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Sample records for excitation spectra spin

  1. Symmetry of spin excitation spectra in 122-ferropnictides

    NASA Astrophysics Data System (ADS)

    Inosov, Dmytro

    2011-03-01

    We have studied the symmetry of spin excitation spectra in 122-ferropnictide superconductors by comparing the results of first-principles calculations with inelastic neutron scattering (INS) measurements on Ni- and Co-doped BaFe 2 As 2 samples close to the optimal doping level, which exhibit neither static magnetic phases nor structural phase transitions. In both the normal and superconducting (SC) states, the spectrum does not follow the I 4 / mmm space group of the crystal, but instead inherits its symmetry from the unfolded Brillouin zone of the Fe- sublattice. This is manifest both in the in-plane anisotropy of the normal- and SC-state spin dynamics and in the out-of-plane dispersion of the spin-resonance mode and the SC spin gap. The in-plane anisotropy is temperature-independent and can be qualitatively reproduced in normal-state density-functional theory calculations without invoking a symmetry-broken (``nematic'') ground state that was previously proposed as an explanation for this effect. Below the SC transition, the energy of the magnetic resonant mode, as well as its intensity and the SC spin gap, inherit the normal-state intensity modulation along the out-of-plane direction. Apparently, it can be traced back to the three-dimensional band structure and the superconducting gap, both of which were reported to disperse along the out-of- plane direction. This work has been supported, in part, by the DFG within the Schwerpunktprogramm 1458, under Grant No. BO3537/1-1.

  2. Excitation spectra and spin gap of the half-filled Holstein-Hubbard model

    NASA Astrophysics Data System (ADS)

    Hohenadler, Martin; Assaad, Fakher F.

    2013-02-01

    Single- and two-particle excitation spectra of the one-dimensional, half-filled Holstein-Hubbard model are calculated using the continuous-time quantum Monte Carlo method. In the metallic phase, the results are consistent with a Luther-Emery liquid that has gapped spin and single-particle excitations but a gapless charge mode. However, given the initially exponential dependence of the spin gap on the backscattering matrix element, the numerical excitation spectra appear gapless in the weak-coupling regime, and therefore resemble those of a Luttinger liquid. The Mott phase has the expected charge gap and gapless spin excitations. The Peierls state shows a charge, spin, and single-particle gap, a soft phonon mode, backfolded shadow bands, and soliton excitations. Arguments and numerical evidence for the existence of a nonzero spin gap throughout the metallic phase are provided in terms of equal-time spin and charge correlation functions.

  3. Symmetry of spin excitation spectra in the tetragonal paramagnetic and superconducting phases of 122-ferropnictides

    NASA Astrophysics Data System (ADS)

    Park, J. T.; Inosov, D. S.; Yaresko, A.; Graser, S.; Sun, D. L.; Bourges, Ph.; Sidis, Y.; Li, Yuan; Kim, J.-H.; Haug, D.; Ivanov, A.; Hradil, K.; Schneidewind, A.; Link, P.; Faulhaber, E.; Glavatskyy, I.; Lin, C. T.; Keimer, B.; Hinkov, V.

    2010-10-01

    We study the symmetry of spin excitation spectra in 122-ferropnictide superconductors by comparing the results of first-principles calculations with inelastic neutron-scattering (INS) measurements on BaFe1.85Co0.15As2 and BaFe1.91Ni0.09As2 samples that exhibit neither static magnetic phases nor structural phase transitions. In both the normal and superconducting (SC) states, the spectrum lacks the three-dimensional 42/m screw symmetry around the ((1)/(2)(1)/(2)L) axis that is implied by the I4/mmm space group. This is manifest both in the in-plane anisotropy of the normal- and SC-state spin dynamics and in the out-of-plane dispersion of the spin-resonance mode. We show that this effect originates from the higher symmetry of the magnetic Fe sublattice with respect to the crystal itself, hence the INS signal inherits the symmetry of the unfolded Brillouin zone (BZ) of the Fe sublattice. The in-plane anisotropy is temperature independent and can be qualitatively reproduced in normal-state density-functional-theory calculations without invoking a symmetry-broken (“nematic”) ground state that was previously proposed as an explanation for this effect. Below the SC transition, the energy of the magnetic resonant mode ωres , as well as its intensity and the SC spin gap inherit the normal-state intensity modulation along the out-of-plane direction L with a period twice larger than expected from the body-centered-tetragonal BZ symmetry. The amplitude of this modulation decreases at higher doping, providing an analogy to the splitting between even and odd resonant modes in bilayer cuprates. Combining our and previous data, we show that at odd L a universal linear relationship ℏωres≈4.3kBTc holds for all the studied Fe-based superconductors, independent of their carrier type. Its validity down to the lowest doping levels is consistent with weaker electron correlations in ferropnictides as compared to the underdoped cuprates.

  4. Excitation spectra of a Bose-Einstein condensate with an angular spin-orbit coupling

    NASA Astrophysics Data System (ADS)

    Vasić, Ivana; Balaž, Antun

    2016-09-01

    A theoretical model of a Bose-Einstein condensate with angular spin-orbit coupling has recently been proposed and it has been established that a half-skyrmion represents the ground state in a certain regime of spin-orbit coupling and interaction. Here we investigate low-lying excitations of this phase by using the Bogoliubov method and numerical simulations of the time-dependent Gross-Pitaevskii equation. We find that a sudden shift of the trap bottom results in a complex two-dimensional motion of the system's center of mass that is markedly different from the response of a competing phase, and comprises two dominant frequencies. Moreover, the breathing mode frequency of the half-skyrmion is set by both the spin-orbit coupling and the interaction strength, while in the competing state it takes a universal value. Effects of interactions are especially pronounced at the transition between the two phases.

  5. Effect of frustration on spin-wave excitation spectra and ground-state properties of the quasi-one-dimensional antiferromagnetic chain with asymmetrical sublattices

    NASA Astrophysics Data System (ADS)

    Jiang, Jian-Jun; Liu, Yong-Jun; Zhang, Song-Jun; Yang, Cui-Hong

    2009-10-01

    We investigate the effect of frustration on spin-wave excitation spectra and the properties of the quasi-one-dimensional Heisenberg chain using a spin-wave-wave analysis, the exact diagonalization method and the density matrix renormalization group method. The results show that frustration can cause the softening of the acoustic excitation spectrum ω3, as well as the hardening of the optical excitation spectrum ω1. As a function of the frustration parameter α, the phase diagram exhibits a ferromagnetic phase, a narrow canted phase and a singlet phase. The results obtained from numerical methods show that the spin gap obviously opens and the tetramer-dimer state dominates the properties of the ground state in the singlet phase.

  6. Angular dependent study on ferromagnetic resonance and spin excitations by spin rectification

    SciTech Connect

    Zhang, Yichao; Fan, Xiaolong Zhao, Xiaobing; Rao, Jinwei; Zhou, Hengan; Guo, Dangwei; Xue, Desheng; Gui, Y. S.; Hu, C.-M.

    2015-01-14

    We report angular dependent spin rectification spectra which are applied to studying spin excitations in single permalloy stripe. Based on planar Hall effect, those spin excitations generate special resonant dc Hall voltages, which have been characterized as functions of the amplitude and direction of applied magnetic field. Through high angular resolution 2D mappings, the evolutions of different spin excitation can be directly presented, and the dynamic magnetic parameters such as the gyromagnetic ratio, effective exchange field, as well as the quantized numbers of standing spin waves can be accurately determined through fitting the angular evolution of each resonance.

  7. Spin excitations of weakly coupled magnetic atoms

    NASA Astrophysics Data System (ADS)

    Goldberg, E. C.; Flores, F.

    2015-04-01

    A theoretical description of the measured differential conductance through magnetic atoms on a C u2N /Cu ( 100 ) substrate is presented [Otte et al., Phys. Rev. Lett. 103, 107203 (2009), 10.1103/PhysRevLett.103.107203]. In particular, we analyze the case of a weakly coupled Co/ Fe dimer. The starting point of our model is an ionic Hamiltonian which describes the inelastic electron tunneling excitations and the Kondo resonances as due to atomic spin fluctuations associated with electron cotunneling processes in the tip-atom-surface system. The interaction terms of this Hamiltonian are written in the basis set of the eigenstates of the atomic part, which in the present case includes the crystalline and Zeeman fields and also, a Heisenberg exchange coupling between the two spins. The appropriate Green's functions that define the differential conductance spectra are calculated by means of the equation-of-motion method. We obtain, in this form, a very satisfactory description of the overall experimental findings related to the behavior of the spin state excitations and Kondo resonance structures in the presence of an applied magnetic field.

  8. Spin Transport by Collective Spin Excitations

    NASA Astrophysics Data System (ADS)

    Hammel, P. Chris

    We report studies of angular momentum transport in insulating materials. Our measurements reveal efficient spin pumping from high wavevector k spin waves in thin film Y3Fe5O12 (YIG): spin pumping is independent of wavevector up to k ~ 20 μm-1. Optical detection of YIG FMR by NV centers in diamond reveals a role for spin waves in this insulator-to-insulator spin transfer process. Spin transport is typically suppressed by insulating barriers, but we find that fluctuating antiferromagnetic correlations enable efficient spin transport at nm-scale thicknesses in insulating antiferromagnets, even in the absence of long-range order, and that the spin decay length increases with the strength of the antiferromagnetic correlations. This research is supported by the U.S. DOE through Grants DE-FG02-03ER46054 and DE-SC0001304, by the NSF MRSEC program through Grant No. 1420451 and by the Army Research Office through Grant W911NF0910147.

  9. Nonreciprocal spin wave elementary excitation in dislocated dimerized Heisenberg chains.

    PubMed

    Liu, Wanguo; Shen, Yang; Fang, Guisheng; Jin, Chongjun

    2016-05-18

    A mechanism for realizing nonreciprocal elementary excitation of spin wave (SW) is proposed. We study a reference model which describes a magnonic crystal (MC) formed by two Heisenberg chains with a lateral displacement (dislocation) and a longitudinal spacer, and derive a criterion to judge whether the elementary excitation spectra are reciprocal in this ferromagnetic lattice. An analytical method based on the spin precession equation is used to solve the elementary excitation spectra. The solution is related to a key factor, the spatio-temporal structure factor [Formula: see text], which can be directly calculated through the structural parameters. When it keeps invariant under the reversions of the external magnetic field [Formula: see text] and the dislocation [Formula: see text], or one of them, the spectra are reciprocal. Otherwise, the SW possesses nonreciprocal spectra with direction-dependent band edges and exhibits a directional magnetoresistance effect. This criterion can be regarded as a necessary and sufficient condition for the (non)reciprocity in the spin lattice. Besides, this novel lattice provides a prototype for spin diodes and spin logic gates. PMID:27092428

  10. Nonreciprocal spin wave elementary excitation in dislocated dimerized Heisenberg chains

    NASA Astrophysics Data System (ADS)

    Liu, Wanguo; Shen, Yang; Fang, Guisheng; Jin, Chongjun

    2016-05-01

    A mechanism for realizing nonreciprocal elementary excitation of spin wave (SW) is proposed. We study a reference model which describes a magnonic crystal (MC) formed by two Heisenberg chains with a lateral displacement (dislocation) and a longitudinal spacer, and derive a criterion to judge whether the elementary excitation spectra are reciprocal in this ferromagnetic lattice. An analytical method based on the spin precession equation is used to solve the elementary excitation spectra. The solution is related to a key factor, the spatio-temporal structure factor {θk}≤ft(Δ x,B\\right) , which can be directly calculated through the structural parameters. When it keeps invariant under the reversions of the external magnetic field B and the dislocation Δ x , or one of them, the spectra are reciprocal. Otherwise, the SW possesses nonreciprocal spectra with direction-dependent band edges and exhibits a directional magnetoresistance effect. This criterion can be regarded as a necessary and sufficient condition for the (non)reciprocity in the spin lattice. Besides, this novel lattice provides a prototype for spin diodes and spin logic gates.

  11. Excitation of coherent propagating spin waves by pure spin currents

    PubMed Central

    Demidov, Vladislav E.; Urazhdin, Sergei; Liu, Ronghua; Divinskiy, Boris; Telegin, Andrey; Demokritov, Sergej O.

    2016-01-01

    Utilization of pure spin currents not accompanied by the flow of electrical charge provides unprecedented opportunities for the emerging technologies based on the electron's spin degree of freedom, such as spintronics and magnonics. It was recently shown that pure spin currents can be used to excite coherent magnetization dynamics in magnetic nanostructures. However, because of the intrinsic nonlinear self-localization effects, magnetic auto-oscillations in the demonstrated devices were spatially confined, preventing their applications as sources of propagating spin waves in magnonic circuits using these waves as signal carriers. Here, we experimentally demonstrate efficient excitation and directional propagation of coherent spin waves generated by pure spin current. We show that this can be achieved by using the nonlocal spin injection mechanism, which enables flexible design of magnetic nanosystems and allows one to efficiently control their dynamic characteristics. PMID:26818232

  12. Dynamical analysis of highly excited molecular spectra

    SciTech Connect

    Kellman, M.E.

    1993-12-01

    The goal of this program is new methods for analysis of spectra and dynamics of highly excited vibrational states of molecules. In these systems, strong mode coupling and anharmonicity give rise to complicated classical dynamics, and make the simple normal modes analysis unsatisfactory. New methods of spectral analysis, pattern recognition, and assignment are sought using techniques of nonlinear dynamics including bifurcation theory, phase space classification, and quantization of phase space structures. The emphasis is chaotic systems and systems with many degrees of freedom.

  13. Spin-Dependent Dissociative Excitation in a Laser Pumped Afterglow.

    NASA Astrophysics Data System (ADS)

    Bohler, Christopher Lee

    The energy and spin dependence of dissociating collisions between two types of noble gas metastable atoms and cadmium dihalide molecules have been studied in a flowing afterglow apparatus. The fluorescence spectra obtained in the range of 3000-7600 A which result from the Ar( ^{3}P_2) + CdX_2 interactions indicate a dominant dissociative excitation production mechanism. On the other hand, for the He(2^3S _1) + CdX_2 collisions, there appears to be competition between dissociative excitation and other "dark" channels. The emission spectra are further used to narrow the uncertainty in the currently accepted values for the dissociation energy of the CdX _2 molecules. The Wigner spin rule (conservation of total electronic spin) was verified for these processes as shown by the dominance of final state triplet production as compared to the virtual absence of singlet spin state production. In an attempt to further study the spin dependence of the dissociative excitation process, transfer of the longitudinal component of the electronic spin from oriented He(2 ^3S_1) atoms to Cd(6 ^3S_1) atoms was monitored. These data showed a null result for the transfor of the spin component, but were limited by a 3% systematic error of the apparatus. The spin dependent measurements rely on the ability to spin-polarize the He(2^3S _1) atoms by laser optical pumping methods. Four laser materials which exhibit promising characteristics for this procedure have been studied, and the results are presented for Nd^{3+}:YAP, La_{rm 1-x}Nd _{rm x}MgAl_ {11}O_{19}, Nd^{3+}:LiNbO _3, and Nd^{3+} :Silicate fibers.

  14. Elementary spin excitations in ultrathin itinerant magnets

    NASA Astrophysics Data System (ADS)

    Zakeri, Khalil

    2014-12-01

    Elementary spin excitations (magnons) play a fundamental role in condensed matter physics, since many phenomena e.g. magnetic ordering, electrical (as well as heat) transport properties, ultrafast magnetization processes, and most importantly electron/spin dynamics can only be understood when these quasi-particles are taken into consideration. In addition to their fundamental importance, magnons may also be used for information processing in modern spintronics. Here the concept of spin excitations in ultrathin itinerant magnets is discussed and reviewed. Starting with a historical introduction, different classes of magnons are introduced. Different theoretical treatments of spin excitations in solids are outlined. Interaction of spin-polarized electrons with a magnetic surface is discussed. It is shown that, based on the quantum mechanical conservation rules, a magnon can only be excited when a minority electron is injected into the system. While the magnon creation process is forbidden by majority electrons, the magnon annihilation process is allowed instead. These fundamental quantum mechanical selection rules, together with the strong interaction of electrons with matter, make the spin-polarized electron spectroscopies as appropriate tools to excite and probe the elementary spin excitations in low-dimensional magnets e.g ultrathin films and nanostructures. The focus is put on the experimental results obtained by spin-polarized electron energy loss spectroscopy and spin-polarized inelastic tunneling spectroscopy. The magnon dispersion relation, lifetime, group and phase velocity measured using these approaches in various ultrathin magnets are discussed in detail. The differences and similarities with respect to the bulk excitations are addressed. The role of the temperature, atomic structure, number of atomic layers, lattice strain, electronic complexes and hybridization at the interfaces are outlined. A possibility of simultaneous probing of magnons and phonons

  15. Theory of spin excitations in Fe(110) monolayers

    NASA Astrophysics Data System (ADS)

    Muniz, R. B.; Mills, D. L.

    2002-11-01

    We present theoretical studies of short-wavelength spin excitations in ferromagnetic Fe(110) monolayers either adsorbed on a W(110) substrate or free standing. We use an itinerant model of electrons as the basis for our analysis, with nine bands (the five 3d bands and the 4sp complex) included. The bands are described within an empirical tight-binding scheme, and the ferromagnetic ground state is generated from on-site intraatomic Coulomb interactions, described in mean-field theory. The random phase approximation (RPA) is employed to describe the spin excitations through analysis of the wave vector and frequency dependence of the dynamic transverse susceptibility. Several issues are explored. We compare the spin-wave stiffness and other features of the spin-wave spectrum for the free standing film and that adsorbed on the substrate to find substantial quantitative differences with origin in spin-spin interactions mediated by the substrate. We also compare the spin-wave spectrum calculated through use of the RPA, an approximate theory, but a scheme that does not invoke the adiabatic approximation, with results generated within the framework of the adiabatic approach. While the spin-wave exchange stiffnesses produced by the two methods are in agreement, there are substantial differences between excitation spectra at short wavelengths. We argue that effective interspin exchange couplings generated within the framework of the adiabatic approximation fail to provide a description of the spin-wave spectrum in the itinerant ferromagnets, beyond the low-frequency, long-wavelength regime where the spin-wave exchange stiffness suffices to describe the spectrum. We also discuss apparent hybridization gaps in the spin-wave spectrum. We show that in some cases they can be artifact of a poorly converged numerical analysis and, in one instance, on use of an inappropriate form for the intra-atomic Coulomb interaction.

  16. Edge Magnon Excitation in Spin Dimer Systems

    NASA Astrophysics Data System (ADS)

    Sakaguchi, Ryo; Matsumoto, Masashige

    2016-10-01

    Magnetic excitation in a spin dimer system on a bilayer honeycomb lattice is investigated in the presence of a zigzag edge, where disordered and ordered phases can be controlled by a quantum phase transition. In analogy with the case of graphene with a zigzag edge, a flat edge magnon mode appears in the disordered phase. In an ordered phase, a finite magnetic moment generates a mean-field potential to the magnon. Since the potential is nonuniform on the edge and bulk sites, it affects the excitation, and the dispersion of the edge mode deviates from the flat shape. We investigate how the edge magnon mode evolves when the phase changes through the quantum phase transition and discuss the similarities to ordered spin systems on a monolayer honeycomb lattice.

  17. Spin voltage generation through optical excitation of complementary spin populations.

    PubMed

    Bottegoni, Federico; Celebrano, Michele; Bollani, Monica; Biagioni, Paolo; Isella, Giovanni; Ciccacci, Franco; Finazzi, Marco

    2014-08-01

    By exploiting the spin degree of freedom of carriers inside electronic devices, spintronics has a huge potential for quantum computation and dissipationless interconnects. Pure spin currents in spintronic devices should be driven by a spin voltage generator, able to drive the spin distribution out of equilibrium without inducing charge currents. Ideally, such a generator should operate at room temperature, be highly integrable with existing semiconductor technology, and not interfere with other spintronic building blocks that make use of ferromagnetic materials. Here we demonstrate a device that matches these requirements by realizing the spintronic equivalent of a photovoltaic generator. Whereas a photovoltaic generator spatially separates photoexcited electrons and holes, our device exploits circularly polarized light to produce two spatially well-defined electron populations with opposite in-plane spin projections. This is achieved by modulating the phase and amplitude of the light wavefronts entering a semiconductor (germanium) with a patterned metal overlayer (platinum). The resulting light diffraction pattern features a spatially modulated chirality inside the semiconductor, which locally excites spin-polarized electrons thanks to electric dipole selection rules. PMID:24952750

  18. Electron Spin Resonance Spectra of Photogenerated Polarons in Poly(Paraphenylene Vinylene)

    NASA Astrophysics Data System (ADS)

    Murata, Kazuhiro; Kuroda, Shin-ichi; Shimoi, Yukihiro; Abe, Shuji; Noguchi, Takanobu; Ohnishi, Toshihiro

    1996-12-01

    Light-induced ESR (LESR) measurements have been performed on undoped poly(parapheny- lene vinylene) (PPV) down to 4 K. The ESR signal increases significantly for the excitation energy above 3.1 3.2 eV, as in the case of the excitation spectra of photocarriers reported in PPV derivatives. The anisotropic light-induced ESR spectra in oriented samples are well reproduced by the spectra calculated using a theoretical polaron spin distribution in the case of finite electron-electron interaction. These spectral features indicate that the observed spins are photogenerated polarons.

  19. Spin-flavor composition of excited baryons

    NASA Astrophysics Data System (ADS)

    Fernando, Ishara; Goity, Jose

    2015-10-01

    The excited baryon masses are analyzed in the framework of the 1 /Nc expansion using the available physical masses and also the masses obtained in lattice QCD for different quark masses. The baryon states are organized into irreducible representations of SU (6) × O (3) , where the [ 56 ,lP =0+ ] ground state and excited baryons, and the [ 56 ,2+ ] and [ 70 ,1- ] excited states are analyzed. The analyses are carried out to O 1 /Nc and first order in the quark masses. The issue of state identifications is discussed. Numerous parameter independent mass relations result at those orders, among them the well known Gell-Mann-Okubo and Equal Spacing relations, as well as additional relations involving baryons with different spins. It is observed that such relations are satisfied at the expected level of precision. Predictions for physically unknown states for each multiplet are obtained. From the quark-mass dependence of the coefficients in the baryon mass formulas an increasingly simpler picture of the spin-flavor composition of the baryons is observed with increasing pion mass (equivalently, increasing mu , d masses), as measured by the number of significant mass operators. This work was supported in part by DOE Contract No. DE-AC05-06OR23177 under which JSA operates the Thomas Jefferson National Accelerator Facility (J. L. G.), and by the NSF (USA) through Grant PHY-0855789 and PHY-1307413 (I. P. F and J. L. G).

  20. [Saltation behavior in excitation spectra of fluorescent molecules].

    PubMed

    Miao, Di; Xu, Yi-zhuang; Yang, Jun; Xu, Zhen-hua; Wu, Jin-guang

    2004-05-01

    Excitation spectra are commonly used to study relationship between molecular structure of fluorescent substances and energy transfer during the fluorescence process. It is generally taken for granted that the excitation spectrum of the sample is equivalent to its absorption spectrum, even a copy of the latter. However, exceptions have been found in many cases. Considering various factors that affect the excitation spectra of solution comprehensively, a model has been established to study the behavior of the excitation spectra. After analyzing the model mathematically, including introducing catastrophe theory, we came into the following conclusions: As far as the topological properties are concerned, the excitation spectra are the same as its absorption spectra, provided the concentration of the substance is below a threshold. However, when the concentration is beyond the threshold, the excitation spectra undergo a series of topological saltation, leading to significant a deviation from the absorption spectra. Comparative studies of both excitation and absorption spectra of naphthalene dissolved in n-hexane confirmed the above hypothesis.

  1. Spin excitations in hole-overdoped iron-based superconductors.

    PubMed

    Horigane, K; Kihou, K; Fujita, K; Kajimoto, R; Ikeuchi, K; Ji, S; Akimitsu, J; Lee, C H

    2016-01-01

    Understanding the overall features of magnetic excitation is essential for clarifying the mechanism of Cooper pair formation in iron-based superconductors. In particular, clarifying the relationship between magnetism and superconductivity is a central challenge because magnetism may play a key role in their exotic superconductivity. BaFe2As2 is one of ideal systems for such investigation because its superconductivity can be induced in several ways, allowing a comparative examination. Here we report a study on the spin fluctuations of the hole-overdoped iron-based superconductors Ba1-xKxFe2As2 (x = 0.5 and 1.0; Tc = 36 K and 3.4 K, respectively) over the entire Brillouin zone using inelastic neutron scattering. We find that their spin spectra consist of spin wave and chimney-like dispersions. The chimney-like dispersion can be attributed to the itinerant character of magnetism. The band width of the spin wave-like dispersion is almost constant from the non-doped to optimum-doped region, which is followed by a large reduction in the overdoped region. This suggests that the superconductivity is suppressed by the reduction of magnetic exchange couplings, indicating a strong relationship between magnetism and superconductivity in iron-based superconductors. PMID:27615691

  2. Spin excitations in hole-overdoped iron-based superconductors

    PubMed Central

    Horigane, K.; Kihou, K.; Fujita, K.; Kajimoto, R.; Ikeuchi, K.; Ji, S.; Akimitsu, J.; Lee, C. H.

    2016-01-01

    Understanding the overall features of magnetic excitation is essential for clarifying the mechanism of Cooper pair formation in iron-based superconductors. In particular, clarifying the relationship between magnetism and superconductivity is a central challenge because magnetism may play a key role in their exotic superconductivity. BaFe2As2 is one of ideal systems for such investigation because its superconductivity can be induced in several ways, allowing a comparative examination. Here we report a study on the spin fluctuations of the hole-overdoped iron-based superconductors Ba1-xKxFe2As2 (x = 0.5 and 1.0; Tc = 36 K and 3.4 K, respectively) over the entire Brillouin zone using inelastic neutron scattering. We find that their spin spectra consist of spin wave and chimney-like dispersions. The chimney-like dispersion can be attributed to the itinerant character of magnetism. The band width of the spin wave-like dispersion is almost constant from the non-doped to optimum-doped region, which is followed by a large reduction in the overdoped region. This suggests that the superconductivity is suppressed by the reduction of magnetic exchange couplings, indicating a strong relationship between magnetism and superconductivity in iron-based superconductors. PMID:27615691

  3. Spin excitations in hole-overdoped iron-based superconductors

    NASA Astrophysics Data System (ADS)

    Horigane, K.; Kihou, K.; Fujita, K.; Kajimoto, R.; Ikeuchi, K.; Ji, S.; Akimitsu, J.; Lee, C. H.

    2016-09-01

    Understanding the overall features of magnetic excitation is essential for clarifying the mechanism of Cooper pair formation in iron-based superconductors. In particular, clarifying the relationship between magnetism and superconductivity is a central challenge because magnetism may play a key role in their exotic superconductivity. BaFe2As2 is one of ideal systems for such investigation because its superconductivity can be induced in several ways, allowing a comparative examination. Here we report a study on the spin fluctuations of the hole-overdoped iron-based superconductors Ba1-xKxFe2As2 (x = 0.5 and 1.0; Tc = 36 K and 3.4 K, respectively) over the entire Brillouin zone using inelastic neutron scattering. We find that their spin spectra consist of spin wave and chimney-like dispersions. The chimney-like dispersion can be attributed to the itinerant character of magnetism. The band width of the spin wave-like dispersion is almost constant from the non-doped to optimum-doped region, which is followed by a large reduction in the overdoped region. This suggests that the superconductivity is suppressed by the reduction of magnetic exchange couplings, indicating a strong relationship between magnetism and superconductivity in iron-based superconductors.

  4. Spectra from nuclear-excited plasmas

    NASA Technical Reports Server (NTRS)

    De Young, R. J.; Weaver, W. R.

    1980-01-01

    The paper discusses the spectra taken from He-3(n,p)H-3 nuclear-induced plasmas under high thermal neutron flux, lasing conditions. Also, initial spectra are presented for U-235F6 generated plasmas. From an evaluation of these spectra, important atomic and molecular processes that occur in the plasma can be inferred. The spectra presented are the first to be generated by He-3 and U-235F6 nuclear reactions under high neutron flux, lasing conditions. The U-235(n,ff)FF reaction, which liberates 165 MeV of fission-fragment kinetic energy, creates plasmas that are of great interest, since at sufficiently high densities of U-235F6 the gas becomes self-critical; thus, there is no need for an external driving reactor (source of neutrons). The spectra from mixtures of He-3 and Ar, Xe, Kr, Ne, Cl2, F2 and N2 indicate little difference between high-pressure nuclear-induced plasmas and high-pressure electrically pulsed afterglow plasmas for noble-gas systems

  5. Probing excitations in insulators via injection of spin currents

    NASA Astrophysics Data System (ADS)

    Chatterjee, Shubhayu; Sachdev, Subir

    2015-10-01

    We propose a spin transport experiment to measure the low-energy excitations in insulators with spin degrees of freedom, with a focus on detecting ground states that lack magnetic order. A general formalism to compute the spin current from a metal with a nonequilibrium distribution of spins to an insulator is developed. It is applied to insulating states with and without long range magnetic order, and salient features in the spin conductance are noted.

  6. On the particle excitations in the XXZ spin chain

    NASA Astrophysics Data System (ADS)

    Ovchinnikov, A. A.

    2013-12-01

    We continue to study the excited states for the XXZ spin chain corresponding to the complex roots of the Bethe Ansatz equations with the imaginary part equal to π/2. We propose the particle-hole symmetry which relates the eigenstates build up from the two different pseudovacuum states. We find the XXX spin chain limit for the eigenstates with the complex roots. We also comment on the low-energy excited states for the XXZ spin chain.

  7. Longitudinal spin dynamics in ferrimagnets: Multiple spin wave nature of longitudinal spin excitations

    NASA Astrophysics Data System (ADS)

    Krivoruchko, V. N.

    2016-08-01

    Motivated by the existing controversy about the physical mechanisms that govern longitudinal magnetization dynamics under the effect of ultrafast laser pulses, in this paper we study the microscopic model of longitudinal spin excitations in a two-sublattice ferrimagnet using the diagrammatic technique for spin operators. The diagrammatic approach provides us with an efficient procedure to derive graphical representations for perturbation expansion series for different spin Green's functions and thus to overcome limitations typical for phenomenological approaches. The infinite series involving all distinct loops built from spin wave propagators are summed up. These result in an expression for the longitudinal spin susceptibility χz z(q ,ω ) applicable in all regions of frequency ω and wave vector q space beyond the hydrodynamical and critical regimes. A strong renormalization of the longitudinal spin oscillations due to processes of virtual creation and annihilation of transverse spin waves has been found. We have shown that the spectrum of longitudinal excitations consists of a quasirelaxation mode forming a central peak in χz z(q ,ω ) and two (acoustic and exchange) precessionlike modes. As the main result, it is predicted that both acoustic and exchange longitudinal excitations are energetically above similar modes of transverse spin waves at the same temperature and wave vector. The existence of the exchange longitudinal mode at such frequencies can result in a new form of excitation behavior in ferrimagnetic system, which could be important for understanding the physics of nonequilibrium magnetic dynamics under the effect of ultrafast laser pulses in multisublattice magnetic materials.

  8. Excitation of plasmons in Ag/Fe/W structure by spin-polarized electrons

    SciTech Connect

    Samarin, Sergey N.; Kostylev, Mikhail; Williams, J. F.; Artamonov, Oleg M.; Baraban, Alexander P.; Guagliardo, Paul

    2015-09-07

    Using Spin-polarized Electron-Energy Loss Spectroscopy (SPEELS), the plasmon excitations were probed in a few atomic layers thick Ag film deposited on an Fe layer or on a single crystal of W(110). The measurements were performed at two specular geometries with either a 25° or 72° angle of incidence. On a clean Fe layer (10 atomic layers thick), Stoner excitation asymmetry was observed, as expected. Deposition of a silver film on top of the Fe layer dramatically changed the asymmetry of the SPEELS spectra. The spin-effect depends on the kinematics of the scattering: angles of incidence and detection. The spin-dependence of the plasmon excitations in the silver film on the W(110) surface and on the ferromagnetic Fe film is suggested to arise from the spin-active Ag/W or Ag/Fe interfaces.

  9. Test of spin symmetry in anti-nucleon spectra

    NASA Astrophysics Data System (ADS)

    He, X. T.; Zhou, S. G.; Meng, J.; Zhao, E. G.; Scheid, W.

    2006-06-01

    The spin symmetry in antinucleon spectra of a nucleus is tested by investigating the relations between the Dirac wave functions of the spin doublets and examining these relations in realistic nuclei within the relativistic mean-field model. In addition to the fact that the dominant components of the Dirac spinors of the spin doublet are nearly identical to each other, there is a differential relation between the smaller components which is found to be almost exactly fulfilled.

  10. Universal entanglement spectra in critical spin chains

    NASA Astrophysics Data System (ADS)

    Lundgren, Rex; Blair, Jonathan; Laurell, Pontus; Regnault, Nicolas; Fiete, Gregory A.; Greiter, Martin; Thomale, Ronny

    2016-08-01

    We advocate that in critical spin chains, and possibly in a larger class of one-dimensional critical models, a gap in the momentum-space entanglement spectrum separates the universal part of the spectrum, which is determined by the associated conformal field theory, from the nonuniversal part, which is specific to the model. To this end, we provide affirmative evidence from multicritical spin chains with low-energy sectors described by the SU(2 ) 2 or the SU(3 ) 1 Wess-Zumino-Witten model.

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

    SciTech Connect

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

    2011-05-01

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

  12. Excitation and propagation of exchange spin waves in films of yttrium iron garnet

    SciTech Connect

    Zil`berman, P.E.; Temiryazev, A.G.; Tikhomirova, M.P.

    1995-07-01

    We investigate resonant microwave absorption in films of yttrium iron garnet (YIG) with magneetic properties varying through the film thickness. Using measurements of the spin-wave resonant absorption spectra for two different directions of the external magnetic field, we calculate the profile of this nonuniformity. In our investigation of the response of nonuniform films to a pulsed microwave signal, we observed the appearance of delayed pulses, which we interpret to be the result of propagation of exchange spin waves transversely through the film. We analyze the dependence of the time delay on frequency for various nonuniformity profiles, and compare the data obtained with the results of experiment. Our investigation of the spin-wave resonance spectra, as well as the results of our pulsed measurements, show that propagation of spin waves is accompanied by the excitation of acoustic waves. We conclude that ferrite films that vary in the transverse direction can on the one hand be used to efficiently excite short-wavelength exchange spin waves with wave numbers 1{approximately}3 {center_dot}10{sup 5} cm{sup {minus}1}, and on the other hand to excite very high-frequency acoustic waves. 25 refs., 15 figs.

  13. Excitation Spectra and Brightness Optimization of Two-Photon Excited Probes

    PubMed Central

    Mütze, Jörg; Iyer, Vijay; Macklin, John J.; Colonell, Jennifer; Karsh, Bill; Petrášek, Zdeněk; Schwille, Petra; Looger, Loren L.; Lavis, Luke D.; Harris, Timothy D.

    2012-01-01

    Two-photon probe excitation data are commonly presented as absorption cross section or molecular brightness (the detected fluorescence rate per molecule). We report two-photon molecular brightness spectra for a diverse set of organic and genetically encoded probes with an automated spectroscopic system based on fluorescence correlation spectroscopy. The two-photon action cross section can be extracted from molecular brightness measurements at low excitation intensities, while peak molecular brightness (the maximum molecular brightness with increasing excitation intensity) is measured at higher intensities at which probe photophysical effects become significant. The spectral shape of these two parameters was similar across all dye families tested. Peak molecular brightness spectra, which can be obtained rapidly and with reduced experimental complexity, can thus serve as a first-order approximation to cross-section spectra in determining optimal wavelengths for two-photon excitation, while providing additional information pertaining to probe photostability. The data shown should assist in probe choice and experimental design for multiphoton microscopy studies. Further, we show that, by the addition of a passive pulse splitter, nonlinear bleaching can be reduced—resulting in an enhancement of the fluorescence signal in fluorescence correlation spectroscopy by a factor of two. This increase in fluorescence signal, together with the observed resemblance of action cross section and peak brightness spectra, suggests higher-order photobleaching pathways for two-photon excitation. PMID:22385865

  14. Simulating electron spin resonance spectra of nitroxide spin labels from molecular dynamics and stochastic trajectories

    PubMed Central

    Sezer, Deniz; Freed, Jack H.; Roux, Benoît

    2008-01-01

    Simulating electron spin resonance spectra of nitroxide spin labels from motional models is necessary for the quantitative analysis of experimental spectra. We present a framework for modeling the spin label dynamics by using trajectories such as those from molecular dynamics (MD) simulations combined with stochastic treatment of the global protein tumbling. This is achieved in the time domain after two efficient numerical integrators are developed: One for the quantal dynamics of the spins and the other for the classical rotational diffusion. For the quantal dynamics, we propagate the relevant part of the spin density matrix in Hilbert space. For the diffusional tumbling, we work with quaternions, which enables the treatment of anisotropic diffusion in a potential expanded as a sum of spherical harmonics. Time-averaging arguments are invoked to bridge the gap between the smaller time step of the MD trajectories and the larger time steps appropriate for the rotational diffusion and∕or quantal spin dynamics. PMID:18447510

  15. Thermally excited proton spin-flip laser emission in tokamaks

    SciTech Connect

    Arunasalam, V.; Greene, G.J.

    1993-07-01

    Based on statistical thermodynamic fluctuation arguments, it is shown here for the first time that thermally excited spin-flip laser emission from the fusion product protons can occur in large tokamak devices that are entering the reactor regime of operation. Existing experimental data from TFTR supports this conjecture, in the sense that these measurements are in complete agreement with the predictions of the quasilinear theory of the spin-flip laser.

  16. Sensitivity enhancement of MQMAS NMR spectra of spin 3/2 nuclei using hyperbolic secant pulses

    NASA Astrophysics Data System (ADS)

    Siegel, Renée; Nakashima, Thomas T.; Wasylishen, Roderick E.

    2005-02-01

    The use of hyperbolic secant (HS) pulses to enhance the intensity of the central transition in MQMAS experiments for spin 3/2 quadrupolar nuclei is investigated by examining 87Rb NMR spectra of a powder sample of RbNO 3. The application of HS pulses prior to the triple-quantum (3Q) excitation provides sensitivity enhancements in MQMAS spectra that are superior to those previously reported. For the conversion of 3Q to single-quantum (1Q) observables, the HS pulses have an efficiency similar to that reported for double frequency sweeps (DFS) but greater than that of the fast amplitude modulation (FAM) technique.

  17. Localized excitation of magnetostatic surface spin waves in yttrium iron garnet by shorted coaxial probe detected via spin pumping and rectification effect

    SciTech Connect

    Soh, Wee Tee Ong, C. K.; Peng, Bin

    2015-04-21

    We demonstrate the localized excitation and dc electrical detection of magnetostatic surface spin waves (MSSWs) in yttrium iron garnet (YIG) by a shorted coaxial probe. Thin films of NiFe and Pt are patterned at different regions onto a common bulk YIG substrate. A shorted coaxial probe is used to excite spin precession locally near various patterned regions. The dc voltages across the corresponding regions are recorded. For excitation of the Pt regions, the dc voltage spectra are dominated by the spin pumping of MSSWs from YIG, where various modes can be clearly distinguished. For the NiFe region, it is also found that spin pumping from MSSWs generated in YIG dominated the spectra, indicating that the spin pumped currents are dissipated into charge currents via the inverse Spin Hall effect (ISHE) in NiFe. For all regions, dc signals from YIG MSSWs are observed to be much stronger than the ferromagnetic resonance (FMR) uniform mode, likely due to the nature of the microwave excitation. The results indicate the potential of this probe for microwave imaging via dc detection of spin dynamics in continuous and patterned films.

  18. Fluorescence Emission and Excitation Spectra of Photo-Fragmented Nitrobenzene.

    NASA Astrophysics Data System (ADS)

    Lue, Christopher J.; Tanjaroon, Chakree; Johnson, J. Bruce; Allen, Susan D.; Reeve, Scott W.

    2012-06-01

    Upon absorption of a UV photon, nitrobenzene readily dissociates into C_6H_5, NO_2, C_6H_5NO, O, C_6H_5O, and NO through three different channels. We have recorded high resolution emission and excitation spectra of the NO resulting from photo-fragmented nitrobenzene using a pulsed picosecond tunable laser and a nanosecond dye laser. Specifically, the lasers probed the A^2Σ^+→ X^2π(1/2,3/2) NO band system between 225-260 nm using an one or two color process. In a one color process, the same energy (wavelength) photon is used to dissociate nitrobenzene and excite NO. In a two color process, photons of a particular energy are used to dissociate the nitrobenzene while photons of a different energy are used to probe the resultant NO. We have determined the rotational and vibrational temperatures of the nascent NO. And, we have examined the effect of the relative timing of the two photons on the fluorescence spectra to extract information about the photodissociation dynamics. Lin, M.-F.; Lee, Y. T.; Ni, C.-K.; Xu, S. and Lin, M. C. J. Chem. Phys., AIP, 2007, 126.

  19. Coupled spin and charge collective excitations in a spin polarized electron gas

    SciTech Connect

    Marinescu, D.C.; Quinn, J.J.; Yi, K.S.

    1997-08-12

    The charge and longitudinal spin responses induced in a spin polarized quantum well by a weak electromagnetic field are investigated within the framework of the linear response theory. The authors evaluate the excitation frequencies for the intra- and inter-subband transitions of the collective charge and longitudinal spin density oscillations including many-body corrections beyond the random phase approximation through the spin dependent local field factors, G{sub {sigma}}{sup {+-}} (q,{omega}). An equation-of-motion method was used to obtain these corrections in the limit of long wavelengths, and the results are given in terms of the equilibrium pair correlation function. The finite degree of spin polarization is shown to introduce coupling between the charge and spin density modes, in contrast with the result for an unpolarized system.

  20. Spin excitations in a monolayer scanned by a magnetic tip

    NASA Astrophysics Data System (ADS)

    Magiera, M. P.; Brendel, L.; Wolf, D. E.; Nowak, U.

    2009-07-01

    Energy dissipation via spin excitations is investigated for a hard ferromagnetic tip scanning a soft magnetic monolayer. We use the classical Heisenberg model with Landau-Lifshitz-Gilbert (LLG) dynamics including a stochastic field representing finite temperatures. The friction force depends linearly on the velocity (provided it is small enough) for all temperatures. For low temperatures, the corresponding friction coefficient is proportional to the phenomenological damping constant of the LLG equation. This dependence is lost at high temperatures, where the friction coefficient decreases exponentially. These findings can be explained by properties of the spin polarisation cloud dragged along with the tip.

  1. Massive Triplet Excitations in a Magnetized Anisotropic Haldane Spin Chain

    SciTech Connect

    Zheludev, Andrey I; Honda, Z.; Broholm, C. L.; Katsumada, K.; Shapiro, S. M.; Kolezhuk, A.; Park, S.; Qiu, Y.

    2003-01-01

    Inelastic neutron scattering experiments on the Haldane-gap quantum antiferromagnet Ni(C{sub 5}D{sub 14}N{sub 2}){sub 2}N{sub 3}(PF{sub 6}) are performed at mK temperatures in magnetic fields of almost twice the critical field H{sub c} applied perpendicular to the spin chains. Above H{sub c} a reopening of the spin gap is clearly observed. In the high-field Neel-ordered state the spectrum is dominated by three distinct excitation branches. A theoretical model consistently describing the experimental data is proposed.

  2. Spin and pseudospin symmetries and the equivalent spectra of relativistic spin-1/2 and spin-0 particles

    SciTech Connect

    Alberto, P.; Castro, A. S. de; Malheiro, M.

    2007-04-15

    We show that the conditions which originate the spin and pseudospin symmetries in the Dirac equation are the same that produce equivalent energy spectra of relativistic spin-1/2 and spin-0 particles in the presence of vector and scalar potentials. The conclusions do not depend on the particular shapes of the potentials and can be important in different fields of physics. When both scalar and vector potentials are spherical, these conditions for isospectrality imply that the spin-orbit and Darwin terms of either the upper component or the lower component of the Dirac spinor vanish, making it equivalent, as far as energy is concerned, to a spin-0 state. In this case, besides energy, a scalar particle will also have the same orbital angular momentum as the (conserved) orbital angular momentum of either the upper or lower component of the corresponding spin-1/2 particle. We point out a few possible applications of this result.

  3. Optimization of excitation transfer in a spin chain

    NASA Astrophysics Data System (ADS)

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

    2016-06-01

    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.

  4. Phase transitions and elementary excitations in spin-1 Bose gases with Raman-induced spin-orbit coupling

    NASA Astrophysics Data System (ADS)

    Yu, Zeng-Qiang

    2016-03-01

    We study the ground-state phase diagram and the quantum phase transitions in spin-1 Bose gases with Raman-induced spin-orbit coupling. In addition to the Bose-Einstein condensates with uniform density, three types of stripe condensation phases that simultaneously break the U(1) symmetry and the translation symmetry are identified. The transitions between these phases are investigated, and the occurrences of the various tricritical points are predicted. The excitation spectra in the plane-wave phase and the zero-momentum phase show rich roton-maxon structures, and their instabilities indicate the tendency to develop the crystalline order. We propose the atomic gas of 23Na could be a candidate for observing the stripe condensate with high contrast fringes.

  5. Temperature impact on the spectra of the spin-wave resonance in two-layer magnetic films

    NASA Astrophysics Data System (ADS)

    Zyuzin, A. M.; Bakulin, M. A.; Radaikin, V. V.; Sabaev, S. N.; Yantsen, N. V.

    2016-05-01

    A sharp difference has been revealed in the behavior of the temperature dependences of the spectra of the spin-wave resonance of two-layer films with different parameters of the pinning layers. The calculations have shown that the effect of the disappearance and subsequent appearance of spin-wave modes in the specific temperature ranges was connected with the decrease in the degree of pinning because of the convergence of the fields of uniform resonance in the layers of excitation and pinning of spin fluctuations.

  6. Quantum gates controlled by spin chain soliton excitations

    SciTech Connect

    Cuccoli, Alessandro; Nuzzi, Davide; Vaia, Ruggero; Verrucchi, Paola

    2014-05-07

    Propagation of soliton-like excitations along spin chains has been proposed as a possible way for transmitting both classical and quantum information between two distant parties with negligible dispersion and dissipation. In this work, a somewhat different use of solitons is considered. Solitons propagating along a spin chain realize an effective magnetic field, well localized in space and time, which can be exploited as a means to manipulate the state of an external spin (i.e., a qubit) that is weakly coupled to the chain. We have investigated different couplings between the qubit and the chain, as well as different soliton shapes, according to a Heisenberg chain model. It is found that symmetry properties strongly affect the effectiveness of the proposed scheme, and the most suitable setups for implementing single qubit quantum gates are singled out.

  7. User-friendly software for modeling collective spin wave excitations

    NASA Astrophysics Data System (ADS)

    Hahn, Steven; Peterson, Peter; Fishman, Randy; Ehlers, Georg

    There exists a great need for user-friendly, integrated software that assists in the scientific analysis of collective spin wave excitations measured with inelastic neutron scattering. SpinWaveGenie is a C + + software library that simplifies the modeling of collective spin wave excitations, allowing scientists to analyze neutron scattering data with sophisticated models fast and efficiently. Furthermore, one can calculate the four-dimensional scattering function S(Q,E) to directly compare and fit calculations to experimental measurements. Its generality has been both enhanced and verified through successful modeling of a wide array of magnetic materials. Recently, we have spent considerable effort transforming SpinWaveGenie from an early prototype to a high quality free open source software package for the scientific community. S.E.H. acknowledges support by the Laboratory's Director's fund, ORNL. Work was sponsored by the Division of Scientific User Facilities, Office of Basic Energy Sciences, US Department of Energy, under Contract No. DE-AC05-00OR22725 with UT-Battelle, LLC.

  8. Magnetic field dependence of spin-forbidden electronic excitations reflects the Haldane or paramagnetic ground state

    NASA Astrophysics Data System (ADS)

    Long, V. C.; Montague, J. R.; Kozen, A. C.; Wei, X.; Landry, B. R.; Pearson, K. R.; Turnbull, M. M.; Landee, C. P.

    2007-03-01

    We compare the zero-field and magnetic field-dependent optical spectra of the Haldane chain compound NENB (Ni[en]2NO2BF4; en = C2N2H8) and the paramagnetic compound, Ni(en) 3(ClO4)2,H2O. Due to similar electronic coordination of Ni^2+, the two materials show similar zero-field d-d electronic transitions, including a spin-forbidden (SF) transition at 1.58 eV, overlapping a broad spin-allowed band at 1.45 eV. The relatively greater intensity of the SF band in the Haldane compound suggests activation by a spin exchange mechanism, whereas a spin-orbit coupling origin is likely in the paramagnet. A second narrower SF spin flip transition appears in NENB at 1.66 eV. In both compounds, the SF excitations are sensitive to applied field H. In NENB, the SF intensity is suppressed by H, consistent with behavior of spin exchange-activated bands. In Ni(en)3(ClO4)-2,H2O, the SF field sensitivity appears to combine an energy shift and intensity decrease. Details of the H dependence reflect the magnetic ground state of the material: the field sensitivity commences only above HC 10 T, in the Haldane compound, whereas the field-induced modifications begin immediately at H = 0 T in the paramagnet.

  9. Spin wave spectra in perpendicularly magnetized permalloy rings

    SciTech Connect

    Zhou, X.; Ding, J.; Adeyeye, A. O.; Kostylev, M.

    2015-03-16

    The dynamic behavior of perpendicularly magnetized permalloy circular rings is systematically investigated as a function of film thickness using broadband field modulated ferromagnetic resonance spectroscopy. We observed the splitting of one spin wave mode into a family of dense resonance peaks for the rings, which is markedly different from the single mode observed for continuous films of the same thickness. As the excitation frequency is increased, the mode family observed for the rings gradually converges into one mode. With the increase in the film thickness, a sparser spectrum of modes is observed. Our experimental results are in qualitative agreement with the dynamic micromagnetic simulations.

  10. Level densities and spin cutoff parameters for 60Co and 62Ni from proton evaporation spectra

    NASA Astrophysics Data System (ADS)

    Voinov, Alexander; Grimes, Steven; Brune, Carl R.; Burger, Alexander; Gorgen, Andreas; Guttormsen, Magne; Larsen, Ann Cecilie; Massey, Tomas; Siem, Sunniva

    2013-10-01

    Prediction of reaction cross sections remains a major problem in applications such as data evaluations or/and astrophysics reaction rate calculations. There is big progress in the development of nuclear reaction codes which now include different reaction mechanisms. However, these codes use many input parameters. The variety of input parameters helps us to describe existing experimental data but it creates problems when it comes to predictions. The uncertainties of the level density and the spin cutoff parameter cause the major concern. The proton spectra from α and lithium induced reactions have been measured and analyzed with the Hauser-Feshbach model. Different input level density models have been tested. The level densities and spin cutoff parameters were obtained with Monte-Carlo technique taking into account known spins of discrete low-lying levels of residual nuclei. It was found that the best description is achieved with the Gilbert and Cameron model functions. Excitation energy dependence of spin cutoff parameters was found to be different for 60Co and 62Ni nuclei. It is inconsistent with Fermi-gas model which is usually used to calculate spin cutoff parameters.

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

    SciTech Connect

    Dobryakov, A. L.; Quick, M.; Ioffe, I. N.; Granovsky, A. A.; Ernsting, N. P.; Kovalenko, S. A.

    2014-05-14

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

  12. Exchange-coupling modified spin wave spectra in the perpendicularly magnetized Permalloy nanodot chain arrays

    NASA Astrophysics Data System (ADS)

    Dou, Jian; Hernandez, Sarah C.; Yu, Chengtao; Pechan, Michael J.; Folks, Liesl; Katine, Jordan A.; Carey, Matthew J.

    2010-05-01

    Spin wave spectra in exchange-coupled nanoscale dot chain arrays were studied using ferromagnetic resonance. The dot chain arrays, with dot diameters of 300 nm and thicknesses of 40 nm, coupled via Permalloy bridges of width ranging from 0 (no bridge) to 60 nm, were fabricated using e-beam lithography. In the perpendicularly magnetized isolated dots, multiple sharp ferromagnetic resonant peaks were observed, which are associated with the quantized in-plane wave vector due to the finite dot radius. These spectrum lines shift to higher fields for samples with wider bridges due to the increasing effective demagnetizing factor. For coupled dots, additional satellite peaks were observed at both sides of higher order spin wave modes and at the lower field side of the uniform mode. We show that these satellite peaks can be attributed to the excitation in each bridged dot and the interdot exchange coupling, respectively.

  13. Low Lying Spin Excitation in the Spin Ice Ho2Ti2O7

    SciTech Connect

    Ehlers, Georg; Mamontov, Eugene; Zamponi, Michaela M; Gardner, Jason S

    2010-01-01

    The high flux and low background of the new backscattering spectrometer at the SNS combine to produce an excellent signal to noise ratio, allowing us to investigate a low lying weak excitation never seen before in the spin ice, Ho{sub 2}Ti{sub 2}O{sub 7}. This non-dispersive excitation has been observed at E = 26.3 {mu}eV below 100 K but is resolution limited only below {approx}65 K. It is indifferent to magnetic fields below {mu}{sub 0}H = 4.5 T, at 1.6 K. These characteristics help us to identify the excitation as due to the nuclear spin system.

  14. Magnetic vortex core reversal by excitation of spin waves

    PubMed Central

    Kammerer, Matthias; Weigand, Markus; Curcic, Michael; Noske, Matthias; Sproll, Markus; Vansteenkiste, Arne; Van Waeyenberge, Bartel; Stoll, Hermann; Woltersdorf, Georg; Back, Christian H.; Schuetz, Gisela

    2011-01-01

    Micron-sized magnetic platelets in the flux-closed vortex state are characterized by an in-plane curling magnetization and a nanometer-sized perpendicularly magnetized vortex core. Having the simplest non-trivial configuration, these objects are of general interest to micromagnetics and may offer new routes for spintronics applications. Essential progress in the understanding of nonlinear vortex dynamics was achieved when low-field core toggling by excitation of the gyrotropic eigenmode at sub-GHz frequencies was established. At frequencies more than an order of magnitude higher vortex state structures possess spin wave eigenmodes arising from the magneto-static interaction. Here we demonstrate experimentally that the unidirectional vortex core reversal process also occurs when such azimuthal modes are excited. These results are confirmed by micromagnetic simulations, which clearly show the selection rules for this novel reversal mechanism. Our analysis reveals that for spin-wave excitation the concept of a critical velocity as the switching condition has to be modified. PMID:21505435

  15. Doping evolution of spin and charge excitations in the Hubbard model

    DOE PAGES

    Kung, Y. F.; Nowadnick, E. A.; Jia, C. J.; Johnston, S.; Moritz, B.; Scalettar, R. T.; Devereaux, T. P.

    2015-11-05

    We shed light on how electronic correlations vary across the phase diagram of the cuprate superconductors, examining the doping evolution of spin and charge excitations in the single-band Hubbard model using determinant quantum Monte Carlo (DQMC). In the single-particle response, we observe that the effects of correlations weaken rapidly with doping, such that one may expect the random phase approximation (RPA) to provide an adequate description of the two-particle response. In contrast, when compared to RPA, we find that significant residual correlations in the two-particle excitations persist up to 40% hole and 15% electron doping (the range of dopings achievedmore » in the cuprates). Ultimately, these fundamental differences between the doping evolution of single- and multi-particle renormalizations show that conclusions drawn from single-particle processes cannot necessarily be applied to multi-particle excitations. Eventually, the system smoothly transitions via a momentum-dependent crossover into a weakly correlated metallic state where the spin and charge excitation spectra exhibit similar behavior and where RPA provides an adequate description.« less

  16. Doping evolution of spin and charge excitations in the Hubbard model

    SciTech Connect

    Kung, Y. F.; Nowadnick, E. A.; Jia, C. J.; Johnston, S.; Moritz, B.; Scalettar, R. T.; Devereaux, T. P.

    2015-11-05

    We shed light on how electronic correlations vary across the phase diagram of the cuprate superconductors, examining the doping evolution of spin and charge excitations in the single-band Hubbard model using determinant quantum Monte Carlo (DQMC). In the single-particle response, we observe that the effects of correlations weaken rapidly with doping, such that one may expect the random phase approximation (RPA) to provide an adequate description of the two-particle response. In contrast, when compared to RPA, we find that significant residual correlations in the two-particle excitations persist up to 40% hole and 15% electron doping (the range of dopings achieved in the cuprates). Ultimately, these fundamental differences between the doping evolution of single- and multi-particle renormalizations show that conclusions drawn from single-particle processes cannot necessarily be applied to multi-particle excitations. Eventually, the system smoothly transitions via a momentum-dependent crossover into a weakly correlated metallic state where the spin and charge excitation spectra exhibit similar behavior and where RPA provides an adequate description.

  17. Superconductivity and spin excitations in orbitally ordered FeSe

    NASA Astrophysics Data System (ADS)

    Kreisel, Andreas; Mukherjee, Shantanu; Hirschfeld, P. J.; Andersen, B. M.

    We provide a band-structure with low-energy properties consistent with recent photoemission and quantum oscillations measurements on the Fe-based superconductor FeSe, including a mean-field like orbital ordering in the dxz /dyz channel, and show that this model also accounts for the temperature dependence of the measured Knight shift and the spin-relaxation rate. An RPA calculation of the dynamical spin susceptibility yields spin excitations which are peaked at wave vector (π , 0) in the 1-Fe Brillouin zone, with a broad maximum at energies of order a few meV. Furthermore, the superconducting gap structure obtained from spin fluctuation theory exhibits nodes on the electron pockets, consistent with the 'V'-shaped density of states measured by tunneling spectroscopy on this material. The redistribution of spectral weight in the superconducting state creates a (π , 0) ''neutron resonance'' as seen in recent experiments. Comparing to various experimental results, we give predictions for further studies A.K. and B.M.A. acknowledge financial support from a Lundbeckfond fellowship (Grant No. A9318). P.J.H. was partially supported by the Department of Energy under Grant No. DE-FG02-05ER46236.

  18. Thermal Hall Effect of Spin Excitations in a Kagome Magnet.

    PubMed

    Hirschberger, Max; Chisnell, Robin; Lee, Young S; Ong, N P

    2015-09-01

    At low temperatures, the thermal conductivity of spin excitations in a magnetic insulator can exceed that of phonons. However, because they are charge neutral, the spin waves are not expected to display a thermal Hall effect. However, in the kagome lattice, theory predicts that the Berry curvature leads to a thermal Hall conductivity κ(xy). Here we report observation of a large κ(xy) in the kagome magnet Cu(1-3, bdc) which orders magnetically at 1.8 K. The observed κ(xy) undergoes a remarkable sign reversal with changes in temperature or magnetic field, associated with sign alternation of the Chern flux between magnon bands. The close correlation between κ(xy) and κ(xx) firmly precludes a phonon origin for the thermal Hall effect. PMID:26382691

  19. Thermal Hall Effect of Spin Excitations in a Kagome Magnet.

    PubMed

    Hirschberger, Max; Chisnell, Robin; Lee, Young S; Ong, N P

    2015-09-01

    At low temperatures, the thermal conductivity of spin excitations in a magnetic insulator can exceed that of phonons. However, because they are charge neutral, the spin waves are not expected to display a thermal Hall effect. However, in the kagome lattice, theory predicts that the Berry curvature leads to a thermal Hall conductivity κ(xy). Here we report observation of a large κ(xy) in the kagome magnet Cu(1-3, bdc) which orders magnetically at 1.8 K. The observed κ(xy) undergoes a remarkable sign reversal with changes in temperature or magnetic field, associated with sign alternation of the Chern flux between magnon bands. The close correlation between κ(xy) and κ(xx) firmly precludes a phonon origin for the thermal Hall effect.

  20. Ultrafast Magic-Angle Spinning: Benefits for the Acquisition of Ultrawide-Line NMR Spectra of Heavy Spin-1/2 Nuclei.

    PubMed

    Pöppler, Ann-Christin; Demers, Jean-Philippe; Malon, Michal; Singh, Amit Pratap; Roesky, Herbert W; Nishiyama, Yusuke; Lange, Adam

    2016-03-16

    The benefits of the ultrafast magic-angle spinning (MAS) approach for the acquisition of ultrawide-line NMR spectra-spectral simplification, increased mass sensitivity allowing the fast study of small amounts of material, efficient excitation, and application to multiple heavy nuclei-are demonstrated for tin(II) oxide (SnO) and the tin complex [(LB)Sn(II) Cl](+) [Sn(II) Cl3 ](-) [LB=2,6-diacetylpyridinebis(2,6-diisopropylanil)] containing two distinct tin environments. The ultrafast MAS experiments provide optimal conditions for the extraction of the chemical-shift anisotropy tensor parameters, anisotropy, and asymmetry for heavy spin-1/2 nuclei.

  1. Hydrodynamic study of edge spin-vortex excitations of fractional quantum Hall fluid

    NASA Astrophysics Data System (ADS)

    Rabiu, M.; Mensah, S. Y.; Seini, I. Y.; Abukari, S. S.

    2016-07-01

    We undertake a theoretical study of edge spin-vortex excitations in fractional quantum Hall fluid. This is done in view of quantised Euler hydrodynamics theory. The dispersions of true excitations for fractions within 0 ≤ ν ≤ 1 are simulated which exhibit universal similarities and differences in behaviour. The differences arise from different edge smoothness and spin (pseudo-spin) polarisations, in addition to spin-charge competition. In particular, tuning the spin-charge factor causes coherent spin flipping associated with partial and total polarisations of edge spin-vortices. This observation is tipped as an ideal mechanism for realisation of functional spintronic devices.

  2. Theoretical grounds of relativistic methods for calculation of spin-spin coupling constants in nuclear magnetic resonance spectra

    NASA Astrophysics Data System (ADS)

    Rusakova, I. L.; Rusakov, Yu Yu; Krivdin, L. B.

    2016-04-01

    The theoretical grounds of the modern relativistic methods for quantum chemical calculation of spin-spin coupling constants in nuclear magnetic resonance spectra are considered. Examples and prospects of application of relativistic calculations of these constants in the structural studies of organic and heteroorganic compounds are discussed. Practical recommendations on relativistic calculations of spin-spin coupling constants using the available software are given. The bibliography includes 622 references.

  3. Probing Spin Excitations Using Magneto-Raman Spectroscopy

    NASA Astrophysics Data System (ADS)

    Thirunavukkuarasu, K.; Lu, Z.; Simpson, J.; Walker, A.; Sears, J.; Kim, Y.-J.; Burch, K.; Smirnov, D.

    The presence of a 2D quantum spin liquid state was recently suggested for the spin-orbit coupled Mott insulator α-RuCl3 with a honeycomb lattice.[Phys. Rev. 90, 041112 (2014)] Optical spectroscopy, Raman scattering, specific heat as well as magnetic susceptibility measurements on α-RuCl3 identified elementary excitations due to electronic correlations and spin-orbit coupling.[arXiv:1503.07593, Phys. Rev. Letters 114, 147201 (2015), and Phys. Rev. 91, 144420 (2015)] These observations appear to be consistent with theoretical expectations for Heisenberg-Kitaev model for QSL.[Phys. Rev. 91, 241110 (2015)] The underlying mechanism for the unconventional magnetism in α-RuCl3 was further investigated by probing the effect of external magnetic field on the Raman spectroscopic signatures. Raman scattering experiments were performed at temperatures down to 5 K and magnetic fields up to 10 T. The intensity of strongest A1g phonon was found to decrease with increasing magnetic field strength suggesting the presence of strong magnetic interactions. The experimental observations and its implications will be presented. Current Affiliation: Florida A and M University.

  4. [Study on the characters of phytoplankton chlorophyll fluorescence excitation spectra based on fourth-derivative].

    PubMed

    Lu, Lu; Su, Rong-Guo; Wang, Xiu-Lin; Zhu, Chen-Jian

    2007-11-01

    Chlorophyll fluorescence excitation spectra of six phytoplankton species, belonging to Bacillariophyta and Dinophyta, were dealt by fourth-derivative analysis with the Matlab program. The results show that between 350 nm and 550 nm six fluorescence peaks were found in the fourth-derivative spectra, which are representatives of non-pigments, chlorophylls and carotenoides respectively. The method makes Bacillariophyta and Dinophyta more distinguishable when the fourth-derivative spectra are compared with the chlorophyll fluorescence excitation spectra. It can be used not only to discriminate the two groups of algaes, but also to reduce the effect of noise. The fluorescence peaks in the fourth-derivative spectra are proved to be stable.

  5. Spin-wave excitations induced by spin current in spin-valve structures

    NASA Astrophysics Data System (ADS)

    Liu, Haoliang; Sun, Dali; Zhang, Chuang; Groesbeck, Matthew; Vardeny, Zeev Valy; Department of Physics; Astronomy, University of Utah, Salt Lake City, Utah 84112, USA Team

    2016-03-01

    We have investigated the magnetization dynamics of NiFe/Pt/Co spin-valve structures with different Pt layer thickness, using a broadband ferromagnetic resonance (FMR) and Brillouin light scattering (BLS) at ambient temperature. We found that the Gilbert damping factor, α of the two ferromagnetic (FM) layer films in the spin-valve structure are significantly larger than α of each individual FM layer. We interpret the increase in α in the spin-valve configuration as due to an interaction between the FM layers mediated by the induced spin current through the Pt interlayer when FMR conditions are met for one of the FM. This was verified by BLS of the spin-valve structure, in which the magnons density in the adjacent FM layer is enhanced upon FMR of the other FM layer. We have studied this spin-current-mediated interaction as a function of the Pt interlayer. Work supported by the MURI-AFOSR Grant FA9550-14-1-0037, and the UofU facility center supported by NSF-MRSEC Grant DMR-1121252.

  6. Resolution of heterogeneous fluorescence into component decay-associated excitation spectra. Application to subtilisins.

    PubMed

    Willis, K J; Szabo, A G; Drew, J; Zuker, M; Ridgeway, J M

    1990-02-01

    Direct and indirect methods are described to combine steady-state and picosecond time-resolved fluorescence decay data to generate decay-associated excitation spectra. The heterogeneous fluorescence from a fluorophore mixture that models protein fluorescence was resolved into individual component excitation spectra. The two methods were also used to determine the excitation spectra associated with each of the decay time components for the proteins subtilisin Carlsberg and BPN'. On the basis of associated spectra, the decay components of both proteins were assigned to individual (or groups of) emitting species. The two approaches used to generate the decay-associated excitation spectra are compared and their general application to protein fluorescence studies is discussed. PMID:2180489

  7. Dipole approximation in the L2,3 electron excited spectra in 3d transition metals

    NASA Astrophysics Data System (ADS)

    Nuroh, K.

    2008-12-01

    A theoretical model based on the autoionization and characteristic decay processes following electron impact ionization of a core electron in solids that has previously been used in calculating electron-energy-loss spectra of transition metals near the 3p -excitation edge has been extended to the 2p -excitation edge for S21c through N27i as well. In the first set of calculations, magnetic effects were ignored and the relative scattering intensity was formulated in terms of the electrostatic interaction U(p,d) between the 3p and 3d electrons of the intermediate resonant configuration state p5dn+1 , using many-body perturbation theory that led to a generalized Fano-type formula for the intensity profiles. In the second set of calculations in which magnetic effects were included as well, an analysis based on the Bethe-Born formalism of inelastic scattering of electrons on atoms was used. The nature of the relative magnitudes of U(p,d) and the spin-orbit parameters ς3p and ς3d and the localized nature of the 3p state necessitated the diagonalization of the intermediate configuration state p5dn+1 to determine the multiplet splitting and their corresponding intensities in the LS -coupling limit using fractional parentage scheme. The nonrelativistic multiconfiguration Hartree-Fock (MCHF) code was used in determining the ground and continuum state wave functions, and the itinerant 3d states in the solid were approximated with an atomic MCHF-wave function. The outline above is applied to the 2p -excitation edge, except that because of the relative magnitudes of U(p,d) , ς2p , and ς3d , it is found that LK coupling is suitable for Sc, Ti, and V, while jK coupling is appropriate for Cr to Ni when it comes to the diagonalization of the configuration p5dn+1 to determine the multiplet splitting and their associated scattering intensities. In the dipole approximation, the scattering intensities separate into two distinct manifolds that arise from the p3/2 and p1/2 states. The

  8. Spin-orbit inversion of excited heavy quark mesons

    SciTech Connect

    Nathan Isgur

    1997-06-01

    The mesonic heavy quark spin multiplets with s{sub l}{sup {pi}{sub l}}=(1/2){sup +} and (3/2){sup +} are expected to be the lowest-lying excitations about the pseudoscalar and vector ground states with s{sub l}{sup {pi}{sub l}}=(1/2){sup {minus}}. The author shows that for charm and bottom these multiplets are probably inverted, with the 2{sup +} and 1{sup +} states with s{sub l}{sup {pi}{sup l}}=(3/2){sup +} about 150 MeV below the 1{sup +} and 0{sup +} states with s{sub l}{sup {pi}{sub l}}=(1/2){sup +}. If verified, such an inversion would both support the expectation that confinement has no dynamical spin-dependence and indicate that heavy and light quark systems may be characterized by the same effective low-energy degrees of freedom. As an important byproduct, this work establishes the dynamics of the strange quark as a critical link between heavy- and light-quark hadrons, justifying efforts toward a much more complete experimental and theoretical understanding of strange mesons and baryons and of strangeonia.

  9. Excitation Spectra of Nucleobases with Multiconfigurational Density Functional Theory.

    PubMed

    Hubert, Mickaël; Jensen, Hans Jørgen Aa; Hedegård, Erik D

    2016-01-14

    Range-separated hybrid methods between wave function theory and density functional theory (DFT) can provide high-accuracy results, while correcting some of the inherent flaws of both the underlying wave function theory and DFT. We here assess the accuracy for excitation energies of the nucleobases thymine, uracil, cytosine, and adenine, using a hybrid between complete active space self-consistent field (CASSCF) and DFT methods. The method is based on range separation, thereby avoiding all double-counting of electron correlation and is denoted long-range CASSCF short-range DFT (CAS-srDFT). Using a linear response extension of CAS-srDFT, we compare the first 7-8 excited states of the nucleobases with perturbative multireference approaches as well as coupled cluster based methods. Our results show that the CAS-srDFT method can provide accurate excitation energies in good correspondence with the computationally more expensive methods. PMID:26669578

  10. Modeling energy-loss spectra due to phonon excitation

    NASA Astrophysics Data System (ADS)

    Forbes, B. D.; Allen, L. J.

    2016-07-01

    We discuss a fundamental theory of how to calculate the phonon-loss sector of the energy-loss spectrum for electrons scattering from crystalline solids. A correlated model for the atomic motion is used for calculating the vibrational modes. Spectra are calculated for crystalline silicon illuminated by a plane wave and by an atomic-scale focused coherent probe, in which case the spectra depend on probe position. These spectra are also affected by the size of the spectrometer aperture. The correlated model is contrasted with the Einstein model in which atoms in the specimen are assumed to vibrate independently. We also discuss how both the correlated and Einstein models relate to a classical view of the energy-loss process.

