WorldWideScience

Sample records for excitation energy transfer

  1. Integrated light in direct excitation and energy transfer luminescence

    OpenAIRE

    Chimczak, Eugeniusz

    2007-01-01

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

  2. A simplified approach for the coupling of excitation energy transfer

    Energy Technology Data Exchange (ETDEWEB)

    Shi Bo [Hefei National Laboratory for Physical Science at Microscale, University of Science and Technology of China, Hefei 230026 (China); Department of Chemical Physics, University of Science and Technology of China, Hefei 230026 (China); Gao Fang, E-mail: gaofang@iim.ac.cn [Institute of Intelligent Machines, Chinese Academy of Sciences, Hefei 230031 (China); State Key Laboratory of Robotics, Shenyang Institute of Automation, Chinese Academy of Sciences, Shenyang 110016 (China); Liang Wanzhen [Hefei National Laboratory for Physical Science at Microscale, University of Science and Technology of China, Hefei 230026 (China); Department of Chemical Physics, University of Science and Technology of China, Hefei 230026 (China)

    2012-02-06

    Highlights: Black-Right-Pointing-Pointer We propose a simple method to calculate the coupling of singlet-to-singlet and triplet-to-triplet energy transfer. Black-Right-Pointing-Pointer Coulomb term are the major contribution to the coupling of singlet-to-singlet energy transfer. Black-Right-Pointing-Pointer Effect from the intermolecular charge-transfer states dorminates in triplet-to-triplet energy transfer. Black-Right-Pointing-Pointer This method can be expanded by including correlated wavefunctions. - Abstract: A simplified approach for computing the electronic coupling of nonradiative excitation-energy transfer is proposed by following Scholes et al.'s construction on the initial and final states [G.D. Scholes, R.D. Harcourt, K.P. Ghiggino, J. Chem. Phys. 102 (1995) 9574]. The simplification is realized through defining a set of orthogonalized localized MOs, which include the polarization effect of the charge densities. The method allows calculating the coupling of both the singlet-to-singlet and triplet-to-triplet energy transfer. Numerical tests are performed for a few of dimers with different intermolecular orientations, and the results demonstrate that Coulomb term are the major contribution to the coupling of singlet-to-singlet energy transfer whereas in the case of triplet-to-triplet energy transfer, the dominant effect is arisen from the intermolecular charge-transfer states. The present application is on the Hartree-Fock level. However, the correlated wavefunctions which are normally expanded in terms of the determinant wavefunctions can be employed in the similar way.

  3. Neutron scattering investigation of magnetic excitations at high energy transfers

    International Nuclear Information System (INIS)

    Loong, C.K.

    1984-01-01

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

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

    International Nuclear Information System (INIS)

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

    1995-01-01

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

  5. Influence of donor-donor transport on excitation energy transfer

    Energy Technology Data Exchange (ETDEWEB)

    Pandey, K K; Joshi, H C; Pant, T C [Kumaun University, Nainital (India). Department of Physics

    1989-01-01

    Energy migration and transfer from acriflavine to rhodamine B and malachite green in poly (methylmethacrylate) have been investigated using the decay function analysis. It is found that the influence of energy migration in energy transfer can be described quite convincingly by making use of the theories of Loring, Andersen and Fayer (LAF) and Huber. At high acceptor concentration direct donor-acceptor transfer occurs through Forster mechanism. (author). 17 refs., 5 figs.

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

    Science.gov (United States)

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

    2015-04-15

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

  7. Low-energy charge transfer excitations in NiO

    International Nuclear Information System (INIS)

    Sokolov, V I; Yermakov, A Ye; Uimin, M A; Gruzdev, N B; Pustovarov, V A; Churmanov, V N; Ivanov, V Yu; Sokolov, P S; Baranov, A N; Moskvin, A S

    2012-01-01

    Comparative analysis of photoluminescence (PL) and photoluminescence excitation (PLE) spectra of NiO poly- and nanocrystals in the spectral range 2-5.5 eV reveals two PLE bands peaked near 3.7 and 4.6 eV with a dramatic rise in the low-temperature PLE spectral weight of the 3.7 eV PLE band in the nanocrystalline NiO as compared with its polycrystalline counterpart. In frames of a cluster model approach we assign the 3.7 eV PLE band to the low-energy bulk-forbidden p-d (t 1g (π)-e g ) charge transfer (CT) transition which becomes the allowed one in the nanocrystalline state while the 4.6 eV PLE band is related to a bulk allowed d-d (e g -e g ) CT transition scarcely susceptible to the nanocrystallization. The PLE spectroscopy of the nanocrystalline materials appears to be a novel informative technique for inspection of different CT transitions.

  8. Vibrational energy transfer in selectively excited diatomic molecules

    International Nuclear Information System (INIS)

    Dasch, C.J.

    1978-09-01

    Single rovibrational states of HCl(v=2), HBr(v=2), DCl(v=2), and CO(v=2) were excited with a pulsed optical parametric oscillator (OPO). Total vibrational relaxation rates near - resonance quenchers were measured at 295 0 K using time resolved infrared fluorescence. These rates are attributed primarily to V - V energy transfer, and they generally conform to a simple energy gap law. A small deviation was found for the CO(v) + DCl(v') relaxation rates. Upper limits for the self relaxation by V - R,T of HCl(v=2) and HBr(v=2) and for the two quantum exchange between HCl and HBr were determined. The HF dimer was detected at 295 0 K and 30 torr HF pressure with an optoacoustic spectrometer using the OPO. Pulsed and chopped, resonant and non-resonant spectrophones are analyzed in detail. From experiments and first order perturbation theory, these V - V exchange rates appear to behave as a first order perturbation in the vibrational coordinates. The rotational dynamics are known to be complicated however, and the coupled rotational - vibrational dynamics were investigated theoreticaly in infinite order by the Dillon and Stephenson and the first Magnus approximations. Large ΔJ transitions appear to be important, but these calculations differ by orders of magnitude on specific rovibrational transition rates. Integration of the time dependent semiclassical equations by a modified Gordon method and a rotationally distorted wave approximation are discussed as methods which would treat the rotational motion more accurately. 225 references

  9. Frequency and wavenumber selective excitation of spin waves through coherent energy transfer from elastic waves

    OpenAIRE

    Hashimoto, Yusuke; Bossini, Davide; Johansen, Tom H.; Saitoh, Eiji; Kirilyuk, Andrei; Rasing, Theo

    2017-01-01

    Using spin-wave tomography (SWaT), we have investigated the excitation and the propagation dynamics of optically-excited magnetoelastic waves, i.e. hybridized modes of spin waves and elastic waves, in a garnet film. By using time-resolved SWaT, we reveal the excitation dynamics of magnetoelastic waves through coherent-energy transfer between optically-excited pure-elastic waves and spin waves via magnetoelastic coupling. This process realizes frequency and wavenumber selective excitation of s...

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

    International Nuclear Information System (INIS)

    Hirakawa, Kazutaka; Segawa, Hiroshi

    2016-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-11-15

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

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

    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...

  13. Excitation energy transfer from dye molecules to doped graphene

    Indian Academy of Sciences (India)

    Recently, we have reported theoretical studies on the rate of energy transfer ... Dirac cone approximation and hence our conclusions are of qualitative nature. 2. .... make another change of variable to r given by r = ki q/2 to get. G1 (q) = Aq2.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-01-15

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

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

    International Nuclear Information System (INIS)

    Armstrong, T.D.

    1994-01-01

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

  16. Coherent excitation-energy transfer and quantum entanglement in a dimer

    International Nuclear Information System (INIS)

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

    2010-01-01

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

  17. Generating Excitement: Build Your Own Generator to Study the Transfer of Energy

    Science.gov (United States)

    Fletcher, Kurt; Rommel-Esham, Katie; Farthing, Dori; Sheldon, Amy

    2011-01-01

    The transfer of energy from one form to another can be difficult to understand. The electrical energy that turns on a lamp may come from the burning of coal, water falling at a hydroelectric plant, nuclear reactions, or gusts of wind caused by the uneven heating of the Earth. The authors have developed and tested an exciting hands-on activity to…

  18. Elastic, excitation, ionization and charge transfer cross sections of current interest in fusion energy research

    Energy Technology Data Exchange (ETDEWEB)

    Schultz, D.R.; Krstic, P.S. [Oak Ridge National Lab. TN (United States). Physics Div.

    1997-01-01

    Due to the present interest in modeling and diagnosing the edge and divertor plasma regions in magnetically confined fusion devices, we have sought to provide new calculations regarding the elastic, excitation, ionization, and charge transfer cross sections in collisions among relevant ions, neutrals, and isotopes in the low-to intermediate-energy regime. We summarize here some of our recent work. (author)

  19. Mechanism and models for collisional energy transfer in highly excited large polyatomic molecules

    International Nuclear Information System (INIS)

    Gilbert, R. G.

    1995-01-01

    Collisional energy transfer in highly excited molecules (say, 200-500 kJ mol -1 above the zero-point energy of reactant, or of product, for a recombination reaction) is reviewed. An understanding of this energy transfer is important in predicting and interpreting the pressure dependence of gas-phase rate coefficients for unimolecular and recombination reactions. For many years it was thought that this pressure dependence could be calculated from a single energy-transfer quantity, such as the average energy transferred per collision. However, the discovery of 'super collisions' (a small but significant fraction of collisions which transfer abnormally large amounts of energy) means that this simplistic approach needs some revision. The 'ordinary' (non-super) component of the distribution function for collisional energy transfer can be quantified either by empirical models (e.g., an exponential-down functional form) or by models with a physical basis, such as biased random walk (applicable to monatomic or diatomic collision partners) or ergodic (for polyatomic collision partners) treatments. The latter two models enable approximate expressions for the average energy transfer to be estimated from readily available molecular parameters. Rotational energy transfer, important for finding the pressure dependence for recombination reactions, can for these purposes usually be taken as transferring sufficient energy so that the explicit functional form is not required to predict the pressure dependence. The mechanism of 'ordinary' energy transfer seems to be dominated by low-frequency modes of the substrate, whereby there is sufficient time during a vibrational period for significant energy flow between the collision partners. Super collisions may involve sudden energy flow as an outer atom of the substrate is squashed between the substrate and the bath gas, and then is moved away from the interaction by large-amplitude motion such as a ring vibration or a rotation; improved

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

    Science.gov (United States)

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

    2018-04-01

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

  1. Is There Excitation Energy Transfer between Different Layers of Stacked Photosystem-II-Containing Thylakoid Membranes?

    Science.gov (United States)

    Farooq, Shazia; Chmeliov, Jevgenij; Trinkunas, Gediminas; Valkunas, Leonas; van Amerongen, Herbert

    2016-04-07

    We have compared picosecond fluorescence decay kinetics for stacked and unstacked photosystem II membranes in order to evaluate the efficiency of excitation energy transfer between the neighboring layers. The measured kinetics were analyzed in terms of a recently developed fluctuating antenna model that provides information about the dimensionality of the studied system. Independently of the stacking state, all preparations exhibited virtually the same value of the apparent dimensionality, d = 1.6. Thus, we conclude that membrane stacking does not affect the efficiency of the delivery of excitation energy toward the reaction centers but ensures a more compact organization of the thylakoid membranes within the chloroplast and separation of photosystems I and II.

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

    Science.gov (United States)

    Wang, Luxia; May, Volkhard

    2017-08-01

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

  3. Environment-assisted Quantum Critical Effect for Excitation Energy Transfer in a LH2-type Trimer

    Science.gov (United States)

    Xu, Lan; Xu, Bo

    2015-10-01

    In this article, we are investigating excitation energy transfer (EET) in a basic unit cell of light-harvesting complex II (LH2), named a LH2-type trimer. Calculation of energy transfer efficiency (ETE) in the framework of non-Markovian environment is also implemented. With these achievements, we theoretically predict the environment-assisted quantum critical effect, where ETE exhibits a sudden change at the critical point of quantum phase transition (QPT) for the LH2-type trimer. It is found that highly efficient EET with nearly unit efficiency may occur in the vicinity of the critical point of QPT.

  4. Radiative transport and collisional transfer of excitation energy in Cs vapors mixed with Ar or He

    International Nuclear Information System (INIS)

    Vadla, Cedomil; Horvatic, Vlasta; Niemax, Kay

    2003-01-01

    This paper is a review (with a few original additions) on the radiative transport and collisional transfer of energy in laser-excited cesium vapors in the presence of argon or helium. Narrow-band excitation of lines with Lorentz, Doppler and Voigt profiles is studied in order to calculate effective rates for pumping of spectral lines with profiles comprising inhomogeneous broadening components. The radiative transport of excitation energy is considered, and a new, simple and robust, but accurate theoretical method for quantitative treatment of radiation trapping in relatively optically thin media is presented. Furthermore, comprehensive lists of experimental values for the excitation energy transfer cross-sections related to thermal collisions in Cs-Ar and Cs-He mixtures are given. Within the collected cross-section data sets, specific regularities with respect to the energy defect, as well as the temperature, are discerned. A particular emphasis is put on the radiative and collisional processes important for the optimization of resonance-fluorescence imaging atomic filters based on Cs-noble gas systems

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

    Science.gov (United States)

    Barklem, P. S.

    2018-05-01

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

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

    Science.gov (United States)

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

    2017-12-21

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

  7. Picosecond excitation energy transfer of allophycocyanin studied in solution and in crystals.

    Science.gov (United States)

    Ranjbar Choubeh, Reza; Sonani, Ravi R; Madamwar, Datta; Struik, Paul C; Bader, Arjen N; Robert, Bruno; van Amerongen, Herbert

    2018-03-01

    Cyanobacteria perform photosynthesis with the use of large light-harvesting antennae called phycobilisomes (PBSs). These hemispherical PBSs contain hundreds of open-chain tetrapyrrole chromophores bound to different peptides, providing an arrangement in which excitation energy is funnelled towards the PBS core from where it can be transferred to photosystem I and/or photosystem II. In the PBS core, many allophycocyanin (APC) trimers are present, red-light-absorbing phycobiliproteins that covalently bind phycocyanobilin (PCB) chromophores. APC trimers were amongst the first light-harvesting complexes to be crystallized. APC trimers have two spectrally different PCBs per monomer, a high- and a low-energy pigment. The crystal structure of the APC trimer reveals the close distance (~21 Å) between those two chromophores (the distance within one monomer is ~51 Å) and this explains the ultrafast (~1 ps) excitation energy transfer (EET) between them. Both chromophores adopt a somewhat different structure, which is held responsible for their spectral difference. Here we used spectrally resolved picosecond fluorescence to study EET in these APC trimers both in crystallized and in solubilized form. We found that not all closely spaced pigment couples consist of a low- and a high-energy pigment. In ~10% of the cases, a couple consists of two high-energy pigments. EET to a low-energy pigment, which can spectrally be resolved, occurs on a time scale of tens of picoseconds. This transfer turns out to be three times faster in the crystal than in the solution. The spectral characteristics and the time scale of this transfer component are similar to what have been observed in the whole cells of Synechocystis sp. PCC 6803, for which it was ascribed to EET from C-phycocyanin to APC. The present results thus demonstrate that part of this transfer should probably also be ascribed to EET within APC trimers.

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

    Science.gov (United States)

    Ghosh, Soumen

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

  9. Excitation and charge transfer in low-energy hydrogen atom collisions with neutral oxygen

    Science.gov (United States)

    Barklem, P. S.

    2018-02-01

    Excitation and charge transfer in low-energy O+H collisions is studied; it is a problem of importance for modelling stellar spectra and obtaining accurate oxygen abundances in late-type stars including the Sun. The collisions have been studied theoretically using a previously presented method based on an asymptotic two-electron linear combination of atomic orbitals (LCAO) model of ionic-covalent interactions in the neutral atom-hydrogen-atom system, together with the multichannel Landau-Zener model. The method has been extended to include configurations involving excited states of hydrogen using an estimate for the two-electron transition coupling, but this extension was found to not lead to any remarkably high rates. Rate coefficients are calculated for temperatures in the range 1000-20 000 K, and charge transfer and (de)excitation processes involving the first excited S-states, 4s.5So and 4s.3So, are found to have the highest rates. Data are 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/vizbin/qcat?J/A+A/610/A57. The data are also available at http://https://github.com/barklem/public-data

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-08-15

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

  11. The mechanism of three-body process of energy transfer from excited xenon atoms to molecules

    International Nuclear Information System (INIS)

    Wojciechowski, K.; Forys, M.

    1999-01-01

    The mechanism of energy transfer from Xe(6 s[3/2] 1 ) resonance state (E=8.44 eV) and higher excited Xe(6p, 6p', 6 d) atoms produced in pulse radiolysis to molecules have been discussed. The analysis of the kinetic data for these processes shows that in the sensitized photolysis and radiolysis of Xe-M mixtures the excited atoms decay in 'ordinary' two-body reaction: Xe(6s[3/2] 1 0 )+M→products (r.1) and in fast 'accelerated' third order process: Xe(6s[3/2] 1 0 )+M+Xe→products (r.2) The discussion shows that three-body process occurs via reactions: Xe(6s[3/2] 1 0 )+Xe k w ↔ k d Xe 2 ** (r.2a) Xe 2 **+M k q →[Xe 2 M]*→products (r.2b) It was shown that this mechanism concerns also higher excited Xe atoms and can explain a similar process in He-M mixtures and suggests that it is a general mechanism of energy transfer in all irradiated rare gas-molecule systems

  12. Charge transfer and excitation in high-energy ion-atom collisions

    International Nuclear Information System (INIS)

    Schlachter, A.S.; Berkner, K.H.; McDonald, R.J.

    1986-11-01

    Coincidence measurements of charge transfer and simultaneous projectile electron excitation provide insight into correlated two-electron processes in energetic ion-atom collisions. Projectile excitation and electron capture can occur simultaneously in a collision of a highly charged ion with a target atom; this process is called resonant transfer and excitation (RTE). The intermediate excited state which is thus formed can subsequently decay by photon emission or by Auger-electron emission. Results are shown for RTE in both the K shell of Ca ions and the L shell of Nb ions, for simultaneous projectile electron loss and excitation, and for the effect of RTE on electron capture

  13. Strategy of ring-shaped aggregates in excitation energy transfer for removing disorder-induced shielding

    International Nuclear Information System (INIS)

    Tei, Go; Nakatani, Masatoshi; Ishihara, Hajime

    2013-01-01

    Peripheral light harvesting complex (LH2), which is found in photosynthetic antenna systems of purple photosynthetic bacteria, has important functions in the photosynthetic process, such as harvesting sunlight and transferring its energy to the photosynthetic reaction center. The key component in excitation energy transfer (EET) between LH2s is B850, which is a characteristic ring-shaped aggregate of pigments usually formed by 18 or 16 bacteriochlorophylls in LH2. We theoretically study the strategy of the ring-shaped aggregate structure, which maximizes EET efficiency, by using the standard Frenkel exciton model and the self-consistent calculation method for the Markovian quantum master equation and Maxwell equation. As a result, we have revealed a simple but ingenious strategy of the ring-shaped aggregate structure. The combination of three key properties of the ring unit system maximizes the EET efficiency, namely the large dipole moment of aggregates causes the basic improvement of EET efficiency, and the isotropic nature and the large occupying area are critically effective to remove the disorder-induced shielding that inhibits EET in the presence of the randomness of orientation and alignment of carriers of excitation energy. (paper)

  14. Strategy of ring-shaped aggregates in excitation energy transfer for removing disorder-induced shielding

    Science.gov (United States)

    Tei, Go; Nakatani, Masatoshi; Ishihara, Hajime

    2013-06-01

    Peripheral light harvesting complex (LH2), which is found in photosynthetic antenna systems of purple photosynthetic bacteria, has important functions in the photosynthetic process, such as harvesting sunlight and transferring its energy to the photosynthetic reaction center. The key component in excitation energy transfer (EET) between LH2s is B850, which is a characteristic ring-shaped aggregate of pigments usually formed by 18 or 16 bacteriochlorophylls in LH2. We theoretically study the strategy of the ring-shaped aggregate structure, which maximizes EET efficiency, by using the standard Frenkel exciton model and the self-consistent calculation method for the Markovian quantum master equation and Maxwell equation. As a result, we have revealed a simple but ingenious strategy of the ring-shaped aggregate structure. The combination of three key properties of the ring unit system maximizes the EET efficiency, namely the large dipole moment of aggregates causes the basic improvement of EET efficiency, and the isotropic nature and the large occupying area are critically effective to remove the disorder-induced shielding that inhibits EET in the presence of the randomness of orientation and alignment of carriers of excitation energy.

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

    Science.gov (United States)

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

    2016-04-01

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

  16. High Excitation Transfer Efficiency from Energy Relay Dyes in Dye-Sensitized Solar Cells

    KAUST Repository

    Hardin, Brian E.

    2010-08-11

    The energy relay dye, 4-(Dicyanomethylene)-2-methyl-6-(4- dimethylaminostyryl)-4H-pyran (DCM), was used with a near-infrared sensitizing dye, TT1, to increase the overall power conversion efficiency of a dye-sensitized solar cell (DSC) from 3.5% to 4.5%. The unattached DCM dyes exhibit an average excitation transfer efficiency (EÌ?TE) of 96% inside TT1-covered, mesostructured TiO2 films. Further performance increases were limited by the solubility of DCM in an acetonitrile based electrolyte. This demonstration shows that energy relay dyes can be efficiently implemented in optimized dye-sensitized solar cells, but also highlights the need to design highly soluble energy relay dyes with high molar extinction coefficients. © 2010 American Chemical Society.

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

    NARCIS (Netherlands)

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

    2010-01-01

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

  18. NO-γ emissions from streamer discharges: direct electron impact excitation versus resonant energy transfer

    International Nuclear Information System (INIS)

    Liu Ningyu; Pasko, Victor P

    2010-01-01

    It has been established that production of NO-γ emission in pulsed corona discharges is dominated by the energy transfer from N 2 (A 3 Σ u + ) to the NO ground state NO(X 2 Π r ) while direct excitation by electron impact is negligible. However, recent studies suggest that the electron impact excitation plays a more important role. In this work, we report modelling results of NO-γ emission associated with streamer discharges using two cross section data sets available in the literature. The first set was originally reported by Mojarrabi et al (1996 Phys. Rev. A 54 2977-82) and later updated by Brunger et al (2000 J. Phys. B: At. Mol. Opt. Phys. 33 809-19); the second set was published by Hayashi (1990 Nonequilibrium Processes in Partially Ionized Gases (NATO Advanced Science Institutes Series, Series B, Physics vol 220) ed M Capitelli and J N Bardsley (New York: Plenum) pp 333-40). According to the results, the role played by the electron impact excitation in the production of NO-γ is drastically different when different cross sections are used. The results indicate that the first data set leads to better agreement with experimental measurements. (fast track communication)

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-12-21

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

  20. Ab initio configuration interaction description of excitation energy transfer between closely packed molecules

    International Nuclear Information System (INIS)

    Fink, R.F.; Pfister, J.; Schneider, A.; Zhao, H.; Engels, B.

    2008-01-01

    We present new, generally applicable protocols for the computation of the coupling parameter, J, of excitation energy transfer with quantum chemical ab initio methods. The protocols allow to select the degree of approximation and computational demand such that they are applicable for realistic systems and still allow to control the quality of the approach. We demonstrate the capabilities of the different protocols using the CO dimer as a first example. Correlation effects are found to scale J by a factor of about 0.7 which is in good agreement to earlier results obtained for the ethene dimer. The various levels of the protocol allow to assess the influence of ionic configurations and the polarisation within the dimer. Further, the interplay between the Foerster and Dexter contribution to J is investigated. The computations also show error compensation within approximations that are widely used for extended systems as in particular the transition density cube method

  1. Ab initio configuration interaction description of excitation energy transfer between closely packed molecules

    Energy Technology Data Exchange (ETDEWEB)

    Fink, R.F. [University of Wuerzburg, Institute of Organic Chemistry, Am Hubland, D-97074 Wuerzburg (Germany)], E-mail: reinhold.fink@rub.de; Pfister, J.; Schneider, A.; Zhao, H.; Engels, B. [University of Wuerzburg, Institute of Organic Chemistry, Am Hubland, D-97074 Wuerzburg (Germany)

    2008-01-29

    We present new, generally applicable protocols for the computation of the coupling parameter, J, of excitation energy transfer with quantum chemical ab initio methods. The protocols allow to select the degree of approximation and computational demand such that they are applicable for realistic systems and still allow to control the quality of the approach. We demonstrate the capabilities of the different protocols using the CO dimer as a first example. Correlation effects are found to scale J by a factor of about 0.7 which is in good agreement to earlier results obtained for the ethene dimer. The various levels of the protocol allow to assess the influence of ionic configurations and the polarisation within the dimer. Further, the interplay between the Foerster and Dexter contribution to J is investigated. The computations also show error compensation within approximations that are widely used for extended systems as in particular the transition density cube method.

  2. Rate for energy transfer from excited cyclohexane to nitrous oxide in the liquid phase

    International Nuclear Information System (INIS)

    Wada, T.; Hatano, Y.

    1975-01-01

    Pure liquid cyclohexane and cyclohexane solutions of nitrous oxide have been photolyzed at 163 nm. The quantum yield of the product hydrogen in the photolysis of pure cyclohexane is found to be 1.0. The addition of nitrous oxide results in the reduction in the yield of hydrogen and in the formation of nitrogen. The decrement of the hydrogen yield is approximately equal to the increment of the nitrogen yield. About 40 percent of the hydrogen yield in pure cyclohexane is found to be produced through a path which is not affected by the addition of nitrous oxide. The effect of the addition of nitrous oxide is attributed to energy transfer from excited cyclohexane to nitrous oxide with the rate constant of k = 1.0 x 10 11 M -1 sec -1 (at 15 0 C). This value is about a factor of 10 larger than that expected as for diffusion-controlled rate. A contribution of the energy transfer process to the formation of nitrogen in the radiolysis of cyclohexane solutions of nitrous oxide has also been discussed. (auth)

  3. A coherent modified Redfield theory for excitation energy transfer in molecular aggregates

    Energy Technology Data Exchange (ETDEWEB)

    Hwang-Fu, Yu-Hsien; Chen, Wei; Cheng, Yuan-Chung, E-mail: yuanchung@ntu.edu.tw

    2015-02-02

    Highlights: • A CMRT method for coherent energy transfer in molecular aggregates was developed. • Applicability of the method was verified in two-site systems with various parameters. • CMRT accurately describes population dynamics in the FMO-complex. • The method is accurate in a large parameter space and computationally efficient. - Abstract: Excitation energy transfer (EET) is crucial in photosynthetic light harvesting, and quantum coherence has been recently proven to be a ubiquitous phenomenon in photosynthetic EET. In this work, we derive a coherent modified Redfield theory (CMRT) that generalizes the modified Redfield theory to treat coherence dynamics. We apply the CMRT method to simulate the EET in a dimer system and compare the results with those obtained from numerically exact path integral calculations. The comparison shows that CMRT provides excellent computational efficiency and accuracy within a large EET parameter space. Furthermore, we simulate the EET dynamics in the FMO complex at 77 K using CMRT. The results show pronounced non-Markovian effects and long-lasting coherences in the ultrafast EET, in excellent agreement with calculations using the hierarchy equation of motion approach. In summary, we have successfully developed a simple yet powerful framework for coherent EET dynamics in photosynthetic systems and organic materials.

  4. Energy transfer and quenching processes of excited uranyl ion and lanthanide ions in solutions

    International Nuclear Information System (INIS)

    Yamamura, Tomoo; Tomiyasu, Hiroshi

    1995-01-01

    Deactivation processes of photoexcited uranyl ion by various lanthanide ions in aqueous solution were studied. Each lanthanide ions show different interaction with excited uranyl ion depending on its lowest excited energy level, the number of 4f electrons and the acid concentration of the solution. (author)

  5. General theory of excitation energy transfer in donor-mediator-acceptor systems.

    Science.gov (United States)

    Kimura, Akihiro

    2009-04-21

    General theory of the excitation energy transfer (EET) in the case of donor-mediator-acceptor system was constructed by using generalized master equation (GME). In this theory, we consider the direct and indirect transitions in the EET consistently. Hence, our theory includes the quantum mechanical interference between the direct and indirect transitions automatically. Memory functions in the GME were expressed by the overlap integrals among the time-dependent emission spectrum of the donor, the absorption spectrum of the mediator, the time-dependent emission spectrum of the mediator, and the absorption spectrum of the acceptor. In the Markov limit of the memory functions, we obtained the rate of EET which consists of three terms due to the direct transition, the indirect transition, and the interference between them. We found that the interference works effectively in the limit of slow thermalization at the intermediate state. The formula of EET rate in this limit was expressed by the convolution of the EET interaction and optical spectra. The interference effect strongly depends on the width of the absorption spectrum of mediator molecule and the energy gap between the donor and the mediator molecules.

  6. Cross sections for energy transfer in collisions between two excited sodium atoms

    International Nuclear Information System (INIS)

    Huennekens, J.; Gallagher, A.

    1983-01-01

    We have measured cross sections, sigma/sub n/L, for the excitation transfer process Na(3P)+Na(3P)→Na(3S)+Na(nL), where nL is the 4D or 5S level. Our results are sigma/sub 4D/ = 23 A 2 +- 35% and sigma/sub 5S/ = 16 A 2 +- 35% at Tapprox.600 K. To obtain these cross sections we have used pulsed excitation and measured the intensities of 4D, 5S, and 3P fluorescence emissions, and the spatial distribution of excited atoms resulting from radiation diffusion, as well as the excited atom density as a function of time. Additionally, we have accounted for (time-dependent) radiation trapping of 3P and nL level radiation and for the resulting anisotropies of these fluorescence emissions. Comparisons of our results with theory have been made, and their relevance to other experiments is discussed

  7. Energy transfer in LH2 of Rhodospirillum Molischianum, studied by subpicosecond spectroscopy and configuration interaction excition calculations.

    NARCIS (Netherlands)

    Ihalainen, J.A.; Linnanto, J.; Myllyperkiö, P.; van Stokkum, I.H.M.; Ücker, B.; Scheer, H.; Korppi-Tommola, J.E.I.

    2001-01-01

    Two color transient absorption measurements were performed on a LH2 complex from Rhodospirillum molischianum by using several excitation wavelengths (790, 800, 810, and 830 nm) and probing in the spectral region from 790 to 870 nm at room temperature. The observed energy transfer time of ∼1.0 ps

  8. Vibrational energy transfer in selectively excited diatomic molecules. [Relaxation rates, self-relaxation, upper limits

    Energy Technology Data Exchange (ETDEWEB)

    Dasch, C.J.

    1978-09-01

    Single rovibrational states of HCl(v=2), HBr(v=2), DCl(v=2), and CO(v=2) were excited with a pulsed optical parametric oscillator (OPO). Total vibrational relaxation rates near - resonance quenchers were measured at 295/sup 0/K using time resolved infrared fluorescence. These rates are attributed primarily to V - V energy transfer, and they generally conform to a simple energy gap law. A small deviation was found for the CO(v) + DCl(v') relaxation rates. Upper limits for the self relaxation by V - R,T of HCl(v=2) and HBr(v=2) and for the two quantum exchange between HCl and HBr were determined. The HF dimer was detected at 295/sup 0/K and 30 torr HF pressure with an optoacoustic spectrometer using the OPO. Pulsed and chopped, resonant and non-resonant spectrophones are analyzed in detail. From experiments and first order perturbation theory, these V - V exchange rates appear to behave as a first order perturbation in the vibrational coordinates. The rotational dynamics are known to be complicated however, and the coupled rotational - vibrational dynamics were investigated theoreticaly in infinite order by the Dillon and Stephenson and the first Magnus approximations. Large ..delta..J transitions appear to be important, but these calculations differ by orders of magnitude on specific rovibrational transition rates. Integration of the time dependent semiclassical equations by a modified Gordon method and a rotationally distorted wave approximation are discussed as methods which would treat the rotational motion more accurately. 225 references.

  9. Resonant electronic excitation energy transfer by Dexter mechanism in the quantum dot system

    Science.gov (United States)

    Samosvat, D. M.; Chikalova-Luzina, O. P.; Vyatkin, V. M.; Zegrya, G. G.

    2016-11-01

    In present work the energy transfer between quantum dots by the exchange (Dexter) mechanism is analysed. The interdot Coulomb interaction is taken into consideration. It is assumed that the quantum dot-donor and the quantum dot-acceptor are made from the same compound A3B5 and embedded in the matrix of other material creating potential barriers for electron and holes. The dependences of the energy transfer rate on the quantum-dot system parameters are found using the Kane model that provides the most adequate description spectra of semiconductors A3B5. Numerical calculations show that the rate of the energy transfer by Dexter mechanism is comparable to the rate of the energy transfer by electrostatic mechanism at the distances approaching to the contact ones.

  10. Resonant electronic excitation energy transfer by Dexter mechanism in the quantum dot system

    International Nuclear Information System (INIS)

    Samosvat, D M; Chikalova-Luzina, O P; Zegrya, G G; Vyatkin, V M

    2016-01-01

    In present work the energy transfer between quantum dots by the exchange (Dexter) mechanism is analysed. The interdot Coulomb interaction is taken into consideration. It is assumed that the quantum dot-donor and the quantum dot-acceptor are made from the same compound A3B5 and embedded in the matrix of other material creating potential barriers for electron and holes. The dependences of the energy transfer rate on the quantum-dot system parameters are found using the Kane model that provides the most adequate description spectra of semiconductors A3B5. Numerical calculations show that the rate of the energy transfer by Dexter mechanism is comparable to the rate of the energy transfer by electrostatic mechanism at the distances approaching to the contact ones. (paper)

  11. Two types of charge transfer excitations in low dimensional cuprates: an electron energy-loss study

    Czech Academy of Sciences Publication Activity Database

    Knupfer, M.; Fink, J.; Drechsler, S.-L.; Hayn, R.; Málek, Jiří; Moskvin, A.S.

    137-140, - (2004), s. 469-473 ISSN 0368-2048 Institutional research plan: CEZ:AV0Z1010914 Keywords : cuprates * electronic excitations * electron energy-loss spectroscopy Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 1.069, year: 2004

  12. Strategies to enhance the excitation energy-transfer efficiency in a light-harvesting system using the intra-molecular charge transfer character of carotenoids

    Energy Technology Data Exchange (ETDEWEB)

    Yukihira, Nao [Department of Applied Chemistry for Environment; School of Science and Technology; Kwansei Gakuin University; Sanda; Japan; Sugai, Yuko [Department of Applied Chemistry for Environment; School of Science and Technology; Kwansei Gakuin University; Sanda; Japan; Fujiwara, Masazumi [Department of Applied Chemistry for Environment; School of Science and Technology; Kwansei Gakuin University; Sanda; Japan; Kosumi, Daisuke [Institute of Pulsed Power Science; Kumamoto University; Kumamoto; Japan; Iha, Masahiko [South Product Co. Ltd.; Uruma-shi; Japan; Sakaguchi, Kazuhiko [Department of Chemistry; Graduate School of Science; Osaka City University; Osaka 558-8585; Japan; Katsumura, Shigeo [Department of Chemistry; Graduate School of Science; Osaka City University; Osaka 558-8585; Japan; Gardiner, Alastair T. [Glasgow Biomedical Research Centre; University of Glasgow; 126 University Place; Glasgow, G12 8QQ; UK; Cogdell, Richard J. [Glasgow Biomedical Research Centre; University of Glasgow; 126 University Place; Glasgow, G12 8QQ; UK; Hashimoto, Hideki [Department of Applied Chemistry for Environment; School of Science and Technology; Kwansei Gakuin University; Sanda; Japan

    2017-01-01

    Fucoxanthin is a carotenoid that is mainly found in light-harvesting complexes from brown algae and diatoms. Due to the presence of a carbonyl group attached to polyene chains in polar environments, excitation produces an excited intra-molecular charge transfer. This intra-molecular charge transfer state plays a key role in the highly efficient (~95%) energy-transfer from fucoxanthin to chlorophyllain the light-harvesting complexes from brown algae. In purple bacterial light-harvesting systems the efficiency of excitation energy-transfer from carotenoids to bacteriochlorophylls depends on the extent of conjugation of the carotenoids. In this study we were successful, for the first time, in incorporating fucoxanthin into a light-harvesting complex 1 from the purple photosynthetic bacterium,Rhodospirillum rubrumG9+ (a carotenoidless strain). Femtosecond pump-probe spectroscopy was applied to this reconstituted light-harvesting complex in order to determine the efficiency of excitation energy-transfer from fucoxanthin to bacteriochlorophyllawhen they are bound to the light-harvesting 1 apo-proteins.

  13. Time-resolved UV-excited microarray reader for fluorescence energy transfer (FRET) measurements

    Science.gov (United States)

    Orellana, Adelina; Hokkanen, Ari P.; Pastinen, Tomi; Takkinen, Kristina; Soderlund, Hans

    2001-05-01

    Analytical systems based on immunochemistry are largely used in medical diagnostics and in biotechnology. There is a significant pressure to develop the present assay formats to become easier to use, faster, and less reagent consuming. Further developments towards high density array--like multianalyte measurement systems would be valuable. To this aim we have studied the applicability of fluorescence resonance energy transfer and time-resolved fluorescence resonance energy transfer in immunoassays on microspots and in microwells. We have used engineered recombinant antibodies detecting the pentameric protein CRP as a model analyte system, and tested different assay formats. We describe also the construction of a time-resolved scanning epifluorometer with which we could measure the FRET interaction between the slow fluorescence decay from europium chelates and its energy transfer to the rapidly decaying fluorophore Cy5.

  14. On isospin excitation energy

    International Nuclear Information System (INIS)

    Li Wenfei; Zhang Fengshou; Chen Liewen

    2001-01-01

    Within the framework of Hartree-Fock theory using the extended Skyrme effective interaction, the isospin excitation energy as a function of relative neutron excess δ was investigated at different temperatures and densities. It was found that the isospin excitation energy decreased with the increment of temperature and/or the decrement of density. The authors pointed out that the decrement of isospin excitation energy was resulted from the weakening of quantum effect with increment of temperature and/or decrement of density. Meanwhile, the relationship between the isospin excitation energy and the symmetry energy was discussed and found that the symmetry energy was just a part of the isospin excitation energy. With increasing temperature and decreasing density, the contribution of the symmetry energy to the isospin excitation energy becomes more and more important. The isospin excitation energy as a function of relative neutron excess was also investigated using different potential parameters. The results shows that the isospin excitation energy is almost independent of the incompressibility and the effective mass, but strongly depends on the symmetry energy strength coefficient, which indicates that it is possible to extract the symmetry energy of the nuclear equation of state by investigating the isospin excitation energy in experiments

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

    Science.gov (United States)

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

    2018-04-01

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

  16. Excited baryon form-factors at high momentum transfer at CEBAF at higher energies

    Energy Technology Data Exchange (ETDEWEB)

    Stoler, P. [Rensselaer Polytechnic Inst., Troy, NY (United States)

    1994-04-01

    The possibilities of measuring the properties of excited nucleons at high Q{sup 2} by means of exclusive single meson production at CEBAF with an electron energy of 8 GeV is considered. The motivation is to access short range phenomena in baryon structure, and to investigate the transition from the low Q{sup 2} non-perturbative QCD regime, where constituent quark models are valid, to higher Q{sup 2} where it is believed perturbative QCD plays an increasingly important role. It is found that high quality baryon decay angular distributions can be obtained for the most prominent states up to Q{sup 2} {approximately} 12 GeV{sup 2}/c{sup 2} using a set of moderate resolution, large solid angle magnetic spectrometers.

  17. Dipole-Dipole Electron Excitation Energy Transfer in the System CdSe/ZnS Quantum Dot - Eosin in Butyral Resin Matrix

    Science.gov (United States)

    Myslitskaya, N. A.; Samusev, I. G.; Bryukhanov, V. V.

    2014-11-01

    The electron excitation energy transfer from CdSe/ZnS quantum dots to eosin molecules in the polymer matrix of butyral resin is investigated. The main characteristics of energy transfer are determined. By means of luminescence microscopy and correlation spectroscopy methods we found that quantum dots in the polymer are in an aggregate state.

  18. Excitation energy transfer in ruthenium (II)-porphyrin conjugates led to enhanced emission quantum yield and 1O2 generation

    International Nuclear Information System (INIS)

    Pan, Jie; Jiang, Lijun; Chan, Chi-Fai; Tsoi, Tik-Hung; Shiu, Kwok-Keung; Kwong, Daniel W.J.; Wong, Wing-Tak; Wong, Wai-Kwok; Wong, Ka-Leung

    2017-01-01

    Porphyrins are good photodynamic therapy (PDT) agents due to its flexibility for modifications to achieve tumor localization and photo-cytotoxicity against cancer. Yet they are not perfect. In a Ru(polypyridyl)-porphyrin system, the Ru(polypyridyl) moiety improves the water solubility and cell permeability. Consider the similar excited state energies between Ru(polypyridyl) and porphyrin moieties; a small perturbation (e.g. Zn(II) metalation) would lead to a marked change in the energy migration process. In this work, we have synthesized a series of porphyrins conjugated with Ru(polypyridyl) complexes using different linkers and investigated their photophysical properties, which included singlet oxygen quantum yield and their in vitro biological properties, resulting from linker variation and porphyrin modification by Zn(II) metalation. - Graphical abstract: Four amphiphilic ruthenium(II)-porphyrin complexes were prepared that display energy transfer conversion with zinc coordination, lysosome specific target, low dark toxicity and efficient photodynamic therapy.

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

    International Nuclear Information System (INIS)

    Samanta, R; Purkait, M

    2012-01-01

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

  20. High energy nuclear excitations

    International Nuclear Information System (INIS)

    Gogny, D.; Decharge, J.

    1983-09-01

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

  1. Hardness and excitation energy

    Indian Academy of Sciences (India)

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

  2. Spectroscopy of nitrophenolates in vacuo: effect of spacer, configuration, and microsolvation on the charge-transfer excitation energy.

    Science.gov (United States)

    Brøndsted Nielsen, Steen; Brøndsted Nielsen, Mogens; Rubio, Angel

    2014-04-15

    In a charge-transfer (CT) transition, electron density moves from one end of the molecule (donor) to the other end (acceptor). This type of transition is of paramount importance in nature, for example, in photosynthesis, and it governs the excitation of several protein biochromophores and luminophores such as the oxyluciferin anion that accounts for light emission from fireflies. Both transition energy and oscillator strength are linked to the coupling between the donor and acceptor groups: The weaker the coupling, the smaller the excitation energy. But a weak coupling necessarily also causes a low oscillator strength possibly preventing direct excitation (basically zero probability in the noncoupling case). The coupling is determined by the actual spacer between the two groups, and whether the spacer acts as an insulator or a conductor. However, it can be difficult or even impossible to distinguish the effect of the spacer from that of local solvent molecules that often cause large solvent shifts due to different ground-state and excited-state stabilization. This calls for gas-phase spectroscopy experiments where absorption by the isolated molecule is identified to unequivocally establish the intrinsic molecular properties with no perturbations from a microenvironment. From such insight, the effect of a protein microenvironment on the CT excited state can be deduced. In this Account, we review our results over the last 5 years from mass spectroscopy experiments using specially designed apparatus on several charged donor-acceptor ions that are based on the nitrophenolate moiety and π-extended derivatives, which are textbook examples of donor-acceptor chromophores. The phenolate oxygen is the donor, and the nitro group is the acceptor. The choice of this system is also based on the fact that phenolate is a common structural motif of biochromophores and luminophores, for example, it is a constituent of the oxyluciferin anion. A presentation of the setups used for

  3. Oxygen auroral transition laser system excited by collisional and photolytic energy transfer

    International Nuclear Information System (INIS)

    Murray, J.R.; Powell, H.T.; Rhodes, C.K.

    1975-06-01

    The properties of laser media involving the auroral transition of atomic oxygen and analogous systems are examined. A discussion of the atomic properties, collisional mechanisms, excitation processes, and collisionally induced radiative phenomena is given. Crossing phenomena play a particularly important role in governing the dynamics of the medium

  4. Excitation energy transfer in molecular complexes: transport processes, optical properties and effects of nearby placed metal nano-particles

    Science.gov (United States)

    May, Volkhard; Megow, Jörg; Zelinskyi, Iaroslav

    2012-04-01

    Excitation energy transfer (EET) in molecular systems is studied theoretically. Chromophore complexes are considered which are formed by a butanediamine dendrimer with four pheophorbide-a molecules. To achieve a description with an atomic resolution and to account for the effect of an ethanol solvent a mixed quantum classical methodology is utilized. Details of the EET and spectra of transient anisotropy showing signatures of EET are presented. A particular control of intermolecular EET is achieved by surface plasmons of nearby placed metal nanoparticles (MNP). To attain a quantum description of the molecule-MNP system a microscopic theory is introduced. As a particular application surface plasmon affected absorption spectra of molecular complexes placed in the proximity of a spherical MNP are discussed.

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

    Science.gov (United States)

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

    2015-07-09

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

  6. High Excitation Transfer Efficiency from Energy Relay Dyes in Dye-Sensitized Solar Cells

    KAUST Repository

    Hardin, Brian E.; Yum, Jun-Ho; Hoke, Eric T.; Jun, Young Chul; Péchy, Peter; Torres, Tomás; Brongersma, Mark L.; Nazeeruddin, Md. Khaja; Grätzel, Michael; McGehee, Michael D.

    2010-01-01

    The energy relay dye, 4-(Dicyanomethylene)-2-methyl-6-(4- dimethylaminostyryl)-4H-pyran (DCM), was used with a near-infrared sensitizing dye, TT1, to increase the overall power conversion efficiency of a dye-sensitized solar cell (DSC) from 3

  7. Behavior of Poisson Bracket Mapping Equation in Studying Excitation Energy Transfer Dynamics of Cryptophyte Phycocyanin 645 Complex

    International Nuclear Information System (INIS)

    Lee, Weon Gyu; Kelly, Aaron; Rhee, Young Min

    2012-01-01

    Recently, it has been shown that quantum coherence appears in energy transfers of various photosynthetic light harvesting complexes at from cryogenic to even room temperatures. Because the photosynthetic systems are inherently complex, these findings have subsequently interested many researchers in the field of both experiment and theory. From the theoretical part, simplified dynamics or semiclassical approaches have been widely used. In these approaches, the quantum-classical Liouville equation (QCLE) is the fundamental starting point. Toward the semiclassical scheme, approximations are needed to simplify the equations of motion of various degrees of freedom. Here, we have adopted the Poisson bracket mapping equation (PBME) as an approximate form of QCLE and applied it to find the time evolution of the excitation in a photosynthetic complex from marine algae. The benefit of using PBME is its similarity to conventional Hamiltonian dynamics. Through this, we confirmed the coherent population transfer behaviors in short time domain as previously reported with a more accurate but more time-consuming iterative linearized density matrix approach. However, we find that the site populations do not behave according to the Boltzmann law in the long time limit. We also test the effect of adding spurious high frequency vibrations to the spectral density of the bath, and find that their existence does not alter the dynamics to any significant extent as long as the associated reorganization energy is changed not too drastically. This suggests that adopting classical trajectory based ensembles in semiclassical simulations should not influence the coherence dynamics in any practical manner, even though the classical trajectories often yield spurious high frequency vibrational features in the spectral density

  8. Energy transfer properties and mechanisms

    International Nuclear Information System (INIS)

    1991-01-01

    This report discusses the energy transfer mechanisms in azulene, benzene, toluene, and isotopomers. Also discussed is the coupled energy reservoirs model, quantum effects in energy transfer, NO 2 energy transfer, densities of states, the reactant states model, and O 3 excited electronic states

  9. Excitation energy transfer in natural photosynthetic complexes and chlorophyll trefoils: hole-burning and single complex/trefoil spectroscopic studies

    Energy Technology Data Exchange (ETDEWEB)

    Ryszard Jankowiak, Kansas State University, Department of Chemistry, CBC Bldg., Manhattan KS, 66505; Phone: (785) 532-6785

    2012-09-12

    In this project we studied both natural photosynthetic antenna complexes and various artificial systems (e.g. chlorophyll (Chl) trefoils) using high resolution hole-burning (HB) spectroscopy and excitonic calculations. Results obtained provided more insight into the electronic (excitonic) structure, inhomogeneity, electron-phonon coupling strength, vibrational frequencies, and excitation energy (or electron) transfer (EET) processes in several antennas and reaction centers. For example, our recent work provided important constraints and parameters for more advanced excitonic calculations of CP43, CP47, and PSII core complexes. Improved theoretical description of HB spectra for various model systems offers new insight into the excitonic structure and composition of low-energy absorption traps in very several antenna protein complexes and reaction centers. We anticipate that better understanding of HB spectra obtained for various photosynthetic complexes and their simultaneous fits with other optical spectra (i.e. absorption, emission, and circular dichroism spectra) provides more insight into the underlying electronic structures of these important biological systems. Our recent progress provides a necessary framework for probing the electronic structure of these systems via Hole Burning Spectroscopy. For example, we have shown that the theoretical description of non-resonant holes is more restrictive (in terms of possible site energies) than those of absorption and emission spectra. We have demonstrated that simultaneous description of linear optical spectra along with HB spectra provides more realistic site energies. We have also developed new algorithms to describe both nonresonant and resonant hole-burn spectra using more advanced Redfield theory. Simultaneous description of various optical spectra for complex biological system, e.g. artificial antenna systems, FMO protein complexes, water soluble protein complexes, and various mutants of reaction centers

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

    Science.gov (United States)

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

    2017-04-01

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

  11. A novel construction of complex-valued Gaussian processes with arbitrary spectral densities and its application to excitation energy transfer.

    Science.gov (United States)

    Chen, Xin; Cao, Jianshu; Silbey, Robert J

    2013-06-14

    The recent experimental discoveries about excitation energy transfer (EET) in light harvesting antenna (LHA) attract a lot of interest. As an open non-equilibrium quantum system, the EET demands more rigorous theoretical framework to understand the interaction between system and environment and therein the evolution of reduced density matrix. A phonon is often used to model the fluctuating environment and convolutes the reduced quantum system temporarily. In this paper, we propose a novel way to construct complex-valued Gaussian processes to describe thermal quantum phonon bath exactly by converting the convolution of influence functional into the time correlation of complex Gaussian random field. Based on the construction, we propose a rigorous and efficient computational method, the covariance decomposition and conditional propagation scheme, to simulate the temporarily entangled reduced system. The new method allows us to study the non-Markovian effect without perturbation under the influence of different spectral densities of the linear system-phonon coupling coefficients. Its application in the study of EET in the Fenna-Matthews-Olson model Hamiltonian under four different spectral densities is discussed. Since the scaling of our algorithm is linear due to its Monte Carlo nature, the future application of the method for large LHA systems is attractive. In addition, this method can be used to study the effect of correlated initial condition on the reduced dynamics in the future.

  12. Processes of the excitation energy migration and transfer in Ce3+-doped alkali gadolinium phosphates studied with time-resolved photoluminescence spectroscopy technique

    International Nuclear Information System (INIS)

    Stryganyuk, G.; Shalapska, T.; Voloshinovskii, A.; Gektin, A.; Krasnikov, A.; Zazubovich, S.

    2011-01-01

    Spectral-kinetic characteristics of Gd 3+ and Ce 3+ luminescence from a series of Ce 3+ -doped alkali gadolinium phosphates of MGdP 4 O 12 type (M=Li, Na, Cs) have been studied within 4.2-300 K temperature range using time-resolved luminescence spectroscopy techniques. The processes of energy migration along the Gd 3+ sub-lattice and energy transfer between the Gd 3+ and Ce 3+ ions have been investigated. Peculiarities of these processes have been compared for MGdP 4 O 12 phosphate hosts with different alkali metal ions. A contribution of different levels from the 6 P j multiplet of the lowest Gd 3+ excited state into the energy migration and transfer processes has been clarified. The phonon-assisted occupation of high-energy 6 P 5/2,3/2 levels by Gd 3+ in the excited 6 P j state has been revealed as a shift of Gd 3+6 P j → 8 S 7/2 emission into the short-wavelength spectral range upon the temperature increase. The relaxation of excited Gd 3+ via phonon-assisted population of Gd 3+6 P 5/2 level (next higher one to the lowest excited 6 P 7/2 ) is supposed to be responsible for the rise in probability of energy migration within the Gd 3+ sub-lattice initiating the Gd 3+ →Ce 3+ energy transfer at T 3+ →Ce 3+ energy transfer at T>150 K is explained by the increase in probability of Gd 3+ relaxation into the highest 6 P 3/2 level of the 6 P j multiplet. An efficient reversed Ce 3+ →Gd 3+ energy transfer has been revealed for the studied phosphates at 4.2 K. - Highlights: →We investigate the Gd 3+ -Ce 3+ energy transfer in alkali gadolinium phosphates. → Thermal population of Gd 3+6 P 5/2 level improves migration along the Gd sub-lattice. → Increasing overlap of Gd 3+ and Ce 3+ states enhances the Gd 3+ -Ce 3+ energy transfer. → In LiGdP 4 O 12 :Ce and NaGdP 4 O 12 :Ce an efficient Ce 3+ -Gd 3+ transfer occurs at 4-300 K. → An effective reverse Gd 3+ -Ce 3+ energy transfer becomes possible at T>150 K.

  13. An accurate full-dimensional potential energy surface for H-Au(111): Importance of nonadiabatic electronic excitation in energy transfer and adsorption.

    Science.gov (United States)

    Janke, Svenja M; Auerbach, Daniel J; Wodtke, Alec M; Kandratsenka, Alexander

    2015-09-28

    We have constructed a potential energy surface (PES) for H-atoms interacting with fcc Au(111) based on fitting the analytic form of the energy from Effective Medium Theory (EMT) to ab initio energy values calculated with density functional theory. The fit used input from configurations of the H-Au system with Au atoms at their lattice positions as well as configurations with the Au atoms displaced from their lattice positions. It reproduces the energy, in full dimension, not only for the configurations used as input but also for a large number of additional configurations derived from ab initio molecular dynamics (AIMD) trajectories at finite temperature. Adiabatic molecular dynamics simulations on this PES reproduce the energy loss behavior of AIMD. EMT also provides expressions for the embedding electron density, which enabled us to develop a self-consistent approach to simulate nonadiabatic electron-hole pair excitation and their effect on the motion of the incident H-atoms. For H atoms with an energy of 2.7 eV colliding with Au, electron-hole pair excitation is by far the most important energy loss pathway, giving an average energy loss ≈3 times that of the adiabatic case. This increased energy loss enhances the probability of the H-atom remaining on or in the Au slab by a factor of 2. The most likely outcome for H-atoms that are not scattered also depends prodigiously on the energy transfer mechanism; for the nonadiabatic case, more than 50% of the H-atoms which do not scatter are adsorbed on the surface, while for the adiabatic case more than 50% pass entirely through the 4 layer simulation slab.

  14. Excited state Intramolecular Proton Transfer in Anthralin

    DEFF Research Database (Denmark)

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

    1998-01-01

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

  15. Excitation energy transfer from the bacteriochlorophyll Soret band to carotenoids in the LH2 light-harvesting complex from Ectothiorhodospira haloalkaliphila is negligible.

