd C bond cleavage affording the nitrile ylide and airine intermediates, while the ring-closure gives rise to a bicyclic species through a 2sbnd 5 bond formation. The azirine and bicyclic intermediates in the S0 state are very likely involved in the phototranspositions of oxazoles. This is different from the previous mechanism in which these intermediates in the T1 state have been proposed for these phototranspositions.
Extended M1 sum rule for excited symmetric and mixed-symmetry states in nuclei
Smirnova, N A; Leviatan, A; Ginocchio, J N; Fransen, C
2002-01-01
A generalized M1 sum rule for orbital magnetic dipole strength from excited symmetric states to mixed-symmetry states is considered within the proton-neutron interacting boson model of even-even nuclei. Analytic expressions for the dominant terms in the B(M1) transition rates from the first and second $2^+$ states are derived in the U(5) and SO(6) dynamic symmetry limits of the model, and the applicability of a sum rule approach is examined at and in-between these limits. Lastly, the sum rule is applied to the new data on mixed-symmetry states of 94Mo and a quadrupole d-boson ratio $nd(0^+_1)/nd(2^+_2) \\approx 0.6$ is obtained in a largely parameter-independent way
Souza, Adelmo S.; Nunes, Luiz A. O.; Silva, Ivan G. N.; Oliveira, Fernando A. M.; da Luz, Leonis L.; Brito, Hermi F.; Felinto, Maria C. F. C.; Ferreira, Rute A. S.; Júnior, Severino A.; Carlos, Luís D.; Malta, Oscar L.
2016-02-01
Temperature measurements ranging from a few degrees to a few hundreds of Kelvin are of great interest in the fields of nanomedicine and nanotechnology. Here, we report a new ratiometric luminescent thermometer using thermally excited state absorption of the Eu3+ ion. The thermometer is based on the simple Eu3+ energy level structure and can operate between 180 and 323 K with a relative sensitivity ranging from 0.7 to 1.7% K-1. The thermometric parameter is defined as the ratio between the emission intensities of the 5D0 --> 7F4 transition when the 5D0 emitting level is excited through the 7F2 (physiological range) or 7F1 (down to 180 K) level. Nano and microcrystals of Y2O3:Eu3+ were chosen as a proof of concept of the operational principles in which both excitation and detection are within the first biological transparent window. A novel and of paramount importance aspect is that the calibration factor can be calculated from the Eu3+ emission spectrum avoiding the need for new calibration procedures whenever the thermometer operates in different media.Temperature measurements ranging from a few degrees to a few hundreds of Kelvin are of great interest in the fields of nanomedicine and nanotechnology. Here, we report a new ratiometric luminescent thermometer using thermally excited state absorption of the Eu3+ ion. The thermometer is based on the simple Eu3+ energy level structure and can operate between 180 and 323 K with a relative sensitivity ranging from 0.7 to 1.7% K-1. The thermometric parameter is defined as the ratio between the emission intensities of the 5D0 --> 7F4 transition when the 5D0 emitting level is excited through the 7F2 (physiological range) or 7F1 (down to 180 K) level. Nano and microcrystals of Y2O3:Eu3+ were chosen as a proof of concept of the operational principles in which both excitation and detection are within the first biological transparent window. A novel and of paramount importance aspect is that the calibration factor can be
Greenfield, Margo
Energetic materials play an important role in aeronautics, the weapon industry, and the propellant industry due to their broad applications as explosives and fuels. RDX (1,3,5-trinitrohexahydro-s-triazine), HMX (octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine), and CL-20 (2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane) are compounds which contain high energy density. Although RDX and HMX have been studied extensively over the past several decades a complete understanding of their decomposition mechanisms and dynamics is unknown. Time of flight mass spectroscopy (TOFMS) UV photodissociation (ns) experiments of gas phase RDX, HMX, and CL-20 generate the NO molecule as the initial decomposition product. Four different vibronic transitions of the initial decomposition product, the NO molecule, are observed: A2Sigma(upsilon'=0)←X 2pi(upsilon"=0,1,2,3). Simulations of the rovibronic intensities for the A←X transitions demonstrate that NO dissociated from RDX, HMX, and CL-20 is rotationally cold (˜20 K) and vibrationally hot (˜1800 K). Conversely, experiments on the five model systems (nitromethane, dimethylnitramine (DMNA), nitropyrrolidine, nitropiperidine and dinitropiperazine) produce rotationally hot and vibrationally cold spectra. Laser induced fluorescence (LIF) experiments are performed to rule out the possible decomposition product OH, generated along with NO, perhaps from the suggested HONO elimination mechanism. The OH radical is not observed in the fluorescence experiments, indicating the HONO decomposition intermediate is not an important pathway for the excited electronic state decomposition of cyclic nitramines. The NO molecule is also employed to measure the dynamics of the excited state decomposition. A 226 nm, 180 fs light pulse is utilized to photodissociate the gas phase systems. Stable ion states of DMNA and nitropyrrolidine are observed while the energetic materials and remaining model systems present the NO molecule as the only
Energy Technology Data Exchange (ETDEWEB)
Natsume, Yuhei; Tada, Shinichiro; Suzuki, Toshihiko [Chiba Univ., Graduate School of Science and Technology, Chiba (Japan)
2002-06-01
Characteristic properties of excited states in antiferromagnetic ladder systems with spin-1/2 are investigated in relation with the theoretical analysis of the quite asymmetric shape of the peak for twice the spin gap {delta}{sub g} in magnetic Raman spectra. Here, the structure of exchange-scattering spectra are reproduced by the numerical calculation for the finite Heisenberg ladder, in which legs with antiferromagnetic bond J{sub c} is connected by rungs with antiferromagnetic bond J{sub r}. The singlet ground state in this system can be expressed as the ordering of singlet dimers on rungs in the ladder for J{sub c}/J{sub r} {yields} +0. In fact, the value of 0.1 is adopted to be the ratio of J{sub c}/J{sub r} in order to discuss the experimental work of the magnetic Raman spectra for the ladder of V{sup 4+} ions in the oxide compound CaV{sub 2}O{sub 5} reported in Konstantinovic et al., Phys. Rev. B61 (2000), 15185. As for this peak of 2{delta}{sub g}, quite an asymmetric observed shape is explained by the present calculation. According to the analysis of spectra, we discuss the expression of excited states by triplet dimers on rungs: The dominant contribution of the pair of triplet dimers on adjacent rungs to the corresponding state for 2{delta}{sub g} peak is pointed out. (author)
Bogner, Lea; Yang, Zechao; Corso, Martina; Fitzner, Roland; Bäuerle, Peter; Franke, Katharina J; Pascual, José Ignacio; Tegeder, Petra
2015-10-28
Dicyanovinyl (DCV)-substituted oligothiophenes are promising donor materials in vacuum-processed small-molecule organic solar cells. Here, we studied the structural and the electronic properties of DCV-dimethyl-pentathiophene (DCV5T-Me2) adsorbed on Au(111) from submonolayer to multilayer coverages. Using a multi-technique experimental approach (low-temperature scanning tunneling microscopy/spectroscopy (STM/STS), atomic force microscopy (AFM), and two-photon photoemission (2PPE) spectroscopy), we determined the energetic position of several affinity levels as well as ionization potentials originating from the lowest unoccupied molecular orbitals (LUMO) and the highest occupied molecular orbitals (HOMO), evidencing a transport gap of 1.4 eV. Proof of an excitonic state was found to be a spectroscopic feature located at 0.6 eV below the LUMO affinity level. With increasing coverage photoemission from excitonic states gains importance. We were able to track the dynamics of several electronically excited states of multilayers by means of femtosecond time-resolved 2PPE. We resolved an intriguing relaxation dynamics involving four processes, ranging from sub-picosecond (ps) to several hundred ps time spans. These show a tendency to increase with increasing coverage. The present study provides important parameters such as energetic positions of transport levels as well as lifetimes of electronically excited states, which are essential for designing organic-molecule-based optoelectronic devices. PMID:26414934
Tirrito, Emanuele; Ran, Shi-Ju
2016-01-01
We demonstrate an efficient method that allows for simultaneous determination of the ground state, low energy excitation properties and excitation gap in quantum many body systems. To this aim we first use the \\textit{ab-initio} optimization principle of tensor networks (TN), to show that the infinite density matrix renormalization group (iDMRG) in the real space is associated in a natural manner to the infinite time-evolving block decimation (iTEBD) implemented on a continuous matrix product state (MPS), and defined in imaginary time. We illustrate this association showing that the (imaginary) time matrix product state (MPS) in iTEBD reproduces accurately the properties of the two-dimensional (2D) classical Ising model, verifying in this way that the time MPS corresponds to a well-defined physical state. We apply then our scheme to the one-dimensional (1D) quantum Ising chain, where the time MPS is defined in continuous imaginary time. It is found that the time MPS at or close to the critical point is always...
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...
Directory of Open Access Journals (Sweden)
Vrakking Marc J.J.
2013-03-01
Full Text Available We used velocity-map-imaging to measure electronic and nuclear dynamics in N2 molecules excited by a train of attosecond pulses. A time-to-space mapping of autoionization channel is demonstrated. It is found that the autoionization becomes energetically allowed when the two nuclei are still very close (~ 3 Å and that it can be coherently manipulated by a strong femtosecond infrared pulse.
International Nuclear Information System (INIS)
The elementary excitation spectrum of a two-component Bose—Einstein condensate in different hyperfine states is obtained by Green's function method. It is found to have two branches. In the long wave-length limit, the two branches of the excitation spectrum are reduced to one phonon excitation and one single-particle excitation. The single-particle one has an energy gap. When the energy gap exists, we study the Landau critical velocity and the depletion of the condensate. With the obtained Green's functions, we calculate the structure factor of a two-component condensate. It is found that the static structure factor comprises only the branch of the phonon excitation and the single-particle excitation makes no contribution to the structure factor. (general)
Institute of Scientific and Technical Information of China (English)
Han Yu-Feng; Chen Liang; Liu Hou-Tong; Huang Xian-Shan
2013-01-01
The elementary excitation spectrum of a two-component Bose-Einstein condensate in different hyperfine states is obtained by Green's function method.It is found to have two branches.In the long wave-length limit,the two branches of the excitation spectrum are reduced to one phonon excitation and one single-particle excitation.The single-particle one has an energy gap.When the energy gap exists,we study the Landau critical velocity and the depletion of the condensate.With the obtained Green's functions,we calculate the structure factor of a two-component condensate.It is found that the static structure factor comprises only the branch of the phonon excitation and the single-particle excitation makes no contribution to the structure factor.
Recent results related to excited states of 6Be and 10He
Wolski R.; Zhukov M. V.; Ter-Akopian G.M.; Stepantsov S.V.; Slepnev R. S.; Sidorchuk S.I.; Sharov P.G.; Parfenova Yu.L.; Mukha I. G.; Nikolskii E. Yu.; Kuzmin E. A.; Krupko S. A.; Kaminski G.; Jaluvkova P.; Grigorenko L.V.