  11. Theoretical formalism for collective spin-wave edge excitations in arrays of dipolarly interacting magnetic nanodots

    NASA Astrophysics Data System (ADS)

    Lisenkov, Ivan; Tyberkevych, Vasyl; Nikitov, Sergey; Slavin, Andrei

    2016-06-01

    A general theory of collective spin-wave edge modes in semi-infinite and finite periodic arrays of magnetic nanodots having uniform dynamic magnetization (macrospin approximation) is developed. The theory is formulated using a formalism of multivectors of magnetization dynamics, which allows one to study edge modes in arrays having arbitrarily complex primitive cells and lattice structure. The developed formalism can describe spin-wave edge modes localized both at the physical edges of the array and at the internal "domain walls" separating the array regions existing in different static magnetization states. Using a perturbation theory, in the framework of the developed formalism, it is possible to calculate damping of the edge modes and to describe their excitation by external variable magnetic fields. The theory is illustrated on the following practically important examples: (i) calculation of the FMR absorption in a finite nanodot array having the shape of a right triangle; (ii) calculation of the spectra of nonreciprocal spin-wave edge modes, including the modes at the physical edges of an array and modes at the domain walls inside the array; and (iii) study of the influence of the domain wall modes on the FMR spectrum of an array existing in a nonideal chessboard antiferromagnetic ground state.

  12. Laser-excited fluorescence spectra of atomic uranium

    SciTech Connect

    Wang Songyue; Jin Changtai; Shen Mingtao; Wang Xiulan

    1987-05-01

    Using a dc-supply hollow-cathode lamp as a source of uranium vapor and a rhodamine 6G dye laser to excite the vapor optically, it was simple and convenient to detect fluorescence from uranium atoms at 753.393, 763.175, and 763.954 nm. We give a detailed discussion of how we eliminated the intense background emissions, which were principally due to the lamp.

  13. Separation and complete analyses of the overlapped and unresolved 1H NMR spectra of enantiomers by spin selected correlation experiments.

    PubMed

    Prabhu, Uday Ramesh; Baishya, Bikash; Suryaprakash, N

    2008-06-26

    NMR spectroscopic discrimination of optical enantiomers is most often carried out using (2)H and (13)C spectra of chiral molecules aligned in a chiral liquid crystalline solvent. The use of proton NMR for such a purpose is severely hindered due to the spectral complexity and the significant loss of resolution arising from numerous short- and long-distance couplings and the indistinguishable overlap of spectra from both R and S enantiomers. The determination of all the spectral parameters by the analyses of such intricate NMR spectra poses challenges, such as, unraveling of the resonances for each enantiomer, spectral resolution, and simplification of the multiplet pattern. The present study exploits the spin state selection achieved by the two-dimensional (1)H NMR correlation of selectively excited isolated coupled spins (Soft-COSY) of the molecules to overcome these problems. The experiment provides the relative signs and magnitudes of all of the proton-proton couplings, which are otherwise not possible to determine from the broad and featureless one-dimensional (1)H spectra. The utilization of the method for quantification of enantiomeric excess has been demonstrated. The studies on different chiral molecules, each having a chiral center, whose spectral complexity increases with the increasing number of interacting spins, and the advantages and limitations of the method over SERF and DQ-SERF experiments have been reported in this work.

  14. Spinon excitation spectra of the J1-J2 chain from analytical calculations in the dimer basis and exact diagonalization

    NASA Astrophysics Data System (ADS)

    Lavarélo, Arthur; Roux, Guillaume

    2014-10-01

    The excitation spectrum of the frustrated spin-1/2 Heisenberg chain is reexamined using variational and exact diagonalization calculations. We show that the overlap matrix of the short-range resonating valence bond states basis can be inverted which yields tractable equations for single and two spinons excitations. Older results are recovered and new ones, such as the bond-state dispersion relation and its size with momentum at the Majumdar-Ghosh point are found. In particular, this approach yields a gap opening at J 2 = 0.25 J 1 and an onset of incommensurability in the dispersion relation at J 2 = 9/17 J 1 as in [S. Brehmer et al., J. Phys.: Condens. Matter 10, 1103 (1998)]. These analytical results provide a good support for the understanding of exact diagonalization spectra, assuming an independent spinons picture.

  15. Quantum spin excitations through the metal-to-insulator crossover in YBa2Cu3O6+y

    SciTech Connect

    Li, Shiliang; Yamani, Zahra; Kang, H. J.; Segawa, Kouji; Ando, Y.; Yao, Xin; Mook Jr, Herbert A; Dai, Pengcheng

    2008-01-01

    We use inelastic neutron scattering to study the temperature dependence of the spin excitations of a detwinned superconducting YBa{sub 2}Cu{sub 3}O{sub 6.45} ({Tc}=48 K). In contrast to earlier work on YBa{sub 2}Cu{sub 3}O{sub 6.5} ({Tc}=58 K), where the prominent features in the magnetic spectra consist of a sharp collective magnetic excitation termed 'resonance' and a large ({Dirac_h}{omega}{approx}15 meV) superconducting spin gap, we find that the spin excitations in YBa{sub 2}Cu{sub 3}O{sub 6.45} are gapless and have a much broader resonance. Our detailed mapping of magnetic scattering along the a*/b*-axis directions at different energies reveals that spin excitations are unisotropic and consistent with the 'hourglass-like' dispersion along the a*-axis direction near the resonance, but they are isotropic at lower energies. Since a fundamental change in the low-temperature normal state of YBa{sub 2}Cu{sub 3}O{sub 6+y} when superconductivity is suppressed takes place at y{approx}0.5 with a metal-to-insulator crossover (MIC), where the ground state transforms from a metallic to an insulating-like phase, our results suggest a clear connection between the large change in spin excitations and the MIC. The resonance therefore is a fundamental feature of metallic ground state superconductors and a consequence of high-{Tc} superconductivity.

  16. Nuclear Spin Orientation Dependence of Magnetoconductance: A New Method for Measuring the Spin of Charged Excitations in the QHE

    SciTech Connect

    Bowers, C.R.; Reno, J.L.; Simmons, J.A.; Vitkalov, S.A.

    1998-12-01

    A new method for measuring the spin of the electrically charged ground state excitations m the Q$j~j quantum Hall effect ia proposed and demonstmted for the tirst time in GaAs/AIGaAs nndtiquantum wells. The method is &sed on the nuclear spin orientation dependence of" the 2D dc conductivity y in the quantum Hall regime due to the nuclear hyperfine interaction. As a demonstration of this method the spin of the electrically charged excitations of the ground state is determined at filling factor v = 1.

  17. Dual fluorescence excitation spectra of methyl salicylate in a free jet

    NASA Astrophysics Data System (ADS)

    Heimbrook, Lou Ann; Kenny, Jonathan E.; Kohler, Bryan E.; Scott, Gary W.

    1981-11-01

    Separate fluorescence excitation spectra of the blue- and UV-emitting forms of methyl salicylate cooled in a free-jet expansion are reported. This study represents the first observation of the detailed vibrational structure of these transitions. The two excitation spectra have no features in common, and their intensity patterns are very different. Many individual lines are ˜2 cm-1 wide (nearly laser limited), although in the excitation spectrum of the UV emission, spectral congestion persists at high energies despite the high degree of cooling. (AIP)

  18. Nonclassical properties of coherent states and excited coherent states for continuous spectra

    NASA Astrophysics Data System (ADS)

    Honarasa, G. R.; Tavassoly, M. K.; Hatami, M.; Roknizadeh, R.

    2011-02-01

    Based on the definition of coherent states for continuous spectra and analogous to photon-added coherent states for discrete spectra, we introduce the excited coherent states for continuous spectra. It is shown that the main axioms of Gazeau-Klauder coherent states will be satisfied, properly. Nonclassical properties and quantum statistics of coherent states, as well as the introduced excited coherent states, are discussed. In particular, through the study of quadrature squeezing and amplitude-squared squeezing, it will be observed that both classes of the above states can be classified in the intelligent states category.

  19. Solid-state proton NMR of paramagnetic metal complexes: DANTE spin echoes for selective excitation in inhomogeneously broadened lines

    NASA Astrophysics Data System (ADS)

    Carnevale, Diego; Perez Linde, A. J.; Bauer, Gerald; Bodenhausen, Geoffrey

    2013-08-01

    The paramagnetic complex bis(oxazolinylphenyl)amine-Fe(III)Cl2 is investigated by means of solid-state proton NMR at 18.8 T (800 MHz) using magic-angle spinning at 65 kHz. Spin echoes that are excited and refocused by combs of rotor-synchronized pulses in the manner of 'Delays Alternating with Nutation for Tailored Excitation' (DANTE) allow one to characterize different chemical environments that severely overlap in conventional MAS spectra. Such sequences combine two apparently contradictory features: an overall bandwidth exceeding several MHz, and very selective irradiation of a few kHz within inhomogeneously broadened sidebands. The experimental hyperfine interactions correlate well with DFT calculations.

  20. Stripe phase and double-roton excitations in interacting spin-orbit-coupled spin-1 Bose-Einstein condensates

    NASA Astrophysics Data System (ADS)

    Sun, Kuei; Qu, Chunlei; Xu, Yong; Zhang, Yongping; Zhang, Chuanwei

    Spin-orbit (SO) coupling plays a major role in many important phenomena in condensed matter physics. However, the SO coupling physics in high-spin systems, especially with superfluids, has not been well explored because of the spin half of electrons in solids. In this context, the recent experimental realization of spin-orbit coupling in spin-1 Bose-Einstein condensates (BECs) has opened a completely new avenue for exploring SO-coupled high-spin superfluids. Nevertheless, the experiment has only revealed the single-particle physics of the system. Here, we study the effects of interactions between atoms on the ground states and collective excitations of SO-coupled spin-1 BECs in the presence of a spin-tensor potential. We find that ferromagnetic interaction between atoms can induce a stripe phase exhibiting two modulating patterns. We characterize the phase transitions between different phases using the spin-tensor density as well as the collective dipole motion of the BEC. We show that there exists a new type of double maxon-roton structure in the Bogoliubov-excitation spectrum, attributing to the three band minima of the SO-coupled spin-1 BEC. Our work could motivate further theoretical and experimental study along this direction.

  1. Pressure dependence of donor excitation spectra in AlSb

    SciTech Connect

    Hsu, L.; McCluskey, M.D.; Haller, E.E.

    2002-01-16

    We have investigated the behavior of ground to bound excited-state electronic transitions of Se and Te donors in AlSb as a function of hydrostatic pressure. Using broadband far-infrared Fourier transform spectroscopy, we observe qualitatively different behaviors of the electronic transition energies of the two donors. While the pressure derivative of the Te transition energy is small and constant, as might be expected for a shallow donor, the pressure derivatives of the Se transition energies are quadratic and large at low pressures, indicating that Se is actually a deep donor. In addition, at pressures between 30 and 50 kbar, we observe evidence of an anti-crossing between one of the selenium electronic transitions and a two-phonon mode.

  2. Spin-wave excitation and propagation in microstructured waveguides of yttrium iron garnet/Pt bilayers

    SciTech Connect

    Pirro, P.; Chumak, A. V.; Lägel, B.; Leven, B.; Hillebrands, B.; Brächer, T.; Dubs, C.; Surzhenko, O.; Görnert, P.

    2014-01-06

    We present an experimental study of spin-wave excitation and propagation in microstructured waveguides consisting of a 100 nm thick yttrium iron garnet/platinum (Pt) bilayer. The life time of the spin waves is found to be more than an order of magnitude higher than in comparably sized metallic structures, despite the fact that the Pt capping enhances the Gilbert damping. Utilizing microfocus Brillouin light scattering spectroscopy, we reveal the spin-wave mode structure for different excitation frequencies. An exponential spin-wave amplitude decay length of 31 μm is observed which is a significant step towards low damping, insulator based micro-magnonics.

  3. Doping dependence of spin excitations and its correlations with high-temperature superconductivity in iron pnictides.

    PubMed

    Wang, Meng; Zhang, Chenglin; Lu, Xingye; Tan, Guotai; Luo, Huiqian; Song, Yu; Wang, Miaoyin; Zhang, Xiaotian; Goremychkin, E A; Perring, T G; Maier, T A; Yin, Zhiping; Haule, Kristjan; Kotliar, Gabriel; Dai, Pengcheng

    2013-01-01

    High-temperature superconductivity in iron pnictides occurs when electrons and holes are doped into their antiferromagnetic parent compounds. Since spin excitations may be responsible for electron pairing and superconductivity, it is important to determine their electron/hole-doping evolution and connection with superconductivity. Here we use inelastic neutron scattering to show that while electron doping to the antiferromagnetic BaFe₂As₂ parent compound modifies the low-energy spin excitations and their correlation with superconductivity (<50 meV) without affecting the high-energy spin excitations (>100 meV), hole-doping suppresses the high-energy spin excitations and shifts the magnetic spectral weight to low-energies. In addition, our absolute spin susceptibility measurements for the optimally hole-doped iron pnictide reveal that the change in magnetic exchange energy below and above T(c) can account for the superconducting condensation energy. These results suggest that high-T(c) superconductivity in iron pnictides is associated with both the presence of high-energy spin excitations and a coupling between low-energy spin excitations and itinerant electrons.

  4. Observations of thermally excited ferromagnetic resonance on spin torque oscillators having a perpendicularly magnetized free layer

    SciTech Connect

    Tamaru, S. Kubota, H.; Yakushiji, K.; Konoto, M.; Nozaki, T.; Fukushima, A.; Imamura, H.; Taniguchi, T.; Arai, H.; Tsunegi, S.; Yuasa, S.; Suzuki, Y.

    2014-05-07

    Measurements of thermally excited ferromagnetic resonance were performed on spin torque oscillators having a perpendicularly magnetized free layer and in-plane magnetized reference layer (abbreviated as PMF-STO in the following) for the purpose of obtaining magnetic properties in the PMF-STO structure. The measured spectra clearly showed a large main peak and multiple smaller peaks on the high frequency side. A Lorentzian fit on the main peak yielded Gilbert damping factor of 0.0041. The observed peaks moved in proportion to the out-of-plane bias field. From the slope of the main peak frequency as a function of the bias field, Lande g factor was estimated to be about 2.13. The mode intervals showed a clear dependence on the diameter of the PMF-STOs, i.e., intervals are larger for a smaller diameter. These results suggest that the observed peaks should correspond to eigenmodes of lateral spin wave resonance in the perpendicularly magnetized free layer.

  5. Resonant optical control of the electrically induced spin polarization by periodic excitation

    NASA Astrophysics Data System (ADS)

    Hernandez, F. G. G.; Gusev, G. M.; Bakarov, A. K.

    2014-07-01

    We show that the electron spin polarization generated by an electrical current may have its direction controlled and magnitude amplified by periodic optical excitation. The electrical and optical spin control methods were combined and implemented in a two-dimensional electron gas. By Kerr rotation in an external transverse magnetic field, we demonstrate unexpected long-lived coherent spin oscillations of the current-induced signal in a system with large spin-orbit interaction. Using a single linearly polarized pulse for spin manipulation and detection, we found a strong dependence on the pulse optical power and sample temperature indicating the relevance of the hole spin in the electron spin initialization. The signal was mapped in a Hall bar as function of the position relative to the injection contact. Finally, the presence of an in-plane spin polarization was directly verified by rotating the experimental geometry.

  6. Low-energy electrodynamics of novel spin excitations in the quantum spin ice Yb₂Ti₂O₇.

    PubMed

    Pan, LiDong; Kim, Se Kwon; Ghosh, A; Morris, Christopher M; Ross, Kate A; Kermarrec, Edwin; Gaulin, Bruce D; Koohpayeh, S M; Tchernyshyov, Oleg; Armitage, N P

    2014-09-18

    In condensed matter systems, formation of long-range order (LRO) is often accompanied by new excitations. However, in many geometrically frustrated magnetic systems, conventional LRO is suppressed, while non-trivial spin correlations are still observed. A natural question to ask is then what is the nature of the excitations in this highly correlated state without broken symmetry? Frequently, applying a symmetry breaking field stabilizes excitations whose properties reflect certain aspects of the anomalous state without LRO. Here we report a THz spectroscopy study of novel excitations in quantum spin ice Yb2Ti2O7 under a <001> directed magnetic field. At large positive fields, both right- and left-handed magnon and two-magnon-like excitations are observed. The g-factors of these excitations are dramatically enhanced in the low-field limit, showing a crossover of these states into features consistent with the quantum string-like excitations proposed to exist in quantum spin ice in small <001> fields.

  7. Transmission of excitations in a spin-1 Bose-Einstein condensate through a barrier

    SciTech Connect

    Watabe, Shohei; Kato, Yusuke

    2011-05-15

    We investigate tunneling of excitations across a potential barrier separating two spin-1 Bose-Einstein condensates. Using mean-field theory at absolute zero temperature, we determine the transmission coefficients of excitations in the saturated magnetization state and unsaturated magnetization states. All excitations, except the quadrupolar spin mode in the saturated magnetization state, show the anomalous tunneling phenomenon characterized as perfect tunneling in the low-momentum limit through a potential barrier. The quadrupolar spin mode in the saturated magnetization state, whose spectrum is massive, shows total reflection. We discuss properties common between excitations showing the anomalous tunneling phenomenon. Excitations showing perfect tunneling have a gapless spectrum in the absence of the magnetic field, and their wave functions in the low-energy limit are the same as the condensate wave function.

  8. Homodyne-detected ferromagnetic resonance of in-plane magnetized nanocontacts: Composite spin-wave resonances and their excitation mechanism

    NASA Astrophysics Data System (ADS)

    Fazlali, Masoumeh; Dvornik, Mykola; Iacocca, Ezio; Dürrenfeld, Philipp; Haidar, Mohammad; Åkerman, Johan; Dumas, Randy K.

    2016-04-01

    This work provides a detailed investigation of the measured in-plane field-swept homodyne-detected ferromagnetic resonance (FMR) spectra of an extended Co/Cu/NiFe pseudo-spin-valve stack using a nanocontact (NC) geometry. The magnetodynamics are generated by a pulse-modulated microwave current, and the resulting rectified dc mixing voltage, which appears across the NC at resonance, is detected using a lock-in amplifier. Most notably, we find that the measured spectra of the NiFe layer are composite in nature and highly asymmetric, consistent with the broadband excitation of multiple modes. Additionally, the data must be fit with two Lorentzian functions in order to extract a reasonable value for the Gilbert damping of the NiFe. Aided by micromagnetic simulations, we conclude that (i) for in-plane fields the rf Oersted field in the vicinity of the NC plays the dominant role in generating the observed spectra, (ii) in addition to the FMR mode, exchange-dominated spin waves are also generated, and (iii) the NC diameter sets the mean wave vector of the exchange-dominated spin wave, in good agreement with the dispersion relation.

  9. Optimization of 1H spin density for dynamic nuclear polarization using photo-excited triplet electron spins.

    PubMed

    Kagawa, Akinori; Murokawa, Yu; Takeda, Kazuyuki; Kitagawa, Masahiro

    2009-03-01

    In dynamic nuclear polarization (DNP) using photo-excited triplet electron spins, known as Microwave-Induced Optical Nuclear Polarization (MIONP), the attainable (1)H polarization is determined by the ratio of the buildup rate and the spin-lattice relaxation rate, in turn depend on the (1)H spin density. It is shown that the final (1)H polarization can be enhanced by diluting the (1)H spins with partial deuteration. The DNP experiments are demonstrated in 0.05 mol% pentacene-doped p-terphenyl for various (1)H abundances. It is also shown that the (1)H spin diffusion coefficient can be determined by examining the initial buildup rate of (1)H polarization for various repetition rates of the DNP sequence.

  10. Excitation spectra and correlation functions of quantum Su-Schrieffer-Heeger models

    NASA Astrophysics Data System (ADS)

    Weber, Manuel; Assaad, Fakher F.; Hohenadler, Martin

    2015-06-01

    We study one-dimensional Su-Schrieffer-Heeger (SSH) models with quantum phonons using a continuous-time quantum Monte Carlo method. Within statistical errors, we obtain identical results for the SSH model with acoustic phonons, and a related model with a coupling to an optical bond phonon mode. Based on this agreement, we first study the Peierls metal-insulator transition of the spinless SSH model, and relate it to the Kosterlitz-Thouless transition of a spinless Luttinger liquid. In the Peierls phase, the spectral functions reveal the single-particle and charge gap, and a central peak related to long-range order. For the spinful SSH model, which has a dimerized ground state for any nonzero coupling, we reveal a symmetry-related degeneracy of spin and charge excitations, and the expected spin and charge gaps as well as a central peak. Finally, we study the SSH-U V model with electron-phonon and electron-electron interaction. We observe a Mott phase with critical spin and bond correlations at weak electron-phonon coupling, and a Peierls phase with gapped spin excitations at strong coupling. We relate our findings to the extended Hubbard model, and discuss the physical origin of the agreement between optical and acoustic phonons.

  11. Investigation of the spectra of luminescence and Raman scattering in water and chlorophyll "a" excited by femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Biryukova, Yu. S.; Ilyin, A. A.; Golik, S. S.; Mayor, A. Y.

    2015-11-01

    The Raman spectra of femtosecond laser pulses in distilled and tap water, and luminescence spectra of aqueous solutions containing dissolved organic matter, chlorophyll "a" and biological objects excited by ultra-short laser pulses was investigated.

  12. Spin excitations in systems with hopping electron transport and strong position disorder in a large magnetic field.

    PubMed

    Shumilin, A V

    2016-10-01

    We discuss the spin excitations in systems with hopping electron conduction and strong position disorder. We focus on the problem in a strong magnetic field when the spin Hamiltonian can be reduced to the effective single-particle Hamiltonian and treated with conventional numerical technics. It is shown that in a 3D system with Heisenberg exchange interaction the spin excitations have a delocalized part of the spectrum even in the limit of strong disorder, thus leading to the possibility of the coherent spin transport. The spin transport provided by the delocalized excitations can be described by a diffusion coefficient. Non-homogenous magnetic fields lead to the Anderson localization of spin excitations while anisotropy of the exchange interaction results in the Lifshitz localization of excitations. We discuss the possible effect of the additional exchange-driven spin diffusion on the organic spin-valve devices. PMID:27484892

  13. Spin excitations in systems with hopping electron transport and strong position disorder in a large magnetic field

    NASA Astrophysics Data System (ADS)

    Shumilin, A. V.

    2016-10-01

    We discuss the spin excitations in systems with hopping electron conduction and strong position disorder. We focus on the problem in a strong magnetic field when the spin Hamiltonian can be reduced to the effective single-particle Hamiltonian and treated with conventional numerical technics. It is shown that in a 3D system with Heisenberg exchange interaction the spin excitations have a delocalized part of the spectrum even in the limit of strong disorder, thus leading to the possibility of the coherent spin transport. The spin transport provided by the delocalized excitations can be described by a diffusion coefficient. Non-homogenous magnetic fields lead to the Anderson localization of spin excitations while anisotropy of the exchange interaction results in the Lifshitz localization of excitations. We discuss the possible effect of the additional exchange-driven spin diffusion on the organic spin-valve devices.

  14. Spin dynamics of an individual Cr atom in a semiconductor quantum dot under optical excitation

    NASA Astrophysics Data System (ADS)

    Lafuente-Sampietro, A.; Utsumi, H.; Boukari, H.; Kuroda, S.; Besombes, L.

    2016-08-01

    We studied the spin dynamics of a Cr atom incorporated in a II-VI semiconductor quantum dot using photon correlation techniques. We used recently developed singly Cr-doped CdTe/ZnTe quantum dots to access the spin of an individual magnetic atom. Auto-correlation of the photons emitted by the quantum dot under continuous wave optical excitation reveals fluctuations of the localized spin with a timescale in the 10 ns range. Cross-correlation gives quantitative transfer time between Cr spin states. A calculation of the time dependence of the spin levels population in Cr-doped quantum dots shows that the observed spin dynamics is dominated by the exciton-Cr interaction. These measurements also provide a lower bound in the 20 ns range for the intrinsic Cr spin relaxation time.

  15. Fluorescence, Absorption, and Excitation Spectra of Polycyclic Aromatic Hydrocarbons as a Tool for Quantitative Analysis

    ERIC Educational Resources Information Center

    Rivera-Figueroa, A. M.; Ramazan, K. A.; Finlayson-Pitts, B. J.

    2004-01-01

    A quantitative and qualitative study of the interplay between absorption, fluorescence, and excitation spectra of pollutants called polycyclic aromatic hydrocarbons (PAHs) is conducted. The study of five PAH displays the correlation of the above-mentioned properties along with the associated molecular changes.

  16. Discernment of lint trash in raw cotton using multivariate analysis of excitation-emission luminescence spectra

    Technology Transfer Automated Retrieval System (TEKTRAN)

    Excitation-Emission luminescence spectra of basic (pH 12.5) phosphate buffer solution extracts were used to distinguish among botanical components of trash within seed cotton. All components were separated from whole plants removed from a field in southern New Mexico. Unfolded Principal Component An...

  17. Microwave excitation of spin wave beams in thin ferromagnetic films

    PubMed Central

    Gruszecki, P.; Kasprzak, M.; Serebryannikov, A. E.; Krawczyk, M.; Śmigaj, W.

    2016-01-01

    An inherent element of research and applications in photonics is a beam of light. In magnonics, which is the magnetic counterpart of photonics, where spin waves are used instead of electromagnetic waves to transmit and process information, the lack of a beam source limits exploration. Here, we present an approach enabling generation of narrow spin wave beams in thin homogeneous nanosized ferromagnetic films by microwave current. We show that the desired beam-type behavior can be achieved with the aid of a properly designed coplanar waveguide transducer generating a nonuniform microwave magnetic field. We test this idea using micromagnetic simulations, confirming numerically that the resulting spin wave beams propagate over distances of several micrometers. The proposed approach requires neither inhomogeneity of the ferromagnetic film nor nonuniformity of the biasing magnetic field. It can be generalized to different magnetization configurations and yield multiple spin wave beams of different width at the same frequency. PMID:26971711

  18. Predicting the spin state of paramagnetic iron complexes by DFT calculation of proton NMR spectra.

    PubMed

    Borgogno, Andrea; Rastrelli, Federico; Bagno, Alessandro

    2014-07-01

    Many transition-metal complexes easily change their spin state S in response to external perturbations (spin crossover). Determining such states and their dynamics can play a central role in the understanding of useful properties such as molecular magnetism or catalytic behavior, but is often far from straightforward. In this work we demonstrate that, at a moderate computational cost, density functional calculations can predict the correct ground spin state of Fe(ii) and Fe(iii) complexes and can then be used to determine the (1)H NMR spectra of all spin states. Since the spectral features are remarkably different according to the spin state, calculated (1)H NMR resonances can be used to infer the correct spin state, along with supporting the structure elucidation of numerous paramagnetic complexes.

  19. Antiferromagnetic spin excitations in single crystals of nonsuperconducting Li$_{1-x}$FeAs

    SciTech Connect

    Wang, Meng; Wang, X.C.; Harriger, Leland W; Luo, H.Q.; Zhao, Yang; Lynn, J. W.; Liu, Q.Q.; Jin, C.Q.; Fang, Chen; Hu, Jiangping; Dai, Pengcheng

    2011-01-01

    We use neutron scattering to determine spin excitations in single crystals of nonsuperconducting Li1 xFeAs throughout the Brillouin zone. Although angle resolved photoemission experiments and local density approximation calculations suggest poor Fermi surface nesting conditions for antiferromagnetic (AF) order, spin excitations in Li1 xFeAs occur at the AF wave vectors Q = (1,0) at low energies, but move to wave vectors Q = ( 0.5, 0.5) near the zone boundary with a total magnetic bandwidth comparable to that of BaFe2As2. These results reveal that AF spin excitations still dominate the low-energy physics of these materials and suggest both itinerancy and strong electron-electron correlations are essential to understand the measured magnetic excitations.

  20. Excitations in a spin-polarized two-dimensional electron gas

    NASA Astrophysics Data System (ADS)

    Kreil, Dominik; Hobbiger, Raphael; Drachta, Jürgen T.; Böhm, Helga M.

    2015-11-01

    A remarkably long-lived spin plasmon may exist in two-dimensional electron liquids with imbalanced spin-up and spin-down population. The predictions for this interesting mode by Agarwal et al. [Phys. Rev. B 90, 155409 (2014), 10.1103/PhysRevB.90.155409] are based on the random phase approximation. Here, we show how to account for spin-dependent correlations from known ground-state pair correlation functions and study the consequences on the various spin-dependent longitudinal response functions. The spin-plasmon dispersion relation and its critical wave vector for Landau damping by minority spins turn out to be significantly lower. We further demonstrate that spin-dependent effective interactions imply a rich structure in the excitation spectrum of the partially spin-polarized system. Most notably, we find a "magnetic antiresonance," where the imaginary part of both, the spin-spin as well as the density-spin response function vanish. The resulting minimum in the double-differential cross section is awaiting experimental confirmation.

  1. Modification of Optical Properties of Seawater Exposed to Oil Contaminants Based on Excitation-Emission Spectra

    NASA Astrophysics Data System (ADS)

    Baszanowska, E.; Otremba, Z.

    2015-10-01

    The optical behaviour of seawater exposed to a residual amount of oil pollution is presented and a comparison of the fluorescence spectra of oil dissolved in both n-hexane and seawater is discussed based on excitation-emission spectra. Crude oil extracted from the southern part of the Baltic Sea was used to characterise petroleum properties after contact with seawater. The wavelength-independent fluorescence maximum for natural seawater and seawater artificially polluted with oil were determined. Moreover, the specific excitation-emission peaks for natural seawater and polluted water were analysed to identify the natural organic matter composition. It was found that fluorescence spectra identification is a promising method to detect even an extremely low concentration of petroleum residues directly in the seawater. In addition, alien substances disturbing the fluorescence signatures of natural organic substances in a marine environment is also discussed.

  2. Spin excitations in ferromagnetic Ni: Electrons and neutrons as a probe

    SciTech Connect

    Hong, Jisang; Mills, D. L.

    2000-01-01

    We present theoretical calculations of the contribution to the spin polarized electron energy loss spectrum of ferromagnetic Ni. We find, save for the wave-vector transfer near the center of the Brillouin zone, the spin-wave loss feature is obscured by low-lying Stoner excitations, in contrast to Fe. Our calculations, and earlier work, show that in inelastic neutron-scattering studies of spin waves in Ni, the spin-wave loss peak dominates. The physical reason for this difference is discussed. (c) 2000 The American Physical Society.

  3. Spin-vibronic quantum dynamics for ultrafast excited-state processes.

    PubMed

    Eng, Julien; Gourlaouen, Christophe; Gindensperger, Etienne; Daniel, Chantal

    2015-03-17

    Ultrafast intersystem crossing (ISC) processes coupled to nuclear relaxation and solvation dynamics play a central role in the photophysics and photochemistry of a wide range of transition metal complexes. These phenomena occurring within a few hundred femtoseconds are investigated experimentally by ultrafast picosecond and femtosecond transient absorption or luminescence spectroscopies, and optical laser pump-X-ray probe techniques using picosecond and femtosecond X-ray pulses. The interpretation of ultrafast structural changes, time-resolved spectra, quantum yields, and time scales of elementary processes or transient lifetimes needs robust theoretical tools combining state-of-the-art quantum chemistry and developments in quantum dynamics for solving the electronic and nuclear problems. Multimode molecular dynamics beyond the Born-Oppenheimer approximation has been successfully applied to many small polyatomic systems. Its application to large molecules containing a transition metal atom is still a challenge because of the nuclear dimensionality of the problem, the high density of electronic excited states, and the spin-orbit coupling effects. Rhenium(I) α-diimine carbonyl complexes, [Re(L)(CO)3(N,N)](n+) are thermally and photochemically robust and highly flexible synthetically. Structural variations of the N,N and L ligands affect the spectroscopy, the photophysics, and the photochemistry of these chromophores easily incorporated into a complex environment. Visible light absorption opens the route to a wide range of applications such as sensors, probes, or emissive labels for imaging biomolecules. Halide complexes [Re(X)(CO)3(bpy)] (X = Cl, Br, or I; bpy = 2,2'-bipyridine) exhibit complex electronic structure and large spin-orbit effects that do not correlate with the heavy atom effects. Indeed, the (1)MLCT → (3)MLCT intersystem crossing (ISC) kinetics is slower than in [Ru(bpy)3](2+) or [Fe(bpy)3](2+) despite the presence of a third-row transition metal

  4. Correlations between metal spin states and vibrational spectra of a trinuclear Fe(II) complex exhibiting spin crossover

    NASA Astrophysics Data System (ADS)

    Gerasimova, Tatiana P.; Katsyuba, Sergey A.; Lavrenova, Ludmila G.; Pelmenschikov, Vladimir; Kaupp, Martin

    2015-12-01

    Combined IR spectroscopic/quantum-chemical analysis of a 4-propyl-1,2,4-triazole trinuclear Fe(II) complex capable of reversible thermal spin crossover has revealed mid-IR bands of the ligand sensitive to the Fe(II) spin state. The character of the correlations found between the intensity and peak position of the triazole bands and the spin state of the metal center depends neither on the identity of the metal nor on the nuclearity of the complex. The found spectral correlations therefore allow analysis of various similar complexes. This is illustrated by the example of experimental IR spectra reported earlier for Fe(II), Co(II), Ni(II), Cu(II) and Zn(II) complexes with triazole ligands. Quantum-chemical IR spectral simulations further suggest that certain ligand bands vary between the states with the same total molecular spin, but different distribution of the spin density between the metal centers. However these variations are too subtle to discriminate between the spin transitions of the central and peripheral Fe(II) ions. The experimentally revealed mid-IR markers are therefore conclusive only for the total molecular spin.

  5. Lifetime-vibrational interference effects in resonantly excited x-ray emission spectra of CO

    SciTech Connect

    Skytt, P.; Glans, P.; Gunnelin, K.

    1997-04-01

    The parity selection rule for resonant X-ray emission as demonstrated for O{sub 2} and N{sub 2} can be seen as an effect of interference between coherently excited degenerate localized core states. One system where the core state degeneracy is not exact but somewhat lifted was previously studied at ALS, namely the resonant X-ray emission of amino-substituted benzene (aniline). It was shown that the X-ray fluorescence spectrum resulting from excitation of the C1s at the site of the {open_quotes}aminocarbon{close_quotes} could be described in a picture separating the excitation and the emission processes, whereas the spectrum corresponding to the quasi-degenerate carbons could not. Thus, in this case it was necessary to take interference effects between the quasi-degenerate intermediate core excited states into account in order to obtain agreement between calculations and experiment. The different vibrational levels of core excited states in molecules have energy splittings which are of the same order of magnitude as the natural lifetime broadening of core excitations in the soft X-ray range. Therefore, lifetime-vibrational interference effects are likely to appear and influence the band shapes in resonant X-ray emission spectra. Lifetime-vibrational interference has been studied in non-resonant X-ray emission, and in Auger spectra. In this report the authors discuss results of selectively excited soft X-ray fluorescence spectra of molecules, where they focus on lifetime-interference effects appearing in the band shapes.

  6. Tunable short-wavelength spin wave excitation from pinned magnetic domain walls.

    PubMed

    Van de Wiele, Ben; Hämäläinen, Sampo J; Baláž, Pavel; Montoncello, Federico; van Dijken, Sebastiaan

    2016-02-17

    Miniaturization of magnonic devices for wave-like computing requires emission of short-wavelength spin waves, a key feature that cannot be achieved with microwave antennas. In this paper, we propose a tunable source of short-wavelength spin waves based on highly localized and strongly pinned magnetic domain walls in ferroelectric-ferromagnetic bilayers. When driven into oscillation by a microwave spin-polarized current, the magnetic domain walls emit spin waves with the same frequency as the excitation current. The amplitude of the emitted spin waves and the range of attainable excitation frequencies depend on the availability of domain wall resonance modes. In this respect, pinned domain walls in magnetic nanowires are particularly attractive. In this geometry, spin wave confinement perpendicular to the nanowire axis produces a multitude of domain wall resonances enabling efficient spin wave emission at frequencies up to 100 GHz and wavelengths down to 20 nm. At high frequency, the emission of spin waves in magnetic nanowires becomes monochromatic. Moreover, pinning of magnetic domain wall oscillators onto the same ferroelectric domain boundary in parallel nanowires guarantees good coherency between spin wave sources, which opens perspectives towards the realization of Mach-Zehnder type logic devices and sensors.

  7. Tunable short-wavelength spin wave excitation from pinned magnetic domain walls

    PubMed Central

    Van de Wiele, Ben; Hämäläinen, Sampo J.; Baláž, Pavel; Montoncello, Federico; van Dijken, Sebastiaan

    2016-01-01

    Miniaturization of magnonic devices for wave-like computing requires emission of short-wavelength spin waves, a key feature that cannot be achieved with microwave antennas. In this paper, we propose a tunable source of short-wavelength spin waves based on highly localized and strongly pinned magnetic domain walls in ferroelectric-ferromagnetic bilayers. When driven into oscillation by a microwave spin-polarized current, the magnetic domain walls emit spin waves with the same frequency as the excitation current. The amplitude of the emitted spin waves and the range of attainable excitation frequencies depend on the availability of domain wall resonance modes. In this respect, pinned domain walls in magnetic nanowires are particularly attractive. In this geometry, spin wave confinement perpendicular to the nanowire axis produces a multitude of domain wall resonances enabling efficient spin wave emission at frequencies up to 100 GHz and wavelengths down to 20 nm. At high frequency, the emission of spin waves in magnetic nanowires becomes monochromatic. Moreover, pinning of magnetic domain wall oscillators onto the same ferroelectric domain boundary in parallel nanowires guarantees good coherency between spin wave sources, which opens perspectives towards the realization of Mach-Zehnder type logic devices and sensors. PMID:26883893

  8. Isotropic Spin Trap EPR Spectra Simulation by Fast Fourier Transform (FFT)

    NASA Astrophysics Data System (ADS)

    Laachir, S.; Moussetad, M.; Adhiri, R.; Fahli, A.

    2005-03-01

    The detection and investigation of free radicals forming in living systems became possible due to the introduction of the method of spin traps. In this work, the electron spin resonance (ESR) spectra of DMPO/HO(.) and MGD-Fe-NO adducts are reproduced by simulation, based on the Fast Fourier Transform (FFT). The calculated spectral parameters as the hyperfine coupling constants, agree reasonably with the experimental data and the results are discussed.

  9. Crossover from spin waves to diffusive spin excitations in underdoped Ba(Fe1-xCox)2 As2

    SciTech Connect

    Tucker, G S; Fernandes, R M; Pratt, D K; Thaler, A; Ni, N; Marty, K; Christianson, A D; Lumsden, M D; Sales, B C; Sefat, A S; Bud'ko, S L; Canfield, P C; Kreyssig, A; Goldman, A I; McQueeney, R J

    2014-05-01

    Using inelastic neutron scattering, we show that the onset of superconductivity in underdoped Ba(Fe1-xCox)2As2 coincides with a crossover from well-defined spin waves to overdamped and diffusive spin excitations. This crossover occurs despite the presence of long-range stripe antiferromagnetic order for samples in a compositional range from x=0.04 to 0.055, and is a consequence of the shrinking spin-density wave gap and a corresponding increase in the particle-hole (Landau) damping. The latter effect is captured by a simple itinerant model relating Co doping to changes in the hot spots of the Fermi surface. We argue that the overdamped spin fluctuations provide a pairing mechanism for superconductivity in these materials.

  10. Mass-number and excitation-energy dependence of the spin cutoff parameter

    NASA Astrophysics Data System (ADS)

    Grimes, S. M.; Voinov, A. V.; Massey, T. N.

    2016-07-01

    The spin cutoff parameter determining the nuclear level density spin distribution ρ (J ) is defined through the spin projection as 1 /2 or equivalently for spherical nuclei, ( 3 ) 1 /2. It is needed to divide the total level density into levels as a function of J . To obtain the total level density at the neutron binding energy from the s -wave resonance count, the spin cutoff parameter is also needed. The spin cutoff parameter has been calculated as a function of excitation energy and mass with a super-conducting Hamiltonian. Calculations have been compared with two commonly used semiempirical formulas. A need for further measurements is also observed. Some complications for deformed nuclei are discussed. The quality of spin cut off parameter data derived from isomeric ratio measurement is examined.

  11. Cotunneling spectroscopy and the properties of excited-state spin manifolds of Mn12 single molecule magnets

    NASA Astrophysics Data System (ADS)

    Rostamzadeh Renani, Fatemeh; Kirczenow, George

    2014-10-01

    We study charge transport through single molecule magnet (SMM) junctions in the cotunneling regime as a tool for investigating the properties of the excited-state manifolds of neutral Mn12 SMs. This study is motivated by a recent transport experiment [S. Kahle et al., Nano Lett. 12, 518 (2012), 10.1021/nl204141z] that probed the details of the magnetic and electronic structure of Mn12 SMMs beyond the ground-state spin manifold. A giant spin Hamiltonian and master equation approach is used to explore theoretically the cotunneling transport through Mn12-Ac SMM junctions. We identify SMM transitions that can account for both the strong and weak features of the experimental differential conductance spectra. We find the experimental results to imply that the excited spin-state manifolds of the neutral SMM have either different anisotropy constants or different g factors in comparison with its ground-state manifold. However, the latter scenario accounts best for the experimental data.

  12. Distribution of tempo-dichlorotriazine spin label on immunoglobulin molecule. Interpretation of ESR spectra

    SciTech Connect

    Nezlin, R.

    1986-03-05

    Spin label TEMPO-dichlorotriazine (DT) has been used previously for determination of the rotational relaxation times of immunoglobulin (Ig) molecules and evaluation of their flexibility. Well defined outer wide extrema as well as sharp inner extrema are characteristic for ESR spectra of spin labeled Ig molecules. Such patterns of the spectrum can be accounted for either by the existence of the spin label in two states, one corresponding to its rapid and another to its restricted rotation or by varying environments of the spin label located in different areas of the Ig molecule. To choose between these possibilities, the distribution of /sup 14/C-TEMPO-DT on human IgG1(k) was studied. The same amount of the label per mg of protein was found in H and L chains as well as in the Fab fragment, and a smaller amount in the pFc'. The label was detected in most of the L chain tryptic peptides. Thus, the spin label is distributed nearly uniformly on IgG molecule, which is due to the regular distribution of amino acid residues reacted with the spin label. ESR spectra can be interpreted as a sum of individual spectra.

  13. The commensurate spin excitation in chromium: A polarised neutron investigation

    SciTech Connect

    Pynn, R. ); Stirling, W.G. . Dept. of Physics); Severing, A. )

    1991-01-01

    A polarised neutron experiment with neutron energy analysis has been performed with a single-Q sample of chromium in a large magnetic field. The 4-meV commensurate'' mode is found to involve spin fluctuations parallel to the ordered chromium moments. 8 refs., 3 figs.

  14. Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols

    SciTech Connect

    Lee, Hyun Ji; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A.

    2013-05-10

    Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of SOA generated from two monoterpenes, limonene and a-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ~100 ppb ammonia vapor in air saturated with water vapor. Absorption and excitation-emission matrix (EEM) spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (~0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for excitation = 420+- 50 nm and emission = 475 +- 38 nm. The window of the strongest fluorescence shifted to excitation = 320 +- 25 nm and emission = 425 +- 38 nm for the a-pinene-derived SOA. Both regions overlap with the excitation-emission matrix (EEM) spectra of some of the fluorophores found in primary biological aerosols. Our study suggests that, despite the low quantum yield, the aged SOA particles should have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.

  15. Observing spin excitations in 3 d transition-metal adatoms on Pt(111) with inelastic scanning tunneling spectroscopy: A first-principles perspective

    NASA Astrophysics Data System (ADS)

    Schweflinghaus, Benedikt; dos Santos Dias, Manuel; Lounis, Samir

    2016-01-01

    Spin excitations in atomic-scale nanostructures have been investigated with inelastic scanning tunneling spectroscopy, sometimes with conflicting results. In this work, we present a theoretical viewpoint on a recent experimental controversy regarding the spin excitations of Co adatoms on Pt(111). While one group [Balashov et al., Phys. Rev. Lett. 102, 257203 (2009), 10.1103/PhysRevLett.102.257203] claims to have detected them, another group reported their observation only after the hydrogenation of the Co adatom [Dubout et al., Phys. Rev. Lett. 114, 106807 (2015), 10.1103/PhysRevLett.114.106807]. Utilizing time-dependent density functional theory in combination with many-body perturbation theory, we demonstrate that, although inelastic spin excitations are possible for Cr, Mn, Fe, and Co adatoms, their efficiency differs. While the excitation signature is less pronounced for Mn and Co adatoms, it is larger for Cr and Fe adatoms. We find that the tunneling matrix elements or the tunneling cross-section related to the nature and symmetry of the relevant electronic states are more favorable for triggering the spin excitations in Fe than in Co. An enhancement of the tunneling and of the inelastic spectra is possible by attaching hydrogen to the adatom at the appropriate position.

  16. Incoherent excitation and switching of spin states in exciton-polariton condensates

    NASA Astrophysics Data System (ADS)

    Li, G.; Liew, T. C. H.; Egorov, O. A.; Ostrovskaya, E. A.

    2015-08-01

    We investigate, theoretically and numerically, the spin dynamics of a two-component exciton-polariton condensate created and sustained by nonresonant spin-polarized optical pumping in a semiconductor microcavity. Using the open-dissipative mean-field model, we show that the existence of well defined phase-locked steady states of the condensate may lead to efficient switching and control of spin (polarization) states with a nonresonant excitation. Spatially inhomogeneous pulsed excitations can cause symmetry breaking in the pseudospin structure of the condensate and lead to formation of nontrivial spin textures. Our model is universally applicable to two linearly coupled polariton condensates, and therefore can also describe the behavior of condensate populations and phases in "double-well" type potentials.

  17. Direct observation of dynamic modes excited in a magnetic insulator by pure spin current

    PubMed Central

    Demidov, V. E.; Evelt, M.; Bessonov, V.; Demokritov, S. O.; Prieto, J. L.; Muñoz, M.; Ben Youssef, J.; Naletov, V. V.; de Loubens, G.; Klein, O.; Collet, M.; Bortolotti, P.; Cros, V.; Anane, A.

    2016-01-01

    Excitation of magnetization dynamics by pure spin currents has been recently recognized as an enabling mechanism for spintronics and magnonics, which allows implementation of spin-torque devices based on low-damping insulating magnetic materials. Here we report the first spatially-resolved study of the dynamic modes excited by pure spin current in nanometer-thick microscopic insulating Yttrium Iron Garnet disks. We show that these modes exhibit nonlinear self-broadening preventing the formation of the self-localized magnetic bullet, which plays a crucial role in the stabilization of the single-mode magnetization oscillations in all-metallic systems. This peculiarity associated with the efficient nonlinear mode coupling in low-damping materials can be among the main factors governing the interaction of pure spin currents with the dynamic magnetization in high-quality magnetic insulators. PMID:27608533

  18. Direct observation of dynamic modes excited in a magnetic insulator by pure spin current

    NASA Astrophysics Data System (ADS)

    Demidov, V. E.; Evelt, M.; Bessonov, V.; Demokritov, S. O.; Prieto, J. L.; Muñoz, M.; Ben Youssef, J.; Naletov, V. V.; de Loubens, G.; Klein, O.; Collet, M.; Bortolotti, P.; Cros, V.; Anane, A.

    2016-09-01

    Excitation of magnetization dynamics by pure spin currents has been recently recognized as an enabling mechanism for spintronics and magnonics, which allows implementation of spin-torque devices based on low-damping insulating magnetic materials. Here we report the first spatially-resolved study of the dynamic modes excited by pure spin current in nanometer-thick microscopic insulating Yttrium Iron Garnet disks. We show that these modes exhibit nonlinear self-broadening preventing the formation of the self-localized magnetic bullet, which plays a crucial role in the stabilization of the single-mode magnetization oscillations in all-metallic systems. This peculiarity associated with the efficient nonlinear mode coupling in low-damping materials can be among the main factors governing the interaction of pure spin currents with the dynamic magnetization in high-quality magnetic insulators.

  19. Direct observation of dynamic modes excited in a magnetic insulator by pure spin current.

    PubMed

    Demidov, V E; Evelt, M; Bessonov, V; Demokritov, S O; Prieto, J L; Muñoz, M; Ben Youssef, J; Naletov, V V; de Loubens, G; Klein, O; Collet, M; Bortolotti, P; Cros, V; Anane, A

    2016-01-01

    Excitation of magnetization dynamics by pure spin currents has been recently recognized as an enabling mechanism for spintronics and magnonics, which allows implementation of spin-torque devices based on low-damping insulating magnetic materials. Here we report the first spatially-resolved study of the dynamic modes excited by pure spin current in nanometer-thick microscopic insulating Yttrium Iron Garnet disks. We show that these modes exhibit nonlinear self-broadening preventing the formation of the self-localized magnetic bullet, which plays a crucial role in the stabilization of the single-mode magnetization oscillations in all-metallic systems. This peculiarity associated with the efficient nonlinear mode coupling in low-damping materials can be among the main factors governing the interaction of pure spin currents with the dynamic magnetization in high-quality magnetic insulators. PMID:27608533

  20. Spin wave excitation in yttrium iron garnet films with micron-sized antennas

    SciTech Connect

    Khivintsev, Y. V. Filimonov, Y. A.; Nikitov, S. A.

    2015-02-02

    In this paper, we explore spin waves excitation in monolithic structures based on yttrium iron garnet (YIG) films with micro-sized antennas. Samples based on plain and patterned YIG film were fabricated and tested for tangential bias field geometries. We observed spin wave excitation and propagation with wave numbers up to 3.5 × 10{sup 4} rad/cm. The corresponding wavelength is thus shorter more than by one order of magnitude compared to previous experiments with such films. For the sample with a periodic array of nanotrenches, we observed the effect of the shape anisotropy resulting in the shift of the spin wave propagation band in comparison to the unpatterned YIG film. Our results are very promising for the exploitation of short spin waves in YIG and provide great opportunity for significant miniaturization of YIG film based microwave devices.

  1. Singlet-to-Triplet Excitations in the Unconventional Spin-Peierls System TiOBr

    SciTech Connect

    Clancy, James P; Gaulin, Bruce D.; Adams, Carl P; Granroth, Garrett E; Kolesnikov, Alexander I; Sherline, Todd E; Chou, F. C.

    2011-01-01

    We have performed time-of-flight neutron scattering measurements on powder samples of the unconventional spin-Peierls compound TiOBr using the fine-resolution Fermi chopper spectrometer (SEQUOIA) at the SNS. These measurements reveal two branches of magnetic excitations within the commensurate and incommensurate spin-Peierls phases, which we associate with n = 1 and n = 2 triplet excitations out of the singlet ground state. These measurements represent the first direct measure of the singlet-triplet energy gap in TiOBr, which is found to have a value of Eg 21 meV.

  2. Kondo screening and spin excitation in few-layer CoPc molecular assembly stacking on Pb(111) surface: A DFT+HEOM study

    NASA Astrophysics Data System (ADS)

    Wang, Yu; Zheng, Xiao; Yang, Jinlong

    2016-10-01

    Transition metal phthalocyanine molecules adsorbed on a metal substrate exhibit rich spin-related phenomena such as magnetic anisotropy, spin excitation, and Kondo effect. In this work, we investigate theoretically few-layer cobalt phthalocyanine (CoPc) molecular assembly stacking on Pb(111) surface with the use of a combined density functional theory (DFT) and hierarchical equations of motion (HEOM) approach. Calculation results indicate that the local spin properties of CoPc/Pb(111) composites depend critically on the number of adsorption layers. The first layer of CoPc on the Pb(111) surface serves as a spin-insulating buffer, while the CoPc molecules in the second layer exhibit spin-1/2 Kondo effect with a Kondo temperature of about 22 K. In a triple-layer CoPc assembly stacking on Pb(111), the antiferromagnetic coupling between the second and third layers leads to local spin-flip excitations under finite bias voltages, which gives rise to characteristic signatures in the differential conductance spectra. The DFT+HEOM approach thus provides a practical means for investigating the local electronic and spin properties of two-dimensional molecular assemblies adsorbed on the metal surface. The insights obtained from the first-principles based simulations could be useful for experimental manipulation or design of magnetic composite systems.

  3. High-spin isomers in 212Rn in the region of triple neutron core-excitations

    NASA Astrophysics Data System (ADS)

    Dracoulis, G. D.; Lane, G. J.; Byrne, A. P.; Davidson, P. M.; Kibédi, T.; Nieminen, P.; Watanabe, H.; Wilson, A. N.

    2008-04-01

    The level scheme of 212Rn has been extended to spins of ∼ 38 ℏ and excitation energies of about 13 MeV using the 204Hg(13C, 5n)212Rn reaction and γ-ray spectroscopy. Time correlated techniques have been used to obtain sensitivity to weak transitions and channel selectivity. The excitation energy of the 22+ core-excited isomer has been established at 6174 keV. Two isomers with τ = 25 (2) ns and τ = 12 (2) ns are identified at 12211 and 12548 keV, respectively. These are the highest-spin nuclear isomers now known, and are attributed to configurations involving triple neutron core-excitations coupled to the aligned valence protons. Semi-empirical shell-model calculations can account for most states observed, but with significant energy discrepancies for some configurations.

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

    SciTech Connect

    Ye, ChuanXiang; Zhao, Yi E-mail: liangwz@xmu.edu.cn; Liang, WanZhen E-mail: liangwz@xmu.edu.cn

    2015-10-21

    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.

  5. Discrimination of nuclear spin isomers exploiting the excited state dynamics of a quinodimethane derivative

    SciTech Connect

    Obaid, Rana; Kinzel, Daniel; Oppel, Markus González, Leticia

    2014-10-28

    Despite the concept of nuclear spin isomers (NSIs) exists since the early days of quantum mechanics, only few approaches have been suggested to separate different NSIs. Here, a method is proposed to discriminate different NSIs of a quinodimethane derivative using its electronic excited state dynamics. After electronic excitation by a laser field with femtosecond time duration, a difference in the behavior of several quantum mechanical operators can be observed. A pump-probe experimental approach for separating these different NSIs is then proposed.

  6. Magnetic order and spin excitations in layered Heisenberg antiferromagnets with compass-model anisotropies

    NASA Astrophysics Data System (ADS)

    Vladimirov, A. A.; Ihle, D.; Plakida, N. M.

    2015-02-01

    The spin-wave excitation spectrum, magnetization, and Néel temperature for the quasi-two-dimensional spin-1/2 antiferromagnetic Heisenberg model with the compass-model interaction in the plane proposed for iridates are calculated in the random phase approximation. The spin-wave spectrum agrees well with data of Lanczos diagonalization. We find that the Néel temperature is enhanced by the compass-model interaction and is close to the experimental value for Ba2IrO4.

  7. Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols.

    PubMed

    Lee, Hyun Ji Julie; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A

    2013-06-01

    Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines, and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of water-soluble SOA generated from two monoterpenes, limonene and α-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ∼100 ppb ammonia in air saturated with water vapor. Absorption and excitation-emission matrix (EEM) spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (∼0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for λexcitation = 420 ± 50 nm and λemission = 475 ± 38 nm. The window of the strongest fluorescence shifted to λexcitation = 320 ± 25 nm and λemission = 425 ± 38 nm for the α-pinene-derived SOA. Both regions overlap with the EEM spectra of some of the fluorophores found in primary biological aerosols. Despite the low quantum yield, the aged SOA particles may have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.

  8. Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes

    DOE PAGES

    Ma, X.; Fang, F.; Li, Q.; Zhu, J.; Yang, Y.; Wu, Y. Z.; Zhao, H. B.; Lüpke, G.

    2015-10-28

    In this study, 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 recoverymore » 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.« less

  9. Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes

    SciTech Connect

    Ma, X.; Fang, F.; Li, Q.; Zhu, J.; Yang, Y.; Wu, Y. Z.; Zhao, H. B.; Lüpke, G.

    2015-10-28

    In this study, 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.

  10. Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes

    PubMed Central

    Ma, X.; Fang, F.; Li, Q.; Zhu, J.; Yang, Y.; Wu, Y. Z.; Zhao, H. B.; Lüpke, G.

    2015-01-01

    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. PMID:26508587

  11. The Role of Spin-Orbit Coupling in the Double-Ionization Photoelectron Spectra of XCN(2+) (X = Cl, Br, and I).

    PubMed

    Manna, Soumitra; Mishra, Sabyashachi

    2016-03-10

    The photoelectron spectra of XCN(2+) (X = Cl, Br, and I) were calculated employing ab initio electronic structure methods with high-level electron correlation and explicit treatment of spin-orbit coupling. Twelve scalar-relativistic excited states of the dicationic systems, calculated from state-averaged CASSCF/MRCI calculations, were used as the electronic basis to evaluate spin-orbit eigenstates. While the spin-orbit effects in ClCN(2+) are found to be negligible, the electronic spectroscopy of BrCN(2+) and ICN(2+) is significantly influenced by interstate spin-orbit coupling. Several electronic degeneracies are lifted, and many unexpected accidental degeneracies occurred due to the spin-orbit coupling. In particular, the spin-orbit interactions between X̃ (3)Σ(-)-b̃ (1)Σ(+), Ã (3)Π-c̃ (1)Π, B̃ (3)Δ-ã (1)Δ, and C̃ (3)Σ(+)-d̃ (1)Σ(-) are found to be strong in BrCN(2+) and ICN(2+). By careful analysis of the effect of spin-orbit coupling parameters and the spin-orbit eigenstate composition, an assignment of the hitherto unidentified experimental photoelectron bands of BrCN(2+) and ICN(2+) is presented.

  12. Spin correlations and spin-wave excitations in Dirac-Weyl semimetals

    NASA Astrophysics Data System (ADS)

    Araki, Yasufumi; Nomura, Kentaro

    We study correlations among magnetic dopants in three-dimensional Dirac and Weyl semimetals. Effective field theory for localized magnetic moments is derived by integrating out the itinerant electron degrees of freedom. We find that spin correlation in the spatial direction parallel to local magnetization is more rigid than that in the perpendicular direction, reflecting spin-momentum locking nature of the Dirac Hamiltonian. Such an anisotropy becomes stronger for Fermi level close to the Dirac points, due to Van Vleck paramagnetism triggered by spin-orbit coupling. One can expect topologically nontrivial spin textures under this anisotropy, such as a hedgehog around a single point, or a radial vortex around an axis, as well as a uniform ferromagnetic order. We further investigate the characteristics of spin waves in the ferromagnetic state. Spin-wave dispersion also shows a spatial anisotropy, which is less dispersed in the direction transverse to the magnetization than that in the longitudinal direction. The spin-wave dispersion anisotropy can be traced back to the rigidity and flexibility of spin correlations discussed above. This work was supported by Grant-in-Aid for Scientific Research (Grants No.15H05854, No.26107505, and No.26400308) from the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan.

  13. Prediction of nitroxide spin label EPR spectra from MD trajectories: application to myoglobin.

    PubMed

    Kuprusevicius, Egidijus; White, Gaye; Oganesyan, Vasily S

    2011-01-01

    We report the prediction of motional EPR spectra of the metalloprotein sperm whale myoglobin spin labelled with nitroxide directly from Molecular Dynamics (MD) simulations at the atomistic scale. We show that an accurate simulation of EPR spectra can be achieved from a single MD trajectory which is in excellent agreement with experiment. Simulations have been carried out using a general method reported previously by us for the simulation of EPR spectra form single dynamical trajectories. Our calculations demonstrate the complex nature of the dynamics of a spin label which is a superposition of the fast librational motions around dihedral states, of slow conformational flips among different rotameric states and of the slow rotational diffusion of the protein itself. The MD-EPR methodology reported does not require any additional stochastic modelling using adjustable parameters and opens, for the first time, the prospect of the simulation of EPR spectra entirely from single MD trajectories. Such a technique not only simplifies the interpretation and analysis of EPR spectra but also opens the possibility, for example, of "computer engineering" of spin-labelled proteins with the desired properties prior to actual EPR experiment. PMID:21322490

  14. Detection of pure inverse spin-Hall effect induced by spin pumping at various excitation

    NASA Astrophysics Data System (ADS)

    Inoue, H. Y.; Harii, K.; Ando, K.; Sasage, K.; Saitoh, E.

    2007-10-01

    Electric-field generation due to the inverse spin-Hall effect (ISHE) driven by spin pumping was detected and separated experimentally from the extrinsic magnetogalvanic effects in a Ni81Fe19/Pt film. By applying a sample-cavity configuration in which the extrinsic effects are suppressed, the spin pumping using ferromagnetic resonance gives rise to a symmetric spectral shape in the electromotive force spectrum, indicating that the motive force is due entirely to ISHE. This method allows the quantitative analysis of the ISHE and the spin-pumping effect. The microwave-power dependence of the ISHE amplitude is consistent with the prediction of a direct current-spin-pumping scenario.

  15. Parametric excitation in a magnetic tunnel junction-based spin torque oscillator

    SciTech Connect

    Dürrenfeld, P.; Iacocca, E.; Åkerman, J.; Muduli, P. K.

    2014-02-03

    Using microwave current injection at room temperature, we demonstrate parametric excitation of a magnetic tunnel junction (MTJ)-based spin-torque oscillator (STO). Parametric excitation is observed for currents below the auto-oscillation threshold, when the microwave current frequency f{sub e} is twice the STO free-running frequency f{sub 0}. Above threshold, the MTJ becomes parametrically synchronized. In the synchronized state, the STO exhibits an integrated power up to 5 times higher and a linewidth reduction of two orders of magnitude, compared to free-running conditions. We also show that the parametric synchronization favors single mode oscillations in the case of multimode excitation.

  16. Properties of the first excited state of nonbipartite Heisenberg spin rings

    NASA Astrophysics Data System (ADS)

    Schnack, J.

    2000-12-01

    Systematic properties of the first excited state are presented for various ring sizes and spin quantum numbers which are only partly covered by the theorem of Lieb, Schultz, and Mattis. For odd ring sizes the first excited energy eigenvalue shows unexpected degeneracy and related shift quantum numbers. As a byproduct the ground state energy as well as the energy of the first excited state of infinite chains are calculated by extrapolating the properties of only a few, finite, antiferromagnetically coupled Heisenberg rings using the powerful Levin sequence acceleration method.

  17. Cumulant approach for electronic excitations in x-ray and electron spectra

    NASA Astrophysics Data System (ADS)

    Rehr, J. J.

    A quantitative treatment of electronic excitations and other many-body effects in x-ray and electron spectra has long been challenging. Physically, electronic correlations and atomic vibrations lead to inelastic losses and damping effects that are ignored in ground state methods or approximations such as TDDFT. Quasi-particle (QP) approaches such as the GW approximation yield significant improvements, as demonstrated in real-space Green's function and GW/Bethe-Salpeter equation calculations, but still ignore multi-electron excitations. Recently such excitations have been treated with considerable success using cumulant expansion techniques and the quasi-boson approximation. In this beyond QP approach, excitations such as plasmons and electron-hole excitations appear as satellites in the spectral function. The method naturally accounts for multiple-satellites and can be extended to include extrinsic losses and interference effects. Extensions for effects of vibrations and strong correlations including charge-transfer satellites may also be possible. These advances are illustrated with a number of applications. Supported by DOE Grant DE-FG02-97ER45623.

  18. Excitation of propagating spin waves in ferromagnetic nanowires by microwave voltage-controlled magnetic anisotropy.

    PubMed

    Verba, Roman; Carpentieri, Mario; Finocchio, Giovanni; Tiberkevich, Vasil; Slavin, Andrei

    2016-01-01

    The voltage-controlled magnetic anisotropy (VCMA) effect, which manifests itself as variation of anisotropy of a thin layer of a conductive ferromagnet on a dielectric substrate under the influence of an external electric voltage, can be used for the development of novel information storage and signal processing devices with low power consumption. Here it is demonstrated by micromagnetic simulations that the application of a microwave voltage to a nanosized VCMA gate in an ultrathin ferromagnetic nanowire results in the parametric excitation of a propagating spin wave, which could serve as a carrier of information. The frequency of the excited spin wave is twice smaller than the frequency of the applied voltage while its amplitude is limited by 2 mechanisms: (i) the so-called "phase mechanism" described by the Zakharov-L'vov-Starobinets "S-theory" and (ii) the saturation mechanism associated with the nonlinear frequency shift of the excited spin wave. The developed extension of the "S-theory", which takes into account the second limitation mechanism, allowed us to estimate theoretically the efficiency of the parametric excitation of spin waves by the VCMA effect. PMID:27113392

  19. Excitation of propagating spin waves in ferromagnetic nanowires by microwave voltage-controlled magnetic anisotropy

    NASA Astrophysics Data System (ADS)

    Verba, Roman; Carpentieri, Mario; Finocchio, Giovanni; Tiberkevich, Vasil; Slavin, Andrei

    2016-04-01

    The voltage-controlled magnetic anisotropy (VCMA) effect, which manifests itself as variation of anisotropy of a thin layer of a conductive ferromagnet on a dielectric substrate under the influence of an external electric voltage, can be used for the development of novel information storage and signal processing devices with low power consumption. Here it is demonstrated by micromagnetic simulations that the application of a microwave voltage to a nanosized VCMA gate in an ultrathin ferromagnetic nanowire results in the parametric excitation of a propagating spin wave, which could serve as a carrier of information. The frequency of the excited spin wave is twice smaller than the frequency of the applied voltage while its amplitude is limited by 2 mechanisms: (i) the so-called “phase mechanism” described by the Zakharov-L’vov-Starobinets “S-theory” and (ii) the saturation mechanism associated with the nonlinear frequency shift of the excited spin wave. The developed extension of the “S-theory”, which takes into account the second limitation mechanism, allowed us to estimate theoretically the efficiency of the parametric excitation of spin waves by the VCMA effect.

  20. Excitation of propagating spin waves in ferromagnetic nanowires by microwave voltage-controlled magnetic anisotropy

    PubMed Central

    Verba, Roman; Carpentieri, Mario; Finocchio, Giovanni; Tiberkevich, Vasil; Slavin, Andrei

    2016-01-01

    The voltage-controlled magnetic anisotropy (VCMA) effect, which manifests itself as variation of anisotropy of a thin layer of a conductive ferromagnet on a dielectric substrate under the influence of an external electric voltage, can be used for the development of novel information storage and signal processing devices with low power consumption. Here it is demonstrated by micromagnetic simulations that the application of a microwave voltage to a nanosized VCMA gate in an ultrathin ferromagnetic nanowire results in the parametric excitation of a propagating spin wave, which could serve as a carrier of information. The frequency of the excited spin wave is twice smaller than the frequency of the applied voltage while its amplitude is limited by 2 mechanisms: (i) the so-called “phase mechanism” described by the Zakharov-L’vov-Starobinets “S-theory” and (ii) the saturation mechanism associated with the nonlinear frequency shift of the excited spin wave. The developed extension of the “S-theory”, which takes into account the second limitation mechanism, allowed us to estimate theoretically the efficiency of the parametric excitation of spin waves by the VCMA effect. PMID:27113392

  1. Spin excitations of ferronematic order in underdoped cuprate superconductors.

    PubMed

    Seibold, G; Di Castro, C; Grilli, M; Lorenzana, J

    2014-01-01

    High-temperature superconductors exhibit a characteristic hourglass-shaped spectrum of magnetic fluctuations which most likely contribute to the pairing glue in the cuprates. Recent neutron scattering experiments in strongly underdoped compounds have revealed a significant low energy anisotropy of these fluctuations which we explain by a model in which topological defects of the antiferromagnet clump to producing domain wall segments with ferronematic order. This state does not invoke global charge order but breaks C4 rotational and inversion symmetry. The incommensurability of the low doping charge-disordered state is in good agreement with experiment and interpolates smoothly with the incommensurability of the stripe phase at higher doping. Within linear spin-wave theory the dynamic structure factor is in very good agreement with inelastic neutron scattering data and can account for the observed energy dependent anisotropy. PMID:24936723

  2. Spin excitations of ferronematic order in underdoped cuprate superconductors

    PubMed Central

    Seibold, G.; Di Castro, C.; Grilli, M.; Lorenzana, J.

    2014-01-01

    High-temperature superconductors exhibit a characteristic hourglass-shaped spectrum of magnetic fluctuations which most likely contribute to the pairing glue in the cuprates. Recent neutron scattering experiments in strongly underdoped compounds have revealed a significant low energy anisotropy of these fluctuations which we explain by a model in which topological defects of the antiferromagnet clump to producing domain wall segments with ferronematic order. This state does not invoke global charge order but breaks C4 rotational and inversion symmetry. The incommensurability of the low doping charge-disordered state is in good agreement with experiment and interpolates smoothly with the incommensurability of the stripe phase at higher doping. Within linear spin-wave theory the dynamic structure factor is in very good agreement with inelastic neutron scattering data and can account for the observed energy dependent anisotropy. PMID:24936723

  3. Detection of nanoscale electron spin resonance spectra demonstrated using nitrogen-vacancy centre probes in diamond

    PubMed Central

    Hall, L. T.; Kehayias, P.; Simpson, D. A.; Jarmola, A.; Stacey, A.; Budker, D.; Hollenberg, L. C. L.

    2016-01-01

    Electron spin resonance (ESR) describes a suite of techniques for characterizing electronic systems with applications in physics, chemistry, and biology. However, the requirement for large electron spin ensembles in conventional ESR techniques limits their spatial resolution. Here we present a method for measuring ESR spectra of nanoscale electronic environments by measuring the longitudinal relaxation time of a single-spin probe as it is systematically tuned into resonance with the target electronic system. As a proof of concept, we extracted the spectral distribution for the P1 electronic spin bath in diamond by using an ensemble of nitrogen-vacancy centres, and demonstrated excellent agreement with theoretical expectations. As the response of each nitrogen-vacancy spin in this experiment is dominated by a single P1 spin at a mean distance of 2.7 nm, the application of this technique to the single nitrogen-vacancy case will enable nanoscale ESR spectroscopy of atomic and molecular spin systems. PMID:26728001

  4. Critical excitation spectrum of a quantum chain with a local three-spin coupling

    SciTech Connect

    McCabe, John F.; Wydro, Tomasz

    2011-09-15

    Using the phenomenological renormalization group (PRG), we evaluate the low-energy excitation spectrum along the critical line of a quantum spin chain having a local interaction between three Ising spins and longitudinal and transverse magnetic fields, i.e., a Turban model. The low-energy excitation spectrum found with the PRG agrees with the spectrum predicted for the (D{sub 4},A{sub 4}) conformal minimal model under a nontrivial correspondence between translations at the critical line and discrete lattice translations. Under this correspondence, the measurements confirm a prediction that the critical line of this quantum spin chain and the critical point of the two-dimensional three-state Potts model are in the same universality class.

  5. Ultrafast spin-transfer torque driven by femtosecond pulsed-laser excitation

    NASA Astrophysics Data System (ADS)

    Koopmans, Bert

    A hot topic in the field of ultrafast laser-induced manipulation of the magnetic state is that of the role and exploitation of laser-induced spin currents. Intense debate has been triggered by claims that such a spin-transfer, e.g. in the form of super-diffusive spin currents over tens of nanometers, might be a main contributor to the demagnetization process in ferromagnetic thin films after femtosecond laser excitation. In this presentation the underlying concepts will be introduced and recent developments reviewed. Particularly we demonstrate the possibility to apply a laser-induced spin transfer torque on a free magnetic layer, using a non-collinear multilayer configuration consisting of a free in-plane layer on top of a perpendicularly magnetized injection layer, as separated by a nonmagnetic spacer. Interestingly, this approach allows for a quantitative measurement of the amount of spin transfer. Moreover, it might provide access to novel device architectures in which the magnetic state is controlled by fs laser pulses. Careful analysis of the resulting precession of the free layer allows us to quantify the applied torque, and distinguish between driving mechanisms based on laser-induced transfer of hot electrons versus a spin Seebeck effect due to the large thermal gradients. Further engineering of the layered structures in order to gain fundamental understanding and optimize efficiencies will be reported. A simple model that treats local non-equilibrium magnetization dynamics to spin transport effects via a spin-dependent chemical potential will be introduced.