    Science.gov (United States)

    Razjivin, A P; Lukashev, E P; Kompanets, V O; Kozlovsky, V S; Ashikhmin, A A; Chekalin, S V; Moskalenko, A A; Paschenko, V Z

    2017-09-01

    Pathways of intramolecular conversion and intermolecular electronic excitation energy transfer (EET) in the photosynthetic apparatus of purple bacteria remain subject to debate. Here we experimentally tested the possibility of EET from the bacteriochlorophyll (BChl) Soret band to the singlet S 2 level of carotenoids using femtosecond pump-probe measurements and steady-state fluorescence excitation and absorption measurements in the near-ultraviolet and visible spectral ranges. The efficiency of EET from the Soret band of BChl to S 2 of the carotenoids in light-harvesting complex LH2 from the purple bacterium Ectothiorhodospira haloalkaliphila appeared not to exceed a few percent.

  16. Excitation decay due to incoherent energy transfer : A comparative study by means of an exact density expansion

    NARCIS (Netherlands)

    Knoester, J.; Himbergen, J.E. Van

    1984-01-01

    In this paper we consider a system of identical, randomly distributed donors, between which incoherent energy transfer takes place, described by coupled rate equations. It is proved, that the well-known diagrammatic series expansion of Gochanour, Andersen, and Fayer for the self-energy, while not an

  17. Cold transfer between deformed, Coulomb excited nuclei

    International Nuclear Information System (INIS)

    Bauer, H.

    1998-01-01

    The scattering system 162 Dy → 116 Sn has been examined at energies in the vicinity of the Coulomb barrier using the Heidelberg-Darmstadt Crystal Ball spectrometer combined with 5 Germanium-CLUSTER detectors. In order to study pairing correlations as a function of angular momentum cold events were selected in the 2n stripping channel by identifying and suppressing the dominant hot part of the transfer with the Crystal Ball. The CLUSTER detectors with their high γ-efficiency were used to identify the transfer channel and to resolve individual final states. Cross sections for the population of individual yrast states in a cold transfer reaction have been measured for the first time indicating the strong influence of higher transfer multipolarities. At small surface distances Coulomb-nuclear interferences were found to be responsible for the stronger decline of the population of higher yrast states in the transfer channel as compared to the Coulex channel. As a preparatory study for 2n transfer measurements between high spin yrast states in the backbending region of deformed nuclei the Coulomb excitation process in the crossing region of two bands in 162 Dy has been analyzed. The gross properties of the measured population probabilities could be interpreted in a simple band mixing model. (orig.)

  18. An accurate and linear-scaling method for calculating charge-transfer excitation energies and diabatic couplings

    Energy Technology Data Exchange (ETDEWEB)

    Pavanello, Michele [Department of Chemistry, Rutgers University, Newark, New Jersey 07102-1811 (United States); Van Voorhis, Troy [Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139-4307 (United States); Visscher, Lucas [Amsterdam Center for Multiscale Modeling, VU University, De Boelelaan 1083, 1081 HV Amsterdam (Netherlands); Neugebauer, Johannes [Theoretische Organische Chemie, Organisch-Chemisches Institut der Westfaelischen Wilhelms-Universitaet Muenster, Corrensstrasse 40, 48149 Muenster (Germany)

    2013-02-07

    Quantum-mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those charge transfer excitations that take place between non-covalently bound molecules. In particular, we present a method that scales linearly with the number of non-covalently bound molecules in the system and is based on a two-pronged approach: The molecular electronic structure of broken-symmetry charge-localized states is obtained with the frozen density embedding formulation of subsystem density-functional theory; subsequently, in a post-SCF calculation, the full-electron Hamiltonian and overlap matrix elements among the charge-localized states are evaluated with an algorithm which takes full advantage of the subsystem DFT density partitioning technique. The method is benchmarked against coupled-cluster calculations and achieves chemical accuracy for the systems considered for intermolecular separations ranging from hydrogen-bond distances to tens of Angstroms. Numerical examples are provided for molecular clusters comprised of up to 56 non-covalently bound molecules.

  19. High energy magnetic excitations

    International Nuclear Information System (INIS)

    Endoh, Yasuo

    1988-01-01

    The report emphasizes that the current development in condensed matter physics opens a research field fit to inelastic neutron scattering experiments in the eV range which is easilly accessed by spallation neutron sources. Several important subjects adopted at thermal reactors are shown. It is desired to extend the implementation of the spectroscopic experiments for investigation of higher energy magnetic excitations. For La 2 CuO 4 , which is the mother crystal of the first high Tc materials found by Bednortz and Muller, it seems to be believed that the magnetism is well characterized by the two-dimensional Heisenberg antiferromagnetic Hamiltonian, and it is widely accepted that the magnetism is a most probable progenitor of high Tc superconductors. The unusual properties of spin correlations in this crystal have been studied extensively by standard neutron scattering techniques with steady neutrons at BNL. FeSi is not ordered magnetically but shows a very unique feature of temperature induced magnetism, which also has been studied extensively by using the thermal neutron scattering technique at BNL. In these experiments, polarized neutrons are indispensable to extract the clean magnetic components out of other components of non-magnetic scattering. (N.K.)

  20. Laser induced energy transfer

    International Nuclear Information System (INIS)

    Falcone, R.W.

    1979-01-01

    Two related methods of rapidly transferring stored energy from one excited chemical species to another are described. The first of these, called a laser induced collision, involves a reaction in which the energy balance is met by photons from an intense laser beam. A collision cross section of ca 10 - 17 cm 2 was induced in an experiment which demonstrated the predicted dependence of the cross section on wavelength and power density of the applied laser. A second type of laser induced energy transfer involves the inelastic scattering of laser radiation from energetically excited atoms, and subsequent absorption of the scattered light by a second species. The technique of producing the light, ''anti-Stokes Raman'' scattering of visible and infrared wavelength laser photons, is shown to be an efficient source of narrow bandwidth, high brightness, tunable radiation at vacuum ultraviolet wavelengths by using it to excite a rare gas transition at 583.7 A. In addition, this light source was used to make the first measurement of the isotopic shift of the helium metastable level at 601 A. Applications in laser controlled chemistry and spectroscopy, and proposals for new types of lasers using these two energy transfer methods are discussed

  1. An efficient method to calculate excitation energy transfer in light-harvesting systems: application to the Fenna-Matthews-Olson complex

    International Nuclear Information System (INIS)

    Ritschel, Gerhard; Roden, Jan; Eisfeld, Alexander; Strunz, Walter T

    2011-01-01

    A master equation derived from non-Markovian quantum state diffusion is used to calculate the excitation energy transfer in the photosynthetic Fenna-Matthews-Olson pigment-protein complex at various temperatures. This approach allows us to treat spectral densities that explicitly contain the coupling to internal vibrational modes of the chromophores. Moreover, the method is very efficient and as a result the transfer dynamics can be calculated within about 1 min on a standard PC, making systematic investigations w.r.t. parameter variations tractable. After demonstrating that our approach is able to reproduce the results of the numerically exact hierarchical equations of motion approach, we show how the inclusion of vibrational modes influences the transfer. (paper)

  2. Resonance Raman and excitation energy dependent charge transfer mechanism in halide-substituted hybrid perovskite solar cells.

    Science.gov (United States)

    Park, Byung-wook; Jain, Sagar M; Zhang, Xiaoliang; Hagfeldt, Anders; Boschloo, Gerrit; Edvinsson, Tomas

    2015-02-24

    Organo-metal halide perovskites (OMHPs) are materials with attractive properties for optoelectronics. They made a recent introduction in the photovoltaics world by methylammonium (MA) lead triiodide and show remarkably improved charge separation capabilities when chloride and bromide are added. Here we show how halide substitution in OMHPs with the nominal composition CH3NH3PbI2X, where X is I, Br, or Cl, influences the morphology, charge quantum yield, and local interaction with the organic MA cation. X-ray diffraction and photoluminescence data demonstrate that halide substitution affects the local structure in the OMHPs with separate MAPbI3 and MAPbCl3 phases. Raman spectroscopies as well as theoretical vibration calculations reveal that this at the same time delocalizes the charge to the MA cation, which can liberate the vibrational movement of the MA cation, leading to a more adaptive organic phase. The resonance Raman effect together with quantum chemical calculations is utilized to analyze the change in charge transfer mechanism upon electronic excitation and gives important clues for the mechanism of the much improved photovoltage and photocurrent also seen in the solar cell performance for the materials when chloride compounds are included in the preparation.

  3. Excitation energy transfer in ruthenium (II)-porphyrin conjugates led to enhanced emission quantum yield and {sup 1}O{sub 2} generation

    Energy Technology Data Exchange (ETDEWEB)

    Pan, Jie; Jiang, Lijun; Chan, Chi-Fai [Department of Chemistry, Hong Kong Baptist University, Kowloon Tong, Hong Kong Special Administrative Region (Hong Kong); Tsoi, Tik-Hung [Department of Applied Biology and Chemical Technology, Hung Hom, Hong Kong Special Administrative Region (Hong Kong); Shiu, Kwok-Keung; Kwong, Daniel W.J. [Department of Chemistry, Hong Kong Baptist University, Kowloon Tong, Hong Kong Special Administrative Region (Hong Kong); Wong, Wing-Tak [Department of Applied Biology and Chemical Technology, Hung Hom, Hong Kong Special Administrative Region (Hong Kong); Wong, Wai-Kwok, E-mail: wkwong@hkbu.edu.hk [Department of Chemistry, Hong Kong Baptist University, Kowloon Tong, Hong Kong Special Administrative Region (Hong Kong); Wong, Ka-Leung, E-mail: klwong@hkbu.edu.hk [Department of Chemistry, Hong Kong Baptist University, Kowloon Tong, Hong Kong Special Administrative Region (Hong Kong)

    2017-04-15

    Porphyrins are good photodynamic therapy (PDT) agents due to its flexibility for modifications to achieve tumor localization and photo-cytotoxicity against cancer. Yet they are not perfect. In a Ru(polypyridyl)-porphyrin system, the Ru(polypyridyl) moiety improves the water solubility and cell permeability. Consider the similar excited state energies between Ru(polypyridyl) and porphyrin moieties; a small perturbation (e.g. Zn(II) metalation) would lead to a marked change in the energy migration process. In this work, we have synthesized a series of porphyrins conjugated with Ru(polypyridyl) complexes using different linkers and investigated their photophysical properties, which included singlet oxygen quantum yield and their in vitro biological properties, resulting from linker variation and porphyrin modification by Zn(II) metalation. - Graphical abstract: Four amphiphilic ruthenium(II)-porphyrin complexes were prepared that display energy transfer conversion with zinc coordination, lysosome specific target, low dark toxicity and efficient photodynamic therapy.

  4. Collisional energy transfer between highly excited vibrational levels of K2 (11Σu+, V=46∼61) and H2

    International Nuclear Information System (INIS)

    Zhang Liping; Cai Qin; Luan Nannan; Dai Kang; Shen Yifan

    2011-01-01

    Using the CARS (Coherent Anti-stokes Raman Spectroscopy) detection technique, the electronic-to-rovibrational levels energy transfer between electronically excited K 2 (which is in the state of 1 1 ∑ u + , V=46∼61) and H 2 has been investigated. The scanned CARS spectra reveals that H 2 molecules are produced only at the V=1, J=2 and V=2, J=0, 1, 2 rovibrational levels during energy transfer processes. From scanned CARS spectral peaks the population ratios are obtained. The n 1 /n 4 9 n 2 /n 4 , and n 3 /n 4 are 3.3±0.5, 2.2±0.3 and 2.0±0.3, respectively, where n 1 , n 2 , n 3 and n 4 represent the number densities of H 2 at rovibrational levels (2, 0), (2, 1), (2, 2) and (1, 2), respectively. The population ratios indicate that the H 2 molecules produced by the energy transfer process are 88% populated at the V=2 level and 12% at V=1. The relative fractions (, , ) of average energy disposal are derived as (0.53, 0.01, 0.46), having major vibrational and translational energy release. Through simple kinetic model at the experimental conditions of T=573 K and P(H 2 ) =5 X 10 3 Pa, collisional transfer rate coefficients k 12 =(3.3±0.7) X 10 -14 and k 2 =(1.4±0.3) X 10 -14 cm 3 s -1 have been obtained. (authors)

  5. [Electron transfer, ionization and excitation in atomic collisions

    International Nuclear Information System (INIS)

    1991-01-01

    The research being carried out at Penn State by Winter and Alston addresses the fundamental atomic-collision processes of electron transfer, ionization, and excitation. Winter has focussed attention on intermediate and, more recently, higher collision energies -- proton energies of at least about 50 keV -- for which coupled-state approaches are appropriate. Alston has concentrated on perturbative approaches to symmetric ion-ion/atom collisions at high energies and to asymmetric collisions at intermediate to high energies

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

    International Nuclear Information System (INIS)

    Theophilou, Iris; Tassi, M.; Thanos, S.

    2014-01-01

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

  7. Transfer of energy in an atom

    International Nuclear Information System (INIS)

    Chemin, J.F.

    2001-01-01

    In most cases the nucleus does not interact with the electron cloud because its energy range is far higher, but in some rare cases electrons from the electron cloud and the nucleus may exchange energy: an electron may de-excite by transferring a part of its energy to the nucleus that becomes itself excited (nuclear excitation by electronic transfer or NEET), conversely electrons can receive energy from the nucleus (bound internal conversion or BIC). For the first time both energy transfers have been observed: a BIC process on a tellurium-125 atom by a French team and a NEET process on a gold-197 atom by a Japanese team. (A.C.)

  8. Mean excitation energies for molecular ions

    Energy Technology Data Exchange (ETDEWEB)

    Jensen, Phillip W.K.; Sauer, Stephan P.A. [Department of Chemistry, University of Copenhagen, Copenhagen (Denmark); Oddershede, Jens [Department of Physics, Chemistry, and Pharmacy, University of Southern Denmark, Odense (Denmark); Quantum Theory Project, Departments of Physics and Chemistry, University of Florida, Gainesville, FL (United States); Sabin, John R., E-mail: sabin@qtp.ufl.edu [Department of Physics, Chemistry, and Pharmacy, University of Southern Denmark, Odense (Denmark); Quantum Theory Project, Departments of Physics and Chemistry, University of Florida, Gainesville, FL (United States)

    2017-03-01

    The essential material constant that determines the bulk of the stopping power of high energy projectiles, the mean excitation energy, is calculated for a range of smaller molecular ions using the RPA method. It is demonstrated that the mean excitation energy of both molecules and atoms increase with ionic charge. However, while the mean excitation energies of atoms also increase with atomic number, the opposite is the case for mean excitation energies for molecules and molecular ions. The origin of these effects is explained by considering the spectral representation of the excited state contributing to the mean excitation energy.

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

    Science.gov (United States)

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

    2011-01-01

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

  10. Energy transfer upon collision of selectively excited CO{sub 2} molecules: State-to-state cross sections and probabilities for modeling of atmospheres and gaseous flows

    Energy Technology Data Exchange (ETDEWEB)

    Lombardi, A., E-mail: ebiu2005@gmail.com; Faginas-Lago, N.; Pacifici, L.; Grossi, G. [Dipartimento di Chimica, Università di Perugia, via Elce di Sotto 8, 06123 Perugia (Italy)

    2015-07-21

    Carbon dioxide molecules can store and release tens of kcal/mol upon collisions, and such an energy transfer strongly influences the energy disposal and the chemical processes in gases under the extreme conditions typical of plasmas and hypersonic flows. Moreover, the energy transfer involving CO{sub 2} characterizes the global dynamics of the Earth-atmosphere system and the energy balance of other planetary atmospheres. Contemporary developments in kinetic modeling of gaseous mixtures are connected to progress in the description of the energy transfer, and, in particular, the attempts to include non-equilibrium effects require to consider state-specific energy exchanges. A systematic study of the state-to-state vibrational energy transfer in CO{sub 2} + CO{sub 2} collisions is the focus of the present work, aided by a theoretical and computational tool based on quasiclassical trajectory simulations and an accurate full-dimension model of the intermolecular interactions. In this model, the accuracy of the description of the intermolecular forces (that determine the probability of energy transfer in molecular collisions) is enhanced by explicit account of the specific effects of the distortion of the CO{sub 2} structure due to vibrations. Results show that these effects are important for the energy transfer probabilities. Moreover, the role of rotational and vibrational degrees of freedom is found to be dominant in the energy exchange, while the average contribution of translations, under the temperature and energy conditions considered, is negligible. Remarkable is the fact that the intramolecular energy transfer only involves stretching and bending, unless one of the colliding molecules has an initial symmetric stretching quantum number greater than a threshold value estimated to be equal to 7.

  11. Energy transfer upon collision of selectively excited CO2 molecules: State-to-state cross sections and probabilities for modeling of atmospheres and gaseous flows.

    Science.gov (United States)

    Lombardi, A; Faginas-Lago, N; Pacifici, L; Grossi, G

    2015-07-21

    Carbon dioxide molecules can store and release tens of kcal/mol upon collisions, and such an energy transfer strongly influences the energy disposal and the chemical processes in gases under the extreme conditions typical of plasmas and hypersonic flows. Moreover, the energy transfer involving CO2 characterizes the global dynamics of the Earth-atmosphere system and the energy balance of other planetary atmospheres. Contemporary developments in kinetic modeling of gaseous mixtures are connected to progress in the description of the energy transfer, and, in particular, the attempts to include non-equilibrium effects require to consider state-specific energy exchanges. A systematic study of the state-to-state vibrational energy transfer in CO2 + CO2 collisions is the focus of the present work, aided by a theoretical and computational tool based on quasiclassical trajectory simulations and an accurate full-dimension model of the intermolecular interactions. In this model, the accuracy of the description of the intermolecular forces (that determine the probability of energy transfer in molecular collisions) is enhanced by explicit account of the specific effects of the distortion of the CO2 structure due to vibrations. Results show that these effects are important for the energy transfer probabilities. Moreover, the role of rotational and vibrational degrees of freedom is found to be dominant in the energy exchange, while the average contribution of translations, under the temperature and energy conditions considered, is negligible. Remarkable is the fact that the intramolecular energy transfer only involves stretching and bending, unless one of the colliding molecules has an initial symmetric stretching quantum number greater than a threshold value estimated to be equal to 7.

  12. Spectroscopic probes of vibrationally excited molecules at chemically significant energies

    Energy Technology Data Exchange (ETDEWEB)

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

    1993-12-01

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

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

    International Nuclear Information System (INIS)

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

    1979-01-01

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

  14. Extracting the cross section angular distributions for 15C high-energy resonance excited via the (18O,16O two-neutron transfer reaction

    Directory of Open Access Journals (Sweden)

    Carbone D.

    2016-01-01

    Full Text Available The 13C(18O,16O15C reaction has been studied at 84 MeV incident energy. The ejectiles have been momentum analized by the MAGNEX spectrometer and 15C excitation energy spectra have been obtained up to about 20 MeV. In the region above the two-neutron separation energy, a bump has been observed at 13.7 MeV. The extracted cross section angular distribution for this structure, obtained by using different models for background, displays a clear oscillating pattern, typical of resonant state of the residual nucleus.

  15. Combined two-photon excitation and d → f energy-transfer in Ir/lanthanide dyads with time-gated selection from a two-component emission spectrum.

    Science.gov (United States)

    Edkins, Robert M; Sykes, Daniel; Beeby, Andrew; Ward, Michael D

    2012-10-14

    In a pair of Ir/Eu and Ir/Tb dyads, two-photon excitation of the Ir-phenylpyridine chromophore at 780 nm is followed by partial d → f energy-transfer to give a combination of short-lived Ir-based (blue) and long-lived lanthanide-based (red or green) emission; these components can be selected separately by time-gated detection.

  16. On the use of analytical approximate expressions for the transfer rate in excitation transfer kinetics

    International Nuclear Information System (INIS)

    Kusba, J.; Sipp, B.

    1985-01-01

    We present a discussion about the range of validity of the usual approximate transfer rate expressions used in the description of the kinetics of diffusion-modulated excitation transfer, for a reactive interaction of exponential functional form. We simulate the features of energy transfer by a numerical inversion of the exact Laplace transform of the transfer rate. It is shown that for high diffusion coefficients of the order of 10 -5 cm 2 s -1 , the kinetics may be well reproduced, even at short times, by the asymptotic form of the transfer rate. For slow molecular displacements, the short time static regime is brought to direct observation, but the transfer rate approaches is asymptotic value at a much later time

  17. Mean excitation energies for molecular ions

    DEFF Research Database (Denmark)

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

    2017-01-01

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

  18. Dexter energy transfer pathways.

    Science.gov (United States)

    Skourtis, Spiros S; Liu, Chaoren; Antoniou, Panayiotis; Virshup, Aaron M; Beratan, David N

    2016-07-19

    Energy transfer with an associated spin change of the donor and acceptor, Dexter energy transfer, is critically important in solar energy harvesting assemblies, damage protection schemes of photobiology, and organometallic opto-electronic materials. Dexter transfer between chemically linked donors and acceptors is bridge mediated, presenting an enticing analogy with bridge-mediated electron and hole transfer. However, Dexter coupling pathways must convey both an electron and a hole from donor to acceptor, and this adds considerable richness to the mediation process. We dissect the bridge-mediated Dexter coupling mechanisms and formulate a theory for triplet energy transfer coupling pathways. Virtual donor-acceptor charge-transfer exciton intermediates dominate at shorter distances or higher tunneling energy gaps, whereas virtual intermediates with an electron and a hole both on the bridge (virtual bridge excitons) dominate for longer distances or lower energy gaps. The effects of virtual bridge excitons were neglected in earlier treatments. The two-particle pathway framework developed here shows how Dexter energy-transfer rates depend on donor, bridge, and acceptor energetics, as well as on orbital symmetry and quantum interference among pathways.

  19. Electron transfer, ionization, and excitation in atomic collisions

    International Nuclear Information System (INIS)

    Winter, T.G.; Alston, S.G.

    1992-01-01

    The research being carried out at Penn State by Winter and Alston addresses the fundamental processes of electron transfer, ionization, and excitation in ion-atom (and ion-ion) collisions. The focus is on intermediate- and higher-energy collisions, corresponding to proton energies of about 25 kilo-electron-volts (keV) or larger. At intermediate energies, where the transition probabilities are not small, many states must be coupled in a large calculation, while at higher energies, perturbative approaches may be used. Several studies have been carried out in the current three-year period; most of these treat systems with only one or two electrons, so that fewer approximations need be made and the basic collisional mechanisms can be more clearly described

  20. [Electron transfer, ionization, and excitation in atomic collisions

    International Nuclear Information System (INIS)

    1992-01-01

    Fundamental processes of electron transfer, ionization, and excitation in ion-atom and ion-ion collisions are studied. Attention is focussed on one- and two-electron systems and, more recently, quasi-one-electron systems whose electron-target-ion core can be accurately modeled by one-electron potentials. The basic computational approaches can then be taken with few, if any, approximations, and the underlying collisional mechanisms can be more clearly revealed. At intermediate collision energies (e.g., proton energies for p-He + collisions on the order of 100 kilo-electron volts), many electronic states are strongly coupled during the collision, a coupled-state approach, such as a coupled-Sturmian-pseudostate approach, is appropriate. At higher collision energies (million electron-volt energies) the coupling is weaker with, however, many more states being coupled together, so that high-order perturbation theory is essential

  1. Energy-dependent collisional deactivation of vibrationally excited azulene

    International Nuclear Information System (INIS)

    Shi, J.; Barker, J.R.

    1988-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-12-14

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

  3. Theoretical study of intermolecular energy transfer involving electronically excited molecules: He(1S) + H2(B 1Σ/sub u/+)

    International Nuclear Information System (INIS)

    Grimes, R.M.

    1986-11-01

    To further understanding of gas phase collision dynamics involving electronically-excited molecules, a fully quantum mechanical study of He + H 2 (B 1 Σ/sub u/ + ) was undertaken. Iterative natural orbital configuration interaction (CI) calculations were performed to obtain the interaction potential between He and H 2 (B 1 Σ/sub u/ + ). The potential energy surface (PES) is highly anisotropic and has a van der Waals well of about 0.03 eV for C/sub 2v/ approach. Avoided PES crossings occur with He + H 2 (E,F 1 Σ/sub g/ + ) and with He + H 2 (X 1 Σ/sub g/ + ) and cause a local maximum and a deep minimum in the He + H 2 (B 1 Σ/sub u/ + ) PES, respectively. The crossing with He + H 2 (X 1 Σ/sub g/ + ) provides a mechanism for fluorescence quenching. The computed CI energies were combined with previous multi-reference double excitation CI calculations and fit with analytic functions for convenience in scattering calculations. Accurate dipole polarizabilities and quadrupole moment of H 2 (B 1 Σ/sub u/ + ) were computed for use in the multipole expansion, which is the analytic form of the long-range PES. 129 refs., 28 figs., 35 tabs

  4. Excitation transfer pathways in excitonic aggregates revealed by the stochastic Schrödinger equation

    Energy Technology Data Exchange (ETDEWEB)

    Abramavicius, Vytautas, E-mail: vytautas.ab@gmail.com; Abramavicius, Darius, E-mail: darius.abramavicius@ff.vu.lt [Faculty of Physics, Department of Theoretical Physics, Vilnius University, Saulėtekio 9, LT-10222 Vilnius (Lithuania)

    2014-02-14

    We derive the stochastic Schrödinger equation for the system wave vector and use it to describe the excitation energy transfer dynamics in molecular aggregates. We suggest a quantum-measurement based method of estimating the excitation transfer time. Adequacy of the proposed approach is demonstrated by performing calculations on a model system. The theory is then applied to study the excitation transfer dynamics in a photosynthetic pigment-protein Fenna-Matthews-Olson (FMO) aggregate using both the Debye spectral density and the spectral density obtained from earlier molecular dynamics simulations containing strong vibrational high-frequency modes. The obtained results show that the excitation transfer times in the FMO system are affected by the presence of the vibrational modes; however, the transfer pathways remain the same.

  5. Vibrational excitation of D2 by low energy electrons

    International Nuclear Information System (INIS)

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

    1985-01-01

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

  6. Energy transfer in a mechanically trapped exciplex.

    Science.gov (United States)

    Klosterman, Jeremy K; Iwamura, Munetaka; Tahara, Tahei; Fujita, Makoto

    2009-07-15

    Host-guest complexes involving M(6)L(4) coordination cages can display unusual photoreactivity, and enclathration of the very large fluorophore bisanthracene resulted in an emissive, mechanically trapped intramolecular exciplex. Mechanically linked intramolecular exciplexes are important for understanding the dependence of energy transfer on donor-acceptor distance, orientation, and electronic coupling but are relatively unexplored. Steady-state and picosecond time-resolved fluorescence measurements have revealed that selective excitation of the encapsulated guest fluorophore results in efficient energy transfer from the excited guest to an emissive host-guest exciplex state.

  7. Excitation methods for energy dispersive analysis

    International Nuclear Information System (INIS)

    Jaklevic, J.M.

    1976-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2017-06-15

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

  9. Transfer matrices and excitations with matrix product states

    International Nuclear Information System (INIS)

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

    2015-01-01

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

  10. High energy excitations in itinerant ferromagnets

    International Nuclear Information System (INIS)

    Prange, R.E.

    1984-01-01

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

  11. The Mean Excitation Energy of Atomic Ions

    DEFF Research Database (Denmark)

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

    2015-01-01

    A method for calculation of the mean excitation energies of atomic ions is presented, making the calculation of the energy deposition of fast ions to plasmas, warm, dense matter, and complex biological systems possible. Results are reported to all ions of helium, lithium, carbon, neon, aluminum...

  12. Long-wave UVA radiation excited warm white-light emitting NaGdTiO4: Tm3+/Dy3+/Eu3+ ions tri-doped phosphors: Synthesis, energy transfer and color tunable properties

    International Nuclear Information System (INIS)

    Bharat, L. Krishna; Du, Peng; Yu, Jae Su

    2016-01-01

    NaGdTiO 4 (NGT) phosphors doped with different activator ions (Tm 3+ , Dy 3+ , and Eu 3+ ) were synthesized by a conventional solid-state reaction method in an ambient atmosphere. These phosphors were characterized by scanning electron microscope images, transmission electron microscope images, X-ray diffraction patterns, Fourier transform infrared spectra, and photoluminescence spectra. All the samples were crystallized in an orthorhombic phase with a space group of Pbcm (57). In Tm 3+ /Dy 3+ ions co-doped samples, white-light emission was observed under near-ultraviolet (NUV) excitation. In addition, the energy transfer between Tm 3+ and Dy 3+ ions was proved to be a resonant type via an electric dipole–dipole mechanism and the critical distance of energy transfer was calculated to be 19.91 Å. Furthermore, Tm 3+ /Dy 3+ /Eu 3+ ions tri-doped NGT phosphors demonstrated warm white-light emission by appropriately tuning the activator content, based on the principle of energy transfer. These NUV wavelength excitable phosphors exhibit great potential as a single-phase full-color emitting phosphor for white light-emitting diode applications. - Highlights: • The pebble shaped NaGdTiO 4 particles were prepared by solid-state reaction method. • Tm 3+ and Dy 3+ single doping gives respective blue and cool white light emission. • The Tm 3+ /Dy 3+ ions co-doped samples give CIE values near to standard white light. • Addition of Eu 3+ ions shifts the CIE values towards warm white light region. • This single phase white light emitting phosphors have lower CCT values (<5000 K).

  13. TD-DFT investigation of the potential energy surface for Excited-State Intramolecular Proton Transfer (ESIPT) reaction of 10-hydroxybenzo[h]quinoline: Topological (AIM) and population (NBO) analysis of the intramolecular hydrogen bonding interaction

    International Nuclear Information System (INIS)

    Paul, Bijan Kumar; Guchhait, Nikhil

    2011-01-01

    Here, we report a Density Functional Theoretical (DFT) study on the photophysics of a potent Excited-State Intramolecular Proton Transfer (ESIPT) molecular system, viz., 10-hydroxybenzo[h]quinoline (HBQ). Particular emphasis has been rendered on the assessment of the proton transfer reaction in HBQ in the ground and excited-states through elucidation and a careful perusal of the potential energy surfaces (PES). The non-viability of Ground-State Intramolecular Proton Transfer (GSIPT) process is dictated by a high-energy barrier coupled with no energy minimum for the proton transferred (K-form) form at the ground-state (S 0 ) PES. Remarkable reduction of the barrier along with thermodynamic stability inversion between the enol (E-form) and the keto forms (K-form) of HBQ upon photoexcitation from S 0 to the S 1 -state advocate for the operation of ESIPT process. These findings have been cross-validated on the lexicon of analysis of optimized geometry parameters, Mulliken's charge distribution on the heavy atoms, and molecular orbitals (MO) of the E- and the K-forms of HBQ. Our computational results also corroborate to experimental observations. From the modulations in optimized geometry parameters in course of the PT process a critical assessment has been endeavoured to delve into the movement of the proton during the process. Additional stress has been placed on the analysis of the intramolecular hydrogen bonding (IMHB) interaction in HBQ. The IMHB interaction has been explored by calculation of electron density ρ(r) and the Laplacian ∇ 2 ρ(r) at the bond critical point (BCP) using Atoms-In-Molecule (AIM) method and by calculation of interaction between σ* of OH with the lone pair of the nitrogen atom using Natural Bond Orbital (NBO) analysis. - Highlights: → Theoretical modelling of the photophysics of an ESIPT probe 10-hydroxybenzo[h]quinoline (HBQ). → Calculation of intramolecular hydrogen bond (IMHB) energy. → Role of hyperconjugative charge transfer

  14. Effect resonance radiation transfer of excitation porous silicon to I sub 2 molecules sorbed in pores

    CERN Document Server

    Zakharchenko, K V; Kuznetsov, M B; Chistyakov, A A; Karavanskij, V A

    2001-01-01

    One studies the effect of resonance radiation-free transfer of electronic excitation between silicon nanocrystals and iodine molecules sorbed in pores. The experiment procedure includes laser-induced luminescence and laser desorption mass spectrometry. One analyzes photoluminescence spectra prior to and upon iodine sorption. Excitation of iodine through the mechanism of resonance transfer is determined to result in desorption of the iodine sorbed molecules with relatively high kinetic energies (3-1 eV). One evaluated the peculiar distance of resonance transfer the approximate value of which was equal to 2 nm

  15. Excitation-energy influence at the scission configuration

    Directory of Open Access Journals (Sweden)

    Ramos D.

    2017-01-01

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

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

    NARCIS (Netherlands)

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

    2007-01-01

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

  17. The momentum transfer dependence of double excitations of helium

    International Nuclear Information System (INIS)

    Zhu Lin-Fan; Liu Xiao-Jing; Yuan Zhen-Sheng; Xu Ke-Zun

    2005-01-01

    The momentum transfer dependence of fundamental double excitation processes of helium is studied with high resolution and fast electron impact. It elucidates the dynamical correlations, in terms of internal correlation quantum numbers, K, T and A. The Fano profile parameters q, f a , ρ 2 , f and S of doubly excited states 2 (1,0) 2 +1se , 2 (0,1) 2 +1p0 and 2 (1,0) 2 +1De are determined as functions of momentum transfer K 2 . (author)

  18. Energy transfer in plasmonic systems

    International Nuclear Information System (INIS)

    Pustovit, Vitaliy N; Urbas, Augustine M; Shahbazyan, Tigran V

    2014-01-01

    We present our results on energy transfer between donor and acceptor molecules or quantum dots near a plasmonic nanoparticle. In such systems, the Förster resonance energy transfer is strongly modified due to plasmon-mediated coupling between donors and acceptors. The transfer efficiency is determined by a competition between transfer, radiation and dissipation that depends sensitively on system parameters. When donor and accepror spectral bands overlap with dipole surface plasmon resonance, the dominant transfer mechanism is through plasmon-enhanced radiative coupling. When transfer takes place from an ensemble of donors to an acceptor, a cooperative amplification of energy transfer takes place in a wide range of system parameters. (paper)

  19. Decision making based on optical excitation transfer via near-field interactions between quantum dots

    International Nuclear Information System (INIS)

    Naruse, Makoto; Nomura, Wataru; Ohtsu, Motoichi; Aono, Masashi; Sonnefraud, Yannick; Drezet, Aurélien; Huant, Serge; Kim, Song-Ju

    2014-01-01

    Optical near-field interactions between nanostructured matters, such as quantum dots, result in unidirectional optical excitation transfer when energy dissipation is induced. This results in versatile spatiotemporal dynamics of the optical excitation, which can be controlled by engineering the dissipation processes and exploited to realize intelligent capabilities such as solution searching and decision making. Here, we experimentally demonstrate the ability to solve a decision making problem on the basis of optical excitation transfer via near-field interactions by using colloidal quantum dots of different sizes, formed on a geometry-controlled substrate. We characterize the energy transfer behavior due to multiple control light patterns and experimentally demonstrate the ability to solve the multi-armed bandit problem. Our work makes a decisive step towards the practical design of nanophotonic systems capable of efficient decision making, one of the most important intellectual attributes of the human brain.

  20. Decision making based on optical excitation transfer via near-field interactions between quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Naruse, Makoto, E-mail: naruse@nict.go.jp [Photonic Network Research Institute, National Institute of Information and Communications Technology, 4-2-1 Nukui-kita, Koganei, Tokyo 184-8795 (Japan); Nomura, Wataru; Ohtsu, Motoichi [Department of Electrical Engineering and Information Systems, Graduate School of Engineering, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo 113-8656 (Japan); Aono, Masashi [Earth-Life Science Institute, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguru-ku, Tokyo 152-8550 (Japan); PRESTO, Japan Science and Technology Agency, 4-1-8 Honcho, Kawaguchi-shi, Saitama 332-0012 (Japan); Sonnefraud, Yannick; Drezet, Aurélien; Huant, Serge [Université Grenoble Alpes, Inst. NEEL, F-38000 Grenoble (France); CNRS, Inst. NEEL, F-38042 Grenoble (France); Kim, Song-Ju [WPI Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044 (Japan)

    2014-10-21

    Optical near-field interactions between nanostructured matters, such as quantum dots, result in unidirectional optical excitation transfer when energy dissipation is induced. This results in versatile spatiotemporal dynamics of the optical excitation, which can be controlled by engineering the dissipation processes and exploited to realize intelligent capabilities such as solution searching and decision making. Here, we experimentally demonstrate the ability to solve a decision making problem on the basis of optical excitation transfer via near-field interactions by using colloidal quantum dots of different sizes, formed on a geometry-controlled substrate. We characterize the energy transfer behavior due to multiple control light patterns and experimentally demonstrate the ability to solve the multi-armed bandit problem. Our work makes a decisive step towards the practical design of nanophotonic systems capable of efficient decision making, one of the most important intellectual attributes of the human brain.

  1. Modeling the efficiency of Förster resonant energy transfer from energy relay dyes in dye-sensitized solar cells

    KAUST Repository

    Hoke, Eric T.; Hardin, Brian E.; McGehee, Michael D.

    2010-01-01

    Förster resonant energy transfer can improve the spectral breadth, absorption and energy conversion efficiency of dye sensitized solar cells. In this design, unattached relay dyes absorb the high energy photons and transfer the excitation

  2. Resonant and nonresonant transfer and excitation in Si11+ + He collisions

    International Nuclear Information System (INIS)

    Clark, M.W.

    1988-01-01

    For many years now, dielectronic recombination (DR) has been discussed as a possible energy loss mechanism in high temperature plasmas (e.g. stars). The process is basically the inverse Auger process and involves the capture of a free electron by an ion and the simultaneous excitation of an inner shell electron of the ion producing a doubly excited state. The DR process also includes the radiative deexcitation of the ion and hence represents an energy loss from the plasma since the plasma is essentially transparent to the photons. If, instead of a free electron, an electron that is weakly bound to an atom is captured and an inner shell electron of the ion is excited, the same excited states are produced as in DR. Because the bound electrons have a momentum distribution (Compton profile), individual doubly excited states cannot, in general, be observed in this case. This new process has been called Resonant Transfer and Excitation (RTE). There is also a competing mechanism for RTE in which excitation occurs via the interaction between a projectile ion electron and a target nucleus and the capture occurs because of the interaction of the projectile nucleus and a target electron. This competing mechanism has been termed Nonresonant Transfer and Excitation (NTE) Measurements have been performed to measure RTE and NTE cross sections. A discussion of the theory, methods, and results is included

  3. Hot nuclei, limiting temperatures and excitation energies

    International Nuclear Information System (INIS)

    Peter, J.

    1986-09-01

    Hot fusion nuclei are produced in heavy ion collisions at intermediate energies (20-100 MeV/U). Information on the maximum excitation energy per nucleon -and temperatures- indicated by the experimental data is compared to the predictions of static and dynamical calculations. Temperatures around 5-6 MeV are reached and seem to be the limit of formation of thermally equilibrated fusion nuclei

  4. Electron transfer, ionization, and excitation atomic collisions

    International Nuclear Information System (INIS)

    Winter, T.G.; Alston, S.G.

    1990-01-01

    Basic atomic-collision processes at intermediate and high energies are being studied theoretically at Penn State by Alston and Winter. In the high velocity regime, single-electron capture is treated using a high order multiple-scattering approach; extensive comparison with experiment and analysis of mechanisms have been made. Fitting the calculated amplitude with a simple analytic form, the asymptotic velocity dependence of the cross section is obtained. The effect on the capture amplitude of altering the inner part of the internuclear potential has also been explored. In the intermediate velocity regime, earlier work on collisions between protons and hydrogenic-ion targets using a coupled-state approach is being extended to the two-electron helium target. 29 refs

  5. Phonons and charge-transfer excitations in HTS superconductors

    International Nuclear Information System (INIS)

    Bishop, A.R.

    1989-01-01

    Some of the experimental and theoretical evidence implicating phonons and charge-transfer excitations in HTS superconductors is reviewed. It is suggested that superconductivity may be driven by a synergistic interplay of (anharmonic) phonons and electronic degrees of freedom (e.g., charge fluctuations, excitons). 47 refs., 5 figs

  6. Anomalous temperature dependence of excitation transfer between quantum dots

    Czech Academy of Sciences Publication Activity Database

    Král, Karel; Menšík, Miroslav

    2015-01-01

    Roč. 7, č. 4 (2015), 325-330 ISSN 2164-6627 R&D Projects: GA MŠk(CZ) LD14011; GA MŠk LH12236; GA MŠk LH12186 Institutional support: RVO:68378271 ; RVO:61389013 Keywords : excitation transfer * quantum dots * temperature dependence * electron-phonon interaction Subject RIV: BM - Solid Matter Physics ; Magnetism

  7. Luminescence and energy transfer of Tm3+ or/and Dy3+ co-doped in Sr3Y(PO4)3 phosphors with UV excitation for WLEDs

    International Nuclear Information System (INIS)

    Wang, Jiyou; Wang, Jianbo; Duan, Ping

    2014-01-01

    Powder samples Sr 3 Y 1−x−y (PO 4 ) 3 :xTm 3+ -yDy 3+ were synthesized by the conventional solid-state reaction method. By appropriate tuning of activator content, the emission color can be adjusted around blue to white and yellow. It was discovered that the energy transfer from Tm 3+ to Dy 3+ was demonstrated to be via the intensity of Dy 3+ emission increase with the increase of Tm 3+ concentration. By changing the doping concentration of Tm 3+ and Dy 3+ in Sr 3 Y(PO 4 ) 3 , white-emitting phosphors are produced by 350 nm excitation wavelength, their corresponding color coordinates are very close to the white color chromaticity coordinates (x=0.33, y=0.33). Finally, Sr 3 Y 1−x−y (PO 4 ) 3 :xTm 3+ −yDy 3+ phosphors could be a good promising single-component white light-emitting UV-convertible phosphor in the field of white LEDs. -- Highlights: • The Sr 3 Y 1−x−y (PO 4 ) 3 :xTm 3+ −yDy 3+ phosphors were synthesized by the conventional solid-state reaction method. • The energy transfer in between Tm 3+ and Dy 3+ was observed and explained. • The phosphors can be efficiently excited by a UV light. • The Sr 3 Y 1−x−y (PO 4 ) 3 :xTm 3+ -yDy 3+ phosphor could be a better candidate white phosphor for UV W-LEDs

  8. Spectral variations and energy transfer processes on both Er 3+ ion concentration and excitation densities in Yb 3+-Er 3+ codoped LaF3 materials

    International Nuclear Information System (INIS)

    Zhang Jisen; Qin Weiping; Zhao Dan; Degejihu; Zhang Jishuang; Wang Yan; Cao Chunyan

    2007-01-01

    In comparison with the up-conversion spectra of Yb 3+ -Er 3+ codopded systems reported previously, the interesting intensity changes of up-conversion luminescence between the violet, the blue, the green and the red on the both Er 3+ ion concentration and excitation density with 978 nm laser diodes as an excitation source were observed in Yb 3+ -Er 3+ codopded LaF 3 powders. In order to clarify the change mechanisms, the up-conversion spectra of LaF 3 : 10 mol% Yb 3+ , 0.5 mol% Er 3+ and LaF 3 : 10 mol% Yb 3+ , 1 mol% Er 3+ were investigated and the results indicated that the cross-relaxation processes between Er 3+ ions and the thermal population of the 2 H 11/2 level play significant roles

  9. Intramolecular Energy Transfer, Charge Transfer & Hydrogen Bond

    Indian Academy of Sciences (India)

    Ultrafast Dynamics of Chemical Reactions in Condensed Phase: Intramolecular Energy Transfer, Charge Transfer & Hydrogen Bond · PowerPoint Presentation · Slide 3 · Slide 4 · Slide 5 · Slide 6 · Slide 7 · Slide 8 · Slide 9 · Slide 10 · Slide 11 · Slide 12 · Slide 13 · Slide 14 · Slide 15 · Slide 16 · Slide 17 · Slide 18 · Slide 19.

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

    Science.gov (United States)

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

    2017-06-22

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

  11. Absence of quantum oscillations in electronic excitation transfer in the Fenna-Matthews-Olson complex

    Science.gov (United States)

    Eisfeld, Alexander; Ritschel, Gerhard; Roden, Jan; Strunz, Walter; Aspuru-Guzik, Alan

    2012-02-01

    Energy transfer in the photosynthetic Fenna-Matthews-Olson (FMO) complex of the Green Sulfur Bacteria is studied theoretically taking all three subunits (monomers) of the FMO trimer and the recently found eighth bacteriochlorophyll (BChl) molecule into account. For the calculations we use the efficient Non-Markovian Quantum State diffusion approach. Since it is believed that the eighth BChl is located near the main light harvesting antenna we look at the differences in transfer between the situation when BChl 8 is initially excited and the usually considered case when BChl 1 or 6 is initially excited. We find strong differences in the transfer dynamics, both qualitatively and quantitatively. When the excited state dynamics is initialized at site eight of the FMO complex, we see a slow exponential-like decay of the excitation. This is in contrast to the oscillations and a relatively fast transfer that occurs when only seven sites or initialization at sites 1 and 6 is considered. Additionally we show that differences in the values of the electronic transition energies found in the literature lead to a large difference in the transfer dynamics.

  12. Atomic excitation and molecular dissociation by low energy electron collisions

    International Nuclear Information System (INIS)

    Weyland, Marvin

    2016-01-01

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

  13. Atomic excitation and molecular dissociation by low energy electron collisions

    Energy Technology Data Exchange (ETDEWEB)

    Weyland, Marvin

    2016-11-16

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

  14. Energy transfer properties and mechanisms

    International Nuclear Information System (INIS)

    Barker, J.R.

    1993-01-01

    Since no single experimental technique is the best method for energy transfer experiments, we have used both time-dependent infrared fluorescence (IRF) and time-dependent thermal lensing (TDTL) to study energy transfer in various systems. We are investigating pump-probe techniques employing resonance enhanced multiphoton ionization (REMPI). IRF was used to study benzene, azulene, and toluene. TDTL was used to study CS 2 and SO 2 (data not given for latter). Large molecule energy transfer mechanisms are discussed. 10 figs

  15. The collision cross sections for excitation energy transfer in Rb*(5P3/2)+K(4S1/2)→Rb(5S1/2)+K*(4PJ) processes

    International Nuclear Information System (INIS)

    Horvatic, V.; Vadla, C.; Movre, M.

    1993-01-01

    The collisional excitation transfer for the processes Rb * (5P 3/2 ) + K(4S 1/2 ) → Rb(5S 1/2 ) + K * (4P J ), J = 1/2, 3/2, was investigated using two-photon laser excitation techniques with a thermionic heat-pipe diode as a detector. The population densities of the K 4P J levels induced by collisions with excited Rb atoms as well as those produced by direct laser excitation of the potassium atoms were probed through the measurement of the thermionic signals generated due to the ionization of the potassium atoms emerging from the K(4P J ) → K(7S 1/2 ) excitation channel. (orig./WL)

  16. Electron transfer by excited benzoquinone anions: slow rates for two-electron transitions.

    Science.gov (United States)

    Zamadar, Matibur; Cook, Andrew R; Lewandowska-Andralojc, Anna; Holroyd, Richard; Jiang, Yan; Bikalis, Jin; Miller, John R

    2013-09-05

    Electron transfer (ET) rate constants from the lowest excited state of the radical anion of benzoquinone, BQ(-•)*, were measured in THF solution. Rate constants for bimolecular electron transfer reactions typically reach the diffusion-controlled limit when the free-energy change, ΔG°, reaches -0.3 eV. The rate constants for ET from BQ(-•)* are one-to-two decades smaller at this energy and do not reach the diffusion-controlled limit until -ΔG° is 1.5-2.0 eV. The rates are so slow probably because a second electron must also undergo a transition to make use of the energy of the excited state. Similarly, ET, from solvated electrons to neutral BQ to form the lowest excited state, is slow, while fast ET is observed at a higher excited state, which can be populated in a transition involving only one electron. A simple picture based on perturbation theory can roughly account for the control of electron transfer by the need for transition of a second electron. The picture also explains how extra driving force (-ΔG°) can restore fast rates of electron transfer.

  17. Ultrafast Energy Transfer in an Artificial Photosynthetic Antenna

    Directory of Open Access Journals (Sweden)

    van Grondelle R.

    2013-03-01

    Full Text Available We temporally resolved energy transfer kinetics in an artificial light-harvesting dyad composed of a phthalocyanine covalently linked to a carotenoid. Upon carotenoid photo-excitation, energy transfers within ≈100fs (≈52% efficiency to the phthalocyanine.

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

    Science.gov (United States)

    Gould, Tim; Kronik, Leeor; Pittalis, Stefano

    2018-05-01

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

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

    International Nuclear Information System (INIS)

    Van Tassle, Aaron Justin

    2006-01-01

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

  20. Superconductivity and charge transfer excitations in high Tc superconductors

    International Nuclear Information System (INIS)

    Balseiro, C.A.; Alascio, B.; Gagliano, E.; Rojo, A.

    1988-01-01

    We present some numerical results to show that in a simple model which includes Cu 3d and O 2p orbitals together with inter and intra atomic correlations pairing between holes can occur due to charge transfer excitations. We present also a simple approximation to derive an effective Hamiltonian containing an interaction between particles which is attractive for some values of the different microscopic parameters

  1. "Inverted" Solvent Effect on Charge Transfer in the Excited State.

    Science.gov (United States)

    Nau; Pischel

    1999-10-04

    Faster in cyclohexane than in acetonitrile is the fluorescence quenching of the azoalkane 2,3-diazabicyclo[2.2.2]oct-2-ene (DBO) by amines and sulfides. Although this photoreaction is induced by charge transfer (CT; see picture) and exciplexes are formed, the increase in the dipole moment of the exciplex is not large enough to offset the solvent stabilization of the excited reactants, and an "inverted" solvent effect results.

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

    CERN Document Server

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

    2002-01-01

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

  3. Lifetime and g-factor measurements of excited states using Coulomb excitation and alpha transfer reactions

    Energy Technology Data Exchange (ETDEWEB)

    Guevara, Z. E., E-mail: zjguevaram@unal.edu.co; Torres, D. A., E-mail: datorresg@unal.edu.co [Physics Department, Universidad Nacional de Colombia, Bogotá D.C. (Colombia)

    2016-07-07

    In this contribution the challenges in the use of a setup to simultaneously measure lifetimes and g-factor values will be presented. The simultaneous use of the transient field technique and the Doppler Shift Attenuation Method, to measure magnetic moments and lifetimes respectively, allows to obtain a complete characterization of the currents of nucleons and the deformation in excited states close to the ground state. The technique is at the moment limited to Coulomb excitation and alpha-transfer reactions, what opens an interesting perspective to consider this type of experiments with radioactive beams. The use of deep-inelastic and fusion-evaporation reactions will be discussed. An example of a setup that makes use of a beam of {sup 106}Cd to study excited states of {sup 110}Sn and the beam nuclei itself will be presented.

  4. Excitation functions for quasielastic transfer reactions induced with heavy ions in bismuth

    International Nuclear Information System (INIS)

    Gardes, D.; Bimbot, R.; Maison, J.; de Reilhac, L.; Rivet, M.F.; Fleury, A.; Hubert, F.; Llabador, Y.

    1978-01-01

    The excitation functions for the production of 210 Bi, 210 Po, /sup 207-211/At, and 211 Rn through quasielastic transfer reactions induced with heavy ions in 209 Bi have been measured. The corresponding reactions involved the transfer of one neutron, one proton, two charges, and three charges from projectile to target. The projectiles used were 12 C, 14 N, 16 O, 19 F, 20 Ne, 40 Ar, 40 Ca, 56 Fe, and 63 Cu. The experimental techniques involved target irradiations and off-line α and γ activity measurements. Chemical separations were used to solve specific problems. Careful measuremnts of incident energies and cross sections were performed close to the reaction thresholds. All excitation functions exhibit the typical features of quasielastic transfer reactions: a sharp increase at low energy, and a constant value at high incident energy. The position of the thresholds are strongly influenced by the energetics of the reaction: High cross sections are observed under the strong interaction barrier if the energy balance at the minimum distance of approach is positive. This balance is equal to the difference between the interaction potentials in the entrance and exit channels, corrected for the mass balance. The constant cross sections observed for the high energy part of a given excitation function are consistent with the assumption that the curve P (R) which represents the transfer probability versus the distance between the nucleus centers does not vary with incident energy. This assumption implies the constancy of the optimum distance of approach R/sub opt/, of the R window ΔR for which P (R) is significant, and of the magnitude of P (R). Moreover the data show that the high energy cross sections for one-proton transfer are independent of the projectile, while odd-even effects of the projectile atomic number Z on the two-charge transfer cross sections are observed for the lightest incident ions 14 N to 20 Ne

  5. Excitation transfer and trapping kinetics in plant photosystem I probed by two-dimensional electronic spectroscopy.

    Science.gov (United States)

    Akhtar, Parveen; Zhang, Cheng; Liu, Zhengtang; Tan, Howe-Siang; Lambrev, Petar H

    2018-03-01

    Photosystem I is a robust and highly efficient biological solar engine. Its capacity to utilize virtually every absorbed photon's energy in a photochemical reaction generates great interest in the kinetics and mechanisms of excitation energy transfer and charge separation. In this work, we have employed room-temperature coherent two-dimensional electronic spectroscopy and time-resolved fluorescence spectroscopy to follow exciton equilibration and excitation trapping in intact Photosystem I complexes as well as core complexes isolated from Pisum sativum. We performed two-dimensional electronic spectroscopy measurements with low excitation pulse energies to record excited-state kinetics free from singlet-singlet annihilation. Global lifetime analysis resolved energy transfer and trapping lifetimes closely matches the time-correlated single-photon counting data. Exciton energy equilibration in the core antenna occurred on a timescale of 0.5 ps. We further observed spectral equilibration component in the core complex with a 3-4 ps lifetime between the bulk Chl states and a state absorbing at 700 nm. Trapping in the core complex occurred with a 20 ps lifetime, which in the supercomplex split into two lifetimes, 16 ps and 67-75 ps. The experimental data could be modelled with two alternative models resulting in equally good fits-a transfer-to-trap-limited model and a trap-limited model. However, the former model is only possible if the 3-4 ps component is ascribed to equilibration with a "red" core antenna pool absorbing at 700 nm. Conversely, if these low-energy states are identified with the P 700 reaction centre, the transfer-to-trap-model is ruled out in favour of a trap-limited model.

  6. Comparison of modified driver circuit and capacitor-transfer circuit in longitudinally excited N2 laser.

    Science.gov (United States)

    Uno, Kazuyuki; Akitsu, Tetsuya; Nakamura, Kenshi; Jitsuno, Takahisa

    2013-04-01

    We developed a modified driver circuit composed of a capacitance and a spark gap, called a direct-drive circuit, for a longitudinally excited gas laser. The direct-drive circuit uses a large discharge impedance caused by a long discharge length of the longitudinal excitation scheme and eliminates the buffer capacitance used in the traditional capacitor-transfer circuit. We compared the direct-drive circuit and the capacitor-transfer circuit in a longitudinally excited N2 laser (wavelength: 337 nm). Producing high output energy with the capacitor-transfer circuit requires a large storage capacitance and a discharge tube with optimum dimensions (an inner diameter of 4 mm and a length of 10 cm in this work); in contrast, the direct-drive circuit requires a high breakdown voltage, achieved with a small storage capacitance and a large discharge tube. Additionally, for the same input energy of 792 mJ, the maximum output energy of the capacitor-transfer circuit was 174.2 μJ, and that of the direct-drive circuit was 344.7 μJ.

  7. Optimization of excitation transfer in a spin chain

    International Nuclear Information System (INIS)

    Gurman, Vladimir I.; Guseva, Irina S.; Fesko, Oles V.

    2016-01-01

    A revised formulation of the problem of fastest transfer of the excitation in a spin chain is considered on the base of Shrödinger equation which Hamiltonian depends linearly on control. It is taken into account that the excitation of the first or last spin means that it has greatest amplitude equal to the chain invariant whereas its phase is undefined and can be considered as an additional control variable. The role of this additional control is analyzed via transformation of the original problem with unbounded linear control to the regular derived problem known from the theory of degenerate problems [1, 2], in the same way as in [2]. The overall procedure is demonstrated in computational experiments with the use of visual examples.