2012-01-01
The 1H(6Li, 6Be)n charge-exchange reaction and the 3H(8He,p)10He two-neutron transfer reaction were recently carried out at the ACCULINNA fragment separator (FLNR, Dubna) to populate the ground and excited states of 6Be and 10He nuclei, respectively. The 6Be ET spectrum (ET is the 6Be energy above its 4He+p+p decay threshold) was obtained with high statistics and described by the well-known 0+ ground state of 6Be at ET = 1.37 MeV, the 2+ state at ET = 3.05 MeV and a broad structure extending ...
Cs 728 nm excited state Faraday anomalous dispersion optical filter with indirect pump
Tao, Zhiming; Zhang, Xiaogang; Chen, Mo; Liu, Zhongzheng; Zhu, Chuanwen; Liu, Zhiwen; Chen, Jingbiao
2016-06-01
We demonstrate a Cs excited state Faraday anomalous dispersion optical filter (ESFADOF) operating at 728 nm using a novel pump method, by which the pump beam and the probe beam in the ESFADOF realized here have no a common energy level. Using this method, the ESFADOF achieves a transmission of 2.39% with a bandwidth of 22.52 MHz, which can be applied to both laser frequency stabilization and future four-level active optical clocks. Under the 455 nm laser pump, in addition to 52D5/2, other states such as 72S1/2, 72P3/2, 62P3/2, 62P1/2 and 52D3/2 have also been populated effectively. Meanwhile, multiple wavelength filters exploiting atomic transitions to these states can be realized.
Excited state free energy calculations of Cy3 in different environments
International Nuclear Information System (INIS)
Cy3, a cyanine dye, is one of the most widely used dyes in investigating the structure and dynamics of biomolecules by means of fluorescence methods. However, Cy3 fluorescence emission is strongly competed by trans-cis isomerization, whose efficiency is dictated by the isomerization energy barrier and the environment of Cy3. The fluorescence quantum yield of Cy3 is very low when the dye is free in homogeneous solution but it is considerably enhanced in an environment that rigidifies the structure, e.g. when it is attached to a DNA strand. In this work, the barriers for isomerization on the excited state of free Cy3, and Cy3 attached to single- and double-stranded DNA in methanol, are presented. The free energy and subsequently the isomerization barrier calculations are performed using the umbrella sampling technique with the weighted histogram analysis method. The hybrid quantum mechanics/molecular mechanics (QM/MM) approach is employed to provide the potential energy surfaces for the excited state dynamics simulations in umbrella sampling. The semiempirical floating occupation molecular orbital configuration interaction method is used for electronic excited state calculations of the QM region (Cy3). From the free energy calculations, the barrier of Cy3 attached to the single-stranded DNA is highest, in agreement with previously reported experimental results. This is likely due to the stacking interaction between Cy3 and DNA. Such a stacking interaction is likely associated with steric hindrance that prevents the rotation around the conjugated bonds of Cy3. If Cy3 experiences high steric hindrance, it has a higher isomerization barrier and thus the efficiency of fluorescence emission increases. (paper)
Energy Technology Data Exchange (ETDEWEB)
Wu, Guorong [National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6 (Canada); State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023 (China); Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026 (China); Neville, Simon P. [Department of Chemistry, University of Ottawa, 10 Marie Curie, Ottawa, Ontario K1N 6N5 (Canada); Schalk, Oliver [National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6 (Canada); Department of Physics, AlbaNova University Center, Stockholm University, Roslagstullsbacken 21, 106 91 Stockholm (Sweden); Sekikawa, Taro [Department of Applied Physics, Hokkaido University, Kita-13 Nishi-8, Kita-ku, Sapporo 060-8628 (Japan); Ashfold, Michael N. R. [School of Chemistry, University of Bristol, Bristol BS8 1TS (United Kingdom); Worth, Graham A. [School of Chemistry, University of Birmingham, Edgbaston, Birmingham B15 2TT (United Kingdom); Stolow, Albert, E-mail: astolow@uottawa.ca [National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6 (Canada); Department of Chemistry, University of Ottawa, 10 Marie Curie, Ottawa, Ontario K1N 6N5 (Canada); Department of Physics, University of Ottawa, 150 Louis Pasteur, Ottawa, Ontario K1N 6N5 (Canada)
2016-01-07
The dynamics of N-methylpyrrole following excitation at wavelengths in the range 241.5-217.0 nm were studied using a combination of time-resolved photoelectron spectroscopy (TRPES), ab initio quantum dynamics calculations using the multi-layer multi-configurational time-dependent Hartree method, as well as high-level photoionization cross section calculations. Excitation at 241.5 and 236.2 nm results in population of the A{sub 2}(πσ{sup ∗}) state, in agreement with previous studies. Excitation at 217.0 nm prepares the previously neglected B{sub 1}(π3p{sub y}) Rydberg state, followed by prompt internal conversion to the A{sub 2}(πσ{sup ∗}) state. In contrast with the photoinduced dynamics of pyrrole, the lifetime of the wavepacket in the A{sub 2}(πσ{sup ∗}) state was found to vary with excitation wavelength, decreasing by one order of magnitude upon tuning from 241.5 nm to 236.2 nm and by more than three orders of magnitude when excited at 217.0 nm. The order of magnitude difference in lifetimes measured at the longer excitation wavelengths is attributed to vibrational excitation in the A{sub 2}(πσ{sup ∗}) state, facilitating wavepacket motion around the potential barrier in the N–CH{sub 3} dissociation coordinate.
Entanglement entropy of excited states in conformal perturbation theory and the Einstein equation
Speranza, Antony J
2016-01-01
For a conformal field theory (CFT) deformed by a relevant operator, the entanglement entropy of a ball-shaped region may be computed as a perturbative expansion in the coupling. A similar perturbative expansion exists for excited states near the vacuum. Using these expansions, this work investigates the behavior of excited state entanglement entropies of small, ball-shaped regions. The motivation for these calculations is Jacobson's recent work on the equivalence of the Einstein equation and the hypothesis of maximal vacuum entropy [arXiv:1505.04753], which relies on a conjecture stating that the behavior of these entropies is sufficiently similar to a CFT. In addition to the expected type of terms which scale with the ball radius as $R^d$, the entanglement entropy calculation gives rise to terms scaling as $R^{2\\Delta}$, where $\\Delta$ is the dimension of the deforming operator. When $\\Delta\\leq\\frac{d}{2}$, the latter terms dominate the former, and suggest that a modification to the conjecture is needed.
Statistical GDR [Giant Dipole Resonances] decay of highly excited states of 63Cu
International Nuclear Information System (INIS)
Continuum γ-ray spectra from decays of 63Cu formed at initial excitation energies of 22.5 to 77.4 MeV and maximum spin up to 40 h-bar, using 4He + 59Co, 6Li + 57Fe, 12C + 51V, and 18O + 45Sc entrance channels, have been measured and analyzed. The parameters of the GDR strength function have been extracted using the statistical code CASCADE in a nonlinear least-squares fitting routine. Except for the cases of 4He and 6Li at the highest bombarding energies, which show evidence for nonstatistical effects, spectra are well-reproduced by statistical calculations. The mean energy and strength of the giant dipole resonance built on excited states of 63Cu are close to the ground-state values, while the width varies smoothly from ∼5 MeV for the ground-state GDR up to 10.6 +- .6 MeV in the temperature range up to 1.9 MeV and mean spin in the range 0 to 23 h-bar. The large range of energies studied permitted different level density formulations to be tested. Measured spectra from 6Li + 98Mo and 6Li + 181Ta at E/sub lab/(6Li) = 36 MeV show a strong nonstatistical enhancement at high γ-ray energies. 52 refs., 14 figs., 3 tabs
Chakraborti, Himadri; Bramhaiah, Kommula; John, Neena Susan; Pal, Suman Kalyan
2013-12-01
The quenching of the fluorescence of 1-aminopyrene (1-Ap) by reduced graphene oxide (rGO) has been investigated using spectroscopic techniques. In spite of the upward curvature in the Stern-Volmer plot, the unchanged spectral signature of the absorption of 1-Ap in the presence of rGO and the decrease in fluorescence lifetime with increasing rGO concentration point toward the dynamic nature of the quenching. Detailed analysis of steady state and time-resolved spectroscopic data has shown that the quenching arises due to the photoinduced electron transfer from 1-Ap to rGO. This is again supported by estimating the Gibb's free energy change for the ground as well as excited state electron transfer. Ab initio calculations under the density functional theory (DFT) formalism reveal that the possibility of π-π stacking is very slim in the 1-Ap-rGO system and the electron density resides completely on 1-Ap in the highest occupied molecular orbital (HOMO) and on graphene in the lowest unoccupied molecular orbital (LUMO), supporting the experimental findings of the intermolecular electron transfer between 1-Ap and rGO in the excited state.
Ground- and excited-state structural orientation of 2-(2`-hydroxyphenyl)benzazoles in cyclodextrins
Energy Technology Data Exchange (ETDEWEB)
Roberts, E.L.; Dey, J.; Warner, I.M. [Louisiana State Univ., Baton Rouge, LA (United States)
1996-12-12
The effects of {alpha}-, {beta}-, {gamma}-, and 2,6-di-O-methyl-{beta}-cyclodextrins (CDs) on the ground- and excited-state properties of 2-(2`-hydroxyphenyl)benzoxazole, 2-(2`-hydroxyphenyl)benzothiazole, and 2-(2`-hydroxyphenyl)benzimidazole in aqueous media are investigated. Steady-state fluorescence measurements are used to characterize the interaction of CDs with these azoles. Absorbance measurements indicate increased solubility of the azoles in aqueous solutions of CDs. Measurements of acidity constants (pK{sub a}) and data from induced circular dichroism indicate increased ground- and excited-state acidities of the phenolic protons of the molecules in the presence of CDs and axial orientation of the molecules within the CD cavity, respectively. The data further suggest a planar structure for HBO and a twisted confirmation for both HBT and HBI. The association constants of the inclusion complexes have also been estimated. These studies are further supplemented by comparative spectroscopic studies of 2-(2`-methoxyphenyl)benzothiazole in aqueous solutions of CDs. On the basis of the spectral data acquired, it is believed that the HBA molecules exist as zwitterionic tautomers in the presence of CDs. 35 refs., 6 figs., 2 tabs.