  6. Magnetic excitations and anomalous spin-wave broadening in multiferroic FeV2O4

    SciTech Connect

    Zhang, Qiang; Ramazanoglu, Mehmet; Chi, Songxue; Liu, Yong; Lograsso, Thomas A.; Vaknin, David

    2014-06-01

    We report on the different roles of two orbital-active Fe2+ at the A site and V3+ at the B site in the magnetic excitations and on the anomalous spin-wave broadening in FeV2O4. FeV2O4 exhibits three structural transitions and successive paramagnetic (PM)–collinear ferrimagnetic (CFI)–noncollinear ferrimagnetic (NCFI)/ferroelectric transitions. The high-temperature tetragonal/PM–orthorhombic/CFI transition is accompanied by the appearance of a large energy gap in the magnetic excitations due to strong spin-orbit-coupling-induced anisotropy at the Fe2+ site. While there is no measurable increase in the energy gap from the orbital ordering of V3+ at the orthorhombic/CFI–tetragonal/NCFI transition, anomalous spin-wave broadening is observed in the orthorhombic/CFI state due to V3+ spin fluctuations at the B site. The spin-wave broadening is also observed at the zone boundary without softening in the NCFI/ferroelectric phase, which is discussed in terms of magnon-phonon coupling. Our study also indicates that the Fe2+ spins without the frustration at the A site may not play an important role in inducing ferroelectricity in the tetragonal/NCFI phase of FeV2O4.

  7. Excited state mass spectra of doubly heavy baryons {Ω _{cc}}, {Ω _{bb}}, and {Ω _{bc}}

    NASA Astrophysics Data System (ADS)

    Shah, Zalak; Thakkar, Kaushal; Rai, Ajay Kumar

    2016-10-01

    We discuss the mass spectrum of Ω baryon with two heavy quarks and one light quark ( ccs, bbs, and bcs). The main goal of the paper is to calculate the ground state masses and after that, the positive and negative parity excited states masses are also obtained within a hypercentral constituent quark model, using Coulomb plus linear potential framework. We also added a first order correction to the potential. The mass spectra up to 5S for radial excited states and 1P-5P, 1D-4D, and 1F-2F states for orbital excited states are computed for Ω _{cc}, Ω _{bb}, and Ω _{bc} baryons. Our obtained results are compared with other theoretical predictions, which could be a useful complementary tool for the interpretation of experimentally unknown heavy baryon spectra. The Regge trajectory is constructed in both the (n_r, M2) and the ( J, M2) planes for Ω _{cc}, Ω _{bb}, and Ω _{bc} baryons and their slopes and intercepts are also determined. Magnetic moments of doubly heavy Ω 's are also calculated.

  8. Excitation and emission spectra of rubidium in rare-gas thin-films

    SciTech Connect

    Gerhardt, Ilja; Sin, Kyungseob; Momose, Takamasa

    2012-07-07

    To understand the optical properties of atoms in solid state matrices, the absorption, excitation, and emission spectra of rubidium doped thin-films of argon, krypton, and xenon were investigated in detail. A two-dimensional spectral analysis extends earlier reports on the excitation and emission properties of rubidium in rare-gas hosts. We found that the doped crystals of krypton and xenon exhibit a simple absorption-emission relation, whereas rubidium in argon showed more complicated spectral structures. Our sample preparation employed in the present work yielded different results for the Ar crystal, but our peak positions were consistent with the prediction based on the linear extrapolation of Xe and Kr data. We also observed a bleaching behavior in rubidium excitation spectra, which suggests a population transfer from one to another spectral feature due to hole-burning. The observed optical response implies that rubidium in rare-gas thin-films is detectable with extremely high sensitivity, possibly down to a single atom level, in low concentration samples.

  9. Tracking the charge and spin dynamics of electronic excited states in inorganic complexes

    NASA Astrophysics Data System (ADS)

    Gaffney, Kelly

    2015-03-01

    Inorganic complexes have many advantageous properties for solar energy applications, including strong visible absorption and photocatalytic activity. Whether used as a photocatalyst or a photosensitizer, the lifetime of electronic excited states and the earth abundance of the molecular components represent a key property for solar energy applications. These dual needs have undermined the usefulness of many coordination compounds. Isoelectronic iron and ruthenium based complexes represent a clear example. Ru-polypyridal based molecules have been the workhorse of solar energy related research and dye sensitized solar cells for decades, but the replacement of low abundance Ru with Fe leads to million-fold reductions in metal to ligand charge transfer (MLCT) excited state lifetimes. Understanding the origin of this million-fold reduction in lifetime and how to control excited state relaxation in 3d-metal complexes motivates the work I will discuss. We have used the spin sensitivity of hard x-ray fluorescence spectroscopy and the intense femtosecond duration pulses generated by the LCLS x-ray laser to probe the spin dynamics in a series of electronically excited [Fe(CN)6-2N(2,2'-bipyridine)N]2 N - 4 complexes, with N = 1-3. These femtosecond resolution measurements demonstrate that modification of the solvent and ligand environment can lengthen the MLCT excited state lifetime by more than two orders of magnitude. They also verify the role of triplet ligand field excited states in the spin crossover dynamics from singlet to quintet spin configurations. Work supported by the AMOS program within the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy.

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

    PubMed

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

    2016-08-01

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

  11. Quasidegenerate scaled opposite spin second order perturbation corrections to single excitation configuration interaction

    NASA Astrophysics Data System (ADS)

    Casanova, David; Rhee, Young Min; Head-Gordon, Martin

    2008-04-01

    Scaled opposite spin (SOS) second order perturbative corrections to single excitation configuration interaction (CIS) are extended to correctly treat quasidegeneracies between excited states. Two viable methods, termed as SOS-CIS(D0) and SOS-CIS(D1), are defined, implemented, and tested. Each involves one empirical parameter (plus a second for the SOS-MP2 ground state), has computational cost that scales with the fourth power of molecule size, and has storage requirements that are cubic, with only quantities of the rank of single excitations produced and stored during iterations. Tests on a set of low-lying adiabatic valence excitation energies and vertical Rydberg excitations of organic and inorganic molecules show that the empirical parameter can be acceptably transferred from the corresponding nondegenerate perturbation theories without any further fitting. Further tests on higher excited states show that the new methods correctly perform for surface crossings for which nondegenerate approaches fail. Numerical results show that SOS-CIS(D0) appears to treat Rydberg excitations in a more balanced way than SOS-CIS(D1) and is, therefore, likely to be the preferred approach. It should be useful for exploring excited state geometries, transition structures, and conical intersections for states of medium to large organic molecules that are dominated by single excitations.

  12. Magnetic phase transitions and monopole excitations in spin ice under uniaxial pressure: A Monte Carlo simulation

    SciTech Connect

    Xie, Y. L. Yan, Z. B.; Liu, J.-M.; Lin, L.

    2015-05-07

    In this work, we explore the spin ice model under uniaxial pressure using the Monte Carlo simulation method. For the known spin ices, the interaction correction (δ) introduced by the uniaxial pressure varies in quite a wide range from positive to negative. When δ is positive, the ground state characterized by the ferromagnetic spin chains is quite unstable, and in real materials it serves as intermediate state connecting the ice state and the long range ordered dipolar spin ice ground state. In the case of negative δ, the system relaxes from highly degenerate ice state to ordered ferromagnetic state via a first order phase transition. Furthermore, the domain walls in such ferromagnetic state are the hotbed of the excitations of magnetic monopoles, thus indicating that the uniaxial pressure can greatly increase the monopole density.

  13. Predicting Near Edge X-ray Absorption Spectra with the Spin-Free Exact-Two-Component Hamiltonian and Orthogonality Constrained Density Functional Theory.

    PubMed

    Verma, Prakash; Derricotte, Wallace D; Evangelista, Francesco A

    2016-01-12

    Orthogonality constrained density functional theory (OCDFT) provides near-edge X-ray absorption (NEXAS) spectra of first-row elements within one electronvolt from experimental values. However, with increasing atomic number, scalar relativistic effects become the dominant source of error in a nonrelativistic OCDFT treatment of core-valence excitations. In this work we report a novel implementation of the spin-free exact-two-component (X2C) one-electron treatment of scalar relativistic effects and its combination with a recently developed OCDFT approach to compute a manifold of core-valence excited states. The inclusion of scalar relativistic effects in OCDFT reduces the mean absolute error of second-row elements core-valence excitations from 10.3 to 2.3 eV. For all the excitations considered, the results from X2C calculations are also found to be in excellent agreement with those from low-order spin-free Douglas-Kroll-Hess relativistic Hamiltonians. The X2C-OCDFT NEXAS spectra of three organotitanium complexes (TiCl4, TiCpCl3, TiCp2Cl2) are in very good agreement with unshifted experimental results and show a maximum absolute error of 5-6 eV. In addition, a decomposition of the total transition dipole moment into partial atomic contributions is proposed and applied to analyze the nature of the Ti pre-edge transitions in the three organotitanium complexes.

  14. Data-adaptive unfolding of nuclear excitation spectra: a time-series approach

    NASA Astrophysics Data System (ADS)

    Torres Vargas, G.; Fossion, R.; Velázquez, V.; López Vieyra, J. C.

    2014-03-01

    A common problem in the statistical characterization of the excitation spectrum of quantum systems is the adequate separation of global system-dependent properties from the local fluctuations that are universal. In this process, called unfolding, the functional form to describe the global behaviour is often imposed externally on the data and can introduce arbitrarities in the statistical results. In this contribution, we show that a quantum excitation spectrum can readily be interpreted as a time series, before any previous unfolding. An advantage of the time-series approach is that specialized methods such as Singular Spectrum Analysis (SSA) can be used to perform the unfolding procedure in a data-adaptive way. We will show how SSA separates the components that describe the global properties from the components that describe the local fluctuations. The partial variances, associated with the fluctuations, follow a definite power law that distinguishes between soft and rigid excitation spectra. The data-adaptive fluctuation and trend components can be used to reconstruct customary fluctuation measures without ambiguities or artifacts introduced by an arbitrary unfolding, and also define the global level density of the excitation spectrum. The method is applied to nuclear shell-model calculations for 48Ca, using a realistic force and Two-Body Random Ensemble (TBRE) interactions. We show that the statistical results are very robust against a variation in the parameters of the SSA method.

  15. The D(D3)-anyon chain: integrable boundary conditions and excitation spectra

    NASA Astrophysics Data System (ADS)

    Finch, Peter E.; Frahm, Holger

    2013-05-01

    Chains of interacting non-Abelian anyons with local interactions invariant under the action of the Drinfeld double of the dihedral group D3 are constructed. Formulated as a spin chain the Hamiltonians are generated from commuting transfer matrices of an integrable vertex model for periodic and braided as well as open boundaries. A different anyonic model with the same local Hamiltonian is obtained within the fusion path formulation. This model is shown to be related to an integrable fusion interaction round the face model. Bulk and surface properties of the anyon chain are computed from the Bethe equations for the spin chain. The low-energy effective theories and operator content of the models (in both the spin chain and fusion path formulation) are identified from analytical and numerical studies of the finite-size spectra. For all boundary conditions considered the continuum theory is found to be a product of two conformal field theories. Depending on the coupling constants the factors can be a Z4 parafermion or a {M}_{(5,6)} minimal model.

  16. Electronic excitation spectra from time-dependent density functional response theory using plane-wave methods

    NASA Astrophysics Data System (ADS)

    Doltsinis, Nikos L.; Sprik, Michiel

    2000-11-01

    The time-dependent density functional response theory method for the computation of electronic excitation spectra has been implemented in a plane-wave basis set/pseudo-potential formalism. We compare our test results for N2 and H2CO to literature atomic basis set calculations and find good agreement. We also discuss some of the technical complications specific to the use of plane-wave basis sets. As an application, the thermally broadened photoabsorption spectrum of formamide at room temperature is computed by averaging over a number of vibrational configurations sampled from an ab initio molecular dynamics run and compared to experiment.

  17. Multiplons in the two-hole excitation spectra of the one-dimensional Hubbard model

    NASA Astrophysics Data System (ADS)

    Rausch, Roman; Potthoff, Michael

    2016-02-01

    Using the density-matrix renormalization group in combination with the Chebyshev polynomial expansion technique, we study the two-hole excitation spectrum of the one-dimensional Hubbard model in the entire filling range from the completely occupied band (n = 2) down to half-filling (n = 1). For strong interactions, the spectra reveal multiplon physics, i.e., relevant final states are characterized by two (doublon), three (triplon), four (quadruplon) and more holes, potentially forming stable compound objects or resonances with finite lifetime. These give rise to several satellites in the spectra with largely different spectral weights as well as to different two-hole, doublon-hole, two-doublon etc continua. The complex multiplon phenomenology is analyzed by interpreting not only local and k-resolved two-hole spectra but also three- and four-hole spectra for the Hubbard model and by referring to effective low-energy models. In addition, a filter-operator technique is presented and applied which allows to extract specific information on the final states at a given excitation energy. While multiplons composed of an odd number of holes do neither form stable compounds nor well-defined resonances unless a nearest-neighbor density interaction V is added to the Hamiltonian, the doublon and the quadruplon are well-defined resonances. The k-resolved four-hole spectrum at n = 2 represents an interesting special case where a completely stable quadruplon turns into a resonance by merging with the doublon-doublon continuum at a critical wave vector. For all fillings with n\\gt 1, the doublon lifetime is strongly k-dependent and is even infinite at the Brillouin zone edges as demonstrated by k-resolved two-hole spectra. This can be traced back to the ‘hidden’ charge-SU(2) symmetry of the model which is explicitly broken off half-filling and gives rise to a massive collective excitation, even for arbitrary higher-dimensional but bipartite lattices.

  18. Quantum spin excitations through the metal-to-insulator crossover in YBa2Cu3O6+y

    SciTech Connect

    Li, Shiliang; Yamani, Zahra; Kang, Hye Jung; Ando, Y.; Yao, Xin; Mook Jr, Herbert A; Dai, Pengcheng

    2008-01-01

    We use inelastic neutron scattering to study the temperature dependence of the spin excitations of a detwinned superconducting YBa{sub 2}Cu{sub 3}O{sub 6.45} (T{sub c} = 48 K). In contrast to earlier work on YBa{sub 2}Cu{sub 3}O{sub 6.5} (T{sub c} = 58 K), where the prominent features in the magnetic spectra consist of a sharp collective magnetic excitation termed 'resonance' and a large ({h_bar} {omega} {approx} 15 meV) superconducting spin gap, we find that the spin excitations in YBa{sub 2}Cu{sub 3}O{sub 6.45} are gapless and have a much broader resonance. Our detailed mapping of magnetic scattering along the a*/b*-axis directions at different energies reveals that spin excitations are unisotropic and consistent with the 'hourglasslike' dispersion along the a*-axis direction near the resonance, but they are isotropic at lower energies. Since a fundamental change in the low-temperature normal state of YBa{sub 2}Cu{sub 3}O{sub 6+y} when superconductivity is suppressed takes place at y {approx} 0.5 with a metal-to-insulator crossover (MIC), where the ground state transforms from a metallic to an insulating like phase, our results suggest a clear connection between the large change in spin excitations and the MIC. The resonance therefore is a fundamental feature of metallic ground state superconductors and a consequence of high-T{sub c} superconductivity.

  19. Fractionalized charge excitations in a spin liquid on partially filled pyrochlore lattices.

    PubMed

    Chen, Gang; Kee, Hae-Young; Kim, Yong Baek

    2014-11-01

    We study the Mott transition from a metal to cluster Mott insulators in the 1/4- and 1/8-filled pyrochlore lattice systems [corrected]. It is shown that such Mott transitions can arise due to charge localization in clusters or in tetrahedron units, driven by the nearest-neighbor repulsive interaction. The resulting cluster Mott insulator is a quantum spin liquid with a spinon Fermi surface, but at the same time a novel fractionalized charge liquid with charge excitations carrying half the electron charge. There exist two emergent U(1) gauge fields or "photons" that mediate interactions between spinons and charge excitations, and between fractionalized charge excitations themselves, respectively. In particular, it is suggested that the emergent photons associated with the fractionalized charge excitations can be measured in x-ray scattering experiments. Various other experimental signatures of the exotic cluster Mott insulator are discussed in light of candidate materials with partially filled bands on the pyrochlore lattice.

  20. Stable oscillation in spin torque oscillator excited by a small in-plane magnetic field

    SciTech Connect

    Taniguchi, Tomohiro; Tsunegi, Sumito; Kubota, Hitoshi; Ito, Takahiro; Utsumi, Yasuhiro

    2015-08-07

    Theoretical conditions to excite self-oscillation in a spin torque oscillator consisting of a perpendicularly magnetized free layer and an in-plane magnetized pinned layer are investigated by analytically solving the Landau-Lifshitz-Gilbert equation. The analytical relation between the current and oscillation frequency is derived. It is found that a large amplitude oscillation can be excited by applying a small field pointing to the direction anti-parallel to the magnetization of the pinned layer. The validity of the analytical results is confirmed by comparing with numerical simulation, showing good agreement especially in a low current region.

  1. Global and short-range entanglement properties in excited, many-body localized spin chains

    NASA Astrophysics Data System (ADS)

    West, Colin; Wei, Tzu-Chieh

    Many-body localization is a manifestation of the violation of the eigenstate thermalization hypothesis. As one of many characteristic features, eigenstates in a many-body localized regime have been observed to obey an area law in the scaling of the entanglement entropy. Consequently, such states can be efficiently represented by matrix product states (MPS). Here, we use the SIMPS algorithm proposed by Yu, Pekker, and Clark to numerically access these excited states in spin chains with disorder, and study them from the perspective of their global and short range entanglement properties, as well as through other local observables. We compare the behavior across excited states as the strength of disorder varies.

  2. The combined effect of quadrupolar and dipolar interactions on the excitation and evolution of triple quantum coherences in ⁷Li solid state magic angle spinning NMR.

    PubMed

    Eliav, Uzi; Goldbourt, Amir

    2013-05-01

    Magic-angle spinning triple-quantum NMR spectra of lithium-7 provide enhanced spectral dispersion for the inherent low chemical shift range of this nucleus, while maintaining linewidths, which are free of any quadrupolar broadening to first order. Since the quadrupolar interaction of (7)Li is very small, in the order of the radio frequency nutation frequencies and only moderately larger than the spinning rates, such spectra are also only marginally affected by the second order quadrupolar interaction under large magnetic fields. In the current study we demonstrate that the existence of two and more proximate (7)Li spins, as encountered in many materials, affects both excitation and evolution of triple-quantum coherences due to the combined effect of quadrupolar and homonuclear dipolar interactions. We show that the generation of (7)Li triple-quantum coherences using two π/2 pulses separated by one-half rotor period is superior in such cases to a single pulse excitation since the excitation time is shorter; thus the maximum signal is only marginally affected by the homonuclear dipolar couplings. When the quadrupolar-dipolar cross terms dominate the spectra, single- and triple-quantum lineshapes are very similar and therefore a true gain in dispersion is maintained in the latter spectrum. The effects of quadrupolar-dipolar cross terms are experimentally demonstrated by comparing a natural abundance and a (6)Li-diluted samples of lithium acetate, resulting in the possibility of efficient excitation of triple quantum coherences over longer periods of time, and in longer life times of triple-quantum coherences.

  3. High-resolution Valence and Core Excitation Spectra via First-Principles Calculations and Experiment

    NASA Astrophysics Data System (ADS)

    Shirley, Eric; Fossard, F.; Gilmore, K.; Hug, G.; Kas, J. J.; Rehr, J. J.; Vila, F.

    We calculate the optical and C K-edge near edge spectra of crystalline and molecular C60 measured with high-resolution electron energy-loss spectroscopy. The calculations are carried out using at least three different methods: Bethe-Salpeter calculations using the NIST Bethe-Salpeter Equation solver (NBSE) in the valence and OCEAN (Obtaining Core Excitation with Ab initio methods and NBSE) suite [Gilmore et al., Comp. Phys. Comm., (2015)]; excited-core-hole calculations using XCH [D. Prendergast and G. Galli, Phys. Rev. Lett. 96, 215502 (2006)]; and constrained occupancy using StoBe (Stockholm-Berlin core-excitation code) [StoBe-deMon version 3.0, K. Hermann et al. (2009)]. They include self-energy effects, lifetime-damping, and Debye-Waller effects. A comparison of spectral features to those observed illustrates the sensitivity of certain features to computation details (e.g., self-energy corrections and core-hole screening). This may point to limitations of various approximations, e.g. in conventional BSE paradigm and/or the incomplete treatment of vibrational effects. Supported in part by DOE BES Grant DE-FG03-97ER45623 (JJR, JJK, FV).

  4. Sorting signals from protein NMR spectra: SPI, a Bayesian protocol for uncovering spin systems.

    PubMed

    Grishaev, Alexander; Llinás, Miguel

    2002-11-01

    Grouping of spectral peaks into J-connected spin systems is essential in the analysis of macromolecular NMR data as it provides the basis for disentangling chemical shift degeneracies. It is a mandatory step before resonance and NOESY cross-peak identities can be established. We have developed SPI, a computational protocol that scrutinizes peak lists from homo- and hetero-nuclear multidimensional NMR spectra and progressively assembles sets of resonances into consensus J- and/or NOE-connected spin systems. SPI estimates the likelihood of nuclear spin resonances appearing at defined frequencies given sets of cross-peaks measured from multi-dimensional experiments. It quantifies spin system matching probabilities via Bayesian inference. The protocol takes advantage of redundancies in the number of connectivities revealed by suites of diverse NMR experiments, systematically tracking the adequacy of each grouping hypothesis. SPI was tested on 2D homonuclear and 2D/3D(15)N-edited data recorded from two protein modules, the col 2 domain of matrix metalloproteinase-2 (MMP-2) and the kringle 2 domain of plasminogen, of 60 and 83 amino acid residues, respectively. For these protein domains SPI identifies approximately 95% unambiguous resonance frequencies, a relatively good performance vis-à-vis the reported 'manual' (interactive) analyses. Abbreviations and Acronyms: SPI, SPin Identification; BMRB, BioMagResBank (Madison, WI).

  5. Superstripes and the excitation spectrum of a spin-orbit-coupled Bose-Einstein condensate.

    PubMed

    Li, Yun; Martone, Giovanni I; Pitaevskii, Lev P; Stringari, Sandro

    2013-06-01

    Using Bogoliubov theory we calculate the excitation spectrum of a spinor Bose-Einstein condensed gas with an equal Rashba and Dresselhaus spin-orbit coupling in the stripe phase. The emergence of a double gapless band structure is pointed out as a key signature of Bose-Einstein condensation and of the spontaneous breaking of translational invariance symmetry. In the long wavelength limit the lower and upper branches exhibit, respectively, a clear spin and density nature. For wave vectors close to the first Brillouin zone, the lower branch acquires an important density character responsible for the divergent behavior of the structure factor and of the static response function, reflecting the occurrence of crystalline order. The sound velocities are calculated as functions of the Raman coupling for excitations propagating orthogonal and parallel to the stripes. Our predictions provide new perspectives for the identification of supersolid phenomena in ultracold atomic gases.

  6. Theoretical probing of inelastic spin-excitations in adatoms on surfaces

    NASA Astrophysics Data System (ADS)

    Lounis, Samir; Schweflinghaus, Benedikt; Dias, Manuel dos Santos; Bouhassoune, Mohammed; Muniz, Roberto B.; Costa, Antonio T.

    2014-12-01

    We review our recent work on the simulation, description and prediction of spin-excitations in adatoms and dimers deposited on metallic surfaces. This work done together with Douglas L. Mills, is an extension of his seminal contribution (with Pascal Lederer) published 50 years ago on the spin-dynamics of transition metal impurities embedded in transition metal hosts [Lederer et al. (1967)]. The main predictions of his model were verified experimentally with state of the art inelastic scanning tunneling spectroscopy on adatoms. Our formalism, presented in this review, is based on time-dependent density functional theory, combined with the Korringa-Kohn-Rostoker Green function method. Comparison to experiments is shown and discussed in detail. Our scheme enables the description and prediction of the main characteristics of these excitations, i.e. their resonance frequency, their lifetime and their behavior upon application of external perturbations such as a magnetic field.

  7. Low-energy singlet excitations in spin-1/2 Heisenberg antiferromagnet on square lattice

    NASA Astrophysics Data System (ADS)

    Aktersky, A. Yu.; Syromyatnikov, A. V.

    2016-05-01

    We present an approach based on a dimer expansion which describes low-energy singlet excitations (singlons) in spin-1/2 Heisenberg antiferromagnet on simple square lattice. An operator ("effective Hamiltonian") is constructed whose eigenvalues give the singlon spectrum. The "effective Hamiltonian" looks like a Hamiltonian of a spin-1/2 magnet in strong external magnetic field and it has a gapped spectrum. It is found that singlet states lie above triplet ones (magnons) in the whole Brillouin zone except in the vicinity of the point (π , 0), where their energies are slightly smaller. Based on this finding, we suggest that a magnon decay is possible near (π , 0) into another magnon and a singlon which may contribute to the dip of the magnon spectrum near (π , 0) and reduce the magnon lifetime. It is pointed out that the singlon-magnon continuum may contribute to the continuum of excitations observed recently near (π , 0).

  8. Spin excitations in the two-dimensional strongly coupled dimer system malachite

    NASA Astrophysics Data System (ADS)

    Canévet, E.; Fâk, B.; Kremer, R. K.; Chun, J. H.; Enderle, M.; Gordon, E. E.; Bettis, J. L.; Whangbo, M.-H.; Taylor, J. W.; Adroja, D. T.

    2015-02-01

    The mineral malachite, Cu 2(OD )2CO 3, has a quantum spin-liquid ground state and no long-range magnetic order down to at least T =0.4 K. Inelastic neutron scattering measurements show that the excitation spectrum consists of dispersive gapped singlet-triplet excitations, characteristic of spin-1/2 dimer-forming Heisenberg antiferromagnets. We identify a distinct two-dimensional dimerized coupling scheme with strong interdimer coupling J'/J1≈0.3 that places malachite between strongly coupled alternating chains, square lattice antiferromagnets, and infinite-legged ladders. The geometry of the interaction scheme resembles the staggered dimer lattice, which may allow unconventional quantum criticality.

  9. Thermal phase transition in artificial spin ice systems induces the formation and migration of monopole-like magnetic excitations

    NASA Astrophysics Data System (ADS)

    León, Alejandro

    2016-11-01

    Artificial spin ice systems exhibit monopole-like magnetic excitations. We develop here a theoretical study of the thermal phase transition of an artificial spin ice system, and we elucidate the role of the monopole excitations in the transition temperature. The dynamics of the spin ice is described by an efficient model based on cellular automata, which considers both thermal effects and dipolar interactions. We have established the critical temperature of the phase transition as function of the magnetic moment and the energy barrier of reversion. In addition, we predict that thermal gradients in the system induce the motion of elementary excitations, which could permit to manipulate monopole-like states.

  10. Analysis of electron spin resonance spectra of irradiated gingers: Organic radical components derived from carbohydrates

    NASA Astrophysics Data System (ADS)

    Yamaoki, Rumi; Kimura, Shojiro; Ohta, Masatoshi

    2010-04-01

    Electron spin resonance (ESR) spectral characterizations of gingers irradiated with electron beam were studied. Complex asymmetrical spectra (near g=2.005) with major spectral components (line width=2.4 mT) and minor signals (at 6 mT apart) were observed in irradiated gingers. The spectral intensity decreased considerably 30 days after irradiation, and continued to decrease steadily thereafter. The spectra simulated on the basis of characteristics of free radical components derived from carbohydrates in gingers are in good agreement with the observed spectra. Analysis showed that shortly after irradiation the major radical components of gingers were composed of radical species derived from amylose and cellulose, and the amylose radicals subsequently decreased considerably. At 30 days after irradiation, the major radical components of gingers were composed of radical species derived from cellulose, glucose, fructose or sucrose.

  11. Determination of Judd-Ofelt intensity parameters from the excitation spectra for rare-earth doped luminescent materials.

    PubMed

    Luo, Wenqin; Liao, Jinsheng; Li, Renfu; Chen, Xueyuan

    2010-04-01

    By utilizing the proportional relationship between the excitation and absorption spectra for some special excited multiplets of rare-earth (RE) ions that are followed by a very fast nonradiative relaxation to the monitored level, we propose a new approach to determine the Judd-Ofelt (JO) intensity parameters that are crucial to the evaluation of laser and luminescent materials via excitation spectra. To validate this approach, the JO parameters of NaGd(WO(4))(2) : Er(3+) and YLiF(4) : Nd(3+) crystals are calculated and compared through both the excitation and absorption spectra. The JO parameters derived from this approach are in good agreement with that determined from the conventional method (absorption spectra). Furthermore, the JO intensity parameters of Y(2)O(3) : Er(3+) nanocrystals are derived from the excitation spectra by taking into account the nano-size effects, which are comparable to the values of the crystal counterpart. The proposed approach is of particular importance for those powders or nanophosphors with low RE doping concentration that their quantitative absorption spectra are difficult to measure.

  12. Calculation of vibrational and electronic excited state absorption spectra of arsenic-water complexes using density functional theory

    NASA Astrophysics Data System (ADS)

    Huang, L.; Lambrakos, S. G.; Shabaev, A.; Massa, L.

    2016-05-01

    Calculations are presented of vibrational and electronic excited-state absorption spectra for As-H2O complexes using density function theory (DFT) and time-dependent density functional theory (TD-DFT). DFT and TD-DFT can provide interpretation of absorption spectra with respect to molecular structure for excitation by electromagnetic waves at frequencies within the IR and UV-visible ranges. The absorption spectrum corresponding to excitation states of As-H2O complexes consisting of relatively small numbers of water molecules should be associated with response features that are intermediate between that of isolated molecules and that of a bulk system. DFT and TD-DFT calculated absorption spectra represent quantitative estimates that can be correlated with additional information obtained from laboratory measurements and other types of theory based calculations. The DFT software GAUSSIAN was used for the calculations of excitation states presented here.

  13. Fully Suspended, Five-Axis, Three-Magnetic-Bearing Dynamic Spin Rig With Forced Excitation

    NASA Technical Reports Server (NTRS)

    Morrison, Carlos R.; Provenza, Andrew; Kurkov, Anatole; Montague, Gerald; Duffy, Kirsten; Mehmed, Oral; Johnson, Dexter; Jansen, Ralph

    2004-01-01

    The Five-Axis, Three-Magnetic-Bearing Dynamic Spin Rig, a significant advancement in the Dynamic Spin Rig (DSR), is used to perform vibration tests of turbomachinery blades and components under rotating and nonrotating conditions in a vacuum. The rig has as its critical components three magnetic bearings: two heteropolar radial active magnetic bearings and a magnetic thrust bearing. The bearing configuration allows full vertical rotor magnetic suspension along with a feed-forward control feature, which will enable the excitation of various natural blade modes in bladed disk test articles. The theoretical, mechanical, electrical, and electronic aspects of the rig are discussed. Also presented are the forced-excitation results of a fully levitated, rotating and nonrotating, unbladed rotor and a fully levitated, rotating and nonrotating, bladed rotor in which a pair of blades was arranged 180 degrees apart from each other. These tests include the bounce mode excitation of the rotor in which the rotor was excited at the blade natural frequency of 144 Hz. The rotor natural mode frequency of 355 Hz was discerned from the plot of acceleration versus frequency. For nonrotating blades, a blade-tip excitation amplitude of approximately 100 g/A was achieved at the first-bending critical (approximately 144 Hz) and at the first-torsional and second-bending blade modes. A blade-tip displacement of 70 mils was achieved at the first-bending critical by exciting the blades at a forced-excitation phase angle of 908 relative to the vertical plane containing the blades while simultaneously rotating the shaft at 3000 rpm.

  14. Analysis of anisotropic spin-label motion in saturation-transfer ESR spectra of spin-labeled cowpea chlorotic mottle virus

    NASA Astrophysics Data System (ADS)

    Hemminga, M. A.; Faber, A. J.

    A saturation-transfer ESR study is carried out on maleimide spin-labeled cowpea chlorotic mottle virus dissolved in various glycerol-water systems. The saturation-transfer ESR spectra were analyzed by comparing them with reference spectra of isotropically reorienting spin labels. The results are interpreted in terms of the overall motion of the virus particle, described by an isotropic rotational correlation time τR, and a local anisotropic spin-label motion with rotational correlation times τ| and τ⊥.

  15. Magnetic structure and spin excitations in BaMn2Bi2

    DOE PAGES

    Calder, Stuart A.; Saparov, Bayrammurad I; Cao, H. B.; Niedziela, Jennifer L.; Lumsden, Mark D.; Sefat, Athena Safa; Christianson, Andrew D.

    2014-02-19

    We present a single crystal neutron scattering study of BaMn2Bi2, a recently synthesized material with the same ThCr2Si2type structure found in several Fe-based unconventional superconducting materials. We show long range magnetic order, in the form of a G-type antiferromagnetic structure, to exist up to 390 K with an indication of a structural transition at 100 K. Utilizing inelastic neutron scattering we observe a spin-gap of 16 meV, with spin-waves extending up to 55 meV. We find these magnetic excitations are well fit to a J1-J2-Jc Heisenberg model and present values for the exchange interactions. The spin wave spectrum appears tomore » be unchanged by the 100 K structural phase transition.« less

  16. Nanometer-scale scanning magnetometry of spin structures and excitations using Nitrogen-vacancy centers

    NASA Astrophysics Data System (ADS)

    Dovzhenko, Yuliya

    The development of increasingly sensitive scanning techniques has led to new insights into the physics of interacting condensed matter systems. Recently, Nitrogen-Vacancy (NV) centers in diamond emerged as a promising scanning magnetic imaging platform capable of operating in a broad range of temperatures and magnetic fields, with sensitivity and resolution capable of imaging a single electron spin with sub-nanometer resolution under ambient conditions. In this talk we will review some of the recent developments in this new scanning platform. We will describe our recent progress in using a single NV center in a scanning diamond nano-pillar to study condensed matter magnetism at both room and low temperatures. In particular, we demonstrate the use of scanning NV magnetometry to image stray fields originating from static chiral spin structures, as well as to detect resonant and off-resonant low-energy spin excitations.

  17. New formulation of Magnetization Equation for Flowing Nuclear Spin under NMR/MRI Excitation(I)

    NASA Astrophysics Data System (ADS)

    de, Dilip; Emetere, Moses; Omotosho, Victor

    2015-03-01

    We have obtained for the first time from the Bloch NMR equations the correct dependence of the single component of magnetization, My and Mz at resonance (NMR/MRI) on relaxation times, rf B1 field (pulsed or continuous), blood(nuclear spin) flow velocity, etc. in the rotating frame of reference. The equations are applicable for both CW and pulsed NMR experiments with or without flow of spins. Our approaches can be extended easily to include gradient fields and diffusion of spins, if needed in NMR/MRI experiments. We also discuss the application of our equations to a specific case of MR excitation scheme: Free induction decay. The first time new equations of single component of MR magnetization and further equations that can be derived with the methodologies used here, can be applied towards accurate simulation of MR images/signals and extraction of parameters of clinical importance through comparison of the measured and the simulated images/signals.

  18. Edge physics of the quantum spin Hall insulator from a quantum dot excited by optical absorption.

    PubMed

    Vasseur, Romain; Moore, Joel E

    2014-04-11

    The gapless edge modes of the quantum spin Hall insulator form a helical liquid in which the direction of motion along the edge is determined by the spin orientation of the electrons. In order to probe the Luttinger liquid physics of these edge states and their interaction with a magnetic (Kondo) impurity, we consider a setup where the helical liquid is tunnel coupled to a semiconductor quantum dot that is excited by optical absorption, thereby inducing an effective quantum quench of the tunneling. At low energy, the absorption spectrum is dominated by a power-law singularity. The corresponding exponent is directly related to the interaction strength (Luttinger parameter) and can be computed exactly using boundary conformal field theory thanks to the unique nature of the quantum spin Hall edge.

  19. Controlled Rephasing of Single Collective Spin Excitations in a Cold Atomic Quantum Memory.

    PubMed

    Albrecht, Boris; Farrera, Pau; Heinze, Georg; Cristiani, Matteo; de Riedmatten, Hugues

    2015-10-16

    We demonstrate active control of inhomogeneous dephasing and rephasing for single collective atomic spin excitations (spin waves) created by spontaneous Raman scattering in a quantum memory based on cold 87Rb atoms. The control is provided by a reversible external magnetic field gradient inducing an inhomogeneous broadening of the atomic hyperfine levels. We demonstrate experimentally that active rephasing preserves the single photon nature of the retrieved photons. Finally, we show that the control of the inhomogeneous dephasing enables the creation of time-separated spin waves in a single ensemble followed by a selective read-out in time. This is an important step towards the implementation of a functional temporally multiplexed quantum repeater node.

  20. Coupling of Spin and Orbital Excitation in the Iron-based Superconductor FeSeTe

    SciTech Connect

    Lee, S.; Xu, G; Ku, W; Wen, J; Lee, C; Katayama, N; Xu, Z; Ji, S; Lin, Z; Gu, G

    2010-01-01

    We present a combined analysis of neutron scattering and photoemission measurements on superconducting FeSe{sub 0.5}Te{sub 0.5}. The low-energy magnetic excitations disperse only in the direction transverse to the characteristic wave vector (1/2,0,0) whereas the electronic Fermi surface near (1/2,0,0) appears to consist of four incommensurate pockets. While the spin resonance occurs at an incommensurate wave vector compatible with nesting, neither spin-wave nor Fermi-surface-nesting models can describe the magnetic dispersion. We propose that a coupling of spin and orbital correlations is key to explaining this behavior. If correct, it follows that these nematic fluctuations are involved in the resonance and could be relevant to the pairing mechanism.

  1. Measurements of magnetic spin excitations in Permalloy microstructures using nitrogen-vacancy magnetometry

    NASA Astrophysics Data System (ADS)

    Liu, H. J. Jason; Yoon, Seungha; McMichael, Robert

    The magnetic properties of nitrogen-vacancy (NV) centers in diamond have enabled emerging applications in fields ranging from cell biology to quantum computing. An NV center is a lattice defect, which behaves like a spin-1 system. NV centers can be prepared in the mz = 0 state by excitation with green light, and the spin state can be detected by the center's fluorescence of red light. The Zeeman splitting of the mz = +/-1 state, combined with a spin coherence time that can approach 1 ms, makes the NV center a sensitive, atom-sized magnetometer. Recently, NV centers have been used to measure spin wave excitations and vortex core dynamics in a Permalloy microdisk. In this talk, we present current NV center measurements on Permalloy micro and nanostructures that build on previous work. Permalloy structures were fabricated on top of a microstrip antenna and the measurements were conducted on a home-built confocal microscope. Preliminary measurements show photoluminescence contrast of ~12% and field detectivity on the order of µT/Hz1/2. This allows for fine field mapping of stray magnetic fields produced by micro and nanostructures, which are typically a few milliteslas in magnitude. Maryland Nanocenter, University of Maryland.

  2. A Magnetic Suspension and Excitation System for Spin Vibration Testing of Turbomachinery Blades

    NASA Technical Reports Server (NTRS)

    Johnson, Dexter; Brown, Gerald V.; Mehmed, Oral

    1998-01-01

    The Dynamic Spin Rig (DSR) is used to perform vibration tests of turbomachinery blades and components under spinning conditions in a vacuum. A heteropolar radial active magnetic bearing was integrated into the DSR to provide non-contact magnetic suspension and mechanical excitation of the rotor to induce turbomachinery blade vibrations. The magnetic bearing replaces one of the two existing conventional radial ball bearings. Prior operation of the DSR used two voice-coil type linear electromagnetic shakers which provided axial excitation of the rotor. The new magnetic suspension and excitation system has provided enhanced testing capabilities. Tests were performed at high rotational speeds for longer duration and higher vibration amplitudes. Some characteristics of the system include magnetic bearing stiffness values up to 60,000 lb./in., closed loop control bandwidth around 500 Hz, and multi-directional radial excitation of the rotor. This paper reports on the implementation and operation of this system and presents some test results using this system.

  3. Spin contamination-free N-electron wave functions in the excitation-based configuration interaction treatment

    NASA Astrophysics Data System (ADS)

    Alcoba, Diego R.; Torre, Alicia; Lain, Luis; Massaccesi, Gustavo E.; Oña, Ofelia B.; Capuzzi, Pablo

    2016-07-01

    This work deals with the spin contamination in N-electron wave functions provided by the excitation-based configuration interaction methods. We propose a procedure to ensure a suitable selection of excited N-electron Slater determinants with respect to a given reference determinant, required in these schemes. The procedure guarantees the construction of N-electron wave functions which are eigenfunctions of the spin-squared operator S ˆ 2 , avoiding any spin contamination. Our treatment is based on the evaluation of the excitation level of the determinants by means of the expectation value of an excitation operator formulated in terms of spin-free replacement operators. We report numerical determinations of energies and < S ˆ 2 > expectation values, arising from our proposal as well as from traditional configuration interaction methods, in selected open-shell systems, in order to compare the behavior of these procedures and their computational costs.

  4. Neutron scattering studies of spin excitations in superconducting Rb0.82Fe1.68Se2

    SciTech Connect

    Wang, Miaoyin; Li, Chunhong; Abernathy, Douglas L; Song, Yu; Carr, Scott V.; Lu, Xiangye; Li, Shiliang; Yamari, Zahra; Hu, Jiangping; Xiang, Tao; Dai, Pengcheng

    2012-01-01

    We use inelastic neutron scattering to show that superconducting (SC) rubidium iron selenide Rb0.82Fe1.68Se2 exhibits antiferromagnetic (AF) spin excitations near the in-plane wave vector Q = ( ,0) identical to that for iron arsenide superconductors. Moreover, we find that these excitations change from incommensurate to commensurate with increasing energy and occur at the expense of spin waves associated with the coexisting 5 5 block AF phase. Since these spin excitations cannot come from Fermi surface nesting based on angle resolved photoemission experiments, our results indicate the presence of local moments in SC Rb0.82Fe1.68Se2 that may have a similar origin as the hourglass-like spin excitations in copper oxide superconductors.

  5. Early excitation of spin-orbit misalignments in close-in planetary systems

    SciTech Connect

    Spalding, Christopher; Batygin, Konstantin

    2014-07-20

    Continued observational characterization of transiting planets that reside in close proximity to their host stars has shown that a substantial fraction of such objects possess orbits that are inclined with respect to the spin axes of their stars. Mounting evidence for the wide-spread nature of this phenomenon has challenged the conventional notion that large-scale orbital transport occurs during the early epochs of planet formation and is accomplished via planet-disk interactions. However, recent work has shown that the excitation of spin-orbit misalignment between protoplanetary nebulae and their host stars can naturally arise from gravitational perturbations in multi-stellar systems as well as magnetic disk-star coupling. In this work, we examine these processes in tandem. We begin with a thorough exploration of the gravitationally facilitated acquisition of spin-orbit misalignment and analytically show that the entire possible range of misalignments can be trivially reproduced. Moreover, we demonstrate that the observable spin-orbit misalignment only depends on the primordial disk-binary orbit inclination. Subsequently, we augment our treatment by accounting for magnetic torques and show that more exotic dynamical evolution is possible, provided favorable conditions for magnetic tilting. Cumulatively, our results suggest that observed spin-orbit misalignments are fully consistent with disk-driven migration as a dominant mechanism for the origin of close-in planets.

  6. Ground state spin and excitation energies in half-filled Lieb lattices

    NASA Astrophysics Data System (ADS)

    Ţolea, M.; Niţǎ, M.

    2016-10-01

    We present detailed spectral calculations for small Lieb lattices having up to N =4 number of cells, in the regime of half-filling, an instance of particular relevance for the nanomagnetism of discrete systems such as quantum dot arrays, due to the degenerate levels at midspectrum. While for the Hubbard interaction model—and even number of sites—the ground state spin is given by the Lieb theorem, the inclusion of long-range interaction—or odd number of sites—makes the spin state not known a priori, which justifies our approach. We calculate also the excitation energies, which are of experimental importance, and find significant variation induced by the interaction potential. One obtains insights on the mechanisms involved that impose as ground state the Lieb state with lower spin rather than the Hund one with maximum spin for the degenerate levels, showing this in the first and second orders of the interaction potential for the smaller lattices. The analytical results agree with the numerical ones, which are performed by exact diagonalization calculations or by a combined mean-field and configuration interaction method. While the Lieb state is always lower in energy than the Hund state, for strong long-range interaction, when possible, another minimal spin state is imposed as ground state.

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

    NASA Astrophysics Data System (ADS)

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

    2016-08-01

    When quantum fluctuations destroy underlying long-range ordered states, novel quantum states emerge. Spin-liquid (SL) states of frustrated quantum antiferromagnets, in which highly correlated spins fluctuate down to very low temperatures, are prominent examples of such quantum states. SL states often exhibit exotic physical properties, but the precise nature of the elementary excitations behind such phenomena remains entirely elusive. Here, we use thermal Hall measurements that can capture the unexplored property of the elementary excitations in SL states, and report the observation of anomalous excitations that may unveil the unique features of the SL state. Our principal finding is a negative thermal Hall conductivity κxyκxy which the charge-neutral spin excitations in a gapless SL state of the 2D kagomé insulator volborthite Cu3V2O7(OH)2ṡ2H2O exhibit, in much the same way in which charged electrons show the conventional electric Hall effect. We find that κxyκxy is absent in the high-temperature paramagnetic state and develops upon entering the SL state in accordance with the growth of the short-range spin correlations, demonstrating that κxyκxy is a key signature of the elementary excitation formed in the SL state. These results suggest the emergence of nontrivial elementary excitations in the gapless SL state which feel the presence of fictitious magnetic flux, whose effective Lorentz force is found to be less than 1/100 of the force

  8. Exchange-coupling modified spin wave spectra in the perpendicularly magnetized permalloy nanodot chain arrays

    NASA Astrophysics Data System (ADS)

    Dou, Jian; Hernandez, Sarah C.; Yu, Chengtao; Pechan, Michael J.; Folks, Liesl; Katine, Jordan A.; Carey, Matthew J.

    2009-03-01

    Spin wave spectra in exchange coupled nanoscale dot chain arrays were studied using ferromagnetic resonance. The dot chain arrays, with dot diameters of 300 nm and thicknesses of 40 nm, coupled via permalloy bridges of width ranging from 0 to 60 nm, were fabricated using e-beam lithography. In the perpendicularly magnetized isolated dots, multiple sharp ferromagnetic resonant peaks were observedootnotetextG.N.Kakazei et al, Appl. Phys. Lett. 85, 443 (2004), which is associated with the quantized in-plane wave vector due to the finite dot radius. These spectrum lines shift to higher fields for samples with wider bridges due to the increasing effective demagnetizing factor. Additional higher order spin wave modes were observed as satellite peaks near the resonance peaks at both higher and lower fields, with larger separation between adjacent spin wave peaks for wider bridge samples. These extra spin wave modes, associated with the inter-dot exchange coupling,will be described in detail. This work is supported by US Dept. of Energy at MU.

  9. Electronic structure and spectra of the RbAr van der Waals system including spin-orbit interaction.

    PubMed

    Dhiflaoui, J; Berriche, H; Herbane, M; Alsehimi, A G; Heaven, M C

    2012-11-01

    The potential energy curves and spectroscopic constants of the ground and excited states of the RbAr van der Waals system have been determined using a one-electron pseudopotential approach. This technique is used to replace the effect of the Rb(+) core and the electron-Ar interactions by effective potentials. The core-core interaction for Rb(+)Ar was incorporated using the accurate CCSD(T) potential of Hickling et al. [Hickling, H. L.; Viehland, L. A.; Shepherd, D. T.; Soldán, P.; Lee, E. P. F.; Wright, T. G. Phys. Chem. Chem. Phys. 2004, 6, 4233-4239]. This model reduces the number of active electrons of the RbAr van der Waals systems to just the single valence electron, permitting the use of very large basis sets for the Rb and Ar atoms. Using this approach, the potential energy curves of the ground and excited states dissociating into Rb(5s, 5p, 4d, 6s, 6p, 6d, and 7s) + Ar are calculated at the SCF level. Spin-orbit interaction was also considered within a semiempirical scheme for the states dissociating into Rb(5p) and Rb(6p). Spectroscopic constants are derived and compared with the available theoretical and experimental data. Such comparisons for RbAr show very good agreement for the ground and the first excited states. Furthermore, we have predicted the B(2)Σ(+)(1/2) ← X(2)Σ(+), A(2)Π(1/2) ← X(2)Σ(+), A(2)Π(3/2) ← X(2)Σ(+), A(2)Π(3/2) ← X(2)Σ(+), 5(2)Σ(+) ← X(2)Σ(+), 3(2)Π(1/2) ← X(2)Σ(+), and 3(2)Π(3/2) ← X(2)Σ(+) absorption spectra.

  10. Spin-flip resolution achieved with a one-proton self-excited oscillator

    NASA Astrophysics Data System (ADS)

    Guise, Nicholas Damien Sun-Wo

    In a Penning trap with an extremely large magnetic gradient, the axial frequency of a one-proton self-excited oscillator is resolved at the level of the shift from a proton spin flip. This sensitivity opens a possible path towards detection of single-proton spin flips, novel measurements of the proton and antiproton g-factors, and a stringent test of CPT invariance by comparing proton and antiproton magnetic moments at precision likely to be a million times higher than achieved to date. The central challenge of extending similar electron magnetic moment measurements to one proton is overcoming the substantially larger mass and weaker magnetic moment, which conspire to greatly reduce the frequency shift that signals a spin flip. Within a magnetic bottle gradient 50 times larger than used in the recent electron g-factor measurements, the proton spin-flip shift is still only 60 mHz out of a 553 kHz axial frequency. In such a large gradient, standard application of sideband cooling to reduce the magnetron radius changes the axial frequency by an amount greater than this spin-flip shift on average. Proton axial frequency resolution at the 60 mHz level is enabled by feedback techniques realized previously only with one electron. Self-excitation produces a narrow feature with large signal-to-noise, ideal for rapid frequency measurements at high precision. Unwanted effects of the strong magnetic gradient are minimized by axial and radial cooling. Feedback cooling is used to reduce the proton axial motion below the temperature of a damping resistor. Axial-magnetron sideband cooling of the undamped radial motion is then demonstrated to reach a 14 mK theoretical limit.

  11. Two-dimensional terahertz correlation spectra of electronic excitations in semiconductor quantum wells.

    PubMed

    Kuehn, W; Reimann, K; Woerner, M; Elsaesser, T; Hey, R

    2011-05-12

    We discuss a novel approach for nonlinear two-dimensional (2D) spectroscopy in the terahertz (THz) frequency range which is based on a collinear interaction geometry of a sequence of THz pulses with the sample. The nonlinear polarization is determined by a phase-resolved measurement of the electric field transmitted through the sample as a function of the delay τ between two phase-locked pulses and the "real" time t. The information provided by a single 2D scan along the τ and t axes is equivalent to that from a noncollinear photon-echo setup equipped with four local oscillators, each interacting with a different diffracted order. We address basic concepts of collinear 2D THz spectroscopy, in particular data analysis and phasing issues. Different rephasing and nonrephasing contributions to the third-order response are separated and 2D correlation spectra derived. As a prototype application, 2D correlation spectra of intersubband excitations of electrons in semiconductor quantum wells are presented.

  12. Absorption spectra of e-beam-excited Ne, Ar, and Kr, pure and in binary mixtures.

    PubMed

    Levchenko, A O; Ustinovskii, N N; Zvorykin, V D

    2010-10-21

    A technique using the broadband emission of a laser plume as probe radiation is applied to record UV-visible (190-510 nm) absorption spectra of Ne, Ar, and Kr, pure and in binary mixtures under moderate e-beam excitation up to 1 MW/cm(3). In all the rare gases and mixtures, the absorption spectra show continuum related to Rg(2) (+) homonuclear ions [peaking at λ∼285, 295, and 320 nm in Ne, Ar, and Kr(Ar/Kr), respectively] and a number of atomic lines related mainly to Rg(∗)(ms) levels, where m is the lowest principal quantum number of the valence electron. In argon, a continuum related to Ar(2) (∗) (λ∼325 nm) is also recorded. There are also trains of narrow bands corresponding to Rg(2) (∗)(npπ (3)Π(g))←Rg(2) (∗)(msσ (3)Σ(u) (+)) transitions. All the spectral features mentioned above were reported in literature but have never been observed simultaneously. Although charge transfer to a homonuclear ion of the heavier additive is commonly believed to dominate in binary rare-gas mixtures, it is found in this study that in Ne/Kr mixture, the charge is finally transferred from the buffer gas Ne(2) (+) ion not to Kr(2) (+) but to heteronuclear NeKr(+) ion.

  13. Orbital Selective Spin Excitations and their Impact on Superconductivity of LiFe_{1-x}Co_{x}As.

    PubMed

    Li, Yu; Yin, Zhiping; Wang, Xiancheng; Tam, David W; Abernathy, D L; Podlesnyak, A; Zhang, Chenglin; Wang, Meng; Xing, Lingyi; Jin, Changqing; Haule, Kristjan; Kotliar, Gabriel; Maier, Thomas A; Dai, Pengcheng

    2016-06-17

    We use neutron scattering to study spin excitations in single crystals of LiFe_{0.88}Co_{0.12}As, which is located near the boundary of the superconducting phase of LiFe_{1-x}Co_{x}As and exhibits non-Fermi-liquid behavior indicative of a quantum critical point. By comparing spin excitations of LiFe_{0.88}Co_{0.12}As with a combined density functional theory and dynamical mean field theory calculation, we conclude that wave-vector correlated low energy spin excitations are mostly from the d_{xy} orbitals, while high-energy spin excitations arise from the d_{yz} and d_{xz} orbitals. Unlike most iron pnictides, the strong orbital selective spin excitations in the LiFeAs family cannot be described by an anisotropic Heisenberg Hamiltonian. While the evolution of low-energy spin excitations of LiFe_{1-x}Co_{x}As is consistent with the electron-hole Fermi surface nesting conditions for the d_{xy} orbital, the reduced superconductivity in LiFe_{0.88}Co_{0.12}As suggests that Fermi surface nesting conditions for the d_{yz} and d_{xz} orbitals are also important for superconductivity in iron pnictides. PMID:27367401

  14. Orbital Selective Spin Excitations and their Impact on Superconductivity of LiFe_{1-x}Co_{x}As.

    PubMed

    Li, Yu; Yin, Zhiping; Wang, Xiancheng; Tam, David W; Abernathy, D L; Podlesnyak, A; Zhang, Chenglin; Wang, Meng; Xing, Lingyi; Jin, Changqing; Haule, Kristjan; Kotliar, Gabriel; Maier, Thomas A; Dai, Pengcheng

    2016-06-17

    We use neutron scattering to study spin excitations in single crystals of LiFe_{0.88}Co_{0.12}As, which is located near the boundary of the superconducting phase of LiFe_{1-x}Co_{x}As and exhibits non-Fermi-liquid behavior indicative of a quantum critical point. By comparing spin excitations of LiFe_{0.88}Co_{0.12}As with a combined density functional theory and dynamical mean field theory calculation, we conclude that wave-vector correlated low energy spin excitations are mostly from the d_{xy} orbitals, while high-energy spin excitations arise from the d_{yz} and d_{xz} orbitals. Unlike most iron pnictides, the strong orbital selective spin excitations in the LiFeAs family cannot be described by an anisotropic Heisenberg Hamiltonian. While the evolution of low-energy spin excitations of LiFe_{1-x}Co_{x}As is consistent with the electron-hole Fermi surface nesting conditions for the d_{xy} orbital, the reduced superconductivity in LiFe_{0.88}Co_{0.12}As suggests that Fermi surface nesting conditions for the d_{yz} and d_{xz} orbitals are also important for superconductivity in iron pnictides.

  15. Orbital Selective Spin Excitations and their Impact on Superconductivity of LiFe1 -xCoxAs

    NASA Astrophysics Data System (ADS)

    Li, Yu; Yin, Zhiping; Wang, Xiancheng; Tam, David W.; Abernathy, D. L.; Podlesnyak, A.; Zhang, Chenglin; Wang, Meng; Xing, Lingyi; Jin, Changqing; Haule, Kristjan; Kotliar, Gabriel; Maier, Thomas A.; Dai, Pengcheng

    2016-06-01

    We use neutron scattering to study spin excitations in single crystals of LiFe0.88Co0.12As , which is located near the boundary of the superconducting phase of LiFe1 -xCoxAs and exhibits non-Fermi-liquid behavior indicative of a quantum critical point. By comparing spin excitations of LiFe0.88Co0.12As with a combined density functional theory and dynamical mean field theory calculation, we conclude that wave-vector correlated low energy spin excitations are mostly from the dx y orbitals, while high-energy spin excitations arise from the dy z and dx z orbitals. Unlike most iron pnictides, the strong orbital selective spin excitations in the LiFeAs family cannot be described by an anisotropic Heisenberg Hamiltonian. While the evolution of low-energy spin excitations of LiFe1 -xCoxAs is consistent with the electron-hole Fermi surface nesting conditions for the dx y orbital, the reduced superconductivity in LiFe0.88Co0.12As suggests that Fermi surface nesting conditions for the dy z and dx z orbitals are also important for superconductivity in iron pnictides.

  16. Fluorescence Excitation-Emission Matrix Regional Integration to Quantify Spectra for Dissolved Organic Matter

    USGS Publications Warehouse

    Chen, W.; Westerhoff, P.; Leenheer, J.A.; Booksh, K.

    2003-01-01

    Excitation-emission matrix (EEM) fluorescence spectroscopy has been widely used to characterize dissolved organic matter (DOM) in water and soil. However, interpreting the >10,000 wavelength-dependent fluorescence intensity data points represented in EEMs has posed a significant challenge. Fluorescence regional integration, a quantitative technique that integrates the volume beneath an EEM, was developed to analyze EEMs. EEMs were delineated into five excitation-emission regions based on fluorescence of model compounds, DOM fractions, and marine waters or freshwaters. Volumetric integration under the EEM within each region, normalized to the projected excitation-emission area within that region and dissolved organic carbon concentration, resulted in a normalized region-specific EEM volume (??i,n). Solid-state carbon nuclear magnetic resonance (13C NMR), Fourier transform infrared (FTIR) analysis, ultraviolet-visible absorption spectra, and EEMs were obtained for standard Suwannee River fulvic acid and 15 hydrophobic or hydrophilic acid, neutral, and base DOM fractions plus nonfractionated DOM from wastewater effluents and rivers in the southwestern United States. DOM fractions fluoresced in one or more EEM regions. The highest cumulative EEM volume (??T,n = ????i,n) was observed for hydrophobic neutral DOM fractions, followed by lower ??T,n values for hydrophobic acid, base, and hydrophilic acid DOM fractions, respectively. An extracted wastewater biomass DOM sample contained aromatic protein- and humic-like material and was characteristic of bacterial-soluble microbial products. Aromatic carbon and the presence of specific aromatic compounds (as indicated by solid-state 13C NMR and FTIR data) resulted in EEMs that aided in differentiating wastewater effluent DOM from drinking water DOM.

  17. A comparative theoretical study on core-hole excitation spectra of azafullerene and its derivatives

    SciTech Connect

    Deng, Yunfeng; Gao, Bin; Deng, Mingsen; Luo, Yi

    2014-03-28

    The core-hole excitation spectra—near-edge x-ray absorption spectroscopy (NEXAFS), x-ray emission spectroscopy (XES), and x-ray photoelectron spectroscopy (XPS) shake-up satellites have been simulated at the level of density functional theory for the azafullerene C{sub 59}N and its derivatives (C{sub 59}N){sup +}, C{sub 59}HN, (C{sub 59}N){sub 2}, and C{sub 59}N–C{sub 60}, in which the XPS shake-up satellites were simulated using our developed equivalent core hole Kohn-Sham (ECH-KS) density functional theory approach [B. Gao, Z. Wu, and Y. Luo, J. Chem. Phys. 128, 234704 (2008)] which aims for the study of XPS shake-up satellites of large-scale molecules. Our calculated spectra are generally in good agreement with available experimental results that validates the use of the ECH-KS method in the present work. The nitrogen K-edge NEXAFS, XES, and XPS shake-up satellites spectra in general can be used as fingerprints to distinguish the azafullerene C{sub 59}N and its different derivatives. Meanwhile, different carbon K-edge spectra could also provide detailed information of (local) electronic structures of different molecules. In particular, a peak (at around 284.5 eV) in the carbon K-edge NEXAFS spectrum of the heterodimer C{sub 59}N–C{sub 60} is confirmed to be related to the electron transfer from the C{sub 59}N part to the C{sub 60} part in this charge-transfer complex.

  18. Fluorescence excitation and ultraviolet absorption spectra and theoretical calculations for benzocyclobutane: Vibrations and structure of its excited S{sub 1}(π,π{sup *}) electronic state

    SciTech Connect

    Shin, Hee Won; Ocola, Esther J.; Laane, Jaan; Kim, Sunghwan

    2014-01-21

    The fluorescence excitation spectra of jet-cooled benzocyclobutane have been recorded and together with its ultraviolet absorption spectra have been used to assign the vibrational frequencies for this molecule in its S{sub 1}(π,π{sup *}) electronic excited state. Theoretical calculations at the CASSCF(6,6)/aug-cc-pVTZ level of theory were carried out to compute the structure of the molecule in its excited state. The calculated structure was compared to that of the molecule in its electronic ground state as well as to the structures of related molecules in their S{sub 0} and S{sub 1}(π,π{sup *}) electronic states. In each case the decreased π bonding in the electronic excited states results in longer carbon-carbon bonds in the benzene ring. The skeletal vibrational frequencies in the electronic excited state were readily assigned and these were compared to the ground state and to the frequencies of five similar molecules. The vibrational levels in both S{sub 0} and S{sub 1}(π,π{sup *}) states were remarkably harmonic in contrast to the other bicyclic molecules. The decreases in the frequencies of the out-of-plane skeletal modes reflect the increased floppiness of these bicyclic molecules in their S{sub 1}(π,π{sup *}) excited state.

  19. Theory of excitations and dielectric response at a spin-orbital quantum critical point

    NASA Astrophysics Data System (ADS)

    Ish, Daniel; Balents, Leon

    2015-09-01

    Despite possessing a local spin-2 moment on the iron site and a Curie-Weiss temperature of 45 K, the A-site spinel FeSc2S4 does not magnetically order down to 50 mK. Previous theoretical work advanced an explanation for this observation in the form of the "J2-λ " model, which places FeSc2S4 close to a quantum critical point on the disordered side of a quantum phase transition between a Néel ordered phase and a "spin-orbital liquid" in which spins and orbitals are entangled, quenching the magnetization. We present new theoretical studies of the optical properties of the J2-λ model, including a computation of the dispersion relation for the quasiparticle excitations and the form of the collective response to electric field. We argue that the latter directly probes a low energy excitation continuum characteristic of quantum criticality, and that our results reinforce the consistency of this model with experiment.

  20. Controlling electronic access to the spin excitations of a single molecule in a tunnel junction

    NASA Astrophysics Data System (ADS)

    Hirjibehedin, Cyrus F.; Warner, Ben; El Hallak, Fadi; Prueser, Henning; Ajibade, Afolabi; Gill, Tobias G.; Fisher, Andrew J.; Persson, Mats

    Spintronic phenomena can be utilized to create new devices with applications in data storage and sensing. Scaling these down to the single molecule level requires controlling the properties of the current-carrying orbitals to enable access to spin states through phenomena such as inelastic electron tunneling. Here we show that the spintronic properties of a tunnel junction containing a single molecule can be controlled by their coupling to the local environment. For tunneling through iron phthalocyanine (FePc) on an insulating copper nitride (Cu2N) monolayer above Cu(001), we find that spin transitions may be strongly excited depending on the binding site of the central Fe atom. Different interactions between the Fe and the underlying Cu or N atoms shift the Fe d-orbitals with respect to the Fermi energy, and control the relative strength of the spin excitations, an effect that can described in a simple co-tunneling model. This work demonstrates the importance of the atomic-scale environment in the development of single molecule spintronic devices.

  1. Modeling Spin Fluctuations and Magnetic Excitations from Time-Dependent Density Functional Theory

    NASA Astrophysics Data System (ADS)

    Gorni, Tommaso; Timrov, Iurii; Dal Corso, Andrea; Baroni, Stefano

    Harnessing spin fluctuations and magnetic excitations in materials is key in many fields of technology, spanning from memory devices to information transfer and processing, to name but a few. A proper understanding of the interplay between collective and single-particle spin excitations is still lacking, and it is expected that first-principle simulations based on TDDFT may shed light on this interplay, as well as on the role of important effects such as relativistic ones and related magnetic anisotropies. All the numerical approaches proposed so far to tackle this problem are based on the computationally demanding solution of the Sternheimer equations for the response orbitals or the even more demanding solution of coupled Dyson equations for the spin and charge susceptibilities. The Liouville-Lanczos approach to TDDFT has already proven to be a valuable alternative, the most striking of its features being the avoidance of sums over unoccupied single-particle states and the frequency-independence of the main numerical bottleneck. In this work we present an extension of this methodology to magnetic systems and its implementation in the Quantum ESPRESSO distribution, together with a few preliminary results on the magnon dispersions in bulk Fe.

  2. Excitation and detection of propagating spin waves at the single magnon level.

    NASA Astrophysics Data System (ADS)

    Karenowska, Alexy; Patterson, Andrew; Peterer, Michael; Magnússon, Einar; Leek, Peter

    2015-03-01

    The fields of spin-wave dynamics and magnonics have made substantial contributions to our understanding of fundamental magnetism, and are increasingly widely acknowledged to be areas of solid-state physics with significant technological potential. To date however, experimental activity has focused on the study and possible application of room-temperature systems operating within classical limits. Here, we report a series of experiments in which we demonstrate, for the first time, the excitation and detection of propagating spin waves at the single magnon level. Our results, which have been obtained at cryogenic temperatures using an yttrium iron garnet spin-wave waveguide, serve as evidence that the experimental tools now exist to permit us to create microwave (i.e. GHz frequency) quantum circuits incorporating dispersive magnon systems. This allows us to anticipate the possibility both of exploring quantum aspects of magnon physics with new experimental clarity, and of examining how this physics -- in particular, the magnon's highly tunable dispersion, its readily accessible nonlinearity, and its capacity to couple to optical excitations and electron-based spintronic systems -- might have a role to play in new microwave quantum technologies.

  3. Topological honeycomb magnon Hall effect: A calculation of thermal Hall conductivity of magnetic spin excitations

    NASA Astrophysics Data System (ADS)

    Owerre, S. A.

    2016-07-01

    Quite recently, the magnon Hall effect of spin excitations has been observed experimentally on the kagome and pyrochlore lattices. The thermal Hall conductivity κxy changes sign as a function of magnetic field or temperature on the kagome lattice, and κxy changes sign upon reversing the sign of the magnetic field on the pyrochlore lattice. Motivated by these recent exciting experimental observations, we theoretically propose a simple realization of the magnon Hall effect in a two-band model on the honeycomb lattice. The magnon Hall effect of spin excitations arises in the usual way via the breaking of inversion symmetry of the lattice, however, by a next-nearest-neighbour Dzyaloshinsky-Moriya interaction. We find that κxy has a fixed sign for all parameter regimes considered. These results are in contrast to the Lieb, kagome, and pyrochlore lattices. We further show that the low-temperature dependence on the magnon Hall conductivity follows a T2 law, as opposed to the kagome and pyrochlore lattices. These results suggest an experimental procedure to measure thermal Hall conductivity within a class of 2D honeycomb quantum magnets and ultracold atoms trapped in a honeycomb optical lattice.

  4. Visible and near-infrared excitation spectra from the neptunyl ion doped into a uranyl tetrachloride lattice

    NASA Astrophysics Data System (ADS)

    Barker, Beau J.; Berg, John M.; Kozimor, Stosh A.; Wozniak, Nicholas R.; Wilkerson, Marianne P.

    2016-03-01

    Visible and near-infrared illumination induces 5f-5f and ligand-to-metal charge-transfer (LMCT) transitions of the neptunyl tetrachloride anion in polycrystalline Cs2U(Np)O2Cl4, and results in near-infrared luminescence from the second electronically excited state to the ground state. This photoluminescence is used as a detection method to collect excitation spectra throughout the near-infrared and visible regions. The excitation spectra of LMCT transitions in excitation spectra were identified in previous work. Here the measurement and analysis is extended to include both LMCT and intra-5f transitions. The results manifest variation in structural properties of the neptunium-oxo bond among the low-lying electronic states. Vibronic intensity patterns and energy spacings are used to compare bond lengths and vibrational frequencies in the excited states, confirming significant characteristic differences between those excited by 5f-5f transitions from those due to LMCT transitions. Results are compared with recently published RASPT2/SO calculations of [NpO2Cl4]2-.

  5. Spin excitations in a single La2CuO4 layer.

    PubMed

    Dean, M P M; Springell, R S; Monney, C; Zhou, K J; Pereiro, J; Božović, I; Dalla Piazza, B; Rønnow, H M; Morenzoni, E; van den Brink, J; Schmitt, T; Hill, J P

    2012-10-01

    Cuprates and other high-temperature superconductors consist of two-dimensional layers that are crucial to their properties. The dynamics of the quantum spins in these layers lie at the heart of the mystery of the cuprates. In bulk cuprates such as La(2)CuO(4), the presence of a weak coupling between the two-dimensional layers stabilizes a three-dimensional magnetic order up to high temperatures. In a truly two-dimensional system however, thermal spin fluctuations melt long-range order at any finite temperature. Here, we measure the spin response of isolated layers of La(2)CuO(4) that are only one-unit-cell-thick. We show that coherent magnetic excitations, magnons, known from the bulk order, persist even in a single layer of La(2)CuO(4), with no evidence for more complex correlations such as resonating valence bond correlations. These magnons are, therefore, well described by spin-wave theory (SWT). On the other hand, we also observe a high-energy magnetic continuum in the isotropic magnetic response that is not well described by two-magnon SWT, or indeed any existing theories. PMID:22941330

  6. Resonant inelastic x-ray scattering study of entangled spin-orbital excitations in superconducting PrFeAsO0.7

    NASA Astrophysics Data System (ADS)

    Nomura, T.; Harada, Y.; Niwa, H.; Ishii, K.; Ishikado, M.; Shamoto, S.; Jarrige, I.

    2016-07-01

    Low-energy electron excitation spectra were measured on a single crystal of a typical iron-based superconductor PrFeAsO0.7 using resonant inelastic x-ray scattering (RIXS) at the Fe -L3 edge. Characteristic RIXS features are clearly observed around 0.5, 1-1.5, and 2-3 eV energy losses. These excitations are analyzed microscopically with theoretical calculations using a 22-orbital model derived from first-principles electronic structure calculation. Based on the agreement with the experiment, the RIXS features are assigned to Fe-d orbital excitations which, at low energies, are accompanied by spin flipping and dominated by Fe dy z and dx z orbital characters. Furthermore, our calculations suggest dispersive momentum dependence of the RIXS excitations below 0.5 eV, and predict remarkable splitting and merging of the lower-energy excitations in momentum space. Those excitations, which were not observed in the present experiment, highlight the potential of RIXS with an improved energy resolution to unravel new details of the electronic structure of the iron-based superconductors.

  7. Multi-reference approach to the calculation of photoelectron spectra including spin-orbit coupling

    SciTech Connect

    Grell, Gilbert; Bokarev, Sergey I. Kühn, Oliver; Winter, Bernd; Seidel, Robert; Aziz, Emad F.; Aziz, Saadullah G.

    2015-08-21

    X-ray photoelectron spectra provide a wealth of information on the electronic structure. The extraction of molecular details requires adequate theoretical methods, which in case of transition metal complexes has to account for effects due to the multi-configurational and spin-mixed nature of the many-electron wave function. Here, the restricted active space self-consistent field method including spin-orbit coupling is used to cope with this challenge and to calculate valence- and core-level photoelectron spectra. The intensities are estimated within the frameworks of the Dyson orbital formalism and the sudden approximation. Thereby, we utilize an efficient computational algorithm that is based on a biorthonormal basis transformation. The approach is applied to the valence photoionization of the gas phase water molecule and to the core ionization spectrum of the [Fe(H{sub 2}O){sub 6}]{sup 2+} complex. The results show good agreement with the experimental data obtained in this work, whereas the sudden approximation demonstrates distinct deviations from experiments.