  8. Photoinduced energy and electron transfer in rubrene-benzoquinone and rubrene-porphyrin systems

    KAUST Repository

    Khan, Jafar Iqbal

    2014-11-01

    Excited-state electron and energy transfer from singlet excited rubrene (Ru) to benzoquinone (BQ) and tetra-(4-aminophenyl) porphyrin (TAPP) were investigated by steady-state absorption and emission, time-resolved transient absorption, and femtosecond (fs)-nanosecond (ns) fluorescence spectroscopy. The low reduction potential of BQ provides the high probability of electron transfer from the excited Ru to BQ. Steady-state and time-resolved results confirm such an excited electron transfer scenario. On the other hand, strong spectral overlap between the emission of Ru and absorption of TAPP suggests that energy transfer is a possible deactivation pathway of the Ru excited state.

  9. Excitation transfer in two two-level systems coupled to an oscillator

    International Nuclear Information System (INIS)

    Hagelstein, P L; Chaudhary, I U

    2008-01-01

    We consider a generalization of the spin-boson model in which two different two-level systems are coupled to an oscillator, under conditions where the oscillator energy is much less than the two-level system energies, and where the oscillator is highly excited. We find that the two-level system transition energy is shifted, producing a Bloch-Siegert shift in each two-level system similar to what would be obtained if the other were absent. At resonances associated with energy exchange between a two-level system and the oscillator, the level splitting is about the same as would be obtained in the spin-boson model at a Bloch-Siegert resonance. However, there occur resonances associated with the transfer of excitation between one two-level system and the other, an effect not present in the spin-boson model. We use a unitary transformation leading to a rotated system in which terms responsible for the shift and splittings can be identified. The level splittings at the anticrossings associated with both energy exchange and excitation transfer resonances are accounted for with simple two-state models and degenerate perturbation theory using operators that appear in the rotated Hamiltonian

  10. Luminescence and energy transfer

    Energy Technology Data Exchange (ETDEWEB)

    Blasse, G; Bleijenberg, K C; Powell, R C

    1980-01-01

    This paper deals with the luminescence of uranate centres in solids. The luminescence properties are influenced by the coordination number of the hexavalent uranium ion and by the crystallographic surroundings of the uranate centre. Transitions playing a role in the luminescence processes within the octahedral UO/sub 6//sup 6 -/ group are discussed using the results from both theoretical and experimental studies on another octahedral uranium complex: UF/sub 6/. The luminescence of the octahedral uranate group in oxidic compounds is discussed. Attention is paid to the vibrational structure, which is observed in the luminescence spectra at low temperatures and to the temperature quenching of the luminescence. The temperature quenching of the uranate luminescence in uranium-doped tungstates with ordered perovskite structure can be described in terms of a three state single configurational coordinate diagram. The complicated luminescence spectra of uranium-activated sodium fluoride (NaF-U) crystals have been unraveled using chemical variation of the crystal compositions and using site selective laser excitation techniques. Four different luminescent uranate centres have been observed in NaF-U. A model for the configurations of the luminescent centres has been deduced using the results from ionic conductivity experiments.

  11. Energy relaxation and transfer in excitonic trimer

    International Nuclear Information System (INIS)

    Herman, Pavel; Barvik, Ivan; Urbanec, Martin

    2004-01-01

    Two models describing exciton relaxation and transfer (the Redfield model in the secular approximation and Capek's model) are compared for a simple example - a symmetric trimer coupled to a phonon bath. Energy transfer within the trimer occurs via resonance interactions and coupling between the trimer and the bath occurs via modulation of the monomer energies by phonons. Two initial conditions are adopted: (1) one of higher eigenstates of the trimer is initially occupied and (2) one local site of the trimer is initially occupied. The diagonal exciton density matrix elements in the representation of eigenstates are found to be the same for both models, but this is not so for the off-diagonal density matrix elements. Only if the off-diagonal density matrix elements vanish initially (initial condition (1)), they then vanish at arbitrary times in both models. If the initial excitation is local, the off-diagonal matrix elements essentially differ

  12. Optical absorption and energy transfer processes in dendrimers

    International Nuclear Information System (INIS)

    Reineker, P.; Engelmann, A.; Yudson, V.I.

    2004-01-01

    For dendrimers of various sizes the energy transfer and the optical absorption is investigated theoretically. The molecular subunits of a dendrimer are modeled as two-level systems. The electronic interaction between them is described via transfer integrals and the influence of vibrational degrees of freedom is taken into account in a first approach using a stochastic model. We discuss the time dependence of the energy transport and show that rim states of the dendrimer dominate the absorption spectra, that in general the electronic excitation energy is concentrated on peripheric molecules, and that the energetically lowest absorption peak is redshifted with increasing dendrimer size due to delocalization of the electronic excitation

  13. Electron transfer from electronic excited states to sub-vacuum electron traps in amorphous ice

    International Nuclear Information System (INIS)

    Vichnevetski, E.; Bass, A.D.; Sanche, L.

    2000-01-01

    We investigate the electron stimulated yield of electronically excited argon atoms (Ar * ) from monolayer quantities of Ar deposited onto thin films of amorphous ice. Two peaks of narrow width ( - electron-exciton complex into exciton states, by the transfer of an electron into a sub-vacuum electron state within the ice film. However, the 10.7 eV feature is shifted to lower energy since electron attachment to Ar occurs within small pores of amorphous ice. In this case, the excess electron is transferred into an electron trap below the conduction band of the ice layer

  14. Excitation functions for quasi-elastic transfer reactions induced with heavy ions in bismuth

    International Nuclear Information System (INIS)

    Gardes, D.; Bimbot, R.; Maison, J.; Reilhac, L. de; Rivet, M.F.; Fleury, A.; Hubert, F.; Llabador, Y.

    1977-01-01

    The excitation functions for the production of 210 Bi, 210 Po, sup(207-211)At and 211 Rn through quasi-elastic transfer reactions induced with heavy ions in 209 Bi have been measured. The corresponding reactions involved the transfer of one neutron, one proton, two and three charges from projectile to target. The projectiles used were 12 C, 14 N, 16 O, 19 F, 20 Ne, 40 Ca, 56 Fe and 63 Cu. The experimental techniques involved target irradiations and off-line α and γ activity measurements. Chemical separations were used to solve specific problems. Careful measurements of incident energies and cross sections were performed close to the reaction thresholds

  15. Effect of collision energy and vibrational excitation on endothermic ion-molecule reactions

    International Nuclear Information System (INIS)

    Turner, T.P.

    1984-07-01

    This thesis is divided into two major parts. In the first part an experimental study of proton and deuteron transfer in H 2 + + He and HD + + He has been carried out as a function of kinetic and vibrational energy. The data gives evidence that at lower kinetic energies, the spectator stripping mechanism indeed plays an important role when H 2 + or HD + is vibrationally excited. The second half of this thesis examines the relative efficiencies between the excitation of C-C stretching vibration and collision energy on the promotion of the H atom transfer reaction of C 2 H 2 + + H 2 → C 2 H 3 + + H

  16. Molecular-alignment dependence in the transfer excitation of H2

    International Nuclear Information System (INIS)

    Wang, Y.D.; McGuire, J.H.; Weaver, O.L.; Corchs, S.E.; Rivarola, R.D.

    1993-01-01

    Molecular-alignment effects in the transfer excitation of H 2 by high-velocity heavy ions are studied using a two-step mechanism with amplitudes evaluated from first-order perturbation theory. Two-electron transfer excitation is treated as a result of two independent collision processes (excitation and electron transfer). Cross sections for each one-electron subprocess as well as the combined two-electron process are calculated as functions of the molecular-alignment angle. Within the independent-electron approximation, the dynamic roles of electron excitation and transfer in conjunction with molecular alignment are explored. While both excitation and transfer cross sections may strongly depend on molecular alignment, it is electron transfer that is largely responsible for the molecular-alignment dependence in the transfer excitation process. Interpretation of some experimental observations based on this model will also be discussed

  17. Directing the path of light-induced electron transfer at a molecular fork using vibrational excitation

    Science.gov (United States)

    Delor, Milan; Archer, Stuart A.; Keane, Theo; Meijer, Anthony J. H. M.; Sazanovich, Igor V.; Greetham, Gregory M.; Towrie, Michael; Weinstein, Julia A.

    2017-11-01

    Ultrafast electron transfer in condensed-phase molecular systems is often strongly coupled to intramolecular vibrations that can promote, suppress and direct electronic processes. Recent experiments exploring this phenomenon proved that light-induced electron transfer can be strongly modulated by vibrational excitation, suggesting a new avenue for active control over molecular function. Here, we achieve the first example of such explicit vibrational control through judicious design of a Pt(II)-acetylide charge-transfer donor-bridge-acceptor-bridge-donor 'fork' system: asymmetric 13C isotopic labelling of one of the two -C≡C- bridges makes the two parallel and otherwise identical donor→acceptor electron-transfer pathways structurally distinct, enabling independent vibrational perturbation of either. Applying an ultrafast UVpump(excitation)-IRpump(perturbation)-IRprobe(monitoring) pulse sequence, we show that the pathway that is vibrationally perturbed during UV-induced electron transfer is dramatically slowed down compared to its unperturbed counterpart. One can thus choose the dominant electron transfer pathway. The findings deliver a new opportunity for precise perturbative control of electronic energy propagation in molecular devices.

  18. Integrated analysis of energy transfers in elastic-wave turbulence.

    Science.gov (United States)

    Yokoyama, Naoto; Takaoka, Masanori

    2017-08-01

    In elastic-wave turbulence, strong turbulence appears in small wave numbers while weak turbulence does in large wave numbers. Energy transfers in the coexistence of these turbulent states are numerically investigated in both the Fourier space and the real space. An analytical expression of a detailed energy balance reveals from which mode to which mode energy is transferred in the triad interaction. Stretching energy excited by external force is transferred nonlocally and intermittently to large wave numbers as the kinetic energy in the strong turbulence. In the weak turbulence, the resonant interactions according to the weak turbulence theory produce cascading net energy transfer to large wave numbers. Because the system's nonlinearity shows strong temporal intermittency, the energy transfers are investigated at active and moderate phases separately. The nonlocal interactions in the Fourier space are characterized by the intermittent bundles of fibrous structures in the real space.

  19. Stray energy transfer during endoscopy.

    Science.gov (United States)

    Jones, Edward L; Madani, Amin; Overbey, Douglas M; Kiourti, Asimina; Bojja-Venkatakrishnan, Satheesh; Mikami, Dean J; Hazey, Jeffrey W; Arcomano, Todd R; Robinson, Thomas N

    2017-10-01

    Endoscopy is the standard tool for the evaluation and treatment of gastrointestinal disorders. While the risk of complication is low, the use of energy devices can increase complications by 100-fold. The mechanism of increased injury and presence of stray energy is unknown. The purpose of the study was to determine if stray energy transfer occurs during endoscopy and if so, to define strategies to minimize the risk of energy complications. A gastroscope was introduced into the stomach of an anesthetized pig. A monopolar generator delivered energy for 5 s to a snare without contacting tissue or the endoscope itself. The endoscope tip orientation, energy device type, power level, energy mode, and generator type were varied to mimic in vivo use. The primary outcome (stray current) was quantified as the change in tissue temperature (°C) from baseline at the tissue closest to the tip of the endoscope. Data were reported as mean ± standard deviation. Using the 60 W coag mode while changing the orientation of the endoscope tip, tissue temperature increased by 12.1 ± 3.5 °C nearest the camera lens (p energy transfer (p = 0.04 and p = 0.002, respectively) as did utilizing the low-voltage cut mode (6.6 ± 0.5 °C, p energy transfer compared to a standard generator (1.5 ± 3.5 °C vs. 9.5 ± 0.8 °C, p energy is transferred within the endoscope during the activation of common energy devices. This could result in post-polypectomy syndrome, bleeding, or perforation outside of the endoscopist's view. Decreasing the power, utilizing low-voltage modes and/or an impedance-monitoring generator can decrease the risk of complication.

  20. Intermolecular energy transfer in binary systems of dye polymers

    Science.gov (United States)

    Liu, Lin-I.; Barashkov, Nikolay N.; Palsule, Chintamani P.; Gangopadhyay, Shubhra; Borst, Walter L.

    2000-10-01

    We present results and physical interpretations for the energy transfer mechanisms in two-component dye polymer systems. The data consist of fluorescence emission spectra and decays. Two dyes were embedded in an epoxypolymer base, and only they participated in the energy transfer. Following pulsed laser excitation of the donor dye, energy transfer took place to the accept dye. The possible transfer paths considered here were nonradiative and radiative transfer. The latter involves two steps, emission and absorption of a photon, and therefore is relatively slow, while nonradiative transfer is a fast single step resulting from direct Coulomb interactions. A predominantly nonradiative transfer is desirable for applications, for instance in wavelength shifters in high energy particle detection. We studied the concentration effects of the dyes on the energy transfer and obtained the relative quantum efficiencies of various wavelength shifters from the fluorescence emission spectra. For low acceptor concentrations, radiative transfer was found to dominate, while nonradiative transfer became dominant at increasing dye concentrations. The fluorescence decays were analyzed with a sum-of-exponentials method and with Förster kinetics. The sum of exponential model yielded mean decay times of the dye polymers useful for a general classification. The decay times decreased as desired with increasing acceptor concentration. The samples, in which nonradiative energy transfer dominated, were analyzed with Förster kinetics. As a result, the natural decay times of the donor and acceptor dyes and the critical radii for nonradiative energy transfer were obtained from a global best fit.

  1. Low energy spin excitations in chromium metal

    International Nuclear Information System (INIS)

    Pynn, R.; Azuah, R.T.; Stirling, W.G.

    1997-01-01

    Neutron scattering experiments with full polarization analysis have been performed with a single crystal of chromium to study the low-energy spin fluctuations in the transverse spin density wave (TSDW) state. A number of remarkable results have been found. Inelastic scattering observed close to the TSDW satellite positions at (1 ± δ,0,0) does not behave as expected for magnon scattering. In particular, the scattering corresponds to almost equally strong magnetization fluctuations both parallel and perpendicular to the ordered moments of the TSDW phase. As the Neel temperature is approached from below, scattering at the commensurate wavevector (1,0,0) increases in intensity as a result of critical scattering at silent satellites (1,0, ± δ) being included within the spectrometer resolution function. This effect, first observed by Sternlieb et al, does not account for all of the inelastic scattering around the (1,0,0) position, however, Rather, there are further collective excitations, apparently emanating from the TSDW satellites, which correspond to magnetic fluctuations parallel to the ordered TSDW moments. These branches have a group velocity that is close to that of (1,0,0) longitudinal acoustic (LA) phonons, but assigning their origin to magneto-elastic scattering raises other unanswered questions

  2. Isotope separation process by transfer of vibrational energy

    International Nuclear Information System (INIS)

    Angelie, C.; Cauchetier, M.; Paris, J.

    1983-01-01

    This process consists in exciting A molecules by absorption of a pulsed light beam, then in exciting until their dissociation X molecules, present in several isotopic forms, by a vibrational transfer between the A molecules and the X molecules, the A molecules having a dissociation energy greater than that of the X molecules, the duration and energy of the light pulses being such that the absorption time by the A molecules is less than the excitation time of the X molecules and the temperature conditions such that the thermal width of the vibration rays is at the most near the isotopic difference between the resonance rays of the two isotopic varieties [fr

  3. Comparative molecular-orbital and atomic-orbital study of electron transfer and excitation in He++Na(3s) collisions at energies of 0.05 to 20 keV/amu

    International Nuclear Information System (INIS)

    Fritsch, W.; Kimura, M.; Lane, N.F.

    1990-01-01

    Electron transfer and excitation in 0.05- to 20-keV/amu He + +Na(3s) collisions is studied theoretically within the close-coupling method with two-electron molecular- and atomic-orbital expansion basis sets. Results agree with the trend of other information on this system. Remaining discrepancies that are larger than those in similar contemporary studies of one-electron systems are discussed with reference to the convergence of this two-electron study. Results for the integral alignment parameter A 20 are also presented as a guideline for future experimental study

  4. Pumped energy transfer stations (STEP)

    International Nuclear Information System (INIS)

    Tournery, Jean-Francois

    2015-12-01

    As objectives of development are high for renewable energies (they are supposed to cover 50 per cent of new energy needs by 2035), pumped energy transfer stations are to play an important role in this respect. The author first discusses the consequences of the development of renewable energies on the exploitation of electric grids: issue of intermittency for some of them, envisaged solutions. Then, he addresses one of the solutions: the storage of electric power. He notices that increasing the potential energy of a volume of water is presently the most mature solution to face massive needs of the power system. Dams and pumped energy transfer stations represent now almost the whole installed storage power in the world. The author then presents these pumped energy transfer stations: principle, brief history (the first appeared in Italy and Switzerland at the end of the 1890's). He indicates the various parameters of assessment of such stations: maximum stored energy, installed power in pumping mode and turbine mode, time constant, efficiency, level of flexibility. He discusses economic issues. He describes and comments the operation of turbine-pump groups: ternary groups, reversible binary groups. He discusses barriers to be overcome and technical advances to be made for varying speed groups and for marine stations. He finally gives an overview (table with number of stations belonging to different power ranges, remarkable installations) of existing stations in China, USA, Japan, Germany, Austria, Spain, Portugal, Italy, Switzerland, France and UK, and indicate predictions regarding storage needs at the world level. Some data are finally indicated for the six existing French installations

  5. Transfer and breakup reactions at intermediate energies

    International Nuclear Information System (INIS)

    Stokstad, R.G.

    1986-04-01

    The origin of the quasi-elastic peak in peripheral heavy-ion reactions is discussed in terms of inelastic scattering and transfer reactions to unbound states of the primary projectile-like fragment. The situation is analogous to the use of reverse kinematics in fusion reactions, a technique in which the object of study is moving with nearly the beam velocity. It appears that several important features of the quasi-elastic peak may be explained by this approach. Projectile-breakup reactions have attractive features for the study of nuclear structure. They may also be used to determine the partition of excitation energy in peripheral reactions. At intermediate energies, neutron-pickup reactions leading to four-body final states become important. Examples of experiments are presented that illustrate these points. 15 refs., 14 figs

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

    International Nuclear Information System (INIS)

    Frascaria, N.

    1987-09-01

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

  7. Reversible Energy Transfer and Fluorescence Decay in Solid Solutions

    Science.gov (United States)

    Shealy, David L.; Hoover, Richard B.; Gabardi, David R.

    1988-07-01

    The article deals with the influence of reversible excitation energy transfer on the fluorescence decay in systems with random distribution of molecules. On the basis of a hopping model, we have obtained an expression for the Laplace transform of the decay function and an expression for the average decay time. The case of dipole-dipole interaction is discussed in detail.

  8. Study of excitation energy dependence of nuclear level density parameter

    International Nuclear Information System (INIS)

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

    2016-01-01

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

  9. On the determination of the mean excitation energy of water

    DEFF Research Database (Denmark)

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

    2013-01-01

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

  10. Dependence of the giant dipole strength function on excitation energy

    International Nuclear Information System (INIS)

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

    1982-01-01

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

  11. Modeling the cooperative energy transfer dynamics of quantum cutting for solar cells

    NARCIS (Netherlands)

    Rabouw, Freddy T.; Meijerink, Andries

    2015-01-01

    Cooperative energy transfer (ET) is a quantum cutting (or downconversion) process where a luminescent center splits its excited state energy in two by simultaneous transfer to two nearby acceptor centers, thus yielding two low-energy photons for each high-energy photon absorbed. It has the potential

  12. Roles of the Excitation in Harvesting Energy from Vibrations.

    Directory of Open Access Journals (Sweden)

    Hui Zhang

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

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

    Science.gov (United States)

    Omidyan, Reza; Iravani, Maryam

    2016-11-01

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

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

    Science.gov (United States)

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

    2018-04-05

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

  15. Excitation energy transfer to luminescence centers in M{sup II}MoO{sub 4} (M{sup II}=Ca, Sr, Zn, Pb) and Li{sub 2}MoO{sub 4}

    Energy Technology Data Exchange (ETDEWEB)

    Spassky, D.A., E-mail: deris2002@mail.ru [Skobeltsyn Institute of Nuclear Physics, M.V. Lomonosov Moscow State University, Leninskie Gory 1, bld.2, 119991 Moscow (Russian Federation); National University of Science and Technology (MISiS), Leninsky Prospekt 4, 119049 Moscow (Russian Federation); Kozlova, N.S. [National University of Science and Technology (MISiS), Leninsky Prospekt 4, 119049 Moscow (Russian Federation); Nagirnyi, V. [Institute of Physics, University of Tartu, W. Ostwaldi 1, 50411 Tartu (Estonia); Savon, A.E. [Skobeltsyn Institute of Nuclear Physics, M.V. Lomonosov Moscow State University, Leninskie Gory 1, bld.2, 119991 Moscow (Russian Federation); Hizhnyi, Yu.A.; Nedilko, S.G. [Taras Shevchenko National University of Kyiv, Volodymyrska str. 64/13, 01601 Kyiv (Ukraine)

    2017-06-15

    Based on the results of spectroscopy studies and electronic band structure calculations, the analysis of excitation energy transformation into luminescence is performed for a set of molybdates M{sup II}MoO{sub 4} (M{sup II}=Ca, Sr, Zn, Pb) and Li{sub 2}MoO{sub 4}. The bandgap energies were determined from comparison of experimental and calculated reflectivity spectra as 3.3 eV for PbMoO{sub 4}, 4.3 eV for ZnMoO{sub 4}, 4.4 eV for CaMoO{sub 4}, 4.7 eV for SrMoO{sub 4}, and 4.9 eV for Li{sub 2}MoO{sub 4}. It is shown that photoluminescence excitation spectra of these materials reveal the specific features of their conduction bands. The threshold of separated charge carriers’ creation is shown to be by 1.3–1.9 eV higher than the bandgap energy in CaMoO{sub 4}, SrMoO{sub 4} and ZnMoO{sub 4}. The effect is explained by the peculiarities of conduction band structure, namely to the presence of gap between the subbands of the conduction band and to the low mobility of electrons in the lower sub-band of the conduction band.

  16. Energy transfer in diatom/diatom molecular collisions

    International Nuclear Information System (INIS)

    Sohlberg, K.W.

    1992-01-01

    In a collision of two molecules, the translational energy of the collision may be redistributed into internal energy of rotation, vibration, or electron motion, in one or both of the colliding partners. In addition, internal energy in one or more of these modes may be open-quotes quenchedclose quotes into translation, leading to a superelastic collision. Such energy transfer may take place by a number of mechanisms. This energy transfer is of fundamental importance in understanding chemical reaction dynamics. Nearly all chemical reactions take place through a bimolecular collision process (or multiple bimolecular collisions) and the quantum state specificity of the reaction can have a major role in determining the kinetics of the reaction, In particular, the author has investigated vibrational energy transfer in collisions between two diatomic molecules. In addition to serving as models for all molecular collision process, gas phase collisions of these species are ubiquitous in atmospheric phenomena which are of critical importance in answering the current questions about the human induced degradation of the earth's atmospheric. Classical trajectory methods have been used to explore the excitation of vibrations in gas-phase collisions of the nitrogen molecular ion with its parent molecule. The near symmetry of the reactants is shown to result in a high probability that the two molecules are excited by an equal amount of energy. This provides a possible explanation of the molecular beam measurements which show that the total number of vibrational energy quanta excited in the collision is, with a high probability that the two molecules are excited by an equal amount of energy. This provides a possible explanation of the molecular beam measurements which show that the total number of vibrational energy quanta excited in the collision is, with a high probability, even

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

    Science.gov (United States)

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

    2012-08-21

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

  18. Dynamics of the excited state intramolecular charge transfer

    International Nuclear Information System (INIS)

    Joo, T.; Kim, C.H.

    2006-01-01

    The 6-dodecanoyl-2-dimethylaminonaphtalene (laurdan), a derivative of 6-propanoyl- 2-dimethylaminonaphthalene (prodan), has been used as a fluorescent probe in cell imaging, especially in visualizing the lipid rafts by the generalized polarization (GP) images, where GP=(I 440 -I 490 )/(I 440 +I 490 ) with I being the fluorescence intensity. The fluorescence spectrum of laurdan is sensitive to its dipolar environment due to the intramolecular charge transfer (ICT) process in S 1 state, which results in a dual emission from the locally excited (LE) and the ICT states. The ICT process and the solvation of the ICT state are very sensitive to the dipolar nature of the environment. In this work, the ICT of laurdan in ethanol has been studied by femtosecond time resolved fluorescence (TRF), especially TRF spectra measurement without the conventional spectral reconstruction method. TRF probes the excited states exclusively, a unique advantage over the pump/probe transient absorption technique, although time resolution of the TRF is generally lower than transient absorption and the TRF spectra measurement was possible only though the spectral reconstruction. Over the years, critical advances in TRF technique have been made in our group to achieve <50 fs time resolution with direct full spectra measurement capability. Detailed ICT and the subsequent solvation processes can be visualized unambiguously from the TRF spectra. Fig. 1 shows the TRF spectra of laurdan in ethanol at several time delays. Surprisingly, two bands at 433 and 476 nm are clearly visible in the TRF spectra of laurdan even at T = 0 fs. As time increases, the band at 476 nm shifts to the red while its intensity increases. The band at 433 nm also shifts slightly to the red, but loses intensity as time increases. The intensity of the 476 nm band reaches maximum at around 5 ps, where it is roughly twice as intense as that at 0 fs, and stays constant until lifetime decay is noticeable. The spectra were fit by

  19. Theoretical study of intermolecular energy transfer involving electronically excited molecules: He(/sup 1/S) + H/sub 2/(B /sup 1/. sigma. /sub u//sup +/). [Solution for coupled channel equations

    Energy Technology Data Exchange (ETDEWEB)

    Grimes, R.M.

    1986-11-01

    To further understanding of gas phase collision dynamics involving electronically-excited molecules, a fully quantum mechanical study of He + H/sub 2/(B /sup 1/..sigma../sub u//sup +/) was undertaken. Iterative natural orbital configuration interaction (CI) calculations were performed to obtain the interaction potential between He and H/sub 2/(B /sup 1/..sigma../sub u//sup +/). The potential energy surface (PES) is highly anisotropic and has a van der Waals well of about 0.03 eV for C/sub 2v/ approach. Avoided PES crossings occur with He + H/sub 2/(E,F /sup 1/..sigma../sub g//sup +/) and with He + H/sub 2/(X /sup 1/..sigma../sub g//sup +/) and cause a local maximum and a deep minimum in the He + H/sub 2/(B /sup 1/..sigma../sub u//sup +/) PES, respectively. The crossing with He + H/sub 2/(X /sup 1/..sigma../sub g//sup +/) provides a mechanism for fluorescence quenching. The computed CI energies were combined with previous multi-reference double excitation CI calculations and fit with analytic functions for convenience in scattering calculations. Accurate dipole polarizabilities and quadrupole moment of H/sub 2/(B /sup 1/..sigma../sub u//sup +/) were computed for use in the multipole expansion, which is the analytic form of the long-range PES. 129 refs., 28 figs., 35 tabs.

  20. The structure of nuclear states at low, intermediate and high excitation energies

    International Nuclear Information System (INIS)

    Soloviev, V.G.

    1976-01-01

    It is shown that within the model based on the quasiparticle-phonon interaction one can obtain the description of few-quasiparticle components of nuclear states at low, intermediate and high excitation energies. For the low-lying states the energy of each level is calculated. The few-quasiparticle components at intermediate and high excitation energies are represented to be averaged in certain energy intervals and their characteri stics are given as the corresponding strength functions. The fragmentation of single-particle states in deformed nuclei is studied. It is shown that in the distribution of the single-particle strength alongside with a large maximum there appear local maxima and the distribution itself has a long tail. The dependence of neutron strength functions on the excitation energy is investigated for the transfer reaction of the type (d,p) and (d,t). The s,- p,- and d-wave neutron strength functions are calculated at the neutron binding energy Bn. A satisfactory agreement with experiment is obtained. The energies and Elambda-strength functions for giant multipole resonances in deformed nuclei are calculated. The energies of giant quadrupole and octupole resonances are calculated. Their widths and fine structure are being studied. It is stated that to study the structure of highly excited states it is necessary to find the values of many-quasiparticle components of the wave functions. The ways of experimental determination of these components based on the study of γ-transitions between highly excited states are discussed

  1. Theoretical Insights Into the Excited State Double Proton Transfer Mechanism of Deep Red Pigment Alkannin.

    Science.gov (United States)

    Zhao, Jinfeng; Dong, Hao; Zheng, Yujun

    2018-02-08

    As the most important component of deep red pigments, alkannin is investigated theoretically in detail based on time-dependent density functional theory (TDDFT) method. Exploring the dual intramolecular hydrogen bonds (O1-H2···O3 and O4-H5···O6) of alkannin, we confirm the O1-H2···O3 may play a more important role in the first excited state than the O4-H5···O6 one. Infrared (IR) vibrational analyses and subsequent charge redistribution also support this viewpoint. Via constructing the S 1 -state potential energy surface (PES) and searching transition state (TS) structures, we illuminate the excited state double proton transfer (ESDPT) mechanism of alkannin is the stepwise process that can be first launched by the O1-H2···O3 hydrogen bond wire in gas state, acetonitrile (CH 3 CN) and cyclohexane (CYH) solvents. We present a novel mechanism that polar aprotic solvents can contribute to the first-step proton transfer (PT) process in the S 1 state, and nonpolar solvents play important roles in lowering the potential energy barrier of the second-step PT reaction.

  2. Ab initio study on electron excitation and electron transfer in tryptophan-tyrosine system

    International Nuclear Information System (INIS)

    Tong Jing; Li Xiangyuan

    2002-01-01

    In this article, ab initio calculation has been performed to evaluate the transition energy of electronic excitation in tryptophan and tyrosine by using semiempirical molecular orbital method AM1 and complete active space self-consistent field method. The solvent effect has been considered by means of the conductor-like screening model. After geometric optimizations of isolated tryptophan and tyrosine, and their corresponding radicals and cations, reaction heat of these electron transfer reactions have been obtained by the means of complete active space self-consistent field method. The transition energies from the ground state, respectively, to the lowest excited state and to the lowest triplet state of these two amino acids are also calculated and compared with the experimentally observed values. The ionization potential and electron affinity are also calculated for tryptophan and tyrosine employing Koopmans' theorem and ab initio calculation. Compared with the experimental measurements, the theoretical results are found satisfactory. Theoretical results give good explanations on the experimental phenomena that N 3 · can preferably oxide the side chain of tryptophan residue and then the electron transfer from tyrosine residue to tryptophan residue follows in peptides involving tryptophan and tyrosine

  3. An estimate of spherical impactor energy transfer for mechanical frequency up-conversion energy harvester

    Directory of Open Access Journals (Sweden)

    L. R. Corr

    2016-08-01

    Full Text Available Vibration energy harvesters, which use the impact mechanical frequency up-conversion technique, utilize an impactor, which gains kinetic energy from low frequency ambient environmental vibrations, to excite high frequency systems that efficiently convert mechanical energy to electrical energy. To take full advantage of the impact mechanical frequency up-conversion technique, it is prudent to understand the energy transfer from the low frequency excitations, to the impactor, and finally to the high frequency systems. In this work, the energy transfer from a spherical impactor to a multi degree of freedom spring / mass system, due to Hertzian impact, is investigated to gain insight on how best to design impact mechanical frequency up-conversion energy harvesters. Through this academic work, it is shown that the properties of the contact (or impact area, i.e., radius of curvature and material properties, only play a minor role in energy transfer and that the equivalent mass of the target system (i.e., the spring / mass system dictates the total amount of energy transferred during the impact. The novel approach of utilizing the well-known Hertzian impact methodology to gain an understanding of impact mechanical frequency up-conversion energy harvesters has made it clear that the impactor and the high frequency energy generating systems must be designed together as one system to ensure maximum energy transfer, leading to efficient ambient vibration energy harvesters.

  4. Design and development of a parametrically excited nonlinear energy harvester

    International Nuclear Information System (INIS)

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

    2016-01-01

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

  5. Photo- and radiation chemical studies of intermediates involved in excited-state electron-transfer reactions

    International Nuclear Information System (INIS)

    Hoffman, M.Z.

    1985-01-01

    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 H 2 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 MV 2+ , 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 MV 2+ with rate constants of 2.8 x 10 9 , 7.6 x 10 9 , and 8.5 x 10 6 M -1 s -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

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

    International Nuclear Information System (INIS)

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

    1987-01-01

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

  7. Energy-optimal electrical excitation of nerve fibers.

    Science.gov (United States)

    Jezernik, Saso; Morari, Manfred

    2005-04-01

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

  8. Excited state intramolecular charge transfer reaction in 4-(1 ...

    Indian Academy of Sciences (India)

    Administrator

    cal reactions to the determination of paleotempera- tures from isotopic ... ordered liquid than H2O due to stronger H-bond in- teractions in the deuterated water ... layer chromatography and monitoring the excitation wavelength dependence of ...

  9. Rotational energy transfer of the A{sup 2}{Sigma}`({nu}`=1) state of OH

    Energy Technology Data Exchange (ETDEWEB)

    Beaud, P; Radi, P; Frey, H B; Mischler, B; Tzannis, A P; Gerber, T [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

    1997-06-01

    Spectrally and temporally resolved laser excited fluorescence of OH is investigated in the picosecond time domain. The total rotational energy transfer (RET) rate from the excited state is determined from the experimental data. Simulated spectra obtained by modelling RET with the energy corrected sudden approximation agree well with the measured spectra. (author) 1 fig., 1 tab., 5 refs.

  10. Energy transfer in porous anodic alumina/rhodamine 110 nanocomposites

    Energy Technology Data Exchange (ETDEWEB)

    Elhouichet, H., E-mail: habib.elhouichet@fst.rnu.tn [Laboratoire de Physico-Chimie des Materiaux Mineraux et leurs Applications, Centre National de Recherches en Sciences des Materiaux, B.P. 95, Hammam-Lif 2050 (Tunisia); Departement de Physique, Faculte des Sciences de Tunis, University of Tunis Elmanar 2092 Tunis (Tunisia); Harima, N.; Koyama, H. [Hyogo University of Teacher Education, Kato, Hyogo 673-1494 (Japan); Gaponenko, N.V. [Belarusian State University of Informatics and Radioelectronics, P. Browki St. 6, 220013 Minsk (Belarus)

    2012-09-15

    We have used porous anodic alumina (PAA) films as templates for embedding rhodamine 110 (Rh110) molecules and examined their photoluminescence (PL) properties in detail. The analysis of the polarization memory (PM) of PL strongly suggests that there is a significant energy transfer from PAA to Rh110 molecules. The effect of annealing the PAA layer on the PL properties of the nanocomposite has been studied. The results show that the energy transfer becomes more efficient in annealed PAA. - Highlights: Black-Right-Pointing-Pointer Porous anodic alumina-rhodamine 110 nanocomposites are elaborated. Black-Right-Pointing-Pointer Efficient energy transfer from the host to Rh110 molecules is evidenced from measurements of photoluminescence and degree of polarization memory spectra. Black-Right-Pointing-Pointer Thermal annealing of porous anodic alumina can improve the process of excitation transfer.

  11. Long range energy transfer in graphene hybrid structures

    International Nuclear Information System (INIS)

    Gonçalves, Hugo; Bernardo, César; Moura, Cacilda; Belsley, Michael; Schellenberg, Peter; Ferreira, R A S; André, P S; Stauber, Tobias

    2016-01-01

    In this work we quantify the distance dependence for the extraction of energy from excited chromophores by a single layer graphene flake over a large separation range. To this end hybrid structures were prepared, consisting of a thin (2 nm) layer of a polymer matrix doped with a well chosen strongly fluorescent organic molecule, followed by an un-doped spacer layer of well-defined thicknesses made of the same polymer material and an underlying single layer of pristine, undoped graphene. The coupling strength is assessed through the variation of the fluorescence decay kinetics as a function of distance between the graphene and the excited chromophore molecules. Non-radiative energy transfer to the graphene was observed at distances of up to 60 nm; a range much greater than typical energy transfer distances observed in molecular systems. (paper)

  12. Direct observation of triplet energy transfer from semiconductor nanocrystals.

    Science.gov (United States)

    Mongin, Cédric; Garakyaraghi, Sofia; Razgoniaeva, Natalia; Zamkov, Mikhail; Castellano, Felix N

    2016-01-22

    Triplet excitons are pervasive in both organic and inorganic semiconductors but generally remain confined to the material in which they originate. We demonstrated by transient absorption spectroscopy that cadmium selenide semiconductor nanoparticles, selectively excited by green light, engage in interfacial Dexter-like triplet-triplet energy transfer with surface-anchored polyaromatic carboxylic acid acceptors, extending the excited-state lifetime by six orders of magnitude. Net triplet energy transfer also occurs from surface acceptors to freely diffusing molecular solutes, further extending the lifetime while sensitizing singlet oxygen in an aerated solution. The successful translation of triplet excitons from semiconductor nanoparticles to the bulk solution implies that such materials are generally effective surrogates for molecular triplets. The nanoparticles could thereby potentially sensitize a range of chemical transformations that are relevant for fields as diverse as optoelectronics, solar energy conversion, and photobiology. Copyright © 2016, American Association for the Advancement of Science.

  13. Bimolecular Excited-State Electron Transfer with Surprisingly Long-Lived Radical Ions

    KAUST Repository

    Alsam, Amani Abdu

    2015-09-02

    We explored the excited-state interactions of bimolecular, non-covalent systems consisting of cationic poly[(9,9-di(3,3’-N,N’-trimethyl-ammonium) propyl fluorenyl-2,7-diyl)-alt-co-(9,9-dioctyl-fluorenyl-2,7-diyl)] diiodide salt (PFN) and 1,4-dicyanobenzene (DCB) using steady-state and time-resolved techniques, including femto- and nanosecond transient absorption and femtosecond infrared spectroscopies with broadband capabilities. The experimental results demonstrated that photo-induced electron transfer from PFN to DCB occurs on the picosecond time scale, leading to the formation of PFN+• and DCB-• radical ions. Interestingly, real-time observations of the vibrational marker modes on the acceptor side provided direct evidence and insight into the electron transfer process indirectly inferred from UV-Vis experiments. The band narrowing on the picosecond time scale observed on the antisymmetric C-N stretching vibration of the DCB radical anion provides clear experimental evidence that a substantial part of the excess energy is channeled into vibrational modes of the electron transfer product and that the geminate ion pairs dissociate. More importantly, our nanosecond time-resolved data indicate that the charge-separated state is very long lived ( 30 ns) due to the dissociation of the contact radical ion pair into free ions. Finally, the fast electron transfer and slow charge recombination anticipate the current donor−acceptor system with potential applications in organic solar cells.

  14. Bimolecular Excited-State Electron Transfer with Surprisingly Long-Lived Radical Ions

    KAUST Repository

    Alsam, Amani Abdu; Aly, Shawkat Mohammede; Usman, Anwar; Parida, Manas R.; Del Gobbo, Silvano; Alarousu, Erkki; Mohammed, Omar F.

    2015-01-01

    We explored the excited-state interactions of bimolecular, non-covalent systems consisting of cationic poly[(9,9-di(3,3’-N,N’-trimethyl-ammonium) propyl fluorenyl-2,7-diyl)-alt-co-(9,9-dioctyl-fluorenyl-2,7-diyl)] diiodide salt (PFN) and 1,4-dicyanobenzene (DCB) using steady-state and time-resolved techniques, including femto- and nanosecond transient absorption and femtosecond infrared spectroscopies with broadband capabilities. The experimental results demonstrated that photo-induced electron transfer from PFN to DCB occurs on the picosecond time scale, leading to the formation of PFN+• and DCB-• radical ions. Interestingly, real-time observations of the vibrational marker modes on the acceptor side provided direct evidence and insight into the electron transfer process indirectly inferred from UV-Vis experiments. The band narrowing on the picosecond time scale observed on the antisymmetric C-N stretching vibration of the DCB radical anion provides clear experimental evidence that a substantial part of the excess energy is channeled into vibrational modes of the electron transfer product and that the geminate ion pairs dissociate. More importantly, our nanosecond time-resolved data indicate that the charge-separated state is very long lived ( 30 ns) due to the dissociation of the contact radical ion pair into free ions. Finally, the fast electron transfer and slow charge recombination anticipate the current donor−acceptor system with potential applications in organic solar cells.

  15. Theory of Excitation Transfer between Two-Dimensional Semiconductor and Molecular Layers

    Science.gov (United States)

    Specht, Judith F.; Verdenhalven, Eike; Bieniek, Björn; Rinke, Patrick; Knorr, Andreas; Richter, Marten

    2018-04-01

    The geometry-dependent energy transfer rate from an electrically pumped inorganic semiconductor quantum well into an organic molecular layer is studied theoretically. We focus on Förster-type nonradiative excitation transfer between the organic and inorganic layers and include quasimomentum conservation and intermolecular coupling between the molecules in the organic film. (Transition) partial charges calculated from density-functional theory are used to calculate the coupling elements. The partial charges describe the spatial charge distribution and go beyond the common dipole-dipole interaction. We find that the transfer rates are highly sensitive to variations in the geometry of the hybrid inorganic-organic system. For instance, the transfer efficiency is improved by up to 2 orders of magnitude by tuning the spatial arrangement of the molecules on the surface: Parameters of importance are the molecular packing density along the effective molecular dipole axis and the distance between the molecules and the surface. We also observe that the device performance strongly depends on the orientation of the molecular dipole moments relative to the substrate dipole moments determined by the inorganic crystal structure. Moreover, the operating regime is identified where inscattering dominates over unwanted backscattering from the molecular layer into the substrate.

  16. Ultrasound acoustic wave energy transfer and harvesting

    Science.gov (United States)

    Shahab, Shima; Leadenham, Stephen; Guillot, François; Sabra, Karim; Erturk, Alper

    2014-04-01

    This paper investigates low-power electricity generation from ultrasound acoustic wave energy transfer combined with piezoelectric energy harvesting for wireless applications ranging from medical implants to naval sensor systems. The focus is placed on an underwater system that consists of a pulsating source for spherical wave generation and a harvester connected to an external resistive load for quantifying the electrical power output. An analytical electro-acoustic model is developed to relate the source strength to the electrical power output of the harvester located at a specific distance from the source. The model couples the energy harvester dynamics (piezoelectric device and electrical load) with the source strength through the acoustic-structure interaction at the harvester-fluid interface. Case studies are given for a detailed understanding of the coupled system dynamics under various conditions. Specifically the relationship between the electrical power output and system parameters, such as the distance of the harvester from the source, dimensions of the harvester, level of source strength, and electrical load resistance are explored. Sensitivity of the electrical power output to the excitation frequency in the neighborhood of the harvester's underwater resonance frequency is also reported.

  17. Ni-Ni ion pair excitation transfer in D sub(3h) symmetry

    International Nuclear Information System (INIS)

    Terrile, M.C.

    1990-01-01

    The mechanisms contributing to excitation transfer are examined for Ni-Ni ion pairs in order to explain the delocalized character of electronic excitations observed in CsNiF sub(3). Using both first-and second-order perturbation theory and from symmetry arguments, the kind of interactions giving matrix elements between states connecting different sites for the position of the excitation are discussed. (author)

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

    International Nuclear Information System (INIS)

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

    2012-01-01

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

  19. Electromechanical capacitor for energy transfer

    International Nuclear Information System (INIS)

    Carroll, T.A.; Chowdhuri, P.; Marshall, J.

    1983-01-01

    Inductive energy transfer between two magnets can be achieved with almost 100% efficiency with a transfer capacitor. However, the bulk and cost will be high, and reliability low if conventional capacitors are used. A homopolar machine, used as a capacitor, will be compact and economical. A homopolar machine was designed with counter-rotating copper disks completely immersed in a liquid metal (NaK-78) to work as a pulse capacitor. Absence of solid-brush collectors minimized wear and frictional losses. Wetting of the copper disks throughout the periphery by the liquid metal minimized the resistive losses at the collector interface. A liquid-metal collector would, however, introduce hydrodynamic and magnetohydrodynamic losses. The selected liquid metal, e.g., NaK-78 will produce the lowest of such losses among the available liquid metals. An electromechanical capacitor of this design was tested at various dc magnetic fields. Its measured capacitance was about 100 farads at a dc magnetic field of 1.15 tesla

  20. Vibration transfers to measure the performance of vibration isolated platforms on site using background noise excitation

    NARCIS (Netherlands)

    Segerink, Franciscus B.; Korterik, Jeroen P.; Offerhaus, Herman L.

    2011-01-01

    This article demonstrates a quick and easy way of quantifying the performance of a vibration-isolated platform. We measure the vibration transfer from floor to table using background noise excitation from the floor. As no excitation device is needed, our setup only requires two identical sensors (in

  1. Energy transfer dynamics in Light-Harvesting Dendrimers

    Science.gov (United States)

    Melinger, Joseph S.; McMorrow, Dale; Kleiman, Valeria D.

    2002-03-01

    We explore energy transfer dynamics in light-harvesting phenylacetylene symmetric and asymmetric dendrimers. Femtosecond pump-probe spectroscopy is used to probe the ultrafast dynamics of electronic excitations in these dendrimers. The backbone of the macromolecule consists of branches of increasing conjugation length, creating an energy gradient, which funnels energy to an accepting perylene trap. In the case of the symmetric dendrimer (nanostar), the energy transfer efficiency is known to approach nearly unity, although the nature and timescale of the energy transfer process is still unknown. For the asymmetric dendrimers, energy transfer efficiencies are very high, with the possibility of more complex transfer processes. We experimentally monitor the transport of excitons through the light-harvesting dendrimer. The transients show a number of components, with timescales ranging from <300fs to several tens of picoseconds, revealing the complex photophysics taking place in these macromolecules. We interpret our results in terms of the Förster mechanism in which energy transfer occurs through dipole-dipole interactions.

  2. Modeling the efficiency of Förster resonant energy transfer from energy relay dyes in dye-sensitized solar cells

    KAUST Repository

    Hoke, Eric T.

    2010-02-11

    Förster resonant energy transfer can improve the spectral breadth, absorption and energy conversion efficiency of dye sensitized solar cells. In this design, unattached relay dyes absorb the high energy photons and transfer the excitation to sensitizing dye molecules by Förster resonant energy transfer. We use an analytic theory to calculate the excitation transfer efficiency from the relay dye to the sensitizing dye accounting for dynamic quenching and relay dye diffusion. We present calculations for pores of cylindrical and spherical geometry and examine the effects of the Förster radius, the pore size, sensitizing dye surface concentration, collisional quenching rate, and relay dye lifetime. We find that the excitation transfer efficiency can easily exceed 90% for appropriately chosen dyes and propose two different strategies for selecting dyes to achieve record power conversion efficiencies. © 2010 Optical Society of America.

  3. Ultrafast Dynamics of Dansylated POPAM Dendrimers and Energy Transfer in their Dye Complexes

    Science.gov (United States)

    Aumanen, J.; Kesti, T.; Sundström, V.; Vögtle, F.; Korppi-Tommola, J.

    We have studied internal dynamics of dansylated poly(propyleneamine) dendrimers of different generations in solution and excitation energy transfer from dansyl chromophores to xanthene dyes that form van der Waals complexes with the dendrimers

  4. Excited state intramolecular charge transfer reaction in non-aqueous ...

    Indian Academy of Sciences (India)

    polar phase and thus leading to less swelling of reverse .... ues were restricted up to the limit at which no phase separation was ..... The lower panel of figure 1 also indicates that the slopes of ... probe in its ground and excited states.55.

  5. Ab initio study of the excited-state coupled electron-proton-transfer process in the 2-aminopyridine dimer

    International Nuclear Information System (INIS)

    Sobolewski, Andrzej L.; Domcke, Wolfgang

    2003-01-01

    The low-lying 1 ππ* excited states of the 2-aminopyridine dimer have been investigated with multi-reference ab initio methods (CASSCF and MRMP2). The 2-aminopyridine dimer can be considered as a mimetic model of Watson-Crick DNA base pairs. The reaction path and the energy profile for single proton transfer in the lowest 1 ππ* inter-monomer charge-transfer state have been obtained. A weakly avoided crossing of the 1 ππ* surface with the electronic ground-state surface has been found near the single-proton-transfer minimum of the 1 ππ* surface. From the splitting of the adiabatic surfaces at the avoided crossing, an internal-conversion lifetime of the excited state of <100 ps has been estimated. The potential relevance of these results for the rationalization of radiation-induced mutations and the photostability of the genetic code is briefly discussed

  6. Range-separated density-functional theory for molecular excitation energies

    International Nuclear Information System (INIS)

    Rebolini, E.

    2014-01-01

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

  7. Energy transfer to xanthene dyes in dansylated POPAM dendrimers

    Science.gov (United States)

    Aumanen, Jukka; Korppi-Tommola, Jouko

    2011-12-01

    Excitation energy transfer (EET) in host-guest complexes of dansylated POPAM dendrimers and xanthene dyes have been studied by transient absorption spectroscopy. EET from dansyl periphery to guests: rose bengal, eosin, or fluorescein, showed non-exponential behaviour as a result of distribution of donor-acceptor distances. Time constants range from 100 fs to 8 ps, independent of the dye and the dendrimer generation. Experiments suggested that in dendrimers binding more than one guest, EET among the guests becomes effective. Guest-host and guest-guest interactions induce non-radiative relaxation channels making excitation decays of the guests clearly faster in complexes than in solution.

  8. Comparative study on contribution of charge-transfer collision to excitations of iron ion between argon radio-frequency inductively-coupled plasma and nitrogen microwave induced plasma

    Energy Technology Data Exchange (ETDEWEB)

    Satoh, Kozue; Wagatsuma, Kazuaki, E-mail: wagatuma@imr.tohoku.ac.jp

    2015-06-01

    This paper describes an ionization/excitation phenomenon of singly-ionized iron occurring in an Okamoto-cavity microwave induced plasma (MIP) as well as an argon radio-frequency inductively-coupled plasma (ICP), by comparing the Boltzmann distribution among iron ionic lines (Fe II) having a wide range of the excitation energy from 4.76 to 9.01 eV. It indicated in both the plasmas that plots of Fe II lines having lower excitation energies (4.76 to 5.88 eV) were fitted on each linear relationship, implying that their excitations were caused by a dominant thermal process such as collision with energetic electron. However, Fe II lines having higher excitation energies (more than 7.55 eV) had a different behavior from each other. In the ICP, Boltzmann plots of Fe II lines assigned to the higher excited levels also followed the normal Boltzmann relationship among the low-lying excited levels, even including a deviation from it in particular excited levels having an excitation energy of ca. 7.8 eV. This deviation can be attributed to a charge-transfer collision with argon ion, which results in the overpopulation of these excited levels, but the contribution is small. On the other hand, the distribution of the high-lying excited levels was non-thermal in the Okamoto-cavity MIP, which did not follow the normal Boltzmann relationship among the low-lying excited levels. A probable reason for the non-thermal characteristics in the MIP is that a charge-transfer collision with nitrogen molecule ion having many vibrational/rotational levels could work for populating the 3d{sup 6}4p (3d{sup 5}4s4p) excited levels of iron ion broadly over an energy range of 7.6–9.0 eV, while collisional excitation by energetic electron would occur insufficiently to excite these high-energy levels. - Highlights: • This paper describes the excitation mechanism of iron ion in Okamoto-cavity MIP in comparison with conventional ICP. • Boltzmann distribution is studied among iron ionic lines of

  9. Realistic level densities in fragment emission at high excitation energies

    International Nuclear Information System (INIS)

    Mustafa, M.G.; Blann, M.; Ignatyuk, A.V.

    1993-01-01

    Heavy fragment emission from a 44 100 Ru compound nucleus at 400 and 800 MeV of excitation is analyzed to study the influence of level density models on final yields. An approach is used in which only quasibound shell-model levels are included in calculating level densities. We also test the traditional Fermi gas model for which there is no upper energy limit to the single particle levels. We compare the influence of these two level density models in evaporation calculations of primary fragment excitations, kinetic energies and yields, and on final product yields

  10. Insights into the energy transfer mechanism in Ce3+-Yb3+ codoped YAG phosphors

    NARCIS (Netherlands)

    Yu, D. C.; Rabouw, F. T.|info:eu-repo/dai/nl/413318036; Boon, W. Q.; Kieboom, T.; Ye, S.; Zhang, Q. Y.; Meijerink, A.|info:eu-repo/dai/nl/075044986

    2014-01-01

    Two distinct energy transfer (ET) mechanisms have been proposed for the conversion of blue to near-infrared (NIR) photons in YAG:Ce3+,Yb3+. The first mechanism involves downconversion by cooperative energy transfer, which would yield two NIR photons for each blue photon excitation. The second

  11. Energies and lifetimes of excited states in copperlike Kr VIII

    International Nuclear Information System (INIS)

    Livingston, A.E.; Curtis, L.J.; Schectman, R.M.; Berry, H.G.

    1980-01-01

    The spectrum of Kr VIII has been observed between 180 and 2000 A by using foil excitation of 2.5--3.5-MeV krypton ions. Twenty new transitions have been classified and eleven new excited-state energies have been determined within the n=4 --7 shells. The ionization potential is derived to be 1 015 800 +- 200 cm -1 . The excited-state energies and fine structures are compared with recent relativistic Hartree-Fock calculations. The 4p-state lifetime has been measured by performing a simultaneous analysis of decay data for the 4p level and for its dominant cascade-repopulating levels. The 4p lifetime is found to be 30% shorter than previously measured values and is in excellent agreement with the result of a recent multiconfiguration Hartree-Fock calculation. The source of the discrepancy between this result and earlier measurements is discussed

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

    Science.gov (United States)

    Chang, Xue-Ping; Fang, Qiu; Cui, Ganglong

    2014-10-01

    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.

  13. Long-wave UVA radiation excited warm white-light emitting NaGdTiO{sub 4}: Tm{sup 3+}/Dy{sup 3+}/Eu{sup 3+} ions tri-doped phosphors: Synthesis, energy transfer and color tunable properties

    Energy Technology Data Exchange (ETDEWEB)

    Bharat, L. Krishna; Du, Peng; Yu, Jae Su, E-mail: jsyu@khu.ac.kr

    2016-05-05

    NaGdTiO{sub 4} (NGT) phosphors doped with different activator ions (Tm{sup 3+}, Dy{sup 3+}, and Eu{sup 3+}) were synthesized by a conventional solid-state reaction method in an ambient atmosphere. These phosphors were characterized by scanning electron microscope images, transmission electron microscope images, X-ray diffraction patterns, Fourier transform infrared spectra, and photoluminescence spectra. All the samples were crystallized in an orthorhombic phase with a space group of Pbcm (57). In Tm{sup 3+}/Dy{sup 3+} ions co-doped samples, white-light emission was observed under near-ultraviolet (NUV) excitation. In addition, the energy transfer between Tm{sup 3+} and Dy{sup 3+} ions was proved to be a resonant type via an electric dipole–dipole mechanism and the critical distance of energy transfer was calculated to be 19.91 Å. Furthermore, Tm{sup 3+}/Dy{sup 3+}/Eu{sup 3+} ions tri-doped NGT phosphors demonstrated warm white-light emission by appropriately tuning the activator content, based on the principle of energy transfer. These NUV wavelength excitable phosphors exhibit great potential as a single-phase full-color emitting phosphor for white light-emitting diode applications. - Highlights: • The pebble shaped NaGdTiO{sub 4} particles were prepared by solid-state reaction method. • Tm{sup 3+} and Dy{sup 3+} single doping gives respective blue and cool white light emission. • The Tm{sup 3+}/Dy{sup 3+} ions co-doped samples give CIE values near to standard white light. • Addition of Eu{sup 3+} ions shifts the CIE values towards warm white light region. • This single phase white light emitting phosphors have lower CCT values (<5000 K).