Excited state fluorescence quenching of the U O2++ ion by monovalent anions
International Nuclear Information System (INIS)
The reactions of the Uranyl ion U O2++ in the excited state with the monovalent inorganic ions N O3- and I O3- in aqueous solutions at normal temperature were studied, using three techniques: Fluorescence in the steady state - Flash photolysis - Fluorescence decay after excitation. With increasing concentration of these ions it was observed a decrease in the normalized intensity and a decrease in the decay time of the fluorescence of the Uranyl ion in the solution and a corresponding appearance of the radicals N O3. or I O3.. In each case the radical was identified by its optical absorption spectrum. These results suggest that the quenching of fluorescence of the Uranyl ion in each case is owing to an electron transfer reaction. In the case of the Nitrate ion the transfer may occur after the formation of an ionic par (U O2+...N O3) in the ground state. Evidence for static quenching in the system Uranyl iodate was not forthcoming. A mechanism for the determination of the velocity constant (probability per ion pair per unit time) is proposed for each of the systems. (author)
First identification of excited states in sup 5 sup 9 Zn
Andreoiu, C; Fahlander, C; Mineva, M N; Rudolph, D; Axiotis, M; Angelis, G D; Farnea, E; Gadea, A; Kröll, T; Martínez, T; Lenzi, S M; Rossi-Alvarez, C; Marginean, N; Ur, C A
2002-01-01
Excited states in sup 5 sup 9 Zn were observed for the first time following the fusion-evaporation reaction sup 2 sup 4 Mg+ sup 4 sup 0 Ca at a beam energy of 60 MeV. The GASP array in conjunction with the ISIS Silicon ball and the NeutronRing allowed for the detection of gamma-rays in coincidence with evaporated light particles. The mirror symmetry of sup 5 sup 9 Zn and sup 5 sup 9 Cu is discussed. (orig.)
Excited State Contributions to the Heavy Baryon Fragmentation Functions in a Quark-Diquark Model
Adamov, A D; Goldstein, Gary R.
2001-01-01
Spin dependent fragmentation functions for heavy flavor quarks to fragment into heavy baryons are calculated in a quark-diquark model. The production of intermediate spin 1/2 and 3/2 excited states is explicity included. The resulting $\\Lambda_b$ production rate and polarization at LEP energies are in agreement with experiment. The $\\Lambda_c$ and $\\Xi_c$ functions are also obtained. The spin independent $f_1(z)$ is compared to data. The integrated values for production rates agree with the data.
Role of excited states in Shockley-Read-Hall recombination in wide-band-gap semiconductors
Alkauskas, Audrius; Dreyer, Cyrus E.; Lyons, John L.; Van de Walle, Chris G.
2016-05-01
Defect-assisted recombination is an important limitation on efficiency of optoelectronic devices. However, since nonradiative capture rates decrease exponentially with the energy of the transition, the mechanisms by which such recombination can take place in wide-band-gap materials are unclear. Using electronic structure calculations we uncover the crucial role of electronic excited states in nonradiative recombination processes. The impact is elucidated with examples for the group-III nitrides, for which accumulating experimental evidence indicates that defect-assisted recombination limits efficiency. Our work provides insights into the physics of nonradiative recombination, and the mechanisms are suggested to be ubiquitous in wide-band-gap semiconductors.
Institute of Scientific and Technical Information of China (English)
FENG; Dongtai(冯东太); DING; Shiliang(丁世良); WANG; Meishan(王美山)
2003-01-01
The highly excited vibrational states of asymmetric linear tetratomic molecules are studied in the framework of Lie algebra. By using symmetric group U1(4) U2(4) U3(4), we construct the Hamiltonian that includes not only Casimir operators but also Majorana operators M12,M13 and M23, which are useful for getting potential energy surface and force constants in Lie algebra method. By Lie algebra treatment, we obtain the eigenvalues of the Hamiltonian, and make the concrete calculation for molecule C2HF.
Study of the effect of excited state concentration on photodegradation of the p3ht polymer
Peters, V. N.; Alexander, Rohan; Peters, D’Angelo A.; Noginov, M. A.
2016-01-01
We have studied photoinduced reduction of absorption and emission in p3ht, a semiconducting polymer, and found that the rate of photodegradation (destruction of the constituent thiophene rings) does not correlate with the luminescence intensity and, correspondingly, does not depend on the excited state concentration. This conclusion rules out Purcell enhancement of radiative decay rate as a possible explanation of the recently discovered reduction of the p3ht photodegradation rate in the vicinity of metallic substrates and lamellar metal-dielectric metamaterials. PMID:27629230
Evidence for Cation-Controlled Excited-State Localization in a Ruthenium Polypyridyl Compound.
Beauvilliers, Evan E; Meyer, Gerald J
2016-08-01
The visible absorption and photoluminescence (PL) properties of the four neutral ruthenium diimine compounds [Ru(bpy)2(dcb)] (B2B), [Ru(dtb)2(dcb)] (D2B), [Ru(bpy)2(dcbq)] (B2Q), and [Ru(dtb)2(dcbq)] (D2Q), where bpy is 2,2'-bipyridine, dcb is 4,4'-(CO2(-))2-bpy, dtb is 4,4'-(tert-butyl)2-bpy, and dcbq is 4,4'-(CO2(-))2-2,2'-biquinoline, are reported in the presence of Lewis acidic cations present in fluid solutions at room temperature. In methanol solutions, the measured spectra were insensitive to the presence of these cations, while in acetonitrile a significant red shift in the PL spectra (≤1400 cm(-1)) was observed consistent with stabilization of the metal-to-ligand charge transfer (MLCT) excited state through Lewis acid-base adduct formation. No significant spectral changes were observed in control experiments with the tetrabutylammonium cation. Titration data with Li(+), Na(+), Mg(2+), Ca(2+), Zn(2+), Al(3+), Y(3+), and La(3+) showed that the extent of stabilization saturated at high cation concentration with magnitudes that scaled roughly with the cation charge-to-size ratio. The visible absorption spectra of D2Q was particularly informative due to the presence of two well-resolved MLCT absorption bands: (1) Ru → bpy, λmax ≈ 450 nm; and (2) Ru → dcbq, λmax ≈ 540 nm. The higher-energy band blue-shifted and the lower-energy band red-shifted upon cation addition. The PL intensity and lifetime of the excited state of B2B first increased with cation addition without significant shifts in the measured spectra, behavior attributed to a cation-induced change in the localization of the emissive excited state from bpy to dcb. The importance of excited-state localization and stabilization for solar energy conversion is discussed. PMID:27391279
Indian Academy of Sciences (India)
Tuhin Pradhan; Piue Ghoshal; Ranjit Biswas
2009-01-01
Excited state intramolecular charge transfer reaction of 4-(1-azetidinyl) benzonitrile (P4C) in deuterated and normal methanol, ethanol and acetonitrile has been studied in order to investigate the solvent isotope effects on reaction rates and yields. These quantities (reaction rates and yields) along with several other properties such as quantum yield and radiative rates have been found to be insensitive to the solvent isotope substitution in all these solvents. The origin of the solvent isotope insensitivity of the reaction is discussed and correlated with the observed slowing down of the solvation dynamics upon isotope substitution.
Electron impact excitation and assignment of the low-lying electronic states of CO2
Hall, R. I.; Trajmar, S.
1973-01-01
Electron scattering spectra of CO2 are reported in the 7 to 10 eV energy-loss range, at energies of 0.2, 0.35, 0.6, 0.7, and 7.0 eV above threshold, and at a scattering angle of 90 deg. Several new distinct overlapping continua with weak, diffuse bands superimposed are observed to lie in this energy-loss range. The experimental spectra are discussed in the light of recent ab initio configuration-interaction calculations of the vertical transition energies of CO2. The experimental spectra are shown to be consistent with the excitation states of CO2.
International Nuclear Information System (INIS)
We report low-temperature photoelectron spectra of isolated gas-phase complexes of the hexachloroplatinate dianion bound to the nucleobases uracil, thymine, cytosine, and adenine. The spectra display well-resolved, distinct peaks that are consistent with complexes where the hexachloroplatinate dianion is largely intact. Adiabatic electron detachment energies for the hexachloroplatinate-nucleobase complexes are measured as 2.26-2.36 eV. The magnitudes of the repulsive Coulomb barriers (RCBs) of the complexes are all ∼1.7 eV, values that are lower than the RCB of the uncomplexed PtCl62− dianion as a result of charge solvation by the nucleobases. In addition to the resolved spectral features, broad featureless bands indicative of delayed electron detachment are observed in the 193 nm photoelectron spectra of the four clusters. The 266 nm spectra of the PtCl62− ⋅ thymine and PtCl62− ⋅ adenine complexes also display very prominent delayed electron emission bands. These results mirror recent results on the related Pt(CN)42− ⋅ nucleobase complexes [A. Sen et al., J. Phys. Chem. B 119, 11626 (2015)]. The observation of delayed electron emission bands in the PtCl62− ⋅ nucleobase spectra obtained in this work, as for the previously studied Pt(CN)42− ⋅ nucleobase complexes, is attributed to one-photon excitation of nucleobase-centred excited states that can effectively couple to the electron detachment continuum, producing strong electron detachment. Moreover, the selective, strong excitation of the delayed emission bands in the 266 nm spectra is linked to fundamental differences in the individual nucleobase photophysics at this excitation energy. This strongly supports our previous suggestion that the dianion within these clusters can be viewed as a “dynamic tag” which has the propensity to emit electrons when the attached nucleobase decays over a time scale long enough to allow autodetachment
Energy Technology Data Exchange (ETDEWEB)
Sen, Ananya; Matthews, Edward M.; Hou, Gao-Lei; Wang, Xue B.; Dessent, Caroline
2015-11-14
We report low-temperature photoelectron spectra of isolated gas-phase complexes of the hexachloroplatinate dianion bound to the nucleobases uracil, thymine, cytosine and adenine. The spectra display well-resolved, distinct peaks that are consistent with complexes where the hexachloroplatinate dianion is largely intact. Adiabatic electron detachment energies for the hexachloroplatinate-nucleobase complexes are measured as 2.26-2.36 eV. The magnitudes of the repulsive Coulomb barriers (RCBs) of the complexes are all ~1.7 eV, values that are lower than the RCB of the uncomplexed PtCl6 2- dianion as a result of charge solvation by the nucleobases. In addition to the resolved spectral features, broad featureless bands indicative of delayed electron detachment are observed in the 193 nm photoelectron spectra of the four clusters. The 266 nm spectra of the PtCl6 2-∙thymine and PtCl6 2-∙adenine complexes also display very prominent delayed electron emission bands. These results mirror recent results on the related Pt(CN)4 2-∙nucleobase complexes [Sen et al, J. Phys. Chem. B, 119, 11626, 2015]. The observation of delayed electron emission bands in the PtCl6 2-∙nucleobase spectra obtained in this work, as for the previously studied Pt(CN)4 2-∙nucleobase complexes, is attributed to onephoton excitation of nucleobase-centred excited states that can effectively couple to the electron detachment continuum, producing strong electron detachment. Moreover, the selective, strong excitation of the delayed emission bands in the 266 nm spectra is linked to fundamental differences in the individual nucleobase photophysics at this excitation energy. This strongly supports our previous suggestion that the dianion within these clusters can be viewed as a “dynamic tag” which has the propensity to emit electrons when the attached nucleobase decays over a timescale long enough to allow autodetachment.