  8. Multi-reference approach to the calculation of photoelectron spectra including spin-orbit coupling

    NASA Astrophysics Data System (ADS)

    Grell, Gilbert; Bokarev, Sergey I.; Winter, Bernd; Seidel, Robert; Aziz, Emad F.; Aziz, Saadullah G.; Kühn, Oliver

    2015-08-01

    X-ray photoelectron spectra provide a wealth of information on the electronic structure. The extraction of molecular details requires adequate theoretical methods, which in case of transition metal complexes has to account for effects due to the multi-configurational and spin-mixed nature of the many-electron wave function. Here, the restricted active space self-consistent field method including spin-orbit coupling is used to cope with this challenge and to calculate valence- and core-level photoelectron spectra. The intensities are estimated within the frameworks of the Dyson orbital formalism and the sudden approximation. Thereby, we utilize an efficient computational algorithm that is based on a biorthonormal basis transformation. The approach is applied to the valence photoionization of the gas phase water molecule and to the core ionization spectrum of the [Fe(H2O)6]2+ complex. The results show good agreement with the experimental data obtained in this work, whereas the sudden approximation demonstrates distinct deviations from experiments.

  9. Influence of structural changes in a periodic antidot waveguide on the spin-wave spectra

    NASA Astrophysics Data System (ADS)

    Kłos, J. W.; Kumar, D.; Krawczyk, M.; Barman, A.

    2014-01-01

    We demonstrate that the magnonic band structure, including the band gap of a ferromagnetic antidot waveguide, can be significantly tuned by a relatively weak modulation of its structural parameters. We study the magnonic band structure in nanoscale spin-wave waveguides with periodically distributed small antidots along their central line by two independent computational methods, namely, a micromagnetic simulation and a plane-wave method. The calculations were performed with consideration of both the exchange and dipolar interactions. For the exchange dominated regime, we discuss, in details, the impact of the changes of the lattice constant, size, and shape of the antidots on the spin-wave spectra. We have shown that a precise choice of these parameters is crucial for achieving desired properties of antidot waveguides, i.e., a large group velocity and filtering properties due to existence of magnonic band gaps. We discuss different mechanisms of magnonic gap opening resulting from Bragg scattering or anticrossing of modes. We have shown that the dipolar interactions start to assert their role in the spin-wave spectrum when the waveguide is scaled up, but even for a period of few hundreds of nanometers, the magnonic band structure preserves qualitatively the properties found in the exchange dominating regime. The obtained results are important for future development of magnonic crystal based devices.

  10. Quantum interference of stored dual-channel spin-wave excitations in a single tripod system

    SciTech Connect

    Wang Hai; Li Shujing; Xu Zhongxiao; Zhao Xingbo; Zhang Lijun; Li Jiahua; Wu Yuelong; Xie Changde; Peng Kunchi; Xiao Min

    2011-04-15

    We present an experimental demonstration of dual-channel memory in a single tripod atomic system. The total readout signal exhibits either constructive or destructive interference when the dual-channel spin-wave excitations (SWEs) are retrieved by two reading beams with a controllable relative phase. When the two reading beams have opposite phases, the SWEs will remain in the medium, which can be retrieved later with two in-phase reading beams. Such a phase-sensitive storage and retrieval scheme can be used to measure and control the relative phase between the two SWEs in the memory medium, which may find applications in quantum-information processing.

  11. Importance of cross-correlated relaxation in the spectra of simple organofluorine compounds: Spectral complexity of A3B3X spin systems compared to ABX spin systems

    NASA Astrophysics Data System (ADS)

    Alemany, Lawrence B.; Malloy, Thomas B.; Nunes, Megan M.; Zaibaq, Nicholas G.

    2012-09-01

    In a continuation of our initial investigation of the complex 13C and 19F spectra exhibited by two simple organofluorine compounds, additional organofluorine compounds expected to exhibit a wide range of spectral complexity were studied. Spectral simulations are critical for analyzing the more complex spin systems, in particular, A3B3X and A6B3X. Cross-correlated relaxation is commonly observed; examples of 13Csbnd 19F cross-correlated relaxation are shown with the signals for each nucleus exhibiting unequal relaxation rates. Higher order effects are particularly noticeable in the spectra of perfluoro-t-butyl alcohol because of a large 4JFF value in the (13CF3)(12CF3)212COH isotopomer. The many additional transitions in an A3B3X spin system compared to an ABX spin system result in much more complex 19F (A3 and B3) and 13C (X) spectra, even though only three types of nuclei are involved in each spin system. The corresponding protio compounds typically constitute a much simpler A3M3X spin system because the long-range nJHH coupling (n ⩾ 4) is much smaller than the corresponding long-range nJFF coupling. Spectra previously published for ethane-1-13C (A3B3X) and hexafluoroethane-1-13C (A3M3X) are notable exceptions and are discussed.

  12. Cluster size dependence of double ionization energy spectra of spin-polarized aluminum and sodium clusters: All-electron spin-polarized GW+T -matrix method

    NASA Astrophysics Data System (ADS)

    Noguchi, Yoshifumi; Ohno, Kaoru; Solovyev, Igor; Sasaki, Taizo

    2010-04-01

    The double ionization energy (DIE) spectra are calculated for the spin-polarized aluminum and sodium clusters by means of the all-electron spin-polarized GW+T -matrix method based on the many-body perturbation theory. Our method using the one- and two-particle Green’s functions enables us to determine the whole spectra at once in a single calculation. The smaller is the size of the cluster, the larger the difference between the minimal double ionization energy and the twice of the ionization potential. This is because the strong Coulomb repulsion between two holes becomes dominant in small confined geometry. Due to Pauli’s exclusion principle, the parallel spin DIE is close to or smaller than the antiparallel spin DIE except for Na4 that has well-separated highest and second highest occupied molecular-orbital levels calculated by the spin-dependent GW calculation. In this paper, we compare the results calculated for aluminum and sodium clusters and discuss the spin-polarized effect and the cluster size dependence of the resulting spectra in detail.

  13. Experimental determination and interpretation of the fluorescence and fluorescence excitation spectra of chrysene cooled in a supersonic jet

    NASA Astrophysics Data System (ADS)

    Borisevich, N. A.; Dyachenko, G. G.; Petukhov, V. A.; Semenov, M. A.

    2008-12-01

    The fluorescence and fluorescence excitation spectra of jet-cooled chrysene are measured. The frequencies of in-plane vibrations in the ground and first excited singlet electronic states, as well as the relative intensities of transitions between them, are calculated with the MO/M8ST method. Based on these data, experimental spectra are interpreted. In the fluorescence excitation spectrum, the position of the line of the 0-0 transition (28 195 ± 1 cm-1), which is the most intense, is determined. In the experimental fluorescence excitation spectrum, 21 lines correspond to fundamental vibrations (altogether, 37 lines are attributed). This supports our assignment and is consistent with the group-theoretical analysis of vibronic interactions. Upon excitation at the frequency of the 0-0 transition, 10 lines corresponding to the excitation of fundamental vibrations are detected, and all 17 lines observed are attributed. In the fluorescence excitation spectrum, the standard deviation between the calculated and measured frequencies of attributed fundamental vibrations is 19 cm-1, while that in the fluorescence spectrum is 15 cm-1.

  14. a Spin Relaxation Model for the Moessbauer Spectra of Barium Tin

    NASA Astrophysics Data System (ADS)

    Irwin, George Michael

    The stochastic relaxation theory of Anderson and Sack is applied to the Mossbauer spectra of seven samples of BaSn_{rm x}Ti _{rm 2-x}Fe _4O_{11} with compositions x = 0.0, 0.4, 0.6, 0.8, 1.2, 1.6, and 2.0. The spectra were obtained at room temperature and in the temperature range 20 K to 170 K. The broad, low temperature spectra were analysed using least square fitting to a simple model for Fe^{3+} in which the ionic moment is subject to a molecular field and a perpendicular random field which induces transitions between spin states. The resulting fits rival the results of analyses on similar systems using static hyperfine field distributions while requiring only two free parameters to mimic the temperature dependence of the spectral lineshapes. The results verify a magnetic double transition in the sample with x = 0.0 which disappears as Sn is added, but suggests that the samples with x = 1.2, 1.6, and 2.0 also show a double transition that has not been observed using other methods.

  15. Solid-state NMR spectra of lipid-anchored proteins under magic angle spinning.

    PubMed

    Nomura, Kaoru; Harada, Erisa; Sugase, Kenji; Shimamoto, Keiko

    2014-03-01

    Solid-state NMR is a promising tool for elucidating membrane-related biological phenomena. We achieved the measurement of high-resolution solid-state NMR spectra for a lipid-anchored protein embedded in lipid bilayers under magic angle spinning (MAS). To date, solid-state NMR measurements of lipid-anchored proteins have not been accomplished due to the difficulty in supplying sufficient amount of stable isotope labeled samples in the overexpression of lipid-anchored proteins requiring complex posttranslational modification. We designed a pseudo lipid-anchored protein in which the protein component was expressed in E. coli and attached to a chemically synthesized lipid-anchor mimic. Using two types of membranes, liposomes and bicelles, we demonstrated different types of insertion procedures for lipid-anchored protein into membranes. In the liposome sample, we were able to observe the cross-polarization and the (13)C-(13)C chemical shift correlation spectra under MAS, indicating that the liposome sample can be used to analyze molecular interactions using dipolar-based NMR experiments. In contrast, the bicelle sample showed sufficient quality of spectra through scalar-based experiments. The relaxation times and protein-membrane interaction were capable of being analyzed in the bicelle sample. These results demonstrated the applicability of two types of sample system to elucidate the roles of lipid-anchors in regulating diverse biological phenomena.

  16. Excitation spectra of photoluminescence and its kinetics in structures with self-assembled Ge:Si nanoislands

    SciTech Connect

    Yablonskiy, A. N. Baidakova, N. A. Novikov, A. V.; Lobanov, D. N.; Shaleev, M. V.

    2015-11-15

    The spectral and time characteristics of photoluminescence associated with the radiative recombination of charge carriers in SiGe/Si(001) multilayer structures with self-assembled Ge:Si islands are investigated. The time dependences of the photoluminescence of Ge:Si islands in a wide range of delay times after the pump pulse are considered at various optical-excitation levels. The photoluminescence-excitation spectra from Ge(Si) islands in the SiGe/Si(001) structures are investigated in the region of band-to-band and subband optical pumping corresponding to various time components in the photoluminescence-relaxation kinetics. A significant difference in the shape of the excitation spectra is revealed for fast (0–100 μs) and slow (100 μs–50 ms) components of the photoluminescence signal from the islands. The significant dependence of the photoluminescence-excitation spectra of Ge(Si)/Si(001) islands on the optical-pump power is shown to be associated with the prolonged diffusion of nonequilibrium charge carriers from bulk-silicon layers to Ge:Si islands at high excitation levels.

  17. First glimpse of the soft x-ray induced excited spin-state trapping effect dynamics on spin cross-over molecules

    SciTech Connect

    Davesne, V.; Gruber, M.; Miyamachi, T.; Da Costa, V.; Boukari, S.; Scheurer, F.; Joly, L.; Bowen, M.; Beaurepaire, E.; Ohresser, P.; Otero, E.; Choueikani, F.; Gaspar, A. B.; Real, J. A.; Wulfhekel, W.

    2013-08-21

    The dynamics of the soft x-ray induced excited spin state trapping (SOXIESST) effect of Fe(phen){sub 2}(NCS){sub 2} (Fe-phen) powder have been investigated by x-ray absorption spectroscopy (XAS) using the total electron yield method, in a wide temperature range. The low-spin (LS) state is excited into the metastable high-spin (HS) state at a rate that depends on the intensity of the x-ray illumination it receives, and both the temperature and the intensity of the x-ray illumination will affect the maximum HS proportion that is reached. We find that the SOXIESST HS spin state transforms back to the LS state at a rate that is similar to that found for the light induced excited spin state trapping (LIESST) effect. We show that it is possible to use the SOXIESST effect in combination with the LIESST effect to investigate the influence of cooperative behavior on the dynamics of both effects. To investigate the impact of molecular cooperativity, we compare our results on Fe-phen with those obtained for Fe([Me{sub 2}Pyrz]{sub 3}BH){sub 2} (Fe-pyrz) powder, which exhibits a similar thermal transition temperature but with a hysteresis. We find that, while the time constant of the dynamic is identical for both molecules, the SOXIESST effect is less efficient at exciting the HS state in Fe-pyrz than in Fe-phen.

  18. Advances in high-resolution RIXS for the study of excitation spectra under high pressure

    NASA Astrophysics Data System (ADS)

    Kim, Jungho

    2016-07-01

    Hard X-ray resonant inelastic X-ray scattering (RIXS) is a promising X-ray spectroscopic tool for measuring low-energy excitation spectra from complex materials under high pressure. In the past, these measurements have been stymied by technical difficulties inherent in measuring a tiny sample, held at high pressure, inside a diamond anvil cell. Now, due to substantial advances in X-ray instrumentation, high-resolution (? meV) RIXS spectrometers at third-generation synchrotron radiation sources have started to successfully address these samples in their extreme environment. However, compared to elastic X-ray scattering and X-ray emission spectroscopy, RIXS is a very photon hungry technique and high-resolution RIXS for samples under high pressure is in its infancy. In this review, the fundamentals of the high-resolution RIXS and associated instrumentation are presented, as well as technical details of diamond anvil cells, sample preparation, and the measurement geometry. Experimental data from measurements of 3d- and 5d-transition metal oxides are shown and future improvements of the RIXS technique in the context of high pressure are discussed.

  19. Spin wave excitations in the tetragonal double perovskite Sr2CuWO6

    NASA Astrophysics Data System (ADS)

    Walker, H. C.; Mustonen, O.; Vasala, S.; Voneshen, D. J.; Le, M. D.; Adroja, D. T.; Karppinen, M.

    2016-08-01

    Sr2CuWO6 is a double perovskite proposed to be at the border between two- and three-dimensional magnetism, with a square lattice of S =1/2 Cu2 + ions. We have used inelastic neutron scattering to investigate the spin wave excitations of the system, to find out how they evolve as a function of temperature, as well as to obtain information about the magnetic exchange interactions. We observed well defined dispersive spin wave modes at 6 K, which partially survive above the magnetic ordering temperature TN=24 K. Linear spin wave theory is used to determine the exchange interactions revealing them to be highly two dimensional in nature. Density functional theory calculations are presented supporting this experimental finding, which is in contrast to a previous ab initio study of the magnetic interactions. Our analysis confirms that not the nearest neighbor, but the next nearest neighbor interactions in the tetragonal a b plane are the strongest. Low incident energy measurements reveal the opening of a 0.6(1) meV gap below TN, which suggests the presence of a very weak single ion anisotropy term in the form of an easy axis along a ̂.

  20. Ultraviolet high-excitation Fe II fluorescence lines excited by O VI, C IV, and H I resonance emission as seen in IUE spectra

    NASA Technical Reports Server (NTRS)

    Feibelman, Walter A.; Bruhweiler, Frederick C.; Johansson, Sveneric

    1991-01-01

    Archival high-dispersion spectra from the IUE are used in a search for Bowen emission lines of Fe II excited by the stronger transition of the O VI resonance doublet. The possibility of using these Fe II emission lines as a diagnostic of the strength of the far-ultraviolet emission of O VI at 1032 A is explored. It is found that the Fe II emission lines are quite common and strong in symbiotic stars, particularly those of the type known as 'symbiotic novae', as well as in normal novae. The lines are observed in central stars of some planetary nebulae of the O VI sequence besides a few central stars of type WR. High density, high excitation, and high temperature are suggested to be requirements for the excitation of the Fe II fluorescence lines. It is pointed out that while these lines were observed in PG 1159-035 and K1-16, they were not observed in AGNs.

  1. Theoretical grounds of relativistic methods for calculation of spin–spin coupling constants in nuclear magnetic resonance spectra

    NASA Astrophysics Data System (ADS)

    Rusakova, I. L.; Rusakov, Yu Yu; Krivdin, L. B.

    2016-04-01

    The theoretical grounds of the modern relativistic methods for quantum chemical calculation of spin–spin coupling constants in nuclear magnetic resonance spectra are considered. Examples and prospects of application of relativistic calculations of these constants in the structural studies of organic and heteroorganic compounds are discussed. Practical recommendations on relativistic calculations of spin–spin coupling constants using the available software are given. The bibliography includes 622 references.

  2. Probing the quantum ground state of a spin-1 Bose-Einstein condensate with cavity transmission spectra

    SciTech Connect

    Zhang, J. M.; Cui, S.; Jing, H.; Zhou, D. L.; Liu, W. M.

    2009-10-15

    We propose to probe the quantum ground state of a spin-1 Bose-Einstein condensate with the transmission spectra of an optical cavity. By choosing a circularly polarized cavity mode with an appropriate frequency, we can realize coupling between the cavity mode and the magnetization of the condensate. The cavity transmission spectra then contain information of the magnetization statistics of the condensate and thus can be used to distinguish the ferromagnetic and antiferromagnetic quantum ground states. This technique may also be useful for continuous observation of the spin dynamics of a spinor Bose-Einstein condensate.

  3. Heisenberg spin exchange effects in powder spectra of weakly perturbed triplet states

    NASA Astrophysics Data System (ADS)

    Chesnut, D. B.; Meinholtz, Dore C.

    1985-12-01

    Heisenberg spin exchange effects on the powder spectra of weakly perturbed triplet states have been studied by simulation techniques. From very small exchange frequencies on, the derivative powder spectrum is dominated by a sharp, essentially constant width, central line whose amplitude exhibits very close to a square-root dependence on the exchange frequency. The derivative powder edge lines are shown to behave according to the single crystal limiting exchange width equation and it is shown that the frequency dependence of the central dominating line provides yet another measure of exchange parameters in physical systems. Application of these methods to the (φ3AsCH+3) (TCNQ)-2 ion radical salt yields results in good agreement with those obtained by other methods.

  4. Spin-wave spectra of perpendicularly magnetized circular submicron dot arrays

    NASA Astrophysics Data System (ADS)

    Kakazei, G. N.; Wigen, P. E.; Guslienko, K. Yu.; Novosad, V.; Slavin, A. N.; Golub, V. O.; Lesnik, N. A.; Otani, Y.

    2004-07-01

    Dynamic microwave properties of arrays of circular Ni and Ni81Fe19 dots were studied by X-band ferromagnetic resonance (FMR) technique. All of the dots had the same radius 0.5μm, thickness 50-70nm, and were arranged into rectangular or square array with different interdot separations. In the case of perpendicular magnetization multiple (up to 8) sharp resonance peaks were observed below the main FMR peak, and the relative positions of these peaks were independent of the interdot separations. Quantitative description of the observed multiresonance FMR spectra is given using the dipole-exchange spin wave dispersion equation for a perpendicularly magnetized film where in-plane wave vector is quantized due to the finite dot radius, and the inhomogenetiy of the intradot static demagnetization field in the nonellipsoidal dot is taken into account.

  5. Modeling of fluorescence line-narrowed spectra in weakly coupled dimers in the presence of excitation energy transfer

    SciTech Connect

    Lin, Chen; Reppert, Mike; Feng, Ximao; Jankowiak, Ryszard

    2014-07-21

    This work describes simple analytical formulas to describe the fluorescence line-narrowed (FLN) spectra of weakly coupled chromophores in the presence of excitation energy transfer (EET). Modeling studies for dimer systems (assuming low fluence and weak coupling) show that the FLN spectra (including absorption and emission spectra) calculated for various dimers using our model are in good agreement with spectra calculated by: (i) the simple convolution method and (ii) the more rigorous treatment using the Redfield approach [T. Renger and R. A. Marcus, J. Chem. Phys. 116, 9997 (2002)]. The calculated FLN spectra in the presence of EET of all three approaches are very similar. We argue that our approach provides a simplified and computationally more efficient description of FLN spectra in the presence of EET. This method also has been applied to FLN spectra obtained for the CP47 antenna complex of Photosystem II reported by Neupane et al. [J. Am. Chem. Soc. 132, 4214 (2010)], which indicated the presence of uncorrelated EET between pigments contributing to the two lowest energy (overlapping) exciton states, each mostly localized on a single chromophore. Calculated and experimental FLN spectra for CP47 complex show very good qualitative agreement.

  6. Excitation Emission Matrix Spectra (EEMS) of Chromophoric Dissolved Organic Matter Produced during Microbial Incubation

    NASA Astrophysics Data System (ADS)

    McDonald, N.; Nelson, N. B.; Parsons, R.

    2013-12-01

    The chromophoric or light-absorbing fraction of dissolved organic matter (CDOM) is present ubiquitously in natural waters and has a significant impact on ocean biogeochemistry, affecting photosynthesis and primary production as well direct and indirect photochemical reactions (Siegel et al., 2002; Nelson et al., 2007). It has been largely researched in the past few decades, however the exact chemical composition remains unknown. Instrumental methods of analysis including simultaneous excitation-emission fluorescence spectra have allowed for further insight into source and chemical composition. While certain excitation-emission peaks have been associated with ';marine' sources, they have not been exclusively linked to bacterial production of CDOM (Coble, 1996; Zepp et al., 2004). In this study, ';grazer diluted' seawater samples (70% 0.2μm filtered water; 30% whole water) were collected at the Bermuda Atlantic Time Series (BATS) site in the Sargasso Sea (31° 41' N; 64° 10' W) and incubated with an amendment of labile dissolved organic carbon (10μM C6H12O6), ammonium (1μM NH4Cl) and phosphate (0.1μM K2HPO4) to facilitate bacterial production. These substrates and concentrations have been previously shown to facilitate optimum bacterial and CDOM production (Nelson et al., 2004). Sample depths were chosen at 1m and 200m as water at these depths has been exposed to UV light (the Subtropical Mode Water at 200m has been subducted from the surface) and therefore has low initial concentrations of CDOM. After the samples were amended, they were incubated at in-situ temperatures in the dark for 72 hours, with bacteria counts, UV-Vis absorption and EEMS measurements taken at 6-8 hour intervals. Dissolved organic carbon (DOC) measurements were collected daily. For the surface water experiment specific bacteria populations were investigated using Fluorescence In-Situ Hybridization (FISH) analysis. Results showed a clear production of bacteria and production of CDOM, which

  7. Optical excitation energies, Stokes shift, and spin-splitting of C24H72Si14.

    PubMed

    Zope, Rajendra R; Baruah, Tunna; Richardson, Steven L; Pederson, Mark R; Dunlap, Brett I

    2010-07-21

    As an initial step toward the synthesis and characterization of sila-diamondoids, such as sila-adamantane (Si(10)H(16),T(d)), the synthesis of a fourfold silylated sila-adamantane molecule (C(24)H(72)Si(14),T(d)) has been reported in literature [Fischer et al., Science 310, 825 (2005)]. We present the electronic structure, ionization energies, quasiparticle gap, and the excitation energies for the Si(14)(CH(3))(24) and the exact silicon analog of adamantane Si(10)H(16) obtained at the all-electron level using the delta-self-consistent-field and transitional state methods within two different density functional models: (i) Perdew-Burke-Ernzerhof generalized gradient approximation and (ii) fully analytic density functional (ADFT) implementation with atom dependent potential. The ADFT is designed so that molecules separate into atoms having exact atomic energies. The calculations within the two models agree well, to within 0.25 eV for optical excitations. The effect of structural relaxation in the presence of electron-hole-pair excitations is examined to obtain its contribution to the luminescence Stokes shift. The spin-influence on exciton energies is also determined. Our calculations indicate overall decrease in the absorption, emission, quasiparticle, and highest occupied molecular orbital-lowest unoccupied molecular orbital gaps, ionization energies, Stokes shift, and exciton binding energy when passivating hydrogens in the Si(10)H(16) are replaced with electron donating groups such as methyl (Me) and trimehylsilyl (-Si(Me)(3)).

  8. Phase relaxed localized excitation pulses for inner volume fast spin echo imaging

    PubMed Central

    Hajnal, Joseph V.

    2015-01-01

    Purpose To design multidimensional spatially selective radiofrequency (RF) pulses for inner volume imaging (IVI) with three‐dimensional (3D) fast spin echo (FSE) sequences. Enhanced background suppression is achieved by exploiting particular signal properties of FSE sequences. Theory and Methods The CPMG condition dictates that echo amplitudes will rapidly decrease if a 90° phase difference between excitation and refocusing pulses is not present, and refocusing flip angles are not precisely 180°. This mechanism is proposed as a means for generating additional background suppression for spatially selective excitation, by biasing residual excitation errors toward violating the CPMG condition. 3D RF pulses were designed using this method with a 3D spherical spiral trajectory, under‐sampled by factor 5.6 for an eight‐channel PTx system, at 3 Tesla. Results 3D‐FSE IVI with pulse durations of approximately 12 ms was demonstrated in phantoms and for T2‐weighted brain imaging in vivo. Good image quality was obtained, with mean background suppression factors of 103 and 82 ± 6 in phantoms and in vivo, respectively. Conclusion Inner Volume Imaging with 3D‐FSE has been demonstrated in vivo with tailored 3D‐RF pulses. The proposed design methods are also applicable to 2D pulses. Magn Reson Med 76:848–861, 2016. © 2015 The Authors. Magnetic Resonance in Medicine published by Wiley Periodicals, Inc. on behalf of International Society for Magnetic Resonance in Medicine PMID:26451691

  9. A Straightforward Way to Determine Relative Intensities of Spin-Spin Splitting Lines of Equivalent Nuclei in NMR Spectra.

    ERIC Educational Resources Information Center

    Orcutt, Ronald H.

    1987-01-01

    Describes a simple way of obtaining a set of relative intensities of spin-spin splitting lines using Pascal's triangle rather than calculating binomial coefficients. Provides tables showing Pascal's triangle and the relative intensities of multiplets for a range of nuclear spins. (TW)

  10. First-principles calculation of ground and excited-state absorption spectra of ruby and alexandrite considering lattice relaxation

    NASA Astrophysics Data System (ADS)

    Watanabe, Shinta; Sasaki, Tomomi; Taniguchi, Rie; Ishii, Takugo; Ogasawara, Kazuyoshi

    2009-02-01

    We performed first-principles calculations of multiplet structures and the corresponding ground-state absorption and excited-state absorption spectra for ruby (Cr3+:α-Al2O3) and alexandrite (Cr3+:BeAl2O4) which included lattice relaxation. The lattice relaxation was estimated using the first-principles total energy and molecular-dynamics method of the CASTEP code. The multiplet structure and absorption spectra were calculated using the configuration-interaction method based on density-functional calculations. For both ruby and alexandrite, the theoretical absorption spectra, which were already in reasonable agreement with experimental spectra, were further improved by consideration of lattice relaxation. In the case of ruby, the peak positions and peak intensities were improved through the use of models with relaxations of 11 or more atoms. For alexandrite, the polarization dependence of the U band was significantly improved, even by a model with a relaxation of only seven atoms.

  11. A simplified Tamm-Dancoff density functional approach for the electronic excitation spectra of very large molecules

    NASA Astrophysics Data System (ADS)

    Grimme, Stefan

    2013-06-01

    Two approximations in the Tamm-Dancoff density functional theory approach (TDA-DFT) to electronically excited states are proposed which allow routine computations for electronic ultraviolet (UV)- or circular dichroism (CD) spectra of molecules with 500-1000 atoms. Speed-ups compared to conventional time-dependent DFT (TD-DFT) treatments of about two to three orders of magnitude in the excited state part at only minor loss of accuracy are obtained. The method termed sTDA ("s" for simplified) employs atom-centered Löwdin-monopole based two-electron repulsion integrals with the asymptotically correct 1/R behavior and perturbative single excitation configuration selection. It is formulated generally for any standard global hybrid density functional with given Fock-exchange mixing parameter ax. The method performs well for two standard benchmark sets of vertical singlet-singlet excitations for values of ax in the range 0.2-0.6. The mean absolute deviations from reference data are only 0.2-0.3 eV and similar to those from standard TD-DFT. In three cases (two dyes and one polypeptide), good mutual agreement between the electronic spectra (up to 10-11 eV excitation energy) from the sTDA method and those from TD(A)-DFT is obtained. The computed UV- and CD-spectra of a few typical systems (e.g., C60, two transition metal complexes, [7]helicene, polyalanine, a supramolecular aggregate with 483 atoms and about 7000 basis functions) compare well with corresponding experimental data. The method is proposed together with medium-sized double- or triple-zeta type atomic-orbital basis sets as a quantum chemical tool to investigate the spectra of huge molecular systems at a reliable DFT level.

  12. Magnetic excitations in the spin-1/2 triangular-lattice antiferromagnet Cs2CuBr4

    DOE PAGES

    Zvyagin, S. A.; Ozerov, M.; Kamenskyi, D.; Wosnitza, J.; Krzystek, J.; Yoshizawa, D.; Hagiwara, M.; Hu, Rongwei; Ryu, Hyejin; Petrovic, C.; et al

    2015-11-27

    We present on high- field electron spin resonance (ESR) studies of magnetic excitations in the spin- 1/2 triangular-lattice antiferromagnet Cs2CuBr4. Frequency- field diagrams of ESR excitations are measured for different orientations of magnetic fields up to 25 T. We show that the substantial zero- field energy gap, Δ ≈ 9.5 K, observed in the low-temperature excitation spectrum of Cs2CuBr4 [Zvyagin et al:, Phys. Rev. Lett. 112, 077206 (2014)], is present well above TN. Noticeably, the transition into the long-range magnetically ordered phase does not significantly affect the size of the gap, suggesting that even below TN the high-energy spin dynamicsmore » in Cs2CuBr4 is determined by short-range-order spin correlations. The experimental data are compared with results of model spin-wave-theory calculations for spin-1/2 triangle-lattice antiferromagnet.« less

  13. Magnetic excitations in the spin-1/2 triangular-lattice antiferromagnet Cs2CuBr4

    NASA Astrophysics Data System (ADS)

    Zvyagin, S. A.; Ozerov, M.; Kamenskyi, D.; Wosnitza, J.; Krzystek, J.; Yoshizawa, D.; Hagiwara, M.; Hu, Rongwei; Ryu, Hyejin; Petrovic, C.; Zhitomirsky, M. E.

    2015-11-01

    We report on high-field electron spin resonance (ESR) studies of magnetic excitations in the spin-1/2 triangular-lattice antiferromagnet Cs2CuBr4. Frequency-field diagrams of ESR excitations are measured for different orientations of magnetic fields up to 25 T. We show that the substantial zero-field energy gap, {{Δ }}≈ 9.5 K, observed in the low-temperature excitation spectrum of Cs2CuBr4, (Zvyagin et al 2014 Phys. Rev. Lett.112 077206) is present well above TN. Noticeably, the transition into the long-range magnetically ordered phase does not significantly affect the size of the gap, suggesting that even below TN the high-energy spin dynamics in Cs2CuBr4 is determined by short-range-order spin correlations. The experimental data are compared with results of model spin-wave-theory calculations for spin-1/2 triangular-lattice antiferromagnet.

  14. Effect of spin fluctuations on quasiparticle excitations: First-principles theory and application to sodium and lithium

    NASA Astrophysics Data System (ADS)

    Lischner, Johannes; Bazhirov, Timur; MacDonald, Allan H.; Cohen, Marvin L.; Louie, Steven G.

    2014-02-01

    We present first-principles calculations for quasiparticle excitations in sodium and lithium, including the effects of charge and spin fluctuations. We employ the Overhauser-Kukkonen form for the electron self-energy arising from spin fluctuations and demonstrate that the coupling of electrons to spin fluctuations gives an important contribution to the quasiparticle lifetime but does not significantly reduce the occupied bandwidth. Including correlation effects beyond the random-phase approximation in the screening from charge fluctuations yields good agreement with experiment.

  15. Deformation increase of high-spin core-excited isomers in the astatine nuclei

    SciTech Connect

    Scheveneels, G.; Hardeman, F.; Neyens, G.; Coussement, R. )

    1991-06-01

    Quadrupole moments of six high-spin isomers in the At isotopes have been measured with the level-mixing-spectroscopy method: {sup 208}At(16{sup {minus}}), {sup 209}At(29/2{sup +}), {sup 210}At(19{sup +},15{sup {minus}}), {sup 211}At(39/2{sup {minus}},29/2{sup +}). The results show that level mixing spectroscopy is a promising technique to determine quadrupole moments of isomers that are difficult to measure by other in-beam hyperfine interaction methods. A large increase of the quadrupole moment is observed if neutrons are excited across or removed from the {ital N}=126 shell closure. This behavior is explained in terms of an enhanced core softness for fewer core neutrons; the aligned valence particles, moving in equatorial orbits, then easily polarize the core towards oblate deformation.

  16. Thermal Excitation of Gadolinium-Based Contrast Agents Using Spin Resonance

    PubMed Central

    Fridjhon, Peter; Rubin, David M.

    2016-01-01

    Theoretical and experimental investigations into the thermal excitation of liquid paramagnetic contrast agents using the spin resonance relaxation mechanism are presented. The electronic spin-lattice relaxation time τ1e of gadolinium-based contrast agents, which is estimated at 0.1 ns, is ten orders of magnitude faster than the relaxation time of protons in water. The shorter relaxation time is found to significantly increase the rate of thermal energy deposition. To the authors’ knowledge this is the first study of gadolinium based contrast agents in a liquid state used as thermal agents. Analysis shows that when τ1e and other experimental parameters are optimally selected, a maximum theoretical heating rate of 29.4 °C.s−1 could be achieved which would suffice for clinical thermal ablation of neoplasms. The experimental results show a statistically significant thermal response for two out of the four contrast agents tested. The results are compared to the simulated estimates via analysis of a detailed model of the system. While these experimentally determined temperature rises are small and thus of no clinical utility, their presence supports the theoretical analysis and strongly suggests that the chemical structure of the selected compounds plays an important role in this mechanism of heat deposition. There exists an opportunity for the development of alternative gadolinium-based compounds with an order of magnitude longer τ1e in a diluted form to be used as an efficient hyperthermia agent for clinical use. PMID:27341338

  17. Thermal Excitation of Gadolinium-Based Contrast Agents Using Spin Resonance.

    PubMed

    Dinger, Steven C; Fridjhon, Peter; Rubin, David M

    2016-01-01

    Theoretical and experimental investigations into the thermal excitation of liquid paramagnetic contrast agents using the spin resonance relaxation mechanism are presented. The electronic spin-lattice relaxation time τ1e of gadolinium-based contrast agents, which is estimated at 0.1 ns, is ten orders of magnitude faster than the relaxation time of protons in water. The shorter relaxation time is found to significantly increase the rate of thermal energy deposition. To the authors' knowledge this is the first study of gadolinium based contrast agents in a liquid state used as thermal agents. Analysis shows that when τ1e and other experimental parameters are optimally selected, a maximum theoretical heating rate of 29.4 °C.s-1 could be achieved which would suffice for clinical thermal ablation of neoplasms. The experimental results show a statistically significant thermal response for two out of the four contrast agents tested. The results are compared to the simulated estimates via analysis of a detailed model of the system. While these experimentally determined temperature rises are small and thus of no clinical utility, their presence supports the theoretical analysis and strongly suggests that the chemical structure of the selected compounds plays an important role in this mechanism of heat deposition. There exists an opportunity for the development of alternative gadolinium-based compounds with an order of magnitude longer τ1e in a diluted form to be used as an efficient hyperthermia agent for clinical use. PMID:27341338

  18. Spin-lozenge thermodynamics and magnetic excitations in Na3RuO4

    SciTech Connect

    Haraldsen, Jason T; Stone, Matthew B; Lumsden, Mark D; Barnes, Ted {F E }; Jin, Rongying; Taylor, J. W.; Fernandez-Alonso, F

    2009-01-01

    We report inelastic and elastic neutron scattering, magnetic susceptibility, and heat capacity measurements of polycrystalline sodium ruthenate (Na3RuO4). Previous work suggests this material consists of isolated tetramers of S = 3/2 Ru5+ ions in a so-called lozenge configuration. Using a Heisenberg antiferromagnet Hamiltonian, we analytically determine the energy eigenstates for general spin S. From this model, the neutron scattering cross-sections for excitations associated with spin-3/2 tetramer configurations is determined. Comparison of magnetic susceptibility and inelastic neutron scattering results shows that the proposed lozenge model is not distinctly supported, but provides evidence that the system may be better described as a pair of non-interacting inequivalent dimers, i.e double dimers. However, the existence of long-range magnetic order below Tc ≈ 28 K immediately questions such a description. Although no evidence of the lozenge model is observed, future studies on single crystals may further clarify the appropriate magnetic Hamiltonian.

  19. Transition from three-dimensional anisotropic spin excitations to two-dimensional spin excitations by electron doping the FeAs-based BaFe1.96Ni0.04As2 superconductor.

    PubMed

    Harriger, Leland W; Schneidewind, Astrid; Li, Shiliang; Zhao, Jun; Li, Zhengcai; Lu, Wei; Dong, Xiaoli; Zhou, Fang; Zhao, Zhongxian; Hu, Jiangping; Dai, Pengcheng

    2009-08-21

    We use neutron scattering to study the effect of electron doping on the structural or magnetic order in BaFe2As2. In the undoped state, BaFe2As2 exhibits simultaneous structural and magnetic phase transitions below 143 K. Upon electron doping to form BaFe1.96Ni0.04As2, the system first displays the lattice distortion near approximately 97 K, and then orders antiferromagnetically at 91 K before developing weak superconductivity below approximately 15 K. The effect of electron doping is to reduce the c-axis exchange coupling in BaFe2As2 and induce quasi-two-dimensional (2D) spin excitations. These results suggest that the transition from 3D spin waves to quasi-2D spin excitations by electron doping is important for the separated structural and magnetic phase transitions in iron arsenides.

  20. Magnetic circular dichroism studies of matrix-isolated atoms: Excited state spin-orbit coupling constant reduction of copper in the noble gases

    NASA Astrophysics Data System (ADS)

    Vala, Martin; Zeringue, Kyle; ShakhsEmampour, Jalal; Rivoal, Jean-Claude; Pyzalski, Robert

    1984-03-01

    The absorption and magnetic circular dichroism spectra of the 2P←2S transition of matrix-isolated copper atoms have been measured in krypton and xenon matrices. A dramatic reversal in the MCD C term pattern is observed. From a spectral band moment analysis it is shown that: (1) noncubic lattice cage vibrational motions are more important than cubic ones in contributing to the observed bandwidths and (2) the Cu excited state spin-orbit coupling constant (λ) in krypton is reduced to 57% of its gas phase value, whereas in xenon it is reduced to -14% of its gas phase value. Calculations using the Moran model show that the excited state geometry of the metal/rare gas cage is distorted via the Jahn-Teller effect in opposite ways in krypton and xenon matrices. The negative sign of λ in xenon reveals a reversal in the order of the 2P state spin-orbit multiplets. Neither this reversal nor the reduction of λ in krypton can be accounted for by the Jahn-Teller effect. We attribute the spin-orbit constant reduction to the overlap of the Cu 4p orbital with the np of the rare gas matrix cage atoms. The calculated spin-orbit reduction factors (in Ar, Kr, and Xe) agree well with the experimental ones if a contracted Cu 4p orbital is used. In the same way the ground state g factor shift with matrix atom type, observed by Kasai and McLeod, is semiquantitatively accounted for by calculation of the overlaps between the Cu 4s orbital and the np orbitals of the rare gas cage atoms.

  1. Electrostatic control of spin polarization in a quantum Hall ferromagnet: a new platform to realize non-Abelian excitations

    NASA Astrophysics Data System (ADS)

    Kazakov, Alexander; Kolkovsky, V.; Adamus, Z.; Karczewski, G.; Wojtowicz, T.; Rokhinson, Leonid

    2015-03-01

    Several experiments detected signatures of Majorana fermions in nanowires, and the focus of current research is shifting toward systems where non-Abelian statistics of excitations can be demonstrated. To achieve this goal we are developing a new platform where non-Abelian excitations can be created and manipulated in a two-dimensional plane, with support for Majorana and higher order non-Abelian excitations. The system is based on CdTe quantum wells non-uniformly doped with paramagnetic impurities, which result in a complicate field-dependence of Zeeman splitting. A unique property of the system is that at high fields we can form a quantum Hall ferromagnet with gate-controllable spin polarization. Helical 1D edge channels formed along the edges of electrostatic gates may support generalized non-Abelian excitations in the fractional qunatum Hall regime, and Majorana and parafermion excitations in the presence of induced superconductivity. We will present results on the gate control of s-d exchange in specially designed heterostructures, demonstrate gate control of spin polarization at filling factor ν = 2 , and show spatial separation of quantum Hall states with different spin polarization using lithographically defined gates.

  2. Spin-orbit excitations and electronic structure of the putative Kitaev magnet α -RuCl3

    NASA Astrophysics Data System (ADS)

    Sandilands, Luke J.; Tian, Yao; Reijnders, Anjan A.; Kim, Heung-Sik; Plumb, K. W.; Kim, Young-June; Kee, Hae-Young; Burch, Kenneth S.

    2016-02-01

    Mott insulators with strong spin-orbit coupling have been proposed to host unconventional magnetic states, including the Kitaev quantum spin liquid. The 4 d system α -RuCl3 has recently come into view as a candidate Kitaev system, with evidence for unusual spin excitations in magnetic scattering experiments. We apply a combination of optical spectroscopy and Raman scattering to study the electronic structure of this material. Our measurements reveal a series of orbital excitations involving localized total angular momentum states of the Ru ion, implying that strong spin-orbit coupling and electron-electron interactions coexist in this material. Analysis of these features allows us to estimate the spin-orbit coupling strength, as well as other parameters describing the local electronic structure, revealing a well-defined hierarchy of energy scales within the Ru d states. By comparing our experimental results with density functional theory calculations, we also clarify the overall features of the optical response. Our results demonstrate that α -RuCl3 is an ideal material system to study spin-orbit coupled magnetism on the honeycomb lattice.

  3. Simulations of molecular dynamics in solid-state NMR spectra of spin-1 nuclei including effects of CSA- and EFG-terms up to second order.

    PubMed

    Larsen, Flemming H

    2007-04-01

    By numerical simulations MAS and QCPMG methods for acquiring spectra of spin-1 nuclei were compared in order to determine the most sensitive experiment for analysis of molecular dynamics. To comply with the large quadrupolar constants for 14N and the CSA reported for 6Li both of these interactions are included up to second order. For 2H and 6Li both QCPMG and single-pulse MAS experiments were suitable for dynamics studies whereas the single-pulse MAS experiment were the method of choice for investigation of 14N dynamics for C(Q)'s larger than 750kHz at 14.1T. This property prohibits excitation of the 14N lineshape using either single hard or softer composite rf-pulses. Focusing on 14N it was demonstrated that the centerband lineshape is sensitive toward both off-MAS and CSA effects. In addition, excitation by real-time pulses showed that proper lineshapes corresponding to a site with a C(Q) of 3MHz may be excited by a very short pulse. PMID:17418539

  4. Effects of Imidazole Deprotonation on Vibrational Spectra of High-Spin Iron(II) Porphyrinates

    PubMed Central

    Hu, Chuanjiang; Peng, Qian; Silvernail, Nathan J.; Barabanschikov, Alexander; Zhao, Jiyong; Alp, E. Ercan; Sturhahn, Wolfgang; Sage, J. Timothy; Scheidt, W. Robert

    2013-01-01

    The effects of the deprotonation of coordinated imidazole on the dynamics of five-coordinate high-spin iron(II) porphyrinates have been investigated using nuclear resonance vibrational spectroscopy. Two complexes have been studied in detail with both powder and oriented single-crystal measurements. Changes in the vibrational spectra are clearly related to structural differences in the molecular structures that occur when imidazole is deprotonated. Most modes involving the simultaneous motion of iron and imidazolate are unresolved but the one mode that is resolved is found at higher frequency in the imidazolates. These out-of-plane results are in accord with earlier resonance Raman studies of heme proteins. We also show the imidazole vs. imidazolate differences in the in-plane vibrations that are not accessible to resonance Raman studies. The in-plane vibrations are at lower frequency in the imidazolate derivatives; the doming mode shifts are inconclusive. The stiffness, an experimentally determined force constant that averages the vibrational details to quantify the nearest-neighbor interactions, confirms that deprotonation inverts the relative strengths of axial and equatorial coordination. PMID:23470205

  5. Orphan spin operators enable the acquisition of multiple 2D and 3D magic angle spinning solid-state NMR spectra

    PubMed Central

    Gopinath, T.; Veglia, Gianluigi

    2013-01-01

    We propose a general method that enables the acquisition of multiple 2D and 3D solid-state NMR spectra for U-13C, 15N-labeled proteins. This method, called MEIOSIS (Multiple ExperIments via Orphan SpIn operatorS), makes it possible to detect four coherence transfer pathways simultaneously, utilizing orphan (i.e., neglected) spin operators of nuclear spin polarization generated during 15N-13C cross polarization (CP). In the MEIOSIS experiments, two phase-encoded free-induction decays are decoded into independent nuclear polarization pathways using Hadamard transformations. As a proof of principle, we show the acquisition of multiple 2D and 3D spectra of U-13C, 15N-labeled microcrystalline ubiquitin. Hadamard decoding of CP coherences into multiple independent spin operators is a new concept in solid-state NMR and is extendable to many other multidimensional experiments. The MEIOSIS method will increase the throughput of solid-state NMR techniques for microcrystalline proteins, membrane proteins, and protein fibrils. PMID:23676036

  6. Orphan spin operators enable the acquisition of multiple 2D and 3D magic angle spinning solid-state NMR spectra

    NASA Astrophysics Data System (ADS)

    Gopinath, T.; Veglia, Gianluigi

    2013-05-01

    We propose a general method that enables the acquisition of multiple 2D and 3D solid-state NMR spectra for U-13C, 15N-labeled proteins. This method, called MEIOSIS (Multiple ExperIments via Orphan SpIn operatorS), makes it possible to detect four coherence transfer pathways simultaneously, utilizing orphan (i.e., neglected) spin operators of nuclear spin polarization generated during 15N-13C cross polarization (CP). In the MEIOSIS experiments, two phase-encoded free-induction decays are decoded into independent nuclear polarization pathways using Hadamard transformations. As a proof of principle, we show the acquisition of multiple 2D and 3D spectra of U-13C, 15N-labeled microcrystalline ubiquitin. Hadamard decoding of CP coherences into multiple independent spin operators is a new concept in solid-state NMR and is extendable to many other multidimensional experiments. The MEIOSIS method will increase the throughput of solid-state NMR techniques for microcrystalline proteins, membrane proteins, and protein fibrils.

  7. Triplet excited state spectra and dynamics of carotenoids from the thermophilic purple photosynthetic bacterium Thermochromatium tepidum

    SciTech Connect

    Niedzwiedzki, Dariusz; Kobayashi, Masayuki; Blankenship, R. E.

    2011-01-13

    Light-harvesting complex 2 from the anoxygenic phototrophic purple bacterium Thermochromatium tepidum was purified and studied by steady-state absorption, fluorescence and flash photolysis spectroscopy. Steady-state absorption and fluorescence measurements show that carotenoids play a negligible role as supportive energy donors and transfer excitation to bacteriochlorophyll-a with low energy transfer efficiency of ~30%. HPLC analysis determined that the dominant carotenoids in the complex are rhodopin and spirilloxanthin. Carotenoid excited triplet state formation upon direct (carotenoid) or indirect (bacteriochlorophyll-a Q{sub x} band) excitation shows that carotenoid triplets are mostly localized on spirilloxanthin. In addition, no triplet excitation transfer between carotenoids was observed. Such specific carotenoid composition and spectroscopic results strongly suggest that this organism optimized carotenoid composition in the light-harvesting complex 2 in order to maximize photoprotective capabilities of carotenoids but subsequently drastically suppressed their supporting role in light-harvesting process.

  8. Excitation spectra of bosons in optical lattices from the Schwinger-Keldysh calculation

    SciTech Connect

    Grass, T. D.; Santos, F. E. A. dos; Pelster, A.

    2011-07-15

    Within the Schwinger-Keldysh formalism we derive a Ginzburg-Landau theory for the Bose-Hubbard model which describes the real-time dynamics of the complex order parameter field. Analyzing the excitations in the vicinity of the quantum phase transition, it turns out that particle-hole dispersions in the Mott phase map continuously onto corresponding amplitude-phase excitations in the superfluid phase, which have been detected recently by Bragg spectroscopy measurements.

  9. Investigation on the spectral properties of 2D asynchronous fluorescence spectra generated by using variable excitation wavelengths as a perturbation

    NASA Astrophysics Data System (ADS)

    Wang, Jingdan; He, Anqi; Guo, Ran; Wei, Yongju; Feng, Juan; Xu, Yizhuang; Noda, Isao; Wu, Jinguang

    2016-11-01

    Properties of 2D asynchronous spectra generated from a series of fluorescence emission spectra are investigated. Variable excitation wavelengths are utilized as an external perturbation. Based on the results of mathematical analysis and computer simulation, we find that no cross peak will be produced on the 2D asynchronous spectrum if the fluorescent solute under investigation occurs in a single micro-environment. The observation of cross peaks implies that the fluorescent molecule may occur in different micro-environments in a solution. Based on these results, we use 2D asynchronous spectra to investigate the emission spectra of anthracene dissolved in cyclohexane. When the concentration of anthracene is low, no cross peak is produced in the resultant 2D asynchronous spectrum, confirming that anthracene is dissolved as single molecule in the solution. As the concentration elevated, cross peaks appear in the corresponding 2D asynchronous spectra. A plausible explanation of this phenomenon is that anthracene may undergo aggregation via π-π interaction or π-C-H interaction.

  10. On the concentration dependence of wings of spectra of spin correlation functions of diluted Heisenberg paramagnets

    NASA Astrophysics Data System (ADS)

    Zobov, V. E.; Kucherov, M. M.

    2016-06-01

    Singular points of the autocorrelation function on the imaginary time axis that is averaged over the location of spins in the magnetically dilute spin lattice with isotropic spin-spin interaction at a high temperature have been studied. For the autocorrelation function in the approximation of the self-consistent fluctuating local field, nonlinear integral equations have been proposed which reflect the separation of the inhomogeneous spin systems into close spins and other spins. The coordinates of the nearest singular points have been determined in terms of the radius of convergence of the expansion in powers of time, the coefficients of which have been calculated from recurrence equations. It has been shown that the coordinates of singular points and, consequently, the wings of the autocorrelation function spectrum at strong magnetic dilution are determined by the modulation of the local field by the nearest pairs of spins leading to its logarithmic concentration dependence.

  11. Collective spin excitations in bicomponent magnonic crystals consisting of bilayer permalloy/Fe nanowires

    NASA Astrophysics Data System (ADS)

    Gubbiotti, G.; Tacchi, S.; Madami, M.; Carlotti, G.; Yang, Z.; Ding, J.; Adeyeye, A. O.; Kostylev, M.

    2016-05-01

    In the developing field of magnonics, it is very important to achieve tailoring of spin wave propagation by both a proper combination of materials with different magnetic properties and their nanostructuring on the submicrometric scale. With this in mind, we have exploited deep ultraviolet lithography, in combination with the tilted shadow deposition technique, to fabricate arrays of closely spaced bilayer nanowires (NWs), with separation d =100 nm and periodicity a =440 nm , having bottom and top layers made of permalloy and iron, respectively. The NWs have either a "rectangular" cross section (bottom and upper layers of equal width) or an "L-shaped" cross section (upper layer of half width). The frequency dispersion of collective spin wave excitations in the above bilayered NW arrays has been measured by the Brillouin light-scattering technique while sweeping the wave vector perpendicularly to the wire length over three Brillouin zones of the reciprocal space. For the rectangular NWs, the lowest-frequency fundamental mode, characterized by a quasiuniform profile of the amplitude of the dynamic magnetization across the NW width, exhibits a sizable and periodic frequency dispersion. A similar dispersive mode is also present in L-shaped NWs, but the mode amplitude is concentrated in the thin side of the NWs. The width and the center frequency of the magnonic band associated with the above fundamental modes have been analyzed, showing that both can be tuned by varying the external applied field. Moreover, for the L-shaped NWs it is shown that there is also a second dispersive mode, at higher frequency, characterized by an amplitude concentrated in the thick side of the NW. These experimental results have been quantitatively reproduced by an original numerical model that includes a two-dimensional Green's function description of the dipole field of the dynamic magnetization and interlayer exchange coupling between the layers.

  12. The mutable nature of particle-core excitations with spin in the one-valence-proton nucleus 133Sb

    NASA Astrophysics Data System (ADS)

    Bocchi, G.; Leoni, S.; Fornal, B.; Colò, G.; Bortignon, P. F.; Bottoni, S.; Bracco, A.; Michelagnoli, C.; Bazzacco, D.; Blanc, A.; de France, G.; Jentschel, M.; Köster, U.; Mutti, P.; Régis, J.-M.; Simpson, G.; Soldner, T.; Ur, C. A.; Urban, W.; Fraile, L. M.; Lozeva, R.; Belvito, B.; Benzoni, G.; Bruce, A.; Carroll, R.; Cieplicka-Oryǹczak, N.; Crespi, F. C. L.; Didierjean, F.; Jolie, J.; Korten, W.; Kröll, T.; Lalkovski, S.; Mach, H.; Mărginean, N.; Melon, B.; Mengoni, D.; Million, B.; Nannini, A.; Napoli, D.; Olaizola, B.; Paziy, V.; Podolyák, Zs.; Regan, P. H.; Saed-Samii, N.; Szpak, B.; Vedia, V.

    2016-09-01

    The γ-ray decay of excited states of the one-valence-proton nucleus 133Sb has been studied using cold-neutron induced fission of 235U and 241Pu targets, during the EXILL campaign at the ILL reactor in Grenoble. By using a highly efficient HPGe array, coincidences between γ-rays prompt with the fission event and those delayed up to several tens of microseconds were investigated, allowing to observe, for the first time, high-spin excited states above the 16.6 μs isomer. Lifetimes analysis, performed by fast-timing techniques with LaBr3(Ce) scintillators, revealed a difference of almost two orders of magnitude in B(M1) strength for transitions between positive-parity medium-spin yrast states. The data are interpreted by a newly developed microscopic model which takes into account couplings between core excitations (both collective and non-collective) of the doubly magic nucleus 132Sn and the valence proton, using the Skyrme effective interaction in a consistent way. The results point to a fast change in the nature of particle-core excitations with increasing spin.

  13. Theoretical Determination of Electronic Spectra and Intersystem Spin-Orbit Coupling: The Case of Isoindole-BODIPY Dyes.

    PubMed

    Alberto, Marta E; De Simone, Bruna C; Mazzone, Gloria; Quartarolo, Angelo D; Russo, Nino

    2014-09-01

    Density functional theory and its time-dependent extension (DFT, TDDFT) has been herein employed to elucidate the structural and electronic properties for a series of isoindole-boron dipyrromethene (isoindole-BODIPY) derivatives. The role played by both the nature and the positions of the substituents on intersystem spin-crossing has been investigated computing the spin-orbit matrix elements between singlet and triplet excited state wave functions weighted by the TDDFT transition coefficients. Their potential therapeutic use as photosensitizers in photodynamic therapy (PDT) is proposed on the basis of their strong absorbance in the red part of the visible spectrum, vertical triplet energies resulting higher than 0.98 eV, and the spin-orbit matrix elements that result to be comparable with different drugs already used in PDT. PMID:26588544

  14. Nucleon, Delta and Omega excited state spectra at three pion mass values

    SciTech Connect

    John Bulava, Robert G. Edwards, Balint Joo, David G. Richards, Eric Engelson, Huey-Wen Lin, Colin Morningstar, Stephen J. Wallace

    2010-06-01

    The energies of the excited states of the Nucleon, Delta and Omega are computed in lattice QCD, using two light quarks and one strange quark on anisotropic lattices. The calculations are performed at three values of the pion mass: 392(4), 438(3) and 521(3) MeV. We employ the variational method with a basis of about ten interpolating operators enabling six energies to be distinguished clearly in each irreducible representation of the octahedral group. We compare our calculations of nucleon excited states with the low-lying experimental spectrum. There is reasonable agreement for the pattern of states.

  15. Nuclear response theory for spin-isospin excitations in a relativistic quasiparticle-phonon coupling framework

    NASA Astrophysics Data System (ADS)

    Robin, Caroline; Litvinova, Elena

    2016-07-01

    A new theoretical approach to spin-isospin excitations in open-shell nuclei is presented. The developed method is based on the relativistic meson-exchange nuclear Lagrangian of Quantum Hadrodynamics and extends the response theory for superfluid nuclear systems beyond relativistic quasiparticle random phase approximation in the proton-neutron channel (pn-RQRPA). The coupling between quasiparticle degrees of freedom and collective vibrations (phonons) introduces a time-dependent effective interaction, in addition to the exchange of pion and ρ -meson taken into account without retardation. The time-dependent contributions are treated in the resonant time-blocking approximation, in analogy to the previously developed relativistic quasiparticle time-blocking approximation (RQTBA) in the neutral (non-isospin-flip) channel. The new method is called proton-neutron RQTBA (pn-RQTBA) and is applied to the Gamow-Teller resonance in a chain of neutron-rich nickel isotopes 68-78Ni . A strong fragmentation of the resonance along with quenching of the strength, as compared to pn-RQRPA, is obtained. Based on the calculated strength distribution, beta-decay half-lives of the considered isotopes are computed and compared to pn-RQRPA half-lives and to experimental data. It is shown that a considerable improvement of the half-life description is obtained in pn-RQTBA because of the spreading effects, which bring the lifetimes to a very good quantitative agreement with data.

  16. The fluorescence action spectra of some saturated hydrocarbon liquids for excitation energies above and below their ionization thresholds

    SciTech Connect

    Ostafin, A.E.; Lipsky, S. )

    1993-04-01

    Fluorescence action spectra have been obtained for the neat liquids, [ital cis]-decalin, [ital trans]-decalin, bicyclohexyl, cyclohexane, methylcyclohexane, isobutylcyclohexane, 2,3,4-trimethylpentane, 2,3-dimethylbutane, 3-methylhexane, 3-methylpentane, [ital n]-decane, [ital n]-dodecane, and [ital n]-pentadecane at excitation energies, [epsilon], ranging from their absorption onsets (at ca. 7 eV) to 10.3 eV. For all compounds, with the exception of [ital cis]-decalin, the fluorescence quantum yield is observed to monotonically decline with increasing [epsilon], reaching a minimum value at an energy, [epsilon][sub [ital m

  17. Two-dimensional attractive Fermi gases' excitations and radio-frequency spectra across the BEC/BCS crossover

    NASA Astrophysics Data System (ADS)

    Hazzard, Kaden

    2012-06-01

    We calculate the radio-frequency spectra of two-dimensional attractive Fermi gases, including final state interactions, motivated by recent measurements by the groups of Koehl, Thomas, and Zwierlein. The calculation includes coherent excitations generated by the radio-frequency probe on top of the mean field solution. We find that although the gap is identical to the two particle theory, spectral shapes are modified both by many-body effects and by final state interactions. We compare these shapes to experimental measurements.

  18. Atomistic modeling of two-dimensional electronic spectra and excited-state dynamics for a Light Harvesting 2 complex.

    PubMed

    van der Vegte, C P; Prajapati, J D; Kleinekathöfer, U; Knoester, J; Jansen, T L C

    2015-01-29

    The Light Harvesting 2 (LH2) complex is a vital part of the photosystem of purple bacteria. It is responsible for the absorption of light and transport of the resulting excitations to the reaction center in a highly efficient manner. A general description of the chromophores and the interaction with their local environment is crucial to understand this highly efficient energy transport. Here we include this interaction in an atomistic way using mixed quantum-classical (molecular dynamics) simulations of spectra. In particular, we present the first atomistic simulation of nonlinear optical spectra for LH2 and use it to study the energy transport within the complex. We show that the frequency distributions of the pigments strongly depend on their positions with respect to the protein scaffold and dynamics of their local environment. Furthermore, we show that although the pigments are closely packed the transition frequencies of neighboring pigments are essentially uncorrelated. We present the simulated linear absorption spectra for the LH2 complex and provide a detailed explanation of the states responsible for the observed two-band structure. Finally, we discuss the energy transfer within the complex by analyzing population transfer calculations and 2D spectra for different waiting times. We conclude that the energy transfer from the B800 ring to the B850 ring is mediated by intermediate states that are delocalized over both rings, allowing for a stepwise downhill energy transport.

  19. Adsorption geometry and core excitation spectra of three phenylpropene isomers on Cu(111)

    SciTech Connect

    Kolczewski, C.; Williams, F. J.; Cropley, R. L.; Vaughan, O. P. H.; Urquhart, A. J.; Tikhov, M. S.; Lambert, R. M.; Hermann, K.

    2006-07-21

    Theoretical C 1s near edge x-ray absorption fine structure (NEXAFS) spectra for the C{sub 9}H{sub 10} isomers trans-methylstyrene, {alpha}-methylstyrene, and allylbenzene in gas phase and adsorbed at Cu(111) surfaces have been obtained from density functional theory calculations where adsorbate geometries were determined by corresponding total energy optimizations. The three species show characteristic differences in widths and peak shapes of the lowest C 1s{yields}{pi}* transitions which are explained by different coupling of the {pi}-electron system of the C{sub 6} ring with that of the side chain in the molecules as well as by the existence of nonequivalent carbon centers. The adsorbed molecules bind only weakly with the substrate which makes the use of theoretical NEXAFS spectra of the oriented free molecules meaningful for an interpretation of experimental angle-resolved NEXAFS spectra of the adsorbate systems obtained in this work. However, a detailed quantitative account of relative peak intensities requires theoretical angle-resolved NEXAFS spectra of the complete adsorbate systems which have been evaluated within the surface cluster approach. The comparison with experiment yields almost perfect agreement and confirms the reliability of the calculated equilibrium geometries of the adsorbates. This can help to explain observed differences in the catalytic epoxidation of the three molecules on Cu(111) based on purely geometric considerations.

  20. Raman spectra of normal and cancerous mouse mammary gland tissue using near infrared excitation energy

    NASA Astrophysics Data System (ADS)

    Naik, Vaman; Serhatkulu, G. K.; Dai, H.; Shukla, N.; Weber, R.; Thakur, J. S.; Freeman, D. C.; Pandya, A. K.; Auner, G. W.; Naik, R.; Miller, R. F.; Cao, A.; Klein, M. D.; Rabah, R.

    2006-03-01

    Raman spectra of normal mammary gland tissues, malignant mammary gland tumors, and lymph nodes have been recorded using fresh tissue from mice. Tumors were induced in mice by subcutaneously injecting 4T1 BALB/c mammary tumor (a highly malignant) cell line. The Raman spectra were collected using the same tissues that were examined by histopathology for determining the cancerous/normal state of the tissue. Differences in various peak intensities, peak shifts and peak ratios were analyzed to determine the Raman spectral features that differentiate mammary gland tumors from non-tumorous tissue. Tissues that were confirmed by pathology as cancerous (tumors) show several distinctive features in the Raman spectra compared to the spectra of the normal tissues. For example, the cancerous tissues show Raman peaks at 621, 642, 1004, 1032, 1175 and 1208 cm-1 that are assignable to amino acids containing aromatic side-chains such as phenylalanine, tryptophan and tyrosine. Further, the cancerous tissues show a greatly reduced level of phospholipids compared to the normal tissues. The Raman spectral regions that are sensitive to pathologic alteration in the tissue will be discussed.

  1. High-spin states in the semimagic nucleus 89Y and neutron-core excitations in the N =50 isotones

    NASA Astrophysics Data System (ADS)

    Li, Z. Q.; Wang, S. Y.; Niu, C. Y.; Qi, B.; Wang, S.; Sun, D. P.; Liu, C.; Xu, C. J.; Liu, L.; Zhang, P.; Wu, X. G.; Li, G. S.; He, C. Y.; Zheng, Y.; Li, C. B.; Yu, B. B.; Hu, S. P.; Yao, S. H.; Cao, X. P.; Wang, J. L.

    2016-07-01

    The semimagic nucleus 89Y 89 has been investigated using the 82Se(11>B,4 n ) reaction at beam energies of 48 and 52 MeV. More than 24 new transitions have been identified, leading to a considerable extension of the level structures of 89Y. The experimental results are compared with the large-basis shell model calculations. They show that cross-shell neutron excitations play a pivotal role in high-spin level structures of 89Y. The systematic features of neutron-core excitations in the N =50 isotones are also discussed.

  2. A generalized tool for accurate time-domain separation of excited modes in spin-torque oscillators

    SciTech Connect

    Siracusano, Giulio Puliafito, Vito; Finocchio, Giovanni

    2014-05-07

    We propose and develop an advanced signal processing technique that, combined with micromagnetic simulations, is able to deeply describe the non-stationary behavior of spin-torque oscillators, both in terms of time domain and spatial distribution of the magnetization dynamics. The Hilbert-Huang Transform is used for the identification of the time traces of each oscillation in a multimode excitation and enhanced with masking signals and the Ensemble Empirical Mode Decomposition. We emphasize that the technique developed here is general and can be used for any physical non-linear system in the presence of multimode dynamical excitation or intermittence.

  3. Effect of Fermi surface nesting on resonant spin excitations in Ba{<_1-x}K{<_x}Fe{<_2}As{<_2}.

    SciTech Connect

    Castellan, J.-P.; Rosenkranz, S.; Goremychkin, E.A.; Chung, D.Y.; Todorov, I.S.; Kanatzidis, M.G.; Eremin, I.; Knolle, J.; Chubukov, A.V.; Maiti, s.; Norman, M.R.; Weber, F.; Claus, H.; Guidi, T.; Bewley, R.I.; Osborn, R.

    2011-01-01

    We report inelastic neutron scattering measurements of the resonant spin excitations in Ba{sub 1-x}K{sub x}Fe{sub 2}As{sub 2} over a broad range of electron band filling. The fall in the superconducting transition temperature with hole doping coincides with the magnetic excitations splitting into two incommensurate peaks because of the growing mismatch in the hole and electron Fermi surface volumes, as confirmed by a tight-binding model with s{sub {+-}}-symmetry pairing. The reduction in Fermi surface nesting is accompanied by a collapse of the resonance binding energy and its spectral weight, caused by the weakening of electron-electron correlations.

  4. Correlation between electron spin resonance spectra and oil yield in eastern oil shales

    USGS Publications Warehouse

    Choudhury, M.; Rheams, K.F.; Harrell, J.W.

    1986-01-01

    Organic free radical spin concentrations were measured in 60 raw oil shale samples from north Alabama and south Tennessee and compared with Fischer assays and uranium concentrations. No correlation was found between spin concentration and oil yield for the complete set of samples. However, for a 13 sample set taken from a single core hole, a linear correlation was obtained. No correlation between spin concentration and uranium concentration was found. ?? 1986.

  5. Excitations, optical absorption spectra, and optical excitonic gaps of heterofullerenes. I. C60, C59N+, and C48N12: theory and experiment.

    PubMed

    Xie, Rui-Hua; Bryant, Garnett W; Sun, Guangyu; Nicklaus, Marc C; Heringer, David; Frauenheim, Th; Manaa, M Riad; Smith, Vedene H; Araki, Yasuyuki; Ito, Osamu

    2004-03-15

    Low-energy excitations and optical absorption spectrum of C(60) are computed by using time-dependent (TD) Hartree-Fock, TD-density functional theory (TD-DFT), TD DFT-based tight-binding (TD-DFT-TB), and a semiempirical Zerner intermediate neglect of diatomic differential overlap method. A detailed comparison of experiment and theory for the excitation energies, optical gap, and absorption spectrum of C(60) is presented. It is found that electron correlations and correlation of excitations play important roles in accurately assigning the spectral features of C(60), and that the TD-DFT method with nonhybrid functionals or a local spin density approximation leads to more accurate excitation energies than with hybrid functionals. The level of agreement between theory and experiment for C(60) justifies similar calculations of the excitations and optical absorption spectrum of a monomeric azafullerene cation C(59)N(+), to serve as a spectroscopy reference for the characterization of carborane anion salts. Although it is an isoelectronic analogue to C(60), C(59)N(+) exhibits distinguishing spectral features different from C(60): (1) the first singlet is dipole-allowed and the optical gap is redshifted by 1.44 eV; (2) several weaker absorption maxima occur in the visible region; (3) the transient triplet-triplet absorption at 1.60 eV (775 nm) is much broader and the decay of the triplet state is much faster. The calculated spectra of C(59)N(+) characterize and explain well the measured ultraviolet-visible (UV-vis) and transient absorption spectra of the carborane anion salt [C(59)N][Ag(CB(11)H(6)Cl(6))(2)] [Kim et al., J. Am. Chem. Soc. 125, 4024 (2003)]. For the most stable isomer of C(48)N(12), we predict that the first singlet is dipole-allowed, the optical gap is redshifted by 1.22 eV relative to that of C(60), and optical absorption maxima occur at 585, 528, 443, 363, 340, 314, and 303 nm. We point out that the characterization of the UV-vis and transient absorption

  6. Excitations, optical absorption spectra, and optical excitonic gaps of heterofullerenes. I. C60, C59N+, and C48N12: Theory and experiment

    NASA Astrophysics Data System (ADS)

    Xie, Rui-Hua; Bryant, Garnett W.; Sun, Guangyu; Nicklaus, Marc C.; Heringer, David; Frauenheim, Th.; Manaa, M. Riad; Smith, Vedene H.; Araki, Yasuyuki; Ito, Osamu

    2004-03-01

    Low-energy excitations and optical absorption spectrum of C60 are computed by using time-dependent (TD) Hartree-Fock, TD-density functional theory (TD-DFT), TD DFT-based tight-binding (TD-DFT-TB), and a semiempirical Zerner intermediate neglect of diatomic differential overlap method. A detailed comparison of experiment and theory for the excitation energies, optical gap, and absorption spectrum of C60 is presented. It is found that electron correlations and correlation of excitations play important roles in accurately assigning the spectral features of C60, and that the TD-DFT method with nonhybrid functionals or a local spin density approximation leads to more accurate excitation energies than with hybrid functionals. The level of agreement between theory and experiment for C60 justifies similar calculations of the excitations and optical absorption spectrum of a monomeric azafullerene cation C59N+, to serve as a spectroscopy reference for the characterization of carborane anion salts. Although it is an isoelectronic analogue to C60, C59N+ exhibits distinguishing spectral features different from C60: (1) the first singlet is dipole-allowed and the optical gap is redshifted by 1.44 eV; (2) several weaker absorption maxima occur in the visible region; (3) the transient triplet-triplet absorption at 1.60 eV (775 nm) is much broader and the decay of the triplet state is much faster. The calculated spectra of C59N+ characterize and explain well the measured ultraviolet-visible (UV-vis) and transient absorption spectra of the carborane anion salt [C59N][Ag(CB11H6Cl6)2] [Kim et al., J. Am. Chem. Soc. 125, 4024 (2003)]. For the most stable isomer of C48N12, we predict that the first singlet is dipole-allowed, the optical gap is redshifted by 1.22 eV relative to that of C60, and optical absorption maxima occur at 585, 528, 443, 363, 340, 314, and 303 nm. We point out that the characterization of the UV-vis and transient absorption spectra of C48N12 isomers is helpful in

  7. Model Calculations with Excited Nuclear Fragmentations and Implications of Current GCR Spectra

    NASA Astrophysics Data System (ADS)

    Saganti, Premkumar

    As a result of the fragmentation process in nuclei, energy from the excited states may also contribute to the radiation damage on the cell structure. Radiation induced damage to the human body from the excited states of oxygen and several other nuclei and its fragments are of a concern in the context of the measured abundance of the current galactic cosmic rays (GCR) environment. Nuclear Shell model based calculations of the Selective-Core (Saganti-Cucinotta) approach are being expanded for O-16 nuclei fragments into N-15 with a proton knockout and O-15 with a neutron knockout are very promising. In our on going expansions of these nuclear fragmentation model calculations and assessments, we present some of the prominent nuclei interactions from a total of 190 isotopes that were identified for the current model expansion based on the Quantum Multiple Scattering Fragmentation Model (QMSFRG) of Cucinotta. Radiation transport model calculations with the implementation of these energy level spectral characteristics are expected to enhance the understanding of radiation damage at the cellular level. Implications of these excited energy spectral calculations in the assessment of radiation damage to the human body may provide enhanced understanding of the space radiation risk assessment.

