Spin crossover in liquid (Mg,Fe)O at extreme conditions

NASA Astrophysics Data System (ADS)

Holmström, E.; Stixrude, L.

2016-05-01

We use first-principles free-energy calculations to predict a pressure-induced spin crossover in the liquid planetary material (Mg,Fe)O, whereby the magnetic moments of Fe ions vanish gradually over a range of hundreds of GPa. Because electronic entropy strongly favors the nonmagnetic low-spin state of Fe, the crossover has a negative effective Clapeyron slope, in stark contrast to the crystalline counterpart of this transition-metal oxide. Diffusivity of liquid (Mg,Fe)O is similar to that of MgO, displaying a weak dependence on element and spin state. Fe-O and Mg-O coordination increases from approximately 4 to 7 as pressure goes from 0 to 200 GPa. We find partitioning of Fe to induce a density inversion between the crystal and melt, implying separation of a basal magma ocean from a surficial one in the early Earth. The spin crossover induces an anomaly into the density contrast, and the oppositely signed Clapeyron slopes for the crossover in the liquid and crystalline phases imply that the solid-liquid transition induces a spin transition in (Mg,Fe)O.

Spin crossover in ferropericlase and velocity heterogeneities in the lower mantle

NASA Astrophysics Data System (ADS)

Wu, Z.; Wentzcovitch, R. M.

2014-12-01

Ferropericlase (Fp) is believed to be the second most abundant phase in the lower mantle. Since the discovery of the high spin (HS) to low spin (LS) crossover in iron in Fp [1], this phenomenon has been investigated extensively experimentally and theoretically. This is a broad and smooth crossover that takes place throughout most of the lower mantle and does not produce an obvious signature in radial velocity or density profiles [2]. Therefore, the spin transition has been generally considered to be invisible to seismic waves. This study, however, shows that it can produce a peculiar effect on lateral velocity heterogeneities at certain depths[3]. Deciphering the origin of seismic velocity heterogeneities in the mantle is crucial to understanding internal structures and processes at work in the Earth. The spin crossover in iron introduces unfamiliar effects on seismic velocities. First principles calculations indicate that anti-correlation between shear velocity (VS) and bulk sound velocity (Vφ) in the mantle, usually interpreted as compositional heterogeneity, can also be produced in homogeneous aggregates containing Fp. The spin crossover also suppresses thermally induced heterogeneity in VP but not in VS. This effect is observed in tomographic models at conditions where the spin crossover in Fp is expected in the lower mantle. In addition, the one-of-a-kind signature of this spin crossover in the RS/P () heterogeneity ratio might be a useful "fingerprint" to detect the presence of Fp in the lower mantle. [1] Badro J, et al. (2003) Science 300(5620):789-791. [2] Wu Z, Justo J. F., and Wentzcovitch R. M., (2013). Phys. Rev. Lett. 110. 228501-5 [3]Wu Z., and Wentzcovitch R. M., (2014) Proc Natl Acad Sci USA. www.pnas.org/cgi/doi/10.1073/pnas.1322427111

Single to Multiquasiparticle Excitations in the Itinerant Helical Magnet CeRhIn 5

DOE PAGES

Stock, C.; Rodriguez-Rivera, J. A.; Schmalzl, K.; ...

2015-06-19

Neutron scattering is used to measure the quantum spin fluctuations in CeRhIn 5 - the parent material of the eXIn 5 superconducting series. Out-of-plane spin fluctuations are gapped and localized in momentum, similar to the spin excitons in CeCoIn5. The in-plane fluctuations consist of sharp spin-wave excitations parameterized by a nearest neighbor exchange J RKKY =0.88 ± 0.05 meV that crossover to a temporally and spatially broad multiparticle spectrum with energies of ~ 2 × J RKKY . This continuum represents composite fluctuations that illustrate the breakdown of single magnons originating from the delicate energy balance between localized 4f andmore » itinerant behavior in a heavy metal. The experiment therefore shows how quasiparticle behavior is changed by the close proximity of quantum criticality.« less

Compression of a multiphase mantle assemblage: Effects of undesirable stress and stress annealing on the iron spin state crossover in ferropericlase: Stresses and HS-LS Crossover in (Mg,Fe)O

DOE PAGES

Glazyrin, Konstantin; Miyajima, Nobuyoshi; Smith, Jesse S.; ...

2016-05-30

Using synchrotron-based X-ray diffraction, we explore characteristic signatures for nonhydrostaticstresses and their effect on the spin state crossover of ferrous iron in (Mg, Fe)O ferropericlase (Fp) uponcompression in a two-phase mixture which includes an Al- and Fe-bearing bridgmanite (Bm). Here, we observe aninfluence of nonhydrostatic stresses on the spin state crossover starting pressure and width. The undesirablestresses discussed here include uniaxial deviatoric stress evolving in the diamond anvil cell and effects ofintergrain interaction. And while the former leads to a pressure overestimation, the latter one lowers the pressure ofthe onset for the high-spin to low-spin electronic transition in Fe 2+more » in ferropericlase (Mg, Fe)O with respect tohydrostatic conditions.« less

Spin state switching of metal complexes by visible light or hard X-rays.

PubMed

Unruh, Daniel; Homenya, Patrick; Kumar, Manish; Sindelar, Ralf; Garcia, Yann; Renz, Franz

2016-09-28

Electromagnetic stimuli of spin crossover compounds restricted to UV-vis light irradiation for many years could be recently extended to X-ray excitation. This review covers a large variety of light-induced effects, as well as recent analogues stimulated by X-ray irradiation which have not yet been reviewed. The focus is also on multistable multinuclear spin crossover compounds which are the subject of lively discussions within the spin crossover community. Their spin transition often occurs incompletely and with different switching mechanisms. In this review, we recall a predicted sequential switching induced thermally as well as a concerted stimulation mechanism by light irradiation for these interesting multifunctional materials.

Coulomb Correlations Intertwined with Spin and Orbital Excitations in LaCoO_{3}.

PubMed

Tomiyasu, K; Okamoto, J; Huang, H Y; Chen, Z Y; Sinaga, E P; Wu, W B; Chu, Y Y; Singh, A; Wang, R-P; de Groot, F M F; Chainani, A; Ishihara, S; Chen, C T; Huang, D J

2017-11-10

We carried out temperature-dependent (20-550 K) measurements of resonant inelastic x-ray scattering on LaCoO_{3} to investigate the evolution of its electronic structure across the spin-state crossover. In combination with charge-transfer multiplet calculations, we accurately quantified the renomalized crystal-field excitation energies and spin-state populations. We show that the screening of the effective on-site Coulomb interaction of 3d electrons is orbital selective and coupled to the spin-state crossover in LaCoO_{3}. The results establish that the gradual spin-state crossover is associated with a relative change of Coulomb energy versus bandwidth, leading to a Mott-type insulator-to-metal transition.

Matrix-assisted relaxation in Fe(phen)2(NCS)2 spin-crossover microparticles, experimental and theoretical investigations

NASA Astrophysics Data System (ADS)

Enachescu, Cristian; Tanasa, Radu; Stancu, Alexandru; Tissot, Antoine; Laisney, Jérôme; Boillot, Marie-Laure

2016-07-01

In this study, we present the influence of the embedding matrix on the relaxation of Fe(phen)2(NCS)2 (phen = 1,10-phenanthroline) spin-transition microparticles as revealed by experiments and provide an explanation within the framework of an elastic model based on a Monte-Carlo method. Experiments show that the shape of the high-spin → low-spin relaxation curves is drastically changed when the particles are dispersed in glycerol. This effect was considered in the model by means of interactions between the microparticles and the matrix. A faster start of the relaxation for microparticles embedded in glycerol is due to an initial positive local pressure acting on the edge spin-crossover molecules from the matrix side. This local pressure diminishes and eventually becomes negative during relaxation, as an effect of the decrease of the volume of spin-crossover microparticles from high-spin to low-spin.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Perron, Justin K., E-mail: jperron@csusm.edu; Joint Quantum Institute, National Institute of Standards and Technology, Gaithersburg, Maryland 20899; National Institute of Standards and Technology, Gaithersburg, Maryland 20899

Pauli-spin blockade (PSB) is a transport phenomenon in double quantum dots that allows for a type of spin to charge conversion often used to probe fundamental physics such as spin relaxation and singlet-triplet coupling. In this paper, we theoretically explore Pauli-spin blockade as a function of magnetic field B applied parallel to the substrate. In the well-studied low magnetic field regime, where PSB occurs in the forward (1, 1) → (0, 2) tunneling direction, we highlight some aspects of PSB that are not discussed in detail in existing literature, including the change in size of both bias triangles measured inmore » the forward and reverse biasing directions as a function of B. At higher fields, we predict a crossover to “reverse PSB” in which current is blockaded in the reverse direction due to the occupation of a spin singlet as opposed to the traditional triplet blockade that occurs at low fields. The onset of reverse PSB coincides with the development of a tail like feature in the measured bias triangles and occurs when the Zeeman energy of the polarized triplet equals the exchange energy in the (0, 2) charge configuration. In Si quantum dots, these fields are experimentally accessible; thus, this work suggests a way to observe a crossover in magnetic field to qualitatively different behavior.« less

Virtual walks in spin space: A study in a family of two-parameter models

NASA Astrophysics Data System (ADS)

Mullick, Pratik; Sen, Parongama

2018-05-01

We investigate the dynamics of classical spins mapped as walkers in a virtual "spin" space using a generalized two-parameter family of spin models characterized by parameters y and z [de Oliveira et al., J. Phys. A 26, 2317 (1993), 10.1088/0305-4470/26/10/006]. The behavior of S (x ,t ) , the probability that the walker is at position x at time t , is studied in detail. In general S (x ,t ) ˜t-αf (x /tα) with α ≃1 or 0.5 at large times depending on the parameters. In particular, S (x ,t ) for the point y =1 ,z =0.5 corresponding to the Voter model shows a crossover in time; associated with this crossover, two timescales can be defined which vary with the system size L as L2logL . We also show that as the Voter model point is approached from the disordered regions along different directions, the width of the Gaussian distribution S (x ,t ) diverges in a power law manner with different exponents. For the majority Voter case, the results indicate that the the virtual walk can detect the phase transition perhaps more efficiently compared to other nonequilibrium methods.

Spin Crossover in Solid and Liquid (Mg,Fe)O at Extreme Conditions

NASA Astrophysics Data System (ADS)

Stixrude, L. P.; Holmstrom, E.

2016-12-01

Ferropericlase, (Mg,Fe)O, is a major constituent of the Earth's lowermantle (24-136 GPa). Understanding the properties of this component is importantnot only in the solid state, but also in the molten state, as theplanet almost certainly hosted an extensive magma ocean initiallyWith increasing pressure, the Fe ions in the material begin to collapse from a magnetic to a nonmagnetic spin state. This crossover affects thermodynamic, transport, and electrical properties.Using first-principles molecular dynamics simulations,thermodynamic integration, and adiabatic switching, we present a phasediagram of the spin crossover In both solid and liquid, we find a broad pressure range of coexisting magnetic and non-magnetic ions due to the favorable enthalpy of mixing of the two. In the solid increasingtemperature favors the high spin state, while in the liquid the oppositeoccurs, due to the higher electronic entropy of the low spin state. Becausethe physics of the crossover differ in solid and liquid, melting produces a large change in spin state that may affect the buoyancy of crystals freezing from the magma ocean in the earliest Earth.

Thermoelectronic transport through spin-crossover single molecule Fe[(H2Bpz2)2bipy

NASA Astrophysics Data System (ADS)

Liu, N.; Zhu, L.; Yao, K. L.

2018-04-01

By means of density functional theory combined with the method of Keldysh nonequilibrium Green’s function, the thermal transport properties of high- and low-spin states of mononuclear FeII molecules with spin-crossover characteristics are studied. It is found that the high-spin molecular junction has a larger current than the low-spin one, producing thermally-induced switching effect. Furthermore, for high spin state molecule, the spin-up thermo-current is strongly blocked, thus achieving a pure thermo spin current. The enhanced Seebeck coefficient and the figure of merit value of high-spin state indicate that it is an ideal candidate for thermoelectric applications.

Electric-field-induced spin switch of endohedral dodecahedrane heterodimers H@C20Hn-C20Hn@M (M= Cu, Ag and Au, n = 15, 18, and 19): a theoretical study.

PubMed

Hou, Jianhua; Yang, Zhixiong; Li, Zhiru; Chai, Haoyu; Zhao, Ruiqi

2017-08-01

We designed nine endohedral dodecahedrane heterodimers H@C 20 H n -C 20 H n @M (M = Cu, Ag, and Au, n = 15, 18, and 19) that may act as single-molecule spin switches, and we predicted theoretically that the ground states of the dimmers shift from low-spin states (S = 0) to the high-spin states (S = 1) under an external electric field applied parallel or perpendicular to the molecular symmetry axes, consisting well with the analyses of Stark effect. Molecular orbitals analyses provide an intuitive insight into the spin crossover behavior. This study expands the application of endohedral chemistry and provides new molecules for designing single-molecule spin switch.

Increasing spin crossover cooperativity in 2D Hofmann-type materials with guest molecule removal

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zenere, Katrina A.; Duyker, Samuel G.; Trzop, Elzbieta

Ambient temperature spin crossover with wide hysteresis has been achieved in 2D Hofmann-type materials, where removal of guest molecules optimises ligand–ligand interactions, resulting in increased cooperativity.

Increasing spin crossover cooperativity in 2D Hofmann-type materials with guest molecule removal

DOE PAGES

Zenere, Katrina A.; Duyker, Samuel G.; Trzop, Elzbieta; ...

2018-01-01

Ambient temperature spin crossover with wide hysteresis has been achieved in 2D Hofmann-type materials, where removal of guest molecules optimises ligand–ligand interactions, resulting in increased cooperativity.

Matrix-assisted relaxation in Fe(phen){sub 2}(NCS){sub 2} spin-crossover microparticles, experimental and theoretical investigations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Enachescu, Cristian, E-mail: cristian.enachescu@uaic.ro; Stancu, Alexandru; Tanasa, Radu

2016-07-18

In this study, we present the influence of the embedding matrix on the relaxation of Fe(phen){sub 2}(NCS){sub 2} (phen = 1,10-phenanthroline) spin-transition microparticles as revealed by experiments and provide an explanation within the framework of an elastic model based on a Monte-Carlo method. Experiments show that the shape of the high-spin → low-spin relaxation curves is drastically changed when the particles are dispersed in glycerol. This effect was considered in the model by means of interactions between the microparticles and the matrix. A faster start of the relaxation for microparticles embedded in glycerol is due to an initial positive local pressure actingmore » on the edge spin-crossover molecules from the matrix side. This local pressure diminishes and eventually becomes negative during relaxation, as an effect of the decrease of the volume of spin-crossover microparticles from high-spin to low-spin.« less

Spin Crossover and the Magnetic P- T Phase Diagram of Hematite at High Hydrostatic Pressures and Cryogenic Temperatures

NASA Astrophysics Data System (ADS)

Gavriliuk, A. G.; Struzhkin, V. V.; Mironovich, A. A.; Lyubutin, I. S.; Troyan, I. A.; Chow, P.; Xiao, Y.

2018-02-01

The magnetic properties of the α-Fe2O3 hematite at a high hydrostatic pressure have been studied by synchrotron Mössbauer spectroscopy (nuclear forward scattering (NFS)) on iron nuclei. Time-domain NFS spectra of hematite have been measured in a diamond anvil cell in the pressure range of 0-72 GPa and the temperature range of 36-300 K in order to study the magnetic properties at a phase transition near a critical pressure of 50 GPa. In addition, Raman spectra at room temperature have been studied in the pressure range of 0-77 GPa. Neon has been used as a pressure-transmitting medium. The appearance of an intermediate electronic state has been revealed at a pressure of 48 GPa. This state is probably related to the spin crossover in Fe3+ ions at their transition from the high-spin state (HS, S = 5/2) to a low-spin one (LS, S = 1/2). It has been found that the transient pressure range of the HS-LS crossover is extended from 48 to 55 GPa and is almost independent of the temperature. This surprising result differs fundamentally from other cases of the spin crossover in Fe3+ ions observed in other crystals based on iron oxides. The transition region of spin crossover appears because of thermal fluctuations between HS and LS states in the critical pressure range and is significantly narrowed at cooling because of the suppression of thermal excitations. The magnetic P- T phase diagram of α-Fe2O3 at high pressures and low temperatures in the spin crossover region has been constructed according to the results of measurements.

Influence of the iron spin crossover in ferropericlase on the lower mantle geotherm

NASA Astrophysics Data System (ADS)

Valencia-Cardona, Juan J.; Shukla, Gaurav; Wu, Zhongqing; Houser, Christine; Yuen, David A.; Wentzcovitch, Renata M.

2017-05-01

The iron spin crossover in ferropericlase introduces anomalies in its thermodynamics and thermoelastic properties. Here we investigate how these anomalies can affect the lower mantle geotherm using thermodynamics properties from ab initio calculations. The anomalous effect is examined in mantle aggregates consisting of mixtures of bridgmanite, ferropericlase, and CaSiO3 perovskite, with different Mg/Si ratios varying from harzburgitic to perovskitic (Mg/Si ˜ 1.5 to 0.8). We find that the anomalies introduced by the spin crossover increase the isentropic gradient and thus the geotherm proportionally to the amount of ferropericlase. The geotherms can be as much as ˜200 K hotter than the conventional adiabatic geotherm at deep lower mantle conditions. Aggregate elastic moduli and seismic velocities are also sensitive to the spin crossover and the geotherm, which impacts analyses of lower mantle velocities and composition.

Reverse spin-crossover and high-pressure kinetics of the heme iron center relevant for the operation of heme proteins under deep-sea conditions.

PubMed

Troeppner, Oliver; Lippert, Rainer; Shubina, Tatyana E; Zahl, Achim; Jux, Norbert; Ivanović-Burmazović, Ivana

2014-10-20

By design of a heme model complex with a binding pocket of appropriate size and flexibility, and by elucidating its kinetics and thermodynamics under elevated pressures, some of the pressure effects are demonstrated relevant for operation of heme-proteins under deep-sea conditions. Opposite from classical paradigms of the spin-crossover and reaction kinetics, a pressure increase can cause deceleration of the small-molecule binding to the vacant coordination site of the heme-center in a confined space and stabilize a high-spin state of its Fe center. This reverse high-pressure behavior can be achieved only if the volume changes related to the conformational transformation of the cavity can offset the volume changes caused by the substrate binding. It is speculated that based on these criteria nature could make a selection of structures of heme pockets that assist in reducing metabolic activity and enzymatic side reactions under extreme pressure conditions. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Pressure dependence of coherence-incoherence crossover behavior in KFe2As2 observed by resistivity and 75As-NMR/NQR

NASA Astrophysics Data System (ADS)

Wiecki, P.; Taufour, V.; Chung, D. Y.; Kanatzidis, M. G.; Bud'ko, S. L.; Canfield, P. C.; Furukawa, Y.

2018-02-01

We present the results of 75As nuclear magnetic resonance (NMR), nuclear quadrupole resonance (NQR), and resistivity measurements in KFe2As2 under pressure (p ). The temperature dependence of the NMR shift, nuclear spin-lattice relaxation time (T1), and resistivity show a crossover between a high-temperature incoherent, local-moment behavior and a low-temperature coherent behavior at a crossover temperature (T*). T* is found to increase monotonically with pressure, consistent with increasing hybridization between localized 3 d orbital-derived bands with the itinerant electron bands. No anomaly in T* is seen at the critical pressure pc=1.8 GPa where a change of slope of the superconducting (SC) transition temperature Tc(p ) has been observed. In contrast, Tc(p ) seems to correlate with antiferromagnetic spin fluctuations in the normal state as measured by the NQR 1 /T1 data, although such a correlation cannot be seen in the replacement effects of A in the A Fe2As2 (A =K , Rb, Cs) family. In the superconducting state, two T1 components are observed at low temperatures, suggesting the existence of two distinct local electronic environments. The temperature dependence of the short T1 s indicates a nearly gapless state below Tc. On the other hand, the temperature dependence of the long component 1 /T1 L implies a large reduction in the density of states at the Fermi level due to the SC gap formation. These results suggest a real-space modulation of the local SC gap structure in KFe2As2 under pressure.

Universal monopole scaling near transitions from the Coulomb phase.

PubMed

Powell, Stephen

2012-08-10

Certain frustrated systems, including spin ice and dimer models, exhibit a Coulomb phase at low temperatures, with power-law correlations and fractionalized monopole excitations. Transitions out of this phase, at which the effective gauge theory becomes confining, provide examples of unconventional criticality. This Letter studies the behavior at nonzero monopole density near such transitions, using scaling theory to arrive at universal expressions for the crossover phenomena. For a particular transition in spin ice, quantitative predictions are made by mapping to the XY model and confirmed using Monte Carlo simulations.

Spin-crossover in [Fe(3-bpp)2][BF4]2 in different solvents--a dramatic stabilisation of the low-spin state in water.

PubMed

Barrett, Simon A; Kilner, Colin A; Halcrow, Malcolm A

2011-12-07

The temperature of spin-crossover in [Fe(3-bpp)(2)][BF(4)](2) (3-bpp = 2,6-di{pyrazol-3-yl}pyridine) tends to increase in associating solvents. In particular, T(½) shifts to 60-70 K higher temperature in water compared to organic solvents.

Guest Programmable Multistep Spin Crossover in a Porous 2-D Hofmann-Type Material.

PubMed

Murphy, Michael J; Zenere, Katrina A; Ragon, Florence; Southon, Peter D; Kepert, Cameron J; Neville, Suzanne M

2017-01-25

The spin crossover (SCO) phenomenon defines an elegant class of switchable materials that can show cooperative transitions when long-range elastic interactions are present. Such materials can show multistepped transitions, targeted both fundamentally and for expanded data storage applications, when antagonistic interactions (i.e., competing ferro- and antiferro-elastic interactions) drive concerted lattice distortions. To this end, a new SCO framework scaffold, [Fe II (bztrz) 2 (Pd II (CN) 4 )]·n(guest) (bztrz = (E)-1-phenyl-N-(1,2,4-triazol-4-yl)methanimine, 1·n(guest)), has been prepared that supports a variety of antagonistic solid state interactions alongside a distinct dual guest pore system. In this 2-D Hofmann-type material we find that inbuilt competition between ferro- and antiferro-elastic interactions provides a SCO behavior that is intrinsically frustrated. This frustration is harnessed by guest exchange to yield a very broad array of spin transition characters in the one framework lattice (one- (1·(H 2 O,EtOH)), two- (1·3H 2 O) and three-stepped (1·∼2H 2 O) transitions and SCO-deactivation (1)). This variety of behaviors illustrates that the degree of elastic frustration can be manipulated by molecular guests, which suggests that the structural features that contribute to multistep switching may be more subtle than previously anticipated.

Ultrastable light sources in the crossover from superradiance to lasing

NASA Astrophysics Data System (ADS)

Xu, Minghui; Tieri, David; Holland, Murray

2013-05-01

We theoretically investigate the crossover from steady-state superradiance to optical lasing. An exact solution of the quantum master equation is difficult to obtain due to the exponential scaling of the Hilbert space dimension with system size. However, since Lindblad operators in the master equation are invariant under SU(4) transformations, we are able to reduce the exponential scaling of the problem to cubic by expanding the density matrix in terms of an SU(4) basis. In this way, we obtain exact quantum solutions of the superradiance-laser crossover. We use this theory to investigate the potential for ultrastable lasers in the millihertz linewidth regime, and find the behavior of important observables, such as intensity, linewidth, spin-correlation, and entanglement. This work was supported by the DARPA QUASAR program and NSF.

Unambiguously identifying spin states of transition-metal ions in the Earth (Invited)

NASA Astrophysics Data System (ADS)

Hsu, H.

2010-12-01

The spin state of a transition-metal ion in crystalline solids, defined by the number of unpaired electrons in the ion’s incomplete 3d shell, may vary with many factors, such as temperature, pressure, strain, and the local atomic configuration, to name a few. Such a phenomenon, known as spin-state crossover, plays a crucial role in spintronic materials. Recently, the pressure-induced spin-state crossover in iron-bearing minerals has been recognized to affect the minerals’ structural and elastic properties. However, the detailed mechanism of such crossover in iron-bearing magnesium silicate perovskite, the most abundant mineral in the Earth, remains unclear. A significant part of this confusion arises from the difficulty in reliably extracting the spin state from experiments. For the same reason, the thermally-induced spin-state crossover in lanthanum cobaltite (LaCoO3) has been controversial for more than four decades. In this talk, I will discuss how first-principle calculations can help clarifying these long-standing controversies. In addition to the total energy, equation of state, and elastic properties of each spin state, first-principle calculations also predict the electric field gradient (EFG) at the nucleus of each transition-metal ion. Our calculations showed that the nuclear EFG, a quantity that can be measured via Mössbauer or nuclear magnetic resonance (NMR) spectroscopy, depends primarily on the spin state, irrespective of the concentration or configuration of transition-metal ions. Such robustness makes EFG a unique fingerprint to identify the spin state. The combination of first-principle calculations and Mössbauer/NMR spectroscopy can therefore be a reliable and efficient approach in tackling spin-state crossover problems in the Earth. This work was primarily supported by the MRSEC Program of NSF under Awards Number DMR-0212302 and DMR-0819885, and partially supported by NSF under ATM-0428774 (V-Lab), EAR-1019853, and EAR-0810272. The computations were performed mainly at the Minnesota Supercomputing Institute (MSI).

Energy-level repulsion by spin-orbit coupling in two-dimensional Rydberg excitons

NASA Astrophysics Data System (ADS)

Stephanovich, V. A.; Sherman, E. Ya.; Zinner, N. T.; Marchukov, O. V.

2018-05-01

We study the effects of Rashba spin-orbit coupling on two-dimensional Rydberg exciton systems. Using analytical and numerical arguments we demonstrate that this coupling considerably modifies the wave functions and leads to a level repulsion that results in a deviation from the Poissonian statistics of the adjacent level distance distribution. This signifies the crossover to nonintegrability of the system and hints at the possibility of quantum chaos emerging. Such behavior strongly differs from the classical realization, where spin-orbit coupling produces highly entangled, chaotic electron trajectories in an exciton. We also calculate the oscillator strengths and show that randomization appears in the transitions between states with different total momenta.

Spin crossover in solid and liquid (Mg,Fe)O at extreme conditions

NASA Astrophysics Data System (ADS)

Stixrude, Lars; Holmstrom, Eero

Ferropericlase, (Mg,Fe)O, is a major constituent of the Earth's lower mantle (24-136 GPa). Understanding the properties of this component is important not only in the solid state, but also in the molten state, as the planet almost certainly hosted an extensive magma ocean initially. With increasing pressure, the Fe ions in the material begin to collapse from a magnetic to a nonmagnetic spin state. This crossover affects thermodynamic, transport, and electrical properties. Using first-principles molecular dynamics simulations, thermodynamic integration, and adiabatic switching, we present a phase diagram of the spin crossover. In both solid and liquid, we find a broad pressure range of coexisting magnetic and non-magnetic ions due to the favorable enthalpy of mixing of the two. In the solid increasing temperature favors the high spin state, while in the liquid the opposite occurs, due to the higher electronic entropy of the low spin state. Because the physics of the crossover differ in solid and liquid, melting produces a large change in spin state that may affect the buoyancy of crystals freezing from the magma ocean in the earliest Earth. This research was supported by the European Research Council under Advanced Grant No. 291432 ``MoltenEarth'' (FP7/2007-2013).

Pressure Dependence of Coherence-Incoherence Crossover Behavior in KFe 2As 2 Observed by Resistivity and 75As-NMR/NQR.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wiecki, P.; Taufour, V.; Chung, D. Y.

We present the results of 75As nuclear magnetic resonance (NMR), nuclear quadrupole resonance (NQR), and resistivity measurements in KFe 2As 2 under pressure (p). The temperature dependence of the NMR shift, nuclear spin-lattice relaxation time (T1), and resistivity show a crossover between a high-temperature incoherent, local-moment behavior and a low-temperature coherent behavior at a crossover temperature (T *). T * is found to increase monotonically with pressure, consistent with increasing hybridization between localized 3d orbitalderived bands with the itinerant electron bands. No anomaly in T * is seen at the critical pressure pc = 1.8 GPa where a change ofmore » slope of the superconducting (SC) transition temperature Tc(p) has been observed. In contrast, Tc(p) seems to correlate with antiferromagnetic spin fluctuations in the normal state as measured by the NQR 1/T1 data, although such a correlation cannot be seen in the replacement effects of A in the KFe 2As 2 (A = K, Rb, Cs) family. In the superconducting state, two T1 components are observed at low temperatures, suggesting the existence of two distinct local electronic environments. The temperature dependence of the short T1s indicates a nearly gapless state below Tc. On the other hand, the temperature dependence of the long component 1/T1L implies a large reduction in the density of states at the Fermi level due to the SC gap formation. These results suggest a real-space modulation of the local SC gap structure in KFe 2As 2 under pressure.« less

Pressure dependence of coherence-incoherence crossover behavior in KFe 2 As 2 observed by resistivity and As 75 -NMR/NQR

DOE PAGES

Wiecki, P.; Taufour, V.; Chung, D. Y.; ...

2018-02-13

We present the results of 75As nuclear magnetic resonance (NMR), nuclear quadrupole resonance (NQR), and resistivity measurements in KF e2 As 2 under pressure (p). The temperature dependence of the NMR shift, nuclear spin-lattice relaxation time (T 1), and resistivity show a crossover between a high-temperature incoherent, local-moment behavior and a low-temperature coherent behavior at a crossover temperature (T*). T* is found to increase monotonically with pressure, consistent with increasing hybridization between localized 3d orbital-derived bands with the itinerant electron bands. No anomaly in T* is seen at the critical pressure p c= 1.8 GPa where a change of slopemore » of the superconducting (SC) transition temperature T c( p ) has been observed. In contrast, T c( p ) seems to correlate with antiferromagnetic spin fluctuations in the normal state as measured by the NQR 1/T 1 data, although such a correlation cannot be seen in the replacement effects of A in the AFe 2As 2 (A=K,Rb,Cs) family. In the superconducting state, two T 1 components are observed at low temperatures, suggesting the existence of two distinct local electronic environments. The temperature dependence of the short T 1s indicates a nearly gapless state below T c. On the other hand, the temperature dependence of the long component 1/T 1Limplies a large reduction in the density of states at the Fermi level due to the SC gap formation. These results suggest a real-space modulation of the local SC gap structure in KFe 2As 2 under pressure.« less

Pressure dependence of coherence-incoherence crossover behavior in KFe 2 As 2 observed by resistivity and As 75 -NMR/NQR

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wiecki, P.; Taufour, V.; Chung, D. Y.

We present the results of 75As nuclear magnetic resonance (NMR), nuclear quadrupole resonance (NQR), and resistivity measurements in KF e2 As 2 under pressure (p). The temperature dependence of the NMR shift, nuclear spin-lattice relaxation time (T 1), and resistivity show a crossover between a high-temperature incoherent, local-moment behavior and a low-temperature coherent behavior at a crossover temperature (T*). T* is found to increase monotonically with pressure, consistent with increasing hybridization between localized 3d orbital-derived bands with the itinerant electron bands. No anomaly in T* is seen at the critical pressure p c= 1.8 GPa where a change of slopemore » of the superconducting (SC) transition temperature T c( p ) has been observed. In contrast, T c( p ) seems to correlate with antiferromagnetic spin fluctuations in the normal state as measured by the NQR 1/T 1 data, although such a correlation cannot be seen in the replacement effects of A in the AFe 2As 2 (A=K,Rb,Cs) family. In the superconducting state, two T 1 components are observed at low temperatures, suggesting the existence of two distinct local electronic environments. The temperature dependence of the short T 1s indicates a nearly gapless state below T c. On the other hand, the temperature dependence of the long component 1/T 1Limplies a large reduction in the density of states at the Fermi level due to the SC gap formation. These results suggest a real-space modulation of the local SC gap structure in KFe 2As 2 under pressure.« less

Dynamic heterogeneity in crossover spin facilitated model of supercooled liquid and fractional Stokes-Einstein relation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Choi, Seo-Woo; Kim, Soree; Jung, YounJoon, E-mail: yjjung@snu.ac.kr

Kinetically constrained models have gained much interest as models that assign the origins of interesting dynamic properties of supercooled liquids to dynamical facilitation mechanisms that have been revealed in many experiments and numerical simulations. In this work, we investigate the dynamic heterogeneity in the fragile-to-strong liquid via Monte Carlo method using the model that linearly interpolates between the strong liquid-like behavior and the fragile liquid-like behavior by an asymmetry parameter b. When the asymmetry parameter is sufficiently small, smooth fragile-to-strong transition is observed both in the relaxation time and the diffusion constant. Using these physical quantities, we investigate fractional Stokes-Einsteinmore » relations observed in this model. When b is fixed, the system shows constant power law exponent under the temperature change, and the exponent has the value between that of the Frederickson-Andersen model and the East model. Furthermore, we investigate the dynamic length scale of our systems and also find the crossover relation between the relaxation time. We ascribe the competition between energetically favored symmetric relaxation mechanism and entropically favored asymmetric relaxation mechanism to the fragile-to-strong crossover behavior.« less

A two-step spin crossover mononuclear iron(II) complex with a [HS-LS-LS] intermediate phase.

PubMed

Bonnet, Sylvestre; Siegler, Maxime A; Costa, José Sánchez; Molnár, Gábor; Bousseksou, Azzedine; Spek, Anthony L; Gamez, Patrick; Reedijk, Jan

2008-11-21

The two-step spin crossover of a new mononuclear iron(ii) complex is studied by magnetic, crystallographic and calorimetric methods revealing two successive first-order phase transitions and an ordered intermediate phase built by the repetition of the unprecedented [HS-LS-LS] motif.

Spin Order and Phase Transitions in Chains of Polariton Condensates.

PubMed

Ohadi, H; Ramsay, A J; Sigurdsson, H; Del Valle-Inclan Redondo, Y; Tsintzos, S I; Hatzopoulos, Z; Liew, T C H; Shelykh, I A; Rubo, Y G; Savvidis, P G; Baumberg, J J

2017-08-11

We demonstrate that multiply coupled spinor polariton condensates can be optically tuned through a sequence of spin-ordered phases by changing the coupling strength between nearest neighbors. For closed four-condensate chains these phases span from ferromagnetic (FM) to antiferromagnetic (AFM), separated by an unexpected crossover phase. This crossover phase is composed of alternating FM-AFM bonds. For larger eight-condensate chains, we show the critical role of spatial inhomogeneities and demonstrate a scheme to overcome them and prepare any desired spin state. Our observations thus demonstrate a fully controllable nonequilibrium spin lattice.

Weak cooperativity in selected iron(II) 1D coordination polymers

NASA Astrophysics Data System (ADS)

Dîrtu, Marinela M.; Gillard, Damien; Naik, Anil D.; Rotaru, Aurelian; Garcia, Yann

2012-03-01

The spin crossover behaviour of a new class of FeII coordination polymers [Fe(phtptrz)3]I2 ( 1), [Fe(phtptrz)3](ReO4)2•CH3OH ( 2) and [Fe(phtptrz)3]TaF7•6H2O ( 3) based on a novel ligand 4-(3' -N-phtalimido-propyl)-1,2,4-triazole (phtptrz), were investigated by temperature dependent 57Fe Mössbauer spectroscopy and magnetic susceptibility measurements. The adverse effect of bulky substituent on 1,2,4-triazole, favorable supramolecular interactions and influence of increasing anion size on spin crossover profile is discussed. 1 and 2 show thermally induced spin conversions of gradual and incomplete nature with associated thermochromism, and transition temperatures T1/2 ~ 163 K and 137 K, respectively. A spin state crossover is also identified for 3.

Spin crossover in (Mg,Fe3+)(Si,Fe3+)O3 bridgmanite: effects of disorder, iron concentration, and temperature

NASA Astrophysics Data System (ADS)

Shukla, Gaurav; Wentzcovitch, Renata

The spin crossover of iron in Fe3+-bearing bridgmanite, the most abundant mineral of the Earth's lower mantle, is by now a well-established phenomenon, though several aspects of this crossover remain unclear. Here we investigate effects of disorder, iron concentration, and temperature on this crossover using ab initio LDA + USC calculations. Disorder and concentration effects are addressed using complete statistical samplings of coupled substituted configurations up to 80 atoms supercells, while the vibrational effects using the quasiharmonic approximation. Our calculated compression curves for iron-free and iron-bearing bridgmanite compare well with the latest experimental measurements. The comparison also suggests that in a closed system, Fe2+ present in the sample may transform into Fe3+ by introduction of Mg and O vacancies with increasing pressure. As in the spin crossover in ferropericlase, this crossover in bridgmanite is accompanied by a clear volume reduction and an anomalous softening of the bulk modulus throughout the crossover pressure range. Though the concentration of [Fe3+]Si in bridgmanite may be small, related elastic anomalies may impact the interpretation of radial and lateral velocity structures of the Earth's lower mantle. This research was supported primarily by NSF Grant EAR 1348066. Computations are performed at the Minnesota Supercomputing Institute (MSI).

Three-dimensional iron(ii) porous coordination polymer exhibiting carbon dioxide-dependent spin crossover.

PubMed

Shin, Jong Won; Jeong, Ah Rim; Jeoung, Sungeun; Moon, Hoi Ri; Komatsumaru, Yuki; Hayami, Shinya; Moon, Dohyun; Min, Kil Sik

2018-04-24

We report a three-dimensional Fe(ii) porous coordination polymer that exhibits a spin crossover temperature change following CO2 sorption (though not N2 sorption). Furthermore, single crystals of the desolvated polymer with CO2 molecules at three different temperatures were characterised by X-ray crystallography.

Emergent superconductivity in an iron-based honeycomb lattice initiated by pressure-driven spin-crossover.

PubMed

Wang, Yonggang; Ying, Jianjun; Zhou, Zhengyang; Sun, Junliang; Wen, Ting; Zhou, Yannan; Li, Nana; Zhang, Qian; Han, Fei; Xiao, Yuming; Chow, Paul; Yang, Wenge; Struzhkin, Viktor V; Zhao, Yusheng; Mao, Ho-Kwang

2018-05-15

The discovery of iron-based superconductors (FeSCs), with the highest transition temperature (T c ) up to 55 K, has attracted worldwide research efforts over the past ten years. So far, all these FeSCs structurally adopt FeSe-type layers with a square iron lattice and superconductivity can be generated by either chemical doping or external pressure. Herein, we report the observation of superconductivity in an iron-based honeycomb lattice via pressure-driven spin-crossover. Under compression, the layered FePX 3 (X = S, Se) simultaneously undergo large in-plane lattice collapses, abrupt spin-crossovers, and insulator-metal transitions. Superconductivity emerges in FePSe 3 along with the structural transition and vanishing of magnetic moment with a starting T c  ~ 2.5 K at 9.0 GPa and the maximum T c  ~ 5.5 K around 30 GPa. The discovery of superconductivity in iron-based honeycomb lattice provides a demonstration for the pursuit of transition-metal-based superconductors via pressure-driven spin-crossover.

A spin-crossover complex based on a 2,6-bis(pyrazol-1-yl)pyridine (1-bpp) ligand functionalized with a carboxylate group.

PubMed

Abhervé, Alexandre; Clemente-León, Miguel; Coronado, Eugenio; Gómez-García, Carlos J; López-Jordà, Maurici

2014-07-07

Combining Fe(ii) with the carboxylate-functionalized 2,6-bis(pyrazol-1-yl)pyridine (bppCOOH) ligand results in the spin-crossover compound [Fe(bppCOOH)2](ClO4)2 which shows an abrupt spin transition with a T1/2 of ca. 380 K and a TLIESST of 60 K due to the presence of a hydrogen-bonded linear network of complexes.

SU(4) Kondo effect in double quantum dots with ferromagnetic leads

NASA Astrophysics Data System (ADS)

Weymann, Ireneusz; Chirla, Razvan; Trocha, Piotr; Moca, Cǎtǎlin Paşcu

2018-02-01

We investigate the spin-resolved transport properties, such as the linear conductance and the tunnel magnetoresistance, of a double quantum dot device attached to ferromagnetic leads and look for signatures of the SU (4 ) symmetry in the Kondo regime. We show that the transport behavior greatly depends on the magnetic configuration of the device, and the spin-SU(2) as well as the orbital and spin-SU(4) Kondo effects become generally suppressed when the magnetic configuration of the leads varies from the antiparallel to the parallel one. Furthermore, a finite spin polarization of the leads lifts the spin degeneracy and drives the system from the SU(4) to an orbital-SU(2) Kondo state. We analyze in detail the crossover and show that the Kondo temperature between the two fixed points has a nonmonotonic dependence on the degree of spin polarization of the leads. In terms of methods used, we characterize transport by using a combination of analytical and numerical renormalization group approaches.

Magnetic properties of transition metal fluorides MF2 (M=Mn, Fe, Co, Ni) via high-energy photon diffraction

NASA Astrophysics Data System (ADS)

Strempfer, J.; Rütt, U.; Bayrakci, S.; Brückel, Th.; Jauch, W.

2004-01-01

We present an overview of recent results from nonresonant magnetic diffraction experiments on the antiferromagnetic compounds MnF2, FeF2, CoF2, and NiF2 using high-energy synchrotron radiation of photon energies above 100 keV. New results are presented on the determination of the spin and of the L/S ratio for CoF2 and NiF2. For CoF2, the saturation value of the long-range-ordered pure spin Sz component Sz=1.11(1) is considerably lower than the value Sz=3/2 for the free Co2+ ion. This is in contrast to our results for NiF2, where the full spin of the free transition-metal ion was found, Sz=0.98(1). The temperature dependence of the magnetization in the critical region as well as in the low-temperature region is also presented. For all compounds, Ising behavior is found in the critical regime, whereas the crossover to the low-temperature spin-wave behavior varies. We attribute this to different anisotropies in this series of compounds.

Field-induced superconducting phase of FeSe in the BCS-BEC cross-over

PubMed Central

Kasahara, Shigeru; Watashige, Tatsuya; Hanaguri, Tetsuo; Kohsaka, Yuhki; Yamashita, Takuya; Shimoyama, Yusuke; Mizukami, Yuta; Endo, Ryota; Ikeda, Hiroaki; Aoyama, Kazushi; Terashima, Taichi; Uji, Shinya; Wolf, Thomas; von Löhneysen, Hilbert; Shibauchi, Takasada; Matsuda, Yuji

2014-01-01

Fermi systems in the cross-over regime between weakly coupled Bardeen–Cooper–Schrieffer (BCS) and strongly coupled Bose–Einstein-condensate (BEC) limits are among the most fascinating objects to study the behavior of an assembly of strongly interacting particles. The physics of this cross-over has been of considerable interest both in the fields of condensed matter and ultracold atoms. One of the most challenging issues in this regime is the effect of large spin imbalance on a Fermi system under magnetic fields. Although several exotic physical properties have been predicted theoretically, the experimental realization of such an unusual superconducting state has not been achieved so far. Here we show that pure single crystals of superconducting FeSe offer the possibility to enter the previously unexplored realm where the three energies, Fermi energy εF, superconducting gap Δ, and Zeeman energy, become comparable. Through the superfluid response, transport, thermoelectric response, and spectroscopic-imaging scanning tunneling microscopy, we demonstrate that εF of FeSe is extremely small, with the ratio Δ/εF∼1(∼0.3) in the electron (hole) band. Moreover, thermal-conductivity measurements give evidence of a distinct phase line below the upper critical field, where the Zeeman energy becomes comparable to εF and Δ. The observation of this field-induced phase provides insights into previously poorly understood aspects of the highly spin-polarized Fermi liquid in the BCS-BEC cross-over regime. PMID:25378706

Selective photoswitching of the binuclear spin crossover compound {[Fe(bt)(NCS)2]2(bpm)} into two distinct macroscopic phases.

PubMed

Moussa, N Ould; Molnár, G; Bonhommeau, S; Zwick, A; Mouri, S; Tanaka, K; Real, J A; Bousseksou, A

2005-03-18

The low-spin (LS-LS, S = 0) diamagnetic form of the binuclear spin crossover complex {[Fe(bt)(NCS)(2)](2)(bpm)} was selectively photoconverted into two distinct macroscopic phases at different excitation wavelengths (1342 or 647.1 nm). These long-lived metastable phases have been identified, respectively, as the symmetry-broken paramagnetic form (HS-LS, S = 2) and the antiferromagnetically coupled (HS-HS, S = 0) high-spin form of the compound. The selectivity may be explained by the strong coupling of the primary excited states to the paramagnetic state.

Scan-rate and vacuum pressure dependence of the nucleation and growth dynamics in a spin-crossover single crystal: the role of latent heat.

PubMed

Ridier, Karl; Rat, Sylvain; Salmon, Lionel; Nicolazzi, William; Molnár, Gábor; Bousseksou, Azzedine

2018-04-04

Using optical microscopy we studied the vacuum pressure dependence (0.1-1000 mbar) of the nucleation and growth dynamics of the thermally induced first-order spin transition in a single crystal of the spin-crossover compound [Fe(HB(tz)3)2] (tz = 1,2,4-triazol-1-yl). A crossover between a quasi-static hysteresis regime and a temperature-scan-rate-dependent kinetic regime is evidenced around 5 mbar due to the change of the heat exchange coupling between the crystal and its external environment. Remarkably, the absorption/dissipation rate of latent heat was identified as the key factor limiting the switching speed of the crystal.

Site-specific spin crossover in F e2Ti O4 post-spinel under high pressure up to nearly a megabar

NASA Astrophysics Data System (ADS)

Xu, W. M.; Hearne, G. R.; Layek, S.; Levy, D.; Itié, J.-P.; Pasternak, M. P.; Rozenberg, G. Kh.; Greenberg, E.

2017-07-01

X-ray diffraction studies to ˜90 GPa at room temperature show that F e2Ti O4 ferrous inverse spinel undergoes the following sequence of structural transitions: cubic (F d 3 ¯m ) →˜8 GPa tetragonal (I 41/a m d ) →˜16 GPa orthorhombic (C m c m ) →˜55 GPa orthorhombic (P m m a ) , at the indicated onset transition pressures. Within the Cmcm phase, site-specific spin crossover is initiated and involves only highly distorted octahedral sites constituting ˜25 % of all Fe locations. This is manifest as a steeper volume decrease of Δ V /V0˜3.5 % beyond ˜40 GPa and an emergent diamagnetic component discerned in 57Fe Mössbauer spectroscopy at variable cryogenic temperatures. A subsequent C m c m →P m m a Fe/Ti disorder-order reconfiguration is facilitated at sixfold coordinated (octahedral) sites. The rest of the high-spin Fe in sixfold and eightfold coordinated sites (˜75 % abundance) in the Pmma phase exhibit average saturation internal magnetic fields of Hh f˜42 T to ˜90 GPa , typical of spin-only (orbitally quenched) Fermi-contact values. By contrast, average Hh f˜20 T values, signifying unquenched orbital moments, occur below the 40 -45 GPa spin-crossover initiation regime in the Cmcm phase. Therefore, site-specific spin crossover invokes a cooperative lattice response and polyhedral distortions at the rest of the high-spin Fe sites, translating to 3 d level (sub-band) changes and consequential orbital moment quenching. Near ˜90 GPa , F e2Ti O4 is a partially spin-converted chemically ordered Pmma post-spinel having a persistent charge gap of ˜100 meV . Despite structural symmetry changes, partial spin crossover and lattice compressibility, resulting in a ˜33 % total reduction in unit-cell volume and corresponding 3 d bandwidth broadening, strong electron correlations persist at high densification.

Proton spin-lattice relaxation in low-dimensional ferromagnetic copper halides (abstract)

NASA Astrophysics Data System (ADS)

Marzke, R. F.; Haines, D. N.; Raffaelle, D. P.; Chamberlin, R. V.; Ramakrishna, B. L.

1991-04-01

1H spin-lattice relaxation times have been measured as functions of temperature and frequency in powder samples of the two-dimensional ferromagnetic compound (CH3NH3)2CuCl4 and in single crystals of the one-dimensional ferromagnets (C6H11NH3)CuB3 (CHAB), (C6H11NH3)CuCl3 (CHAC), and (C4H12N)CuCl3 (TMCuC). Sample temperatures were varied between 4.2 and 298 K, and NMR frequencies ranging from 12.6 to 54.0 MHz were used. Widths and shapes of the lines, typically several hundred Gauss broad at low temperatures, were recorded. The dependence of T1 upon magnetic field orientation was measured for the one-dimensional (1D) single crystal samples. Each compound showed basically two temperature regimes of different spin-lattice relaxation behavior, separated by a narrow transition temperature region. From 4.2 K, T1 in the compounds decreased strongly as the temperature was raised, a behavior expected for second-order Raman processes [K. M. Kopinga, A. M. C. Tinus, W. J. M. de Jonge, and G. C. de Vries, Phys. Rev. B 36, 5398 (1987)]. At the transition temperature region the decrease of T1 ceased, and T1 began to increase weakly and quasilinearly to 300 K. In the three 1D compounds, the transition regions occurred well below temperatures corresponding to 1D exchange interaction strengths in CHAC (˜70 K), CHAB (˜55 K), and TMCuC (˜30 K), and also above the compounds' 3D ordering temperatures (˜1.5 K and below). We noted a correlation between the T1 transition temperatures and temperatures at which spin dimensionality ``crossovers'' are observed in magnetic susceptibilities, going from Heisenberg to non-Heisenberg behavior as the temperature is decreased. The latter occur at approximately 10 K in CHAC. TMCuC, which has the most isotropic J tensor of these compounds and also the lowest weak-strong T1 transition, does not show a spin dimensionality crossover in susceptibility down to 2 K, but based on our NMR results one would be expected at or below this temperature. Further theoretical work appears to be necessary in order to elucidate the role of magnons and solitons in the transition behavior of the temperature dependence of T1.

DFT Analysis of Spin Crossover in Mn(III) Complexes: Is a Two-Electron S = 2 to S = 0 Spin Transition Feasible?

PubMed

Amabilino, Silvia; Deeth, Robert J

2017-03-06

Six-coordinate, rigorously octahedral d 4 Mn(III) spin crossover (SCO) complexes are limited by symmetry to an S = 1 (intermediate spin, IS) to S = 2 (high spin, HS) transition. In order to realize the potential S = 0 to S = 2 transition, a lower symmetry and/or change in coordination number is needed, which we explore here computationally. First, a number of complexes are analyzed to develop a reliable and relatively fast DFT protocol for reproducing known Mn(III) spin state energetics. The hybrid meta-GGA functional TPSSh with a modest split valence plus polarization basis set and an empirical dispersion correction is found to predict correctly the ground spin state of Mn(III) complexes, including true low-spin (LS) S = 0 systems, with a range of donor sets including the hexadentate [N 4 O 2 ] Schiff base ligands. The electronic structure design criteria necessary for realizing a ΔS = 2 SCO transition are described, and a number of model complexes are screened for potential SCO behavior. Five-coordinate trigonal-bipyramidal symmetry fails to yield any suitable systems. Seven-coordinate, approximately pentagonal bipyramidal symmetry is more favorable, and when a known pentadentate macrocyclic donor is combined with π-acceptor axial ligands, a novel Mn(III) complex, [Mn(PABODP)(PF 3 ) 2 ] 3+ (PABODP = 2,13-dimethyl-3,6,9,12,18-pentaazabicyclo[12.3.1]octadeca-1(18),2,12,14,16-pentaene), is predicted to have the right spin state energetics for an S = 0 to S = 2 transition. Successful synthesis of such a complex could provide the first example of a ΔS = 2 SCO transition for d 4 Mn(III). However, the combination of a rigid macrocycle and a high coordination number dilutes the stereochemical activity of the d electrons, leading to relatively small structural changes between HS and LS systems. It may therefore remain a challenge to realize strong cooperative effects in Mn(III) systems.

Pressure-induced cooperative spin transition in ironII 2D coordination polymers: room-temperature visible spectroscopic study.

PubMed

Levchenko, G; Bukin, G V; Terekhov, S A; Gaspar, A B; Martínez, V; Muñoz, M C; Real, J A

2011-06-30

For the 2D coordination polymers [Fe(3-Fpy)(2)M(II)(CN)(4)] (M(II) = Ni, Pd, Pt), the pressure-induced spin crossover behavior has been investigated at 298 K by monitoring the distinct optical properties associated with each spin state. Cooperative first-order spin transition characterized by a piezohysteresis loop ca. 0.1 GPa wide was observed for the three derivatives. Application of the mean field regular solution theory has enabled estimation of the cooperative parameter, Γ(p), and the enthalpy, ΔH(HL)(p), associated with the spin transition for each derivative. These values, found in the intervals 6.8-7.9 and 18.6-20.8 kJ mol(-1), respectively, are consistent with those previously reported for thermally induced spin transition at constant pressure for the title compounds (Chem.-Eur. J.2009, 15, 10960). Relevance of the elastic energy, Δ(elast), as a corrective parameter accounting for the pressure dependence of the critical temperature of thermally induced spin transitions (Clausius-Clapeiron equation) is also demonstrated and discussed.

Spin-crossover phenomena of the mononuclear Mn(III) complex tuned by metal dithiolene counteranions.

PubMed

Chen, Ying; Cao, Fan; Wei, Rong-Min; Zhang, Yang; Zhang, Yi-Quan; Song, You

2014-03-07

Three ion-pair complexes based on spin-crossover [Mn(5-Br-sal-N-1,5,8,12)]ClO4 with TBA2[Ni(mnt)2], TBA2[Pt(mnt)2] (mnt = maleonitriledithiolate) and TBA[Ni(dmit)2] respectively (dmit = 2-thioxo-1,3-dithiole-4,5-dithiolato) have been synthesized and structurally characterized. Complexes [Mn(5-Br-sal-N-1,5,8,12)]2[Ni(mnt)2] and [Mn(5-Br-sal-N-1,5,8,12)]2[Pt(mnt)2] are isomorphic and show the axial compression of the octahedral coordination environment of Mn(III) ions. With the temperature increasing the equatorial metal-ligand bond lengths show significant elongation, but the axial bond lengths remain unchanged. Complex [Mn(5-Br-sal-N-1,5,8,12)][Ni(dmit)2]·CH3CN contains π-π, p-π and H-bonds weak interactions. Magnetic investigation shows the spin-crossover phenomena for and , and T1/2 has been increased by 230 K comparing with the reactant complex. However, no spin-crossover was observed in complex , and theoretical calculations show that there are weak antiferromagnetic couplings mediated through π-π interactions.

Spin-crossover in an iron(III)-bispidine-alkylperoxide system.

PubMed

Bautz, Jochen; Comba, Peter; Que, Lawrence

2006-09-04

The iron(II) complex of a tetradentate bispidine ligand with two tertiary amines and two pyridine groups (L = dimethyl [3,7-dimethyl-9,9'-dihydroxy-2,4-di-(2-pyridyl)-3,7-diazabicyclo nonan-1,5-dicaboxylate]) is oxidized with tert-butyl hydroperoxide to the corresponding end-on tert-butylperoxo complex [Fe(III)(L)(OOtBu)(X)]n+ (X = solvent, anion). UV-vis, resonance Raman, and EPR spectroscopy, as a function of the solvent, show that this is a spin-crossover compound. The experimentally observed Raman vibrations for both low-spin and high-spin isomers are in good agreement with those computed by DFT.

Equilibrium, metastability, and hysteresis in a model spin-crossover material with nearest-neighbor antiferromagnetic-like and long-range ferromagnetic-like interactions

NASA Astrophysics Data System (ADS)

Rikvold, Per Arne; Brown, Gregory; Miyashita, Seiji; Omand, Conor; Nishino, Masamichi

2016-02-01

Phase diagrams and hysteresis loops were obtained by Monte Carlo simulations and a mean-field method for a simplified model of a spin-crossover material with a two-step transition between the high-spin and low-spin states. This model is a mapping onto a square-lattice S =1 /2 Ising model with antiferromagnetic nearest-neighbor and ferromagnetic Husimi-Temperley (equivalent-neighbor) long-range interactions. Phase diagrams obtained by the two methods for weak and strong long-range interactions are found to be similar. However, for intermediate-strength long-range interactions, the Monte Carlo simulations show that tricritical points decompose into pairs of critical end points and mean-field critical points surrounded by horn-shaped regions of metastability. Hysteresis loops along paths traversing the horn regions are strongly reminiscent of thermal two-step transition loops with hysteresis, recently observed experimentally in several spin-crossover materials. We believe analogous phenomena should be observable in experiments and simulations for many systems that exhibit competition between local antiferromagnetic-like interactions and long-range ferromagnetic-like interactions caused by elastic distortions.

Numerically exploring the 1D-2D dimensional crossover on spin dynamics in the doped Hubbard model

DOE PAGES

Kung, Y. F.; Bazin, C.; Wohlfeld, K.; ...

2017-11-02

Using determinant quantum Monte Carlo (DQMC) simulations, we systematically study the doping dependence of the crossover from one to two dimensions and its impact on the magnetic properties of the Hubbard model. A square lattice of chains is used, in which the dimensionality can be tuned by varying the interchain coupling t ⊥. The dynamical spin structure factor and static quantities, such as the static spin susceptibility and nearest-neighbor spin correlation function, are characterized in the one- and two-dimensional limits as a benchmark. When the dimensionality is tuned between these limits, the magnetic properties, while evolving smoothly from one tomore » two dimensions, drastically change regardless of the doping level. This suggests that the spin excitations in the two-dimensional Hubbard model, even in the heavily doped case, cannot be explained using the spinon picture known from one dimension. In conclusion, the DQMC calculations are complemented by cluster perturbation theory studies to form a more complete picture of how the crossover occurs as a function of doping and how doped holes impact magnetic order.« less

Spacer type mediated tunable spin crossover (SCO) characteristics of pyrene decorated 2,6-bis(pyrazol-1-yl)pyridine (bpp) based Fe(ii) molecular spintronic modules.

PubMed

Kumar, Kuppusamy Senthil; Šalitroš, Ivan; Moreno-Pineda, Eufemio; Ruben, Mario

2017-08-14

A simple "isomer-like" variation of the spacer group in a set of Fe(ii) spin crossover (SCO) complexes designed to probe spin state dependence of electrical conductivity in graphene-based molecular spintronic junctions led to the observation of remarkable variations in the thermal- and light-induced magnetic characteristics, paving a simple route for the design of functional SCO complexes with different temperature switching regimes based on a 2,6-bis(pyrazol-1-yl)pyridine ligand skeleton.

Coexistence of spin crossover and magnetic ordering in a dendrimeric Fe(III) complex

NASA Astrophysics Data System (ADS)

Vorobeva, V. E.; Domracheva, N. E.; Pyataev, A. V.; Gruzdev, M. S.; Chervonova, U. V.

2015-01-01

The magnetic properties of a new dendrimeric spin crossover Fe(III) complex, [Fe(L)2]+PF6-, where L = 3,5-di[3,4,5-tris(tetradecyloxy) benzoyloxy]benzoyl-4-salicylidene-N-ethyl-N-ethylene-diamine, are reported for the first time. EPR studies show that this compound undergoes a gradual spin transition in the temperature range 70-300 K and has antiferromagnetic ordering below 10 K. Mössbauer spectroscopy at 5 K confirms the presence of magnetic ordering in the dendrimeric iron complex.

A model of spin crossover in manganese(III) compounds: effects of intra- and intercenter interactions.

PubMed

Klokishner, Sophia I; Roman, Marianna A; Reu, Oleg S

2011-11-21

A microscopic approach to the problem of cooperative spin crossover in the [MnL2]NO3 crystal, which contains Mn(III) ions as structural units, is elaborated on, and the main mechanisms governing this effect are revealed. The proposed model also takes into account the splitting of the low-spin 3T1 (t(2)(4)) and high-spin 5E (t(2)(3)e) terms by the low-symmetry crystal field. The low-spin → high-spin transition has been considered as a cooperative phenomenon driven by interaction of the electronic shells of the Mn(III) ions with the all-around full-symmetric deformation that is extended over the crystal lattice via the acoustic phonon field. The model well explains the observed thermal dependencies of the magnetic susceptibility and the effective magnetic moment.

Photomagnetic studies on spin-crossover solid solutions containing two different metal complexes, [Fe(1-bpp)(2)](x)[M(terpy)2](1-x)[BF4]2 (M = Ru or Co).

PubMed

Chastanet, Guillaume; Tovee, Clare A; Hyett, Geoffrey; Halcrow, Malcolm A; Létard, Jean-François

2012-04-28

The photomagnetic properties of two series of spin-crossover solid solutions, [Fe(1-bpp)(2)](x)[Ru(terpy)(2)](1-x)(BF(4))(2) and [Fe(1-bpp)(2)](x)[Co(terpy)(2)](1-x)(BF(4))(2) (1-bpp = 2,6-bis[pyrazol-1-yl]pyridine), have been investigated. For all the materials, the evolution of the T(LIESST) value, the high-spin → low-spin relaxation parameters and the LITH loops were thoroughly studied. Interestingly in the Fe:Co series, along the photo-excitation, cobalt ions are concomitantly converted from low-spin to high-spin states with the iron centres, and also fully relax after light excitation. This journal is © The Royal Society of Chemistry 2012

Electron Density Distribution Changes of Magnesiowüstite With Pressure

NASA Astrophysics Data System (ADS)

Diamond, M. R.; Popov, D.; Shen, G.; Jeanloz, R.

2017-12-01

Magnesiowüstite is one of the dominant minerals in the earth's lower mantle; its density and elasticity, substantially altered by its spin crossover, have direct consequence to interpreting deep-earth geophysical data. High-resolution single-crystal x-ray diffraction data can portray the 3-dimensional distribution of electron density through the Fourier transform of measured form factors. Here we present experimentally measured changes in electron density distribution of single-crystal (Mg.85,Fe.15)O as it goes through its iron(II) high-spin to low-spin electronic transition between about 40 and 60 GPa [Lin and Tsuchiya, 2008], in a diamond-anvil cell. As (Mg,Fe)O undergoes a pressure induced spin crossover (from high spin at low pressure to low spin at high pressure) due to overlap of its eg orbitals, the t2g orbitals become more pronounced to due a higher population of electrons, while the eg orbitals diminish. The spin splitting energy becomes increasingly unfavorable compared to the spin orbital pairing energy. By looking at the population of electrons at different directions in real space, we directly observe these changes in orbital occupation leading up to and during the spin crossover. Since high-Mg magnesiowüstite has a high symmetry structure at these pressure conditions, detecting relative changes in electron density distribution (comparing subsequent pressure steps) is feasible by collecting high resolution data offered by high-energy X rays and wide opening-angle diamond-anvil cells.

Periodic density functional theory study of spin crossover in the cesium iron hexacyanochromate prussian blue analog

NASA Astrophysics Data System (ADS)

Wojdeł, Jacek C.; Moreira, Ibério de P. R.; Illas, Francesc

2009-01-01

This paper presents a detailed theoretical analysis of the electronic structure of the CsFe[Cr(CN)6] prussian blue analog with emphasis on the structural origin of the experimentally observed spin crossover transition in this material. Periodic density functional calculations using generalized gradient approximation (GGA)+U and nonlocal hybrid exchange-correlation potentials show that, for the experimental low temperature crystal structure, the t2g6eg0 low spin configuration of FeII is the most stable and CrIII (S =3/2, t2g3eg0) remains the same in all cases. This is also found to be the case for the low spin GGA+U fully relaxed structure with the optimized unit cell. A completely different situation emerges when calculations are carried out using the experimental high temperature structure. Here, GGA+U and hybrid density functional theory calculations consistently predict that the t2g4eg2 FeII high spin configuration is the ground state. However, the two spin configurations appear to be nearly degenerate when calculations are carried out for the geometries arising from a GGA+U full relaxation of the atomic structure carried out at experimental high temperature lattice constant. A detailed analysis of the energy difference between the two spin configurations as a function of the lattice constant strongly suggests that the observed spin crossover transition has a structural origin with non-negligible entropic contributions of the high spin state.

Disordered artificial spin ices: Avalanches and criticality (invited)

NASA Astrophysics Data System (ADS)

Reichhardt, Cynthia J. Olson; Chern, Gia-Wei; Libál, Andras; Reichhardt, Charles

2015-05-01

We show that square and kagome artificial spin ices with disconnected islands exhibit disorder-induced nonequilibrium phase transitions. The critical point of the transition is characterized by a diverging length scale and the effective spin reconfiguration avalanche sizes are power-law distributed. For weak disorder, the magnetization reversal is dominated by system-spanning avalanche events characteristic of a supercritical regime, while at strong disorder, the avalanche distributions have subcritical behavior and are cut off above a length scale that decreases with increasing disorder. The different type of geometrical frustration in the two lattices produces distinct forms of critical avalanche behavior. Avalanches in the square ice consist of the propagation of locally stable domain walls separating the two polarized ground states, and we find a scaling collapse consistent with an interface depinning mechanism. In the fully frustrated kagome ice, however, the avalanches branch strongly in a manner reminiscent of directed percolation. We also observe an interesting crossover in the power-law scaling of the kagome ice avalanches at low disorder. Our results show that artificial spin ices are ideal systems in which to study a variety of nonequilibrium critical point phenomena as the microscopic degrees of freedom can be accessed directly in experiments.