Dirac Coupled Channel Analyses of the high-lying excited states at $^{22}$Ne(p,p$'$)$^{22}$Ne
Shim, Sugie
2015-01-01
Dirac phenomenological coupled channel analyses are performed using an optical potential model for the high-lying excited vibrational states at 800 MeV unpolarized proton inelastic scatterings from $^{22}$Ne nucleus. Lorentz-covariant scalar and time-like vector potentials are used as direct optical potentials and the first-order vibrational collective model is used for the transition optical potentials to describe the high-lying excited vibrational collective states. The complicated Dirac coupled channel equations are solved phenomenologically using a sequential iteration method by varying the optical potential and the deformation parameters. Relativistic Dirac coupled channel calculations are able to describe the high-lying excited states of the vibrational bands in $^{22}$Ne clearly better than the nonrelativistic coupled channel calculations. The channel-coupling effects of the multistep process for the excited states of the vibrational bands are investigated. The deformation parameters obtained from the ...
Ground-state and excited-state properties of LaMnO3 from full-potential calculations
International Nuclear Information System (INIS)
The ground-state and excited-state properties of the perovskite LaMn03, the mother material of colossal magnetoresistance manganites, are calculated based on the generalized-gradient-corrected relativistic full- potential method. The electronic structure, magnetism, and energetics of various spin configurations for LaMnO3 in the ideal cubic perovskite structure and the experimentally observed distorted orthorhombic structure are obtained. The excited-state properties such as the optical, magneto-optical x-ray photoemission bremsstrahlung isochromat, and x-ray absorption near-edge structure spectra are calculated and found to be in excellent agreement with available experimental results. Consistent with earlier observations the insulating behavior can be obtained only when we take into account the structural distortions and the correct antiferro magnetic ordering in the calculations. The present results suggest that the correlation effect is not significant in LaMnO3 and the presence of ferromagnetic coupling within the ab plane as well as the antiferromagnetic coupling perpendicular too this plane can be explained through the itinerant band picture. Our calculations show that the Mn 3d eg-like electrons are present in the whole valence-band region. We have calculated the hyperfine field parameters for the A-type antiferromagnetic and the ferromagnetic phases of LaMnO3 and compared the findings with the available experimental results. The role of the orthorhombic distortion on electronic structure, magnetism, and optical anisotropy is analyzed. (author)
Generation of excited coherent states for a charged particle in a uniform magnetic field
International Nuclear Information System (INIS)
We introduce excited coherent states, |β,α;nÐ³Ð‚‰≔a†n|β,αÐ³Ð‚‰, where n is an integer and states |β,αÐ³Ð‚‰ denote the coherent states of a charged particle in a uniform magnetic field. States |β,αÐ³Ð‚‰ minimize the Schrödinger-Robertson uncertainty relation while having the nonclassical properties. It has been shown that the resolution of identity condition is realized with respect to an appropriate measure on the complex plane. Some of the nonclassical features such as sub-Poissonian statistics and quadrature squeezing of these states are investigated. Our results are compared with similar Agarwal’s type photon added coherent states (PACSs) and it is shown that, while photon-counting statistics of |β,α,nÐ³Ð‚‰ are the same as PACSs, their squeezing properties are different. It is also shown that for large values of |β|, while they are squeezed, they minimize the uncertainty condition. Additionally, it has been demonstrated that by changing the magnitude of the external magnetic field, Bext, the squeezing effect is transferred from one component to another. Finally, a new scheme is proposed to generate states |β,α;nÐ³Ð‚‰ in cavities.
Observation of an Excited $B^{\\pm}_c$ Meson State with the ATLAS Detector
Aad, Georges; Abdallah, Jalal; Abdel Khalek, Samah; Abdinov, Ovsat; Aben, Rosemarie; Abi, Babak; Abolins, Maris; AbouZeid, Ossama; Abramowicz, Halina; Abreu, Henso; Abreu, Ricardo; Abulaiti, Yiming; Acharya, Bobby Samir; Adamczyk, Leszek; Adams, David; Adelman, Jahred; Adomeit, Stefanie; Adye, Tim; Agatonovic-Jovin, Tatjana; Aguilar-Saavedra, Juan Antonio; Agustoni, Marco; Ahlen, Steven; Ahmadov, Faig; Aielli, Giulio; Akerstedt, Henrik; Åkesson, Torsten Paul Ake; Akimoto, Ginga; Akimov, Andrei; Alberghi, Gian Luigi; Albert, Justin; Albrand, Solveig; Alconada Verzini, Maria Josefina; Aleksa, Martin; Aleksandrov, Igor; Alexa, Calin; Alexander, Gideon; Alexandre, Gauthier; Alexopoulos, Theodoros; Alhroob, Muhammad; Alimonti, Gianluca; Alio, Lion; Alison, John; Allbrooke, Benedict; Allison, Lee John; Allport, Phillip; Almond, John; Aloisio, Alberto; Alonso, Alejandro; Alonso, Francisco; Alpigiani, Cristiano; Altheimer, Andrew David; Alvarez Gonzalez, Barbara; Alviggi, Mariagrazia; Amako, Katsuya; Amaral Coutinho, Yara; Amelung, Christoph; Amidei, Dante; Amor Dos Santos, Susana Patricia; Amorim, Antonio; Amoroso, Simone; Amram, Nir; Amundsen, Glenn; Anastopoulos, Christos; Ancu, Lucian Stefan; Andari, Nansi; Andeen, Timothy; Anders, Christoph Falk; Anders, Gabriel; Anderson, Kelby; Andreazza, Attilio; Andrei, George Victor; Anduaga, Xabier; Angelidakis, Stylianos; Angelozzi, Ivan; Anger, Philipp; Angerami, Aaron; Anghinolfi, Francis; Anisenkov, Alexey; Anjos, Nuno; Annovi, Alberto; Antonaki, Ariadni; Antonelli, Mario; Antonov, Alexey; Antos, Jaroslav; Anulli, Fabio; Aoki, Masato; Aperio Bella, Ludovica; Apolle, Rudi; Arabidze, Giorgi; Aracena, Ignacio; Arai, Yasuo; Araque, Juan Pedro; Arce, Ayana; Arguin, Jean-Francois; Argyropoulos, Spyridon; Arik, Metin; Armbruster, Aaron James; Arnaez, Olivier; Arnal, Vanessa; Arnold, Hannah; Arratia, Miguel; Arslan, Ozan; Artamonov, Andrei; Artoni, Giacomo; Asai, Shoji; Asbah, Nedaa; Ashkenazi, Adi; Åsman, Barbro; Asquith, Lily; Assamagan, Ketevi; Astalos, Robert; Atkinson, Markus; Atlay, Naim Bora; Auerbach, Benjamin; Augsten, Kamil; Aurousseau, Mathieu; Avolio, Giuseppe; Azuelos, Georges; Azuma, Yuya; Baak, Max; Baas, Alessandra; Bacci, Cesare; Bachacou, Henri; Bachas, Konstantinos; Backes, Moritz; Backhaus, Malte; Backus Mayes, John; Badescu, Elisabeta; Bagiacchi, Paolo; Bagnaia, Paolo; Bai, Yu; Bain, Travis; Baines, John; Baker, Oliver Keith; Balek, Petr; Balli, Fabrice; Banas, Elzbieta; Banerjee, Swagato; Bannoura, Arwa A E; Bansal, Vikas; Bansil, Hardeep Singh; Barak, Liron; Baranov, Sergei; Barberio, Elisabetta Luigia; Barberis, Dario; Barbero, Marlon; Barillari, Teresa; Barisonzi, Marcello; Barklow, Timothy; Barlow, Nick; Barnett, Bruce; Barnett, Michael; Barnovska, Zuzana; Baroncelli, Antonio; Barone, Gaetano; Barr, Alan; Barreiro, Fernando; Barreiro Guimarães da Costa, João; Bartoldus, Rainer; Barton, Adam Edward; Bartos, Pavol; Bartsch, Valeria; Bassalat, Ahmed; Basye, Austin; Bates, Richard; Batkova, Lucia; Batley, Richard; Battaglia, Marco; Battistin, Michele; Bauer, Florian; Bawa, Harinder Singh; Beau, Tristan; Beauchemin, Pierre-Hugues; Beccherle, Roberto; Bechtle, Philip; Beck, Hans Peter; Becker, Anne Kathrin; Becker, Sebastian; Beckingham, Matthew; Becot, Cyril; Beddall, Andrew; Beddall, Ayda; Bedikian, Sourpouhi; Bednyakov, Vadim; Bee, Christopher; Beemster, Lars; Beermann, Thomas; Begel, Michael; Behr, Katharina; Belanger-Champagne, Camille; Bell, Paul; Bell, William; Bella, Gideon; Bellagamba, Lorenzo; Bellerive, Alain; Bellomo, Massimiliano; Belotskiy, Konstantin; Beltramello, Olga; Benary, Odette; Benchekroun, Driss; Bendtz, Katarina; Benekos, Nektarios; Benhammou, Yan; Benhar Noccioli, Eleonora; Benitez Garcia, Jorge-Armando; Benjamin, Douglas; Bensinger, James; Benslama, Kamal; Bentvelsen, Stan; Berge, David; Bergeaas Kuutmann, Elin; Berger, Nicolas; Berghaus, Frank; Beringer, Jürg; Bernard, Clare; Bernat, Pauline; Bernius, Catrin; Bernlochner, Florian Urs; Berry, Tracey; Berta, Peter; Bertella, Claudia; Bertoli, Gabriele; Bertolucci, Federico; Bertsche, David; Besana, Maria Ilaria; Besjes, Geert-Jan; Bessidskaia, Olga; Bessner, Martin Florian; Besson, Nathalie; Betancourt, Christopher; Bethke, Siegfried; Bhimji, Wahid; Bianchi, Riccardo-Maria; Bianchini, Louis; Bianco, Michele; Biebel, Otmar; Bieniek, Stephen Paul; Bierwagen, Katharina; Biesiada, Jed; Biglietti, Michela; Bilbao De Mendizabal, Javier; Bilokon, Halina; Bindi, Marcello; Binet, Sebastien; Bingul, Ahmet; Bini, Cesare; Black, Curtis; Black, James; Black, Kevin; Blackburn, Daniel
2014-01-01
A search for excited states of the $B^{\\pm}_c$ meson is performed using 4.9 fb$^{-1}$ of 7 TeV and 19.2 fb$^{-1}$ of 8 TeV $pp$ collision data collected by the ATLAS experiment at the LHC. A new state is observed through its hadronic transition to the ground state, with the latter detected in the decay $B_c^{\\pm} \\to J/\\psi \\pi^{\\pm}$. The state appears in the $m(B_c^{\\pm}\\pi^{+}\\pi^{-})-m(B_c^{\\pm})-2m(\\pi^{\\pm})$ mass difference distribution with a significance of 5.2 standard deviations. The mass of the observed state is $6842 \\pm 4 \\pm 5$~MeV, where the first error is statistical and the second is systematic. The mass and decay of this state are consistent with expectations for the second $S\\mbox{-}$wave state of the $B^{\\pm}_c$ meson, $B^{\\pm}_c(2S)$.