  8. Laser-excited fluorescence and electron-spin resonance of Er3+ in polycrystalline AlCl3

    NASA Astrophysics Data System (ADS)

    Ceotto, G.; Pires, M. A.; Sanjurjo, J. A.; Rettori, C.; Barberis, G. E.

    1990-07-01

    The green fluorescence transitions among the levels corresponding to the 4S3/2 and 4I15/2 configurations of Er3+ diluted in AlCl3 have been measured using laser excitation. The data allow us to determine the crystalline-field splittings of these levels and, in turn, the spin-Hamiltonian parameters. The electron-paramagnetic-resonance spectrum observed at low temperatures is in good agreement with that expected from these parameters.

  9. [Density functional theory study of surface-enhanced raman spectra and excited state of 1,4-benzenedithiol].

    PubMed

    Shao, Yang-Fan; Li, Chong-Yang; Feng, Yuan-Ming; Lin, Wang

    2014-02-01

    Raman scattering spectra and optimized geometries of the 1,4-benzenedithiol molecule and complexes have been calculated using density functional theory (DFT) with B3LYP functional at the level of 6-311G+(d) basis set for C, H, S atoms and LanL2DZ for Ag, Au atoms, respectively. The optimized 1,4-benzenedithiol molecule was non-planar structure and the angle between benzene ring plane and S-H is 20.20. By means of the simulation of molecule adsorbed on gold and silver cluster, we concluded that gold clusters are nearly parallel to the benzenedithiol molecule and silver clusters are almost perpendicular to the molecular surface. The authors studied the interaction between Raman intensity and molecular properties, such as static polarizablity and charge distribution. The Raman intensity of 1,4-BDT-Au2, 1,4-BDT-Ag2 and Ag2-1,4-BDT-Au2 were in good agreement with static polarizability. The excited states of Ag2-1,4-BDT-Au2 complex were calculated using time-dependent density functional theory (TDDFT). And the simulated absorption spectra and several allowed singlet excited states were analyzed to investigate the surface-enhanced Raman chemical enhancement mechanism. PMID:24822413

  10. Magnetic structure and spin excitations in BaMn2Bi2

    SciTech Connect

    Calder, Stuart A.; Saparov, Bayrammurad I; Cao, H. B.; Niedziela, Jennifer L.; Lumsden, Mark D.; Sefat, Athena Safa; Christianson, Andrew D.

    2014-02-19

    We present a single crystal neutron scattering study of BaMn2Bi2, a recently synthesized material with the same ThCr2Si2type structure found in several Fe-based unconventional superconducting materials. We show long range magnetic order, in the form of a G-type antiferromagnetic structure, to exist up to 390 K with an indication of a structural transition at 100 K. Utilizing inelastic neutron scattering we observe a spin-gap of 16 meV, with spin-waves extending up to 55 meV. We find these magnetic excitations are well fit to a J1-J2-Jc Heisenberg model and present values for the exchange interactions. The spin wave spectrum appears to be unchanged by the 100 K structural phase transition.

  11. Multi-angle Spectra Evolution of Langmuir Turbulence Excited by RF Ionospheric Interactions at HAARP

    NASA Astrophysics Data System (ADS)

    Sheerin, J. P.; Rayyan, N.; Watkins, B. J.; Bristow, W. A.; Spaleta, J.; Watanabe, N.; Golkowski, M.; Bernhardt, P. A.

    2013-12-01

    The high power HAARP HF transmitter is employed to generate and study strong Langmuir turbulence (SLT) in the interaction region of overdense ionospheric plasma. Diagnostics included the Modular UHF Ionospheric Radar (MUIR) sited at HAARP, the SuperDARN-Kodiak HF radar, and HF receivers to record stimulated electromagnetic emissions (SEE). Dependence of diagnostic signals on HAARP HF parameters, including pulselength, duty-cycle, aspect angle, and frequency were recorded. Short pulse, low duty cycle experiments demonstrate control of artificial field-aligned irregularities (AFAI) and isolation of ponderomotive effects. Among the effects observed and studied are: SLT spectra including cascade, collapse, and co-existence spectra and an outshifted plasma line under certain ionospheric conditions. High time resolution studies of the temporal evolution of the plasma line reveal the appearance of an overshoot effect on ponderomotive timescales. Bursty turbulence is observed in the collapse and cascade lines. For the first time, simultaneous multi-angle radar measurements of plasma line spectra are recorded demonstrating marked dependence on aspect angle with the strongest interaction region observed displaced southward of the HF zenith pointing angle. Numerous measurements of the outshifted plasma line are observed. Experimental results are compared to previous high latitude experiments and predictions from recent modeling efforts.

  12. Floquet-Magnus expansion for general N-coupled spins systems in magic-angle spinning nuclear magnetic resonance spectra

    NASA Astrophysics Data System (ADS)

    Mananga, Eugene Stephane; Charpentier, Thibault

    2015-04-01

    In this paper we present a theoretical perturbative approach for describing the NMR spectrum of strongly dipolar-coupled spin systems under fast magic-angle spinning. Our treatment is based on two approaches: the Floquet approach and the Floquet-Magnus expansion. The Floquet approach is well known in the NMR community as a perturbative approach to get analytical approximations. Numerical procedures are based on step-by-step numerical integration of the corresponding differential equations. The Floquet-Magnus expansion is a perturbative approach of the Floquet theory. Furthermore, we address the " γ -encoding" effect using the Floquet-Magnus expansion approach. We show that the average over " γ " angle can be performed for any Hamiltonian with γ symmetry.

  13. Solvent Effects on the Electronic Absorption and Fluorescence Spectra of HNP: Estimation of Ground and Excited State Dipole Moments.

    PubMed

    Desai, Vani R; Hunagund, Shirajahammad M; Basanagouda, Mahantesha; Kadadevarmath, Jagadish S; Sidarai, Ashok H

    2016-07-01

    We report the effect of solvents on absorption and fluorescence spectra of biologically active 3(2H)-pyridazinone namely 5-(2-hydroxy-naphthalen-1-yl)-2-phenyl-2H-pyridazin-3-one (HNP) in different solvents at room temperature. The ground and the excited state dipole moments of HNP molecule was estimated from Lippert's, Bakshiev's and Kawski-Chamma-Viallet's equations using the solvatochromic shift method. The ground state dipole moment (μ g ) was also estimated by Guggenheim and Higasi method using the dielectric constant and refractive index of solute at different concentrations, the μ g value obtained from these two methods are comparable to the μ g value obtained by the solvatochromic shift method. The excited state dipole moment (μ e ) is greater than the ground state dipole moment (μ g ), which indicates that the excited state is more polar than the ground state. Further, we have evaluated the change in dipole moment (Δμ) from the solvatochromic shift method and on the basis of molecular-microscopic solvent polarity parameter[Formula: see text], later on the values were compared. PMID:27220623

  14. Assignments of Lowest Triplet State in Ir Complexes by Observation of Phosphorescence Excitation Spectra at 6 K

    NASA Astrophysics Data System (ADS)

    Kodate, Satoshi; Suzuka, Isamu

    2006-01-01

    We tried the assignment of the origin of phosphorescent bands in Ir complexes. It is important to elucidate the luminescent mechanism in order to design organic light-emitting devices (OLEDs) besed on new materials. The Stokes shift between the phosphorescence and phosphorescence excitation spectra of Ir complexes such as fac-tris(2-phenylpyridine) iridium(III) [Ir(ppy)3], fac-tris(2-(2-thienyl)pyridine) iridium(III) [Ir(thpy)3], bis(2-phenylpyridine) iridium(III)benzo[h]quinoline [Ir(ppy)2bzq], fac-tris(benzo[h]quinoline) iridium(III) [Ir(bzq)3] and bis[(4,6-difluorophenyl)pyridinato](picolinato) iridium(III) [FIrpic] was measured in a solution and (phenyl)4Sn at 6 K. The amount of Stokes shift corresponds to the nature of the lowest triplet state. We discovered that the amount of Stokes shift clearly differs depending on whether the lowest triplet state of each Ir complex is triplet metal-to-ligand charge transfer (3MLCT) or 3π-π*. Namely, the case of 3MLCT shows a large shift, while the case of 3π-π* shows a small shift. We also present the resolved phosphorescence and phosphorescence excitation spectra of Ir complexes in (phenyl)4Sn. The sharp bands were assigned to the 3π-π* transition, and the broad bands were assigned to the 3MLCT state. The nature of the lowest triplet state is also discussed on the basis of resolved spectra.

  15. On the truncation of the number of excited states in density functional theory sum-over-states calculations of indirect spin spin coupling constants

    NASA Astrophysics Data System (ADS)

    Zarycz, M. Natalia C.; Provasi, Patricio F.; Sauer, Stephan P. A.

    2015-12-01

    It is investigated, whether the number of excited (pseudo)states can be truncated in the sum-over-states expression for indirect spin-spin coupling constants (SSCCs), which is used in the Contributions from Localized Orbitals within the Polarization Propagator Approach and Inner Projections of the Polarization Propagator (IPPP-CLOPPA) approach to analyzing SSCCs in terms of localized orbitals. As a test set we have studied the nine simple compounds, CH4, NH3, H2O, SiH4, PH3, SH2, C2H2, C2H4, and C2H6. The excited (pseudo)states were obtained from time-dependent density functional theory (TD-DFT) calculations with the B3LYP exchange-correlation functional and the specialized core-property basis set, aug-cc-pVTZ-J. We investigated both how the calculated coupling constants depend on the number of (pseudo)states included in the summation and whether the summation can be truncated in a systematic way at a smaller number of states and extrapolated to the total number of (pseudo)states for the given one-electron basis set. We find that this is possible and that for some of the couplings it is sufficient to include only about 30% of the excited (pseudo)states.

  16. On the truncation of the number of excited states in density functional theory sum-over-states calculations of indirect spin spin coupling constants

    SciTech Connect

    Zarycz, M. Natalia C. Provasi, Patricio F.; Sauer, Stephan P. A.

    2015-12-28

    It is investigated, whether the number of excited (pseudo)states can be truncated in the sum-over-states expression for indirect spin-spin coupling constants (SSCCs), which is used in the Contributions from Localized Orbitals within the Polarization Propagator Approach and Inner Projections of the Polarization Propagator (IPPP-CLOPPA) approach to analyzing SSCCs in terms of localized orbitals. As a test set we have studied the nine simple compounds, CH{sub 4}, NH{sub 3}, H{sub 2}O, SiH{sub 4}, PH{sub 3}, SH{sub 2}, C{sub 2}H{sub 2}, C{sub 2}H{sub 4}, and C{sub 2}H{sub 6}. The excited (pseudo)states were obtained from time-dependent density functional theory (TD-DFT) calculations with the B3LYP exchange-correlation functional and the specialized core-property basis set, aug-cc-pVTZ-J. We investigated both how the calculated coupling constants depend on the number of (pseudo)states included in the summation and whether the summation can be truncated in a systematic way at a smaller number of states and extrapolated to the total number of (pseudo)states for the given one-electron basis set. We find that this is possible and that for some of the couplings it is sufficient to include only about 30% of the excited (pseudo)states.

  17. On the truncation of the number of excited states in density functional theory sum-over-states calculations of indirect spin spin coupling constants.

    PubMed

    Zarycz, M Natalia C; Provasi, Patricio F; Sauer, Stephan P A

    2015-12-28

    It is investigated, whether the number of excited (pseudo)states can be truncated in the sum-over-states expression for indirect spin-spin coupling constants (SSCCs), which is used in the Contributions from Localized Orbitals within the Polarization Propagator Approach and Inner Projections of the Polarization Propagator (IPPP-CLOPPA) approach to analyzing SSCCs in terms of localized orbitals. As a test set we have studied the nine simple compounds, CH4, NH3, H2O, SiH4, PH3, SH2, C2H2, C2H4, and C2H6. The excited (pseudo)states were obtained from time-dependent density functional theory (TD-DFT) calculations with the B3LYP exchange-correlation functional and the specialized core-property basis set, aug-cc-pVTZ-J. We investigated both how the calculated coupling constants depend on the number of (pseudo)states included in the summation and whether the summation can be truncated in a systematic way at a smaller number of states and extrapolated to the total number of (pseudo)states for the given one-electron basis set. We find that this is possible and that for some of the couplings it is sufficient to include only about 30% of the excited (pseudo)states.

  18. A simple method to determine bond lengths and excited state surfaces from electronic-vibrational spectra

    NASA Astrophysics Data System (ADS)

    Lee, Soo-Y.; Lai, Choy-Heng

    1990-03-01

    A fast and efficient method using the spectral moments of an electronic—vibrational spectrum is described to determine the harmonic and Morse potential fits to the excited state potential in the Franck—Condon region. Some of the drawbacks of the Franck—Condon least-squares fitting procedure are overcome by the moment method. The method is applied to some diatomics of current interest, spanning a wide range of bond length change in the electronic transition. The accuracy of the results suggests that the spectral moment method can be a replacement for the traditional and still popular Franck—Condon analysis.

  19. Analytically useful spectra excited in an atmospheric pressure active nitrogen afterglow

    SciTech Connect

    Rice, G.W.; D'Silva, A.P.; Fassel, V.A.

    1984-03-01

    An atmospheric pressure active nitrogen (APAN) discharge has been utilized for producing characteristic molecular emissions from nonmetallic species introduced into the afterglow region of the discharge. The addition of inorganic S-, P-, B-, Cl-, and Br-containing compounds into the afterglow has resulted in the formation of excited S/sub 2/, PN, BO, NCl, and NBr species, respectively. Intense molecular Br/sub 2/ emission and I/sub 2/ emission, as well as atomic I emission, have also been observed. Preliminary analytical utilization of the molecular or atomic emissions observed revealed that the APAN afterglow may serve as a potentially useful detector for the aforementioned elements.

  20. Jet-Cooled Excitation Spectra of Large Benzannulated Benzyl Radicals: 9-ANTHRACENYLMETHYL (C_{15}H_{11}) and 1-PYRENYLMETHYL (C_{17}H_{11})

    NASA Astrophysics Data System (ADS)

    O'Connor, Gerard D.; Bacskay, George B.; Woodhouse, Gabrielle V. G.; Troy, Tyler P.; Nauta, Klaas; Kable, Scott H.; Schmidt, Timothy W.

    2013-06-01

    The jet-cooled D_1 ← D_0 excitation spectra of two benzannulated benzyl radicals (BBRs), 9-anthracenylmethyl (9-AnMe) and 1-pyrenylmethyl (9-PyMe), have been obtained using mass-resolved resonant two-colour two-photon ionization spectroscopy (R2C2PI). Analysis of the spectra in view of symmetry and calculated vibrational frequencies indicate significant vibronic coupling. From the spectrum of 9-AnMe we elucidate significant anharmonicity in the excited state. This anharmonic behaviour is examined computationally through both TDDFT and ab initio methods. Excited state properties of 9-AnMe and 1-PyMe are examined with reference to the existing spectra of smaller BBRs. Trends in the observed spectra of BBRs allow spectroscopic properties of larger BBRs to be predicted. These predictions suggest the D_1 ← D_0 transitions of large BBRs are unlikely to be carriers of the diffuse interstellar bands.

  1. Frequency spectra of magnetostrictive and Lorentz forces generated in ferromagnetic materials by a CW excited EMAT

    NASA Astrophysics Data System (ADS)

    Rouge, C.; Lhémery, A.; Aristégui, C.

    2014-04-01

    Magnetostriction arises in ferromagnetic materials subjected to magnetization, e.g., when an EMAT (Electro-Magnetic Acoustic Transducer) is used to generate ultrasonic waves. In such a case, the magnetostriction force must be taken into account as a transduction process that adds up to the Lorentz force. When the static magnetic field is high compared to the dynamic field, both forces are driven by the excitation frequency. For lower static relative values of the magnetic fields, the Lorentz force comprises both the excitation frequency and its first harmonic. In this work, a model is derived to predict the frequency content of the magnetostrictive force that comprises several harmonics. The discrete frequency spectrum strongly depends on both the static field and the relative amplitude of the dynamic field. The only material input data needed to predict it is the curve of macroscopic magnetostrictive strain that can be measured in the direction of an imposed magnetic field. Then, the various frequency-dependent distributions of Lorentz and magnetostriction body forces can be transformed into equivalent surface stresses. Examples of computation are given for different static and dynamic magnetic fields to study their influence on the frequency content of waves generated in ferromagnetic materials.

  2. Theoretical investigation of the molecular structures and excitation spectra of triphenylamine and its derivatives

    NASA Astrophysics Data System (ADS)

    Sumimoto, Michinori; Yokogawa, Daisuke; Komeda, Masahiro; Yamamoto, Hidetoshi; Hori, Kenji; Fujimoto, Hitoshi

    2011-10-01

    The molecular geometries, electronic structures, and excitation energies of NPh 3, NPh 2Me, NPhMe 2, and NMe 3, were investigated using DFT and post-Hartree Fock methods. When the structural stabilities of these compounds were compared to results obtained by using MP4(SDQ) method, it was confirmed that the optimized geometries by using MP2 method were sufficiently reliable. The excited states with large oscillator strengths consisted of transition components from the HOMO. It should be noted that the orbitals of the nitrogen atom mix with the π-orbital of the phenyl group in an anti-bonding way in the HOMO, and the orbital energy increases with this mixing. The unoccupied orbitals are generated from bonding and anti-bonding type interactions between the π-orbitals of the phenyl groups; therefore, the number of phenyl groups strongly affects the energy diagram of the compounds studied. The differences in the energy diagram cause a spectral change in these compounds in the ultraviolet region.

  3. Technical aspects of fast magic-angle turning NMR for dilute spin-1/2 nuclei with broad spectra.

    PubMed

    Hu, Y-Y; Schmidt-Rohr, K

    2011-09-01

    For obtaining sideband-free spectra of high-Z spin-1/2 nuclei with large (>1000 ppm) chemical-shift anisotropies and broad isotropic-shift dispersion, we recently identified Gan's modified five-pulse magic-angle turning (MAT) experiment as the best available broadband pulse sequence, and adapted it to fast magic-angle spinning. Here, we discuss technical aspects such as pulse timings that compensate for off-resonance effects and are suitable for large CSAs over a range of 1.8γB(1); methods to minimize the duration of z-periods by cyclic decrementation; shearing without digitization artifacts, by sharing between channels (points); and maximizing the sensitivity by echo-matched full-Gaussian filtering. The method is demonstrated on a model sample of mixed amino acids and its large bandwidth is highlighted by comparison with the multiple-π-pulse PASS technique. Applications to various tellurides are shown; these include GeTe, Sb(2)Te(3) and Ag(0.53)Pb(18)Sb(1.2)Te(20), with spectra spanning up to 190 kHz, at 22 kHz MAS. We have also determined the (125)Te chemical shift anisotropies from the intensities of the spinning sidebands resolved by isotropic-shift separation. PMID:21782396

  4. Elementary modes of excitation caused by the quadratic Zeeman term and the sensitivity of spin structures of small spin-2 condensates against the magnetic field

    SciTech Connect

    He, Y. Z.; Bao, C. G.

    2011-12-15

    The response of spin-2 small condensates to an external magnetic field B is studied. The parameters of the interaction are considered as variable. The emphasis is placed on clarifying the modes of excitation caused by the quadratic Zeeman term. The theoretical method used is beyond the mean-field theory. A set of eigenstates with the U(5) superset of SO(5) superset of SO(3) symmetry is introduced to facilitate the analysis. To obtain a quantitative evaluation on the response, the fidelity susceptibility and the B-dependent average populations of spin components have been calculated. Mostly the particle number N=30 is assumed. The effect with a larger or smaller N is also considered. It was found that the sensitivity of the response depends strongly both on the interaction and on the inherent symmetry.

  5. Evidence of Polaron Excitations in Low Temperature Raman Spectra of Oxalic Acid Dihydrate.

    PubMed

    Mohaček-Grošev, Vlasta; Grdadolnik, Jože; Hadži, Dušan

    2016-05-12

    Low temperature Raman spectra of oxalic acid dihydrate (8-300 K) for both the polycrystalline and single crystal phase show strong variation with temperature in the interval from 1200 to 2000 cm(-1). Previous low temperature diffraction studies all confirmed the stability of the crystal P21/n phase with no indications of any phase transition, reporting the existence of a strong hydrogen bond between the oxalic acid and a water molecule. A new group of Raman bands in the 1200-1300 cm(-1) interval below 90 K is observed, caused by possible loss of the center of inversion. This in turn could originate either due to disorder in hydroxyl proton positions or due to proton transfer from carboxylic group to water molecule. The hypothesis of proton transfer is further supported by the emergence of new bands centered at 1600 and 1813 cm(-1), which can be explained with vibrations of H3O(+) ions. The broad band at 1600 cm(-1) looses intensity, while the band at 1813 cm(-1) gains intensity on cooling. The agreement between quantum calculations of vibrational spectra and experimentally observed Raman bands of hydronium ions in oxalic acid sesquihydrate crystal corroborates this hypothesis. PMID:27093217

  6. Solid-State Selective 13C Excitation and Spin Diffusion NMR to Resolve Spatial Dimensions in Plant Cell Walls

    SciTech Connect

    Foston, M.; Katahira, R.; Gjersing, E.; Davis, M. F.; Ragauskas, A. J.

    2012-02-15

    The average spatial dimensions between major biopolymers within the plant cell wall can be resolved using a solid-state NMR technique referred to as a {sup 13}C cross-polarization (CP) SELDOM (selectively by destruction of magnetization) with a mixing time delay for spin diffusion. Selective excitation of specific aromatic lignin carbons indicates that lignin is in close proximity to hemicellulose followed by amorphous and finally crystalline cellulose. {sup 13}C spin diffusion time constants (T{sub SD}) were extracted using a two-site spin diffusion theory developed for {sup 13}C nuclei under magic angle spinning (MAS) conditions. These time constants were then used to calculate an average lower-limit spin diffusion length between chemical groups within the plant cell wall. The results on untreated {sup 13}C enriched corn stover stem reveal that the lignin carbons are, on average, located at distances {approx}0.7-2.0 nm from the carbons in hemicellulose and cellulose, whereas the pretreated material had larger separations.

  7. Excitations, optical absorption spectra, and optical excitonic gaps of heterofullerenes: I. C60, C59N+ and C48N12

    SciTech Connect

    Xie, R; Bryant, G W; Sun, G; C.Nicklaus, M; Heringer, D; Frauenheim, T; Manaa, M R; Smith, Jr., V H; Araki, Y; Ito, O

    2003-10-02

    Low-energy excitations and optical absorption spectrum of C{sub 60} are computed by using time-dependent (TD) Hartree-Fock (HF), TD-density functional theory (TD-DFT), TD-DFT-based tight-binding (TD-DFT-TB) and a semiempirical ZINDO method. A detailed comparison of experiment and theory for the excitation energies, optical gap and absorption spectrum of C{sub 60} is presented. It is found that electron correlations and collective effects of exciton pairs play important roles in assigning accurately the spectral features of C{sub 60} and the TD-DFT method with non-hybrid functionals or a local spin density approximation leads to more accurate excitation energies than with hybrid functionals. The level of agreement between theory and experiment for C{sub 60} justifies similar calculations of the excitations and optical absorption spectrum of a monomeric azafullerene cation C{sub 59}N{sup +} exhibits distinguishing spectral features different from C{sub 60}: (1) the first singlet is dipole-allowed and the optical gap is redshifted by 1.44 eV; (2) several weaker absorption maxima occur in the visible region; (3) the transient triplet-triplet absorption at 1.60 eV (775 nm) is much broader and the decay of the triplet state is much faster. The calculated spectra of C{sub 59}N{sup +} characterize and explain well our measured ultraviolet-visible (UV-vis) and transient absorption spectra of the carborane anion salt [C{sub 59}N][Ag(CB{sub 11}H{sub 6}Cl{sub 6}){sub 2}]. For the most stable isomer of C{sub 48}N{sub 12}, we predict that the first singlet is dipole-allowed, the optical gap is redshifted by 1.22 eV relative to that of C{sub 60}, and optical absorption maxima occur at 585, 528, 443, 363, 340, 314 and 303 nm. We point out that the characterization of the UV-vis and transient absorption spectra of C{sub 48}N{sub 12} isomers is helpful in distinguishing the isomer structures required for applications in molecular electronics. For C{sub 59}N{sup +} and C{sub 48}N

  8. TREPR spectra of micelle-confined spin correlated radical pairs: II. Spectral decomposition and asymmetric line shapes.

    PubMed

    Tarasov, Valery F; Jarocha, Lauren E; Forbes, Malcolm D E

    2014-02-01

    In the second paper, spectral decomposition is used to explain the origin of the asymmetry of the anti-phase structure (APS) and its temperature dependence in dynamic spin correlated radical pairs (SCRPs) created via the photoreduction of benzophenone (BP) in sodium dodecyl sulfate (SDS) micelles. It is shown that the main parameters defining the spectral shape of the TREPR spectra are the effectiveness of the electron spin exchange in contact pairs, and the ratio of the frequency of enforced encounters (Z) to the frequency of singlet-triplet mixing (q) in the separated radical pairs. The Z/q ratio is particularly important for the creation of the APS asymmetry. The existence of different q values in the same TREPR spectrum in this system affords the observation of SCRPs in both regimes: exchange broadening (large |q|/Z) and exchange narrowing (small |q|/Z). An important observation, supported by the successful simulation of the TREPR spectra, is that the S-component of the APS can be shifted in a direction opposite to that predicted by the earlier Closs-Forbes-Norris (CFN) model. This result is naturally explained in terms of a spectral exchange approach. Dispersion-like components in the spectra further amplify the asymmetry of the APS.

  9. Exchange-only optimized effective potential calculation of excited state spectra for He and Be atoms.

    SciTech Connect

    Desjarlais, Michael Paul; Muller, Richard Partain

    2006-02-01

    The optimized effective potential (OEP) method allows orbital-dependent functionals to be used in density functional theory (DFT), which, in particular, allows exact exchange formulations of the exchange energy to be used in DFT calculations. Because the exact exchange is inherently self-interaction correcting, the resulting OEP calculations have been found to yield superior band-gaps for condensed-phase systems. Here we apply these methods to the isolated atoms He and Be, and compare to high quality experiments and calculations to demonstrate that the orbital energies accurately reproduce the excited state spectrum for these species. These results suggest that coupling the exchange-only OEP calculations with proper (orbital-dependent or other) correlation functions might allow quantitative accuracy from DFT calculations.

  10. Polarization Dependence of the Spin-Density-Wave Excitations in Single-Domain Chromium

    SciTech Connect

    Boeni, P.; Sternlieb, B.J.; Shirane, G.; Roessli, B.; Werner, S.A.; Lorenzo, J.E.

    1997-12-31

    A polarised neutron scattering experiment has been performed on a single-Q, single domain sample of Cr in a magnetic field of 4 T in the transverse spin-density-wave phase. It is confirmed that the longitudinal fluctuations are enhanced for energy transfers E {lt} 8 meV similarly as in the longitudinal spin-density-wave phase. The spin wave modes with deltaS parallel and perpendicular to Q are isotropic within the E-range investigated.

  11. Spin-wave spectra and stability of the in-plane vortex state in two-dimensional magnetic nanorings

    SciTech Connect

    Mamica, S.

    2013-12-21

    We study theoretically two-dimensional nanorings assumed to have the in-plane vortex magnetic configuration. Using a discrete dipole model we examine the spectrum of normal spin-wave modes vs. the dipolar-to-exchange interaction ratio. We systematize the spin-wave excitations by their azimuthal and radial wave numbers. The lowest-frequency mode, the fundamental (quasiuniform) mode, and the mode hybridization are analyzed; the discussion of the influence of effective pinning at the ring boundaries is provided as well. We study the stability of the in-plane vortex state and discuss the role of the size of the ring and the type of lattice arrangement of the magnetic moments within it. To facilitate comparison with our results we provide the relationships between microscopic parameters, used in our model, and those used in the case of continuous medium.

  12. Spin-wave spectra and stability of the in-plane vortex state in two-dimensional magnetic nanorings

    NASA Astrophysics Data System (ADS)

    Mamica, S.

    2013-12-01

    We study theoretically two-dimensional nanorings assumed to have the in-plane vortex magnetic configuration. Using a discrete dipole model we examine the spectrum of normal spin-wave modes vs. the dipolar-to-exchange interaction ratio. We systematize the spin-wave excitations by their azimuthal and radial wave numbers. The lowest-frequency mode, the fundamental (quasiuniform) mode, and the mode hybridization are analyzed; the discussion of the influence of effective pinning at the ring boundaries is provided as well. We study the stability of the in-plane vortex state and discuss the role of the size of the ring and the type of lattice arrangement of the magnetic moments within it. To facilitate comparison with our results we provide the relationships between microscopic parameters, used in our model, and those used in the case of continuous medium.

  13. Excitation of XPS spectra from nanoscaled particles by local generation of x-rays

    SciTech Connect

    Mallinson, Christopher F.; Castle, James E.

    2015-09-15

    In preliminary work, the authors have shown that use of an aluminum substrate to support a distribution of copper particles enables their characteristic photoelectrons to be observed within the Auger electron spectrum generated by an incident electron beam. This observation raises the possibility of the use of chemical shifts and the corresponding Auger parameter to identify the chemical states present on the surface of individual submicrometer particles within a mixture. In this context, the technique has an advantage in that, unlike conventional Auger electron spectroscopy, the electron beam does not dwell on the particle but on the substrate adjacent to it. Given the importance, for both medical and toxicological reasons, of the surface composition of such particles, the authors have continued to explore the potential of this development. In this contribution, the authors show that proximal excitation of x-rays is equally successful with magnesium substrates. In some regions of the x-ray photoelectron spectrum, the much larger Auger peaks generated by the electron beam can cause inconvenient clustering of Auger and photoelectron peaks. As in conventional x-ray photoelectron spectroscopy, the ability to switch between Al and Mg sources is useful in such situations. In this context, the authors have extended the studies to iron particles where the authors show that use of Al or Mg substrates, as necessary, can make a contribution to clear identification of individual components in the Fe 2p peaks. For this development in electron spectroscopy to achieve its full potential, it is necessary to optimize the beam conditions used to generate the local x-ray to give good selectivity of a given particle. Measurements made in support of this will be given. Of greater concern is a possible problem of local heating associated with x-ray generation. The authors continue to explore this problem and report some progress in minimizing heating of the particle while maintaining

  14. New method for measuring time-resolved spectra of lanthanide emission using square-wave excitation

    SciTech Connect

    Qin, Feng; Zhao, Hua; Cai, Wei; Duan, Qianqian; Zhang, Zhiguo; Cao, Wenwu

    2013-11-15

    A method using modulated continuous wave (CW) visible laser to measure time-resolved fluorescence spectra of trivalent rare-earth ions has been developed. Electro-optic modulator was used to modulate the CW pumping laser with a rise time of 2 μs. CW Nd{sup 3+} lasers were used as examples to present the method. Upconversion dynamic process of Ho{sup 3+} was studied utilizing a 532 nm CW laser. Quantum cutting dynamic process from Tb{sup 3+} to Yb{sup 3+} was analyzed by a 473 nm CW laser. This method can be applied to any CW laser such as He-Ne laser, Ar{sup +} laser, Kr{sup +} laser, Ti:sapphire laser, etc.

  15. GAS-PHASE ELECTRONIC SPECTRA OF POLYACETYLENE CATIONS: RELEVANCE OF HIGHER EXCITED STATES

    SciTech Connect

    Rice, C. A.; Rudnev, V.; Dietsche, R.; Maier, J. P.

    2010-07-15

    Transitions to higher electronic states of polyacetylene cations (HC{sub 2n}H{sup +}, n = 4, 5, 6) have been measured in the gas phase at {approx}20 K. The absorption spectra were obtained using a resonant two-color, two-photon fragmentation technique in an ion trap, allowing a direct comparison between laboratory and astrophysical data. The purpose was to investigate the relevance of such transitions to astronomical observations because the general expectation is that the bands could be too broad due to fast intramolecular processes. It is shown that the origin bands are still narrow enough (1-10 cm{sup -1}) to be considered, especially as the higher-lying transitions often possess large oscillator strengths.

  16. New method for measuring time-resolved spectra of lanthanide emission using square-wave excitation.

    PubMed

    Qin, Feng; Zhao, Hua; Duan, Qianqian; Cai, Wei; Zhang, Zhiguo; Cao, Wenwu

    2013-11-01

    A method using modulated continuous wave (CW) visible laser to measure time-resolved fluorescence spectra of trivalent rare-earth ions has been developed. Electro-optic modulator was used to modulate the CW pumping laser with a rise time of 2 μs. CW Nd(3+) lasers were used as examples to present the method. Upconversion dynamic process of Ho(3+) was studied utilizing a 532 nm CW laser. Quantum cutting dynamic process from Tb(3+) to Yb(3+) was analyzed by a 473 nm CW laser. This method can be applied to any CW laser such as He-Ne laser, Ar(+) laser, Kr(+) laser, Ti:sapphire laser, etc.

  17. Effects of antidot shape on the spin wave spectra of two-dimensional Ni{sub 80}Fe{sub 20} antidot lattices

    SciTech Connect

    Mandal, Ruma; Laha, Pinaki; Das, Kaustuv; Saha, Susmita; Barman, Saswati; Raychaudhuri, A. K.; Barman, Anjan

    2013-12-23

    We show that the optically induced spin wave spectra of nanoscale Ni{sub 80}Fe{sub 20} (permalloy) antidot lattices can be tuned by changing the antidot shape. The spin wave spectra also show an anisotropy with the variation of the in-plane bias field orientation. Analyses show this is due to various quantized and extended modes, whose nature changes with the antidot shape and bias field orientation as a result of the variation of the internal magnetic field profile. The observed variation and anisotropy in the spin waves with the internal and external parameters are important for their applications in magnonic devices.

  18. Multi-band Bloch equations and gain spectra of highly excited II-VI semiconductor quantum wells

    SciTech Connect

    Girndt, A.; Jahnke, F.; Knorr, A.; Koch, S.W.; Chow, W.W.

    1997-04-21

    Quasi-equilibrium excitation dependent optical probe spectra of II-VI semiconductor quantum wells at room temperature are investigated within the framework of multi-band semiconductor Bloch equations. The calculations include correlation effects beyond the Hartree-Fock level which describe dephasing, interband Coulomb correlations and band-gap renormalization in second Born approximation. In addition to the carrier-Coulomb interaction, the influence of carrier-phonon scattering and inhomogeneous broadening is considered. The explicit calculation of single particle properties like band structure and dipole matrix elements using k {center_dot} p theory makes it possible to investigate various II-VI material combinations. Numerical results are presented for CdZnSe/ZnSe and CdZnSe/MnZnSSe semiconductor quantum-well systems.

  19. Rotational Spectra of Urea in its Ground and First Excited Vibrational States

    NASA Astrophysics Data System (ADS)

    Thomas, Jessica; Medvedev, Ivan; Kisiel, Zbigniew

    2014-06-01

    Urea is an important terrestrial bio-molecule, which has been tentatively detected in the interstellar medium. To match the much improved range and sensitivities of modern sub-millimeter telescopes a broad laboratory assay of rotational transitions needs to be recorded in order to aid in the definitive identification of this molecule. This paper focuses on the spectroscopic assignment of the rotational transitions of urea in the 207-500 GHz range which belong to its ground and first excited vibrational states. Remijan, A.J., L.E. Snyder, B.A. McGuire, H.-L. Kuo, L.W. Looney, D.N. Friedel, G.Y. Golubiatnikov, F.J. Lovas, V.V. Ilyushin, E.A. Alekseev, S.F. Dyubko, B.J. McCall, and J.M. Hollis, Observational Results of a Multi-Telescope Campaign in Search of Interstellar Urea [NH22CO]. The Astrophysical Journal, 2014. 783(2): p. 77

  20. The optical jet of RW Aurigae: excitation temperature and ionization state from long-slit spectra.

    NASA Astrophysics Data System (ADS)

    Bacciotti, F.; Hirth, G. A.; Natta, A.

    1996-06-01

    The physical properties of the optical jet associated with the T Tauri star RW Aurigae are discussed. The excitation temperature, the hydrogen ionization fraction, the electron and gas densities are estimated in various positions along the flow axis using a diagnostic technique originally developed for the study of the physical conditions in highly collimated Herbig-Haro jets (Bacciotti, Chiuderi & Oliva 1995). The receding portion of the jet (red lobe) has an ionization fraction which is slowly decreasing from about 25% near the star to about 2% at a distance of 6-7" (~1000AU); the hydrogen density is roughly constant with a value of about 10^4^cm^-3^; the temperature shows a slight decline, with typical values of about 4500K. These results are consistent with the idea that the gas is initially ionized in the jet acceleration zone and that the physical conditions in the visible part of the jet are determined by time-dependent hydrogen recombination. It has not been possible to obtain any result for the blue lobe, due to the weakness of the [SII] 6716,6731A lines. The mass-loss and momentum rate in the flow (red lobe) are ˙(M)~5x10^-8^Msun_/yr and ˙(P)~6.5x10^-6^Msun_/yr.km/s.

  1. Regge spectra of excited mesons, harmonic confinement, and QCD vacuum structure

    NASA Astrophysics Data System (ADS)

    Nedelko, Sergei N.; Voronin, Vladimir E.

    2016-05-01

    An approach to QCD vacuum as a medium describable in terms of a statistical ensemble of almost everywhere homogeneous Abelian (anti-)self-dual gluon fields is briefly reviewed. These fields play the role of the confining medium for color charged fields as well as underline the mechanism of realization of chiral S UL(Nf)×S UR(Nf) and UA(1 ) symmetries. Hadronization formalism based on this ensemble leads to manifestly defined quantum effective meson action. Strong, electromagnetic, and weak interactions of mesons are represented in the action in terms of nonlocal n -point interaction vertices given by the quark-gluon loops averaged over the background ensemble. New systematic results for the mass spectrum and decay constants of radially excited light, heavy-light mesons, and heavy quarkonia are presented. The interrelation between the present approach, models based on ideas of soft-wall anti-de Sitter/QCD, light-front holographic QCD, and the picture of harmonic confinement is outlined.

  2. Collective excitations and sum rules for the Hubbard model in the spin-density-wave regime

    NASA Astrophysics Data System (ADS)

    Monien, H.; Bedell, K. S.

    1992-02-01

    A variational estimate for the spin-wave velocity of the one-band Hubbard model on a square lattice in the spin-density-wave regime is studied. The estimate is given by the ratio of the f-sum rule to the static structure factor of the transverse-spin response function. The known results for the Heisenberg model are used to obtain results for those quantities in the large-U limit of the Hubbard model. The f-sum rule and static structure factor are calculated using the random-phase approximation (RPA). The spin-wave velocity calculated in the RPA, in the spin-density wave ground state, violates the variational bound.

  3. Multi-angle Spectra Evolution of Ionospheric Turbulence Excited by RF Interactions at HAARP

    NASA Astrophysics Data System (ADS)

    Sheerin, J. P.; Rayyan, N.; Watkins, B. J.; Watanabe, N.; Golkowski, M.; Bristow, W. A.; Bernhardt, P. A.; Briczinski, S. J., Jr.

    2014-12-01

    The high power HAARP HF transmitter is employed to generate and study strong Langmuir turbulence (SLT) in the interaction region of overdense ionospheric plasma. Diagnostics included the Modular UHF Ionospheric Radar (MUIR) sited at HAARP, the SuperDARN-Kodiak HF radar, and HF receivers to record stimulated electromagnetic emissions (SEE). Dependence of diagnostic signals on HAARP HF parameters, including pulselength, duty-cycle, aspect angle, and frequency were recorded. Short pulse, low duty cycle experiments demonstrate control of artificial field-aligned irregularities (AFAI) and isolation of ponderomotive effects. For the first time, simultaneous multi-angle radar measurements of plasma line spectra are recorded demonstrating marked dependence on aspect angle with the strongest interaction region observed displaced southward of the HF zenith pointing angle. For a narrow range of HF pointing between Spitze and magnetic zenith, a reduced threshold for AFAI is observed. High time resolution studies of the temporal evolution of the plasma line reveal the appearance of an overshoot effect on ponderomotive timescales. Numerous measurements of the outshifted plasma line are observed. Experimental results are compared to previous high latitude experiments and predictions from recent modeling efforts

  4. Pure absorption electron spin echo envelope modulation spectra by using the filter-diagonalization method for harmonic inversion.

    PubMed

    Jeschke, G; Mandelshtam, V A; Shaka, A J

    1999-03-01

    Harmonic inversion of electron spin echo envelope (ESEEM) time-domain signals by filter diagonalization is investigated as an alternative to Fourier transformation. It is demonstrated that this method features enhanced resolution compared to Fourier-transform magnitude spectra, since it can eliminate dispersive contributions to the line shape, even if no linear phase correction is possible. Furthermore, instrumental artifacts can be easily removed from the spectra if they are narrow either in time or frequency domain. This applies to echo crossings that are only incompletely eliminated by phase cycling and to spurious spectrometer frequencies, respectively. The method is computationally efficient and numerically stable and does not require extensive parameter adjustments or advance knowledge of the number of spectral lines. Experiments on gamma-irradiated methyl-alpha-d-glucopyranoside show that more information can be obtained from typical ESEEM time-domain signals by filter-diagonalization than by Fourier transformation.

  5. Extraction of the vibrational dynamics from the spectra of highly excited molecules and periodic orbit quantization by harmonic inversion

    NASA Astrophysics Data System (ADS)

    Atilgan, Erdinc

    Part I. The effective spectroscopic Hamiltonian fitted to experiment by Troellsch and Temps {A. Troellsch, F. Temps Zeitschrift fuer Physikalische Chemie 215, 207, (2001)} and describing high vibrational excitation to bound and resonant states, is used in conjunction with methods of nonlinear classical dynamics and semiclassical mechanics to extract for all the observed highly excited resonance levels in Polyad 8, the molecular motions upon which they are quantized. Two types of interlaced dynamically distinct ladders of states are revealed. The rungs of these ladders intersperse making the spectra complex. The resonant 2:2:1 frequency ratio of the DC, CO stretches and the bend respectively is what causes the complexity and is what caused past attempts at interpretation to be at best incomplete. All states are assigned with physically meaningful quantum numbers corresponding to quasiconserved quantities. Most interestingly it is pointed out that much of the information and assignment can be done without any calculations at all, using only the qualitative ideas from nonlinear, semiclassical and quantum mechanics along with the information supplied by the experimentalist. Part II. In systems with few degrees of freedom modern quantum calculations are, in general, numerically more efficient than semiclassical methods. However, this situation can be reversed with increasing dimension of the problem. For a three-dimensional system, viz. the hyperbolic four-sphere scattering system, we demonstrate the superiority of semiclassical versus quantum calculations. Semiclassical resonances can easily be obtained even in energy regions which are unattainable with the currently available quantum techniques.

  6. Determination of the in vivo redox potential using roGFP and fluorescence spectra obtained from one-wavelength excitation

    NASA Astrophysics Data System (ADS)

    Wierer, S.; Elgass, K.; Bieker, S.; Zentgraf, U.; Meixner, A. J.; Schleifenbaum, F.

    2011-02-01

    The analysis of molecular processes in living (plant) cells such as signal transduction, DNA replication, carbon metabolism and senescence has been revolutionized by the use of green fluorescent protein (GFP) and its variants as specific cellular markers. Many cell biological processes are accompanied by changes in the intracellular redox potential. To monitor the redox potential, a redox-sensitive mutant of GFP (roGFP) was created, which shows changes in its optical properties in response to changes in the redox state of its surrounding medium. For a quantitative analysis in living systems, it is essential to know the optical properties of roGFP in vitro. Therefore, we applied spectrally resolved fluorescence spectroscopy on purified roGFP exposed to different redox potentials to determine shifts in both the absorption and the emission spectra of roGFP. Based on these in vitro findings, we introduce a new approach using one-wavelength excitation to use roGFP for the in vivo analysis of cell biological processes. We demonstrate the ability this technique by investigating chloroplast-located Grx1-roGFP2 expressing Arabidopsis thaliana cells as example for dynamically moving intracellular compartments. This is not possible with the two-wavelength excitation technique established so far, which hampers a quantitative analysis of highly mobile samples due to the time delay between the two measurements and the consequential displacement of the investigated area.

  7. Electronic spectra of azaindole and its excited state mixing: A symmetry-adapted cluster configuration interaction study

    NASA Astrophysics Data System (ADS)

    Arulmozhiraja, Sundaram; Coote, Michelle L.; Hasegawa, Jun-ya

    2015-11-01

    Electronic structures of azaindole were studied using symmetry-adapted cluster configuration interaction theory utilizing Dunning's cc-pVTZ basis set augmented with appropriate Rydberg spd functions on carbon and nitrogen atoms. The results obtained in the present study show good agreement with the available experimental values. Importantly, and contrary to previous theoretical studies, the excitation energy calculated for the important n-π∗ state agrees well with the experimental value. A recent study by Pratt and co-workers concluded that significant mixing of π-π∗ and n-π∗ states leads to major change in the magnitude and direction of the dipole moment of the upper state vibrational level in the 0,0 + 280 cm-1 band in the S1←S0 transition when compared to that of the zero-point level of the S1 state. The present study, however, shows that all the four lowest lying excited states, 1Lb π-π∗, 1La π-π∗, n-π∗, and π-σ∗, cross each other in one way or another, and hence, significant state mixing between them is likely. The upper state vibrational level in the 0,0 + 280 cm-1 band in the S1←S0 transition benefits from this four-state mixing and this can explain the change in magnitude and direction of the dipole moment of the S1 excited vibrational level. This multistate mixing, and especially the involvement of π-σ∗ state in mixing, could also provide a route for hydrogen atom detachment reactions. The electronic spectra of benzimidazole, a closely related system, were also investigated in the present study.

  8. Electronic spectra of azaindole and its excited state mixing: A symmetry-adapted cluster configuration interaction study

    SciTech Connect

    Arulmozhiraja, Sundaram Coote, Michelle L.; Hasegawa, Jun-ya

    2015-11-28

    Electronic structures of azaindole were studied using symmetry-adapted cluster configuration interaction theory utilizing Dunning’s cc-pVTZ basis set augmented with appropriate Rydberg spd functions on carbon and nitrogen atoms. The results obtained in the present study show good agreement with the available experimental values. Importantly, and contrary to previous theoretical studies, the excitation energy calculated for the important n–π{sup ∗} state agrees well with the experimental value. A recent study by Pratt and co-workers concluded that significant mixing of π-π{sup ∗} and n-π{sup ∗} states leads to major change in the magnitude and direction of the dipole moment of the upper state vibrational level in the 0,0 + 280 cm{sup −1} band in the S{sub 1}←S{sub 0} transition when compared to that of the zero-point level of the S{sub 1} state. The present study, however, shows that all the four lowest lying excited states, {sup 1}L{sub b} π-π{sup ∗}, {sup 1}L{sub a} π-π{sup ∗}, n-π{sup ∗}, and π-σ{sup ∗}, cross each other in one way or another, and hence, significant state mixing between them is likely. The upper state vibrational level in the 0,0 + 280 cm{sup −1} band in the S{sub 1}←S{sub 0} transition benefits from this four-state mixing and this can explain the change in magnitude and direction of the dipole moment of the S{sub 1} excited vibrational level. This multistate mixing, and especially the involvement of π-σ{sup ∗} state in mixing, could also provide a route for hydrogen atom detachment reactions. The electronic spectra of benzimidazole, a closely related system, were also investigated in the present study.

  9. X-Ray Spectra of Young Pulsars and Their Wind Nebulae: Dependence on Spin-Down Energy Loss Rate

    NASA Technical Reports Server (NTRS)

    Gotthelf, E. V.

    2003-01-01

    An observational model is presented for the spectra of young rotation-powered pulsars and their nebulae based on a study of nine bright Crab-like pulsar systems observed with the Chandra X-ray observatory. A significant correlation is discovered between the X-ray spectra of these pulsars and that of their associated pulsar wind nebulae, both of which are observed to be a function of the spin-down energy loss rate, E. The 2-10 keV spectra of these objects are well characterized by an absorbed power-law model with photon indices, Gamma, in the range of 0.6 < Gamma (sub PSR) < 2.1 and 1.3 < Gamma(sub PWN) < 2.3, for the pulsars and their nebulae, respectively. A linear regression fit relating these two sets of indexes yields Gamma(sub PWN) = 0.91 +/- 0.18 + (0.66 +/- 0.11) Gamma (sub PSR), with a correlation coefficient of r = 0.97. The spectra of these pulsars are found to steepen as Gamma = Gamma(sub max) + alpha E (exp -1/2), with Gamma(sub max) providing an observational limit on the spectral slopes of young rotation-powered pulsars. These results reveal basic properties of young pulsar systems, allow new observational constraints on models of pulsar wind emission, and provide a means of predicting the energetics of pulsars lacking detected pulsations.

  10. Non-orthogonal spin-adaptation of coupled cluster methods: A new implementation of methods including quadruple excitations

    SciTech Connect

    Matthews, Devin A.; Stanton, John F.

    2015-02-14

    The theory of non-orthogonal spin-adaptation for closed-shell molecular systems is applied to coupled cluster methods with quadruple excitations (CCSDTQ). Calculations at this level of detail are of critical importance in describing the properties of molecular systems to an accuracy which can meet or exceed modern experimental techniques. Such calculations are of significant (and growing) importance in such fields as thermodynamics, kinetics, and atomic and molecular spectroscopies. With respect to the implementation of CCSDTQ and related methods, we show that there are significant advantages to non-orthogonal spin-adaption with respect to simplification and factorization of the working equations and to creating an efficient implementation. The resulting algorithm is implemented in the CFOUR program suite for CCSDT, CCSDTQ, and various approximate methods (CCSD(T), CC3, CCSDT-n, and CCSDT(Q))

  11. Optical orientation of spins in GaAs:Mn/AlGaAs quantum wells via impurity-to-band excitation

    NASA Astrophysics Data System (ADS)

    Petrov, P. V.; Kokurin, I. A.; Ivanov, Yu. L.; Averkiev, N. S.; Campion, R. P.; Gallagher, B. L.; Koenraad, P. M.; Silov, A. Yu.

    2016-08-01

    The paper reports optical orientation experiments performed in the narrow GaAs/AlGaAs quantum wells doped with Mn. We experimentally demonstrate a control over the spin polarization by means of the optical orientation via the impurity-to-band excitation and observe a sign inversion of the luminescence polarization depending on the pump power. The g factor of a hole localized on the Mn acceptor in the quantum well was also found to be considerably modified from its bulk value due to the quantum confinement effect. This finding shows the importance of the local environment on magnetic properties of the dopants in semiconductor nanostructures.

  12. Effects of orbital and spin current interference in E1 and M2 nuclear excitations

    SciTech Connect

    Goncharova, N. G.

    2015-12-15

    The interference of contributions from the orbital and spin currents to the E1 and M2 resonances is investigated. The results of the current interference analysis within the shell model are compared with the experimental data.

  13. Parallel parametric amplification of coherently excited propagating spin waves in a microscopic Ni{sub 81}Fe{sub 19} waveguide

    SciTech Connect

    Brächer, T.; Pirro, P.; Meyer, T.; Heussner, F.; Lägel, B.; Serga, A. A.; Hillebrands, B.

    2014-05-19

    We present parallel parametric amplification of coherently excited, propagating spin waves in a microstructured magnonic Ni{sub 81}Fe{sub 19} waveguide. Amplification is achieved by the pumping field generated by a microwave current flowing through a Cu micro-stripline underneath the waveguide. By employing microfocussed Brillouin light scattering spectroscopy, we investigate the spatial decay of the propagating spin waves and their amplification by means of parallel pumping. We analyze the dependence of the intensity of the amplified spin waves on the spin-wave excitation power, pumping power, and pumping duration, revealing the most efficient working point for a noise-free amplification. This paves the way for a frequency selective amplification of spin waves in microstructured magnonic circuits.

  14. Orbital elementary excitations as probes of entanglement and quantum phase transitions of collective spins in an entangled Bose-Einstein condensate

    SciTech Connect

    Wu Rukuan; Shi Yu

    2011-02-15

    A mixture of two species of pseudospin-(1/2) Bose gases exhibits interesting interplay between spin and orbital degrees of freedom. Expectation values of various quantities of the collective spins of the two species play crucial roles in the Gross-Pitaevskii-like equations governing the four orbital wave functions in which Bose-Einstein condensation occurs. Consequently, the elementary excitations of these orbital wave functions reflect properties of the collective spins. When the coupling between the two collective spins is isotropic, the energy gap of the gapped orbital excitation peaks. There is a quantum phase transition in the ground state of the effective Hamiltonian of the two collective spins, which have previously been found to be maximally entangled.

  15. Excitation and recombination dynamics of vacancy-related spin centers in silicon carbide

    SciTech Connect

    Hain, T. C.; Hertel, T.; Fuchs, F.; Astakhov, G. V.; Soltamov, V. A.; Baranov, P. G.; Dyakonov, V.

    2014-04-07

    We generate silicon vacancy related defects in high-quality epitaxial silicon carbide layers by means of electron irradiation. By controlling the irradiation fluence, the defect concentration is varied over several orders of magnitude. We establish the excitation profile for optical pumping of these defects and evaluate the optimum excitation wavelength of 770 nm. We also measure the photoluminescence dynamics at room temperature and find a monoexponential decay with a characteristic lifetime of 6.1 ns. The integrated photoluminescence intensity depends linear on the excitation power density up to 20 kW/cm{sup 2}, indicating a relatively small absorption cross section of these defects.

  16. Clues and criteria for designing a Kitaev spin liquid revealed by thermal and spin excitations of the honeycomb iridate Na2IrO3

    NASA Astrophysics Data System (ADS)

    Yamaji, Youhei; Suzuki, Takafumi; Yamada, Takuto; Suga, Sei-ichiro; Kawashima, Naoki; Imada, Masatoshi

    2016-05-01

    Contrary to the original expectation, Na2IrO3 is not a Kitaev's quantum spin liquid (QSL) but shows a zigzag-type antiferromagnetic order in experiments. Here, we propose experimental clues and criteria to measure how a material in hand is close to the Kitaev's QSL state. For this purpose, we systematically study thermal and spin excitations of a generalized Kitaev-Heisenberg model studied by Chaloupka et al., Phys. Rev. Lett. 110, 097204 (2013), 10.1103/PhysRevLett.110.097204 and an effective ab initio Hamiltonian for Na2IrO3 proposed by Yamaji et al., Phys. Rev. Lett. 113, 107201 (2014), 10.1103/PhysRevLett.113.107201, by employing a numerical diagonalization method. We reveal that closeness to the Kitaev's QSL is characterized by the following properties, besides trivial criteria such as reduction of magnetic ordered moments and Néel temperatures. (1) Two peaks in the temperature dependence of specific heat at Tℓ and Th caused by the fractionalization of spin to two types of Majorana fermions. (2) In between the double peak, a prominent plateau or shoulder pinned at R/2 ln2 in the temperature dependence of entropy, where R is the gas constant. (3) Failure of the linear spin wave approximation at the low-lying excitations of dynamical structure factors. (4) Small ratio Tℓ/Th close to or less than 0.03. According to the proposed criteria, Na2IrO3 is categorized to a compound close to the Kitaev's QSL, and is proven to be a promising candidate for the realization of the QSL if the relevant material parameters can further be tuned by making thin film of Na2IrO3 on various substrates or applying axial pressure perpendicular to the honeycomb networks of iridium ions. Applications of these characterization to (Na1-xLix) 2IrO3 and other related materials are also discussed.

  17. Research program in nuclear and solid state physics. [including pion absorption spectra and muon spin precession

    NASA Technical Reports Server (NTRS)

    1974-01-01

    The survey of negative pion absorption reactions on light and medium nuclei was continued. Muon spin precession was studied using an iron target. An impulse approximation model of the pion absorption process implied that the ion will absorb almost exclusively on nucleon pairs, single nucleon absorption being suppressed by energy and momentum conservation requirements. For measurements on both paramagnetic and ferromagnetic iron, the external magnetic field was supplied by a large C-type electromagnet carrying a current of about 100 amperes.

  18. Vibrational spectra and intramolecular vibrational redistribution in highly excited deuterobromochlorofluoromethane CDBrClF: Experiment and theory

    NASA Astrophysics Data System (ADS)

    Beil, Andreas; Hollenstein, Hans; Monti, Oliver L. A.; Quack, Martin; Stohner, Jürgen

    2000-08-01

    The rovibrational spectra of deuterobromochlorofluoromethane (CDBrClF) were measured at intermediate (0.1 cm-1) and high resolution (0.0024 cm-1 full bandwidth, half-maximum) by interferometric Fourier transform infrared spectroscopy in the range from the far infrared at 200 cm-1 to the near infrared (12 000 cm-1) covering all the fundamentals and CD stretching overtones up to polyad N=5. The spectra are completely analyzed in terms of their vibrational assignments to fundamentals, combinations and overtones. At high excitation the analysis reveals the dominant anharmonic coupling between four high frequency vibrational modes; the CD stretching (ν1), two CD bending (ν2,ν3), and the CF stretching mode (ν4). The analysis is carried out using effective model Hamiltonians including three and four vibrational degrees of freedom. We also present vibrational variational calculations on a grid in a four-dimensional normal coordinate subspace. The potential energy and the dipole moment function are calculated ab initio on this grid using self-consistent field second order Møller-Plesset perturbation theory (MP2). Experimental and theoretical results for band positions and integrated intensities as well as effective spectroscopic parameters are found to be in good agreement. The important anharmonic coupling between the CD chromophore and the CF stretching vibration can be described by an effective cubic Fermi resonance coupling constant ksff'≈(50±10) cm-1, which leads to intramolecular vibrational redistribution between the CD and CF chromophores on the femtosecond time scale. Time dependent intramolecular vibrational redistribution processes in CDBrClF are derived in various representations, including time dependent probability densities ("wave packets") in coordinate space and finally time dependent entropy.

  19. New Approach on Quantification of Porosity of Thin Films via Electron-Excited X-ray Spectra.

    PubMed

    Ortel, Erik; Hertwig, Andreas; Berger, Dirk; Esposito, Pasquale; Rossi, Andrea M; Kraehnert, Ralph; Hodoroaba, Vasile-Dan

    2016-07-19

    One of the crucial characteristics of functionalized thin films is their porosity (i.e., the ratio between the pore volume and the volume of the whole film). Due to the very low amount of material per coated area corresponding to thin films, it is a challenge for analytics to measure the film porosity. In this work, we present an approach to determine the porosity of thin films by means of electron probe microanalysis (EPMA) either by wavelength-dispersive X-ray spectrometry (WDX) or by energy-dispersive X-ray spectrometry (EDX) with a scanning electron microscope (SEM). The procedure is based on the calculation of the film mass deposition from electron-excited X-ray spectra. The mass deposition is converted into film density by division of measured film thickness. Finally, the film porosity is calculated from the measured film density and the density of bulk, nonporous film material. The general applicability of the procedure to determine the porosity is demonstrated on thin templated mesoporous TiO2 films, dip-coated on silicon wafer, with controlled porosity in the range of 15 to 50%. The high accuracy of the mass deposition as determined from X-ray spectra was validated with independent methods (ICP-OES and weighing). Furthermore, for the validation of the porosity results, ellipsometry, interference fringes method (IFM), and focused ion beam (FIB) cross sectioning were employed as independent techniques. Hence, the approach proposed in the present study is proven to be suited as a new analytical tool for accurate and relatively fast determination of the porosity of thin films. PMID:27334649

  20. Spin excitations in optimally P-doped BaFe2(As0.7P0.3)2 superconductor

    NASA Astrophysics Data System (ADS)

    Hu, Ding; Yin, Zhiping; Zhang, Wenliang; Ewings, R. A.; Ikeuchi, Kazuhiko; Nakamura, Mitsutaka; Roessli, Bertrand; Wei, Yuan; Zhao, Lingxiao; Chen, Genfu; Li, Shiliang; Luo, Huiqian; Haule, Kristjan; Kotliar, Gabriel; Dai, Pengcheng

    2016-09-01

    We use inelastic neutron scattering to study the temperature and energy dependence of spin excitations in an optimally P-doped BaFe2(As0.7P0.3 )2 superconductor (Tc=30 K) throughout the Brillouin zone. In the undoped state, spin waves and paramagnetic spin excitations of BaFe2As2 stem from an antiferromagnetic (AF) ordering wave vector QAF=(±1 ,0 ) , and peak near the zone boundary at (±1 ,±1 ) around 180 meV. Replacing 30% As by smaller P to induce superconductivity, low-energy spin excitations of BaFe2(As0.7P0.3 )2 form a resonance in the superconducting state and high-energy spin excitations now peak around 220 meV near (±1 ,±1 ) . These results are consistent with calculations from a combined density functional theory and dynamical mean field theory, and suggest that the decreased average pnictogen height in BaFe2(As0.7P0.3 )2 reduces the strength of electron correlations and increases the effective bandwidth of magnetic excitations.

  1. Spin-lozenge thermodynamics and magnetic excitations in Na3RuO4

    NASA Astrophysics Data System (ADS)

    Haraldsen, J. T.; Stone, M. B.; Lumsden, M. D.; Barnes, T.; Jin, R.; Taylor, J. W.; Fernandez-Alonso, F.

    2009-12-01

    We report inelastic and elastic neutron scattering, magnetic susceptibility, and heat capacity measurements for polycrystalline sodium ruthenate (Na3RuO4). Previous work suggests that this material consists of isolated tetramers of S = 3/2 Ru5+ ions in a so-called lozenge configuration. Comparisons of magnetic susceptibility and inelastic and elastic neutron scattering results with analytic calculations for several cluster models show that although there may be significant spin-spin correlations within the lozenge cluster, a simple isolated lozenge model is not appropriate for Na3RuO4.

  2. Spin-lozenge thermodynamics and magnetic excitations in Na(3)RuO(4).

    PubMed

    Haraldsen, J T; Stone, M B; Lumsden, M D; Barnes, T; Jin, R; Taylor, J W; Fernandez-Alonso, F

    2009-12-16

    We report inelastic and elastic neutron scattering, magnetic susceptibility, and heat capacity measurements for polycrystalline sodium ruthenate (Na(3)RuO(4)). Previous work suggests that this material consists of isolated tetramers of S = 3/2  Ru(5+) ions in a so-called lozenge configuration. Comparisons of magnetic susceptibility and inelastic and elastic neutron scattering results with analytic calculations for several cluster models show that although there may be significant spin-spin correlations within the lozenge cluster, a simple isolated lozenge model is not appropriate for Na(3)RuO(4). PMID:21836228

  3. Spin excitations in the quasi-two-dimensional charge-ordered insulator α -(BEDT-TTF ) 2I3 probed via 13C NMR

    NASA Astrophysics Data System (ADS)

    Ishikawa, Kyohei; Hirata, Michihiro; Liu, Dong; Miyagawa, Kazuya; Tamura, Masafumi; Kanoda, Kazushi

    2016-08-01

    The spin excitations from the nonmagnetic charge-ordered insulating state of α -(BEDT-TTF ) 2I3 at ambient pressure have been investigated by probing the static and low-frequency dynamic spin susceptibilities via site-selective nuclear magnetic resonance at 13C sites. The site-dependent values of the shift and the spin-lattice relaxation rate 1 /T1 below the charge-ordering transition temperature (TCO≈135 K ) demonstrate a spin density imbalance in the unit cell, in accord with the charge-density ratio reported earlier. The shift and 1 /T1 show activated temperature dependence with a static (shift) gap ΔS≈47 -52 meV and a dynamic (1 /T1 ) gap ΔR≈40 meV . The sizes of the gaps are well described in terms of a localized spin model, where spin-1/2 antiferromagnetic dimer chains are weakly coupled with each other.

  4. Site-selective excitation and polarized absorption and emission spectra of trivalent thulium and erbium in strontium fluorapatite

    NASA Astrophysics Data System (ADS)

    Gruber, John B.; Wright, Andrew O.; Seltzer, Michael D.; Zandi, Bahram; Merkle, Larry D.; Hutchinson, J. Andrew; Morrison, Clyde A.; Allik, Toomas H.; Chai, Bruce H. T.

    1997-05-01

    Polarized fluorescence spectra produced by site-selective excitation, and conventional polarized absorption spectra were obtained for Tm3+ and Er3+ ions individually incorporated into single crystals of strontium fluorapatite, Sr5(PO4)3F, also known as SFAP. Substitution of the trivalent rare earth ion for divalent strontium was achieved by passive charge compensation during Czochralski growth of the fluorapatite crystals. Spectra were obtained between 1780 and 345 nm at temperatures from 4 K to room temperature on crystals having the hexagonal structure [P63/m(C6h2)]. The polarized fluorescence spectra due to transitions from multiplet manifolds of Tm3+(4f12), including 1D2, 1G4, and 3H4 to manifolds 3H6 (the ground-state manifold), 3F4, 3H5, 3H4, and 3F3 were analyzed for the details of the crystal-field splitting of the manifolds. Fluorescence lifetimes were measured for Tm3+ transitions from 1D2, 1G4, and 3H4 at room temperature and from 1G4 at 16 K. Results of the analysis indicate that the majority of Tm3+ ions occupy sites having Cs symmetry. A point-charge lattice-sum calculation was made in which the crystal-field components, Anm, were determined assuming that trivalent thulium replaces divalent strontium in the metal site having Cs symmetry. Results support the conclusion that the nearest-neighbor fluoride (F-) is replaced by divalent oxygen (O2-), thus preserving overall charge neutrality and local symmetry. Crystal-field splitting calculations predict energy levels in agreement with results obtained from an analysis of the experimental data. By varying the crystal-field parameters, Bnm, we obtained a rms difference of 7 cm-1 between 43 calculated and experimental Stark levels for Tm3+(4f12) in Tm:SFAP. Absorption and fluorescence spectra are also reported for Er3+ ions in Er:SFAP. Measurement of the temporal decay of the room temperature fluorescence from the 4I11/2 and 4I13/2 manifolds yielded fluorescence lifetimes of 230±20 μs and 8.9±0.1 ms

  5. Spin excitations and superconductivity in cuprate oxide and heavy electron superconductors

    NASA Astrophysics Data System (ADS)

    Pines, David

    1990-04-01

    The experimental evidence for a temperature-dependent build up of antiferromagnetic correlations between Cu 2+ planar spins in the normal state of cuprate oxide superconductors is reviewed, and a phenomenological one-component model, developed in collaboration with A. Millis and H. Monien, which appears capable of providing a quantitative account of existing experiments is described. A scaling law which relates the superconducting transaction temperature to the measurable spin-spin correlation length is proposed. The NMR experimental results in the superconducting state are shown to be consistent with d-wave pairing in a strong coupling superconductor. Comparison of the results of NMR experiments on the cuprate oxide and heavy electron superconductors reveals striking similarities. I conclude that the cuprate oxide superconductors are unconventional superconductors in which the superconductivity is of (primarily) electronic origin and results from an attractive interaction of antiferromagnetic character between itinerant quasiparticles in the spin antisymmetric channel, and discuss similarities and differences between cuprate oxide and heavy electron systems.

  6. Studies of the optical spectra and spin-Hamiltonian parameters for the trivalent ytterbium ions in lithium yttrium fluoride crystals

    NASA Astrophysics Data System (ADS)

    Feng, W. L.; Han, Z.; Zhong, Y. C.

    In this paper, the crystal field (CF) levels and spin-Hamiltonian (SH) parameters (g factors g∥ and g⊥ and hyperfine structure constants A∥ and A⊥) of the rare-earth ion Yb3+ in lithium yttrium fluoride crystals are calculated under D2d point symmetry assumption. Two main methods are used in the calculation to study the SH parameters: one is the perturbation theory method and the other is the complete diagonalization (energy matrix) method (CDM). Comparing the calculated results with the experimental data, we can see that the CDM is more effective to calculate the SH parameters. In addition, the CF J-mixing of all excited-state multiplets into the ground-state multiplet 2F7/2 is considered. The validity of the calculated results is discussed.

  7. Calculation of the spin-wave spectra in planar magnonic crystals with metallic overlayers

    NASA Astrophysics Data System (ADS)

    Sokolovskyy, M. L.; Klos, J. W.; Mamica, S.; Krawczyk, M.

    2012-04-01

    Planar one-dimensional magnonic crystals of nanoscale lattice constant having different types of overlayers, dielectric and metallic, are studied. The dynamics of magnetization is described by the Landau-Lifshitz equation, which is solved using the plane-wave method. The calculations are performed with the nonuniform dynamic dipolar field. At the same time, the finite thickness of the studied structures is taken into account. New possibilities for shaping dispersion relations of spin waves and magnonic bandgaps in planar magnonic crystals by adding metallic/dielectric overlayers on the top of it are found.

  8. Influence of the physical structure of irradiated starches on their electron spin resonance spectra kinetics

    SciTech Connect

    Raffi, J.J.; Agnel, J.P.L.

    1983-06-23

    This study deals with the shape and kinetic changes of the ESR spectra of eight irradiated starchs, from several hours to several months after ..gamma..-irradiation. Whatever the origin and water content of the starches two major radicals or groups of radicals are observed. The kinetic law depends on the water content; two main zones are pointed out which are relative to the amorphous and crystalline parts of starches.

  9. Scaled opposite-spin CC2 for ground and excited states with fourth order scaling computational costs

    NASA Astrophysics Data System (ADS)

    Winter, Nina O. C.; Hättig, Christof

    2011-05-01

    An implementation of scaled opposite-spin CC2 (SOS-CC2) for ground and excited state energies is presented that requires only fourth order scaling computational costs. The SOS-CC2 method yields results with an accuracy comparable to the unscaled method. Furthermore the time-determining fifth order scaling steps in the algorithm can be replaced by only fourth order scaling computational costs using a "resolution of the identity" approximation for the electron repulsion integrals and a Laplace transformation of the orbital energy denominators. This leads to a significant reduction of computational costs especially for large systems. Timings for ground and excited state calculations are shown and the error of the Laplace transformation is investigated. An application to a chlorophyll molecule with 134 atoms results in a speed-up by a factor of five and demonstrates how the new implementation extends the applicability of the method. A SOS variant of the algebraic diagrammatic construction through second order ADC(2), which arises from a simplification of the SOS-CC2 model, is also presented. The SOS-ADC(2) model is a cost-efficient alternative in particular for future extensions to spectral intensities and excited state structure optimizations.

  10. Computational tools for the interpretation of electron spin resonance spectra in solution

    NASA Astrophysics Data System (ADS)

    Zerbetto, Mirco; Licari, Daniele; Barone, Vincenzo; Polimeno, Antonino

    2013-10-01

    Spectroscopic observables can be used for monitoring relaxation processes of molecules. In particular, electron spin resonance of stable multi-radicals is sensitive to the details of the rotational and internal dynamics in rigid and flexible molecules. Integration with advanced theoretical/computational methods proves to be particularly effective to acquire direct information on long-range relaxation processes, based on molecular dynamics, multi-scale approaches and coarse-graining treatments. Together, experimental data and computational interpretation provide a way to understand the effect of chemical changes on specific systems. In this paper we review computational tools aimed at the characterisation of dynamical properties of molecules gathered from electron spin resonance measurements. Stochastic models are employed, based on a number of structural parameters that are calculated at atomistic and/or mesoscopic level depending on their nature. Open source software tools built as user-friendly 'virtual spectroscopes' targeted for use by experimentalists are provided as a kind of extension of the laboratory equipment. An overview of their range of applicability is provided.