Disordered artificial spin ices: Avalanches and criticality (invited)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reichhardt, Cynthia J. Olson, E-mail: cjrx@lanl.gov; Chern, Gia-Wei; Reichhardt, Charles

2015-05-07

We show that square and kagome artificial spin ices with disconnected islands exhibit disorder-induced nonequilibrium phase transitions. The critical point of the transition is characterized by a diverging length scale and the effective spin reconfiguration avalanche sizes are power-law distributed. For weak disorder, the magnetization reversal is dominated by system-spanning avalanche events characteristic of a supercritical regime, while at strong disorder, the avalanche distributions have subcritical behavior and are cut off above a length scale that decreases with increasing disorder. The different type of geometrical frustration in the two lattices produces distinct forms of critical avalanche behavior. Avalanches in themore » square ice consist of the propagation of locally stable domain walls separating the two polarized ground states, and we find a scaling collapse consistent with an interface depinning mechanism. In the fully frustrated kagome ice, however, the avalanches branch strongly in a manner reminiscent of directed percolation. We also observe an interesting crossover in the power-law scaling of the kagome ice avalanches at low disorder. Our results show that artificial spin ices are ideal systems in which to study a variety of nonequilibrium critical point phenomena as the microscopic degrees of freedom can be accessed directly in experiments.« less

Spin crossover and Mott—Hubbard transition under high pressure and high temperature in the low mantle of the Earth

NASA Astrophysics Data System (ADS)

Ovchinnikov, S. G.; Ovchinnikova, T. M.; Plotkin, V. V.; Dyad'kov, P. G.

2015-11-01

Effect of high pressure induced spin crossover on the magnetic, electronic and structural properties of the minerals forming the Earth's low mantle is discussed. The low temperature P, T phase diagram of ferropericlase has the quantum phase transition point Pc = 56 GPa at T = 0 confirmed recently by the synchrotron Mössbauer spectroscopy. The LDA+GTB calculated phase diagram describes the experimental data. Its extension to the high temperature resulted earlier in prediction of the metallic properties of the Earth's mantle at the depth 1400 km < h < 1800 km. Estimation of the electrical conductivity based on the percolation theory is given. We discuss also the thermodynamic properties and structural anomalies resulting from the spin crossover and metal-insulator transition and compare them with the experimental seismic and geomagnetic field data.

An electron transfer driven magnetic switch: ferromagnetic exchange and spin delocalization in iron verdazyl complexes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brook, David J. R.; Fleming, Connor; Chung, Dorothy

A single electron reduction of an iron bis(verdazyl) complex results in a large change in spin multiplicity resulting from a combination of spin crossover and exceptionally strong ferromagnetic exchange.

An electron transfer driven magnetic switch: ferromagnetic exchange and spin delocalization in iron verdazyl complexes

DOE PAGES

Brook, David J. R.; Fleming, Connor; Chung, Dorothy; ...

2018-01-01

A single electron reduction of an iron bis(verdazyl) complex results in a large change in spin multiplicity resulting from a combination of spin crossover and exceptionally strong ferromagnetic exchange.

Thermal hysteresis kinetic effects of spin crossover nanoparticulated systems studied by FORC diagram method on an Ising-like model

NASA Astrophysics Data System (ADS)

Atitoaie, Alexandru; Stoleriu, Laurentiu; Tanasa, Radu; Stancu, Alexandru; Enachescu, Cristian

2016-04-01

The scientific community is manifesting a high research interest on spin crossover compounds and their recently synthesized nanoparticles, due to their various appealing properties, such as the bistability between a diamagnetic low spin state and a paramagnetic high spin state (HS), inter-switchable by temperature or pressure changes, light irradiation or magnetic field. The utility of these compounds showing hysteresis covers a broad area of applications, from the development of more efficient designs of temperature and pressure sensors to automotive and aeronautic industries and even a new type of molecular actuators. We are proposing in this work a study regarding the kinetic effects and the distribution of reversible and irreversible components on the thermal hysteresis of spin crossover nanoparticulated systems. We are considering here tridimensional systems with different sizes and also systems of nanoparticles with a Gaussian size distribution. The correlations between the kinetics of the thermal hysteresis, the distributions of sizes and intermolecular interactions and the transition temperature distributions were established by using the FORC (First Order Reversal Curves) method using a Monte Carlo technique within an Ising-like system.

Phase diagrams and free-energy landscapes for model spin-crossover materials with antiferromagnetic-like nearest-neighbor and ferromagnetic-like long-range interactions

NASA Astrophysics Data System (ADS)

Chan, C. H.; Brown, G.; Rikvold, P. A.

2017-11-01

We present phase diagrams, free-energy landscapes, and order-parameter distributions for a model spin-crossover material with a two-step transition between the high-spin and low-spin states (a square-lattice Ising model with antiferromagnetic-like nearest-neighbor and ferromagnetic-like long-range interactions) [P. A. Rikvold et al., Phys. Rev. B 93, 064109 (2016), 10.1103/PhysRevB.93.064109]. The results are obtained by a recently introduced, macroscopically constrained Wang-Landau Monte Carlo simulation method [Phys. Rev. E 95, 053302 (2017), 10.1103/PhysRevE.95.053302]. The method's computational efficiency enables calculation of thermodynamic quantities for a wide range of temperatures, applied fields, and long-range interaction strengths. For long-range interactions of intermediate strength, tricritical points in the phase diagrams are replaced by pairs of critical end points and mean-field critical points that give rise to horn-shaped regions of metastability. The corresponding free-energy landscapes offer insights into the nature of asymmetric, multiple hysteresis loops that have been experimentally observed in spin-crossover materials characterized by competing short-range interactions and long-range elastic interactions.

Tunable Mode Coupling in Nanocontact Spin-Torque Oscillators

DOE PAGES

Zhang, Steven S. -L.; Iacocca, Ezio; Heinonen, Olle

2017-07-27

Recent experiments on spin-torque oscillators have revealed interactions between multiple magneto-dynamic modes, including mode coexistence, mode hopping, and temperature-driven crossover between modes. The initial multimode theory indicates that a linear coupling between several dominant modes, arising from the interaction of the subdynamic system with a magnon bath, plays an essential role in the generation of various multimode behaviors, such as mode hopping and mode coexistence. In this work, we derive a set of rate equations to describe the dynamics of coupled magneto-dynamic modes in a nanocontact spin-torque oscillator. Here, expressions for both linear and nonlinear coupling terms are obtained, whichmore » allow us to analyze the dependence of the coupled dynamic behaviors of modes on external experimental conditions as well as intrinsic magnetic properties. For a minimal two-mode system, we further map the energy and phase difference of the two modes onto a two-dimensional phase space and demonstrate in the phase portraits how the manifolds of periodic orbits and fixed points vary with an external magnetic field as well as with the temperature.« less

Tunable Mode Coupling in Nanocontact Spin-Torque Oscillators

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Steven S. -L.; Iacocca, Ezio; Heinonen, Olle

Recent experiments on spin-torque oscillators have revealed interactions between multiple magneto-dynamic modes, including mode coexistence, mode hopping, and temperature-driven crossover between modes. The initial multimode theory indicates that a linear coupling between several dominant modes, arising from the interaction of the subdynamic system with a magnon bath, plays an essential role in the generation of various multimode behaviors, such as mode hopping and mode coexistence. In this work, we derive a set of rate equations to describe the dynamics of coupled magneto-dynamic modes in a nanocontact spin-torque oscillator. Here, expressions for both linear and nonlinear coupling terms are obtained, whichmore » allow us to analyze the dependence of the coupled dynamic behaviors of modes on external experimental conditions as well as intrinsic magnetic properties. For a minimal two-mode system, we further map the energy and phase difference of the two modes onto a two-dimensional phase space and demonstrate in the phase portraits how the manifolds of periodic orbits and fixed points vary with an external magnetic field as well as with the temperature.« less

Quasi-One-Dimensional Ultracold Fermi Gases

NASA Astrophysics Data System (ADS)

Revelle, Melissa C.

Ultracold atoms have become an essential tool in studying condensed matter phenomena. The advantage of atomic physics experiments is that they provide an easily tunable system. This experiment uses the lowest two ground state hyperfine levels of fermionic lithium. Having two different states creates a pseudo-spin- 1/2 system and allows us to emulate electronic systems, such as superconductors and crystal lattices. In our experiment, we can control the ratio between these two states resulting in either a spin-balanced or a spin-imbalanced gas. Imposing an imbalance is analogous to applying a magnetic field to a superconductor which causes the electrons in the material to align to the field (thus breaking the electron pairs which cause superconductivity). This motivates us to understand the phases created when a spin-imbalance is created and the effect of changing the atomic interactions. In a 3D system, we find where superfluidity is suppressed throughout the BEC to BCS crossover. Using phase separation as a guide, we probe the dimensional crossover between 1D and 3D. The phase separation in 1D is inverted from that in 3D, which provides a unique characteristic to distinguish between the dimensions. By varying the tunneling between tubes and the atomic interactions in a 2D optical lattice, we control whether the system is 1D, 3D, or in between. Using the properties of a 3D gas as a guide, we directly observe when the gas has crossed over from being dominated by 1D-like behavior to 3D. In this way, we have found a universal value for the dimensional crossover. The 1D-3D crossover paves the way to search for the exotic FFLO (Fulde-Ferrell-Larkin-Ovchinnikov) superconductor. While most superconductors do not coexist with magnetism, the FFLO phase requires large magnetic fields to support its pairing mechanism. Additionally, this phase is more likely to be found in lower dimensional systems. However, at low dimensions, the effect of temperature fluctuations on the phase is destabilizing, but these temperature effects are reduced with higher dimensionality. Thus, the quasi-1D regime is the optimal region of parameter space to find this phase. The search for direct evidence of FFLO continues in this regime.

Predicting critical temperatures of iron(II) spin crossover materials: Density functional theory plus U approach

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Yachao, E-mail: yczhang@nano.gznc.edu.cn

2014-12-07

A first-principles study of critical temperatures (T{sub c}) of spin crossover (SCO) materials requires accurate description of the strongly correlated 3d electrons as well as much computational effort. This task is still a challenge for the widely used local density or generalized gradient approximations (LDA/GGA) and hybrid functionals. One remedy, termed density functional theory plus U (DFT+U) approach, introduces a Hubbard U term to deal with the localized electrons at marginal computational cost, while treats the delocalized electrons with LDA/GGA. Here, we employ the DFT+U approach to investigate the T{sub c} of a pair of iron(II) SCO molecular crystals (αmore » and β phase), where identical constituent molecules are packed in different ways. We first calculate the adiabatic high spin-low spin energy splitting ΔE{sub HL} and molecular vibrational frequencies in both spin states, then obtain the temperature dependent enthalpy and entropy changes (ΔH and ΔS), and finally extract T{sub c} by exploiting the ΔH/T − T and ΔS − T relationships. The results are in agreement with experiment. Analysis of geometries and electronic structures shows that the local ligand field in the α phase is slightly weakened by the H-bondings involving the ligand atoms and the specific crystal packing style. We find that this effect is largely responsible for the difference in T{sub c} of the two phases. This study shows the applicability of the DFT+U approach for predicting T{sub c} of SCO materials, and provides a clear insight into the subtle influence of the crystal packing effects on SCO behavior.« less

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

DOE PAGES

Zhang, Wenkai; Kjaer, Kasper S.; Alonso-Mori, Roberto; ...

2016-08-25

Developing light-harvesting and photocatalytic molecules made with iron could provide a cost effective, scalable, and environmentally benign path for solar energy conversion. To date these developments have been limited by the sub-picosecond metal-to-ligand charge transfer (MLCT) electronic excited state lifetime of iron based complexes due to spin crossover – the extremely fast intersystem crossing and internal conversion to high spin metal-centered excited states. We revitalize a 30 year old synthetic strategy for extending the MLCT excited state lifetimes of iron complexes by making mixed ligand iron complexes with four cyanide (CN –) ligands and one 2,2'-bipyridine (bpy) ligand. This enablesmore » MLCT excited state and metal-centered excited state energies to be manipulated with partial independence and provides a path to suppressing spin crossover. We have combined X-ray Free-Electron Laser (XFEL) Kβ hard X-ray fluorescence spectroscopy with femtosecond time-resolved UV-visible absorption spectroscopy to characterize the electronic excited state dynamics initiated by MLCT excitation of [Fe(CN) 4(bpy)] 2–. The two experimental techniques are highly complementary; the time-resolved UV-visible measurement probes allowed electronic transitions between valence states making it sensitive to ligand-centered electronic states such as MLCT states, whereas the Kβ fluorescence spectroscopy provides a sensitive measure of changes in the Fe spin state characteristic of metal-centered excited states. Here, we conclude that the MLCT excited state of [Fe(CN) 4(bpy)] 2– decays with roughly a 20 ps lifetime without undergoing spin crossover, exceeding the MLCT excited state lifetime of [Fe(2,2'-bipyridine) 3] 2+ by more than two orders of magnitude.« less

Structural, thermal and photomagnetic properties of spin crossover [Fe(bpp)2]2+ salts bearing [Cr(L)(ox)2]- anions.

PubMed

Clemente-León, Miguel; Coronado, Eugenio; Giménez-López, M Carmen; Romero, Francisco M; Asthana, Saket; Desplanches, Cédric; Létard, Jean-François

2009-10-14

This paper is divided into two parts: in the first part, the influence of solvate molecules on the magnetic properties of spin crossover salts of [Fe(bpp)(2)][Cr(L)(ox)(2)]ClO(4) x nS (bpp = 2,6-bis(pyrazol-3yl)pyridine; L = 2,2'-bipyridine (bpy) or 1,10-phenanthroline (phen); ox = oxalate dianion; S = solvent) is analyzed. The second part is devoted to the photomagnetic properties of the previously reported [Fe(bpp)(2)][Cr(L)(ox)(2)](2) family of compounds. The study describes the crystal structure, differential scanning calorimetry (DSC) and magnetic properties of [Fe(bpp)(2)][Cr(bpy)(ox)(2)]ClO(4) x EtOH x 4 H(2)O (1) and [Fe(bpp)(2)][Cr(phen)(ox)(2)]ClO(4) x 1.5 EtOH x 4 H(2)O (2). Both salts are high-spin (HS) compounds. Desolvation of 1 yields a material exhibiting a gradual spin crossover that involves 50% of the Fe(2+) cations. Rehydration of this desolvated salt induces a significant increase in the low-spin (LS) population. Desolvation of 2 affords a material showing a more abrupt spin crossover with thermal hysteresis (T(1/2)(increasing) = 286 K and T(1/2)(decreasing) = 273 K). This material is not very sensitive to rehydration. The anhydrous compounds [Fe(bpp)(2)][Cr(bpy)(ox)(2)](2) (3) and [Fe(bpp)(2)][Cr(phen)(ox)(2)](2) (4) display some quantitative photomagnetic conversion with T(LIESST) values of 41 and 51 K, respectively. Kinetic parameters governing the photo-induced HS-LS relaxation process have been determined and used to reproduce the T(LIESST) curves.

Crossover from Commensurate to Incommensurate Antiferromagnetism in Stoichiometric NaFeAs Revealed by Single-Crystal 23Na,75As-NMR Experiments

NASA Astrophysics Data System (ADS)

Kitagawa, Kentaro; Mezaki, Yuji; Matsubayashi, Kazuyuki; Uwatoko, Yoshiya; Takigawa, Masashi

2011-03-01

We report the results of 23Na and 75As nuclear magnetic resonance (NMR) experiments on a self-flux grown high-quality single crystal of stoichiometric NaFeAs. The NMR spectra reveal a tetragonal to twinned-orthorhombic structural phase transition at TO = 57 K and an antiferromagnetic (AF) transition at TAF = 45 K. The divergent behavior of nuclear relaxation rate near TAF shows significant anisotropy, indicating that the critical slowing down of stripe-type AF fluctuations are strongly anisotropic in spin space. The NMR spectra at sufficiently low temperatures consist of sharp peaks showing a commensurate stripe AF order with a small moment of ˜0.3 μB. However, the spectra just below TAF exhibit a highly asymmetric broadening pointing to an incommensurate modulation. The commensurate-incommensurate crossover in NaFeAs shows a certain similarity to the behavior of SrFe2As2 under high pressure.

Spin-orbit coupling induced two-electron relaxation in silicon donor pairs

NASA Astrophysics Data System (ADS)

Song, Yang; Das Sarma, S.

2017-09-01

We unravel theoretically a key intrinsic relaxation mechanism among the low-lying singlet and triplet donor-pair states in silicon, an important element in the fast-developing field of spintronics and quantum computation. Despite the perceived weak spin-orbit coupling (SOC) in Si, we find that our discovered relaxation mechanism, combined with the electron-phonon and interdonor interactions, drives the transitions in the two-electron states over a large range of donor coupling regimes. The scaling of the relaxation rate with interdonor exchange interaction J goes from J5 to J4 at the low to high temperature limits. Our analytical study draws on the symmetry analysis over combined band, donor envelope, and valley configurations. It uncovers naturally the dependence on the donor-alignment direction and triplet spin orientation, and especially on the dominant SOC source from donor impurities. While a magnetic field is not necessary for this relaxation, unlike in the single-donor spin relaxation, we discuss the crossover behavior with increasing Zeeman energy in order to facilitate comparison with experiments.

Metal-insulator transition and magnetic fluctuations in polycrystalline Ru1 -xRhxP investigated by 31P NMR

NASA Astrophysics Data System (ADS)

Li, Shang; Kobayashi, Yoshiaki; Itoh, Masayuki; Hirai, Daigorou; Takagi, Hidenori

2017-04-01

31P NMR measurements have been made on polycrystalline samples to study a metal-insulator (MI) transition and magnetic fluctuations in Ru1 -xRhxP which has metallic (M), pseudogap (PG), insulating (I), and superconducting (SC) phases. We find that RuP undergoes a crossover from the high-temperature (high-T ) M phase to the PG phase with the pseudo spin-gap behavior probed by the nuclear spin-lattice relaxation rate at TPG=330 K . The first-order MI transition is observed to take place from the PG phase to the low-T nonmagnetic I phase with the spin-gap energy of 1250 K at TMI=270 K . In the PG phase of Ru1 -xRhxP with 0 ≤x <0.45 , an analysis based on the modified Korringa relation, which is applicable to an itinerant paramagnet with weak electron correlation, shows that antiferromagnetic (AFM) fluctuations described in the random-phase approximation are enhanced in the low-T and low-x region. Around the PG-M phase boundary at xc˜0.45 , there is the SC phase whose normal state has negligible electron-electron interaction. We discuss the MI transition, the crossover from the M phase to the PG phase, and the magnetic properties of each phase based on the band structure.

Semiclassical theory for liquidlike behavior of the frustrated magnet Ca10Cr7O28

NASA Astrophysics Data System (ADS)

Biswas, Sounak; Damle, Kedar

2018-03-01

We identify the low energy effective Hamiltonian that is expected to describe the low temperature properties of the frustrated magnet Ca10Cr7O28 . Motivated by the fact that this effective Hamiltonian has S =3 /2 effective moments as its degrees of freedom, we use semiclassical spin-wave theory to study the T =0 physics of this effective model and argue that singular spin-wave fluctuations destabilize the spiral order favored by the exchange couplings of this effective Hamiltonian. We also use a combination of classical Monte-Carlo simulations and molecular dynamics, as well as analytical approximations, to study the physics at low, nonzero temperatures. The results of these nonzero temperature calculations capture the liquidlike structure factors observed in the temperature range accessed by recent experiments. Additionally, at still lower temperatures, they predict that a transition to nematic order in the bond energies reflects itself in the spin channel in the form of a crossover to a regime with large but finite correlation length for spiral spin correlations and a corresponding slowing down of spin dynamics.

Guest-tuned spin crossover in flexible supramolecular assemblies templated by a halide (Cl -, Br - or I - )

DOE Office of Scientific and Technical Information (OSTI.GOV)

Darawsheh, M. D.; Barrios, L. A.; Roubeau, O.

Ligand 1,3-bis(3-(pyridin-2-yl)-1H-pyrazol-5-yl)benzene, L, forms mononuclear spin crossover complexes [FeL 3] 2+ with pendant arms that cause them to dimerize through numerous intermolecular interactions forming supramolecular (X@[FeL 3] 2) 3+ cations. Finally, hey have the flexibility to encapsulate Cl -, Br - or I -, which allow tuning the magnetic properties, in the solid state and in solution.

Guest-tuned spin crossover in flexible supramolecular assemblies templated by a halide (Cl -, Br - or I - )

DOE PAGES

Darawsheh, M. D.; Barrios, L. A.; Roubeau, O.; ...

2016-12-05

Ligand 1,3-bis(3-(pyridin-2-yl)-1H-pyrazol-5-yl)benzene, L, forms mononuclear spin crossover complexes [FeL 3] 2+ with pendant arms that cause them to dimerize through numerous intermolecular interactions forming supramolecular (X@[FeL 3] 2) 3+ cations. Finally, hey have the flexibility to encapsulate Cl -, Br - or I -, which allow tuning the magnetic properties, in the solid state and in solution.

Unravelling the spin-state of solvated [Fe(bpp)2]2+ spin-crossover complexes: structure-function relationship.

PubMed

Giménez-López, Maria Del Carmen; Clemente-León, Miguel; Giménez-Saiz, Carlos

2018-05-23

This paper reports firstly the syntheses, crystal structures, and thermal and magnetic properties of spin crossover salts of formulae [Fe(bpp)2]3[Cr(CN)6]2·13H2O (1) and [Fe(bpp)2][N(CN)2]2·H2O (2) (bpp = 2,6-bis(pyrazol-3-yl)pyridine) exhibiting hydrogen-bonded networks of low-spin [Fe(bpp)2]2+ complexes and [Cr(CN)6]3- or [N(CN)2]- anions, with solvent molecules located in the voids. Desolvation of 1 is accompanied by a complete low-spin (LS) to a high-spin (HS) transformation that becomes reversible after rehydration by exposing the sample to the humidity of air. The influence of the lattice water on the magnetic properties of spin-crossover [Fe(bpp)2]X2 complex salts has been documented. In most cases, it stabilises the LS state over the HS one. In other cases, it is rather the contrary. The second part of this paper is devoted to unravelling the reasons why the lattice solvent stabilises one form over the other through magneto-structural correlations of [Fe(bpp)2]2+ salts bearing anions with different charge/size ratios (Xn-). The [Fe(bpp)2]2+ stacking explaining these two different behaviours is correlated here with the composition of the second coordination sphere of the Fe centers and the ability of these anions to form hydrogen bonds and/or π-π stacking interactions between them or the bpp ligand.

Mechanochemical effect in the iron(III) spin crossover complex [Fe(3-MeO-salenEt2]PF6 as studied by heat capacity calorimetry.

PubMed

Sorai, Michio; Burriel, Ramón; Westrum, Edgar F; Hendrickson, David N

2008-04-10

Magnetic and thermal properties of the iron(III) spin crossover complex [Fe(3MeO-salenEt)(2)]PF(6) are very sensitive to mechanochemical perturbations. Heat capacities for unperturbed and differently perturbed samples were precisely determined by adiabatic calorimetry at temperatures in the 10-300 K range. The unperturbed compound shows a cooperative spin crossover transition at 162.31 K, presenting a hysteresis of 2.8 K. The anomalous enthalpy and entropy contents of the transition were evaluated to be Delta(trs)H = 5.94 kJ mol(-1) and Delta(trs)S = 36.7 J K(-1) mol(-1), respectively. By mechanochemical treatments, (1) the phase transition temperature was lowered by 1.14 K, (2) the enthalpy and entropy gains at the phase transition due to the spin crossover phenomenon were diminished to Delta(trs)H = 4.94 kJ mol(-1) and Delta(trs)S = 31.1 J K(-1) mol(-1), and (3) the lattice heat capacities were larger than those of the unperturbed sample over the whole temperature range. In spite of different mechanical perturbations (grinding with a mortar and pestle and grinding in a ball-mill), two sets of heat capacity measurements provided basically the same results. The mechanochemical perturbation exerts its effect more strongly on the low-spin state than on the high-spin state. It shows a substantial increase of the number of iron(III) ions in the high-spin state below the transition temperature. The heat capacities of the diamagnetic cobalt(III) analogue [Co(3MeO-salenEt)(2)]PF(6) also were measured. The lattice heat capacity of the iron compounds has been estimated from either the measurements on the cobalt complex using a corresponding states law or the effective frequency distribution method. These estimations have been used for the evaluation of the transition anomaly.

Mechanism of spin crossover in LaCoO3 resolved by shape magnetostriction in pulsed magnetic fields.

PubMed

Rotter, M; Wang, Z-S; Boothroyd, A T; Prabhakaran, D; Tanaka, A; Doerr, M

2014-11-11

In the scientific description of unconventional transport properties of oxides (spin-dependent transport, superconductivity etc.), the spin-state degree of freedom plays a fundamental role. Because of this, temperature- or magnetic field-induced spin-state transitions are in the focus of solid-state physics. Cobaltites, e.g. LaCoO3, are prominent examples showing these spin transitions. However, the microscopic nature of the spontaneous spin crossover in LaCoO3 is still controversial. Here we report magnetostriction measurements on LaCoO3 in magnetic fields up to 70 T to study the sharp, field-induced transition at Hc ≈ 60 T. Measurements of both longitudinal and transversal magnetostriction allow us to separate magnetovolume and magnetodistortive changes. We find a large increase in volume, but only a very small increase in tetragonal distortion at Hc. The results, supported by electronic energy calculations by the configuration interaction cluster method, provide compelling evidence that above Hc LaCoO3 adopts a correlated low spin/high spin state.

Mechanism of spin crossover in LaCoO3 resolved by shape magnetostriction in pulsed magnetic fields

PubMed Central

Rotter, M.; Wang, Z.-S.; Boothroyd, A. T.; Prabhakaran, D.; Tanaka, A.; Doerr, M.

2014-01-01

In the scientific description of unconventional transport properties of oxides (spin-dependent transport, superconductivity etc.), the spin-state degree of freedom plays a fundamental role. Because of this, temperature- or magnetic field-induced spin-state transitions are in the focus of solid-state physics. Cobaltites, e.g. LaCoO3, are prominent examples showing these spin transitions. However, the microscopic nature of the spontaneous spin crossover in LaCoO3 is still controversial. Here we report magnetostriction measurements on LaCoO3 in magnetic fields up to 70 T to study the sharp, field-induced transition at Hc ≈ 60 T. Measurements of both longitudinal and transversal magnetostriction allow us to separate magnetovolume and magnetodistortive changes. We find a large increase in volume, but only a very small increase in tetragonal distortion at Hc. The results, supported by electronic energy calculations by the configuration interaction cluster method, provide compelling evidence that above Hc LaCoO3 adopts a correlated low spin/high spin state. PMID:25384532

Mechanism of spin crossover in LaCoO3 resolved by shape magnetostriction in pulsed magnetic fields

NASA Astrophysics Data System (ADS)

Rotter, M.; Wang, Z.-S.; Boothroyd, A. T.; Prabhakaran, D.; Tanaka, A.; Doerr, M.

2014-11-01

In the scientific description of unconventional transport properties of oxides (spin-dependent transport, superconductivity etc.), the spin-state degree of freedom plays a fundamental role. Because of this, temperature- or magnetic field-induced spin-state transitions are in the focus of solid-state physics. Cobaltites, e.g. LaCoO3, are prominent examples showing these spin transitions. However, the microscopic nature of the spontaneous spin crossover in LaCoO3 is still controversial. Here we report magnetostriction measurements on LaCoO3 in magnetic fields up to 70 T to study the sharp, field-induced transition at Hc ~ 60 T. Measurements of both longitudinal and transversal magnetostriction allow us to separate magnetovolume and magnetodistortive changes. We find a large increase in volume, but only a very small increase in tetragonal distortion at Hc. The results, supported by electronic energy calculations by the configuration interaction cluster method, provide compelling evidence that above Hc LaCoO3 adopts a correlated low spin/high spin state.

Spin-orbit torque in a three-dimensional topological insulator-ferromagnet heterostructure: Crossover between bulk and surface transport

NASA Astrophysics Data System (ADS)

Ghosh, S.; Manchon, A.

2018-04-01

Current-driven spin-orbit torques are investigated in a heterostructure composed of a ferromagnet deposited on top of a three-dimensional topological insulator using the linear response formalism. We develop a tight-binding model of the heterostructure adopting a minimal interfacial hybridization scheme that promotes induced magnetic exchange on the topological surface states, as well as induced Rashba-like spin-orbit coupling in the ferromagnet. Therefore our model accounts for the spin Hall effect from bulk states together with inverse spin galvanic and magnetoelectric effects at the interface on equal footing. By varying the transport energy across the band structure, we uncover a crossover from surface-dominated to bulk-dominated transport regimes. We show that the spin density profile and the nature of the spin-orbit torques differ substantially in both regimes. Our results, which compare favorably with experimental observations, demonstrate that the large dampinglike torque reported recently is more likely attributed to the Berry curvature of interfacial states, while spin Hall torque remains small even in the bulk-dominated regime.

Boson-mediated quantum spin simulators in transverse fields: X Y model and spin-boson entanglement

NASA Astrophysics Data System (ADS)

Wall, Michael L.; Safavi-Naini, Arghavan; Rey, Ana Maria

2017-01-01

The coupling of spins to long-wavelength bosonic modes is a prominent means to engineer long-range spin-spin interactions, and has been realized in a variety of platforms, such as atoms in optical cavities and trapped ions. To date, much of the experimental focus has been on the realization of long-range Ising models, but generalizations to other spin models are highly desirable. In this work, we explore a previously unappreciated connection between the realization of an X Y model by off-resonant driving of a single sideband of boson excitation (i.e., a single-beam Mølmer-Sørensen scheme) and a boson-mediated Ising simulator in the presence of a transverse field. In particular, we show that these two schemes have the same effective Hamiltonian in suitably defined rotating frames, and analyze the emergent effective X Y spin model through a truncated Magnus series and numerical simulations. In addition to X Y spin-spin interactions that can be nonperturbatively renormalized from the naive Ising spin-spin coupling constants, we find an effective transverse field that is dependent on the thermal energy of the bosons, as well as other spin-boson couplings that cause spin-boson entanglement not to vanish at any time. In the case of a boson-mediated Ising simulator with transverse field, we discuss the crossover from transverse field Ising-like to X Y -like spin behavior as a function of field strength.

Bethe lattice approach and relaxation dynamics study of spin-crossover materials

NASA Astrophysics Data System (ADS)

Oke, Toussaint Djidjoho; Hontinfinde, Félix; Boukheddaden, Kamel

2015-07-01

Dynamical properties of Prussian blue analogs and spin-crossover materials are investigated in the framework of a Blume-Emery-Griffiths (BEG) spin-1 model, where states ±1 and 0 represent the high-spin (HS) state and the low-spin state, respectively. The quadrupolar interaction depends on the temperature in the form . Magnetic interactions are controlled by a factor such that for (), magnetic ordering is not expected. The model is exactly solved using the Bethe lattice approach for the equilibrium properties. The results are closer to those calculated by numerical simulations with suitable Arrhenius-type transition rates. The study of relaxation processes of non-equilibrium HS states revealed one-step nonlinear sigmoidal relaxation curves of the HS fraction at low temperatures. We found that increasing the magnetic interactions leads to the appearance of a plateau in the thermal hysteresis as well as in the relaxation curves of the HS fraction at low temperature.

Numerical Investigations of the Thermal, Pressure and Size Effects on 2D Spin Crossover Nanoparticles

NASA Astrophysics Data System (ADS)

Harlé, C.; Allal, S. E.; Sohier, D.; Dufaud, T.; Caballero, R.; de Zela, F.; Dahoo, P. R.; Boukheddaden, K.; Linares, J.

2017-12-01

In the framework of the Ising-like model, the thermal and pressure effects on the spin crossover systems are evaluated through two-states fictitious spin operators σ with eigenvalues 𝜎 = -1 and 𝜎 = +1 respectively associated with the low-spin (LS) and highspin (HS) states of each spin-crossover (SCO) molecule. Based on each configurational state, the macroscopic SCO system, is described by the following variables: m=Σ σi, s=Σ σi σj and c=Σ σk standing respectively for the total magnetization, the short-range correlations and surface magnetization. To solve this problem, we first determine the density of macrostates d[m][s][c], giving the number of microscopic configurations with the same m, s and c values. In this contribution, two different ways have been performed to calculate this important quantity: (i) the entropic sampling method, based on Monte Carlo simulations and (ii) a new algorithm based on specific dynamic programming. These two methods were tested on the 2D SCO nanoparticles for which, we calculated the average magnetization < σ> taking into account for short-, long-range interactions as well as for the interaction between surface molecules with their surrounding matrix. We monitored the effect of the pressure, temperature and size on the properties of the SCO nanoparticles.

Pressure-Driven Spin Crossover Involving Polyhedral Transformation in Layered Perovskite Cobalt Oxyfluoride

PubMed Central

Tsujimoto, Yoshihiro; Nakano, Satoshi; Ishimatsu, Naoki; Mizumaki, Masaichiro; Kawamura, Naomi; Kawakami, Takateru; Matsushita, Yoshitaka; Yamaura, Kazunari

2016-01-01

We report a novel pressure-driven spin crossover in layered cobalt oxyfluoride Sr2CoO3F with a distorted CoO5 square pyramid loosely bound with a fluoride ion. Upon increasing pressure, the spin state of the Co(III) cation gradually changes from a high spin state (S = 2) to a low spin state (S = 0) accompanied by a anomalously large volume contraction (bulk modulus, 76.8(5) GPa). The spin state change occurs on the CoO5 pyramid in a wide pressure range, but the concomitant gradual shrinkage of the Co–F bond length with pressure gives rise to a polyhedral transformation to the CoO5F octahedron without a structural phase transition, leading to the full conversion to the LS state at 12 GPa. The present results provide new effective strategy to fine-tune electronic properties of mixed anion systems by controlling the covalency in metal-ligand bonds under pressure. PMID:27805031

Numerical simulation of a device with two spin crossover complexes: application for temperature and pressure sensors

NASA Astrophysics Data System (ADS)

Linares, Jorge; Eddine Allal, Salah; Dahoo, Pierre Richard; Garcia, Yann

2017-12-01

The spin-crossover (SCO) phenomenon is related to the ability of a transition metal to change its spin state vs. a given perturbation. For an iron(II) SCO complexes the reversible changes involve the diamagnetic low-spin (S = 0) and the paramagnetic high-spin (HS S = 2) states [1,2,3]. In this contribution we simulate the HS Fraction (nHS) for different set values of temperature and pressure for a device using two SCO complexes with weak elastic interactions. We improve the calculation given by Linares et al. [4], taking also into account different volume (VHS, VLS) changes of the SCO. We perform all the calculation in the frame work of an Ising-like model solved in the mean-field approximation. The two SCO show in the case of “weak elastic interactions”, gradual spin transitions such that both temperature and pressure values can be obtained from the optical observation in the light of calculations discussed in this article.

Femtosecond time-resolved optical and Raman spectroscopy of photoinduced spin crossover: temporal resolution of low-to-high spin optical switching.

PubMed

Smeigh, Amanda L; Creelman, Mark; Mathies, Richard A; McCusker, James K

2008-10-29

A combination of femtosecond electronic absorption and stimulated Raman spectroscopies has been employed to determine the kinetics associated with low-spin to high-spin conversion following charge-transfer excitation of a FeII spin-crossover system in solution. A time constant of tau = 190 +/- 50 fs for the formation of the 5T2 ligand-field state was assigned based on the establishment of two isosbestic points in the ultraviolet in conjunction with changes in ligand stretching frequencies and Raman scattering amplitudes; additional dynamics observed in both the electronic and vibrational spectra further indicate that vibrational relaxation in the high-spin state occurs with a time constant of ca. 10 ps. The results set an important precedent for extremely rapid, formally forbidden (DeltaS = 2) nonradiative relaxation as well as defining the time scale for intramolecular optical switching between two electronic states possessing vastly different spectroscopic, geometric, and magnetic properties.

Nonequilibrium spin crossover in copper phthalocyanine

NASA Astrophysics Data System (ADS)

Siegert, Benjamin; Donarini, Andrea; Grifoni, Milena

2016-03-01

We demonstrate the nonequilibrium tip induced control of the spin state of copper phthalocyanine on an insulator coated substrate. We find that, under the condition of energetic proximity of many-body neutral excited states to the anionic ground state, the system can undergo a population inversion towards these excited states. The resulting state of the system is accompanied by a change in the total spin quantum number. Experimental signatures of the crossover are the appearance of additional nodal planes in the topographical scanning tunneling microscopy images as well as a strong suppression of the current near the center of the molecule. The robustness of the effect against moderate charge conserving relaxation processes has also been tested.

Hysteretic Four-Step Spin Crossover within a Three-Dimensional Porous Hofmann-like Material

DOE Office of Scientific and Technical Information (OSTI.GOV)

Clements, John E.; Price, Jason R.; Neville, Suzanne M.

Materials that display multiple stepped spin crossover (SCO) transitions with accompanying hysteresis present the opportunity for ternary, quaternary, and quinary electronic switching and data storage but are rare in existence. Herein, we present the first report of a four-step hysteretic SCO framework. Single-crystal structure analysis of a porous 3D Hofmann-like material showed long-range ordering of spin states: HS, HS 0.67LS 0.33, HS 0.5LS 0.5, HS 0.33LS 0.67, and LS. These detailed structural studies provide insight into how multistep SCO materials can be rationally designed through control of host–host and host–guest interactions.

Femtosecond Measurements Of Size-Dependent Spin Crossover In FeII(pyz)Pt(CN)4 Nanocrystals

DOE PAGES

Sagar, D. M.; Baddour, Frederick G.; Konold, Patrick; ...

2016-01-07

We report a femtosecond time-resolved spectroscopic study of size-dependent dynamics in nanocrystals (NCs) of Fe(pyz)Pt(CN) 4. We observe that smaller NCs (123 or 78 nm cross section and < 25 nm thickness) exhibit signatures of spin crossover (SCO) with time constants of ~ 5-10 ps whereas larger NCs with 375 nm cross section and 43 nm thickness exhibit a weaker SCO signature accompanied by strong spectral shifting on a ~20 ps time scale. For the small NCs, the fast dynamics appear to result from thermal promotion of residual low-spin states to high-spin states following nonradiative decay, and the size dependencemore » is postulated to arise from differing high-spin vs low-spin fractions in domains residing in strained surface regions. The SCO is less efficient in larger NCs owing to their larger size and hence lower residual LS/HS fractions. Our results suggest that size-dependent dynamics can be controlled by tuning surface energy in NCs with dimensions below ~25 nm for use in energy harvesting, spin switching, and other applications.« less

Correlation between non-Fermi-liquid behavior and superconductivity in (Ca, La)(Fe,Co)As2 iron arsenides: A high-pressure study

NASA Astrophysics Data System (ADS)

Zhou, W.; Ke, F.; Xu, Xiaofeng; Sankar, R.; Xing, X.; Xu, C. Q.; Jiang, X. F.; Qian, B.; Zhou, N.; Zhang, Y.; Xu, M.; Li, B.; Chen, B.; Shi, Z. X.

2017-11-01

Non-Fermi-liquid (NFL) phenomena associated with correlation effects have been widely observed in the phase diagrams of unconventional superconducting families. Exploration of the correlation between the normal state NFL, regardless of its microscopic origins, and the superconductivity has been argued as a key to unveiling the mystery of the high-Tc pairing mechanism. Here we systematically investigate the pressure-dependent in-plane resistivity (ρ ) and Hall coefficient (RH) of a high-quality 112-type Fe-based superconductor Ca1 -xLaxFe1 -yCoyAs2 (x =0.2 ,y =0.02 ). With increasing pressure, the normal-state resistivity of the studied sample exhibits a pronounced crossover from non-Fermi-liquid to Fermi-liquid behaviors. Accompanied with this crossover, Tc is gradually suppressed. In parallel, the extremum in the Hall coefficient RH(T ) curve, possibly due to anisotropic scattering induced by spin fluctuations, is also gradually suppressed. The symbiosis of NFL and superconductivity implies that these two phenomena are intimately related. Further study on the pressure-dependent upper critical field reveals that the two-band effects are also gradually weakened with increasing pressure and reduced to the one-band Werthamer-Helfand-Hohenberg limit in the low-Tc regime. Overall, our paper supports the picture that NFL, multigap, and extreme RH(T ) are all of the same magnetic origin, i.e., the spin fluctuations in the 112 iron arsenide superconductors.

One dimensionalization in the spin-1 Heisenberg model on the anisotropic triangular lattice

NASA Astrophysics Data System (ADS)

Gonzalez, M. G.; Ghioldi, E. A.; Gazza, C. J.; Manuel, L. O.; Trumper, A. E.

2017-11-01

We investigate the effect of dimensional crossover in the ground state of the antiferromagnetic spin-1 Heisenberg model on the anisotropic triangular lattice that interpolates between the regime of weakly coupled Haldane chains (J'≪J ) and the isotropic triangular lattice (J'=J ). We use the density-matrix renormalization group (DMRG) and Schwinger boson theory performed at the Gaussian correction level above the saddle-point solution. Our DMRG results show an abrupt transition between decoupled spin chains and the spirally ordered regime at (J'/J) c˜0.42 , signaled by the sudden closing of the spin gap. Coming from the magnetically ordered side, the computation of the spin stiffness within Schwinger boson theory predicts the instability of the spiral magnetic order toward a magnetically disordered phase with one-dimensional features at (J'/J) c˜0.43 . The agreement of these complementary methods, along with the strong difference found between the intra- and the interchain DMRG short spin-spin correlations for sufficiently large values of the interchain coupling, suggests that the interplay between the quantum fluctuations and the dimensional crossover effects gives rise to the one-dimensionalization phenomenon in this frustrated spin-1 Hamiltonian.

Spin crossover behaviour in Hofmann-like coordination polymer Fe(py)2[Pd(CN)4] with 57Fe Mössbauer spectra

NASA Astrophysics Data System (ADS)

Kitazawa, Takafumi; Kishida, Takanori; Kawasaki, Takeshi; Takahashi, Masashi

2017-11-01

We have prepared the 2D spin crossover complexes Fe(L)2Pd(CN)4 (L = py : 1a; py-D5 : 1b and py-15N : 1c). 1a has been characterised by 57Fe Mossbauer spectroscopic measurements, single crystal X-ray determination and SQUID measurements. The Mössbauer spectra for 1a indicate that the iron(II) spin states are in high spin states at 298 K and are in low spin states at 77 K. The crystal structures of 1a at 298 K and 90 K also show the high spin state and the low spin state respectively, associated with the Fe(II)-N distances. The spin transition temperature range of 1a is higher than that of Fe(py)2Ni(CN)4 since Pd(II) ions are larger and heavier than Ni(II) ions. SQUID data indicate isotope effects among 1a, 1b and 1c are observed in very small shifts of the transition temperatures probably due to larger and heavier Pd(II) ions. The delicate shifts would be associated with subtle balances between different vibrations around Fe(II) atoms and electronic factors.

Parametric representation of open quantum systems and cross-over from quantum to classical environment.

PubMed

Calvani, Dario; Cuccoli, Alessandro; Gidopoulos, Nikitas I; Verrucchi, Paola

2013-04-23

The behavior of most physical systems is affected by their natural surroundings. A quantum system with an environment is referred to as open, and its study varies according to the classical or quantum description adopted for the environment. We propose an approach to open quantum systems that allows us to follow the cross-over from quantum to classical environments; to achieve this, we devise an exact parametric representation of the principal system, based on generalized coherent states for the environment. The method is applied to the s = 1/2 Heisenberg star with frustration, where the quantum character of the environment varies with the couplings entering the Hamiltonian H. We find that when the star is in an eigenstate of H, the central spin behaves as if it were in an effective magnetic field, pointing in the direction set by the environmental coherent-state angle variables (θ, ϕ), and broadened according to their quantum probability distribution. Such distribution is independent of ϕ, whereas as a function of θ is seen to get narrower as the quantum character of the environment is reduced, collapsing into a Dirac-δ function in the classical limit. In such limit, because ϕ is left undetermined, the Von Neumann entropy of the central spin remains finite; in fact, it is equal to the entanglement of the original fully quantum model, a result that establishes a relation between this latter quantity and the Berry phase characterizing the dynamics of the central spin in the effective magnetic field.

Spin fluctations and heavy fermions in the Kondo lattice

DOE Office of Scientific and Technical Information (OSTI.GOV)

Khaliullin, G.G.

1994-09-01

This paper studies the spectrum of the spin and electronic excitations of the Kondo lattice at low temperatures. To avoid unphysical states, the Mattis {open_quotes}drone{close_quotes}-fermion representation for localized spins is employed. First, the known Fermi liquid properties of a single impurity are examined. The behavior of the correlator between a localized spin and the electron spin density at large distances shows that the effective interaction between electrons on the Fermi level and low-energy localized spin fluctuations scales as {rho}{sup {minus}1}, where {rho} is the band-state density. This fact is developed into a renormalization of the band spectrum in a periodicmore » lattice. If the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction between localized spins is much smaller than the Kondo fluctuation frequency {omega}{sub k}, the temperature of the crossover to the single-parameter Fermi liquid mode is determined by {omega}{sub k}. When the RKKY interaction becomes of order {omega}{sub k}, there is a new scale {omega}{sub sf}, the energy of the (antiferromagnetic) paramagnon mode, with {omega}{sub sf}{much_lt}{omega}{sub k}. Here the coherent Fermi liquid regime is realized only below a temperature T{sub coh} of order {omega}{sub sf}, while above T{sub coh} quasiparticle damping exhibits a linear temperature dependence. Finally, the nuclear-spin relaxation rate is calculated. 42 refs.« less

Temperature and field dependent electronic structure and magnetic properties of LaCoO3 and GdCoO3

NASA Astrophysics Data System (ADS)

Ovchinnikov, S. G.; Orlov, Yu. S.; Dudnikov, V. A.

2012-10-01

The transformation of the band structure of LaCoO3 in the applied magnetic field has been theoretically studied. If the field is below its critical value BC≈65 T, the dielectric band gap decreases with the field, thus giving rise to negative magnetoresistance that is highest at T≈300÷500 K. The critical field is related to the crossover between the low- and high-spin terms of Co3+ ions. The spin crossover results in an insulator-metal transition induced by an increase in the magnetic field. Similar calculations have been done for GdCoO3 which is characterized by large spin gap∼2000 K.

The Electronic Structure Signature of the Spin Cross-Over Transition of [Co(dpzca)2

NASA Astrophysics Data System (ADS)

Zhang, Xin; Mu, Sai; Liu, Yang; Luo, Jian; Zhang, Jian; N'Diaye, Alpha T.; Enders, Axel; Dowben, Peter A.

2018-05-01

The unoccupied electronic structure of the spin crossover molecule cobalt (II) N-(2-pyrazylcarbonyl)-2-pyrazinecarboxamide, [Co(dpzca)2] was investigated, using X-ray absorption spectroscopy (XAS) and compared with magnetometry (SQUID) measurements. The temperature dependence of the XAS and molecular magnetic susceptibility χmT are in general agreement for [Co(dpzca)2], and consistent with density functional theory (DFT). This agreement of magnetic susceptibility and X-ray absorption spectroscopy provides strong evidence that the changes in magnetic moment can be ascribed to changes in electronic structure. Calculations show the choice of Coulomb correlation energy U has a profound effect on the electronic structure of the low spin state, but has little influence on the electronic structure of the high spin state. In the temperature dependence of the XAS, there is also evidence of an X-ray induced excited state trapping for [Co(dpzca)2] at 15 K.

Neutron-scattering-based evidence for interacting magnetic excitons in LaCo O 3

DOE Office of Scientific and Technical Information (OSTI.GOV)

El-Khatib, S.; Phelan, D.; Barker, J. G.

Recent progress with the thermally-driven spin-state crossover in LaCoO3 has made it increasingly apparent that the nominally non-magnetic low spin ground state of this material actually hosts novel defect-'based magnetism. This is investigated here via a small-angle neutron scattering (SANS) study of LaCoO3-s crystals. The results provide: (i) the surprising finding that the spin-state crossover is clearly reflected in SANS via quasielastic/inelastic scattering from paramagnetic spin fluctuations/excitations, and (ii) evidence for the formation, likely around oxygen defects, of local entities known as magnetic excitons. The latter generate distinct magnetic scattering below 60 K, providing valuable quantitative information on exciton densitiesmore » and interactions. Potential relevance to the unexpected ferromagnetism recently discovered in epitaxial LaCoO3 films is discussed.« less

Universal Knight shift anomaly in the periodic Anderson model

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jiang, M.; Curro, N. J.; Scalettar, R. T.

Here, we report a Determinant Quantum Monte Carlo investigation which quantifies the behavior of the susceptibility and the entropy in the framework of the periodic Anderson model (PAM), focussing on the evolution with different degree of conduction electron (c) -local moment (f) hybridization. These results capture the behavior observed in several experiments, including the universal behavior of the NMR Knight shift anomaly below the crossover temperature, T*. We find that T* is a measure of the onset of c-f correlations and grows with increasing hybridization. Our results suggest that the NMR Knight shift and spin-lattice relaxation rate measurements in non-Fermimore » liquid materials are strongly influenced by temperature-dependent hybridization processes. Furthermore, our results provide a microscopic basis for the phenomenological two-fluid model of Kondo lattice behavior, and its evolution with pressure and temperature.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gavriliuk, A.G.; Lin, J.F.; Lyubutin, I.S.

The effect of the experimental conditions on the shape of the nuclear resonant forward scattering (NFS) from (Mg{sub 0.75}Fe{sub 0.25})O magnesiowustite has been studied at high pressures up to 100 GPa in diamond anvil cells by the method of the NFS of synchrotron radiation from the Fe-57 nuclei at room temperature. The behavior of the system in the electronic transition of the Fe{sup 2+} ion from the high-spin to low-spin state (spin crossover) near 62 GPa is analyzed as a function of the sample thickness, degree of nonhydrostaticity, and focusing and collimation conditions of a synchrotron beam. It is foundmore » that the inclusion of dynamical beats associated with the sample thickness is very important in the approximation of the experimental NFS spectra. It is shown that the electronic transition occurs in a much narrower pressure range ({+-}6 GPa) rather than in a broad range as erroneously follows from experiments with thick samples under strongly nonhydrostatic conditions.« less

Time-dependent nonequilibrium soft x-ray response during a spin crossover

DOE Office of Scientific and Technical Information (OSTI.GOV)

van Veenendaal, Michel

The rapid development of high-brilliance pulsed X-ray sources with femtosecond time resolution has created a need for a better theoretical understanding of the time-dependent soft-X-ray response of dissipative many-body quantum systems. It is demonstrated how soft-X-ray spectroscopies, such as X-ray absorption and resonant inelastic X-ray scattering at transition-metal L-edges, can provide insight into intersystem crossings, such as a spin crossover. The photoinduced doublet-to-quartet spin crossover on cobalt in Fe-Co Prussian blue analogues is used as an example to demonstrate how the X-ray response is affected by the dissipative nonequilibrium dynamics. The time-dependent soft-X-ray spectra provide a wealth of information thatmore » reflect the changes in the nonequilibrium initial state via continuously changing spectral lineshapes that cannot be decomposed into initial photoexcited and final metastable spectra, strong broadenings, a collapse of clear selection rules during the intersystem crossing, strong fluctuations in the isotropic branching ratio in X-ray absorption, and crystal-field collapse/oscillations and strongly time-dependent anti-Stokes processes in RIXS.« less

Effects of spin crossover on iron isotope fractionation in Earth's mantle

NASA Astrophysics Data System (ADS)

Qin, T.; Shukla, G.; Wu, Z.; Wentzcovitch, R.

2017-12-01

Recent studies have revealed that the iron isotope composition of mid-ocean ridge basalts (MORBs) is +0.1‰ richer in heavy Fe (56Fe) relative to chondrites, while basalts from Mars and Vesta have similar Fe isotopic composition as chondrites. Several hypotheses could explain these observations. For instance, iron isotope fractionation may have occurred during core formation or Earth may have lost some light Fe isotope during the high temperature event in the early Earth. To better understand what drove these isotopic observations, it is important to obtain accurate Fe isotope fractionation factors among mantle and core phases at the relevant P-T conditions. In bridgmanite, the most voluminous mineral in the lower mantle, Fe can occupy more than one crystalline site, be in ferrous and/or ferric states, and may undergo a spin crossover in the lower mantle. Iron isotopic fractionation properties under spin crossover are poorly constrained, while this may be relevant to differentiation of Earth's magma ocean. In this study we address the effect of these multiple states on the iron isotope fractionation factors between mantle and core phases.

Dissipative structure in the photo-induced phase under steady light irradiation in the spin crossover complex.

PubMed

Nishihara, Taishi; Bousseksou, Azzdine; Tanaka, Koichiro

2013-12-16

We report the spatial and temporal dynamics of the photo-induced phase in the iron (II) spin crossover complex Fe(ptz)(6)(BF(4))(2) studied by image measurement under steady light irradiation and transient absorption measurement. The dynamic factors are derived from the spatial and temporal fluctuation of the image in the steady state under light irradiation between 65 and 100 K. The dynamic factors clearly indicate that the fluctuation has a resonant frequency that strongly depends on the temperature, and is proportional to the relaxation rate of the photo-induced phase. This oscillation of the speckle pattern under steady light irradiation is ascribed to the nonlinear interaction between the spin state and the lattice volume at the surface.

Study of. lambda. parameters and crossover phenomena in SU(N) x SU(N) sigma models in two dimensions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shigemitsu, J; Kogut, J B

1981-01-01

The spin system analogues of recent studies of the string tension and ..lambda.. parameters of SU(N) gauge theories in 4 dimensions are carried out for the SU(N) x SU(N) and O(N) models in 2 dimensions. The relations between the ..lambda.. parameters of both the Euclidean and Hamiltonian formulation of the lattice models and the ..lambda.. parameter of the continuum models are obtained. The one loop finite renormalization of the speed of light in the lattice Hamiltonian formulations of the O(N) and SU(N) x SU(N) models is calculated. Strong coupling calculations of the mass gaps of these spin models are donemore » for all N and the constants of proportionality between the gap and the ..lambda.. parameter of the continuum models are obtained. These results are contrasted with similar calculations for the SU(N) gauge models in 3+1 dimensions. Identifying suitable coupling constants for discussing the N ..-->.. infinity limits, the numerical results suggest that the crossover from weak to strong coupling in the lattice O(N) models becomes less abrupt as N increases while the crossover for the SU(N) x SU(N) models becomes more abrupt. The crossover in SU(N) gauge theories also becomes more abrupt with increasing N, however, at an even greater rate than in the SU(N) x SU(N) spin models.« less

Antiferromagnetic spin correlations and pseudogaplike behavior in Ca(Fe 1-xCo x) 2As 2 studied by 75As nuclear magnetic resonance and anisotropic resistivity

DOE PAGES

Cui, J.; Roy, B.; Tanatar, M. A.; ...

2015-11-06

We report 75As nuclear magnetic resonance (NMR) measurements of single-crystalline Ca(Fe 1–xCo x) 2As 2 (x=0.023, 0.028, 0.033, and 0.059) annealed at 350°C for 7 days. From the observation of a characteristic shape of 75As NMR spectra in the stripe-type antiferromagnetic (AFM) state, as in the case of x=0 (T N=170 K), clear evidence for the commensurate AFM phase transition with the concomitant structural phase transition is observed in x=0.023 (T N=106 K) and x=0.028 (T N=53 K). Through the temperature dependence of the Knight shifts and the nuclear spin lattice relaxation rates (1/T 1), although stripe-type AFM spin fluctuationsmore » are realized in the paramagnetic state as in the case of other iron pnictide superconductors, we found a gradual decrease of the AFM spin fluctuations below a crossover temperature T* that was nearly independent of Co-substitution concentration, and it is attributed to a pseudogaplike behavior in the spin excitation spectra of these systems. The T* feature finds correlation with features in the temperature-dependent interplane resistivity, ρc(T), but not with the in-plane resistivity ρa(T). The temperature evolution of anisotropic stripe-type AFM spin fluctuations is tracked in the paramagnetic and pseudogap phases by the 1/T 1 data measured under magnetic fields parallel and perpendicular to the c axis. As a result, based on our NMR data, we have added a pseudogaplike phase to the magnetic and electronic phase diagram of Ca(Fe 1–xCo x) 2As 2.« less

First-principles study of intermediate-spin ferrous iron in the Earth's lower mantle

NASA Astrophysics Data System (ADS)

Hsu, Han; Wentzcovitch, Renata M.

2014-11-01

Spin crossover of iron is of central importance in solid Earth geophysics. It impacts all physical properties of minerals that altogether constitute ˜95 vol% of the Earth's lower mantle: ferropericlase [(Mg,Fe)O] and Fe-bearing magnesium silicate (MgSiO3) perovskite. Despite great strides made in the past decade, the existence of an intermediate-spin (IS) state in ferrous iron (Fe2 +) (with total electron spin S =1 ) and its possible role in the pressure-induced spin crossover in these lower-mantle minerals still remain controversial. Using density functional theory + self-consistent Hubbard U (DFT+Usc ) calculations, we investigate all possible types of IS states of Fe2 + in (Mg,Fe)O and (Mg,Fe)SiO3 perovskite. Among the possible IS states in these minerals, the most probable IS state has an electronic configuration that significantly reduces the electron overlap and the iron nuclear quadrupole splitting (QS). These most probable IS states, however, are still energetically disfavored, and their QSs are inconsistent with Mössbauer spectra. We therefore conclude that IS Fe2 + is highly unlikely in the Earth's lower mantle.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kung, Y. F.; Bazin, C.; Wohlfeld, K.

Using determinant quantum Monte Carlo (DQMC) simulations, we systematically study the doping dependence of the crossover from one to two dimensions and its impact on the magnetic properties of the Hubbard model. A square lattice of chains is used, in which the dimensionality can be tuned by varying the interchain coupling t ⊥. The dynamical spin structure factor and static quantities, such as the static spin susceptibility and nearest-neighbor spin correlation function, are characterized in the one- and two-dimensional limits as a benchmark. When the dimensionality is tuned between these limits, the magnetic properties, while evolving smoothly from one tomore » two dimensions, drastically change regardless of the doping level. This suggests that the spin excitations in the two-dimensional Hubbard model, even in the heavily doped case, cannot be explained using the spinon picture known from one dimension. In conclusion, the DQMC calculations are complemented by cluster perturbation theory studies to form a more complete picture of how the crossover occurs as a function of doping and how doped holes impact magnetic order.« less

Finite size induces crossover temperature in growing spin chains

NASA Astrophysics Data System (ADS)

Sienkiewicz, Julian; Suchecki, Krzysztof; Hołyst, Janusz A.

2014-01-01

We introduce a growing one-dimensional quenched spin model that bases on asymmetrical one-side Ising interactions in the presence of external field. Numerical simulations and analytical calculations based on Markov chain theory show that when the external field is smaller than the exchange coupling constant J there is a nonmonotonous dependence of the mean magnetization on the temperature in a finite system. The crossover temperature Tc corresponding to the maximal magnetization decays with system size, approximately as the inverse of the Lambert W function. The observed phenomenon can be understood as an interplay between the thermal fluctuations and the presence of the first cluster determined by initial conditions. The effect exists also when spins are not quenched but fully thermalized after the attachment to the chain. By performing tests on real data we conceive the model is in part suitable for a qualitative description of online emotional discussions arranged in a chronological order, where a spin in every node conveys emotional valence of a subsequent post.

Finite size induces crossover temperature in growing spin chains.

PubMed

Sienkiewicz, Julian; Suchecki, Krzysztof; Hołyst, Janusz A

2014-01-01

We introduce a growing one-dimensional quenched spin model that bases on asymmetrical one-side Ising interactions in the presence of external field. Numerical simulations and analytical calculations based on Markov chain theory show that when the external field is smaller than the exchange coupling constant J there is a nonmonotonous dependence of the mean magnetization on the temperature in a finite system. The crossover temperature Tc corresponding to the maximal magnetization decays with system size, approximately as the inverse of the Lambert W function. The observed phenomenon can be understood as an interplay between the thermal fluctuations and the presence of the first cluster determined by initial conditions. The effect exists also when spins are not quenched but fully thermalized after the attachment to the chain. By performing tests on real data we conceive the model is in part suitable for a qualitative description of online emotional discussions arranged in a chronological order, where a spin in every node conveys emotional valence of a subsequent post.

Hysteresis, nucleation and growth phenomena in spin-crossover solids

NASA Astrophysics Data System (ADS)

Ridier, Karl; Molnár, Gábor; Salmon, Lionel; Nicolazzi, William; Bousseksou, Azzedine

2017-12-01

The observation and the study of first-order phase transitions in cooperative spin-crossover (SCO) solids exhibiting hysteresis behaviours are of particular interest and currently constitute a burgeoning area in the field of bistable molecular materials. The understanding and the control of the transition mechanisms (nucleation and growth processes) and their dynamics within the hysteresis region appear to be a general and appealing problem from a fundamental point of view and for technological applications as well. This review reports on the recent progresses and most important findings made on the spatiotemporal dynamics of the spin transition in SCO solids, particularly through the universal nucleation and growth process. Both thermally induced and light-induced spin transitions are discussed. We open up this review to the central question of the evolution of the transition mechanisms and dynamics in SCO nano-objects, which constitute promising systems to reach ultra-fast switching, and the experimental issues inherent to such studies at the micro- and nanometric scale.

Topological Properties and the Dynamical Crossover from Mixed-Valence to Kondo-Lattice Behavior in the Golden Phase of SmS.

PubMed

Kang, Chang-Jong; Choi, Hong Chul; Kim, Kyoo; Min, B I

2015-04-24

We have investigated temperature-dependent behaviors of electronic structure and resistivity in a mixed-valent golden phase of SmS, based on the dynamical mean-field-theory band-structure calculations. Upon cooling, the coherent Sm 4f bands are formed to produce the hybridization-induced pseudogap near the Fermi level, and accordingly the topology of the Fermi surface is changed to exhibit a Lifshitz-like transition. The surface states emerging in the bulk gap region are found to be not topologically protected states but just typical Rashba spin-polarized states, indicating that SmS is not a topological Kondo semimetal. From the analysis of anomalous resistivity behavior in SmS, we have identified universal energy scales, which characterize the Kondo-mixed-valent semimetallic systems.

Kinetic effects on double hysteresis in spin crossover molecular magnets analyzed with first order reversal curve diagram technique

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stan, Raluca-Maria; Gaina, Roxana; Enachescu, Cristian, E-mail: cristian.enachescu@uaic.ro, E-mail: radu.tanasa@uaic.ro

2015-05-07

In this paper, we analyze two types of hysteresis in spin crossover molecular magnets compounds in the framework of the First Order Reversal Curve (FORC) method. The switching between the two stable states in these compounds is accompanied by hysteresis phenomena if the intermolecular interactions are higher than a threshold. We have measured the static thermal hysteresis (TH) and the kinetic light induced thermal hysteresis (LITH) major loops and FORCs for the polycrystalline Fe(II) spin crossover compound [Fe{sub 1−x}Zn{sub x}(bbtr){sub 3}](ClO{sub 4}){sub 2} (bbtr = 1,4-di(1,2,3-triazol-1-yl)butane), either in a pure state (x = 0) or doped with Zn ions (x = 0.33) considering different sweeping rates.more » Here, we use this method not only to infer the domains distribution but also to disentangle between kinetic and static components of the LITH and to estimate the changes in the intermolecular interactions introduced by dopants. We also determined the qualitative relationship between FORC distributions measured for TH and LITH.« less

Structural, thermal, and magnetic study of solvation processes in spin-crossover [Fe(bpp)(2)][Cr(L)(ox)(2)](2).nH(2)O complexes.