  14. Molding resonant energy transfer by colloidal crystal: Dexter transfer and electroluminescence

    Science.gov (United States)

    González-Urbina, Luis; Kolaric, Branko; Libaers, Wim; Clays, Koen

    2010-05-01

    Building photonic crystals by combination of colloidal ordering and metal sputtering we were able to construct a system sensitive to an electrical field. In corresponding crystals we embedded the Dexter pair (Ir(ppy3) and BAlq) and investigated the influence of the band gap on the resonant energy transfer when the system is excited by light and by an electric field respectively. Our investigations extend applications of photonic crystals into the field of electroluminescence and LED technologies.

  15. Frenkel and Charge-Transfer Excitations in Donor-acceptor Complexes from Many-Body Green's Functions Theory.

    Science.gov (United States)

    Baumeier, Björn; Andrienko, Denis; Rohlfing, Michael

    2012-08-14

    Excited states of donor-acceptor dimers are studied using many-body Green's functions theory within the GW approximation and the Bethe-Salpeter equation. For a series of prototypical small-molecule based pairs, this method predicts energies of local Frenkel and intermolecular charge-transfer excitations with the accuracy of tens of meV. Application to larger systems is possible and allowed us to analyze energy levels and binding energies of excitons in representative dimers of dicyanovinyl-substituted quarterthiophene and fullerene, a donor-acceptor pair used in state of the art organic solar cells. In these dimers, the transition from Frenkel to charge transfer excitons is endothermic and the binding energy of charge transfer excitons is still of the order of 1.5-2 eV. Hence, even such an accurate dimer-based description does not yield internal energetics favorable for the generation of free charges either by thermal energy or an external electric field. These results confirm that, for qualitative predictions of solar cell functionality, accounting for the explicit molecular environment is as important as the accurate knowledge of internal dimer energies.

  16. Collisional excitation transfer between Rb(5P) states in 50–3000 Torr of 4He

    International Nuclear Information System (INIS)

    Sell, J F; Gearba, M A; Patterson, B M; Byrne, D; Jemo, G; Meeter, R; Knize, R J; Lilly, T C

    2012-01-01

    Measurements of the mixing rates and cross sections for collisional excitation transfer between the 5P 1/2 and 5P 3/2 states of rubidium (Rb) in the presence of 4 He buffer gas are presented. Selected pulses from a high repetition rate, mode-locked femtosecond laser are used to excite either Rb state with the fluorescence due to collisional excitation transfer observed by time-correlated single-photon counting. The time dependence of this fluorescence is fitted to the solution of rate equations which include the mixing rate, atomic lifetimes and any quenching processes. The variation in the mixing rate over a large range of buffer gas densities allows the determination of both the binary collisional transfer cross section and a three-body collisional transfer rate. We do not observe any collisional quenching effects at 4 He pressures up to 6 atm and discuss in detail other systematic effects considered in the experiment. (paper)

  17. Complex fragment emission at low and high excitation energy

    International Nuclear Information System (INIS)

    Moretto, L.G.

    1986-08-01

    Complex fragment emission has been certified as a compound nucleus process at low energies. An extension of the measurements to heavy ion reactions up to 50 MeV/u shows that most complex fragments are emitted by highly excited compound nuclei formed in incomplete fusion reactions. 12 refs., 26 figs

  18. El strength function at high spin and excitation energy

    International Nuclear Information System (INIS)

    Barrette, J.

    1983-04-01

    Recently giant dipole resonance-like concentration of the dipole strength function in nuclei was observed at both high excitation energies and high spins. This observation raises the possibility of obtaining new information on the shape of rapidly rotating heated nuclei. Recent experimental results on this subject are reviewed

  19. Novel DNA sequence detection method based on fluorescence energy transfer

    International Nuclear Information System (INIS)

    Kobayashi, S.; Tamiya, E.; Karube, I.

    1987-01-01

    Recently the detection of specific DNA sequence, DNA analysis, has been becoming more important for diagnosis of viral genomes causing infections disease and human sequences related to inherited disorders. These methods typically involve electrophoresis, the immobilization of DNA on a solid support, hybridization to a complementary probe, the detection using labeled with /sup 32/P or nonisotopically with a biotin-avidin-enzyme system, and so on. These techniques are highly effective, but they are very time-consuming and expensive. A principle of fluorescene energy transfer is that the light energy from an excited donor (fluorophore) is transferred to an acceptor (fluorophore), if the acceptor exists in the vicinity of the donor and the excitation spectrum of donor overlaps the emission spectrum of acceptor. In this study, the fluorescence energy transfer was applied to the detection of specific DNA sequence using the hybridization method. The analyte, single-stranded DNA labeled with the donor fluorophore is hybridized to a probe DNA labeled with the acceptor. Because of the complementary DNA duplex formation, two fluorophores became to be closed to each other, and the fluorescence energy transfer was occurred

  20. Measurements of vibrational excitation of N2, CO, and NO by low energy proton impact

    International Nuclear Information System (INIS)

    Krutein, J.; Linder, F.

    1979-01-01

    Differential scattering experiments are reported for proton impact on N 2 , CO, and NO in the energy range E/sub lab/=30--80 eV. The measurements include the range of very small scattering angles around 0 0 as well as the rainbow region. The vibrationally resolved energy-loss spectra show a relatively low vibrational inelasticity for all three systems. Differential cross sections, transition probabilities, and the mean vibrational energy transfer are presented. Rotational excitation is indicated by the broadening of the energy-loss peaks which is most significant for H + --NO. The small-angle scattering data for vibrational excitation in CO show good agreement with the impact parameter theory using the known long-range interactions for this system

  1. Mott transition: Low-energy excitations and superconductivity

    International Nuclear Information System (INIS)

    Ioffe, L.B.; Larkin, A.I.

    1988-09-01

    It is possible that metal-dielectric transition does not result in changes of magnetic or crystallographic symmetry. In this case a fermionic spectrum is not changed at the transition, but additional low-energy excitations appear which can be described as a gauge field that has the same symmetry as an electromagnetic one. In the case of a non half-filled band gapless scalar Bose excitations also appear. Due to the presence of additional gauge field the physical conductivity is determined by the lowest conductivity of the Fermi or Bose subsystems. (author). 11 refs

  2. Energy transfer mechanism between manganese and neodymium

    Energy Technology Data Exchange (ETDEWEB)

    Kumar, R [Department of Physics, Government Raza Post-Graduate College, Rampur 244901, U.P., India

    1977-01-01

    The mechanism of energy transfer between Mn/sup 2 +/ ..-->.. Nd/sup 3 +/ in barium borate glass has been investigated. The change in emission intensities and lifetimes of Mn/sup 2 +/ (donor) due to the presence of Nd/sup 3 +/ (acceptor) are observed. It has been concluded that the mechanism of energy transfer involves a nonradiative resonance process. The electrostatic multiple interaction responsible for the transfer is dipole-dipole in nature.

  3. Quantum electrodynamics of resonant energy transfer in condensed matter

    International Nuclear Information System (INIS)

    Juzeliunas, G.; Andrews, D.L.

    1994-01-01

    A microscopic many-body QED theory for dipole-dipole resonance energy transfer has been developed from first principles. A distinctive feature of the theory is full incorporation of the dielectric effects of the supporting medium. The approach employs the concept of bath polaritons mediating the energy transfer. The transfer rate is derived in terms of the Green's operator corresponding to the polariton matrix Hamiltonian. In contrast to the more common lossless polariton models, the present theory accommodates an arbitrary number of energy levels for each molecule of the medium. This includes, a case of special interest, where the excitation energy spectrum of the bath molecules is sufficiently dense that it can be treated as a quasicontinuum in the energy region in question, as in the condensed phase normally results from homogeneous and inhomogeneous line broadening. In such a situation, the photon ''dressed'' by the medium polarization (the polariton) acquires a finite lifetime, the role of the dissipative subsystem being played by bath molecules. It is this which leads to the appearance of the exponential decay factor in the microscopically derived pair transfer rates. Accordingly, the problem associated with potentially infinite total ensemble rates, due to the divergent R -2 contribution, is solved from first principles. In addition, the medium modifies the distance dependence of the energy transfer function A(R) and also produces extra modifications due to screening contributions and local field effects. The formalism addresses cases where the surrounding medium is either absorbing or lossless over the range of energies transferred. In the latter case the exponential factor does not appear and the dielectric medium effect in the near zone reduces to that which is familiar from the theory of radiationless (Foerster) energy transfer

  4. Interactive Joint Transfer of Energy and Information

    DEFF Research Database (Denmark)

    Popovski, Petar; Fouladgar, A. M.; Simeone, Osvaldo

    2013-01-01

    In some communication networks, such as passive RFID systems, the energy used to transfer information between a sender and a recipient can be reused for successive communication tasks. In fact, from known results in physics, any system that exchanges information via the transfer of given physical...... key design insights. Index Terms— Two-way channel, interactive communication, energy transfer, energy harvesting....... resources, such as radio waves, particles and qubits, can conceivably reuse, at least part, of the received resources. This paper aims at illustrating some of the new challenges that arise in the design of communication networks in which the signals exchanged by the nodes carry both information and energy...

  5. Energy-transfer properties and mechanisms:

    International Nuclear Information System (INIS)

    Barker, J.R.

    1988-02-01

    This project continues the research on vibrational energy transfer involving large molecules. The motivation of the research is to advance knowledge concerning molecular energy in the electronic ground state so that meaningful predictions can be made. The experimental program will use several techniques on several different molecules with the aim of eliminating experimental artifacts and gaining more insight into energy transfer processes. The theoretical effort will be directed toward assessing the validity of the Biased Random Walk theory and toward developing simpler models that adequately describe the energy transfer process. 6 figs

  6. Comparison of vibrational conductivity and radiative energy transfer methods

    Science.gov (United States)

    Le Bot, A.

    2005-05-01

    This paper is concerned with the comparison of two methods well suited for the prediction of the wideband response of built-up structures subjected to high-frequency vibrational excitation. The first method is sometimes called the vibrational conductivity method and the second one is rather known as the radiosity method in the field of acoustics, or the radiative energy transfer method. Both are based on quite similar physical assumptions i.e. uncorrelated sources, mean response and high-frequency excitation. Both are based on analogies with some equations encountered in the field of heat transfer. However these models do not lead to similar results. This paper compares the two methods. Some numerical simulations on a pair of plates joined along one edge are provided to illustrate the discussion.

  7. Direct observation of coherent energy transfer in nonlinear micromechanical oscillators.

    Science.gov (United States)

    Chen, Changyao; Zanette, Damián H; Czaplewski, David A; Shaw, Steven; López, Daniel

    2017-05-26

    Energy dissipation is an unavoidable phenomenon of physical systems that are directly coupled to an external environmental bath. In an oscillatory system, it leads to the decay of the oscillation amplitude. In situations where stable oscillations are required, the energy dissipated by the vibrations is usually compensated by replenishment from external energy sources. Consequently, if the external energy supply is removed, the amplitude of oscillations start to decay immediately, since there is no means to restitute the energy dissipated. Here, we demonstrate a novel dissipation engineering strategy that can support stable oscillations without supplying external energy to compensate losses. The fundamental intrinsic mechanism of resonant mode coupling is used to redistribute and store mechanical energy among vibrational modes and coherently transfer it back to the principal mode when the external excitation is off. To experimentally demonstrate this phenomenon, we exploit the nonlinear dynamic response of microelectromechanical oscillators to couple two different vibrational modes through an internal resonance.

  8. Energy transfer in isolated LHC II studied by femtosecond pump-probe technique

    CERN Document Server

    Yang Yi; Liu Yuan; Liu Wei Min; Zhu Rong Yi; Qian Shi Xiong; Xu Chun He

    2003-01-01

    Excitation energy transfer in the isolated light-harvesting chlorophyll (Chl)-a/b protein complex of photosystem II (LHC II) was studied by the one-colour pump-probe technique with femtosecond time resolution. After exciting Chl-b by 638nm beam, the dynamic behaviour shows that the ultrafast energy transfer from Chl-b at positions of B2, B3, and B5 to the corresponding Chl-a molecules in monomeric subunit of LHC II is in the time scale of 230fs. While with the excitation of Chl-a at 678nm, the energy transfer between excitons of Chl-a molecules has the lifetime of about 370 fs, and two other slow decay components are due to the energy transfer between different Chl-a molecules in a monomeric subunit of LHC II or in different subunits, or due to change of molecular conformation. (20 refs).

  9. Ab initio calculation of electron excitation energies in solids

    International Nuclear Information System (INIS)

    Louie, S.G.

    1996-02-01

    Progress in the first-principles calculation of electron excitation energies in solids is discussed. Quasiparticle energies are computed by expanding the electron self energy to first order in the screened Coulomb interaction in the so-called GW approximation. The method was applied to explain and predict spectroscopic properties of a variety of systems. Several illustrative applications to semiconductors, materials under pressure, chemisorption, and point defects in solids are presented. A recent reformulation of the method employing mixed- space functions and imaginary time techniques is also discussed

  10. Rydberg energies using excited state density functional theory

    International Nuclear Information System (INIS)

    Cheng, C.-L.; Wu Qin; Van Voorhis, Troy

    2008-01-01

    We utilize excited state density functional theory (eDFT) to study Rydberg states in atoms. We show both analytically and numerically that semilocal functionals can give quite reasonable Rydberg energies from eDFT, even in cases where time dependent density functional theory (TDDFT) fails catastrophically. We trace these findings to the fact that in eDFT the Kohn-Sham potential for each state is computed using the appropriate excited state density. Unlike the ground state potential, which typically falls off exponentially, the sequence of excited state potentials has a component that falls off polynomially with distance, leading to a Rydberg-type series. We also address the rigorous basis of eDFT for these systems. Perdew and Levy have shown using the constrained search formalism that every stationary density corresponds, in principle, to an exact stationary state of the full many-body Hamiltonian. In the present context, this means that the excited state DFT solutions are rigorous as long as they deliver the minimum noninteracting kinetic energy for the given density. We use optimized effective potential techniques to show that, in some cases, the eDFT Rydberg solutions appear to deliver the minimum kinetic energy because the associated density is not pure state v-representable. We thus find that eDFT plays a complementary role to constrained DFT: The former works only if the excited state density is not the ground state of some potential while the latter applies only when the density is a ground state density.

  11. Experimental determination of fragment excitation energies in multifragmentation events

    International Nuclear Information System (INIS)

    Marie, N.; Natowitz, J.B.; Assenard, M.; Bacri, Ch.O.

    1998-01-01

    For 50 MeV/nucleon 129 Xe + nat Sn multifragmentation events, by means of correlation techniques, the multiplicities of the hydrogen and helium isotopes which were emitted by the hot primary excited fragments produced at the stage of the disassembly of an equilibrated hot source are determined. The relative kinetic energy distributions between the primary clusters and the light charged particles that they evaporate are also derived. From the comparison between the secondary multiplicities observed experimentally and the multiplicities predicted by the GEMINI model, it is concluded that the source breaks into primary fragments which are characterized by the same N/Z ratio as the combined system. Knowing the secondary light charged particle multiplicities and kinetic energies, the average charges of the hot fragments and are reconstructed their mean excitation energies are estimated. The fragment excitation energies are equal to 3.0 MeV/nucleon for the full range of intermediate mass fragment atomic number. This global constancy indicates that, on the average, thermodynamical equilibrium was achieved at the disassembly stage of the source. (author)

  12. Experimental determination of fragment excitation energies in multifragmentation events

    Energy Technology Data Exchange (ETDEWEB)

    Marie, N.; Natowitz, J.B. [Texas A and M Univ., College Station, TX (United States). Cyclotron Inst.; Chbihi, A.; Le Fevre, A.; Salou, S.; Wieleczko, J.P.; Gingras, L.; Auger, G. [Grand Accelerateur National d`Ions Lourds, 14 - Caen (France); Assenard, M. [Nantes Univ., 44 (France); Bacri, Ch.O. [Centre National de la Recherche Scientifique, CNRS, 91 - Orsay (France)] [and others

    1998-03-17

    For 50 MeV/nucleon {sup 129}Xe + {sup nat}Sn multifragmentation events, by means of correlation techniques, the multiplicities of the hydrogen and helium isotopes which were emitted by the hot primary excited fragments produced at the stage of the disassembly of an equilibrated hot source are determined. The relative kinetic energy distributions between the primary clusters and the light charged particles that they evaporate are also derived. From the comparison between the secondary multiplicities observed experimentally and the multiplicities predicted by the GEMINI model, it is concluded that the source breaks into primary fragments which are characterized by the same N/Z ratio as the combined system. Knowing the secondary light charged particle multiplicities and kinetic energies, the average charges of the hot fragments and are reconstructed their mean excitation energies are estimated. The fragment excitation energies are equal to 3.0 MeV/nucleon for the full range of intermediate mass fragment atomic number. This global constancy indicates that, on the average, thermodynamical equilibrium was achieved at the disassembly stage of the source. (author) 25 refs.

  13. Plasmonic energy transfer in periodically doped graphene

    International Nuclear Information System (INIS)

    Silveiro, I; Manjavacas, A; Thongrattanasiri, S; García de Abajo, F J

    2013-01-01

    We predict unprecedentedly large values of the energy-transfer rate between an optical emitter and a layer of periodically doped graphene. The transfer exhibits divergences at photon frequencies corresponding to the Van Hove singularities of the plasmonic band structure of the graphene. In particular, we find flat bands associated with regions of vanishing doping charge, which appear in graphene when it is patterned through gates of spatially alternating signs, giving rise to intense transfer rate singularities. Graphene is thus shown to provide a unique platform for fast control of optical energy transfer via fast electrostatic inhomogeneous doping. (paper)

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

    DEFF Research Database (Denmark)

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

    2017-01-01

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

  15. Forster resonance energy transfer in the system of human serum albumin-xanthene dyes

    Science.gov (United States)

    Kochubey, V. I.; Pravdin, A. B.; Melnikov, A. G.; Konstantinova, I.; Alonova, I. V.

    2016-04-01

    The processes of interaction of fluorescent probes: eosin and erythrosine with human serum albumin (HSA) were studied by the methods of absorption and fluorescence spectroscopy. Extinction coefficients of probes were determined. Critical transfer radius and the energy transfer efficiency were defined by fluorescence quenching of HSA. Analysis of the excitation spectra of HSA revealed that the energy transfer process is carried out mainly between tryptophanyl and probes.

  16. Coherence and relaxation in energy transfer processes in condensed phases

    International Nuclear Information System (INIS)

    Shelby, R.M.

    1978-03-01

    Investigations of electronic triplet and vibrational energy transfer dynamics and relaxation processes are presented. Emphasis is placed on understanding the role of coherence and interactions which tend to destroy the coherence. In the case of triplet excitons at low temperatures, the importance of coherence in energy migration can be established, and the average coherence parameters can be experimentally determined. In the case of vibrational excitations, both picosecond spectroscopic studies of vibrational relaxation and spontaneous Raman spectroscopy are used to characterize the dynamics and give increased insight into the nature of the mechanisms responsible for vibrational dephasing. The design and operation of the picosecond apparatus used in these experiments is also described

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

    Science.gov (United States)

    Schwabe, Tobias

    2016-10-21

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

  18. Energy transfer mechanisms in layered 2D perovskites.

    Science.gov (United States)

    Williams, Olivia F; Guo, Zhenkun; Hu, Jun; Yan, Liang; You, Wei; Moran, Andrew M

    2018-04-07

    Two-dimensional (2D) perovskite quantum wells are generating broad scientific interest because of their potential for use in optoelectronic devices. Recently, it has been shown that layers of 2D perovskites can be grown in which the average thicknesses of the quantum wells increase from the back to the front of the film. This geometry carries implications for light harvesting applications because the bandgap of a quantum well decreases as its thickness increases. The general structural formula for the 2D perovskite systems under investigation in this work is (PEA) 2 (MA) n-1 [Pb n I 3n+1 ] (PEA = phenethyl ammonium, MA = methyl ammonium). Here, we examine two layered 2D perovskites with different distributions of quantum well thicknesses. Spectroscopic measurements and model calculations suggest that both systems funnel electronic excitations from the back to the front of the film through energy transfer mechanisms on the time scales of 100's of ps (i.e., energy transfer from thinner to thicker quantum wells). In addition, the model calculations demonstrate that the transient absorption spectra are composed of a progression of single exciton and biexciton resonances associated with the individual quantum wells. We find that exciton dissociation and/or charge transport dynamics make only minor contributions to the transient absorption spectra within the first 1 ns after photo-excitation. An analysis of the energy transfer kinetics indicates that the transitions occur primarily between quantum wells with values of n that differ by 1 because of the spectral overlap factor that governs the energy transfer rate. Two-dimensional transient absorption spectra reveal a pattern of resonances consistent with the dominance of sequential energy transfer dynamics.

  19. Energy transfer mechanisms in layered 2D perovskites

    Science.gov (United States)

    Williams, Olivia F.; Guo, Zhenkun; Hu, Jun; Yan, Liang; You, Wei; Moran, Andrew M.

    2018-04-01

    Two-dimensional (2D) perovskite quantum wells are generating broad scientific interest because of their potential for use in optoelectronic devices. Recently, it has been shown that layers of 2D perovskites can be grown in which the average thicknesses of the quantum wells increase from the back to the front of the film. This geometry carries implications for light harvesting applications because the bandgap of a quantum well decreases as its thickness increases. The general structural formula for the 2D perovskite systems under investigation in this work is (PEA)2(MA)n-1[PbnI3n+1] (PEA = phenethyl ammonium, MA = methyl ammonium). Here, we examine two layered 2D perovskites with different distributions of quantum well thicknesses. Spectroscopic measurements and model calculations suggest that both systems funnel electronic excitations from the back to the front of the film through energy transfer mechanisms on the time scales of 100's of ps (i.e., energy transfer from thinner to thicker quantum wells). In addition, the model calculations demonstrate that the transient absorption spectra are composed of a progression of single exciton and biexciton resonances associated with the individual quantum wells. We find that exciton dissociation and/or charge transport dynamics make only minor contributions to the transient absorption spectra within the first 1 ns after photo-excitation. An analysis of the energy transfer kinetics indicates that the transitions occur primarily between quantum wells with values of n that differ by 1 because of the spectral overlap factor that governs the energy transfer rate. Two-dimensional transient absorption spectra reveal a pattern of resonances consistent with the dominance of sequential energy transfer dynamics.

  20. Resonance energy transfer: Dye to metal nanoparticles

    Energy Technology Data Exchange (ETDEWEB)

    Wari, M. N.; Pujar, G. H.; Inamdar, S. R., E-mail: him-lax3@yahoo.com [Laser Spectroscopy Programme, Department of Physics, Karnatak University, Dharwad-580003 (India)

    2015-06-24

    In the present study, surface energy transfer (SET) from Coumarin 540A (C540 A) to Gold nanoparticle (Au) is demonstrated. The observed results show pronounced effect on the photoluminescence intensity and shortening of the lifetime of Coumarin 540A upon interaction with the spherical gold nanoparticle, also there are measured effects on radiative rate of the dye. Experimental results are analyzed with fluorescence resonance energy transfer (FRET) and SET theories. The results obtained from distance-dependent quenching provide experimental evidence that the efficiency curve slope and distance of quenching is best modeled by surface energy transfer process.

  1. Energy transfer during the hydroentanglement of fibres

    CSIR Research Space (South Africa)

    Moyo, D

    2012-10-01

    Full Text Available .kashan.co.za] ABSTRACT The hydroentanglement of fibres is achieved by the energy of the high-velocity waterjets. This method is highly energy intensive and costly, hence the attempt to study the energy transfer during the process. Generally, the amount of energy used... in the nonwoven fabric strength were studied. In the study, the energies of the waterjets transferred to every fabric sample as a function of the waterjet pressure, machine speed, machine efficiency and the web area weight were quantified, and the resultant...

  2. Observation of Electronic Excitation Transfer Through Light Harvesting Complex II Using Two-Dimensional Electronic-Vibrational Spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Lewis, NHC; Gruenke, NL; Oliver, TAA; Ballottari, M; Bassi, R; Fleming, GR

    2016-10-05

    Light-harvesting complex II (LHCII) serves a central role in light harvesting for oxygenic photosynthesis and is arguably the most important photosynthetic antenna complex. In this article, we present two-dimensional electronic–vibrational (2DEV) spectra of LHCII isolated from spinach, demonstrating the possibility of using this technique to track the transfer of electronic excitation energy between specific pigments within the complex. We assign the spectral bands via comparison with the 2DEV spectra of the isolated chromophores, chlorophyll a and b, and present evidence that excitation energy between the pigments of the complex are observed in these spectra. Lastly, we analyze the essential components of the 2DEV spectra using singular value decomposition, which makes it possible to reveal the relaxation pathways within this complex.

  3. The population transfer of high excited states of Rydberg lithium atoms in a microwave field

    International Nuclear Information System (INIS)

    Jiang Lijuan; Zhang Xianzhou; Ma Huanqiang; Jia Guangrui; Zhang Yonghui; Xia Lihua

    2012-01-01

    Using the time-dependent multilevel approach (TDMA), the properties of high excited Rydberg lithium atom have been obtained in the microwave field. The population transfer of lithium atom are studied on numerical calculation, quantum states are controlled and manipulated by microwave field. It shows that the population can be completely transferred to the target state by changing the chirped rate and field amplitude. (authors)

  4. Dynamics of Excited State Proton Transfer in Nitro Substituted 10-Hydroxybenzo[h]quinolines

    DEFF Research Database (Denmark)

    Marciak, H; Hristova, S.; Deneva, V

    2017-01-01

    The ground state tautomerism and excited state intramolecular proton transfer (ESIPT) of 10-hydroxybenzo[h]quinoline (HBQ) and its nitro derivatives, 7-nitrobenzo[h]quinolin-10-ol (2) and 7,9-dinitrobenzo[h]quinolin-10-ol (3), have been studied in acetonitrile using steady state as well as time d...

  5. Symmetry-breaking intramolecular charge transfer in the excited state of meso-linked BODIPY dyads

    KAUST Repository

    Whited, Matthew T.; Patel, Niral M.; Roberts, Sean T.; Allen, Kathryn; Djurovich, Peter I.; Bradforth, Stephen E.; Thompson, Mark E.

    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.

  6. On the rate of triplet excitation transfer in the diffuse limit

    International Nuclear Information System (INIS)

    Davidovich, M.A.; Knox, R.S.

    1979-11-01

    The usefulness of spectral data in estimating intermolecular triplet excitation transfer rates in found to be rather limited and to depend explicitly on the mechaisms which allow the optical transitions. Necessary conditions for the validity of such use of spectra are given, and the otherwise required correction factors are discussed and estimated. (Author) [pt

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

    Energy Technology Data Exchange (ETDEWEB)

    Chang, Xue-Ping; Fang, Qiu, E-mail: fangqiu917@bnu.edu.cn; Cui, Ganglong, E-mail: ganglong.cui@bnu.edu.cn [Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875 (China)

    2014-10-21

    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 S{sub 0}, T{sub 1}, and S{sub 1} states. We have uncovered four nonadiabatic photodecarboxylation paths. (i) The S{sub 1} system relaxes via an excited-state intramolecular proton transfer (ESIPT) to a hydrogen-transferred tautomer, near which an S{sub 1}/S{sub 0} conical intersection funnels the S{sub 1} to S{sub 0} state. Then, some trajectories continue completing the decarboxylation reaction in the S{sub 0} state; the remaining trajectories via a reverse hydrogen transfer return to the S{sub 0} minimum, from which a thermal decarboxylation reaction occurs. (ii) Due to a small S{sub 1} −T{sub 1} energy gap and a large S{sub 1}/T{sub 1} spin-orbit coupling, an efficient S{sub 1} → T{sub 1} intersystem crossing process happens again near this S{sub 1}/S{sub 0} conical intersection. When decaying to T{sub 1} state, a direct photodecarboxylation proceeds. (iii) Prior to ESIPT, the S{sub 1} system first decays to the T{sub 1} state via an S{sub 1} → T{sub 1} intersystem crossing; then, the T{sub 1} system evolves to a hydrogen-transferred tautomer. Therefrom, an adiabatic T{sub 1} decarboxylation takes place due to a small barrier of 7.7 kcal/mol. (iv) Besides the aforementioned T{sub 1} ESIPT process, there also exists a comparable Norrish type I reaction in the T{sub 1} state, which forms the ground-state products of CH{sub 3}CO and COOH. Finally, we have found that ESIPT plays an important role. It closes the S{sub 1}-T{sub 1} and S{sub 1}-S{sub 0} energy gaps, effecting an S{sub 1}/T{sub 1}/S{sub 0} three-state intersection region, and mediating nonadiabatic photodecarboxylation reactions of pyruvic acid.

  8. Targeting Low-Energy Ballistic Lunar Transfers

    Science.gov (United States)

    Parker, Jeffrey S.

    2010-01-01

    Numerous low-energy ballistic transfers exist between the Earth and Moon that require less fuel than conventional transfers, but require three or more months of transfer time. An entirely ballistic lunar transfer departs the Earth from a particular declination at some time in order to arrive at the Moon at a given time along a desirable approach. Maneuvers may be added to the trajectory in order to adjust the Earth departure to meet mission requirements. In this paper, we characterize the (Delta)V cost required to adjust a low-energy ballistic lunar transfer such that a spacecraft may depart the Earth at a desirable declination, e.g., 28.5(white bullet), on a designated date. This study identifies the optimal locations to place one or two maneuvers along a transfer to minimize the (Delta)V cost of the transfer. One practical application of this study is to characterize the launch period for a mission that aims to launch from a particular launch site, such as Cape Canaveral, Florida, and arrive at a particular orbit at the Moon on a given date using a three-month low-energy transfer.

  9. Risk transfer via energy savings insurance

    OpenAIRE

    Mills, Evan

    2001-01-01

    Among the key barriers to investment in energy efficiency improvements are uncertainties about attaining projected energy savings and apprehension about potential disputes over these savings. The fields of energy management and risk management are thus intertwined. While many technical methods have emerged to manage performance risks (e.g. building commissioning), financial risk transfer techniques are less developed in the energy management arena than in other more mature segments of t...

  10. Resonant transfer excitation of fluorine-like Mo{sup 33+} ion

    Energy Technology Data Exchange (ETDEWEB)

    Ramadan, Hassan [Ain Shams Univ., Cairo (Egypt). Dept. of Basic Sciences; Elkilany, Sabbah [Kafr El-sheikh Univ. (Egypt). Dept. of Mathematics

    2010-06-15

    Dielectronic recombination (DR) cross sections (anti {sigma}{sup DR}) and rate coefficients ({alpha}{sup DR}) for Mo{sup 33+} are calculated using the angular momentum average scheme (AMA). Moreover, the resonant transfer excitation followed by X-ray emission (RTEX) cross sections ({sigma}{sup RTEX}) for the collision of Mo{sup 33+} with H{sub 2} and He targets are calculated and studied. The calculations of the cross sections are performed for both K- and L-shell excitations. A smooth change with the temperatures for {alpha}{sup DR} is found for all kinds of excitations. The rates for K-shell excitation are very small in comparison with the rates for L-shell excitation. The RTEX cross sections for Mo{sup 33+} ions are obtained from their corresponding DR cross sections by the method of folding in the impulse approximation (IMA). {sigma}{sup RTEX} for the K-shell excitation shows two overlapped peaks which may be attributed to the two groups in this excitation process. The present calculations are considered as a database for future comparison with theoretical and experimental data using other coupling schemes. Multiple Auger channels are complicating the dependence of the cross sections on principal quantum numbers. (orig.)

  11. Wireless energy transfer between anisotropic metamaterials shells

    Energy Technology Data Exchange (ETDEWEB)

    Díaz-Rubio, Ana; Carbonell, Jorge; Sánchez-Dehesa, José, E-mail: jsdehesa@upv.es

    2014-06-15

    The behavior of strongly coupled Radial Photonic Crystals shells is investigated as a potential alternative to transfer electromagnetic energy wirelessly. These sub-wavelength resonant microstructures, which are based on anisotropic metamaterials, can produce efficient coupling phenomena due to their high quality factor. A configuration of selected constitutive parameters (permittivity and permeability) is analyzed in terms of its resonant characteristics. The coupling to loss ratio between two coupled resonators is calculated as a function of distance, the maximum (in excess of 300) is obtained when the shells are separated by three times their radius. Under practical conditions an 83% of maximum power transfer has been also estimated. -- Highlights: •Anisotropic metamaterial shells exhibit high quality factors and sub-wavelength size. •Exchange of electromagnetic energy between shells with high efficiency is analyzed. •Strong coupling is supported with high wireless transfer efficiency. •End-to-end energy transfer efficiencies higher than 83% can be predicted.

  12. Wireless energy transfer between anisotropic metamaterials shells

    International Nuclear Information System (INIS)

    Díaz-Rubio, Ana; Carbonell, Jorge; Sánchez-Dehesa, José

    2014-01-01

    The behavior of strongly coupled Radial Photonic Crystals shells is investigated as a potential alternative to transfer electromagnetic energy wirelessly. These sub-wavelength resonant microstructures, which are based on anisotropic metamaterials, can produce efficient coupling phenomena due to their high quality factor. A configuration of selected constitutive parameters (permittivity and permeability) is analyzed in terms of its resonant characteristics. The coupling to loss ratio between two coupled resonators is calculated as a function of distance, the maximum (in excess of 300) is obtained when the shells are separated by three times their radius. Under practical conditions an 83% of maximum power transfer has been also estimated. -- Highlights: •Anisotropic metamaterial shells exhibit high quality factors and sub-wavelength size. •Exchange of electromagnetic energy between shells with high efficiency is analyzed. •Strong coupling is supported with high wireless transfer efficiency. •End-to-end energy transfer efficiencies higher than 83% can be predicted

  13. Probing nuclear shell structure beyond the N=40 subshell using multiple Coulomb excitation and transfer experiments

    Energy Technology Data Exchange (ETDEWEB)

    Hellgartner, Stefanie Christine

    2015-11-13

    In this work, the N=40 subshell closure is investigated with two complementary methods using a radioactive {sup 72}Zn ISOLDE beam: One- and two-neutron transfer reactions and multiple Coulomb excitation. In the one-neutron transfer reaction, two new levels of {sup 73}Zn were discovered. The two-neutron transfer channel allowed to study the differential cross section of the ground state and the 2{sup +}{sub 1} state of {sup 74}Zn. In the Coulomb excitation experiment, the measured B(E2) values and quadrupole moments of {sup 72}Zn showed that the yrast states 0{sup +}{sub 1}, 2{sup +}{sub 1} and 4{sup +}{sub 1} are moderately collective. Contrary, the 0{sup +}{sub 2} state has a different structure, since it features a stronger closed N=40 configuration compared to the ground state.

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

    DEFF Research Database (Denmark)

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

    2018-01-01

    The excited state dynamics of solvated [Fe(bpy)(CN)4]2-, where bpy = 2,2'-bipyridine, show significant sensitivity to the solvent Lewis acidity. Using a combination of optical absorption and X-ray emission transient spectroscopies, we have previously shown that the metal to ligand charge transfer...... the MLCT excited state relaxation dynamics of [Fe(bpy)(CN)4]2- in water, a strong Lewis acid solvent. The charge-transfer excited state is now found to decay in less than 100 femtoseconds, forming a quasi-stable metal centered excited state with a 13 picosecond lifetime. We find that this MC excited state...... developed for solar applications....

  15. Energy transfer in turbulence under rotation

    Science.gov (United States)

    Buzzicotti, Michele; Aluie, Hussein; Biferale, Luca; Linkmann, Moritz

    2018-03-01

    It is known that rapidly rotating turbulent flows are characterized by the emergence of simultaneous upscale and downscale energy transfer. Indeed, both numerics and experiments show the formation of large-scale anisotropic vortices together with the development of small-scale dissipative structures. However the organization of interactions leading to this complex dynamics remains unclear. Two different mechanisms are known to be able to transfer energy upscale in a turbulent flow. The first is characterized by two-dimensional interactions among triads lying on the two-dimensional, three-component (2D3C)/slow manifold, namely on the Fourier plane perpendicular to the rotation axis. The second mechanism is three-dimensional and consists of interactions between triads with the same sign of helicity (homochiral). Here, we present a detailed numerical study of rotating flows using a suite of high-Reynolds-number direct numerical simulations (DNS) within different parameter regimes to analyze both upscale and downscale cascade ranges. We find that the upscale cascade at wave numbers close to the forcing scale is generated by increasingly dominant homochiral interactions which couple the three-dimensional bulk and the 2D3C plane. This coupling produces an accumulation of energy in the 2D3C plane, which then transfers energy to smaller wave numbers thanks to the two-dimensional mechanism. In the forward cascade range, we find that the energy transfer is dominated by heterochiral triads and is dominated primarily by interaction within the fast manifold where kz≠0 . We further analyze the energy transfer in different regions in the real-space domain. In particular, we distinguish high-strain from high-vorticity regions and we uncover that while the mean transfer is produced inside regions of strain, the rare but extreme events of energy transfer occur primarily inside the large-scale column vortices.

  16. Coulomb excitation of 206Hg at relativistic energies

    Science.gov (United States)

    Alexander, Tom

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

  17. Optically nonlinear energy transfer in light-harvesting dendrimers

    Science.gov (United States)

    Andrews, David L.; Bradshaw, David S.

    2004-08-01

    Dendrimeric polymers are the subject of intense research activity geared towards their implementation in nanodevice applications such as energy harvesting systems, organic light-emitting diodes, photosensitizers, low-threshold lasers, and quantum logic elements, etc. A recent development in this area has been the construction of dendrimers specifically designed to exhibit novel forms of optical nonlinearity, exploiting the unique properties of these materials at high levels of photon flux. Starting from a thorough treatment of the underlying theory based on the principles of molecular quantum electrodynamics, it is possible to identify and characterize several optically nonlinear mechanisms for directed energy transfer and energy pooling in multichromophore dendrimers. Such mechanisms fall into two classes: first, those where two-photon absorption by individual donors is followed by transfer of the net energy to an acceptor; second, those where the excitation of two electronically distinct but neighboring donor groups is followed by a collective migration of their energy to a suitable acceptor. Each transfer process is subject to minor dissipative losses. In this paper we describe in detail the balance of factors and the constraints that determines the favored mechanism, which include the excitation statistics, structure of the energy levels, laser coherence factors, chromophore selection rules and architecture, possibilities for the formation of delocalized excitons, spectral overlap, and the overall distribution of donors and acceptors. Furthermore, it transpires that quantum interference between different mechanisms can play an important role. Thus, as the relative importance of each mechanism determines the relevant nanophotonic characteristics, the results reported here afford the means for optimizing highly efficient light-harvesting dendrimer devices.

  18. Failures of TDDFT in describing the lowest intramolecular charge-transfer excitation in para-nitroanilin

    DEFF Research Database (Denmark)

    Eriksen, J.J.; Sauer, S.P.A.; Mikkelsen, K.V.

    2013-01-01

    We investigate the failure of Time{Dependent Density Functional Theory (TDDFT) with the CAM{B3LYP exchange{correlation (xc) functional coupled to the Polarizable Embedding (PE) scheme (PE-CAM-B3LYP) in reproducing the solvatochromic shift of the lowest intense charge{transfer excitation in para...... the electric dipole moments in the gas phase and for 100 solvent congurations. We find that CAM-B3LYP overestimates the amount of charge separation inherent in the ground state and TDDFT/CAM-B3LYP drastically underestimates this amount in the excited charge-transfer state. As the errors in the solvatochromatic...... to benchmark results of TDDFT calculations with CAM-B3LYP for intramolecular charge{transfer excitations in molecular systems similar to pNA against higher{level ab initio wave function methods, like, e.g., CCSD, prior to their use. Using the calculated change in dipole moment upon excitation as a measure...

  19. Optical Energy Transfer and Conversion System

    Science.gov (United States)

    Hogan, Bartholomew P. (Inventor); Stone, William C. (Inventor)

    2018-01-01

    An optical energy transfer and conversion system comprising a fiber spooler and an electrical power extraction subsystem connected to the spooler with an optical waveguide. Optical energy is generated at and transferred from a base station through fiber wrapped around the spooler, and ultimately to the power extraction system at a remote mobility platform for conversion to another form of energy. The fiber spooler may reside on the remote mobility platform which may be a vehicle, or apparatus that is either self-propelled or is carried by a secondary mobility platform either on land, under the sea, in the air or in space.

  20. Excitation of higher lying energy states in a rubidium DPAL

    Science.gov (United States)

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

    2018-02-01

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

  1. Structural, photophysical, and theoretical studies of imidazole-based excited-state intramolecular proton transfer molecules

    Science.gov (United States)

    Somasundaram, Sivaraman; Kamaraj, Eswaran; Hwang, Su Jin; Park, Sanghyuk

    2018-02-01

    Imidazole-based excited state intramolecular proton transfer (ESIPT) blue fluorescent molecules, 2-(1-(4-chlorophenyl)-4,5-diphenyl-1H-imidazol-2-yl)phenol (BHPI-Cl) and 2-(1-(4-bromophenyl)-4,5-diphenyl-1H-imidazol-2-yl)phenol (BHPI-Br) were designed and synthesized by Debus-Radziszewski method through a one-pot multicomponent reaction in high yield. The synthesized compounds were fully characterized by 1H NMR, 13C NMR, FT-IR, FT-Raman, GC-Mass, and elemental analysis. The molecular structures in single crystal lattice were studied by X-ray crystallographic analysis. Because of the intramolecular hydrogen bonding, hydroxyphenyl group is planar to the central imidazole ring, while the other phenyl rings gave distorted conformations to the central heterocyclic ring. BHPI-Cl and BHPI-Br molecules showed intense ESIPT fluorescence at 480 nm, because the two twisted phenyl rings on 4- and 5-positions have reduced intermolecular interaction between adjacent molecules in each crystal through a head-to-tail packing manner. Quantum chemical calculations of energies were carried out by (TD-)DFT using B3LYP/6-31G(d, p) basis set to predict the electronic absorption spectra of the compounds, and they showed good agreement between the computational and the experimental values. The thermal analyses of the synthesized molecules were also carried out by TGA/DSC method.

  2. Boltzmann rovibrational collisional coarse-grained model for internal energy excitation and dissociation in hypersonic flows.

    Science.gov (United States)

    Munafò, A; Panesi, M; Magin, T E

    2014-02-01

    A Boltzmann rovibrational collisional coarse-grained model is proposed to reduce a detailed kinetic mechanism database developed at NASA Ames Research Center for internal energy transfer and dissociation in N(2)-N interactions. The coarse-grained model is constructed by lumping the rovibrational energy levels of the N(2) molecule into energy bins. The population of the levels within each bin is assumed to follow a Boltzmann distribution at the local translational temperature. Excitation and dissociation rate coefficients for the energy bins are obtained by averaging the elementary rate coefficients. The energy bins are treated as separate species, thus allowing for non-Boltzmann distributions of their populations. The proposed coarse-grained model is applied to the study of nonequilibrium flows behind normal shock waves and within converging-diverging nozzles. In both cases, the flow is assumed inviscid and steady. Computational results are compared with those obtained by direct solution of the master equation for the rovibrational collisional model and a more conventional multitemperature model. It is found that the proposed coarse-grained model is able to accurately resolve the nonequilibrium dynamics of internal energy excitation and dissociation-recombination processes with only 20 energy bins. Furthermore, the proposed coarse-grained model provides a superior description of the nonequilibrium phenomena occurring in shock heated and nozzle flows when compared with the conventional multitemperature models.

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

    Science.gov (United States)

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

    2015-08-11

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

  4. Targeted Energy Transfer Phenomena in Vibro-Impact Oscillators

    International Nuclear Information System (INIS)

    Lee, Young S.; McFarland, D. Michael; Bergman, Lawrence A.; Nucera, Francesco; Vakakis, Alexander F.

    2008-01-01

    We study targeted energy transfer (TET) in a coupled oscillator, consisting of a single-degree-of-freedom primary linear oscillator coupled to a vibro-impact nonlinear energy sink (VI NES). For this purpose, we first compute the VI periodic orbits of the underlying hamiltonian VI system, and construct the corresponding frequency-energy plot (FEP). Then, considering inelastic impacts and viscous dissipation, we examine VI damped transitions on the FEP to identify a TET phenomenon by exciting a VI impulsive orbit, which is the most efficient mechanism for TET. Not only can the VI TET involve passive absorption and local dissipation of significant portions of the energy from the primary systems, but it occurs at sufficiently fast time scales. This renders VI NESs suitable for applications, like seismic mitigation, where shock elimination in the early, highly energetic regime of the motion is a critical requirement

  5. Ultrafast energy transfer in dansylated POPAM--eosin complexes

    Science.gov (United States)

    Aumanen, Jukka; Lehtovuori, Viivi; Werner, Nicole; Richardt, Gabriele; van Heyst, Jeroen; Vögtle, Fritz; Korppi-Tommola, Jouko

    2006-12-01

    Excitation energy transfer (EET) in dendritic host-guest complexes has been studied. Three generations G2, G3 and G4 of dansyl substituted poly(propyleneamine) dendrimers (POPAM) were complexed with a fluorescent dye eosin in chloroform solution. Arrival of excitation from dansyls to eosin was monitored by femtosecond transient absorption spectroscopy. EET rates from the dansyls to eosin(s) are characterised by two time constants 1 ps and 6 ps independent of dendrimer generation. Relaxation processes in eosin were clearly faster when complexed with dendrimer than in solution. As several eosins are bound to G3 and G4 dendrimers, besides host-guest interaction, also eosin-eosin interactions may contribute to the faster relaxation observed in these complexes.

  6. Dual fluorescence of excited state intra-molecular proton transfer of HBFO: mechanistic understanding, substituent and solvent effects.

    Science.gov (United States)

    Yang, Wenjing; Chen, Xuebo

    2014-03-07

    A combined approach of the multiconfigurational perturbation theory with the Rice-Ramsperger-Kassel-Marcus methodology has been employed to calculate the minimum potential energy profiles and the rates of excited state intra-molecular proton transfer (ESIPT) for the WOLED material molecule of HBFO and its four meta- or para-substituted compounds in gas phase, acetonitrile and cyclohexane solvents. The kinetic control for these reactions is quantitatively determined and extensively studied on the basis of the accurate potential energy surfaces when the thermodynamic factor associated with the free energy change becomes negligible in the case of the existence of a significant barrier in the ESIPT process. These computational efforts contribute to a deep understanding of the ESIPT mechanism, dual emission characteristics, kinetic controlling factor, substituent and solvent effects for these material molecules. The white light emission is generated by the establishment of dynamic equilibrium between enol and keto forms in the charge transfer excited SCT((1)ππ*) state. The performance of white light emission is quantitatively demonstrated to be mainly sensitive to the molecular tailoring approach of the electronic properties of meta- or para- substituents by the modulation of the forward/backward ESIPT rate ratio. The quality of white light emission is slightly tunable through its surrounding solvent environment. These computational results will provide a useful strategy for the molecular design of OLED and WOLED materials.

  7. Energy technology transfer to developing countries

    International Nuclear Information System (INIS)

    Goldemberg, J.

    1991-01-01

    This paper gives some examples of how technology transfer can successfully be given to third world countries to allow them to benefit in their quest for economic growth and better standards of living through reduced energy consumption and environmental pollution. It also suggests methods by which obstacles such as high investment costs, lack of information, market demand, etc., can be overcome in order to motivate technological transfer by industrialized countries

  8. Nuclear energy technology transfer: the security barriers

    International Nuclear Information System (INIS)

    Rinne, R.L.

    1975-08-01

    The problems presented by security considerations to the transfer of nuclear energy technology are examined. In the case of fusion, the national security barrier associated with the laser and E-beam approaches is discussed; for fission, the international security requirements, due to the possibility of the theft or diversion of special nuclear materials or sabotage of nuclear facilities, are highlighted. The paper outlines the nuclear fuel cycle and terrorist threat, examples of security barriers, and the current approaches to transferring technology. (auth)

  9. Energy-donor phosphorescence quenching study of triplet–triplet energy transfer between UV absorbers

    International Nuclear Information System (INIS)

    Kikuchi, Azusa; Nakabai, Yuya; Oguchi-Fujiyama, Nozomi; Miyazawa, Kazuyuki; Yagi, Mikio

    2015-01-01

    The intermolecular triplet–triplet energy transfer from a photounstable UV-A absorber, 4-tert-butyl-4′-methoxydibenzoylmethane (BMDBM), to UV-B absorbers, 2-ethylhexyl 4-methoxycinnamate (octyl methoxycinnamate, OMC), octocrylene (OCR) and dioctyl 4-methoxybenzylidenemalonate (DOMBM) has been observed using a 355 nm laser excitation in rigid solutions at 77 K. The decay curves of the energy-donor phosphorescence in the presence of the UV-B absorbers deviate from the exponential decay at the initial stage of the decay. The Stern–Volmer formulation is not valid in rigid solutions because molecular diffusion is impossible. The experimental results indicate that the rate constant of triplet–triplet energy transfer from BMDBM to the UV-B absorbers, k T–T , decreases in the following order: k T–T (BMDBM–DOMBM)>k T–T (BMDBM–OMC)≥k T–T (BMDBM–OCR). The presence of DOMBM enhances the photostability of the widely used combination of UV-A and UV-B absorbers, BMDBM and OCR. The effects of the triplet–triplet energy transfer on the photostability of BMDBM are discussed. - Highlights: • The intermolecular triplet–triplet energy transfer between UV absorbers was observed. • The phosphorescence decay deviates from exponential at the initial stage of decay. • The effects of triplet–triplet energy transfer on the photostability are discussed

  10. Electron energy distributions and excitation rates in high-frequency argon discharges

    International Nuclear Information System (INIS)

    Ferreira, C.M.; Loureiro, J.

    1983-06-01

    The electron energy distribution functions and rate coefficients for excitation and ionisation in argon under the action of an uniform high-frequency electric field were calculated by numerically solving the homogeneous Boltzmann equation. Analytic calculations in the limiting cases ω>>νsub(c) and ω<<νsub(c), where ω is the wave angular frequency and νsub(c) is the electron-neutral collision frequency for momentum transfer, are also presented and shown to be in very good agreement with the numerical computations. The results reported here are relevant for the modelling of high-frequency discharges in argon and, in particular, for improving recent theoretical descriptions of a plasma column sustained by surface microwaves. The properties of surface wave produced plasmas make them interesting as possible substitutes for other more conventional plasma sources for such important applications as plasma chemistry laser excitation, plasma etching spectroscopic sources etc...

  11. [Electron transfer, ionization, and excitation in atomic collisions]. Final technical report, June 15, 1986 - June 14, 1998

    International Nuclear Information System (INIS)

    1998-01-01

    The research on theoretical atomic collisions that was funded at The Pennsylvania State University's Wilkes-Barre Campus by DOE from 1986 to 1998 was carried out by Winger from 1986 to 1989 and by Winter and Alston from 1989 to 1998. The fundamental processes of electron transfer, ionization, and excitation in ion-ion, ion-atom, and, more recently, ion-molecule collisions were addressed. These collision processes were treated in the context of simple one-electron, quasi-one-electron, or two-electron systems in order to provide unambiguous results and reveal more clearly the collisional mechanisms. Winter's work generally focused on the intermediate projectile-energy range corresponding to proton energies from about ten to a few hundred keV. In this velocity-matching energy range, the electron-transfer cross section reaches a peak, and many states, including electron-transfer and ionization states, contribute to the overall electron-cloud distribution and transition probabilities; a large number of states are coupled, and therefore perturbative approaches are generally inappropriate. These coupled-state calculations were sometimes also extended to higher energies to join with perturbative results. Alston concentrated on intermediate-energy asymmetric collision systems, for which coupling with the projectile is weaker, but many target states are included, and on high energies (MeV energies). Thus, while perturbation theory for electron transfer is valid, it is not adequate to first order. The studies by Winter and Alston described were often done in parallel. Alston also developed formal perturbative approaches not tied to any particular system. Materials studied included He + , Li 2+ , Be 3+ , B 4+ , C 5+ , and the H + + Na system

  12. Photophysical properties and energy transfer mechanism of PFO/Fluorol 7GA hybrid thin films

    Energy Technology Data Exchange (ETDEWEB)

    Al-Asbahi, Bandar Ali, E-mail: alasbahibandar@gmail.com [School of Applied Physics, Faculty of Science and Technology, Universiti Kebangsaan Malaysia (UKM), 43600 Bangi, Selangor (Malaysia); Department of Physics, Faculty of Science, Sana' a University (Yemen); Jumali, Mohammad Hafizuddin Haji, E-mail: hafizhj@ukm.my [School of Applied Physics, Faculty of Science and Technology, Universiti Kebangsaan Malaysia (UKM), 43600 Bangi, Selangor (Malaysia); Yap, Chi Chin; Flaifel, Moayad Husein [School of Applied Physics, Faculty of Science and Technology, Universiti Kebangsaan Malaysia (UKM), 43600 Bangi, Selangor (Malaysia); Salleh, Muhamad Mat [Institute of Microengineering and Nanoelectronics (IMEN), Universiti Kebangsaan Malaysia (UKM), 43600 Bangi, Selangor (Malaysia)

    2013-10-15

    Photophysical properties of poly (9,9′-di-n-octylfluorenyl-2.7-diyl) (PFO)/2-butyl-6- (butylamino)benzo [de] isoquinoline-1,3-dione (Fluorol 7GA) and energy transfer between them have been investigated. In this work, both PFO and Fluorol 7GA act as donor and acceptor, respectively. Based on the absorption and luminescence measurements, the photophysical and energy transfer properties such as fluorescence quantum yield (Φ{sub f}), fluorescence lifetime (τ), radiative rate constant (k{sub r}), non-radiative rate constant (k{sub nr}), quenching rate constant (k{sub SV}), energy transfer rate constant (k{sub ET}), energy transfer probability (P{sub DA}), energy transfer efficiency (η), critical concentration of acceptor (C{sub o}), energy transfer time (τ{sub ET}) and critical distance of energy transfer (R{sub o}) were calculated. Large values of k{sub SV}, k{sub ET} and R{sub o} suggested that Förster-type energy transfer was the dominant mechanism for the energy transfer between the excited donor and ground state acceptor molecules. It was observed that the Förster energy transfer together with the trapping process are crucial for performance improvement in ITO/(PFO/Fluorol7GA)/Al device. -- Highlights: • The efficient of energy transfer from PFO to Fluorol 7GA was evidenced. • The resonance energy transfer (Förster type) is the dominant mechanism. • Hsu et al. model was used to calculate Φ{sub f}, τ, k{sub r} and k{sub nr} of PFO thin film. • Several of the photophysical and energy transfer properties were calculated. • Trapping process and Förster energy transfer led to improve the device performance.