DEFF Research Database (Denmark)
Kjaergaard, Magnus; Andersen, Lisbeth; Nielsen, Lau Dalby;
2013-01-01
Intrinsically disordered proteins are renowned for their structural plasticity when they undergo coupled folding and binding to partner proteins. The nuclear coactivator binding domain of CBP is a remarkable example of this adaptability as it folds into two different conformations depending...... experience conformational exchange. The dispersion data can be described by a global two-state exchange process between a ground state and an excited state populated to 8%. The three helices are still folded in the excited state but have a different packing from the ground state; the contact between helices...
The estimation of CO bond length changes in the excited states of transition metal carbonyls
Morrison, Sara L.; Turner, James J.
1994-01-01
Advances in vibrational spectroscopy have led to increased knowledge of shortlived excited states. In the case of transition metal carbonyl compounds, time-resolved infrared spectra can be measured directly. The CO energy factored force constants are used to estimate the CO bond length distortions upon excitation. The new empirical relationship rCO = 1.674 - 0.184 ln kCO allows excited states CO bond lenghts to be calculated with a standard deviation of ±0.005 Å. For energy factored systems it is deemed unnecessary to calculate pseudodiatomic frequencies ( vPD) from the potential energy distribution.
Time-resolved measurement of G values of solute excited states in cyclohexane and n-hexane
International Nuclear Information System (INIS)
The number of solute excited states produced per 100 eV absorbed is determined for several scintillators dissolved in cyclohexane and n-hexane over the concentration range 0.001-0.05 M. These yields are determined at 5 ns after a 30-ps pulse of electrons. The part of the yield arising from excitation of the solute by absorption of Cerenkov light is determined on the basis of solutions of scintillators in ethanol, where essentially all of the solute excited state results from this process
Measurement of excited states of Sb impurity in Si by traveling–wave method
International Nuclear Information System (INIS)
The ground and excited states of Sb atom in Si, 1s (A1), 1s (T2), 1s (E), and 2p0, were measured by using a traveling-wave method. The Sb-doped Si crystal with donor concentration of 2 × 1015 cm−3 was placed the distance of 5 μm above a piezoelectric crystal in the fringe field of a surface acoustic wave. The free electrons excited from the bound states of the Sb atom are drifted by the traveling-wave, and thus lose their energy as the Joule heat through lattice and ion scattering processes. A strong temperature-dependent energy loss of the traveling-wave can be observed at temperatures below 200 K. The values of the bound states of the Sb atom can be characterized by using the Arrhenius plot for thermal activation process of the electrons in the bound states. The measurements were carried out at two frequencies of the traveling-wave, 50 MHz and 200 MHz. At the frequency of 50 MHz, the dielectric properties of the Si crystal are governed by dopant polarization but by electronic polarization at 200 MHz. We found that measurement accuracy of the bound states depends mainly on the electron mobility and the dielectric constant of the Si crystal, which are sensitive to the frequency and strength of the traveling-wave as well as electronic polarization properties of the Si crystal.
Energy Technology Data Exchange (ETDEWEB)
Chibisov, M.I. [Russian Research Center, Kurchatov Institute, Kurchatov strasse 1, Institute of Nuclear Fusion, Moscow 123182 (Russia); Mitchell, J.B.; Van der Donk, P.J. [Department of Physics, University of Western Ontario, London, Ontario, N6A3K7 (CANADA); Yousif, F.B. [Instituto de Fisica, UNAM, Cuernavaca, (Mexico) 62191; Morgan, T.J. [Physics Department, Wesleyan University, Middletown, Connecticut 06459-0155 (United States)
1997-07-01
The dissociative recombination (DR) of vibrationally excited H{sub 2}{sup +} ions to form products in high Rydberg states has been investigated experimentally and theoretically for small (0.01{minus}0.1 eV) center-of-mass energies of the projectile electron. The merged beam method was used in the experiment and very large cross sections were found for DR from highly vibrationally excited states. The Rydberg states population was analyzed by the application of an electric field ionizer with an axial electric field in excess of 70 kV/cm, which is sufficient to ionize Rydberg states with n{ge}10. Experiments with and without the ionizer were performed and cross sections {sigma}(0{lt}n{le}21), {sigma}(n{lt}10), and {sigma}(10{le}n{le}21) were measured. The dipole approximation was used for the interpretation of the experimental results. Molecular rovibrational transitions were considered quantum mechanically. At low collision energy (0.01 eV), DR cross sections with high n=10{minus}21 Rydberg products arise from initial vibrational states v{ge}15. Absolute values of these cross sections are found to be of the order of magnitude of 10{sup {minus}12}{minus}10{sup {minus}13} cm{sup 2}. Comparison of theoretical and experimental results has shown that the modified back autoionization (involving transitions to the continuum and to very high n; that is the {open_quotes}indirect{close_quotes} mechanism of DR) plays a significant role for all cross sections. {copyright} {ital 1997} {ital The American Physical Society}
Scaling of collision strengths for highly-excited states of ions of the H- and He-like sequences
Fernández-Menchero, L.; Del Zanna, G.; Badnell, N. R.
2016-08-01
Emission lines from highly-excited states (n ≥ 5) of H- and He-like ions have been detected in astrophysical sources and fusion plasmas. For such excited states, R-matrix or distorted wave calculations for electron-impact excitation are very limited, due to the large size of the atomic basis set needed to describe them. Calculations for n ≥ 6 are also not generally available. We study the behaviour of the electron-impact excitation collision strengths and effective collision strengths for the most important transitions used to model electron collision dominated astrophysical plasmas, solar, for example. We investigate the dependence on the relevant parameters: the principal quantum number n or the nuclear charge Z. We also estimate the importance of coupling to highly-excited states and the continuum by comparing the results of different sized calculations. We provide analytic formulae to calculate the electron-impact excitation collision strengths and effective collision strengths to highly-excited states (n ≥ 8) of H- and He-like ions. These extrapolated effective collision strengths can be used to interpret astrophysical and fusion plasma via collisional-radiative modelling. Tables of atomic data for Si xiii and S xv are only available at the CDS via anonymous ftp to http://cdsarc.u-strasbg.fr (http://130.79.128.5) or via http://cdsarc.u-strasbg.fr/viz-bin/qcat?J/A+A/592/A135
International Nuclear Information System (INIS)
The time-dependent density functional theory (TDDFT) has become the most popular method to calculate the electronic excitation energies, describe the excited-state properties, and perform the excited-state geometric optimization of medium and large-size molecules due to the implementation of analytic excited-state energy gradient and Hessian in many electronic structure software packages. To describe the molecules in condensed phase, one usually adopts the computationally efficient hybrid Quantum Mechanics/Molecular Mechanics (QM/MM) models. Here, we extend our previous work on the energy gradient of TDDFT/MM excited state to account for the mutual polarization effects between QM and MM regions, which is believed to hold a crucial position in the potential energy surface of molecular systems when the photoexcitation-induced charge rearrangement in the QM region is drastic. The implementation of a simple polarizable TDDFT/MM (TDDFT/MMpol) model in Q-Chem/CHARMM interface with both the linear response and the state-specific features has been realized. Several benchmark tests and preliminary applications are exhibited to confirm our implementation and assess the effects of different treatment of environmental polarization on the excited-state properties, and the efficiency of parallel implementation is demonstrated as well
The separation of vibrational coherence from ground- and excited-electronic states in P3HT film
Song, Yin
2015-06-07
© 2015 AIP Publishing LLC. Concurrence of the vibrational coherence and ultrafast electron transfer has been observed in polymer/fullerene blends. However, it is difficult to experimentally investigate the role that the excited-state vibrational coherence plays during the electron transfer process since vibrational coherence from the ground- and excited-electronic states is usually temporally and spectrally overlapped. Here, we performed 2-dimensional electronic spectroscopy (2D ES) measurements on poly(3-hexylthiophene) (P3HT) films. By Fourier transforming the whole 2D ES datasets (S (λ 1, T∼ 2, λ 3)) along the population time (T∼ 2) axis, we develop and propose a protocol capable of separating vibrational coherence from the ground- and excited-electronic states in 3D rephasing and nonrephasing beating maps (S (λ 1, ν∼ 2, λ 3)). We found that the vibrational coherence from pure excited electronic states appears at positive frequency (+ ν∼ 2) in the rephasing beating map and at negative frequency (- ν∼ 2) in the nonrephasing beating map. Furthermore, we also found that vibrational coherence from excited electronic state had a long dephasing time of 244 fs. The long-lived excited-state vibrational coherence indicates that coherence may be involved in the electron transfer process. Our findings not only shed light on the mechanism of ultrafast electron transfer in organic photovoltaics but also are beneficial for the study of the coherence effect on photoexcited dynamics in other systems.
Energy Technology Data Exchange (ETDEWEB)
Zeng, Qiao; Liang, WanZhen, E-mail: liangwz@xmu.edu.cn [State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005 (China)
2015-10-07
The time-dependent density functional theory (TDDFT) has become the most popular method to calculate the electronic excitation energies, describe the excited-state properties, and perform the excited-state geometric optimization of medium and large-size molecules due to the implementation of analytic excited-state energy gradient and Hessian in many electronic structure software packages. To describe the molecules in condensed phase, one usually adopts the computationally efficient hybrid Quantum Mechanics/Molecular Mechanics (QM/MM) models. Here, we extend our previous work on the energy gradient of TDDFT/MM excited state to account for the mutual polarization effects between QM and MM regions, which is believed to hold a crucial position in the potential energy surface of molecular systems when the photoexcitation-induced charge rearrangement in the QM region is drastic. The implementation of a simple polarizable TDDFT/MM (TDDFT/MMpol) model in Q-Chem/CHARMM interface with both the linear response and the state-specific features has been realized. Several benchmark tests and preliminary applications are exhibited to confirm our implementation and assess the effects of different treatment of environmental polarization on the excited-state properties, and the efficiency of parallel implementation is demonstrated as well.
The Influence of Surface Plasmons on Excited State Dynamics in PTCDA
Azarova, N. A.
Organic thin film solar cells can be paired with nanostructured substrates to overcome the issue of narrow spectral absorption in a thin-film configuration. The nanostructured surface acts not only as an effective scattering back reflector to increase the light path within the absorbing thin film but also affords plasmonic activity. The interface between the metal and the absorbing chromophore supports surface plasmon modes. The associated strong electromagnetic field can potentially couple with excitations of the chromophore, altering its exciton dynamics. Such a plasmon-exciton coupling can lead to control over excitation processes, namely singlet fission. Singlet fission is a sharing of excited state energy between chromophores that may regulate instances of multi-exciton generation, allowing the solar cell efficiency to exceed the thermodynamical Shockley-Queisser limit. The current investigation focuses on hybridization of the plasmon and molecular exciton. We coat an organic semiconductor, 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA), on the nanogratings consisting of lines of Ag on a substrate coated with a thick Ag backing. A dielectric spacer layer is included between the organic and the metal in some samples to eliminate any reaction between the two. The SP resonance of the grating is tuned through a PTCDA exciton line by sweeping the incident wave vector. Successful anticrossing between the plasmon and the exciton peaks would be observed in steady-state reflectance data as a function of angle. Though a detailed analysis of reflectance spectra has not been completed, the potential for plasmon-exciton hybdridization is demonstrated.