PubMed

Clemente-León, Miguel; Coronado, Eugenio; Giménez-López, M Carmen; Romero, Francisco M

2007-12-24

The influence of lattice water in the magnetic properties of spin-crossover [Fe(bpp)2]X2.nH2O salts [bpp = 2,6-bis(pyrazol-3-yl)pyridine] is well-documented. In most cases, it stabilizes the low-spin state compared to the anhydrous compound. In other cases, it is rather the contrary. Unraveling this mystery implies the study of the microscopic changes that accompany the loss of water. This might be difficult from an experimental point of view. Our strategy is to focus on some salts that undergo a nonreversible dehydration-hydration process without loss of crystallinity. By comparison of the structural and magnetic properties of original and rehydrated samples, several rules concerning the role of water at the microscopic level can be deduced. This paper reports on the crystal structure, thermal studies, and magnetic properties of [Fe(bpp)2][Cr(bpy)(ox)2]2.2H2O (1), [Fe(bpp)2][Cr(phen)(ox)2]2.0.5H2O.0.5MeOH (2), and [Fe(bpp)2][Cr(phen)(ox)2]2.5.5H2O.2.5MeOH (3). Salt 1 contains both high-spin (HS) and low-spin (LS) Fe2+ cations in a 1:1 ratio. Dehydration yields the anhydrous spin-crossover compound with T1/2 downward arrow = 353 K and T1/2 upward arrow = 369 K. Rehydration affords the dihydrate [Fe(bpp)2][Cr(bpy)(ox)2]2.2H2O (1r) with 100% HS Fe2+ sites. Salt 2 also contains both HS and LS Fe2+ cations in a 1:1 ratio. Dehydration yields the anhydrous spin-crossover compound with T1/2 downward arrow = 343 K and T1/2 upward arrow = 348 K. Rehydration affords [Fe(bpp)2][Cr(phen)(ox)2]2.0.5H2O (2r) with 72% Fe2+ sites in the LS configuration. The structural, magnetic, and thermal properties of these rehydrated compounds 1r and 2r are also discussed. Finally, 1 has been dehydrated and resolvated with MeOH to give [Fe(bpp)2][Cr(bpy)(ox)2]2.MeOH (1s) with 33% HS Fe2+ sites. The influence of the guest solvent in the Fe2+ spin state can anticipate the future applications of these compounds in solvent sensing.

Spin-state crossover and low-temperature magnetic state in yttrium-doped Pr0.7Ca0.3CoO3

NASA Astrophysics Data System (ADS)

Knížek, K.; Hejtmánek, J.; Maryško, M.; Novák, P.; Šantavá, E.; Jirák, Z.; Naito, T.; Fujishiro, H.; de la Cruz, Clarina

2013-12-01

The structural and magnetic properties of two mixed-valence cobaltites with a formal population of 0.30 Co4+ ions per f.u., (Pr1-yYy)0.7Ca0.3CoO3 (y=0 and 0.15), have been studied down to very low temperatures by means of high-resolution neutron diffraction, SQUID magnetometry, and heat-capacity measurements. The results are interpreted within the scenario of the spin-state crossover from a room-temperature mixture of the intermediate-spin Co3+ and low-spin Co4+ (IS/LS) to the LS/LS mixture in the sample ground states. In contrast to the yttrium-free y=0 that retains the metallic-like character and exhibits ferromagnetic (FM) ordering below 55 K, the doped system y=0.15 undergoes a first-order metal-insulator transition at 132 K, during which not only the crossover to low-spin states but also a partial electron transfer from Pr3+ 4f to cobalt 3d states takes place simultaneously. Taking into account the nonmagnetic character of LS Co3+, such a valence shift electronic transition causes a magnetic dilution, formally to 0.12 LS Co4+ or 0.12 t2g hole spins per f.u., which is the reason for an insulating, highly nonuniform magnetic ground state without long-range order. Nevertheless, even in that case there exists a relatively strong molecular field distributed over all the crystal lattice. It is argued that the spontaneous FM order in y=0 and the existence of strong FM correlations in y=0.15 apparently contradict the single t2g band character of LS/LS phase. The explanation we suggest relies on a model of the defect-induced, itinerant hole-mediated magnetism, where the defects are identified with the magnetic high-spin Co3+ species stabilized near oxygen vacancies.

Doping evolution of spin and charge excitations in the Hubbard model

DOE PAGES

Kung, Y. F.; Nowadnick, E. A.; Jia, C. J.; ...

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

Multiple crossovers between positive and negative magnetoresistance versus field due to fragile spin structure in metallic GdPd 3 [Oscillating magnetoresistance due to fragile spin structure in metallic GdPd 3

DOE PAGES

Pandey, Abhishek; Mazumdar, Chandan; Ranganathan, R.; ...

2017-02-17

Here, studies on the phenomenon of magnetoresistance (MR) have produced intriguing and application-oriented outcomes for decades–colossal MR, giant MR and recently discovered extremely large MR of millions of percents in semimetals can be taken as examples. We report here the discovery of novel multiple sign changes versus applied magnetic field of the MR in the cubic intermetallic compound GdPd 3. Our study shows that a very strong correlation between magnetic, electrical and magnetotransport properties is present in this compound. The magnetic structure in GdPd 3 is highly fragile since applied magnetic fields of moderate strength significantly alter the spin arrangementmore » within the system–a behavior that manifests itself in the oscillating MR. Intriguing magnetotransport characteristics of GdPd 3 are appealing for field-sensitive device applications, especially if the MR oscillation could materialize at higher temperature by manipulating the magnetic interaction through perturbations caused by chemical substitutions.« less

Multiple crossovers between positive and negative magnetoresistance versus field due to fragile spin structure in metallic GdPd 3 [Oscillating magnetoresistance due to fragile spin structure in metallic GdPd 3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pandey, Abhishek; Mazumdar, Chandan; Ranganathan, R.

Here, studies on the phenomenon of magnetoresistance (MR) have produced intriguing and application-oriented outcomes for decades–colossal MR, giant MR and recently discovered extremely large MR of millions of percents in semimetals can be taken as examples. We report here the discovery of novel multiple sign changes versus applied magnetic field of the MR in the cubic intermetallic compound GdPd 3. Our study shows that a very strong correlation between magnetic, electrical and magnetotransport properties is present in this compound. The magnetic structure in GdPd 3 is highly fragile since applied magnetic fields of moderate strength significantly alter the spin arrangementmore » within the system–a behavior that manifests itself in the oscillating MR. Intriguing magnetotransport characteristics of GdPd 3 are appealing for field-sensitive device applications, especially if the MR oscillation could materialize at higher temperature by manipulating the magnetic interaction through perturbations caused by chemical substitutions.« less

The role of iron(II) dilution in the magnetic and photomagnetic properties of the series [Fe(x)Zn(1-x)(bpp)₂](NCSe)₂.

PubMed

Baldé, Chérif; Desplanches, Cédric; Le Gac, Fréderic; Guionneau, Philippe; Létard, Jean-François

2014-06-07

The effects of metal dilution on the spin-crossover behavior of iron(II) in the mixed crystal series [Fe(x)Zn(1-x)(bpp)2](NCSe)2 (bpp = 2,6-bis(pyrazol-3-yl)pyridine) have been studied using magnetic susceptibility, photomagnetism and diffuse reflectivity measurements. For each mixed-crystal system, the thermal spin transition temperature, T(1/2), and the relaxation temperature of the photo-induced high-spin state, T(LIESST), have been systematically determined. It appears that T(1/2) decreases with the metal dilution while T(LIESST) remains unchanged. Dilution also tends to decrease the hysteresis width and smooth the transition curves. These effects were discussed first qualitatively and then quantitatively on the basis of a kinetic study governing the photo-induced back conversion taking into account the relative sizes of Zn(II) and Fe(II) ions. Interestingly, single crystals were obtained for [Fe(0.6)Zn(0.4)(bpp)2](NCSe)2 allowing the X-ray diffraction crystal-structure determination.

First iron and cobalt(II) hexabromoclathrochelates: structural, magnetic, redox, and electrocatalytic behavior.

PubMed

Dolganov, Alexander V; Belov, Alexander S; Novikov, Valentin V; Vologzhanina, Anna V; Romanenko, Galina V; Budnikova, Yulia G; Zelinskii, Genrikh E; Buzin, Michail I; Voloshin, Yan Z

2015-02-07

Template condensation of dibromoglyoxime with n-butylboronic acid on the corresponding metal ion as a matrix under vigorous reaction conditions afforded iron and cobalt(ii) hexabromoclathrochelates. The paramagnetic cobalt clathrochelate was found to be a low-spin complex at temperatures below 100 K, with a gradual increase in the effective magnetic moment at higher temperatures due to the temperature 1/2↔3/2 spin crossover and a gap caused by the structure phase transition. The multitemperature X-ray and DSC studies of this complex and its iron(ii)-containing analog also showed temperature structural transitions. The variation of an encapsulated metal ion's radius, electronic structure and spin state caused substantial differences in the geometry of its coordination polyhedron; these differences increase with the decrease in temperature due to Jahn-Teller distortion of the encapsulated cobalt(ii) ion with an electronic configuration d(7). As follows from CV and GC data, these cage iron and cobalt complexes undergo both oxidation and reduction quasireversibly, and showed an electrocatalytic activity for hydrogen production in different producing systems.

Helical order and multiferroicity in the S =1/2 quasi-kagome system KCu3As2O7(OD)3

NASA Astrophysics Data System (ADS)

Nilsen, G. J.; Okamoto, Y.; Ishikawa, H.; Simonet, V.; Colin, C. V.; Cano, A.; Chapon, L. C.; Hansen, T.; Mutka, H.; Hiroi, Z.

2014-04-01

Several Cu2+ hydroxide minerals have been recently identified as candidate realizations of the S=1/2 kagome Heisenberg model. In this context, we have studied the distorted system KCu3As2O7(OD)3 using neutron scattering and bulk measurements. Although the distortion favors magnetic order over a spin liquid ground state, refinement of the magnetic diffraction pattern below TN1=7.05(5) K yields a complex helical structure with k =(0.77,0,0.11). This structure, as well as the spin excitation spectrum, are well described by a classical Heisenberg model with ferromagnetic nearest neighbor couplings. Multiferroicity is observed below TN1, with an unusual crossover between improper and pseudoproper behavior occurring at TN2=5.5 K. The polarization at T =2 K is P =1.5μCm-2. The properties of KCu3As2O7(OD)3 highlight the variety of physics which arise from the interplay of spin and orbital degrees of freedom in Cu2+ kagome systems.

Time-dependent nonequilibrium soft x-ray response during a spin crossover

NASA Astrophysics Data System (ADS)

van Veenendaal, Michel

2018-03-01

A theoretical framework is developed for better understanding the time-dependent soft-x-ray response of dissipative quantum many-body systems. It is shown how x-ray absorption and resonant inelastic x-ray scattering (RIXS) at transition-metal L edges can provide insight into ultrafast intersystem crossings of importance for energy conversion, ultrafast magnetism, and catalysis. The photoinduced doublet-to-quartet spin crossover on cobalt in Fe-Co Prussian blue analogs is used as a model system to demonstrate how the x-ray response is affected by the nonequilibrium dynamics on a femtosecond time scale. Changes in local spin and symmetry and the underlying mechanism are reflected in strong broadenings, a collapse of clear selection rules during the intersystem crossing, fluctuations in the isotropic branching ratio in x-ray absorption, crystal-field collapse and/or oscillations, and time-dependent anti-Stokes processes in RIXS.

Opposite Surface and Bulk Solvatochromic Effects in a Molecular Spin-Crossover Compound Revealed by Ambient Pressure X-ray Absorption Spectroscopy.

PubMed

Borgatti, Francesco; Torelli, Piero; Brucale, Marco; Gentili, Denis; Panaccione, Giancarlo; Castan Guerrero, Celia; Schäfer, Bernhard; Ruben, Mario; Cavallini, Massimiliano

2018-03-27

We investigate the solvatochromic effect of a Fe-based spin-crossover (SCO) compound via ambient pressure soft X-ray absorption spectroscopy (AP-XAS) and atomic force microscopy (AFM). AP-XAS provides the direct evidence of the spin configuration for the Fe(II) 3d states of the SCO material upon in situ exposure to specific gas or vapor mixtures; concurrent changes in nanoscale topography and mechanical characteristics are revealed via AFM imaging and AFM-based force spectroscopy, respectively. We find that exposing the SCO material to gaseous helium promotes an effective decrease of the transition temperature of its surface layers, while the exposure to methanol vapor causes opposite surfacial and bulk solvatochromic effects. Surfacial solvatochromism is accompanied by a dramatic reduction of the surface layers stiffness. We propose a rationalization of the observed effects based on interfacial dehydration and solvation phenomena.

Selecting the spin crossover profile with controlled crystallization of mononuclear Fe(iii) polymorphs.

PubMed

Vicente, Ana I; Ferreira, Liliana P; Carvalho, Maria de Deus; Rodrigues, Vítor H N; Dîrtu, Marinela M; Garcia, Yann; Calhorda, Maria José; Martinho, Paulo N

2018-05-08

Two polymorphic species of the [Fe(5-Br-salEen)2]ClO4 compound were obtained, each of them being selectively recovered after evaporation of the solvent at a controlled rate. While polymorph 1a is formed during slow evaporation, fast evaporation favors polymorph 1b. The importance of the evaporation rate was recognized after detailed studies of the reaction temperature, solvent evaporation rate and crystallization temperature effects. The complex in the new polymorphic form 1a showed an abrupt spin crossover at 172 K with a small 1 K hysteresis window and over a narrow 10 K range. 57Fe Mössbauer spectroscopy and differential scanning calorimetry, complemented by X-ray studies for both the high-spin and low-spin forms, were used to further characterize the new polymorphic phase 1a. Both polymorphs are based on the same Fe(iii) complex cation hydrogen bonded to the perchlorate anion. These units are loosely bound in the crystals via weak interactions. In the new polymorph 1a, the hydrogen bonds are stronger, while the weak hydrogen and halogen bonds, as well as π-π stacking, create a cooperative network, not present in 1b, responsible for the spin transition profile.

Hydrogen-bonded networks of [Fe(bpp)2]2+ spin crossover complexes and dicarboxylate anions: structural and photomagnetic properties.

PubMed

Jornet-Mollá, Verónica; Duan, Yan; Giménez-Saiz, Carlos; Waerenborgh, João C; Romero, Francisco M

2016-11-28

The paper reports the syntheses, crystal structures, thermal and (photo)magnetic properties of spin crossover salts of formula [Fe(bpp) 2 ](C 6 H 8 O 4 )·4H 2 O (1·4H 2 O), [Fe(bpp) 2 ](C 8 H 4 O 4 )·2CH 3 OH·H 2 O (2·2MeOH·H 2 O) and [Fe(bpp) 2 ](C 8 H 4 O 4 )·5H 2 O (2·5H 2 O) (bpp = 2,6-bis(pyrazol-3yl)pyridine; C 6 H 8 O 4 = adipate dianion; C 8 H 4 O 4 = terephthalate dianion). The salts exhibit an intricate network of hydrogen bonds between low-spin iron(ii) complexes and carboxylate dianions, with solvent molecules sitting in the voids. Desolvation is accompanied by a low-spin (LS) to high-spin (HS) transformation in the materials. The dehydrated phase 2 undergoes a two-step transition with a second step showing thermal hysteresis (T 1/2 ↑ = 139 K and T 1/2 ↓ = 118 K). 2 displays a quantitative LS to HS photomagnetic conversion, with a T(LIESST) value of 63 K.

Equilibrium, metastability, and hysteresis in a model spin-crossover material with nearest-neighbor antiferromagnetic-like and long-range ferromagnetic-like interactions

DOE PAGES

Rikvold, Per Arne; Brown, Gregory; Miyashita, Seiji; ...

2016-02-16

Phase diagrams and hysteresis loops were obtained by Monte Carlo simulations and a mean- field method for a simplified model of a spin-crossovermaterialwith a two-step transition between the high-spin and low-spin states. This model is a mapping onto a square-lattice S = 1/2 Ising model with antiferromagnetic nearest-neighbor and ferromagnetic Husimi-Temperley ( equivalent-neighbor) long-range interactions. Phase diagrams obtained by the two methods for weak and strong long-range interactions are found to be similar. However, for intermediate-strength long-range interactions, the Monte Carlo simulations show that tricritical points decompose into pairs of critical end points and mean-field critical points surrounded by horn-shapedmore » regions of metastability. Hysteresis loops along paths traversing the horn regions are strongly reminiscent of thermal two-step transition loops with hysteresis, recently observed experimentally in several spin-crossover materials. As a result, we believe analogous phenomena should be observable in experiments and simulations for many systems that exhibit competition between local antiferromagnetic-like interactions and long-range ferromagnetic-like interactions caused by elastic distortions.« less

Properties of Prussian blue materials manifested in molecular complexes: observation of cyanide linkage isomerism and spin-crossover behavior in pentanuclear cyanide clusters.

PubMed

Shatruk, Mikhail; Dragulescu-Andrasi, Alina; Chambers, Kristen E; Stoian, Sebastian A; Bominaar, Emile L; Achim, Catalina; Dunbar, Kim R

2007-05-16

Pentanuclear, cyanide-bridged clusters [M(tmphen)2]3[M'(CN)6]2 (M/M' = Zn/Cr (1), Zn/Fe (2), Fe/Fe (3), Fe/Co (4), and Fe/Cr (5); tmphen = 3,4,7,8-tetramethyl-1,10-phenanthroline) were prepared by combining [M'III(CN)6]3- anions with mononuclear complexes of MII ions with two capping tmphen ligands. The clusters consist of a trigonal bipyramidal (TBP) core with three MII ions in the equatorial positions and two M'III ions in the axial positions. Compounds 1-4 are isostructural and crystallize in the monoclinic space group P21/c. Complex 5 crystallizes in the enantiomorphic space group P3221. The magnetic properties of compounds 1 and 2 reflect the contributions of the individual [CrIII(CN)6]3- and [FeIII(CN)6]3- ions. The FeII ions in compounds 3 and 4 exhibit a gradual, temperature-induced spin transition between high spin (HS) and low spin (LS), as determined by the combination of Mössbauer spectroscopy, magnetic measurements, and single-crystal X-ray studies. The investigation of compound 5 by these methods and by IR spectroscopy indicates that cyanide linkage isomerism occurs during cluster formation. The magnetic behavior of 5 is determined by weak ferromagnetic coupling between the axial CrIII centers mediated by the equatorial diamagnetic FeII ions. Mössbauer spectra collected in the presence of a high applied field have allowed, for the first time, the direct experimental observation of uncompensated spin density at diamagnetic metal ions that bridge paramagnetic metal ions.

Elasticity of ferropericlase across the spin crossover in the Earth’s lower mantle

DOE PAGES

Yang, Jing; Tong, Xinyue; Lin, Jung-Fu; ...

2015-12-01

Knowing the elasticity of ferropericlase across the spin transition can help explain seismic and mineralogical models of the lower-mantle including the origin of seismic heterogeneities in the middle to lowermost parts of the lower mantle1–4. However, the effects of spin transition on full elastic constants of ferropericlase remain experimentally controversial due to technical challenges in directly measuring sound velocities under lower-mantle conditions1–5. Here we have reliably measured both V P and V S of a single-crystal ferropericlase ((Mg 0.92,Fe 0.08)O) using complementary Brillouin Light Scattering and Impulsive Stimulated Light Scattering coupled with a diamond anvil cell up to 96 GPa.more » The derived elastic constants show drastically softened C 11 and C 12 within the spin transition at 40–60 GPa while C 44 is not affected. The spin transition is associated with a significant reduction of the aggregate V P/V S via the aggregate V P softening because V S softening does not visibly occur within the transition. Based on thermoelastic modelling along an expected geotherm, the spin crossover in ferropericlase can contribute to 2% reduction in V P/V S in a pyrolite mineralogical model in mid lower-mantle. Our results indicate that the middle to lowermost parts of the lower-mantle would exhibit enhanced seismic heterogeneities due to the occurrence of the mixed-spin and low-spin ferropericlase.« less

Non-Fermi-liquid to Fermi-liquid transports in iron-pnictide Ba(Fe1-x Co x )2As2 and the electronic correlation strength in superconductors newly probed by the normal-state Hall angle

NASA Astrophysics Data System (ADS)

Wang, L. M.; Wang, Chih-Yi; Zen, Sha-Min; Chang, Jin-Yuan; Kuo, C. N.; Lue, C. S.; Chang, L. J.; Su, Y.; Wolf, Th; Adelmann, P.

2017-03-01

Electrical transports in iron-pnictide Ba(Fe1-x Co x )2As2 (BFCA) single crystals are heavily debated in terms of the hidden Fermi-liquid (HFL) and holographic theories. Both HFL and holographic theories provide consistent physic pictures and propose a universal expression of resistivity to describe the crossover of transports from the non-Fermi-liquid (FL) to FL behavior in these so-called ‘strange metal’ systems. The deduced spin exchange energy J and model-dependent energy scale W in BFCA are almost the same, or are of the same order of several hundred Kelvin for over-doped BFCA, which is in agreement with the HFL theory. Moreover, a drawn line of W/3.5 for BFCA in the higher-doping region up to the right demonstrates the crossover from non-FL-like behavior to FL-like behavior at high doping, and shows a new phase diagram of BFCA. The electronic correlation strength in superconductors has been newly probed by the normal-state Hall angle, which found that, for the first time, correlation strength can be characterized by the ratios of T c to the Fermi temperature T F, J/T F, and the transverse mass to longitudinal mass.

Accelerating Chemical Discovery with Machine Learning: Simulated Evolution of Spin Crossover Complexes with an Artificial Neural Network.

PubMed

Janet, Jon Paul; Chan, Lydia; Kulik, Heather J

2018-03-01

Machine learning (ML) has emerged as a powerful complement to simulation for materials discovery by reducing time for evaluation of energies and properties at accuracy competitive with first-principles methods. We use genetic algorithm (GA) optimization to discover unconventional spin-crossover complexes in combination with efficient scoring from an artificial neural network (ANN) that predicts spin-state splitting of inorganic complexes. We explore a compound space of over 5600 candidate materials derived from eight metal/oxidation state combinations and a 32-ligand pool. We introduce a strategy for error-aware ML-driven discovery by limiting how far the GA travels away from the nearest ANN training points while maximizing property (i.e., spin-splitting) fitness, leading to discovery of 80% of the leads from full chemical space enumeration. Over a 51-complex subset, average unsigned errors (4.5 kcal/mol) are close to the ANN's baseline 3 kcal/mol error. By obtaining leads from the trained ANN within seconds rather than days from a DFT-driven GA, this strategy demonstrates the power of ML for accelerating inorganic material discovery.

Mott-metal transition in layered perovskite iridate thin films via field-effect doping

NASA Astrophysics Data System (ADS)

Cheema, Suraj; Turcaud, Jeremy; Nelson, Chris; Salahuddin, Sayeef; Ramesh, Ramamoorthy

We report on electrostatic gating of spin-orbit coupled Mott insulator Sr2IrO4 (Sr214) via ferroelectric field effect doping. Field effect doping has been used to modulate electronic phenomena in emerging 2D systems and strongly correlated oxides, but 5 d systems with large spin-orbit coupling have yet to be explored. Upon switching the polarization field of ferroelectric Pb(Zr20Ti80)O3 (PZT) to the down-poled (electron-accumulation) state, temperature-dependent resistivity measurements indicate extremely metallic behavior in the ultrathin Sr214 channel. This work successfully closes the Mott gap in Sr214 in a ''clean'' doping environment free of chemical disorder, thereby strengthening the link to the isostrucutral high-Tc cuprates, as Sr214 has been predicted to host d-wave superconductivity upon electron doping the parent antiferromagnetic insulating phase. Furthermore, the metallic behavior in Sr214 persists for thickness beyond the expected screening length, suggestive of a collective carrier delocalization mechanism. Electrostatically doped carriers prove to be a useful method for tuning the competition between spin-orbit and Coulomb interactions in order to trigger novel phase transitions, such as the Mott-metal crossover. This work was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy, under Contract No. DE-AC02-05CH11231.

Numerically exact full counting statistics of the nonequilibrium Anderson impurity model

NASA Astrophysics Data System (ADS)

Ridley, Michael; Singh, Viveka N.; Gull, Emanuel; Cohen, Guy

2018-03-01

The time-dependent full counting statistics of charge transport through an interacting quantum junction is evaluated from its generating function, controllably computed with the inchworm Monte Carlo method. Exact noninteracting results are reproduced; then, we continue to explore the effect of electron-electron interactions on the time-dependent charge cumulants, first-passage time distributions, and n -electron transfer distributions. We observe a crossover in the noise from Coulomb blockade to Kondo-dominated physics as the temperature is decreased. In addition, we uncover long-tailed spin distributions in the Kondo regime and analyze queuing behavior caused by correlations between single-electron transfer events.

Numerically exact full counting statistics of the nonequilibrium Anderson impurity model

DOE PAGES

Ridley, Michael; Singh, Viveka N.; Gull, Emanuel; ...

2018-03-06

The time-dependent full counting statistics of charge transport through an interacting quantum junction is evaluated from its generating function, controllably computed with the inchworm Monte Carlo method. Exact noninteracting results are reproduced; then, we continue to explore the effect of electron-electron interactions on the time-dependent charge cumulants, first-passage time distributions, and n-electron transfer distributions. We observe a crossover in the noise from Coulomb blockade to Kondo-dominated physics as the temperature is decreased. In addition, we uncover long-tailed spin distributions in the Kondo regime and analyze queuing behavior caused by correlations between single-electron transfer events

Numerically exact full counting statistics of the nonequilibrium Anderson impurity model

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ridley, Michael; Singh, Viveka N.; Gull, Emanuel

The time-dependent full counting statistics of charge transport through an interacting quantum junction is evaluated from its generating function, controllably computed with the inchworm Monte Carlo method. Exact noninteracting results are reproduced; then, we continue to explore the effect of electron-electron interactions on the time-dependent charge cumulants, first-passage time distributions, and n-electron transfer distributions. We observe a crossover in the noise from Coulomb blockade to Kondo-dominated physics as the temperature is decreased. In addition, we uncover long-tailed spin distributions in the Kondo regime and analyze queuing behavior caused by correlations between single-electron transfer events

Randomly diluted xy and resistor networks near the percolation threshold

NASA Astrophysics Data System (ADS)

Harris, A. B.; Lubensky, T. C.

1987-05-01

A formulation based on that of Stephen for randomly diluted systems near the percolation threshold is analyzed in detail. By careful consideration of various limiting procedures, a treatment of xy spin models and resistor networks is given which shows that previous calculations (which indicate that these systems having continuous symmetry have the same crossover exponents as the Ising model) are in error. By studying the limit wherein the energy gap goes to zero, we exhibit the mathematical mechanism which leads to qualitatively different results for xy-like as contrasted to Ising-like systems. A distinctive feature of the results is that there is an infinite sequence of crossover exponents needed to completely describe the probability distribution for R(x,x'), the resistance between sites x and x'. Because of the difference in symmetry between the xy model and the resistor network, the former has an infinite sequence of crossover exponents in addition to those of the resistor network. The first crossover exponent φ1=1+ɛ/42 governs the scaling behavior of R(x,x') with ||x-x'||≡r: [R(x,x')]c~xφ1/ν, where [ ]c indicates a conditional average, subject to x and x' being in the same cluster, ν is the correlation length exponent for percolation, and ɛ=6-d, where d is the spatial dimensionality. We give a detailed analysis of the scaling properties of the bulk conductivity and the anomalous diffusion constant introduced by Gefen et al. Our results show conclusively that the Alexander-Orbach conjecture, while numerically quite accurate, is not exact, at least in high spatial dimension. We also evaluate various amplitude ratios associated with susceptibilities, χn involving the nth power of the resistance R(x,x'), e.g., &χ2χ0/χ21=2[1+(19ɛ/420)]. In an appendix we outline how the calculation can be extended to treat the diluted m-component spin model for m>2. As expected, the results for φ1 remain valid for m>2. The techniques described here have led to several recent calculations of various infinite families of exponents.

Snake instability of dark solitons across the BEC-BCS crossover: An effective-field-theory perspective

NASA Astrophysics Data System (ADS)

Lombardi, G.; Van Alphen, W.; Klimin, S. N.; Tempere, J.

2017-09-01

In the present article the snake instability mechanism for dark solitons in superfluid Fermi gases is studied in the context of a recently developed effective field theory [S. N. Klimin et al., Eur. Phys. J. B 88, 122 (2015), 10.1140/epjb/e2015-60213-4]. This theoretical treatment has proven to be suitable to study stable dark solitons in quasi-one-dimensional setups across the BEC-BCS crossover. In this paper the nodal plane of the stable soliton solution is perturbed by adding a transverse modulation. The numerical solution of the system of coupled nonlinear differential equations describing the amplitude of the perturbation leads to an estimate of the growth rate and characteristic length scale of the instability, which are calculated for a wide range of interaction regimes and compared to other theoretical predictions. The behavior of the maximum transverse size that the atomic cloud can have in order to preserve the stability is described across the BEC-BCS crossover. The analysis of the effects of spin imbalance on this critical length reveals a stabilization of the soliton with increasing imbalance and therefore provides the experimental community with a method to achieve the realization of stable solitons in real three-dimensional configurations, without reducing the system dimensionality.

Out-of-equilibrium dynamics of photoexcited spin-state concentration waves

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marino, Andrea; Buron-Le Cointe, M.; Lorenc, M.

2015-01-28

The spin crossover compound [Fe IIH 2L 2-Me][PF 6]2 presents a two-step phase transition. In the intermediate phase, a spin state concentration wave (SSCW) appears resulting from a symmetry breaking (cell doubling) associated with a long-range order of alternating high and low spin molecular states. Lastly, by combining time-resolved optical and X-ray diffraction measurements on a single crystal, we study how such a system responds to femtosecond laser excitation and we follow in real time the erasing and rewriting of the SSCW

Tunable Magnetic Alignment between Trapped Exciton-Polariton Condensates.

PubMed

Ohadi, H; Del Valle-Inclan Redondo, Y; Dreismann, A; Rubo, Y G; Pinsker, F; Tsintzos, S I; Hatzopoulos, Z; Savvidis, P G; Baumberg, J J

2016-03-11

Tunable spin correlations are found to arise between two neighboring trapped exciton-polariton condensates which spin polarize spontaneously. We observe a crossover from an antiferromagnetic to a ferromagnetic pair state by reducing the coupling barrier in real time using control of the imprinted pattern of pump light. Fast optical switching of both condensates is then achieved by resonantly but weakly triggering only a single condensate. These effects can be explained as the competition between spin bifurcations and spin-preserving Josephson coupling between the two condensates, and open the way to polariton Bose-Hubbard ladders.

Aging, rejuvenation, and memory effects in short-range Ising spin glass: Cu0.5Co0.5Cl2-FeCl3 graphite bi-intercalation compound

NASA Astrophysics Data System (ADS)

Suzuki, M.; Suzuki, I. S.

2004-10-01

Non-equilibrium aging dynamics in 3D Ising spin glass Cu0.5Co0.5Cl2-FeCl3 GBIC has been studied by zero-field cooled (ZFC) magnetization and low frequency AC magnetic susceptibility ( f = 0.05 Hz), where Tg = 3.92 ± 0.11 K. The time dependence of the relaxation rate S( t) = (1/ H)dM_ZFC/dln t for the ZFC magnetization after the ZFC aging protocol, shows a peak at a characteristic time t cr near a wait time t w (aging behavior), corresponding to a crossover from quasi equilibrium dynamics to non-equilibrium. The time t cr strongly depends on t w , temperature ( T), magnetic field ( H), and the temperature shift (Δ T). The rejuvenation effect is observed in both χ^' and χ^'' under the T-shift and H-shift procedures. The memory of the specific spin configurations imprinted during the ZFC aging protocol can be recalled when the system is re-heated at a constant heating rate. The aging, rejuvenation, and memory effects observed in the present system are discussed in terms of the scaling concepts derived from numerical studies on 3D Edwards-Anderson spin glass model.

Homoleptic versus Heteroleptic Formation of Mononuclear Fe(II) Complexes with Tris-Imine Ligands

DOE PAGES

Barrios, Leoni A.; Bartual-Murgui, Carlos; Peyrecave-Lleixa, Eugenia; ...

2016-04-13

In this paper, we show a marked tendency of Fe(II) to form heteroleptic [Fe(L)(L')](ClO 4) 2 complexes from pairs of chelating tris-imine 3bpp, tpy, or 2bbp ligands. New synthetic avenues for spin crossover research become thus available, here illustrated with three new heteroleptic compounds with differing magnetic behaviors: [Fe(H 4L1)(Cl-tpy)](ClO 4) 2 ·C 3H 6O (1), [Fe(H 2L3)(Me3bpp)](ClO 4) 2 ·C 3H 6O (2), [Fe(H 4L1)(2bbp)](ClO 4) 2 ·3C 3H 6O (3). Structural studies demonstrate that 1 is in the low-spin (LS) state up to 350 K, while complexes 2 and 3 are, by contrast, in the high-spin (HS) statemore » down to 2 K, as corroborated through magnetic susceptibility measurements. Upon exposure to the atmosphere, the latter exhibits the release of three molecules of acetone per complex, turning into the solvent-free analogue [Fe(H 4L1)(2bbp)](ClO 4) 2 (3a), through a single-crystal-to-single-crystal transformation. Lastly, this guest extrusion process is accompanied by a spin switch, from HS to LS.« less

Critical behavior of the anisotropic Heisenberg model by effective-field renormalization group

NASA Astrophysics Data System (ADS)

de Sousa, J. Ricardo; Fittipaldi, I. P.

1994-05-01

A real-space effective-field renormalization-group method (ERFG) recently derived for computing critical properties of Ising spins is extended to treat the quantum spin-1/2 anisotropic Heisenberg model. The formalism is based on a generalized but approximate Callen-Suzuki spin relation and utilizes a convenient differential operator expansion technique. The method is illustrated in several lattice structures by employing its simplest approximation version in which clusters with one (N'=1) and two (N=2) spins are used. The results are compared with those obtained from the standard mean-field (MFRG) and Migdal-Kadanoff (MKRG) renormalization-group treatments and it is shown that this technique leads to rather accurate results. It is shown that, in contrast with the MFRG and MKRG predictions, the EFRG, besides correctly distinguishing the geometries of different lattice structures, also provides a vanishing critical temperature for all two-dimensional lattices in the isotropic Heisenberg limit. For the simple cubic lattice, the dependence of the transition temperature Tc with the exchange anisotropy parameter Δ [i.e., Tc(Δ)], and the resulting value for the critical thermal crossover exponent φ [i.e., Tc≂Tc(0)+AΔ1/φ ] are in quite good agreement with results available in the literature in which more sophisticated treatments are used.

Elastic interaction among transition metals in one-dimensional spin-crossover solids

NASA Astrophysics Data System (ADS)

Boukheddaden, K.; Miyashita, S.; Nishino, M.

2007-03-01

We present an exact examination of a one-dimensional (1D) spin-phonon model describing the thermodynamical properties of spin-crossover (SC) solids. This model has the advantage of giving a physical mechanism for the interaction between the SC units. The origin of the interaction comes from the fact that the elastic constant of the spring linking two atoms depends on their electronic states. This leads to local variation of the elastic constant. Up to now, all the statistical studies of this model have been performed in the frame of the mean-field (MF) approach, which is not adequate to describe 1D systems with short-range interactions. An alternative method, based on the variational approach and taking into account the short-range correlations between neighboring molecules, was also suggested, but it consists in an extension of the previous MF approximation. Here, we solve exactly this Hamiltonian in the frame of classical statistical mechanics using the transfer-matrix technique. The temperature dependence of the high spin fraction and that of the total energy are obtained analytically. Our results clearly show that there is a clear tendency to a sharp transition when we tune the elastic constants adequately, which indicates that first-order phase transition takes place at higher dimensions. In addition, we demonstrate the existence of an interesting isomorphism between the present model and Ising model under effective interaction and effective ligand field energy, in which both depend linearly on temperature and both come from the phonon contribution. We have also studied the effect of the pressure (the tension) on the thermodynamical properties of the high spin (HS) fraction and have found a nontrivial pressure effect that while for weak tension values, the low spin state is stabilized for the pressure above a threshold value, it enhances the interaction between the HS states. Finally, we have also introduced elastic interactions between the chains. Treating exactly (in mean field) the intrachain (interchain) contributions, we found that our model leads us to obtain first-order spin transitions when both short- and long-range interactions are ferroelastic. We show also that competing (antiferroelastic short-range and ferroelastic long-range) interactions between spin-state ions reproduce qualitatively the two-step-like spin-crossover transitions.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yan, Qiang; Zhou, Liping, E-mail: zhoulp@suda.edu.cn; Cheng, Jue-Fei

Electronic structures and coherent quantum transport properties are explored for spin-crossover molecule iron-benzene Fe(Bz){sub 2} using density functional theory combined with non-equilibrium Green’s function. High- and low-spin states are investigated for two different lead-molecule junctions. It is found that the asymmetrical T-shaped contact junction in the high-spin state behaves as an efficient spin filter while it has a smaller conductivity than that in the low-spin state. Large spin Seebeck effect is also observed in asymmetrical T-shaped junction. Spin-polarized properties are absent in the symmetrical H-shaped junction. These findings strongly suggest that both the electronic and contact configurations play significant rolesmore » in molecular devices and metal-benzene complexes are promising materials for spintronics and thermo-spintronics.« less

Core structure of two-dimensional Fermi gas vortices in the BEC-BCS crossover region

DOE Office of Scientific and Technical Information (OSTI.GOV)

Madeira, Lucas; Gandolfi, Stefano; Schmidt, Kevin E.

2017-05-02

We report T = 0 diffusion Monte Carlo results for the ground-state and vortex excitation of unpolarized spin-1/2 fermions in a two-dimensional disk. We investigate how vortex core structure properties behave over the BEC-BCS crossover. We calculate the vortex excitation energy, density pro les, and vortex core properties related to the current. We nd a density suppression at the vortex core on the BCS side of the crossover and a depleted core on the BEC limit. Size-effect dependencies in the disk geometry were carefully studied.

Detection of crossover time scales in multifractal detrended fluctuation analysis

NASA Astrophysics Data System (ADS)

Ge, Erjia; Leung, Yee

2013-04-01

Fractal is employed in this paper as a scale-based method for the identification of the scaling behavior of time series. Many spatial and temporal processes exhibiting complex multi(mono)-scaling behaviors are fractals. One of the important concepts in fractals is crossover time scale(s) that separates distinct regimes having different fractal scaling behaviors. A common method is multifractal detrended fluctuation analysis (MF-DFA). The detection of crossover time scale(s) is, however, relatively subjective since it has been made without rigorous statistical procedures and has generally been determined by eye balling or subjective observation. Crossover time scales such determined may be spurious and problematic. It may not reflect the genuine underlying scaling behavior of a time series. The purpose of this paper is to propose a statistical procedure to model complex fractal scaling behaviors and reliably identify the crossover time scales under MF-DFA. The scaling-identification regression model, grounded on a solid statistical foundation, is first proposed to describe multi-scaling behaviors of fractals. Through the regression analysis and statistical inference, we can (1) identify the crossover time scales that cannot be detected by eye-balling observation, (2) determine the number and locations of the genuine crossover time scales, (3) give confidence intervals for the crossover time scales, and (4) establish the statistically significant regression model depicting the underlying scaling behavior of a time series. To substantive our argument, the regression model is applied to analyze the multi-scaling behaviors of avian-influenza outbreaks, water consumption, daily mean temperature, and rainfall of Hong Kong. Through the proposed model, we can have a deeper understanding of fractals in general and a statistical approach to identify multi-scaling behavior under MF-DFA in particular.

Crossover phenomena in the critical range near magnetic ordering transition

NASA Astrophysics Data System (ADS)

Köbler, U.

2018-05-01

Among the most important issues of Renormalization Group (RG) theory are crossover events and relevant (or non-relevant) interactions. These terms are unknown to atomistic theories but they will be decisive for future field theories of magnetism. In this experimental study the importance of these terms for the critical dynamics above and below magnetic ordering transition is demonstrated on account of new analyses of published data. When crossover events are overlooked and critical data are fitted by a single power function of temperature over a temperature range including a crossover event, imprecise critical exponents result. The rather unsystematic and floating critical exponents reported in literature seem largely to be due to this problem. It is shown that for appropriate data analyses critical exponents are obtained that are to a good approximation rational numbers. In fact, rational critical exponents can be expected when spin dynamics is controlled by the bosons of the continuous magnetic medium (Goldstone bosons). The bosons are essentially magnetic dipole radiation generated by the precessing spins. As a result of the here performed data analyses, critical exponents for the magnetic order parameter of β = 1/2, 1/3, 1/4 and 1/6 are obtained. For the critical paramagnetic susceptibility the exponents are γ = 1 and γ = 4/3.

Nonlinear spin conductance of yttrium iron garnet thin films driven by large spin-orbit torque

NASA Astrophysics Data System (ADS)

Thiery, N.; Draveny, A.; Naletov, V. V.; Vila, L.; Attané, J. P.; Beigné, C.; de Loubens, G.; Viret, M.; Beaulieu, N.; Ben Youssef, J.; Demidov, V. E.; Demokritov, S. O.; Slavin, A. N.; Tiberkevich, V. S.; Anane, A.; Bortolotti, P.; Cros, V.; Klein, O.

2018-02-01

We report high power spin transfer studies in open magnetic geometries by measuring the spin conductance between two nearby Pt wires deposited on top of an epitaxial yttrium iron garnet thin film. Spin transport is provided by propagating spin waves that are generated and detected by direct and inverse spin Hall effects. We observe a crossover in spin conductance from a linear transport dominated by exchange magnons (low current regime) to a nonlinear transport dominated by magnetostatic magnons (high current regime). The latter are low-damping magnetic excitations, located near the spectral bottom of the magnon manifold, with a sensitivity to the applied magnetic field. This picture is supported by microfocus Brillouin light-scattering spectroscopy. Our findings could be used for the development of controllable spin conductors by variation of relatively weak magnetic fields.

Oxygen hyperstoichiometric hexagonal ferrite CaBaFe4O7+δ (δ≈0.14): Coexistence of ferrimagnetism and spin glass behavior

NASA Astrophysics Data System (ADS)

Sarkar, Tapati; Duffort, V.; Pralong, V.; Caignaert, V.; Raveau, B.

2011-03-01

An oxygen hyperstoichiometric ferrite CaBaFe4O7+δ (δ ≈ 0.14) has been synthesized using “soft” reduction of CaBaFe4O8. Like the oxygen stoichiometric ferrimagnet CaBaFe4O7, this oxide also keeps the hexagonal symmetry (space group P63mc), and exhibits the same high Curie temperature of 270 K. However, the introduction of extra oxygen into the system weakens the ferrimagnetic interaction significantly at the cost of increased magnetic frustration at low temperature. Moreover, this canonical spin glass (Tg~166 K) exhibits an intriguing crossover from de Almeida-Thouless type to Gabay-Toulouse type critical line in the field temperature plane above a certain field strength, which can be identified as the anisotropy field. Domain-wall pinning is also observed below 110 K. These results are interpreted on the basis of cationic disordering on the iron sites.

One Dimensional(1D)-to-2D Crossover of Spin Correlations in the 3D Magnet ZnMn 2O 4

DOE PAGES

Disseler, S. M.; Chen, Y.; Yeo, S.; ...

2015-12-08

In this paper we report on the intriguing evolution of the dynamical spin correlations of the frustrated spinel ZnMn 2O 4. Inelastic neutron scattering and magnetization studies reveal that the dynamical correlations at high temperatures are 1D. At lower temperature, these dynamical correlations become 2D. Surprisingly, the dynamical correlations condense into a quasi 2D Ising-like ordered state, making this a rare observation of two dimensional order on the spinel lattice. Remarkably, 3D ordering is not observed down to temperatures as low as 300 mK. This unprecedented dimensional crossover stems from frustrated exchange couplings due to the huge Jahn-Teller distortions aroundmore » Mn 3+ ions on the spinel lattice.« less

Comment on ?Spin crossover in (Mg,Fe)O: A M?ssbauer effect study with an alternative interpretation of x-ray emission spectroscopy data?

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, J; Struzhkin, V V; Garriliuk, A

2006-05-23

Electronic spin-pairing transition of iron in magnesiow{umlt u}stite-(Mg,Fe)O has been recently studied with X-ray emission and M{umlt o}ssbauer spectroscopies under high pressures. While these studies reported a high-spin to low-spin transition of iron to occur at pressures above approximately 50 GPa, the width of the observed transition varies significantly. In particular, Kantor et al. reported that the transition in (Mg0.8,Fe0.2)O occurs over a pressure range of approximately 50 GPa in high-pressure M{umlt o}ssbauer measurements. To account for the discrepancy in the transition pressure, Kantor et al. reanalyzed the X-ray emission spectra by Lin et al. using a simple spectral decompositionmore » method and claimed that X-ray emission measurements are also consistent with a spin crossover of iron at high pressures. Here we show that the proposed fitting method is inadequate to describe the X-ray emission spectrum of the low-spin FeS2 and would give an erroneous satellite peak (K{sub beta}') intensity, leading to an artificial high-spin component and, consequently, to invalid conclusions regarding the width of the pressure-induced transition in magnesiow{umlt u}stite. Furthermore, we compare Kantor's M{umlt o}ssbauer data with other recent high-pressure M{umlt o}ssbauer studies and show that the width of the transition can be simply explained by different experimental conditions (sample thickness, diameter, and hydrostaticity).« less

Insights into the crystal-packing effects on the spin crossover of [Fe(II)(1-bpp)](2+)-based materials.

PubMed

Vela, Sergi; Novoa, Juan J; Ribas-Arino, Jordi

2014-12-28

Iron(II) complexes of the [Fe(II)(1-bpp2)](2+) type (1-bpp = 2,6-di(pyrazol-1-yl)pyridine) have been intensively investigated in the context of crystal engineering of switchable materials because their spin-crossover (SCO) properties dramatically depend on the counterions. Here, by means of DFT + U calculations at the molecular and solid state levels we provide a rationale for the different SCO behaviour of the BF4(-) and ClO4(-) salts of the parent complex; the former features Fe(II) complexes with a regular coordination geometry and undergoes a spin transition, whereas the Fe(II) complexes of the latter adopt a distorted structure and remain in the high-spin state at all temperatures. The different SCO behaviour of both salts can be explained on the basis of a combination of thermodynamic and kinetic effects. The shape of the SCO units at high temperature is thermodynamically controlled by the intermolecular interactions between the SCO units and counterions within the crystal. The spin trapping at low temperatures in the ClO4(-) salt, in turn, is traced back to a kinetic effect because our calculations have revealed the existence of a more stable polymorph having SCO units in their low-spin state that feature a regular structure. From the computational point of view, it is the first time that the U parameter is fine-tuned on the basis of CASPT2 calculations, thereby enabling an accurate description of the energetics of the spin transition at both molecular and solid-state levels.

Halogen Substitution Effects on N2 O Schiff Base Ligands in Unprecedented Abrupt FeII Spin Crossover Complexes.

PubMed

Phonsri, Wasinee; Macedo, David S; Vignesh, Kuduva R; Rajaraman, Gopalan; Davies, Casey G; Jameson, Guy N L; Moubaraki, Boujemaa; Ward, Jas S; Kruger, Paul E; Chastanet, Guillaume; Murray, Keith S

2017-05-23

A family of halogen-substituted Schiff base iron(II) complexes, [Fe II (qsal-X) 2 ], (qsal-X=5-X-N-(8-quinolyl)salicylaldimines)) in which X=F (1), Cl (2), Br (3) or I (4) has been investigated in detail. Compound 1 shows a temperature invariant high spin state, whereas the others all show abrupt spin transitions, at or above room temperature, namely, 295 K (X=I) up to 342 K (X=Br), these being some of the highest T 1/2 values obtained, to date, for Fe II N/O species. We have recently reported subtle symmetry breaking in [Fe II (qsal-Cl) 2 ] 2 with two spin transition steps occurring at 308 and 316 K. A photomagnetic study reveals almost full HS conversion of [Fe II (qsal-I) 2 ] 4 at low temperature (T(LIESST)=54 °K). The halogen substitution effects on the magnetic properties, as well as the crystal packing of the [Fe II (qsal-X) 2 ] compounds and theoretical calculations, are discussed in depth, giving important knowledge for the design of new spin crossover materials. In comparison to the well known iron(III) analogues, [Fe III (qsal-X) 2 ] + , the two extra π-π and P4AE interactions found in [Fe II (qsal-X) 2 ] compounds, are believed to be accountable for the spin transitions occurring at ambient temperatures. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Phenomenological model of spin crossover in molecular crystals as derived from atom-atom potentials.

PubMed

Sinitskiy, Anton V; Tchougréeff, Andrei L; Dronskowski, Richard

2011-08-07

The method of atom-atom potentials, previously applied to the analysis of pure molecular crystals formed by either low-spin (LS) or high-spin (HS) forms (spin isomers) of Fe(II) coordination compounds (Sinitskiy et al., Phys. Chem. Chem. Phys., 2009, 11, 10983), is used to estimate the lattice enthalpies of mixed crystals containing different fractions of the spin isomers. The crystals under study were formed by LS and HS isomers of Fe(phen)(2)(NCS)(2) (phen = 1,10-phenanthroline), Fe(btz)(2)(NCS)(2) (btz = 5,5',6,6'-tetrahydro-4H,4'H-2,2'-bi-1,3-thiazine), and Fe(bpz)(2)(bipy) (bpz = dihydrobis(1-pyrazolil)borate, and bipy = 2,2'-bipyridine). For the first time the phenomenological parameters Γ pertinent to the Slichter-Drickamer model (SDM) of several materials were independently derived from the microscopic model of the crystals with use of atom-atom potentials of intermolecular interaction. The accuracy of the SDM was checked against the numerical data on the enthalpies of mixed crystals. Fair semiquantitative agreement with the experimental dependence of the HS fraction on temperature was achieved with use of these values. Prediction of trends in Γ values as a function of chemical composition and geometry of the crystals is possible with the proposed approach, which opens a way to rational design of spin crossover materials with desired properties. This journal is © the Owner Societies 2011

Velocity of the high-spin low-spin interface inside the thermal hysteresis loop of a spin-crossover crystal, via photothermal control of the interface motion.

PubMed

Slimani, Ahmed; Varret, François; Boukheddaden, Kamel; Garrot, Damien; Oubouchou, Hassane; Kaizaki, Sumio

2013-02-22

We investigated by optical microscopy the thermal transition of the spin-crossover dinuclear iron(II) compound [(Fe(NCSe)(py)(2))(2)(m-bpypz)]. In a high-quality crystal the high-spin (HS) low-spin (LS) thermal transition took place with a sizable hysteresis, at ~108 K and ~116 K on cooling and heating, respectively, through the growth of a single macroscopic domain with a straight LS and HS interface. The interface orientation was almost constant and its propagation velocity was close to ~6 and 26 μ m s(-1) for the on-cooling and on-heating processes, respectively. We found that the motion of the interface was sensitive to the intensity of the irradiation beam of the microscope, through a photothermal effect. By fine-tuning the intensity we could stop and even reverse the interface motion. This way we stabilized a biphasic state of the crystal, and we followed the spontaneous motion of the interface at different temperatures inside the thermal hysteresis loop. This experiment gives access for the first time to an accurate determination of the equilibrium temperature in the case of thermal hysteresis--which was not accessible by the usual quasistatic investigations. The temperature dependence of the propagation velocity inside the hysteretic interval was revealed to be highly nonlinear, and it was quantitatively reproduced by a dynamical mean-field theory, which made possible an estimate of the macroscopic energy barrier.

Engineering On-Surface Spin Crossover: Spin-State Switching in a Self-Assembled Film of Vacuum-Sublimable Functional Molecule.

PubMed

Kumar, Kuppusamy Senthil; Studniarek, Michał; Heinrich, Benoît; Arabski, Jacek; Schmerber, Guy; Bowen, Martin; Boukari, Samy; Beaurepaire, Eric; Dreiser, Jan; Ruben, Mario

2018-03-01

The realization of spin-crossover (SCO)-based applications requires study of the spin-state switching characteristics of SCO complex molecules within nanostructured environments, especially on surfaces. Except for a very few cases, the SCO of a surface-bound thin molecular film is either quenched or heavily altered due to: (i) molecule-surface interactions and (ii) differing intermolecular interactions in films relative to the bulk. By fabricating SCO complexes on a weakly interacting surface, the interfacial quenching problem is tackled. However, engineering intermolecular interactions in thin SCO active films is rather difficult. Here, a molecular self-assembly strategy is proposed to fabricate thin spin-switchable surface-bound films with programmable intermolecular interactions. Molecular engineering of the parent complex system [Fe(H 2 B(pz) 2 ) 2 (bpy)] (pz = pyrazole, bpy = 2,2'-bipyridine) with a dodecyl (C 12 ) alkyl chain yields a classical amphiphile-like functional and vacuum-sublimable charge-neutral Fe II complex, [Fe(H 2 B(pz) 2 ) 2 (C 12 -bpy)] (C 12 -bpy = dodecyl[2,2'-bipyridine]-5-carboxylate). Both the bulk powder and 10 nm thin films sublimed onto either quartz glass or SiO x surfaces of the complex show comparable spin-state switching characteristics mediated by similar lamellar bilayer like self-assembly/molecular interactions. This unprecedented observation augurs well for the development of SCO-based applications, especially in molecular spintronics. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Cobalt spin states and hyperfine interactions in LaCoO3 investigated by LDA+U calculations

NASA Astrophysics Data System (ADS)

Hsu, Han; Blaha, Peter; Wentzcovitch, Renata M.; Leighton, C.

2010-09-01

With a series of local-density approximation plus Hubbard U calculations, we have demonstrated that for lanthanum cobaltite (LaCoO3) , the electric field gradient at the cobalt nucleus can be used as a fingerprint to identify the spin state of the cobalt ion. Therefore, in principle, the spin state of the cobalt ion can be unambiguously determined from nuclear magnetic resonance spectra. Our calculations also suggest that a crossover from the low-spin to intermediate-spin state in the temperature range of 0-90 K is unlikely, based on the half-metallic band structure associated with isolated IS Co ions, which is incompatible with the measured conductivity.

Iron Spin Crossover in the New Hexagonal Aluminous (NAL) Phase

NASA Astrophysics Data System (ADS)

Hsu, H.

2017-12-01

The new hexagonal aluminous (NAL) phase, chemical formula AB2C6O12 (A = Na+, K+, Ca2+; B = Mg2+, Fe2+, Fe3+; C = Al3+, Si4+, Fe3+), is considered a major component ( 20 vol%) of mid-ocean ridge basalt (MORB) at lower-mantle conditions. Given that MORB can be transported back into the Earth's lower mantle via subduction, a thorough knowledge of the NAL phase is essential to fully understand the fate of subducted MORB and its role in mantle dynamics and heterogeneity. In this presentation, the complicated spin crossover of the Fe-bearing NAL phase will be discussed based on a series of first-principles calculations [1], in which the local density approximation + self-consistent Hubbard U (LDA+Usc) method was adopted. As revealed by these calculations, only the ferric iron (Fe3+) substituting Al/Si in the octahedral (C) site undergoes a crossover from the high-spin (HS) to the low-spin (LS) state at 40 GPa, while iron substituting Mg in the trigonal-prismatic (B) site remains in the HS state, regardless of its oxidation state (Fe2+ or Fe3+). The volume/elastic anomalies, iron nuclear quadrupole splittings, and crystal field spltting determined by calculations are in great agreement with experiments [2,3]. The calculations further predict that the HS-LS transition pressure of the NAL phase barely increases with temperature due to the three nearly degenerate LS states of Fe3+, suggesting that the elastic anomalies of this mineral can occur at the top lower mantle. [1] H. Hsu, Phys. Rev. B 95, 020406(R) (2017). [2] Y. Wu et al. Earth Planet. Sci. Lett. 434, 91-100 (2016). [3] S. S. Lobanov et al., J. Geophys. Res. Solid Earth 122, 3565 (2017).

Crossover to the anomalous quantum regime in the extrinsic spin Hall effect of graphene

NASA Astrophysics Data System (ADS)

Ferreira, Aires; Milletari, Mirco

Recent reports of spin-orbit coupling enhancement in chemically modified graphene have opened doors to studies of the spin Hall effect with massless chiral fermions. Here, we theoretically investigate the interaction and impurity density dependence of the extrinsic spin Hall effect in spin-orbit coupled graphene. We present a nonperturbative quantum diagrammatic calculation of the spin Hall response function in the strong-coupling regime that incorporates skew scattering and anomalous impurity density-independent contributions on equal footing. The spin Hall conductivity dependence on Fermi energy and electron-impurity interaction strength reveals the existence of experimentally accessible regions where anomalous quantum processes dominate. Our findings suggest that spin-orbit-coupled graphene is an ideal model system for probing the competition between semiclassical and bona fide quantum scattering mechanisms underlying the spin Hall effect. A.F. gratefully acknowledges the financial support of the Royal Society (U.K.).

Transient electronic anisotropy in overdoped NaF e1 -xC oxAs superconductors

NASA Astrophysics Data System (ADS)

Liu, Shenghua; Zhang, Chunfeng; Deng, Qiang; Wen, Hai-hu; Li, Jian-xin; Chia, Elbert E. M.; Wang, Xiaoyong; Xiao, Min

2018-01-01

By combining polarized pump-probe spectroscopic and Laue x-ray diffraction measurements, we have observed nonequivalent transient optical responses with the probe beam polarized along the x and y axes in overdoped NaF e1 -xC oxAs superconductors. Such transient anisotropic behavior has been uncovered in the tetragonal phase with the doping level and temperature range far from the borders of static nematic phases. The measured transient anisotropy can be well explained as a result of nematic fluctuation driven by an orbital order with energy splitting of the dx z- and dy z-dominant bands. In addition, the doping level dependence and the pressure effect of the crossover temperature show significant differences between the transient nematic fluctuation and static nematic phase, implying spin and orbital orders may play different roles in static and transient nematic behaviors.

Magnetic-field-temperature phase diagram of alternating ferrimagnetic chains: Spin-wave theory from a fully polarized vacuum

NASA Astrophysics Data System (ADS)

da Silva, W. M.; Montenegro-Filho, R. R.

2017-12-01

Quantum critical (QC) phenomena can be accessed by studying quantum magnets under an applied magnetic field (B ). The QC points are located at the end points of magnetization plateaus and separate gapped and gapless phases. In one dimension, the low-energy excitations of the gapless phase form a Luttinger liquid (LL), and crossover lines bound insulating (plateau) and LL regimes, as well as the QC regime. Alternating ferrimagnetic chains have a spontaneous magnetization at T =0 and gapped excitations at zero field. Besides the plateau at the fully polarized (FP) magnetization, due to the gap there is another magnetization plateau at the ferrimagnetic (FRI) magnetization. We develop spin-wave theories to study the thermal properties of these chains under an applied magnetic field: one from the FRI classical state and another from the FP state, comparing their results with quantum Monte Carlo data. We deepen the theory from the FP state, obtaining the crossover lines in the T vs B low-T phase diagram. In particular, from local extreme points in the susceptibility and magnetization curves, we identify the crossover between an LL regime formed by excitations from the FRI state to another built from excitations of the FP state. These two LL regimes are bounded by an asymmetric domelike crossover line, as observed in the phase diagram of other quantum magnets under an applied magnetic field.

Polarized-neutron study of spin dynamics in the Kondo insulator YbB12.

PubMed

Nemkovski, K S; Mignot, J-M; Alekseev, P A; Ivanov, A S; Nefeodova, E V; Rybina, A V; Regnault, L-P; Iga, F; Takabatake, T

2007-09-28

Inelastic neutron scattering experiments have been performed on the archetype compound YbB(12), using neutron polarization analysis to separate the magnetic signal from the phonon background. With decreasing temperature, components characteristic for a single-site spin-fluctuation dynamics are suppressed, giving place to specific, strongly Q-dependent, low-energy excitations near the spin-gap edge. This crossover is discussed in terms of a simple crystal-field description of the incoherent high-temperature state and a predominantly local mechanism for the formation of the low-temperature singlet ground state.

On the zeroth-order hamiltonian for CASPT2 calculations of spin crossover compounds.

PubMed

Vela, Sergi; Fumanal, Maria; Ribas-Ariño, Jordi; Robert, Vincent

2016-04-15

Complete active space self-consistent field theory (CASSCF) calculations and subsequent second-order perturbation theory treatment (CASPT2) are discussed in the evaluation of the spin-states energy difference (ΔH(elec)) of a series of seven spin crossover (SCO) compounds. The reference values have been extracted from a combination of experimental measurements and DFT + U calculations, as discussed in a recent article (Vela et al., Phys Chem Chem Phys 2015, 17, 16306). It is definitely proven that the critical IPEA parameter used in CASPT2 calculations of ΔH(elec), a key parameter in the design of SCO compounds, should be modified with respect to its default value of 0.25 a.u. and increased up to 0.50 a.u. The satisfactory agreement observed previously in the literature might result from an error cancellation originated in the default IPEA, which overestimates the stability of the HS state, and the erroneous atomic orbital basis set contraction of carbon atoms, which stabilizes the LS states. © 2015 Wiley Periodicals, Inc.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Galle, G.; Degert, J.; Freysz, E.

We have studied the low spin to high spin phase transition induced by nanosecond laser pulses outside and within the thermal hysteresis loop of the [Fe(Htrz){sub 2} trz](BF{sub 4}){sub 2}-H{sub 2}O spin crossover nanoparticles. We demonstrate that, whatever the temperature of the compound, the photo-switching is achieved in less than 12.5 ns. Outside the hysteresis loop, the photo-induced high spin state remains up to 100 {mu}s and then relaxes. Within the thermal hysteresis loop, the photo-induced high spin state remains as long as the temperature of the sample is kept within the thermal loop. A Raman study indicates that themore » photo-switching can be completed using single laser pulse excitation.« less

Activation of coherent lattice phonon following ultrafast molecular spin-state photo-switching: A molecule-to-lattice energy transfer

PubMed Central

Marino, A.; Cammarata, M.; Matar, S. F.; Létard, J.-F.; Chastanet, G.; Chollet, M.; Glownia, J. M.; Lemke, H. T.; Collet, E.

2015-01-01

We combine ultrafast optical spectroscopy with femtosecond X-ray absorption to study the photo-switching dynamics of the [Fe(PM-AzA)2(NCS)2] spin-crossover molecular solid. The light-induced excited spin-state trapping process switches the molecules from low spin to high spin (HS) states on the sub-picosecond timescale. The change of the electronic state (<50 fs) induces a structural reorganization of the molecule within 160 fs. This transformation is accompanied by coherent molecular vibrations in the HS potential and especially a rapidly damped Fe-ligand breathing mode. The time-resolved studies evidence a delayed activation of coherent optical phonons of the lattice surrounding the photoexcited molecules. PMID:26798836

Itinerant magnetism in doped semiconducting β-FeSi2 and CrSi2

PubMed Central

Singh, David J.; Parker, David

2013-01-01

Novel or unusual magnetism is a subject of considerable interest, particularly in metals and degenerate semiconductors. In such materials the interplay of magnetism, transport and other Fermi liquid properties can lead to fascinating physical behavior. One example is in magnetic semiconductors, where spin polarized currents may be controlled and used. We report density functional calculations predicting magnetism in doped semiconducting β-FeSi2 and CrSi2 at relatively low doping levels particularly for n-type. In this case, there is a rapid cross-over to a half-metallic state as a function of doping level. The results are discussed in relation to the electronic structure and other properties of these compounds. PMID:24343332

Collective modes of a two-dimensional spin-1/2 Fermi gas in a harmonic trap

NASA Astrophysics Data System (ADS)

Baur, Stefan K.; Vogt, Enrico; Köhl, Michael; Bruun, Georg M.

2013-04-01

We derive analytical expressions for the frequency and damping of the lowest collective modes of a two-dimensional Fermi gas using kinetic theory. For strong coupling, we furthermore show that pairing correlations overcompensate the effects of Pauli blocking on the collision rate for a large range of temperatures, resulting in a rate which is larger than that of a classical gas. Our results agree well with experimental data, and they recover the observed crossover from collisionless to hydrodynamic behavior with increasing coupling for the quadruple mode. Finally, we show that a trap anisotropy within the experimental bounds results in a damping of the breathing mode which is comparable to what is observed, even for a scale-invariant system.

Absence of ferroelectric features in Eu2BaNiO5: An anomalous case within this rare-earth family

NASA Astrophysics Data System (ADS)

Upadhyay, Sanjay Kumar; Sampathkumaran, E. V.

2018-04-01

We report the results of magnetization, heat-capacity, magnetodielectric and pyrocurrent measurements above 2 K for the compound, Eu2BaNiO5, a Haldane spin-chain compound. This compound has been known to exhibit a magnetic transition in the vicinity of 5 K from Eu and Ni, but we do not find any evidence for ferroelectricity above 2 K, in sharp contrast to the multiferroic behavior reported for other members of this Haldane spin-chain family. Instead, there is a pyrocurrent peak around 40 K, which is sensitive to the rate of change of temperature thereby providing an evidence for thermally stimulated depolarization current. Additionally, this study brings out two more features: (i) There is a dielectric anomaly in the range 75-100 K, attributable to short-range magnetic correlations, similar to the situation encountered in another spin-chain system Ca3Co2O6, and (ii) there is a sign crossover of magnetodielectric effect (MDE) with varying magnetic field well below 8 K only, with relatively negligible values of MDE above 4 K, and this observation establishes the existence of a coupling between magnetic and electric dipoles at the onset of long-range magnetic order.

Vogel-Fulcher-Tammann freezing of a thermally fluctuating artificial spin ice probed by x-ray photon correlation spectroscopy

DOE PAGES

Morley, S. A.; Alba Venero, D.; Porro, J. M.; ...