  11. Low energy nuclear spin excitations in Ho metal investigated by high resolution neutron spectroscopy.

    PubMed

    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.

  12. Spin and charge excitations in optimally doped Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8-delta}.

    SciTech Connect

    Rubhausen, M.; Guptasarma, P.; Hinks, D. G.; Klein, M. V.; Materials Science Division; Univ. Hamburg; Univ. of Illinois

    1998-01-01

    We present Raman spectra of low and high-energy charge and spin excitations in Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8-{delta}} single crystals with an optimized critical temperature of 95 K. The prominent feature of the high-energy background at around 250 meV is a rearrangement of spectral weight in B{sub 1g} and A{sub 1g}+B{sub 2g} symmetry below the critical temperature, similar to the observations in underdoped and optimally doped Y-123 compounds. In the low-energy region, which is influenced by the effects at higher energies, a gap feature in B{sub 1g} symmetry is observed yielding a value for the magnitude of the superconducting order parameter of A=34 meV. This gap feature is influenced by the orthorhombicity of the crystals and except for a small loss of spectral weight below 25 meV, no gap feature is visible in A{sub 1g} scattering geometry.

  13. Description of excited states in [Re(Imidazole)(CO)3 (Phen)](+) including solvent and spin-orbit coupling effects: Density functional theory versus multiconfigurational wavefunction approach.

    PubMed

    Fumanal, Maria; Daniel, Chantal

    2016-10-15

    The low-lying electronic excited states of [Re(imidazole)(CO)3 (phen)](+) (phen = 1,10-phenanthroline) ranging between 420 nm and 330 nm have been calculated by means of relativistic spin-orbit time-dependent density functional theory (TD-DFT) and wavefunction approaches (state-average-CASSCF/CASPT2). A direct comparison between the theoretical absorption spectra obtained with different methods including SOC and solvent corrections for water points to the difficulties at describing on the same footing the bands generated by metal-to-ligand charge transfer (MLCT), intraligand (IL) transition, and ligand-to-Ligand- charge transfer (LLCT). While TD-DFT and three-roots-state-average CASSCF (10,10) reproduce rather well the lowest broad MLCT band observed in the experimental spectrum between 420 nm and 330 nm, more flexible wavefunctions enlarged either by the number of roots or by the number of active orbitals and electrons destabilize the MLCT states by introducing IL and LLCT character in the lowest part of the absorption spectrum. © 2016 Wiley Periodicals, Inc. PMID:27510636

  14. Description of excited states in [Re(Imidazole)(CO)3 (Phen)](+) including solvent and spin-orbit coupling effects: Density functional theory versus multiconfigurational wavefunction approach.

    PubMed

    Fumanal, Maria; Daniel, Chantal

    2016-10-15

    The low-lying electronic excited states of [Re(imidazole)(CO)3 (phen)](+) (phen = 1,10-phenanthroline) ranging between 420 nm and 330 nm have been calculated by means of relativistic spin-orbit time-dependent density functional theory (TD-DFT) and wavefunction approaches (state-average-CASSCF/CASPT2). A direct comparison between the theoretical absorption spectra obtained with different methods including SOC and solvent corrections for water points to the difficulties at describing on the same footing the bands generated by metal-to-ligand charge transfer (MLCT), intraligand (IL) transition, and ligand-to-Ligand- charge transfer (LLCT). While TD-DFT and three-roots-state-average CASSCF (10,10) reproduce rather well the lowest broad MLCT band observed in the experimental spectrum between 420 nm and 330 nm, more flexible wavefunctions enlarged either by the number of roots or by the number of active orbitals and electrons destabilize the MLCT states by introducing IL and LLCT character in the lowest part of the absorption spectrum. © 2016 Wiley Periodicals, Inc.

  15. The structure of the high-energy spin excitations in YBa2Cu3O6+x

    NASA Astrophysics Data System (ADS)

    Hayden, Stephen

    2005-03-01

    The most obvious feature in the magnetic excitations of high-Tc superconductors is the so-called `resonance-mode'. This mode is strongly coupled to the superconductivity, however, it has not been found in the La2-x(Ba,Sr)xCuO4 family and is not universally present in Bi2Sr2CaCu2O8+δ. Here we use inelastic neutron scattering to characterize other excitations at higher energies which may be relevant to the superconductive pairing in YBa2Cu3O6.6. We observe a square-shaped continuum of excitations in reciprocal space [1]. These excitations have energies greater than the superconducting pairing energy, are present at Tc, and have spectral weight far exceeding that of the `resonance'. The discovery of similar excitations in La2-xBaxCuO4 [2] suggests that they are a general property of the copper oxides, and a candidate for mediating the electron pairing. Our data show that the high-energy magnetic excitations in the high-temperature superconductor YBa2Cu3O6.6 consists of a continuum of scattering bounded by a square and peaked at wavevector positions Qɛ =(1/2±ɛ,1/2±ɛ) and (1/2±ɛ,1/2ɛ). A similar structure is observed in the high-energy magnetic excitations of the magnetically ordered but weakly superconducting compound La1.85Ba0.125CuO4 [2]. This suggests there is universality, both in the low-energy and the high-energy spin dynamics between two very different classes of high-Tc superconductor. [1] S.M. Hayden, H.A. Mook, P.C. Dai, T.G. Perring, and F. Dogan, Nature 429, 531-534 (2004) [2] J.M. Tranquada, H. Woo, T.G. Perring, H. Goka, G.D. Gu , G. Xu, M. Fujita, K.Yamada K, Nature 429, 534-538 (2004).

  16. DOTAP/DOPE and DC-Chol/DOPE lipoplexes for gene delivery: zeta potential measurements and electron spin resonance spectra.

    PubMed

    Ciani, Laura; Ristori, Sandra; Salvati, Anna; Calamai, Luca; Martini, Giacomo

    2004-07-01

    Non-viral vectors represent an important alternative in gene delivery. Among these vectors, cationic liposomes are widely studied, because of their ability to form stable complexes with DNA fragments (lipoplexes). In the present work, we report on the characterization by electron spin resonance (ESR) spectroscopy and zeta potential measurements of cationic liposomes and of their complexes with oligonucleotides. Liposomes were made with a zwitterionic lipid, DOPE, and a cationic lipid, either DOTAP or DC-Chol. Oligonucleotides were the 20-base single strand polyA, the 20-base single strand polyT, and the corresponding double strand dsAT. The zeta potential as a function of the oligonucleotide/lipid+ ratio gave an S-shaped titration curve. Well-defined surface potential changes took place upon charge compensation between the cationic lipid heads and the phosphate groups on the oligonucleotides. The inversion point depended on the specific system under study. The bilayer properties and the changes that occurred with the incorporation of DNA fragments were also monitored by ESR spectroscopy of appropriately tailored spin probes. For all the systems investigated, the ESR spectra showed that no major alteration took place after lipoplex formation and molecular packing remained substantially unchanged. Both zeta potential and ESR measurements were in favor of an external mode of packing of the lipoplexes.

  17. Spin-wave energy dispersion of a frustrated spin-½ Heisenberg antiferromagnet on a stacked square lattice.

    PubMed

    Majumdar, Kingshuk

    2011-03-23

    The effects of interlayer coupling and spatial anisotropy on the spin-wave excitation spectra of a three-dimensional spatially anisotropic, frustrated spin-½ Heisenberg antiferromagnet (HAFM) are investigated for the two ordered phases using second-order spin-wave expansion. We show that the second-order corrections to the spin-wave energies are significant and find that the energy spectra of the three-dimensional HAFM have similar qualitative features to the energy spectra of the two-dimensional HAFM on a square lattice. We also discuss the features that can provide experimental measures for the strength of the interlayer coupling, spatial anisotropy parameter, and magnetic frustration.

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

    PubMed

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

    2016-09-14

    We report on spectroscopic studies of resonances related to ladder of states of a charged exciton in single GaAlAs/AlAs quantum dot structures. Polarization-resolved photoluminescence, photoluminescence excitation and photon-correlation measurements were performed at low (T  =  4.2 K) temperature also in magnetic field applied in Faraday configuration. The investigated resonances are assigned to three different configurations of a positively charged exciton. Together with a singlet ground state and a conventional triplet state (involving an electron from the ground state electronic s-shell), an excited triplet state, which involved an electron from the excited electronic p-shell was identified in single dots. The appearance of an emission line related to the latter complex is due to a partially suppressed electron relaxation in the investigated dots. An analysis of this emission line allows us to scrupulously determine properties of the excited triplet state and compare them with those of the conventional triplet state. Both triplets exhibit similar patterns of anisotropic fine structure and Zeeman splitting, however their amplitudes significantly differ for those two states. Presented results emphasize the role of the symmetry of the electronic state on the properties of the triplet states of two holes  +  electron excitonic complex. PMID:27391126

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

    NASA Astrophysics Data System (ADS)

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

    2016-09-01

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

  20. Magnetic excitations in the spin-1/2 triangular-lattice antiferromagnet Cs2CuBr4

    SciTech Connect

    Zvyagin, S. A.; Ozerov, M.; Kamenskyi, D.; Wosnitza, J.; Krzystek, J.; Yoshizawa, D.; Hagiwara, M.; Hu, Rongwei; Ryu, Hyejin; Petrovic, C.; Zhitomirsky, M. E.

    2015-11-27

    We present on high- field electron spin resonance (ESR) studies of magnetic excitations in the spin- 1/2 triangular-lattice antiferromagnet Cs2CuBr4. Frequency- field diagrams of ESR excitations are measured for different orientations of magnetic fields up to 25 T. We show that the substantial zero- field energy gap, Δ ≈ 9.5 K, observed in the low-temperature excitation spectrum of Cs2CuBr4 [Zvyagin et al:, Phys. Rev. Lett. 112, 077206 (2014)], is present well above TN. Noticeably, the transition into the long-range magnetically ordered phase does not significantly affect the size of the gap, suggesting that even below TN the high-energy spin dynamics in Cs2CuBr4 is determined by short-range-order spin correlations. The experimental data are compared with results of model spin-wave-theory calculations for spin-1/2 triangle-lattice antiferromagnet.

  1. IRAS observations of the exciting stars of Herbig-Haro objects. II - The Reipurth and Graham sample and low-resolution spectra

    NASA Technical Reports Server (NTRS)

    Cohen, Martin

    1990-01-01

    Using IRAS COADDed images, candidates are suggested for the exciting stars of Herbig-Haro objects from the Reipurth and Graham sample. The IRAS low-resolution spectrometer provides spectra for 20 of the 46 candidate stars so far identified as exciting young, unevolved H-H systems. These reveal 10-micron silicate absorption features, or are too red to show detectable flux near 10 microns. The histogram of bolometric luminosities for 46 young Herbig-Haro exciting stars has a median of 13 solar luminosities and a mode between 16 and 32 solar luminosities. Although the enlarged sample of known exciting stars has more of the higher luminosity objects than an earlier sample, the histogram still represents a generally low-luminosity distribution.

  2. Solvent effects on the absorption and fluorescence spectra of quinine sulphate: Estimation of ground and excited-state dipole moments

    NASA Astrophysics Data System (ADS)

    Joshi, Sunita; Pant, Debi D.

    2012-06-01

    Ground and excited state dipole moments of probe quinine sulphate (QS) was obtained using Solvatochromic shift method. Higher dipole moment is observed for excited state as compared to the ground state which is attributed to the higher polarity of excited state.

  3. Transient resonance Raman spectra of benzophenone and its four isotopic analogues in the lowest excited triplet state

    SciTech Connect

    Tahara, T.; Hamaguchi, H.; Tasumi, M.

    1987-11-05

    Transient resonance Raman spectra of T/sub 1/ benzophenone (T/sub 1/BP) and its four isotopic analogues in carbon tetrachloride solutions were measured. Vibrational assignments of eight T/sub 1/ bands have been made on the basis of the observed isotopic frequency shifts. The assignments clarified the following three points concerning the structure of T/sub 1/ BP in solution. (1) The CO bond order in T/sub 1/ BP is much lower than that in the ground-state benzophenone (S/sub 0/ BP). The CO stretching frequency in T/sub 1/ is found to be 1222 cm/sup -1/, whereas the corresponding value in S/sub 0/ is 1665 cm/sup -1/. The former frequency indicates a single-bond-like character of the CO bonding in the T/sub 1/ state. (2) Vibrational frequencies of several ring modes show marked downshifts in going from S/sub 0/ to T/sub 1/. This suggests the delocalization of the ..pi..* electron into the ring part. (3) The assignment (1302 cm/sup -1/) of the symmetric C-phenyl stretch mode in the T/sub 1/ withdraws S/sub 0/ absorption spectrum is questioned. According to the present assignment, the frequency of this mode (approx. 1100 cm/sup -1/) is slightly lower than that in the ground state (1150 cm/sup -1/). The simple quantum chemical picture of T/sub 1/ BP, which predicted the increase of the C-phenyl bond order with the ..pi..* withdraws n excitation, should therefore be reconsidered.

  4. Spin-orbit interaction driven collective electron-hole excitations in a noncentrosymmetric nodal loop Weyl semimetal

    NASA Astrophysics Data System (ADS)

    Ahn, Kyo-Hoon; Lee, Kwan-Woo; Pickett, Warren E.

    2015-09-01

    NbP is one member of a new class of nodal loop semimetals characterized by the cooperative effects of spin-orbit coupling (SOC) and a lack of inversion center. Here transport and spectroscopic properties of NbP are evaluated using density functional theory methods. SOC together with the lack of inversion symmetry splits degeneracies, giving rise to "Russian doll nested" Fermi surfaces containing 4 ×10-4 electron (hole) carriers/f.u. Due to the modest SOC strength in Nb, the Fermi surfaces map out the Weyl nodal loops. Calculated structure around T*≈100 K in transport properties reproduces well the observed transport behavior only when SOC is included, attesting to the precision of the (delicate) calculations and the stoichiometry of the samples. Low-energy collective electron-hole excitations (plasmons) in the 20-60 meV range result from the nodal loop splitting.

  5. High spin spectroscopy near the N=Z line: Channel selection and excitation energy systematics

    SciTech Connect

    Svensson, C.E.; Cameron, J.A.; Flibotte, S.

    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.

  6. Extensive spin-orbit multi-reference computations on the excited states of the phosphorus monochloride molecule

    NASA Astrophysics Data System (ADS)

    Zhang, Xiaomei; Yan, Peiyuan; Li, Rui; Gai, Zhiqiang; Liang, Guiying; Xu, Haifeng; Yan, Bing

    2016-09-01

    Total 34 Λ-S states of the PCl molecule have been studied by using the multi-reference configuration interaction plus the Davidson correction (MRCI+Q) method with the correlation consistent quadruple-zeta quality basis set. These states are correlated to three dissociation limits P(4Su)+Cl(2Pu), P(2Du)+Cl(2Pu), and P(2Pu)+Cl(2Pu), respectively. The potential energy curves (PECs) of the Λ-S states have been calculated, from which the spectroscopic constants of the bound states are determined. The calculated spectroscopic results well reproduce the available measurements. The spin-orbit matrix elements between the Λ-S states have been calculated, which indicate that the perturbations exist in the interacting system 11Π-23Π and 11Π-23Σ-. And the excited a1Δ, b1Σ+, 21Σ+ states could be predissociated induced by the spin-orbit coupling (SOC) effect. The SOC calculation on the PCl molecule has been performed with the state interaction method. This is the first time that the SOC effect of the PCl has been studied theoretically. The SOC effect leads to the 34 Λ-S states split into the 74 Ω states. The ground state X3Σ- splits into the X3 Σ0-+ (X10+) and X3Σ1- (X21) states. For the zero-field splitting of the X3Σ- state, the spin-orbit contribution of 6 cm-1 is much larger than spin-spin contribution of 0.32 cm-1. Under the influence of the SOC effect, the spectroscopic results of the a1Δ and b1Σ+ states have very small changes, but the dissociation energies strongly decrease. The transition properties of PCl are also predicted, including the E1, M1, and E2 transition moments, the Franck-Condon factors, the transition probabilities, and the radiative lifetimes. For the transitions from a1Δ-X3Σ- and b1Σ+-X3Σ-, the transition probabilities are in order of AE1 > AM1 ≫ AE2. The lifetimes for the b1Σ+(v'=0) state are 4.87ms (E1) and 4.57 ms (E1+M1), in good agreement with the available experimental result of 4.9±0.8 ms.

  7. Picosecond near-infrared excited transient Raman spectra of β-carotene in the excited S 2 state: Solvent effects on the in-phase C dbnd C stretching band and vibronic coupling

    NASA Astrophysics Data System (ADS)

    Sakamoto, Akira; Matsuno, Shinya; Tasumi, Mitsuo

    2010-07-01

    Picosecond time-resolved Raman spectra of β-carotene in the excited S 2 ( 1Bu+) state have been obtained in resonance with its near-infrared transient absorption. The Raman band due to the in-phase C dbnd C stretching mode of β-carotene in the S 2 state has been observed at about 1550 cm -1. The solvent effects on this band are discussed in comparison with the previous results on the corresponding bands in the ground S 0 ( 1Ag-) state and the excited S 1 ( 2Ag-) state.

  8. Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7.

    PubMed

    Calder, S; Vale, J G; Bogdanov, N A; Liu, X; Donnerer, C; Upton, M H; Casa, D; Said, A H; Lumsden, M D; Zhao, Z; Yan, J-Q; Mandrus, D; Nishimoto, S; van den Brink, J; Hill, J P; McMorrow, D F; Christianson, A D

    2016-01-01

    Much consideration has been given to the role of spin-orbit coupling (SOC) in 5d oxides, particularly on the formation of novel electronic states and manifested metal-insulator transitions (MITs). SOC plays a dominant role in 5d(5) iridates (Ir(4+)), undergoing MITs both concurrent (pyrochlores) and separated (perovskites) from the onset of magnetic order. However, the role of SOC for other 5d configurations is less clear. For example, 5d(3) (Os(5+)) systems are expected to have an orbital singlet with reduced effective SOC. The pyrochlore Cd2Os2O7 nonetheless exhibits a MIT entwined with magnetic order phenomenologically similar to pyrochlore iridates. Here, we resolve the magnetic structure in Cd2Os2O7 with neutron diffraction and then via resonant inelastic X-ray scattering determine the salient electronic and magnetic energy scales controlling the MIT. In particular, SOC plays a subtle role in creating the electronic ground state but drives the magnetic order and emergence of a multiple spin-flip magnetic excitation. PMID:27273216

  9. Physical states and finite-size effects in Kitaev's honeycomb model: Bond disorder, spin excitations, and NMR line shape

    NASA Astrophysics Data System (ADS)

    Zschocke, Fabian; Vojta, Matthias

    2015-07-01

    Kitaev's compass model on the honeycomb lattice realizes a spin liquid whose emergent excitations are dispersive Majorana fermions and static Z2 gauge fluxes. We discuss the proper selection of physical states for finite-size simulations in the Majorana representation, based on a recent paper by F. L. Pedrocchi, S. Chesi, and D. Loss [Phys. Rev. B 84, 165414 (2011), 10.1103/PhysRevB.84.165414]. Certain physical observables acquire large finite-size effects, in particular if the ground state is not fermion-free, which we prove to generally apply to the system in the gapless phase and with periodic boundary conditions. To illustrate our findings, we compute the static and dynamic spin susceptibilities for finite-size systems. Specifically, we consider random-bond disorder (which preserves the solubility of the model), calculate the distribution of local flux gaps, and extract the NMR line shape. We also predict a transition to a random-flux state with increasing disorder.

  10. Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7

    PubMed Central

    Calder, S.; Vale, J. G.; Bogdanov, N. A.; Liu, X.; Donnerer, C.; Upton, M. H.; Casa, D.; Said, A. H.; Lumsden, M. D.; Zhao, Z.; Yan, J. -Q.; Mandrus, D.; Nishimoto, S.; van den Brink, J.; Hill, J. P.; McMorrow, D. F.; Christianson, A. D.

    2016-01-01

    Much consideration has been given to the role of spin-orbit coupling (SOC) in 5d oxides, particularly on the formation of novel electronic states and manifested metal-insulator transitions (MITs). SOC plays a dominant role in 5d5 iridates (Ir4+), undergoing MITs both concurrent (pyrochlores) and separated (perovskites) from the onset of magnetic order. However, the role of SOC for other 5d configurations is less clear. For example, 5d3 (Os5+) systems are expected to have an orbital singlet with reduced effective SOC. The pyrochlore Cd2Os2O7 nonetheless exhibits a MIT entwined with magnetic order phenomenologically similar to pyrochlore iridates. Here, we resolve the magnetic structure in Cd2Os2O7 with neutron diffraction and then via resonant inelastic X-ray scattering determine the salient electronic and magnetic energy scales controlling the MIT. In particular, SOC plays a subtle role in creating the electronic ground state but drives the magnetic order and emergence of a multiple spin-flip magnetic excitation. PMID:27273216

  11. Spin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7

    NASA Astrophysics Data System (ADS)

    Calder, S.; Vale, J. G.; Bogdanov, N. A.; Liu, X.; Donnerer, C.; Upton, M. H.; Casa, D.; Said, A. H.; Lumsden, M. D.; Zhao, Z.; Yan, J.-Q.; Mandrus, D.; Nishimoto, S.; van den Brink, J.; Hill, J. P.; McMorrow, D. F.; Christianson, A. D.

    2016-06-01

    Much consideration has been given to the role of spin-orbit coupling (SOC) in 5d oxides, particularly on the formation of novel electronic states and manifested metal-insulator transitions (MITs). SOC plays a dominant role in 5d5 iridates (Ir4+), undergoing MITs both concurrent (pyrochlores) and separated (perovskites) from the onset of magnetic order. However, the role of SOC for other 5d configurations is less clear. For example, 5d3 (Os5+) systems are expected to have an orbital singlet with reduced effective SOC. The pyrochlore Cd2Os2O7 nonetheless exhibits a MIT entwined with magnetic order phenomenologically similar to pyrochlore iridates. Here, we resolve the magnetic structure in Cd2Os2O7 with neutron diffraction and then via resonant inelastic X-ray scattering determine the salient electronic and magnetic energy scales controlling the MIT. In particular, SOC plays a subtle role in creating the electronic ground state but drives the magnetic order and emergence of a multiple spin-flip magnetic excitation.

  12. Fluorescent excitation of Fe 2, Mn 2, Ti 2, N 1 lines by V 4, N 5, O 6: Emission lines in the spectra of symbiotic stars and Seyfert galaxies

    NASA Technical Reports Server (NTRS)

    Gilra, D. P.

    1984-01-01

    Analysis of the published IUE and ground based high resolution spectra of symbiotic stars, particularly RR Tel, shows that the dominant excitation mechanism of Fe II, Mn II, Ti II, and N I lines is the selective fluorescent excitation of some levels by the strong C IV, N V, and O VI emission lines. The same mechanism should work for the excitation of Fe II lines in the spectra of Seyfert galaxies and Q60's whose emission spectra are quite similar to those of symbiotic stars. The similarities and differences between the fluroescent excitation mechanism reported herein and the Bowen's mechanism is analyzed.

  13. Tilted cranking classification of multiband spectra

    NASA Astrophysics Data System (ADS)

    Frauendorf, S.; May, F. R.

    1992-06-01

    The existence of TDHF-solutions rotating uniformly about a nonprincipal axis of the deformed axial potential is demonstrated. The solutions represent Delta(I) = 1 bands. Self consistency and symmetry are discussed. The transformation of experimental spectra to the rotating frame of reference is introduced. Excitation spectra at high spin are calculated and found to agree well with recent data on Er-163 and Hf-174.

  14. Direct observation of low energy nuclear spin excitations in HoCrO3 by high resolution neutron spectroscopy.

    PubMed

    Chatterji, T; Jalarvo, N; Kumar, C M N; Xiao, Y; Brückel, Th

    2013-07-17

    We have investigated low energy nuclear spin excitations in the strongly correlated electron compound HoCrO3. We observe clear inelastic peaks at E = 22.18 ± 0.04 μeV in both energy loss and gain sides. The energy of the inelastic peaks remains constant in the temperature range 1.5-40 K at which they are observed. The intensity of the inelastic peak increases at first with increasing temperature and then decreases at higher temperatures. The temperature dependence of the energy and intensity of the inelastic peaks is very unusual compared to that observed in other Nd, Co, V and also simple Ho compounds. Huge quasielastic scattering appears at higher temperatures presumably due to the fluctuating electronic moments of the Ho ions that get increasingly disordered at higher temperatures. The strong quasielastic scattering may also originate in the first Ho crystal-field excitations at about 1.5 meV.

  15. Modeling the effects of structure and dynamics of the nitroxide side-chain on the ESR spectra of spin labeled proteins

    PubMed Central

    Tombolato, Fabio; Ferrarini, Alberta; Freed, Jack H.

    2010-01-01

    In a companion paper (Tombolato, F.; Ferrarini, A.; Freed, J.H., ... ) a study of the conformational dynamics of methanethiosulfonate spin probes linked at a surface exposed α-helix has been presented. Here, on the basis of this analysis, X-band ESR spectra of these spin labels are simulated, within the framework of the Stochastic Liouville Equation methodology. Slow reorientations of the whole protein are superimposed on fast chain motions, which have been identified with conformational jumps and fluctuations in the minima of the chain torsional potential. Fast chain motions are introduced in the SLE for the protein reorientations through partially averaged magnetic tensors and relaxation times calculated according to the motional narrowing theory. The 72R1 and 72R2 mutants of T4 lysozyme, which bear the spin label at a solvent-exposed helix site, have been taken as test systems. For the side-chain of the R2 spin label, only a few non-interconverting conformers are possible, whose mobility is limited to torsional fluctuations, yielding almost identical spectra, typical of slightly mobile nitroxides. In the case of R1, more complex spectra result from the simultaneous presence of constrained and mobile chain conformers, with relative weights which can depend on the local environment. The model provides an explanation for the experimentally observed dependence of the spectral lineshapes on temperature, solvent, and pattern of substituents in the pyrroline ring. The relatively simple methodology presented here allows the introduction of realistic features of the spin probe dynamics into the simulation of ESR spectra of spin labeled proteins; moreover, it provides suggestions for a proper account of such dynamics in more sophisticated approaches. PMID:17181284

  16. Properties of Haldane Excitations and Multiparticle States in the Antiferromagnetic Spin-1 Chain Compound CsNiCl3

    SciTech Connect

    Kenzelmann, M.; Cowley, R. A.; Buyers, W. J. L.; Tun, Z.; Coldea, Radu; Enderle, M.

    2002-01-01

    We report inelastic time-of-flight and triple-axis neutron scattering measurements of the excitation spectrum of the coupled antiferromagnetic spin-1 Heisenberg chain system CsNiCl{sub 3}. Measurements over a wide range of wave-vector transfers along the chain confirm that above T{sub N} CsNiCl{sub 3} is in a quantum-disordered phase with an energy gap in the excitation spectrum. The spin correlations fall off exponentially with increasing distance with a correlation length {zeta} = 4.0(2) sites at T = 6.2K. This is shorter than the correlation length for an antiferromagnetic spin-1 Heisenberg chain at this temperature, suggesting that the correlations perpendicular to the chain direction and associated with the interchain coupling lower the single-chain correlation length. A multiparticle continuum is observed in the quantum-disordered phase in the region in reciprocal space where antiferromagnetic fluctuations are strongest, extending in energy up to twice the maximum of the dispersion of the well-defined triplet excitations. We show that the continuum satisfies the Hohenberg-Brinkman sum rule. The dependence of the multiparticle continuum on the chain wave vector resembles that of the two-spinon continuum in antiferromagnetic spin-1/2 Heisenberg chains. This suggests the presence of spin-1/2 degrees of freedom in CsNiCl{sub 3} for T {approx}< 12 K, possibly caused by multiply frustrated interchain interactions.

  17. Evidence for phonon-like charge and spin fluctuations from an analysis of angle-resolved photoemission spectra of La2-xSrxCuO4 superconductors

    NASA Astrophysics Data System (ADS)

    Mazza, G.; Grilli, M.; Di Castro, C.; Caprara, S.

    2013-01-01

    In high temperature superconductors we provide evidence of spin and mixed phonon-charge collective modes as mediators of the effective electron-electron interaction and suggestive of a charge and spin density wave instability competing with superconductivity. Indeed, we show that the so-called kinks and waterfalls observed in angle-resolved photoemission spectra of La2-xSrxCuO4, a prototypical high-Tc superconducting cuprate, are due to the coupling of quasiparticles with two distinct nearly critical collective modes with finite characteristic wave vectors, typical of charge and spin fluctuations. The simultaneous presence of these two modes reconciles the long standing dichotomy whether kinks are due to phonons or spin waves.

  18. Synchrotron-radiation study of weak fluorescence from neat liquids of simple alkenes: Anomalous excitation spectra as evidence for wavelength-dependent photochemistry

    SciTech Connect

    Inoue, Yoshihisa; Daino, Yoshihiko; Tai, Akira; Hakushi, Tadao ); Okada, Tadashi )

    1989-07-19

    Fluorescence excitation spectra of trans-2-octene, trans-cyclooctene, 2-methyl-2-butene, and 2,3-dimethyl-2-butene were measured by using synchrotron radiation as a tunable light source in the vacuum UV and UV region. The wavelength dependence of the fluorescence yields provides direct evidence for the long-proposed assignment that the emissive state is the {pi},R(3s) Rydberg state, which in turn gives the carbene-derived photoproducts.

  19. Special features of the excitation spectra and kinetics of photoluminescence of the Si{sub 1-x}Ge{sub x}:Er/Si structures with relaxed heterolayers

    SciTech Connect

    Krasilnikova, L. V. Yablonskiy, A. N.; Stepikhova, M. V.; Drozdov, Yu. N.; Shengurov, V. G.; Krasilnik, Z. F.

    2010-11-15

    Luminescent properties of heteroepitaxial Si{sub 1-x}Ge{sub x}:Er/Si structures with relaxed heterolayers are studied. The results of combined studies of the excitation spectra and kinetics of photoluminescence (PL) are used to single out the components providing the largest contribution to the PL signal of the Si{sub 1-x}Ge{sub x}:Er/Si structures in the wavelength region of 1.54 {mu}m. It is shown that relaxation of elastic stresses in the Si{sub 1-x}Ge{sub x}:Er heterolayer affects only slightly the kinetic characteristics of erbium luminescence and manifests itself in insignificant contribution of the defects and defect-impurity complexes to the luminescent response of the Si{sub 1-x}Ge{sub x}:Er/Si structures. In the excitation spectra of the erbium PL, special features related to the possibility of the rare-earth impurity excitation at energies lower than the band gap of the Si{sub 1} {sub -x}Ge{sub x} solid solution are revealed. It is shown that a peak the width of which depends on the band gap of the solid solution and the extent of its relaxation is observed in the excitation spectra of the erbium-related PL in the Si{sub 1-x}Ge{sub x}:Er/Si structures in the wavelength region of 1040-1050 nm. The observed specific features are accounted for by involvement of intermediate levels in the band gap of the Si{sub 1-x}Ge{sub x}:Er solid solution in the process of excitation of an Er{sup 3+} ion.

  20. Comparative assessment of density functional methods for evaluating essential parameters to simulate SERS spectra within the excited state energy gradient approximation

    NASA Astrophysics Data System (ADS)

    Mohammadpour, Mozhdeh; Jamshidi, Zahra

    2016-05-01

    The prospect of challenges in reproducing and interpretation of resonance Raman properties of molecules interacting with metal clusters has prompted the present research initiative. Resonance Raman spectra based on the time-dependent gradient approximation are examined in the framework of density functional theory using different methods for representing the exchange-correlation functional. In this work the performance of different XC functionals in the prediction of ground state properties, excitation state energies, and gradients are compared and discussed. Resonance Raman properties based on time-dependent gradient approximation for the strongly low-lying charge transfer states are calculated and compared for different methods. We draw the following conclusions: (1) for calculating the binding energy and ground state geometry, dispersion-corrected functionals give the best performance in comparison to ab initio calculations, (2) GGA and meta GGA functionals give good accuracy in calculating vibrational frequencies, (3) excited state energies determined by hybrid and range-separated hybrid functionals are in good agreement with EOM-CCSD calculations, and (4) in calculating resonance Raman properties GGA functionals give good and reasonable performance in comparison to the experiment; however, calculating the excited state gradient by using the hybrid functional on the hessian of GGA improves the results of the hybrid functional significantly. Finally, we conclude that the agreement of charge-transfer surface enhanced resonance Raman spectra with experiment is improved significantly by using the excited state gradient approximation.

  1. Electronic excitation spectra of molecules in solution calculated using the symmetry-adapted cluster-configuration interaction method in the polarizable continuum model with perturbative approach.

    PubMed

    Fukuda, Ryoichi; Ehara, Masahiro; Cammi, Roberto

    2014-02-14

    A perturbative approximation of the state specific polarizable continuum model (PCM) symmetry-adapted cluster-configuration interaction (SAC-CI) method is proposed for efficient calculations of the electronic excitations and absorption spectra of molecules in solutions. This first-order PCM SAC-CI method considers the solvent effects on the energies of excited states up to the first-order with using the zeroth-order wavefunctions. This method can avoid the costly iterative procedure of the self-consistent reaction field calculations. The first-order PCM SAC-CI calculations well reproduce the results obtained by the iterative method for various types of excitations of molecules in polar and nonpolar solvents. The first-order contribution is significant for the excitation energies. The results obtained by the zeroth-order PCM SAC-CI, which considers the fixed ground-state reaction field for the excited-state calculations, are deviated from the results by the iterative method about 0.1 eV, and the zeroth-order PCM SAC-CI cannot predict even the direction of solvent shifts in n-hexane for many cases. The first-order PCM SAC-CI is applied to studying the solvatochromisms of (2,2(')-bipyridine)tetracarbonyltungsten [W(CO)4(bpy), bpy = 2,2(')-bipyridine] and bis(pentacarbonyltungsten)pyrazine [(OC)5W(pyz)W(CO)5, pyz = pyrazine]. The SAC-CI calculations reveal the detailed character of the excited states and the mechanisms of solvent shifts. The energies of metal to ligand charge transfer states are significantly sensitive to solvents. The first-order PCM SAC-CI well reproduces the observed absorption spectra of the tungsten carbonyl complexes in several solvents.

  2. Electronic excitation spectra of molecules in solution calculated using the symmetry-adapted cluster-configuration interaction method in the polarizable continuum model with perturbative approach

    NASA Astrophysics Data System (ADS)

    Fukuda, Ryoichi; Ehara, Masahiro; Cammi, Roberto

    2014-02-01

    A perturbative approximation of the state specific polarizable continuum model (PCM) symmetry-adapted cluster-configuration interaction (SAC-CI) method is proposed for efficient calculations of the electronic excitations and absorption spectra of molecules in solutions. This first-order PCM SAC-CI method considers the solvent effects on the energies of excited states up to the first-order with using the zeroth-order wavefunctions. This method can avoid the costly iterative procedure of the self-consistent reaction field calculations. The first-order PCM SAC-CI calculations well reproduce the results obtained by the iterative method for various types of excitations of molecules in polar and nonpolar solvents. The first-order contribution is significant for the excitation energies. The results obtained by the zeroth-order PCM SAC-CI, which considers the fixed ground-state reaction field for the excited-state calculations, are deviated from the results by the iterative method about 0.1 eV, and the zeroth-order PCM SAC-CI cannot predict even the direction of solvent shifts in n-hexane for many cases. The first-order PCM SAC-CI is applied to studying the solvatochromisms of (2,2'-bipyridine)tetracarbonyltungsten [W(CO)4(bpy), bpy = 2,2'-bipyridine] and bis(pentacarbonyltungsten)pyrazine [(OC)5W(pyz)W(CO)5, pyz = pyrazine]. The SAC-CI calculations reveal the detailed character of the excited states and the mechanisms of solvent shifts. The energies of metal to ligand charge transfer states are significantly sensitive to solvents. The first-order PCM SAC-CI well reproduces the observed absorption spectra of the tungsten carbonyl complexes in several solvents.

  3. Electronic excitation spectra of molecules in solution calculated using the symmetry-adapted cluster-configuration interaction method in the polarizable continuum model with perturbative approach

    SciTech Connect

    Fukuda, Ryoichi Ehara, Masahiro; Cammi, Roberto

    2014-02-14

    A perturbative approximation of the state specific polarizable continuum model (PCM) symmetry-adapted cluster-configuration interaction (SAC-CI) method is proposed for efficient calculations of the electronic excitations and absorption spectra of molecules in solutions. This first-order PCM SAC-CI method considers the solvent effects on the energies of excited states up to the first-order with using the zeroth-order wavefunctions. This method can avoid the costly iterative procedure of the self-consistent reaction field calculations. The first-order PCM SAC-CI calculations well reproduce the results obtained by the iterative method for various types of excitations of molecules in polar and nonpolar solvents. The first-order contribution is significant for the excitation energies. The results obtained by the zeroth-order PCM SAC-CI, which considers the fixed ground-state reaction field for the excited-state calculations, are deviated from the results by the iterative method about 0.1 eV, and the zeroth-order PCM SAC-CI cannot predict even the direction of solvent shifts in n-hexane for many cases. The first-order PCM SAC-CI is applied to studying the solvatochromisms of (2,2{sup ′}-bipyridine)tetracarbonyltungsten [W(CO){sub 4}(bpy), bpy = 2,2{sup ′}-bipyridine] and bis(pentacarbonyltungsten)pyrazine [(OC){sub 5}W(pyz)W(CO){sub 5}, pyz = pyrazine]. The SAC-CI calculations reveal the detailed character of the excited states and the mechanisms of solvent shifts. The energies of metal to ligand charge transfer states are significantly sensitive to solvents. The first-order PCM SAC-CI well reproduces the observed absorption spectra of the tungsten carbonyl complexes in several solvents.

  4. Describing synchronization and topological excitations in arrays of magnetic spin torque oscillators through the Kuramoto model.

    PubMed

    Flovik, Vegard; Macià, Ferran; Wahlström, Erik

    2016-01-01

    The collective dynamics in populations of magnetic spin torque oscillators (STO) is an intensely studied topic in modern magnetism. Here, we show that arrays of STO coupled via dipolar fields can be modeled using a variant of the Kuramoto model, a well-known mathematical model in non-linear dynamics. By investigating the collective dynamics in arrays of STO we find that the synchronization in such systems is a finite size effect and show that the critical coupling-for a complete synchronized state-scales with the number of oscillators. Using realistic values of the dipolar coupling strength between STO we show that this imposes an upper limit for the maximum number of oscillators that can be synchronized. Further, we show that the lack of long range order is associated with the formation of topological defects in the phase field similar to the two-dimensional XY model of ferromagnetism. Our results shed new light on the synchronization of STO, where controlling the mutual synchronization of several oscillators is considered crucial for applications. PMID:27580938

  5. Describing synchronization and topological excitations in arrays of magnetic spin torque oscillators through the Kuramoto model

    NASA Astrophysics Data System (ADS)

    Flovik, Vegard; Macià, Ferran; Wahlström, Erik

    2016-09-01

    The collective dynamics in populations of magnetic spin torque oscillators (STO) is an intensely studied topic in modern magnetism. Here, we show that arrays of STO coupled via dipolar fields can be modeled using a variant of the Kuramoto model, a well-known mathematical model in non-linear dynamics. By investigating the collective dynamics in arrays of STO we find that the synchronization in such systems is a finite size effect and show that the critical coupling—for a complete synchronized state—scales with the number of oscillators. Using realistic values of the dipolar coupling strength between STO we show that this imposes an upper limit for the maximum number of oscillators that can be synchronized. Further, we show that the lack of long range order is associated with the formation of topological defects in the phase field similar to the two-dimensional XY model of ferromagnetism. Our results shed new light on the synchronization of STO, where controlling the mutual synchronization of several oscillators is considered crucial for applications.

  6. Describing synchronization and topological excitations in arrays of magnetic spin torque oscillators through the Kuramoto model

    PubMed Central

    Flovik, Vegard; Macià, Ferran; Wahlström, Erik

    2016-01-01

    The collective dynamics in populations of magnetic spin torque oscillators (STO) is an intensely studied topic in modern magnetism. Here, we show that arrays of STO coupled via dipolar fields can be modeled using a variant of the Kuramoto model, a well-known mathematical model in non-linear dynamics. By investigating the collective dynamics in arrays of STO we find that the synchronization in such systems is a finite size effect and show that the critical coupling—for a complete synchronized state—scales with the number of oscillators. Using realistic values of the dipolar coupling strength between STO we show that this imposes an upper limit for the maximum number of oscillators that can be synchronized. Further, we show that the lack of long range order is associated with the formation of topological defects in the phase field similar to the two-dimensional XY model of ferromagnetism. Our results shed new light on the synchronization of STO, where controlling the mutual synchronization of several oscillators is considered crucial for applications. PMID:27580938

  7. Processing of high resolution magic angle spinning spectra of breast cancer cells by the filter diagonalization method.

    PubMed

    Maria, Roberta Manzano; Moraes, Tiago Bueno; Magon, Claudio José; Venâncio, Tiago; Altei, Wanessa Fernanda; Andricopulo, Adriano Defini; Colnago, Luiz Alberto

    2012-10-01

    Proton nuclear magnetic resonance ((1)H NMR) spectroscopy for detection of biochemical changes in biological samples is a successful technique. However, the achieved NMR resolution is not sufficiently high when the analysis is performed with intact cells. To improve spectral resolution, high resolution magic angle spinning (HR-MAS) is used and the broad signals are separated by a T(2) filter based on the CPMG pulse sequence. Additionally, HR-MAS experiments with a T(2) filter are preceded by a water suppression procedure. The goal of this work is to demonstrate that the experimental procedures of water suppression and T(2) or diffusing filters are unnecessary steps when the filter diagonalization method (FDM) is used to process the time domain HR-MAS signals. Manipulation of the FDM results, represented as a tabular list of peak positions, widths, amplitudes and phases, allows the removal of water signals without the disturbing overlapping or nearby signals. Additionally, the FDM can also be used for phase correction and noise suppression, and to discriminate between sharp and broad lines. Results demonstrate the applicability of the FDM post-acquisition processing to obtain high quality HR-MAS spectra of heterogeneous biological materials.

  8. Selective excitation enables assignment of proton resonances and (1)H-(1)H distance measurement in ultrafast magic angle spinning solid state NMR spectroscopy.

    PubMed

    Zhang, Rongchun; Ramamoorthy, Ayyalusamy

    2015-07-21

    Remarkable developments in ultrafast magic angle spinning (MAS) solid-state NMR spectroscopy enabled proton-based high-resolution multidimensional experiments on solids. To fully utilize the benefits rendered by proton-based ultrafast MAS experiments, assignment of (1)H resonances becomes absolutely necessary. Herein, we propose an approach to identify different proton peaks by using dipolar-coupled heteronuclei such as (13)C or (15)N. In this method, after the initial preparation of proton magnetization and cross-polarization to (13)C nuclei, transverse magnetization of desired (13)C nuclei is selectively prepared by using DANTE (Delays Alternating with Nutations for Tailored Excitation) sequence and then, it is transferred to bonded protons with a short-contact-time cross polarization. Our experimental results demonstrate that protons bonded to specific (13)C atoms can be identified and overlapping proton peaks can also be assigned. In contrast to the regular 2D HETCOR experiment, only a few 1D experiments are required for the complete assignment of peaks in the proton spectrum. Furthermore, the finite-pulse radio frequency driven recoupling sequence could be incorporated right after the selection of specific proton signals to monitor the intensity buildup for other proton signals. This enables the extraction of (1)H-(1)H distances between different pairs of protons. Therefore, we believe that the proposed method will greatly aid in fast assignment of peaks in proton spectra and will be useful in the development of proton-based multi-dimensional solid-state NMR experiments to study atomic-level resolution structure and dynamics of solids. PMID:26203019

  9. Selective excitation enables assignment of proton resonances and (1)H-(1)H distance measurement in ultrafast magic angle spinning solid state NMR spectroscopy.

    PubMed

    Zhang, Rongchun; Ramamoorthy, Ayyalusamy

    2015-07-21

    Remarkable developments in ultrafast magic angle spinning (MAS) solid-state NMR spectroscopy enabled proton-based high-resolution multidimensional experiments on solids. To fully utilize the benefits rendered by proton-based ultrafast MAS experiments, assignment of (1)H resonances becomes absolutely necessary. Herein, we propose an approach to identify different proton peaks by using dipolar-coupled heteronuclei such as (13)C or (15)N. In this method, after the initial preparation of proton magnetization and cross-polarization to (13)C nuclei, transverse magnetization of desired (13)C nuclei is selectively prepared by using DANTE (Delays Alternating with Nutations for Tailored Excitation) sequence and then, it is transferred to bonded protons with a short-contact-time cross polarization. Our experimental results demonstrate that protons bonded to specific (13)C atoms can be identified and overlapping proton peaks can also be assigned. In contrast to the regular 2D HETCOR experiment, only a few 1D experiments are required for the complete assignment of peaks in the proton spectrum. Furthermore, the finite-pulse radio frequency driven recoupling sequence could be incorporated right after the selection of specific proton signals to monitor the intensity buildup for other proton signals. This enables the extraction of (1)H-(1)H distances between different pairs of protons. Therefore, we believe that the proposed method will greatly aid in fast assignment of peaks in proton spectra and will be useful in the development of proton-based multi-dimensional solid-state NMR experiments to study atomic-level resolution structure and dynamics of solids.

  10. Selective excitation enables assignment of proton resonances and {sup 1}H-{sup 1}H distance measurement in ultrafast magic angle spinning solid state NMR spectroscopy

    SciTech Connect

    Zhang, Rongchun; Ramamoorthy, Ayyalusamy

    2015-07-21

    Remarkable developments in ultrafast magic angle spinning (MAS) solid-state NMR spectroscopy enabled proton-based high-resolution multidimensional experiments on solids. To fully utilize the benefits rendered by proton-based ultrafast MAS experiments, assignment of {sup 1}H resonances becomes absolutely necessary. Herein, we propose an approach to identify different proton peaks by using dipolar-coupled heteronuclei such as {sup 13}C or {sup 15}N. In this method, after the initial preparation of proton magnetization and cross-polarization to {sup 13}C nuclei, transverse magnetization of desired {sup 13}C nuclei is selectively prepared by using DANTE (Delays Alternating with Nutations for Tailored Excitation) sequence and then, it is transferred to bonded protons with a short-contact-time cross polarization. Our experimental results demonstrate that protons bonded to specific {sup 13}C atoms can be identified and overlapping proton peaks can also be assigned. In contrast to the regular 2D HETCOR experiment, only a few 1D experiments are required for the complete assignment of peaks in the proton spectrum. Furthermore, the finite-pulse radio frequency driven recoupling sequence could be incorporated right after the selection of specific proton signals to monitor the intensity buildup for other proton signals. This enables the extraction of {sup 1}H-{sup 1}H distances between different pairs of protons. Therefore, we believe that the proposed method will greatly aid in fast assignment of peaks in proton spectra and will be useful in the development of proton-based multi-dimensional solid-state NMR experiments to study atomic-level resolution structure and dynamics of solids.

  11. Selective excitation enables assignment of proton resonances and 1H-1H distance measurement in ultrafast magic angle spinning solid state NMR spectroscopy

    NASA Astrophysics Data System (ADS)

    Zhang, Rongchun; Ramamoorthy, Ayyalusamy

    2015-07-01

    Remarkable developments in ultrafast magic angle spinning (MAS) solid-state NMR spectroscopy enabled proton-based high-resolution multidimensional experiments on solids. To fully utilize the benefits rendered by proton-based ultrafast MAS experiments, assignment of 1H resonances becomes absolutely necessary. Herein, we propose an approach to identify different proton peaks by using dipolar-coupled heteronuclei such as 13C or 15N. In this method, after the initial preparation of proton magnetization and cross-polarization to 13C nuclei, transverse magnetization of desired 13C nuclei is selectively prepared by using DANTE (Delays Alternating with Nutations for Tailored Excitation) sequence and then, it is transferred to bonded protons with a short-contact-time cross polarization. Our experimental results demonstrate that protons bonded to specific 13C atoms can be identified and overlapping proton peaks can also be assigned. In contrast to the regular 2D HETCOR experiment, only a few 1D experiments are required for the complete assignment of peaks in the proton spectrum. Furthermore, the finite-pulse radio frequency driven recoupling sequence could be incorporated right after the selection of specific proton signals to monitor the intensity buildup for other proton signals. This enables the extraction of 1H-1H distances between different pairs of protons. Therefore, we believe that the proposed method will greatly aid in fast assignment of peaks in proton spectra and will be useful in the development of proton-based multi-dimensional solid-state NMR experiments to study atomic-level resolution structure and dynamics of solids.

  12. Spin polarization of the split Kondo state.

    PubMed

    von Bergmann, Kirsten; Ternes, Markus; Loth, Sebastian; Lutz, Christopher P; Heinrich, Andreas J

    2015-02-20

    Spin-resolved scanning tunneling microscopy is employed to quantitatively determine the spin polarization of the magnetic field-split Kondo state. Tunneling conductance spectra of a Kondo-screened magnetic atom are evaluated within a simple model taking into account inelastic tunneling due to spin excitations and two Kondo peaks positioned symmetrically around the Fermi energy. We fit the spin state of the Kondo-screened atom with a spin Hamiltonian independent of the Kondo effect and account for Zeeman splitting of the Kondo peak in the magnetic field. We find that the width and the height of the Kondo peaks scales with the Zeeman energy. Our observations are consistent with full spin polarization of the Kondo peaks, i.e., a majority spin peak below the Fermi energy and a minority spin peak above. PMID:25763966

  13. Spin wave and vortex excitations of superfluid 3He-A in parallel-plate geometry.

    PubMed

    Yamashita, Minoru; Izumina, Ken; Matsubara, Akira; Sasaki, Yutaka; Ishikawa, Osamu; Takagi, Takeo; Kubota, Minoru; Mizusaki, Takao

    2008-07-11

    Quantized vortices with half-integer circulation, which are forbidden from existing in a conventional superfluid because of the single valueness of the wave function, are theoretically predicted to exist in superfluid 3He-A if the order parameters l over and d over form l over perpendicular d over texture. To form the l over perpendicular d over texture, we confined the superfluid between parallel plates with a 12.5 microm gap and applied a magnetic field of H=26.7 mT perpendicular to the plates to take NMR and orient d over perpendicular to l over. NMR spectra exhibit a negative-shift peak which probes that the uniform l over perpendicular d over texture is realized in our cell and show a new satellite signal under rotation. The rotation dependence of the satellite signal is interpreted that a Fréedericksz transition of l over texture is induced by rotation above 1.0 rad/s and vortices start to appear above 1.8 rad/s.

  14. Direct on-strip analysis of size- and time-resolved aerosol impactor samples using laser induced fluorescence spectra excited at 263 and 351 nm.

    PubMed

    Wang, Chuji; Pan, Yong-Le; James, Deryck; Wetmore, Alan E; Redding, Brandon

    2014-04-11

    We report a novel atmospheric aerosol characterization technique, in which dual wavelength UV laser induced fluorescence (LIF) spectrometry marries an eight-stage rotating drum impactor (RDI), namely UV-LIF-RDI, to achieve size- and time-resolved analysis of aerosol particles on-strip. The UV-LIF-RDI technique measured LIF spectra via direct laser beam illumination onto the particles that were impacted on a RDI strip with a spatial resolution of 1.2mm, equivalent to an averaged time resolution in the aerosol sampling of 3.6 h. Excited by a 263 nm or 351 nm laser, more than 2000 LIF spectra within a 3-week aerosol collection time period were obtained from the eight individual RDI strips that collected particles in eight different sizes ranging from 0.09 to 10 μm in Djibouti. Based on the known fluorescence database from atmospheric aerosols in the US, the LIF spectra obtained from the Djibouti aerosol samples were found to be dominated by fluorescence clusters 2, 5, and 8 (peaked at 330, 370, and 475 nm) when excited at 263 nm and by fluorescence clusters 1, 2, 5, and 6 (peaked at 390 and 460 nm) when excited at 351 nm. Size- and time-dependent variations of the fluorescence spectra revealed some size and time evolution behavior of organic and biological aerosols from the atmosphere in Djibouti. Moreover, this analytical technique could locate the possible sources and chemical compositions contributing to these fluorescence clusters. Advantages, limitations, and future developments of this new aerosol analysis technique are also discussed.

  15. Direct on-strip analysis of size- and time-resolved aerosol impactor samples using laser induced fluorescence spectra excited at 263 and 351 nm.

    PubMed

    Wang, Chuji; Pan, Yong-Le; James, Deryck; Wetmore, Alan E; Redding, Brandon

    2014-04-11

    We report a novel atmospheric aerosol characterization technique, in which dual wavelength UV laser induced fluorescence (LIF) spectrometry marries an eight-stage rotating drum impactor (RDI), namely UV-LIF-RDI, to achieve size- and time-resolved analysis of aerosol particles on-strip. The UV-LIF-RDI technique measured LIF spectra via direct laser beam illumination onto the particles that were impacted on a RDI strip with a spatial resolution of 1.2mm, equivalent to an averaged time resolution in the aerosol sampling of 3.6 h. Excited by a 263 nm or 351 nm laser, more than 2000 LIF spectra within a 3-week aerosol collection time period were obtained from the eight individual RDI strips that collected particles in eight different sizes ranging from 0.09 to 10 μm in Djibouti. Based on the known fluorescence database from atmospheric aerosols in the US, the LIF spectra obtained from the Djibouti aerosol samples were found to be dominated by fluorescence clusters 2, 5, and 8 (peaked at 330, 370, and 475 nm) when excited at 263 nm and by fluorescence clusters 1, 2, 5, and 6 (peaked at 390 and 460 nm) when excited at 351 nm. Size- and time-dependent variations of the fluorescence spectra revealed some size and time evolution behavior of organic and biological aerosols from the atmosphere in Djibouti. Moreover, this analytical technique could locate the possible sources and chemical compositions contributing to these fluorescence clusters. Advantages, limitations, and future developments of this new aerosol analysis technique are also discussed. PMID:24745745

  16. Glass-like recovery of antiferromagnetic spin ordering in a photo-excited manganite Pr0.7Ca0.3MnO3

    SciTech Connect

    Zhou, S.Y.; Langner, M.C.; Zhu, Y.; Chuang, Y.-D.; Rini, M.; Glover, T.E.; Hertlein, M.P.; Gonzalez, A.G. Cruz; Tahir, N.; Tomioka, Y.; Tokura, Y.; Hussain, Z.; Schoenlein, R.W.

    2014-01-16

    Electronic orderings of charges, orbitals and spins are observed in many strongly correlated electron materials, and revealing their dynamics is a critical step toward understanding the underlying physics of important emergent phenomena. Here we use time-resolved resonant soft x-ray scattering spectroscopy to probe the dynamics of antiferromagnetic spin ordering in the manganite Pr0:7Ca0:3MnO3 following ultrafast photo-exitation. Our studies reveal a glass-like recovery of the spin ordering and a crossover in the dimensionality of the restoring interaction from quasi-1D at low pump fluence to 3D at high pump fluence. This behavior arises from the metastable state created by photo-excitation, a state characterized by spin disordered metallic droplets within the larger charge- and spin-ordered insulating domains. Comparison with time-resolved resistivity measurements suggests that the collapse of spin ordering is correlated with the insulator-to-metal transition, but the recovery of the insulating phase does not depend on the re-establishment of the spin ordering.

  17. Near-yrast, medium-spin, excited states of {sup 91}Rb, {sup 93}Rb, and {sup 95}Rb

    SciTech Connect

    Simpson, G. S.; Sieja, K.; Dare, J. A.; Orlandi, R.; Smith, A. G.; Tsekhanovich, I.; Varley, B. J.; Durell, J. L.; Smith, J. F.; Jolie, J.; Linneman, A.; Scherillo, A.; Soldner, T.; Faust, H.; Zlomaniec, A.; Rzaca-Urban, T.; Ahmad, I.; Greene, J. P.

    2010-08-15

    The medium-spin structure of the nuclei {sup 93}Rb and {sup 95}Rb is studied following the neutron-induced fission of {sup 235}U at the PF1B neutron guide, using the FIFI spectrometer, and at the Lohengrin mass spectrometer of the Institut Laue-Langevin Grenoble. These nuclei, plus {sup 91}Rb, are also studied following the spontaneous fission of {sup 248}Cm and {sup 252}Cf sources, using the EUROGAM-II and Gammasphere detector arrays, respectively. A high-spin isomeric state, with a half-life of 111(11) ns, is found in {sup 93}Rb at an excitation energy of 4422.4 keV, which most likely corresponds to the fully aligned [{pi}(g{sub 9/2}) x {nu}(g{sub 7/2}h{sub 11/2})]{sub 27/2}{sup -} configuration. An analogous configuration is proposed for the 5297.9-keV level observed in {sup 91}Rb. A new E3 decay branch of the 1133.9-keV isomer in {sup 91}Rb is found, for which the rather low transition rate of B(E3)=3.8(10) W.u. is determined. The energy of the isomeric state of {sup 95}Rb is now proposed to be at 810.6 keV, with a spin of (9/2{sup +}), and its half-life determined to be T{sub 1/2}=94(7) ns. A cascade of prompt transitions is observed on top of the 810.6-keV isomer in {sup 95}Rb. The near-yrast structures of {sup 91}Rb, {sup 93}Rb, and {sup 95}Rb are compared to the results of shell-model calculations, which support the proposed 27/2{sup -} interpretation of states in {sup 91}Rb and {sup 93}Rb. An analogous 27/2{sup -} state is expected to occur in {sup 95}Rb, as a long-lived isomer at 3.24 MeV. No such isomeric decay could be observed in a measurement using the Lohengrin spectrometer, which shows that, if it exists, its population, following the fission of {sup 235}U, is at least four times lower than that of the analogous 27/2{sup -} isomer in {sup 97}Y.

  18. Quantum dynamics of excitations and decoherence in many-spin systems detected with Loschmidt echoes: its relation to their spreading through the Hilbert space.

    PubMed

    Sánchez, C M; Levstein, P R; Buljubasich, L; Pastawski, H M; Chattah, A K

    2016-06-13

    In this work, we overview time-reversal nuclear magnetic resonance (NMR) experiments in many-spin systems evolving under the dipolar Hamiltonian. The Loschmidt echo (LE) in NMR is the signal of excitations which, after evolving with a forward Hamiltonian, is recovered by means of a backward evolution. The presence of non-diagonal terms in the non-equilibrium density matrix of the many-body state is directly monitored experimentally by encoding the multiple quantum coherences. This enables a spin counting procedure, giving information on the spreading of an excitation through the Hilbert space and the formation of clusters of correlated spins. Two samples representing different spin systems with coupled networks were used in the experiments. Protons in polycrystalline ferrocene correspond to an 'infinite' network. By contrast, the liquid crystal N-(4-methoxybenzylidene)-4-butylaniline in the nematic mesophase represents a finite proton system with a hierarchical set of couplings. A close connection was established between the LE decay and the spin counting measurements, confirming the hypothesis that the complexity of the system is driven by the coherent dynamics.

  19. Energy dependence of the spin excitation anisotropy in uniaxial-strained BaFe1.9Ni0.1As2

    DOE PAGES

    Song, Yu; Lu, Xingye; Abernathy, Douglas L.; Tam, David W.; Niedziela, Jennifer L.; Tian, Wei; Si, Qimiao; Dai, Pengcheng; Luo, Huiqian

    2015-11-06

    In this study, we use inelastic neutron scattering to study the temperature and energy dependence of the spin excitation anisotropy in uniaxial-strained electron-doped iron pnictide BaFe1.9Ni0.1As2 near optimal superconductivity (Tc = 20K). Our work has been motivated by the observation of in-plane resistivity anisotropy in the paramagnetic tetragonal phase of electron-underdoped iron pnictides under uniaxial pressure, which has been attributed to a spin-driven Ising-nematic state or orbital ordering. Here we show that the spin excitation anisotropy, a signature of the spin-driven Ising-nematic phase, exists for energies below 60 meV in uniaxial-strained BaFe1.9Ni0.1As2. Since this energy scale is considerably larger thanmore » the energy splitting of the dxz and dyz bands of uniaxial-strained Ba(Fe1–xCox)2As2 near optimal superconductivity, spin Ising-nematic correlations are likely the driving force for the resistivity anisotropy and associated electronic nematic correlations.« less

  20. Quantum dynamics of excitations and decoherence in many-spin systems detected with Loschmidt echoes: its relation to their spreading through the Hilbert space.

    PubMed

    Sánchez, C M; Levstein, P R; Buljubasich, L; Pastawski, H M; Chattah, A K

    2016-06-13

    In this work, we overview time-reversal nuclear magnetic resonance (NMR) experiments in many-spin systems evolving under the dipolar Hamiltonian. The Loschmidt echo (LE) in NMR is the signal of excitations which, after evolving with a forward Hamiltonian, is recovered by means of a backward evolution. The presence of non-diagonal terms in the non-equilibrium density matrix of the many-body state is directly monitored experimentally by encoding the multiple quantum coherences. This enables a spin counting procedure, giving information on the spreading of an excitation through the Hilbert space and the formation of clusters of correlated spins. Two samples representing different spin systems with coupled networks were used in the experiments. Protons in polycrystalline ferrocene correspond to an 'infinite' network. By contrast, the liquid crystal N-(4-methoxybenzylidene)-4-butylaniline in the nematic mesophase represents a finite proton system with a hierarchical set of couplings. A close connection was established between the LE decay and the spin counting measurements, confirming the hypothesis that the complexity of the system is driven by the coherent dynamics. PMID:27140972

  1. Simulated infrared emission spectra of highly excited polyatomic molecules: a detailed model of the PAH-UIR hypothesis

    NASA Technical Reports Server (NTRS)

    Cook, D. J.; Saykally, R. J.

    1998-01-01

    A detailed description of the polycyclic aromatic hydrocarbon (PAH)/unidentified infrared band (UIR) mechanism is presented in which experimental spectral bandshape functions are used to simulate IR emission spectra for individual molecules. These spectra are additively superimposed to produce a conglomerate spectrum representative of a family of PAH molecules. Ab initio vibrational frequencies and intensities for nine PAHs (neutral and cationic) as large as ovalene are used in conjunction with measured bandshape and temperature-dependent redshift data to simulate the UIR bands. The calculated spectra of cations provide a closer match to the UIRs than do those of the neutrals. However, the PAH cations used in the simulations fail to reproduce the details of the UIR emission spectra. The discrepancies are potentially alleviated if both larger PAHs and a greater number of PAHs were included in the simulation.

  2. Simulated infrared emission spectra of highly excited polyatomic molecules: a detailed model of the PAH-UIR hypothesis.

    PubMed

    Cook, D J; Saykally, R J

    1998-02-01

    A detailed description of the polycyclic aromatic hydrocarbon (PAH)/unidentified infrared band (UIR) mechanism is presented in which experimental spectral bandshape functions are used to simulate IR emission spectra for individual molecules. These spectra are additively superimposed to produce a conglomerate spectrum representative of a family of PAH molecules. Ab initio vibrational frequencies and intensities for nine PAHs (neutral and cationic) as large as ovalene are used in conjunction with measured bandshape and temperature-dependent redshift data to simulate the UIR bands. The calculated spectra of cations provide a closer match to the UIRs than do those of the neutrals. However, the PAH cations used in the simulations fail to reproduce the details of the UIR emission spectra. The discrepancies are potentially alleviated if both larger PAHs and a greater number of PAHs were included in the simulation.

  3. An efficient computational scheme for electronic excitation spectra of molecules in solution using the symmetry-adapted cluster–configuration interaction method: The accuracy of excitation energies and intuitive charge-transfer indices

    SciTech Connect

    Fukuda, Ryoichi Ehara, Masahiro

    2014-10-21

    Solvent effects on electronic excitation spectra are considerable in many situations; therefore, we propose an efficient and reliable computational scheme that is based on the symmetry-adapted cluster-configuration interaction (SAC-CI) method and the polarizable continuum model (PCM) for describing electronic excitations in solution. The new scheme combines the recently proposed first-order PCM SAC-CI method with the PTE (perturbation theory at the energy level) PCM SAC scheme. This is essentially equivalent to the usual SAC and SAC-CI computations with using the PCM Hartree-Fock orbital and integrals, except for the additional correction terms that represent solute-solvent interactions. The test calculations demonstrate that the present method is a very good approximation of the more costly iterative PCM SAC-CI method for excitation energies of closed-shell molecules in their equilibrium geometry. This method provides very accurate values of electric dipole moments but is insufficient for describing the charge-transfer (CT) indices in polar solvent. The present method accurately reproduces the absorption spectra and their solvatochromism of push-pull type 2,2{sup ′}-bithiophene molecules. Significant solvent and substituent effects on these molecules are intuitively visualized using the CT indices. The present method is the simplest and theoretically consistent extension of SAC-CI method for including PCM environment, and therefore, it is useful for theoretical and computational spectroscopy.

  4. Zero-field splitting of the ground and excited triplet states of 2-naphthylphenylcarbene studied by hole-burning on triplet-triplet fluorescence excitation spectra

    NASA Astrophysics Data System (ADS)

    Kozankiewicz, B.; Bernard, J.; Migirdicyan, E.; Orrit, M.; Platz, M. S.

    1995-11-01

    Spectral holes were burned in the two main lines of the triplet-triplet 0-0 fluorescence excitation spectrum of 2-napththylphenylcarbene in n-hexane at 1.8 K. For the line assigned to pseudo-E/trans conformer, the central hole at the frequency of burning light has several narrow components separated by 0.3 ± 0.05 and 1.0 ± 0.1 GHz and a satellite doublet line on the low energy side, 14.5 ± 0.5 and 15.5 ± 0.5 GHz away. For the line assigned to the psuedo-Z/cis conformer, the central hole is accompanied by holes burned on the low energy side, 0.8 ± 0.1, 5.2 ± 0.1, 11.9 ± 0.1 and 16.2 ± 0.1 GHz away. The hole-burning pattern is explained by a model taking into account the zero-field splitting (ZFS) of the ground T 0 and excited T 1 triplet states as well as the selectivity of excitation relaxation by the intersystem crossing channel. Analysis provides information about the ZFS parameters of the T 1 state. For the pseudo-E/trans 2-NPC they are: D0 = 0.47 ± 0.02 cm -1, E0 = 0.017 ± 0.003 cm -1, D1 = 0.038 ± 0.003 cm -1 and E1 = 0.005 ± 0.001 cm -1.

  5. Distinguishing the laser-induced spin precession excitation mechanism in Fe/MgO(001) through field orientation dependent measurements

    SciTech Connect

    Ma, T. P.; Zhang, S. F.; Yang, Y.; Chen, Z. H.; Zhao, H. B.; Wu, Y. Z.

    2015-01-07

    Rotational field dependence of laser-induced magnetization precession in a single-crystal Fe/MgO(001) sample was studied by the time resolved magneto-optical Kerr effect. Polar and longitudinal magnetization components were separated by measuring precession dynamics under opposite fields. When the applied field is weaker than the anisotropy field of an Fe film, the precession amplitude is small for the field direction near the easy axis and becomes larger as the field rotates towards the hard axis, showing a four-fold symmetry in agreement with the in-plane magnetic anisotropy; whereas at higher fields, the amplitude displays a drop near the hard axis. Such precession behavior can be well reproduced using an excitation model with rapidly modified but slowly recovered magnetic anisotropy and considering the elliptical precession trajectory. Our results indicate that the dominant mechanism for triggering Fe spin precession is the anisotropy modulation correlating with the lattice thermalization, rather than the transient anisotropy modulation due to the high electron temperature within 1 ps.

  6. S1←S0 vibronic spectra and structure of cyclopropanecarboxaldehyde molecule in the S1 lowest excited singlet electronic state

    NASA Astrophysics Data System (ADS)

    Godunov, I. A.; Yakovlev, N. N.; Terentiev, R. V.; Maslov, D. V.; Bataev, V. A.; Abramenkov, A. V.

    2016-11-01

    The S1←S0 vibronic spectra of gas-phase absorption at room temperature and fluorescence excitation of jet-cooled cyclopropanecarboxaldehyde (CPCA, c-C3H5CHO)were obtained and analyzed. In addition, the quantum chemical calculation (CASPT2/cc-pVTZ)was carried out for CPCA in the ground (S0) and lowest excited singlet (S1) electronic states. As a result, it was proved that the S1←S0 electronic excitation of the CPCA conformers (syn and anti) causes (after geometrical relaxation) significant structural changes, namely, the carbonyl fragments become non-planar and the cyclopropyl groups rotate around the central C-C bond. As a consequence, the potential energy surface of CPCA in the S1 state has six minima, 1ab, 2ab, and 3ab, corresponding to three pairs of mirror symmetry conformers: a and b. It was shown that vibronic bands of experimental spectra can be assigned to the 2(S1)←syn(S0) electronic transition with the origin at 30,481 cm-1. A number of fundamental vibrational frequencies for the 2 conformer of CPCA were assigned. In addition, several inversional energy levels for the 2 conformer were found and the 2a↔2b potential function of inversion was determined. The experimental barrier to inversion and the equilibrium angle between the CH bond and the CCO plane were calculated as 570 cm-1 and 28°, respectively.

  7. Estimation of ground and excited state dipole moment of laser dyes C504T and C521T using solvatochromic shifts of absorption and fluorescence spectra

    NASA Astrophysics Data System (ADS)

    Basavaraja, Jana; Suresh Kumar, H. M.; Inamdar, S. R.; Wari, M. N.

    2016-02-01

    The absorption and fluorescence spectra of laser dyes: coumarin 504T (C504T) and coumarin 521T (C521T) have been recorded at room temperature in a series of non-polar and polar solvents. The spectra of these dyes showed bathochromic shift with increasing in solvent polarity indicating the involvement of π → π* transition. Kamlet-Taft and Catalan solvent parameters were used to analyze the effect of solvents on C504T and C521T molecules. The study reveals that both general solute-solvent interactions and specific interactions are operative in these two systems. The ground state dipole moment was estimated using Guggenheim's method and also by quantum mechanical calculations. The solvatochromic data were used to determine the excited state dipole moment (μe). It is observed that dipole moment value of excited state (μe) is higher than that of the ground state in both the laser dyes indicating that these dyes are more polar in nature in the excited state than in the ground state.

  8. Effect of anthocyanins, carotenoids, and flavonols on chlorophyll fluorescence excitation spectra in apple fruit: signature analysis, assessment, modelling, and relevance to photoprotection.

    PubMed

    Merzlyak, Mark N; Melø, Thor Bernt; Naqvi, K Razi

    2008-01-01

    Whole apple fruit (Malus domestica Borkh.) widely differing in pigment content and composition has been examined by recording its chlorophyll fluorescence excitation and diffuse reflection spectra in the visible and near UV regions. Spectral bands sensitive to the pigment concentration have been identified, and linear models for non-destructive assessment of anthocyanins, carotenoids, and flavonols via chlorophyll fluorescence measurements are put forward. The adaptation of apple fruit to high light stress involves accumulation of these protective pigments, which absorb solar radiation in broad spectral ranges extending from UV to the green and, in anthocyanin-containing cultivars, to the red regions of the spectrum. In ripening apples the protective effect in the blue region could be attributed to extrathylakoid carotenoids. A simple model, which allows the simulation of chlorophyll fluorescence excitation spectra in the visible range and a quantitative evaluation of competitive absorption by anthocyanins, carotenoids, and flavonols, is described. Evidence is presented to support the view that anthocyanins, carotenoids, and flavonols play, in fruit with low-to-moderate pigment content, the role of internal traps (insofar as they compete with chlorophylls for the absorption of incident light in specific spectral bands), affecting thereby the shape of the chlorophyll fluorescence excitation spectrum.