  13. On the intramolecular proton transfer of 3-hydroxyflavone in the first singlet excited state: A theoretical study

    International Nuclear Information System (INIS)

    Casadesus, Ricard; Vendrell, Oriol; Moreno, Miquel; Lluch, Jose M.; Morokuma, Keiji

    2006-01-01

    The intramolecular proton-transfer reaction in 3-hydroxyflavone (3HF) is theoretically studied both in the ground (S 0 ) and first singlet excited (S 1 ) electronic states. In S 0 the proton-transfer reaction is shown to be quite unfavorable at the DFT (B3LYP) level. However, the back proton transfer is found to be a feasible process with a small energy barrier, both results being in qualitative agreement with known experimental facts. Different theoretical levels are considered and compared for S 1 . The ab initio configuration interaction singles (CIS) method overestimates the energy of S 1 and give too high energy barriers for the proton-transfer reaction. The complete active space SCF (CASSCF) method gives a more reasonable value but the inclusion of the dynamical correlation through second-order perturbation theory (CASPT2) upon CASSCF geometries or the use of the time-dependent DFT (TDDFT) method upon CIS geometries gives a barrierless process. Optimization of geometries (minima and transition-state structures) at the TDDFT level leads to a small but non-negligible energy barrier for the proton-transfer reaction in S 1 and global energies that fit quite well with the known experimental (spectroscopic and femtochemistry) data. Finally the effect of a polar environment is analyzed through a continuum model, which gives only a small difference from the previous gas-phase results. This points out that the remarkable changes in the photochemistry of 3HF observed experimentally are not to be solely attributed to the polarity of the surrounding media

  14. On the intramolecular proton transfer of 3-hydroxyflavone in the first singlet excited state: A theoretical study

    Energy Technology Data Exchange (ETDEWEB)

    Casadesus, Ricard [Departament de Quimica, Universitat Autonoma de Barcelona, 08193 Bellaterra, Barcelona (Spain); Cherry L. Emerson Center for Scientific Computation and Department of Chemistry, Emory University, Atlanta, GA 30322 (United States); Vendrell, Oriol [Departament de Quimica, Universitat Autonoma de Barcelona, 08193 Bellaterra, Barcelona (Spain); Moreno, Miquel [Departament de Quimica, Universitat Autonoma de Barcelona, 08193 Bellaterra, Barcelona (Spain)], E-mail: mmf@klingon.uab.es; Lluch, Jose M. [Departament de Quimica, Universitat Autonoma de Barcelona, 08193 Bellaterra, Barcelona (Spain); Morokuma, Keiji [Cherry L. Emerson Center for Scientific Computation and Department of Chemistry, Emory University, Atlanta, GA 30322 (United States)

    2006-06-20

    The intramolecular proton-transfer reaction in 3-hydroxyflavone (3HF) is theoretically studied both in the ground (S{sub 0}) and first singlet excited (S{sub 1}) electronic states. In S{sub 0} the proton-transfer reaction is shown to be quite unfavorable at the DFT (B3LYP) level. However, the back proton transfer is found to be a feasible process with a small energy barrier, both results being in qualitative agreement with known experimental facts. Different theoretical levels are considered and compared for S{sub 1}. The ab initio configuration interaction singles (CIS) method overestimates the energy of S{sub 1} and give too high energy barriers for the proton-transfer reaction. The complete active space SCF (CASSCF) method gives a more reasonable value but the inclusion of the dynamical correlation through second-order perturbation theory (CASPT2) upon CASSCF geometries or the use of the time-dependent DFT (TDDFT) method upon CIS geometries gives a barrierless process. Optimization of geometries (minima and transition-state structures) at the TDDFT level leads to a small but non-negligible energy barrier for the proton-transfer reaction in S{sub 1} and global energies that fit quite well with the known experimental (spectroscopic and femtochemistry) data. Finally the effect of a polar environment is analyzed through a continuum model, which gives only a small difference from the previous gas-phase results. This points out that the remarkable changes in the photochemistry of 3HF observed experimentally are not to be solely attributed to the polarity of the surrounding media.

  15. Investigations of the valence-shell excitations of molecular ethane by high-energy electron scattering

    Science.gov (United States)

    Xu, Wei-Qing; Xu, Long-Quan; Qi, De-Guang; Chen, Tao; Liu, Ya-Wei; Zhu, Lin-Fan

    2018-04-01

    The differential cross sections and generalized oscillator strengths for the low-lying excitations of the valence-shell 1eg orbital electron in ethane have been measured for the first time at a high incident electron energy of 1500 eV and a scattering angular range of 1.5°-10°. A weak feature, termed X here, with a band center of about 7.5 eV has been observed, which was also announced by the previous experimental and theoretical studies. The dynamic behaviors of the generalized oscillator strengths for the 3s (8.7 eV), 3s+3p (9.31 eV, 9.41 eV), and X (˜7.5 eV) transitions on the momentum transfer squared have been obtained. The integral cross sections of these transitions from their thresholds to 5000 eV have been obtained with the aid of the BE-scaling (B is the binding energy and E is the excitation energy) method. The optical oscillator strengths of the above transitions determined by extrapolating their generalized oscillator strengths to the limit of the squared momentum transfer K2 → 0 are in good agreement with the ones from the photoabsorption spectrum [J. W. Au et al., Chem. Phys. 173, 209 (1993)], which indicates that the present differential cross sections, generalized oscillator strengths, and integral cross sections can serve as benchmark data.

  16. Power law scaling for rotational energy transfer

    International Nuclear Information System (INIS)

    Pritchard, D.E.; Smith, N.; Driver, R.D.; Brunner, T.A.

    1979-01-01

    We have applied a new scaling law to several sets of rotational energy transfer cross sections. The new law asserts that the square of the T-matrix depends on the amount of energy transferred as a power law. Two different kinds of angular momentum statistics are assumed, one corresponding to m/sub j/ being conserved and the other corresponding to m/sub j/ being completely randomized. Numerical fits are presented which demonstrate that the data follow the power law better than the widely used exponential gap law

  17. Theory of coherent resonance energy transfer

    International Nuclear Information System (INIS)

    Jang, Seogjoo; Cheng, Y.-C.; Reichman, David R.; Eaves, Joel D.

    2008-01-01

    A theory of coherent resonance energy transfer is developed combining the polaron transformation and a time-local quantum master equation formulation, which is valid for arbitrary spectral densities including common modes. The theory contains inhomogeneous terms accounting for nonequilibrium initial preparation effects and elucidates how quantum coherence and nonequilibrium effects manifest themselves in the coherent energy transfer dynamics beyond the weak resonance coupling limit of the Foerster and Dexter (FD) theory. Numerical tests show that quantum coherence can cause significant changes in steady state donor/acceptor populations from those predicted by the FD theory and illustrate delicate cooperation of nonequilibrium and quantum coherence effects on the transient population dynamics.

  18. Spontaneous Emission and Energy Transfer Rates Near a Coated Metallic Cylinder

    OpenAIRE

    BRADLEY, LOUISE

    2014-01-01

    PUBLISHED The spontaneous emission and energy transfer rates of quantum systems in proximity to a dielectrically coated metallic cylinder are investigated using a Green's tensor formalism. The excitation of surface plasmon modes can significantly modify these rates. The spontaneous emission and energy transfer rates are investigated as a function of the material and dimensions of the core and coating, as well as the emission wavelength of the donor. For the material of the core we consider...

  19. Graphene-based chemiluminescence resonance energy transfer for homogeneous immunoassay.

    Science.gov (United States)

    Lee, Joon Seok; Joung, Hyou-Arm; Kim, Min-Gon; Park, Chan Beum

    2012-04-24

    We report on chemiluminescence resonance energy transfer (CRET) between graphene nanosheets and chemiluminescent donors. In contrast to fluorescence resonance energy transfer, CRET occurs via nonradiative dipole-dipole transfer of energy from a chemiluminescent donor to a suitable acceptor molecule without an external excitation source. We designed a graphene-based CRET platform for homogeneous immunoassay of C-reactive protein (CRP), a key marker for human inflammation and cardiovascular diseases, using a luminol/hydrogen peroxide chemiluminescence (CL) reaction catalyzed by horseradish peroxidase. According to our results, anti-CRP antibody conjugated to graphene nanosheets enabled the capture of CRP at the concentration above 1.6 ng mL(-1). In the CRET platform, graphene played a key role as an energy acceptor, which was more efficient than graphene oxide, while luminol served as a donor to graphene, triggering the CRET phenomenon between luminol and graphene. The graphene-based CRET platform was successfully applied to the detection of CRP in human serum samples in the range observed during acute inflammatory stress.

  20. Dynamics of excited-state intramolecular proton transfer reactions in piroxicam. Role of triplet states

    Science.gov (United States)

    Cho, Dae Won; Kim, Yong Hee; Yoon, Minjoong; Jeoung, Sae Chae; Kim, Dongho

    1994-08-01

    The picosecond time-resolved fluorescence and transient absorption behavior of piroxicam at room temperature are reported. The keto tautomer in the excited singlet state ( 1K*) formed via the fast intramolecular proton transfer (≈ 20 ps) is observed. The short-lived (7.5 ns) triplet state of keto tauomer ( 3K*) is generated from 1K * in toluene whereas it is hardly observed in ethanol. Consequently, rapid reverse proton transfer takes place from 3K * to the enol triplet state ( 3E *.

  1. 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.

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

    International Nuclear Information System (INIS)

    Blom, Alex Jason

    2009-01-01

    Excited state charge transfer processes are studied using the fs/ps-CARS probe technique. This probe allows for multiplexed detection of Raman active vibrational modes. Systems studied include Michler's Ketone, Coumarin 120, 4-dimethylamino-4(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

  3. 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.

  4. Resonant vibrational energy transfer in ice Ih

    Energy Technology Data Exchange (ETDEWEB)

    Shi, L.; Li, F.; Skinner, J. L. [Theoretical Chemistry Institute and Department of Chemistry, University of Wisconsin, Madison, Wisconsin 53706 (United States)

    2014-06-28

    Fascinating anisotropy decay experiments have recently been performed on H{sub 2}O ice Ih by Timmer and Bakker [R. L. A. Timmer, and H. J. Bakker, J. Phys. Chem. A 114, 4148 (2010)]. The very fast decay (on the order of 100 fs) is indicative of resonant energy transfer between OH stretches on different molecules. Isotope dilution experiments with deuterium show a dramatic dependence on the hydrogen mole fraction, which confirms the energy transfer picture. Timmer and Bakker have interpreted the experiments with a Förster incoherent hopping model, finding that energy transfer within the first solvation shell dominates the relaxation process. We have developed a microscopic theory of vibrational spectroscopy of water and ice, and herein we use this theory to calculate the anisotropy decay in ice as a function of hydrogen mole fraction. We obtain very good agreement with experiment. Interpretation of our results shows that four nearest-neighbor acceptors dominate the energy transfer, and that while the incoherent hopping picture is qualitatively correct, vibrational energy transport is partially coherent on the relevant timescale.

  5. Exciplex formation and energy transfer in a self-assembled metal-organic hybrid system.

    Science.gov (United States)

    Haldar, Ritesh; Rao, K Venkata; George, Subi J; Maji, Tapas Kumar

    2012-05-07

    Exciting assemblies: A metal-organic self-assembly of pyrenebutyric acid (PBA), 1,10-phenanthroline (o-phen), and Mg(II) shows solid-state fluorescence originating from a 1:1 PBA-o-phen exciplex. This exciplex fluorescence is sensitized by another residual PBA chromophore through an excited-state energy-transfer process. The solvent polarity modulates the self-assembly and the corresponding exciplex as well as the energy transfer, resulting in tunable emission of the hybrid (see figure). Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  6. A method of measurement of lifetimes of excited ion levels, using orientation transfer by Penning collisions

    International Nuclear Information System (INIS)

    Hamel, J.; Barrat, J.-P.

    1978-01-01

    A method for measuring the lifetimes of ionic excited levels is described. This method uses the transfer of coherence in a Penning collision using metastable optically oriented He 2 3 S 1 atoms. If R.F. transitions are induced in the (2 3 S 1 )He level, a transverse component of the magnetic moment of this level is created, which precesses coherently at the angular frequency ω of the R.F. field. The helium transverse orientation is partially transferred to the ions produced by Penning collisions. After the collision, the orientation transferred precesses around the external magnetic field at the Larmor frequency ω 0 ' of the ion excited level. The degree of orientation of the excited ion level depends, in the stationary state, on the average phase shift, during the lifetime tau prime of this level, between the Larmor precession at angular frequency ω 0 ' and the forced precession of helium (at angular frequency ω). The orientation of the ions is monitored by the modulation of the light emitted during their radiative decay. It is possible to determine the lifetime tau prime by measuring the degree of modulation of the reemitted light as a function of ω [fr

  7. Electronic structure and charge transfer excited states of endohedral fullerene containing electron donoracceptor complexes utilized in organic photovoltaics

    Science.gov (United States)

    Amerikheirabadi, Fatemeh

    Organic Donor-Acceptor complexes form the main component of the organic photovoltaic devices (OPVs). The open circuit voltage of OPVs is directly related to the charge transfer excited state energies of these complexes. Currently a large number of different molecular complexes are being tested for their efficiency in photovoltaic devices. In this work, density functional theory as implemented in the NRLMOL code is used to investigate the electronic structure and related properties of these donor-acceptor complexes. The charge transfer excitation energies are calculated using the perturbative delta self-consistent field method recently developed in our group as the standard time dependent density functional approaches fail to accurately provide them. The model photovoltaics systems analyzed are as follows: Sc3N C 80--ZnTPP, Y3 N C80-- ZnTPP and Sc3 N C80-- ZnPc. In addition, a thorough analysis of the isolated donor and acceptor molecules is also provided. The studied acceptors are chosen from a class of fullerenes named trimetallic nitride endohedral fullerenes. These molecules have shown to possess advantages as acceptors such as long lifetimes of the charge-separated states.

  8. Vibrational energy transfer in hydrogen liquid and its isotopes

    International Nuclear Information System (INIS)

    Gale, G.M.; Delalande, C.

    1978-01-01

    The transfer of vibrational energy (V-V) from H 2 to isotopic impurities (HD or D 2 ) has been studied in the liquid state, between 15 and 30 K. The subsequent ralaxation (V-T) of the excited impurity by the H 2 liquid host has also been measured and contrasted with the vibrational relaxation behaviour of pure H 2 and D 2 liquids. The isothermal density dependence of both V-V and V-T transfer has been investigated in the fluid state at 30 K. High density relaxation rates are also compared to the data in the pure gases and to other available gas phase results. Measurements in the solid, near the triple-point temperature, are equally reported for each process studied. (Auth.)

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

    Science.gov (United States)

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

    2017-09-01

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

  10. A new energy transfer channel from carotenoids to chlorophylls in purple bacteria.

    Science.gov (United States)

    Feng, Jin; Tseng, Chi-Wei; Chen, Tingwei; Leng, Xia; Yin, Huabing; Cheng, Yuan-Chung; Rohlfing, Michael; Ma, Yuchen

    2017-07-10

    It is unclear whether there is an intermediate dark state between the S 2 and S 1 states of carotenoids. Previous two-dimensional electronic spectroscopy measurements support its existence and its involvement in the energy transfer from carotenoids to chlorophylls, but there is still considerable debate on the origin of this dark state and how it regulates the energy transfer process. Here we use ab initio calculations on excited-state dynamics and simulated two-dimensional electronic spectrum of carotenoids from purple bacteria to provide evidence supporting that the dark state may be assigned to a new A g + state. Our calculations also indicate that groups on the conjugation backbone of carotenoids may substantially affect the excited-state levels and the energy transfer process. These results contribute to a better understanding of carotenoid excited states.Carotenoids harvest energy from light and transfer it to chlorophylls during photosynthesis. Here, Feng et al. perform ab initio calculations on excited-state dynamics and simulated 2D electronic spectrum of carotenoids, supporting the existence of a new excited state in carotenoids.

  11. Energy transfer mechanism in CsI:Eu crystal

    International Nuclear Information System (INIS)

    Yakovlev, V.; Trefilova, L.; Karnaukhova, A.; Ovcharenko, N.

    2014-01-01

    This paper studies the scintillation process in CsI:Eu crystal exposed to the pulse electron irradiation (E=0.25 MeV, t 1/2 =15 ns and W=0.003 J/cm 2 ). It has been proved that the energy transfer from the lattice to Eu 2+ ions in CsI:Eu occurs through the re-absorption of STE emission. The proposed model rests on the following experimental facts: (1) the activator emission at 2.68 eV rises gradually after the decay of the excitation pulse even at temperature lower than 90 K when V k centers are immobile; (2) the rise time of 2.68 eV emission and the decay time of STE emission have the same temperature dependences at T=78–300 K; (3) the excitation spectrum of 2.68 eV emission overlaps the emission spectrum of STE. -- Highlights: • The scintillation process in CsI:Eu was studied under pulsed electron irradiation. • A model of the energy transfer from the lattice to Eu 2+ ions in CsI:Eu was proposed. • Eu 2+ ions in CsI:Eu reabsorb the π-emission of self-trapped excitons

  12. Energy transfer in scattering by rotating potentials

    Indian Academy of Sciences (India)

    R. Narasimhan (Krishtel eMaging) 1461 1996 Oct 15 13:05:22

    Quantum mechanical scattering theory is studied for time-dependent. Schrödinger ... the energy transferred to a particle by collision with a rotating blade. Keywords. ..... terms of the unitary group for some time-independent generator. This will ...

  13. Contribution of Jahn-Teller and charge transfer excitations to the photovoltaic effect of manganite/titanite heterojunctions

    Science.gov (United States)

    Ifland, Benedikt; Hoffmann, Joerg; Kressdorf, Birte; Roddatis, Vladimir; Seibt, Michael; Jooss, Christian

    2017-06-01

    The effect of correlation effects on photovoltaic energy conversion at manganite/titanite heterojunctions is investigated. As a model system we choose a heterostructure consisting of the small polaron absorber Pr0.66Ca0.34MnO3 (PCMO) epitaxially grown on single-crystalline Nb-doped SrTi0.998Nb0.002O3 (STNO) substrates. The high structural and chemical quality of the interfaces is proved by detailed characterization using high-resolution transmission electron microscopy (TEM) and electron energy loss spectroscopy (EELS) studies. Spectrally resolved and temperature-dependent photovoltaic measurements show pronounced contributions of both the Jahn-Teller (JT) excitations and the charge transfer (CT) transitions to the photovoltaic effect at different photon energies. A linear temperature dependence of the open-circuit voltage for an excitation in the PCMO manganite is only observed below the charge-ordering temperature, indicating that the diffusion length of the photocarrier exceeds the size of the space charge region. The photovoltaic response is compared to that of a heterojunction of lightly doped Pr0.05Ca0.95MnO3 (CMO)/STNO, where the JT transition is absent. Here, significant contributions of the CT transition to the photovoltaic effect set in below the Neel temperature. We conclude that polaronic correlations and ordering effects are essentials for photovoltaic energy conversion in manganites.

  14. Luminescence of the SrCl2:Pr crystals under high-energy excitation

    International Nuclear Information System (INIS)

    Antonyak, O.T.; Voloshinovskii, A.S.; Vistovskyy, V.V.; Stryganyuk, G.B.; Kregel, O.P.

    2014-01-01

    The present research was carried out in order to elucidate the mechanisms of energy transfer from the crystal lattice to Pr 3+ ions in SrCl 2 . The luminescence excitation and emission spectra as well as luminescence kinetics of the SrCl 2 :Pr single crystals containing 0.2 mol% Pr were investigated at 300 and 10 K using the vacuum ultraviolet (VUV) synchrotron radiation. The X-ray excited luminescence spectra of the SrCl 2 :Pr (C Pr =0.2 and 0.5 mol%) and SrCl 2 :Pr, K (C Pr =1.5 mol%; C K =1.5 mol%) crystals were studied at 294 and 80 K. Under optical excitation of the samples in the Pr 3+ absorption bands, there were observed five fast ultraviolet emissions assigned to the 4f 1 5d→4f 2 transitions, and two long-wave bands corresponding to the f–f transitions. Furthermore, the intrinsic emission bands of SrCl 2 were observed at 10 K. The X-ray excited luminescence spectrum of the SrCl 2 :Pr crystal containing 0.2 mol% Pr, besides intrinsic emission band near 400 nm, has got a long-wave band at about 490 nm of the Pr 3+ centers. There were not observed any emission bands of the Pr 3+ centers corresponding to the 4f 1 5d–4f 2 transitions in the X-ray excited luminescence spectrum of the SrCl 2 :Pr crystal. The possible mechanisms of energy transfer from the SrCl 2 matrix to the Pr 3+ centers are discussed. -- Highlights: • Spectral-luminescent properties of SrCl 2 :Pr have been investigated. • The identification of emission 4f–4f and 5d–4f bands of Pr 3+ ions was performed. • Adding of potassium prevents clustering of the Pr 3+ centers in the SrCl 2 :Pr, K crystals. • Under X-ray excitation at 80–300 K only Pr 3+ 4f–4f and intrinsic emission is observed

  15. Excited State Charge Transfer reaction with dual emission from 5-(4-dimethylamino-phenyl)-penta-2,4-dienenitrile: Spectral measurement and theoretical density functional theory calculation

    Science.gov (United States)

    Jana, Sankar; Dalapati, Sasanka; Ghosh, Shalini; Kar, Samiran; Guchhait, Nikhil

    2011-07-01

    The excited state intramolecular charge transfer process in donor-chromophore-acceptor system 5-(4-dimethylamino-phenyl)-penta-2,4-dienenitrile (DMAPPDN) has been investigated by steady state absorption and emission spectroscopy in combination with Density Functional Theory (DFT) calculations. This flexible donor acceptor molecule DMAPPDN shows dual fluorescence corresponding to emission from locally excited and charge transfer state in polar solvent. Large solvatochromic emission shift, effect of variation of pH and HOMO-LUMO molecular orbital pictures support excited state intramolecular charge transfer process. The experimental findings have been correlated with the calculated structure and potential energy surfaces based on the Twisted Intramolecular Charge Transfer (TICT) model obtained at DFT level using B3LYP functional and 6-31+G( d, p) basis set. The theoretical potential energy surfaces for the excited states have been generated in vacuo and acetonitrile solvent using Time Dependent Density Functional Theory (TDDFT) and Time Dependent Density Functional Theory Polarized Continuum Model (TDDFT-PCM) method, respectively. All the theoretical results show well agreement with the experimental observations.

  16. Plunger lifetime measurements after Coulomb excitation at intermediate beam energies

    Energy Technology Data Exchange (ETDEWEB)

    Hackstein, Matthias; Dewald, Alfred; Fransen, Christoph; Ilie, Gabriela; Jolie, Jan; Melon, Barbara; Pissulla, Thomas; Rother, Wolfram; Zell, Karl-Oskar [University of Cologne (Germany); Petkov, Pavel [University of Cologne (Germany); INRNE (Bulgaria); Chester, Aaron; Adrich, Przemyslaw; Bazin, Daniel; Bowen, Matt; Gade, Alexandra; Glasmacher, Thomas; Miller, Dave; Moeller, Victoria; Starosta, Krzysztof; Stolz, Andreas; Vaman, Constantin; Voss, Philip; Weissharr, Dirk [Michigan State Univerity (United States); Moeller, Oliver [TU Darmstadt (Germany)

    2008-07-01

    Two recoil-distance-doppler-shift (RDDS) experiments were performed at the NSCL/MSU using Coulomb excitations of the projectile nuclei {sup 110}Pd, {sup 114}Pd at beam energies of 54 MeV/u in order to investigate the evolution of deformation of neutron rich paladium isotopes. The experimental set-up consisted of a dedicated plunger device, developed at the University of Cologne, the SEGA Ge-array and the S800 spectrometer. Lifetimes of the 2{sub 1}{sup +}-states in {sup 110}Pd and {sup 114}Pd were derived from the analysis of the {gamma}-line-shapes as well as from the measured decay-curves. Special features of the data analysis, e.g. features originating from the very high recoil velocities, are discussed.

  17. Collective and single-particle states at high excitation energy

    International Nuclear Information System (INIS)

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

    2000-01-01

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

  18. Homopolar machine for reversible energy storage and transfer systems

    Science.gov (United States)

    Stillwagon, Roy E.

    1978-01-01

    A homopolar machine designed to operate as a generator and motor in reversibly storing and transferring energy between the machine and a magnetic load coil for a thermo-nuclear reactor. The machine rotor comprises hollow thin-walled cylinders or sleeves which form the basis of the system by utilizing substantially all of the rotor mass as a conductor thus making it possible to transfer substantially all the rotor kinetic energy electrically to the load coil in a highly economical and efficient manner. The rotor is divided into multiple separate cylinders or sleeves of modular design, connected in series and arranged to rotate in opposite directions but maintain the supply of current in a single direction to the machine terminals. A stator concentrically disposed around the sleeves consists of a hollow cylinder having a number of excitation coils each located radially outward from the ends of adjacent sleeves. Current collected at an end of each sleeve by sleeve slip rings and brushes is transferred through terminals to the magnetic load coil. Thereafter, electrical energy returned from the coil then flows through the machine which causes the sleeves to motor up to the desired speed in preparation for repetition of the cycle. To eliminate drag on the rotor between current pulses, the brush rigging is designed to lift brushes from all slip rings in the machine.

  19. Homopolar machine for reversible energy storage and transfer systems

    International Nuclear Information System (INIS)

    Stillwagon, R.E.

    1981-01-01

    A homopolar machine designed to operate as a generator and motor in reversibly storing and transferring energy between the machine and a magnetic load coil for a thermo-nuclear reactor. The machine rotor comprises hollow thin-walled cylinders or sleeves which form the basis of the system by utilizing substantially all of the rotor mass as a conductor thus making it possible to transfer substantially all the rotor kinetic energy electrically to the load coil in a highly economical and efficient manner. The rotor is divided into multiple separate cylinders or sleeves of modular design, connected in series and arranged to rotate in opposite directions but maintain the supply of current in a single direction to the machine terminals. A stator concentrically disposed around the sleeves consists of a hollow cylinder having a number of excitation coils each located radially outward from the ends of adjacent sleeves. Current collected at an end of each sleeve by sleeve slip rings and brushes is transferred through terminals to the magnetic load coil. Thereafter, electrical energy returned from the coil then flows through the machine which causes the sleeves to motor up to the desired speed in preparation for repetition of the cycle. To eliminate drag on the rotor between current pulses, the brush rigging is designed to lift brushes from all slip rings in the machine

  20. Radiative charge-transfer lifetime of the excited state of (NaCa)+

    International Nuclear Information System (INIS)

    Makarov, Oleg P.; Cote, R.; Michels, H.; Smith, W.W.

    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. We study the collisional cooling of laser precooled Ca + ions by ultracold Na atoms. Modeling this process requires knowledge of the radiative lifetime of the excited singlet A 1 Σ + 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 Moeller-Plesset second-order perturbation theory 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 rate coefficient for charge transfer was found to be 2.3x10 -16 cm 3 /sec, while those for the elastic and spin-exchange cross sections were found to be several orders of magnitude higher (1.1x10 -8 cm 3 /sec and 2.3x10 -9 cm 3 /sec, respectively). This confirms our assumption that the milli-Kelvin regime of collisional cooling of calcium ions by sodium atoms is favorable with the respect to low loss of calcium ions due to the charge transfer

  1. Risk transfer via energy savings insurance

    Energy Technology Data Exchange (ETDEWEB)

    Mills, Evan

    2001-10-01

    Among the key barriers to investment in energy efficiency improvements are uncertainties about attaining projected energy savings and apprehension about potential disputes over these savings. The fields of energy management and risk management are thus intertwined. While many technical methods have emerged to manage performance risks (e.g. building commissioning), financial risk transfer techniques are less developed in the energy management arena than in other more mature segments of the economy. Energy Savings Insurance (ESI) - formal insurance of predicted energy savings - is one method of transferring financial risks away from the facility owner or energy services contractor. ESI offers a number of significant advantages over other forms of financial risk transfer, e.g. savings guarantees or performance bonds. ESI providers manage risk via pre-construction design review as well as post-construction commissioning and measurement and verification of savings. We found that the two mos t common criticisms of ESI - excessive pricing and onerous exclusions - are not born out in practice. In fact, if properly applied, ESI can potentially reduce the net cost of energy savings projects by reducing the interest rates charged by lenders, and by increasing the level of savings through quality control. Debt service can also be ensured by matching loan payments to projected energy savings while designing the insurance mechanism so that payments are made by the insurer in the event of a savings shortfall. We estimate the U.S. ESI market potential of $875 million/year in premium income. From an energy-policy perspective, ESI offers a number of potential benefits: ESI transfers performance risk from the balance sheet of the entity implementing the energy savings project, thereby freeing up capital otherwise needed to ''self-insure'' the savings. ESI reduces barriers to market entry of smaller energy services firms who do not have sufficiently strong balance

  2. Risk transfer via energy savings insurance; TOPICAL

    International Nuclear Information System (INIS)

    Mills, Evan

    2001-01-01

    Among the key barriers to investment in energy efficiency improvements are uncertainties about attaining projected energy savings and apprehension about potential disputes over these savings. The fields of energy management and risk management are thus intertwined. While many technical methods have emerged to manage performance risks (e.g. building commissioning), financial risk transfer techniques are less developed in the energy management arena than in other more mature segments of the economy. Energy Savings Insurance (ESI) - formal insurance of predicted energy savings - is one method of transferring financial risks away from the facility owner or energy services contractor. ESI offers a number of significant advantages over other forms of financial risk transfer, e.g. savings guarantees or performance bonds. ESI providers manage risk via pre-construction design review as well as post-construction commissioning and measurement and verification of savings. We found that the two mos t common criticisms of ESI - excessive pricing and onerous exclusions - are not born out in practice. In fact, if properly applied, ESI can potentially reduce the net cost of energy savings projects by reducing the interest rates charged by lenders, and by increasing the level of savings through quality control. Debt service can also be ensured by matching loan payments to projected energy savings while designing the insurance mechanism so that payments are made by the insurer in the event of a savings shortfall. We estimate the U.S. ESI market potential of$875 million/year in premium income. From an energy-policy perspective, ESI offers a number of potential benefits: ESI transfers performance risk from the balance sheet of the entity implementing the energy savings project, thereby freeing up capital otherwise needed to ''self-insure'' the savings. ESI reduces barriers to market entry of smaller energy services firms who do not have sufficiently strong balance sheets to self

  3. Charge-transfer excited state in pyrene-1-carboxylic acids adsorbed on titanium dioxide nanoparticles

    Science.gov (United States)

    Krawczyk, S.; Nawrocka, A.; Zdyb, A.

    2018-06-01

    The electronic structure of excited photosensitizer adsorbed at the surface of a solid is the key factor in the electron transfer processes that underlie the efficiency of dye-sensitized solar cells and photocatalysts. In this work, Stark effect (electroabsorption) spectroscopy has been used to measure the polarizability and dipole moment changes in electronic transitions of pyrene-1-carboxylic (PCA), -acetic (PAA) and -butyric (PBA) acids in ethanol, both free and adsorbed on colloidal TiO2, in glassy ethanol at low temperature. The lack of appreciable increase of dipole moment in the excited state of free and adsorbed PAA and PBA points that two or more single bonds completely prevent the expansion of π-electrons from the aromatic ring towards the carboxylic group, thus excluding the possibility of direct electron injection into TiO2. In free PCA, the pyrene's forbidden S0 → S1 transition has increased intensity, exhibits a long progression in 1400 cm-1 Ag mode and is associated with |Δμ| of 2 D. Adsorption of PCA on TiO2 causes a broadening and red shift of the S0 → S1 absorption band and an increase in dipole moment change on electronic excitation to |Δμ| = 6.5 D. This value increased further to about 15 D when the content of acetic acid in the colloid was changed from 0.2% to 2%, and this effect is ascribed to the surface electric field. The large increase of |Δμ| points that the electric field effect can not only change the energetics of electron transfer from the excited sensitizer into the solid, but can also shift the molecular electronic density, thus directly influencing the electronic coupling factor relevant for electron transfer at the molecule-solid interface.

  4. Geometry effect on energy transfer rate in a coupled-quantum-well structure: nonlinear regime

    International Nuclear Information System (INIS)

    Salavati-fard, T; Vazifehshenas, T

    2014-01-01

    We study theoretically the effect of geometry on the energy transfer rate at nonlinear regime in a coupled-quantum-well system using the balance equation approach. To investigate comparatively the effect of both symmetric and asymmetric geometry, different structures are considered. The random phase approximation dynamic dielectric function is employed to include the contributions from both quasiparticle and plasmon excitations. Also, the short-range exchange interaction is taken into account through the Hubbard approximation. Our numerical results show that the energy transfer rate increases by increasing the well thicknesses in symmetric structures. Furthermore, by increasing spatial asymmetry, the energy transfer rate decreases for the electron temperature range of interest. From numerical calculations, it is obtained that the nonlinear energy transfer rate is proportional to the square of electron drift velocity in all structures and also, found that the influence of Hubbard local field correction on the energy transfer rate gets weaker by increasing the strength of applied electric field. (paper)

  5. Dielectronic recombination and resonant transfer excitation processes for helium-like krypton

    Institute of Scientific and Technical Information of China (English)

    Hu Xiao-Li; Qu Yi-Zhi; Zhang Song-Bin; Zhang Yu

    2012-01-01

    The relativistic configuration interaction method is employed to calculate the dielectronic recombination (DR) cross sections of helium-like krypton via the 1s21nl' (n =2,3,...,15) resonances.Then,the resonant transfer excitation (RTE) processes of Kr34+ colliding with H,He,H2,and CHx (x =0-4) targets are investigated under the impulse approximation.The needed Compton profiles of targets are obtained from the Hartree-Fock wave functions.The RTE cross sections are strongly dependent on DR resonant energies and strengths,and the electron momentum distributions of the target.For H2 and H targets,the ratio of their RTE cross sections changes from 1.85 for the 1s2121' to 1.88 for other resonances,which demonstrates the weak molecular effects on the Compton profiles of H2.For CHx (x =0-4) targets,the main contribution to the RTE cross section comes from the carbon atom since carbon carries 6 electrons;as the number of hydrogen increases in CHx,the RTE cross section almost increases by the same value,displaying the strong separate atom character for the hydrogen.However,further comparison of the individual orbital contributions of C(2p,2s,ls) and CH4(1t2,2a1,1a1) to the RTE cross sections shows that the molecular effects induce differences of about 25.1%,19.9%,and 0.2% between 2p-1t2,2s-2a1,and 1s-1a1 orbitals,respectively.

  6. Resonance Raman spectra of organic molecules absorbed on inorganic semiconducting surfaces: Contribution from both localized intramolecular excitation and intermolecular charge transfer excitation

    International Nuclear Information System (INIS)

    Ye, ChuanXiang; Zhao, Yi; Liang, WanZhen

    2015-01-01

    The time-dependent correlation function approach for the calculations of absorption and resonance Raman spectra (RRS) of organic molecules absorbed on semiconductor surfaces [Y. Zhao and W. Z. Liang, J. Chem. Phys. 135, 044108 (2011)] is extended to include the contribution of the intermolecular charge transfer (CT) excitation from the absorbers to the semiconducting nanoparticles. The results demonstrate that the bidirectionally interfacial CT significantly modifies the spectral line shapes. Although the intermolecular CT excitation makes the absorption spectra red shift slightly, it essentially changes the relative intensities of mode-specific RRS and causes the oscillation behavior of surface enhanced Raman spectra with respect to interfacial electronic couplings. Furthermore, the constructive and destructive interferences of RRS from the localized molecular excitation and CT excitation are observed with respect to the electronic coupling and the bottom position of conductor band. The interferences are determined by both excitation pathways and bidirectionally interfacial CT

  7. Risk transfer via energy-savings insurance

    International Nuclear Information System (INIS)

    Mills, Evan

    2003-01-01

    Among the key barriers to investment in energy efficiency are uncertainties about attaining projected energy savings and potential disputes over stipulated savings. The fields of energy management and risk management are thus intertwined. While many technical methods have emerged to manage performance risks (e.g. building diagnostics and commissioning), financial methods are less developed in the energy management arena than in other segments of the economy. Energy-savings insurance (ESI) - formal insurance of predicted energy savings - transfers and spreads both types of risk over a larger pool of energy efficiency projects and reduces barriers to market entry of smaller energy service firms who lack sufficiently strong balance sheets to self-insure the savings. ESI encourages those implementing energy-saving projects to go beyond standard measures and thereby achieve more significant levels of energy savings. Insurance providers are proponents of improved savings measurement and verification techniques, as well as maintenance, thereby contributing to national energy-saving objectives. If properly applied, ESI can potentially reduce the net cost of energy-saving projects by reducing the interest rates charged by lenders, and by increasing the level of savings through quality control. Governmental agencies have been pioneers in the use of ESI and could continue to play a role

  8. Spin–transfer torque oscillator in magnetic tunneling junction with short–wavelength magnon excitation

    Directory of Open Access Journals (Sweden)

    Shizhu Qiao

    2018-05-01

    Full Text Available Bloch–Bloembergen–Slonczewski (BBS equation is established by extending Bloch–Bloembergen equation, and it is used to study magnetization oscillation in the free magnetic layer of a magnetic tunneling junction. Since both short–wavelength magnon excitation and spin–transfer torque are taken into account in the BBS equation, it is distinguished from Landau–Lifshitz–Gilbert–Slonczewski equation. The macro–spin BBS model predicts that the transverse relaxation time in free magnetic layer should be long enough, as compared with the longitudinal relaxation time, to achieve stable magnetization oscillation for spin–transfer torque oscillator application. Moreover, field–like torque favors the tolerance of fast transverse relaxation, which makes magnetic tunneling junction a better choice than spin valve for the spin–transfer torque oscillator application.

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

    International Nuclear Information System (INIS)

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

    1997-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1997-04-01

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

  11. Excitation energy of the fragments produced in central collisions of Xe + Sn at intermediate energies

    International Nuclear Information System (INIS)

    Hudan, S.; Chbihi, A.; Frankland, J.D.

    2000-01-01

    Characteristics of the primary fragments produced in central collisions of Xe + Sn system from 32 to 50 AMeV have been deduced. By using the relative velocity correlation technique between the light charged particles (LCP) and detected fragments, we were able to extract the multiplicities and average kinetic energy of the secondary evaporated LCP. We then reconstructed the size and excitation energy of the primary fragments. For each bombarding energy a constant value of the excitation energy per nucleon, over the whole range of fragment charge has been found, suggesting that on the average thermodynamical equilibrium has been achieved at the freeze-out. This value increases slightly from 2.8 to 3.8 AMeV with a large increase of bombarding energy, 32 to 50 AMeV. (authors)

  12. Excitation energy of the fragments produced in central collisions of Xe + Sn at intermediate energies

    Energy Technology Data Exchange (ETDEWEB)

    Hudan, S.; Chbihi, A.; Frankland, J.D. [Grand Accelerateur National d' Ions Lourds (GANIL), 14 - Caen (France)] [and others

    2000-07-01

    Characteristics of the primary fragments produced in central collisions of Xe + Sn system from 32 to 50 AMeV have been deduced. By using the relative velocity correlation technique between the light charged particles (LCP) and detected fragments, we were able to extract the multiplicities and average kinetic energy of the secondary evaporated LCP. We then reconstructed the size and excitation energy of the primary fragments. For each bombarding energy a constant value of the excitation energy per nucleon, over the whole range of fragment charge has been found, suggesting that on the average thermodynamical equilibrium has been achieved at the freeze-out. This value increases slightly from 2.8 to 3.8 AMeV with a large increase of bombarding energy, 32 to 50 AMeV. (authors)

  13. Electronic energy transfer through non-adiabatic vibrational-electronic resonance. I. Theory for a dimer

    Science.gov (United States)

    Tiwari, Vivek; Peters, William K.; Jonas, David M.

    2017-10-01

    Non-adiabatic vibrational-electronic resonance in the excited electronic states of natural photosynthetic antennas drastically alters the adiabatic framework, in which electronic energy transfer has been conventionally studied, and suggests the possibility of exploiting non-adiabatic dynamics for directed energy transfer. Here, a generalized dimer model incorporates asymmetries between pigments, coupling to the environment, and the doubly excited state relevant for nonlinear spectroscopy. For this generalized dimer model, the vibrational tuning vector that drives energy transfer is derived and connected to decoherence between singly excited states. A correlation vector is connected to decoherence between the ground state and the doubly excited state. Optical decoherence between the ground and singly excited states involves linear combinations of the correlation and tuning vectors. Excitonic coupling modifies the tuning vector. The correlation and tuning vectors are not always orthogonal, and both can be asymmetric under pigment exchange, which affects energy transfer. For equal pigment vibrational frequencies, the nonadiabatic tuning vector becomes an anti-correlated delocalized linear combination of intramolecular vibrations of the two pigments, and the nonadiabatic energy transfer dynamics become separable. With exchange symmetry, the correlation and tuning vectors become delocalized intramolecular vibrations that are symmetric and antisymmetric under pigment exchange. Diabatic criteria for vibrational-excitonic resonance demonstrate that anti-correlated vibrations increase the range and speed of vibronically resonant energy transfer (the Golden Rule rate is a factor of 2 faster). A partial trace analysis shows that vibronic decoherence for a vibrational-excitonic resonance between two excitons is slower than their purely excitonic decoherence.

  14. Ion-ion interaction and energy transfer of 4+ transuranium ions in cerium tetrafluoride

    International Nuclear Information System (INIS)

    Liu, G.K.; Beitz, J.V.

    1990-01-01

    Dynamics of excited 5f electron states of the transuranium ions Cm 4+ and Bk 4+ in CeF 4 are compared. Based on time- and wavelength-resolved laser-induced fluorescence, excitation energy transfer processes have been probed. Depending on concentration and electronic energy level structure of the studied 4+ transuranium ion, the dominant energy transfer mechanisms were identified as cross relaxation, exciton-exciton annihilation, and trapping. Energy transfer rates derived from the fitting of the observed fluorescence decays to theoretical models, based on electric multipolar ion-ion interactions, are contrasted with prior studies of 4f states of 3+ lanthanide and 3d states of transition metal ions. 16 refs., 1 tab

  15. Far-field RF energy transfer and harvesting

    NARCIS (Netherlands)

    Visser, H.J.; Vullers, R.; Briand, D.; Yeatman, E.; Roundy, S.

    2015-01-01

    This chapter deals with radio frequency (RF) energy transfer over a distance. After explaining the differences between nonradiative and radiative RF energy transfer, the chapter gives definitions for transfer and harvesting. Nonradiative RF energy transfer is mostly employed in inductive systems,

  16. Modelling excitonic energy transfer in the photosynthetic unit of purple bacteria

    International Nuclear Information System (INIS)

    Linnanto, J.M.; Korppi-Tommola, J.E.I.

    2009-01-01

    Molecular mechanics and quantum chemical configuration interaction calculations in combination with exciton theory were used to predict vibronic energies and eigenstates of light harvesting antennae and the reaction centre and to evaluate excitation energy transfer rates in the photosynthetic unit of purple bacteria. Excitation energy transfer rates were calculated by using the transition matrix formalism and exciton basis sets of the interacting antenna systems. Energy transfer rates of 600-800 fs from B800 ring to B850 ring in the LH2 antenna, 3-10 ps from LH2 to LH2 antenna, 2-8 ps from LH2 to LH1 antenna and finally 30-70 ps from LH1 to the reaction centre were obtained. Dependencies of energy transfer rates on lateral and vertical inter-complex distances were determined. The results indicate that a fair amount of spatial heterogeneity of antenna complexes in the photosynthetic membrane is tolerated without much loss in excitation energy transfer efficiency

  17. Modelling excitonic energy transfer in the photosynthetic unit of purple bacteria

    Energy Technology Data Exchange (ETDEWEB)

    Linnanto, J.M. [Department of Chemistry, P.O. Box 35, FIN-40014 University of Jyvaeskylae, Jyvaeskylae (Finland)], E-mail: juha.m.linnanto@jyu.fi; Korppi-Tommola, J.E.I. [Department of Chemistry, P.O. Box 35, FIN-40014 University of Jyvaeskylae, Jyvaeskylae (Finland)

    2009-02-23

    Molecular mechanics and quantum chemical configuration interaction calculations in combination with exciton theory were used to predict vibronic energies and eigenstates of light harvesting antennae and the reaction centre and to evaluate excitation energy transfer rates in the photosynthetic unit of purple bacteria. Excitation energy transfer rates were calculated by using the transition matrix formalism and exciton basis sets of the interacting antenna systems. Energy transfer rates of 600-800 fs from B800 ring to B850 ring in the LH2 antenna, 3-10 ps from LH2 to LH2 antenna, 2-8 ps from LH2 to LH1 antenna and finally 30-70 ps from LH1 to the reaction centre were obtained. Dependencies of energy transfer rates on lateral and vertical inter-complex distances were determined. The results indicate that a fair amount of spatial heterogeneity of antenna complexes in the photosynthetic membrane is tolerated without much loss in excitation energy transfer efficiency.

  18. Direct determination of resonance energy transfer in photolyase: structural alignment for the functional state.

    Science.gov (United States)

    Tan, Chuang; Guo, Lijun; Ai, Yuejie; Li, Jiang; Wang, Lijuan; Sancar, Aziz; Luo, Yi; Zhong, Dongping

    2014-11-13

    Photoantenna is essential to energy transduction in photoinduced biological machinery. A photoenzyme, photolyase, has a light-harvesting pigment of methenyltetrahydrofolate (MTHF) that transfers its excitation energy to the catalytic flavin cofactor FADH¯ to enhance DNA-repair efficiency. Here we report our systematic characterization and direct determination of the ultrafast dynamics of resonance energy transfer from excited MTHF to three flavin redox states in E. coli photolyase by capturing the intermediates formed through the energy transfer and thus excluding the electron-transfer quenching pathway. We observed 170 ps for excitation energy transferring to the fully reduced hydroquinone FADH¯, 20 ps to the fully oxidized FAD, and 18 ps to the neutral semiquinone FADH(•), and the corresponding orientation factors (κ(2)) were determined to be 2.84, 1.53 and 1.26, respectively, perfectly matching with our calculated theoretical values. Thus, under physiological conditions and over the course of evolution, photolyase has adopted the optimized orientation of its photopigment to efficiently convert solar energy for repair of damaged DNA.

  19. Electron emission from materials at low excitation energies

    International Nuclear Information System (INIS)

    Urma, N.; Kijek, M.; Millar, J.J.

    1996-01-01

    Full text: An experimental system has been designed and developed with the purpose of measuring the total electron emission yield from materials at low energy excitation. In the first instance the reliability of the system was checked by measuring the total electron emission yield for a well defined surface (aluminium 99.45%). The obtained data was in the expected range given by the literature, and consequently the system will be used further for measuring the total electron yield for a range of materials with interest in the instrumentation industry. We intend to measure the total electron emission yield under electron bombardment as a function of incident electron energy up to 1200 eV, angle of incidence, state of the surface and environment to which the surface has been exposed. Dependence of emission on total electron irradiated dose is also of interest. For many practical application of the 'Secondary Electron Emission', the total electron yield is desired to be as large as possible. The above phenomenon has practical applicability in electron multiplier tube and Scanning electron microscopy - when by means of the variation of the yield of the emitted electrons one may produce visible images of small sample areas. The electron multiplier tube, is a device which utilises the above effect to detect and amplify both single particles and low currents streams of charged particles. The majority of electron tubes use electrons with low energy, hundreds of eV. Not a lot has been published in the literature about this regime and also about the emission when the impinging electrons have small energy, up to 1 KeV. The information obtained from the experimental measurements concerning the total electron emission yield is used to asses the investigated materials as a potential electron emitting surfaces or dynodes in an electron multiplier tube

  20. Classical/quantum correspondence in state selective charge transfer and excitation reactions involving highly charged ions and hydrogen

    International Nuclear Information System (INIS)

    Purkait, M

    2009-01-01

    State selective charge transfer and excitation cross sections for collisions of Ne q+ (q = 1-10) with atomic hydrogen are calculated within the framework of Classical Trajectory Monte Carlo (CTMC) method and Boundary Corrected Continuum Intermediate State (BCCIS) approximation.

  1. Energy harvesting from human motion: exploiting swing and shock excitations

    International Nuclear Information System (INIS)

    Ylli, K; Hoffmann, D; Willmann, A; Becker, P; Folkmer, B; Manoli, Y

    2015-01-01

    Modern compact and low power sensors and systems are leading towards increasingly integrated wearable systems. One key bottleneck of this technology is the power supply. The use of energy harvesting techniques offers a way of supplying sensor systems without the need for batteries and maintenance. In this work we present the development and characterization of two inductive energy harvesters which exploit different characteristics of the human gait. A multi-coil topology harvester is presented which uses the swing motion of the foot. The second device is a shock-type harvester which is excited into resonance upon heel strike. Both devices were modeled and designed with the key constraint of device height in mind, in order to facilitate the integration into the shoe sole. The devices were characterized under different motion speeds and with two test subjects on a treadmill. An average power output of up to 0.84 mW is achieved with the swing harvester. With a total device volume including the housing of 21 cm 3 a power density of 40 μW cm −3 results. The shock harvester generates an average power output of up to 4.13 mW. The power density amounts to 86 μW cm −3 for the total device volume of 48 cm 3 . Difficulties and potential improvements are discussed briefly. (paper)

  2. Elementary Energy Transfer Pathways in Allochromatium vinosum Photosynthetic Membranes

    Energy Technology Data Exchange (ETDEWEB)

    Lüer, Larry; Carey, Anne-Marie; Henry, Sarah; Maiuri, Margherita; Hacking, Kirsty; Polli, Dario; Cerullo, Giulio; Cogdell, Richard J.

    2015-11-01

    Allochromatium vinosum (formerly Chromatium vinosum) purple bacteria are known to adapt their light-harvesting strategy during growth according to environmental factors such as temperature and average light intensity. Under low light illumination or low ambient temperature conditions, most of the LH2 complexes in the photosynthetic membranes form a B820 exciton with reduced spectral overlap with LH1. To elucidate the reason for this light and temperature adaptation of the LH2 electronic structure, we performed broadband femtosecond transient absorption spectroscopy as a function of excitation wavelength in A. vinosum membranes. A target analysis of the acquired data yielded individual rate constants for all relevant elementary energy transfer (ET) processes. We found that the ET dynamics in high-light-grown membranes was well described by a homogeneous model, with forward and backward rate constants independent of the pump wavelength. Thus, the overall B800→B850→B890→ Reaction Center ET cascade is well described by simple triexponential kinetics. In the low-light-grown membranes, we found that the elementary backward transfer rate constant from B890 to B820 was strongly reduced compared with the corresponding constant from B890 to B850 in high-light-grown samples. The ET dynamics of low-light-grown membranes was strongly dependent on the pump wavelength, clearly showing that the excitation memory is not lost throughout the exciton lifetime. The observed pump energy dependence of the forward and backward ET rate constants suggests exciton diffusion via B850→ B850 transfer steps, making the overall ET dynamics nonexponential. Our results show that disorder plays a crucial role in our understanding of low-light adaptation in A. vinosum.

  3. Elementary Energy Transfer Pathways in Allochromatium vinosum Photosynthetic Membranes.

    Science.gov (United States)

    Lüer, Larry; Carey, Anne-Marie; Henry, Sarah; Maiuri, Margherita; Hacking, Kirsty; Polli, Dario; Cerullo, Giulio; Cogdell, Richard J

    2015-11-03

    Allochromatium vinosum (formerly Chromatium vinosum) purple bacteria are known to adapt their light-harvesting strategy during growth according to environmental factors such as temperature and average light intensity. Under low light illumination or low ambient temperature conditions, most of the LH2 complexes in the photosynthetic membranes form a B820 exciton with reduced spectral overlap with LH1. To elucidate the reason for this light and temperature adaptation of the LH2 electronic structure, we performed broadband femtosecond transient absorption spectroscopy as a function of excitation wavelength in A. vinosum membranes. A target analysis of the acquired data yielded individual rate constants for all relevant elementary energy transfer (ET) processes. We found that the ET dynamics in high-light-grown membranes was well described by a homogeneous model, with forward and backward rate constants independent of the pump wavelength. Thus, the overall B800→B850→B890→ Reaction Center ET cascade is well described by simple triexponential kinetics. In the low-light-grown membranes, we found that the elementary backward transfer rate constant from B890 to B820 was strongly reduced compared with the corresponding constant from B890 to B850 in high-light-grown samples. The ET dynamics of low-light-grown membranes was strongly dependent on the pump wavelength, clearly showing that the excitation memory is not lost throughout the exciton lifetime. The observed pump energy dependence of the forward and backward ET rate constants suggests exciton diffusion via B850→ B850 transfer steps, making the overall ET dynamics nonexponential. Our results show that disorder plays a crucial role in our understanding of low-light adaptation in A. vinosum. Copyright © 2015 Biophysical Society. Published by Elsevier Inc. All rights reserved.

  4. Investigation of collisional excitation-transfer processes in a plasma by laser perturbation method

    International Nuclear Information System (INIS)

    Sakurai, Takeki

    1983-01-01

    The theoretical background and the experimental method of the laser perturbation method applied to the study of collisional excitation transfer process in plasma are explained. The atomic density at some specified level can be evaluated theoretically. By using the theoretical results and the experimentally obtained data, the total attenuation probability, the collisional transfer probability and natural emission probability were estimated. For the experiments, continuous wave laser (cw) and pulse laser are employed. It is possible by using pulse dye laser to observe the attenuation curve directly, and to bring in resonance to any atomic spectra. At the beginning, the experimental studies were made on He-Ne discharge. The pulse dye laser has been used for the excitation of alkali atoms. The first application of pulse laser to the study of plasma physics was the study on He. The cross section of disalignment has also been studied by the laser perturbation. The alignment of atoms, step and cascade transfer, the confinement of radiation and optogalvanic effect are discussed in this paper. (Kato, T.)

  5. Stochastic Modelling of Wireless Energy Transfer

    Science.gov (United States)

    Veilleux, Shaun; Almaghasilah, Ahmed; Abedi, Ali; Wilkerson, DeLisa

    2017-01-01

    This study investigates the efficiency of a new method of powering remote sensors by the means of wireless energy transfer. The increased use of sensors for data collection comes with the inherent cost of supplying power from sources such as power cables or batteries. Wireless energy transfer technology eliminates the need for power cables or periodic battery replacement. The time and cost of setting up or expanding a sensor network will be reduced while allowing sensors to be placed in areas where running power cables or battery replacement is not feasible. This paper models wireless channels for power and data separately. Smart scheduling for the data channel is proposed to avoid transmitting data on a noisy channel where the probability of data loss is high to improve power efficiency. Analytical models have been developed and verified using simulations.

  6. Wireless Energy Transfer Through Magnetic Reluctance Coupling

    International Nuclear Information System (INIS)

    Pillatsch, P

    2014-01-01

    Energy harvesting from human motion for body worn or implanted devices faces the problem of the wearer being still, e.g. while asleep. Especially for medical devices this can become an issue if a patient is bed-bound for prolonged periods of time and the internal battery of a harvesting system is not recharged. This article introduces a mechanism for wireless energy transfer based on a previously presented energy harvesting device. The internal rotor of the energy harvester is made of mild steel and can be actuated through a magnetic reluctance coupling to an external motor. The internal piezoelectric transducer is consequently actuated and generates electricity. This paper successfully demonstrates energy transfer over a distance of 16 mm in air and an achieved power output of 85 μW at 25 Hz. The device functional volume is 1.85 cm 3 . Furthermore, it was demonstrated that increasing the driving frequency beyond 25 Hz did not yield a further increase in power output. Future research will focus on improving the reluctance coupling, e.g. by investigating the use of multiple or stronger magnets, in order to increase transmission distance

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

    Science.gov (United States)

    Kowalski, Karol

    2009-05-21

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

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

    International Nuclear Information System (INIS)

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

    1981-01-01

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

  9. On the theory of excitation transfer process in slow collisions between identical particles

    International Nuclear Information System (INIS)

    Chibisov, M.I.