2017-03-16

We report on the crossover from the thermal to the athermal regime of an artificial spin ice formed from a square array of magnetic islands whose lateral size, 30 nm × 70 nm, is small enough that they are dynamic at room temperature.We used resonant magnetic soft x-ray photon correlation spectroscopy as a method to observe the time-time correlations of the fluctuating magnetic configurations of spin ice during cooling, which are found to slow abruptly as a freezing temperature of T 0 = 178 ± 5 K is approached. This slowing is well described by a Vogel-Fulcher-Tammann law, implying thatmore » the frozen state is glassy, with the freezing temperature being commensurate with the strength of magnetostatic interaction energies in the array. The activation temperature, T A = 40 ± 10 K, is much less than that expected from a Stoner-Wohlfarth coherent rotation model. Zerofield- cooled/field-cooled magnetometry reveals a freeing up of fluctuations of states within islands above this temperature, caused by variation in the local anisotropy axes at the oxidised edges. This Vogel-Fulcher-Tammann behavior implies that the system enters a glassy state upon freezing, which is unexpected for a system with a well-defined ground state.« less

Vogel-Fulcher-Tammann freezing of a thermally fluctuating artificial spin ice probed by x-ray photon correlation spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Morley, S. A.; Alba Venero, D.; Porro, J. M.

We report on the crossover from the thermal to the athermal regime of an artificial spin ice formed from a square array of magnetic islands whose lateral size, 30 nm × 70 nm, is small enough that they are dynamic at room temperature.We used resonant magnetic soft x-ray photon correlation spectroscopy as a method to observe the time-time correlations of the fluctuating magnetic configurations of spin ice during cooling, which are found to slow abruptly as a freezing temperature of T 0 = 178 ± 5 K is approached. This slowing is well described by a Vogel-Fulcher-Tammann law, implying thatmore » the frozen state is glassy, with the freezing temperature being commensurate with the strength of magnetostatic interaction energies in the array. The activation temperature, T A = 40 ± 10 K, is much less than that expected from a Stoner-Wohlfarth coherent rotation model. Zerofield- cooled/field-cooled magnetometry reveals a freeing up of fluctuations of states within islands above this temperature, caused by variation in the local anisotropy axes at the oxidised edges. This Vogel-Fulcher-Tammann behavior implies that the system enters a glassy state upon freezing, which is unexpected for a system with a well-defined ground state.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cui, J.; Roy, B.; Tanatar, M. A.

We report 75As nuclear magnetic resonance (NMR) measurements of single-crystalline Ca(Fe 1–xCo x) 2As 2 (x=0.023, 0.028, 0.033, and 0.059) annealed at 350°C for 7 days. From the observation of a characteristic shape of 75As NMR spectra in the stripe-type antiferromagnetic (AFM) state, as in the case of x=0 (T N=170 K), clear evidence for the commensurate AFM phase transition with the concomitant structural phase transition is observed in x=0.023 (T N=106 K) and x=0.028 (T N=53 K). Through the temperature dependence of the Knight shifts and the nuclear spin lattice relaxation rates (1/T 1), although stripe-type AFM spin fluctuationsmore » are realized in the paramagnetic state as in the case of other iron pnictide superconductors, we found a gradual decrease of the AFM spin fluctuations below a crossover temperature T* that was nearly independent of Co-substitution concentration, and it is attributed to a pseudogaplike behavior in the spin excitation spectra of these systems. The T* feature finds correlation with features in the temperature-dependent interplane resistivity, ρc(T), but not with the in-plane resistivity ρa(T). The temperature evolution of anisotropic stripe-type AFM spin fluctuations is tracked in the paramagnetic and pseudogap phases by the 1/T 1 data measured under magnetic fields parallel and perpendicular to the c axis. As a result, based on our NMR data, we have added a pseudogaplike phase to the magnetic and electronic phase diagram of Ca(Fe 1–xCo x) 2As 2.« less

Doping evolution of spin fluctuations and their peculiar suppression at low temperatures in Ca(Fe 1 -xCox)2As2

NASA Astrophysics Data System (ADS)

Sapkota, A.; Das, P.; Böhmer, A. E.; Ueland, B. G.; Abernathy, D. L.; Bud'ko, S. L.; Canfield, P. C.; Kreyssig, A.; Goldman, A. I.; McQueeney, R. J.

2018-05-01

Results of inelastic neutron scattering measurements are reported for two annealed compositions of Ca(Fe 1 -xCox)2As2,x =0.026 and 0.030, which possess stripe-type antiferromagnetically ordered and superconducting ground states, respectively. In the AFM ground state, well-defined and gapped spin waves are observed for x =0.026 , similar to the parent CaFe2As2 compound. We conclude that the well-defined spin waves are likely to be present for all x corresponding to the AFM state. This behavior is in contrast to the smooth evolution to overdamped spin dynamics observed in Ba(Fe 1 -xCox)2As2 , wherein the crossover corresponds to microscopically coexisting AFM order and SC at low temperature. The smooth evolution is likely absent in Ca(Fe 1 -xCox)2As2 due to the mutual exclusion of AFM ordered and SC states. Overdamped spin dynamics characterize paramagnetism of the x =0.030 sample and high-temperature x =0.026 sample. A sizable loss of magnetic intensity is observed over a wide energy range upon cooling the x =0.030 sample, at temperatures just above and within the superconducting phase. This phenomenon is unique amongst the iron-based superconductors and is consistent with a temperature-dependent reduction in the fluctuating moment. One possible scenario ascribes this loss of moment to a sensitivity to the c -axis lattice parameter in proximity to the nonmagnetic collapsed tetragonal phase and another scenario ascribes the loss to a formation of a pseudogap.

Density matrix-based time-dependent configuration interaction approach to ultrafast spin-flip dynamics

NASA Astrophysics Data System (ADS)

Wang, Huihui; Bokarev, Sergey I.; Aziz, Saadullah G.; Kühn, Oliver

2017-08-01

Recent developments in attosecond spectroscopy yield access to the correlated motion of electrons on their intrinsic timescales. Spin-flip dynamics is usually considered in the context of valence electronic states, where spin-orbit coupling is weak and processes related to the electron spin are usually driven by nuclear motion. However, for core-excited states, where the core-hole has a nonzero angular momentum, spin-orbit coupling is strong enough to drive spin-flips on a much shorter timescale. Using density matrix-based time-dependent restricted active space configuration interaction including spin-orbit coupling, we address an unprecedentedly short spin-crossover for the example of L-edge (2p→3d) excited states of a prototypical Fe(II) complex. This process occurs on a timescale, which is faster than that of Auger decay (∼4 fs) treated here explicitly. Modest variations of carrier frequency and pulse duration can lead to substantial changes in the spin-state yield, suggesting its control by soft X-ray light.

100 MHz high-speed strain monitor using fiber Bragg grating and optical filter applied for magnetostriction measurements of cobaltite at magnetic fields beyond 100 T

NASA Astrophysics Data System (ADS)

Ikeda, Akihiko; Nomura, Toshihiro; Matsuda, Yasuhiro H.; Tani, Shuntaro; Kobayashi, Yohei; Watanabe, Hiroshi; Sato, Keisuke

2018-05-01

High-speed 100 MHz strain monitor using fiber Bragg grating (FBG) and an optical filter has been devised for the magnetostriction measurements under ultrahigh magnetic fields. The longitudinal magnetostriction of LaCoO 3 has been measured at room temperature, 115, 7 and 4.2 K up to the maximum magnetic field of 150 T. The field-induced lattice elongations are observed, which are attributed to the spin-state crossover from the low-spin ground state to excited spin-states.

Ground-state magnetization of the Ising spin glass: A recursive numerical method and Chen-Ma scaling

NASA Astrophysics Data System (ADS)

Sepehrinia, Reza; Chalangari, Fartash

2018-03-01

The ground-state properties of quasi-one-dimensional (Q1D) Ising spin glass are investigated using an exact numerical approach and analytical arguments. A set of coupled recursive equations for the ground-state energy are introduced and solved numerically. For various types of coupling distribution, we obtain accurate results for magnetization, particularly in the presence of a weak external magnetic field. We show that in the weak magnetic field limit, similar to the 1D model, magnetization exhibits a singular power-law behavior with divergent susceptibility. Remarkably, the spectrum of magnetic exponents is markedly different from that of the 1D system even in the case of two coupled chains. The magnetic exponent makes a crossover from being dependent on a distribution function to a constant value independent of distribution. We provide an analytic theory for these observations by extending the Chen-Ma argument to the Q1D case. We derive an analytical formula for the exponent which is in perfect agreement with the numerical results.

Hadron-quark crossover and hot neutron stars at birth

NASA Astrophysics Data System (ADS)

Masuda, Kota; Hatsuda, Tetsuo; Takatsuka, Tatsuyuki

2016-02-01

We construct a new isentropic equation of state (EOS) at finite temperature, "CRover," on the basis of the hadron-quark crossover at high density. By using the new EOS, we study the structure of hot neutron stars at birth with typical lepton fraction (Y_l=0.3-0.4) and typical entropy per baryon (hat {S}=1{-}2). Due to the gradual appearance of quark degrees of freedom at high density, the temperature T and the baryon density ρ at the center of hot neutron stars with hadron-quark crossover are found to be smaller than those without the crossover by a factor of two or more. Typical energy release due to the contraction of a hot neutron star to a cold neutron star with mass M=1.4 M_{⊙} is shown to be about 0.04 M_{⊙}, with a spin-up rate of about 14%.

Aging, rejuvenation, and memory effects in short-range Ising spin glass: Cu_0.5Co_0.5Cl_2-FeCl3 GBIC

NASA Astrophysics Data System (ADS)

Suzuki, M.; Suzuki, I. S.

2004-03-01

Cu_0.5Co_0.5Cl_2-FeCl3 GBIC undergoes a spin glass (SG) transition at Tg (= 3.92 ± 0.11 K). The system shows a dynamic behavior that has some similarities and some significant differences compared to a 3D Ising SG.^1 Here we report on non-equilibrium aging dynamics which has been studied using zero-field cooled (ZFC) magnetization and low frequency AC magnetic susceptibility.^2 The time dependence of the relaxation rate S(t) = (1/H)dM_ZFC/dln t for the ZFC magnetization after the ZFC aging protocol, shows a peak at a characteristic time t_cr near a wait time t_w, corresponding to a crossover from quasi equilibrium dynamics to non-equilibrium. The time t_cr strongly depends on t_w, temperature, magnetic field, and the temperature shift. The rejuvenation effect is observed in both i^' and i^'' under the T-shift and H-shift procedures. The memory of the specific spin configurations imprinted during the ZFC aging protocol can be recalled when the system is re-heated at a constant heating rate. The aging, rejuvenation, and memory effects are discussed in terms of the scaling concepts derived from numerical studies on 3D Edwards-Anderson spin glass model. 1. I.S. Suzuki and M. Suzuki, Phys. Rev. B 68, 094424 (2003) 2. M. Suzuki and I.S. Suzuki, cond-mat/0308285

A mononuclear iron(II) complex: cooperativity, kinetics and activation energy of the solvent-dependent spin transition.

PubMed

Bushuev, Mark B; Pishchur, Denis P; Logvinenko, Vladimir A; Gatilov, Yuri V; Korolkov, Ilya V; Shundrina, Inna K; Nikolaenkova, Elena B; Krivopalov, Viktor P

2016-01-07

The system [FeL2](BF4)2 (1)-EtOH-H2O (L is 4-(3,5-dimethyl-1H-pyrazol-1-yl)-2-(pyridin-2-yl)-6-methylpyrimidine) shows a complicated balance between the relative stabilities of solvatomorphs and polymorphs of the complex [FeL2](BF4)2. New solvatomorphs, 1(LS)·EtOH·H2O and β-1(LS)·xH2O, were isolated in this system. They were converted into four daughter phases, 1(A/LS), 1(D/LS), 1(E/LS)·yEtOH·zH2O and 1(F/LS). On thermal cycling in sealed ampoules, the phases 1(LS)·EtOH·H2O and β-1(LS)·xH2O transform into the anhydrous phase 1(A/LS). The hysteresis loop width for the (A/LS) ↔ (A/HS) spin transition depends on the water and ethanol contents in the ampoule and varies from ca. 30 K up to 145 K. The reproducible hysteresis loop of 145 K is the widest ever reported one for a spin crossover complex. The phase 1(A/LS) combines the outstanding spin crossover properties with thermal robustness allowing for multiple cycling in sealed ampoules without degradation. The kinetics of the 1(A/LS) → 1(A/HS) transition is sigmoidal which is indicative of strong cooperative interactions. The cooperativity of the 1(A/LS) → 1(A/HS) transition is related to the formation of a 2D supramolecular structure of the phase 1(A/LS). The activation energy for the spin transition is very high (hundreds of kJ mol(-1)). The kinetics of the 1(A/HS) → 1(A/LS) transition can either be sigmoidal or exponential depending on the water and ethanol contents in the ampoule. The phases 1(D/LS) and 1(F/LS) show gradual crossover, whereas the phase 1(E/LS)·yEtOH·yH2O shows a reversible hysteretic transition associated with the solvent molecule release and uptake.

Theoretical Study of Spin Crossover in 30 Iron Complexes.

PubMed

Kepp, Kasper P

2016-03-21

Iron complexes are important spin crossover (SCO) systems with vital roles in oxidative metabolism and promising technological potential. The SCO tendency depends on the free energy balance of high- and low-spin states, which again depends on physical effects such as dispersion, relativistic effects, and vibrational entropy. This work studied 30 different iron SCO systems with experimentally known thermochemical data, using 12 different density functionals. Remarkably general entropy-enthalpy compensation across SCO systems was identified (R = 0.82, p = 0.002) that should be considered in rational SCO design. Iron(II) complexes displayed higher ΔH and ΔS values than iron(III) complexes and also less steep compensation effects. First-coordination sphere ΔS values computed from numerical frequencies reproduce most of the experimental entropy and should thus be included when modeling spin-state changes in inorganic chemistry (R = 0.52, p = 3.4 × 10(-3); standard error in TΔS ≈ 4.4 kJ/mol at 298 K vs 16 kJ/mol of total TΔS on average). Zero-point energies favored high-spin states by 9 kJ/mol on average. Interestingly, dispersion effects are surprisingly large for the SCO process (average: 9 kJ/mol, but up to 33 kJ/mol) and favor the more compact low-spin state. Relativistic effects favor low-spin by ∼9 kJ/mol on average, but up to 24 kJ/mol. B3LYP*, TPSSh, B2PLYP, and PW6B95 performed best for the typical calculation scheme that includes ZPE. However, if relativistic and dispersion effects are included, only B3LYP* remained accurate. On average, high-spin was favored by LYP by 11-15 kJ/mol relative to other correlation functionals, and by 4.2 kJ/mol per 1% HF exchange in hybrids. 13% HF exchange was optimal without dispersion, and 15% was optimal with all effects included for these systems.

Multiscale Experimental and Theoretical Investigations of Spin Crossover FeII Complexes: Examples of [Fe(phen)2(NCS)2] and [Fe(PM-BiA)2(NCS)2

PubMed Central

Matar, Samir F.; Guionneau, Philippe; Chastanet, Guillaume

2015-01-01

For spin crossover (SCO) complexes, computation results are reported and confirmed with experiments at multiscale levels of the isolated molecule and extended solid on the one hand and theory on the other hand. The SCO phenomenon which characterizes organometallics based on divalent iron in an octahedral FeN6-like environment with high spin (HS) and low spin (LS) states involves the LS/HS switching at the cost of small energies provided by temperature, pressure or light, the latter connected with Light-Induced Excited Spin-State Trapping (LIESST) process. Characteristic infra red (IR) and Raman vibration frequencies are computed within density functional theory (DFT) framework. In [Fe(phen)2(NCS)2] a connection of selected frequencies is established with an ultra-fast light-induced LS → HS photoswitching mechanism. In the extended solid, density of state DOS and electron localization function (ELF) are established for both LS and HS forms, leading to characterizion of the compound as an insulator in both spin states with larger gaps for LS configuration, while keeping molecular features in the solid. In [Fe(PM-BiA)2(NCS)2], by combining DFT and classical molecular dynamics, the properties and the domains of existence of the different phases are obtained by expressing the potential energy surfaces in a short range potential for Fe–N interactions. Applying such Fe–N potentials inserted in a classical force field and carrying out molecular dynamics (MD) in so-called “semi-classical MD” calculations, lead to the relative energies of HS/LS configurations of the crystal and to the assessment of the experimental (P, T) phase diagram. PMID:25686037

Ab Initio Ligand Field Molecular Mechanics and the Nature of Metal-Ligand π-Bonding in Fe(II) 2,6-di(pyrazol-1-yl)pyridine Spin Crossover Complexes.

PubMed

Deeth, Robert J; Halcrow, Malcolm A; Kershaw Cook, Laurence J; Raithby, Paul R

2018-04-06

A ligand field molecular mechanics (LFMM) force field has been constructed for the spin states of [Fe(bpp) 2 ] 2+ (bpp=2,6-di(pyrazol-1-yl)pyridine) and related complexes. A new charge scheme is employed which interpolates between partial charges for neutral bpp and protonated [H 3 bpp] 3+ to achieve a target metal charge. The LFMM angular overlap model (AOM) parameters are fitted to fully ab initio d orbital energies. However, several AOM parameter sets are possible. The ambiguity is resolved by calculating the Jahn-Teller distortion mode for high spin, which indicates that in [Fe(bpp) 2 ] 2+ pyridine is a π-acceptor and pyrazole a weak π-donor. The alternative fit, assumed previously, where both ligands act as π-donors leads to an inconsistent distortion. LFMM optimisations in the presence of [BF 4 ] - or [PF 6 ] - anions are in good agreement with experiment and the model also correctly predicts the spin state energetics for 3-pyrazolyl substituents where the interactions are mainly steric. However, for 4-pyridyl or 4-pyrazolyl substituents, LFMM only treats the electrostatic contribution which, for the pyridyl substituents, generates a fair correlation with the spin crossover transition temperatures, T 1/2 , but in the reverse sense to the dominant electronic effect. Thus, LFMM generates its smallest spin state energy difference for the substituent with the highest T 1/2 . One parameter set for all substituted bpp ligands is insufficient and further LFMM development will be required. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Compensation effects and relation between the activation energy of spin transition and the hysteresis loop width for an iron(ii) complex.

PubMed

Bushuev, Mark B; Pishchur, Denis P; Nikolaenkova, Elena B; Krivopalov, Viktor P

2016-06-22

The enthalpy-entropy compensation was observed for the cooperative → spin transition (the phase is a mononuclear complex [FeL2](BF4)2, L is 4-(3,5-dimethyl-1H-pyrazol-1-yl)-2-(pyridin-2-yl)-6-methylpyrimidine). The physical origin of this effect is the fact that the → spin transition is the first order phase transition accompanied by noticeable variations in the Tonset↑, ΔH and ΔS values. Higher ΔH and ΔS values are correlated with higher Tonset↑ values. The higher the enthalpy and entropy of the spin transition, the wider the hysteresis loop. The kinetic compensation effect, i.e. a linear relationship between ln A and Ea, was observed for the → spin transition. Moreover, an isokinetic relationship was detected in this system: the Arrhenius lines (ln k vs. 1/T) obtained from magnetochemical data for different samples of the phase undergoing the → transition show a common point of intersection (Tiso = 490 ± 2 K, ln kiso = -6.0 ± 0.2). The validity of this conclusion was confirmed by the Exner-Linert statistical method. This means that the isokinetic relationship and the kinetic compensation effect (ln A vs. Ea) in this system are true ones. The existence of a true kinetic compensation effect is supported independently by the fact that the hysteresis loop width for the cooperative spin transition ↔ increases with increasing activation barrier height. Estimating the energy of excitations for the phase with Tiso ∼ 490 K yields wavenumbers of ca. 340 cm(-1) corresponding to the frequencies of the stretching vibrations of the Fe(LS)-N bonds, i.e. the bonds directly involved in the mechanism of the spin transition. This is the first observation of the kinetic compensation effect (ln A vs. Ea) and the isokinetic relationship for a cooperative spin crossover system showing thermal hysteresis. Our results provide the first experimental evidence that the higher the activation barrier for the spin transition, the wider the hysteresis loop for a series of related spin crossover systems.

Matrix product states for su(2) invariant quantum spin chains

NASA Astrophysics Data System (ADS)

Zadourian, Rubina; Fledderjohann, Andreas; Klümper, Andreas

2016-08-01

A systematic and compact treatment of arbitrary su(2) invariant spin-s quantum chains with nearest-neighbour interactions is presented. The ground-state is derived in terms of matrix product states (MPS). The fundamental MPS calculations consist of taking products of basic tensors of rank 3 and contractions thereof. The algebraic su(2) calculations are carried out completely by making use of Wigner calculus. As an example of application, the spin-1 bilinear-biquadratic quantum chain is investigated. Various physical quantities are calculated with high numerical accuracy of up to 8 digits. We obtain explicit results for the ground-state energy, entanglement entropy, singlet operator correlations and the string order parameter. We find an interesting crossover phenomenon in the correlation lengths.

Electronic transition and electrical transport properties of delafossite CuCr1-xMgxO2 (0 ≤ x ≤ 12%) films prepared by the sol-gel method: A composition dependence study

NASA Astrophysics Data System (ADS)

Han, M. J.; Duan, Z. H.; Zhang, J. Z.; Zhang, S.; Li, Y. W.; Hu, Z. G.; Chu, J. H.

2013-10-01

Highly transparent CuCr1-xMgxO2 (0 ≤ x ≤ 12%) films were prepared on (001) sapphire substrates by sol-gel method. The microstructure, phonon modes, optical band gap, and electrical transport properties have been systematically discussed. It was found that Mg-doping improved the crystal quality and enhanced the (00l) preferred orientation. The spectral transmittance of films approaches about 70%-75% in the visible-near-infrared wavelength region. With increasing Mg-composition, the optical band gap first declines and climbs up due to the band gap renormalization and Burstein-Moss effect. The direct and indirect band gaps of CuCr0.94Mg0.06O2 film are 3.00 and 2.56 eV, respectively. In addition, it shows a crossover from the thermal activation behavior to that of three-dimensional variable range hopping from temperature-dependent electrical conductivity. The crossover temperature decreases with increasing Mg-doping composition, which can be ascribed to the change of spin-charge coupling between the hole and the local spin at Cr site. It should be noted that the electrical conductivity of CuCr1-xMgxO2 films becomes larger with increasing x value. The highest electrical conductivity of 3.85 S cm-1 at room temperature for x = 12% is four-order magnitude larger than that (8.81 × 10-4 S cm-1) for pure CuCrO2 film. The high spectral transmittance and larger conductivity indicate that Mg-doped CuCrO2 films are promising for optoelectronic device applications.

Quantum Discord in a Spin System with Symmetry Breaking

NASA Astrophysics Data System (ADS)

Tomasello, Bruno; Rossini, Davide; Hamma, Alioscia; Amico, Luigi

2013-06-01

We analyze the quantum discord Q throughout the low temperature phase diagram of the quantum XY model in transverse field. We first focus on the T = 0 order-disorder quantum phase transition QPT both in the symmetric ground state and in the symmetry broken one. Beside it, we highlight how Q displays clear anomalies also at a noncritical value of the control parameter inside the ordered phase, where the ground state is completely factorized. We evidence how the phenomenon is in fact of collective nature and displays universal features. We also study Q at finite temperature. We show that, close to the QPT, Q exhibits quantum-classical crossover of the system with universal scaling behavior. We evidence a nontrivial pattern of thermal correlations resulting from the factorization phenomenon.

Quantum Discord in a Spin System with Symmetry Breaking

NASA Astrophysics Data System (ADS)

Tomasello, Bruno; Rossini, Davide; Hamma, Alioscia; Amico, Luigi

2012-11-01

We analyze the quantum discordQ throughout the low temperature phase diagram of the quantum XY model in transverse field. We first focus on the T = 0 order-disorder quantum phase transition QPT both in the symmetric ground state and in the symmetry broken one. Beside it, we highlight how Q displays clear anomalies also at a noncritical value of the control parameter inside the ordered phase, where the ground state is completely factorized. We evidence how the phenomenon is in fact of collective nature and displays universal features. We also study Q at finite temperature. We show that, close to the QPT, Q exhibits quantum-classical crossover of the system with universal scaling behavior. We evidence a nontrivial pattern of thermal correlations resulting from the factorization phenomenon.

NMR and Electrochemical Investigation of the Transport Properties of Methanol and Water in Nafion and Clay-Nanocomposites Membranes for DMFCs

PubMed Central

Nicotera, Isabella; Angjeli, Kristina; Coppola, Luigi; Aricò, Antonino S.; Baglio, Vincenzo

2012-01-01

Water and methanol transport behavior, solvents adsorption and electrochemical properties of filler-free Nafion and nanocomposites based on two smectite clays, were investigated using impedance spectroscopy, DMFC tests and NMR methods, including spin-lattice relaxation and pulsed-gradient spin-echo (PGSE) diffusion under variable temperature conditions. Synthetic (Laponite) and natural (Swy-2) smectite clays, with different structural and physical parameters, were incorporated into the Nafion for the creation of exfoliated nanocomposites. Transport mechanism of water and methanol appears to be influenced from the dimensions of the dispersed platelike silicate layers as well as from their cation exchange capacity (CEC). The details of the NMR results and the effect of the methanol solution concentration are discussed. Clays particles, and in particular Swy-2, demonstrate to be a potential physical barrier for methanol cross-over, reducing the methanol diffusion with an evident blocking effect yet nevertheless ensuring a high water mobility up to 130 °C and for several hours, proving the exceptional water retention property of these materials and their possible use in the DMFCs applications. Electrochemical behavior is investigated by cell resistance and polarization measurements. From these analyses it is derived that the addition of clay materials to recast Nafion decreases the ohmic losses at high temperatures extending in this way the operating range of a direct methanol fuel cell. PMID:24958179

Are Emotions Transmitted From Work to Family? A Crossover Model of Psychological Contract Breach.

PubMed

Liang, Huai-Liang

2018-01-01

Based on affective events theory and the crossover model, this study examines the effect of psychological contract breach on employee dysfunctional behavior and partner family undermining and explores the crossover effect of employee dysfunctional behavior on partner family undermining in work-family issues. This study collected 370 employee-partner dyads (277 male employees, 93 female employees, M age = 43.59 years) from a large manufacturing organization. The results of this study support the conception that employees' psychological contract breach results in frustration in the workplace. In addition, mediation analysis results reveal that psychological contract breach relates to employee dysfunctional behavior in the workplace. The findings show that partners' psychological strain mediates the relationship between employee dysfunctional behavior and partner family undermining. Furthermore, these findings provide investigations for the crossover model to display the value of psychological contract breach in family issues.

2D Spin Crossover Nanoparticles described by the Ising-like model solved in Local Mean-Field Approximation

NASA Astrophysics Data System (ADS)

Eddine Allal, Salah; Linares, Jorge; Boukheddaden, K.; Dahoo, Pierre Richard; de Zela, F.

2017-12-01

Some six-coordinate iron (II) coordination compounds exhibit thermal-, optical-, electrical-, magnetic- and pressure-induced switching between the diamagnetic low-spin (LS, S=0) and the paramagnetic high-spin (HS; S=2) states [1]. This may lead to potential application of these complexes in molecular devices such as temperature and pressure sensors [2]. An Ising-like model has been proposed to explain the occurrence of the thermal hysteresis behaviour [3,4] of this switchable solids. In this contribution, the local mean field approximation is applied to solve the Hamiltonian modelling interactions pertaining to 2D nanoparticles embedded in a magnetically-inactive matrix.

Dynamical properties of the S =1/2 random Heisenberg chain

NASA Astrophysics Data System (ADS)

Shu, Yu-Rong; Dupont, Maxime; Yao, Dao-Xin; Capponi, Sylvain; Sandvik, Anders W.

2018-03-01

We study dynamical properties at finite temperature (T ) of Heisenberg spin chains with random antiferromagnetic exchange couplings, which realize the random singlet phase in the low-energy limit, using three complementary numerical methods: exact diagonalization, matrix-product-state algorithms, and stochastic analytic continuation of quantum Monte Carlo results in imaginary time. Specifically, we investigate the dynamic spin structure factor S (q ,ω ) and its ω →0 limit, which are closely related to inelastic neutron scattering and nuclear magnetic resonance (NMR) experiments (through the spin-lattice relaxation rate 1 /T1 ). Our study reveals a continuous narrow band of low-energy excitations in S (q ,ω ) , extending throughout the q space, instead of being restricted to q ≈0 and q ≈π as found in the uniform system. Close to q =π , the scaling properties of these excitations are well captured by the random-singlet theory, but disagreements also exist with some aspects of the predicted q dependence further away from q =π . Furthermore we also find spin diffusion effects close to q =0 that are not contained within the random-singlet theory but give non-negligible contributions to the mean 1 /T1 . To compare with NMR experiments, we consider the distribution of the local relaxation rates 1 /T1 . We show that the local 1 /T1 values are broadly distributed, approximately according to a stretched exponential. The mean 1 /T1 first decreases with T , but below a crossover temperature it starts to increase and likely diverges in the limit of a small nuclear resonance frequency ω0. Although a similar divergent behavior has been predicted and experimentally observed for the static uniform susceptibility, this divergent behavior of the mean 1 /T1 has never been experimentally observed. Indeed, we show that the divergence of the mean 1 /T1 is due to rare events in the disordered chains and is concealed in experiments, where the typical 1 /T1 value is accessed.

Discovering phases, phase transitions, and crossovers through unsupervised machine learning: A critical examination

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hu, Wenjian; Singh, Rajiv R. P.; Scalettar, Richard T.

Here, we apply unsupervised machine learning techniques, mainly principal component analysis (PCA), to compare and contrast the phase behavior and phase transitions in several classical spin models - the square and triangular-lattice Ising models, the Blume-Capel model, a highly degenerate biquadratic-exchange spin-one Ising (BSI) model, and the 2D XY model, and examine critically what machine learning is teaching us. We find that quantified principal components from PCA not only allow exploration of different phases and symmetry-breaking, but can distinguish phase transition types and locate critical points. We show that the corresponding weight vectors have a clear physical interpretation, which ismore » particularly interesting in the frustrated models such as the triangular antiferromagnet, where they can point to incipient orders. Unlike the other well-studied models, the properties of the BSI model are less well known. Using both PCA and conventional Monte Carlo analysis, we demonstrate that the BSI model shows an absence of phase transition and macroscopic ground-state degeneracy. The failure to capture the 'charge' correlations (vorticity) in the BSI model (XY model) from raw spin configurations points to some of the limitations of PCA. Finally, we employ a nonlinear unsupervised machine learning procedure, the 'antoencoder method', and demonstrate that it too can be trained to capture phase transitions and critical points.« less

Discovering phases, phase transitions, and crossovers through unsupervised machine learning: A critical examination

DOE PAGES

Hu, Wenjian; Singh, Rajiv R. P.; Scalettar, Richard T.

2017-06-19

Here, we apply unsupervised machine learning techniques, mainly principal component analysis (PCA), to compare and contrast the phase behavior and phase transitions in several classical spin models - the square and triangular-lattice Ising models, the Blume-Capel model, a highly degenerate biquadratic-exchange spin-one Ising (BSI) model, and the 2D XY model, and examine critically what machine learning is teaching us. We find that quantified principal components from PCA not only allow exploration of different phases and symmetry-breaking, but can distinguish phase transition types and locate critical points. We show that the corresponding weight vectors have a clear physical interpretation, which ismore » particularly interesting in the frustrated models such as the triangular antiferromagnet, where they can point to incipient orders. Unlike the other well-studied models, the properties of the BSI model are less well known. Using both PCA and conventional Monte Carlo analysis, we demonstrate that the BSI model shows an absence of phase transition and macroscopic ground-state degeneracy. The failure to capture the 'charge' correlations (vorticity) in the BSI model (XY model) from raw spin configurations points to some of the limitations of PCA. Finally, we employ a nonlinear unsupervised machine learning procedure, the 'antoencoder method', and demonstrate that it too can be trained to capture phase transitions and critical points.« less

Discovering phases, phase transitions, and crossovers through unsupervised machine learning: A critical examination

NASA Astrophysics Data System (ADS)

Hu, Wenjian; Singh, Rajiv R. P.; Scalettar, Richard T.

2017-06-01

We apply unsupervised machine learning techniques, mainly principal component analysis (PCA), to compare and contrast the phase behavior and phase transitions in several classical spin models—the square- and triangular-lattice Ising models, the Blume-Capel model, a highly degenerate biquadratic-exchange spin-1 Ising (BSI) model, and the two-dimensional X Y model—and we examine critically what machine learning is teaching us. We find that quantified principal components from PCA not only allow the exploration of different phases and symmetry-breaking, but they can distinguish phase-transition types and locate critical points. We show that the corresponding weight vectors have a clear physical interpretation, which is particularly interesting in the frustrated models such as the triangular antiferromagnet, where they can point to incipient orders. Unlike the other well-studied models, the properties of the BSI model are less well known. Using both PCA and conventional Monte Carlo analysis, we demonstrate that the BSI model shows an absence of phase transition and macroscopic ground-state degeneracy. The failure to capture the "charge" correlations (vorticity) in the BSI model (X Y model) from raw spin configurations points to some of the limitations of PCA. Finally, we employ a nonlinear unsupervised machine learning procedure, the "autoencoder method," and we demonstrate that it too can be trained to capture phase transitions and critical points.

Influence of deposition conditions on the nature of epitaxial SrIrO3 on STO (001)

NASA Astrophysics Data System (ADS)

Bhat, Shwetha G.; Sebastian, Nirmal K.; Kumar, P. S. Anil

2018-05-01

SrIrO3 (SIO) is one of the materials known to exhibit a high spin-orbit coupling with correlated semi-metallic ground state, along with the topological states, as proven in recent times. In this regard, the SIO thin films grown by us on SrTiO3 (001) at certain deposition conditions, exhibit a low temperature magneto-transport behavior which is analogous to the materials with topological states. Further, we have explored various deposition conditions of SIO such as partial pressure of O2 and different temperatures of growth for different thickness of SIO. In addition, from the electrical transport properties, SIO thin films found to exhibit semi-metallic nature with either insulating-like or a crossover from metal-like to insulating-like behavior based on the conditions chosen for the growth. Moreover, the magneto-transport data of various SIO thin films are found to be obeying the usual B2 (Lorentzian) behavior in majority of the cases. At the same time, we have also observed the weak-localization and weak-antilocalization effects; along with a linear magneto-resistance at low temperature ranges. Thus, from our extensive measurements, it becomes clear that SIO thin films can exhibit wide varieties of magneto-transport properties based on the deposition conditions. Plethora of interesting properties exhibited by the highly spin-orbit coupled SIO epitaxial thin films at lower temperatures in the presence of magnetic field makes the material to be promising for the future applications in the field of spintronics.

First-principles study of crystal and electronic structure of rare-earth cobaltites

DOE Office of Scientific and Technical Information (OSTI.GOV)

Topsakal, M.; Leighton, C.; Wentzcovitch, R. M.

Using density functional theory plus self-consistent Hubbard U (DFT + U{sub sc}) calculations, we have investigated the structural and electronic properties of the rare-earth cobaltites RCoO{sub 3} (R = Pr – Lu). Our calculations show the evolution of crystal and electronic structure of the insulating low-spin RCoO{sub 3} with increasing rare-earth atomic number (decreasing ionic radius), including the invariance of the Co-O bond distance (d{sub Co–O}), the decrease of the Co-O-Co bond angle (Θ), and the increase of the crystal field splitting (Δ{sub CF}) and band gap energy (E{sub g}). Agreement with experiment for the latter improves considerably with the use of DFT + U{sub sc}more » and all trends are in good agreement with the experimental data. These trends enable a direct test of prior rationalizations of the trend in spin-gap associated with the spin crossover in this series, which is found to expose significant issues with simple band based arguments. We also examine the effect of placing the rare-earth f-electrons in the core region of the pseudopotential. The effect on lattice parameters and band structure is found to be small, but distinct for the special case of PrCoO{sub 3} where some f-states populate the middle of the gap, consistent with the recent reports of unique behavior in Pr-containing cobaltites. Overall, this study establishes a foundation for future predictive studies of thermally induced spin excitations in rare-earth cobaltites and similar systems.« less

Abrupt spin transition with thermal hysteresis of iron(III) complex [Fe(III)(Him)2(hapen)]AsF6 (Him = imidazole, H2hapen = N,N'-bis(2-hydroxyacetophenylidene)ethylenediamine).

PubMed

Fujinami, Takeshi; Koike, Masataka; Matsumoto, Naohide; Sunatsuki, Yukinari; Okazawa, Atsushi; Kojima, Norimichi

2014-02-17

The solvent-free spin crossover iron(III) complex [Fe(III)(Him)2(hapen)]AsF6 (Him = imidazole, H2hapen = N,N'-bis(2-hydroxyacetophenylidene)ethylenediamine), exhibiting thermal hysteresis, was synthesized and characterized. The Fe(III) ion has an octahedral coordination geometry, with N2O2 donor atoms of the planar tetradentate ligand (hapen) and two nitrogen atoms of two imidazoles at the axial positions. One of two imidazoles is hydrogen-bonded to the phenoxo oxygen atom of hapen of the adjacent unit to give a hydrogen-bonded one-dimensional chain, while the other imidazole group is free from hydrogen bonding. The temperature dependencies of the magnetic susceptibilities and Mössbauer spectra revealed an abrupt spin transition between the high-spin (S = 5/2) and low-spin (S = 1/2) states, with thermal hysteresis.

The reduction of carbon dioxide in iron biocatalyst catalytic hydrogenation reaction: a theoretical study.

PubMed

Yang, Longhua; Wang, Hongming; Zhang, Ning; Hong, Sanguo

2013-08-21

The reaction mechanism of CO₂ hydrogenation catalyzed by [FeH(PP₃)]BF₄ (PP₃ = P(CH₂CH₂PPh₂)₃) had been investigated by DFT calculations. Our calculations indicated that the reduction of carbon dioxide could be carried out via two spin states, the high-spin (HS) triplet state and the low-spin (LS) singlet state. The minimum energy crossing points (MECPs) on the seam of two intersecting PESs (potential energy surfaces) were searched out. Some interesting phenomena, such as the open-loop phenomenon, and the O-rebound process, were demonstrated to be the important causes of the spin crossover. All these calculations gave us insight into the essence of the related experiment from the macro point of view, and helped to verify which spin states the related complexes pertinent were in. All of these researches would help advance the development of efficient and structurally tailorable CO₂ hydrogenation catalysts.

Six different roles for crossover inhibition in the retina: correcting the nonlinearities of synaptic transmission.

PubMed

Werblin, Frank S

2010-03-01

Early retinal studies categorized ganglion cell behavior as either linear or nonlinear and rectifying as represented by the familiar X- and Y-type ganglion cells in cat. Nonlinear behavior is in large part a consequence of the rectifying nonlinearities inherent in synaptic transmission. These nonlinear signals underlie many special functions in retinal processing, including motion detection, motion in motion, and local edge detection. But linear behavior is also required for some visual processing tasks. For these tasks, the inherently nonlinear signals are "linearized" by "crossover inhibition." Linearization utilizes a circuitry whereby nonlinear ON inhibition adds with nonlinear OFF excitation or ON excitation adds with OFF inhibition to generate a more linear postsynaptic voltage response. Crossover inhibition has now been measured in most bipolar, amacrine, and ganglion cells. Functionally crossover inhibition enhances edge detection, allows ganglion cells to recognize luminance-neutral patterns with their receptive fields, permits ganglion cells to distinguish contrast from luminance, and maintains a more constant conductance during the light response. In some cases, crossover extends the operating range of cone-driven OFF ganglion cells into the scotopic levels. Crossover inhibition is also found in neurons of the lateral geniculate nucleus and V1.

Kinetic consequences of introducing a proximal selenocysteine ligand into cytochrome P450cam.

PubMed

Vandemeulebroucke, An; Aldag, Caroline; Stiebritz, Martin T; Reiher, Markus; Hilvert, Donald

2015-11-10

The structural, electronic, and catalytic properties of cytochrome P450cam are subtly altered when the cysteine that coordinates to the heme iron is replaced with a selenocysteine. To map the effects of the sulfur-to-selenium substitution on the individual steps of the catalytic cycle, we conducted a comparative kinetic analysis of the selenoenzyme and its cysteine counterpart. Our results show that the more electron-donating selenolate ligand has only negligible effects on substrate, product, and oxygen binding, electron transfer, catalytic turnover, and coupling efficiency. Off-pathway reduction of oxygen to give superoxide is the only step significantly affected by the mutation. Incorporation of selenium accelerates this uncoupling reaction approximately 50-fold compared to sulfur, but because the second electron transfer step is much faster, the impact on overall catalytic turnover is minimal. Density functional theory calculations with pure and hybrid functionals suggest that superoxide formation is governed by a delicate interplay of spin distribution, spin state, and structural effects. In light of the remarkably similar electronic structures and energies calculated for the sulfur- and selenium-containing enzymes, the ability of the heavier atom to enhance the rate of spin crossover may account for the experimental observations. Because the selenoenzyme closely mimics wild-type P450cam, even at the level of individual steps in the reaction cycle, selenium represents a unique mechanistic probe for analyzing the role of the proximal ligand and spin crossovers in P450 chemistry.

Scan Rate Dependent Spin Crossover Iron(II) Complex with Two Different Relaxations and Thermal Hysteresis fac-[Fe(II)(HL(n-Pr))3]Cl·PF6 (HL(n-Pr) = 2-Methylimidazol-4-yl-methylideneamino-n-propyl).

PubMed

Fujinami, Takeshi; Nishi, Koshiro; Hamada, Daisuke; Murakami, Keishiro; Matsumoto, Naohide; Iijima, Seiichiro; Kojima, Masaaki; Sunatsuki, Yukinari

2015-08-03

Solvent-free spin crossover Fe(II) complex fac-[Fe(II)(HL(n-Pr))3]Cl·PF6 was prepared, where HL(n-Pr) denotes 2-methylimidazol-4-yl-methylideneamino-n-propyl. The magnetic susceptibility measurements at scan rate of 0.5 K min(-1) showed two successive spin transition processes consisting of the first spin transition T1 centered at 122 K (T1↑ = 127.1 K, T1↓ = 115.8 K) and the second spin transition T2 centered at ca. 105 K (T2↑ = 115.8 K, T2↓ = 97.2 K). The magnetic susceptibility measurements at the scan rate of 2.0, 1.0, 0.5, 0.25, and 0.1 K min(-1) showed two scan speed dependent spin transitions, while the Mössbauer spectra detected only the first spin transition T1. The crystal structures were determined at 160, 143, 120, 110, 95 K in the cooling mode, and 110, 120, and 130 K in the warming mode so as to follow the spin transition process of high-spin HS → HS(T1) → HS(T2) → low-spin LS → LS(T2) → LS(T1) → HS. The crystal structures at all temperatures have a triclinic space group P1̅ with Z = 2. The complex-cation has an octahedral N6 coordination geometry with three bidentate ligands and assume a facial-isomer with Δ- and Λ-enantimorphs. Three imidazole groups of fac-[Fe(II)(HL(n-Pr))3](2+) are hydrogen-bonded to three Cl(-) ions. The 3:3 NH(imidazole)···Cl(-) hydrogen-bonds form a stepwise ladder assembly structure, which is maintained during the spin transition process. The spin transition process is related to the structural changes of the FeN6 coordination environment, the order-disorder of PF6(-) anion, and the conformation change of n-propyl groups. The Fe-N bond distance in the HS state is longer by 0.2 Å than that in the LS state. Disorder of PF6(-) anion is not observed in the LS state but in the HS state. The conformational changes of n-propyl groups are found in the spin transition processes except for HS → HS(T1) → HS(T2).

Spin crossover in liquid Fe2SiO4 at high pressures: an ab initio Molecular Dynamics study

NASA Astrophysics Data System (ADS)

Munoz Ramo, D.; Stixrude, L. P.

2010-12-01

Liquid iron silicate (Fe2SiO4) is an important component of natural silicate liquids appearing in Earth’s interior. The effect of iron in the properties of these melts is a crucial issue, as it displays a high-spin to low-spin transition at high pressures which is accompanied by volume reduction and changes in the optical absorption spectrum. This phenomenon has a major influence on properties like the buoyancy or the thermal conductivity of the melt, and ultimately on the chemical and thermal evolution of our planet. Computer simulations using ab initio methods have proven to be a powerful approach to the study of liquid silicate systems[1,2], although not yet including Fe. In this paper, we report ab initio molecular dynamics studies of liquid iron silicate at high pressure (up to 300 GPa) and high temperatures (from 3000K to 6000K) that allow us to predict different properties of the system. We use mainly the GGA density functional for the calculation of the electronic structure. We also perform simulations with the GGA+U formalism to estimate the impact of strong electron correlation effects in the properties of the system at high pressures. The spin-polarized formalism is also used in order to keep track of the evolution of the iron magnetic moments in the system. By means of these simulations we predict the short and medium-range structure and thermodynamic properties of the liquid. We compute the theoretical Hugoniot for the system and find very good agreement between the GGA results and the equation of state values obtained from shock experiments [3], while the GGA+U results overestimate the Hugoniot curve at high pressures. Density crossover with the solid is obtained at about 110 GPa at 3000 K. Our calculations show that the spin crossover in this system takes place at a wide pressure interval, dependent on temperature. At 3000K, the spin transition starts at around 10 GPa and finishes at pressures around 250 Gpa. Increase of the temperature to 6000K reduces the interval of the transition to 180 GPa. [1] N. P. de Koker, L. Stixrude, B. B. Karki, Geochim Cosmochim Acta 2008, 72, 1427. [2] B. B. Karki, D. Bhattarai, L. Stixrude, Phys. Rev. B 2007, 76, 104205. [3] G. Q. Chen, T. J. Ahrens, E. M. Stolper, Phys. Earth Planet. Inter. 2002, 134, 35.

Ligand manipulation of charge transfer excited state relaxation and spin crossover in [Fe(2,2'-bipyridine) 2(CN) 2

DOE PAGES

Kjaer, Kasper S.; Zhang, Wenkai; Alonso-Mori, Roberto; ...

2017-07-06

Here, we have used femtosecond resolution UV-visible and Kβ x-ray emission spectroscopy to characterize the electronic excited state dynamics of [Fe(bpy) 2(CN) 2], where bpy=2,2'-bipyridine, initiated by metal-to-ligand charge transfer (MLCT) excitation. The excited-state absorption in the transient UV-visible spectra, associated with the 2,2'-bipyridine radical anion, provides a robust marker for the MLCT excited state, while the transient Kβ x-ray emission spectra provide a clear measure of intermediate and high spin metal-centered excited states. From these measurements, we conclude that the MLCT state of [Fe(bpy) 2(CN) 2] undergoes ultrafast spin crossover to a metal-centered quintet excited state through a shortmore » lived metal-centered triplet transient species. These measurements of [Fe(bpy) 2(CN) 2] complement prior measurement performed on [Fe(bpy) 3] 2+ and [Fe(bpy)(CN) 4] 2– in dimethylsulfoxide solution and help complete the chemical series [Fe(bpy) N(CN) 6–2N] 2N-4, where N = 1–3. The measurements confirm that simple ligand modifications can significantly change the relaxation pathways and excited state lifetimes and support the further investigation of light harvesting and photocatalytic applications of 3 d transition metal complexes.« less

Ligand manipulation of charge transfer excited state relaxation and spin crossover in [Fe(2,2'-bipyridine) 2(CN) 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kjaer, Kasper S.; Zhang, Wenkai; Alonso-Mori, Roberto

Here, we have used femtosecond resolution UV-visible and Kβ x-ray emission spectroscopy to characterize the electronic excited state dynamics of [Fe(bpy) 2(CN) 2], where bpy=2,2'-bipyridine, initiated by metal-to-ligand charge transfer (MLCT) excitation. The excited-state absorption in the transient UV-visible spectra, associated with the 2,2'-bipyridine radical anion, provides a robust marker for the MLCT excited state, while the transient Kβ x-ray emission spectra provide a clear measure of intermediate and high spin metal-centered excited states. From these measurements, we conclude that the MLCT state of [Fe(bpy) 2(CN) 2] undergoes ultrafast spin crossover to a metal-centered quintet excited state through a shortmore » lived metal-centered triplet transient species. These measurements of [Fe(bpy) 2(CN) 2] complement prior measurement performed on [Fe(bpy) 3] 2+ and [Fe(bpy)(CN) 4] 2– in dimethylsulfoxide solution and help complete the chemical series [Fe(bpy) N(CN) 6–2N] 2N-4, where N = 1–3. The measurements confirm that simple ligand modifications can significantly change the relaxation pathways and excited state lifetimes and support the further investigation of light harvesting and photocatalytic applications of 3 d transition metal complexes.« less

Ligand manipulation of charge transfer excited state relaxation and spin crossover in [Fe(2,2′-bipyridine)2(CN)2

PubMed Central

Kjær, Kasper S.; Zhang, Wenkai; Alonso-Mori, Roberto; Bergmann, Uwe; Chollet, Matthieu; Hadt, Ryan G.; Hartsock, Robert W.; Harlang, Tobias; Kroll, Thomas; Kubiček, Katharina; Lemke, Henrik T.; Liang, Huiyang W.; Liu, Yizhu; Nielsen, Martin M.; Robinson, Joseph S.; Solomon, Edward I.; Sokaras, Dimosthenis; van Driel, Tim B.; Weng, Tsu-Chien; Zhu, Diling; Persson, Petter; Wärnmark, Kenneth; Sundström, Villy; Gaffney, Kelly J.

2017-01-01

We have used femtosecond resolution UV-visible and Kβ x-ray emission spectroscopy to characterize the electronic excited state dynamics of [Fe(bpy)2(CN)2], where bpy=2,2′-bipyridine, initiated by metal-to-ligand charge transfer (MLCT) excitation. The excited-state absorption in the transient UV-visible spectra, associated with the 2,2′-bipyridine radical anion, provides a robust marker for the MLCT excited state, while the transient Kβ x-ray emission spectra provide a clear measure of intermediate and high spin metal-centered excited states. From these measurements, we conclude that the MLCT state of [Fe(bpy)2(CN)2] undergoes ultrafast spin crossover to a metal-centered quintet excited state through a short lived metal-centered triplet transient species. These measurements of [Fe(bpy)2(CN)2] complement prior measurement performed on [Fe(bpy)3]2+ and [Fe(bpy)(CN)4]2− in dimethylsulfoxide solution and help complete the chemical series [Fe(bpy)N(CN)6–2N]2N-4, where N = 1–3. The measurements confirm that simple ligand modifications can significantly change the relaxation pathways and excited state lifetimes and support the further investigation of light harvesting and photocatalytic applications of 3d transition metal complexes. PMID:28653021

Anomalies of the electronic structure and physical properties of rare-earth cobaltites near spin crossover

NASA Astrophysics Data System (ADS)

Dudnikov, V. A.; Orlov, Yu. S.; Kazak, N. V.; Platunov, M. S.; Ovchinnikov, S. G.

2016-10-01

The features of the characteristics of LnCoO3 cobaltites, where Ln is a rare-earth element, are discussed. Both experiment and theory demonstrate that their essentials are related to the low-spin ground state of cobalt ions. The thermally induced occupation of the excited high-spin state gives rise to peaks in the magnetic susceptibility, specific heat, and thermal expansion, as well as to a smooth insulator-metal transition. The analysis is based both on the data from the current literature concerning LaCoO3 and in many aspects on our own studies of GdCoO3 and La1- x Gd x CoO3 solid solutions.

Monte Carlo investigations on surface elastic energy of spin-crossover solids: Direct access to image pressure and the Eshelby constant

NASA Astrophysics Data System (ADS)

Boukheddaden, Kamel

2013-10-01

We present theoretical investigations on surface elastic energy in spin-crossover (SC) solids studied in the frame of a microscopic elastic model, coupling spin, and lattice deformations. Although surface energy plays a crucial role in driving the SC transition, specific quantitative investigations on its effect have been neglected in most of the recent theoretical works based on atomistic descriptions of the SC transitions, resolved by Monte Carlo or by molecular dynamics simulations. Here, we perform a quantitative study of the surface energy resulting from an inserted high-spin (HS) domain in a low-spin (LS) lattice. This situation may be produced experimentally in SC solids, at low temperature, through a photoexcitation by a single pulse laser shot. We demonstrate that the surface energy depends on the ratio between the local molecular volume misfit (between the LS and HS sites) δυ and the lattice volume V, such as Esurf˜δυ2/V for the HS atom at the center of lattice, while it is Esurf˜δυ2/L (L is the length of the lattice) in the case of the HS atom located on the edge of the lattice. We then derived the image pressure (negative in the case of embedded dilatation centers) through the work of the free surface atoms and evaluated the Eshelby constant, which was found equal to γ˜1.90, in very good agreement with the available data of literature. Energetic configuration diagrams in the homogeneous (HS and LS) and heterogeneous (coexistence of HS and LS) are calculated, from which estimations of the macroscopic bulk modulus were deduced.

Spin transition in a four-coordinate iron oxide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kawakami, T.; Sutou, S.; Hirama, H.

2009-01-01

The spin transition, or spin crossover, is a manifestation of electronic instability induced by external constraints such as pressure1. Among known examples that exhibit spin transition, 3d ions with d6 electron configurations represent the vast majority, but the spin transition observed thus far has been almost exclusively limited to that between high-spin (S = 2) and low-spin (S = 0) states2-9. Here we report a novel high-spin to intermediate-spin (S = 1) state transition at 33 GPa induced by pressurization of an antiferromagnetic insulator SrFeO2 with a square planar coordination10. The change in spin multiplicity brings to ferromagnetism as wellmore » as metallicity, yet keeping the ordering temperature far above ambient. First-principles calculations attribute the origin of the transition to the strong inlayer hybridization between Fe dx 2 -y 2 O p , leading to a pressure-induced electronic instability toward the depopulation of Fe dx 2 -y 2 O p antibonding states. Furthermore, the ferromagnetic S = 1 state is half-metallic due to the inception of half-occupied spin-down (dxz, dyz) degenerate states upon spin transition. These results highlight the square-planar coordinated iron oxides as a new class of magnetic and electric materials and provide new avenues toward realizing multi-functional sensors and data-storage devices.« less

Prominent metallic surface conduction and the singular magnetic response of topological Dirac fermion in three-dimensional topological insulator Bi1.5Sb0.5Te1.7Se1.3.

PubMed

Dutta, Prithwish; Pariari, Arnab; Mandal, Prabhat

2017-07-07

We report semiconductor to metal-like crossover in the temperature dependence of resistivity (ρ) due to the switching of charge transport from bulk to surface channel in three-dimensional topological insulator Bi 1.5 Sb 0.5 Te 1.7 Se 1.3 . Unlike earlier studies, a much sharper drop in ρ(T) is observed below the crossover temperature due to the dominant surface conduction. Remarkably, the resistivity of the conducting surface channel follows a rarely observable T 2 dependence at low temperature, as predicted theoretically for a two-dimensional Fermi liquid system. The field dependence of magnetization shows a cusp-like paramagnetic peak in the susceptibility (χ) at zero field over the diamagnetic background. The peak is found to be robust against temperature and χ decays linearly with the field from its zero-field value. This unique behavior of the χ is associated with the spin-momentum locked topological surface state in Bi 1.5 Sb 0.5 Te 1.7 Se 1.3 . The reconstruction of the surface state with time is clearly reflected through the reduction of the peak height with the age of the sample.

Aging processes in disordered materials: High-Tc superconductors and ferromagnets

NASA Astrophysics Data System (ADS)

Pleimling, Michel

2013-03-01

Physical aging is generically encountered in systems far from equilibrium that evolve with slow dynamics. Well known examples can be found in structural glasses, spin glasses, magnetic systems, and colloids. Recent years have seen major breakthroughs in our understanding of aging processes in non-disordered systems. Progress in understanding aging in disordered systems has been much slower though. In this talk I discuss non-equilibrium relaxation in two different types of disordered systems: coarsening ferromagnets with disorder, characterized by a crossover from an initial power-law like growth of domains to a slower logarithmic growth regime, and interacting vortex lines in disordered type-II superconductors, where the interplay of vortex-vortex interaction and pinning results in a very rich non-equilibrium behavior. This work is supported by the US Department of Energy through grant DE-FG02-09ER46613.

The BCS-BEC crossover: From ultra-cold Fermi gases to nuclear systems

NASA Astrophysics Data System (ADS)

Strinati, Giancarlo Calvanese; Pieri, Pierbiagio; Röpke, Gerd; Schuck, Peter; Urban, Michael

2018-04-01

This report addresses topics and questions of common interest in the fields of ultra-cold gases and nuclear physics in the context of the BCS-BEC crossover. By this crossover, the phenomena of Bardeen-Cooper-Schrieffer (BCS) superfluidity and Bose-Einstein condensation (BEC), which share the same kind of spontaneous symmetry breaking, are smoothly connected through the progressive reduction of the size of the fermion pairs involved as the fundamental entities in both phenomena. This size ranges, from large values when Cooper pairs are strongly overlapping in the BCS limit of a weak inter-particle attraction, to small values when composite bosons are non-overlapping in the BEC limit of a strong inter-particle attraction, across the intermediate unitarity limit where the size of the pairs is comparable with the average inter-particle distance. The BCS-BEC crossover has recently been realized experimentally, and essentially in all of its aspects, with ultra-cold Fermi gases. This realization, in turn, has raised the interest of the nuclear physics community in the crossover problem, since it represents an unprecedented tool to test fundamental and unanswered questions of nuclear many-body theory. Here, we focus on the several aspects of the BCS-BEC crossover, which are of broad joint interest to both ultra-cold Fermi gases and nuclear matter, and which will likely help to solve in the future some open problems in nuclear physics (concerning, for instance, neutron stars). Similarities and differences occurring in ultra-cold Fermi gases and nuclear matter will then be emphasized, not only about the relative phenomenologies but also about the theoretical approaches to be used in the two contexts. Common to both contexts is the fact that at zero temperature the BCS-BEC crossover can be described at the mean-field level with reasonable accuracy. At finite temperature, on the other hand, inclusion of pairing fluctuations beyond mean field represents an essential ingredient of the theory, especially in the normal phase where they account for precursor pairing effects. After an introduction to present the key concepts of the BCS-BEC crossover, this report discusses the mean-field treatment of the superfluid phase, both for homogeneous and inhomogeneous systems, as well as for symmetric (spin- or isospin-balanced) and asymmetric (spin- or isospin-imbalanced) matter. Pairing fluctuations in the normal phase are then considered, with their manifestations in thermodynamic and dynamic quantities. The last two Sections provide a more specialized discussion of the BCS-BEC crossover in ultra-cold Fermi gases and nuclear matter, respectively. The separate discussion in the two contexts aims at cross communicating to both communities topics and aspects which, albeit arising in one of the two fields, share a strong common interest.

Enhanced specific heat jump in electron-doped CaMnO3: Spin ordering driven by charge separation

NASA Astrophysics Data System (ADS)

Moritomo, Y.; Machida, A.; Nishibori, E.; Takata, M.; Sakata, M.

2001-12-01

Temperature variation of the magnetic susceptibility χ, resistivity ρ, specific heat C, and lattice constants has been investigated in electron-doped CaMnO3. The parent CaMnO3 is an antiferromagnetic band insulator, and shows an insulator-metal crossover with electron doping, together with an enhanced ferromagnetic component. We have found an enhancement of the specific heat jump ΔC at the spin-ordering temperature Tspin and interpreted the enhancement in terms of the intrinsic charge separation.

Effect of sorbed methanol, current, and temperature on multicomponent transport in nafion-based direct methanol fuel cells.

PubMed

Rivera, Harry; Lawton, Jamie S; Budil, David E; Smotkin, Eugene S

2008-07-24

The CO2 in the cathode exhaust of a liquid feed direct methanol fuel cell (DMFC) has two sources: methanol diffuses through the membrane electrode assembly (MEA) to the cathode where it is catalytically oxidized to CO2; additionally, a portion of the CO2 produced at the anode diffuses through the MEA to the cathode. The potential-dependent CO2 exhaust from the cathode was monitored by online electrochemical mass spectrometry (ECMS) with air and with H2 at the cathode. The precise determination of the crossover rates of methanol and CO2, enabled by the subtractive normalization of the methanol/air to the methanol/H2 ECMS data, shows that methanol decreases the membrane viscosity and thus increases the diffusion coefficients of sorbed membrane components. The crossover of CO2 initially increases linearly with the Faradaic oxidation of methanol, reaches a temperature-dependent maximum, and then decreases. The membrane viscosity progressively increases as methanol is electrochemically depleted from the anode/electrolyte interface. The crossover maximum occurs when the current dependence of the diffusion coefficients and membrane CO2 solubility dominate over the Faradaic production of CO2. The plasticizing effect of methanol is corroborated by measurements of the rotational diffusion of TEMPONE (2,2,6,6-tetramethyl-4-piperidone N-oxide) spin probe by electron spin resonance spectroscopy. A linear inverse relationship between the methanol crossover rate and current density confirms the absence of methanol electro-osmotic drag at concentrations relevant to operating DMFCs. The purely diffusive transport of methanol is explained in terms of current proton solvation and methanol-water incomplete mixing theories.

Quantum Spin Liquids in Frustrated Spin-1 Diamond Antiferromagnets

NASA Astrophysics Data System (ADS)

Buessen, Finn Lasse; Hering, Max; Reuther, Johannes; Trebst, Simon

2018-01-01

Motivated by the recent synthesis of the spin-1 A -site spinel NiRh2 O4 , we investigate the classical to quantum crossover of a frustrated J1-J2 Heisenberg model on the diamond lattice upon varying the spin length S . Applying a recently developed pseudospin functional renormalization group approach for arbitrary spin-S magnets, we find that systems with S ≥3 /2 reside in the classical regime, where the low-temperature physics is dominated by the formation of coplanar spirals and a thermal (order-by-disorder) transition. For smaller local moments S =1 or S =1 /2 , we find that the system evades a thermal ordering transition and forms a quantum spiral spin liquid where the fluctuations are restricted to characteristic momentum-space surfaces. For the tetragonal phase of NiRh2 O4 , a modified J1-J2--J2⊥ exchange model is found to favor a conventionally ordered Néel state (for arbitrary spin S ), even in the presence of a strong local single-ion spin anisotropy, and it requires additional sources of frustration to explain the experimentally observed absence of a thermal ordering transition.

Strong competition between orbital ordering and itinerancy in a frustrated spinel vanadate

DOE PAGES

Ma, Jie; Lee, Jun Hee; Hahn, Steven E.; ...

2015-01-26

In this study, the crossover from localized to itinerant electron regimes in the geometrically frustrated spinel system Mn 1-xCo xV 2O 4 is explored by neutron-scattering measurements, first-principles calculations, and spin models. At low Co doping, the orbital ordering (OO) of the localized V 3+ spins suppresses magnetic frustration by triggering a tetragonal distortion. At high Co doping levels, however, electronic itinerancy melts the OO and lessens the structural and magnetic anisotropies, thus increasing the amount of geometric frustration for the V-site pyrochlore lattice. Contrary to the predicted paramagentism induced by chemical pressure, the measured noncollinear spin states in themore » Co-rich region of the phase diagram provide a unique platform where localized spins and electronic itinerancy compete in a geometrically frustrated spinel.« less

Crossover between collective and independent-particle excitations in quasi-2D electron gas with one filled subband

NASA Astrophysics Data System (ADS)

Nazarov, Vladimir U.

2018-05-01

While it has been recently demonstrated that, for quasi-two-dimensional electron gas (Q2DEG) with one filled subband, the dynamic exchange f x and Hartree f H kernels cancel each other in the low-density regime r s → ∞ (by half and completely, for the spin-neutral and fully spin-polarized cases, respectively), here we analytically show that the same happens at arbitrary densities at short distances. This motivates us to study the confinement dependence of the excitations in Q2DEG. Our calculations unambiguously confirm that, at strong confinements, the time-dependent exact exchange excitation energies approach the single-particle Kohn-Sham ones for the spin-polarized case, while the same, but less pronounced, tendency is observed for spin-neutral Q2DEG.

Synthesis of [Fe(Leq)(Lax)] n coordination polymer nanoparticles using blockcopolymer micelles.