  9. Origin of French virgin olive oil registered designation of origins predicted by chemometric analysis of synchronous excitation-emission fluorescence spectra.

    PubMed

    Dupuy, Nathalie; Le Dréau, Yveline; Ollivier, Denis; Artaud, Jacques; Pinatel, Christian; Kister, Jacky

    2005-11-30

    The authentication of virgin olive oil samples requires usually the use of sophisticated and very expensive analytical techniques, so there is a need for fast and inexpensive analytical techniques for use in a quality control methodology. Virgin olive oils present an intense fluorescence spectra. Synchronous excitation-emission fluorescence spectroscopy (SEEFS) was assessed for origin determination of virgin olive oil samples from five French registered designation of origins (RDOs) (Nyons, Vallée des Baux, Aix-en-Provence, Haute-Provence, and Nice). The spectra present bands between 600 and 700 nm in emission due to chlorophylls a and b and pheophytins a and b. The bands between 275 and 400 nm in emission were attributed to alpha-, beta-, and gamma-tocopherols and to phenolic compounds, which characterize the virgin olive oils compared to other edible oils. The chemometric treatment (PLS1) of synchronous excitation-emission fluorescence spectra allows one to determine the origin of the oils from five French RDOs (Baux, Aix, Haute-Provence, Nice, and Nyons). Results were quite satisfactory, despite the similarity between two denominations of origin (Baux and Aix) that are composed by some common cultivars (Aglandau and Salonenque). The interpretation of the regression coefficients shows that RDOs are correlated to chlorophylls, pheophytins, tocopherols, and phenols compounds, which are different for each origin. SEEFS is part of a global analytic methodology that associates spectroscopic and chromatographic techniques. This approach can be used for traceability and vindicates the RDOs.

  10. Recent research directions in Fribourg: nuclear dynamics in resonances revealed by 2-dimensional EEL spectra, electron collisions with ionic liquids and electronic excitation of pyrimidine

    NASA Astrophysics Data System (ADS)

    Allan, Michael; Regeta, Khrystyna; Gorfinkiel, Jimena D.; Mašín, Zdeněk; Grimme, Stefan; Bannwarth, Christoph

    2016-05-01

    The article briefly reviews three subjects recently investigated in Fribourg: (i) electron collisions with surfaces of ionic liquids, (ii) two-dimensional (2D) electron energy loss spectra and (iii) resonances in absolute cross sections for electronic excitation of unsaturated compounds. Electron energy loss spectra of four ionic liquids revealed a number of excited states, including triplet states. A solution of a dye in an ionic liquid showed an energy-loss band of the solute, but not in all ionic liquids. 2D spectra reveal state-to-state information (given resonance to given final state) and are shown to be an interesting means to gain insight into dynamics of nuclear motion in resonances. Absolute cross sections for pyrimidine are reported as a function of scattering angle and as a function of electron energy. They reveal resonant structure which was reproduced very nicely by R-matrix calculations. The calculation provided an assignment of the resonances which reveals common patterns in compounds containing double bonds.

  11. Analysis of saturation transfer electron paramagnetic resonance spectra of a spin-labeled integral membrane protein, band 3, in terms of the uniaxial rotational diffusion model.

    PubMed Central

    Hustedt, E J; Beth, A H

    1995-01-01

    Algorithms have been developed for the calculation of saturation transfer electron paramagnetic resonance (ST-EPR) spectra of a nitroxide spin-label assuming uniaxial rotational diffusion, a model that is frequently used to describe the global rotational dynamics of large integral membrane proteins. One algorithm explicitly includes terms describing Zeeman overmodulation effects, whereas the second more rapid algorithm treats these effects approximately using modified electron spin-lattice and spin-spin relaxation times. Simulations are presented to demonstrate the sensitivity of X-band ST-EPR spectra to the rate of uniaxial rotational diffusion and the orientation of the nitroxide probe with respect to the diffusion axis. Results obtained by using the algorithms presented, which are based on the transition-rate formalism, are in close agreement with those obtained by using an eigenfunction expansion approach. The effects of various approximations used in the simulation algorithms are considered in detail. Optimizing the transition-rate formalism to model uniaxial rotational diffusion results in over an order of magnitude reduction in computation time while allowing treatment of nonaxial A- and g-tensors. The algorithms presented here are used to perform nonlinear least-squares analyses of ST-EPR spectra of the anion exchange protein of the human erythrocyte membrane, band 3, which has been affinity spin-labeled with a recently developed dihydrostilbene disulfonate derivative, [15N,2H13]-SL-H2DADS-MAL. These results suggest that all copies of band 3 present in intact erythrocytes undergo rotational diffusion about the membrane normal axis at a rate consistent with a band 3 dimer. PMID:8534811

  12. Crossover from inelastic magnetic scattering of Cooper pairs to spin-wave dispersion produces the low-energy kink structure in the spectra of cuprate superconductors

    NASA Astrophysics Data System (ADS)

    Das, Tanmoy; Markiewicz, R. S.; Bansil, A.

    2012-04-01

    We present GW-based-self-energy calculations for the state of the coexisting spin-density-wave and d-wave superconductivity in a series of cuprate superconductors. The spin-resonance spectrum is found to exhibit the typical “hourglass” form whose upward and downward dispersion branches come from the gapped-spin-wave and magnetic scattering, of Cooper pairs, respectively. We show that the crossover between these two different dispersion features leads to an abrupt change of slope in the quasiparticle self-energy, and hence, the low-energy kink commences in the single-particle quasiparticle spectrum. The calculated electron-boson-coupling strength agrees well with experimental data as a function of temperature, doping, and material. The results demonstrate that electronic correlations dominate the quasiparticle spectra of cuprates near the low-energy kink, suggesting a relatively smaller role for phonons in this energy range.

  13. Spin Excitations in CARBON-14 and MAGNESIUM-26: a Complementary Analysis of Electron, Pion, and Proton Scattering Data

    NASA Astrophysics Data System (ADS)

    Plum, Michael Andrew

    Inelastic magnetic electron scattering measurements on ('14)C have been performed at the Bates Linear Accelerator. Candidate J('(pi)) =4('-) states are identified at E(,x) = 11.7, 17.3, and 24.4 MeV, and the corresponding M4 strengths are extracted. These M4 strengths are combined with existing ((pi),(pi)') data to determine the isoscalar and isovector spin transition amplitudes, or Z-coefficients Z(,0) and Z(,1). Shell model calculations are found to correctly predict the observed excitation energies to within 1.7 MeV. These calculations are also found to correctly predict the isospin dependent amplitudes of the spin transition density. However, these calculations overpredict the "isoscalar strength" and "isovector strength" by factors of 3.6 and 2.3, respectively. The deduced Z-coefficients are also used to predict the results of ('14)C(p,p') and ('14)C(p,n) experiments. Forthcoming results of these experiments will provide a sensitive test of the proton-nucleus force. Electron scattering measurements have also been performed for the low lying transverse electric states in ('14)C at E(,x) = 6.091, 6.728, 7.012, and 8.318 MeV, and also for states at E(,x) = 9.84, 10.50, 11.29, 12.20, 12.86, 13.62, 14.03, 14.92, 15.96, 16.53, and 22.1 MeV. The previously unobserved 16.53 MeV state has a form factor shape which is consistent with E2 and M2 transitions. The 22.1 MeV state is the isobaric analog of the ('14)B gound state, and based upon its excitation energy, the ('14)B -('14)C Coulomb energy is calculated to be 2.25 (+OR-) 0.10 MeV. Electron scattering measurements were also performed on ('26)Mg. Candidate 6('-) states are identified at E(,x) = 7.54, 9.17, 12.50, 12.88, 13.00, 13.97, 14.50, 15.36, 15.46, 16.5, and 18.05 MeV, and the M6 strengths for these states are extracted. Shell model calculations are found to be in disagreement with the observed excitation energies and M6 strengths. Candidate 4('-) states are also identified at E(,x) = 8.04, 8.44, 8.70, 10

  14. Infrared and electronic absorption spectra as well as ultrafast spin dynamics in isolated Co3+(EtOH) and Co3+(EtOH,H2O) clusters

    NASA Astrophysics Data System (ADS)

    Jin, Wei; Becherer, Markus; Bellaire, Daniel; Lefkidis, Georgios; Gerhards, Markus; Hübner, Wolfgang

    2014-04-01

    We present a combined theoretical and experimental study of the infrared (IR) and electronic absorption spectra in a molecular beam experiment as well as an analysis of spin dynamics in the clusters Co3+(EtOH) and Co3+(EtOH,H2O). The calculated IR and ground-state absorption spectra show very good agreement with experiment. By using high-level quantum chemistry methods, laser-induced ultrafast spin-flip scenarios in these structures are predicted. For the spin flip in Co3+(EtOH), our investigation indicates a 5 meV tolerance with respect to the laser detuning and a 6.5 meV tolerance with respect to the pulse spectral broadening, which are quite acceptable for the experimental implementation. In addition, we find that with the increase of the laser detuning the fitness of the processes gradually decays to zero on both sides but with different origins. This joint study of the homotrinuclear clusters provides insight into the experimentally observed spectra and optical properties, and steps towards the optical control of molecular magnetism for future spintronics application.

  15. Separated spin-up and spin-down evolution of degenerated electrons in two-dimensional systems: Dispersion of longitudinal collective excitations in plane and nanotube geometry

    NASA Astrophysics Data System (ADS)

    Andreev, Pavel A.; Kuz'menkov, L. S.

    2016-01-01

    Applying the separated spin evolution quantum hydrodynamics to the two-dimensional electron gas in plane samples and nanotubes located in external magnetic fields we have found a novel type of waves in the electron gas which is called spin-electron acoustic wave. A separate spin-up and spin-down electrons' evolution reveals the replacement of the Langmuir wave by a pair of hybrid waves. One of the two hybrid waves is a modified Langmuir wave. Another hybrid wave is a spin-electron acoustic wave. We studied the dispersion of these waves in two-dimensional structures of electrons. We also considered the dependence of dispersion properties on spin polarization of electrons in an external magnetic field.

  16. Haldane-Hubbard Mott Insulator: From Tetrahedral Spin Crystal to Chiral Spin Liquid

    NASA Astrophysics Data System (ADS)

    Hickey, Ciaran; Cincio, Lukasz; Papic, Zlatko; Paramekanti, Arun

    Motivated by recent experimental realizations of artificial gauge fields in ultracold atoms, we study the honeycomb lattice Haldane-Hubbard Mott insulator of spin- 1 / 2 fermions using exact diagonalization and density matrix renormalization group methods. We show that this model exhibits various chiral magnetic orders including a wide regime of triple-Q tetrahedral order. Incorporating third-neighbor hopping frustrates and ultimately melts this tetrahedral spin crystal. From analyzing low energy spectra, many-body Chern numbers, entanglement spectra, and modular matrices, we identify the molten state as a chiral spin liquid with gapped semion excitations.

  17. Characterizing the Structures, Spectra, and Energy Landscapes Involved in the Excited-State Proton Transfer Process of Red Fluorescent Protein LSSmKate1.

    PubMed

    Chen, Fasheng; Zeng, Qiao; Zhuang, Wei; Liang, WanZhen

    2016-09-22

    By applying molecular dynamics (MD) simulations and quantum chemical calculations, we have characterized the states and processes involved in the excited-state proton transfer (ESPT) of LSSmKate1. MD simulations identify two stable structures in the electronic ground state of LSSmKate1, one with a protonated chromophore and the other with a deprotonated chromophore, thus leading to two separate low-energy absorption maxima with a large energy spacing, as observed in the calculated and experimentally measured absorption spectra. Proton transfer is induced by electronic excitation. When LSSmKate1 is excited, the electrons in the chromophore are transferred from the phenol ring to the N-acylimine moiety; the acidity of a phenolic hydroxyl group is thus enhanced. The calculated potential energy curves (PECs) exhibit energetic feasibility in the generation of the fluorescent species in LSSmKate1, and the exact agreement between the calculated and experimentally measured values of the large Stokes shift further provides solid theoretical evidence for the ESPT process taking place in photoexcited LSSmKate1. The molecular environments play a significant role in the geometries and absorption/emission energies of the chromophores. Overall, TD-ωB97X-D/molecular mechanics (MM) provides a better description of the optical properties of LSSmKate1 than TD-B3LYP/MM, although it always overestimates the excitation energies. PMID:27581731

  18. Characterizing the Structures, Spectra, and Energy Landscapes Involved in the Excited-State Proton Transfer Process of Red Fluorescent Protein LSSmKate1.

    PubMed

    Chen, Fasheng; Zeng, Qiao; Zhuang, Wei; Liang, WanZhen

    2016-09-22

    By applying molecular dynamics (MD) simulations and quantum chemical calculations, we have characterized the states and processes involved in the excited-state proton transfer (ESPT) of LSSmKate1. MD simulations identify two stable structures in the electronic ground state of LSSmKate1, one with a protonated chromophore and the other with a deprotonated chromophore, thus leading to two separate low-energy absorption maxima with a large energy spacing, as observed in the calculated and experimentally measured absorption spectra. Proton transfer is induced by electronic excitation. When LSSmKate1 is excited, the electrons in the chromophore are transferred from the phenol ring to the N-acylimine moiety; the acidity of a phenolic hydroxyl group is thus enhanced. The calculated potential energy curves (PECs) exhibit energetic feasibility in the generation of the fluorescent species in LSSmKate1, and the exact agreement between the calculated and experimentally measured values of the large Stokes shift further provides solid theoretical evidence for the ESPT process taking place in photoexcited LSSmKate1. The molecular environments play a significant role in the geometries and absorption/emission energies of the chromophores. Overall, TD-ωB97X-D/molecular mechanics (MM) provides a better description of the optical properties of LSSmKate1 than TD-B3LYP/MM, although it always overestimates the excitation energies.

  19. Excited state solvatochromic and prototropic behaviour of 4-aminodiphenylamine and 4,4'-diaminodiphenylamine—A comparative study by electronic spectra

    NASA Astrophysics Data System (ADS)

    Nayaki, S. Kothai; Swaminathan, M.

    2006-06-01

    Solvatochromic and prototropic behaviour of 4-aminodiphenylamine (4ADA) and 4,4'-diaminodiphenylamine (DADA) have been investigated in the solvents of different polarity and at various acid-base concentrations in the ground and excited states using absorption and fluorescence spectra. Solvatochromic shifts have been analysed and observed shifts are explained by the hydrogen bonding interactions. The prototropic study reveals that (i) absorption maximum of monocation of DADA is red shifted to its neutral form, and (ii) the fluorescence of 4ADA is red shifted on protonation. The abnormal fluorescence of 4ADA + is found to be due to large solvent relaxation in polar medium.

  20. Electronic Raman scattering with excitation between localized states observed in the zinc M{sub 2,3} soft x-ray spectra of ZnS

    SciTech Connect

    Zhou, L.; Callcott, T.A.; Jia, J.J.

    1997-04-01

    Zn M{sub 2,3} soft x-ray fluorescence (SXF) spectra of ZnS and ZnS{sub .5}Se{sub .5} excited near threshold show strong inelastic scattering effects that can be explained using a simple model and an inelastic scattering theory based on second order perturbation theory. This scattering is often called electronic resonance Raman scattering. Tulkki and Aberg have developed this theory in detail for atomic systems, but their treatment can be applied to solid systems by utilizing electronic states characteristic of solids rather than of atomic systems.

  1. Impact of magnetic fluctuations on lattice excitations in fcc nickel.

    PubMed

    Körmann, Fritz; Ma, Pui-Wai; Dudarev, Sergei L; Neugebauer, Jörg

    2016-02-24

    The spin-space averaging formalism is applied to compute atomic forces and phonon spectra for magnetically excited states of fcc nickel. Transverse and longitudinal magnetic fluctuations are taken into account by a combination of magnetic special quasi random structures and constrained spin-density-functional theory. It turns out that for fcc Ni interatomic force constants and phonon spectra are almost unaffected by both kinds of spin fluctuations. Given the computational expense to simulate coupled magnetic and atomic fluctuations, this insight facilitates computational modeling of magnetic alloys such as Ni-based superalloys.

  2. Storage and retrieval of collective excitations on a long-lived spin transition in a rare-earth ion-doped crystal.

    PubMed

    Goldschmidt, E A; Beavan, S E; Polyakov, S V; Migdall, A L; Sellars, M J

    2013-04-22

    Robust, long-lived optical quantum memories are important components of many quantum information and communication protocols. We demonstrate coherent generation, storage, and retrieval of excitations on a long-lived spin transition via spontaneous Raman scattering in a rare-earth ion-doped crystal. We further study the time dynamics of the optical correlations in this system. This is the first demonstration of its kind in a solid and an enabling step toward realizing a solid-state quantum repeater.

  3. Study of the Effect of the Pulse Width of the Excitation Source on the Two-Photon Absorption and Two-Photon Circular Dichroism Spectra of Biaryl Derivatives.

    PubMed

    Vesga, Yuly; Hernandez, Florencio E

    2016-09-01

    Herein we report on the expanded theoretical calculations and the experimental measurements of the two-photon absorption (TPA) and two-photon circular dichroism (TPCD) spectra of a series of optically active biaryl derivatives (R-BINOL, R-VANOL, and R-VAPOL) using femtosecond pulses. The comparative analysis of the experimental TPCD spectra obtained with our tunable amplified femtosecond system with those previously measured in our group on the same series of compounds in the picosecond regime reveals a decrease in the amplitude of the signal and an improvement in matching with the theory in the former. These results can be explained based on the negligible contribution of excited state absorption (ESA) using femtosecond pulses compared to the picosecond regime. We show how ESA affects both the strength of the signal and the shape of the TPA and TPCD spectra. TPA and TPCD spectra were obtained using the double L-scan technique over a broad spectral range (450-750 nm) using 90 fs pulses at 50 Hz repetition rate produced by an amplified femtosecond system. The theoretical calculations were performed using modern analytical response theory within the time-dependent density functional theory (TD-DFT) approach using CAM-B3LYP and 6-311++G(d,p) basis sets. PMID:27525702

  4. Coupling of spin and orbital excitations in the iron-based superconductor FeSe0.5Te0.5

    SciTech Connect

    Lee, S.-H.; Xu, Guangyong; Ku, Wei; Wen, J.S.; Lee, C.C.; Katayama, N.; Xu, Z.J.; Ji, S.; Lin, Z.W.; Gu, G.D.; Yang, H.-B.; Johnson, Peter D.; Pan, Z.-H.; Valla, Tonica; Fujita, M.; Sato, T.J.; Chang, S.; Yamada, K.; Tranquada, John M.

    2010-06-14

    We present a combined analysis of neutron scattering and photoemission measurements on superconducting FeSe{sub 0.5} Te{sub 0.5} . The low-energy magnetic excitations disperse only in the direction transverse to the characteristic wave vector (1/2 ,0,0) whereas the electronic Fermi surface near (1/2 ,0,0) appears to consist of four incommensurate pockets. While the spin resonance occurs at an incommensurate wave vector compatible with nesting, neither spin-wave nor Fermi-surface-nesting models can describe the magnetic dispersion. We propose that a coupling of spin and orbital correlations is key to explaining this behavior. If correct, it follows that these nematic fluctuations are involved in the resonance and could be relevant to the pairing mechanism.

  5. Coupling of Spin and Orbital Excitations in the Iron-based Superconductor FeSe0.5Te0.5

    SciTech Connect

    Lee, S.H.; Xu, G.; Ku, W.; Wen, J.S.; Lee, C.C.: Katayama, N.; Xu, Z.J.; Ji, S.; Lin, Z.W.; Gu, G. D.; Yang, H.-B.; Johnson, P.D.; Pan, Z.-H.; Valla, T.; Fujita, M.; Sato, T.J.; Chang, S.; Yamada, K.; Tranquada, J.M.

    2010-06-14

    We present a combined analysis of neutron scattering and photoemission measurements on superconducting FeSe{sub 0.5}Te{sub 0.5}. The low-energy magnetic excitations disperse only in the direction transverse to the characteristic wave vector (1/2,0,0) whereas the electronic Fermi surface near (1/2,0,0) appears to consist of four incommensurate pockets. While the spin resonance occurs at an incommensurate wave vector compatible with nesting, neither spin-wave nor Fermi-surface-nesting models can describe the magnetic dispersion. We propose that a coupling of spin and orbital correlations is key to explaining this behavior. If correct, it follows that these nematic fluctuations are involved in the resonance and could be relevant to the pairing mechanism.

  6. Quasi-two-dimensional spin and phonon excitations in La1.965Ba0.035CuO4

    DOE PAGES

    Wagman, J. J.; Parshall, D.; Stone, Matthew B.; Savici, Andrei T.; Zhao, Yang; Dabkowska, H. A.; Gaulin, B. D.

    2015-06-03

    Here, we present time-of-fight inelastic neutron scattering measurements of La1.965Ba0.035CuO4 (LBCO), a lightly doped member of the high temperature superconducting La-based cuprate family. By using time-of-flight neutron instrumentation coupled with single crystal sample rotation we obtain a four-dimensional data set (three Q and one energy) that is both comprehensive and spans a large region of reciprocal space. Our measurements identify rich structure in the energy dependence of the highly dispersive spin excitations, which are centered at equivalent (1/2, 1/2, L) wave-vectors. These structures correlate strongly with several crossings of the spin excitations with the lightly dispersive phonons found in thismore » system. These eects are signicant and account for on the order of 25% of the total inelastic scattering for energies between ≈5 and 40meV at low |Q|. Interestingly, this scattering also presents little or no L-dependence. As the phonons and dispersive spin excitations centred at equivalent (1/2, 1/2, L) wave-vectors are common to all members of La-based 214 copper oxides, we conclude such strong quasi-two dimensional scattering enhancements are likely to occur in all such 214 families of materials, including those concentrations corresponding to superconducting ground states. Such a phenomenon appears to be a fundamental characteristic of these materials and is potentially related to superconducting pairing.« less

  7. Low-temperature heat transport of spin-gapped quantum magnets

    NASA Astrophysics Data System (ADS)

    Zhao, Xia; Zhao, ZhiYing; Liu, XuGuang; Sun, XueFeng

    2016-11-01

    This article reviews low-temperature heat transport studies of spin-gapped quantum magnets in the last few decades. Quantum magnets with small spins and low dimensionality exhibit a variety of novel phenomena. Among them, some systems are characteristic of having quantum-mechanism spin gap in their magnetic excitation spectra, including spin-Peierls systems, S=1 Haldane chains, S= 1/2 spin ladders, and spin dimmers. In some particular spin-gapped systems, the XY-type antiferromagnetic state induced by magnetic field that closes the spin gap can be described as a magnon Bose-Einstein condensation (BEC). Heat transport is effective in probing the magnetic excitations and magnetic phase transitions, and has been extensively studied for the spin-gapped systems. A large and ballistic spin thermal conductivity was observed in the two-leg Heisenberg S=1/2 ladder compounds. The characteristic of magnetic thermal transport of the Haldane chain systems is quite controversial on both the theoretical and experimental results. For the spin-Peierls system, the spin excitations can also act as heat carriers. In spin-dimer compounds, the magnetic excitations mainly play a role of scattering phonons. The magnetic excitations in the magnon BEC systems displayed dual roles, carrying heat or scattering phonons, in different materials.

  8. Comparative analysis of the vibrational structure of the absorption spectra of acrolein in the excited ( S 1) electronic state

    NASA Astrophysics Data System (ADS)

    Koroleva, L. A.; Tyulin, V. I.; Matveev, V. K.; Pentin, Yu. A.

    2012-04-01

    The assignments of absorption bands of the vibrational structure of the UV spectrum are compared with the assignments of bands obtained by the CRDS method in a supersonic jet from the time of laser radiation damping for the trans isomer of acrolein in the excited ( S 1) electronic state. The ν00 trans = 25861 cm-1 values and fundamental frequencies, including torsional vibration frequency, obtained by the two methods were found to coincide in the excited electronic state ( S 1) for this isomer. The assignments of several absorption bands of the vibrational structure of the spectrum obtained by the CRDS method were changed. Changes in the assignment of (0-v') transition bands of the torsional vibration of the trans isomer in the Deslandres table from the ν00 trans trans origin allowed the table to be extended to high quantum numbers v'. The torsional vibration frequencies up to v' = 5 were found to be close to the frequencies found by analyzing the vibrational structure of the UV spectrum and calculated quantum-mechanically. The coincidence of the barrier to internal rotation (the cis-trans transition) in the one-dimensional model with that calculated quantum-mechanically using the two-dimensional model corresponds to a planar structure of the acrolein molecule in the excited ( S 1) electronic state.

  9. Singlet-triplet excitations and long range entanglement in the spin-orbital liquid candidate FeSc2S4

    NASA Astrophysics Data System (ADS)

    Laurita, N. J.; Deisenhofer, J.; Pan, Lidong; Morris, C. M.; Schmidt, M.; Johnsson, M.; Tsurkan, V.,; Loidl, A.; Armitage, N. P.

    2015-03-01

    Theoretical models of the spin-orbital liquid (SOL) FeSc2S4 have predicted it to be in close proximity to a quantum critical point separating a spin-orbital liquid phase from a long-range ordered magnetic phase. Here, we examine the magnetic excitations of FeSc2S4 through time-domain terahertz spectroscopy under an applied magnetic field. At low temperatures an excitation emerges that we attribute to a singlet-triplet excitation from the SOL ground state. A three-fold splitting of this excitation is observed as a function of applied magnetic field. Using experimentally obtained parameters we compare to existing theoretical models to determine FeSc2S4's proximity to the quantum critical point and establish FeSc2S4 as a SOL with long-range entanglement. Work at Johns Hopkins was supported by the Gordon and Betty Moore Foundation through Grant GBMF2628, the DOE-BES through DE-FG02-08ER46544, and the ARCS Foundation.

  10. Fluorescence Excitation Spectra of Photo-Fragmented Nitrobenzene Using a Picosecond Laser: Potential Evidence for no Produced by Two Distinct Channels.

    NASA Astrophysics Data System (ADS)

    Lue, Christopher J.; Tanjaroon, Chakree; Johnson, J. Bruce; Reeve, Scott W.; Allen, Susan D.

    2013-06-01

    Upon absorption of a UV photon, nitrobenzene can dissociate into C_6H_5O and NO through two different mechanisms. Evidence for these mechanisms was obtained from velocity map imaging (VMI) studies and theoretical calculations. VMI experiments showed NO produced with two distinct rotational distributions, which the calculations explained as a fast and a slow channel for NO production. We have recorded high resolution fluorescence excitation spectra of the NO resulting from photo-fragmented nitrobenzene using a pulsed picosecond tunable laser (pulse width ≈ 15 ps) by means of a two-color process. In the two-color process, photons of a particular energy dissociated the nitrobenzene while photons of a different energy probed the A^2Σ^+← X^2Π_{(1/2,3/2)} NO band system between 225-260 nm. This laser system allowed us to vary the delay between the photolysis and excitation pulses. At longer delays (>1 ns), we observed an increase in the population of NO, which may be evidence that at least two photolysis channels produce NO. We present the spectra we recorded at various photolysis/probe delays ranging from 0.025 to 1.5 ns. The spectral subtraction method we used to observe the production increase is introduced. Hause, M. L.; Herath, N.; Zhu, R.; Lin, M. C. and Suits, A. G. Nat Chem, Nature Publishing Group, 2011, 3, 932-937

  11. Spectra, Emission Yields, Cross Sections, and Kinetic Energy Distributions of Hydrogen Atoms from H2 X 1Eg+-d 3IIu Excitation by Electron Impact

    NASA Astrophysics Data System (ADS)

    Liu, Xianming; Shemansky, Donald E.; Yoshii, Jean; Johnson, Paul V.; Malone, Charles P.; Ajello, Joseph M.

    2016-02-01

    Electron-impact excitation of H2 triplet states plays an important role in the heating of outer planet upper thermospheres. The {d}3{{{\\Pi }}}u state is the third ungerade triplet state, and the {d}3{{{\\Pi }}}u-a{}3{{{Σ }}}g+ emission is the largest cascade channel for the a{}3{{{Σ }}}g+ state. Accurate energies of the d{}3{{{\\Pi }}}u-(v, J) levels are calculated from an ab initio potential energy curve. Radiative lifetimes of the {d}3{{{\\Pi }}}u(v, J) levels are obtained by an accurate evaluation of the {d}3{{{\\Pi }}}u-a{}3{{{Σ }}}g+ transition probabilities. The emission yields are determined from experimental lifetimes and calculated radiative lifetimes and are further verified by comparing experimental and synthetic {d}3{{{\\Pi }}}u-a{}3{{{Σ }}}g+ spectra at 20 eV impact energy. Spectral analysis revealed that multipolar components beyond the dipolar term are required to model the {X}1{{{Σ }}}g+-{d}3{{{\\Pi }}}u excitation, and significant cascade excitation occurs at the {d}3{{{\\Pi }}}u(v = 0,1) levels. Kinetic energy (Ek) distributions of H atoms produced via predissociation of the {d}3{{{\\Pi }}}u state and the {d}3{{{\\Pi }}}u-a{}3{{{Σ }}}g+-b{}3{{{Σ }}}u+ cascade dissociative emission are obtained. Predissociation of the {d}3{{{\\Pi }}}u state produces H atoms with an average Ek of 2.3 ± 0.4 eV/atom, while the Ek distribution of the {d}3{{{\\Pi }}}u-a{}3{{{Σ }}}g+-b{}3{{{Σ }}}u+ channel is similar to that of the {X}1{{{Σ }}}g+-a{}3{{{Σ }}}g+-b{}3{{{Σ }}}u+ channel and produces H(1s) atoms with an average Ek of 1.15 ± 0.05 eV/atom. On average, each H2 excited to the {d}3{{{\\Pi }}}u state in an H2-dominated atmosphere deposits 3.3 ± 0.4 eV into the atmosphere, while each H2 directly excited to the a{}3{{{Σ }}}g+ state gives 2.2-2.3 eV to the atmosphere. The spectral distribution of the calculated a{}3{{{Σ }}}g+ -b{}3{{{Σ }}}u+ continuum emission due to the {X}1{{{Σ }}}g+-{d}3{{{\\Pi }}}u excitation is significantly different from

  12. Lowest excited states and optical absorption spectra of donor-acceptor copolymers for organic photovoltaics: a new picture emerging from tuned long-range corrected density functionals.

    PubMed

    Pandey, Laxman; Doiron, Curtis; Sears, John S; Brédas, Jean-Luc

    2012-11-01

    Polymers with low optical gaps are of importance to the organic photovoltaics community due to their potential for harnessing a large portion of the solar energy spectrum. The combination along their backbones of electron-rich and electron-deficient fragments contributes to the presence of low-lying excited states that are expected to display significant charge-transfer character. While conventional hybrid functionals are known to provide unsatisfactory results for charge-transfer excitations at the time-dependent DFT level, long-range corrected (LRC) functionals have been reported to give improved descriptions in a number of systems. Here, we use such LRC functionals, considering both tuned and default range-separation parameters, to characterize the absorption spectra of low-optical-gap systems of interest. Our results indicate that tuned LRC functionals lead to simulated optical-absorption properties in good agreement with experimental data. Importantly, the lowest-lying excited states (excitons) are shown to present a much more localized nature than initially anticipated.

  13. Near infrared excited micro-Raman spectra of 4:1 methanol-ethanol mixture and ruby fluorescence at high pressure

    NASA Astrophysics Data System (ADS)

    Wang, X. B.; Shen, Z. X.; Tang, S. H.; Kuok, M. H.

    1999-06-01

    Near infrared (NIR) lasers, as a new excitation source for Raman spectroscopy, has shown its unique advantages and is being increasingly used for some special samples, such as those emitting strong fluorescence in the visible region. This article focuses on some issues related to high-pressure micro-Raman spectroscopy using NIR excitation source. The Raman spectra of 4:1 methanol-ethanol mixture (4:1 M-E) show a linear variation in both Raman shifts and linewidths under pressure up to 18 GPa. This result is useful in distinguishing Raman scattering of samples from that of the alcohol mixture, an extensively used pressure-transmitting medium. The R1 fluorescence in the red region induced by two-photon absorption of the NIR laser is strong enough to be used as pressure scale. The frequency and line width of the R1 lines are very sensitive to pressure change and the glass transition of the pressure medium. Our results manifest that it is reliable and convenient to use NIR induced two-photon excited fluorescence of ruby for both pressure calibration and distribution of pressure in the 4:1 M-E pressure transmitting medium.

  14. Spin-flip, tensor equation-of-motion configuration interaction with a density-functional correction: A spin-complete method for exploring excited-state potential energy surfaces

    NASA Astrophysics Data System (ADS)

    Zhang, Xing; Herbert, John M.

    2015-12-01

    We revisit the formalism of the spin-adapted, spin-flip (SA-SF) configuration-interaction singles (CIS) method based on a tensor equation-of-motion formalism that affords proper spin eigenstates without sacrificing single-reference simplicity. Matrix elements for SA-SF-CIS are then modified in a manner similar to collinear spin-flip time-dependent density functional theory (SF-TDDFT), to include a DFT exchange-correlation correction. The performance of this method, which we call SA-SF-DFT, is evaluated numerically and we find that it systematically improves the energies of electronic states that exhibit significant spin contamination within the conventional SF-TDDFT approach. The new method cures the state assignment problem that plagues geometry optimizations and ab initio molecular dynamics simulations using traditional SF-TDDFT, without sacrificing computational efficiency, and furthermore provides correct topology at conical intersections, including those that involve the ground state, unlike conventional TDDFT. As such, SA-SF-DFT appears to be a promising method for generating excited-state potential energy surfaces at DFT cost.

  15. Spin-flip, tensor equation-of-motion configuration interaction with a density-functional correction: A spin-complete method for exploring excited-state potential energy surfaces

    SciTech Connect

    Zhang, Xing; Herbert, John M.

    2015-12-21

    We revisit the formalism of the spin-adapted, spin-flip (SA-SF) configuration-interaction singles (CIS) method based on a tensor equation-of-motion formalism that affords proper spin eigenstates without sacrificing single-reference simplicity. Matrix elements for SA-SF-CIS are then modified in a manner similar to collinear spin-flip time-dependent density functional theory (SF-TDDFT), to include a DFT exchange-correlation correction. The performance of this method, which we call SA-SF-DFT, is evaluated numerically and we find that it systematically improves the energies of electronic states that exhibit significant spin contamination within the conventional SF-TDDFT approach. The new method cures the state assignment problem that plagues geometry optimizations and ab initio molecular dynamics simulations using traditional SF-TDDFT, without sacrificing computational efficiency, and furthermore provides correct topology at conical intersections, including those that involve the ground state, unlike conventional TDDFT. As such, SA-SF-DFT appears to be a promising method for generating excited-state potential energy surfaces at DFT cost.

  16. Determination of X-ray excitation spectra in micro X-ray fluorescence spectrometry with capillary optics

    NASA Astrophysics Data System (ADS)

    Perez, R. D.; Sosa, C.; Sbarato, V.; Leani, J.; Sánchez, H. J.

    2016-03-01

    The quantitative X-ray fluorescence microanalysis by fundamental parameters requires the knowledge of the energy distribution of the excitation beam. When this beam is produced by capillary optics, its high intensity and anisotropy complicate a direct determination. An alternative is an indirect determination based on measurement of induced X-ray fluorescence in a set of targets. In this work the X-ray excitation spectrum is determined by an iterative deconvolution process of the fundamental parameter expression for the X-ray fluorescence intensities. The method has the advantage that it does not require any assumption about the energy distribution of the X-ray source or the energy dependence of the lens transmission. Numerous XRF targets of pure elements with emission lines covering the full energy range of the X-ray source are employed. The only requirement on the targets is a high homogeneity in its composition. In fact, it does not impose any condition on the sample thickness. The accuracy observed in the validation process implemented with reference materials is similar to that reported with alternative approaches: 5% for main components, 10% for minor elements and 15% for trace elements.

  17. One-Dimensional Fluorescent Silicon Nanorods Featuring Ultrahigh Photostability, Favorable Biocompatibility, and Excitation Wavelength-Dependent Emission Spectra.

    PubMed

    Song, Bin; Zhong, Yiling; Wu, Sicong; Chu, Binbin; Su, Yuanyuan; He, Yao

    2016-04-13

    We herein report a kind of one-dimensional biocompatible fluorescent silicon nanorods (SiNRs) with tunable lengths ranging ∼100-250 nm, which can be facilely prepared through one-pot microwave synthesis. In addition to the strong fluorescence (quantum yield value: ∼15%) and negligible toxicity, the resultant SiNRs exhibit excitation wavelength-dependent photoluminescence whose maximum emission wavelength ranges from ∼450 to ∼600 nm under serial excitation wavelengths from 390 to 560 nm, providing feasibility for multicolor biological imaging. More significantly, the SiNRs are ultrahighly photostable, preserving strong and nearly unchanged fluorescence under 400 min high-power UV irradiation, which is in sharp contrast to severe fluorescence quenching of organic dyes (e.g., FITC) or II-VI quantum dots (QDs) (e.g., CdTe QDs and CdSe/ZnS QDs) within 15 or 160 min UV treatment under the same experiment conditions, respectively. Taking advantage of these attractive merits, we further exploit the SiNRs as a novel type of color converters for the construction of white light-emitting diodes (LED), which is the first proof-of-concept demonstration of LED device fabricated using the one-dimensional fluorescent silicon nanostructures. PMID:27010956

  18. Fluorescence-excitation and emission spectra from LH2 antenna complexes of Rhodopseudomonas acidophila as a function of the sample preparation conditions.

    PubMed

    Kunz, Ralf; Timpmann, Kõu; Southall, June; Cogdell, Richard J; Köhler, Jürgen; Freiberg, Arvi

    2013-10-10

    The high sensitivity of optical spectra of pigment-protein complexes to temperature and pressure is well known. In the present study, we have demonstrated the significant influence of the environments commonly used in bulk and single-molecule spectroscopic studies at low temperatures on the LH2 photosynthetic antenna complex from Rhodopseudomonas acidophila. A transfer of this LH2 complex from a bulk-buffer solution into a spin-coated polymer film results in a 189 cm(-1) blue shift of the B850 excitonic absorption band at 5 K. Within the molecular exciton model, the origin of this shift could be disentangled into three parts, namely to an increase of the local site energies, a contraction of the exciton band, and a decrease of the displacement energy.

  19. Excited light meson spectroscopy from lattice QCD

    SciTech Connect

    Christopher Thomas, Hadron Spectrum Collaboration

    2012-04-01

    I report on recent progress in calculating excited meson spectra using lattice QCD, emphasizing results and phenomenology. With novel techniques we can now extract extensive spectra of excited mesons with high statistical precision, including spin-four states and those with exotic quantum numbers. As well as isovector meson spectra, I will present new calculations of the spectrum of excited light isoscalar mesons, something that has up to now been a challenge for lattice QCD. I show determinations of the flavor content of these mesons, including the eta-eta' mixing angle, providing a window on annihilation dynamics in QCD. I will also discuss recent work on using lattice QCD to map out the energy-dependent phase shift in pi-pi scattering and future applications of the methodology to the study of resonances and decays.

  20. Using nitroxide spin labels. How to obtain T1e from continuous wave electron paramagnetic resonance spectra at all rotational rates.

    PubMed Central

    Haas, D A; Mailer, C; Robinson, B H

    1993-01-01

    Historically, the continuous wave electron paramagnetic resonance (CW-EPR) progressive saturation method has been used to obtain information on the spin-lattice relaxation time (T1e) and those processes, such as motion and spin exchange, that occur on a competitive timescale. For example, qualitative information on local dynamics and solvent accessibility of proteins and nucleic acids has been obtained by this method. However, making quantitative estimates of T1e from CW-EPR spectra have been frustrated by a lack of understanding of the role of T1e (and T2e) in the slow-motion regime. Theoretical simulation of the CW-EPR lineshapes in the slow-motion region under increasing power levels has been used in this work to test whether the saturation technique can produce quantitative estimates of the spin-lattice relaxation rates. A method is presented by which the correct T1e may be extracted from an analysis of the power-saturation rollover curve, regardless of the amount of inhomogeneous broadening or the rates of molecular reorientation. The range of motional correlation times from 10 to 200 ns should be optimal for extracting quantitative estimates of T1e values in spin-labeled biomolecules. The progressive-saturation rollover curve method should find wide application in those areas of biophysics where information on molecular interactions and solvent exposure as well as molecular reorientation rates are desired. PMID:8386009

  1. Frequency-Selective Heteronuclear Dephasing and Selective Carbonyl Labeling to Deconvolute Crowded Spectra of Membrane Proteins By Magic Angle Spinning NMR

    PubMed Central

    Traaseth, Nathaniel J.; Veglia, Gianluigi

    2011-01-01

    We present a new method that combines carbonyl-selective labeling with frequency-selective heteronuclear recoupling to resolve the spectral overlap of magic angle spinning (MAS) NMR spectra of membrane proteins in fluid lipid membranes with broad lines and high redundancy in the primary sequence. We implemented this approach in both heteronuclear 15N-13Cα and homonuclear 13C-13C dipolar assisted rotational resonance (DARR) correlation experiments. We demonstrate its efficacy for the membrane protein phospholamban reconstituted in fluid PC/PE/PA lipid bilayers. The main advantage of this method is to discriminate overlapped 13Cα resonances by strategically labeling the preceding residue. This method is highly complementary to 13C′i-1-15Ni-13Cαi and 13Cαi-1-15Ni-1-13C′i experiments to discriminate inter-residue spin systems at a minimal cost to signal-to-noise. PMID:21482162

  2. A Comparison of NMR Spectra Obtained for Solid-Phase-Synthesis Resins Using Conventional High-Resolution, Magic-Angle-Spinning, and High-Resolution Magic-Angle-Spinning Probes

    NASA Astrophysics Data System (ADS)

    Keifer, Paul A.; Baltusis, Laima; Rice, David M.; Tymiak, Adrienne A.; Shoolery, James N.

    It has recently been shown that high-resolution 1H NMR spectra can be obtained for samples covalently bound to polystyrene-based (Tentagel) solid-phase-synthesis resins by the use of magic-angle spinning (MAS) combined with high-resolution-probe technology. The attainable spectral resolution in the 1H and 13C NMR spectra of these resins is affected by molecular mobility and magnetic-susceptibility mismatches, both within the sample and in the probe itself. Using new high-resolution MAS probes called Nano·nmr probes, the importance of magnetic-susceptibility matching in the construction of these probes is demonstrated, and the limitations of using MAS alone to generate line narrowing in both 1H and 13C NMR are explored using a solvent-swollen functionalized Wang resin. The effects of presaturation, temperature, spin rate, and different solvents upon spectral quality have also been investigated, and advanced 1D- and 2D-experimental capability is demonstrated. This ability to generate high-resolution NMR spectra of samples still bound to the resins is expected to be of extreme interest in not only solid-phase synthesis, but also in the rapidly growing field of combinatorial chemistry.

  3. Electronic spectra and excited state dynamics of pentafluorophenol: Effects of low-lying πσ{sup ∗} states

    SciTech Connect

    Karmakar, Shreetama; Mukhopadhyay, Deb Pratim; Chakraborty, Tapas

    2015-05-14

    Multiple fluorine atom substitution effect on photophysics of an aromatic chromophore has been investigated using phenol as the reference system. It has been noticed that the discrete vibronic structure of the S{sub 1}←S{sub 0} absorption system of phenol vapor is completely washed out for pentafluorophenol (PFP), and the latter also shows very large Stokes shift in the fluorescence spectrum. For excitations beyond S{sub 1} origin, the emission yield of PFP is reduced sharply with increase in excess vibronic energy. However, in a collisional environment like liquid hydrocarbon, the underlying dynamical process that drives the non-radiative decay is hindered drastically. Electronic structure theory predicts a number of low-lying dark electronic states of πσ{sup ∗} character in the vicinity of the lowest valence ππ{sup ∗} state of this molecule. Tentatively, we have attributed the excitation energy dependent non-radiative decay of the molecule observed only in the gas phase to an interplay between the lowest ππ{sup ∗} and a nearby dissociative πσ{sup ∗} state. Measurements in different liquids reveal that some of the dark excited states light up with appreciable intensity only in protic liquids like methanol and water due to hydrogen bonding between solute and solvents. Electronic structure theory methods indeed predict that for PFP-(H{sub 2}O){sub n} clusters (n = 1-11), intensities of a number of πσ{sup ∗} states are enhanced with increase in cluster size. In contrast with emitting behavior of the molecule in the gas phase and solutions of nonpolar and polar aprotic liquids, the fluorescence is completely switched off in polar protic liquids. This behavior is a chemically significant manifestation of perfluoro effect, because a very opposite effect occurs in the case of unsubstituted phenol for which fluorescence yield undergoes a very large enhancement in protic liquids. Several dynamical mechanisms have been suggested to interpret the

  4. Highly excited and exotic meson spectroscopy from lattice QCD

    SciTech Connect

    Christopher Thomas

    2011-05-01

    I will discuss recent progress in extracting highly excited and exotic meson spectra using lattice QCD. New results in the light meson sector will be presented, where a combination of techniques have enabled us to confidently identify the spin of extracted states. Highlights include many states with exotic quantum numbers and, for the first time in a lattice QCD calculation, spin-four states. I will conclude with comments on future prospects.

  5. Nucleon, {Delta}, and {Omega} excited state spectra in N{sub f}=2+1 lattice QCD

    SciTech Connect

    Bulava, J.; Edwards, R. G.; Joo, B.; Richards, D. G.; Engelson, E.; Wallace, S. J.; Lin, H-W.; Morningstar, C.

    2010-07-01

    The energies of the excited states of the nucleon, {Delta}, and {Omega} are computed in lattice QCD, using two light quarks and one strange quark on anisotropic lattices. The calculation is performed at three values of the light quark mass, corresponding to pion masses m{sub {pi}=}392(4), 438(3), and 521(3) MeV. We employ the variational method with a large basis of interpolating operators enabling six energies in each irreducible representation of the lattice to be distinguished clearly. We compare our calculation with the low-lying experimental spectrum, with which we find reasonable agreement in the pattern of states. The need to include operators that couple to the expected multihadron states in the spectrum is clearly identified.

  6. Photoabsorption and fluorescence excitation spectra of CF 3CN in the region of 6-41 eV

    NASA Astrophysics Data System (ADS)

    Ibuki, Toshio; Okada, Kazumasa

    1996-12-01

    Photoabsorption and fluorescence cross sections of CF 3CN have been measured in the region of 6-41 eV by using synchrotron radiation. The bands observed have been assigned as the Rydberg transitions of the lone pair electrons on N and F atoms. It has been found that the CN and CF stretching and FCF bending frequencies are excited in the Rydberg states. Emissions from the CN(A 2IIIi, B 2Σ+ → X 2Σ+) transitions have been observed even in the ionization region, and increased at ≈ 22 eV by the ionization of the (2e) -1 and (4a 1) -1 valence electrons.

  7. The spin chemistry and magnetic resonance of H2@C60. From the Pauli principle to trapping a long lived nuclear excited spin state inside a buckyball.

    PubMed

    Turro, Nicholas J; Chen, Judy Y-C; Sartori, Elena; Ruzzi, Marco; Marti, Angel; Lawler, Ronald; Jockusch, Steffen; López-Gejo, Juan; Komatsu, Koichi; Murata, Yasujiro

    2010-02-16

    One of the early triumphs of quantum mechanics was Heisenberg's prediction, based on the Pauli principle and wave function symmetry arguments, that the simplest molecule, H(2), should exist as two distinct species-allotropes of elemental hydrogen. One allotrope, termed para-H(2) (pH(2)), was predicted to be a lower energy species that could be visualized as rotating like a sphere and possessing antiparallel ( upward arrow downward arrow) nuclear spins; the other allotrope, termed ortho-H(2) (oH(2)), was predicted to be a higher energy state that could be visualized as rotating like a cartwheel and possessing parallel ( upward arrow upward arrow) nuclear spins. This remarkable prediction was confirmed by the early 1930s, and pH(2) and oH(2) were not only separated and characterized but were also found to be stable almost indefinitely in the absence of paramagnetic "spin catalysts", such as molecular oxygen, or traces of paramagnetic impurities, such as metal ions. The two allotropes of elemental hydrogen, pH(2) and oH(2), may be quantitatively incarcerated in C(60) to form endofullerene guest@host complexes, symbolized as pH(2)@C(60) and oH(2)@C(60), respectively. How does the subtle difference in nuclear spin manifest itself when hydrogen allotropes are incarcerated in a buckyball? Can the incarcerated "guests" communicate with the outside world and vice versa? Can a paramagnetic spin catalyst in the outside world cause the interconversion of the allotropes and thereby effect a chemical transformation inside a buckyball? How close are the measurable properties of H(2)@C(60) to those computed for the "quantum particle in a spherical box"? Are there any potential practical applications of this fascinating marriage of the simplest molecule, H(2), with one of the most beautiful of all molecules, C(60)? How can one address such questions theoretically and experimentally? A goal of our studies is to produce an understanding of how the H(2) guest molecules incarcerated in

  8. Insight into the light-induced spin crossover of [Fe(bpy)3](2+) in aqueous solution from molecular dynamics simulation of d-d excited states.

    PubMed

    Iuchi, Satoru; Koga, Nobuaki

    2016-02-14

    Molecular dynamics (MD) simulations are performed for d-d excited states of the aqueous [Fe(bpy)3](2+) system using a previously developed model Hamiltonian. Specifically, the characters of d-d excited states and of transitions among these states are explored to gain clues about electronic relaxation during the photo-excited metal-to-ligand charge transfer (MLCT) to the lowest quintet d-d states. By evaluating the spin-orbit couplings in various nuclear configurations through MD simulations, strong mixing among low-lying d-d states with different spin multiplicities is found not to be expected in most of the sampled nuclear configurations except for surface crossing regions. The lifetimes of triplet d-d states are evaluated by Fermi's golden rule using equilibrium MD simulations. The internal conversion from upper-lying triplet to lower-lying triplet states is estimated to occur with a lifetime of order 100 fs accompanied by the distortion of the [Fe(bpy)3](2+) complex structure. This result is consistent with the discussion in another computational study, which evaluated the intersystem crossing rates by Fermi's golden rule using electronic structure calculations. In contrast, the present MD simulations cannot provide a clear picture of intersystem crossings from the lowest triplet d-d state after the above-mentioned internal conversion. Based on this result, possible relaxation mechanisms are discussed. PMID:26806402

  9. Experimental confirmation of photon-induced spin-flip transitions in helium via triplet metastable yield spectra

    SciTech Connect

    Rubensson, Jan-Erik; Moise, Angelica; Richter, Robert; Mihelic, Andrej; Bucar, Klemen; Zitnik, Matjaz

    2010-06-15

    Doubly excited states below the N=2 ionization threshold are populated by exciting helium atoms in a supersonic beam with monochromatized synchrotron radiation. The fluorescence decay of these states triggers a radiative cascade back to the ground state with large probability to populate long lived singlet and triplet helium metastable states. The yield of metastables is measured using a multichannel plate detector after the beam has passed a singlet-quenching discharge lamp. The variation of the yield observed with the lamp switched on or off is related to the triplet-singlet mixing of the doubly excited states.

  10. Excited metastables electronic spin states in spin crossover compounds studies by atom-phonon coupling model: Gradual and two-step transition cases

    NASA Astrophysics Data System (ADS)

    Gindulescu, A.; Rotaru, A.; Linares, J.; Dimian, M.; Nasser, J.

    2010-05-01

    This contribution reports the study of metastable spin states in spin-crossover materials in the framework of the atom-phonon coupling model. Using this model for a linear chain we show theoretically for the first time that, even if the cooperativity is not strong enough to obtain hysteresis at high temperatures, metastable states exist at low temperatures for a high spin (HS) fraction of nHS=1. This gradual thermal transition featuring metastable states at low temperature has been observed experimentally by [Létard et al., J. Phys.: Conf. Ser. 21, 23 (2005)]. Moreover, for compounds showing a two-step thermal transition, we show that metastable states, corresponding to a HS fraction nHS=0.5, are present. This metastable states appear up to 50 K, fact that was observed by [Moussa et al., Phys. Rev. Lett. 94, 107205 (2005)] and [Matsumoto et al., J. Phys.: Conf. Ser. 148, 012029 (2009)].

  11. Scaling and labeling the high-resolution isotropic axis of two-dimensional multiple-quantum magic-angle-spinning spectra of half-integer quadrupole spins

    NASA Astrophysics Data System (ADS)

    Man, Pascal P.

    1998-08-01

    The dynamics of half-integer quadrupole spins (I=32, 52, 72, and 92) during the multiple-quantum (MQ) magic-angle spinning experiment with the two-pulse sequence, a recent NMR method, is analyzed in order to scale in frequency unit and label in ppm (the chemical shift unit) the high-resolution isotropic axis of a two-dimensional (2D) spectrum. Knowledge of the two observed chemical shifts (δ(obs)G1 and δ(obs)G2) of the center of gravity of an MQ-filtered central-transition peak in the two dimensions allows us to determine the true isotropic chemical shift of an absorption line, which is related to the mean bond angle in a compound. Only the isotropic chemical shift and the second-order quadrupole interaction for a sample rotating at the magic angle at a high spinning rate are considered during the free precession of the spin system. On the other hand, only the first-order quadrupole interaction for a static sample is considered during the pulses. The hypercomplex detection method is used to obtain a pure 2D absorption spectrum. The pulse program and the successive stages of data processing are described. For simplicity, only the density matrix for a spin I=32 at the end of the first pulse of phase φ is calculated in detail, which allows us to deduce the phase cycling of the pulse sequence that selectively detects the +/-3-quantum coherences generated by the first pulse. The positions of the echo and antiecho relative to the second pulse, and that of the MQ-filtered central-transition peak relative to the carrier frequency (ω0) along the F1 dimension are derived for the four half-integer quadrupole spins. The frequency offset of ω0 relative to an external aqueous solution in the F1 dimension is linearly related to that in the F2 dimension. The shearing transformation, whose main interest is to shift the beginning of the acquisition period from the end of the second pulse to the echo position and to yield a high-resolution spectrum along the F1 dimension, is

  12. The influence of visible light and inorganic pigments on fluorescence excitation emission spectra of egg-, casein- and collagen-based painting media

    NASA Astrophysics Data System (ADS)

    Nevin, A.; Anglos, D.; Cather, S.; Burnstock, A.

    2008-07-01

    Spectrofluorimetric analysis of proteinaceous binding media is particularly promising because proteins employed in paintings are often fluorescent and media from different sources have significantly different fluorescence spectral profiles. Protein-based binding media derived from eggs, milk and animal tissue have been used for painting and for conservation, but their analysis using non-destructive techniques is complicated by interferences with pigments, their degradation and their low concentration. Changes in the fluorescence excitation emission spectra of films of binding media following artificial ageing to an equivalent of 50 and 100 years of museum lighting include the reduction of bands ascribed to tyrosine, tryptophan and Maillard reaction products and an increase in fluorescent photodegradation. Fluorescence of naturally aged paint is dependent on the nature of the pigment present and, with egg-based media, in comparison with un-pigmented films, emissions ascribed to amino acids are more pronounced.

  13. Coexistence of Haldane-gap excitations and long-range antiferromagnetic order in mixed-spin nickelates R{sub 2}BaNiO{sub 5}

    SciTech Connect

    Maslov, S.; Zheludev, A.

    1998-01-01

    The spin dynamics of the S=1 Ni chains in mixed-spin antiferromagnets Pr{sub 2}BaNiO{sub 5} and Nd{sub x}Y{sub 2{minus}x}BaNiO{sub 5} is described in terms of a simple Ginzburg-Landau Lagrangian coupled to the sublattice of rare-earth ions. Within this framework we obtain a theoretical explanation for the experimentally observed coexistence of Haldane-gap excitations and long-range magnetic order, as well as for the increase of the Haldane-gap energy below the N{acute e}el point. We also predict that the degeneracy of the Haldane triplet is lifted in the magnetically ordered phase. The growth of both gaps are shown to follow from the magnon repulsion. The theoretical results are consistent with the available experimental data. {copyright} {ital 1998} {ital The American Physical Society}

  14. Oxygen-assisted excitation of methyl iodide as a test of double spin-flip transition in van der Waals complex CH3I-O2

    NASA Astrophysics Data System (ADS)

    Bogomolov, Alexandr S.; Kochubei, Sergei A.; Baklanov, Alexey V.

    2016-09-01

    Photoexcitation of van der Waals (vdW) complex CH3I-O2 has been studied with velocity map imaging of I atoms arising in photodissociation. A new scheme of resonance-enhanced multiphoton ionization of iodine atoms has been applied with simultaneous use of UV and VIS radiation. The measured kinetic energy of I(2P3/2) atoms indicates photogeneration of precursor CH3I molecules via complex-specific channel with excitation energy expected for double spin-flip transition in complex CH3I-O2. The angular distribution for recoil directions of I(2P3/2) atoms coming from vdW complexes also corresponds to that expected for double spin-flip transition.

  15. Ab initio calculations of the ground and excited states of the ZrN molecule including spin-orbit effects.

    PubMed

    Farhat, Ayman; Abdul-Al, Saleh N

    2015-06-15

    The electronic structures with spin-orbit effects of the zirconium nitride ZrN molecule are investigated by the methods of multireference single and double configuration interaction. The potential energy curves are calculated along with the spectroscopic constants for the lowest-lying 34 spin-orbit states Ω in ZrN. A good agreement is displayed by comparing the calculated spectroscopic constants with those available experimentally. The permanent dipole moments are calculated along with the vibrational energies. New results are obtained in this work for 29 spin-orbit states and their spectroscopic constants calculated. PMID:25899865

  16. Hydride stretch infrared spectra in the excited electronic states of indole and its derivatives: Direct evidence for the 1πσ* state

    NASA Astrophysics Data System (ADS)

    Dian, Brian C.; Longarte, Asier; Zwier, Timothy S.

    2003-02-01

    The hydride stretch infrared spectra of indole, indole-H2O, 3-methyl indole, 3-methyl indole-H2O, the main conformer of tryptamine (TRA), two conformers of N-acetyl tryptophan amide (NATA), and three conformers of N-acetyl tryptophan methyl amide (NATMA), have been recorded in the electronically excited singlet states using excited-state fluorescence-dip infrared spectroscopy. NATA and NATMA are methyl-capped dipeptides of tryptophan that have conformational flexibility and exhibit sensitivity in their electronic spectra to the conformation of the dipeptide backbone. In the indole monomer, the indole NH stretch fundamental at the S1 origin is shifted from its ground-state value (3525 cm-1) to 3478 cm-1. The corresponding band in the indole-H2O complex appears at 3387 cm-1, shifted by a similar amount from its ground-state position (3436 cm-1). Higher vibronic levels within 1500 cm-1 of the S1 origin, which have been identified previously [B. J. Fender et al., Chem. Phys. Lett. 239, 31 (1995)] as being 1Lb or 1La in character, all show similar excited state indole NH stretch absorptions. The corresponding spectra in 3-methyl indole, 3-methyl indole-H2O, TRA, and in the C5 conformers of NATA and NATMA all are missing the indole NH stretch absorption. In its place, a broad background absorption appears, spread over the entire 2800-3800 cm-1 region. In these molecules, other CH stretch or amide NH stretch absorptions remain sharp, appearing in their expected frequency ranges. Finally, the C7 conformations of NATA and NATMA, which possess an intramolecular hydrogen bond in the dipeptide backbone, have all infrared transitions washed out, replaced by a stronger broad background absorption. The entire data set can be explained by the presence of an excited 1πσ* state which is dissociative along the indole NH stretch coordinate, as recently predicted by Sobolewski and Domcke [Chem. Phys. Lett. 315, 293 (1999)]. In the weak coupling case (indole, indole-H2O), the gap

  17. Seasonal and spatial constraints of fluorophores in the midwestern Bay of Bengal by PARAFAC analysis of excitation emission matrix spectra

    NASA Astrophysics Data System (ADS)

    Chari, N. V. H. K.; Sarma, Nittala S.; Pandi, Sudarsana Rao; Murthy, K. Narasimha

    2012-03-01

    Dissolved organic matter (DOM) fluorescence was measured along with hydrochemical constituents and chlorophyll a of water collected monthly from the midwestern Bay of Bengal (Indian Ocean) that included the Godavari estuary and its adjoining coastal region during the period March-October 2009. By applying parallel factor (PARAFAC) modelling of the excitation emission matrix spectral data, five components - three humic (A, C, and M peaks) and two protein (B and T) were noticed. The tyrosine like component (B) is the most abundant throughout except for the estuary during monsoon when the UV humic like component (A) surpassed it. During the pre-monsoon season, the B, C and M fluorophores are enriched due to a higher bacterial decay of organic matter. The fluorescence index (FI) was higher and the humification index (HIX) lower during pre-monsoon. Similarly, the FI was higher and HIX lower for the coastal region than the estuary. The A:C ratio and A:M ratio are essentially seasonal indicators - they were <1 in the pre-monsoon and >5 during monsoon. The M:C ratio is essentially a spatial indicator, being <1 in the estuary and >1 in the coastal region during both seasons.

  18. Pigment-pigment interactions in thylakoids and LHCII of chlorophyll a/ c containing alga Pleurochloris meiringensis: analysis of fluorescence-excitation and triplet-minus-singlet spectra

    NASA Astrophysics Data System (ADS)

    Büchel, C.; Razi Naqvi, K.; Melø, T. B.

    1998-05-01

    Time-resolved triplet-minus-singlet (TmS) difference spectra, Δ A( λ; t), fluorescence excitation spectra, X( λ), and absorption spectra, A( λ), are used for probing pigment-pigment interactions in the thylakoids (Chl a/ c-Thyl) and isolated light-harvesting complexes associated with photosystem II (Chl a/ c-LHCII) of the alga Pleurochloris meiringensis, whose chromophores comprise chlorophyll a (Chl a), chlorophyll c (Chl c), and several carotenoids. The data provide information about interactions between Car*-and-Chl a0, Chl a†-and-Car 0, Car †-and-Chl a0 (where the abbreviation Car stands for carotenoid, an asterisk and a dagger denote singlet and triplet excitation, respectively, and the superscript 0 denotes a molecule in the ground state). In Chl a/c-Thyl, the efficiency of Car*→Chl a* transfer ( φLH), determined by comparing A( λ) and X( λ), is slightly less than unity (ca. 0.85), whereas the efficiency of Chl a†→Car † transfer of triplet energy ( φTT) must be much closer to unity, since no long-lived Chl a† could be detected; an interaction between Car † and Chl a0, already familiar from investigations concerning the TmS spectra of the trimers and aggregates of Chl a/ b-LHCII (the light-harvesting complex associated with the photosystem II of higher plants), which manifests itself through a depletion signal (in the Qy region of Chl a) decaying at the same rate as the Car TmS signal, is observed, and explained likewise. In Chl a/ c-LHCII, both efficiencies are found to be much lower; the drastic reduction in the two yields is attributed to the perturbation of the native molecular architecture of the complex by the detergent used in the isolation procedure. The overall TmS signal from Chl a/ c-LHCII can be decomposed into two contributions, Δ A( λ; t)=Δ 1A( λ; t)+Δ 2A( λ; t), where Δ 1A( λ; t) with a lifetime of about 8 μs; Δ 2A( λ; t), which persists for several hundred microseconds, is contributed by those Chl a

  19. Increasing spin-flips and decreasing cost: Perturbative corrections for external singles to the complete active space spin flip model for low-lying excited states and strong correlation

    SciTech Connect

    Mayhall, Nicholas J.; Head-Gordon, Martin

    2014-07-28

    An approximation to the spin-flip extended configuration interaction singles method is developed using a second-order perturbation theory approach. In addition to providing significant efficiency advantages, the new framework is general for an arbitrary number of spin-flips, with the current implementation being applicable for up to around 4 spin-flips. Two new methods are introduced: one which is developed using non-degenerate perturbation theory, spin-flip complete active-space (SF-CAS(S)), and a second quasidegenerate perturbation theory method, SF-CAS(S){sub 1}. These two approaches take the SF-CAS wavefunction as the reference, and then perturbatively includes the effect of single excitations. For the quasidegenerate perturbation theory method, SF-CAS(S){sub 1}, the subscripted “1” in the acronym indicates that a truncated denominator expansion is used to obtain an energy-independent down-folded Hamiltonian. We also show how this can alternatively be formulated in terms of an extended Lagrangian, by introducing an orthonormality constraint on the first-order wavefunction. Several numerical examples are provided, which demonstrate the ability of SF-CAS(S) and SF-CAS(S){sub 1} to describe bond dissociations, singlet-triplet gaps of organic molecules, and exchange coupling parameters for binuclear transition metal complexes.

  20. Application of the multireference equation of motion coupled cluster method, including spin-orbit coupling, to the atomic spectra of Cr, Mn, Fe and Co

    NASA Astrophysics Data System (ADS)

    Liu, Zhebing; Huntington, Lee M. J.; Nooijen, Marcel

    2015-10-01

    The recently introduced multireference equation of motion (MR-EOM) approach is combined with a simple treatment of spin-orbit coupling, as implemented in the ORCA program. The resulting multireference equation of motion spin-orbit coupling (MR-EOM-SOC) approach is applied to the first-row transition metal atoms Cr, Mn, Fe and Co, for which experimental data are readily available. Using the MR-EOM-SOC approach, the splittings in each L-S multiplet can be accurately assessed (root mean square (RMS) errors of about 70 cm-1). The RMS errors for J-specific excitation energies range from 414 to 783 cm-1 and are comparable to previously reported J-averaged MR-EOM results using the ACESII program. The MR-EOM approach is highly efficient. A typical MR-EOM calculation of a full spin-orbit spectrum takes about 2 CPU hours on a single processor of a 12-core node, consisting of Intel XEON 2.93 GHz CPUs with 12.3 MB of shared cache memory.

  1. Simulating One-Photon Absorption and Resonance Raman Scattering Spectra Using Analytical Excited State Energy Gradients within Time-Dependent Density Functional Theory

    SciTech Connect

    Silverstein, Daniel W.; Govind, Niranjan; van Dam, Hubertus J. J.; Jensen, Lasse

    2013-12-10

    A parallel implementation of analytical time-dependent density functional theory gradients is presented for the quantum chemistry program NWChem. The implementation is based on the Lagrangian approach developed by Furche and Ahlrichs. To validate our implementation, we first calculate the Stokes shifts for a range of organic dye molecules using a diverse set of exchange-correlation functionals (traditional density functionals, global hybrids, and range-separated hybrids) followed by simulations of the one-photon absorption and resonance Raman scattering spectrum of the phenoxyl radical, the well-studied dye molecule rhodamine 6G, and a molecular host–guest complex (TTFcCBPQT4+). The study of organic dye molecules illustrates that B3LYP and CAM-B3LYP generally give the best agreement with experimentally determined Stokes shifts unless the excited state is a charge transfer state. Absorption, resonance Raman, and fluorescence simulations for the phenoxyl radical indicate that explicit solvation may be required for accurate characterization. For the host–guest complex and rhodamine 6G, it is demonstrated that absorption spectra can be simulated in good agreement with experimental data for most exchange-correlation functionals. Finally, however, because one-photon absorption spectra generally lack well-resolved vibrational features, resonance Raman simulations are necessary to evaluate the accuracy of the exchange-correlation functional for describing a potential energy surface.

  2. Magnetic excitations and spin-gap phenomenon in the BCS-BEC crossover regime of an ultracold Fermi gas

    NASA Astrophysics Data System (ADS)

    Tajima, Hiroyuki; Kashimura, Takashi; Hanai, Ryo; Watanabe, Ryota; Ohashi, Yoji

    2014-03-01

    We investigate the uniform spin susceptibility χ and strong-coupling corrections in the BCS-BEC crossover regime of an ultracold Fermi gas. Within the framework of an extended T-matrix theory,[2] we show that χ exhibits non-monotonic temperature dependence in the normal state, and is suppressed near the superfluid phase transition temperature Tc. This spin-gap phenomenon is found to be deeply related to the pseudogap phenomenon appearing in the single-particle density of states. To characterize this magnetic phenomenon, we introduce the spin-gap temperature Ts as the temperature at which χ takes a maximum value. Determining Ts in the entire BCS-BEC crossover region, we identify the spin-gap regime in the phase diagram of a Fermi gas with respect to the temperature and the strength of a pairing interaction. Since the spin-gap is crucial key phenomenon in high-Tc cuprates, our results would be useful for the study of this many-body phenomenon using ultracold Fermi gases, as well as in observing the pseudogap phenomenon through the spin-gap phenomenon. H. T. was supported by the Research Grant of Keio Leading-edge Laboratory of Science & Technology.

  3. The effects of general anesthetics on ESR spectra of spin labels in phosphatidylcholine vesicles containing purified Na,K-ATPase or microsomal protein

    NASA Astrophysics Data System (ADS)

    Shibuya, Makiko; Hiraoki, Toshifumi; Kimura, Kunie; Fukushima, Kazuaki; Suzuki, Kuniaki

    2012-12-01

    We investigated the effects of general anesthetics on liposome containing spin labels, 5-doxyl stearic acid (5-DSA) and 16-doxyl stearic acid (16-DSA), and purified Na,K-ATPase or membrane protein of microsome using an electron spin resonance (ESR) spectroscopy. The spectra of 16-DSA in liposomes with both proteins showed three sharp signals compared with 5-DSA. The difference in the order parameter S value of 5-DSA and 16-DSA suggested that the nitroxide radical location of 5-DSA and 16-DSA were different in the membrane bilayer. The results were almost the same as those obtained in liposomes without proteins. The addition of sevoflurane, isoflurane, halothane, ether, ethanol and propofol increased the intensity of the signals, but the clinical concentrations of anesthetics did not significantly alter the S and τ values, which are indices of the fluidity of the membrane. These results suggest that anesthetics remain on the surface of the lipid bilayer and do not act on both the inside hydrophobic area and the relatively hydrophilic area near the surface. These results and others also suggest that the existence of Na,K-ATPase and microsomal proteins did not affect the environment around the spin labels in the liposome and the effects of anesthetics on liposome as a model membrane.

  4. Low-spin states of /sup 250/Cf populated in the electron capture decay of 2. 22-h /sup 250/Es. [ULTIPOLE TRANSITIONS; PARITY; ROTATIONAL STATES; SPIN; VIBRATIONAL STATES; GAMMA SPECTRA

    SciTech Connect

    Ahmad, I.; Sjoblom, R.K.

    1980-09-01

    Low-spin states of /sup 250/Cf have been investigated by measuring ..gamma.. rays and conversion electrons associated with the electron capture decay of 2.22-h /sup 250/Es. Mass-separated /sup 250/Es samples produced by the /sup 249/Cf(d,n) reaction were used for these measurements. The ..gamma..-ray spectra were measured with a 25-cm/sup 3/ coaxial Ge(Li) spectrometer and the electron spectra were measured with a cooled Si(Li) detector. Multipolarities of intense transitions in /sup 250/Cf were deduced and logft values of electron capture transitions were derived from measured electron capture intensities. On the basis of the results of the present investigation the following bandheads were identified in /sup 250/Cf: E (keV),K,I..pi..=871.6, 2,2-; 1031.9, 2,2+; 1154.2, 0,0+; 1175.5, 1,1-; 1210.0, 2,2-; 1244.4, 2,2+; 1266.5, 0,0+; and 1658.1, 2,2+. The 2.22-h state in /sup 250/Es has been given a spin-parity assignment of 1- with configuration )n(734)9/2-; p(633)7/2+)/sub 1//sub -/.