International Nuclear Information System (INIS)
Excited-state inter- and intramolecular electron-transfer reactions lie at the heart of the most photochemical solar energy conversion schemes. The authors research, which has utilized the techniques of continuous and pulsed photolysis and radiolysis, has focused on three general aspects of these reactions involving transition metal coordination complexes and electron donor-acceptor complexes: i) the effect of solution medium on the properties and quenching of the excited states; ii) the control of the quantum yields of formation of redox products; iii) the mechanism by which reduced species interact with water to yield H2 homogeneously and heterogeneously. EDTA is among the most popular sacrificial electron donors used in model systems. Its role is to scavenge the oxidized form of the photosensitizer in order to prevent its rapid reaction with the reduced form of the electron relay species that results from the electron-transfer quenching of the excited photosensitizer. In systems involving MV2+, the radicals resulting from the oxidation of EDTA can eventually lead to the generation of a second equivalent of MV+; the reducing agent is believed to be a radical localized on the carbon atom alpha to the carboxylate group. The reaction of radiolytically-generated OH/H with EDTA produces this radical directly via H-abstraction or indirectly via deprotonation of the carbon atom adjacent to the nitrogen radical site in the oxidized amine moiety; it reduces MV2+ with rate constants of 2.8 x 109, 7.6 x 109, and 8.5 x 106M-1s-1 at pH 12.5, 8.3, and 4.7, respectively. Degradative decarboxylation of EDTA-radicals and their back electron-transfer reactions are enhanced in acidic solution causing the yield of MV+ to be severely diminished
Energy transfer kinetics of the np5(n + 1)p excited states of Ne and Kr.
Kabir, Md Humayun; Heaven, Michael C
2011-09-01
Energy transfer rate constants for Ne(2p(5)3p) and Kr(4p(5)5p) atoms colliding with ground state rare gas atoms (Rg) have been measured. In part, this study is motivated by the possibility of using excited rare gas atoms as the active species in optically pumped laser systems. Rg(np(5)(n + 1)s) metastable states may be produced using low-power electrical discharges. The potential then exits for optical pumping and laser action on the np(5)(n + 1)p ↔ np(5)(n + 1)s transitions. Knowledge of the rate constants for collisional energy transfer and deactivation of the np(5)(n + 1)p states is required to evaluate the laser potential for various Rg + buffer gas combinations. In the present study we have characterized energy transfer processes for Ne (2p(5)3p) + He for the six lowest energy states of the multiplet. Rate constants for state-to-state transfer have been determined. Deactivation of the lowest energy level of Kr (4p(5)5p) by He, Ne, and Kr has also been characterized. Initial results suggest that Kr (4p(5)5p) + Ne mixtures may be the best suited for optically pumped laser applications.
You, Pei-Lin
2008-01-01
The linear Stark effect shows that the first excited state of hydrogen atom has large permanent electric dipole moment (EDM), d(H)=3eao (ao is Bohr radius). Using special capacitors our experiments discovered that the ground state K, Rb or Cs atom is polar atom with a large EDM of the order of eao as hydrogen atom of excited state. Their capacitance(C) at different voltage (V) was measured. The C-V curve shows that the saturation polarization of K, Rb or Cs vapor has be observed when the field E more than ten to the fifth power V/m. When the saturation polarization appeared, nearly all K, Rb or Cs atoms(more than 98 percent) turned toward the direction of the field, and C is approximately equal to Co (Co is vacuum capacitance) or their dielectric constant is nearly the same as vacuum! K, Rb or Cs vapor just exist in the lowest energy state, so we see the vacuum state containing a large number of atoms! Due to the saturation polarization of hydrogen vapor of excited state is easily appears, we conjecture that ...
Soulé, Paul; Jolicoeur, Thierry
2011-01-01
We study fractional quantum Hall states in the cylinder geometry with open boundaries. By truncating the Coulomb interactions between electrons we show that it is possible to construct infinitely many exact eigenstates including the ground state, quasiholes, quasielectrons and the magnetoroton branch of excited states.
Excited state proton transfer in 9-aminoacridine carboxamides in water and in DNA
Energy Technology Data Exchange (ETDEWEB)
Smith, C.A.
1995-11-01
The 9-aminoacridine molecule is important in several different fields of chemistry. The absorption and fluorescence spectra of this compound are pH sensitive and it is this property that allowed it to be used as a pH probe in different chemical environments. The compound exhibits proton transfer reactions which are among the most fundamental of chemical reactions. The planarity of 9-aminoacridine allows it to intercalate into DNA. Intercalation is a process in which the aromatic flat surface of the intercalator inserts between adjacent base pairs of DNA. The large surface area of 9-aminoacridine`s fused tricyclic ring system allows strong intercalative binding through van der Waals attractions. 9-aminoacridine and many of its derivatives have been tried as possible antitumor drugs. The cytotoxicity of an antitumor agent can be dramatically increased through the addition of one or two cationic side chains. This increase in cytotoxicity using the 9-aminoacridine compound as a parent molecule has been investigated through various derivatives with cationic side chains consisting of different number of carbon atoms between the proximal and distal N atoms. Similar derivatives varied the position of the carboxamide side chain on the aromatic ring system. The objective of this work is to first create a baseline study of the excited state kinetics of the 9-aminoacridine carboxamides in the absence of DNA. The baseline study will allow the excited state kinetics of these antitumor drugs when placed in DNA to be more fully understood.
Studies of excited-state properties of multibranched triarylamine end-capped triazines.
Liu, Chun; Tang, Kuo-Chun; Zhang, Hao; Pan, Hsiao-An; Hua, Jianli; Li, Bo; Chou, Pi-Tai
2012-12-20
Electron donor-acceptor types of multibranched triarylamine end-capped triazines have been systematically investigated by steady-state electronic spectroscopy, electrochemistry, femtosecond fluorescence anisotropy and solvent relaxation dynamics. The results, together with computational approach, have gained in-depth insight into their excited-state properties, especially the interactions between branches. Among different branched triarylamines of one, two and three arms, the interbranch interaction between each arm is weak, as evidenced by their nearly identical absorption spectral profile and frontier orbitals analyses. Upon S(0) → S(1) excitation, the electronic delocalization in the three-branched triarylamine end-capped triazine is resolved to be 680 ± 130 fs, followed by a slow (28 ± 3 ps) electronic localization into one branch and consequently a rotational depolarization of 2.0 ± 0.1 ns. Similar delocalization dynamics was resolved for the two-branched triarylamine end-capped triazine (electronic delocalization, 500 ± 90 fs; twisting localization, 21 ± 5 ps; rotational depolarization, 700 ± 30 ps). The comparable electron delocalization and solvent relaxation time scale may set up a new paradigm to investigate their specific correlation in the early time domain. PMID:23198687
Ground and excited states for exotic three-body atomic systems
Directory of Open Access Journals (Sweden)
Gasaneo G.
2010-04-01
Full Text Available An Angular Correlated Conﬁguration Interaction method is extended and applied to exotic threebody atomic systems with general masses. A recently proposed angularly correlated basis set is used to construct, simultaneously and with a single diagonalization, ground and excited states wave functions which: (i satisfy exactly Kato cusp conditions at the two-body coalescence points; (ii have only linear parameters; (iii show a fast convergency rate for the energy; (iv form an orthogonal set. The eﬃciency of the construction is illustrated by the study a variety of three-body atomic systems [m1− m2− m3z3+ ] with two negatively charged light particles, with 123 diverse masses m1− and m2−, and a heavy positively charged nucleus m3z3+. The calculated ground 11S and several excited n1,3S state energies are compared with those given in the literature, when available. We also present a short discussion on the critical charge necessary to get a stable three-body system supporting two electrons, an electron and a muon, or two muons.
Radiative charge transfer lifetime of the excited state of (NaCa)$^+$
Makarov, O P; Michels, H J; Smith, W W; Makarov, Oleg P.
2003-01-01
New experiments were proposed recently to investigate the regime of cold atomic and molecular ion-atom collision processes in a special hybrid neutral-atom--ion trap under high vacuum conditions. The collisional cooling of laser pre-cooled Ca$^+$ ions by ultracold Na atoms is being studied. Modeling this process requires knowledge of the radiative lifetime of the excited singlet A$^1\\Sigma^+$ state of the (NaCa)$^+$ molecular system. We calculate the rate coefficient for radiative charge transfer using a semiclassical approach. The dipole radial matrix elements between the ground and the excited states, and the potential curves were calculated using Complete Active Space Self-Consistent field and M\\"oller-Plesset second order perturbation theory (CASSCF/MP2) with an extended Gaussian basis, 6-311+G(3df). The semiclassical charge transfer rate coefficient was averaged over a thermal Maxwellian distribution. In addition we also present elastic collision cross sections and the spin-exchange cross section. The ra...
Evidence for an Excited Hyperon State in pp -> p K^+ Y^{0*}
Zychor, I; Büscher, M; Dzyuba, A; Keshelashvili, I; Kleber, V; Koch, R; Krewald, S; Maeda, Y; Mikirtichyants, S; Nekipelov, M; Ströher, H; Wilkin, C
2006-01-01
Indications for the production of a neutral excited hyperon in the reaction pp -> p K^+ Y^{0*} are observed in an experiment performed with the ANKE spectrometer at COSY-J\\"ulich at a beam momentum of 3.65 GeV/c. Two final states were investigated simultaneously, viz. Y^{0*} -> pi^+X^- and pi^-X^+, and consistent results were obtained in spite of the quite different experimental conditions. The parameters of the hyperon state are M(Y^{0*})= (1480 +/- 15) MeV/c^2 and Gamma(Y^{0*})= (60 +/- 15) MeV/c^2. The production cross section is of the order of few hundred nanobarns. Since the isospin of the Y^{0*} has not been determined here, it could either be an observation of the Sigma(1480), a one-star resonance of the PDG tables, or alternatively a Lambda hyperon. Relativistic quark models for the baryon spectrum do not predict any excited hyperon in this mass range and so the Y^{0*} may be of exotic nature.
Skobelev, N. K.
2016-07-01
Experimental data on the cross sections for channels of fusion and transfer reactions induced by beams of radioactive halo nuclei and clustered and stable loosely bound nuclei were analyzed, and the results of this analysis were summarized. The interplay of the excitation of single-particle states in reaction-product nuclei and direct reaction channels was established for transfer reactions. Respective experiments were performed in stable (6Li) and radioactive (6He) beams of the DRIBs accelerator complex at the Flerov Laboratory of Nuclear Reactions, Joint Institute for Nuclear Research, and in deuteron and 3He beams of the U-120M cyclotron at the Nuclear Physics Institute, Academy Sciences of Czech Republic (Řež and Prague, Czech Republic). Data on subbarrier and near-barrier fusion reactions involving clustered and loosely bound light nuclei (6Li and 3He) can be described quite reliably within simple evaporation models with allowance for different reaction Q-values and couple channels. In reactions involving halo nuclei, their structure manifests itself most strongly in the region of energies below the Coulomb barrier. Neutron transfer occurs with a high probability in the interactions of all loosely bound nuclei with light and heavy stable nuclei at positive Q-values. The cross sections for such reactions and the respective isomeric ratios differ drastically for nucleon stripping and nucleon pickup mechanisms. This is due to the difference in the population probabilities for excited single-particle states.