PubMed

Göbel, Christoph; Klimm, Ottokar; Puchtler, Florian; Rosenfeldt, Sabine; Förster, Stephan; Weber, Birgit

2017-01-01

Spin-crossover compounds are a class of materials that can change their spin state from high spin (HS) to low spin (LS) by external stimuli such as light, pressure or temperature. Applications demand compounds with defined properties concerning the size and switchability that are maintained when the compound is integrated into composite materials. Here, we report the synthesis of [Fe(L eq )(L ax )] n coordination polymer (CP) nanoparticles using self-assembled polystyrene- block -poly(4-vinylpyridine) (PS- b -P4VP) block copolymer (BCP) micelles as template. Variation of the solvent (THF and toluene) and the rigidity of the axial ligand L ax (L ax = 1,2-di(pyridin-4-yl)ethane) (bpea), trans -1,2-di(pyridin-4-yl)ethene (bpee), and 1,2-di(pyridin-4-yl)ethyne) (bpey); L eq = 1,2-phenylenebis(iminomethylidyne)-bis(2,4-pentanedionato)(2-)) allowed the determination of the preconditions for the selective formation of nanoparticles. A low solubility of the CP in the used solvent and a high stability of the Fe-L bond with regard to ligand exchange are necessary for the formation of composite nanoparticles where the BCP micelle is filled with the CP, as in the case of the [FeL eq (bpey)] n @BCP. Otherwise, in the case of more flexible ligands or ligands that lead to high spin complexes, the formation of microcrystals next to the CP-BCP nanoparticles is observed above a certain concentration of [Fe(L eq )(L ax )] n . The core of the nanoparticles is about 45 nm in diameter due to the templating effect of the BCP micelle, independent of the used iron complex and [Fe(L eq )(L ax )] n concentration. The spin-crossover properties of the composite material are similar to those of the bulk for FeL eq (bpea)] n @BCP while pronounced differences are observed in the case of [FeL eq (bpey)] n @BCP nanoparticles.

Driving spin transition at interface: Role of adsorption configurations

NASA Astrophysics Data System (ADS)

Zhang, Yachao

2018-01-01

A clear insight into the electrical manipulation of molecular spins at interface is crucial to the design of molecule-based spintronic devices. Here we report on the electrically driven spin transition in manganocene physisorbed on a metallic surface in two different adsorption configurations predicted by ab initio techniques, including a Hubbard-U correction at the manganese site and accounting for the long-range van der Waals interactions. We show that the application of an electric field at the interface induces a high-spin to low-spin transition in the flat-lying manganocene, while it could hardly alter the high-spin ground state of the standing-up molecule. This phenomenon cannot be explained by either the molecule-metal charge transfer or the local electron correlation effects. We demonstrate a linear dependence of the intra-molecular spin-state splitting on the energy difference between crystal-field splitting and on-site Coulomb repulsion. After considering the molecule-surface binding energy shifts upon spin transition, we reproduce the obtained spin-state energetics. We find that the configuration-dependent responses of the spin-transition originate from the binding energy shifts instead of the variation of the local ligand field. Through these analyses, we obtain an intuitive understanding of the effects of molecule-surface contact on spin-crossover under electrical bias.

Ultrafast intersystem crossings in Fe-Co Prussian blue analogues

DOE Office of Scientific and Technical Information (OSTI.GOV)

van Veenendaal, Michel

Ultrafast spincrossover is studied in Fe-Co Prussian blue analogues using a dissipative quantum-mechanical model of a cobalt ion coupled to a breathing mode. All electronic interactions are treated on an equal footing. It is theoretically demonstrated that the divalent cobalt ion reaches 90% of the S = 3/2 value within 20 fs after photoexciting a low-spin Co 3+ ion by an iron-to-cobalt charge transfer. The doublet-to-quartet spin crossover is significantly faster than the oscillation period of the breathing mode. The system relaxes to the lowest manifold of divalent cobalt ( 4T 1) in 150-200 fs. In conclusion, strong oscillations inmore » spin-orbit coupling and the involvement of higher-lying quartets are found.« less

Ultrafast intersystem crossings in Fe-Co Prussian blue analogues

DOE PAGES

van Veenendaal, Michel

2017-07-27

Ultrafast spincrossover is studied in Fe-Co Prussian blue analogues using a dissipative quantum-mechanical model of a cobalt ion coupled to a breathing mode. All electronic interactions are treated on an equal footing. It is theoretically demonstrated that the divalent cobalt ion reaches 90% of the S = 3/2 value within 20 fs after photoexciting a low-spin Co 3+ ion by an iron-to-cobalt charge transfer. The doublet-to-quartet spin crossover is significantly faster than the oscillation period of the breathing mode. The system relaxes to the lowest manifold of divalent cobalt ( 4T 1) in 150-200 fs. In conclusion, strong oscillations inmore » spin-orbit coupling and the involvement of higher-lying quartets are found.« less

On the Crossover from Classical to Fermi Liquid Behavior in Dense Plasmas

NASA Astrophysics Data System (ADS)

Daligault, Jerome

2017-10-01

We explore the crossover from classical plasma to quantum Fermi liquid behavior of electrons in dense plasmas. To this end, we analyze the evolution with density and temperature of the momentum lifetime of a test electron introduced in a dense electron gas. This allows us 1) to determine the boundaries of the crossover region in the temperature-density plane and to shed light on the evolution of scattering properties across it, 2) to quantify the role of the fermionic nature of electrons on electronic collisions across the crossover region, and 3) to explain how the concept of Coulomb logarithm emerges at high enough temperature but disappears at low enough temperature. Work supported by LDRD Grant No. 20170490ER.

Spin-orbit torque in a thin film of the topological insulator Bi2Se3: Crossover from the ballistic to diffusive regime

NASA Astrophysics Data System (ADS)

Ren, Y. J.; Deng, W. Y.; Geng, H.; Shen, R.; Shao, L. B.; Sheng, L.; Xing, D. Y.

2017-12-01

The spin-orbit torque provides an efficient method for switching the direction of a magnetization by using an electric field. Owing to the spin-orbit coupling, when an electric field is applied, a nonequilibrium spin density is generated, which exerts a torque on the local magnetization. Here, we investigate the spin-orbit torque in a thin film of topological insulator \\text{Bi}2\\text{Se}3 based upon a Boltzmann equation, with proper boundary conditions, which is applicable from the ballistic regime to the diffusive regime. It is shown that due to the spin-momentum interlocking of the electron surface states, the magnitude of the field-like torque is simply in linear proportion to the longitudinal electrical current. For a fixed electric field, the spin-orbit torque is proportional to the sample length in the ballistic limit, and saturates to a constant in the diffusive limit. The dependence of the torque on the magnetization direction and exchange coupling strength is also studied. Our theory may offer useful guidance for experimental investigations of the spin-orbit torque in finite-size systems.

Metastability on the hierarchical lattice

NASA Astrophysics Data System (ADS)

den Hollander, Frank; Jovanovski, Oliver

2017-07-01

We study metastability for Glauber spin-flip dynamics on the N-dimensional hierarchical lattice with n hierarchical levels. Each vertex carries an Ising spin that can take the values -1 or +1 . Spins interact with an external magnetic field h>0 . Pairs of spins interact with each other according to a ferromagnetic pair potential J=\\{J_i\\}i=1n , where J_i>0 is the strength of the interaction between spins at hierarchical distance i. Spins flip according to a Metropolis dynamics at inverse temperature β. In the limit as β\\to∞ , we analyse the crossover time from the metastable state \\boxminus (all spins -1 ) to the stable state \\boxplus (all spins +1 ). Under the assumption that J is non-increasing, we identify the mean transition time up to a multiplicative factor 1+o_β(1) . On the scale of its mean, the transition time is exponentially distributed. We also identify the set of configurations representing the gate for the transition. For the special case where Ji = \\tilde{J}/Ni , 1 ≤slant i ≤slant n , with \\tilde{J}>0 the relevant formulas simplify considerably. Also the hierarchical mean-field limit N\\to∞ can be analysed in detail.

Spin-orbit tuned metal-insulator transitions in single-crystal Sr₂Ir 1–xRh xO₄ (0≤x≤1)

DOE PAGES

Qi, T. F.; Korneta, O. B.; Li, L.; ...

2012-09-06

Sr₂IrO₄ is a magnetic insulator driven by spin-orbit interaction (SOI) whereas the isoelectronic and isostructural Sr₂RhO₄ is a paramagnetic metal. The contrasting ground states have been shown to result from the critical role of the strong SOI in the iridate. Our investigation of structural, transport, magnetic, and thermal properties reveals that substituting 4d Rh⁴⁺ (4d⁵) ions for 5d Ir⁴⁺ (5d⁵) ions in Sr₂IrO₄ directly reduces the SOI and rebalances the competing energies so profoundly that it generates a rich phase diagram for Sr₂Ir 1–xRh xO₄ featuring two major effects: (1) Light Rh doping (0 ≤ x ≤ 0.16) prompts amore » simultaneous and precipitous drop in both the electrical resistivity and the magnetic ordering temperature TC, which is suppressed to zero at x = 0.16 from 240 K at x = 0. (2) However, with heavier Rh doping [0.24 < x < 0.85 (±0.05)] disorder scattering leads to localized states and a return to an insulating state with spin frustration and exotic magnetic behavior that only disappears near x = 1. The intricacy of Sr₂Ir 1–xRh xO₄ is further highlighted by comparison with Sr₂Ir 1–xRu xO₄ where Ru⁴⁺ (4d⁴) drives a direct crossover from the insulating to metallic states.« less

Exploring the anisotropic Kondo model in and out of equilibrium with alkaline-earth atoms

NASA Astrophysics Data System (ADS)

Kanász-Nagy, Márton; Ashida, Yuto; Shi, Tao; Moca, Cǎtǎlin Paşcu; Ikeda, Tatsuhiko N.; Fölling, Simon; Cirac, J. Ignacio; Zaránd, Gergely; Demler, Eugene A.

2018-04-01

We propose a scheme to realize the Kondo model with tunable anisotropy using alkaline-earth atoms in an optical lattice. The new feature of our setup is Floquet engineering of interactions using time-dependent Zeeman shifts, that can be realized either using state-dependent optical Stark shifts or magnetic fields. The properties of the resulting Kondo model strongly depend on the anisotropy of the ferromagnetic interactions. In particular, easy-plane couplings give rise to Kondo singlet formation even though microscopic interactions are all ferromagnetic. We discuss both equilibrium and dynamical properties of the system that can be measured with ultracold atoms, including the impurity spin susceptibility, the impurity spin relaxation rate, as well as the equilibrium and dynamical spin correlations between the impurity and the ferromagnetic bath atoms. We analyze the nonequilibrium time evolution of the system using a variational non-Gaussian approach, which allows us to explore coherent dynamics over both short and long timescales, as set by the bandwidth and the Kondo singlet formation, respectively. In the quench-type experiments, when the Kondo interaction is suddenly switched on, we find that real-time dynamics shows crossovers reminiscent of poor man's renormalization group flow used to describe equilibrium systems. For bare easy-plane ferromagnetic couplings, this allows us to follow the formation of the Kondo screening cloud as the dynamics crosses over from ferromagnetic to antiferromagnetic behavior. On the other side of the phase diagram, our scheme makes it possible to measure quantum corrections to the well-known Korringa law describing the temperature dependence of the impurity spin relaxation rate. Theoretical results discussed in our paper can be measured using currently available experimental techniques.

Strain-sensitive spin-state ordering in thin films of perovskite LaCoO3

NASA Astrophysics Data System (ADS)

Fujioka, J.; Yamasaki, Y.; Doi, A.; Nakao, H.; Kumai, R.; Murakami, Y.; Nakamura, M.; Kawasaki, M.; Arima, T.; Tokura, Y.

2015-11-01

We have investigated the lattice distortion coupled to the Co 3 d -spin-state ordering in thin films of perovskite LaCoO3 with various epitaxial strains by measurements of the magnetization, x-ray diffraction, and optical spectra. In the system with tensile strain about 0.5%, a lattice distortion characterized by the modulation vector q =(1 /6 ,1 /6 ,1 /6 ) emerges at 40 K, followed by a ferromagnetic ordering at 24 K. Alternatively, in systems with tensile strain exceeding 1%, the lattice distortion characterized by q =(1 /4 ,1 /4 ,1 /4 ) emerges at 120 K or higher, and subsequently the ferromagnetic or ferrimagnetic ordering occurs around 90 K. The evolution of infrared phonon spectra and resonant x-ray scattering at the Co K edge suggests that the population change in the Co 3 d spin state causes the strain-induced switching of spin-state ordering as well as of magnetic ordering in this canonical spin-state crossover system.

Coordination preference and magnetic properties of FeII assemblies with a bis-azole bearing 1,2,4-triazole and tetrazole

NASA Astrophysics Data System (ADS)

Naik, Anil D.; Railliet, Antoine P.; Dîrtu, Marinela M.; Garcia, Yann

2012-03-01

With a new bis-azole molecular fragment ( Htt) bearing 1,2,4-triazole and tetrazole, a mononuclear complex [Fe(tt)2(H2O)4]·2H2O ( 1), a trinuclear complex [Fe3(tt)6(H2O)6]·2H2O ( 2) and a 1D coordination polymer [Fe(tt)(Htt)2]BF4·2CH3OH ( 3) were obtained by varying reaction conditions. Htt acts either as an anionic or neutral ligand depending upon the reaction medium and pH. Thermal variation of spin states of 1- 3 were investigated in the range 77-300 K by 57Fe Mössbauer spectroscopy. 1 totally remains in high-spin state over the entire temperature range whereas no spin crossover was evidenced in 2. Nearly 1:1 high-spin and low-spin population ratio is found in 3, which remains constant over the entire temperature range investigated.

Spectrum of the Nuclear Environment for GaAs Spin Qubits.

PubMed

Malinowski, Filip K; Martins, Frederico; Cywiński, Łukasz; Rudner, Mark S; Nissen, Peter D; Fallahi, Saeed; Gardner, Geoffrey C; Manfra, Michael J; Marcus, Charles M; Kuemmeth, Ferdinand

2017-04-28

Using a singlet-triplet spin qubit as a sensitive spectrometer of the GaAs nuclear spin bath, we demonstrate that the spectrum of Overhauser noise agrees with a classical spin diffusion model over 6 orders of magnitude in frequency, from 1 mHz to 1 kHz, is flat below 10 mHz, and falls as 1/f^{2} for frequency f≳1  Hz. Increasing the applied magnetic field from 0.1 to 0.75 T suppresses electron-mediated spin diffusion, which decreases the spectral content in the 1/f^{2} region and lowers the saturation frequency, each by an order of magnitude, consistent with a numerical model. Spectral content at megahertz frequencies is accessed using dynamical decoupling, which shows a crossover from the few-pulse regime (≲16π pulses), where transverse Overhauser fluctuations dominate dephasing, to the many-pulse regime (≳32 π pulses), where longitudinal Overhauser fluctuations with a 1/f spectrum dominate.

Isolation of EPR spectra and estimation of spin-states in two-component mixtures of paramagnets.

PubMed

Chabbra, Sonia; Smith, David M; Bode, Bela E

2018-04-26

The presence of multiple paramagnetic species can lead to overlapping electron paramagnetic resonance (EPR) signals. This complication can be a critical obstacle for the use of EPR to unravel mechanisms and aid the understanding of earth abundant metal catalysis. Furthermore, redox or spin-crossover processes can result in the simultaneous presence of metal centres in different oxidation or spin states. In this contribution, pulse EPR experiments on model systems containing discrete mixtures of Cr(i) and Cr(iii) or Cu(ii) and Mn(ii) complexes demonstrate the feasibility of the separation of the EPR spectra of these species by inversion recovery filters and the identification of the relevant spin states by transient nutation experiments. We demonstrate the isolation of component spectra and identification of spin states in a mixture of catalyst precursors. The usefulness of the approach is emphasised by monitoring the fate of the chromium species upon activation of an industrially used precatalyst system.

A Simple Demonstration of the Curie-Weiss Law and a Spin-Crossover Compound.

ERIC Educational Resources Information Center

Hutchinson, Bennett; And Others

1980-01-01

Discusses an addition to an apparatus which allows the effect of temperature on a paramagnetic compound to be measured, therefore demonstrating the Curie-Weiss law. The experiment can be used as a demonstration or student experiment to stimulate discussion of magnetic susceptibility and ligand field trips. (Author/JN)

Dimensional crossover and cold-atom realization of topological Mott insulators

PubMed Central

Scheurer, Mathias S.; Rachel, Stephan; Orth, Peter P.

2015-01-01

Interacting cold-atomic gases in optical lattices offer an experimental approach to outstanding problems of many body physics. One important example is the interplay of interaction and topology which promises to generate a variety of exotic phases such as the fractionalized Chern insulator or the topological Mott insulator. Both theoretically understanding these states of matter and finding suitable systems that host them have proven to be challenging problems. Here we propose a cold-atom setup where Hubbard on-site interactions give rise to spin liquid-like phases: weak and strong topological Mott insulators. They represent the celebrated paradigm of an interacting and topological quantum state with fractionalized spinon excitations that inherit the topology of the non-interacting system. Our proposal shall help to pave the way for a controlled experimental investigation of this exotic state of matter in optical lattices. Furthermore, it allows for the investigation of a dimensional crossover from a two-dimensional quantum spin Hall insulating phase to a three-dimensional strong topological insulator by tuning the hopping between the layers. PMID:25669431

Ultrafast Spin Crossover in [FeII (bpy)3 ]2+ : Revealing Two Competing Mechanisms by Extreme Ultraviolet Photoemission Spectroscopy.

PubMed

Moguilevski, Alexandre; Wilke, Martin; Grell, Gilbert; Bokarev, Sergey I; Aziz, Saadullah G; Engel, Nicholas; Raheem, Azhr A; Kühn, Oliver; Kiyan, Igor Yu; Aziz, Emad F

2017-03-03

Photoinduced spin-flip in Fe II complexes is an ultrafast phenomenon that has the potential to become an alternative to conventional processing and magnetic storage of information. Following the initial excitation by visible light into the singlet metal-to-ligand charge-transfer state, the electronic transition to the high-spin quintet state may undergo different pathways. Here we apply ultrafast XUV (extreme ultraviolet) photoemission spectroscopy to track the low-to-high spin dynamics in the aqueous iron tris-bipyridine complex, [Fe(bpy) 3 ] 2+ , by monitoring the transient electron density distribution among excited states with femtosecond time resolution. Aided by first-principles calculations, this approach enables us to reveal unambiguously both the sequential and direct de-excitation pathways from singlet to quintet state, with a branching ratio of 4.5:1. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Spin State Control of the Perovskite Rh/Co Oxides

PubMed Central

Terasaki, Ichiro; Shibasaki, Soichiro; Yoshida, Shin; Kobayashi, Wataru

2010-01-01

We show why and how the spin state of transition-metal ions affects the thermoelectric properties of transition-metal oxides by investigating two perovskite-related oxides. In the A-site ordered cobalt oxide Sr3YCo4O10.5, partial substitution of Ca for Sr acts as chemical pressure, which compresses the unit cell volume to drive the spin state crossover, and concomitantly changes the magnetization and thermopower. In the perovskite rhodium oxide LaRhO3, partial substitution of Sr for La acts as hole-doping, and the resistivity and thermopower decrease systematically with the Sr concentration. The thermopower remains large values at high temperatures (>150 μV/K at 800 K), which makes a remarkable contrast to La1−xSrxCoO3. We associate this with the stability of the low spin state of the Rh3+ ions.

Spin-Driven Emergent Antiferromagnetism and Metal-Insulator Transition in Nanoscale p-Si

NASA Astrophysics Data System (ADS)

Lou, Paul C.; Kumar, Sandeep

2018-04-01

The entanglement of the charge, spin and orbital degrees of freedom can give rise to emergent behavior especially in thin films, surfaces and interfaces. Often, materials that exhibit those properties require large spin orbit coupling. We hypothesize that the emergent behavior can also occur due to spin, electron and phonon interactions in widely studied simple materials such as Si. That is, large intrinsic spin-orbit coupling is not an essential requirement for emergent behavior. The central hypothesis is that when one of the specimen dimensions is of the same order (or smaller) as the spin diffusion length, then non-equilibrium spin accumulation due to spin injection or spin-Hall effect (SHE) will lead to emergent phase transformations in the non-ferromagnetic semiconductors. In this experimental work, we report spin mediated emergent antiferromagnetism and metal insulator transition in a Pd (1 nm)/Ni81Fe19 (25 nm)/MgO (1 nm)/p-Si (~400 nm) thin film specimen. The spin-Hall effect in p-Si, observed through Rashba spin-orbit coupling mediated spin-Hall magnetoresistance behavior, is proposed to cause the spin accumulation and resulting emergent behavior. The phase transition is discovered from the diverging behavior in longitudinal third harmonic voltage, which is related to the thermal conductivity and heat capacity.

Low Dimensionality Effects in Complex Magnetic Oxides

NASA Astrophysics Data System (ADS)

Kelley, Paula J. Lampen

Complex magnetic oxides represent a unique intersection of immense technological importance and fascinating physical phenomena originating from interwoven structural, electronic and magnetic degrees of freedom. The resulting energetically close competing orders can be controllably selected through external fields. Competing interactions and disorder represent an additional opportunity to systematically manipulate the properties of pure magnetic systems, leading to frustration, glassiness, and other novel phenomena while finite sample dimension plays a similar role in systems with long-range cooperative effects or large correlation lengths. A rigorous understanding of these effects in strongly correlated oxides is key to manipulating their functionality and device performance, but remains a challenging task. In this dissertation, we examine a number of problems related to intrinsic and extrinsic low dimensionality, disorder, and competing interactions in magnetic oxides by applying a unique combination of standard magnetometry techniques and unconventional magnetocaloric effect and transverse susceptibility measurements. The influence of dimensionality and disorder on the nature and critical properties of phase transitions in manganites is illustrated in La0.7 Ca0.3MnO3, in which both size reduction to the nanoscale and chemically-controlled quenched disorder are observed to induce a progressive weakening of the first-order nature of the transition, despite acting through the distinct mechanisms of surface effects and site dilution. In the second-order material La0.8Ca0.2MnO3, a strong magnetic field is found to drive the system toward its tricritical point as competition between exchange interactions in the inhomogeneous ground state is suppressed. In the presence of large phase separation stabilized by chemical disorder and long-range strain, dimensionality has a profound effect. With the systematic reduction of particle size in microscale-phase-separated (La, Pr, Ca)MnO3 we observe a disruption of the long-range glassy strains associated with the charge-ordered phase in the bulk, lowering the field and pressure threshold for charge-order melting and increasing the ferromagnetic volume fraction as particle size is decreased. The long-range charge-ordered phase becomes completely suppressed when the particle size falls below 100 nm. In contrast, low dimensionality in the geometrically frustrated pseudo-1D spin chain compound Ca3Co2O6 is intrinsic, arising from the crystal lattice. We establish a comprehensive phase diagram for this exotic system consistent with recent reports of an incommensurate ground state and identify new sub-features of the ferrimagnetic phase. When defects in the form of grain boundaries are incorporated into the system the low-temperature slow-dynamic state is weakened, and new crossover phenomena emerge in the spin relaxation behavior along with an increased distribution of relaxation times. The presence of both disorder and randomness leads to a spin-glass-like state, as observed in gammaFe2O3 hollow nanoparticles, where freezing of surface spins at low temperature generates an irreversible magnetization component and an associated exchange-biasing effect. Our results point to distinct dynamic behaviors on the inner and outer surfaces of the hollow structures. Overall, these studies yield new physical insights into the role of dimensionality and disorder in these complex oxide systems and highlight the sensitivity of their manifested magnetic ground states to extrinsic factors, leading in many cases to crossover behaviors where the balance between competing phases is altered, or to the emergence of entirely new magnetic phenomena.

Vindication of Yb2Ti2O7 as a model exchange quantum spin ice.

PubMed

Applegate, R; Hayre, N R; Singh, R R P; Lin, T; Day, A G R; Gingras, M J P

2012-08-31

We use numerical linked-cluster expansions to compute the specific heat C(T) and entropy S(T) of a quantum spin ice Hamiltonian for Yb2Ti2O7 using anisotropic exchange interactions, recently determined from inelastic neutron scattering measurements, and find good agreement with experimental calorimetric data. This vindicates Yb2Ti2O7 as a model quantum spin ice. We find that in the perturbative weak quantum regime, such a system has a ferrimagnetic ordered ground state, with two peaks in C(T): a Schottky anomaly signaling the paramagnetic to spin ice crossover, followed at a lower temperature by a sharp peak accompanying a first-order phase transition to the ordered state. We suggest that the two C(T) features observed in Yb2Ti2O7 are associated with the same physics. Spin excitations in this regime consist of weakly confined spinon-antispinon pairs. We anticipate that the conventional ground state with exotic quantum dynamics will prove a prevalent characteristic of many real quantum spin ice materials.

Fruit fly scale robots can hover longer with flapping wings than with spinning wings.

PubMed

Hawkes, Elliot W; Lentink, David

2016-10-01

Hovering flies generate exceptionally high lift, because their wings generate a stable leading edge vortex. Micro flying robots with a similar wing design can generate similar high lift by either flapping or spinning their wings. While it requires less power to spin a wing, the overall efficiency depends also on the actuator system driving the wing. Here, we present the first holistic analysis to calculate how long a fly-inspired micro robot can hover with flapping versus spinning wings across scales. We integrate aerodynamic data with data-driven scaling laws for actuator, electronics and mechanism performance from fruit fly to hummingbird scales. Our analysis finds that spinning wings driven by rotary actuators are superior for robots with wingspans similar to hummingbirds, yet flapping wings driven by oscillatory actuators are superior at fruit fly scale. This crossover is driven by the reduction in performance of rotary compared with oscillatory actuators at smaller scale. Our calculations emphasize that a systems-level analysis is essential for trading-off flapping versus spinning wings for micro flying robots. © 2016 The Author(s).

Fruit fly scale robots can hover longer with flapping wings than with spinning wings

PubMed Central

Lentink, David

2016-01-01

Hovering flies generate exceptionally high lift, because their wings generate a stable leading edge vortex. Micro flying robots with a similar wing design can generate similar high lift by either flapping or spinning their wings. While it requires less power to spin a wing, the overall efficiency depends also on the actuator system driving the wing. Here, we present the first holistic analysis to calculate how long a fly-inspired micro robot can hover with flapping versus spinning wings across scales. We integrate aerodynamic data with data-driven scaling laws for actuator, electronics and mechanism performance from fruit fly to hummingbird scales. Our analysis finds that spinning wings driven by rotary actuators are superior for robots with wingspans similar to hummingbirds, yet flapping wings driven by oscillatory actuators are superior at fruit fly scale. This crossover is driven by the reduction in performance of rotary compared with oscillatory actuators at smaller scale. Our calculations emphasize that a systems-level analysis is essential for trading-off flapping versus spinning wings for micro flying robots. PMID:27707903

Dynamical Jahn-Teller effect of fullerene anions

NASA Astrophysics Data System (ADS)

Liu, Dan; Iwahara, Naoya; Chibotaru, Liviu F.

2018-03-01

The dynamical Jahn-Teller effect of C60n - anions (n =1 -5) is studied using the numerical diagonalization of the linear pn⊗8 d Jahn-Teller Hamiltonian with the currently established coupling parameters. It is found that in all anions the Jahn-Teller effect stabilizes the low-spin states, resulting in the violation of Hund's rule. The energy gain due to the Jahn-Teller dynamics is found to be comparable to the static Jahn-Teller stabilization. The Jahn-Teller dynamics influences the thermodynamic properties via strong variation of the density of vibronic states with energy. Thus the large vibronic entropy in the low-spin states enhances the effective spin gap of C603 - quenching the spin crossover. From the calculations of the effective spin gap as a function of the Hund's rule coupling, we found that the latter should amount 40 ±5 meV in order to cope with the violation of Hund's rule and to reproduce the large spin gap. With the obtained numerical solutions, the matrix elements of electronic operators for the low-lying vibronic levels and the vibronic reduction factors are calculated for all anions.

Symmetry-enriched Bose-Einstein condensates in a spin-orbit-coupled bilayer system

NASA Astrophysics Data System (ADS)

Cheng, Jia-Ming; Zhou, Xiang-Fa; Zhou, Zheng-Wei; Guo, Guang-Can; Gong, Ming

2018-01-01

We consider the fate of Bose-Einstein condensation with time-reversal symmetry and inversion symmetry in a spin-orbit-coupled bilayer system. When these two symmetry operators commute, all the single-particle bands are exactly twofold degenerate in the momentum space. The scattering in the twofold-degenerate rings can relax the spin-momentum locking effect from spin-orbit-coupling interaction and thus can realize the spin-polarized plane-wave phase even when the interparticle interaction dominates. When these two operators anticommute, the lowest two bands may have the same minimal energy, but with totally different spin structures. As a result, the competition between different condensates in these two energetically degenerate rings can give rise to different stripe phases with atoms condensed at two or four collinear momenta. We find that the crossover between these two cases is accompanied by the excited band condensation when the interference energy can overcome the increased single-particle energy in the excited band. This effect is not based on strong interaction and thus can be realized even with moderate interaction strength.

Crossover from the Luttinger-liquid to Coulomb-blockade regime in carbon nanotubes.

PubMed

Bellucci, S; González, J; Onorato, P

2005-10-28

We develop a theoretical approach to the low-energy properties of one-dimensional electron systems aimed to encompass the mixed features of Luttinger-liquid and Coulomb-blockade behavior observed in the crossover between the two regimes. For this aim, we extend the Luttinger-liquid description by incorporating the effects of a discrete single-particle spectrum. The intermediate regime is characterized by a power-law behavior of the conductance, but with an exponent oscillating with the gate voltage, in agreement with recent experimental observations. Our construction also accounts naturally for the existence of a crossover in the zero-bias conductance, mediating between two temperature ranges where the power-law behavior is preserved but with a different exponent.

Native Silk Feedstock as a Model Biopolymer: A Rheological Perspective.

PubMed

Laity, Peter R; Holland, Chris

2016-08-08

Variability in silk's rheology is often regarded as an impediment to understanding or successfully copying the natural spinning process. We have previously reported such variability in unspun native silk extracted straight from the gland of the domesticated silkworm Bombyx mori and discounted classical explanations such as differences in molecular weight and concentration. We now report that variability in oscillatory measurements can be reduced onto a simple master-curve through normalizing with respect to the crossover. This remarkable result suggests that differences between silk feedstocks are rheologically simple and not as complex as originally thought. By comparison, solutions of poly(ethylene-oxide) and hydroxypropyl-methyl-cellulose showed similar normalization behavior; however, the resulting curves were broader than for silk, suggesting greater polydispersity in the (semi)synthetic materials. Thus, we conclude Nature may in fact produce polymer feedstocks that are more consistent than typical man-made counterparts as a model for future rheological investigations.

EPR investigations of silicon carbide nanoparticles functionalized by acid doped polyaniline

NASA Astrophysics Data System (ADS)

Karray, Fekri; Kassiba, Abdelhadi

2012-06-01

Nanocomposites (SiC-PANI) based on silicon carbide nanoparticles (SiC) encapsulated in conducting polyaniline (PANI) are synthesized by direct polymerization of PANI on the nanoparticle surfaces. The conductivity of PANI and the nanocomposites was modulated by several doping levels of camphor sulfonic acid (CSA). Electron paramagnetic resonance (EPR) investigations were carried out on representative SiC-PANI samples over the temperature range [100-300 K]. The features of the EPR spectra were analyzed taking into account the paramagnetic species such as polarons with spin S=1/2 involved in two main environments realized in the composites as well as their thermal activation. A critical temperature range 200-225 K was revealed through crossover changes in the thermal behavior of the EPR spectral parameters. Insights on the electronic transport properties and their thermal evolutions were inferred from polarons species probed by EPR and the electrical conductivity in doped nanocomposites.

Quantum many-body theory for electron spin decoherence in nanoscale nuclear spin baths.

PubMed

Yang, Wen; Ma, Wen-Long; Liu, Ren-Bao

2017-01-01

Decoherence of electron spins in nanoscale systems is important to quantum technologies such as quantum information processing and magnetometry. It is also an ideal model problem for studying the crossover between quantum and classical phenomena. At low temperatures or in light-element materials where the spin-orbit coupling is weak, the phonon scattering in nanostructures is less important and the fluctuations of nuclear spins become the dominant decoherence mechanism for electron spins. Since the 1950s, semi-classical noise theories have been developed for understanding electron spin decoherence. In spin-based solid-state quantum technologies, the relevant systems are in the nanometer scale and nuclear spin baths are quantum objects which require a quantum description. Recently, quantum pictures have been established to understand the decoherence and quantum many-body theories have been developed to quantitatively describe this phenomenon. Anomalous quantum effects have been predicted and some have been experimentally confirmed. A systematically truncated cluster-correlation expansion theory has been developed to account for the many-body correlations in nanoscale nuclear spin baths that are built up during electron spin decoherence. The theory has successfully predicted and explained a number of experimental results in a wide range of physical systems. In this review, we will cover this recent progress. The limitations of the present quantum many-body theories and possible directions for future development will also be discussed.

Dimensional crossover in fragmentation

NASA Astrophysics Data System (ADS)

Sotolongo-Costa, Oscar; Rodriguez, Arezky H.; Rodgers, G. J.

2000-11-01

Experiments in which thick clay plates and glass rods are fractured have revealed different behavior of fragment mass distribution function in the small and large fragment regions. In this paper we explain this behavior using non-extensive Tsallis statistics and show how the crossover between the two regions is caused by the change in the fragments’ dimensionality during the fracture process. We obtain a physical criterion for the position of this crossover and an expression for the change in the power-law exponent between the small and large fragment regions. These predictions are in good agreement with the experiments on thick clay plates.

Relevance of supramolecular interactions, texture and lattice occupancy in the designer iron(II) spin crossover complexes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Naik, Anil D.; Tinant, Bernard; Muffler, Kai

New Fe{sup II} complexes of formula [Fe(3-Br-phen){sub 2}(NCS){sub 2}].Solvent (Solvent=0.5 CH{sub 3}OH (1), 2 CH{sub 2}Cl{sub 2} (2), desolvation of 2 (3), 0.5 CH{sub 3}COCH{sub 3} (4) and 0 (5)) have been synthesized. {sup 57}Fe Moessbauer and magnetic investigation reveal unique features atypical of classic [Fe(phen){sub 2}(NCS){sub 2}] polymorphs. Complex 1, prepared by precipitation in MeOH, undergoes upon cooling below room temperature an incomplete and gradual thermally induced spin conversion, while 4 prepared by an extraction method remains mostly in the low-spin state. The non solvated compounds 3 and 5, display a more abrupt spin crossover on cooling around T{submore » 1/2}=175 K and T{sub 1/2}=198 K, respectively. Defects/soft lattice inclusion due to different methods of material synthesis, extent of aging, reaction medium and associated solvent molecules have enormous influence on the particle size and magnetic properties of these complexes. Scanning electron micrographs helps to establish a logical relationship among methods employed for synthesis, texture of materials and their effect on magnetic properties. The crystal structure of 2 determined in the monoclinic space group P2/c (100 K) reveals a mononuclear complex consisting of a distorted FeN{sub 6} octahedron in the low-spin state, constructed from two 3-bromo-1, 10-phenanthroline and two isothiocyanato anions in cis position. Intermolecular interactions between mononuclear units of the S...Br, S...C(H) and pi-pi type afford a 2D supramolecular network. DFT calculations for the single molecule 2 reveals an energy difference between high-spin and low-spin isomers of 7 kJ/mol suggesting a slight destabilization of the low-spin state compared to [Fe(phen){sub 2}(NCS){sub 2}]. Normal co-ordinate analysis was also carried out for 3 and compared with experimental temperature dependent Raman spectra for 5. - Graphical abstract: New Fe{sup II} complexes of formula [Fe(3-Br-phen){sub 2}(NCS){sub 2}].Solvent have been synthesized by precipitation (1) and extraction (4) methods. {sup 57}Fe Moessbauer and magnetic investigation reveal unique features atypical of classic [Fe(phen){sub 2}(NCS){sub 2}] polymorphs. Complex 1, undergoes upon cooling below room temperature an incomplete and gradual thermally induced spin conversion, while 4 remains mostly in the low-spin state. Role of supramolecular interactions, particles size, lattice solvents have profound influence on magnetic properties.« less

Progress in Developing a New Field-theoretical Crossover Equation-of-State

NASA Technical Reports Server (NTRS)

Rudnick, Joseph; Barmatz, M.; Zhong, Fang

2003-01-01

A new field-theoretical crossover equation-of-state model is being developed. This model of a liquid-gas critical point provides a bridge between the asymptotic equation-of-state behavior close to the transition, obtained by the Guida and Zinn-Justin parametric model [J. Phys. A: Math. Gen. 31, 8103 (1998)], and the expected mean field behavior farther away. The crossover is based on the beta function for the renormalized fourth-order coupling constant and incorporates the correct crossover exponents and critical amplitude ratios in both regimes. A crossover model is now being developed that is consistent with predictions along the critical isochore and along the coexistence curve of the minimal subtraction renormalization approach developed by Dohm and co-workers and recently applied to the O(1) universality class [Phys. Rev. E, 67, 021106 (2003)]. Experimental measurements of the heat capacity at constant volume, isothermal susceptibility, and coexistence curve near the He-3 critical point are being compared to the predictions of this model. The results of these comparisons will be presented.

Realization of two-dimensional spin-orbit coupling for Bose-Einstein condensates.

PubMed

Wu, Zhan; Zhang, Long; Sun, Wei; Xu, Xiao-Tian; Wang, Bao-Zong; Ji, Si-Cong; Deng, Youjin; Chen, Shuai; Liu, Xiong-Jun; Pan, Jian-Wei

2016-10-07

Cold atoms with laser-induced spin-orbit (SO) interactions provide a platform to explore quantum physics beyond natural conditions of solids. Here we propose and experimentally realize two-dimensional (2D) SO coupling and topological bands for a rubidium-87 degenerate gas through an optical Raman lattice, without phase-locking or fine-tuning of optical potentials. A controllable crossover between 2D and 1D SO couplings is studied, and the SO effects and nontrivial band topology are observed by measuring the atomic cloud distribution and spin texture in momentum space. Our realization of 2D SO coupling with advantages of small heating and topological stability opens a broad avenue in cold atoms to study exotic quantum phases, including topological superfluids. Copyright © 2016, American Association for the Advancement of Science.

Electron transport through a spin crossover junction. Perspectives from a wavefunction-based approach

NASA Astrophysics Data System (ADS)

Vela, Sergi; Verot, Martin; Fromager, Emmanuel; Robert, Vincent

2017-02-01

The present paper reports the application of a computational framework, based on the quantum master equation, the Fermi's golden Rule, and conventional wavefunction-based methods, to describe electron transport through a spin crossover molecular junction (Fe(bapbpy) (NCS)2, 1, bapbpy = N-(6-(6-(Pyridin-2-ylamino)pyridin-2-yl)pyridin-2-yl)-pyridin-2-amine). This scheme is an alternative to the standard approaches based on the relative position and nature of the frontier orbitals, as it evaluates the junction's Green's function by means of accurate state energies and wavefunctions. In the present work, those elements are calculated for the relevant states of the high- and low-spin species of 1, and they are used to evaluate the output conductance within a given range of bias- and gate-voltages. The contribution of the ground and low-lying excited states to the current is analyzed, and inspected in terms of their 2S + 1 Ms-states. In doing so, it is shown the relevance of treating not only the ground state in its maximum-Ms projection, as usually done in most computational-chemistry packages, but the whole spectrum of low-energy states of the molecule. Such improved representation of the junction has a notable impact on the total conductivity and, more importantly, it restores the equivalence between alpha and beta transport, which means that no spin polarization is observed in the absence of Zeeman splitting. Finally, this work inspects the strong- and weak-points of the suggested theoretical framework to understand electron transport through molecular switchable materials, identifies a pathway for future improvement, and offers a new insight into concepts that play a key role in spintronics.

Probing the Impact of Solvation on Photoexcited Spin Crossover Complexes with High-Precision X-ray Transient Absorption Spectroscopy

DOE PAGES

Liu, Cunming; Zhang, Jianxin; Lawson Daku, Latevi M.; ...

2017-11-10

Investigating the photoinduced electronic and structural response of bistable molecular building blocks incorporating transition metals in solution phase constitutes a necessary stepping stone for steering their properties towards applications and perfomance optimizations. Here, this paper presents a detailed X-ray transient absorption (XTA) spectroscopy study of a prototypical spin crossover (SCO) complex [Fe II(mbpy) 3] 2+ (where mbpy=4,4’-dimethyl-2,2’-bipyridine) with a [Fe IIN 6] first coordination shell in water (H 2O) and acetonitrile (CH 3CN). The unprecedented data quality of the XTA spectra together with the direct fitting of the difference spectra in k space using a large number of scattering pathsmore » enables resolving the subtle difference in the photoexcited structures of an Fe II complex in two solvents for the first time. Also, compared to the low spin (LS) 1A 1 state, the average Fe-N bond elongations for the photoinduced high spin (HS) 5T 2 state are found to be 0.181 ± 0.003 Å in H 2O and 0.199 ± 0.003 Å in CH 3CN. This difference in structural response is attributed to ligand-solvent interactions that are stronger in H 2O than in CH 3CN for the HS excited state. Our studies demonstrate that, although the metal center of [Fe II(mbpy) 3] 2+ could have been expected to be rather shielded by the three bidentate ligands with quasi-octahedral-coordination, the ligand field strength in the HS excited state is nevertheless indirectly affected by solvation that modifies the charge distribution within the Fe-N covalent bonds. More generally, this work highlights the importance of including solvation effects in order to develop a generalized understanding of the spin-state switching at the atomic level.« less

Mott transition between a spin-liquid insulator and a metal in three dimensions.

PubMed

Podolsky, Daniel; Paramekanti, Arun; Kim, Yong Baek; Senthil, T

2009-05-08

We study a bandwidth controlled Mott metal-insulator transition (MIT) from a Fermi-liquid metal to a quantum spin-liquid insulator in three dimensions. Using a slave rotor approach including gauge fluctuations, we obtain a continuous MIT and discuss finite temperature crossovers in its vicinity. We show that the specific heat C approximately Tlnln(1/T) at the MIT and that the metallic state near the MIT should exhibit a "conductivity minimum" as a function of temperature. We suggest Na4Ir3O8 as a candidate to test our predictions and compute its electron spectral function at the MIT.

Metal-to-insulator crossover in alkali doped zeolite

PubMed Central

Igarashi, Mutsuo; Jeglič, Peter; Krajnc, Andraž; Žitko, Rok; Nakano, Takehito; Nozue, Yasuo; Arčon, Denis

2016-01-01

We report a systematic nuclear magnetic resonance investigation of the 23Na spin-lattice relaxation rate, 1/T1, in sodium loaded low-silica X (LSX) zeolite, Nan/Na12-LSX, for various loading levels of sodium atoms n across the metal-to-insulator crossover. For high loading levels of n ≥ 14.2, 1/T1T shows nearly temperature-independent behaviour between 10 K and 25 K consistent with the Korringa relaxation mechanism and the metallic ground state. As the loading levels decrease below n ≤ 11.6, the extracted density of states (DOS) at the Fermi level sharply decreases, although a residual DOS at Fermi level is still observed even in the samples that lack the metallic Drude-peak in the optical reflectance. The observed crossover is a result of a complex loading-level dependence of electric potential felt by the electrons confined to zeolite cages, where the electronic correlations and disorder both play an important role. PMID:26725368

Magnetic-field-induced crossover from the inverse Faraday effect to the optical orientation in EuTe

NASA Astrophysics Data System (ADS)

Pavlov, V. V.; Pisarev, R. V.; Nefedov, S. G.; Akimov, I. A.; Yakovlev, D. R.; Bayer, M.; Henriques, A. B.; Rappl, P. H. O.; Abramof, E.

2018-05-01

A time-resolved optical pump-probe technique has been applied for studying the ultrafast dynamics in the magnetic semiconductor EuTe near the absorption band gap. We show that application of external magnetic field up to 6 T results in crossover from the inverse Faraday effect taking place on the femtosecond time scale to the optical orientation phenomenon with an evolution in the picosecond time domain. We propose a model which includes both these processes, possessing different spectral and temporal properties. The circularly polarized optical pumping induces the electronic transition 4 f 7 5 d 0 → 4 f 6 5 d 1 forming the absorption band gap in EuTe. The observed crossover is related to a strong magnetic-field shift of the band gap in EuTe at low temperatures. It was found that manipulation of spin states on intrinsic defect levels takes place on a time scale of 19 ps in the applied magnetic field of 6 T.

Fast Xe-129 relaxation in solid xenon near its melting point: Cross-over from Raman scattering of phonons to vacancy diffusion.

NASA Astrophysics Data System (ADS)

Kuzma, N. N.; Patton, B.; Raman, K.; Happer, W.

2002-03-01

NMR measurements of longitudinal relaxation times T1 in pure solid xenon were carried out using both natural-abundance and isotopically-enriched samples of hyperpolarized ^129Xe. At temperatures below 120 K and fields above 500 Gauss, the relaxation rate 1/T1 is field- and abundance-independent, consistent with the model of ^129Xe spin-flip Raman scattering of phonons(R. J. Fitzgerald et al.), Phys. Rev. B 59, 8795 (1999).. Above 120 K, vacancies invade the xenon lattice(P. R. Granfors et al.) Phys. Rev. B 24, 4753 (1981)., and a dramatic cross-over to the nuclear dipole-dipole relaxation due to the diffusion of vacancies is observed. As a result, the measured relaxation times of xenon near its melting point strongly depend on field and somewhat on ^129Xe abundance, and can be as short as several seconds, leading to potential difficulties in cryogenic applications of hyperpolarized ^129Xe. The data are analyzed using the theory of nuclear relaxation due to spin diffusion in cubic crystals(C. A. Sholl, J. Phys. C 21), 319 (1988)., and some estimates of the vacancy density and jump rates are discussed.

Heavy-fermion superconductivity in CeAg2Si2 - Interplay of spin and valence fluctuations

NASA Astrophysics Data System (ADS)

Scheerer, Gernot W.; Ren, Zhi; Lapertot, Gérard; Garbarino, Gaston; Jaccard, Didier

2018-05-01

We present the pressure-temperature phase diagram of the antiferromagnet CeAg2Si2 established via resistivity and calorimetry measurements under quasi-hydrostatic conditions up to 22.5 GPa. With increasing pressure, the Néel temperature [TN (p = 0) = 8.6 K] slowly increases up to TN = 13.4 K at 9.4 GPa and then vanishes abruptly at the magnetic critical pressure pc ∼ 13 GPa. For the first time, heavy fermion superconductivity is observed in CeAg2Si2. Superconductivity emerges at ∼ 11 GPa and persists over roughly 10 GPa. Partial- and bulk-transition temperatures are highest at p = 16 GPa, with a maximal Tcbulk = 1.25 K. In the pressure region of superconductivity, Kondo and crystal-field splitting energies become comparable and resistivity exhibits clear signatures of a Ce-ion valence crossover. The crossover line is located at a rapid collapse in resistivity as function of pressure and extrapolates to a valence transition critical endpoint at critical pressure and temperature of pcr ∼ 17 GPa and Tcr ∼ - 13 K , respectively. Both critical spin and valence fluctuations may build up superconductivity in CeAg2Si2.

Crossover between weak anti-localization and weak localization by Co doping and annealing in gapless PbPdO{sub 2} and spin gapless Co-doped PbPdO{sub 2}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Choo, S. M.; Lee, K. J.; Park, S. M.

2015-04-27

The magnetotransport properties of Pb(Pd,Co)O{sub 2} and PbPdO{sub 2} thin films were investigated. In magnetoconductance curves, we observed a crossover between weak anti-localization (WAL) and weak localization (WL) depending on the annealing and Co doping in PbPdO{sub 2} thin films. For the Pb(Pd,Co)O{sub 2} case showing WAL signals, the ex-situ annealing weakens the Pd-O hybridization by stabilizing Co{sup 3+} states and generating Pd{sup 1+} states, instead of Pd{sup 2+}, so that the spin-orbit coupling (SOC) strength is significantly reduced. It causes the dominant magnetotransport mechanism change from WAL to WL. This annealing effect is compared with the PbPdO{sub 2} case,more » which possesses WL signals. The annealing process stabilizes the oxygen states and enhances the Pd-O hybridization, and consequently the SOC strength is enhanced. Our experimental results are well explained by the Hikami-Larkin-Nagaoka theory in terms of two important physical parameters; SOC strength-related α and inelastic scattering length l{sub ϕ}.« less

Thermoelasticity of Fe2+-bearing bridgmanite

NASA Astrophysics Data System (ADS)

Shukla, Gaurav; Wu, Zhongqing; Hsu, Han; Floris, Andrea; Cococcioni, Matteo; Wentzcovitch, Renata M.

2015-03-01

We present local density approximation augmented by the Hubbard-type correction calculations of high-temperature elastic properties of bridgmanite with composition (Mg(1-x)Fex2+)SiO3 for 0≤×≤0.125. Results of elastic moduli and acoustic velocities for the Mg end-member (x=0) agree very well with the latest high-pressure and high-temperature experimental measurements. In the iron-bearing system, we focus particularly on the change in thermoelastic parameters across the state change that occurs in ferrous iron above ˜30 GPa, often attributed to a high-spin (HS) to intermediate-spin (IS) crossover but explained by first-principles calculations as a lateral displacement of substitutional iron in the perovskite cage. We show that the measured effect of this change on the equation of state of this system can be explained by the lateral displacement of substitutional iron and not by the HS to IS crossover. The calculated elastic properties of (Mg0.875Fe0.1252+)SiO3 along an adiabatic mantle geotherm somewhat overestimate longitudinal velocities but produce densities and shear velocities quite consistent with the Preliminary Reference Earth Model data throughout most of the lower mantle.

Thermoelasticity of (Mg,Fe)SiO3 perovskite

NASA Astrophysics Data System (ADS)

Shukla, Gaurav; Wu, Zhongqing; Hsu, Han; Cococcioni, Matteo; Wentzcovitch, Renata

2015-03-01

We present LDA+U calculations of high temperature elastic properties of (Mg(1 - x)Fex2+)SiO3 bridgemanite (0 <= x <= 0 . 125), the most abundant constituent of Earth's lower mantle. Calculations of aggregate elastic moduli and acoustic velocities for the Mg-end member (x=0) are in excellent agreement with the latest high pressure and high temperature experimental measurements. In the iron bearing system, we particularly focus on the change in thermoelastic parameters across the state change that occurs in ferrous iron above ~30 GPa, often attributed to a high-spin (HS) to intermediate spin (IS) crossover but explained by calculations as a lateral displacement of substitutional iron in the perovskite cage. We show that the measured effect on the equation of state of this change in the state of iron can be explained by the lateral displacement of substitutional iron, not by the HS to IS crossover. Calculated elastic properties of (Mg0.875 Fe0.125 2 +)SiO3 along an adiabatic mantle geotherm, somewhat overestimate longitudinal velocities but produce densities and shear velocities consistent with Preliminary Reference Earth Model data throughout most of the lower mantle. Research supported by NSF/EAR and NSF/CAREER.

Bidirectional Photoswitching via Alternating NIR and UV Irradiation on a Core-Shell UCNP-SCO Nanosphere.

PubMed

Luo, Yang-Hui; Wang, Jing-Wen; Wang, Wen; He, Xiao-Tong; Hong, Dan-Li; Chen, Chen; Xu, Tao; Shao, Qiyue; Sun, Bai-Wang

2018-05-16

Bidirectional photoswitching of molecular materials under ambient condition is of significant importance. Herein, we present for the first time that a core-shell UCNP-SCO nanosphere (UCNP = upconversion nanophosphor, SCO = spin crossover), which was composed of a UCNP core (NaYF 4 : 20 mol % Yb 3+ , 1 mol % Er 3+ ) and an SCO iron(II) shell ([Fe(H 2 Bpz) 2 (bipy-COOH)], H 2 Bpz = dihydrobis(1-pyrazolyl)borate, bipy-COOH = 4,4'-dicarboxy-2,2'-bipyridine), can be reversibly photoswitched between the high-spin and low-spin states at room temperature in the solid state, via alternating irradiation with near-infrared (λ = 980 nm) and ultraviolet (λ = 310 nm) light. What's more, this reversible spin-state switching was accompanied by a variation of fluorescent spectrum and dielectric constants. The strategy here, that is, integrating the SCO iron(II) complex into a UCNP-SCO nanosphere for molecular photoswitching, may open a new area in the development of photocontrolled molecular devices.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rikvold, Per Arne; Brown, Gregory; Miyashita, Seiji

Phase diagrams and hysteresis loops were obtained by Monte Carlo simulations and a mean- field method for a simplified model of a spin-crossovermaterialwith a two-step transition between the high-spin and low-spin states. This model is a mapping onto a square-lattice S = 1/2 Ising model with antiferromagnetic nearest-neighbor and ferromagnetic Husimi-Temperley ( equivalent-neighbor) long-range interactions. Phase diagrams obtained by the two methods for weak and strong long-range interactions are found to be similar. However, for intermediate-strength long-range interactions, the Monte Carlo simulations show that tricritical points decompose into pairs of critical end points and mean-field critical points surrounded by horn-shapedmore » regions of metastability. Hysteresis loops along paths traversing the horn regions are strongly reminiscent of thermal two-step transition loops with hysteresis, recently observed experimentally in several spin-crossover materials. As a result, we believe analogous phenomena should be observable in experiments and simulations for many systems that exhibit competition between local antiferromagnetic-like interactions and long-range ferromagnetic-like interactions caused by elastic distortions.« less

Magnetic moments induce strong phonon renormalization in FeSi.

PubMed

Krannich, S; Sidis, Y; Lamago, D; Heid, R; Mignot, J-M; Löhneysen, H v; Ivanov, A; Steffens, P; Keller, T; Wang, L; Goering, E; Weber, F

2015-11-27

The interactions of electronic, spin and lattice degrees of freedom in solids result in complex phase diagrams, new emergent phenomena and technical applications. While electron-phonon coupling is well understood, and interactions between spin and electronic excitations are intensely investigated, only little is known about the dynamic interactions between spin and lattice excitations. Noncentrosymmetric FeSi is known to undergo with increasing temperature a crossover from insulating to metallic behaviour with concomitant magnetic fluctuations, and exhibits strongly temperature-dependent phonon energies. Here we show by detailed inelastic neutron-scattering measurements and ab initio calculations that the phonon renormalization in FeSi is linked to its unconventional magnetic properties. Electronic states mediating conventional electron-phonon coupling are only activated in the presence of strong magnetic fluctuations. Furthermore, phonons entailing strongly varying Fe-Fe distances are damped via dynamic coupling to the temperature-induced magnetic moments, highlighting FeSi as a material with direct spin-phonon coupling and multiple interaction paths.

Quench dynamics of the spin-imbalanced Fermi-Hubbard model in one dimension

NASA Astrophysics Data System (ADS)

Yin, Xiao; Radzihovsky, Leo

2016-12-01

We study a nonequilibrium dynamics of a one-dimensional spin-imbalanced Fermi-Hubbard model following a quantum quench of on-site interaction, realizable, for example, in Feshbach-resonant atomic Fermi gases. We focus on the post-quench evolution starting from the initial BCS and Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) ground states and analyze the corresponding spin-singlet, spin-triplet, density-density, and magnetization-magnetization correlation functions. We find that beyond a light-cone crossover time, rich post-quench dynamics leads to thermalized and pre-thermalized stationary states that display strong dependence on the initial ground state. For initially gapped BCS state, the long-time stationary state resembles thermalization with the effective temperature set by the initial value of the Hubbard interaction. In contrast, while the initial gapless FFLO state reaches a stationary pre-thermalized form, it remains far from equilibrium. We suggest that such post-quench dynamics can be used as a fingerprint for identification and study of the FFLO phase.

Electronic structure and quantum spin fluctuations at the magnetic phase transition in MnSi

NASA Astrophysics Data System (ADS)

Povzner, A. A.; Volkov, A. G.; Nogovitsyna, T. A.

2018-05-01

The effect of spin fluctuations on the heat capacity and homogeneous magnetic susceptibility of the chiral magnetic MnSi in the vicinity of magnetic transition has been investigated by using the free energy functional of the coupled electron and spin subsystems and taking into account the Dzyaloshinsky-Moriya interaction. For helical ferromagnetic ordering, we found that zero-point fluctuations of the spin density are large and comparable with fluctuations of the non-uniform magnetization. The amplitude of zero-point spin fluctuations shows a sharp decrease in the region of the magnetic phase transition. It is shown that sharp decrease of the amplitude of the quantum spin fluctuations results in the lambda-like maxima of the heat capacity and the homogeneous magnetic susceptibility. Above the temperature of the lambda anomaly, the spin correlation radius becomes less than the period of the helical structure and chiral fluctuations of the local magnetization appear. It is shown that formation of a "shoulder" on the temperature dependence of the heat capacity is due to disappearance of the local magnetization. Our finding allows to explain the experimentally observed features of the magnetic phase transition of MnSi as a result of the crossover of quantum and thermodynamic phase transitions.

Electronic spin state of Fe,Al-containing MgSiO3 perovskite at lower mantle conditions

NASA Astrophysics Data System (ADS)

Kupenko, I.; McCammon, C.; Sinmyo, R.; Prescher, C.; Chumakov, A. I.; Kantor, A.; Rüffer, R.; Dubrovinsky, L.

2014-02-01

We have investigated silicate perovskite with composition Mg0.83Fe0.21Al0.06Si0.91O3 relevant for the lower mantle at pressures up to 81 GPa and temperatures up to 2000 K using conventional Mössbauer spectroscopy and synchrotron Nuclear Forward Scattering (NFS) combined with double-sided laser heating in a diamond anvil cell. Room temperature Mössbauer and NFS spectra at low pressure are dominated by high-spin Fe2 +, with minor amounts of Fe3 + and a component assigned to a metastable position of high-spin Fe2 + in the A-site predicted by computational studies. NFS data show a sharp transition (< 20 GPa) from high-spin Fe2 + to a new component with extremely high quadrupole splitting, similar to previous studies. Mössbauer data show the same transition, but over a broader pressure range likely due to the higher pressure gradient. The new Fe2 + component is assigned to intermediate-spin Fe2 +, consistent with previous X-ray emission studies. NFS data at high temperatures and high pressures comparable to those in the lower mantle are consistent with the presence of Fe2 + only in the intermediate-spin state and Fe3 + only in the high-spin state. Our results are therefore consistent with the occurrence of spin crossover only in Fe2 + in Fe-, Al-containing perovskite within the lower mantle.

Magnetic structure and magnetization of helical antiferromagnets in high magnetic fields perpendicular to the helix axis at zero temperature

DOE PAGES

Johnston, David

2017-09-05

The zero-temperature angles of magnetic moments in a helix or sinusoidal fan confined to the x y plane, with respect to an in-plane magnetic field H x applied perpendicular to the z axis of a helix or fan, are calculated for commensurate helices and fans with field-independent turn angles k d between moments in adjacent layers of the helix or fan using the classical J 0 - J 1 - J 2 Heisenberg model. For 0 < k d < 4 π / 9 , first-order transitions from helix to a fan structure occur at fields H t as previouslymore » inferred, where the fan is found to be approximately sinusoidal. However, for 4 π / 9 ≤ k d ≤ π , different behaviors are found depending on the value of k d and these properties vary nonmonotonically with k d . In this k d range, the change from helix to fanlike structure is usually a crossover with no phase transition between them, although first-order transitions are found for k d = 3 π / 5 and 8 π / 11 and a second-order transition for k d = 3 π / 4 . At a critical field H c , the fan or fanlike structures exhibit a second-order transition to the paramagnetic state. The H c for a helix undergoing a field-induced change to a fan or fanlike structure is found to be the same as for a sinusoidal fan with the same k d and interlayer interactions. We present analytical expressions for H c versus k d. We also calculated the average x -axis moment per spin μ x ave versus H x for helices and fans with crossovers and phase transitions between them. When smooth helix to fanlike crossovers occur in the range 4 π / 9 ≤ k d ≤ π , μ x ave exhibits an S-shape behavior with increasing H x . The behavior we predict is consistent with μ x ave ( H x ) data previously reported by Sangeetha et al. [Phys. Rev. B 94, 014422 (2016)] for single-crystal EuCo 2 P 2 possessing a helix ground state with k d ≈ 0.85 π . The low-field magnetic susceptibility and the ratio H t / H c are calculated analytically or numerically versus k d for helices, and are shown to approach the respective known limits for k d → 0 .« less

Magnetic structure and magnetization of helical antiferromagnets in high magnetic fields perpendicular to the helix axis at zero temperature

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnston, David

The zero-temperature angles of magnetic moments in a helix or sinusoidal fan confined to the x y plane, with respect to an in-plane magnetic field H x applied perpendicular to the z axis of a helix or fan, are calculated for commensurate helices and fans with field-independent turn angles k d between moments in adjacent layers of the helix or fan using the classical J 0 - J 1 - J 2 Heisenberg model. For 0 < k d < 4 π / 9 , first-order transitions from helix to a fan structure occur at fields H t as previouslymore » inferred, where the fan is found to be approximately sinusoidal. However, for 4 π / 9 ≤ k d ≤ π , different behaviors are found depending on the value of k d and these properties vary nonmonotonically with k d . In this k d range, the change from helix to fanlike structure is usually a crossover with no phase transition between them, although first-order transitions are found for k d = 3 π / 5 and 8 π / 11 and a second-order transition for k d = 3 π / 4 . At a critical field H c , the fan or fanlike structures exhibit a second-order transition to the paramagnetic state. The H c for a helix undergoing a field-induced change to a fan or fanlike structure is found to be the same as for a sinusoidal fan with the same k d and interlayer interactions. We present analytical expressions for H c versus k d. We also calculated the average x -axis moment per spin μ x ave versus H x for helices and fans with crossovers and phase transitions between them. When smooth helix to fanlike crossovers occur in the range 4 π / 9 ≤ k d ≤ π , μ x ave exhibits an S-shape behavior with increasing H x . The behavior we predict is consistent with μ x ave ( H x ) data previously reported by Sangeetha et al. [Phys. Rev. B 94, 014422 (2016)] for single-crystal EuCo 2 P 2 possessing a helix ground state with k d ≈ 0.85 π . The low-field magnetic susceptibility and the ratio H t / H c are calculated analytically or numerically versus k d for helices, and are shown to approach the respective known limits for k d → 0 .« less

Spatiotemporal dynamics of the spin transition in [Fe (HB(tz)3) 2] single crystals

NASA Astrophysics Data System (ADS)

Ridier, Karl; Rat, Sylvain; Shepherd, Helena J.; Salmon, Lionel; Nicolazzi, William; Molnár, Gábor; Bousseksou, Azzedine

2017-10-01

The spatiotemporal dynamics of the spin transition have been thoroughly investigated in single crystals of the mononuclear spin-crossover (SCO) complex [Fe (HB (tz )3)2] (tz = 1 ,2 ,4-triazol-1-yl) by optical microscopy. This compound exhibits an abrupt spin transition centered at 334 K with a narrow thermal hysteresis loop of ˜1 K (first-order transition). Most single crystals of this compound reveal exceptional resilience upon repeated switching (several hundred cycles), which allowed repeatable and quantitative measurements of the spatiotemporal dynamics of the nucleation and growth processes to be carried out. These experiments revealed remarkable properties of the thermally induced spin transition: high stability of the thermal hysteresis loop, unprecedented large velocities of the macroscopic low-spin/high-spin phase boundaries up to 500 µm/s, and no visible dependency on the temperature scan rate. We have also studied the dynamics of the low-spin → high-spin transition induced by a local photothermal excitation generated by a spatially localized (Ø = 2 μ m ) continuous laser beam. Interesting phenomena have been evidenced both in quasistatic and dynamic conditions (e.g., threshold effects and long incubation periods, thermal activation of the phase boundary propagation, stabilization of the crystal in a stationary biphasic state, and thermal cutoff frequency). These measurements demonstrated the importance of thermal effects in the transition dynamics, and they enabled an accurate determination of the thermal properties of the SCO compound in the framework of a simple theoretical model.

Husimi-cactus approximation study on the diluted spin ice

NASA Astrophysics Data System (ADS)

Otsuka, Hiromi; Okabe, Yutaka; Nefedev, Konstantin

2018-04-01

We investigate dilution effects on the classical spin-ice materials such as Ho2Ti2O7 and Dy2Ti2O7 . In particular, we derive a formula of the thermodynamic quantities as functions of the temperature and a nonmagnetic ion concentration based on a Husimi-cactus approximation. We find that the formula predicts a dilution-induced crossover from the cooperative to the conventional paramagnets in a ground state, and that it also reproduces the "generalized Pauling's entropy" given by Ke et al. To verify the formula from a numerical viewpoint, we compare these results with Monte Carlo simulation calculation data, and then find good agreement for all parameter values.

Magnetic moment evolution and spin freezing in doped BaFe2As2

DOE PAGES

Pelliciari, Jonathan; Huang, Yaobo; Ishii, Kenji; ...

2017-08-14

Fe-K β X-ray emission spectroscopy measurements reveal an asymmetric doping dependence of the magnetic moments μ bare in electron- and hole-doped BaFe 2As 2. At low temperature, μ bare is nearly constant in hole-doped samples, whereas it decreases upon electron doping. Increasing temperature substantially enhances μ bare in the hole-doped region, which is naturally explained by the theoretically predicted crossover into a spin-frozen state. Our measurements demonstrate the importance of Hund’s-coupling and electronic correlations, especially for hole-doped BaFe 2As 2, as well as the inadequacy of a fully localized or fully itinerant description of the 122 family of Fe pnictides.