    1978-01-01

    Asymptotics has been investigated at R → infinity (R is internuclear distance) of exchange interaction for the quasimolecule of two identical one-electron atoms. It is shown that the theory of exchange interaction developed previously which does not take into account the symmetry on permutations of electron is not rigid. The exchange contribution to term splitting in alkali metal atoms determines the effective cross section for transfer of excitation at 10 3 K. The Van der Waals contribution is less than the exchange one. The cross section is of the order of 10 -14 cm 2 . The cross section dependence on temperature is weak, sigma approximately ln 2 T

  10. Control of base-excited dynamical systems through piezoelectric energy harvesting absorber

    Science.gov (United States)

    Abdelmoula, H.; Dai, H. L.; Abdelkefi, A.; Wang, L.

    2017-09-01

    The spring-mass absorber usually offers a good control to dynamical systems under direct base excitations for a specific value of the excitation frequency. As the vibrational energy of a primary dynamical system is transferred to the absorber, it gets dissipated. In this study, this energy is no longer dissipated but converted to available electrical power by designing efficient energy harvesters. A novel design of a piezoelectric beam installed inside an elastically-mounted dynamical system undergoing base excitations is considered. A design is carried out in order to determine the properties and dimensions of the energy harvester with the constraint of simultaneously decreasing the oscillating amplitudes of the primary dynamical system and increasing the harvested power of the energy harvesting absorber. An analytical model for the coupled system is constructed using Euler-Lagrange principle and Galerkin discretization. Different strategies for controlling the primary structure displacement and enhancing the harvested power as functions of the electrical load resistance and thickness of the beam substrate are performed. The linear polynomial approximation of the system’s key parameters as a function of the beam’s substrate thickness is first carried out. Then, the gradient method is applied to determine the adequate values of the electrical load resistance and thickness of the substrate under the constraints of minimizing the amplitudes of the primary structure or maximizing the levels of the harvested power. After that, an iterative strategy is considered in order to simultaneously minimize the amplitudes of the primary structure and maximize the levels of the harvested power as functions of the thickness of the substrate and electrical load resistance. In addition to harmonic excitations, the coupled system subjected to a white noise is explored. Through this analysis, the load resistance and thickness of the substrate of the piezoelectric energy harvester

  11. Imaging and Manipulating Energy Transfer Among Quantum Dots at Individual Dot Resolution.

    Science.gov (United States)

    Nguyen, Duc; Nguyen, Huy A; Lyding, Joseph W; Gruebele, Martin

    2017-06-27

    Many processes of interest in quantum dots involve charge or energy transfer from one dot to another. Energy transfer in films of quantum dots as well as between linked quantum dots has been demonstrated by luminescence shift, and the ultrafast time-dependence of energy transfer processes has been resolved. Bandgap variation among dots (energy disorder) and dot separation are known to play an important role in how energy diffuses. Thus, it would be very useful if energy transfer could be visualized directly on a dot-by-dot basis among small clusters or within films of quantum dots. To that effect, we report single molecule optical absorption detected by scanning tunneling microscopy (SMA-STM) to image energy pooling from donor into acceptor dots on a dot-by-dot basis. We show that we can manipulate groups of quantum dots by pruning away the dominant acceptor dot, and switching the energy transfer path to a different acceptor dot. Our experimental data agrees well with a simple Monte Carlo lattice model of energy transfer, similar to models in the literature, in which excitation energy is transferred preferentially from dots with a larger bandgap to dots with a smaller bandgap.

  12. Resonance Energy Transfer Molecular Imaging Application in Biomedicine

    Directory of Open Access Journals (Sweden)

    NIE Da-hong1,2;TANG Gang-hua1,3

    2016-11-01

    Full Text Available Resonance energy transfer molecular imaging (RETI can markedly improve signal intensity and tissue penetrating capacity of optical imaging, and have huge potential application in the deep-tissue optical imaging in vivo. Resonance energy transfer (RET is an energy transition from the donor to an acceptor that is in close proximity, including non-radiative resonance energy transfer and radiative resonance energy transfer. RETI is an optical imaging technology that is based on RET. RETI mainly contains fluorescence resonance energy transfer imaging (FRETI, bioluminescence resonance energy transfer imaging (BRETI, chemiluminescence resonance energy transfer imaging (CRETI, and radiative resonance energy transfer imaging (RRETI. RETI is the hot field of molecular imaging research and has been widely used in the fields of biology and medicine. This review mainly focuses on RETI principle and application in biomedicine.

  13. Charge-Transfer Dynamics in the Lowest Excited State of a Pentacene–Fullerene Complex: Implications for Organic Solar Cells

    KAUST Repository

    Joseph, Saju

    2017-10-02

    We characterize the dynamic nature of the lowest excited state in a pentacene/C60 complex on the femtosecond time scale, via a combination of ab initio molecular dynamics and time-dependent density functional theory. We analyze the correlations between the molecular vibrations of the complex and the oscillations in the electron-transfer character of its lowest excited state, which point to vibration-induced coherences between the (pentacene-based) local-excitation (LE) state and the complex charge-transfer (CT) state. We discuss the implications of our results on this model system for the exciton-dissociation process in organic solar cells.

  14. Quantum transfer energy in the framework of time-dependent dipole-dipole interaction

    Science.gov (United States)

    El-Shishtawy, Reda M.; Haddon, Robert C.; Al-Heniti, Saleh H.; Raffah, Bahaaudin M.; Berrada, K.; Abdel-Khalek, S.; Al-Hadeethi, Yas F.

    2018-03-01

    In this work, we examine the process of the quantum transfer of energy considering time-dependent dipole-dipole interaction in a dimer system characterized by two-level atom systems. By taking into account the effect of the acceleration and speed of the atoms in the dimer coupling, we demonstrate that the improvement of the probability for a single-excitation transfer energy extremely benefits from the incorporation of atomic motion effectiveness and the energy detuning. We explore the relevance between the population and entanglement during the time-evolution and show that this kind of nonlocal correlation may be generated during the process of the transfer of energy. Our work may provide optimal conditions to implement realistic experimental scenario in the transfer of the quantum energy.

  15. Direct observation of multistep energy transfer in LHCII with fifth-order 3D electronic spectroscopy.

    Science.gov (United States)

    Zhang, Zhengyang; Lambrev, Petar H; Wells, Kym L; Garab, Győző; Tan, Howe-Siang

    2015-07-31

    During photosynthesis, sunlight is efficiently captured by light-harvesting complexes, and the excitation energy is then funneled towards the reaction centre. These photosynthetic excitation energy transfer (EET) pathways are complex and proceed in a multistep fashion. Ultrafast two-dimensional electronic spectroscopy (2DES) is an important tool to study EET processes in photosynthetic complexes. However, the multistep EET processes can only be indirectly inferred by correlating different cross peaks from a series of 2DES spectra. Here we directly observe multistep EET processes in LHCII using ultrafast fifth-order three-dimensional electronic spectroscopy (3DES). We measure cross peaks in 3DES spectra of LHCII that directly indicate energy transfer from excitons in the chlorophyll b (Chl b) manifold to the low-energy level chlorophyll a (Chl a) via mid-level Chl a energy states. This new spectroscopic technique allows scientists to move a step towards mapping the complete complex EET processes in photosynthetic systems.

  16. Probing energy transfer events in the light harvesting complex 2 (LH2) of Rhodobacter sphaeroides with two-dimensional spectroscopy.

    Science.gov (United States)

    Fidler, Andrew F; Singh, Ved P; Long, Phillip D; Dahlberg, Peter D; Engel, Gregory S

    2013-10-21

    Excitation energy transfer events in the photosynthetic light harvesting complex 2 (LH2) of Rhodobacter sphaeroides are investigated with polarization controlled two-dimensional electronic spectroscopy. A spectrally broadened pulse allows simultaneous measurement of the energy transfer within and between the two absorption bands at 800 nm and 850 nm. The phased all-parallel polarization two-dimensional spectra resolve the initial events of energy transfer by separating the intra-band and inter-band relaxation processes across the two-dimensional map. The internal dynamics of the 800 nm region of the spectra are resolved as a cross peak that grows in on an ultrafast time scale, reflecting energy transfer between higher lying excitations of the B850 chromophores into the B800 states. We utilize a polarization sequence designed to highlight the initial excited state dynamics which uncovers an ultrafast transfer component between the two bands that was not observed in the all-parallel polarization data. We attribute the ultrafast transfer component to energy transfer from higher energy exciton states to lower energy states of the strongly coupled B850 chromophores. Connecting the spectroscopic signature to the molecular structure, we reveal multiple relaxation pathways including a cyclic transfer of energy between the two rings of the complex.

  17. Probing energy transfer events in the light harvesting complex 2 (LH2) of Rhodobacter sphaeroides with two-dimensional spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Fidler, Andrew F.; Singh, Ved P.; Engel, Gregory S. [Department of Chemistry, The Institute for Biophysical Dynamics, and The James Franck Institute, The University of Chicago, Chicago, Illinois 60637 (United States); Long, Phillip D.; Dahlberg, Peter D. [Graduate Program in the Biophysical Sciences, The University of Chicago, Chicago, Illinois 60637 (United States)

    2013-10-21

    Excitation energy transfer events in the photosynthetic light harvesting complex 2 (LH2) of Rhodobacter sphaeroides are investigated with polarization controlled two-dimensional electronic spectroscopy. A spectrally broadened pulse allows simultaneous measurement of the energy transfer within and between the two absorption bands at 800 nm and 850 nm. The phased all-parallel polarization two-dimensional spectra resolve the initial events of energy transfer by separating the intra-band and inter-band relaxation processes across the two-dimensional map. The internal dynamics of the 800 nm region of the spectra are resolved as a cross peak that grows in on an ultrafast time scale, reflecting energy transfer between higher lying excitations of the B850 chromophores into the B800 states. We utilize a polarization sequence designed to highlight the initial excited state dynamics which uncovers an ultrafast transfer component between the two bands that was not observed in the all-parallel polarization data. We attribute the ultrafast transfer component to energy transfer from higher energy exciton states to lower energy states of the strongly coupled B850 chromophores. Connecting the spectroscopic signature to the molecular structure, we reveal multiple relaxation pathways including a cyclic transfer of energy between the two rings of the complex.

  18. Probing energy transfer events in the light harvesting complex 2 (LH2) of Rhodobacter sphaeroides with two-dimensional spectroscopy

    International Nuclear Information System (INIS)

    Fidler, Andrew F.; Singh, Ved P.; Engel, Gregory S.; Long, Phillip D.; Dahlberg, Peter D.

    2013-01-01

    Excitation energy transfer events in the photosynthetic light harvesting complex 2 (LH2) of Rhodobacter sphaeroides are investigated with polarization controlled two-dimensional electronic spectroscopy. A spectrally broadened pulse allows simultaneous measurement of the energy transfer within and between the two absorption bands at 800 nm and 850 nm. The phased all-parallel polarization two-dimensional spectra resolve the initial events of energy transfer by separating the intra-band and inter-band relaxation processes across the two-dimensional map. The internal dynamics of the 800 nm region of the spectra are resolved as a cross peak that grows in on an ultrafast time scale, reflecting energy transfer between higher lying excitations of the B850 chromophores into the B800 states. We utilize a polarization sequence designed to highlight the initial excited state dynamics which uncovers an ultrafast transfer component between the two bands that was not observed in the all-parallel polarization data. We attribute the ultrafast transfer component to energy transfer from higher energy exciton states to lower energy states of the strongly coupled B850 chromophores. Connecting the spectroscopic signature to the molecular structure, we reveal multiple relaxation pathways including a cyclic transfer of energy between the two rings of the complex

  19. Competition between electronic energy transfer and relaxation in Xe doped Ar and Ne matrices studied by photoelectron spectroscopy

    International Nuclear Information System (INIS)

    Schwentner, N.; Koch, E.E.

    1976-01-01

    Thin films of solid Ar and Ne doped with 1% Xe were excited with photons in the energy range from 10 eV to 20 eV in order to measure the energy distribution of the emitted electrons. Binding energies of th host and guest levels are deduced. When host excitons are excited, strong emission of electrons is observed indicating an efficient transfer of the host exciton energy to the Xe guest atoms. The energy of the free excitons is transferred, as can be deduced from the kinetic energy of the photoemitted electrons, rather than the energy of the bound (self-trapped) excitons which are observed in luminescence experiments. Furthermore, there is a striking difference between the Ar and the Ne matrix: In the Ne matrix a fast relaxation from the n = 2 to the n = 1 state was observed and only the energy of the n = 1 exciton is transferred even when higher excitons are excited, in contrast to Ar, where the transferred energy is higher for excitation of the n = 2 excitons than for n = 1. From these observations, time hierarchies for the competition between electronic energy transfer and relaxation are deduced. (orig.) [de

  20. A pair natural orbital implementation of the coupled cluster model CC2 for excitation energies.

    Science.gov (United States)

    Helmich, Benjamin; Hättig, Christof

    2013-08-28

    We demonstrate how to extend the pair natural orbital (PNO) methodology for excited states, presented in a previous work for the perturbative doubles correction to configuration interaction singles (CIS(D)), to iterative coupled cluster methods such as the approximate singles and doubles model CC2. The original O(N(5)) scaling of the PNO construction is reduced by using orbital-specific virtuals (OSVs) as an intermediate step without spoiling the initial accuracy of the PNO method. Furthermore, a slower error convergence for charge-transfer states is analyzed and resolved by a numerical Laplace transformation during the PNO construction, so that an equally accurate treatment of local and charge-transfer excitations is achieved. With state-specific truncated PNO expansions, the eigenvalue problem is solved by combining the Davidson algorithm with deflation to project out roots that have already been determined and an automated refresh with a generation of new PNOs to achieve self-consistency of the PNO space. For a large test set, we found that truncation errors for PNO-CC2 excitation energies are only slightly larger than for PNO-CIS(D). The computational efficiency of PNO-CC2 is demonstrated for a large organic dye, where a reduction of the doubles space by a factor of more than 1000 is obtained compared to the canonical calculation. A compression of the doubles space by a factor 30 is achieved by a unified OSV space only. Moreover, calculations with the still preliminary PNO-CC2 implementation on a series of glycine oligomers revealed an early break even point with a canonical RI-CC2 implementation between 100 and 300 basis functions.

  1. Non-typical fluorescence studies of excited and ground state proton and hydrogen transfer

    KAUST Repository

    Gil, Michał; Kijak, Michał; Piwonski, Hubert Marek; Herbich, Jerzy; Waluk, Jacek

    2017-01-01

    Fluorescence studies of tautomerization have been carried out for various systems that exhibit single and double proton or hydrogen translocation in various environments, such as liquid and solid condensed phases, ultracold supersonic jets, and finally, polymer matrices with single emitters.We focus on less explored areas of application of fluorescence for tautomerization studies, using porphycene, a porphyrin isomer, as an example. Fluorescence anisotropy techniques allow investigations of self-exchange reactions, where the reactant and product are formally identical. Excitation with polarized light makes it possible to monitor tautomerization in single molecules and to detect their three-dimensional orientation. Analysis of fluorescence from single vibronic levels of jet-isolated porphycene not only demonstrates coherent tunneling of two internal protons, but also indicates that the process is vibrational mode-specific. Next, we present bifunctional proton donoracceptor systems, molecules that are able, depending on the environment, to undergo excited state single intramolecular or double intermolecular proton transfer. For molecules that have donor and acceptor groups located in separate moieties linked by a single bond, excited state tautomerization can be coupled to mutual twisting of the two subunits.

  2. Non-typical fluorescence studies of excited and ground state proton and hydrogen transfer

    KAUST Repository

    Gil, Michał

    2017-02-03

    Fluorescence studies of tautomerization have been carried out for various systems that exhibit single and double proton or hydrogen translocation in various environments, such as liquid and solid condensed phases, ultracold supersonic jets, and finally, polymer matrices with single emitters.We focus on less explored areas of application of fluorescence for tautomerization studies, using porphycene, a porphyrin isomer, as an example. Fluorescence anisotropy techniques allow investigations of self-exchange reactions, where the reactant and product are formally identical. Excitation with polarized light makes it possible to monitor tautomerization in single molecules and to detect their three-dimensional orientation. Analysis of fluorescence from single vibronic levels of jet-isolated porphycene not only demonstrates coherent tunneling of two internal protons, but also indicates that the process is vibrational mode-specific. Next, we present bifunctional proton donoracceptor systems, molecules that are able, depending on the environment, to undergo excited state single intramolecular or double intermolecular proton transfer. For molecules that have donor and acceptor groups located in separate moieties linked by a single bond, excited state tautomerization can be coupled to mutual twisting of the two subunits.

  3. Influence of different environments on the excited-state proton transfer and dual fluorescence of fisetin

    Science.gov (United States)

    Guharay, Jayanti; Dennison, S. Moses; Sengupta, Pradeep K.

    1999-05-01

    The influence of different protic and aprotic solvent environments on the excited-state intramolecular proton transfer (ESIPT) leading to a dual fluorescence behaviour of a biologically important, naturally occurring, polyhydroxyflavone, fisetin (3,3',4',7-tetrahydroxyflavone), has been investigated. The normal fluorescence band, in particular, is extremely sensitive to solvent polarity with νmax shifting from 24 510 cm -1 in dioxane ( ET(30)=36.0) to 20 790 cm -1 in methanol ( ET(30)=55.5). This is rationalized in terms of solvent dipolar relaxation process, which also accounts for the red edge excitation shifts (REES) observed in viscous environments such as glycerol at low temperatures. Significant solvent dependence of the tautomer fluorescence properties ( νmax, yield and decay kinetics) reveals the influence of external hydrogen bonding perturbation on the internal hydrogen bond of the molecule. These excited-state relaxation phenomena and their relevant parameters have been used to probe the microenvironment of fisetin in a membrane mimetic system, namely AOT reverse micelles in n-heptane at different water/surfactant molar ratio ( w0).

  4. Charge-transfer and Mott-Hubbard Excitations in FeBo3: Fe K-edge resonant Inelastic x-ray scattering study

    International Nuclear Information System (INIS)

    Kim, J.; Shvydko, Y.

    2011-01-01

    Momentum-resolved resonant inelastic x-ray scattering (RIXS) spectroscopy has been carried out successfully at the Fe K-edge for the first time. The RIXS spectra of a FeBO 3 single crystal reveal a wealth of information on ∼ 1-10 eV electronic excitations. The IXS signal resonates when the incident photon energy approaches the pre-edge (1s - -3d) and the main-edge (1s - -4p) of the Fe K-edge absorption spectrum. The RIXS spectra measured at the pre-edge and the main-edge show quantitatively different dependences on the incident photon energy, momentum transfer, photon polarization, and temperature. We present a multielectron analysis of the Mott-Hubbard (MH) and charge transfer (CT) excitations, and calculate their energies. Electronic excitations observed in the pre-edge and main-edge RIXS spectra are interpreted as MH and CT excitations, respectively. We propose the electronic structure around the chemical potential in FeBO 3 based on the experimental data.

  5. A new pathway for transmembrane electron transfer in photosynthetic reaction centers of Rhodobacter sphaeroides not involving the excited special pair.

    NARCIS (Netherlands)

    van Brederode, M.E.; Jones, M.R.; van Mourik, F.; van Stokkum, I.H.M.; van Grondelle, R.

    1997-01-01

    It is generally accepted that electron transfer in bacterial photosynthesis is driven by the first singlet excited state of a special pair of bacteriochlorophylls (P*). We have examined the first steps of electron transfer in a mutant of the Rhodobacter sphaeroides reaction center in which charge

  6. A new pathway for transmembrane electron transfer in photosyntetic reaction centers of Rhodobacter sphaeroides not involving the excited special pair.

    NARCIS (Netherlands)

    van Brederode, M.E.; Jones, M.R.; van Mourik, F.; van Stokkum, I.H.M.; van Grondelle, R.

    1997-01-01

    It is generally accepted that electron transfer in bacterial photosynthesis is driven by the first singlet excited state of a special pair of bacteriochlorophylls (P*). We have examined the first steps of electron transfer in a mutant of the Rhodobacter sphaeroides reaction center in which charge

  7. Energy Transfer Kinetics and Dynamics of Relevance to Iodine Lasers

    National Research Council Canada - National Science Library

    Heaven, Michael C

    2001-01-01

    ...). Energy transfer between I(2 P(1/2)) and 02(X) has been studied in detail. Rate constants for electronic energy transfer and nuclear spin relaxation were measured over the temperature range from 150-300K...

  8. Energy transfer and kinetics in mechanochemistry.

    Science.gov (United States)

    Chen, Zhiliang; Lu, Shengyong; Mao, Qiongjing; Buekens, Alfons; Wang, Yuting; Yan, Jianhua

    2017-11-01

    Mechanochemistry (MC) exerts extraordinary degradation and decomposition effects on many chlorinated, brominated, and even fluorinated persistent organic pollutants (POPs). However, its application is still limited by inadequate study of its reaction kinetic aspects. In the present work, the ball motion and energy transfer in planetary ball mill are investigated in some detail. Almost all milling parameters are summarised in a single factor-total effective impact energy. Furthermore, the MC kinetic between calcium oxide/Al and hexachlorobenzene is well established and modelled. The results indicate that total effective impact energy and reagent ratio are the two factors sufficient for describing the MC degradation degree of POPs. The reaction rate constant only depends on the chemical properties of reactants, so it could be used as an important index to appraise the quality of MC additives. This model successfully predicts the reaction rate for different operating conditions, indicating that it could be suitably applied for conducting MC reactions in other reactors.

  9. Energy Cascade from Internal Modes in Non-uniformly Stratified Fluid through Excitation of Superharmonic Disturbances

    Science.gov (United States)

    Sutherland, B. R.

    2016-02-01

    It is well established that two-dimensional internal plane waves and modes in uniformly stratified fluid efficiently transfer energy to smaller scale waves and ultimately turbulent mixing through parametric subharmonic instability (PSI). The numerical simulations of MacKinnon & Winters (GRL 2005) predicted PSI should act efficiently to disrupt the internal tide. However, while in situ observations showed the presence of PSI, it was not found to be appreciable. One reason for the discrepancy between simulations and observations is that the former examined an internal mode in uniformly stratified fluid whereas, in reality, the internal tide exists in non-uniform stratification and is manifest as sinusoidal oscillations of the thermocline. Through theory supported by numerical simulations, it is shown that internal modes in non-uniform stratification immediately excite superharmonics, not subharmonic disturbances. These have double the horizontal wavenumber and double the frequency of the parent mode and hence move with the same horizontal phase speed of the parent mode. As the disturbances grow in amplitude, however, they interact with the parent mode generating small-scale vertically propagating internal waves within the strongly stratified layer. The occurrence of PSI over very long times can occur, as in the simulations of Hazewinkel and Winters (JPO 2011). However, a comprehensive understanding of the energy cascade from the internal tide to small scales must consider the evolution of excited superharmonic disturbances.

  10. Selective excitation, relaxation, and energy channeling in molecular systems

    International Nuclear Information System (INIS)

    Rhodes, W.C.

    1993-08-01

    Research involves theoretical studies of response, relaxation, and correlated motion in time-dependent behavior of large molecular systems ranging from polyatomic molecules to protein molecules in their natural environment. Underlying theme is subsystem modulation dynamics. Main idea is that quantum mechanical correlations between components of a system develop with time, playing a major role in determining the balance between coherent and dissipative forces. Central theme is interplay of coherence and dissipation in determining the nature of dynamic structuring and energy flow in molecular transformation mechanisms. Subsystem equations of motion are being developed to show how nonlinear, dissipative dynamics of a particular subsystem arise from correlated interactions with the rest of the system (substituent groups, solvent, lattice modes, etc.); one consequence is resonance structures and networks. Quantum dynamics and thermodynamics are being applied to understand control and energy transfer mechanisms in biological functions of protein molecules; these mechanisms are both global and local. Besides the above theory, the research deals with phenomenological aspects of molecular systems

  11. Excitations

    International Nuclear Information System (INIS)

    Dorner, B.

    1996-01-01

    A short introduction to instrumental resolution is followed by a discussion of visibilities of phonon modes due to their eigenvectors. High precision phonon dispersion curves in GaAs are presented together with 'ab initio' calculations. Al 2 O 3 is taken as an example of selected visibility due to group theory. By careful determination of phonon intensities eigenvectors can be determined, such as in Silicon and Diamond. The investigation of magnon modes is shown for the garnet Fe 2 Ca 3 (GeO 4 ) 3 , where also a quantum gap due to zero point spin fluctuations was observed. The study of the splitting of excitons in CsFeCl 3 in an applied magnetic field demonstrates the possibilities of neutron polarisation analysis, which made it possible to observe a mode crossing. An outlook to inelastic X-ray scattering with very high energy resolution of synchrotron radiation is given with the examples of phonons in Beryllium and in water. (author) 19 figs., 36 refs

  12. Effects of variable specific heat on energy transfer in a high-temperature supersonic channel flow

    Science.gov (United States)

    Chen, Xiaoping; Li, Xiaopeng; Dou, Hua-Shu; Zhu, Zuchao

    2018-05-01

    An energy transfer mechanism in high-temperature supersonic turbulent flow for variable specific heat (VSH) condition through turbulent kinetic energy (TKE), mean kinetic energy (MKE), turbulent internal energy (TIE) and mean internal energy (MIE) is proposed. The similarities of energy budgets between VSH and constant specific heat (CSH) conditions are investigated by introducing a vibrational energy excited degree and considering the effects of fluctuating specific heat. Direct numerical simulation (DNS) of temporally evolving high-temperature supersonic turbulent channel flow is conducted at Mach number 3.0 and Reynolds number 4800 combined with a constant dimensional wall temperature 1192.60 K for VSH and CSH conditions to validate the proposed energy transfer mechanism. The differences between the terms in the two kinetic energy budgets for VSH and CSH conditions are small; however, the magnitude of molecular diffusion term for VSH condition is significantly smaller than that for CSH condition. The non-negligible energy transfer is obtained after neglecting several small terms of diffusion, dissipation and compressibility related. The non-negligible energy transfer involving TIE includes three processes, in which energy can be gained from TKE and MIE and lost to MIE. The same non-negligible energy transfer through TKE, MKE and MIE is observed for both the conditions.

  13. Distributed Wireless Power Transfer With Energy Feedback

    Science.gov (United States)

    Lee, Seunghyun; Zhang, Rui

    2017-04-01

    Energy beamforming (EB) is a key technique for achieving efficient radio-frequency (RF) transmission enabled wireless energy transfer (WET). By optimally designing the waveforms from multiple energy transmitters (ETs) over the wireless channels, they can be constructively combined at the energy receiver (ER) to achieve an EB gain that scales with the number of ETs. However, the optimal design of EB waveforms requires accurate channel state information (CSI) at the ETs, which is challenging to obtain practically, especially in a distributed system with ETs at separate locations. In this paper, we study practical and efficient channel training methods to achieve optimal EB in a distributed WET system. We propose two protocols with and without centralized coordination, respectively, where distributed ETs either sequentially or in parallel adapt their transmit phases based on a low-complexity energy feedback from the ER. The energy feedback only depends on the received power level at the ER, where each feedback indicates one particular transmit phase that results in the maximum harvested power over a set of previously used phases. Simulation results show that the two proposed training protocols converge very fast in practical WET systems even with a large number of distributed ETs, while the protocol with sequential ET phase adaptation is also analytically shown to converge to the optimal EB design with perfect CSI by increasing the training time. Numerical results are also provided to evaluate the performance of the proposed distributed EB and training designs as compared to other benchmark schemes.

  14. Wireless energy transfer through non-resonant magnetic coupling

    DEFF Research Database (Denmark)

    Peng, Liang; Breinbjerg, Olav; Mortensen, Asger

    2010-01-01

    could be properly designed to minimize undesired energy dissipation in the source coil when the power receiver is out of the range. Our basic observation paves the way for more flexible design and fabrication of non-resonant mid-range wireless energy transfer systems, thus potentially impacting......We demonstrate by theoretical analysis and experimental verification that mid-range wireless energy transfer systems may take advantage of de-tuned coupling devices, without jeopardizing the energy transfer efficiency. Allowing for a modest de-tuning of the source coil, energy transfer systems...... practical implementations of wireless energy transfer....

  15. Z-dependence of Mean Excitation Energies for Second and Third Row Atoms and Their Ions

    DEFF Research Database (Denmark)

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

    2018-01-01

    All mean excitations energies for second and third row atoms and their ions are calculated in the random‐phase approximation using large basis sets. To a very good approximation it turns out that mean excitation energies within an isoelectronic series is a quadratic function of the nuclear charge...

  16. Excitation energy of a helium 3 quasiparticle in the bulk mixture at constant pressure

    International Nuclear Information System (INIS)

    Yim, M.B.

    1981-01-01

    A 3 He quasiparticle excitation energy in bulk mixture at zero pressure and 6% solution is calculated to O(x) using the bulk effective interaction of Yim and Massey. The present 3 He quasiparticle excitation energy is in agreement with the experimental result of Hilton, Scherm and Stirling. (author)

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

    International Nuclear Information System (INIS)

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

    2014-01-01

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

  18. Energy transfer in purple bacterial photosynthetic units from cells grown in various light intensities.

    Science.gov (United States)

    Niedzwiedzki, Dariusz M; Gardiner, Alastair T; Blankenship, Robert E; Cogdell, Richard J

    2018-05-03

    Three photosynthetic membranes, called intra-cytoplasmic membranes (ICMs), from wild-type and the ∆pucBA abce mutant of the purple phototrophic bacterium Rps. palustris were investigated using optical spectroscopy. The ICMs contain identical light-harvesting complex 1-reaction centers (LH1-RC) but have various spectral forms of light-harvesting complex 2 (LH2). Spectroscopic studies involving steady-state absorption, fluorescence, and femtosecond time-resolved absorption at room temperature and at 77 K focused on inter-protein excitation energy transfer. The studies investigated how energy transfer is affected by altered spectral features of the LH2 complexes as those develop under growth at different light conditions. The study shows that LH1 → LH2 excitation energy transfer is strongly affected if the LH2 complex alters its spectroscopic signature. The LH1 → LH2 excitation energy transfer rate modeled with the Förster mechanism and kinetic simulations of transient absorption of the ICMs demonstrated that the transfer rate will be 2-3 times larger for ICMs accumulating LH2 complexes with the classical B800-850 spectral signature (grown in high light) compared to the ICMs from the same strain grown in low light. For the ICMs from the ∆pucBA abce mutant, in which the B850 band of the LH2 complex is blue-shifted and almost degenerate with the B800 band, the LH1 → LH2 excitation energy transfer was not observed nor predicted by calculations.

  19. Excitation energy deactivation funnel in 3-substituted BODIPY-porphyrin conjugate

    International Nuclear Information System (INIS)

    Nguyen, Nguyen Tran; Verbelen, Bram; Leen, Volker; Waelkens, Etienne; Dehaen, Wim; Kruk, Mikalai

    2016-01-01

    BODIPYs absorb in the visible region which is complementary to that of porphyrins and therefore can be suggested as promising antenna groups to improve the light-harvesting potential of porphyrins. A boron-dipyrromethene dye was combined at the 3-position with a Zn-porphyrin to afford a conjugate. The fluorescence of the conjugate was found to originate from the BODIPY moiety independently of the excitation wavelength due to an unique set of energy transfer rates between the BODIPY and Zn-porphyrin moieties. The fluorescence intensity was shown to be tunable over a wide range using the solvent properties. This feature makes the studied BODIPY-porphyrin conjugate a promising compound for the design of new photochromic devices.

  20. Excitation energy deactivation funnel in 3-substituted BODIPY-porphyrin conjugate

    Energy Technology Data Exchange (ETDEWEB)

    Nguyen, Nguyen Tran [Chemistry Department, University of Education, The University of DaNang, Ton Duc Thang 459, Da Nang (Viet Nam); Molecular Design and Synthesis, Department of Chemistry, KU Leuven, Celestijnenlaan 200F, B-3001 Leuven (Belgium); Verbelen, Bram; Leen, Volker [Molecular Design and Synthesis, Department of Chemistry, KU Leuven, Celestijnenlaan 200F, B-3001 Leuven (Belgium); Waelkens, Etienne [Department of Cellular and Molecular Medicine, KU Leuven, Herestraat 49, Box 901, 3000 Leuven (Belgium); Dehaen, Wim, E-mail: wim.dehaen@kuleuven.be [Molecular Design and Synthesis, Department of Chemistry, KU Leuven, Celestijnenlaan 200F, B-3001 Leuven (Belgium); Kruk, Mikalai, E-mail: m.kruk@belstu.by [Belarusian State Technological University, Physics Department, Sverdlov Str., 13a, Minsk 220006 (Belarus)

    2016-11-15

    BODIPYs absorb in the visible region which is complementary to that of porphyrins and therefore can be suggested as promising antenna groups to improve the light-harvesting potential of porphyrins. A boron-dipyrromethene dye was combined at the 3-position with a Zn-porphyrin to afford a conjugate. The fluorescence of the conjugate was found to originate from the BODIPY moiety independently of the excitation wavelength due to an unique set of energy transfer rates between the BODIPY and Zn-porphyrin moieties. The fluorescence intensity was shown to be tunable over a wide range using the solvent properties. This feature makes the studied BODIPY-porphyrin conjugate a promising compound for the design of new photochromic devices.

  1. Energy transfer in contact binary systems

    International Nuclear Information System (INIS)

    Robertson, J.A.

    1980-01-01

    A simple model for the transfer of energy by steady circulation within the envelope of a contact binary system is presented. The model describes the fully compressible, two-dimensional flow of a perfect gas within a rectangular region in a uniform gravitational field. The region is heated non-uniformly from below. Coriolis forces are neglected but the interaction of the circulation with convection is discussed briefly. Numerical solutions of the linearized equations of the problem are discussed in detail, and the results of some non-linear calculations are also presented. The influence of alternative boundary conditions is examined. (author)

  2. Nanophotonics: Energy Transfer towards Enhanced Luminescent Chemosensing

    Science.gov (United States)

    Aad, Roy; Couteau, Christophe; Lérondel, Gilles

    2015-01-01

    We discuss a recently proposed novel photonic approach for enhancing the fluorescence of extremely thin chemosensing polymer layers. We present theoretical and experimental results demonstrating the concept of gain-assisted waveguided energy transfer (G-WET) on a very thin polymer nanolayer spincoated on an active ZnO thin film. The G-WET approach is shown to result in an 8-fold increase in polymer fluorescence. We then extend the G-WET concept to nanostructured media. The benefits of using active nanostructured substrates on the sensitivity and fluorescence of chemosensing polymers are discussed. Preliminary theoretical results on enlarged sensing surface and photonic band-gap are presented. PMID:28788025

  3. Spectral energy transfer of atmospheric gravity waves through sum and difference nonlinear interactions

    Energy Technology Data Exchange (ETDEWEB)

    Huang, K.M. [Wuhan Univ. (China). School of Electronic Information; Chinese Academey of Sciences, Hefei (China). Key Lab. of Geospace Environment; Embry Riddle Aeronautical Univ., Daytona Beach, FL (United States). Dept. of Physical Science; Ministry of Education, Wuhan (China). Key Lab. of Geospace Environment and Geodesy; State Observatory for Atmospheric Remote Sensing, Wuhan (China); Liu, A.Z.; Li, Z. [Embry Riddle Aeronautical Univ., Daytona Beach, FL (United States). Dept. of Physical Science; Zhang, S.D.; Yi, F. [Wuhan Univ. (China). School of Electronic Information; Ministry of Education, Wuhan (China). Key Lab. of Geospace Environment and Geodesy; State Observatory for Atmospheric Remote Sensing, Wuhan (China)

    2012-07-01

    Nonlinear interactions of gravity waves are studied with a two-dimensional, fully nonlinear model. The energy exchanges among resonant and near-resonant triads are examined in order to understand the spectral energy transfer through interactions. The results show that in both resonant and near-resonant interactions, the energy exchange between two high frequency waves is strong, but the energy transfer from large to small vertical scale waves is rather weak. This suggests that the energy cascade toward large vertical wavenumbers through nonlinear interaction is inefficient, which is different from the rapid turbulence cascade. Because of considerable energy exchange, nonlinear interactions can effectively spread high frequency spectrum, and play a significant role in limiting wave amplitude growth and transferring energy into higher altitudes. In resonant interaction, the interacting waves obey the resonant matching conditions, and resonant excitation is reversible, while near-resonant excitation is not so. Although near-resonant interaction shows the complexity of match relation, numerical experiments show an interesting result that when sum and difference near-resonant interactions occur between high and low frequency waves, the wave vectors tend to approximately match in horizontal direction, and the frequency of the excited waves is also close to the matching value. (orig.)

  4. Ultrafast Single and Multiexciton Energy Transfer in Semiconductor Nanoplatelets

    Science.gov (United States)

    Schaller, Richard

    Photophysical processes such as fluorescence resonance energy transfer (FRET) enable optical antennas, wavelength down-conversion in light-emitting diodes (LEDs), and optical bio-sensing schemes. The rate and efficiency of this donor to acceptor transfer of excitation between chromophores dictates the utility of FRET and can unlock new device operation motifs including quantum-funnel solar cells and reduced gain thresholds. However, the fastest reported FRET time constants involving spherical quantum dots (QDs) (0.12-1 ns), do not outpace biexciton Auger recombination (0.01-0.1 ns), which impedes multiexciton-driven applications including electrically-pumped lasers and carrier-multiplication-enhanced photovoltaics. Precisely controlled, few-monolayer thick semiconductor nano-platelets with tens-of-nanometer diameters exhibit intense optical transitions and hundreds-of-picosecond Auger recombination, but heretofore lack FRET characterizations. We examine binary CdSe NPL solids and show that inter-plate FRET (~6-23 ps, presumably for co-facial arrangements) can occur 15-50 times faster than Auger recombination and demonstrate multiexcitonic FRET, making such materials ideal candidates for advanced technologies. This work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility under Contract No. DE-AC02-06CH11357.

  5. Low-Energy Ballistic Transfers to Lunar Halo Orbits

    Science.gov (United States)

    Parker, Jeffrey S.

    2009-01-01

    Recent lunar missions have begun to take advantage of the benefits of low-energy ballistic transfers between the Earth and the Moon rather than implementing conventional Hohmann-like lunar transfers. Both Artemis and GRAIL plan to implement low-energy lunar transfers in the next few years. This paper explores the characteristics and potential applications of many different families of low-energy ballistic lunar transfers. The transfers presented here begin from a wide variety of different orbits at the Earth and follow several different distinct pathways to the Moon. This paper characterizes these pathways to identify desirable low-energy lunar transfers for future lunar missions.

  6. L-dependence in the 6Li induced three nucleon transfer excitation function

    International Nuclear Information System (INIS)

    Kraus, L.; Linck, I.

    1980-01-01

    The three nucleon transfer reactions induced by 6 Li on 12 C were studied from 5 to 9 MeV/n. The bell-shaped energy variation is used to select cluster states of progressively higher angular momentum. A modification to the Brink semi-classical model equations is proposed in order to reproduce the observed features

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

    Directory of Open Access Journals (Sweden)

    N. Davari

    2014-03-01

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

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

    Science.gov (United States)

    Heßelmann, Andreas

    2015-04-14

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

  9. Conditional Lyapunov exponents and transfer entropy in coupled bursting neurons under excitation and coupling mismatch

    Science.gov (United States)

    Soriano, Diogo C.; Santos, Odair V. dos; Suyama, Ricardo; Fazanaro, Filipe I.; Attux, Romis

    2018-03-01

    This work has a twofold aim: (a) to analyze an alternative approach for computing the conditional Lyapunov exponent (λcmax) aiming to evaluate the synchronization stability between nonlinear oscillators without solving the classical variational equations for the synchronization error dynamical system. In this first framework, an analytic reference value for λcmax is also provided in the context of Duffing master-slave scenario and precisely evaluated by the proposed numerical approach; (b) to apply this technique to the study of synchronization stability in chaotic Hindmarsh-Rose (HR) neuronal models under uni- and bi-directional resistive coupling and different excitation bias, which also considered the root mean square synchronization error, information theoretic measures and asymmetric transfer entropy in order to offer a better insight of the synchronization phenomenon. In particular, statistical and information theoretical measures were able to capture similarity increase between the neuronal oscillators just after a critical coupling value in accordance to the largest conditional Lyapunov exponent behavior. On the other hand, transfer entropy was able to detect neuronal emitter influence even in a weak coupling condition, i.e. under the increase of conditional Lyapunov exponent and apparently desynchronization tendency. In the performed set of numerical simulations, the synchronization measures were also evaluated for a two-dimensional parameter space defined by the neuronal coupling (emitter to a receiver neuron) and the (receiver) excitation current. Such analysis is repeated for different feedback couplings as well for different (emitter) excitation currents, revealing interesting characteristics of the attained synchronization region and conditions that facilitate the emergence of the synchronous behavior. These results provide a more detailed numerical insight of the underlying behavior of a HR in the excitation and coupling space, being in accordance

  10. Intramolecular energy transfer and mode-specific effects in unimolecular reactions of 1,2-difluoroethane

    Science.gov (United States)

    Raff, Lionel M.

    1989-06-01

    The unimolecular decomposition reactions of 1,2-difluoroethane upon mode-specific excitation to a total internal energy of 7.5 eV are investigated using classical trajectory methods and a previously formulated empirical potential-energy surface. The decomposition channels for 1,2-difluoroethane are, in order of importance, four-center HF elimination, C-C bond rupture, and hydrogen-atom dissociation. This order is found to be independent of the particular vibrational mode excited. Neither fluorine-atom nor F2 elimination reactions are ever observed even though these dissociation channels are energetically open. For four-center HF elimination, the average fraction of the total energy partitioned into internal HF motion varies between 0.115-0.181 depending upon the particular vibrational mode initially excited. The internal energy of the fluoroethylene product lies in the range 0.716-0.776. Comparison of the present results with those previously obtained for a random distribution of the initial 1,2-difluoroethane internal energy [J. Phys. Chem. 92, 5111 (1988)], shows that numerous mode-specific effects are present in these reactions in spite of the fact that intramolecular energy transfer rates for this system are 5.88-25.5 times faster than any of the unimolecular reaction rates. Mode-specific excitation always leads to a total decomposition rate significantly larger than that obtained for a random distribution of the internal energy. Excitation of different 1,2-difluoroethane vibrational modes is found to produce as much as a 51% change in the total decomposition rate. Mode-specific effects are also seen in the product energy partitioning. The rate coefficients for decomposition into the various channels are very sensitive to the particular mode excited. A comparison of the calculated mode-specific effects with the previously determined mode-to-mode energy transfer rate coefficients [J. Chem. Phys. 89, 5680 (1988)] shows that, to some extent, the presence of mode

  11. Exogenous quinones inhibit photosynthetic electron transfer in Chloroflexus aurantiacus by specific quenching of the excited bacteriochlorophyll c antenna

    DEFF Research Database (Denmark)

    Frigaard, N-U; Tokita, S; Matsuura, K

    1999-01-01

    In the photosynthetic green filamentous bacterium Chloroflexus aurantiacus, excitation energy is transferred from a large bacteriochlorophyll (BChl) c antenna via smaller BChl a antennas to the reaction center. The effects of substituted 1,4-naphthoquinones on BChl c and BChl a fluorescence and o...... antenna. Our results provide a model system for studying the redox-dependent antenna quenching in green sulfur bacteria because the antennas in these bacteria inherently exhibit a sensitivity to O(2) similar to the quinone-supplemented cells of Cfx. aurantiacus....... and on flash-induced cytochrome c oxidation were studied in whole cells under aerobic conditions. BChl c fluorescence in a cell suspension with 5.4 microM BChl c was quenched to 50% by addition of 0.6 microM shikonin ((R)-2-(1-hydroxy-4-methyl-3-pentenyl)-5,8-dihydroxy-1, 4-naphthoquinone), 0.9 microM 5......-hydroxy-1,4-naphthoquinone, or 4 microM 2-acetyl-3-methyl-1,4-naphthoquinone. Between 25 and 100 times higher quinone concentrations were needed to quench BChl a fluorescence to a similar extent. These quinones also efficiently inhibited flash-induced cytochrome c oxidation when BChl c was excited...

  12. Excitation energy and angular momentum of quasiprojectiles produced in the Xe+Sn collisions at incident energies between 25 and 50 MeV/nucleon

    International Nuclear Information System (INIS)

    Steckmeyer, J.C.; Genouin-Duhamel, E.; Vient, E.; Colin, J.; Durand, D.; Auger, G.; Bacri, C.O.; Bellaize, N.; Borderie, B.; Bougault, R.; Bouriquet, B.; Brou, R.; Buchet, P.; Charvet, J.L.; Chbihi, A.; Cussol, D.; Dayras, R.; De Cesare, N.; Demeyer, A.; Dore, D.; Frankland, J.D.; Galichet, E.; Gerlic, E.; Guinet, D.; Hudan, S.; Lautesse, P.; Lavaud, F.; Laville, J.L.; Lecolley, J.F.; Leduc, C.; Legrain, R.; Le Neindre, N.; Lopez, O.; Louvel, M.; Maskay, A.M.; Nalpas, L.; Normand, J.; Parlog, M.; Pawlowski, P.; Plagnol, E.; Rivet, M.F.; Rosato, E.; Saint-Laurent, F.; Tabacaru, G.; Tamain, B.; Tassan-Got, L.; Tirel, O.; Turzo, K.; Vigilante, M.; Volant, C.; Wieleczko, J.P.

    2001-01-01

    The excitation energy and angular momentum transferred to quasiprojectiles have been measured in the 129 Xe+ nat Sn collisions at bombarding energies between 25 and 50 MeV/nucleon. The excitation energy of quasiprojectiles has been determined from the kinetic energy of all decay products (calorimetry). It increases with the violence of the collision, approaching 10 MeV/nucleon in the most dissipative ones. The angular momentum has been deduced from the kinetic energies and angular distributions of the emitted light charged particles (p, d, t, 3 He and α). The (apparent) spin value decreases with the violence of the collision. Larger spin values are observed at the lowest bombarding energy. Data are compared with the predictions of dynamical and statistical models. They reproduce the data in a quantitative way indicating that large spin values are transferred to quasiprojectiles during the interaction. The results show that the one-body dissipation formalism still applies at intermediate bombarding energies and low-energy dissipations. With the increase of the energy, the data seem to be better described when the two-body interaction is accounted for

  13. Heat Transfer from Optically Excited Gold Nanostructures into Water, Sugar, and Salt Solutions

    Science.gov (United States)

    Green, Andrew J.

    Nanotechnology has introduced a wide variety of new behaviors to study and understand. Metal nanostructures are of particular interest due to their ability to generate large amounts of heat when irradiated at the plasmon resonance. Furthermore, heat dissipation at the nanoscale becomes exceedingly more complicated with respect to bulk behavior. What are the credentials for a heat carrier to move across an interface? Is it important for both materials to have similar vibrational density of states? What changes if one material is a liquid? All of these questions have open ended answers, each of which hold potential for new technologies to be exploited once understood. This dissertation will discuss topics exploring the transfer of heat from an optically excited gold nanoparticle into a surrounding liquid. Gold nanostructures are created using conventional electron beam lithography with lift-off. The nanostructures are deposited onto a thin film thermal sensor composed of AlGaN:Er3+. Erbium(III) has two thermally coupled excited states that can be excited with a 532nm laser. The relative photoluminescence from these excited states are related by a Boltzmann factor and are thusly temperature dependent. A scanning optical microscope collects an image of Er3+ photoluminescence while simultaneously exciting the gold nanostructure. The nanostructure temperature is imaged which is directly related to the surrounding's heat dissipation properties. The first of two topics discuss the heat dissipation and phase change properties of water. A gold nanostructure is submersed under water and subsequently heated with a 532 nm laser. The water immediately surrounding the nanodot is can be superheated beyond the boiling point up to the spinodal decomposition temperature at 594 +/- 17 K. The spinodal decomposition has been confirmed with the observation of critical opalescence. We characterize the laser scattering that occurs in unison with spinodal decomposition due to an increased

  14. Characterising excited states in and around the semi-magic nucleus $^{68}$ Ni using Coulomb excitation and one-neutron transfer

    CERN Multimedia

    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.

  15. Excited-state intramolecular hydrogen transfer (ESIHT) of 1,8-Dihydroxy-9,10-anthraquinone (DHAQ) characterized by ultrafast electronic and vibrational spectroscopy and computational modeling

    KAUST Repository

    Mohammed, Omar F.

    2014-05-01

    We combine ultrafast electronic and vibrational spectroscopy and computational modeling to investigate the photoinduced excited-state intramolecular hydrogen-transfer dynamics in 1,8-dihydroxy-9,10-anthraquinone (DHAQ) in tetrachloroethene, acetonitrile, dimethyl sulfoxide, and methanol. We analyze the electronic excited states of DHAQ with various possible hydrogen-bonding schemes and provide a general description of the electronic excited-state dynamics based on a systematic analysis of femtosecond UV/vis and UV/IR pump-probe spectroscopic data. Upon photoabsorption at 400 nm, the S 2 electronic excited state is initially populated, followed by a rapid equilibration within 150 fs through population transfer to the S 1 state where DHAQ exhibits ESIHT dynamics. In this equilibration process, the excited-state population is distributed between the 9,10-quinone (S2) and 1,10-quinone (S1) states while undergoing vibrational energy redistribution, vibrational cooling, and solvation dynamics on the 0.1-50 ps time scale. Transient UV/vis pump-probe data in methanol also suggest additional relaxation dynamics on the subnanosecond time scale, which we tentatively ascribe to hydrogen bond dynamics of DHAQ with the protic solvent, affecting the equilibrium population dynamics within the S2 and S1 electronic excited states. Ultimately, the two excited singlet states decay with a solvent-dependent time constant ranging from 139 to 210 ps. The concomitant electronic ground-state recovery is, however, only partial because a large fraction of the population relaxes to the first triplet state. From the similarity of the time scales involved, we conjecture that the solvent plays a crucial role in breaking the intramolecular hydrogen bond of DHAQ during the S2/S1 relaxation to either the ground or triplet state. © 2014 American Chemical Society.

  16. Recent development of organic light-emitting diode utilizing energy transfer from exciplex to phosphorescent emitter

    Science.gov (United States)

    Seo, Satoshi; Shitagaki, Satoko; Ohsawa, Nobuharu; Inoue, Hideko; Suzuki, Kunihiko; Nowatari, Hiromi; Takahashi, Tatsuyoshi; Hamada, Takao; Watabe, Takeyoshi; Yamada, Yui; Mitsumori, Satomi

    2016-09-01

    This study investigates an organic light-emitting diode (OLED) utilizing energy transfer from an excited complex (exciplex) comprising donor and acceptor molecules to a phosphorescent dopant. An exciplex has a very small energy gap between the lowest singlet and triplet excited states (S1 and T1). Thus, both S1 and T1 energies of the exciplex can be directly transferred to the T1 of the phosphorescent dopant by adjusting the emission energy of the exciplex to the absorption-edge energy of the dopant. Such an exciplex‒triplet energy transfer (ExTET) achieves high efficiency at low drive voltage because the electrical excitation energy of the exciplex approximates the T1 energy of the dopant. Furthermore, the efficiency of the reverse intersystem crossing (RISC) of the exciplex does not affect the external quantum efficiency (EQE) of the ExTET OLED. The RISC of the exciplex is inhibited when the T1 energy of either donor or acceptor molecules is close to or lower than that of the exciplex itself. Even in this case, however, the ExTET OLED maintains its high efficiency because the T1 energy of each component of the exciplex or the T1 energy of the exciplex itself can be transferred to the dopant. We also varied the emission colors of ExTET OLEDs from sky-blue to red by introducing various phosphorescent dopants. These devices achieved high EQEs (≍30%), low drive voltages (≍3 V), and extremely long lifetimes (e.g., 1 million hours for the orange OLED) at a luminance of 1,000 cd/m2.

  17. Maximizing direct current power delivery from bistable vibration energy harvesting beams subjected to realistic base excitations

    Science.gov (United States)

    Dai, Quanqi; Harne, Ryan L.

    2017-04-01

    Effective development of vibration energy harvesters is required to convert ambient kinetic energy into useful electrical energy as power supply for sensors, for example in structural health monitoring applications. Energy harvesting structures exhibiting bistable nonlinearities have previously been shown to generate large alternating current (AC) power when excited so as to undergo snap-through responses between stable equilibria. Yet, most microelectronics in sensors require rectified voltages and hence direct current (DC) power. While researchers have studied DC power generation from bistable energy harvesters subjected to harmonic excitations, there remain important questions as to the promise of such harvester platforms when the excitations are more realistic and include both harmonic and random components. To close this knowledge gap, this research computationally and experimentally studies the DC power delivery from bistable energy harvesters subjected to such realistic excitation combinations as those found in practice. Based on the results, it is found that the ability for bistable energy harvesters to generate peak DC power is significantly reduced by introducing sufficient amount of stochastic excitations into an otherwise harmonic input. On the other hand, the elimination of a low amplitude, coexistent response regime by way of the additive noise promotes power delivery if the device was not originally excited to snap-through. The outcomes of this research indicate the necessity for comprehensive studies about the sensitivities of DC power generation from bistable energy harvester to practical excitation scenarios prior to their optimal deployment in applications.

  18. Transfer reactions and multiple Coulomb excitation in the $^{100}$Sn Region

    CERN Multimedia

    It is proposed to continue our REX-ISOLDE program in the $^{100}$Sn region at HIE-ISOLDE at ~5 MeV/u. Earlier measurements, with a precision of 10-20%, at 3 MeV/u with REX-ISOLDE point to a deviation between the measured B(E2) values for the first excited 2$^{+}$ states in $^{110,108,106}$Sn compared to theoretical predictions. In addition, the trend of B(E2) values for the lighter isotopes, in particular $^{106}$Sn, appear to differ between low- and high-energy measurements. In line with our letter-of-intent we aim in a first step to address the electromagnetic properties of the first 2$^{+}$and 4$^{+}$ states in $^{110,108,106}$Sn using Coulomb excitation. In these measurements we will directly access the lifetimes of the first excited 4$^{+}$ states in $^{110,108,106}$Sn for the first time. The yield of $^{104}$Sn from the LaC$_{x}$ target will be revisited to clarify if the new solid state RILIS gives sufficient yield to expand the measurements to this isotope. Following this proposal we plan similar meas...