Emission of highly excited electronic states of potassium from cryptomelane nanorods.
Stelmachowski, P; Legutko, P; Jakubek, T; Indyka, P; Sojka, Z; Holmlid, L; Kotarba, A
2015-10-21
Cryptomelane (KMn8O16) nanorods were synthesized, characterized (XRD, Raman spectroscopy, TEM/SAED) and investigated by species resolved thermal desorption of potassium from the material in the range of 20-620 °C. The desorbing fluxes of ions, atoms and highly excited electronic states (field ionizable Rydberg states) were measured using an ion collector, surface ionization and field ionization detectors, respectively, in a vacuum apparatus. The non-equilibrium emission of potassium Rydberg species (principal quantum number > 30) strongly depends on the surface positive voltage bias with a broad maximum at 1-8 V. The stimulation of Rydberg species emission is discussed in terms of spatial and energetic overlapping between the electron cloud above the cryptomelane surface and the desorbing potassium ion. PMID:26388253
Relative entropy of excited states in two dimensional conformal field theories
Sárosi, Gábor
2016-01-01
We study the relative entropy and the trace square distance, both of which measure the distance between reduced density matrices of two excited states in two dimensional conformal field theories. We find a general formula for the relative entropy between two primary states with the same conformal dimension in the limit of a single small interval and find that in this case the relative entropy is proportional to the trace square distance. We check our general formulae by calculating the relative entropy between two generalized free fields and the trace square distance between the spin and disorder operators of the critical Ising model. We also give the leading term of the relative entropy in the small interval expansion when the two operators have different conformal dimensions. This turns out to be universal when the CFT has no primaires lighter than the stress tensor. The result reproduces the previously known special cases.
The one-dimensional Gross-Pitaevskii equation and its some excitation states
Energy Technology Data Exchange (ETDEWEB)
Prayitno, T. B., E-mail: trunk-002@yahoo.com [Physics Department, Faculty of Mathematics and Natural Science, Universitas Negeri Jakarta, Jl. Pemuda Rawamangun no. 10, Jakarta, 13220 (Indonesia)
2015-04-16
We have derived some excitation states of the one-dimensional Gross-Pitaevskii equation coupled by the gravitational potential. The methods that we have used here are taken by pursuing the recent work of Kivshar et. al. by considering the equation as a macroscopic quantum oscillator. To obtain the states, we have made the appropriate transformation to reduce the three-dimensional Gross-Pitaevskii equation into the one-dimensional Gross-Pitaevskii equation and applying the time-independent perturbation theory in the general solution of the one-dimensional Gross-Pitaevskii equation as a linear superposition of the normalized eigenfunctions of the Schrödinger equation for the harmonic oscillator potential. Moreover, we also impose the condition by assuming that some terms in the equation should be so small in order to preserve the use of the perturbation method.
Lifetime measurement of the first excited 2+ state in 108Te
Bäck, T.; Qi, C.; Ghazi Moradi, F.; Cederwall, B.; Johnson, A.; Liotta, R.; Wyss, R.; Al-Azri, H.; Bloor, D.; Brock, T.; Wadsworth, R.; Grahn, T.; Greenlees, P. T.; Hauschild, K.; Herzan, A.; Jacobsson, U.; Jones, P. M.; Julin, R.; Juutinen, S.; Ketelhut, S.; Leino, M.; Lopez-Martens, A.; Nieminen, P.; Peura, P.; Rahkila, P.; Rinta-Antila, S.; Ruotsalainen, P.; Sandzelius, M.; Sarén, J.; Scholey, C.; Sorri, J.; Uusitalo, J.; Go, S.; Ideguchi, E.; Cullen, D. M.; Procter, M. G.; Braunroth, T.; Dewald, A.; Fransen, C.; Hackstein, M.; Litzinger, J.; Rother, W.
2011-10-01
The lifetime of the first excited 2+ state in the neutron deficient nuclide 108Te has been measured for the first time, using a combined recoil decay tagging and recoil distance Doppler shift technique. The deduced reduced transition probability is B(E2;0g.s.+→2+)=0.39-0.04+0.05e2b2. Compared to previous experimental data on neutron deficient tellurium isotopes, the new data point constitutes a large step (six neutrons) toward the N=50 shell closure. In contrast to what has earlier been reported for the light tin isotopes, our result for tellurium does not show any enhanced transition probability with respect to the theoretical predictions and the tellurium systematics including the new data is successfully reproduced by state-of-the-art shell model calculations.
Contribution of excited states to stellar weak-interaction rates in odd-A nuclei
Sarriguren, Pedro
2016-01-01
Weak-interaction rates, including beta-decay and electron capture, are studied in several odd-A nuclei in the pf-shell region at various densities and temperatures of astrophysical interest. Special attention is paid to the relative contribution to these rates of thermally populated excited states in the decaying nucleus. The nuclear structure involved in the weak processes is studied within a quasiparticle random-phase approximation with residual interactions in both particle-hole and particle-particle channels on top of a deformed Skyrme Hartree-Fock mean field with pairing correlations. In the range of densities and temperatures considered, it is found that the total rates do not differ much from the rates of the ground state fully populated. In any case, the changes are not larger than the uncertainties due to the nuclear model dependence of the rates.
Fernandez-Alberti, Sebastian; Makhov, Dmitry V; Tretiak, Sergei; Shalashilin, Dmitrii V
2016-04-21
Photoinduced dynamics of electronic and vibrational unidirectional energy transfer between meta-linked building blocks in a phenylene ethynylene dendrimer is simulated using a multiconfigurational Ehrenfest in time-dependent diabatic basis (MCE-TDDB) method, a new variant of the MCE approach developed by us for dynamics involving multiple electronic states with numerous abrupt crossings. Excited-state energies, gradients and non-adiabatic coupling terms needed for dynamics simulation are calculated on-the-fly using the Collective Electron Oscillator (CEO) approach. A comparative analysis of our results obtained using MCE-TDDB, the conventional Ehrenfest method and the surface-hopping approach with and without decoherence corrections is presented. PMID:27004611
Xie, Weiwei; Domcke, Wolfgang; Farantos, Stavros C.; Grebenshchikov, Sergy Yu.
2016-03-01
A trajectory method of calculating tunneling probabilities from phase integrals along straight line tunneling paths, originally suggested by Makri and Miller [J. Chem. Phys. 91, 4026 (1989)] and recently implemented by Truhlar and co-workers [Chem. Sci. 5, 2091 (2014)], is tested for one- and two-dimensional ab initio based potentials describing hydrogen dissociation in the 1B1 excited electronic state of pyrrole. The primary observables are the tunneling rates in a progression of bending vibrational states lying below the dissociation barrier and their isotope dependences. Several initial ensembles of classical trajectories have been considered, corresponding to the quasiclassical and the quantum mechanical samplings of the initial conditions. It is found that the sampling based on the fixed energy Wigner density gives the best agreement with the quantum mechanical dissociation rates.
Study of ground and excited state decays in N ≈ Z Ag nuclei
Directory of Open Access Journals (Sweden)
Moschner K.
2015-01-01
Full Text Available A decay spectroscopy experiment was performed within the EURICA campaign at RIKEN in 2012. It aimed at the isomer and particle spectroscopy of excited states and ground states in the mass region below the doubly magic 100Sn. The N = Z nuclei 98In, 96Cd and 94Ag were of particular interest for the present study. Preliminary results on the neutron deficient nuclei 93Ag and 94Ag are presented. In 94Ag a more precise value for the half-life of the ground state’s superallowed Fermi transition was deduced. In addition the energy spectra of the mentioned decay could be reproduced through precise Geant4 simulations of the used active stopper SIMBA. This will enable us to extract Qβ values from the measured data. The decay of 93Ag is discussed based on the observed implantation-decay correlation events.
Excitation energy transfer in light-harvesting system: Effect of initial state
Cui, B; Oh, C H
2012-01-01
The light-harvesting is a problem of long interest. It becomes active again in recent years stimulated by suggestions of quantum effects in energy transport. Recent experiments found evidence that BChla 1 and BChla 6 are the first to be excited in the Fenna-Matthews-Olson(FMO) protein, theoretical studies, however, are mostly restricted to consider the exciton in BChla 1 initially. In this paper, we study the energy transport in the FMO complex by taking different initial states into account. Optimizations are performed for the decoherence rates as to maximal transport efficiency. Dependence of the energy transfer efficiency on the initial states is given and discussed. Effects of fluctuations in the site energies and couplings are also examined.
Energy Technology Data Exchange (ETDEWEB)
Karmakar, Shreetama; Mukhopadhyay, Deb Pratim; Chakraborty, Tapas, E-mail: pctc@iacs.res.in [Physical Chemistry Department, Indian Association for the Cultivation of Science, Jadavpur, Kolkata 700032 (India)
2015-05-14
Multiple fluorine atom substitution effect on photophysics of an aromatic chromophore has been investigated using phenol as the reference system. It has been noticed that the discrete vibronic structure of the S{sub 1}←S{sub 0} absorption system of phenol vapor is completely washed out for pentafluorophenol (PFP), and the latter also shows very large Stokes shift in the fluorescence spectrum. For excitations beyond S{sub 1} origin, the emission yield of PFP is reduced sharply with increase in excess vibronic energy. However, in a collisional environment like liquid hydrocarbon, the underlying dynamical process that drives the non-radiative decay is hindered drastically. Electronic structure theory predicts a number of low-lying dark electronic states of πσ{sup ∗} character in the vicinity of the lowest valence ππ{sup ∗} state of this molecule. Tentatively, we have attributed the excitation energy dependent non-radiative decay of the molecule observed only in the gas phase to an interplay between the lowest ππ{sup ∗} and a nearby dissociative πσ{sup ∗} state. Measurements in different liquids reveal that some of the dark excited states light up with appreciable intensity only in protic liquids like methanol and water due to hydrogen bonding between solute and solvents. Electronic structure theory methods indeed predict that for PFP-(H{sub 2}O){sub n} clusters (n = 1-11), intensities of a number of πσ{sup ∗} states are enhanced with increase in cluster size. In contrast with emitting behavior of the molecule in the gas phase and solutions of nonpolar and polar aprotic liquids, the fluorescence is completely switched off in polar protic liquids. This behavior is a chemically significant manifestation of perfluoro effect, because a very opposite effect occurs in the case of unsubstituted phenol for which fluorescence yield undergoes a very large enhancement in protic liquids. Several dynamical mechanisms have been suggested to interpret the
McCoy, Anne B.; Ford, Jason E.; Marlett, Melanie L.; Petit, Andrew S.