Universal and measurable entanglement entropy in the spin-boson model.

PubMed

Kopp, Angela; Le Hur, Karyn

2007-06-01

We study the entanglement between a qubit and its environment from the spin-boson model with Ohmic dissipation. Through a mapping to the anisotropic Kondo model, we derive the entropy of entanglement of the spin E(alpha,Delta,h), where alpha is the dissipation strength, Delta is the tunneling amplitude between qubit states, and h is the level asymmetry. For 1-alpha>Delta/omegac and (Delta,h)TK, E vanishes as (TK/h)2-2alpha, up to a logarithmic correction. For a given h, the maximum entanglement occurs at a value of alpha which lies in the crossover regime h approximately TK. We emphasize the possibility of measuring this entanglement using charge qubits subject to electromagnetic noise.

Quantum impurity models for magnetic adsorbates on superconductor surfaces

NASA Astrophysics Data System (ADS)

Žitko, Rok

2018-05-01

Magnetic atoms adsorbed on surfaces have a quenched orbital moment while their ground-state spin multiplet is partially split as a consequence of the spin-orbit coupling which, even if intrinsically weak, has a large effect due to the abrupt change of the potential at the surface. Such metal adsorbates should be modelled using quantum impurity models that include the relevant internal degrees of freedom and the interaction terms, in particular the magnetic anisotropy and the Kondo exchange coupling. When adsorbed on superconducting surfaces, these impurities have complex spectra of sub-gap excitations due to magnetic anisotropy splitting and Kondo screening. Both anisotropy splitting and Zeeman splitting due to the external magnetic field are significantly renormalized by the coupling to the substrate electrons. In this work I discuss the quantum-to-classical crossover and the applicability of classical static-local-spin picture for discussing magnetic nanostructures on superconductors.

Extreme Field Sensitivity of Magnetic Tunneling in Fe-Doped Li3 N

NASA Astrophysics Data System (ADS)

Fix, M.; Atkinson, J. H.; Canfield, P. C.; del Barco, E.; Jesche, A.

2018-04-01

The magnetic properties of dilute Li2 (Li1 -xFex )N with x ˜0.001 are dominated by the spin of single, isolated Fe atoms. Below T =10 K the spin-relaxation times become temperature independent indicating a crossover from thermal excitations to the quantum tunneling regime. We report on a strong increase of the spin-flip probability in transverse magnetic fields that proves the resonant character of this tunneling process. Longitudinal fields, on the other hand, lift the ground-state degeneracy and destroy the tunneling condition. An increase of the relaxation time by 4 orders of magnitude in applied fields of only a few milliTesla reveals exceptionally sharp tunneling resonances. Li2 (Li1 -xFex )N represents a comparatively simple and clean model system that opens the possibility to study quantum tunneling of the magnetization at liquid helium temperatures.

Extreme Field Sensitivity of Magnetic Tunneling in Fe-Doped Li 3 N

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fix, M.; Atkinson, J. H.; Canfield, P. C.

Here, the magnetic properties of dilute Li 2(Li 1–xFe x)N with x~0.001 are dominated by the spin of single, isolated Fe atoms. Below T=10 K the spin-relaxation times become temperature independent indicating a crossover from thermal excitations to the quantum tunneling regime. We report on a strong increase of the spin-flip probability in transverse magnetic fields that proves the resonant character of this tunneling process. Longitudinal fields, on the other hand, lift the ground-state degeneracy and destroy the tunneling condition. An increase of the relaxation time by 4 orders of magnitude in applied fields of only a few milliTesla revealsmore » exceptionally sharp tunneling resonances. Li 2(Li 1–xFe x)N represents a comparatively simple and clean model system that opens the possibility to study quantum tunneling of the magnetization at liquid helium temperatures.« less

Extreme Field Sensitivity of Magnetic Tunneling in Fe-Doped Li 3 N

DOE PAGES

Fix, M.; Atkinson, J. H.; Canfield, P. C.; ...

2018-04-04

Here, the magnetic properties of dilute Li 2(Li 1–xFe x)N with x~0.001 are dominated by the spin of single, isolated Fe atoms. Below T=10 K the spin-relaxation times become temperature independent indicating a crossover from thermal excitations to the quantum tunneling regime. We report on a strong increase of the spin-flip probability in transverse magnetic fields that proves the resonant character of this tunneling process. Longitudinal fields, on the other hand, lift the ground-state degeneracy and destroy the tunneling condition. An increase of the relaxation time by 4 orders of magnitude in applied fields of only a few milliTesla revealsmore » exceptionally sharp tunneling resonances. Li 2(Li 1–xFe x)N represents a comparatively simple and clean model system that opens the possibility to study quantum tunneling of the magnetization at liquid helium temperatures.« less

Extreme Field Sensitivity of Magnetic Tunneling in Fe-Doped Li_{3}N.

PubMed

Fix, M; Atkinson, J H; Canfield, P C; Del Barco, E; Jesche, A

2018-04-06

The magnetic properties of dilute Li_{2}(Li_{1-x}Fe_{x})N with x∼0.001 are dominated by the spin of single, isolated Fe atoms. Below T=10  K the spin-relaxation times become temperature independent indicating a crossover from thermal excitations to the quantum tunneling regime. We report on a strong increase of the spin-flip probability in transverse magnetic fields that proves the resonant character of this tunneling process. Longitudinal fields, on the other hand, lift the ground-state degeneracy and destroy the tunneling condition. An increase of the relaxation time by 4 orders of magnitude in applied fields of only a few milliTesla reveals exceptionally sharp tunneling resonances. Li_{2}(Li_{1-x}Fe_{x})N represents a comparatively simple and clean model system that opens the possibility to study quantum tunneling of the magnetization at liquid helium temperatures.

Polar materials with isolated V 4+ S = 1/2 Triangles: NaSr 2V 3O 3(Ge 4O 13)Cl and KSr 2V 3O 3(Ge 4O 13)Cl

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sanjeewa, Liurukara D.; McGuire, Michael A.; McMillen, Colin D.

Here, crystals of ASr 2V 3O 3(Ge 4O 13)Cl, A = Na, K, were synthesized from high-temperature hydrothermal brines, and their structure and magnetic properties were investigated. These materials present a unique combination of a salt inclusion lattice, a polar crystal structure, and isolated V 4+ ( S = 1/2) trimer magnetic clusters. The structures consist of a trimeric V 3O 13 unit based on V 4+ ( S = 1/2), having rigorous 3-fold symmetry with a short V–V separation of 3.325(3) Å. The trinuclear V 4+ units are formed by three edge shared VO 6 octahedra sharing a centralmore » μ3-oxygen atom, which also imparts a polar sense on the structure. The V 3O 13 units are isolated from one another by tetranuclear Ge 4O 13 units, which are similarly arranged in a polar fashion, providing a unique opportunity to study the magnetic behavior of this triangular d 1 system as a discrete unit. Magnetization measurements indicate spin-1/2 per V atom at high temperature, and spin-1/2 per V 3 trimer at low temperature, where two V moments in each triangle are antiferromagnetically aligned and the third remains paramagnetic. The crossover between these two behaviors occurs between 20 and 100 K and is well-described by a model incorporating strong antiferromagnetic intra-trimer interactions and weak but nonzero inter-trimer interactions. More broadly, the study highlights the ability to obtain new materials with interesting structure–property relationships via chemistry involving unconventional solvents and reaction conditions.« less

Polar materials with isolated V 4+ S = 1/2 Triangles: NaSr 2V 3O 3(Ge 4O 13)Cl and KSr 2V 3O 3(Ge 4O 13)Cl

DOE PAGES

Sanjeewa, Liurukara D.; McGuire, Michael A.; McMillen, Colin D.; ...

2017-01-03

Here, crystals of ASr 2V 3O 3(Ge 4O 13)Cl, A = Na, K, were synthesized from high-temperature hydrothermal brines, and their structure and magnetic properties were investigated. These materials present a unique combination of a salt inclusion lattice, a polar crystal structure, and isolated V 4+ ( S = 1/2) trimer magnetic clusters. The structures consist of a trimeric V 3O 13 unit based on V 4+ ( S = 1/2), having rigorous 3-fold symmetry with a short V–V separation of 3.325(3) Å. The trinuclear V 4+ units are formed by three edge shared VO 6 octahedra sharing a centralmore » μ3-oxygen atom, which also imparts a polar sense on the structure. The V 3O 13 units are isolated from one another by tetranuclear Ge 4O 13 units, which are similarly arranged in a polar fashion, providing a unique opportunity to study the magnetic behavior of this triangular d 1 system as a discrete unit. Magnetization measurements indicate spin-1/2 per V atom at high temperature, and spin-1/2 per V 3 trimer at low temperature, where two V moments in each triangle are antiferromagnetically aligned and the third remains paramagnetic. The crossover between these two behaviors occurs between 20 and 100 K and is well-described by a model incorporating strong antiferromagnetic intra-trimer interactions and weak but nonzero inter-trimer interactions. More broadly, the study highlights the ability to obtain new materials with interesting structure–property relationships via chemistry involving unconventional solvents and reaction conditions.« less

Crossover behavior of stock returns and mean square displacements of particles governed by the Langevin equation

NASA Astrophysics Data System (ADS)

Ma, Wen-Jong; Wang, Shih-Chieh; Chen, Chi-Ning; Hu, Chin-Kun

2013-06-01

It is found that the mean square log-returns calculated from the high-frequency one-day moving average of US and Taiwan stocks with the time internal τ show ballistic behavior \\theta \\tau^{\\alpha_1} with the exponent \\alpha_1 \\approx 2 for small τ and show diffusion-like behavior D \\tau^{\\alpha_2} with the exponent \\alpha_2 \\approx 1 for large τ. Such a crossover behavior can be well described by the mean square displacements of particles governed by the Langevin equation of motion. Thus, θ and D can be considered, respectively, as the temperature-like and diffusivity-like kinetic parameters of the market, and they can be used to characterize the behavior of the market.

ESR and PALS detection of the dynamic crossover in the supercooled liquid states of short and medium-sized n-alkanes

NASA Astrophysics Data System (ADS)

Bartoš, J.; Zgardzinska, B.; Švajdlenková, H.; Lukešová, M.; Zaleski, R.

2018-05-01

A joint study of the spin probe TEMPO dynamics by ESR and the annihilation rate of ortho-positronium by PALS in four short-and medium-sized n-alkanes is presented. In addition to the usually observed changes in both the reorientation dynamics and size of free volumes at the temperature of melting, Tm, and solid-solid phase transition, Tss, an additional coincidence between the characteristic ESR and PALS temperatures TX1fast ≅ Tb1sol < Tm, Tss was found. The phenomenological analysis of the viscosity data of n-alkanes using the power law equation indicates a presence of locally disordered regions in which the dynamic change occurs at the crossover temperature TX ≅ TX1fast ≅ Tb1sol.

Universality of modulation length and time exponents.

PubMed

Chakrabarty, Saurish; Dobrosavljević, Vladimir; Seidel, Alexander; Nussinov, Zohar

2012-10-01

We study systems with a crossover parameter λ, such as the temperature T, which has a threshold value λ(*) across which the correlation function changes from exhibiting fixed wavelength (or time period) modulations to continuously varying modulation lengths (or times). We introduce a hitherto unknown exponent ν(L) characterizing the universal nature of this crossover and compute its value in general instances. This exponent, similar to standard correlation length exponents, is obtained from motion of the poles of the momentum (or frequency) space correlation functions in the complex k-plane (or ω-plane) as the parameter λ is varied. Near the crossover (i.e., for λ→λ(*)), the characteristic modulation wave vector K(R) in the variable modulation length "phase" is related to that in the fixed modulation length "phase" q via |K(R)-q|[proportionality]|T-T(*)|(νL). We find, in general, that ν(L)=1/2. In some special instances, ν(L) may attain other rational values. We extend this result to general problems in which the eigenvalue of an operator or a pole characterizing general response functions may attain a constant real (or imaginary) part beyond a particular threshold value λ(*). We discuss extensions of this result to multiple other arenas. These include the axial next-nearest-neighbor Ising (ANNNI) model. By extending our considerations, we comment on relations pertaining not only to the modulation lengths (or times), but also to the standard correlation lengths (or times). We introduce the notion of a Josephson time scale. We comment on the presence of aperiodic "chaotic" modulations in "soft-spin" and other systems. These relate to glass-type features. We discuss applications to Fermi systems, with particular application to metal to band insulator transitions, change of Fermi surface topology, divergent effective masses, Dirac systems, and topological insulators. Both regular periodic and glassy (and spatially chaotic behavior) may be found in strongly correlated electronic systems.

Crossover between the Gaussian orthogonal ensemble, the Gaussian unitary ensemble, and Poissonian statistics.

PubMed

Schweiner, Frank; Laturner, Jeanine; Main, Jörg; Wunner, Günter

2017-11-01

Until now only for specific crossovers between Poissonian statistics (P), the statistics of a Gaussian orthogonal ensemble (GOE), or the statistics of a Gaussian unitary ensemble (GUE) have analytical formulas for the level spacing distribution function been derived within random matrix theory. We investigate arbitrary crossovers in the triangle between all three statistics. To this aim we propose an according formula for the level spacing distribution function depending on two parameters. Comparing the behavior of our formula for the special cases of P→GUE, P→GOE, and GOE→GUE with the results from random matrix theory, we prove that these crossovers are described reasonably. Recent investigations by F. Schweiner et al. [Phys. Rev. E 95, 062205 (2017)2470-004510.1103/PhysRevE.95.062205] have shown that the Hamiltonian of magnetoexcitons in cubic semiconductors can exhibit all three statistics in dependence on the system parameters. Evaluating the numerical results for magnetoexcitons in dependence on the excitation energy and on a parameter connected with the cubic valence band structure and comparing the results with the formula proposed allows us to distinguish between regular and chaotic behavior as well as between existent or broken antiunitary symmetries. Increasing one of the two parameters, transitions between different crossovers, e.g., from the P→GOE to the P→GUE crossover, are observed and discussed.

Field-driven quantum phase transitions in S =1/2 spin chains

NASA Astrophysics Data System (ADS)

Iaizzi, Adam; Damle, Kedar; Sandvik, Anders W.

2017-05-01

We study the magnetization process of a one-dimensional extended Heisenberg model, the J -Q model, as a function of an external magnetic field h . In this model, J represents the traditional antiferromagnetic Heisenberg exchange and Q is the strength of a competing four-spin interaction. Without external field, this system hosts a twofold-degenerate dimerized (valence-bond solid) state above a critical value qc≈0.85 where q ≡Q /J . The dimer order is destroyed and replaced by a partially polarized translationally invariant state at a critical field value. We find magnetization jumps (metamagnetism) between the partially polarized and fully polarized state for q >qmin , where we have calculated qmin=2/9 exactly. For q >qmin , two magnons (flipped spins on a fully polarized background) attract and form a bound state. Quantum Monte Carlo studies confirm that the bound state corresponds to the first step of an instability leading to a finite magnetization jump for q >qmin . Our results show that neither geometric frustration nor spin anisotropy are necessary conditions for metamagnetism. Working in the two-magnon subspace, we also find evidence pointing to the existence of metamagnetism in the unfrustrated J1-J2 chain (J1>0 ,J2<0 ), but only if J2 is spin anisotropic. In addition to the studies at zero temperature, we also investigate quantum-critical scaling near the transition into the fully polarized state for q ≤qmin at T >0 . While the expected "zero-scale-factor" universality is clearly seen for q =0 and q ≪qmin , for q closer to qmin we find that extremely low temperatures are required to observe the asymptotic behavior, due to the influence of the tricritical point at qmin. In the low-energy theory, one can expect the quartic nonlinearity to vanish at qmin and a marginal sixth-order term should govern the scaling, which leads to a crossover at a temperature T*(q ) between logarithmic tricritical scaling and zero-scale-factor universality, with T*(q ) →0 when q →qmin .

Crossover from antipersistent to persistent behavior in time series possessing the generalyzed dynamic scaling law

NASA Astrophysics Data System (ADS)

Balankin, Alexander S.; Morales Matamoros, Oswaldo; Gálvez M., Ernesto; Pérez A., Alfonso

2004-03-01

The behavior of crude oil price volatility is analyzed within a conceptual framework of kinetic roughening of growing interfaces. We find that the persistent long-horizon volatilities satisfy the Family-Viscek dynamic scaling ansatz, whereas the mean-reverting in time short horizon volatilities obey the generalized scaling law with continuously varying scaling exponents. Furthermore we find that the crossover from antipersistent to persistent behavior is accompanied by a change in the type of volatility distribution. These phenomena are attributed to the complex avalanche dynamics of crude oil markets and so a similar behavior may be observed in a wide variety of physical systems governed by avalanche dynamics.

Spin-Hall effect and emergent antiferromagnetic phase transition in n-Si

NASA Astrophysics Data System (ADS)

Lou, Paul C.; Kumar, Sandeep

2018-04-01

Spin current experiences minimal dephasing and scattering in Si due to small spin-orbit coupling and spin-lattice interactions is the primary source of spin relaxation. We hypothesize that if the specimen dimension is of the same order as the spin diffusion length then spin polarization will lead to non-equilibrium spin accumulation and emergent phase transition. In n-Si, spin diffusion length has been reported up to 6 μm. The spin accumulation in Si will modify the thermal transport behavior of Si, which can be detected with thermal characterization. In this study, we report observation of spin-Hall effect and emergent antiferromagnetic phase transition behavior using magneto-electro-thermal transport characterization. The freestanding Pd (1 nm)/Ni80Fe20 (75 nm)/MgO (1 nm)/n-Si (2 μm) thin film specimen exhibits a magnetic field dependent thermal transport and spin-Hall magnetoresistance behavior attributed to Rashba effect. An emergent phase transition is discovered using self-heating 3ω method, which shows a diverging behavior at 270 K as a function of temperature similar to a second order phase transition. We propose that spin-Hall effect leads to the spin accumulation and resulting emergent antiferromagnetic phase transition. We propose that the length scale for Rashba effect can be equal to the spin diffusion length and two-dimensional electron gas is not essential for it. The emergent antiferromagnetic phase transition is attributed to the site inversion asymmetry in diamond cubic Si lattice.

Cyclic and Coherent States in Flocks with Topological Distance

NASA Astrophysics Data System (ADS)

Bhattacherjee, Biplab; Bhattacharya, Kunal; Manna, Subhrangshu

2014-01-01

A simple model of the two dimensional collective motion of a group of mobile agents have been studied. Like birds, these agents travel in open free space where each of them interacts with the first n neighbors determined by the topological distance with a free boundary condition. Using the same prescription for interactions used in the Vicsek model with scalar noise it has been observed that the flock, in absence of the noise, arrives at a number of interesting stationary states. One of the two most prominent states is the `single sink state' where the entire flock travels along the same direction maintaining perfect cohesion and coherence. The other state is the `cyclic state' where every individual agent executes a uniform circular motion, and the correlation among the agents guarantees that the entire flock executes a pulsating dynamics i.e., expands and contracts periodically between a minimum and a maximum size of the flock. We have studied another limiting situation when refreshing rate of the interaction zone is the fastest. In this case the entire flock gets fragmented into smaller clusters of different sizes. On introduction of scalar noise a crossover is observed when the agents cross over from a ballistic motion to a diffusive motion. Expectedly the crossover time is dependent on the strength of the noise η and diverges as η → 0. An even more simpler version of this model has been studied by suppressing the translational degrees of freedom of the agents but retaining their angular motion. Here agents are the spins, placed at the sites of a square lattice with periodic boundary condition. Every spin interacts with its n = 2, 3 or 4 nearest neighbors. In the stationary state the entire spin pattern moves as a whole when interactions are anisotropic with n = 2 and 3; but it is completely frozen when the interaction is isotropic with n=4$. These spin configu

Effect of Acceleration Frequency on Spatial Orientation Mechanisms

DTIC Science & Technology

2010-09-30

by aircraft, ground vehicle, and ship motion. Method. With controlled laboratory off-vertical axis rotation (OVAR), gaze reflexes respond to low...finding that vestibular gaze reflexes become altered at the same frequency where OVAR becomes most sickening will have important implications for...the collected data, a revised crossover rate of 0.42 Hz was extrapolated as the most probable spin frequency for inducing gaze reflex changes with the

Simultaneous First-Order Valence and Oxygen Vacancy Order/Disorder Transitions in (Pr 0.85 Y 0.15 ) 0.7 Ca 0.3 CoO 3-δ via Analytical Transmission Electron Microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gulec, Ahmet; Phelan, Daniel; Leighton, Chris

Perovskite cobaltites have been studied for years as some of the few solids to exhibit thermally driven spin-state crossovers. The unanticipated first-order spin and electronic transitions recently discovered in Pr-based cobaltites are notably different from these conventional crossovers, and are understood in terms of a unique valence transition. In essence, the Pr valence is thought to spontaneously shift from 3+ toward 4+ on cooling, driving subsequent transitions in Co valence and electronic/magnetic properties. Here, we apply temperature-dependent transmission electron microscopy and spectroscopy to study this phenomenon, for the first time with atomic spatial resolution, in the prototypical (Pr 0.85Y 0.15)(0.70)more » Ca 0.30CoO 3-δ. In addition to the direct spectroscopic observation of charge transfer between Pr and Co at the 165 K transition (on both the Pr and O edges), we also find a simultaneous order/disorder transition associated with O vacancies. Remarkably, the first-order valence change drives a transition between ordered and random O vacancies, at constant O vacancy density, demonstrating reversible crystallization of such vacancies even at cryogenic temperatures.« less

Weak Localization and Antilocalization in Topological Materials with Impurity Spin-Orbit Interactions

PubMed Central

Hankiewicz, Ewelina M.; Culcer, Dimitrie

2017-01-01

Topological materials have attracted considerable experimental and theoretical attention. They exhibit strong spin-orbit coupling both in the band structure (intrinsic) and in the impurity potentials (extrinsic), although the latter is often neglected. In this work, we discuss weak localization and antilocalization of massless Dirac fermions in topological insulators and massive Dirac fermions in Weyl semimetal thin films, taking into account both intrinsic and extrinsic spin-orbit interactions. The physics is governed by the complex interplay of the chiral spin texture, quasiparticle mass, and scalar and spin-orbit scattering. We demonstrate that terms linear in the extrinsic spin-orbit scattering are generally present in the Bloch and momentum relaxation times in all topological materials, and the correction to the diffusion constant is linear in the strength of the extrinsic spin-orbit. In topological insulators, which have zero quasiparticle mass, the terms linear in the impurity spin-orbit coupling lead to an observable density dependence in the weak antilocalization correction. They produce substantial qualitative modifications to the magnetoconductivity, differing greatly from the conventional Hikami-Larkin-Nagaoka formula traditionally used in experimental fits, which predicts a crossover from weak localization to antilocalization as a function of the extrinsic spin-orbit strength. In contrast, our analysis reveals that topological insulators always exhibit weak antilocalization. In Weyl semimetal thin films having intermediate to large values of the quasiparticle mass, we show that extrinsic spin-orbit scattering strongly affects the boundary of the weak localization to antilocalization transition. We produce a complete phase diagram for this transition as a function of the mass and spin-orbit scattering strength. Throughout the paper, we discuss implications for experimental work, and, at the end, we provide a brief comparison with transition metal dichalcogenides. PMID:28773167

Hyperfine interaction and its effects on spin dynamics in organic solids

NASA Astrophysics Data System (ADS)

Yu, Z. G.; Ding, Feizhi; Wang, Haobin

2013-05-01

Hyperfine interaction (HFI) and spin-orbit coupling are two major sources that affect electron spin dynamics. Here we present a systematic study of the HFI and its role in organic spintronic applications. For electron spin dynamics in disordered π-conjugated organics, the HFI can be characterized by an effective magnetic field whose modular square is a weighted sum of contact and dipolar contributions. We determine the effective HFI fields of some common π-conjugated organics studied in the literature via first-principles calculations. Most of them are found to be less than 2 mT. While the H atoms are the major source of the HFI in organics containing only the C and H atoms, many organics contain other nuclear spins, such as Al and N in tris-(8-hydroxyquinoline) aluminum, that contribute to the total HFI. Consequently, the deuteration effect on the HFI in the latter may be much weaker than in the former. The HFI gives rise to multiple resonance peaks in electron spin resonance. In disordered organic solids, these individual resonances are unresolved, leading to a broad peak whose width is proportional to the effective HFI field. As electrons hop among adjacent organic molecules, they experience a randomly varying local HFI field, inducing electron spin relaxation and diffusion. This is analyzed rigorously based on master equations. Electron spin relaxation undergoes a crossover along the ratio between the electron hopping rate η¯ and the Larmor frequency Ω of the HFI field. The spin relaxation rate increases (decreases) with η¯ when η¯≪Ω (η¯≫Ω). A coherent beating of electron spin at Ω is possible when the external field is small compared to the HFI. In this regime, the magnetic field is found to enhance the spin relaxation.

PREFACE: Dynamic crossover phenomena in water and other glass-forming liquids Dynamic crossover phenomena in water and other glass-forming liquids

NASA Astrophysics Data System (ADS)

Chen, Sow-Hsin; Baglioni, Piero

2012-02-01

This special section has been inspired by the workshop on Dynamic Crossover Phenomena in Water and Other Glass-Forming Liquids, held during November 11-13, 2010 at Pensione Bencistà, Fiesole, Italy, a well-preserved 14th century Italian villa tucked high in the hills overlooking Florence. The meeting, an assembly of world renowned scientists, was organized as a special occasion to celebrate the 75th birthday of Professor Sow-Hsin Chen of MIT, a pioneer in several aspects of complex fluids and soft matter physics. The workshop covered a large variety of experimental and theoretical research topics of current interest related to dynamic crossover phenomena in water and, more generally, in other glass-forming liquids. The 30 invited speakers/lecturers and approximately 60 participants were a select group of prominent physicists and chemists from the USA, Europe, Asia and Mexico, who are actively working in the field. Some highlights of this special issue include the following works. Professor Yamaguchi's group and their collaborators present a neutron spin echo study of the coherent intermediate scattering function of heavy water confined in cylindrical pores of MCM-41-C10 silica material in the temperature range 190-298 K. They clearly show that a fragile-to-strong (FTS) dynamic crossover occurs at about 225 K. They attribute the FTS dynamic crossover to the formation of a tetrahedral-like structure, which is preserved in the bulk-like water confined to the central part of the cylindrical pores. Mamontov and Kolesnikov et al study the collective excitations in an aqueous solution of lithium chloride over a temperature range of 205-270 K using neutron and x-ray Rayleigh-Brillouin (coherent) scattering. They detect both the low-frequency and the high-frequency sounds known to exist in pure bulk water above the melting temperature. They also perform neutron (incoherent) and x-ray (coherent) elastic intensity scan measurements. Clear evidence of the crossover in the dynamics of the water molecules in the solution is observed in the single-particle relaxational dynamics in the μeV (nanosecond) time scale, but not in the collective dynamics on the meV (picosecond) time scale. Mallamace et al discuss the dynamic crossover phenomenon in both bulk water and protein hydration water. They collect previous and new experimental data from different experimental techniques and molecular dynamic simulations, and are able to develop a unified picture for the different dynamical findings. Gallo et al present a MD study of confined water in MCM-41S-15 in order to test the applicability of Mode Coupling Theory (MCT) to the dynamics of the hydration water confined in the cylindrical pores of nominal diameter 15 Å. They find that the self dynamics of the hydration water is well described by MCT down to the crossover temperature TC. However, below TC the predictions of idealized MCT no longer apply, since hopping processes intervene and water turns into a strong liquid. Soper raises some questions as to the validity of the analysis method employed to determine the density of water confined in porous silica material MCM-41-S15 from recent neutron scattering experiments. Professors Stanley, Franzese and his collaborators describe an efficient Monte Carlo simulation of a coarse-grained model of water to study the phase diagram of a water monolayer confined in a fixed disordered matrix of hydrophobic nanoparticles between two hydrophobic plates. They find a drastic change of phase behavior of the confined water, such as shortening of the liquid-liquid phase transition line, upon increasing the concentration of the hydrophobic nano-particles. Sciortino and collaborators compute the equilibrium phase diagram of two simple models for patchy particles with three and five patches in a very broad range of pressure and temperature. The three-patch model produces a stable gas-liquid critical point. Yun Liu et al investigate, via small angle neutron scattering and neutron spin echo measurements, the effect of temperature on dynamic cluster formation of concentrated lysozyme solutions. Xin Li et al explore the use of the newly developed technique of spin echo small angle neutron scattering (SESANS) to investigate the structure of a colloid. They find the SESANS is able to resolve structural heterogeneity, at both intra- and inter-colloidal length scales. The choice of the topics and their elaboration reflects both the diversified current and past research interests of Professor Chen to whom this special section of Journal of Physics: Condensed Matter is dedicated. The issue contains papers from a substantial number of the invited speakers. The papers are arranged in the three categories of water, other glass-forming liquids, and colloids. It is our pleasure to thank all speakers, section chairs and participants who contributed to the great success of the workshop, and to all authors for their additional efforts in preparing their manuscripts. The scientific program of the workshop was organized by Professor Sow-Hsin Chen and Professor Piero Baglioni. The meeting was only possible with the generous financial support of the Consorzio per lo Sviluppo dei Sistemi a Grande Interfase (CSGI) and the University of Florence, Italy. Finally, we express our warmest gratitude to all the members of the local organizing committee and to the staff of the CSGI for all their assistance and great efforts in organizing this meeting. Dynamic crossover phenomena in water and other glass-forming liquids contents Water Neutron spin echo measurements of monolayer and capillary condensed water in MCM-41 at low temperaturesK Yoshida, T Yamaguchi, S Kittaka, M-C Bellissent-Funel and P Fouquet Water dynamics in a lithium chloride aqueous solution probed by Brillouin neutron and x-ray scatteringE Mamontov, A De Francesco, F Formisano, A Laloni, L Sani, B M Leu, A H Said and A I Kolesnikov The dynamical crossover phenomenon in bulk water, confined water and protein hydration water Francesco Mallamace, Carmelo Corsaro, Piero Baglioni, Emiliano Fratini and Sow-Hsin Chen Common features in the microscopic dynamics of hydration water on organic and inorganic surfacesE Mamontov, H O'Neill, Q Zhang, W Wang and D J Wesolowski Water dynamics as affected by interaction with biomolecules and change of thermodynamic state: a neutron scattering studyA Orecchini, A Paciaroni, C Petrillo, F Sebastiani, A De Francesco and F Sacchetti Temperature dependence of structure and density for D2O confined in MCM-41-SWilliam A Kamitakahara, Antonio Faraone, Kao-Hsiang Liu and Chung-Yuan Mou Density profile of water confined in cylindrical pores in MCM-41 silicaAlan K Soper Dynamic crossover in hydration water of curing cement paste: the effect of superplasticizerHua Li, Wei-Shan Chiang, Emiliano Fratini, Francesca Ridi, Francesco Bausi, Piero Baglioni, Madhu Tyagi and Sow-Hsin Chen Water confined in MCM-41: a mode coupling theory analysisP Gallo, M Rovere and S-H Chen Computer simulations of dynamic crossover phenomena in nanoconfined waterG B Suffritti, P Demontis, J Gulín-Gonźlez and M Masia Hydrophobic nanoconfinement suppresses fluctuations in supercooled waterE G Strekalova, M G Mazza, H E Stanley and G Franzese Other glass-forming liquids Quasi-elastic neutron scattering studies of the slow dynamics of supercooled and glassy aspirinYang Zhang, Madhusudan Tyagi, Eugene Mamontov and Sow-Hsin Chen Colloids Phase diagram of trivalent and pentavalent patchy particlesFlavio Romano, Eduardo Sanz, Piero Tartaglia and Francesco Sciortino Distinguishing the monomer to cluster phase transition in concentrated lysozyme solutions by studying the temperature dependence of the short-time dynamicsPéter Falus, Lionel Porcar, Emiliano Fratini, Wei-Ren Chen, Antonio Faraone, Kunlun Hong, Piero Baglioni and Yun Liu Contrast variation in spin-echo small angle neutron scatteringXin Li, Bin Wu, Yun Liu, Roger Pynn, Chwen-Yang Shew, Gregory S Smith, Kenneth W Herwig, J Lee Robertson, Wei-Ren Chen and Li Liu Structural response of polyelectrolyte dendrimer towards molecular protonation: the inconsistency revealed by SANS and NMRKunlun Hong, Yun Liu, Lionel Porcar, Dazhi Liu, Carrie Y Gao, Gregory S Smith, Kenneth W Herwig, Sheng Cai, Xin Li, Bin Wu, Wei-Ren Chen and Li Liu

Mean-field Ising crossover and the critical exponents γ, ν, and η for a polymer blend: d-PB/PS studied by small-angle neutron scattering

NASA Astrophysics Data System (ADS)

Janssen, S.; Schwahn, D.; Springer, T.

1992-05-01

The critical behavior of the polymer blend d-PB/PS was investigated by small-angle neutron scattering experiments. 3D Ising behavior was clearly observed with the critical exponents γ=1.26+/-0.01, ν=0.59+/-0.01, and η=0.047+/-0.004. The crossover to mean-field behavior occurs at T*=Tc+5.4 K. This is compared with the results of other experiments and the Landau-Ginzburg criterion. The Q dependence of the structure factor S(Q) follows the Ornstein-Zernike form in both regimes.

Superaging and Subaging Phenomena in a Nonequilibrium Critical Behavior of the Structurally Disordered Two-Dimensional XY Model

NASA Astrophysics Data System (ADS)

Prudnikov, V. V.; Prudnikov, P. V.; Popov, I. S.

2018-03-01

A Monte Carlo numerical simulation of the specific features of nonequilibrium critical behavior is carried out for the two-dimensional structurally disordered XY model during its evolution from a low-temperature initial state. On the basis of the analysis of the two-time dependence of autocorrelation functions and dynamic susceptibility for systems with spin concentrations of p = 1.0, 0.9, and 0.6, aging phenomena characterized by a slowing down of the relaxation system with increasing waiting time and the violation of the fluctuation-dissipation theorem (FDT) are revealed. The values of the universal limiting fluctuation-dissipation ratio (FDR) are obtained for the systems considered. As a result of the analysis of the two-time scaling dependence for spin-spin and connected spin autocorrelation functions, it is found that structural defects lead to subaging phenomena in the behavior of the spin-spin autocorrelation function and superaging phenomena in the behavior of the connected spin autocorrelation function.

Demonstration of simultaneous experiments using thin crystal multiplexing at the Linac Coherent Light Source

DOE PAGES

Feng, Y.; Alonso-Mori, R.; Barends, T. R. M.; ...

2015-04-10

Multiplexing of the Linac Coherent Light Source beam was demonstrated for hard X-rays by spectral division using a near-perfect diamond thin-crystal monochromator operating in the Bragg geometry. The wavefront and coherence properties of both the reflected and transmitted beams were well preserved, thus allowing simultaneous measurements at two separate instruments. In this report, the structure determination of a prototypical protein was performed using serial femtosecond crystallography simultaneously with a femtosecond time-resolved XANES studies of photoexcited spin transition dynamics in an iron spin-crossover system. The results of both experiments using the multiplexed beams are similar to those obtained separately, using amore » dedicated beam, with no significant differences in quality.« less

A parametric study of the behavior of the angular momentum vector during spin rate changes of rigid body spacecraft

NASA Technical Reports Server (NTRS)

Longuski, J. M.

1982-01-01

During a spin-up or spin-down maneuver of a spinning spacecraft, it is usual to have not only a constant body-fixed torque about the desired spin axis, but also small undesired constant torques about the transverse axes. This causes the orientation of the angular momentum vector to change in inertial space. Since an analytic solution is available for the angular momentum vector as a function of time, this behavior can be studied for large variations of the dynamic parameters, such as the initial spin rate, the inertial properties and the torques. As an example, the spin-up and spin-down maneuvers of the Galileo spacecraft was studied and as a result, very simple heuristic solutions were discovered which provide very good approximations to the parametric behavior of the angular momentum vector orientation.

Effects of coarse-graining on the scaling behavior of long-range correlated and anti-correlated signals.

PubMed

Xu, Yinlin; Ma, Qianli D Y; Schmitt, Daniel T; Bernaola-Galván, Pedro; Ivanov, Plamen Ch

2011-11-01

We investigate how various coarse-graining (signal quantization) methods affect the scaling properties of long-range power-law correlated and anti-correlated signals, quantified by the detrended fluctuation analysis. Specifically, for coarse-graining in the magnitude of a signal, we consider (i) the Floor, (ii) the Symmetry and (iii) the Centro-Symmetry coarse-graining methods. We find that for anti-correlated signals coarse-graining in the magnitude leads to a crossover to random behavior at large scales, and that with increasing the width of the coarse-graining partition interval Δ, this crossover moves to intermediate and small scales. In contrast, the scaling of positively correlated signals is less affected by the coarse-graining, with no observable changes when Δ < 1, while for Δ > 1 a crossover appears at small scales and moves to intermediate and large scales with increasing Δ. For very rough coarse-graining (Δ > 3) based on the Floor and Symmetry methods, the position of the crossover stabilizes, in contrast to the Centro-Symmetry method where the crossover continuously moves across scales and leads to a random behavior at all scales; thus indicating a much stronger effect of the Centro-Symmetry compared to the Floor and the Symmetry method. For coarse-graining in time, where data points are averaged in non-overlapping time windows, we find that the scaling for both anti-correlated and positively correlated signals is practically preserved. The results of our simulations are useful for the correct interpretation of the correlation and scaling properties of symbolic sequences.

Effects of coarse-graining on the scaling behavior of long-range correlated and anti-correlated signals

PubMed Central

Xu, Yinlin; Ma, Qianli D.Y.; Schmitt, Daniel T.; Bernaola-Galván, Pedro; Ivanov, Plamen Ch.

2014-01-01

We investigate how various coarse-graining (signal quantization) methods affect the scaling properties of long-range power-law correlated and anti-correlated signals, quantified by the detrended fluctuation analysis. Specifically, for coarse-graining in the magnitude of a signal, we consider (i) the Floor, (ii) the Symmetry and (iii) the Centro-Symmetry coarse-graining methods. We find that for anti-correlated signals coarse-graining in the magnitude leads to a crossover to random behavior at large scales, and that with increasing the width of the coarse-graining partition interval Δ, this crossover moves to intermediate and small scales. In contrast, the scaling of positively correlated signals is less affected by the coarse-graining, with no observable changes when Δ < 1, while for Δ > 1 a crossover appears at small scales and moves to intermediate and large scales with increasing Δ. For very rough coarse-graining (Δ > 3) based on the Floor and Symmetry methods, the position of the crossover stabilizes, in contrast to the Centro-Symmetry method where the crossover continuously moves across scales and leads to a random behavior at all scales; thus indicating a much stronger effect of the Centro-Symmetry compared to the Floor and the Symmetry method. For coarse-graining in time, where data points are averaged in non-overlapping time windows, we find that the scaling for both anti-correlated and positively correlated signals is practically preserved. The results of our simulations are useful for the correct interpretation of the correlation and scaling properties of symbolic sequences. PMID:25392599

A feasibility study of developing toroidal tanks for a spinning spacecraft. Part 2: Evaluation of fluid behavior in spinning toroidal tanks

NASA Technical Reports Server (NTRS)

Anderson, J. E.

1974-01-01

An experimental program was conducted for the purpose of evaluating propellant behavior characteristics in spinning toroidal tanks. The effects of typical mission requirements, and related phenomena upon propellant slosh and settling, and orientation and stability of the ullage were investigated in a subscale model tank under both one-g and low-g acceleration environments. Specific conditions included were axial acceleration, spin rate, spinrate change, and spacecraft wobble, both singly and in combination. Methanol and water in combination with appropriate spin-rates and accelerations of the scale model system were used to simulate the behavior of fluorine, nitrogen tetroxide, monomethylhydrazine, and hydrazine. The experimental results indicate that no major fluid behavior problems would be encountered with the use of toroidal tanks containing any of the four propellants in a proposed spin-stabilized orbiter spacecraft.

Work-family enrichment, work-family conflict, and marital satisfaction: a dyadic analysis.

PubMed

van Steenbergen, Elianne F; Kluwer, Esther S; Karney, Benjamin R

2014-04-01

This study was designed to examine whether spouses' work-to-family (WF) enrichment experiences account for their own and their partner's marital satisfaction, beyond the effects of WF conflict. Data were collected from both partners of 215 dual-earner couples with children. As hypothesized, structural equation modeling revealed that WF enrichment experiences accounted for variance in individuals' marital satisfaction, over and above WF conflict. In line with our predictions, this positive link between individuals' WF enrichment and their marital satisfaction was mediated by more positive marital behavior, and more positive perceptions of the partner's behavior. Furthermore, evidence for crossover was found. Husbands who experienced more WF enrichment were found to show more marital positivity (according to their wives), which related to increased marital satisfaction in their wives. No evidence of such a crossover effect from wives to husbands was found. The current findings not only highlight the added value of studying positive spillover and crossover effects of work into the marriage, but also suggest that positive spillover and crossover effects on marital satisfaction might be stronger than negative spillover and crossover are. These results imply that organizational initiatives of increasing job enrichment may make employees' marital life happier and can contribute to a happy, healthy, and high-performing workforce.

Dynamic crossover in deeply cooled water confined in MCM-41 at 4 kbar and its relation to the liquid-liquid transition hypothesis

NASA Astrophysics Data System (ADS)

Wang, Zhe; Le, Peisi; Ito, Kanae; Leão, Juscelino B.; Tyagi, Madhusudan; Chen, Sow-Hsin

2015-09-01

With quasi-elastic neutron scattering, we study the single-particle dynamics of the water confined in a hydrophilic silica material, MCM-41, at 4 kbar. A dynamic crossover phenomenon is observed at 219 K. We compare this dynamic crossover with the one observed at ambient pressure and find that (a) above the crossover temperature, the temperature dependence of the characteristic relaxation time at ambient pressure exhibits a more evident super-Arrhenius behavior than that at 4 kbar. Especially, at temperatures below about 230 K, the relaxation time at 4 kbar is even smaller than that at ambient pressure. This feature is different from many other liquids. (b) Below the crossover temperature, the Arrhenius behavior found at ambient pressure has a larger activation energy compared to the one found at 4 kbar. We ascribe the former to the difference between the local structure of the low-density liquid (LDL) phase and that of the high-density liquid (HDL) phase, and the latter to the difference between the strength of the hydrogen bond of the LDL and that of the HDL. Therefore, we conclude that the phenomena observed in this paper are consistent with the LDL-to-HDL liquid-liquid transition hypothesis.

Dynamic crossover in deeply cooled water confined in MCM-41 at 4 kbar and its relation to the liquid-liquid transition hypothesis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Zhe; Le, Peisi; Ito, Kanae

With quasi-elastic neutron scattering, we study the single-particle dynamics of the water confined in a hydrophilic silica material, MCM-41, at 4 kbar. A dynamic crossover phenomenon is observed at 219 K. We compare this dynamic crossover with the one observed at ambient pressure and find that (a) above the crossover temperature, the temperature dependence of the characteristic relaxation time at ambient pressure exhibits a more evident super-Arrhenius behavior than that at 4 kbar. Especially, at temperatures below about 230 K, the relaxation time at 4 kbar is even smaller than that at ambient pressure. This feature is different from manymore » other liquids. (b) Below the crossover temperature, the Arrhenius behavior found at ambient pressure has a larger activation energy compared to the one found at 4 kbar. We ascribe the former to the difference between the local structure of the low-density liquid (LDL) phase and that of the high-density liquid (HDL) phase, and the latter to the difference between the strength of the hydrogen bond of the LDL and that of the HDL. Therefore, we conclude that the phenomena observed in this paper are consistent with the LDL-to-HDL liquid-liquid transition hypothesis.« less

Prescription Drug Use among College Students: A Test of Criminal Spin Theory

ERIC Educational Resources Information Center

Lin, Wan-Chun

2017-01-01

Criminal spin theory developed by Ronel intends to provide a more comprehensive explanation of criminal behavior. It includes wide-ranging factors that impact human behavior at an individual, group, and cultural level. According to criminal spin theory, an event or a set of events can impact human emotions, thoughts, and behaviors. With the…

Visualizing the BEC-BCS crossover in a two-dimensional Fermi gas: Pairing gaps and dynamical response functions from ab initio computations

NASA Astrophysics Data System (ADS)

Vitali, Ettore; Shi, Hao; Qin, Mingpu; Zhang, Shiwei

2017-12-01

Experiments with ultracold atoms provide a highly controllable laboratory setting with many unique opportunities for precision exploration of quantum many-body phenomena. The nature of such systems, with strong interaction and quantum entanglement, makes reliable theoretical calculations challenging. Especially difficult are excitation and dynamical properties, which are often the most directly relevant to experiment. We carry out exact numerical calculations, by Monte Carlo sampling of imaginary-time propagation of Slater determinants, to compute the pairing gap in the two-dimensional Fermi gas from first principles. Applying state-of-the-art analytic continuation techniques, we obtain the spectral function and the density and spin structure factors providing unique tools to visualize the BEC-BCS crossover. These quantities will allow for a direct comparison with experiments.

Structure and thermodynamic properties of (C5H12N)CuBr3: a new weakly coupled antiferromagnetic spin-1/2 chain complex lying in the 1D-3D dimensional cross-over regime.

PubMed

Pan, Bingying; Wang, Yang; Zhang, Lijuan; Li, Shiyan

2014-04-07

Single crystals of a metal organic complex (C5H12N)CuBr3 (C5H12N = piperidinium, pipH for short) have been synthesized, and the structure was determined by single-crystal X-ray diffraction. (pipH)CuBr3 crystallizes in the monoclinic group C2/c. Edging-sharing CuBr5 units link to form zigzag chains along the c axis, and the neighboring Cu(II) ions with spin-1/2 are bridged by bibromide ions. Magnetic susceptibility data down to 1.8 K can be well fitted by the Bonner-Fisher formula for the antiferromagnetic spin-1/2 chain, giving the intrachain magnetic coupling constant J ≈ -17 K. At zero field, (pipH)CuBr3 shows three-dimensional (3D) order below TN = 1.68 K. Calculated by the mean-field theory, the interchain coupling constant J' = -0.91 K is obtained and the ordered magnetic moment m0 is about 0.23 μB. This value of m0 makes (pipH)CuBr3 a rare compound suitable to study the 1D-3D dimensional cross-over problem in magnetism, since both 3D order and one-dimensional (1D) quantum fluctuations are prominent. In addition, specific heat measurements reveal two successive magnetic transitions with lowering temperature when external field μ0H ≥ 3 T is applied along the a' axis. The μ0H-T phase diagram of (pipH)CuBr3 is roughly constructed.

Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO) 5 to Fe(CO) 4EtOH

DOE PAGES

Kunnus, K.; Josefsson, I.; Rajkovic, I.; ...

2016-02-09

We utilized femtosecond time-resolved resonant inelastic X-ray scattering and ab initio theory to study the transient electronic structure and the photoinduced molecular dynamics of a model metal carbonyl photocatalyst Fe(CO) 5 in ethanol solution. We propose mechanistic explanation for the parallel ultrafast intra-molecular spin crossover and ligation of the Fe(CO) 4 which are observed following a charge transfer photoexcitation of Fe(CO) 5 as reported in our previous study [Wernet et al., Nature 520, 78 (2015)]. We find that branching of the reaction pathway likely happens in the 1A 1 state of Fe(CO) 4. A sub-picosecond time constant of themore » spin crossover from 1B 2 to 3B 2 is rationalized by the proposed 1B 2 → 1A 1 → 3B 2 mechanism. Ultrafast ligation of the 1B 2 Fe(CO) 4 state is significantly faster than the spin-forbidden and diffusion limited ligation process occurring from the 3B 2 Fe(CO) 4 ground state that has been observed in the previous studies. We propose that the ultrafast ligation occurs via 1B 2 → 1A 1 → 1A' Fe(CO) 4EtOH pathway and the time scale of the 1A 1 Fe(CO) 4 state ligation is governed by the solute-solvent collision frequency. In conclusion, our study emphasizes the importance of understanding the interaction of molecular excited states with the surrounding environment to explain the relaxation pathways of photoexcited metal carbonyls in solution.« less

Cobalt spin states and hyperfine interactions in LaCoO3 investigated by LDA+U calculations

NASA Astrophysics Data System (ADS)

Leighton, C.; Hsu, H.; Blaha, P.; Wentzcovitch, R. M.

2010-12-01

The spin states of cobalt ions in the bulk and epitaxial-thin-film lanthanum cobaltite (LaCoO3) have been controversial for years. The controversial point is mainly the presence of intermediate-spin (IS) Co in the temperature range of 0-85 K. In this region, bulk LaCoO3 experiences a crossover from a diamagnetic to a paramagnetic phase, and the thin-film LaCoO3 is ferromagnetic and insulator. An approach to probe the Co spin state is thus of interest. With a series of LDA+U calculations, we have demonstrated that the electric field gradient (EFG) at the Co nucleus can be used as a fingerprint to identify the spin state of the Co ion in each case. Therefore, in principle, the spin state of the Co ion can be unambiguously determined from nuclear magnetic resonance (NMR) spectra. Our calculations also suggest that the presence of IS Co in this temperature range is unlikely, based not only on its relatively higher energy, but also on its associated conducting band structure incompatible with the measured insulating conductivity. This work was primarily supported by the MRSEC Program of NSF under Awards Number DMR-0212302 and DMR-0819885, and partially supported by NSF under ATM-0428774 (V-Lab), EAR-1019853, and EAR-0810272. The computations were performed mainly at the Minnesota Supercomputing Institute (MSI).

Competition of mesoscales and crossover to theta-point tricriticality in near-critical polymer solutions.

PubMed

Anisimov, M A; Kostko, A F; Sengers, J V; Yudin, I K

2005-10-22

The approach to asymptotic critical behavior in polymer solutions is governed by a competition between the correlation length of critical fluctuations diverging at the critical point of phase separation and an additional mesoscopic length scale, the radius of gyration. In this paper we present a theory for crossover between two universal regimes: a regime with Ising (fluctuation-induced) asymptotic critical behavior, where the correlation length prevails, and a mean-field tricritical regime with theta-point behavior controlled by the mesoscopic polymer chain. The theory yields a universal scaled description of existing experimental phase-equilibria data and is in excellent agreement with our light-scattering experiments on polystyrene solutions in cyclohexane with polymer molecular weights ranging from 2 x 10(5) up to 11.4 x 10(6). The experiments demonstrate unambiguously that crossover to theta-point tricriticality is controlled by a competition of the two mesoscales. The critical amplitudes deduced from our experiments depend on the polymer molecular weight as predicted by de Gennes [Phys. Lett. 26A, 313 (1968)]. Experimental evidence for the presence of logarithmic corrections to mean-field tricritical theta-point behavior in the molecular-weight dependence of the critical parameters is also presented.

Relationship Between Unusual High-Temperature Fatigue Crack Growth Threshold Behavior in Superalloys and Sudden Failure Mode Transitions

NASA Technical Reports Server (NTRS)

Telesman, J.; Smith, T. M.; Gabb, T. P.; Ring, A. J.

2017-01-01

An investigation of high temperature cyclic fatigue crack growth (FCG) threshold behavior of two advanced nickel disk alloys was conducted. The focus of the study was the unusual crossover effect in the near-threshold region of these type of alloys where conditions which produce higher crack growth rates in the Paris regime, produce higher resistance to crack growth in the near threshold regime. It was shown that this crossover effect is associated with a sudden change in the fatigue failure mode from a predominant transgranular mode in the Paris regime to fully intergranular mode in the threshold fatigue crack growth region. This type of a sudden change in the fracture mechanisms has not been previously reported and is surprising considering that intergranular failure is typically associated with faster crack growth rates and not the slow FCG rates of the near-threshold regime. By characterizing this behavior as a function of test temperature, environment and cyclic frequency, it was determined that both the crossover effect and the onset of intergranular failure are caused by environmentally driven mechanisms which have not as yet been fully identified. A plausible explanation for the observed behavior is proposed.

Genetic Recombination at the Buff Spore Color Locus in SORDARIA BREVICOLLIS. II. Analysis of Flanking Marker Behavior in Crosses between Buff Mutants.

PubMed

Sang, H; Whitehouse, H L

1983-02-01

Aberrant asci containing one or more wild-type spores were selected from crosses between pairs of alleles of the buff locus in the presence of closely linked flanking markers. Data were obtained relating to the site of aberrant segregation and the position of any associated crossover giving recombination of flanking markers. Aberrant segregation at a proximal site within the buff gene may be associated with a crossover proximal to the site of aberrant segregation or, with equal frequency, with a crossover distal to the site of the second mutant present in the cross. Similarly, segregation at a distal site may be associated with a crossover distal to the site or, with lower frequency, with a crossover proximal to the site of the proximal mutant present in the cross. Crossovers between the alleles were rare. This evidence for the relationship between hybrid DNA and crossing over is discussed in terms of current models for the mechanism of recombination.

Mixed-Spin Diamond Chain Cu2FePO4F4(H2O)4 with a Noncollinear Spin Order and Possible Successive Phase Transitions.

PubMed

Lu, Hongcheng; Hayashi, Naoaki; Matsumoto, Yuki; Takatsu, Hiroshi; Kageyama, Hiroshi

2017-08-07

A diamond spin chain system, one of the one-dimensional frustrated lattices, is known to exhibit novel properties, but experimental studies have been exclusively confined to materials with a single spin component. Here, we report on the synthesis, structure, and magnetic properties of a new diamond chain compound Cu 2 FePO 4 F 4 (H 2 O) 4 1 composed of mixed-spins of Cu 2+ (S = 1/2 × 2) and Fe 3+ (S = 5/2). Compound 1 crystallizes in the space group C2/c of the monoclinic crystal system with a = 7.7546(4) Å, b = 12.1290(6) Å, c = 9.9209(6) Å, β = 105.29(1)°, and Z = 4. DC magnetization, Mössbauer spectroscopy, and heat capacity measurements revealed an antiferromagnetic order at 11.3 K with a small ferromagnetic component. It is suggested that ferrimagnetic diamond chains are arranged in an antiferromagnetic fashion (i.e., [...Fe(↑)-2Cu(↓↓)-Fe(↑)...] and [...Fe(↓)-2Cu(↑↑)-Fe(↓)...]) within the ab plane to cancel net magnetization, and the spin orientation of the diamond chains changes alternately along the c axis due to the magnetic anisotropy, leading to a noncollinear spin order. Furthermore, another anomaly is observed in the heat capacity at around 3 K, suggesting a successive magnetic transition or crossover due to competing magnetic interactions.

Spin-resolved electron waiting times in a quantum-dot spin valve

NASA Astrophysics Data System (ADS)

Tang, Gaomin; Xu, Fuming; Mi, Shuo; Wang, Jian

2018-04-01

We study the electronic waiting-time distributions (WTDs) in a noninteracting quantum-dot spin valve by varying spin polarization and the noncollinear angle between the magnetizations of the leads using the scattering matrix approach. Since the quantum-dot spin valve involves two channels (spin up and down) in both the incoming and outgoing channels, we study three different kinds of WTDs, which are two-channel WTD, spin-resolved single-channel WTD, and cross-channel WTD. We analyze the behaviors of WTDs in short times, correlated with the current behaviors for different spin polarizations and noncollinear angles. Cross-channel WTD reflects the correlation between two spin channels and can be used to characterize the spin-transfer torque process. We study the influence of the earlier detection on the subsequent detection from the perspective of cross-channel WTD, and define the influence degree quantity as the cumulative absolute difference between cross-channel WTDs and first-passage time distributions to quantitatively characterize the spin-flip process. We observe that influence degree versus spin-transfer torque for different noncollinear angles as well as different polarizations collapse into a single curve showing universal behaviors. This demonstrates that cross-channel WTDs can be a pathway to characterize spin correlation in spintronics system.

Turbulent drag reduction by flexible and rodlike polymers: Crossover effects at small concentrations.

PubMed

Ching, Emily S C; Lo, T S; Procaccia, Itamar

2006-08-01

Drag reduction by polymers is bounded between two universal asymptotes, the von Kármán log law of the law and the maximum drag reduction (MDR) asymptote. It is theoretically understood why the MDR asymptote is universal, independent of whether the polymers are flexible or rodlike. The crossover behavior from the Newtonian von Kármán log law to the MDR is, however, not universal, showing different characteristics for flexible and rodlike polymers. In this paper we provide a theory for this crossover phenomenology.

ESR evidence for 2 coexisting liquid phases in deeply supercooled bulk water

PubMed Central

Banerjee, D.; Bhat, S. N.; Bhat, S. V.; Leporini, D.

2009-01-01

Using electron spin resonance spectroscopy (ESR), we measure the rotational mobility of probe molecules highly diluted in deeply supercooled bulk water and negligibly constrained by the possible ice fraction. The mobility increases above the putative glass transition temperature of water, Tg = 136 K, and smoothly connects to the thermodynamically stable region by traversing the so called “no man's land” (the range 150–235 K), where it is believed that the homogeneous nucleation of ice suppresses the liquid water. Two coexisting fractions of the probe molecules are evidenced. The 2 fractions exhibit different mobility and fragility; the slower one is thermally activated (low fragility) and is larger at low temperatures below a fragile-to-strong dynamic cross-over at ≈225 K. The reorientation of the probe molecules decouples from the viscosity below ≈225 K. The translational diffusion of water exhibits a corresponding decoupling at the same temperature [Chen S-H, et al. (2006) The violation of the Stokes–Einstein relation in supercooled water. Proc Natl Acad Sci USA 103:12974–12978]. The present findings are consistent with key issues concerning both the statics and the dynamics of supercooled water, namely the large structural fluctuations [Poole PH, Sciortino F, Essmann U, Stanley HE (1992) Phase behavior of metastable water. Nature 360:324–328] and the fragile-to-strong dynamic cross-over at ≈228 K [Ito K, Moynihan CT, Angell CA (1999) Thermodynamic determination of fragility in liquids and a fragile-to-strong liquid transition in water. Nature 398:492–494]. PMID:19556546

Pressure Induced Iron Spin Crossover in MgGeO3 Perovskite and Post-perovskite

NASA Astrophysics Data System (ADS)

Wentzcovitch, R. M.; Shukla, G.; Topsakal, M.

2014-12-01

MgGeO3-perovskite is known to be a low-pressure analog of MgSiO3-perovskite in many respects, but especially in regard to the post-perovskite transition. As such, investigation of spin state changes in Fe-bearing MgGeO3 might help to clarify some aspects of this type of state change in Fe-bearing MgSiO3. Using DFT+U calculations, we have investigated pressure induced state changes in Fe-bearing MgGeO3 perovskite and post-perovskite. Owing to the relatively larger atomic size of germanium compared to silicon, germanate phases have larger unit cell volume and interatomic distances than equivalent silicate phases at same pressures. As a result, all pressure induced state changes in iron occur at higher pressures in germanate phases than in the silicate ones, be it a spin state change or position change of (ferrous) iron in the perovskite cage. The effect of iron in the post-perovskite transition is also investigated.

Chemical trend of exchange coupling in diluted magnetic II-VI semiconductors: Ab initio calculations

NASA Astrophysics Data System (ADS)

Chanier, T.; Virot, F.; Hayn, R.

2009-05-01

We have calculated the chemical trend of magnetic exchange parameters ( Jdd , Nα , and Nβ ) of Zn-based II-VI semiconductors ZnA ( A=O , S, Se, and Te) doped with Co or Mn. We show that a proper treatment of electron correlations by the local spin-density approximation (LSDA)+U method leads to good agreement between experimental and theoretical values of the nearest-neighbor exchange coupling Jdd between localized 3d spins in contrast to the LSDA method. The exchange couplings between localized spins and doped electrons in the conduction band Nα are in good agreement with experiment as well. But the values for Nβ (coupling to doped holes in the valence band) indicate a crossover from weak coupling (for A=Te and Se) to strong coupling (for A=O ) and a localized hole state in ZnO:Mn. This hole localization explains the apparent discrepancy between photoemission and magneto-optical data for ZnO:Mn.

Finite-temperature dynamics of the Mott insulating Hubbard chain

NASA Astrophysics Data System (ADS)

Nocera, Alberto; Essler, Fabian H. L.; Feiguin, Adrian E.

2018-01-01

We study the dynamical response of the half-filled one-dimensional Hubbard model for a range of interaction strengths U and temperatures T by a combination of numerical and analytical techniques. Using time-dependent density matrix renormalization group computations we find that the single-particle spectral function undergoes a crossover to a spin-incoherent Luttinger liquid regime at temperatures T ˜J =4 t2/U for sufficiently large U >4 t . At smaller values of U and elevated temperatures the spectral function is found to exhibit two thermally broadened bands of excitations, reminiscent of what is found in the Hubbard-I approximation. The dynamical density-density response function is shown to exhibit a finite-temperature resonance at low frequencies inside the Mott gap, with a physical origin similar to the Villain mode in gapped quantum spin chains. We complement our numerical computations by developing an analytic strong-coupling approach to the low-temperature dynamics in the spin-incoherent regime.

Observation of multicellular spinning behavior of Proteus mirabilis by atomic force microscopy and multifunctional microscopy.

PubMed

Liu, Yanxia; Deng, Yuanxin; Luo, Shuxiu; Deng, Yu; Guo, Linming; Xu, Weiwei; Liu, Lei; Liu, Junkang

2014-01-01

This study aimed to observe the multicellular spinning behavior of Proteus mirabilis by atomic force microscopy (AFM) and multifunctional microscopy in order to understand the mechanism underlying this spinning movement and its biological significance. Multifunctional microscopy with charge-coupled device (CCD) and real-time AFM showed changes in cell structure and shape of P. mirabilis during multicellular spinning movement. Specifically, the morphological characteristics of P. mirabilis, multicellular spinning dynamics, and unique movement were observed. Our findings indicate that the multicellular spinning behavior of P. mirabilis may be used to collect nutrients, perform colonization, and squeeze out competitors. The movement characteristics of P. mirabilis are vital to the organism's biological adaptability to the surrounding environment. Copyright © 2013 Elsevier Ltd. All rights reserved.

Breakdown of single spin-fluid model in the heavily hole-doped superconductor CsFe2As2

NASA Astrophysics Data System (ADS)

Zhao, D.; Li, S. J.; Wang, N. Z.; Li, J.; Song, D. W.; Zheng, L. X.; Nie, L. P.; Luo, X. G.; Wu, T.; Chen, X. H.

2018-01-01

Although Fe-based superconductors are correlated electronic systems with multiorbital, previous nuclear magnetic resonance (NMR) measurement suggests that a single spin-fluid model is sufficient to describe its spin behavior. Here, we first observed the breakdown of single spin-fluid model in a heavily hole-doped Fe-based superconductor CsFe2As2 by site-selective NMR measurement. At high-temperature regime, both Knight shift and nuclear spin-lattice relaxation at 133Cs and 75As nuclei exhibit distinct temperature-dependent behavior, suggesting the breakdown of the single spin-fluid model in CsFe2As2 . This is ascribed to the coexistence of both localized and itinerant spin degree of freedom at 3 d orbitals, which is consistent with the orbital-selective Mott phase. With decreasing temperature, the single spin-fluid behavior is recovered below T*˜75 K due to a coherent state among 3 d orbitals. The Kondo liquid scenario is proposed to understand the low-temperature coherent state.

Dynamical arrest with zero complexity: The unusual behavior of the spherical Blume-Emery-Griffiths disordered model

NASA Astrophysics Data System (ADS)

Rainone, Corrado; Ferrari, Ulisse; Paoluzzi, Matteo; Leuzzi, Luca

2015-12-01

The short- and long-time dynamics of model systems undergoing a glass transition with apparent inversion of Kauzmann and dynamical arrest glass transition lines is investigated. These models belong to the class of the spherical mean-field approximation of a spin-1 model with p -body quenched disordered interaction, with p >2 , termed spherical Blume-Emery-Griffiths models. Depending on temperature and chemical potential the system is found in a paramagnetic or in a glassy phase and the transition between these phases can be of a different nature. In specific regions of the phase diagram coexistence of low-density and high-density paramagnets can occur, as well as the coexistence of spin-glass and paramagnetic phases. The exact static solution for the glassy phase is known to be obtained by the one-step replica symmetry breaking ansatz. Different scenarios arise for both the dynamic and the thermodynamic transitions. These include: (i) the usual random first-order transition (Kauzmann-like) for mean-field glasses preceded by a dynamic transition, (ii) a thermodynamic first-order transition with phase coexistence and latent heat, and (iii) a regime of apparent inversion of static transition line and dynamic transition lines, the latter defined as a nonzero complexity line. The latter inversion, though, turns out to be preceded by a dynamical arrest line at higher temperature. Crossover between different regimes is analyzed by solving mode-coupling-theory equations near the boundaries of paramagnetic solutions and the relationship with the underlying statics is discussed.

Evaluation of fluid behavior in spinning toroidal tanks

NASA Technical Reports Server (NTRS)

Anderson, J. E.; Fester, D. A.; Dugan, D. W.