  19. Enhancing radiative energy transfer through thermal extraction

    Science.gov (United States)

    Tan, Yixuan; Liu, Baoan; Shen, Sheng; Yu, Zongfu

    2016-06-01

    Thermal radiation plays an increasingly important role in many emerging energy technologies, such as thermophotovoltaics, passive radiative cooling and wearable cooling clothes [1]. One of the fundamental constraints in thermal radiation is the Stefan-Boltzmann law, which limits the maximum power of far-field radiation to P0 = σT4S, where σ is the Boltzmann constant, S and T are the area and the temperature of the emitter, respectively (Fig. 1a). In order to overcome this limit, it has been shown that near-field radiations could have an energy density that is orders of magnitude greater than the Stefan-Boltzmann law [2-7]. Unfortunately, such near-field radiation transfer is spatially confined and cannot carry radiative heat to the far field. Recently, a new concept of thermal extraction was proposed [8] to enhance far-field thermal emission, which, conceptually, operates on a principle similar to oil immersion lenses and light extraction in light-emitting diodes using solid immersion lens to increase light output [62].Thermal extraction allows a blackbody to radiate more energy to the far field than the apparent limit of the Stefan-Boltzmann law without breaking the second law of thermodynamics. Thermal extraction works by using a specially designed thermal extractor to convert and guide the near-field energy to the far field, as shown in Fig. 1b. The same blackbody as shown in Fig. 1a is placed closely below the thermal extractor with a spacing smaller than the thermal wavelength. The near-field coupling transfers radiative energy with a density greater than σT4. The thermal extractor, made from transparent and high-index or structured materials, does not emit or absorb any radiation. It transforms the near-field energy and sends it toward the far field. As a result, the total amount of far-field radiative heat dissipated by the same blackbody is greatly enhanced above SσT4, where S is the area of the emitter. This paper will review the progress in thermal

  20. Radioactive beam EXperiments at ISOLDE : Coulomb excitation and neutron transfer reactions of exotic nuclei.

    CERN Multimedia

    Kugler, E; Ratzinger, U; Wenander, F J C

    2002-01-01

    % IS347 \\\\ \\\\We propose to perform a pilot experiment to study very neutron rich (A<32) Na-Mg and (A<52) K-Ca isotopes in the region around the neutron shell closures of N=20 and N=28 after Coulomb excitation and neutron transfer, and to demonstrate highly efficient and cost-effective ways to bunch, charge-state breed and accelerate already existing mass-separated singly-charged radioactive ion beams. \\\\ \\\\To do this we plan to accelerate the ISOLDE beams up to 2~MeV/u by means of a novel acceleration scheme and to install an efficient $\\gamma$-ray array for low-multiplicity events around the target position.

  1. Excited state proton transfer in 9-aminoacridine carboxamides in water and in DNA

    Energy Technology Data Exchange (ETDEWEB)

    Smith, Charles A. [Iowa State Univ., Ames, IA (United States)

    1995-09-26

    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.

  2. Pulsed magnetization transfer contrast MRI by a sequence with water selective excitation

    Energy Technology Data Exchange (ETDEWEB)

    Schick, F. [Univ. of Tuebingen (Germany)

    1996-01-01

    A water selective SE imaging sequence was developed providing suitable properties for the assessment of magnetization transfer (MT) effects in tissues with considerable amounts of fat. The sequence with water selective excitation and slice selective refocusing combines the following features: The RIF exposure on the macromolecular protons is relatively low for single slice imaging without MT prepulses, since no additional pulses for fat saturation are necessary. Water selection by frequency selective excitation diminishes faults in the subtraction of images recorded with and without MT prepulses (which might arise from movements). High differences in the signal amplitudes from hyaline cartilage and muscle tissue were obtained comparing images recorded with irradiation of the series of prepulses for MT and those lacking MT prepulses. Utilizations of the described water selective approach for the assessment of MT effects in lesions of cartilage and bone are demonstrated. MT saturation was also examined in muscles with fatty degeneration of patients suffering from progressive muscular dystrophy. The described technique allows determination of MT effects with good precision in a single slice, especially in regions with dominating fat signals. 22 refs., 5 figs.

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

    Science.gov (United States)

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

    2010-12-28

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

  4. Luminescence decay in condensed argon under high energy excitation

    International Nuclear Information System (INIS)

    Carvalho, M.J.; Klein, G.

    1978-01-01

    α and β particles were used to study the luminescence of condensed argon. The scintillation decay has always two components independently of the phase and the kind of the exciting particles. Decay time constants are given for solid, liquid and also gaseous argon. Changes in the relative intensity values of the two components are discussed in terms of track effects

  5. Ordering and low energy excitations in strongly correlated bronzes

    NARCIS (Netherlands)

    Sagara, Dodderi Manjunatha

    2006-01-01

    Summary In any solid system, whether it is superconducting, shows a charge-density-wave behavior, or any other kind of ground state, two aspects drag the attention of the scientific community. They are order and excitations in solids. The ordering may be due to electronic, lattice, spin or orbital

  6. Enhancing radiative energy transfer through thermal extraction

    Directory of Open Access Journals (Sweden)

    Tan Yixuan

    2016-06-01

    Full Text Available Thermal radiation plays an increasingly important role in many emerging energy technologies, such as thermophotovoltaics, passive radiative cooling and wearable cooling clothes [1]. One of the fundamental constraints in thermal radiation is the Stefan-Boltzmann law, which limits the maximum power of far-field radiation to P0 = σT4S, where σ is the Boltzmann constant, S and T are the area and the temperature of the emitter, respectively (Fig. 1a. In order to overcome this limit, it has been shown that near-field radiations could have an energy density that is orders of magnitude greater than the Stefan-Boltzmann law [2-7]. Unfortunately, such near-field radiation transfer is spatially confined and cannot carry radiative heat to the far field. Recently, a new concept of thermal extraction was proposed [8] to enhance far-field thermal emission, which, conceptually, operates on a principle similar to oil immersion lenses and light extraction in light-emitting diodes using solid immersion lens to increase light output [62].Thermal extraction allows a blackbody to radiate more energy to the far field than the apparent limit of the Stefan-Boltzmann law without breaking the second law of thermodynamics.

  7. Energy Transfer Using Gradient Index Metamaterial

    Directory of Open Access Journals (Sweden)

    Boopalan Ganapathy

    2018-01-01

    Full Text Available The gradient refractive index structure in this paper is used to increase the quantum of energy transfer. This is done by improving the directive gain of the pyramidal horn antenna at a frequency of 10 GHz. A three-dimensional array of closed square rings is placed in front of the horn antenna aperture to form a gradient refractive index structure. This structure increases the directive gain by 1.6 dB as compared to that of the conventional horn antenna. The structure nearly doubles the wireless power transfer quantum between the transmitter and the receiver when placed at both ends. The increase in the directivity is achieved by converting the spherical wave emanating from the horn to a plane wave once it passes through the structure. This transformation is realized by the gradient refractive index structure being placed perpendicular to the direction of propagation. The gradient refractive index is constructed by changing the dimensions of a closed square ring placed in the unit cell of the array. The change in the refractive index gives rise to an improvement of the half power beam width and side lobe level compared to that of the normal horn. The design and simulation were done using CST Studio software.

  8. Solvent effects on the excited-state double proton transfer mechanism in the 7-azaindole dimer: a TDDFT study with the polarizable continuum model.

    Science.gov (United States)

    Yu, Xue-Fang; Yamazaki, Shohei; Taketsugu, Tetsuya

    2017-08-30

    Solvent effects on the excited-state double proton transfer (ESDPT) mechanism in the 7-azaindole (7AI) dimer were investigated using the time-dependent density functional theory (TDDFT) method. Excited-state potential energy profiles along the reaction paths in a locally excited (LE) state and a charge transfer (CT) state were calculated using the polarizable continuum model (PCM) to include the solvent effect. A series of non-polar and polar solvents with different dielectric constants were used to examine the polarity effect on the ESDPT mechanism. The present results suggest that in a non-polar solvent and a polar solvent with a small dielectric constant, ESDPT follows a concerted mechanism, similar to the case in the gas phase. In a polar solvent with a relatively large dielectric constant, however, ESDPT is likely to follow a stepwise mechanism via a stable zwitterionic intermediate in the LE state on the adiabatic potential energy surface, although inclusion of zero-point vibrational energy (ZPE) corrections again suggests the concerted mechanism. In the meantime, the stepwise reaction path involving the CT state with neutral intermediates is also examined, and is found to be less competitive than the concerted or stepwise path in the LE state in both non-polar and polar solvents. The present study provides a new insight into the experimental controversy of the ESDPT mechanism of the 7AI dimer in a solution.

  9. Fluorescence energy transfer on erythrocyte membranes

    International Nuclear Information System (INIS)

    Fuchs, H.M.; Hof, M.; Lawaczeck, R.

    1995-08-01

    Stationary and time-dependent fluorescence have been measured for a donor/acceptor (DA) pair bound to membrane proteins of bovine erythrocyte ghosts. The donor N-(p-(2-benzoxazolyl)phenyl)-maleimid (BMI) and the acceptor fluram bind to SH- and NH 2 -residues, respectively. The fluorescence spectra and the time-dependent emission are consistent with a radiationless fluorescence energy transfer (RET). The density of RET-effective acceptor binding sites c=0.072 nm -2 was calculated on the basis of the two-dimensional Foerster-kinetic. Band3 protein is the only membrane spanning protein with accessible SH-groups, and therefore only effective binding sites on the band3 protein are counted for the RET measurements performed. (author). 23 refs, 4 figs, 2 tabs

  10. Nanophotonics: Energy Transfer towards Enhanced Luminescent Chemosensing

    Directory of Open Access Journals (Sweden)

    Roy Aad

    2015-04-01

    Full Text Available We discuss a recently proposed novel photonic approach for enhancing the fluorescence of extremely thin chemosensing polymer layers. We present theoretical and experimental results demonstrating the concept of gain-assisted waveguided energy transfer (G-WET on a very thin polymer nanolayer spincoated on an active ZnO thin film. The G-WET approach is shown to result in an 8-fold increase in polymer fluorescence. We then extend the G-WET concept to nanostructured media. The benefits of using active nanostructured substrates on the sensitivity and fluorescence of chemosensing polymers are discussed. Preliminary theoretical results on enlarged sensing surface and photonic band-gap are presented.

  11. Energy transfer in structured and unstructured environments

    DEFF Research Database (Denmark)

    Iles-Smith, Jake; Dijkstra, Arend G.; Lambert, Neill

    2016-01-01

    of motion over a wide range of parameters. Furthermore, we show that the Zusman equations, which may be obtained in a semiclassical limit of the reaction coordinate model, are often incapable of describing the correct dynamical behaviour. This demonstrates the necessity of properly accounting for quantum......We explore excitonic energy transfer dynamics in a molecular dimer system coupled to both structured and unstructured oscillator environments. By extending the reaction coordinate master equation technique developed by Iles-Smith et al. [Phys. Rev. A 90, 032114 (2014)], we go beyond the commonly...... correlations generated between the system and its environment when the Born-Markov approximations no longer hold. Finally, we apply the reaction coordinate formalism to the case of a structured environment comprising of both underdamped (i.e., sharply peaked) and overdamped (broad) components simultaneously...

  12. Energy harvesting from coherent resonance of horizontal vibration of beam excited by vertical base motion

    Energy Technology Data Exchange (ETDEWEB)

    Lan, C. B.; Qin, W. Y. [Department of Engineering Mechanics, Northwestern Polytechnical University, Xi' an 710072 (China)

    2014-09-15

    This letter investigates the energy harvesting from the horizontal coherent resonance of a vertical cantilever beam subjected to the vertical base excitation. The potential energy of the system has two symmetric potential wells. So, under vertical excitation, the system can jump between two potential wells, which will lead to the large vibration in horizontal direction. Two piezoelectric patches are pasted to harvest the energy. From experiment, it is found that the vertical excitation can make the beam turn to be bistable. The system can transform vertical vibration into horizontal vibration of low frequency when excited by harmonic motion. The horizontal coherence resonance can be observed when excited by a vertical white noise. The corresponding output voltages of piezoelectric films reach high values.

  13. Collisions involving energy transfer between atoms with large angular moments

    International Nuclear Information System (INIS)

    Vdovin, Yu.A.; Galitskij, V.M.

    1975-01-01

    Study is made of the collisions of excited and nonexcited atoms with a small resonance defect, assuming that the excited and ground states of each atom are bound via an allowed dipole transition and that intrinsic moments of states are great. In such an approximation the atomic interaction is defined by a dipole-dipole interaction operator. Equations for amplitudes are derived for two cases: (1) the first atom is in an excited state while the second is in the ground state and (2) the first atom is in the ground state while the second is in an excited state. The problem is solved in the approximation that the moments of the excited and ground states of each atom are equal. An expression for the excitation transfer cross section is written down. Analysis of this expression shows that the excitation transfer cross section at first increases with removal from the exact resonance and reaches resonance at lambda approximately 0.1 (lambda is a dimensionless parameter which is equal to the ratio of the resonance defect Δ to the interaction at spacings of the order of the Weisskopf radius). Only at lambda >0.16 does the cross section become smaller than the resonance one. This effect is due to the interaction Hamiltonian approximation adopted in the present study

  14. Ioniclike energy structure of neutral core-excited states in free Kr clusters

    International Nuclear Information System (INIS)

    Peredkov, S.; Sorensen, S.L.; Kivimaeki, A.; Schulz, J.; Maartensson, N.; Oehrwall, G.; Lundwall, M.; Rander, T.; Lindblad, A.; Bergersen, H.; Svensson, S.; Bjoerneholm, O.; Tchaplyguine, M.

    2005-01-01

    The development of electronic states in krypton clusters is investigated by high-resolution core-level electron spectroscopy. The energy ordering of bulk versus surface 3d -1 np(n>5) core-excited states in neutral clusters is demonstrated to be reversed to the 3d -1 5p level situation. The cluster 3d -1 6p,7p states are proven to be at a lower energy than the corresponding atomic levels. These findings reveal the ioniclike energy structure of the neutral cluster core-excited levels. The phenomenon is explained by a spatial spread of the excited orbitals over the cluster lattice

  15. Deviation from Boltzmann distribution in excited energy levels of singly-ionized iron in an argon glow discharge plasma for atomic emission spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Zhang Lei; Kashiwakura, Shunsuke; Wagatsuma, Kazuaki, E-mail: wagatuma@imr.tohoku.ac.jp

    2012-01-15

    A Boltzmann plot for many iron ionic lines having excitation energies of 4.7-9.1 eV was investigated in an argon glow discharge plasma when the discharge parameters, such as the voltage/current and the gas pressure, were varied. A Grimm-style radiation source was employed in a DC voltage range of 400-800 V at argon pressures of 400-930 Pa. The plot did not follow a linear relationship over a wide range of the excitation energy, but it yielded a normal Boltzmann distribution in the range of 4.7-5.8 eV and a large overpopulation in higher-lying excitation levels of iron ion. A probable reason for this phenomenon is that excitations for higher excited energy levels of iron ion would be predominantly caused by non-thermal collisions with argon species, the internal energy of which is received by iron atoms for the ionization. Particular intense ionic lines, which gave a maximum peak of the Boltzmann plot, were observed at an excitation energy of ca. 7.7 eV. They were the Fe II 257.297-nm and the Fe II 258.111-nm lines, derived from the 3d{sup 5}4s4p {sup 6}P excited levels. The 3d{sup 5}4s4p {sup 6}P excited levels can be highly populated through a resonance charge transfer from the ground state of argon ion, because of good matching in the excitation energy as well as the conservation of the total spin before and after the collision. An enhancement factor of the emission intensity for various Fe II lines could be obtained from a deviation from the normal Boltzmann plot, which comprised the emission lines of 4.7-5.8 eV. It would roughly correspond to a contribution of the charge transfer excitation to the excited levels of iron ion, suggesting that the charge-transfer collision could elevate the number density of the corresponding excited levels by a factor of ca.10{sup 4}. The Boltzmann plots give important information on the reason why a variety of iron ionic lines can be emitted from glow discharge plasmas.

  16. Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes

    Science.gov (United States)

    Ma, X.; Fang, F.; Li, Q.; Zhu, J.; Yang, Y.; Wu, Y. Z.; Zhao, H. B.; Lüpke, G.

    2015-10-01

    Optical control of spin is of central importance in the research of ultrafast spintronic devices utilizing spin dynamics at short time scales. Recently developed optical approaches such as ultrafast demagnetization, spin-transfer and spin-orbit torques open new pathways to manipulate spin through its interaction with photon, orbit, charge or phonon. However, these processes are limited by either the long thermal recovery time or the low-temperature requirement. Here we experimentally demonstrate ultrafast coherent spin precession via optical charge-transfer processes in the exchange-coupled Fe/CoO system at room temperature. The efficiency of spin precession excitation is significantly higher and the recovery time of the exchange-coupling torque is much shorter than for the demagnetization procedure, which is desirable for fast switching. The exchange coupling is a key issue in spin valves and tunnelling junctions, and hence our findings will help promote the development of exchange-coupled device concepts for ultrafast coherent spin manipulation.

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

    Science.gov (United States)

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

    2018-06-01

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

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

    Science.gov (United States)

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

    2015-03-17

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

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

    Science.gov (United States)

    Frank, Marius S.; Hättig, Christof

    2018-04-01

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

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

    DEFF Research Database (Denmark)

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

    2015-01-01

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

  1. Hadron fragment emission in cluster excitation processes at medium energies

    International Nuclear Information System (INIS)

    Kovacs, Zs.

    1985-12-01

    An extended version of the cluster excitation model is proposed to describe the emission of various particle types in nuclear reactions in a consistent way. At first pion, proton deuteron and triton spectra from neutron-carbon interactions at 545 MeV in the angular region from deg 73 to deg 165 were tried to interpret by the model. The results are compared with model calculations. (author)

  2. Quasi-particle excitations in low energy fission

    International Nuclear Information System (INIS)

    Ashgar, M.; Djebara, M.; Bocquet, J.P.; Brissot, R.; Maurel, M.; Nifenecker, H.; Ristori, C.

    1985-05-01

    Proton odd-even effect for 229 Th(nsub(th),f) and 232 U(nsub(th),f) has been determined with a ΔE-Esub(R) gas telescope. These data indicate that the qp-particle excitation probability at the saddle point is small and most of its results, when the nucleus moves from saddle to scission and the neck ruptures into final fragments. These results are discussed in terms of the different ideas and models

  3. Energy transfer dynamics in trimers and aggregates of light-harvesting complex II probed by 2D electronic spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Enriquez, Miriam M.; Zhang, Cheng; Tan, Howe-Siang, E-mail: howesiang@ntu.edu.sg [Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371 (Singapore); Akhtar, Parveen; Garab, Győző; Lambrev, Petar H., E-mail: lambrev@brc.hu [Institute of Plant Biology, Biological Research Centre, Hungarian Academy of Sciences, P.O. Box 521, H-6701 Szeged (Hungary)

    2015-06-07

    The pathways and dynamics of excitation energy transfer between the chlorophyll (Chl) domains in solubilized trimeric and aggregated light-harvesting complex II (LHCII) are examined using two-dimensional electronic spectroscopy (2DES). The LHCII trimers and aggregates exhibit the unquenched and quenched excitonic states of Chl a, respectively. 2DES allows direct correlation of excitation and emission energies of coupled states over population time delays, hence enabling mapping of the energy flow between Chls. By the excitation of the entire Chl b Q{sub y} band, energy transfer from Chl b to Chl a states is monitored in the LHCII trimers and aggregates. Global analysis of the two-dimensional (2D) spectra reveals that energy transfer from Chl b to Chl a occurs on fast and slow time scales of 240–270 fs and 2.8 ps for both forms of LHCII. 2D decay-associated spectra resulting from the global analysis identify the correlation between Chl states involved in the energy transfer and decay at a given lifetime. The contribution of singlet–singlet annihilation on the kinetics of Chl energy transfer and decay is also modelled and discussed. The results show a marked change in the energy transfer kinetics in the time range of a few picoseconds. Owing to slow energy equilibration processes, long-lived intermediate Chl a states are present in solubilized trimers, while in aggregates, the population decay of these excited states is significantly accelerated, suggesting that, overall, the energy transfer within the LHCII complexes is faster in the aggregated state.

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

    Science.gov (United States)

    Jennings, Robert C; Zucchelli, Giuseppe

    2014-01-01

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

  5. Exciplex-exciplex energy transfer and annihilation in solid films of porphyrin-fullerene dyads.

    Science.gov (United States)

    Lehtivuori, Heli; Lemmetyinen, Helge; Tkachenko, Nikolai V

    2006-12-20

    Exciplex-exciplex annihilation was observed for the first time in porphyrin-fullerene molecular films. The films were prepared using Langmuir-Blodgett and drop casting methods. The exciplex-exciplex interactions were studied using femtosecond pump-probe method. The exciplex-exciplex annihilation can be seen as a fast (within few picoseconds) decay of the transient absorption at excitation densities higher than 0.4 mJ/cm2. Analysis of the excitation density dependences indicates that in average four dyads are involved in the exciplex-exciplex interaction, suggesting that an exciplex-exciplex energy transfer may precede the annihilation.

  6. Spectroscopic studies of the energy transfer processes important to obtain holmium laser action in the Er:Tm:Ho:YLF

    International Nuclear Information System (INIS)

    Tarelho, Luiz Vicente Gomes

    1995-01-01

    There are several processes of energy transfer between Er, Tm and Ho ions in YLF crystal that could be evaluated using the Foerster-Dexter method. Energy transfer processes, important to understand Holmium laser action, were studied, specially involving the energy transfer between the first excited states of Er and Tm donors and Ho acceptor. The back-transfer processes were evaluated too in order to minimize the system losses. Another important process to understand Ho laser action in the host is the energy diffusion mechanism between donor ions due to excitation migration processes which take place before the energy transfer to Ho. The proposed model of energy transfer was developed to include the diffusion mechanism between donors in the absence and presence of the acceptors. The energy transfer probability was evaluated including the back-transfer processes besides the diffusion assistance. A laser medium model based on the fundamental spectroscopic parameters was used in order to determine the ideal donor acceptor concentrations in order to maximize the laser action of Ho at 2,1 μm. (author)

  7. Low energy nuclear spin excitations in Ho metal investigated by high resolution neutron spectroscopy.

    Science.gov (United States)

    Chatterji, Tapan; Jalarvo, Niina

    2013-04-17

    We have investigated the low energy excitations in metallic Ho by high resolution neutron spectroscopy. We found at T = 3 K clear inelastic peaks in the energy loss and energy gain sides, along with the central elastic peak. The energy of this low energy excitation, which is 26.59 ± 0.02 μeV at T = 3 K, decreased continuously and became zero at TN ≈ 130 K. By fitting the data in the temperature range 100-127.5 K with a power law we obtained the power-law exponent β = 0.37 ± 0.02, which agrees with the expected value β = 0.367 for a three-dimensional Heisenberg model. Thus the energy of the low energy excitations can be associated with the order parameter.

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

    International Nuclear Information System (INIS)

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

    1983-01-01

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

  9. Proceedings of the 1984 workshop on high-energy excitations in condensed matter. Volume II

    International Nuclear Information System (INIS)

    Silver, R.N.

    1984-12-01

    This volume covers electronic excitations, momentum distributions, high energy photons, and a wrap-up session. Abstracts of individual items from the conference were prepared separately for the data base

  10. Effect of Optical Excitation Energy on the Red Luminescence of Eu(3+) in GaN

    National Research Council Canada - National Science Library

    Peng, H. Y; Lee, C. W; Everitt, H. O; Lee, D. S; Steckl, A. J; Zavada, J. M

    2005-01-01

    ...)] transition from GaN:Eu. Time-resolved PL measurements revealed that for excitation at the GaN bound exciton energy, the decay transients are almost temperature insensitive between 86 K and 300 K, indicating an efficient...

  11. Ultrafast electron and energy transfer in dye-sensitized iron oxide and oxyhydroxide nanoparticles

    DEFF Research Database (Denmark)

    Gilbert, Benjamin; Katz, Jordan E.; Huse, Nils

    2013-01-01

    photo-initiated interfacial electron transfer. This approach enables time-resolved study of the fate and mobility of electrons within the solid phase. However, complete analysis of the ultrafast processes following dye photoexcitation of the sensitized iron(iii) oxide nanoparticles has not been reported....... We addressed this topic by performing femtosecond transient absorption (TA) measurements of aqueous suspensions of uncoated and DCF-sensitized iron oxide and oxyhydroxide nanoparticles, and an aqueous iron(iii)–dye complex. Following light absorption, excited state relaxation times of the dye of 115...... a four-state model of the dye-sensitized system, finding electron and energy transfer to occur on the same ultrafast timescale. The interfacial electron transfer rates for iron oxides are very close to those previously reported for DCF-sensitized titanium dioxide (for which dye–oxide energy transfer...

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

    International Nuclear Information System (INIS)

    Frey, R.W.

    1978-01-01

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

  13. Förster Resonance Energy Transfer between Quantum Dot Donors and Quantum Dot Acceptors

    Directory of Open Access Journals (Sweden)

    Kenny F. Chou

    2015-06-01

    Full Text Available Förster (or fluorescence resonance energy transfer amongst semiconductor quantum dots (QDs is reviewed, with particular interest in biosensing applications. The unique optical properties of QDs provide certain advantages and also specific challenges with regards to sensor design, compared to other FRET systems. The brightness and photostability of QDs make them attractive for highly sensitive sensing and long-term, repetitive imaging applications, respectively, but the overlapping donor and acceptor excitation signals that arise when QDs serve as both the donor and acceptor lead to high background signals from direct excitation of the acceptor. The fundamentals of FRET within a nominally homogeneous QD population as well as energy transfer between two distinct colors of QDs are discussed. Examples of successful sensors are highlighted, as is cascading FRET, which can be used for solar harvesting.

  14. Förster Resonance Energy Transfer between Quantum Dot Donors and Quantum Dot Acceptors

    Science.gov (United States)

    Chou, Kenny F.; Dennis, Allison M.

    2015-01-01

    Förster (or fluorescence) resonance energy transfer amongst semiconductor quantum dots (QDs) is reviewed, with particular interest in biosensing applications. The unique optical properties of QDs provide certain advantages and also specific challenges with regards to sensor design, compared to other FRET systems. The brightness and photostability of QDs make them attractive for highly sensitive sensing and long-term, repetitive imaging applications, respectively, but the overlapping donor and acceptor excitation signals that arise when QDs serve as both the donor and acceptor lead to high background signals from direct excitation of the acceptor. The fundamentals of FRET within a nominally homogeneous QD population as well as energy transfer between two distinct colors of QDs are discussed. Examples of successful sensors are highlighted, as is cascading FRET, which can be used for solar harvesting. PMID:26057041

  15. LIME - a flexible, non-LTE line excitation and radiation transfer method for millimeter and far-infrared wavelengths

    DEFF Research Database (Denmark)

    Brinch, Christian; Hogerheijde, Michiel

    2010-01-01

    We present a new code for solving the molecular and atomic excitation and radiation transfer problem in a molecular gas and predicting emergent spectra. This code works in arbitrary three dimensional geometry using unstructured Delaunay latices for the transport of photons. Various physical model...

  16. Environment-sensitive quinolone demonstrating long-lived fluorescence and unusually slow excited-state intramolecular proton transfer kinetics

    Czech Academy of Sciences Publication Activity Database

    Zamotaiev, O. M.; Shvadchak, Volodymyr; Sych, T. P.; Melnychuk, N. A.; Yushchenko, Dmytro A.; Mely, Y.; Pivovarenko, V. G.

    2016-01-01

    Roč. 4, č. 3 (2016), č. článku 034004. ISSN 2050-6120 Institutional support: RVO:61388963 Keywords : quinolone * fluorescent probes * local polarity * hydration * excited-state intramolecular proton transfer * kinetics Subject RIV: CC - Organic Chemistry Impact factor: 2.656, year: 2016

  17. ANISOTROPY EFFECTS IN SINGLE-ELECTRON TRANSFER BETWEEN LASER-EXCITED ATOMS AND HIGHLY-CHARGED IONS

    NARCIS (Netherlands)

    Recent collision experiments are reviewed in which one-electron transfer between laser excited target atoms and (highly charged) keV-ions has been studied. Especially results showing a dependence of the charge exchange on the initial target orbital alignment are discussed. The question to what

  18. An intramolecular charge transfer state of carbonyl carotenoids: implications for excited state dynamics of apo-carotenals and retinal

    Czech Academy of Sciences Publication Activity Database

    Polívka, Tomáš; Kaligotla, S.; Chábera, P.; Frank, H.A.

    2011-01-01

    Roč. 13, č. 22 (2011), s. 1463-9076 ISSN 1463-9076 Institutional research plan: CEZ:AV0Z50510513 Keywords : carotenoid * retinal * excited-state dynamics * charge-transfer state Subject RIV: BO - Biophysics Impact factor: 3.573, year: 2011

  19. Excited-state intramolecular proton transfer of 2-acetylindan-1,3-dione studied by ultrafast absorption and fluorescence spectroscopy

    Directory of Open Access Journals (Sweden)

    Pramod Kumar Verma

    2016-03-01

    Full Text Available We employ transient absorption from the deep-UV to the visible region and fluorescence upconversion to investigate the photoinduced excited-state intramolecular proton-transfer dynamics in a biologically relevant drug molecule, 2-acetylindan-1,3-dione. The molecule is a ß-diketone which in the electronic ground state exists as exocyclic enol with an intramolecular H-bond. Upon electronic excitation at 300 nm, the first excited state of the exocyclic enol is initially populated, followed by ultrafast proton transfer (≈160 fs to form the vibrationally hot endocyclic enol. Subsequently, solvent-induced vibrational relaxation takes place (≈10 ps followed by decay (≈390 ps to the corresponding ground state.

  20. Identification of the low-energy excitations in a quantum critical system

    Directory of Open Access Journals (Sweden)

    Tom Heitmann

    2017-05-01

    Full Text Available We have identified low-energy magnetic excitations in a doped quantum critical system by means of polarized neutron scattering experiments. The presence of these excitations could explain why Ce(Fe0.76Ru0.242Ge2 displays dynamical scaling in the absence of local critical behavior or long-range spin-density wave criticality. The low-energy excitations are associated with the reorientations of the superspins of fully ordered, isolated magnetic clusters that form spontaneously upon lowering the temperature. The system houses both frozen clusters and dynamic clusters, as predicted by Hoyos and Vojta [Phys. Rev. B 74, 140401(R (2006].

  1. The security energy encryption in wireless power transfer

    Science.gov (United States)

    Sadzali, M. N.; Ali, A.; Azizan, M. M.; Albreem, M. A. M.

    2017-09-01

    This paper presents a concept of security in wireless power transfer (WPT) by applying chaos theory. Chaos theory is applied as a security system in order to safeguard the transfer of energy from a transmitter to the intended receiver. The energy encryption of the wireless power transfer utilizes chaos theory to generate the possibility of a logistic map for the chaotic security key. The simulation for energy encryption wireless power transfer system was conducted by using MATLAB and Simulink. By employing chaos theory, the chaotic key ensures the transmission of energy from transmitter to its intended receiver.

  2. Dynamics of electron solvation in methanol: Excited state relaxation and generation by charge-transfer-to-solvent

    International Nuclear Information System (INIS)

    Elkins, Madeline H.; Williams, Holly L.; Neumark, Daniel M.

    2015-01-01

    The charge-transfer-to-solvent dynamics (CTTS) and excited state relaxation mechanism of the solvated electron in methanol are studied by time-resolved photoelectron spectroscopy on a liquid methanol microjet by means of two-pulse and three-pulse experiments. In the two-pulse experiment, CTTS excitation is followed by a probe photoejection pulse. The resulting time-evolving photoelectron spectrum reveals multiple time scales characteristic of relaxation and geminate recombination of the initially generated electron which are consistent with prior results from transient absorption. In the three-pulse experiment, the relaxation dynamics of the solvated electron following electronic excitation are measured. The internal conversion lifetime of the excited electron is found to be 130 ± 40 fs, in agreement with extrapolated results from clusters and the non-adiabatic relaxation mechanism

  3. Dynamics of electron solvation in methanol: Excited state relaxation and generation by charge-transfer-to-solvent

    Science.gov (United States)

    Elkins, Madeline H.; Williams, Holly L.; Neumark, Daniel M.

    2015-06-01

    The charge-transfer-to-solvent dynamics (CTTS) and excited state relaxation mechanism of the solvated electron in methanol are studied by time-resolved photoelectron spectroscopy on a liquid methanol microjet by means of two-pulse and three-pulse experiments. In the two-pulse experiment, CTTS excitation is followed by a probe photoejection pulse. The resulting time-evolving photoelectron spectrum reveals multiple time scales characteristic of relaxation and geminate recombination of the initially generated electron which are consistent with prior results from transient absorption. In the three-pulse experiment, the relaxation dynamics of the solvated electron following electronic excitation are measured. The internal conversion lifetime of the excited electron is found to be 130 ± 40 fs, in agreement with extrapolated results from clusters and the non-adiabatic relaxation mechanism.

  4. Dynamics of electron solvation in methanol: Excited state relaxation and generation by charge-transfer-to-solvent

    Energy Technology Data Exchange (ETDEWEB)

    Elkins, Madeline H.; Williams, Holly L. [Department of Chemistry, University of California, Berkeley, California 94720 (United States); Neumark, Daniel M. [Department of Chemistry, University of California, Berkeley, California 94720 (United States); Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)

    2015-06-21

    The charge-transfer-to-solvent dynamics (CTTS) and excited state relaxation mechanism of the solvated electron in methanol are studied by time-resolved photoelectron spectroscopy on a liquid methanol microjet by means of two-pulse and three-pulse experiments. In the two-pulse experiment, CTTS excitation is followed by a probe photoejection pulse. The resulting time-evolving photoelectron spectrum reveals multiple time scales characteristic of relaxation and geminate recombination of the initially generated electron which are consistent with prior results from transient absorption. In the three-pulse experiment, the relaxation dynamics of the solvated electron following electronic excitation are measured. The internal conversion lifetime of the excited electron is found to be 130 ± 40 fs, in agreement with extrapolated results from clusters and the non-adiabatic relaxation mechanism.

  5. Excitation energy of the lowest 2+ and 3- levels in 32Mg and 146Gd

    International Nuclear Information System (INIS)

    Barranco, M.; Lombard, R.J.

    1978-06-01

    The excitation energy of the lowest 2 + and 3 - levels are calculated for neutron rich Mg-isotopes as well as for N=82 isotones. The calculations are made by assuming quadrupole-quadrupole and octupole-octupole forces. The quasi-particles energies and occupation numbers are taken from the energy density method

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

    Indian Academy of Sciences (India)

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

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

    Indian Academy of Sciences (India)

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

  8. Energy risk management through self-exciting marked point process

    International Nuclear Information System (INIS)

    Herrera, Rodrigo

    2013-01-01

    Crude oil is a dynamically traded commodity that affects many economies. We propose a collection of marked self-exciting point processes with dependent arrival rates for extreme events in oil markets and related risk measures. The models treat the time among extreme events in oil markets as a stochastic process. The main advantage of this approach is its capability to capture the short, medium and long-term behavior of extremes without involving an arbitrary stochastic volatility model or a prefiltration of the data, as is common in extreme value theory applications. We make use of the proposed model in order to obtain an improved estimate for the Value at Risk in oil markets. Empirical findings suggest that the reliability and stability of Value at Risk estimates improve as a result of finer modeling approach. This is supported by an empirical application in the representative West Texas Intermediate (WTI) and Brent crude oil markets. - Highlights: • We propose marked self-exciting point processes for extreme events in oil markets. • This approach captures the short and long-term behavior of extremes. • We improve the estimates for the VaR in the WTI and Brent crude oil markets

  9. Proposal for probing energy transfer pathway by single-molecule pump-dump experiment

    OpenAIRE

    Tao, Ming-Jie; Ai, Qing; Deng, Fu-Guo; Cheng, Yuan-Chung

    2016-01-01

    The structure of Fenna-Matthews-Olson (FMO) light-harvesting complex has long been recognized as containing seven bacteriochlorophyll (BChl) molecules. Recently, an additional BChl molecule was discovered in the crystal structure of the FMO complex, which may serve as a link between baseplate and the remaining seven molecules. Here, we investigate excitation energy transfer (EET) process by simulating single-molecule pump-dump experiment in the eight-molecules complex. We adopt the coherent m...

  10. An excited-state intramolecular photon transfer fluorescence probe for localizable live cell imaging of cysteine

    Science.gov (United States)

    Liu, Wei; Chen, Wen; Liu, Si-Jia; Jiang, Jian-Hui

    2017-03-01

    Small molecule probes suitable for selective and specific fluorescence imaging of some important but low-concentration intracellular reactive sulfur species such as cysteine (Cys) pose a challenge in chemical biology. We present a readily available, fast-response fluorescence probe CHCQ-Ac, with 2-(5‧-chloro-2-hydroxyl-phenyl)-6-chloro-4(3 H)-quinazolinone (CHCQ) as the fluorophore and acrylate group as the functional moiety, that enables high-selectivity and high-sensitivity for detecting Cys in both solution and biological system. After specifically reacted with Cys, the probe undergoes a seven-membered intramolecular cyclization and released the fluorophore CHCQ with excited-state intramolecular photon transfer effect. A highly fluorescent, insoluble aggregate was then formed to facilitate high-sensitivity and high-resolution imaging. The results showed that probe CHCQ-Ac affords a remarkably large Stokes shift and can detect Cys under physiological pH condition with no interference from other analytes. Moreover, this probe was proved to have excellent chemical stability, low cytotoxicity and good cell permeability. Our design of this probe provides a novel potential tool to visualize and localize cysteine in bioimaging of live cells that would greatly help to explore various Cys-related physiological and pathological cellular processes in cell biology and diagnostics.

  11. The study of quasi-projectiles produced in Ni+Ni and Ni+Au collisions: excitation energy and spin

    International Nuclear Information System (INIS)

    Buta, A.

    2003-02-01

    During the collision between the projectile and the target nuclei in the intermediate energy regime (E < 100 MeV/nucleon) two excited nuclei are mainly observed in the exit channel, the quasi projectile (QP) and the quasi target. They disintegrate by particle emission. However, this binary picture is perturbed by the emission of particles and light fragments with velocities intermediate between the projectile velocity and the target one, all along the interaction (midrapidity component). This work aim to determine the excitation energy and the intrinsic angular momentum (or spin) of quasi-projectiles produced in the Ni+Ni and Ni+Au collisions at 52 and 90 MeV/nucleon. The excitation energy is deduced from the kinematical characteristics of particles emitted by the quasi-projectile. They have to be separated from midrapidity particles. Three different scenarios have been used for this purpose. The spin of the quasi-projectile has been extracted from the experimental data by mean of proton and alpha particles multiplicities emitted by the QP in the Ni+Au at 52 MeV/nucleon reaction. The results have been compared to the predictions of a theoretical model based on nucleon transfers. Their evolution is qualitatively reproduced as a function of the violence of the collision. (author)

  12. Controlling resonance energy transfer in nanostructure emitters by positioning near a mirror

    Science.gov (United States)

    Weeraddana, Dilusha; Premaratne, Malin; Gunapala, Sarath D.; Andrews, David L.

    2017-08-01

    The ability to control light-matter interactions in quantum objects opens up many avenues for new applications. We look at this issue within a fully quantized framework using a fundamental theory to describe mirror-assisted resonance energy transfer (RET) in nanostructures. The process of RET communicates electronic excitation between suitably disposed donor and acceptor particles in close proximity, activated by the initial excitation of the donor. Here, we demonstrate that the energy transfer rate can be significantly controlled by careful positioning of the RET emitters near a mirror. The results deliver equations that elicit new insights into the associated modification of virtual photon behavior, based on the quantum nature of light. In particular, our results indicate that energy transfer efficiency in nanostructures can be explicitly expedited or suppressed by a suitably positioned neighboring mirror, depending on the relative spacing and the dimensionality of the nanostructure. Interestingly, the resonance energy transfer between emitters is observed to "switch off" abruptly under suitable conditions of the RET system. This allows one to quantitatively control RET systems in a new way.

  13. Ligand manipulation of charge transfer excited state relaxation and spin crossover in [Fe(2,2′-bipyridine)2(CN)2

    DEFF Research Database (Denmark)

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

    2017-01-01

    We have used femtosecond resolution UV-visible and Kβ x-ray emission spectroscopy to characterize the electronic excited state dynamics of [Fe(bpy)2(CN)2], where bpy=2,2′-bipyridine, initiated by metal-to-ligand charge transfer (MLCT) excitation. The excited-state absorption in the transient UV-visible...

  14. Isobar excitations and low energy spectra of light nuclei

    International Nuclear Information System (INIS)

    Czerski, P.

    1984-01-01

    The aim of this investigation is to study the possible influence of inner excitations of nucleons into the Δ(3,3)-resonance on the low lying spectra of light nuclei like 12 C and 16 O. Before we can study the effect of such exotic configurations one has to perform a reliable investigation within the normal nuclear model, which is based on a microscopic theory. This is achieved by performing RPA (Random Phase Approximation) calculations using a realistic residual interaction derived from the Brueckner G-matrix. An efficient parametrisation of the residual interaction is introduced and the reliability of the more phenomenological parametrisations which are generally used is discussed. Within such realistic calculations, the isobar effects are small. (orig.) [de

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

    Science.gov (United States)

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

    2017-12-07

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

  16. Energy and Information Transfer Via Coherent Exciton Wave Packets

    Science.gov (United States)

    Zang, Xiaoning

    associated excitations were dubbed twisted excitons. Twisted exciton packets can be manipulated as they travel down molecular chains, and this has applications in quantum information science as well. In each setting considered, exciton dynamics were initially studied using a simple tight-binding formalism. This misses the actual many-body interactions and multiple energy levels associated real systems. To remedy this, I adapted an existing time-domain Density Functional Theory code and applied it to study the dynamics of exciton wave packets on quasi-one-dimensional systems. This required the use of high-performance computing and the construction of a number of key auxiliary codes. Establishing the requisite methodology constituted a substantial part of the entire thesis. Surprisingly, this effort uncovered a computational issue associated with Rabi oscillations that had been incorrectly characterized in the literature. My research elucidated the actual problem and a solution was found. This new methodology was an integral part of the overall computational analysis. The thesis then takes up the a detailed consideration of the prospect for creating systems that support a strong measure of transport coherence. While physical implementations include molecular assemblies, solid-state superlattices, and even optical lattices, I decided to focus on assemblies of nanometer-sized silicon quantum dots. First principles computational analysis was used to quantify reorganization within individual dots and excitonic coupling between dots. Quantum dot functionalizations were identified that make it plausible to maintain a measure of excitonic coherence even at room temperatures. Attention was then turned to the use of covalently bonded bridge material to join quantum dots in a way that facilitates efficient exciton transfer. Both carbon and silicon structures were considered by considering the way in which subunits might be best brought together. This resulted in a set of design criteria

  17. Energy and charge transfer dynamics between Alq3 and CdSeS nanocrystals.

    Science.gov (United States)

    Zhang, Shuping; Liu, Yuqiang; Yang, Yanqiang

    2010-03-01

    The photoluminescence properties of the blend films consisting of organic small molecules and nanocrystals (NCs)--Alq3 and CdSeS NCs--were studied by steady-state and time-resolved photoluminescence (PL) spectroscopy with different excited wavelengths. Both the fluorescence intensity and lifetime are intensively dependent on the NC concentration. The detailed analysis of experiment data proves that Forster energy transfer from the Alq3 to the NCs exists simultaneously with the charge transfer and both compete with each other in the blend films.

  18. Mode-to-mode energy transfers in convective patterns

    Indian Academy of Sciences (India)

    Abstract. We investigate the energy transfer between various Fourier modes in a low- dimensional model for thermal convection. We have used the formalism of mode-to-mode energy transfer rate in our calculation. The evolution equations derived using this scheme is the same as those derived using the hydrodynamical ...

  19. Solvent-dependent excited-state hydrogen transfer and intersystem crossing in 2-(2′-hydroxyphenyl)-benzothiazole

    KAUST Repository

    Aly, Shawkat Mohammede

    2015-02-12

    The excited-state intramolecular hydrogen transfer (ESIHT) of 2-(2′-hydroxyphenyl) benzothiazole (HBT) has been investigated in a series of nonpolar, polar aprotic, and polar protic solvents. A variety of state-of-the-art experimental methods were employed, including femto- and nanosecond transient absorption and fluorescence upconversion spectroscopy with broadband capabilities. We show that the dynamics and mechanism of ESIHT of the singlet excited HBT are strongly solvent-dependent. In nonpolar solvents, the data demonstrate that HBT molecules adopt a closed form stabilized by O-H⋯N chelated hydrogen bonds with no twisting angle, and the photoinduced H transfer occurs within 120 fs, leading to the formation of a keto tautomer. In polar solvents, owing to dipole-dipole cross talk and hydrogen bonding interactions, the H transfer process is followed by ultrafast nonradiative deactivation channels, including ultrafast internal conversion (IC) and intersystem crossing (ISC). This is likely to be driven by the twisting motion around the C-C bond between the hydroxyphenyl and thiazole moieties, facilitating the IC back to the enol ground state or to the keto triplet state. In addition, our femtosecond time-resolved fluorescence experiments indicate, for the first time, that the lifetime of the enol form in ACN is approximately 280 fs. This observation indicates that the solvent plays a crucial role in breaking the H bond and deactivating the excited state of the HBT. Interestingly, the broadband transient absorption and fluorescence up-conversion data clearly demonstrate that the intermolecular proton transfer from the excited HBT to the DMSO solvent is about 190 fs, forming the HBT anion excited state.

  20. Solvent-dependent excited-state hydrogen transfer and intersystem crossing in 2-(2′-hydroxyphenyl)-benzothiazole

    KAUST Repository

    Aly, Shawkat Mohammede; Usman, Anwar; Alzayer, Maytham; Hamdi, Ghada A.; Alarousu, Erkki; Mohammed, Omar F.

    2015-01-01

    The excited-state intramolecular hydrogen transfer (ESIHT) of 2-(2′-hydroxyphenyl) benzothiazole (HBT) has been investigated in a series of nonpolar, polar aprotic, and polar protic solvents. A variety of state-of-the-art experimental methods were employed, including femto- and nanosecond transient absorption and fluorescence upconversion spectroscopy with broadband capabilities. We show that the dynamics and mechanism of ESIHT of the singlet excited HBT are strongly solvent-dependent. In nonpolar solvents, the data demonstrate that HBT molecules adopt a closed form stabilized by O-H⋯N chelated hydrogen bonds with no twisting angle, and the photoinduced H transfer occurs within 120 fs, leading to the formation of a keto tautomer. In polar solvents, owing to dipole-dipole cross talk and hydrogen bonding interactions, the H transfer process is followed by ultrafast nonradiative deactivation channels, including ultrafast internal conversion (IC) and intersystem crossing (ISC). This is likely to be driven by the twisting motion around the C-C bond between the hydroxyphenyl and thiazole moieties, facilitating the IC back to the enol ground state or to the keto triplet state. In addition, our femtosecond time-resolved fluorescence experiments indicate, for the first time, that the lifetime of the enol form in ACN is approximately 280 fs. This observation indicates that the solvent plays a crucial role in breaking the H bond and deactivating the excited state of the HBT. Interestingly, the broadband transient absorption and fluorescence up-conversion data clearly demonstrate that the intermolecular proton transfer from the excited HBT to the DMSO solvent is about 190 fs, forming the HBT anion excited state.

  1. Influence of collision energy and vibrational excitation on the ...

    Indian Academy of Sciences (India)

    tions of potential energy surface (PES) for BrH2 system are more ... rier heights for both the exchange and abstraction are smaller than ... The complete picture on the dynamics of ..... Kurosaki Y and Takayanagi T private communication. 20.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-11-14

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

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

    International Nuclear Information System (INIS)

    Shamim, Md; Harbola, Manoj K

    2010-01-01

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

  4. Competitive photocyclization/rearrangement of 4-aryl-1,1-dicyanobutenes controlled by intramolecular charge-transfer interaction. Effect of medium polarity, temperature, pressure, excitation wavelength, and confinement.

    Science.gov (United States)

    Ito, Tadashi; Nishiuchi, Emi; Fukuhara, Gaku; Inoue, Yoshihisa; Mori, Tadashi

    2011-09-01

    A series of 4-aryl-1,1-dicyanobutenes (1a-1f) with different substituents were synthesized to control the intramolecular donor-acceptor or charge-transfer (C-T) interactions in the ground state. Photoexcitation of these C-T substrates led to competitive cyclization and rearrangement, the ratio being critically controlled by various environmental factors, such as solvent polarity, temperature and static pressure, and also by excitation wavelength and supramolecular confinement (polyethylene voids). In non-polar solvents, the rearrangement was dominant (>10 : 1) for all examined substrates, while the cyclization was favoured in polar solvents, in particular at low temperatures. Selective excitation at the C-T band further enhanced the cyclization up to >50 : 1 ratios. More importantly, the cyclization/rearrangement ratio was revealed to be a linear function of the C-T transition energy. However, the substrates with a sterically demanding or highly electron-donating substituent failed to give the cyclization product.

  5. Coherent population transfer and superposition of atomic states via stimulated Raman adiabatic passage using an excited-doublet four-level atom

    International Nuclear Information System (INIS)

    Jin Shiqi; Gong Shangqing; Li Ruxin; Xu Zhizhan

    2004-01-01

    Coherent population transfer and superposition of atomic states via a technique of stimulated Raman adiabatic passage in an excited-doublet four-level atomic system have been analyzed. It is shown that the behavior of adiabatic passage in this system depends crucially on the detunings between the laser frequencies and the corresponding atomic transition frequencies. Particularly, if both the fields are tuned to the center of the two upper levels, the four-level system has two degenerate dark states, although one of them contains the contribution from the excited atomic states. The nonadiabatic coupling of the two degenerate dark states is intrinsic, it originates from the energy difference of the two upper levels. An arbitrary superposition of atomic states can be prepared due to such nonadiabatic coupling effect

  6. Fluorescence Resonance Energy Transfer in Polydiacetylene Liposomes

    Science.gov (United States)

    Li, Xuelian; Matthews, Shelton; Kohli, Punit

    2009-01-01

    Conjugated polydiacetylene (PDA) possessing stimuli-responsive properties has been intensively investigated for developing efficient sensors. We report here fluorescence resonance energy transfer (FRET) in liposomes synthesized using different molar ratios of dansyl-tagged diacetylene and diacetylene–carboxylic acid monomers. Photopolymerization of diacetylene resulted in cross-linked PDA liposomes. We used steady-state electronic absorption, emission, and fluorescence anisotropy (FA) analysis to characterize the thermal-induced FRET between dansyl fluorophores (donor) and PDA (acceptor). We found that the monomer ratio of acceptor to donor (Rad) and length of linkers (functional part that connects dansyl fluorophores to the diacetylene group in the monomer) strongly affected FRET. For Rad = 10 000, the acceptor emission intensity was amplified by more than 18 times when the liposome solution was heated from 298 to 338 K. A decrease in Rad resulted in diminished acceptor emission amplification. This was primarily attributed to lower FRET efficiency between donors and acceptors and a higher background signal. We also found that the FRET amplification of PDA emissions after heating the solution was much higher when dansyl was linked to diacetylene through longer and flexible linkers than through shorter linkers. We attributed this to insertion of dansyl in the bilayer of the liposomes, which led to an increased dansyl quantum yield and a higher interaction of multiple acceptors with limited available donors. This was not the case for shorter and more rigid linkers where PDA amplification was much smaller. The present studies aim at enhancing our understanding of FRET between fluorophores and PDA-based conjugated liposomes. Furthermore, receptor tagged onto PDA liposomes can interact with ligands present on proteins, enzymes, and cells, which will produce emission sensing signal. Therefore, using the present approach, there exist opportunities for designing FRET

  7. Toward understanding as photosynthetic biosignatures: light harvesting and energy transfer calculation

    Science.gov (United States)

    Komatsu, Y.; Umemura, M.; Shoji, M.; Shiraishi, K.; Kayanuma, M.; Yabana, K.

    2014-03-01

    Among several proposed biosignatures, red edge is a direct evidence of photosynthetic life if it is detected (Kiang et al 2007). Red edge is a sharp change in reflectance spectra of vegetation in NIR region (about 700-750 nm). The sign of red edge is observed by Earthshine or remote sensing (Wolstencroft & Raven 2002, Woolf et al 2002). But, why around 700-750 nm? The photosynthetic organisms on Earth have evolved to optimize the sunlight condition. However, if we consider about photosynthetic organism on extrasolar planets, they should have developed to utilize the spectra of its principal star. Thus, it is not strange even if it shows different vegetation spectra. In this study, we focused on the light absorption mechanism of photosynthetic organisms on Earth and investigated the fundamental properties of the light harvesting mechanisms, which is the first stage for the light absorption. Light harvesting complexes contain photosynthetic pigments like chlorophylls. Effective light absorption and the energy transfer are accomplished by the electronic excitations of collective photosynthetic pigments. In order to investigate this mechanism, we constructed an energy transfer model by using a dipole-dipole approximation for the interactions between electronic excitations. Transition moments and transition energies of each pigment are calculated at the time-dependent density functional theory (TDDFT) level (Marques & Gross 2004). Quantum dynamics simulation for the excitation energy transfer was calculated by the Liouvelle's equation. We adopted the model to purple bacteria, which has been studied experimentally and known to absorb lower energy. It is meaningful to focus on the mechanism of this bacteria, since in the future mission, M planets will become a important target. We calculated the oscillator strengths in one light harvesting complex and confirmed the validity by comparing to the experimental data. This complex is made of an inner and an outer ring. The

  8. Controlling energy transfer between multiple dopants within a single nanoparticle

    Science.gov (United States)

    DiMaio, Jeffrey R.; Sabatier, Clément; Kokuoz, Baris; Ballato, John

    2008-01-01

    Complex core-shell architectures are implemented within LaF3 nanoparticles to allow for a tailored degree of energy transfer (ET) between different rare earth dopants. By constraining specific dopants to individual shells, their relative distance to one another can be carefully controlled. Core-shell LaF3 nanoparticles doped with Tb3+ and Eu3+ and consisting of up to four layers were synthesized with an outer diameter of ≈10 nm. It is found that by varying the thicknesses of an undoped layer between a Tb3+-doped layer and a Eu3+-doped layer, the degree of ET can be engineered to allow for zero, partial, or total ET from a donor ion to an acceptor ion. More specifically, the ratio of the intensities of the 541-nm Tb3+ and 590 nm Eu3+ peaks was tailored from core-shell configuration that restricts ET is used. Beyond simply controlling ET, which can be limiting when designing materials for optical applications, this approach can be used to obtain truly engineered spectral features from nanoparticles and composites made from them. Further, it allows for a single excitation source to yield multiple discrete emissions from numerous lanthanide dopants that heretofore would have been quenched in a more conventional active optical material. PMID:18250307

  9. Study of primary energy transfer process in ultrafast plastic scintillators

    International Nuclear Information System (INIS)

    Bengtson, B.; Moszynski, M.

    1978-01-01

    The study of the light-pulse shape, the initial delay of light pulses and the light yield of plastics prepared by a modification of the NE111 scintillator were performed. The NE111 scintillator doped with several quench agents, the plastics prepared as a solution of butyl PBD in PVT of different concentration and PVT alone were studied. The study confirmed that the light pulse shape from fast binary plastics is well described analytically by the convolution of the clipped Gaussian and exponential functions. The investigation of the PVT-butyl PBD plastics shows that even more than three times larger concentration of butyl PBD compared to that of PBD in the NE111 solution does not improve the rise of the light pulse. Thus the rise time seems to be not controlled by the intermolecular energy transfer process. Finally, the observed rise time of the light pulse from the PVT sample was also approximated well by the Gaussian function. Altogether it brought a strong support for the earlier hypothesis that the initial slow rise of light pulses from plastic scintillators may come from the deexcitation of several higher levels of the solvent molecules excited by nuclear particles. (Auth.)

  10. X-ray spectroscopy studies of nonradiative energy transfer processes in luminescent lanthanide materials

    Science.gov (United States)

    Pacold, Joseph I.