  5. New high-spin level schemes and excitation modes of 117,118,119,120,122 Cd

    SciTech Connect

    J. D. Cole

    2012-01-01

    High-spin level schemes of {sup 117,118,119,120,122}Cd are expanded by analyzing our high-statistics triple and higher-fold coincidence events of prompt fission {gamma} rays from {sup 252}Cf at Gammasphere. Spin/parity assignments were made based on new {gamma}-{gamma} angular correlation measurements and level systematics in the neighboring isotopes. Stretch-aligned band structures observed in low-lying levels in {sup 117,119,121}Cd are seen to weaken with increasing spins, with a quasi-rotational degree of freedom manifested at higher spins. The{sup 5-}levels in even-N{sup 118,120}Cd were tentatively interpreted as candidates of quadrupole-octupole (QOC) coupling. The model-independent spin versus {h_bar}{omega} curves for even-N and odd-N Cd isotopes imply quasirotational alignment of an h11/2 neutron pair in the even-N Cd isotopes. The relative energies of the lowest 11/{sup 2-}, 9/{sup 2-}, 7/{sup 2-}, and 15/{sup 2-} levels in {sup 117}Cd and {sup 119}Cd suggest triaxial shapes based on Meyer-Ter-Vehn theory for these odd-N Cd nuclei. For the even-N Cd isotopes evidence of triaxiality may also be provided by the Shell Correction version of the Tilted Axis Cranking model (SCTAC).

  6. Probing Ground and Excited States of Phospholamban in Model and Native Lipid Membranes by Magic Angle Spinning NMR Spectroscopy

    PubMed Central

    Gustavsson, Martin; Traaseth, Nathaniel J.; Veglia, Gianluigi

    2013-01-01

    In this paper, we analyzed the ground and excited states of phospholamban (PLN), a membrane protein that regulates sarcoplasmic reticulum calcium ATPase (SERCA), in different membrane mimetic environments. Previously, we proposed that the conformational equilibria of PLN are central to SERCA regulation. Here, we show that these equilibria detected in micelles and bicelles are also present in native sarcoplasmic reticulum lipid membranes as probed by MAS solid-state NMR. Importantly, we found that the kinetics of conformational exchange and the extent of ground and excited states in detergent micelles and lipid bilayers are different, revealing a possible regulatory role of the membrane composition on the allosteric regulation of SERCA. Since the extent of excited states is directly correlated to SERCA inhibition, these findings open up the exciting possibility that calcium transport in the heart can be controlled by the lipid bilayer composition. PMID:21839724

  7. Spin-orbit coupling in the dissociative excitation of alkali atoms at the surface of rare gas clusters: A theoretical study

    NASA Astrophysics Data System (ADS)

    Gervais, B.; Zanuttini, D.; Douady, J.

    2016-05-01

    We analyze the role of the spin-orbit (SO) coupling in the dissociative dynamics of excited alkali atoms at the surface of small rare gas clusters. The electronic structure of the whole system is deduced from a one-electron model based on core polarization pseudo-potentials. It allows us to obtain in the same footing the energy, forces, and non-adiabatic couplings used to simulate the dynamics by means of a surface hopping method. The fine structure state population is analyzed by considering the relative magnitude of the SO coupling ξ, with respect to the spin-free potential energy. We identify three regimes of ξ-values leading to different evolution of adiabatic state population after excitation of the system in the uppermost state of the lowest np 2P shell. For sufficiently small ξ, the final population of the J = /1 2 atomic states, P /1 2 , grows up linearly from P /1 2 = /1 3 at ξ = 0 after a diabatic dynamics. For large values of ξ, we observe a rather adiabatic dynamics with P /1 2 decreasing as ξ increases. For intermediate values of ξ, the coupling is extremely efficient and a complete transfer of population is observed for the set of parameters associated to NaAr3 and NaAr4 clusters.

  8. A Novel Detection Scheme for High-Resolution Two-Dimensional Spin-Echo Correlated Spectra in Inhomogeneous Fields

    PubMed Central

    Huang, Yuqing; Zhang, Zhiyong; Cai, Shuhui; Chen, Zhong

    2014-01-01

    Background Two-dimensional (2D) nuclear magnetic resonance (NMR) spectroscopy is a powerful and non-invasive tool for the analysis of molecular structures, conformations, and dynamics. However, the inhomogeneity of magnetic fields experienced by samples will destroy spectral information and hinder spectral analysis. In this study, a new pulse sequence is proposed based on the modulation of distant dipolar field to recover high-resolution 2D spin-echo correlated spectroscopy (SECSY) from inhomogeneous fields. Method and Material By using the new sequence, the correlation information between coupled spins and the J coupled information with straightforward multiplet patterns can be obtained free from inhomogeneous line broadening. In addition, the new sequence is also suitable for non-J coupled spin systems. Although three-dimensional acquisition is needed, the evolution of indirect detection dimensions is carefully designed and the ultrafast acquisition scheme is utilized to improve the acquisition efficiency. A chemical solution of butyl methacrylate (C8H14O2) in DMSO (C2H6SO) in a deshimmed magnetic field was tested to demonstrate the implementation details of the new sequence. The performance of the new sequence relative to the conventional SECSY sequence was shown by using an aqueous solution of main brain metabolites in a deshimmed magnetic field. Conclusion The results reveal that the new sequence provides an attractive way to eliminate the inhomogeneous spectral line broadening for the spin-echo correlated spectrum and is a promising tool for the study of metabolites in metabonomics, even for the applications on in vivo and in situ high-resolution 2D NMR spectroscopy. PMID:24392105

  9. Visibility of lipid resonances in HR-MAS spectra of brain biopsies subject to spinning rate variation.

    PubMed

    Precht, C; Diserens, G; Oevermann, A; Vermathen, M; Lang, J; Boesch, C; Vermathen, P

    2015-12-01

    Lipid resonances from mobile lipids can be observed by ¹H NMR spectroscopy in multiple tissues and have also been associated with malignancy. In order to use lipid resonances as a marker for disease, a reference standard from a healthy tissue has to be established taking the influence of variable factors like the spinning rate into account. The purpose of our study was to investigate the effect of spinning rate variation on the HR-MAS pattern of lipid resonances in non-neoplastic brain biopsies from different regions and visualize polar and non-polar lipids by fluorescence microscopy using Nile Red staining. ¹H HR-MAS NMR spectroscopy demonstrated higher lipid peak intensities in normal sheep brain pure white matter biopsies compared to mixed white and gray matter biopsies and pure gray matter biopsies. High spinning rates increased the visibility particularly of the methyl resonances at 1.3 and the methylene resonance at 0.89 ppm in white matter biopsies stronger compared to thalamus and brainstem biopsies, and gray matter biopsies. The absence of lipid droplets and presence of a large number of myelin sheaths observed in white matter by Nile Red fluorescence microscopy suggest that the observed lipid resonances originate from the macromolecular pool of lipid protons of the myelin sheath's plasma membranes. When using lipid contents as a marker for disease, the variable behavior of lipid resonances in different neuroanatomical regions of the brain and at variable spinning rates should be considered. The findings may open up interesting possibilities for investigating lipids in myelin sheaths.

  10. Ultrafast Time-Resolved Emission and Absorption Spectra of meso-Pyridyl Porphyrins upon Soret Band Excitation Studied by Fluorescence Up-Conversion and Transient Absorption Spectroscopy.

    PubMed

    Venkatesh, Yeduru; Venkatesan, M; Ramakrishna, B; Bangal, Prakriti Ranjan

    2016-09-01

    thermally equilibrated Qx state by vibrational cooling/relaxations of excess energy within solvent. This relaxed Qx state decays to ground as well as triplet state by 7-8 ns time scale. The femtosecond transient absorption studies of TpyPs in three different excitations at S2 (400 nm), Qy (515 nm), and Qx (590 nm) along with extensive global and target model analysis of TA data exclusively generate the true spectra of each excited species/state with their respective lifetimes along with microscopic rate constants associated with each state. The following five exponential components with lifetime values of 65-70 fs, ∼0.3-0.5 ps, ∼20 ± 2 ps, ∼7 ± 1 ns, and 1-2 μs are observed which are associated with S2, Qy, hot Qx, thermally relaxed Qx, and lowest triplet (T1) states, respectively, when excited at S2, and four (Qy, hot Qx, thermally relaxed Qx, and lowest triplet (T1) states) and three (hot Qx, thermally relaxed Qx, and lowest triplet (T1) states) states are obtained when excited at 515 nm (Qy) and 590 nm (Qx), respectively, as expected. The TA results parallel the fluorescence up-conversion studies, and both the results not only compliment each other but also unveil the ultrafast internal conversion from S2 to Qy, S2 to Qx, and Qy to Qx for all three isomers in a similar fashion with nearly equal characteristic decay times.

  11. Ultrafast Time-Resolved Emission and Absorption Spectra of meso-Pyridyl Porphyrins upon Soret Band Excitation Studied by Fluorescence Up-Conversion and Transient Absorption Spectroscopy.

    PubMed

    Venkatesh, Yeduru; Venkatesan, M; Ramakrishna, B; Bangal, Prakriti Ranjan

    2016-09-01

    thermally equilibrated Qx state by vibrational cooling/relaxations of excess energy within solvent. This relaxed Qx state decays to ground as well as triplet state by 7-8 ns time scale. The femtosecond transient absorption studies of TpyPs in three different excitations at S2 (400 nm), Qy (515 nm), and Qx (590 nm) along with extensive global and target model analysis of TA data exclusively generate the true spectra of each excited species/state with their respective lifetimes along with microscopic rate constants associated with each state. The following five exponential components with lifetime values of 65-70 fs, ∼0.3-0.5 ps, ∼20 ± 2 ps, ∼7 ± 1 ns, and 1-2 μs are observed which are associated with S2, Qy, hot Qx, thermally relaxed Qx, and lowest triplet (T1) states, respectively, when excited at S2, and four (Qy, hot Qx, thermally relaxed Qx, and lowest triplet (T1) states) and three (hot Qx, thermally relaxed Qx, and lowest triplet (T1) states) states are obtained when excited at 515 nm (Qy) and 590 nm (Qx), respectively, as expected. The TA results parallel the fluorescence up-conversion studies, and both the results not only compliment each other but also unveil the ultrafast internal conversion from S2 to Qy, S2 to Qx, and Qy to Qx for all three isomers in a similar fashion with nearly equal characteristic decay times. PMID:27494567

  12. The Distribution of Interstellar Thermal Pressures in the Milky Way: New Data on the Fine-structure Excitation of C I from STIS Spectra in the HST Archive

    NASA Astrophysics Data System (ADS)

    Jenkins, Edward B.; Tripp, T. M.

    2006-06-01

    We have used the method of Jenkins & Tripp (2001: ApJS, 137, 297) to extract velocity profiles of the absorption by interstellar neutral carbon atoms in the 3 different fine-structure levels of the ground electronic state. The populations of these levels are governed by the balance between collisional excitations (and de-excitations) against radiative decay. By studying these populations, we can determine the different combinations of local temperatures and densities of the C I-bearing gas. We have analyzed virtually all of the stellar spectra in HST Archive that show clearly the multiplets of C I recorded with the E140H echelle grating of STIS. We have now expanded our coverage from the 21 stars in our original survey to a new total of 102 stars. This new study increases the coverage in Galactic longitudes well beyond that of the earlier observing program, which was mostly restricted to the intersections of the two HST continuous viewing zones and the plane of the Galaxy. We propose that substantial deviations of thermal pressures above and below a mean value are caused by interstellar turbulence, and we correlate these deviations with the kinematic properties of the gas. We derive an overall C I-weighted distribution function for the thermal pressures, and this distribution can be converted to one that applies to all of the neutral gas after we correct for changes in the ionization equilibrium between the neutral and ionized forms of carbon.This research was supported by grant HST-AR-09534.01 from the Space Telescope Science Institute, operated by the Association of Universities for Research in Astronomy, Inc., under NASA contract NAS5-26555.

  13. Parallel factor analysis of excitation-emission matrix fluorescence spectra of water soluble soil organic matter as basis for the determination of conditional metal binding parameters.

    PubMed

    Ohno, Tsutomu; Amirbahman, Aria; Bro, Rasmus

    2008-01-01

    Organic matter-metal complexes in soil solution and aquatic systems are involved in important environmental and ecological processes such as plant nutrient availability and the solubilization and transport of metals. Our work presented here extends the use of fluorescence spectrometry for determining conditional stability constants for such complexes. We combine the use of excitation-emission matrix (EEM) fluorescence spectrometry and parallel factor analysis (PARAFAC) to determine the stability constants of the chemically meaningful components modeled by PARAFAC. Water-soluble organic matter (WSOM) from O-horizon soils of deciduous and coniferous forest stands were extracted and titrated at pH = 4.7 with iron(lll) (Fe) and aluminum (Al) which are important metals in acid soil systems. The EEM spectra were then recorded and PARAFAC analysis showed that the WSOM contained three humic-substance-like components. Fe titration led to fluorescence quenching of the three components, while Al titration enhanced fluorescence for two components and quenched one of the components. The average Ryan-Weber stability constants at pH 4.7 ranged from log K of 4.28 to 4.91 for Fe and 4.84 to 5.96 for Al. The conditional stability constants were similar for Fe binding for deciduous and coniferous stand-derived WSOM, while they were stronger for Al binding with coniferous stand-derived WSOM. This difference in binding strengths for Al may affect the chemical behavior of Al in soil and aquatic systems. Determining the individual binding parameters of organic matter components with metals represents a significant advance over current approaches that utilize fluorescence quenching at a single excitation-emission wavelength pair to characterize organic matter-metal interactions.

  14. On the Determination of the Spin of the Black Hole in Cyg X-1 from X-Ray Reflection Spectra

    NASA Technical Reports Server (NTRS)

    Fabian, A. C.; Wilkins, D.; Miller, J. M.; Reis, R. C.; Reynolds, C. S.; Cackett, E. M.; Nowak, M. A.; Pooley, G.; Pottschmidt, K.; Sanders, J. S.; Ross, R. R.; Wilms, J.

    2012-01-01

    The spin of Cygnus X-I is measured by fitting reflection models to Suzaku data covering the energy band 0.9-400 keY. The inner radius of the accretion disc is found to lie within 2 gravitational radii (rg = GM/c(exp 2)) and a value for the dimensionless black hole spin is obtained of 0.97(sup .0.14) (sup -0.02). This agrees with recent measurements using the continuum fitting method by Gou et al. and of the broad iron line by Duro et al. The disc inclination is measured at 23.7(sup +6.7) (sup -5.4) deg. which is consistent with the recent optical measurement of the binary system inclination by Orosz et al of 27+/- 0.8 deg. We pay special attention to the emissivity profile caused by irradiation of the inner disc by the hard power-law source. 1be X-ray observations and simulations show that the index q of that profile deviates from the commonly used, Newtonian, value of 3 within 3r(sub g), steepening considerably within 2r(sub g). as expected in the strong gravity regime.

  15. Evolution of spin wave excitations with Co-doping in the spinel MnV2O4

    NASA Astrophysics Data System (ADS)

    Hahn, Steven; Ma, Jie; Lee, Jun Hee; Hong, Tao; Cao, Huibo; Aczel, Adam; Dun, Zhiling; Stone, Matthew; Tian, Wei; Qiu, Yiming; Copley, John; Zhou, Haidong; Fishman, Randy; Matsuda, Masaaki

    2015-03-01

    Spin waves were measured at several levels of Co-doping in the spinel system MnV2O4 by inelastic neutron scattering and analyzed with first-principles-guided spin models. Co-doping creates a rich phase diagram encompassing the transition from localized- to itinerant-electron regimes. Increasing Co concentration weakens the single-ion anisotropy and increases both the magnitude and isotropy of the nearest-neighbor exchange interactions. First principles calculations emphasize the the distinctly different microscopic origins of the two-in-two-out magnetic structure at the Mn-rich and Co-rich limits. Research at HFIR and SNS, ORNL, were sponsored by the Scientific User Facilities Division and Materials Science and Engineering Division, Office of Basic Energy Sciences, US Department of Energy.

  16. Spin pumping by magnetopolaritons

    NASA Astrophysics Data System (ADS)

    Cao, Yunshan; Yan, Peng; Huebl, Hans; Goennenwein, Sebastian; Bauer, Gerrit

    2015-03-01

    Recent experiments report the strong coupling of microwaves to the magnetic insulator yttrium iron garnet with weakly damped magnetization dynamics. We developed a scattering approach to study the coupled magnetization and microwave cavities beyond the paramagnetic/macrospin and rotating wave approximations that are implicit in the Tavis-Cummings model. To this end we solve the coupled Landau-Lifshitz-Gilbert and Maxwell's equations for a thin film magnet in a microwave cavity, leading to rich ferromagnetic spin wave resonance spectra of the transmitted or absorbed microwaves. Our method is valid for the full parameter range spanning the weak to strong coupling limits. We demonstrate strong coupling achievement not only for the FMR mode but also for standing spin waves, although the lowest excitation has a decisive leading role for coupling strength. Spin pumping in FI|N bilayers as detected by inverse spin Hall voltages provides additional access to study strong coupling electrically. Funding from the European Union Seventh Framework Programme [FP7-People-2012-ITN] under Grant Agreement 316657 (SpinIcur).

  17. Re-Analysis of the Spin-Orbit Perturbation for the Phillips System and the Ballik-Ramsay System of the Spectra of C_{2}

    NASA Astrophysics Data System (ADS)

    Chen, Wang; Tang, Jian; Kawaguchi, Kentarou

    2013-06-01

    The Phillips system and the Ballik-Ramsay system of the spectra of C_{2} have been studied extensively before, and the energy difference between the ground X^{1}Σ^{+}_{g} state and the first triplet a^{3}Π_{u} state has been determined by analyzing the spin-orbit interaction between the X^{1}Σ^{+}_{g} and b^{3}Σ^{-}_{g} states. However, the analysis was carried out previously for the individual vibronic bands, and the perturbation parameters of the spin-orbit interaction determined for the different vibronic states lead to the very different values of A_{so}^{bX}. In the present study, we re-analyzed the previous spectral data^{a,} by using the overlap integrals (Franck-Condon factors) and r-centroids between the vibronic states of X^{1}Σ^{+}_{g} and b^{3}Σ^{-}_{g} calculated from the RKR potential and by fitting all the vibronic states simultaneously. A new set of molecular parameters was obtained, including the single-valued spin-orbit interaction constant A_{so}^{bX}=3.067(9) cm^{-1} and the energy difference Δ E=719.84(6) cm^{-1} between the X^{1}Σ^{+}_{g} and a^{3}Π_{u} states, the latter of which is about 1.5 cm^{-1} larger than the previously determined value.^{a} This new result may guide for searching the forbidden transitions between the singlet and triplet states of C_{2}. C. Amiot, J. Chauville and J. -P. Maillard, J. Mol. Spectrosc. {75}, 19 (1979). S. P. Davis et al., J. Opt. Sol. Am. B. {5}, 1838 (1988). M. Douay, R. Nietmann and P. -F. Bernath, J. Mol. Spectrosc. {131}, 250 (1988). M-C. Chan et al., Chem. Phys. Lett. {390}, 340 (2004).

  18. Effect of adsorbed iron on thermoluminescence and electron spin resonance spectra of Ca-Fe-exchanged montmorillonite

    NASA Technical Reports Server (NTRS)

    Coyne, Lelia M.; Banin, Amos

    1986-01-01

    The ESR spectra and the natural and gamma-induced thermoluminescence (TL) glow curves of a series of variably cation-exchanged Fe-Ca-clays prepared from SWy-1 montmorillonite were examined. The ESR signal intensity associated with surface Fe increased linearly with surface Fe content up to a nominal concentration of 50 percent exchangeable Fe. At above 50 percent exchangeable Fe, no appreciable increase in the signal was noted. The TL intensity decreased linearly with increasing surface Fe up to 50 percent nominal exchangeable Fe. At above 50 percent, the signal was not appreciably further diminished. Possible effects of Fe on quenching of TL are considered.

  19. Measuring nonequilibrium retarded spin-spin Green's functions in an ion-trap-based quantum simulator

    NASA Astrophysics Data System (ADS)

    Yoshimura, Bryce T.; Freericks, J. K.

    2016-05-01

    Recently a variant on Ramsey interferometry for coupled spin-1 /2 systems was proposed to directly measure the retarded spin-spin Green's function. In conventional experimental situations, the spin system is initially in a nonequilibrium state before the Ramsey interferometry is performed, so we examine the nonequilibrium retarded spin-spin Green's functions within the transverse-field Ising model. We derive the lowest four spectral moments to understand the short-time behavior and we employ a Lehmann-like representation to determine the spectral behavior. We simulate a Ramsey protocol for a nonequilibrium quantum spin system that consists of a coherent superposition of the ground state and diabatically excited higher-energy states via a temporally ramped transverse magnetic field. We then apply the Ramsey spectroscopy protocol to the final Hamiltonian, which has a constant transverse field. The short time allows us to extract the initial transport of many-body correlations, while the long-time behavior relates to the excitation spectra of the Hamiltonian. Compressive sensing is employed in the data analysis to efficiently extract that spectra.

  20. Low-amplitude magnetic vortex core reversal by non-linear interaction between azimuthal spin waves and the vortex gyromode

    SciTech Connect

    Sproll, Markus; Noske, Matthias; Kammerer, Matthias; Dieterle, Georg; Weigand, Markus; Stoll, Hermann; Schütz, Gisela; Bauer, Hans; Gangwar, Ajay; Woltersdorf, Georg; Back, Christian H.

    2014-01-06

    We show, by experiments and micromagnetic simulations in vortex structures, that an active “dual frequency” excitation of both the sub-GHz vortex gyromode and multi-GHz spin waves considerably changes the frequency response of spin wave mediated vortex core reversal. Besides additional minima in the switching threshold, a significant broadband reduction of the switching amplitudes is observed, which can be explained by non-linear interaction between the vortex gyromode and the spin waves. We conclude that the well known frequency spectra of azimuthal spin waves in vortex structures are altered substantially, when the vortex gyromode is actively excited simultaneously.

  1. Linewidth narrowing in the epr spectra of Gd 3+ impurity ions due to the spin-lattice relaxation of lanthanide Kramers' host ions

    NASA Astrophysics Data System (ADS)

    Malhotra, V. M.; Dixon, J. M.; Buckmaster, H. A.

    1980-08-01

    Electron paramagnetic resonance (EPR) of Gd 3+ doped in some lanthanide Kramers' host ion single crytals of the sulfate octahydrates (Ln 2(SO 4) 3·8H 2O;Ln≡Nd,Sm,Dy and Er) and trichloride hexahydrates (LnCl 3·6H 2O;Ln≡Nd, Sm, Dy, Er and Yb) has been studied at T ≅ 297 K using a 9.4 GHz EPR spectrometer. The effect of the Kramers' host Ln 3+ ions on the g-values and linewidths of Gd 3+ spectra has been determined by comparison with those for the isostructural diamagnetic La, Y lattices. At 297 K,in the EPR transitions of Gd 3+ ions have narrow linewidths in spite of the presence of paramagnetic host ions like Nd 3+, Sm 3+ and Yb 3+, whereas an unusual variation in the linewidth is observed in the Dy 3+, Er 3+ hosts as well as a negative g-value shift. In these latter hosts, the linewidths of the Δ M = ± 1 transitions decrease progressively as the magnitude of M increases. The observation of resolved Gd 3+ spectra at 297 K in the above hosts has been interpreted in terms of a random modulation of the interactions between the Gd 3+ and the host Ln 3+ ions by the rapid spin-lattice relaxation of Ln 3+ ions following the generalized theory of magnetic resonance by Kubo and Tomita [15]. τ 1 for Ln 3+ has been estimated in the above mentioned Kramers' hosts from the observed EPR linewidths of Gd 3+ spectra. Values for τ 1 have also been computed for Ln 3+ ions in Ln(C 2H 5SO 4) 3. 9H 2O and LnF 3 from linewidth data in the literature. The results are consistent with an effective host spin-lattice time which is due to Orbach and/or Raman processes, depending upon the temperature and the ground state energy level scheme.

  2. Theoretical study on the low-lying excited states of the phosphorus monoiodide (PI) including the spin-orbit coupling

    NASA Astrophysics Data System (ADS)

    Zhang, Xiaomei; Liu, Xiaoting; Liang, Guiying; Li, Rui; Xu, Haifeng; Yan, Bing

    2016-01-01

    The potential energy curves (PECs) of the 22 Λ-S states of the phosphorus monoiodide (PI) molecule have been calculated at the level of MRCI+Q method with correlation-consistent quadruple-ζ quality basis set. The spectroscopic constants of the bound states are determined, which well reproduce the available measurements. The metastable a1Δ state has been reported for the first time, which lies between the X3Σ- and b1Σ+ states and have much deeper well than the ground state. The R-dependent spin-orbit (SO) matrix elements are calculated with the full-electron Breit-Pauli operator. Based on the SO matrix elements, the perturbations that the 23Π state may suffer from are analyzed in detail. The SOC effect makes the original Λ-S states split into 51 Ω states. In the zero-field splitting of the ground state X3Σ-, the spin-spin coupling contribution (2.23 cm-1) is found to be much smaller compared to the spin-orbit coupling contribution (50 cm-1). The avoided crossings between the Ω states lead to much shallower potential wells and the change of dissociation relationships of the states. The Ω-state wavefunctions are analyzed depending on their Λ-S compositions, showing the strong interactions among several quasidegenerate Λ-S states of the same total SO symmetry. The transition properties including electric dipole (E1), magnetic dipole (M1), and electric quadrupole (E2) transition moments (TMs), the Franck-Condon factors, the transition probabilities and the radiative lifetimes are computed for the transitions between Ω components of a1Δ and b1Σ+ states and ground state. The transition probabilities induced by the E1, E2, and M1 transitions are evaluated. The E2 makes little effect on transition probabilities. In contrast, the E1 transition makes the main contribution to the transition probability and the M1 transition also brings the influence that cannot be neglected. Finally, the radiative lifetimes are determined with the transition moments including E

  3. Magnetic ordering, spin waves, and Haldane-gap excitations in (Nd{sub x}Y{sub 1{minus}x}){sub 2}BaNiO{sub 5} linear-chain mixed-spin antiferromagnets

    SciTech Connect

    Yokoo, T.; Raymond, S.; Zheludev, A.; Maslov, S.; Ressouche, E.; Nakamura, M.; Akimitsu, J.

    1998-12-01

    Linear-chain nickelates with the composition (Nd{sub x}Y{sub 1{minus}x}){sub 2}BaNiO{sub 5} (x=1, x=0.75, x=0.5, and x=0.25) are studied in a series of neutron-scattering experiments. Powder diffraction is used to determine the temperature dependence of the magnetic structure in all four systems. Single-crystal inelastic neutron scattering is employed to investigate the temperature dependence of the Haldane-gap excitations and low-energy spin waves in the x=1 compound Nd{sub 2}BaNiO{sub 5}. The results of these experiments are discussed in the context of the {open_quotes}Haldane chain in a staggered field{close_quotes} model for R{sub 2}BaNiO{sub 5} systems, and quantitative agreement with theory is obtained. {copyright} {ital 1998} {ital The American Physical Society}

  4. Spin-Sensitive and Angular Dependent Detection of Resonant Excitations at the K Absorption Pre-Edge of {alpha}-Fe2O3

    SciTech Connect

    Glatzel, Pieter; Mirone, Alessandro; Eeckhout, Sigrid G.; Sikora, Marcin; Giuli, Gabriele

    2007-02-02

    An experimental and theoretical study of the K absorption pre-edge in hematite ({alpha}-Fe2O3) is presented. Resonant inelastic X-ray scattering with a 3p hole in the final states was used to obtain spin-selective absorption spectra. Spectral variations with changing the orientation of the incident X-ray polarization vector with respect to the crystal c-axis in single crystalline hematite are discussed. The experimental results can be successfully modeled using a band-structure approach (WIEN2k with LDA+U). A pre-edge absorption feature is assigned to unoccupied p electronic states due to Fe-Fe interactions, i.e. they are due to non-local transitions.

  5. Ab initio study on the low-lying excited states of gas-phase PH+ cation including spin-orbit coupling

    NASA Astrophysics Data System (ADS)

    Li, Xia; Zhang, Xiaomei; Yan, Bing

    2015-05-01

    Ab initio calculations have been performed on the low-lying excited and ground states of PH+. The potential energy curves (PECs) of the Λ-S states were calculated with multi-reference configuration interaction (MRCI) method along with the basis sets at 5-ξ level. In order to improve the PECs, the Davidson(+Q) correction and the Scalar relativistic effect are included. The corresponding spectroscopic constants were determined and good agreements with the available measurement were found. The interactions of the A2Δ-4Π and 12Σ+-4Π by the spin-orbit coupling (SOC) effect were well described by the spin-orbit matrix elements. The SOC effect makes the original 8 Λ-S states split into 15 Ω states. The Ω = 1/2 state generated from the X2Π state is confirmed to the ground Ω state. And the SOC splitting for the X2Π is calculated to be 294 cm-1. The SOC effect has large effect on the PECs of the A2Δ and 12Σ+ states, leading to much more shallow potential wells as well as potential barriers. The analysis of the wavefunction for the Ω states shows that the strong spin-orbit interaction exists near the crossing points of the PECs for the Λ-S states. The transition dipole moments (TDMs) of transitions A2Δ-X2Π and 12Σ--X2Π are evaluated with the MRCI wavefunction. Based on the TDMs along with the calculated Franck-Condon factors, the radiative lifetimes for the selected vibrational levels of A2Δ and 12Σ- states are predicted at the microseconds (μs). Good agreement with the measurement shows that the lowest vibrational level for A2Δ state is almost uninfluenced by the perturbation via the SOC effect.

  6. Source indicators of humic substances and proto-kerogen - Stable isotope ratios, elemental compositions and electron spin resonance spectra

    NASA Technical Reports Server (NTRS)

    Stuermer, D. H.; Peters, K. E.; Kaplan, I. R.

    1978-01-01

    Stable isotope ratios of C, N and H, elemental compositions, and electron spin resonance (ESR) data of humic acids and proto-kerogens from twelve widely varying sampling locations are presented. Humic acids and proto-kerogens from algal sources are more aliphatic and higher in N than those from higher plant sources. Oxygen content appears to represent a measure of maturation, even in Recent sediments, and S content may reflect redox conditions in the environment of deposition. The ESR data indicate that the transformation of humic substances to proto-kerogens in Recent sediments is accompanied by an increase in aromatic character. A combination of stable carbon isotope ratio and H/C ratio may be a simple but reliable source indicator which allows differentiation of marine-derived from terrestrially-derived organic matter. The stable nitrogen isotope ratios are useful indicators of nitrogen nutrient source. Deuterium/hydrogen isotope ratios appear to reflect variations in meteoric waters and are not reliable source indicators.

  7. Electronically excited-state properties and predissociation mechanisms of phosphorus monofluoride: A theoretical study including spin-orbit coupling

    NASA Astrophysics Data System (ADS)

    Yu, Le; Bian, Wensheng

    2012-07-01

    The 51 Ω states generated from the 22 Λ - S states of phosphors monofluoride have been investigated using the valence internally contracted multireference configuration interaction method with the Davidson correction and the entirely uncontracted aug-cc-pV5Z basis set. The spin-orbit coupling is computed using the state interaction approach with the Breit-Pauli Hamiltonian. Based on the calculated potential energy curves, the spectroscopic constants of the bound and quasibound Λ - S and Ω states are obtained, and very good agreement with experiment is achieved. Several quasibound states caused by avoided crossings are found. Various curve crossings and avoided crossings are revealed, and with the help of our computed spin-orbit coupling matrix elements, the predissociation mechanisms of the a1Δ, b1Σ+, e3Π, g1Π, and (3)3Π states are analyzed. The intricate couplings among different electronic states are investigated. We propose that the avoided crossing between the A3Π0 + and b^1 {Σ }_{{0 + }}^{+ } states may be responsible for the fact that the A3Π ν' ⩾ 12 vibrational levels can not be observed in experiment. The transition properties of the A3Π - X3Σ- transition are studied, and our computed Franck-Condon factors and radiative lifetimes match the experimental results very well.

  8. Optical diode effect at THz frequencies of spin-wave excitations in the room-temperature multiferroic BiFeO3

    NASA Astrophysics Data System (ADS)

    Rõõm, Toomas; Nagel, U.; Bordács, S.; Kézsmárki, I.; Yi, H. T.; Cheong, S.-W.; Lee, J. H.; Fishman, R. S.

    We studied the unidirectional transmission of THz radiation in BiFeO3 crystals, the unique multiferroic compound offering a real potential for room-temperature applications. We found that the optical magnetoelectric effect generated by spin waves in BiFeO3 is robust enough to cause considerable nonreciprocal directional dichroism in the GHz-THz range even at room temperature. The optical magnetoelectric effect in BiFeO3 is dominated by two types of spin-current induced polarizations, while the exchange-striction and single-ion polarization terms do not significantly contribute to it. Our work demonstrates that the nonreciprocal directional dichroism spectra and their theoretical analysis provide microscopic model of the magnetoelectric couplings in multiferroic materials. We acknowledge the Estonian Grant IUT23-3; the Hungarian OTKA K 108918, OTKA PD 111756, Bolyai 00565/14/11; the DOE, Office of Sciences, Basic Energy Sciences, Mat. Sciences and Eng. Div., and the DOE Grant DE-FG02-07ER46382.

  9. Investigation of low/medium spin excited states in 150-154Sm via the (p,d) and (p,t) reactions

    NASA Astrophysics Data System (ADS)

    Humby, P.; Simon, A.; Beausang, C.; Gell, K.; Tarlow, T.; Vyas, G.; Ross, T. J.; Hughes, R. O.; Burke, J. T.; Casperson, R. J.; Koglin, J.; Ota, S.; Allmond, J. M.; McCleskey, M.; McCleskey, E.; Saastamoinen, A.; Chyzh, R.; Dag, M.

    2014-03-01

    Low/medium spin excited states of 151,153Sm and 150,152Sm were studied via the (p,d) and (p,t) reactions, respectively, utilizing the STARLITER arrays at the Cyclotron Institute of Texas A&M University. In the experiment 152Sm and 154Sm targets were bombarded with 25 MeV protons and the outgoing light charged particles (p, d and t) in the exit channels were detected using the STARS ΔE - E silicon telescope, thus allowing particle identification and a measurement of the nuclear excitation energy. Six BGO shielded HPGe detectors were used to observe the emitted gamma rays in coincidence with the particles. A post-run measurement of gamma rays emitted from the activated target allowed an improved measurement of the half life of the 96 minute Jπ =8- isomer of 152Eu. Preliminary results are presented. This work was partly supported by the US Department of Energy under Grants No. DE-FG52-06NA26206 and No. DE-FG02-05ER41379.

  10. Spin-wave excitations: the main source of the temperature dependence of interlayer exchange coupling in nanostructures.

    PubMed

    Schwieger, S; Kienert, J; Lenz, K; Lindner, J; Baberschke, K; Nolting, W

    2007-02-01

    Quantum mechanical calculations based on an extended Heisenberg model are compared with ferromagnetic resonance experiments on prototype trilayer systems Ni(7)/Cu(n)/Co(2)/Cu(001) in order to determine and separate for the first time quantitatively the sources of the temperature dependence of interlayer exchange coupling. Magnon excitations are responsible for about 75% of the reduction of the coupling strength from zero to room temperature. The remaining 25% are due to temperature effects in the effective quantum well and the spacer-magnet interfaces.

  11. Optical diode effect at spin-wave excitations in the room-temperature multiferroic BiFeO3.

    DOE PAGES

    Kezsmarki, I.; Nagel, U.; Bordacs, S.; Fishman, Randy Scott; Lee, Jun Hee; Yi, Hee Taek; Cheong, Sang-Wook; Room, T.

    2015-09-15

    The ability to read and write a magnetic state current-free by an electric voltage would provide a huge technological advantage. Dynamic or optical ME effects are equally interesting, because they give rise to unidirectional light propagation as recently observed in low-temperature multiferroics. This phenomenon, if realized at room temperature, would allow the development of optical diodes which transmit unpolarized light in one, but not in the opposite, direction. Here, we report strong unidirectional transmission in the room-temperature multiferroic BiFeO3 over the gigahertz-terahertz frequency range. The supporting theory attributes the observed unidirectional transmission to the spin-current-driven dynamic ME effect. Our findingsmore » are an important step toward the realization of optical diodes, supplemented by the ability to switch the transmission direction with a magnetic or electric field.« less

  12. Conservation laws, radiative decay rates, and excited state localization in organometallic complexes with strong spin-orbit coupling.

    PubMed

    Powell, B J

    2015-01-01

    There is longstanding fundamental interest in 6-fold coordinated d(6) (t(2g)(6)) transition metal complexes such as [Ru(bpy)3](2+) and Ir(ppy)3, particularly their phosphorescence. This interest has increased with the growing realisation that many of these complexes have potential uses in applications including photovoltaics, imaging, sensing, and light-emitting diodes. In order to design new complexes with properties tailored for specific applications a detailed understanding of the low-energy excited states, particularly the lowest energy triplet state, T1, is required. Here we describe a model of pseudo-octahedral complexes based on a pseudo-angular momentum representation and show that the predictions of this model are in excellent agreement with experiment - even when the deviations from octahedral symmetry are large. This model gives a natural explanation of zero-field splitting of T1 and of the relative radiative rates of the three sublevels in terms of the conservation of time-reversal parity and total angular momentum modulo two. We show that the broad parameter regime consistent with the experimental data implies significant localization of the excited state. PMID:26123864

  13. Conservation laws, radiative decay rates, and excited state localization in organometallic complexes with strong spin-orbit coupling.

    PubMed

    Powell, B J

    2015-06-30

    There is longstanding fundamental interest in 6-fold coordinated d(6) (t(2g)(6)) transition metal complexes such as [Ru(bpy)3](2+) and Ir(ppy)3, particularly their phosphorescence. This interest has increased with the growing realisation that many of these complexes have potential uses in applications including photovoltaics, imaging, sensing, and light-emitting diodes. In order to design new complexes with properties tailored for specific applications a detailed understanding of the low-energy excited states, particularly the lowest energy triplet state, T1, is required. Here we describe a model of pseudo-octahedral complexes based on a pseudo-angular momentum representation and show that the predictions of this model are in excellent agreement with experiment - even when the deviations from octahedral symmetry are large. This model gives a natural explanation of zero-field splitting of T1 and of the relative radiative rates of the three sublevels in terms of the conservation of time-reversal parity and total angular momentum modulo two. We show that the broad parameter regime consistent with the experimental data implies significant localization of the excited state.

  14. Investigations on thermodynamic properties of the three sub-lattice spin frustrated chain

    NASA Astrophysics Data System (ADS)

    Wang, Jue; Zhou, Hong-Fei; Li, Qian-Chun; Dong, Hui-Ning

    2015-08-01

    The spin frustration related to the high-Tc superconductivity has received much attention. In this paper, based on the Jordan-Wigner transformation and Green’s function method, we study the magnetic and thermodynamic properties of the three sub-lattice spin frustrated chains. It is found that there are three branches for the spin-wave excitation spectra at zero temperature. Among them, two belong to nature excitation patterns with antiferromagnetic interaction and the third one is band gap excitation spectrum with ferromagnetic nature. The specific heat capacity of sub-lattice spin system presents complex characteristics with the change of temperature due to the intense competition between the ferromagnetic and antiferromagnetic interactions. It is also shown that the increase of the ferromagnetic action is helpful to the value of net spin.

  15. Use of Nuclear Spin Noise Spectroscopy to Monitor Slow Magnetization Buildup at Millikelvin Temperatures

    PubMed Central

    Pöschko, Maria Theresia; Peat, David; Owers‐Bradley, John

    2016-01-01

    Abstract At ultralow temperatures, longitudinal nuclear magnetic relaxation times become exceedingly long and spectral lines are very broad. These facts pose particular challenges for the measurement of NMR spectra and spin relaxation phenomena. Nuclear spin noise spectroscopy is used to monitor proton spin polarization buildup to thermal equilibrium of a mixture of glycerol, water, and copper oxide nanoparticles at 17.5 mK in a static magnetic field of 2.5 T. Relaxation times determined in such a way are essentially free from perturbations caused by excitation radiofrequency pulses, radiation damping, and insufficient excitation bandwidth. The experimental spin‐lattice relaxation times determined on resonance by saturation recovery with spin noise detection are consistently longer than those determined by using pulse excitation. These longer values are in better accordance with the expected field dependence trend than those obtained by on‐resonance experiments with pulsed excitation. PMID:27305629

  16. Comment on 'Mapping of localized spin-wave excitations by near-field Brillouin light scattering' [Appl. Phys. Lett. 97, 152502 (2010)].

    SciTech Connect

    Giovannini, L.; Montoncello, F.; Nizzoli, F.; Vavassori, P.; Grimsditch, M.

    2011-11-04

    The authors reported in their letter some outstanding experimental results of spin excitations in nano-particles investigated by near-field Brillouin scattering. They conclude from their observations that existing theories -- in particular micromagnetic simulations -- do not correctly describe the behavior of the spin modes. Since excellent agreement has been reported between spin-wave mode frequencies obtained from Brillouin scattering experiments and those obtained from micromagnetic-based simulations, it is somewhat surprising that the simulations should fail for the particles investigated in Ref. 1. In the literature, there is also evidence of various kinds and degrees of mode localization when exchange competes with dipolar interactions. When dipolar long-range interactions are taken into account, the eigenmodes can be seen as the superposition of plane waves, leading to different localizations and in particular to the appearence of bulk-dead modes. We have simulated the normal modes of the particles used in Ref. 1, with the dynamical matrix method; the results are shown in Fig. 1 for different values of the applied field. In addition to the lowest frequency non-localized mode (1-BA), several localized modes are present. Large particles exhibit modes with oscillations along the field direction;8 for such modes, we use the label n-BA-loc, with n the number of nodes. While the profile of the pure end-mode, i.e., 0-BA-loc, has its maximum at the edge with the amplitude monotonously decreasing toward the interior of the ellipse, as correctly described by the authors, the localized modes with n > 0, not considered by them, do not have this characteristic: see inset of Fig. 1. Based on Fig. 1, we believe that the assumption that the mode they observe is 'the' localized spin mode is not correct. Instead, we believe that the mode detected in the experiment at H > 700 Oe is a combinations (due to non-linear excitation conditions of the experiment) of several n

  17. Mapping chiral symmetry breaking in the excited baryon spectrum

    NASA Astrophysics Data System (ADS)

    Bicudo, Pedro; Cardoso, Marco; Llanes-Estrada, Felipe J.; Van Cauteren, Tim

    2016-09-01

    We study the conjectured "insensitivity to chiral symmetry breaking" in the highly excited light baryon spectrum. While the experimental spectrum is being measured at JLab and CBELSA/TAPS, this insensitivity remains to be computed theoretically in detail. As the only existing option to have both confinement, highly excited states, and chiral symmetry, we adopt the truncated Coulomb-gauge formulation of QCD, considering a linearly confining Coulomb term. Adopting a systematic and numerically intensive variational treatment up to 12 harmonic oscillator shells we are able to access several angular and radial excitations. We compute both the excited spectra of I =1 /2 and I =3 /2 baryons, up to large spin J =13 /2 , and study in detail the proposed chiral multiplets. While the static-light and light-light spectra clearly show chiral symmetry restoration high in the spectrum, the realization of chiral symmetry is more complicated in the baryon spectrum than earlier expected.

  18. Spin Polarized Electron Probes and Magnetic Nanostructures

    SciTech Connect

    D.L. Mills

    2003-10-15

    OAK B188 This report summarizes progress to date in our theoretical research program, for the period from July 1, 2002 to November 1, 2003. In addition, our research priorities for the coming year are set forth. The reporting period has been a most exciting and significant one. For the past several years, one of our principal thrust areas has been development of the theory of spin dynamics in magnetic nanostructures with emphasis on the use of spin polarized electrons as probes of short wavelength spin dynamics in such entities. Our program stimulated the first experiment which detected large wave vector spin waves in ultrathin films in 1999 through spin polarized electron loss spectroscopy (SPEELS); the publication which announced this discovery was a joint publication between a group in Halle (Germany) with our theory effort. The continued collaboration has led to the design and implementation of the new SPEELS spectrometer and we now have in hand the first detailed measurements of spin wave dispersion in an ultrathin film. A second such spectrometer is now operational in the laboratory of Prof. H. Hopster, at UC Irvine. We are thus entering a most exciting new era in the spectroscopy of spin excitations in magnetic nanostructures. During the reporting period, we have completed very important new analyses which predict key aspects of the spectra which will be uncovered by these new instruments, and the calculations continue to be developed and to expand our understanding. In addition, we have initiated a new series of theoretical studies directed toward spin dynamics of single magnetic adatoms on metal surfaces, with STM based studies of this area n mind. In the near future, these studies will continue, and we will expand our effort into new areas of spin dynamics in magnetic nanostructures.

  19. Optical Diode Effect at Spin-Wave Excitations of the Room-Temperature Multiferroic BiFeO_{3}.

    PubMed

    Kézsmárki, I; Nagel, U; Bordács, S; Fishman, R S; Lee, J H; Yi, Hee Taek; Cheong, S-W; Rõõm, T

    2015-09-18

    Multiferroics permit the magnetic control of the electric polarization and the electric control of the magnetization. These static magnetoelectric (ME) effects are of enormous interest: The ability to read and write a magnetic state current-free by an electric voltage would provide a huge technological advantage. Dynamic or optical ME effects are equally interesting, because they give rise to unidirectional light propagation as recently observed in low-temperature multiferroics. This phenomenon, if realized at room temperature, would allow the development of optical diodes which transmit unpolarized light in one, but not in the opposite, direction. Here, we report strong unidirectional transmission in the room-temperature multiferroic BiFeO_{3} over the gigahertz-terahertz frequency range. The supporting theory attributes the observed unidirectional transmission to the spin-current-driven dynamic ME effect. These findings are an important step toward the realization of optical diodes, supplemented by the ability to switch the transmission direction with a magnetic or electric field.

  20. Optical Diode Effect at Spin-Wave Excitations of the Room-Temperature Multiferroic BiFeO3

    NASA Astrophysics Data System (ADS)

    Kézsmárki, I.; Nagel, U.; Bordács, S.; Fishman, R. S.; Lee, J. H.; Yi, Hee Taek; Cheong, S.-W.; Rõõm, T.

    2015-09-01

    Multiferroics permit the magnetic control of the electric polarization and the electric control of the magnetization. These static magnetoelectric (ME) effects are of enormous interest: The ability to read and write a magnetic state current-free by an electric voltage would provide a huge technological advantage. Dynamic or optical ME effects are equally interesting, because they give rise to unidirectional light propagation as recently observed in low-temperature multiferroics. This phenomenon, if realized at room temperature, would allow the development of optical diodes which transmit unpolarized light in one, but not in the opposite, direction. Here, we report strong unidirectional transmission in the room-temperature multiferroic BiFeO3 over the gigahertz-terahertz frequency range. The supporting theory attributes the observed unidirectional transmission to the spin-current-driven dynamic ME effect. These findings are an important step toward the realization of optical diodes, supplemented by the ability to switch the transmission direction with a magnetic or electric field.

  1. Nuclear Spin Locking and Extended Two-Electron Spin Decoherence Time in an InAs Quantum Dot Molecule

    NASA Astrophysics Data System (ADS)

    Chow, Colin; Ross, Aaron; Steel, Duncan; Sham, L. J.; Bracker, Allan; Gammon, Daniel

    2015-03-01

    The spin eigenstates for two electrons confined in a self-assembled InAs quantum dot molecule (QDM) consist of the spin singlet state, S, with J = 0 and the triplet states T-, T0 and T+, with J = 1. When a transverse magnetic field (Voigt geometry) is applied, the two-electron system can be initialized to the different states with appropriate laser excitation. Under the excitation of a weak probe laser, non-Lorentzian lineshapes are obtained when the system is initialized to either T- or T+, where T- results in a ``resonance locking'' lineshape while T+ gives a ``resonance avoiding '' lineshape: two different manifestations of hysteresis showing the importance of memory in the system. These observations signify dynamic nuclear spin polarization (DNSP) arising from a feedback mechanism involving hyperfine interaction between lattice nuclei and delocalized electron spins, and Overhauser shift due to nuclear spin polarization. Using pump configurations that generate coherent population trapping, the isolation of the electron spin from the optical excitation shows the stabilization of the nuclear spin ensemble. The dark-state lineshape measures the lengthened electron spin decoherence time, from 1 ns to 1 μs. Our detailed spectra highlight the potential of QDM for realizing a two-qubit gate. This work is supported by NSF, ARO, AFOSR, DARPA, and ONR.

  2. Resonant Spin Excitation in the High Temperature Superconductor Ba0.6K0.4Fe2As2

    SciTech Connect

    Christianson, Andrew D; Goremychkin, E. A.; Osborn, R.; Rosenkranz, Stephen; Lumsden, Mark D; Malliakas, C.; Todorov, L.; Claus, H.; Chung, D.Y.; Kanatzidis, M.; Bewley, Robert I.; Guidi, T.

    2008-12-18

    A new family of superconductors containing layers of iron arsenide has attracted considerable interest because of their high transition temperatures (T{sub c}), some of which are >50 K, and because of similarities with the high-{sub c} copper oxide superconductors. In both the iron arsenides and the copper oxides, superconductivity arises when an antiferromagnetically ordered phase has been suppressed by chemical doping. A universal feature of the copper oxide superconductors is the existence of a resonant magnetic excitation, localized in both energy and wavevector, within the superconducting phase. This resonance, which has also been observed in several heavy-fermion superconductors is predicted to occur when the sign of the superconducting energy gap takes opposite values on different parts of the Fermi surface, an unusual gap symmetry which implies that the electron pairing interaction is repulsive at short range. Angle-resolved photoelectron spectroscopy shows no evidence of gap anisotropy in the iron arsenides, but such measurements are insensitive to the phase of the gap on separate parts of the Fermi surface. Here we report inelastic neutron scattering observations of a magnetic resonance below T{sub c} in Ba{sub 0.6}K{sub 0.4}Fe{sub 2}As{sub 2}, a phase-sensitive measurement demonstrating that the superconducting energy gap has unconventional symmetry in the iron arsenide superconductors.

  3. Broadband excitation in solid-state NMR of paramagnetic samples using Delays Alternating with Nutation for Tailored Excitation ('Para-DANTE')

    NASA Astrophysics Data System (ADS)

    Carnevale, Diego; Vitzthum, Veronika; Lafon, Olivier; Trébosc, Julien; Amoureux, Jean-Paul; Bodenhausen, Geoffrey

    2012-11-01

    This Letter shows that interleaved sequences of short pulses in the manner of 'Delays Alternating with Nutation for Tailored Excitation' (DANTE) with N = 1, 2, 3 … equidistant pulses per rotor period extending over K rotor periods can be used to excite, invert or refocus a large number of spinning sidebands of spin-1/2 nuclei in paramagnetic samples where hyperfine couplings lead to very broad spectra that extend over more than 1 MHz. The breadth of the response is maintained for rf-field amplitudes as low as 30 kHz since it results from cumulative effects of individual pulses with very short durations.

  4. A mixed quantum-classical molecular dynamics study of anti-tetrol and syn-tetrol dissolved in liquid chloroform II: infrared emission spectra, vibrational excited-state lifetimes, and nonequilibrium hydrogen-bond dynamics.

    PubMed

    Kwac, Kijeong; Geva, Eitan

    2013-11-21

    The effect of vibrational excitation and relaxation of the hydroxyl stretch on the hydrogen-bond structure and dynamics of stereoselectively synthesized syn-tetrol and anti-tetrol dissolved in deuterated chloroform are investigated via a mixed quantum-classical molecular dynamics simulation. Emphasis is placed on the changes in hydrogen-bond structure upon photoexcitation and the nonequilibrium hydrogen-bond dynamics that follows the subsequent relaxation from the excited to the ground vibrational state. The propensity to form hydrogen bonds is shown to increase upon photoexcitation of the hydroxyl stretch, thereby leading to a sizable red-shift of the infrared emission spectra relative to the corresponding absorption spectra. The vibrational excited state lifetimes are calculated within the framework of Fermi's golden rule and the harmonic-Schofield quantum correction factor, and found to be sensitive reporters of the underlying hydrogen-bond structure. The energy released during the relaxation from the excited to the ground state is shown to break hydrogen bonds involving the relaxing hydroxyl. The spectral signature of this nonequilibrium relaxation process is analyzed in detail.

  5. Changes of the local magnetic properties of the optically excited Nd3+ ions and their manifestation in the near IR spectra of the Nd0.5Gd0.5Fe3(BO3)4 crystal

    NASA Astrophysics Data System (ADS)

    Malakhovskii, A. V.; Gnatchenko, S. L.; Kachur, I. S.; Piryatinskaya, V. G.; Temerov, V. L.

    2016-02-01

    Polarized absorption spectra of f-f transitions 4I9/2 → 4F3/2 and (2H9/2 + 4F5/2) in the Nd3+ ion in the Nd0.5Gd0.5Fe3(BO3)4 single crystal were studied as a function of temperature in the range of 2-40 K and as a function of magnetic field in the range of 0-65 kOe at 2 K. It was found out that the selection rules for f-f electron transitions substantially changed in the magnetically ordered state of the crystal, and they strongly depended on the orientation of the Fe and Nd ions magnetic moments relative to the light polarization. The splitting of the ground and excited states of the Nd3+ ion in the exchange field of the Fe sublattice were determined. It was revealed that the value of the exchange splitting (the exchange interaction) in the excited states did not correlate with the theoretical Landé factors. The Landé factors of the excited states were experimentally found. In general, the local magnetic properties in the vicinity of the excited ion depend substantially on its electron state. In particular: (1) in one of the excited states a weak ferromagnetic moment appears, (2) the changes of type of the local magnetic anisotropy take place in some excited states, and (3) in some excited states the energetically favorable orientation of the Nd3+ ion magnetic moment is opposite to that in the ground state. In some excited states the nonequivalent Nd3+ centers were found out.

  6. Energy dependence of the spin excitation anisotropy in uniaxial-strained BaFe1.9Ni0.1As2

    SciTech Connect

    Song, Yu; Lu, Xingye; Abernathy, Douglas L.; Tam, David W.; Niedziela, Jennifer L.; Tian, Wei; Si, Qimiao; Dai, Pengcheng; Luo, Huiqian

    2015-11-06

    In this study, we use inelastic neutron scattering to study the temperature and energy dependence of the spin excitation anisotropy in uniaxial-strained electron-doped iron pnictide BaFe1.9Ni0.1As2 near optimal superconductivity (Tc = 20K). Our work has been motivated by the observation of in-plane resistivity anisotropy in the paramagnetic tetragonal phase of electron-underdoped iron pnictides under uniaxial pressure, which has been attributed to a spin-driven Ising-nematic state or orbital ordering. Here we show that the spin excitation anisotropy, a signature of the spin-driven Ising-nematic phase, exists for energies below 60 meV in uniaxial-strained BaFe1.9Ni0.1As2. Since this energy scale is considerably larger than the energy splitting of the dxz and dyz bands of uniaxial-strained Ba(Fe1–xCox)2As2 near optimal superconductivity, spin Ising-nematic correlations are likely the driving force for the resistivity anisotropy and associated electronic nematic correlations.

  7. Temperature dependence of the magnetic excitations in Gd

    SciTech Connect

    Cable, J.W.; Nicklow, R.M.; Wakabayashi, N.

    1985-08-01

    Magnetic excitation spectra were measured for Gd in the and directions over the temperature range from 9 to 320/sup 0/K (T/sub c/ = 292.7/sup 0/K). Spin-wave-like modes are observed at T greater than or equal to T/sub c/. The critical wavevector for the appearance of these modes is proportional to the inverse correlation length.

  8. Magnetic Resonant Mode in the Low-Energy Spin-Excitation Spectrum of Superconducting Rb2Fe4Se5 Single Crystals

    NASA Astrophysics Data System (ADS)

    Park, J. T.; Friemel, G.; Li, Yuan; Kim, J.-H.; Tsurkan, V.; Deisenhofer, J.; Krug von Nidda, H.-A.; Loidl, A.; Ivanov, A.; Keimer, B.; Inosov, D. S.

    2011-10-01

    We have studied the low-energy spin-excitation spectrum of the single-crystalline Rb2Fe4Se5 superconductor (Tc=32K) by means of inelastic neutron scattering. In the superconducting state, we observe a magnetic resonant mode centered at an energy of ℏωres=14meV and at the (0.5 0.25 0.5) wave vector (unfolded Fe-sublattice notation), which differs from the ones characterizing magnetic resonant modes in other iron-based superconductors. Our finding suggests that the 245-iron selenides are unconventional superconductors with a sign-changing order parameter, in which bulk superconductivity coexists with the 5×5 magnetic superstructure. The estimated ratios of ℏωres/kBTc≈5.1±0.4 and ℏωres/2Δ≈0.7±0.1, where Δ is the superconducting gap, indicate moderate pairing strength in this compound, similar to that in optimally doped 1111 and 122 pnictides.

  9. Neutron Scattering Study of Magnetic Excitations in the Spin S= 1 One-Dimensional Heisenberg Antiferromagnet Y2BaNiO5

    NASA Astrophysics Data System (ADS)

    Sakaguchi, Takehiro; Kakurai, Kazuhisa; Yokoo, Tetsuya; Akimitsu, Jun

    1996-09-01

    Magnetic excitations of the ideal one-dimensional, spin S=1, antiferromagnet Y2BaNiO5 are studied by means of inelastic neutron scattering on single crystal sample. Our experimental results at low temperature indicate that Y2BaNiO5 can be regarded as the best isotropic Haldane-system sofar studied with the intrachain exchange energy J/k B=-24.1 meV and the averaged gap Δ(T=7 K)=8.5 meV. Y2BaNiO5 exhibits a good magnetic one-dimensionality with the inter-/intrachain exchange ratio of |J‧/J|≤10-4 and has only very small easy-axis and in-plane single ion anisotropy of |D/J|=0.03 and |E/J|˜0.01. In addition the temperature dependence of the Haldane gap Δ(T) and its damping rate was determined.

  10. Excitation spectrum of the attractive Hubbard model

    SciTech Connect

    Micnas, R.; Pedersen, M.H.; Schafroth, S.; Schneider, T.; Rodriguez-Nunez, J.J.; Beck, H.

    1995-12-01

    We study excitation-spectrum and normal-state properties of the two-dimensional attractive Hubbard model using the conserving, self-consistent {ital T}-matrix formalism in the intermediate coupling regime and at low electron concentration. Numerical results are presented for one-particle and two-particle excitation spectra, the one-particle momentum distribution, the chemical potential, and the static spin susceptibility. For a coupling strength of {ital U}/{ital t}=4.0, the one-particle spectral function, {ital A}(k,{omega}), shows two peaks of different weights. One peak can be associated with pair formation, whereas the other corresponds to renormalized quasiparticle excitation. It turns out that the two-band feature is reasonably well described by an ansatz for {ital A}(k,{omega}), which satisfies the first four frequency moments.

  11. Massively parallel implementations of coupled-cluster methods for electron spin resonance spectra. I. Isotropic hyperfine coupling tensors in large radicals

    SciTech Connect

    Verma, Prakash; Morales, Jorge A.; Perera, Ajith

    2013-11-07

    experimental ESR spectra, to interpret spin-density distributions, and to characterize and identify radical species is illustrated with our results from large organic radicals. Those include species relevant for organic chemistry, petroleum industry, and biochemistry, such as the cyclo-hexyl, 1-adamatyl, and Zn-porphycene anion radicals, inter alia.

  12. Massively parallel implementations of coupled-cluster methods for electron spin resonance spectra. I. Isotropic hyperfine coupling tensors in large radicals.

    PubMed

    Verma, Prakash; Perera, Ajith; Morales, Jorge A

    2013-11-01

    Coupled cluster (CC) methods provide highly accurate predictions of molecular properties, but their high computational cost has precluded their routine application to large systems. Fortunately, recent computational developments in the ACES III program by the Bartlett group [the OED∕ERD atomic integral package, the super instruction processor, and the super instruction architecture language] permit overcoming that limitation by providing a framework for massively parallel CC implementations. In that scheme, we are further extending those parallel CC efforts to systematically predict the three main electron spin resonance (ESR) tensors (A-, g-, and D-tensors) to be reported in a series of papers. In this paper inaugurating that series, we report our new ACES III parallel capabilities that calculate isotropic hyperfine coupling constants in 38 neutral, cationic, and anionic radicals that include the (11)B, (17)O, (9)Be, (19)F, (1)H, (13)C, (35)Cl, (33)S,(14)N, (31)P, and (67)Zn nuclei. Present parallel calculations are conducted at the Hartree-Fock (HF), second-order many-body perturbation theory [MBPT(2)], CC singles and doubles (CCSD), and CCSD with perturbative triples [CCSD(T)] levels using Roos augmented double- and triple-zeta atomic natural orbitals basis sets. HF results consistently overestimate isotropic hyperfine coupling constants. However, inclusion of electron correlation effects in the simplest way via MBPT(2) provides significant improvements in the predictions, but not without occasional failures. In contrast, CCSD results are consistently in very good agreement with experimental results. Inclusion of perturbative triples to CCSD via CCSD(T) leads to small improvements in the predictions, which might not compensate for the extra computational effort at a non-iterative N(7)-scaling in CCSD(T). The importance of these accurate computations of isotropic hyperfine coupling constants to elucidate experimental ESR spectra, to interpret spin

  13. Massively parallel implementations of coupled-cluster methods for electron spin resonance spectra. I. Isotropic hyperfine coupling tensors in large radicals

    NASA Astrophysics Data System (ADS)

    Verma, Prakash; Perera, Ajith; Morales, Jorge A.

    2013-11-01

    Coupled cluster (CC) methods provide highly accurate predictions of molecular properties, but their high computational cost has precluded their routine application to large systems. Fortunately, recent computational developments in the ACES III program by the Bartlett group [the OED/ERD atomic integral package, the super instruction processor, and the super instruction architecture language] permit overcoming that limitation by providing a framework for massively parallel CC implementations. In that scheme, we are further extending those parallel CC efforts to systematically predict the three main electron spin resonance (ESR) tensors (A-, g-, and D-tensors) to be reported in a series of papers. In this paper inaugurating that series, we report our new ACES III parallel capabilities that calculate isotropic hyperfine coupling constants in 38 neutral, cationic, and anionic radicals that include the 11B, 17O, 9Be, 19F, 1H, 13C, 35Cl, 33S,14N, 31P, and 67Zn nuclei. Present parallel calculations are conducted at the Hartree-Fock (HF), second-order many-body perturbation theory [MBPT(2)], CC singles and doubles (CCSD), and CCSD with perturbative triples [CCSD(T)] levels using Roos augmented double- and triple-zeta atomic natural orbitals basis sets. HF results consistently overestimate isotropic hyperfine coupling constants. However, inclusion of electron correlation effects in the simplest way via MBPT(2) provides significant improvements in the predictions, but not without occasional failures. In contrast, CCSD results are consistently in very good agreement with experimental results. Inclusion of perturbative triples to CCSD via CCSD(T) leads to small improvements in the predictions, which might not compensate for the extra computational effort at a non-iterative N7-scaling in CCSD(T). The importance of these accurate computations of isotropic hyperfine coupling constants to elucidate experimental ESR spectra, to interpret spin-density distributions, and to

  14. Valence excitation energies of alkenes, carbonyl compounds, and azabenzenes by time-dependent density functional theory: Linear response of the ground state compared to collinear and noncollinear spin-flip TDDFT with the Tamm-Dancoff approximation

    NASA Astrophysics Data System (ADS)

    Isegawa, Miho; Truhlar, Donald G.

    2013-04-01

    Time-dependent density functional theory (TDDFT) holds great promise for studying photochemistry because of its affordable cost for large systems and for repeated calculations as required for direct dynamics. The chief obstacle is uncertain accuracy. There have been many validation studies, but there are also many formulations, and there have been few studies where several formulations were applied systematically to the same problems. Another issue, when TDDFT is applied with only a single exchange-correlation functional, is that errors in the functional may mask successes or failures of the formulation. Here, to try to sort out some of the issues, we apply eight formulations of adiabatic TDDFT to the first valence excitations of ten molecules with 18 density functionals of diverse types. The formulations examined are linear response from the ground state (LR-TDDFT), linear response from the ground state with the Tamm-Dancoff approximation (TDDFT-TDA), the original collinear spin-flip approximation with the Tamm-Dancoff (TD) approximation (SF1-TDDFT-TDA), the original noncollinear spin-flip approximation with the TDA approximation (SF1-NC-TDDFT-TDA), combined self-consistent-field (SCF) and collinear spin-flip calculations in the original spin-projected form (SF2-TDDFT-TDA) or non-spin-projected (NSF2-TDDFT-TDA), and combined SCF and noncollinear spin-flip calculations (SF2-NC-TDDFT-TDA and NSF2-NC-TDDFT-TDA). Comparing LR-TDDFT to TDDFT-TDA, we observed that the excitation energy is raised by the TDA; this brings the excitation energies underestimated by full linear response closer to experiment, but sometimes it makes the results worse. For ethylene and butadiene, the excitation energies are underestimated by LR-TDDFT, and the error becomes smaller making the TDA. Neither SF1-TDDFT-TDA nor SF2-TDDFT-TDA provides a lower mean unsigned error than LR-TDDFT or TDDFT-TDA. The comparison between collinear and noncollinear kernels shows that the noncollinear kernel

  15. Neutron-scattering measurements of spin excitations in LaFeAsO and Ba(Fe0.953Co0.047)2As2: Evidence for a sharp enhancement of spin fluctuations by nematic order [Sharp enhancement of spin fluctuations by nematic order in iron pnictides

    DOE PAGES

    Zhang, Qiang; Fernandes, Rafael M.; Lamsal, Jagat; Yan, Jiaqiang; Chi, Songxue; Tucker, Gregory S.; Pratt, Daniel K.; Lynn, Jeffrey W.; McCallum, R. W.; Canfield, Paul C.; et al

    2015-02-04

    Inelastic neutron scattering is employed to investigate the impact of electronic nematic order on the magnetic spectra of LaFeAsO and Ba(Fe0.953Co0.047)2As2. These materials are ideal to study the paramagnetic-nematic state, since the nematic order, signaled by the tetragonal-to-orthorhombic transition at TS, sets in well above the stripe antiferromagnetic ordering at TN. We find that the temperature-dependent dynamic susceptibility displays an anomaly at TS followed by a sharp enhancement in the spin-spin correlation length, revealing a strong feedback effect of nematic order on the low-energy magnetic spectrum. As a result, our findings can be consistently described by a model that attributesmore » the structural or nematic transition to magnetic fluctuations, and unveils the key role played by nematic order in promoting the long-range stripe antiferromagnetic order in iron pnictides.« less

  16. Experimental Overview of the Excited Baryon Program

    NASA Astrophysics Data System (ADS)

    Crede, Volker

    2011-05-01

    High-energy electrons and photons are a remarkably clean probe of hadronic matter, essentially providing a microscope for examining atomic nuclei and the strong nuclear force. For more than a decade, laboratories worldwide have accumulated data for such investigations, resulting in a number of surprising discoveries and contributing to our understanding of the nucleon, its underlying quark structure, and the dynamics of the strong interaction. One notable discovery has been the unexpected Q2 variation of the ratio of the proton elastic form-factors GEp/GMp, which suggests an important contribution from quark orbital angular momentum to the spin of the nucleon. Moreover, the spectrum of excited hadrons can serve as an excellent probe of Quantum Chromodynamics (QCD), the fundamental theory of strong interactions. Since nucleons are complex systems of confined quarks, they exhibit the characteristic spectra of excited states. Highly excited nucleon states are sensitive to details of quark confinement which is poorly understood within QCD. The current effort at facilities worldwide studying the systematics of hadron spectra is to utilize highly-polarized frozen-spin (butanol) and deuterium targets in combination with polarized photon beams. These are important steps toward complete experiments that allow us to unambiguously determine the scattering amplitude in the underlying reactions and to identify resonance contributions.

  17. Haldane-Hubbard Mott Insulator: From Tetrahedral Spin Crystal to Chiral Spin Liquid.

    PubMed

    Hickey, Ciarán; Cincio, Lukasz; Papić, Zlatko; Paramekanti, Arun

    2016-04-01

    Motivated by cold atom experiments on Chern insulators, we study the honeycomb lattice Haldane-Hubbard Mott insulator of spin-1/2 fermions using exact diagonalization and density matrix renormalization group methods. We show that this model exhibits various chiral magnetic orders including a wide regime of triple-Q tetrahedral order. Incorporating third-neighbor hopping frustrates and ultimately melts this tetrahedral spin crystal. From analyzing the low energy spectrum, many-body Chern numbers, entanglement spectra, and modular matrices, we identify the molten state as a chiral spin liquid (CSL) with gapped semion excitations. We formulate and study the Chern-Simons-Higgs field theory of the exotic CSL-to-tetrahedral spin crystallization transition.

  18. Haldane-Hubbard Mott Insulator: From Tetrahedral Spin Crystal to Chiral Spin Liquid

    NASA Astrophysics Data System (ADS)

    Hickey, Ciarán; Cincio, Lukasz; Papić, Zlatko; Paramekanti, Arun

    2016-04-01

    Motivated by cold atom experiments on Chern insulators, we study the honeycomb lattice Haldane-Hubbard Mott insulator of spin-1 /2 fermions using exact diagonalization and density matrix renormalization group methods. We show that this model exhibits various chiral magnetic orders including a wide regime of triple-Q tetrahedral order. Incorporating third-neighbor hopping frustrates and ultimately melts this tetrahedral spin crystal. From analyzing the low energy spectrum, many-body Chern numbers, entanglement spectra, and modular matrices, we identify the molten state as a chiral spin liquid (CSL) with gapped semion excitations. We formulate and study the Chern-Simons-Higgs field theory of the exotic CSL-to-tetrahedral spin crystallization transition.

  19. Haldane-Hubbard Mott Insulator: From Tetrahedral Spin Crystal to Chiral Spin Liquid.

    PubMed

    Hickey, Ciarán; Cincio, Lukasz; Papić, Zlatko; Paramekanti, Arun

    2016-04-01

    Motivated by cold atom experiments on Chern insulators, we study the honeycomb lattice Haldane-Hubbard Mott insulator of spin-1/2 fermions using exact diagonalization and density matrix renormalization group methods. We show that this model exhibits various chiral magnetic orders including a wide regime of triple-Q tetrahedral order. Incorporating third-neighbor hopping frustrates and ultimately melts this tetrahedral spin crystal. From analyzing the low energy spectrum, many-body Chern numbers, entanglement spectra, and modular matrices, we identify the molten state as a chiral spin liquid (CSL) with gapped semion excitations. We formulate and study the Chern-Simons-Higgs field theory of the exotic CSL-to-tetrahedral spin crystallization transition. PMID:27082001

  20. Spin Chain in Magnetic Field: Limitations of the Large-N Mean-Field Theory

    DOE PAGES

    Wohlfeld, K.; Chen, Cheng-Chien; van Veenendaal, M.; Devereaux, T. P.

    2015-02-01

    Motivated by the recent success in describing the spin and orbital spectrum of a spin-orbital chain using a large-N mean-field approximation [Phys. Rev. B 91, 165102 (2015)], we apply the same formalism to the case of a spin chain in the external magnetic field. It occurs that in this case, which corresponds to N=2 in the approximation, the large-N mean-field theory cannot qualitatively reproduce the spin excitation spectra at high magnetic fields, which polarize more than 50% of the spins in the magnetic ground state. This, rather counterintuitively, shows that the physics of a spin chain can under some circumstancesmore » be regarded as more complex than the physics of a spin-orbital chain.« less