1976-01-01

An experimental study was conducted to evaluate propellant behavior in spinning toroidal tanks that could be used in a retro-propulsion system of an advanced outer-planet Pioneer orbiter. Information on propellant slosh and settling and on ullage orientation and stability was obtained. The effects of axial acceleration, spin rate, spin rate change, and spacecraft wobble, both singly and in combination, were evaluated using a 1/8-scale transparent tank in one-g and low-g environments. Liquid loadings ranged from 5% to 96% full. The impact of a surface tension acquisition device was assessed. Testing simulated the behavior of F2/N2H4 and N2O4/MMH propellants. Results are presented which indicate no major fluid behavior problems would be encountered with any of the four propellants in the toroidal tanks of a spin-stabilized orbiter spacecraft.

A Crossover Study of Risperidone in Children, Adolescents and Adults with Mental Retardation

ERIC Educational Resources Information Center

Hellings, Jessica A.; Zarcone, Jennifer R.; Reese, R. Matthew; Valdovinos, Maria G.; Marquis, Janet G.; Fleming, Kandace K.; Schroeder, Stephen R.

2006-01-01

Risperidone has shown safety and efficacy for aggressive and destructive behaviors in short-term studies. This longer-duration study includes a broad sample. Forty subjects, aged 8-56 years (mean=22), all with mental retardation and 36 with autism spectrum disorders participated in this 22-week crossover study, with 24 weeks of open maintenance…

A Crossover Trial Evaluating an Educational-Behavioral Joint Protection Programme for People with Rheumatoid Arthritis.

ERIC Educational Resources Information Center

Hammond, A.; Lincoln, N.; Sutcliffe, L.

1999-01-01

Joint protection, a self-management technique taught to people with rheumatoid arthritis, was used in a group education program. A crossover trial (N=35) was conducted. No significant changes in measures of pain, functional disability, grip strength, self-efficacy or helplessness occurred post-education, although this may have been due to the…

Simple and advanced ferromagnet/molecule spinterfaces

NASA Astrophysics Data System (ADS)

Gruber, M.; Ibrahim, F.; Djedhloul, F.; Barraud, C.; Garreau, G.; Boukari, S.; Isshiki, H.; Joly, L.; Urbain, E.; Peter, M.; Studniarek, M.; Da Costa, V.; Jabbar, H.; Bulou, H.; Davesne, V.; Halisdemir, U.; Chen, J.; Xenioti, D.; Arabski, J.; Bouzehouane, K.; Deranlot, C.; Fusil, S.; Otero, E.; Choueikani, F.; Chen, K.; Ohresser, P.; Bertran, F.; Le Fèvre, P.; Taleb-Ibrahimi, A.; Wulfhekel, W.; Hajjar-Garreau, S.; Wetzel, P.; Seneor, P.; Mattana, R.; Petroff, F.; Scheurer, F.; Weber, W.; Alouani, M.; Beaurepaire, E.; Bowen, M.

2016-10-01

Spin-polarized charge transfer between a ferromagnet and a molecule can promote molecular ferromagnetism 1, 2 and hybridized interfacial states3, 4. Observations of high spin-polarization of Fermi level states at room temperature5 designate such interfaces as a very promising candidate toward achieving a highly spin-polarized, nanoscale current source at room temperature, when compared to other solutions such as half-metallic systems and solid-state tunnelling over the past decades. We will discuss three aspects of this research. 1) Does the ferromagnet/molecule interface, also called an organic spinterface, exhibit this high spin-polarization as a generic feature? Spin-polarized photoemission experiments reveal that a high spin-polarization of electronics states at the Fermi level also exist at the simple interface between ferromagnetic cobalt and amorphous carbon6. Furthermore, this effect is general to an array of ferromagnetic and molecular candidates7. 2) Integrating molecules with intrinsic properties (e.g. spin crossover molecules) into a spinterface toward enhanced functionality requires lowering the charge transfer onto the molecule8 while magnetizing it1,2. We propose to achieve this by utilizing interlayer exchange coupling within a more advanced organic spinterface architecture. We present results at room temperature across the fcc Co(001)/Cu/manganese phthalocyanine (MnPc) system9. 3) Finally, we discuss how the Co/MnPc spinterface's ferromagnetism stabilizes antiferromagnetic ordering at room temperature onto subsequent molecules away from the spinterface, which in turn can exchange bias the Co layer at low temperature10. Consequences include tunnelling anisotropic magnetoresistance across a CoPc tunnel barrier11. This augurs new possibilities to transmit spin information across organic semiconductors using spin flip excitations12.

Critical behavior of the spin-1 and spin-3/2 Baxter-Wu model in a crystal field.

PubMed

Dias, D A; Xavier, J C; Plascak, J A

2017-01-01

The phase diagram and the critical behavior of the spin-1 and the spin-3/2 two-dimensional Baxter-Wu model in a crystal field are studied by conventional finite-size scaling and conformal invariance theory. The phase diagram of this model, for the spin-1 case, is qualitatively the same as those of the diluted 4-states Potts model and the spin-1 Blume-Capel model. However, for the present case, instead of a tricritical point one has a pentacritical point for a finite value of the crystal field, in disagreement with previous work based on finite-size calculations. On the other hand, for the spin-3/2 case, the phase diagram is much richer and can present, besides a pentacritical point, an additional multicritical end point. Our results also support that the universality class of the critical behavior of the spin-1 and spin-3/2 Baxter-Wu model in a crystal field is the same as the pure Baxter-Wu model, even at the multicritical points.

Low-dimensional materials for organic electronic applications

NASA Astrophysics Data System (ADS)

Beniwal, Sumit

This thesis explores the self-assembly, surface interactions and electronic properties of functional molecules that have potential applications in electronics. Three classes of molecules - organic ferroelectric, spin-crossover complex, and molecules that assemble into a 2D semiconductor, have been studied through scanning tunneling microscopy and surfacesensitive spectroscopic methods. The scientific goal of this thesis is to understand the self-assembly of these molecules in low-dimensional (2D) configurations and the influence of substrate on their properties.

Reentrant Resistive Behavior and Dimensional Crossover in Disordered Superconducting TiN Films.

PubMed

Postolova, Svetlana V; Mironov, Alexey Yu; Baklanov, Mikhail R; Vinokur, Valerii M; Baturina, Tatyana I

2017-05-11

A reentrant temperature dependence of the normal state resistance often referred to as the N-shaped temperature dependence, is omnipresent in disordered superconductors - ranging from high-temperature cuprates to ultrathin superconducting films - that experience superconductor-to-insulator transition. Yet, despite the ubiquity of this phenomenon its origin still remains a subject of debate. Here we investigate strongly disordered superconducting TiN films and demonstrate universality of the reentrant behavior. We offer a quantitative description of the N-shaped resistance curve. We show that upon cooling down the resistance first decreases linearly with temperature and then passes through the minimum that marks the 3D-2D crossover in the system. In the 2D temperature range the resistance first grows with decreasing temperature due to quantum contributions and eventually drops to zero as the system falls into a superconducting state. Our findings demonstrate the prime importance of disorder in dimensional crossover effects.

Electronic and structural aspects of spin transitions observed by optical microscopy. The case of [Fe(ptz)6](BF4)2.

PubMed

Chong, Christian; Mishra, Haritosh; Boukheddaden, Kamel; Denise, Stéphane; Bouchez, Guillaume; Collet, Eric; Ameline, Jean-Claude; Naik, Anil D; Garcia, Yann; Varret, François

2010-02-11

The colorimetric analysis of images recorded with an optical microscope during the onset of the spin crossover transformation allows monitoring separately the involved electronic and structural aspects, through the separation of resonant absorption and scattering effects. Complementary information can also be obtained by using the polarized modes of the microscope. These potentialities are illustrated by the observation of [Fe(ptz)(6)](BF(4))(2) single crystals during the onset of the thermal transitions in the 110-140 K range. We characterized the interplay between the electronic (HS <--> LS) and structural (order <--> disorder) transformations. Elastic stresses and mechanical effects (hopping, self-cleavage) generated by the volume change upon electronic transition are also illustrated, with their impact on the photoswitching properties of the crystals.

Re-appearance of cooperativity in ultra-small spin-crossover [Fe(pz){Ni(CN)₄}] nanoparticles.

PubMed

Peng, Haonan; Tricard, Simon; Félix, Gautier; Molnár, Gábor; Nicolazzi, William; Salmon, Lionel; Bousseksou, Azzedine

2014-10-06

A reverse nanoemulsion technique was used for the elaboration of [Fe(pz){Ni(CN)4}] nanoparticles. Low-temperature micellar exchange made it possible to elaborate ultra-small nanoparticles with sizes down to 2 nm. When decreasing the size of the particles from 110 to 12 nm the spin transition shifts to lower temperatures, becomes gradual, and the hysteresis shrinks. On the other hand, a re-opening of the hysteresis was observed for smaller (2 nm) particles. A detailed (57)Fe Mössbauer spectroscopy analysis was used to correlate this unusual phenomenon to the modification of the stiffness of the nanoparticles thanks to the determination of their Debye temperature. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Entropy perspective on the thermal crossover in a fermionic Hubbard chain

NASA Astrophysics Data System (ADS)

Bonnes, Lars; Pichler, Hannes; Läuchli, Andreas M.

2013-10-01

We study the Renyi entropy in the finite-temperature crossover regime of a Hubbard chain using quantum Monte Carlo. The ground-state entropy has characteristic features such as a logarithmic divergence with block size and 2kF oscillations that are a hallmark of its Luttinger liquid nature. The interplay between the (extensive) thermal entropy and the ground-state features is studied and we analyze the temperature-induced decay of the amplitude of the oscillations as well as the scaling of the purity. Furthermore, we show how the spin and charge velocities can be extracted from the temperature dependence of the Renyi entropy, bridging our findings to recent experimental proposals on how to implement the measurement of Renyi entropies in the cold atom system. Studying the Renyi mutual information, we also demonstrate how constraints such as particle number conservation can induce persistent correlations visible in the mutual information even at high temperature.

Kondo destruction in a quantum paramagnet with magnetic frustration

NASA Astrophysics Data System (ADS)

Zhang, Jiahao; Zhao, Hengcan; Lv, Meng; Hu, Sile; Isikawa, Yosikazu; Yang, Yi-feng; Si, Qimiao; Steglich, Frank; Sun, Peijie

2018-06-01

We report results of isothermal magnetotransport and susceptibility measurements at elevated magnetic fields B down to very low temperatures T on single crystals of the frustrated Kondo-lattice system CePdAl. They reveal a B*(T ) line within the paramagnetic part of the phase diagram. This line denotes a thermally broadened "small"-to-"large" Fermi-surface crossover which substantially narrows upon cooling. At B0 *=B*(T =0 ) =(4.6 ±0.1 ) T , this B*(T ) line merges with two other crossover lines, viz. Tp(B ) below and TFL(B ) above B0 *. Tp characterizes a frustration-dominated spin-liquid state, while TFL is the Fermi-liquid temperature associated with the lattice Kondo effect. Non-Fermi-liquid phenomena which are commonly observed near a "Kondo-destruction" quantum-critical point cannot be resolved in CePdAl. Our observations reveal a rare case where Kondo coupling, frustration, and quantum criticality are closely intertwined.

Meissner mechanism for the spin supercurrent and interplay between quantum phase transition and spin transport in the frustrated Heisenberg model

NASA Astrophysics Data System (ADS)

Lima, Leonardo S.

2018-04-01

We have propose the Meissner mechanism for the spin supercurrent in quantum spin systems. Besides, we study the behavior of the AC spin conductivity in neighborhood of quantum phase transition in a frustrated spin model such as the antiferromagnet in the union jack lattice with single ion anisotropy at T = 0 . We investigate the spin conductivity for this model that presents exchange interactions J1 and J2 . Our results show a single peak for the conductivity with the height varying with the behavior of critical anisotropy Dc with J2 . We obtain the conductivity tending to zero in the limit ω → 0 .

Observation of magnetization reversal behavior in Sm0.9Gd0.1Cr0.85Mn0.15O3 orthochromites

NASA Astrophysics Data System (ADS)

Panwar, Neeraj; Joby, Jostin P.; Kumar, Surendra; Coondoo, Indrani; Vasundhara, M.; Kumar, Nitu; Palai, Ratnakar; Singhal, Rahul; Katiyar, Ram S.

2018-05-01

Impact of co-doping (Gd and Mn) on the magnetic properties has been systematically investigated in SmCrO3 compound. For the synthesized compound Sm0.9Gd0.1Cr0.85Mn0.15O3 (SGCMO), below the Neel transition temperature and under low applied magnetic field, temperature induced magnetization reversal at 105 K (crossover temperature) was noticed in the field cooled magnetization curve. Magnetization reversal attained maximum value of -1.03 emu/g at 17 K where spin reorientation occurred. The magnetization reversal disappeared under higher applied field. From the M-H plots an enhancement in the magnetization was observed due to Gd doping. Magnetocaloric effect at low temperatures measured through the magnetic entropy change was found sixteen times higher for this compound as compared to pristine SmCrO3 and twice to that of SmCr0.85Mn0.15O3 compound. The study reveals the importance of co-doping in tailoring the magnetic properties of rare-earth chromites.

Enhanced electrocaloric effect in displacive-type organic ferroelectrics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ding, L. J., E-mail: dinglinjie82@126.com; Zhong, Y.; Fan, S. W.

2015-08-07

We explore the intrinsic feature of electrocaloric effect (ECE) accompanied by ferroelectric (FE)-paraelectric (PE) transition for displacive-type organic ferroelectrics using Green's function theory. It is demonstrated that decreasing elastic constant K or increasing spin-lattice coupling λ can enhance the ECE, as well as polarization P and transition temperature T{sub C}. Indeed, one expects that the optimal operating temperature for solid-state refrigeration is around room temperature, at which the ECE achieves its maximum. As T{sub C} is tuned to ∼310 K, it presents larger ECE response and remanent polarization with lower coercive field for smaller K value, suggesting that well flexible displacive-typemore » organic ferroelectrics are excellent candidates both for electric cooling and data storage in the design of nonvolatile FE random-access memories. Furthermore, in an electric field, it provides a bridge between a Widom line that denotes FE-PE crossover above T{sub C} and a metaelectric transition line below T{sub C} that demonstrates an FE switching behavior with an antiparallel field.« less

Spin quenching assisted by a strongly anisotropic compression behavior in MnP

NASA Astrophysics Data System (ADS)

Han, Fei; Wang, Di; Wang, Yonggang; Li, Nana; Bao, Jin-Ke; Li, Bing; Botana, Antia S.; Xiao, Yuming; Chow, Paul; Chung, Duck Young; Chen, Jiuhua; Wan, Xiangang; Kanatzidis, Mercouri G.; Yang, Wenge; Mao, Ho-Kwang

2018-02-01

We studied the crystal structure and spin state of MnP under high pressure with synchrotron x-ray diffraction and x-ray emission spectroscopy (XES). MnP has an exceedingly strong anisotropy in compressibility, with the primary compressible direction along the b axis of the Pnma structure. XES reveals a pressure-driven quenching of the spin state in MnP. First-principles calculations suggest that the strongly anisotropic compression behavior significantly enhances the dispersion of the Mn d-orbitals and the splitting of the d-orbital levels compared to the hypothetical isotropic compression behavior. Thus, we propose spin quenching results mainly from the significant enhancement of the itinerancy of d electrons and partly from spin rearrangement occurring in the split d-orbital levels near the Fermi level. This explains the fast suppression of magnetic ordering in MnP under high pressure. The spin quenching lags behind the occurrence of superconductivity at ˜8 GPa implying that spin fluctuations govern the electron pairing for superconductivity.

Spin quenching assisted by a strongly anisotropic compression behavior in MnP

DOE Office of Scientific and Technical Information (OSTI.GOV)

Han, Fei; Wang, Di; Wang, Yonggang

We studied the crystal structure and spin state of MnP under high pressure with synchrotron X-ray diffraction and X-ray emission spectroscopy. MnP has an exceedingly strong anisotropy in compressibility, with the primary compressible direction along the b axis of the Pnma structure. X-ray emission spectroscopy reveals a pressure-driven quenching of the spin state in MnP. First-principles calculations suggest that the strongly anisotropic compression behavior significantly enhances the dispersion of the Mn d-orbitals and the splitting of the d-orbital levels compared to the hypothetical isotropic compression behavior. Thus, we propose spin quenching results mainly from the significant enhancement of the itinerancymore » of d electrons and partly from spin rearrangement occurring in the split d-orbital levels near the Fermi level. This explains the fast suppression of magnetic ordering in MnP under high pressure. The spin quenching lags behind the occurrence of superconductivity at ~8 GPa implying that spin fluctuations govern the electron pairing for superconductivity.« less

Spin resolved electronic transport through N@C20 fullerene molecule between Au electrodes: A first principles study

NASA Astrophysics Data System (ADS)

Caliskan, Serkan

2018-05-01

Using first principles study, through Density Functional Theory combined with Non Equilibrium Green's Function Formalism, electronic properties of endohedral N@C20 fullerene molecule joining Au electrodes (Au-N@C20) was addressed in the presence of spin property. The electronic transport behavior across the Au-N@C20 molecular junction was investigated by spin resolved transmission, density of states, molecular orbitals, differential conductance and current-voltage (I-V) characteristics. Spin asymmetric variation was clearly observed in the results due to single N atom encapsulated in the C20 fullerene cage, where the N atom played an essential role in the electronic behavior of Au-N@C20. This N@C20 based molecular bridge, exhibiting a spin dependent I-V variation, revealed a metallic behavior within the bias range from -1 V to 1 V. The induced magnetic moment, spin polarization and other relevant quantities associated with the spin resolved transport were elucidated.

Valley-spin filtering through a nonmagnetic resonant tunneling structure in silicene

NASA Astrophysics Data System (ADS)

Wu, Xiuqiang; Meng, Hao; Zhang, Haiyang; Bai, Yujie; Xu, Xing

2018-07-01

We theoretically investigate how a silecene-based nonmagnetic resonant-tunneling structure, i.e. a double electrostatic potential structure, can be tailored to generate valley- and spin-polarized filtering by using the scattering matrix method. This method allows us to find simple analytical expressions for the scattering amplitudes. It is found that the transmissions of electrons from opposite spin and valley show exactly opposite behaviors, leading to valley and spin filtering in a wide range of transmission directions. These directional-dependent valley-spin polarization behaviors can be used to select preferential directions along which the valley-spin polarization of an initially unpolarized carrier can be strongly enhanced. We also find that this phenomenon arises from the combinations of the coherent effect, electrostatic potential and external electric field. Especially when the direction of the external electric field is changed, the spin filtering properties are contained, while the valley filtering properties can be switched. In addition, the filtering behaviors can be conveniently controlled by electrical gating. Therefore, the results can offer an all-electric method to construct a valley-spin filter in silicene.

Pressure driven spin transition in siderite and magnesiosiderite single crystals.

PubMed

Weis, Christopher; Sternemann, Christian; Cerantola, Valerio; Sahle, Christoph J; Spiekermann, Georg; Harder, Manuel; Forov, Yury; Kononov, Alexander; Sakrowski, Robin; Yavaş, Hasan; Tolan, Metin; Wilke, Max

2017-11-28

Iron-bearing carbonates are candidate phases for carbon storage in the deep Earth and may play an important role for the Earth's carbon cycle. To elucidate the properties of carbonates at conditions of the deep Earth, we investigated the pressure driven magnetic high spin to low spin transition of synthetic siderite FeCO 3 and magnesiosiderite (Mg 0.74 Fe 0.26 )CO 3 single crystals for pressures up to 57 GPa using diamond anvil cells and x-ray Raman scattering spectroscopy to directly probe the iron 3d electron configuration. An extremely sharp transition for siderite single crystal occurs at a notably low pressure of 40.4 ± 0.1 GPa with a transition width of 0.7 GPa when using the very soft pressure medium helium. In contrast, we observe a broadening of the transition width to 4.4 GPa for siderite with a surprising additional shift of the transition pressure to 44.3 ± 0.4 GPa when argon is used as pressure medium. The difference is assigned to larger pressure gradients in case of argon. For magnesiosiderite loaded with argon, the transition occurs at 44.8 ± 0.8 GPa showing similar width as siderite. Hence, no compositional effect on the spin transition pressure is observed. The spectra measured within the spin crossover regime indicate coexistence of regions of pure high- and low-spin configuration within the single crystal.

Quantum-ring spin interference device tuned by quantum point contacts

DOE Office of Scientific and Technical Information (OSTI.GOV)

Diago-Cisneros, Leo; Mireles, Francisco

2013-11-21

We introduce a spin-interference device that comprises a quantum ring (QR) with three embedded quantum point contacts (QPCs) and study theoretically its spin transport properties in the presence of Rashba spin-orbit interaction. Two of the QPCs conform the lead-to-ring junctions while a third one is placed symmetrically in the upper arm of the QR. Using an appropriate scattering model for the QPCs and the S-matrix scattering approach, we analyze the role of the QPCs on the Aharonov-Bohm (AB) and Aharonov-Casher (AC) conductance oscillations of the QR-device. Exact formulas are obtained for the spin-resolved conductances of the QR-device as a functionmore » of the confinement of the QPCs and the AB/AC phases. Conditions for the appearance of resonances and anti-resonances in the spin-conductance are derived and discussed. We predict very distinctive variations of the QR-conductance oscillations not seen in previous QR proposals. In particular, we find that the interference pattern in the QR can be manipulated to a large extend by varying electrically the lead-to-ring topological parameters. The latter can be used to modulate the AB and AC phases by applying gate voltage only. We have shown also that the conductance oscillations exhibits a crossover to well-defined resonances as the lateral QPC confinement strength is increased, mapping the eigenenergies of the QR. In addition, unique features of the conductance arise by varying the aperture of the upper-arm QPC and the Rashba spin-orbit coupling. Our results may be of relevance for promising spin-orbitronics devices based on quantum interference mechanisms.« less

Covert Modeling vs. Behavior Rehearsal in the Training and Generalization of Assertive Behaviors: A Crossover Design.

ERIC Educational Resources Information Center

Zielinski, Joseph J.; Williams, Leslie J.

1979-01-01

Twenty-four underassertive adults were randomly assigned to two treatment orders that included covert modeling and behavior rehearsal. No measurable difference in treatments was found, but participants preferred and had greater expectations of behavior rehearsal. Skill generalization to untrained situations occurred on 8 of 11 behavioral measures.…

SPIN90 Modulates Long-Term Depression and Behavioral Flexibility in the Hippocampus

PubMed Central

Kim, Dae Hwan; Kang, Minkyung; Kim, Chong-Hyun; Huh, Yun Hyun; Cho, In Ha; Ryu, Hyun-Hee; Chung, Kyung Hwun; Park, Chul-Seung; Rhee, Sangmyung; Lee, Yong-Seok; Song, Woo Keun

2017-01-01

The importance of actin-binding proteins (ABPs) in the regulation of synapse morphology and plasticity has been well established. SH3 protein interacting with Nck, 90 kDa (SPIN90), an Nck-interacting protein highly expressed in synapses, is essential for actin remodeling and dendritic spine morphology. Synaptic targeting of SPIN90 to spine heads or dendritic shafts depends on its phosphorylation state, leading to blockage of cofilin-mediated actin depolymerization and spine shrinkage. However, the physiological role of SPIN90 in long-term plasticity, learning and memory are largely unknown. In this study, we demonstrate that Spin90-knockout (KO) mice exhibit substantial deficits in synaptic plasticity and behavioral flexibility. We found that loss of SPIN90 disrupted dendritic spine density in CA1 neurons of the hippocampus and significantly impaired long-term depression (LTD), leaving basal synaptic transmission and long-term potentiation (LTP) intact. These impairments were due in part to deficits in AMPA receptor endocytosis and its pre-requisites, GluA1 dephosphorylation and postsynaptic density (PSD) 95 phosphorylation, but also by an intrinsic activation of Akt-GSK3β signaling as a result of Spin90-KO. In accordance with these defects, mice lacking SPIN90 were found to carry significant deficits in object-recognition and behavioral flexibility, while learning ability was largely unaffected. Collectively, these findings demonstrate a novel modulatory role for SPIN90 in hippocampal LTD and behavioral flexibility. PMID:28979184

Spin-dependent transport behavior in C{sub 60} and Alq{sub 3} based spin valves with a magnetite electrode (invited)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Xianmin, E-mail: xmzhang@wpi-aimr.tohoku.ac.jp; Mizukami, Shigemi; Ma, Qinli

2014-05-07

The spin-dependent transport behavior in organic semiconductors (OSs) is generally observed at low temperatures, which likely results from poor spin injection efficiency at room temperature from the ferromagnetic metal electrodes to the OS layer. Possible reasons for this are the low Curie temperature and/or the small spin polarization efficiency for the ferromagnetic electrodes used in these devices. Magnetite has potential as an advanced candidate for use as the electrode in spintronic devices, because it can achieve 100% spin polarization efficiency in theory, and has a high Curie temperature (850 K). Here, we fabricated two types of organic spin valves using magnetitemore » as a high efficiency electrode. C{sub 60} and 8-hydroxyquinoline aluminum (Alq{sub 3}) were employed as the OS layers. Magnetoresistance ratios of around 8% and over 6% were obtained in C{sub 60} and Alq{sub 3}-based spin valves at room temperature, respectively, which are two of the highest magnetoresistance ratios in organic spin valves reported thus far. The magnetoresistance effect was systemically investigated by varying the thickness of the Alq{sub 3} layer. Moreover, the temperature dependence of the magnetoresistance ratios for C{sub 60} and Alq{sub 3}-based spin valves were evaluated to gain insight into the spin-dependent transport behavior. This study provides a useful method in designing organic spin devices operated at room temperature.« less

Single-molecule quantum dot as a Kondo simulator

NASA Astrophysics Data System (ADS)

Hiraoka, R.; Minamitani, E.; Arafune, R.; Tsukahara, N.; Watanabe, S.; Kawai, M.; Takagi, N.

2017-06-01

Structural flexibility of molecule-based systems is key to realizing the novel functionalities. Tuning the structure in the atomic scale enables us to manipulate the quantum state in the molecule-based system. Here we present the reversible Hamiltonian manipulation in a single-molecule quantum dot consisting of an iron phthalocyanine molecule attached to an Au electrode and a scanning tunnelling microscope tip. We precisely controlled the position of Fe2+ ion in the molecular cage by using the tip, and tuned the Kondo coupling between the molecular spins and the Au electrode. Then, we realized the crossover between the strong-coupling Kondo regime and the weak-coupling regime governed by spin-orbit interaction in the molecule. The results open an avenue to simulate low-energy quantum many-body physics and quantum phase transition through the molecular flexibility.

Magnetic properties of graphene quantum dots

NASA Astrophysics Data System (ADS)

Espinosa-Ortega, T.; Luk'yanchuk, I. A.; Rubo, Y. G.

2013-05-01

Using the tight-binding approximation we calculated the diamagnetic susceptibility of graphene quantum dots (GQDs) of different geometrical shapes and characteristic sizes of 2-10 nm, when the magnetic properties are governed by the electron edge states. Two types of edge states can be discerned: the zero-energy states (ZESs), located exactly at the zero-energy Dirac point, and the dispersed edge states (DESs), with the energy close but not exactly equal to zero. DESs are responsible for a temperature-independent diamagnetic response, while ZESs provide a temperature-dependent spin paramagnetism. Hexagonal, circular, and randomly shaped GQDs contain mainly DESs, and, as a result, they are diamagnetic. The edge states of the triangular GQDs are of ZES type. These dots reveal the crossover between spin paramagnetism, dominating for small dots and at low temperatures, and orbital diamagnetism, dominating for large dots and at high temperatures.

Cycles, scaling and crossover phenomenon in length of the day (LOD) time series

NASA Astrophysics Data System (ADS)

Telesca, Luciano

2007-06-01

The dynamics of the temporal fluctuations of the length of the day (LOD) time series from January 1, 1962 to November 2, 2006 were investigated. The power spectrum of the whole time series has revealed annual, semi-annual, decadal and daily oscillatory behaviors, correlated with oceanic-atmospheric processes and interactions. The scaling behavior was analyzed by using the detrended fluctuation analysis (DFA), which has revealed two different scaling regimes, separated by a crossover timescale at approximately 23 days. Flicker-noise process can describe the dynamics of the LOD time regime involving intermediate and long timescales, while Brownian dynamics characterizes the LOD time series for small timescales.

Pressure-Induced Valence Crossover and Novel Metamagnetic Behavior near the Antiferromagnetic Quantum Phase Transition of YbNi3Ga9

NASA Astrophysics Data System (ADS)

Matsubayashi, K.; Hirayama, T.; Yamashita, T.; Ohara, S.; Kawamura, N.; Mizumaki, M.; Ishimatsu, N.; Watanabe, S.; Kitagawa, K.; Uwatoko, Y.

2015-02-01

We report electrical resistivity, ac magnetic susceptibility, and x-ray absorption spectroscopy measurements of intermediate valence YbNi3Ga9 under pressure and magnetic field. We have revealed a characteristic pressure-induced Yb valence crossover within the temperature-pressure phase diagram, and a first-order metamagnetic transition is found below Pc˜9 GPa where the system undergoes a pressure-induced antiferromagnetic transition. As a possible origin of the metamagnetic behavior, a critical valence fluctuation emerging near the critical point of the first-order valence transition is discussed on the basis of the temperature-field-pressure phase diagram.

Transport properties of glass-forming liquids suggest that dynamic crossover temperature is as important as the glass transition temperature.

PubMed

Mallamace, Francesco; Branca, Caterina; Corsaro, Carmelo; Leone, Nancy; Spooren, Jeroen; Chen, Sow-Hsin; Stanley, H Eugene

2010-12-28

It is becoming common practice to partition glass-forming liquids into two classes based on the dependence of the shear viscosity η on temperature T. In an Arrhenius plot, ln η vs 1/T, a strong liquid shows linear behavior whereas a fragile liquid exhibits an upward curvature [super-Arrhenius (SA) behavior], a situation customarily described by using the Vogel-Fulcher-Tammann law. Here we analyze existing data of the transport coefficients of 84 glass-forming liquids. We show the data are consistent, on decreasing temperature, with the onset of a well-defined dynamical crossover η(×), where η(×) has the same value, η(×) ≈ 10(3) Poise, for all 84 liquids. The crossover temperature, T(×), located well above the calorimetric glass transition temperature T(g), marks significant variations in the system thermodynamics, evidenced by the change of the SA-like T dependence above T(×) to Arrhenius behavior below T(×). We also show that below T(×) the familiar Stokes-Einstein relation D/T ∼ η(-1) breaks down and is replaced by a fractional form D/T ∼ η(-ζ), with ζ ≈ 0.85.

Transport properties of glass-forming liquids suggest that dynamic crossover temperature is as important as the glass transition temperature

PubMed Central

Mallamace, Francesco; Branca, Caterina; Corsaro, Carmelo; Leone, Nancy; Spooren, Jeroen; Chen, Sow-Hsin; Stanley, H. Eugene

2010-01-01

It is becoming common practice to partition glass-forming liquids into two classes based on the dependence of the shear viscosity η on temperature T. In an Arrhenius plot, ln η vs 1/T, a strong liquid shows linear behavior whereas a fragile liquid exhibits an upward curvature [super-Arrhenius (SA) behavior], a situation customarily described by using the Vogel–Fulcher–Tammann law. Here we analyze existing data of the transport coefficients of 84 glass-forming liquids. We show the data are consistent, on decreasing temperature, with the onset of a well-defined dynamical crossover η×, where η× has the same value, η× ≈ 103 Poise, for all 84 liquids. The crossover temperature, T×, located well above the calorimetric glass transition temperature Tg, marks significant variations in the system thermodynamics, evidenced by the change of the SA-like T dependence above T× to Arrhenius behavior below T×. We also show that below T× the familiar Stokes–Einstein relation D/T ∼ η-1 breaks down and is replaced by a fractional form D/T ∼ η-ζ, with ζ ≈ 0.85. PMID:21148100

Crossover transition in the fluctuation of Internet

NASA Astrophysics Data System (ADS)

Qian, Jiang-Hai

2018-06-01

The inconsistent fluctuation behavior of Internet predicted by preferential attachment(PA) and Gibrat's law requires empirical investigations on the actual system. By using the interval-tunable Gibrat's law statistics, we find the actual fluctuation, characterized by the conditional standard deviation of the degree growth rate, changes with the interval length and displays a crossover transition from PA type to Gibrat's law type, which has not yet been captured by any previous models. We characterize the transition dynamics quantitatively and determine the applicative range of PA and Gibrat's law. The correlation analysis indicates the crossover transition may be attributed to the accumulative correlation between the internal links.

Temperature Sensing Above 1000 C Using Cr-Doped GdAlO3 Spin-Allowed Broadband Luminescence

NASA Technical Reports Server (NTRS)

Eldridge, Jeffrey I.; Chambers, Matthew D.

2012-01-01

Cr-doped GdAlO3 (Cr:GdAlO3) is shown to produce remarkably high-intensity spin-allowed broadband luminescence with sufficiently long decay times to make effective luminescence-decay-time based temperature measurements above 1000 C. This phosphor is therefore an attractive alternative to the much lower luminescence intensity rare-earth-doped thermographic phosphors that are typically utilized at these elevated temperatures. In particular, Cr:GdAlO3 will be preferred over rare-earth-doped phosphors, such as Dy:YAG, at temperatures up to 1200 C for intensity-starved situations when the much lower emission intensity from rare-earth-doped phosphors is insufficient for accurate temperature measurements in the presence of significant radiation background. While transition-metal-doped phosphors such as Cr:Al2O3 (ruby) are known to exhibit high luminescence intensity at low dopant concentrations, quenching due to nonradiative decay pathways competing with the (sup 2)E to (sup 4)A(sub 2) radiative transition (R line) has typically restricted their use for temperature sensing to below 600 C. Thermal quenching of the broadband (sup 4)T(sub 2) to (sup 4)A(sub 2) radiative transition from Cr:GdAlO3, however, is delayed until much higher temperatures (above 1000 C). This spin-allowed broadband emission persists to high temperatures because the lower-lying (sup 2)E energy level acts as a reservoir to thermally populate the higher shorter-lived (sup 4)T(sub 2) energy level and because the activation energy for nonradiative crossover relaxation from the (sup 4)T(sub 2) level to the (sup 4)A(sub 2) ground state is high. The strong crystal field associated with the tight bonding of the AlO6 octahedra in the GdAlO3 perovskite structure is responsible for this behavior.

Vacancy-induced spin-glass behavior of Prussian blue analogue Fe II1.1Cr IIx[Cr III (CN) 6] 0.6- x· nH 2O nanowires

NASA Astrophysics Data System (ADS)

Gao, Bo; Yao, Jinli; Xue, Desheng

2010-09-01

Prussian blue analogue Fe II1.1Cr IIx[Cr III(CN) 6] 0.6- x· nH 2O nanowires were synthesized by electrodeposition. The magnetic properties investigation indicates that the nanowires exhibit cluster spin-glass behavior, which undergoes a magnetic transition to a frozen state below about 62 K. Spin disorder arising from reduced coordination and broken exchange bonds between spin centers due to the structural defects may be the reason that causes the spin-glass freezing behavior. The negative magnetization observed at temperature lower than the compensation temperature ( Tcomp˜43 K) at a field of 10 Oe may be due to the different temperature dependences of the ferromagnetic site Fe-Cr and antiferromagnetic site Cr-Cr.

Fluid interaction with spinning toroidal tanks

NASA Technical Reports Server (NTRS)

Fester, D. A.; Anderson, J. E.

1977-01-01

An experimental study was conducted to evaluate propellant behavior in spinning torroidal tanks that could be used in a retropropulsion system of an advanced outer-planet Pioneer orbiter. Information on propellant slosh and settling and on ullage orientation and stability was obtained. The effects of axial acceleration, spin rate, spin-rate change, and spacecraft wobble, both singly and in combination, were evaluated using a one-eighth scale transparent tank in one-g and low-g environments. Liquid loadings ranged from 5% to 96% full. The impact of a surface tension acquisition device was assessed by comparison with bare-tank results. The testing simulated the behavior of the fluorine/hydrazine and nitrogen textroxide/monomethylhydrazine propellants. Results are presented that indicate that no major fluid behavior problems would be encountered with any of the four propellants in the toroidal tanks of a spin-stabilized orbiter spacecraft.

Scaling in the aggregation dynamics of a magnetorheological fluid.

PubMed

Domínguez-García, P; Melle, Sonia; Pastor, J M; Rubio, M A

2007-11-01

We present experimental results on the aggregation dynamics of a magnetorheological fluid, namely, an aqueous suspension of micrometer-sized superparamagnetic particles, under the action of a constant uniaxial magnetic field using video microscopy and image analysis. We find a scaling behavior in several variables describing the aggregation kinetics. The data agree well with the Family-Vicsek scaling ansatz for diffusion-limited cluster-cluster aggregation. The kinetic exponents z and z' are obtained from the temporal evolution of the mean cluster size S(t) and the number of clusters N(t), respectively. The crossover exponent Delta is calculated in two ways: first, from the initial slope of the scaling function; second, from the evolution of the nonaggregated particles, n1(t). We report on results of Brownian two-dimensional dynamics simulations and compare the results with the experiments. Finally, we discuss the differences obtained between the kinetic exponents in terms of the variation in the crossover exponent and relate this behavior to the physical interpretation of the crossover exponent.

Hybridization effects on wave packet dynamics in topological insulator thin films.

PubMed

Yar, Abdullah; Naeem, Muhammad; Khan, Safi Ullah; Sabeeh, Kashif

2017-11-22

Theoretical study of electron wave packet dynamics in topological insulator (TI) thin films is presented. We have investigated real space trajectories and spin dynamics of electron wave packets in TI thin films. Our focus is on the role of hybridization between the electronic states of the two surfaces. This allows us to access the crossover regime of a thick film with no hybridization to a thin film with finite hybridization. We show that the electron wave packet undergoes side-jump motion in addition to zitterbewegung. The oscillation frequency of zitterbewegung can be tuned by the strength of hybridization, which in turn can be tuned by the thickness of the film. We find that the spin expectations also exhibit zitterbewegung tunable by hybridization. We also show that it is possible to obtain persistent zitterbewegung, oscillations which do not decay, in both the real space trajectories as well as spin dynamics. The zitterbewegung oscillation frequency in TI thin films falls in a parameter regime where it might be possible to observe these effects using present day experimental techniques.

Dynamic magnetic hysteresis properties of two-dimensional ferrimagnetic structures containing high-spin (S = 5/2) and low-spin (S = 1/2)

NASA Astrophysics Data System (ADS)

Batı, Mehmet; Ertaş, Mehmet

2017-09-01

The dynamic hysteresis behaviors of a containing high spin-5/2 and low spin-1/2 Ising ferrimagnetic system on a square lattice are studied by using the dynamic mean-field approximation. The influences of the temperature, the single-ion anisotropy and the frequency on dynamic hysteresis behaviors are investigated in detail. Somewhat characteristic behaviors are found, such as the presence of triple hysteresis loop for appropriate values of the crystal field or temperature. Besides, we observed that, hysteresis loop area and phase transition points are very sensitive to changes in frequency and thus have profound importance in device application.

Magnetic Properties of selected Prussian Blue Analogs

NASA Astrophysics Data System (ADS)

Shrestha, Manjita

Prussian Blue Analogs (PBAs) of composition M[M(C,N)6 ] 2.xH2O are bimetallic cyanide complexes, where M and M are bivalent or trivalent transition metals and x is number of water molecule per unit cell. The PBAs form cubic framework structures, which consist mostly of alternating MIIIN6 and MIIC 6 octahedrals. However, occupancies of the octrahedrals are not perfect: they may be empty and the charges are balanced by the guest water molecules at the lattice site (C or N site) or the interstitial site (between the octahedrals) of the unit cell. Most (but not all) PBAs exhibit negative thermal expansion behavior, i.e. volume decrease with increasing temperature. Another area of interest in PBA research is the occurrence of unusual magnetic properties. Similar to other molecular magnets, large crystal-field splitting due to the octrahedral environment may result in a combination of low- or high-spin configurations of the localized magnetic moments, i.e. spin crossover effects may be found. My dissertation focuses on the magnetic properties of the selected 3d transition-metal PBAs, namely metal hexacyanochromates M3[Cr(C,N)6 ]2.xH2O, metal hexcyanoferrates M3[Fe(C,N)6]2.xH2O and metal hexcyanocobaltates M3[Co(C,N)6]2 .xH2O where M = Mn, Co, Ni and Cu. In particular, I analyzed the temperature and field dependencies of the bulk magnetic response of those PBAs. My results show that the magnetic susceptibility of all studied PBAs follows the Curie-Weiss behavior in the paramagnetic region up to room temperature; however, some of the compounds exhibit long-range magnetic order at lower temperatures (ferromagnetic or antiferromagnetic). In particular, the data provide evidence for magnetic ground states for most of the metal hexacyanochromates and all of the metal hexacyanoferrates but none of the hexacyanocobaltates that were studied. For each of the compounds, my analysis provides a measure of the effective magnetic moment, which is then compared with the predicted moments assuming high- and/or low-spin configurations. Finally, I provide a discussion as to whether magnetism may play any role into the occurrence of negative thermal expansion for most PBAs.

Critical Behavior and Macroscopic Phase Diagram of the Monoaxial Chiral Helimagnet Cr 1/3NbS 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Clements, Eleanor M.; Das, Raja; Li, Ling

2017-07-26

Cr 1/3NbS 2 is a unique example of a hexagonal chiral helimagnet with high crystalline anisotropy, and has generated growing interest for a possible magnetic field control of the incommensurate spin spiral. Here, we construct a comprehensive phase diagram based on detailed magnetization measurements of a high quality single crystal of Cr 1/3NbS 2 over three magnetic field regions. An analysis of the critical properties in the forced ferromagnetic region yields 3D Heisenberg exponents β = 0.3460 ± 0.040, γ = 1.344 ± 0.002, and T C = 130.78 K ± 0.044, which are consistent with the localized nature themore » of Cr 3+ moments and suggest short-range ferromagnetic interactions. We exploit the temperature and magnetic field dependence of magnetic entropy change (ΔS M) to accurately map the nonlinear crossover to the chiral soliton lattice regime from the chiral helimagnetic phase. Our observations in the low field region are consistent with the existence of chiral ordering in a temperature range above the Curie temperature, T C < T < T*, where a first-order transition has been previously predicted. An analysis of the universal behavior of ΔS M(T,H) experimentally demonstrates for the first time the first-order nature of the onset of chiral ordering.« less

Gas-liquid phase coexistence and crossover behavior of binary ionic fluids with screened Coulomb interactions.

PubMed

Patsahan, O

2014-06-01

We study the effects of an interaction range on the gas-liquid phase diagram and the crossover behavior of a simple model of ionic fluids: an equimolar binary mixture of equisized hard spheres interacting through screened Coulomb potentials which are repulsive between particles of the same species and attractive between particles of different species. Using the collective variables theory, we find explicit expressions for the relevant coefficients of the effective φ{4} Ginzburg-Landau Hamiltonian in a one-loop approximation. Within the framework of this approximation, we calculate the critical parameters and gas-liquid phase diagrams for varying inverse screening length z. Both the critical temperature scaled by the Yukawa potential contact value and the critical density rapidly decrease with an increase of the interaction range (a decrease of z) and then for z<0.05 they slowly approach the values found for a restricted primitive model (RPM). We find that gas-liquid coexistence region reduces with an increase of z and completely vanishes at z≃2.78. Our results clearly show that an increase in the interaction range leads to a decrease of the crossover temperature. For z≃0.01, the crossover temperature is the same as for the RPM.

Exploiting pressure to induce a "guest-blocked" spin transition in a framework material

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sciortino, Natasha F.; Ragon, Florence; Zenere, Katrina A.

A new functionalized 1,2,4-trizole ligand 4-[(E)-2-(5-methyl-2-thienyl)vinyl]-1,2,4-triazole (thiome) was prepared to assess the structural and magnetic consequence of ligand steric bulk in the resultant framework material [FeIIPd(CN)4(thiome)2]·2(H2O) (A·2(H2O)). Structural studies reveal that the pore size is smaller than realted 2-D Hofmann-type materials and that the water molecules can be reversibly removed with retention of the porous host framework. Magnetic measurements show ‘on-off’ sensing to the presence of water. The hydrated phase is spin crossover (SCO) inactive whereas the dehydrated phase undergoes an abrupt and hysteretic one-step spin transition. Partial dehydration (A·n(H2O), 0 ≤ n ≤ 2) leads to systematically varying spinmore » transition temperatures further demonstrating qualitative sensing. These studies suggest that the SCO properties are governed by internal lattice pressure effects. Variable pressure structure and magnetic studies on the hydrated phase, A·2(H2O), reveal that such internal guest pressure effects can be overcome with moderate external pressure application (0 – 0.68 GPa) resulting in a two-step spin transition at ambient temperatures at 0.68 GPa.« less

Coordination-induced spin crossover (CISCO) through axial bonding of substituted pyridines to nickel-porphyrins: sigma-donor versus pi-acceptor effects.

PubMed

Thies, Steffen; Bornholdt, Claudia; Köhler, Felix; Sönnichsen, Frank D; Näther, Christian; Tuczek, Felix; Herges, Rainer

2010-09-03

Nickel-porphyrins, with their rigid quadratic planar coordination framework, provide an excellent model to study the coordination-induced spin crossover (CISCO) effect because bonding of one or two axial ligands to the metal center leads to a spin transition from S=0 to S=1. Herein, both equilibrium constants K(1S) and K(2), and for the first time also the corresponding thermodynamic parameters DeltaH(1S), DeltaH(2), DeltaS(1S), and DeltaS(2), are determined for the reaction of a nickel-porphyrin (Ni-tetrakis(pentafluorophenyl)porphyrin) with different 4-substituted pyridines by temperature-dependent NMR spectroscopy. The association constants K(1S) and K(2) are correlated with the basicity of the 4-substituted pyridines (R: OMe>H>CO(2)Et>NO(2)) whereas the DeltaH(1S) values exhibit a completely different order (OMeCO(2)Et>NO(2)). 4-Nitropyridine exhibits the largest binding enthalpy, which, however, is overcompensated by a large negative binding entropy. We attribute the large association enthalpy of nitropyridine with porphyrin to the back donation of electrons from the Ni d(xz) and d(yz) orbitals into the pi orbitals of pyridine, and the negative association entropy to a decrease in vibrational and internal rotation entropy of the more rigid porphyrin-pyridine complex. Back donation for the nitro- and cyanopyridine complexes is also confirmed by IR spectroscopy, and shows a shift of the N-O and C-N vibrations, respectively, to lower wave numbers. X-ray structures of 2:1 complexes with nitro-, cyano-, and dimethylaminopyridine provide further indication of a back donation. A further trend has been observed: the more basic the pyridine the larger is K(1S) relative to K(2). For nitropyridine K(2) is 17 times larger than K(1S) and in the case of methoxypyridine K(2) and K(1S) are almost equal.

Dielectric response to the low-temperature magnetic defect structure and spin state transition in polycrystalline LaCoO3

NASA Astrophysics Data System (ADS)

Schmidt, Rainer; Wu, J.; Leighton, C.; Terry, I.

2009-03-01

The dielectric and magnetic properties and their correlations were investigated in polycrystalline perovskite LaCoO3-δ . The intrinsic bulk and grain-boundary (GB) dielectric relaxation processes were deconvoluted using impedance spectroscopy between 20 and 120 K, and resistivity and capacitance were analyzed separately. A thermally induced magnetic transition from a Co3+ low-spin (LS) (S=0;t2g6eg0) to a higher spin state occurs at Ts1≈80K , which is controversial in nature and has been suggested to be an intermediate-spin (IS) state (S=1;t2g5eg1) or a high-spin (HS) state (S=2;t2g4eg2) transition. This spin state transition was confirmed by magnetic-susceptibility measurements and was reflected in the impedance by a split of the single GB relaxation process into two coexisting contributions. This apparent electronic phase coexistence at T>80K was interpreted as a reflection of the coexistence of magnetic LS and IS/HS states. At lower temperatures (T≤40K) perceptible variation in bulk dielectric permittivity with temperature appeared to be correlated with the magnetic susceptibility associated with a magnetic defect structure. At 40K

The enhanced spin-polarized transport behaviors through cobalt benzene-porphyrin-benzene molecular junctions: the effect of functional groups

NASA Astrophysics Data System (ADS)

Cheng, Jue-Fei; Zhou, Liping; Wen, Zhongqian; Yan, Qiang; Han, Qin; Gao, Lei

2017-05-01

The modification effects of the groups amino (NH2) and nitro (NO2) on the spin polarized transport properties of the cobalt benzene-porphyrin-benzene (Co-BPB) molecule coupled to gold (Au) nanowire electrodes are investigated by the nonequilibrium Green’s function method combined with the density functional theory. The calculation results show that functional groups can lead to the significant spin-filter effect, enhanced low-bias negative differential resistance (NDR) behavior and novel reverse rectifying effect in Co-BPB molecular junction. The locations and types of functional groups have distinct influences on spin-polarized transport performances. The configuration with NH2 group substituting H atom in central porphyrin ring has larger spin-down current compared to that with NO2 substitution. And Co-BPB molecule junction with NH2 group substituting H atom in side benzene ring shows reverse rectifying effect. Detailed analyses confirm that NH2 and NO2 group substitution change the spin-polarized transferred charge, which makes the highest occupied molecular orbitals (HOMO) of spin-down channel of Co-BPB closer to the Fermi level. And the shift of HOMO strengthens the spin-polarized coupling between the molecular orbitals and the electrodes, leading to the enhanced spin-polarized behavior. Our findings might be useful in the design of multi-functional molecular devices in the future.

Critical behavior and dimension crossover of pion superfluidity

NASA Astrophysics Data System (ADS)

Wang, Ziyue; Zhuang, Pengfei

2016-09-01

We investigate the critical behavior of pion superfluidity in the framework of the functional renormalization group (FRG). By solving the flow equations in the SU(2) linear sigma model at finite temperature and isospin density, and making comparison with the fixed point analysis of a general O (N ) system with continuous dimension, we find that the pion superfluidity is a second order phase transition subject to an O (2 ) universality class with a dimension crossover from dc=4 to dc=3 . This phenomenon provides a concrete example of dimension reduction in thermal field theory. The large-N expansion gives a temperature independent critical exponent β and agrees with the FRG result only at zero temperature.

Finite-size scaling and integer-spin Heisenberg chains

NASA Astrophysics Data System (ADS)

Bonner, Jill C.; Müller, Gerhard

1984-03-01

Finite-size scaling (phenomenological renormalization) techniques are trusted and widely applied in low-dimensional magnetism and, particularly, in lattice gauge field theory. Recently, investigations have begun which subject the theoretical basis to systematic and intensive scrutiny to determine the validity of finite-size scaling in a variety of situations. The 2D ANNNI model is an example of a situation where finite-size scaling methods encounter difficulty, related to the occurrence of a disorder line (one-dimensional line). A second example concerns the behavior of the spin-1/2 antiferromagnetic XXZ model where the T=0 critical behavior is exactly known and features an essential singularity at the isotropic Heisenberg point. Standard finite-size scaling techniques do not convincingly reproduce the exact phase behavior and this is attributable to the essential singularity. The point is relevant in connection with a finite-size scaling analysis of a spin-one antiferromagnetic XXZ model, which claims to support a conjecture by Haldane that the T=0 phase behavior of integer-spin Heisenberg chains is significantly different from that of half-integer-spin Heisenberg chains.

Quasiparticle Excitations in the Superconducting State of FeSe Probed by Thermal Hall Conductivity in the Vicinity of the BCS-BEC Crossover

NASA Astrophysics Data System (ADS)

Watashige, Tatsuya; Arsenijević, Stevan; Yamashita, Takuya; Terazawa, Daiki; Onishi, Takafumi; Opherden, Lars; Kasahara, Shigeru; Tokiwa, Yoshifumi; Kasahara, Yuichi; Shibauchi, Takasada; von Löhneysen, Hilbert; Wosnitza, Jochen; Matsuda, Yuji

2017-01-01

There is growing evidence that the superconducting semimetal FeSe (Tc ˜ 8 K) is in the crossover regime between weak-coupling Bardeen-Cooper-Schrieffer (BCS) and strong-coupling Bose-Einstein-condensate (BEC) limits. We report on longitudinal and transverse thermal conductivities, κxx and κxy, respectively, in magnetic fields up to 20 T. The field dependences of κxx and κxy imply that a highly anisotropic small superconducting gap forms at the electron Fermi-surface pocket whereas a more isotropic and larger gap forms at the hole pocket. Below ˜1.0 K, both κxx and κxy exhibit distinct anomalies (kinks) at the upper critical field Hc2 and at a field H* slightly below Hc2. The analysis of the thermal Hall angle (κxy/κxx) indicates a change of the quasiparticle scattering rate at H*. These results provide strong support to the previous suggestion that above H* a distinct field-induced superconducting phase emerges with an unprecedented large spin imbalance.

Switchable molecular magnets

PubMed Central

SATO, Osamu

2012-01-01

Various molecular magnetic compounds whose magnetic properties can be controlled by external stimuli have been developed, including electrochemically, photochemically, and chemically tunable bulk magnets as well as a phototunable antiferromagnetic phase of single chain magnet. In addition, we present tunable paramagnetic mononuclear complexes ranging from spin crossover complexes and valence tautomeric complexes to Co complexes in which orbital angular momentum can be switched. Furthermore, we recently developed several switchable clusters and one-dimensional coordination polymers. The switching of magnetic properties can be achieved by modulating metals, ligands, and molecules/ions in the second sphere of the complexes. PMID:22728438

Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids.

PubMed

Jaiswal, Abhishek; Egami, Takeshi; Kelton, K F; Schweizer, Kenneth S; Zhang, Yang

2016-11-11

We report the observation of a distinct correlation between the kinetic fragility index m and the reduced Arrhenius crossover temperature θ_{A}=T_{A}/T_{g} in various glass-forming liquids, identifying three distinguishable groups. In particular, for 11 glass-forming metallic liquids, we universally observe a crossover in the mean diffusion coefficient from high-temperature Arrhenius to low-temperature super-Arrhenius behavior at approximately θ_{A}≈2 which is in the stable liquid phases. In contrast, for fragile molecular liquids, this crossover occurs at much lower θ_{A}≈1.4 and usually in their supercooled states. The θ_{A} values for strong network liquids spans a wide range higher than 2. Intriguingly, the high-temperature activation barrier E_{∞} is universally found to be ∼11k_{B}T_{g} and uncorrelated with the fragility or the reduced crossover temperature θ_{A} for metallic and molecular liquids. These observations provide a way to estimate the low-temperature glassy characteristics (T_{g} and m) from the high-temperature liquid quantities (E_{∞} and θ_{A}).

Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jaiswal, Abhishek; Egami, Takeshi; Kelton, K. F.

2016-11-10

In this paper, we report the observation of a distinct correlation between the kinetic fragility index m and the reduced Arrhenius crossover temperature θ A = T A/T g in various glass-forming liquids, identifying three distinguishable groups. In particular, for 11 glass-forming metallic liquids, we universally observe a crossover in the mean diffusion coefficient from high-temperature Arrhenius to low-temperature super-Arrhenius behavior at approximately θ A ≈ 2 which is in the stable liquid phases. In contrast, for fragile molecular liquids, this crossover occurs at much lower θ A ≈ 1.4 and usually in their supercooled states. The θ A valuesmore » for strong network liquids spans a wide range higher than 2. Intriguingly, the high-temperature activation barrier E ∞ is universally found to be ~11k BT g and uncorrelated with the fragility or the reduced crossover temperature θ A for metallic and molecular liquids. Finally, these observations provide a way to estimate the low-temperature glassy characteristics (T g and m) from the high-temperature liquid quantities (E ∞ and θ A).« less

Oxygen octahedra distortion induced structural and magnetic phase transitions in Bi{sub 1−x}Ca{sub x}Fe{sub 1−x}Mn{sub x}O{sub 3} ceramics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kumar, Pawan; Kar, Manoranjan, E-mail: mano@iitp.ac.in; Shankhwar, Nisha

2015-05-21

The co-doping of Ca and Mn in respective Bi and Fe-sites of BiFeO{sub 3} lattice leads to structural transition from rhombohedral (R3c space group) to orthorhombic (Pbnm space group) crystal symmetry. The tilt angle for anti-phase rotation of the oxygen octahedra of BiFeO{sub 3} at room temperature is observed to be ∼13.8°. It decreases with the increase in the co-doping percentage which suggests the composition-driven structural phase transition. The remnant magnetization for sample with 15% of co-doping becomes about 16 times that of BiFeO{sub 3}. It may be attributed to the suppression of cycloid spin structure and uncompensated spins atmore » the surface of nanocrystallites. Further increase in co-doping percentage results in the sharp reduction of remnant magnetization due to the dominant contribution from the collinear antiferromagnetic ordering in the Pbnm space group. The Arrott plot analysis clearly indicates the composition-driven crossover from the antiferromagnetic to weak ferromagnetic ordering and vice versa. Electron spin resonance results provide the evidence for the composition-driven phase transitions from an incommensurate spin cycloidal modulated state to one with nearly homogeneous spin order. The band gap (2.17 eV) of BiFeO{sub 3} measured using UV-Vis spectra was supported by the resonance Raman spectra.« less

Thermodynamic properties of the S =1 /2 twisted triangular spin tube

NASA Astrophysics Data System (ADS)

Ito, Takuya; Iino, Chihiro; Shibata, Naokazu

2018-05-01

Thermodynamic properties of the twisted three-leg spin tube under magnetic field are studied by the finite-T density-matrix renormalization group method. The specific heat, spin, and chiral susceptibilities of the infinite system are calculated for both the original and its low-energy effective models. The obtained results show that the presence of the chirality is observed as a clear peak in the specific heat at low temperature and the contribution of the chirality dominates the low-temperature part of the specific heat as the exchange coupling along the spin tube decreases. The peak structures in the specific heat, spin, and chiral susceptibilities are strongly modified near the quantum phase transition where the critical behaviors of the spin and chirality correlations change. These results confirm that the chirality plays a major role in characteristic low-energy behaviors of the frustrated spin systems.

Current-based detection of nonlocal spin transport in graphene for spin-based logic applications

NASA Astrophysics Data System (ADS)

Wen, Hua; Zhu, Tiancong; Luo, Yunqiu Kelly; Amamou, Walid; Kawakami, Roland K.

2014-05-01

Graphene has been proposed for novel spintronic devices due to its robust and efficient spin transport properties at room temperature. Some of the most promising proposals require current-based readout for integration purposes, but the current-based detection of spin accumulation has not yet been developed. In this work, we demonstrate current-based detection of spin transport in graphene using a modified nonlocal geometry. By adding a variable shunt resistor in parallel to the nonlocal voltmeter, we are able to systematically cross over from the conventional voltage-based detection to current-based detection. As the shunt resistor is reduced, the output current from the spin accumulation increases as the shunt resistance drops below a characteristic value R*. We analyze this behavior using a one-dimensional drift-diffusion model, which accounts well for the observed behavior. These results provide the experimental and theoretical foundation for current-based detection of nonlocal spin transport.

Magnetized liquid 3He at finite temperature: A variational calculation approach

NASA Astrophysics Data System (ADS)

Bordbar, Gholam Hossein; Mohammadi Sabet, Mohammad Taghi

2016-08-01

Using the spin-dependent (SD) and spin-independent (SI) correlation functions, we have investigated the properties of liquid 3He in the presence of magnetic field at finite temperature. Our calculations have been done using the variational method based on cluster expansion of the energy functional. Our results show that the low field magnetic susceptibility obeys Curie law at high temperatures. This behavior is in a good agreement with the experimental data as well as the molecular field theory results in which the spin dependency has been introduced in correlation function. Reduced susceptibility as a function of temperature as well as reduced temperature has been also investigated, and again we have seen that the spin-dependent correlation function leads to a good agreement with the experimental data. The Landau parameter, F0a, has been calculated, and for this parameter, a value about - 0.75 has been found in the case of spin-spin correlation. In the case of spin-independent correlation function, this value is about - 0.7. Therefore, inclusion of spin dependency in the correlation function leads to a more compatible value of F0a with experimental data. The magnetization and susceptibility of liquid 3He have also been investigated as a function of magnetic field. Our results show a downward curvature in magnetization of system with spin-dependent correlation for all densities and relevant temperatures. A metamagnetic behavior has been observed as a maximum in susceptibility versus magnetic field, when the spin-spin correlation has been considered. This maximum occurs at 45T ≤ B ≤ 100T for all densities and temperatures. This behavior has not been observed in the case of spin-independent correlation function.

Rattleback dynamics and its reversal time of rotation.

PubMed

Kondo, Yoichiro; Nakanishi, Hiizu

2017-06-01

A rattleback is a rigid, semielliptic toy which exhibits unintuitive behavior; when it is spun in one direction, it soon begins pitching and stops spinning, then it starts to spin in the opposite direction, but in the other direction, it seems to spin just steadily. This puzzling behavior results from the slight misalignment between the principal axes for the inertia and those for the curvature; the misalignment couples the spinning with the pitching and the rolling oscillations. It has been shown that under the no-slip condition and without dissipation the spin can reverse in both directions, and Garcia and Hubbard obtained the formula for the time required for the spin reversal t_{r} [Proc. R. Soc. Lond. A 418, 165 (1988)1364-502110.1098/rspa.1988.0078]. In this work, we reformulate the rattleback dynamics in a physically transparent way and reduce it to a three-variable dynamics for spinning, pitching, and rolling. We obtain an expression of the Garcia-Hubbard formula for t_{r} by a simple product of four factors: (1) the misalignment angle, (2) the difference in the inverses of inertia moment for the two oscillations, (3) that in the radii for the two principal curvatures, and (4) the squared frequency of the oscillation. We perform extensive numerical simulations to examine validity and limitation of the formula, and find that (1) the Garcia-Hubbard formula is good for both spinning directions in the small spin and small oscillation regime, but (2) in the fast spin regime especially for the steady direction, the rattleback may not reverse and shows a rich variety of dynamics including steady spinning, spin wobbling, and chaotic behavior reminiscent of chaos in a dissipative system.

Rattleback dynamics and its reversal time of rotation

NASA Astrophysics Data System (ADS)

Kondo, Yoichiro; Nakanishi, Hiizu

2017-06-01

A rattleback is a rigid, semielliptic toy which exhibits unintuitive behavior; when it is spun in one direction, it soon begins pitching and stops spinning, then it starts to spin in the opposite direction, but in the other direction, it seems to spin just steadily. This puzzling behavior results from the slight misalignment between the principal axes for the inertia and those for the curvature; the misalignment couples the spinning with the pitching and the rolling oscillations. It has been shown that under the no-slip condition and without dissipation the spin can reverse in both directions, and Garcia and Hubbard obtained the formula for the time required for the spin reversal tr [Proc. R. Soc. Lond. A 418, 165 (1988), 10.1098/rspa.1988.0078]. In this work, we reformulate the rattleback dynamics in a physically transparent way and reduce it to a three-variable dynamics for spinning, pitching, and rolling. We obtain an expression of the Garcia-Hubbard formula for tr by a simple product of four factors: (1) the misalignment angle, (2) the difference in the inverses of inertia moment for the two oscillations, (3) that in the radii for the two principal curvatures, and (4) the squared frequency of the oscillation. We perform extensive numerical simulations to examine validity and limitation of the formula, and find that (1) the Garcia-Hubbard formula is good for both spinning directions in the small spin and small oscillation regime, but (2) in the fast spin regime especially for the steady direction, the rattleback may not reverse and shows a rich variety of dynamics including steady spinning, spin wobbling, and chaotic behavior reminiscent of chaos in a dissipative system.

Origin of Large and Highly Variable Changes in the Apparent Spin Frequencies of Accretion-Powered Millisecond Pulsars

NASA Astrophysics Data System (ADS)

Lamb, Frederick K.; Dorris, D.; Clare, A.; Van Wassenhove, S.; Yu, W.; Miller, M. C.

2006-09-01

The spin-frequency behavior of accretion-powered millisecond pulsars is usually inferred by power spectral analysis of their X-ray waveforms. The reported behavior of the spin frequencies of several accretion-powered millisecond pulsars is puzzling in two respects. First, analysis of the waveforms of these pulsars indicates that their spin frequencies are changing faster than predicted by the standard model of accretion torques. Second, there are wild swings of both signs in their apparent spin frequencies that are not correlated with the mass accretion rates inferred from their X-ray fluxes. We have computed the expected X-ray waveforms of pulsars like these, including special and general relativistic effects, and find that the changes in their waveforms produced by physically plausible changes in the flow of accreting matter onto their surfaces can explain their apparently anomalous spin-frequency behavior. This research was supported in part by NASA grant NAG 5-12030, NSF grant AST 0098399, and funds of the Fortner Endowed Chair at Illinois, and NSF grant AST 0098436 at Maryland.

Self-organized critical behavior and marginality in Ising spin glasses

NASA Astrophysics Data System (ADS)

Sharma, Auditya; Yeo, Joonhyun; Moore, M. A.