    Luminescent materials play important roles in energy sciences, through solid state lighting and possible applications in solar energy utilization, and in biomedical research and applications, such as in immunoassays and fluorescence microscopy. The initial excitation of a luminescent material leads to a sequence of transitions between excited states, ideally ending with the emission of one or more optical-wavelength photons. It is essential to understand the microscopic physics of this excited state cascade in order to rationally design materials with high quantum efficiencies or with other fine-tuning of materials response. While optical-wavelength spectroscopies have unraveled many details of the energy transfer pathways in luminescent materials, significant questions remain open for many lanthanide-based luminescent materials. For organometallic dyes in particular, quantum yields remain limited in comparison with inorganic phosphors. This dissertation reports on a research program of synchrotron x-ray studies of the excited state electronic structure and energy-relaxation cascade in trivalent lanthanide phosphors and dyes. To this end, one of the primary results presented here is the first time-resolved x-ray absorption near edge spectroscopy studies of the transient 4f excited states in lanthanide-activated luminescent dyes and phosphors. This is a new application of time-resolved x-ray absorption spectroscopy that makes it possible to directly observe and, to some extent, quantify intramolecular nonradiative energy transfer processes. We find a transient increase in 4f spectral weight associated with an excited state confined to the 4f shell of trivalent Eu. This result implies that it is necessary to revise the current theoretical understanding of 4f excitation in trivalent lanthanide activators: either transient 4f-5d mixing effects are much stronger than previously considered, or else the lanthanide 4f excited state has an unexpectedly large contribution

  11. Competition between excited core states and 1homega single-particle excitations at comparable energies in {sup 207}Pb from photon scattering

    Energy Technology Data Exchange (ETDEWEB)

    Pietralla, N., E-mail: pietralla@ikp.tu-darmstadt.d [Institut fuer Kernphysik, Technische Universitaet Darmstadt, 64289 Darmstadt (Germany); Nuclear Structure Laboratory, SUNY at Stony Brook, Stony Brook, NY 11794-3800 (United States); Institut fuer Kernphysik, Universitaet zu Koeln, 50937 Koeln (Germany); Li, T.C. [Nuclear Structure Laboratory, SUNY at Stony Brook, Stony Brook, NY 11794-3800 (United States); Fritzsche, M. [Institut fuer Kernphysik, Technische Universitaet Darmstadt, 64289 Darmstadt (Germany); Ahmed, M.W. [Triangle Universities Nuclear Laboratory (TUNL), Duke University, Durham, NC 27708 (United States); Ahn, T.; Costin, A. [Institut fuer Kernphysik, Technische Universitaet Darmstadt, 64289 Darmstadt (Germany); Nuclear Structure Laboratory, SUNY at Stony Brook, Stony Brook, NY 11794-3800 (United States); Institut fuer Kernphysik, Universitaet zu Koeln, 50937 Koeln (Germany); Enders, J. [Institut fuer Kernphysik, Technische Universitaet Darmstadt, 64289 Darmstadt (Germany); Li, J. [Duke Free Electron Laser Laboratory (DFELL), Duke University, Durham, NC 27708 (United States); Mueller, S.; Neumann-Cosel, P. von [Institut fuer Kernphysik, Technische Universitaet Darmstadt, 64289 Darmstadt (Germany); Pinayev, I.V. [Duke Free Electron Laser Laboratory (DFELL), Duke University, Durham, NC 27708 (United States); Ponomarev, V.Yu.; Savran, D. [Institut fuer Kernphysik, Technische Universitaet Darmstadt, 64289 Darmstadt (Germany); Tonchev, A.P.; Tornow, W.; Weller, H.R. [Triangle Universities Nuclear Laboratory (TUNL), Duke University, Durham, NC 27708 (United States); Werner, V. [A.W. Wright Nuclear Structure Laboratory (WNSL), Yale University, New Haven, CT (United States); Wu, Y.K. [Duke Free Electron Laser Laboratory (DFELL), Duke University, Durham, NC 27708 (United States); Zilges, A. [Institut fuer Kernphysik, Universitaet zu Koeln, 50937 Koeln (Germany)

    2009-10-26

    The Pb(gamma{sup -}>,gamma{sup '}) photon scattering reaction has been studied with the nearly monochromatic, linearly polarized photon beams at the High Intensity gamma-ray Source (HIgammaS) at the DFELL. Azimuthal scattering intensity asymmetries measured with respect to the polarization plane of the beam have been used for the first time to assign both the spin and parity quantum numbers of dipole excited states of {sup 206,207,208}Pb at excitation energies in the vicinity of 5.5 MeV. Evidence for dominant particle-core coupling is deduced from these results along with information on excitation energies and electromagnetic transition matrix elements. Implications of the existence of weakly coupled states built on highly excited core states in competition with 1homega single particle (hole) excitations at comparable energies are discussed.

  12. Molecular structures and excited states of CpM(CO)(2) (Cp = eta(5)-C(5)H(5); M = Rh, Ir) and [Cl(2)Rh(CO)(2)](-). Theoretical evidence for a competitive charge transfer mechanism.

    Science.gov (United States)

    Hu, Zhenming; Boyd, Russell J; Nakatsuji, Hiroshi

    2002-03-20

    Molecular structures and excited states of CpM(CO)(2) (Cp = eta(5)-C(5)H(5); M = Rh, Ir) and [Cl(2)Rh(CO)(2)](-) complexes have been investigated using the B3LYP and the symmetry-adapted cluster (SAC)/SAC-configuration interaction (SAC-CI) theoretical methods. All the dicarbonyl complexes have singlet ground electronic states with large singlet-triplet separations. Thermal dissociations of CO from the parent dicarbonyls are energetically unfavorable. CO thermal dissociation is an activation process for [Cl(2)Rh(CO)(2)](-) while it is a repulsive potential for CpM(CO)(2). The natures of the main excited states of CpM(CO)(2) and [Cl(2)Rh(CO)(2)](-) are found to be quite different. For [Cl(2)Rh(CO)(2)](-), all the strong transitions are identified to be metal to ligand CO charge transfer (MLCT) excitations. A significant feature of the excited states of CpM(CO)(2) is that both MLCT excitation and a ligand Cp to metal and CO charge transfer excitation are strongly mixed in the higher energy states with the latter having the largest oscillator strength. A competitive charge transfer excited state has therefore been identified theoretically for CpRh(CO)(2) and CpIr(CO)(2). The wavelength dependence of the quantum efficiencies for the photoreactions of CpM(CO)(2) reported by Lees et al. can be explained by the existence of two different types of excited states. The origin of the low quantum efficiencies for the C-H/S-H bond activations of CpM(CO)(2) can be attributed to the smaller proportion of the MLCT excitation in the higher energy states.

  13. Photophysical properties of 1-acetoxy-8-hydroxy-1,4,4a,9a-tetrahydroanthraquinone: Evidence for excited state proton transfer reaction

    International Nuclear Information System (INIS)

    Singh, Rupashree Balia; Mahanta, Subrata; Guchhait, Nikhil

    2007-01-01

    The photophysical properties of 1-acetoxy-8-hydroxy-1,4,4a,9a-tetrahydroanthraquinone (HTHQ) have been investigated by steady state and time resolved spectroscopy in combination with quantum chemical calculations. The effects of various parameters such as the nature of solvent and pH of the medium on the spectral properties confirm the existence of different neutral and ionic species in the ground and excited states. In the ground state, HTHQ exists as intramolecularly hydrogen bonded closed conformer in non-polar and polar aprotic solvents. Apart from the closed conformer, the intermolecular hydrogen bonded solvated species and the anion of HTHQ are present in hydroxylic solvents. The closed conformer shows excited state intramolecular proton transfer in all solvents and the solvent polarity independent red shifted emission indicates only keto-enol tautomerism. Evaluation of the potential energy surfaces by quantum chemical calculation using density functional theory point towards the possibility of proton transfer reaction in the first excited state but not in the ground state

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

    International Nuclear Information System (INIS)

    Gardner, J.W.

    1980-01-01

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

  15. Light harvesting via energy transfer in the dye solar cell

    Energy Technology Data Exchange (ETDEWEB)

    Siegers, Conrad

    2007-11-09

    ratio was varied between 1 and 9. The different donor acceptor sensitizers were then incorporated into dye solar cells. Additionally, cells were prepared by the coadsorption of [Ru(dcbpy)2(NCS)2] (N719), which is today's standard dye for DSC applications, and a carboxy-functionalized Fluorol. Hence DSCs resulted that were sensitized via (i) coadsorbed chromophores, (ii) the dyad, and (iii) above-mentioned polymers. The resulting devices were characterized via current-voltage, transmission and external quantum efficiency (EQE) measurements. The current-voltage measurements were carried out under simulated sunlight (AM1.5G) as well as under monochromatic blue and green illumination. This data allowed the calculation of the ratio of short circuit currents acquired under blue and green illumination, which indicates to what extent the current output of the solar cell may be enhanced by energy transfer. Furthermore, the energy transfer efficiency (ETE) was calculated from the DSC's spectral properties. All three concepts for the implementation of donor acceptor systems in the DSC revealed high ETEs (up to 90%). The introduction of an additional donor chromophore via coadsorption led to an increase of the monochromatic power conversion efficiency. The last-mentioned increase was more pronounced if covalently assembled donor acceptor sensitizers were used. The relative energy-transfer-mediated current gain was 21%, 24% and up to 179%, when coadsorbed chromophores, the dyad and donor acceptor polymers were used as sensitizers, respectively (in relation to the current generated by selective excitation of the acceptor component within the cell). These values confirm that energy transfer from fluorescent dyes being poor electron donors in themselves to good electroactive dyes (e.g. Ru-complexes) is also a viable process for light-to-electricity conversion in DSCs. Further optimization of the concepts investigated in this thesis (notably with respect to enhancing the light

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

    International Nuclear Information System (INIS)

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

    1997-01-01

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

  17. Study of excitation energy sharing in heavy ion collisions as a function of their inelasticity

    International Nuclear Information System (INIS)

    Lott, B.

    1986-01-01

    The excitation energy sharing between the fragments of a heavy ion collision has been studied for quasi-elastic and deep inelastic mechanisms. A 32 S beam of 232 MeV incident energy has been used to bombard several targets (S, 58 Ni, 93 Nb). The evaporated charged particle multiplicities have been measured by inclusive measurements of the projectile-like nuclei and exclusive measurements of the two final nuclei. Evaporation calculations using the Hauser-Feshbach formalism allows us to deduce from the multiplicity measurements the projectile-like excitation energy. These results are compatible with the assumption of an equal sharing of excitation energies for quasi-elastic reaction products, and with the assumption of a mass ratio sharing for fully relaxed reaction products. Limiting values for the relaxation time of this mode have been deduced and are in agreement with predictions from the model developed by Randrup [fr

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

    Science.gov (United States)

    Becke, Axel D.

    2018-01-01

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

  19. Differential cross sections for electron-impact vibrational-excitation of tetrahydrofuran at intermediate impact energies

    Energy Technology Data Exchange (ETDEWEB)

    Do, T. P. T. [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, South Australia 5001 (Australia); School of Education, Can Tho University, Campus II, 3/2 Street, Xuan Khanh, Ninh Kieu, Can Tho City (Viet Nam); Duque, H. V. [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, South Australia 5001 (Australia); Departamento de Física, Universidade Federal de Juiz de Fora, 36036-330 Juiz de Fora, Minas Gerais (Brazil); Lopes, M. C. A. [Departamento de Física, Universidade Federal de Juiz de Fora, 36036-330 Juiz de Fora, Minas Gerais (Brazil); Konovalov, D. A.; White, R. D. [College of Science, Technology and Engineering, James Cook University, Townsville (Australia); Brunger, M. J., E-mail: michael.brunger@flinders.edu.au, E-mail: darryl.jones@flinders.edu.au [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, South Australia 5001 (Australia); Institute of Mathematical Sciences, University of Malaya, 50603 Kuala Lumpur (Malaysia); Jones, D. B., E-mail: michael.brunger@flinders.edu.au, E-mail: darryl.jones@flinders.edu.au [School of Chemical and Physical Sciences, Flinders University, GPO Box 2100, Adelaide, South Australia 5001 (Australia)

    2015-03-28

    We report differential cross sections (DCSs) for electron-impact vibrational-excitation of tetrahydrofuran, at intermediate incident electron energies (15-50 eV) and over the 10°-90° scattered electron angular range. These measurements extend the available DCS data for vibrational excitation for this species, which have previously been obtained at lower incident electron energies (≤20 eV). Where possible, our data are compared to the earlier measurements in the overlapping energy ranges. Here, quite good agreement was generally observed where the measurements overlapped.

  20. Inner-shell excitation in heavy ion collisions up to intermediate incident energies

    International Nuclear Information System (INIS)

    Reus, T. de.

    1987-04-01

    Electronic excitations in collisions of very heavy ions with a total nuclear charge Z greater than 1/α ≅ 137 at bombarding energies reaching from 3.6 MeV/n up to 100 MeV/n are the subject of this thesis. The dynamical behaviour of the electron-positron-field is described within a semiclassical model, which is reviewed and extended to include electronic interactions via a mean field. A detailed comparison with experimental data of K-vacancy formation, δ-electron and positron emission shows an improved agreement compared with former calculations. Structures in spectra of positrons emitted in sub- and supercritical collision are discussed in two respects: Firstly as a signal of the vacuum decay in supercritical electromagnetic fields which evolve in the vicinity of long living giant nuclear molecules. Secondly as an atomic effect, which might be related to an instaneous formation of molecular 1sσ- and 2p 1/2 σ- levels. However, beyond this speculation the emission spectra of electrons and positrons in deep inelastic reactions have proven to be a powerful tool for measuring nuclear reaction or delay times in the order of 10 -21 s. This property was transfered to the domain of intermediate energy collisions. In first order perturbation theory we derived a scaling law, exhibiting how nuclear stopping times could be extracted from the emission spectra of high energetic δ-electrons. Quantitative calculations within a coupled channel code have been carried out for the system Pb+Pb, yielding cross sections of up to 20 nb for the emission of electrons with a kinetic energy of 50 MeV in 60 MeV/n-collisions. (orig./HSI)

  1. A schematic model for energy and charge transfer in the chlorophyll complex

    DEFF Research Database (Denmark)

    Bohr, Henrik; Malik, F.B.

    2011-01-01

    A theory for simultaneous charge and energy transfer in the carotenoid-chlorophyll-a complex is presented here and discussed. The observed charge transfer process in these chloroplast complexes is reasonably explained in terms of this theory. In addition, the process leads to a mechanism to drive...... an electron in a lower to a higher-energy state, thus providing a mechanism for the ejection of the electron to a nearby molecule (chlorophyll) or into the environment. The observed lifetimes of the electronically excited states are in accord/agreement with the investigations of Sundström et al....... and are in the range of pico-seconds and less. The change in electronic charge distribution in internuclear space as the system undergoes an electronic transition to a higher-energy state could, under appropriate physical conditions, lead to oscillating dipoles capable of transmitting energy from the carotenoid-chlorophylls...

  2. The EDDA experiment: proton-proton elastic scattering excitation functions at intermediate energies

    International Nuclear Information System (INIS)

    Hinterberher, F.

    1996-01-01

    The EDDA experiment is designed to provide a high precision measurement of proton-proton elastic scattering excitation functions ranging from 0.5 to 2.5 GeV of (lab) incident kinetic energy. It is an internal target experiment utilizing the proton beam of the cooler synchrotron COSY operated by KFA Juelich. The excitation functions are measured during the acceleration ramp of COSY. (author)

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

    CERN Multimedia

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

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

    Science.gov (United States)

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

    2017-12-01

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

  5. Energy technology transfer to developing countries

    International Nuclear Information System (INIS)

    Butera, F.; Farinelli, U.

    1992-01-01

    With the use of critical analyses of some examples of technology transfer by industrialized to third world countries, this paper illustrates the importance, in technology transfer, of giving due consideration to the specific social and marketing contexts of the targeted developing country and its physical and financial capability to acquire all the technology necessary to make the total realization of a desired industrial scheme feasible from the economic, technical and social points of view. It also indicates that the most effective transfers are those in which efforts are made to optimize local work force learning levels, process scheme efficiency and cost through the careful integration of innovative with conventional technologies

  6. Luminescence and energy transfer mechanisms in CaWO{sub 4} single crystals

    Energy Technology Data Exchange (ETDEWEB)

    Spassky, D., E-mail: deris2002@mail.ru [Skobeltsyn Institute of Nuclear Physics, M.V. Lomonosov Moscow State University, Vorob' evy Gory, 119991 Moscow (Russian Federation); Mikhailin, V. [Skobeltsyn Institute of Nuclear Physics, M.V. Lomonosov Moscow State University, Vorob' evy Gory, 119991 Moscow (Russian Federation); Nazarov, M. [School of Materials and Mineral Resources Engineering, Universiti Sains Malaysia, 14300 Nibong Tebal, Penang (Malaysia); Institute of Applied Physics, Academiei Street 5, Chisinau MD-2028 (Moldova, Republic of); Ahmad-Fauzi, M.N. [School of Materials and Mineral Resources Engineering, Universiti Sains Malaysia, 14300 Nibong Tebal, Penang (Malaysia); Zhbanov, A. [Department of Medical System Engineering, Gwangju Institute of Science and Technology, 1 Oryong-dong, Buk-gu, Gwangju 500-712 (Korea, Republic of)

    2012-10-15

    The processes of the excitation energy transfer to the emission centers have been investigated for calcium tungstate crystals taking into account features of the electronic structure of valence band and conduction band. The calculations of the electronic structure of host lattice CaWO{sub 4} were performed in the framework of density functional theory. The underestimation of the bandgap value in the calculations has been corrected according to the experimental data. Luminescence of two samples grown using Czochralski (cz) and hydrothermal (ht) techniques were studied. Intrinsic emission band related to excitons, self-trapped on WO{sub 4} complexes has been observed for the both samples while the additional low-energy emission band related to the defects of crystal structure has been observed only for (ht) sample indicating the enhanced concentration of the defects in the sample. It was shown that the features of the conduction band electronic structure are reproduced in the excitation spectrum of intrinsic luminescence only for the (ht) sample while for (cz) sample the correlation is absent. The enhanced role of the competitive channels in the process of excitation energy transfer to intrinsic emission centers in (ht) sample is responsible for the observed difference. - Highlights: Black-Right-Pointing-Pointer The band structure of CaWO{sub 4} was calculated in the framework of DFT LAPW method. Black-Right-Pointing-Pointer Calculation results were validated via joint analysis with experimental data. Black-Right-Pointing-Pointer The bandgap E{sub g} of CaWO{sub 4} was determined as 4.90{+-}0.15 eV. Black-Right-Pointing-Pointer The correlation between the band structure and excitation spectrum is demonstrated. Black-Right-Pointing-Pointer Influence of competitive relaxation channel on energy transfer to STE is shown.

  7. Excitation and dissociation of molecules by low-energy (0-15 eV) electrons

    International Nuclear Information System (INIS)

    Verhaart, G.J.

    1980-01-01

    The author deals with excitation and dissociation processes which result from the interaction between low-energy (0.15 eV) electrons and molecules. Low-energy electron-impact spectroscopy is used to gain a better knowledge of the electronic structure of halomethanes, ethylene and some of its halogen substituted derivatives, and some more complex organic molecules. (Auth.)

  8. Impact of undamped and damped intramolecular vibrations on the efficiency of photosynthetic exciton energy transfer

    Science.gov (United States)

    Juhász, Imre Benedek; Csurgay, Árpád I.

    2018-04-01

    In recent years, the role of molecular vibrations in exciton energy transfer taking place during the first stage of photosynthesis attracted increasing interest. Here, we present a model formulated as a Lindblad-type master equation that enables us to investigate the impact of undamped and especially damped intramolecular vibrational modes on the exciton energy transfer, particularly its efficiency. Our simulations confirm the already reported effects that the presence of an intramolecular vibrational mode can compensate the energy detuning of electronic states, thus promoting the energy transfer; and, moreover, that the damping of such a vibrational mode (in other words, vibrational relaxation) can further enhance the efficiency of the process by generating directionality in the energy flow. As a novel result, we show that this enhancement surpasses the one caused by pure dephasing, and we present its dependence on various system parameters (time constants of the environment-induced relaxation and excitation processes, detuning of the electronic energy levels, frequency of the intramolecular vibrational modes, Huang-Rhys factors, temperature) in dimer model systems. We demonstrate that vibrational-relaxation-enhanced exciton energy transfer (VREEET) is robust against the change of these characteristics of the system and occurs in wide ranges of the investigated parameters. With simulations performed on a heptamer model inspired by the Fenna-Matthews-Olson (FMO) complex, we show that this mechanism can be even more significant in larger systems at T = 300 K. Our results suggests that VREEET might be prevalent in light-harvesting complexes.

  9. Energy transfer mechanism between Ce and Tb ions in sol–gel synthesized YSO crystals

    International Nuclear Information System (INIS)

    Chiriu, Daniele; Stagi, Luigi; Carbonaro, Carlo Maria; Corpino, Riccardo; Ricci, Pier Carlo

    2016-01-01

    The luminescence properties of Tb and Ce in Rare Earth Doped crystalline oxides largely depend on their relative concentrations: by increasing the dopant concentration, the luminescence profile changes from blue to green because of the energy transfer among centers. The kinetic properties of the luminescence of optically excited Terbium–Cerium co-doped Y_2SiO_5 sol–gel synthesized crystal powders have been investigated as a function of the Tb dopant concentration (Ce content fixed at 1% atomic). The interaction among different Tb emitting centers and their relation with Ce centers was explained within the Inokuti-Hirayama model for a dipole–dipole energy transfer mechanism in the low-middle Tb concentration range whilst the Forster–Dexter model was applied in the middle-high Tb concentration range. The kinetic model allows elucidating the role of sensitizer and activator ion as a function of Tb concentration, successfully estimating the energy transfer mechanism efficiency and calculating the critical Tb concentration. - Highlights: • The kinetic properties of Ce, Tb recombination in YSO matrix were studied. • The Inokuti-Hirayama and Forster–Dexter models were applied. • At high Tb content, the Ce to Tb energy transfer acts through the dipole−quadrupole. • At low Tb content, the Ce to Tb energy transfer acts through the dipole−dipole. • The presence of Ce reduces the critical Tb concentration (at low Tb content).

  10. Energy transfer mechanism between Ce and Tb ions in sol–gel synthesized YSO crystals

    Energy Technology Data Exchange (ETDEWEB)

    Chiriu, Daniele; Stagi, Luigi; Carbonaro, Carlo Maria; Corpino, Riccardo; Ricci, Pier Carlo, E-mail: carlo.ricci@dsf.unica.it

    2016-03-01

    The luminescence properties of Tb and Ce in Rare Earth Doped crystalline oxides largely depend on their relative concentrations: by increasing the dopant concentration, the luminescence profile changes from blue to green because of the energy transfer among centers. The kinetic properties of the luminescence of optically excited Terbium–Cerium co-doped Y{sub 2}SiO{sub 5} sol–gel synthesized crystal powders have been investigated as a function of the Tb dopant concentration (Ce content fixed at 1% atomic). The interaction among different Tb emitting centers and their relation with Ce centers was explained within the Inokuti-Hirayama model for a dipole–dipole energy transfer mechanism in the low-middle Tb concentration range whilst the Forster–Dexter model was applied in the middle-high Tb concentration range. The kinetic model allows elucidating the role of sensitizer and activator ion as a function of Tb concentration, successfully estimating the energy transfer mechanism efficiency and calculating the critical Tb concentration. - Highlights: • The kinetic properties of Ce, Tb recombination in YSO matrix were studied. • The Inokuti-Hirayama and Forster–Dexter models were applied. • At high Tb content, the Ce to Tb energy transfer acts through the dipole−quadrupole. • At low Tb content, the Ce to Tb energy transfer acts through the dipole−dipole. • The presence of Ce reduces the critical Tb concentration (at low Tb content).

  11. Visual prosthesis wireless energy transfer system optimal modeling.

    Science.gov (United States)

    Li, Xueping; Yang, Yuan; Gao, Yong

    2014-01-16

    Wireless energy transfer system is an effective way to solve the visual prosthesis energy supply problems, theoretical modeling of the system is the prerequisite to do optimal energy transfer system design. On the basis of the ideal model of the wireless energy transfer system, according to visual prosthesis application condition, the system modeling is optimized. During the optimal modeling, taking planar spiral coils as the coupling devices between energy transmitter and receiver, the effect of the parasitic capacitance of the transfer coil is considered, and especially the concept of biological capacitance is proposed to consider the influence of biological tissue on the energy transfer efficiency, resulting in the optimal modeling's more accuracy for the actual application. The simulation data of the optimal model in this paper is compared with that of the previous ideal model, the results show that under high frequency condition, the parasitic capacitance of inductance and biological capacitance considered in the optimal model could have great impact on the wireless energy transfer system. The further comparison with the experimental data verifies the validity and accuracy of the optimal model proposed in this paper. The optimal model proposed in this paper has a higher theoretical guiding significance for the wireless energy transfer system's further research, and provide a more precise model reference for solving the power supply problem in visual prosthesis clinical application.

  12. Excitation functions for some evaporation residues identified in the interaction of 20Ne and 93Nb at moderate excitation energies

    International Nuclear Information System (INIS)

    Agarwal, Avinash; Rizvi, I.A.; Gupta, Meenal; Ahamad, Tauseef; Ghugre, S.S.; Sinha, A.K.; Chaubey, A.K.

    2008-01-01

    With the motivation of studying the complete and incomplete fusion reactions, excitation functions for the reactions 93 Nb(Ne, p2n) 110 Sn, 93 Nb(Ne, 2pn) 110 In, 93 Nb(Ne, 2p2n) 109 In, 93 Nb(Ne, αn) 108 In, 93 Nb(Neα2n) 107 In and 93 Nb(Ne, α p n) 107 Cd have been measured at the incident energy ranging from 91.4 MeV - 145 MeV. The well established activation technique followed by off line high purity gamma- ray spectroscopy was employed. The measured excitation functions were compared with the statistical model calculations by using the codes ALICE-91 and Pace-4. The effect of variation of different parameters including level density parameter involved in these codes has also been studied. Excellent agreement was found between theoretical and experimental values in some of the fusion evaporation reaction channels. However, significant enhancement of cross-section observed in α-emission channels may be due to incomplete fusion process. (author)

  13. Energy transfer in LH2 of Rhodospirillum Molischianum, studied by subpicosecond spectroscopy and configuration interaction exciton calculations.

    NARCIS (Netherlands)

    Ihalainen, J.A.; Linnanto, J.; Myllyperkio, P.; van Stokkum, I.H.M.; Ucker, B.; Scheer, H.; Korppi-Tommola, J.E.I.

    2001-01-01

    Two color transient absorption measurements were performed on a LH2 complex from Rhodospirillum molischianum by using several excitation wavelengths (790, 800, 810, and 830 nm) and probing in the spectral region from 790 to 870 nm at room temperature. The observed energy transfer time of ∼1.0 ps

  14. Continuum emission of excited sodium dimer

    International Nuclear Information System (INIS)

    Pardo, A.; Poyato, J.M.L.; Alonso, J.I.; Rico, F.R.

    1980-01-01

    A study has been made of the behaviour of excited molecular sodium using high-power Ar + laser radiation. A continuum emission was observed in the red wavelength region. This emission was thought to be caused by the formation of excited triatomic molecules. Energy transfer was observed from excited molecules to atoms. (orig.)

  15. Fusion-fission of superheavy nuclei at low excitation energies

    International Nuclear Information System (INIS)

    Itkis, M.G.; Oganesyan, Yu.Ts.; Kozulin, E.M.

    2000-01-01

    The process of fusion-fission of superheavy nuclei with Z = 102 -122 formed in the reactions with 22 Ne, 26 Mg, 48 Ca, 58 Fe and 86 Kr ions at energies near and below the Coulomb barrier has been studied. The experiments were carried out at the U-400 accelerator of the Flerov Laboratory of Nuclear Reactions (JINR) using a time-of-flight spectrometer of fission fragments CORSET and a neutron multi-detector DEMON. As a result of the experiments, mass and energy distributions of fission fragments, fission and quasi-fission cross sections, multiplicities of neutrons and gamma-rays and their dependence on the mechanism of formation and decay of compound superheavy systems have been studied

  16. Comparison of sensitivities and detection limits between direct excitation and secondary excitation modes in energy dispersive x-ray fluorescence analysis

    International Nuclear Information System (INIS)

    Artz, B.E.; Short, M.A.

    1976-01-01

    A comparison was made between the direct tube excitation mode and the secondary target excitation mode using a Kevex 0810 energy dispersive x-ray fluorescence system. Relative sensitivities and detection limits were determined with two system configurations. The first configuration used a standard, high power, x-ray fluorescence tube to directly excite the specimen. Several x-ray tubes, including chromium, molybdenum, and tungsten, both filtered and not filtered, were employed. The second configuration consisted of using the x-ray tube to excite a secondary target which in turn excited the specimen. Appropriate targets were compared to the direct excitation results. Relative sensitivities and detection limits were determined for K-series lines for elements from magnesium to barium contained in a low atomic number matrix and in a high atomic number matrix

  17. The Grover energy transfer algorithm for relativistic speeds

    Energy Technology Data Exchange (ETDEWEB)

    Garcia-Escartin, Juan Carlos; Chamorro-Posada, Pedro, E-mail: juagar@yllera.tel.uva.e [Dpto. de TeorIa de la Senal y Comunicaciones e Ingenieria Telematica, Universidad de Valladolid, ETSI de Telecomunicacion, Campus Miguel Delibes, Paseo Belen 15, 47011 Valladolid (Spain)

    2010-11-12

    Grover's algorithm for quantum search can also be applied to classical energy transfer. The procedure takes a system in which the total energy is equally distributed among N subsystems and transfers most of it to one marked subsystem. We show that in a relativistic setting the efficiency of this procedure can be improved. We will consider the transfer of relativistic kinetic energy in a series of elastic collisions. In this case, the number of steps of the energy transfer procedure approaches 1 as the initial velocities of the objects become closer to the speed of light. This is a consequence of introducing nonlinearities in the procedure. However, the maximum attainable transfer will depend on the particular combination of speed and number of objects. In the procedure, we will use N elements, as in the classical non-relativistic case, instead of the log{sub 2}(N) states of the quantum algorithm.

  18. The Grover energy transfer algorithm for relativistic speeds

    International Nuclear Information System (INIS)

    Garcia-Escartin, Juan Carlos; Chamorro-Posada, Pedro

    2010-01-01

    Grover's algorithm for quantum search can also be applied to classical energy transfer. The procedure takes a system in which the total energy is equally distributed among N subsystems and transfers most of it to one marked subsystem. We show that in a relativistic setting the efficiency of this procedure can be improved. We will consider the transfer of relativistic kinetic energy in a series of elastic collisions. In this case, the number of steps of the energy transfer procedure approaches 1 as the initial velocities of the objects become closer to the speed of light. This is a consequence of introducing nonlinearities in the procedure. However, the maximum attainable transfer will depend on the particular combination of speed and number of objects. In the procedure, we will use N elements, as in the classical non-relativistic case, instead of the log 2 (N) states of the quantum algorithm.

  19. Near-field effects and energy transfer in hybrid metal-oxide nanostructures.

    Science.gov (United States)

    Herr, Ulrich; Kuerbanjiang, Balati; Benel, Cahit; Papageorgiou, Giorgos; Goncalves, Manuel; Boneberg, Johannes; Leiderer, Paul; Ziemann, Paul; Marek, Peter; Hahn, Horst

    2013-01-01

    One of the big challenges of the 21st century is the utilization of nanotechnology for energy technology. Nanoscale structures may provide novel functionality, which has been demonstrated most convincingly by successful applications such as dye-sensitized solar cells introduced by M. Grätzel. Applications in energy technology are based on the transfer and conversion of energy. Following the example of photosynthesis, this requires a combination of light harvesting, transfer of energy to a reaction center, and conversion to other forms of energy by charge separation and transfer. This may be achieved by utilizing hybrid nanostructures, which combine metallic and nonmetallic components. Metallic nanostructures can interact strongly with light. Plasmonic excitations of such structures can cause local enhancement of the electrical field, which has been utilized in spectroscopy for many years. On the other hand, the excited states in metallic structures decay over very short lifetimes. Longer lifetimes of excited states occur in nonmetallic nanostructures, which makes them attractive for further energy transfer before recombination or relaxation sets in. Therefore, the combination of metallic nanostructures with nonmetallic materials is of great interest. We report investigations of hybrid nanostructured model systems that consist of a combination of metallic nanoantennas (fabricated by nanosphere lithography, NSL) and oxide nanoparticles. The oxide particles were doped with rare-earth (RE) ions, which show a large shift between absorption and emission wavelengths, allowing us to investigate the energy-transfer processes in detail. The main focus is on TiO2 nanoparticles doped with Eu(3+), since the material is interesting for applications such as the generation of hydrogen by photocatalytic splitting of water molecules. We use high-resolution techniques such as confocal fluorescence microscopy for the investigation of energy-transfer processes. The experiments are

  20. Pair transfer processes probed at deep sub barrier energies

    International Nuclear Information System (INIS)

    Corradi, L.; Mason, P.; Fioretto, E.; Michelagnoli, C.; Stefanini, A.M.; Valiente-Dobon, J.J.; Szinler, S.; Jelavic-Malenica, D.; Soic, N.; Pollarolo, G.; Farnea, E.; Montagnoli, G.; Montanari, D.; Scarlassara, F.; Ur, C.A.; Gadea, A.; Haas, F.; Marginean, N.

    2011-01-01

    Multinucleon transfer cross sections in the system 40 Ca+ 96 Zr have been measured at bombarding energies ranging from the Coulomb barrier to ∼ 25% below. Target-like (lighter) recoils in inverse kinematics have been completely identified in A,Z and Q-value with the large solid angle magnetic spectrometer PRISMA. The experimental slopes of the neutron transfer probabilities at large internuclear separation are consistent with the values derived from the binding energies. A phenomenological interpretation of the transfer probabilities indicates the presence of enhanced values for the even number of neutron transfers. (authors)

  1. Modeling of charge-transfer transitions and excited states in d6 transition metal complexes by DFT techniques

    Czech Academy of Sciences Publication Activity Database

    Vlček, Antonín; Záliš, Stanislav

    2007-01-01

    Roč. 251, 3-4 (2007), s. 258-287 ISSN 0010-8545 R&D Projects: GA MŠk 1P05OC068; GA MŠk OC 139 Institutional research plan: CEZ:AV0Z40400503 Keywords : charge-transfer transition * DFT technique * excited states * spectroscopy Subject RIV: CG - Electrochemistry Impact factor: 8.568, year: 2007

  2. Calculations of the excitation energies of all-trans and 11,12s-dicis retinals using localized molecular orbitals obtained by the elongation method

    Science.gov (United States)

    Kurihara, Youji; Aoki, Yuriko; Imamura, Akira

    1997-09-01

    In the present article, the excitation energies of the all-trans and the 11,12s-dicis retinals were calculated by using the elongation method. The geometries of these molecules were optimized with the 4-31G basis set by using the GAUSSIAN 92 program. The wave functions for the calculation of the excitation energies were obtained with CNDO/S approximation by the elongation method, which enables us to analyze electronic structures of aperiodic polymers in terms of the exciton-type local excitation and the charge transfer-type excitation. The excitation energies were calculated by using the single excitation configuration interaction (SECI) on the basis of localized molecular orbitals (LMOs). The LMOs were obtained in the process of the elongation method. The configuration interaction (CI) matrices were diagonalized by Davidson's method. The calculated results were in good agreement with the experimental data for absorption spectra. In order to consider the isomerization path from 11,12s-dicis to all-trans retinals, the barriers to the rotations about C11-C12 double and C12-C13 single bonds were evaluated.

  3. Nonlinear dynamic analysis of cantilevered piezoelectric energy harvesters under simultaneous parametric and external excitations

    Science.gov (United States)

    Fang, Fei; Xia, Guanghui; Wang, Jianguo

    2018-02-01

    The nonlinear dynamics of cantilevered piezoelectric beams is investigated under simultaneous parametric and external excitations. The beam is composed of a substrate and two piezoelectric layers and assumed as an Euler-Bernoulli model with inextensible deformation. A nonlinear distributed parameter model of cantilevered piezoelectric energy harvesters is proposed using the generalized Hamilton's principle. The proposed model includes geometric and inertia nonlinearity, but neglects the material nonlinearity. Using the Galerkin decomposition method and harmonic balance method, analytical expressions of the frequency-response curves are presented when the first bending mode of the beam plays a dominant role. Using these expressions, we investigate the effects of the damping, load resistance, electromechanical coupling, and excitation amplitude on the frequency-response curves. We also study the difference between the nonlinear lumped-parameter and distributed-parameter model for predicting the performance of the energy harvesting system. Only in the case of parametric excitation, we demonstrate that the energy harvesting system has an initiation excitation threshold below which no energy can be harvested. We also illustrate that the damping and load resistance affect the initiation excitation threshold.

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

    Science.gov (United States)

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

    2018-03-01

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

  5. Carotenoid-to-bacteriochlorophyll energy transfer through vibronic coupling in LH2 from Phaeosprillum molischianum.

    Science.gov (United States)

    Thyrhaug, Erling; Lincoln, Craig N; Branchi, Federico; Cerullo, Giulio; Perlík, Václav; Šanda, František; Lokstein, Heiko; Hauer, Jürgen

    2018-03-01

    The peripheral light-harvesting antenna complex (LH2) of purple photosynthetic bacteria is an ideal testing ground for models of structure-function relationships due to its well-determined molecular structure and ultrafast energy deactivation. It has been the target for numerous studies in both theory and ultrafast spectroscopy; nevertheless, certain aspects of the convoluted relaxation network of LH2 lack a satisfactory explanation by conventional theories. For example, the initial carotenoid-to-bacteriochlorophyll energy transfer step necessary on visible light excitation was long considered to follow the Förster mechanism, even though transfer times as short as 40 femtoseconds (fs) have been observed. Such transfer times are hard to accommodate by Förster theory, as the moderate coupling strengths found in LH2 suggest much slower transfer within this framework. In this study, we investigate LH2 from Phaeospirillum (Ph.) molischianum in two types of transient absorption experiments-with narrowband pump and white-light probe resulting in 100 fs time resolution, and with degenerate broadband 10 fs pump and probe pulses. With regard to the split Q x band in this system, we show that vibronically mediated transfer explains both the ultrafast carotenoid-to-B850 transfer, and the almost complete lack of transfer to B800. These results are beyond Förster theory, which predicts an almost equal partition between the two channels.

  6. Energy principle for excitations in plasmas with counterstreaming electron flows

    Science.gov (United States)

    Kumar, Atul; Shukla, Chandrasekhar; Das, Amita; Kaw, Predhiman

    2018-05-01

    A relativistic electron beam propagating through plasma induces a return electron current in the system. Such a system of interpenetrating forward and return electron current is susceptible to a host of instabilities. The physics of such instabilities underlies the conversion of the flow kinetic energy to the electromagnetic field energy. Keeping this in view, an energy principle analysis has been enunciated in this paper. Such analyses have been widely utilized earlier in the context of conducting fluids described by MHD model [I. B. Bernstein et al., Proceedings of the Royal Society of London A: Mathematical, Physical and Engineering Sciences 244(1236), 17-40 (1958)]. Lately, such an approach has been employed for the electrostatic two stream instability for the electron beam plasma system [C. N. Lashmore-Davies, Physics of Plasmas 14(9), 092101 (2007)]. In contrast, it has been shown here that even purely growing mode like Weibel/current filamentation instability for the electron beam plasma system is amenable to such a treatment. The treatment provides an understanding of the energetics associated with the growing mode. The growth rate expression has also been obtained from it. Furthermore, it has been conclusively demonstrated in this paper that for identical values of S4=∑αn0 αv0α 2/n0γ0 α, the growth rate is higher when the counterstreaming beams are symmetric (i.e. S3 = ∑αn0αv 0α/n0γ0α = 0) compared to the case when the two beams are asymmetric (i.e. when S3 is finite). Here, v 0α, n0α and γ0α are the equilibrium velocity, electron density and the relativistic factor for the electron species `α' respectively and n0 = ∑αn0α is the total electron density. Particle - In - Cell simulations have been employed to show that the saturated amplitude of the field energy is also higher in the symmetric case.

  7. Relativistic Energy Density Functionals: Exotic modes of excitation

    International Nuclear Information System (INIS)

    Vretenar, D.; Paar, N.; Marketin, T.

    2008-01-01

    The framework of relativistic energy density functionals has been applied to the description of a variety of nuclear structure phenomena, not only in spherical and deformed nuclei along the valley of β-stability, but also in exotic systems with extreme isospin values and close to the particle drip-lines. Dynamical aspects of exotic nuclear structure have been investigated with the relativistic quasiparticle random-phase approximation. We present results for the evolution of low-lying dipole (pygmy) strength in neutron-rich nuclei, and charged-current neutrino-nucleus cross sections.

  8. Energy transfers and magnetic energy growth in small-scale dynamo

    KAUST Repository

    Kumar, Rohit Raj; Verma, Mahendra K.; Samtaney, Ravi

    2013-01-01

    In this letter we investigate the dynamics of magnetic energy growth in small-scale dynamo by studying energy transfers, mainly energy fluxes and shell-to-shell energy transfers. We perform dynamo simulations for the magnetic Prandtl number Pm = 20

  9. A planning framework for transferring building energy technologies

    Energy Technology Data Exchange (ETDEWEB)

    Farhar, B C; Brown, M A; Mohler, B L; Wilde, M; Abel, F H

    1990-07-01

    Accelerating the adoption of new and existing cost-effective technologies has significant potential to reduce the energy consumed in US buildings. This report presents key results of an interlaboratory technology transfer planning effort in support of the US Department of Energy's Office of Building Technologies (OBT). A guiding assumption for planning was that OBT's R D program should forge linkages with existing programs whose goals involved enhancing energy efficiency in buildings. An ad hoc Technology Transfer Advisory Group reviewed the existing analysis and technology transfer program, brainstormed technology transfer approaches, interviewed DOE program managers, identified applicable research results, and developed a framework that management could use in deciding on the best investments of technology transfer resources. Representatives of 22 organizations were interviewed on their views of the potential for transferring energy efficiency technologies through active linking with OBT. The report describes these programs and interview results; outlines OBT tools, technologies, and practices to be transferred; defines OBT audiences; identifies technology transfer functions and presents a framework devised using functions and audiences; presents some 60 example technology transfer activities; and documents the Advisory Group's recommendations. 37 refs., 3 figs., 12 tabs.

  10. The form of electron-atom excitation amplitudes at high momentum transfers in the Faddeev-Watson approximation

    International Nuclear Information System (INIS)

    Catalan, G.; Roberts, M.J.

    1979-01-01

    A form of the off-shell Coulomb T matrix, which has a well defined on-shell limit, is used in the Faddeev-Watson multiple-scattering expansion for a direct three-body collision process. Using the excitation of atomic hydrogen by electron impact as an example, approximations to the second-order terms, which are valid for high momentum transfers of the incident electron, are derived. It is shown how the resulting asymptotic behaviour of the second-order Faddeev-Watson approximation is related to the high momentum transfer limit of the second Born approximation. The results are generalised to the excitation of more complex atoms. The asymptotic forms of the Faddeev-Watson and Born approximations are compared with other theories and with measurements of differential cross sections and angular correlation parameters for the excitation of H(2p) and He(2 1 P). The results indicate that the Faddeev-Watson approximation converges more rapidly at high momentum transfers than does the Born approximation. (author)

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

    International Nuclear Information System (INIS)

    Erturk, A; Inman, D J

    2009-01-01

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

  12. Vibronic coupling explains the ultrafast carotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

    Energy Technology Data Exchange (ETDEWEB)

    Perlík, Václav; Seibt, Joachim; Šanda, František; Mančal, Tomáš [Institute of Physics, Faculty of Mathematics and Physics, Charles University in Prague, Ke Karlovu 5, Prague 121 16 (Czech Republic); Cranston, Laura J.; Cogdell, Richard J. [Institute of Molecular Cell and System Biology, College of Medical, Veterinary and Life Sciences, University of Glasgow, Glasgow Biomedical Research Centre, 120 University Place, Glasgow G12 8TA, Scotland (United Kingdom); Lincoln, Craig N.; Hauer, Jürgen, E-mail: juergen.hauer@tuwien.ac.at [Photonics Institute, Vienna University of Technology, Gusshausstrasse 27, 1040 Vienna (Austria); Savolainen, Janne [Department of Physical Chemistry II, Ruhr-University Bochum, 44780 Bochum (Germany)

    2015-06-07

    The initial energy transfer steps in photosynthesis occur on ultrafast timescales. We analyze the carotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatium purpuratum as well as in an artificial light-harvesting dyad system by using transient grating and two-dimensional electronic spectroscopy with 10 fs time resolution. We find that Förster-type models reproduce the experimentally observed 60 fs transfer times, but overestimate coupling constants, which lead to a disagreement with both linear absorption and electronic 2D-spectra. We show that a vibronic model, which treats carotenoid vibrations on both electronic ground and excited states as part of the system’s Hamiltonian, reproduces all measured quantities. Importantly, the vibronic model presented here can explain the fast energy transfer rates with only moderate coupling constants, which are in agreement with structure based calculations. Counterintuitively, the vibrational levels on the carotenoid electronic ground state play the central role in the excited state population transfer to bacteriochlorophyll; resonance between the donor-acceptor energy gap and the vibrational ground state energies is the physical basis of the ultrafast energy transfer rates in these systems.

  13. Vibronic coupling explains the ultrafast carotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

    International Nuclear Information System (INIS)

    Perlík, Václav; Seibt, Joachim; Šanda, František; Mančal, Tomáš; Cranston, Laura J.; Cogdell, Richard J.; Lincoln, Craig N.; Hauer, Jürgen; Savolainen, Janne

    2015-01-01

    The initial energy transfer steps in photosynthesis occur on ultrafast timescales. We analyze the carotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatium purpuratum as well as in an artificial light-harvesting dyad system by using transient grating and two-dimensional electronic spectroscopy with 10 fs time resolution. We find that Förster-type models reproduce the experimentally observed 60 fs transfer times, but overestimate coupling constants, which lead to a disagreement with both linear absorption and electronic 2D-spectra. We show that a vibronic model, which treats carotenoid vibrations on both electronic ground and excited states as part of the system’s Hamiltonian, reproduces all measured quantities. Importantly, the vibronic model presented here can explain the fast energy transfer rates with only moderate coupling constants, which are in agreement with structure based calculations. Counterintuitively, the vibrational levels on the carotenoid electronic ground state play the central role in the excited state population transfer to bacteriochlorophyll; resonance between the donor-acceptor energy gap and the vibrational ground state energies is the physical basis of the ultrafast energy transfer rates in these systems

  14. Intramolecular singlet-singlet energy transfer in antenna-substituted azoalkanes.

    Science.gov (United States)

    Pischel, Uwe; Huang, Fang; Nau, Werner M

    2004-03-01

    Two novel azoalkane bichromophores and related model compounds have been synthesised and photophysically characterised. Dimethylphenylsiloxy (DPSO) or dimethylnaphthylsiloxy (DNSO) serve as aromatic donor groups (antenna) and the azoalkane 2,3-diazabicyclo[2.2.2]oct-2-ene (DBO) as the acceptor. The UV spectral window of DBO (250-300 nm) allows selective excitation of the donor. Intramolecular singlet-singlet energy transfer to DBO is highly efficient and proceeds with quantum yields of 0.76 with DPSO and 0.99 with DNSO. The photophysical and spectral properties of the bichromophoric systems suggest that energy transfer occurs through diffusional approach of the donor and acceptor within a van der Waals contact at which the exchange mechanism is presumed to dominate. Furthermore, akin to the behaviour of electron-transfer systems in the Marcus inverted region, a rate of energy transfer 2.5 times slower was observed for the system with the more favourable energetics, i.e. singlet-singlet energy transfer from DPSO proceeded slower than from DNSO, although the process is more exergonic for DPSO (-142 kJ mol(-1) for DPSO versus-67 kJ mol(-1) for DNSO).

  15. Energy transfers in dynamos with small magnetic Prandtl numbers

    KAUST Repository

    Kumar, Rohit; Verma, Mahendra K.; Samtaney, Ravi

    2015-01-01

    We perform numerical simulation of dynamo with magnetic Prandtl number Pm = 0.2 on 10243 grid, and compute the energy fluxes and the shell-to-shell energy transfers. These computations indicate that the magnetic energy growth takes place mainly due

  16. Energy transfer dynamics in an RC-LH1-PufX tubular photosynthetic membrane

    Energy Technology Data Exchange (ETDEWEB)

    Hsin, J; Sener, M; Schulten, K [Department of Physics and Beckman Institute, University of Illinois at Urbana-Champaign, Urbana (United States); Struempfer, J [Center for Biophysics and Computational Biology and Beckman Institute, University of Illinois at Urbana-Champaign, Urbana (United States); Qian, P; Hunter, C N, E-mail: kschulte@ks.uiuc.ed [Department of Molecular Biology and Biotechnology, University of Sheffield, Sheffield S10 2TN (United Kingdom)

    2010-08-15

    Light absorption and the subsequent transfer of excitation energy are the first two steps in the photosynthetic process, carried out by protein-bound pigments, mainly bacteriochlorophylls (BChls), in photosynthetic bacteria. BChls are anchored in light-harvesting (LH) complexes, such as light-harvesting complex I (LH1), which directly associates with the reaction center (RC), forming the RC-LH1 core complex. In Rhodobacter sphaeroides, RC-LH1 core complexes contain an additional protein, PufX, and assemble into dimeric RC-LH1-PufX core complexes. In the absence of LH complex II (LH2), the former complexes can aggregate into a helically ordered tubular photosynthetic membrane. We have examined the excitation transfer dynamics in a single RC-LH1-PufX core complex dimer using the hierarchical equations of motion for dissipative quantum dynamics that accurately, yet in a computationally costly manner, treat the coupling between BChls and their protein environment. A widely employed description, the generalized Foerster (GF) theory, was also used to calculate the transfer rates of the same excitonic system in order to verify the accuracy of this computationally cheap method. Additionally, in light of the structural uncertainties in the Rba. sphaeroides RC-LH1-PufX core complex, geometrical alterations were introduced into the BChl organization. It is shown that the energy transfer dynamics are not affected by the considered changes in the BChl organization and that the GF theory provides accurate transfer rates. An all-atom model for a tubular photosynthetic membrane is then constructed on the basis of electron microscopy data, and the overall energy transfer properties of this membrane are computed.

  17. Energy transfer dynamics in an RC-LH1-PufX tubular photosynthetic membrane

    International Nuclear Information System (INIS)

    Hsin, J; Sener, M; Schulten, K; Struempfer, J; Qian, P; Hunter, C N

    2010-01-01

    Light absorption and the subsequent transfer of excitation energy are the first two steps in the photosynthetic process, carried out by protein-bound pigments, mainly bacteriochlorophylls (BChls), in photosynthetic bacteria. BChls are anchored in light-harvesting (LH) complexes, such as light-harvesting complex I (LH1), which directly associates with the reaction center (RC), forming the RC-LH1 core complex. In Rhodobacter sphaeroides, RC-LH1 core complexes contain an additional protein, PufX, and assemble into dimeric RC-LH1-PufX core complexes. In the absence of LH complex II (LH2), the former complexes can aggregate into a helically ordered tubular photosynthetic membrane. We have examined the excitation transfer dynamics in a single RC-LH1-PufX core complex dimer using the hierarchical equations of motion for dissipative quantum dynamics that accurately, yet in a computationally costly manner, treat the coupling between BChls and their protein environment. A widely employed description, the generalized Foerster (GF) theory, was also used to calculate the transfer rates of the same excitonic system in order to verify the accuracy of this computationally cheap method. Additionally, in light of the structural uncertainties in the Rba. sphaeroides RC-LH1-PufX core complex, geometrical alterations were introduced into the BChl organization. It is shown that the energy transfer dynamics are not affected by the considered changes in the BChl organization and that the GF theory provides accurate transfer rates. An all-atom model for a tubular photosynthetic membrane is then constructed on the basis of electron microscopy data, and the overall energy transfer properties of this membrane are computed.

  18. Analyzing powers of inelastic dp-scattering in the energy region of delta and roper resonances excitation

    International Nuclear Information System (INIS)

    Malinina, L.V.; Alkhazov, G.D.; Augustyniak, W.

    2001-01-01

    A study of inelastic scattering of polarized 3.73 GeV/c deuterons on protons in the energy region of the Roper N* (1440) and the Δ(1232) resonances excitation has been performed in an exclusive experiment at LNS (Laboratoire National SATURNE, Saclay, France) using the SPES4-π setup. Tensor and vector analyzing powers of pion production for the reactions d+p→d+n+π + , d+p→d+p+π 0 , d+p→d+N+ππ have been measured as functions of the squared deuteron 4-momentum transfer t, of the effective mass of the subsystems (Nπ), (Nππ) and of the pion emission angle. A strong dependence of these analyzing powers upon the pion emission angle is observed. It is found that A yy values for the considered reaction channels are systematically larger than the known inclusive p(d,d')X world data at the nearest beam energy

  19. Analyzing Powers of Inelastic dp-Scattering in the Energy Region of Delta and Roper Resonances Excitation

    CERN Document Server

    Malinina, L V; Augustyniak, W; Boivin, M; Boyard, J L; Dahl, R; Drews, M; Ellegaard, C; Fahri, L; Gaarde, C; Hennino, T; Jourdain, J C; Kagarlis, M A; Kravtsov, A V; Künne, R A; Larsen, J C; Morsch, P; Mylnikov, V A; Orichtchin, E M; Perdrisat, C F; Piskunov, N M; Prokofiev, A N; Punjabi, V; Radvanyi, P; Ramstein, B; Razmyslovich, B V; Roy-Stephan, M; Sitnik, I M; Skousen, M; Strokovsky, E A; Tkach, I I; Tomasi-Gustafsson, E; Volkov, S S; Zhdanov, A A; Zupranski, P

    2001-01-01

    A study of inelastic scattering of polarized 3.73 GeV/c deuterons on protons in the energy region of the Roper N*(1440) and the {DELTA}(1232) resonances excitation has been performed in an exclusive experiment at LNS (Laboratoire National SATURNE, Saclay, France) using the SPES-{pi} setup.Tensor and vector analyzing powers of pion production for the reactions d + p {\\to} d + n + pi^{+}, d + p {\\to} d + p + pi^{0}, d + p {\\to} d + N + pi pi have been measured as functions of the squared deuteron 4-momentum transfer t, of the effective mass of the subsystems (N pi), (N pi pi) and of the pion emission angle. A strong dependence of these analyzing powers upon the pion emission angle is observed. It is found that A_{yy} values for the considered reaction channels are systematically larger than the known inclusive {p (d, d {\\prime}) X} world data at the nearest beam energy.

  20. High spin spectroscopy near the N=Z line: Channel selection and excitation energy systematics

    Energy Technology Data Exchange (ETDEWEB)

    Svensson, C.E.; Cameron, J.A.; Flibotte, S. [McMaster Univ., Ontario (Canada)] [and others

    1996-12-31

    The total {gamma}-ray and charged-particle energies emitted in fusion-evaporation reactions leading to N=Z compound systems in the A = 50-70 mass region have been measured with the 8{pi} {gamma}-ray spectrometer and the miniball charged-particle detector array. A new method of channel selection has been developed which combines particle identification with these total energy measurements and greatly improves upon the selectivity possible with particle detection alone. In addition, the event by event measurement of total {gamma}-ray energies using the BGO ball of the 8{pi} spectrometer has allowed a determination of excitation energies following particle evaporation for a large number of channels in several different reactions. The new channel selection procedure and excitation energy systematics are illustrated with data from the reaction of {sup 24}Mg on {sup 40}Ca at E{sub lab} = 80MeV.