2014-06-01
In this work, an extension to diffusion Monte Carlo (DMC) is proposed, allowing for the simultaneous calculation of the energy and wave function of multiple rotationally excited states of floppy molecules. The total wave function is expanded into a set of Dirac δ-functions called walkers, while the rotational portion of the wave function is expanded in a symmetric top basis set. Each walker is given a rotational state vector containing coefficients for all states of interest. The positions of the atoms and the coefficients in the state vector evolve according to the split operator approximation of the quantum propagator. The method was benchmarked by comparing calculated rotation-vibration energies for H_3^+, H_2D^+, and H_3O^+ to experimental values. For low to moderate values of J, the resulting energies are within the statistical uncertainty of the calculation. Rotation-vibration coupling is captured through flexibility introduced in the form of the vibrational wave function. This coupling is found to increase with increasing J-values. Based on the success achieved through these systems, the method was applied to CH_5^+ and its deuterated isotopologues for v = 0, J ≥ 10. Based on these calculations, the energy level structure of CH_5^+ is found to resemble that for a of a spherical top, and excitations up to J = 10 displayed insignificant rotation-vibration coupling. Extensions of this approach that explicitly account for vibrations will also be discussed. ` A. S. Petit, J. E. Ford and A. B. McCoy, J. Phys. Chem. A, in press, K. D. Jordan Festschrift, DOI: 10.1021/jp408821a
Beta decay of neutron-rich {sup 118}Rh and the lowest excited states in {sup 118}Pd
Energy Technology Data Exchange (ETDEWEB)
Jokinen, A.; Wang, J.C.; Aeystoe, J.; Dendooven, P.; Nummela, S.; Huikari, J.; Kolhinen, V.; Nieminen, A.; Peraejaervi, K.; Rinta-Antila, S. [Jyvaeskylae Univ. (Finland). Dept. of Physics
2000-09-01
Beta decay of a refractory isotope {sup 118}Rh produced in symmetric fission and mass separated by the ion guide technique has been applied for the study of low-lying excited states of {sup 118}Pd. The yrast band in {sup 118}Pd has been observed up to a 6{sup +} state and the lowest states of the asymmetric {gamma}-band have been identified. The measured half-life of {sup 118}Rh is (300{+-}60)ms. The systematics of the excited states in neutron-rich Pd-isotopes implies the saturation towards an O(6) symmetry at N=70. (orig.)
Ground-state and low-lying excitations of the Heisenberg antiferromagnet
International Nuclear Information System (INIS)
Monte Carlo methods are used to determine the exact ground-state energy of the spin-1/2 Heisenberg antiferromagnet on two-dimensional square periodic lattices up to size 32 x 32. The extrapolated ground-state energy for infinite lattice size is -0.33459+-0.000 05. In addition, splittings between the ground state and the lowest spin-1 and -2 excitations are determined as a function of lattice size. The scaling of both the ground-state energy and the gap are in agreement with that predicted by spin-wave theory over a wide range of lattice sizes. In particular, numerical results demonstrate convincingly the lack of a gap for infinite systems, and that the gap for finite systems scales with the inverse volume of the lattice. Finally, we present results for the ground-state spin-correlation function. Our approximate results for larger lattices indicate that the staggered magnetization is 0.34+-0.01 units where the saturated value is
Zaouris, Dimitris; Kartakoullis, Andreas; Glodic, Pavle; Samartzis, Peter C; Rafn Hróðmarsson, Helgi; Kvaran, Ágúst
2015-04-28
Photoexcitation dynamics of the E((1)Σ(+)) (v' = 0) Rydberg state and the V((1)Σ(+)) (v') ion-pair vibrational states of HBr are investigated by velocity map imaging (VMI). H(+) photoions, produced through a number of vibrational and rotational levels of the two states were imaged and kinetic energy release (KER) and angular distributions were extracted from the data. In agreement with previous work, we found the photodissociation channels forming H*(n = 2) + Br((2)P3/2)/Br*((2)P1/2) to be dominant. Autoionization pathways leading to H(+) + Br((2)P3/2)/Br*((2)P1/2) via either HBr(+)((2)Π3/2) or HBr(+)*((2)Π1/2) formation were also present. The analysis of KER and angular distributions and comparison with rotationally and mass resolved resonance enhanced multiphoton ionization (REMPI) spectra revealed the excitation transition mechanisms and characteristics of states involved as well as the involvement of the E-V state interactions and their v' and J' dependence. PMID:25801122
Intermediate Coupling For Core-Level Excited States: Consequences For X-Ray Absorption Spectroscopy
Energy Technology Data Exchange (ETDEWEB)
Bagus, Paul S.; Sassi, Michel JPC; Rosso, Kevin M.
2015-04-15
The origin of the complex NEXAFS features of X-Ray Absorption, XAS, spectra in transition metal complexes is analyzed and interpreted in terms of the angular momentum coupling of the open shell electrons. Especially for excited configurations where a core-electron is promoted to an open valence shell, the angular momentum coupling is intermediate between the two limits of Russell- Saunders, RS, coupling where spin-orbit splitting of the electron shells is neglected and j-j coupling where this splitting is taken as dominant. The XAS intensities can be understood in terms of two factors: (1) The dipole selection rules that give the allowed excited RS multiplets and (2) The contributions of these allowed multiplets to the wavefunctions of the intermediate coupled levels. It is shown that the origin of the complex XAS spectra is due to the distribution of the RS allowed multiplets over several different intermediate coupled excited levels. The specific case that is analyzed is the L2,3 edge XAS of an Fe3+ cation, because this cation allows a focus on the angular momentum coupling to the exclusion of other effects; e.g., chemical bonding. Arguments are made that the properties identified for this atomic case are relevant for more complex materials. The analysis is based on the properties of fully relativistic, ab initio, many-body wavefunctions for the initial and final states of the XAS process. The wavefunction properties considered include the composition of the wavefunctions in terms of RS multiplets and the occupations of the spin-orbit split open shells; the latter vividly show whether the coupling is j-j or not.
Dietzek, Benjamin; Kiefer, Wolfgang; Blumhoff, Jörg; Böttcher, Lars; Rau, Sven; Walther, Dirk; Uhlemann, Ute; Schmitt, Michael; Popp, Jürgen
2006-06-23
A detailed study on the excited-state-excitation migration taking place within the tetranuclear complex [{(tbbpy)(2)Ru(tmbi)}(2){Pd(allyl)}(2)](PF(6))(2) (tbbpy = 4,4'-di-tert-butyl-2,2'-bipyridine and tmbi = 5,6,5',6'-tetramethyl-2,2'-bibenzimidazolate) is presented. The charge transfer is initiated by the photoexcitation into the lowest metal-to-ligand charge-transfer (MLCT) band of one of the peripheral ruthenium(II) chromophores and terminates on the central structurally complex Pd(2) (II)(allyl)(2) subunit. Thus, the system under investigation can be thought of as a functional model for the photosynthesis reaction center in plants. The kinetic steps involved in the overall process are inferred from femtosecond time-resolved transient-grating kinetics recorded at spectral positions within the regions of ground-state bleach and transient absorption. The kinetics features a complex non-exponential time behavior and can be fitted to a bi-exponential rise (tau(1)> or =200 fs, tau(2) approximately 1.5 ps) and a mono- or bi-exponential decay, depending on the experimental situation. The data leads to the formulation of a model for the intramolecular excitation-hopping ascribing intersystem crossing and subsequent cooling as the two fastest observed processes. Following these initial steps, charge transfer from the ruthenium to the central complex Pd(2)(allyl)(2) moiety is observed with a characteristic time constant of 50 ps. A 220-ps component that is observed in the ground-state recovery only is attributed to excitation equilibration between the two identical Pd(allyl) chromophores. PMID:16628758
Excited-state dynamics of size-dependent colloidal TiO2-Au nanocomposites
Karam, Tony E.; Khoury, Rami A.; Haber, Louis H.
2016-03-01
The ultrafast excited-state dynamics of size-dependent TiO2-Au nanocomposites synthesized by reducing gold nanoclusters to the surface of colloidal TiO2 nanoparticles are studied using pump-probe transient absorption spectroscopy with 400 nm excitation pulses. The results show that the relaxation processes of the plasmon depletion band, which are described by electron-phonon and phonon-phonon scattering lifetimes, are independent of the gold nanocluster shell size surrounding the TiO2 nanoparticle core. The dynamics corresponding to interfacial electron transfer between the gold nanoclusters and the TiO2 bandgap are observed to spectrally overlap with the gold interband transition signal, and the electron transfer lifetimes are shown to significantly decrease as the nanocluster shell size increases. Additionally, size-dependent periodic oscillations are observed and are attributed to acoustic phonons of a porous shell composed of aggregated gold nanoclusters around the TiO2 core, with frequencies that decrease and damping times that remain constant as the nanocluster shell size increases. These results are important for the development of improved catalytic nanomaterial applications.
Coulomb Excitation of a Neutron-Rich $^{88}$Kr Beam Search for Mixed Symmetry States
Andreoiu, C; Napiorkowski, P J; Iwanicki, J S
2002-01-01
We propose to use the ISOLDE/REX/MINIBALL/CD set-up to perform a Coulomb Excitation experiment with a $^{88}$Kr radioactive beam. The motivation includes a search for $Mixed$ $Symmetry$ states predicted by the IBM-2 model, gathering more spectroscopy data about the $^{88}$Kr nucleus and extending shape coexistence studies (performed previously by the proposers for neutron-deficient Kr isotopes) to the neutron-rich side. The proposed experiment will provide data complementary to the Coulomb Excitation of a relativistic $^{88}$Kr beam proposed by D. Tonev et al. for a RISING experiment. A total of 12 days of beam time is necessary for the experiment, equally divided into two runs. One run with a 2.2 MeV/A beam energy on a $^{48}$Ti target and a second run with the maximum available REX energy of 3.1 MeV/A on a $^{208}$Pb target are requested. Using either a UC$_{x}$ or ThC$_{x}$ fissioning primary target coupled with a plasma source by a cooled transfer line seems to be the best choice for the proposed experime...
Gamow-Teller (GT$\\pm$) strength distributions of $^{56}Ni$ for ground and excited states
Nabi, Jameel-Un; Sajjad, Muhammad
2016-01-01
Gamow-Teller (GT) transitions play an important and consequential role in many astrophysical phenomena. These include, but are not limited to, electron and positron capture rates which determine the fate of massive stars and play an intricate role in the dynamics of core collapse. These $GT_{\\pm}$ transitions rates are the significant inputs in the description of supernova explosions. $GT_{\\pm}$ strength function values are sensitive to the $^{56}Ni$ core excitation in the middle \\textit{pf}-shell region and to the size of the model space as well. We used the pn-QRPA theory for extracting the GT strength for ground and excited states of $^{56}Ni$. We then used these GT strength distributions to calculate the electron \\textit{and} positron capture rates which show differences with the earlier calculations. One curious finding of this paper is our enhanced electron capture rates on $^{56}Ni$ at presupernova temperatures. These differences need to be taken into account for the modeling of the early stages of Typ...