2018-05-01

We have studied numerically the states reached in a quench from various temperatures in the one-dimensional fully-connected Kotliar, Anderson and Stein Ising spin glass model. This is a model where there are long-range interactions between the spins which falls off as a power σ of their separation. We have made a detailed study in particular of the energies of the states reached in a quench from infinite temperature and their overlaps, including the spin glass susceptibility. In the regime where , where the model is similar to the Sherrington–Kirkpatrick model, we find that the spin glass susceptibility diverges logarithmically with increasing N, the number of spins in the system, whereas for it remains finite. We attribute the behavior for to self-organized critical behavior, where the system after the quench is close to the transition between states which have trivial overlaps and those with the non-trivial overlaps associated with replica symmetry breaking. We have also found by studying the distribution of local fields that the states reached in the quench have marginal stability but only when .

Modafinil In Debilitating fatigue After Stroke (MIDAS): study protocol for a randomised, double-blinded, placebo-controlled, crossover trial.

PubMed

Lillicrap, Thomas; Krishnamurthy, Venkatesh; Attia, John; Nilsson, Michael; Levi, Christopher R; Parsons, Mark W; Bivard, Andrew

2016-08-17

Fatigue is a common symptom in stroke survivors for which there is currently no proven therapy. Modafinil is a wakefulness-promoting agent with established benefits in other disease models. We aim to test if modafinil will improve patient's self-reported fatigue scores when compared to placebo and if therapy results in increased quality of life. MIDAS is a phase II, single-centre, prospective, double-blinded, randomised, crossover trial of modafinil for the treatment of persistent fatigue in survivors of ischaemic stroke. The inclusion criteria will require an average score of 12 or more across all domains of the Multi-dimensional Fatigue Inventory (MFI-20) and the diagnosis of a stroke more than 6 months prior. Patients will be randomised 1:1 to receive either modafinil 200 mg daily or placebo for a period of 6 weeks, after which a crossover will occur where patients who are on modafinil will begin taking placebo and vice versa. The primary outcome will be improvement in fatigue as measured by the MFI-20. Secondary outcomes will include changes in the Fatigue Severity Scale, improved cognition measured using the Montreal Cognitive Assessment, improvement in mood as determined by the Depression, Anxiety and Stress Scale and improvement in each patient's stroke-specific quality of life score. All participants will also undergo magnetic resonance imaging (MRI) at baseline, crossover and study conclusion to measure cerebral blood flow on arterial spin labelling and brain activity on resting state functional MRI. This study will comply with the CONSORT guidelines. The projected sample size requirement is 36 participants in a crossover trial giving a power of 80 % and a type-1 error rate of 0.05. MIDAS seeks to enhance the quality of life in stroke survivors by assisting or resolving stroke-associated fatigue. ACTRN12615000350527 , registered on the 17 April 2015. Protocol version 3, approved 16 June 2015.

Bilayer Ising system designed with half-integer spins: Magnetic hysteresis, compensation behaviors and phase diagrams

NASA Astrophysics Data System (ADS)

Kantar, Ersin

2016-08-01

In this paper, within the framework of the effective-field theory with correlation, mixed spin-1/2 and spin-3/2 bilayer system on a square lattice is studied. The characteristic behaviors for the magnetic hysteresis, compensation types and phase diagrams depending on effect of the surface and interface exchange parameters as well as crystal field are investigated. From the behavior of total magnetization as a function of the magnetic field and temperature, we obtain the single, double and triple hysteresis loops and the L-, Q-, P-, S-, and N-type compensation behaviors in the system. Moreover, we detect the more effective the J1 and crystal field parameters on the bilayer Ising model according to the behaviors of the phase diagrams.

Spin-polarized electron transport in hybrid graphene-BN nanoribbons

NASA Astrophysics Data System (ADS)

Gao, Song; Lu, Wei; Zheng, Guo-Hui; Jia, Yalei; Ke, San-Huang

2017-05-01

The experimental realization of hybrid graphene and h-BN provides a new way to modify the electronic and transport properties of graphene-based materials. In this work, we investigate the spin-polarized electron transport in hybrid graphene-BN zigzag nanoribbons by performing first-principles nonequilibrium Green’s function method calculations. A 100% spin-polarized electron transport in a large energy window around the Fermi level is found and this behavior is independent of the ribbon width as long as there contain 3 zigzag carbon chains. This behavior may be useful in making perfect spin filters.

Applications of the First-principles LDA+Usc Method to Spin-crossover Minerals: the NAL Phase and (Mg,Fe)CO3 ferromagnesite

NASA Astrophysics Data System (ADS)

Hsu, H.

2016-12-01

Spin crossover (SCO) in iron-bearing minerals has attracted tremendous attention in recent years, as SCO usually leads to anomalous changes of the elastic, conducting, and thermodynamic properties of these minerals. Possible geophysical effects of SCO have been anticipated as well. With the development of the local density approximation + self-consistent Hubbard U (LDA+Usc) method, first-principles calculations have elucidated SCO in many lower-mantle minerals. The success of LDA+Usc lies in its capability to correctly identify the ground state in a wide pressure range and to accurately determine the mechanism of SCO, including the transition pressure PT. In this talk, two recent LDA+Usc studies of SCO minerals are presented: the "new aluminous (NAL) phase" [1] and (Mg,Fe)CO3 ferromagnesite [2]. The former is considered as a main host of aluminum in the subducted basalt and may be related to the seismic heterogeneities, and the latter is believed to be the major carbon carrier in the Earth's lower mantle and play a key role in the deep carbon cycle. For both minerals, the abrupt change of iron quadrupole splitting and the volume/elastic anomalies accompanying the SCO obtained in our calculations are in great agreement with experiments. Our calculations also suggest that the spin transition pressure PT in the NAL phase is not very sensitive to temperature, due to its nearly degenerate low-spin (LS) states, in contrast with (Mg,Fe)O ferropericlase and (Mg,Fe)CO3 systems, in which PT significantly increases with temperature. By examining the overall performance of the LDA+Usc method in the NAL phase and ferromagnesite, along with our previous calculations for ferropericlase and Fe-bearing MgSiO3 bridgmanite [3-5], we have established LDA+Usc a highly reliable method to study iron-bearing minerals and related materials under high pressure. [1] H. Hsu, in preparation. [2] S.-C. Huang and H. Hsu, Phys. Rev. B (Rapid Comm.), in press. [3] H. Hsu and R. M. Wentzcovitch, Phys. Rev. B 90, 195205 (2014). [4] H. Hsu et al., Earth Planet. Sci. Lett. 359-360, 34 (2012). [5] H. Hsu et al., Phys. Rev. Lett. 106, 118501 (2011).

Role of initial correlation in coarsening of a ferromagnet

NASA Astrophysics Data System (ADS)

Chakraborty, Saikat; Das, Subir K.

2015-06-01

We study the dynamics of ordering in ferromagnets via Monte Carlo simulations of the Ising model, employing the Glauber spin-flip mechanism, in space dimensions d = 2 and 3, on square and simple cubic lattices. Results for the persistence probability and the domain growth are discussed for quenches to various temperatures (Tf) below the critical one (Tc), from different initial temperatures Ti ≥ Tc. In long time limit, for Ti>Tc, the persistence probability exhibits power-law decay with exponents θ ≃ 0.22 and ≃ 0.18 in d = 2 and 3, respectively. For finite Ti, the early time behavior is a different power-law whose life-time diverges and exponent decreases as Ti → Tc. The two steps are connected via power-law as a function of domain length and the crossover to the second step occurs when this characteristic length exceeds the equilibrium correlation length at T = Ti. Ti = Tc is expected to provide a new universality class for which we obtain θ ≡ θc ≃ 0.035 in d = 2 and ≃0.105 in d = 3. The time dependence of the average domain size ℓ, however, is observed to be rather insensitive to the choice of Ti.

Individual-collective crossover driven by particle size in dense assemblies of superparamagnetic nanoparticles

NASA Astrophysics Data System (ADS)

Ridier, Karl; Gillon, Béatrice; Chaboussant, Grégory; Catala, Laure; Mazérat, Sandra; Rivière, Eric; Mallah, Talal

2017-02-01

Prussian blue analogues (PBA) ferromagnetic nanoparticles CsIxNiII[CrIII(CN)6 ]z·3(H2O) embedded in CTA+ (cetyltrimethylammonium) matrix have been investigated by magnetometry and magnetic small-angle neutron scattering (SANS). Choosing particle sizes (diameter D = 4.8 and 8.6 nm) well below the single-domain radius and comparable volume fraction of particle, we show that the expected superparamagnetic regime for weakly anisotropic isolated magnetic particles is drastically affected due to the interplay of surface/volume anisotropies and dipolar interactions. For the smallest particles (D = 4.8 nm), magnetocrystalline anisotropy is enhanced by surface spins and drives the system into a regime of ferromagnetically correlated clusters characterized by a temperature-dependent magnetic correlation length Lmag which is experimentally accessible using magnetic SANS. For D = 8.6 nm particles, a superparamagnetic regime is recovered in a wide temperature range. We propose a model of interacting single-domain particles with axial anisotropy that accounts quantitatively for the observed behaviors in both magnetic regimes. Supplementary material in the form of one pdf file available from the Journal web page at http://https://doi.org/10.1140/epjb/e2017-70534-9

Investigation of charge injection and transport behavior in multilayer structure consisted of ferromagnetic metal and organic polymer under external fields

NASA Astrophysics Data System (ADS)

Zhao, Hua; Meng, Wei-Feng

2017-10-01

In this paper a five layer organic electronic device with alternately placed ferromagnetic metals and organic polymers: ferromagnetic metal/organic layer/ferromagnetic metal/organic layer/ferromagnetic metal, which is injected a spin-polarized electron from outsides, is studied theoretically using one-dimensional tight binding model Hamiltonian. We calculated equilibrium state behavior after an electron with spin is injected into the organic layer of this structure, charge density distribution and spin polarization density distribution of this injected spin-polarized electron, and mainly studied possible transport behavior of the injected spin polarized electron in this multilayer structure under different external electric fields. We analyze the physical process of the injected electron in this multilayer system. It is found by our calculation that the injected spin polarized electron exists as an electron-polaron state with spin polarization in the organic layer and it can pass through the middle ferromagnetic layer from the right-hand organic layer to the left-hand organic layer by the action of increasing external electric fields, which indicates that this structure may be used as a possible spin-polarized charge electronic device and also may provide a theoretical base for the organic electronic devices and it is also found that in the boundaries between the ferromagnetic layer and the organic layer there exist induced interface local dipoles due to the external electric fields.

Spin-up studies of the Space Shuttle Orbiter main gear tire

NASA Technical Reports Server (NTRS)

Daugherty, Robert H.; Stubbs, Sandy M.

1988-01-01

One of the factors needed to describe the wear behavior of the Space Shuttle Orbiter main gear tires is their behavior during the spin-up process. An experimental investigation of tire spin-up processes was conducted at the NASA Langley Research Center's Aircraft Landing Dynamics Facility. During the investigation, the influence of various parameters such as forward speed and sink speed on tire spin-up forces were evaluated. A mathematical model was developed to estimate drag forces and spin-up times and is presented. The effect of prerotation was explored and is discussed. Also included is a means of determining the sink speed of the orbiter at touchdown based upon the appearance of the rubber deposits left on the runway during spinup.

Influence of quantum phase transition on spin transport in the quantum antiferromagnet in the honeycomb lattice

NASA Astrophysics Data System (ADS)

Lima, L. S.

2017-06-01

We use the SU(3) Schwinger boson theory to study the spin transport properties of the two-dimensional anisotropic frustrated Heisenberg model in a honeycomb lattice at T = 0 with single ion anisotropy and third neighbor interactions. We have investigated the behavior of the spin conductivity for this model that presents exchange interactions J1 , J2 and J3 . We study the spin transport in the Bose-Einstein condensation regime where the bosons tz are condensed. Our results show an influence of the quantum phase transition point on the spin conductivity behavior. We also have made a diagrammatic expansion for the Green-function and did not obtain any significant change of the results.

Widom line, dynamical crossover, and percolation transition of supercritical oxygen via molecular dynamics simulations.

PubMed

Raman, Abhinav S; Li, Huiyong; Chiew, Y C

2018-01-07

Supercritical oxygen, a cryogenic fluid, is widely used as an oxidizer in jet propulsion systems and is therefore of paramount importance in gaining physical insights into processes such as transcritical and supercritical vaporization. It is well established in the scientific literature that the supercritical state is not homogeneous but, in fact, can be demarcated into regions with liquid-like and vapor-like properties, separated by the "Widom line." In this study, we identified the Widom line for oxygen, constituted by the loci of the extrema of thermodynamic response functions (heat capacity, volumetric thermal expansion coefficient, and isothermal compressibility) in the supercritical region, via atomistic molecular dynamics simulations. We found that the Widom lines derived from these response functions all coincide near the critical point until about 25 bars and 15-20 K, beyond which the isothermal compressibility line begins to deviate. We also obtained the crossover from liquid-like to vapor-like behavior of the translational diffusion coefficient, shear viscosity, and rotational relaxation time of supercritical oxygen. While the crossover of the translational diffusion coefficient and shear viscosity coincided with the Widom lines, the rotational relaxation time showed a crossover that was largely independent of the Widom line. Further, we characterized the clustering behavior and percolation transition of supercritical oxygen molecules, identified the percolation threshold based on the fractal dimension of the largest cluster and the probability of finding a cluster that spans the system in all three dimensions, and found that the locus of the percolation threshold also coincided with the isothermal compressibility Widom line. It is therefore clear that supercritical oxygen is far more complex than originally perceived and that the Widom line, dynamical crossovers, and percolation transitions serve as useful routes to better our understanding of the supercritical state.

Widom line, dynamical crossover, and percolation transition of supercritical oxygen via molecular dynamics simulations

NASA Astrophysics Data System (ADS)

Raman, Abhinav S.; Li, Huiyong; Chiew, Y. C.

2018-01-01

Supercritical oxygen, a cryogenic fluid, is widely used as an oxidizer in jet propulsion systems and is therefore of paramount importance in gaining physical insights into processes such as transcritical and supercritical vaporization. It is well established in the scientific literature that the supercritical state is not homogeneous but, in fact, can be demarcated into regions with liquid-like and vapor-like properties, separated by the "Widom line." In this study, we identified the Widom line for oxygen, constituted by the loci of the extrema of thermodynamic response functions (heat capacity, volumetric thermal expansion coefficient, and isothermal compressibility) in the supercritical region, via atomistic molecular dynamics simulations. We found that the Widom lines derived from these response functions all coincide near the critical point until about 25 bars and 15-20 K, beyond which the isothermal compressibility line begins to deviate. We also obtained the crossover from liquid-like to vapor-like behavior of the translational diffusion coefficient, shear viscosity, and rotational relaxation time of supercritical oxygen. While the crossover of the translational diffusion coefficient and shear viscosity coincided with the Widom lines, the rotational relaxation time showed a crossover that was largely independent of the Widom line. Further, we characterized the clustering behavior and percolation transition of supercritical oxygen molecules, identified the percolation threshold based on the fractal dimension of the largest cluster and the probability of finding a cluster that spans the system in all three dimensions, and found that the locus of the percolation threshold also coincided with the isothermal compressibility Widom line. It is therefore clear that supercritical oxygen is far more complex than originally perceived and that the Widom line, dynamical crossovers, and percolation transitions serve as useful routes to better our understanding of the supercritical state.

SQUID picovoltometry of single crystal Bi2Sr2CaCu2O(8+delta) - Observation of the crossover from high-temperature Arrhenius to low-temperature vortex-glass behavior

NASA Astrophysics Data System (ADS)

Safar, H.; Gammel, P. L.; Bishop, D. J.; Mitzi, D. B.; Kapitulnik, A.

1992-04-01

A SQUID voltmeter has been used to measure current-voltage curves in untwinned crystals of Bi2Sr2CaCu2O(8+delta) as a function of temperature and magnetic field. The data show a clear crossover from high-temperature Arrhenius behavior to a critical region associated with the low-temperature three-dimensional vortex-glass phase transition. The critical exponents v(z - 1) = 7 +/- 1 in this system are in accord with theoretical models and previous measurements in YBa2Cu3O7. The width of the critical region collapses below 2 T, reflecting the changing role of dimensionality with field.

Spin crossover in the CsFeII[CrIII(CN)6] Prussian blue analog: Phonons and thermodynamics from hybrid functionals

NASA Astrophysics Data System (ADS)

Middlemiss, Derek S.; Portinari, Damiano; Grey, Clare P.; Morrison, Carole A.; Wilson, Chick C.

2010-05-01

Solid-state lattice-dynamics calculations within the hybrid density-functional approach are applied to the study of the thermally induced Fe2+ lowspin(LS;S=0)↔highspin(HS;S=2) crossover (SCO) in the extended network of the CsFe[Cr(CN)6] Prussian blue analog. The variations in the thermodynamic parameters defining the SCO transition with the Fock exchange content (F0) of the functional are obtained and discussed, where, in keeping with the findings of previous studies of isolated complexes, it is found that an admixture F0≈14% provides reliable values. The transition is shown to be dominated by the entropy difference, ΔS , associated with the softening of low-frequency vibrational (vib) modes in the HS state, as has been suggested previously for a wide range of SCO materials, more than half of ΔSvib deriving from modes with wave numbers of 250cm-1 or less. Analysis of the influence of the spectroscopic selection rules upon the apparent SCO thermodynamics reveals that determinations based solely upon infrared or Raman frequencies, or upon their combination, lead to significant errors. The effect upon the SCO transition of the electronic entropy associated with the degenerate Fe2+ HS (eg2t2g4) configurations is also detailed, evidence for the existence of an associated dynamic Jahn-Teller distortion being presented. Optimized structures, bulk moduli, Γ -point vibrational frequencies, and crystal-field energy models are discussed for all relevant spin states.

Magnon-phonon interconversion in a dynamically reconfigurable magnetic material

NASA Astrophysics Data System (ADS)

Guerreiro, Sergio C.; Rezende, Sergio M.

2015-12-01

The ferrimagnetic insulator yttrium iron garnet (YIG) is an important material in the field of magnon spintronics, mainly because of its low magnetic losses. YIG also has very low acoustic losses, and for this reason the conversion of a state of magnetic excitation (magnons) into a state of lattice vibration (phonons), or vice versa, broadens its possible applications in spintronics. Since the magnetic parameters can be varied by some external action, the magnon-phonon interconversion can be tuned to perform a desired function. We present a quantum theory of the interaction between magnons and phonons in a ferromagnetic material subject to a dynamic variation of the applied magnetic field. It is shown that when the field gradient at the magnetoelastic crossover region is much smaller than a critical value, an initial elastic excitation can be completely converted into a magnetic excitation, or vice versa. This occurs with conservation of linear momentum and spin angular momentum, implying that phonons created by the conversion of magnons have spin angular momentum and carry spin current. It is shown further that if the system is initially in a quantum coherent state, its coherence properties are maintained regardless of the time dependence of the field.

Agent-based spin model for financial markets on complex networks: Emergence of two-phase phenomena

NASA Astrophysics Data System (ADS)

Kim, Yup; Kim, Hong-Joo; Yook, Soon-Hyung

2008-09-01

We study a microscopic model for financial markets on complex networks, motivated by the dynamics of agents and their structure of interaction. The model consists of interacting agents (spins) with local ferromagnetic coupling and global antiferromagnetic coupling. In order to incorporate more realistic situations, we also introduce an external field which changes in time. From numerical simulations, we find that the model shows two-phase phenomena. When the local ferromagnetic interaction is balanced with the global antiferromagnetic interaction, the resulting return distribution satisfies a power law having a single peak at zero values of return, which corresponds to the market equilibrium phase. On the other hand, if local ferromagnetic interaction is dominant, then the return distribution becomes double peaked at nonzero values of return, which characterizes the out-of-equilibrium phase. On random networks, the crossover between two phases comes from the competition between two different interactions. However, on scale-free networks, not only the competition between the different interactions but also the heterogeneity of underlying topology causes the two-phase phenomena. Possible relationships between the critical phenomena of spin system and the two-phase phenomena are discussed.

Spin filter effect of hBN/Co detector electrodes in a 3D topological insulator spin valve

NASA Astrophysics Data System (ADS)

Vaklinova, Kristina; Polyudov, Katharina; Burghard, Marko; Kern, Klaus

2018-03-01

Topological insulators emerge as promising components of spintronic devices, in particular for applications where all-electrical spin control is essential. While the capability of these materials to generate spin-polarized currents is well established, only very little is known about the spin injection/extraction into/out of them. Here, we explore the switching behavior of lateral spin valves comprising the 3D topological insulator Bi2Te2Se as channel, which is separated from ferromagnetic Cobalt detector contacts by an ultrathin hexagonal boron nitride (hBN) tunnel barrier. The corresponding contact resistance displays a notable variation, which is correlated with a change of the switching characteristics of the spin valve. For contact resistances below ~5 kΩ, the hysteresis in the switching curve reverses upon reversing the applied current, as expected for spin-polarized currents carried by the helical surface states. By contrast, for higher contact resistances an opposite polarity of the hysteresis loop is observed, which is independent of the current direction, a behavior signifying negative spin detection efficiency of the multilayer hBN/Co contacts combined with bias-induced spin signal inversion. Our findings suggest the possibility to tune the spin exchange across the interface between a ferromagnetic metal and a topological insulator through the number of intervening hBN layers.

Magnetic properties of magnetic bilayer Kekulene structure: A Monte Carlo study

NASA Astrophysics Data System (ADS)

Jabar, A.; Masrour, R.

2018-06-01

In the present work, we have studied the magnetic properties of magnetic bilayer Kekulene structure with mixed spin-5/2 and spin-2 Ising model using Monte Carlo study. The magnetic phase diagrams of mixed spins Ising model have been given. The thermal total, partial magnetization and magnetic susceptibilities of the mixed spin-5/2 and spin-2 Ising model on a magnetic bilayer Kekulene structure are obtained. The transition temperature has been deduced. The effect of crystal field and exchange interactions on the this bilayers has been studied. The partial and total magnetic hysteresis cycles of the mixed spin-5/2 and spin-2 Ising model on a magnetic bilayer Kekulene structure have been given. The superparamagnetism behavior is observed in magnetic bilayer Kekulene structure. The magnetic coercive field decreases with increasing the exchange interactions between σ-σ and temperatures values and increases with increasing the absolute value of exchange interactions between σ-S. The multiple hysteresis behavior appears.

Sudden transition and sudden change from open spin environments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hu, Zheng-Da; School of Science, Jiangnan University, Wuxi 214122; Xu, Jing-Bo, E-mail: xujb@zju.edu.cn

2014-11-15

We investigate the necessary conditions for the existence of sudden transition or sudden change phenomenon for appropriate initial states under dephasing. As illustrative examples, we study the behaviors of quantum correlation dynamics of two noninteracting qubits in independent and common open spin environments, respectively. For the independent environments case, we find that the quantum correlation dynamics is closely related to the Loschmidt echo and the dynamics exhibits a sudden transition from classical to quantum correlation decay. It is also shown that the sudden change phenomenon may occur for the common environment case and stationary quantum discord is found at themore » high temperature region of the environment. Finally, we investigate the quantum criticality of the open spin environment by exploring the probability distribution of the Loschmidt echo and the scaling transformation behavior of quantum discord, respectively. - Highlights: • Sudden transition or sudden change from open spin baths are studied. • Quantum discord is related to the Loschmidt echo in independent open spin baths. • Steady quantum discord is found in a common open spin bath. • The probability distribution of the Loschmidt echo is analyzed. • The scaling transformation behavior of quantum discord is displayed.« less

Composition-dependent magnetic response properties of Mn1 -xFexGe alloys

NASA Astrophysics Data System (ADS)

Mankovsky, S.; Wimmer, S.; Polesya, S.; Ebert, H.

2018-01-01

The composition-dependent behavior of the Dzyaloshinskii-Moriya interaction (DMI), the spin-orbit torque (SOT), as well as anomalous and spin Hall conductivities of Mn1 -xFexGe alloys have been investigated by first-principles calculations using the relativistic multiple scattering Korringa-Kohn-Rostoker (KKR) formalism. The Dxx component of the DMI exhibits a strong dependence on the Fe concentration, changing sign at x ≈0.85 in line with previous theoretical calculations as well as with experimental results demonstrating the change of spin helicity at x ≈0.8 . A corresponding behavior with a sign change at x ≈0.5 is predicted also for the Fermi-sea contribution to the SOT, because this is closely related to the DMI. In the case of anomalous and spin Hall effects it is shown that the calculated Fermi-sea contributions are rather small and the composition-dependent behavior of these effects are determined mainly by the electronic states at the Fermi level. The spin-orbit-induced scattering mechanisms responsible for both these effects suggest a common origin of the minimum of the anomalous Hall effect and the sign change of the spin Hall effect conductivities.

Surprising Behavior of Spinning Tops and Eggs on an Inclined Plane

ERIC Educational Resources Information Center

Cross, Rod

2016-01-01

A spinning top or a spinning hard-boiled egg is fascinating to observe since both objects can remain upright for a relatively long time without falling over. If spun at sufficient speed on a horizontal surface, the spin axis rises to a vertical position and the bottom end tends to remain fixed in position on the surface. If the initial spin is…

Effects of Spatio-Temporal Aliasing on Pilot Performance in Active Control Tasks

NASA Technical Reports Server (NTRS)

Zaal, Peter; Sweet, Barbara

2010-01-01

Spatio-temporal aliasing affects pilot performance and control behavior. For increasing refresh rates: 1) Significant change in control behavior: a) Increase in visual gain and neuromuscular frequency. b) Decrease in visual time delay. 2) Increase in tracking performance: a) Decrease in RMSe. b) Increase in crossover frequency.

Manipulating spins of magnetic molecules: Hysteretic behavior with respect to bias voltage

NASA Astrophysics Data System (ADS)

Płomińska, Anna; Misiorny, Maciej; Weymann, Ireneusz

2018-02-01

Formation of a magnetic hysteresis loop with respect to a bias voltage is investigated theoretically in a spin-valve device based on a single magnetic molecule. We consider a device consisting of two ferromagnetic electrodes bridged by a carbon nanotube, acting as a quantum dot, to which a spin-anisotropic molecule is exchange-coupled. Such a coupling allows for transfer of angular momentum between the molecule and a spin current flowing through the dot, and thus, for switching orientation of the molecular spin. We demonstrate that this current-induced switching process exhibits a hysteretic behavior with respect to a bias voltage applied to the device. The analysis is carried out with the use of the real-time diagrammatic technique in the lowest-order expansion of the tunnel coupling of the dot to electrodes. The influence of both the intrinsic properties of the spin-valve device (the spin polarization of electrodes and the coupling strength of the molecule to the dot) and those of the molecule itself (magnetic anisotropy and spin relaxation) on the size of the magnetic hysteresis loop is discussed.

Anisotropy of magnetic interactions and spin filter behavior in hexagonal (Ga,Mn)As nanoribbons

NASA Astrophysics Data System (ADS)

Nie, Ya; Lan, Mu; Zhang, Xi; Xiang, Gang

2017-09-01

The electronic and magnetic properties of Mn doped hexagonal GaAs nanoribbons ((Ga,Mn)As NRs) have been investigated using spin-polarized density functional theory (DFT), and the spin-resolved transport behaviors of (Ga,Mn)As NRs have also been studied with non-equilibrium Green function theory. The calculations show that every Mn dopant brings 4 Bohr magneton (μB) magnetic moment and the ground states of (Ga,Mn)As NRs are ferromagnetic (FM). The investigation of magnetic anisotropies shows that magnetic interactions are dependent on both the distribution directions of Mn atoms and the edge effect of the NRs. The studies of electronic structures and transport properties show that incorporation of Mn atom turns GaAs NR from semiconducting to half-metallic, which significantly enhances the spin-up conductivity and strongly weakens the spin-down conductivity, resulting in non-monatomic variations of spin-dependent conductivities. The nearly 100% spin polarization shown in (Ga,Mn)As NR may be used for low dimensional spin filters, even with as large a bias as 0.9 V. Also, (Ga,Mn)As NR can be used to generate a relatively stable spin-polarized current in a wide bias interval.

Assessment of long-range correlation in animal behavior time series: The temporal pattern of locomotor activity of Japanese quail (Coturnix coturnix) and mosquito larva (Culex quinquefasciatus)

NASA Astrophysics Data System (ADS)

Kembro, Jackelyn M.; Flesia, Ana Georgina; Gleiser, Raquel M.; Perillo, María A.; Marin, Raul H.

2013-12-01

Detrended Fluctuation Analysis (DFA) is a method that has been frequently used to determine the presence of long-range correlations in human and animal behaviors. However, according to previous authors using statistical model systems, in order to correctly use DFA different aspects should be taken into account such as: (1) the establishment by hypothesis testing of the absence of short term correlation, (2) an accurate estimation of a straight line in the log-log plot of the fluctuation function, (3) the elimination of artificial crossovers in the fluctuation function, and (4) the length of the time series. Taking into consideration these factors, herein we evaluated the presence of long-range correlation in the temporal pattern of locomotor activity of Japanese quail (Coturnix coturnix) and mosquito larva (Culex quinquefasciatus). In our study, modeling the data with the general autoregressive integrated moving average (ARFIMA) model, we rejected the hypothesis of short-range correlations (d=0) in all cases. We also observed that DFA was able to distinguish between the artificial crossover observed in the temporal pattern of locomotion of Japanese quail and the crossovers in the correlation behavior observed in mosquito larvae locomotion. Although the test duration can slightly influence the parameter estimation, no qualitative differences were observed between different test durations.

Cyanide-bridged decanuclear cobalt-iron cage.

PubMed

Shiga, Takuya; Tetsuka, Tamaki; Sakai, Kanae; Sekine, Yoshihiro; Nihei, Masayuki; Newton, Graham N; Oshio, Hiroki

2014-06-16

A cyanide-bridged decanuclear [Co6Fe4] cluster was synthesized by a one-pot reaction, and the magnetic properties and electronic configuration were investigated. The complex displayed thermally controlled electron-transfer-coupled spin transition (ETCST) behavior between Co(III) low-spin-NC-Fe(II) low-spin and Co(II) high-spin-NC-Fe(III) low-spin states, as confirmed by single-crystal X-ray, magnetic, and Mössbauer analyses.

Universality and phase diagrams of the Baxter-Wu Model in a Crystal Field: spin-1 and spin-3/2

NASA Astrophysics Data System (ADS)

Dias, D. A.; Xavier, J. C.; Plascak, J. A.

2017-11-01

Conventional finite-size scaling and conformal invariance theory are used in order to study the critical behavior of the spin-1 and spin-3/2 Baxter-Wu model. For spin-1 the results are similar to the Blume-Capel model. However, for spin-3/2, the phase diagram is much richer, and presents, besides a pentacritical point, an additional multicritical endpoint. In both cases, the universality class is the same as the spin-1/2 model, even at the multicritical points.

Atomic-scale dynamics of a model glass-forming metallic liquid: Dynamical crossover, dynamical decoupling, and dynamical clustering

DOE PAGES

Jaiswal, Abhishek; Egami, Takeshi; Zhang, Yang

2015-04-01

The phase behavior of multi-component metallic liquids is exceedingly complex because of the convoluted many-body and many-elemental interactions. Herein, we present systematic studies of the dynamic aspects of such a model ternary metallic liquid Cu 40Zr 51Al 9 using molecular dynamics simulation with embedded atom method. We observed a dynamical crossover from Arrhenius to super-Arrhenius behavior in the transport properties (diffusion coefficient, relaxation times, and shear viscosity) bordered at T x ~1300K. Unlike in many molecular and macromolecular liquids, this crossover phenomenon occurs in the equilibrium liquid state well above the melting temperature of the system (T m ~ 900K),more » and the crossover temperature is roughly twice of the glass-transition temperature (T g). Below T x, we found the elemental dynamics decoupled and the Stokes-Einstein relation broke down, indicating the onset of heterogeneous spatially correlated dynamics in the system mediated by dynamic communications among local configurational excitations. To directly characterize and visualize the correlated dynamics, we employed a non-parametric, unsupervised machine learning technique and identified dynamical clusters of atoms with similar atomic mobility. The revealed average dynamical cluster size shows an accelerated increase below T x and mimics the trend observed in other ensemble averaged quantities that are commonly used to quantify the spatially heterogeneous dynamics such as the non-Gaussian parameter and the four-point correlation function.« less

The unusual magnetism of nanoparticle LaCoO3.

PubMed

Durand, A M; Belanger, D P; Hamil, T J; Ye, F; Chi, S; Fernandez-Baca, J A; Booth, C H; Abdollahian, Y; Bhat, M

2015-05-08

Bulk and nanoparticle powders of LaCoO3 (LCO) were synthesized and their magnetic and structural properties were studied using SQUID magnetometry and neutron diffraction. The bulk and large nanoparticles exhibit weak ferromagnetism (FM) below T ≈ 85 K and a crossover from strong to weak antiferromagnetic (AFM) correlations near a transition expressed in the lattice parameters, To≈40 K. This crossover does not occur in the smallest nanoparticles; instead, the magnetic behavior is predominantly ferromagnetic. The amount of FM in the nanoparticles depends on the amount of Co3O4 impurity phase, which induces tensile strain on the LCO lattice. A core-interface model is introduced, with the core region exhibiting the AFM crossover and with FM in the interface region near surfaces and impurity phases.

The unusual magnetism of nanoparticle LaCoO 3

DOE PAGES

Durand, A. M.; Belanger, D. P.; Hamil, T. J.; ...

2015-04-15

Bulk and nanoparticle powders of LaCoO 3 (LCO) were synthesized and their magnetic and structural properties were studied using SQUID magnetometry and neutron diffraction. The bulk and large nanoparticles exhibit weak ferromagnetism (FM) below T≈85K and a crossover from strong to weak antiferromagnetic (AFM) correlations near a transition expressed in the lattice parameters, To ≈ 40 K. This crossover does not occur in the smallest nanoparticles; instead, the magnetic behavior is predominantly ferromagnetic. The amount of FM in the nanoparticles depends on the amount of Co 3O 4 impurity phase, which induces tensile strain on the LCO lattice. A core-interfacemore » model is introduced, with the core region exhibiting the AFM crossover and with FM in the interface region near surfaces and impurity phases.« less

The unusual magnetism of nanoparticle LaCoO3

NASA Astrophysics Data System (ADS)

Durand, A. M.; Belanger, D. P.; Hamil, T. J.; Ye, F.; Chi, S.; Fernandez-Baca, J. A.; Booth, C. H.; Abdollahian, Y.; Bhat, M.

2015-05-01

Bulk and nanoparticle powders of LaCoO3 (LCO) were synthesized and their magnetic and structural properties were studied using SQUID magnetometry and neutron diffraction. The bulk and large nanoparticles exhibit weak ferromagnetism (FM) below T ≈ 85 K and a crossover from strong to weak antiferromagnetic (AFM) correlations near a transition expressed in the lattice parameters, To≈40 K. This crossover does not occur in the smallest nanoparticles; instead, the magnetic behavior is predominantly ferromagnetic. The amount of FM in the nanoparticles depends on the amount of Co3O4 impurity phase, which induces tensile strain on the LCO lattice. A core-interface model is introduced, with the core region exhibiting the AFM crossover and with FM in the interface region near surfaces and impurity phases.

Persistent-random-walk approach to anomalous transport of self-propelled particles

NASA Astrophysics Data System (ADS)

Sadjadi, Zeinab; Shaebani, M. Reza; Rieger, Heiko; Santen, Ludger

2015-06-01

The motion of self-propelled particles is modeled as a persistent random walk. An analytical framework is developed that allows the derivation of exact expressions for the time evolution of arbitrary moments of the persistent walk's displacement. It is shown that the interplay of step length and turning angle distributions and self-propulsion produces various signs of anomalous diffusion at short time scales and asymptotically a normal diffusion behavior with a broad range of diffusion coefficients. The crossover from the anomalous short-time behavior to the asymptotic diffusion regime is studied and the parameter dependencies of the crossover time are discussed. Higher moments of the displacement distribution are calculated and analytical expressions for the time evolution of the skewness and the kurtosis of the distribution are presented.

Creation of artificial skyrmions and antiskyrmions by anisotropy engineering

NASA Astrophysics Data System (ADS)

Zhang, S.; Petford-Long, A. K.; Phatak, C.

2016-08-01

Topologically non-trivial spin textures form a fundamental paradigm in solid-state physics and present unique opportunities to explore exciting phenomena such as the topological Hall effect. One such texture is a skyrmion, in which the spins can be mapped to point in all directions wrapping around a sphere. Understanding the formation of these spin textures, and their energetic stability, is crucial in order to control their behavior. In this work, we report on controlling the perpendicular anisotropy of continuous Co/Pt multilayer films with ion irradiation to form unique spin configurations of artificial skyrmions and antiskyrmions that are stabilized by their demagnetization energy. We elucidate their behavior using aberration-corrected Lorentz transmission electron microscopy. We also discuss the energetic stability of these structures studied through in-situ magnetizing experiments performed at room temperature, combined with micromagnetic simulations that successfully reproduce the spin textures and behavior. This research offers new opportunities towards creation of artificial skyrmion or antiskyrmion lattices that can be used to investigate not only fundamental properties of their interaction with electron currents but also technological applications such as artificial magnonic crystals.

Creation of artificial skyrmions and antiskyrmions by anisotropy engineering

DOE PAGES

Zhang, S.; Petford-Long, A. K.; Phatak, C.

2016-08-10

Topological spin textures form a fundamental paradigm in solid state physics and present unique opportunities to explore exciting phenomena such as the quantum Hall effect. One such non-trivial spin texture is a skyrmion, in which the spins can be mapped to point in all directions wrapping around a sphere. Understanding the formation of these spin textures, and their topological and energetic stability, is crucial in order to control their behavior. In this work, we report on controlling the anisotropy of continuous Co/Pt multilayer films with ion irradiation to form unique domain configurations of artificial skyrmions and antiskyrmions. We elucidate theirmore » behavior using aberration-corrected Lorentz transmission electron microscopy. We also discuss the energetic stability of these structures studied through in-situ magnetizing experiments performed at room temperature, combined with micromagnetic simulations that successfully reproduce the spin textures and behavior. As a result, this research offers new opportunities towards creation of artificial skyrmion or antiskyrmion lattices that can be used to investigate not only fundamental properties of their interaction with electron currents but also technological applications such as artificial magnonic crystals.« less

Creation of artificial skyrmions and antiskyrmions by anisotropy engineering

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, S.; Petford-Long, A. K.; Phatak, C.

Topological spin textures form a fundamental paradigm in solid state physics and present unique opportunities to explore exciting phenomena such as the quantum Hall effect. One such non-trivial spin texture is a skyrmion, in which the spins can be mapped to point in all directions wrapping around a sphere. Understanding the formation of these spin textures, and their topological and energetic stability, is crucial in order to control their behavior. In this work, we report on controlling the anisotropy of continuous Co/Pt multilayer films with ion irradiation to form unique domain configurations of artificial skyrmions and antiskyrmions. We elucidate theirmore » behavior using aberration-corrected Lorentz transmission electron microscopy. We also discuss the energetic stability of these structures studied through in-situ magnetizing experiments performed at room temperature, combined with micromagnetic simulations that successfully reproduce the spin textures and behavior. As a result, this research offers new opportunities towards creation of artificial skyrmion or antiskyrmion lattices that can be used to investigate not only fundamental properties of their interaction with electron currents but also technological applications such as artificial magnonic crystals.« less

Antiferromagnetic d-Electron Exchange via a Spin-Singlet π-Electron Ground State in an Organic Conductor

NASA Astrophysics Data System (ADS)

Tokumoto, T.; Brooks, J. S.; Oshima, Y.; Choi, E. S.; Brunel, L. C.; Akutsu, H.; Kaihatsu, T.; Yamada, J.; van Tol, J.

2008-04-01

Electron spin resonance reveals the spin behavior of conduction (π) and localized (d) electrons in β-(BDA-TTP)2MCl4 (M=Fe, Ga). Both the Ga3+(S=0) and Fe3+(S=5/2) compounds exhibit a metal-insulator transition at 113 K with the simultaneous formation of a spin-singlet ground state in the π electron system of the donor molecules. The behavior is consistent with charge ordering in β-(BDA-TTP)2MCl4 at the metal-insulator transition. At 5 K, the Fe3+ compound orders antiferromagnetically, even though the π electrons, which normally would facilitate magnetic exchange, are localized nonmagnetic singlets.

Behavioral and cognitive effect of theophylline: a dose-response study.

PubMed

Stein, M A; Lerner, C A

1993-02-01

The behavioral and cognitive effects of theophylline were studied in 14 asymptomatic asthmatic children. A double-blind crossover design was used with two dosage levels. Conners parent ratings suggest behavioral improvement by the second week of treatment, regardless of dosage or order of administration. No effects were found on cognitive measures. We conclude that the majority of behavior problems associated with theophylline occur during the induction phase, and that for most children behavior and attention problems rapidly return to baseline or improve.

Nutrition Education Brings Behavior and Knowledge Change in Limited-Resource Older Adults

ERIC Educational Resources Information Center

McClelland, Jacquelyn W.; Jayaratne, K.S.U.; Bird, Carolyn L.

2013-01-01

A prospective, controlled, randomized, crossover design was used to examine a nutrition education curriculum's effects on knowledge and behavior of 463 limited-resource older adults in 13 counties. Counties were randomized to begin with the treatment or control curriculum and then the remaining curriculum. Participants completed a pre-test…

Dynamical properties of water-methanol solutions

NASA Astrophysics Data System (ADS)

Mallamace, Francesco; Corsaro, Carmelo; Mallamace, Domenico; Vasi, Cirino; Vasi, Sebastiano; Stanley, H. Eugene

2016-02-01

We study the relaxation times tα in the water-methanol system. We examine new data and data from the literature in the large temperature range 163 < T < 335 K obtained using different experimental techniques and focus on how tα affects the hydrogen bond structure of the system and the hydrophobicity of the alcohol methyl group. We examine the relaxation times at a fixed temperature as a function of the water molar fraction XW and observe two opposite behaviors in their curvature when the system moves from high to low T regimes. This behavior differs from that of an ideal solution in that it has excess values located at different molar fractions (XW = 0.5 for high T and 0.75 in the deep supercooled regime). We analyze the data and find that above a crossover temperature T ˜ 223 K, hydrophobicity plays a significant role and below it the water tetrahedral network dominates. This temperature is coincident with the fragile-to-strong dynamical crossover observed in confined water and supports the liquid-liquid phase transition hypothesis. At the same time, the reported data suggest that this crossover temperature (identified as the Widom line temperature) also depends on the alcohol concentration.

Synchronization in scale-free networks: The role of finite-size effects

NASA Astrophysics Data System (ADS)

Torres, D.; Di Muro, M. A.; La Rocca, C. E.; Braunstein, L. A.

2015-06-01

Synchronization problems in complex networks are very often studied by researchers due to their many applications to various fields such as neurobiology, e-commerce and completion of tasks. In particular, scale-free networks with degree distribution P(k)∼ k-λ , are widely used in research since they are ubiquitous in Nature and other real systems. In this paper we focus on the surface relaxation growth model in scale-free networks with 2.5< λ <3 , and study the scaling behavior of the fluctuations, in the steady state, with the system size N. We find a novel behavior of the fluctuations characterized by a crossover between two regimes at a value of N=N* that depends on λ: a logarithmic regime, found in previous research, and a constant regime. We propose a function that describes this crossover, which is in very good agreement with the simulations. We also find that, for a system size above N* , the fluctuations decrease with λ, which means that the synchronization of the system improves as λ increases. We explain this crossover analyzing the role of the network's heterogeneity produced by the system size N and the exponent of the degree distribution.

Comment on ``Size-dependent scaling of perpendicular exchange bias in magnetic nanostructures''

NASA Astrophysics Data System (ADS)

Baltz, V.; Bollero, A.; Rodmacq, B.; Dieny, B.; Sort, J.

2008-01-01

From results at one given temperature (300K) , Malinowski [Phys. Rev. B 75, 012413 (2007)] draw the conclusion that lateral confinement of ferromagnetic-antiferromagnetic exchange-biased structures does not enhance thermally activated unpinning of the antiferromagnetic spins, which would thus contrast with a recent report [Phys. Rev. Lett. 94, 117201 (2005)], as explicitly mentioned in their manuscript. In this Comment, we discuss why such a conclusion might need revision above a “crossover temperature,” as evidenced in the literature. The value of such a crossover temperature certainly depends on the magnetic parameters of each system studied, e.g., anisotropy and exchange stiffness. From the above reasons, and contrary to the statement of Malinowski , we rather think that their results might well agree with the report to which they refer to. In our Comment we notably aim at complementing the conclusion of Malinowski by explaining why some differences between the two studies are observed at one given temperature, and why it might be expected to observe similar trends over a whole range of temperatures.

Spin manipulating vector & tensor polarized deuterons stored in COSY

NASA Astrophysics Data System (ADS)

Morozov, V. S.; Krisch, A. D.; Leonova, M. A.; Raymond, R. S.; Sivers, D. W.; Wong, V. K.; Yonehara, K.; Gebel, R.; Lehrach, A.; Lorentz, B.; Maier, R.; Prasuhn, D.; Schnase, A.; Stockhorst, H.; Eversheim, D.; Hinterberger, F.; Rohdjess, H.; Ulbrich, K.

2006-04-01

We recently studied the spin manipulation of a simultaneously vector and tensor polarized deuteron beam stored at 1.85 GeV/c in the COSY Cooler Synchrotron. Using the EDDA detector, we first calibrated the vector and tensor analyzing powers, which were earlier unmeasured at 1.85 GeV/c; this allowed us to measure the absolute values of both the vector and tensor polarizations. Then we manipulated the deuteron's polarization by sweeping the frequency of a ferrite rf dipole through an rf-induced spin resonance. We first experimentally determined the resonance's frequency and then varied the rf dipole's frequency sweep range δf and frequency ramp time δt to maximize the spin-flip efficiency. We then obtained a measured vector spin-flip efficiency of 98.5 ± 0.3% [1]. We also studied, in detail, the behavior of the tensor polarization during spin manipulation; these new data may allow a better understanding of the interesting quantum behavior of spin-1 bosons. This research was supported by the German BMBF Science Ministry. [1] V.S. Morozov et al., Phys. Rev. ST Accel. Beams 8, 061001 (2005).

Random crystal field effect on the magnetic and hysteresis behaviors of a spin-1 cylindrical nanowire

NASA Astrophysics Data System (ADS)

Zaim, N.; Zaim, A.; Kerouad, M.

2017-02-01

In this work, the magnetic behavior of the cylindrical nanowire, consisting of a ferromagnetic core of spin-1 atoms surrounded by a ferromagnetic shell of spin-1 atoms is studied in the presence of a random crystal field interaction. Based on Metropolis algorithm, the Monte Carlo simulation has been used to investigate the effects of the concentration of the random crystal field p, the crystal field D and the shell exchange interaction Js on the phase diagrams and the hysteresis behavior of the system. Some characteristic behaviors have been found, such as the first and second-order phase transitions joined by tricritical point for appropriate values of the system parameters, triple and isolated critical points can be also found. Depending on the Hamiltonian parameters, single, double and para hysteresis regions are explicitly determined.

Spin-Dependent Phenomena in Graphene

DTIC Science & Technology

2012-03-15

scattering on spin relaxation: By investigating the effect of gold dopants on spin transport, we concluded that charged impurity scattering is not...transport in graphene spin valves consisting of an ultrathin sheet of graphene (single or bilayer) contacted by ferromagnetic cobalt electrodes...workfunction cannot explain the observed behavior. The second effect was that the mobility was reduced by the transition metal dopants , as indicated by

Spin transport in epitaxial graphene

NASA Astrophysics Data System (ADS)

Tbd, -

2014-03-01

Spintronics is a paradigm focusing on spin as the information vector in fast and ultra-low-power non volatile devices such as the new STT-MRAM. Beyond its widely distributed application in data storage it aims at providing more complex architectures and a powerful beyond CMOS solution for information processing. The recent discovery of graphene has opened novel exciting opportunities in terms of functionalities and performances for spintronics devices. We will present experimental results allowing us to assess the potential of graphene for spintronics. We will show that unprecedented highly efficient spin information transport can occur in epitaxial graphene leading to large spin signals and macroscopic spin diffusion lengths (~ 100 microns), a key enabler for the advent of envisioned beyond-CMOS spin-based logic architectures. We will also show that how the device behavior is well explained within the framework of the Valet-Fert drift-diffusion equations. Furthermore, we will show that a thin graphene passivation layer can prevent the oxidation of a ferromagnet, enabling its use in novel humide/ambient low-cost processes for spintronics devices, while keeping its highly surface sensitive spin current polarizer/analyzer behavior and adding new enhanced spin filtering property. These different experiments unveil promising uses of graphene for spintronics.

Critical behavior of the quantum spin- {1}/{2} anisotropic Heisenberg model

NASA Astrophysics Data System (ADS)

Sousa, J. Ricardo de

A two-step renormalization group approach - a decimation followed by an effective field renormalization group (EFRG) - is proposed in this work to study the critical behavior of the quantum spin- {1}/{2} anisotropic Heisenberg model. The new method is illustrated by employing approximations in which clusters with one, two and three spins are used. The values of the critical parameter and critical exponent, in two- and three-dimensional lattices, for the Ising and isotropic Heisenberg limits are calculated and compared with other renormalization group approaches and exact (or series) results.

Divergent Coordination Chemistry: Parallel Synthesis of [2×2] Iron(II) Grid-Complex Tauto-Conformers.

PubMed

Schäfer, Bernhard; Greisch, Jean-François; Faus, Isabelle; Bodenstein, Tilmann; Šalitroš, Ivan; Fuhr, Olaf; Fink, Karin; Schünemann, Volker; Kappes, Manfred M; Ruben, Mario

2016-08-26

The coordination of iron(II) ions by a homoditopic ligand L with two tridentate chelates leads to the tautomerism-driven emergence of complexity, with isomeric tetramers and trimers as the coordination products. The structures of the two dominant [Fe(II) 4 L4 ](8+) complexes were determined by X-ray diffraction, and the distinctness of the products was confirmed by ion-mobility mass spectrometry. Moreover, these two isomers display contrasting magnetic properties (Fe(II) spin crossover vs. a blocked Fe(II) high-spin state). These results demonstrate how the coordination of a metal ion to a ligand that can undergo tautomerization can increase, at a higher hierarchical level, complexity, here expressed by the formation of isomeric molecular assemblies with distinct physical properties. Such results are of importance for improving our understanding of the emergence of complexity in chemistry and biology. © 2016 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.

Tunable magnetism in metal adsorbed fluorinated nanoporous graphene

DOE PAGES

Kumar, Pankaj; Sharma, Vinit; Reboredo, Fernando A.; ...

2016-08-24

Developing nanostructures with tunable magnetic states is crucial for designing novel data storage and quantum information devices. Using density functional theory, we study the thermodynamic stability and magnetic properties of tungsten adsorbed tri-vacancy fluorinated (TVF) graphene. We demonstrate a strong structure-property relationship and its response to external stimuli via defect engineering in graphene-based materials. Complex interplay between defect states and the chemisorbed atom results in a large magnetic moment of 7 μ B along with high in-plane magneto-crystalline anisotropy energy (MAE) of 17 meV. Under the influence of electric field, spin crossover effect accompanied by a change in the MAEmore » is observed. The ascribed change in spin-configuration is caused by the modification of exchange coupling between defect states and a change in the occupation of d-orbitals of the metal complex. In conclusion, our predictions open a promising way towards controlling the magnetic properties in graphene based spintronic and non-volatile memory devices.« less

Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide

PubMed Central

Plechinger, Gerd; Nagler, Philipp; Arora, Ashish; Schmidt, Robert; Chernikov, Alexey; del Águila, Andrés Granados; Christianen, Peter C.M.; Bratschitsch, Rudolf; Schüller, Christian; Korn, Tobias

2016-01-01

Monolayer transition-metal dichalcogenides have recently emerged as possible candidates for valleytronic applications, as the spin and valley pseudospin are directly coupled and stabilized by a large spin splitting. The optical properties of these two-dimensional crystals are dominated by tightly bound electron–hole pairs (excitons) and more complex quasiparticles such as charged excitons (trions). Here we investigate monolayer WS2 samples via photoluminescence and time-resolved Kerr rotation. In photoluminescence and in energy-dependent Kerr rotation measurements, we are able to resolve two different trion states, which we interpret as intravalley and intervalley trions. Using time-resolved Kerr rotation, we observe a rapid initial valley polarization decay for the A exciton and the trion states. Subsequently, we observe a crossover towards exciton–exciton interaction-related dynamics, consistent with the formation and decay of optically dark A excitons. By contrast, resonant excitation of the B exciton transition leads to a very slow decay of the Kerr signal. PMID:27586517

Quasiclassical analysis of vortex lattice states in Rashba noncentrosymmetric superconductors

NASA Astrophysics Data System (ADS)

Dan, Yuichiro; Ikeda, Ryusuke

2015-10-01

Vortex lattice states occurring in noncentrosymmetric superconductors with a spin-orbit coupling of Rashba type under a magnetic field parallel to the symmetry plane are examined by assuming the s -wave pairing case and in an approach combining the quasiclassical theory with the Landau level expansion of the superconducting order parameter. The resulting field-temperature phase diagrams include not only a discontinuous transition but a continuous crossover between different vortex lattice structures, and, further, a critical end point of a structural transition line is found at an intermediate field and a low temperature in the present approach. It is pointed out that the strange field dependence of the vortex lattice structure is a consequence of that of its anisotropy stemming from the Rashba spin-orbit coupling, and that the critical end point is related to the helical phase modulation peculiar to these materials in the ideal Pauli-limited case. Furthermore, calculation results on the local density of states detectable in STM experiments are also presented.

Electron-nuclear coherent spin oscillations probed by spin-dependent recombination

NASA Astrophysics Data System (ADS)

Azaizia, S.; Carrère, H.; Sandoval-Santana, J. C.; Ibarra-Sierra, V. G.; Kalevich, V. K.; Ivchenko, E. L.; Bakaleinikov, L. A.; Marie, X.; Amand, T.; Kunold, A.; Balocchi, A.

2018-04-01

We demonstrate the triggering and detection of coherent electron-nuclear spin oscillations related to the hyperfine interaction in Ga deep paramagnetic centers in GaAsN by band-to-band photoluminescence without an external magnetic field. In contrast to other point defects such as Cr4 + in SiC, Ce3 + in yttrium aluminum garnet crystals, nitrogen-vacancy centers in diamond, and P atoms in silicon, the bound-electron spin in Ga centers is not directly coupled to the electromagnetic field via the spin-orbit interaction. However, this apparent drawback can be turned into an advantage by exploiting the spin-selective capture of conduction band electrons to the Ga centers. On the basis of a pump-probe photoluminescence experiment we measure directly in the temporal domain the hyperfine constant of an electron coupled to a gallium defect in GaAsN by tracing the dynamical behavior of the conduction electron spin-dependent recombination to the defect site. The hyperfine constants and the relative abundance of the nuclei isotopes involved can be determined without the need of an electron spin resonance technique and in the absence of any magnetic field. Information on the nuclear and electron spin relaxation damping parameters can also be estimated from the oscillation amplitude decay and the long-time-delay behavior.

Complex Terahertz and Direct Current Inverse Spin Hall Effect in YIG/Cu1-xIrx Bilayers Across a Wide Concentration Range.

PubMed

Cramer, Joel; Seifert, Tom; Kronenberg, Alexander; Fuhrmann, Felix; Jakob, Gerhard; Jourdan, Martin; Kampfrath, Tobias; Kläui, Mathias

2018-02-14

We measure the inverse spin Hall effect of Cu 1-x Ir x thin films on yttrium iron garnet over a wide range of Ir concentrations (0.05 ⩽ x ⩽ 0.7). Spin currents are triggered through the spin Seebeck effect, either by a continuous (dc) temperature gradient or by ultrafast optical heating of the metal layer. The spin Hall current is detected by electrical contacts or measurement of the emitted terahertz radiation. With both approaches, we reveal the same Ir concentration dependence that follows a novel complex, nonmonotonous behavior as compared to previous studies. For small Ir concentrations a signal minimum is observed, whereas a pronounced maximum appears near the equiatomic composition. We identify this behavior as originating from the interplay of different spin Hall mechanisms as well as a concentration-dependent variation of the integrated spin current density in Cu 1-x Ir x . The coinciding results obtained for dc and ultrafast stimuli provide further support that the spin Seebeck effect extends to terahertz frequencies, thus enabling a transfer of established spintronic measurement schemes into the terahertz regime. Our findings also show that the studied material allows for efficient spin-to-charge conversion even on ultrafast time scales.

2D CFT partition functions at late times

NASA Astrophysics Data System (ADS)

Dyer, Ethan; Gur-Ari, Guy

2017-08-01

We consider the late time behavior of the analytically continued partition function Z( β + it) Z( β - it) in holographic 2 d CFTs. This is a probe of information loss in such theories and in their holographic duals. We show that each Virasoro character decays in time, and so information is not restored at the level of individual characters. We identify a universal decaying contribution at late times, and conjecture that it describes the behavior of generic chaotic 2 d CFTs out to times that are exponentially large in the central charge. It was recently suggested that at sufficiently late times one expects a crossover to random matrix behavior. We estimate an upper bound on the crossover time, which suggests that the decay is followed by a parametrically long period of late time growth. Finally, we discuss gravitationally-motivated integrable theories and show how information is restored at late times by a series of characters. This hints at a possible bulk mechanism, where information is restored by an infinite sum over non-perturbative saddles.

Anomalous Composition-Induced Crossover in the Magnetic Properties of the Itinerant-Electron Antiferromagnet Ca 1 - x Sr x Co 2 - y As 2

DOE PAGES

Sangeetha, N. S.; Smetana, V.; Mudring, A. -V.; ...

2017-12-20

We report the inference of Ying et al. [Europhys. Lett. 104, 67005 (2013)] of a composition-induced change from c-axis ordered-moment alignment in a collinear A-type antiferromagnetic (AFM) structure at small x to ab-plane alignment in an unknown AFM structure at larger x in Ca 1-xSr xCo 2-yAs 2 with the body-centered tetragonal ThCr 2Si 2 structure is confirmed. Our major finding is an anomalous magnetic behavior in the crossover region 0.2 ≲ x ≲ 0.3 between these two phases. Also, in this region the magnetic susceptibility vs temperature χ ab(T) measured with magnetic fields H applied in the ab planemore » exhibit typical AFM behaviors with cusps at the Néel temperatures of ~ 65 K, whereas χ c(T) and the low-temperature isothermal magnetization M c(H) with H aligned along the c axis exhibit extremely soft ferromagneticlike behaviors.« less

Anomalous Composition-Induced Crossover in the Magnetic Properties of the Itinerant-Electron Antiferromagnet Ca 1 - x Sr x Co 2 - y As 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sangeetha, N. S.; Smetana, V.; Mudring, A. -V.

We report the inference of Ying et al. [Europhys. Lett. 104, 67005 (2013)] of a composition-induced change from c-axis ordered-moment alignment in a collinear A-type antiferromagnetic (AFM) structure at small x to ab-plane alignment in an unknown AFM structure at larger x in Ca 1-xSr xCo 2-yAs 2 with the body-centered tetragonal ThCr 2Si 2 structure is confirmed. Our major finding is an anomalous magnetic behavior in the crossover region 0.2 ≲ x ≲ 0.3 between these two phases. Also, in this region the magnetic susceptibility vs temperature χ ab(T) measured with magnetic fields H applied in the ab planemore » exhibit typical AFM behaviors with cusps at the Néel temperatures of ~ 65 K, whereas χ c(T) and the low-temperature isothermal magnetization M c(H) with H aligned along the c axis exhibit extremely soft ferromagneticlike behaviors.« less

A Sequential Method to Prepare Polymorphs and Solvatomorphs of [Fe(1,3-bpp)2 ](ClO4 )2 ⋅nH2 O (n=0, 1, 2) with Varying Spin-Crossover Behaviour.

PubMed

Bartual-Murgui, Carlos; Codina, Carlota; Roubeau, Olivier; Aromí, Guillem

2016-08-26

Two polymorphs of the spin crossover (SCO) compound [Fe(1,3-bpp)2 ](ClO4 )2 (1 and 2; 1,3-bpp=2-(pyrazol-1-yl)-6-(pyrazol-3-yl)pyridine) were prepared using a novel, stepwise procedure. Crystals of 1 deposit from dry solvents, while 2 is obtained from a solid-state procedure, by sequentially removing lattice H2 O molecules from the solvatomorph [Fe(1,3-bpp)2 ](ClO4 )2 ⋅2 H2 O (2⋅2 H2 O), using single-crystal-to-single-crystal (SCSC) transformations. Hydrate 2⋅2 H2 O is obtained through the same reaction as 1, now with 2.5 % of water added. Compounds 2 and 2⋅2 H2 O are unstable in the atmosphere and absorb or lose one equivalent of water, respectively, to both yield the stable solvatomorph [Fe(1,3-bpp)2 ](ClO4 )2 ⋅H2 O (2⋅H2 O), also following SCSC processes. The four derivatives have been characterised by single-crystal X-ray diffraction (SCXRD). Furthermore, the homogeneity of the various compounds as well as their SCSC interconversions have been confirmed by powder X-ray diffraction (PXRD). Polymorphs 1 and 2 exhibit abrupt SCO behaviour near room temperature with T1/2↑ =279/316 K and T1/2↓ =276/314 K (near 40 K of shift) and different cooperativity. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Iron spin transitions in the lower mantle

NASA Astrophysics Data System (ADS)

McCammon, C.; Dubrovinsky, L.; Potapkin, V.; Glazyrin, K.; Kantor, A.; Kupenko, I.; Prescher, C.; Sinmyo, R.; Smirnov, G.; Chumakov, A.; Rüffer, R.

2012-04-01

Iron has the ability to adopt different electronic configurations (spin states), which can significantly influence mantle properties and dynamics. It is now generally accepted as a result of studies over the past decade that ferrous iron in (Mg,Fe)O undergoes a high-spin to low-spin transition in the mid-part of the lower mantle; however results on (Mg,Fe)(Si,Al)O3 perovskite, the dominant phase of the lower mantle, remain controversial. Identifying spin transitions in (Mg,Fe)(Si,Al)O3 perovskite presents a significant challenge. X-ray emission spectroscopy provides information on the bulk spin number, but cannot separate individual contributions. Nuclear forward scattering measures hyperfine interactions, but is not well suited to complex materials due to the non-uniqueness of fitting models. Energy-domain Mössbauer spectroscopy generally enables an unambiguous resolution of all hyperfine parameters which can be used to infer spin states; however high pressure measurements using conventional radioactive point sources require extremely long counting times. To solve this problem, we have developed an energy-domain synchrotron Mössbauer source that enables rapid measurement of spectra under extreme conditions (both high pressure and high temperature) with a quality generally sufficient to unambiguously deconvolute even highly complex spectra. We have used the newly developed method to measure high quality Mössbauer spectra of different compositions of (Mg,Fe)O and (Mg,Fe)(Si,Al)O3 perovskite at pressures up to 122 GPa and temperatures up to 2400 K. Experiments were carried out at the European Synchrotron Radiation Facility on the nuclear resonance beamline ID18 equipped with a portable laser heating system for diamond anvil cells. Our results confirm previous observations for (Mg,Fe)O that show a broad spin crossover region at high pressures and high temperatures, and show unambiguously that ferric iron in (Mg,Fe)(Si,Al)O3 perovskite remains in the high-spin state at conditions throughout the lower mantle. Electrical conductivity data of (Mg,Fe)(Si,Al)O3 perovskite are known to show a drop in conductivity above 50 GPa, which combined with our new results suggests that the currently controversial high-pressure transition of ferrous iron is indeed due to a high-spin to intermediate-spin transition at conditions near the top of the lower mantle. Our current picture of iron in the lower mantle is therefore of a relatively homogeneous spin state in (Mg,Fe)(Si,Al)O3 perovskite throughout most of the lower mantle: intermediate-spin ferrous iron and high-spin ferric iron. Different spin states are expected in ferrous iron in (Mg,Fe)(Si,Al)O3 perovskite only at the very top of the lower mantle (high spin) and at the very bottom (low spin). There is a broad transition from high-spin to low-spin ferrous iron in (Mg,Fe)O in the mid part of the lower mantle. Implications of these results for mantle properties and dynamics will be presented.

Scaling Behavior of the Spin Pumping Effect in Ferromagnet-Platinum Bilayers

NASA Astrophysics Data System (ADS)

Czeschka, F. D.; Dreher, L.; Brandt, M. S.; Weiler, M.; Althammer, M.; Imort, I.-M.; Reiss, G.; Thomas, A.; Schoch, W.; Limmer, W.; Huebl, H.; Gross, R.; Goennenwein, S. T. B.

2011-07-01

We systematically measured the dc voltage VISH induced by spin pumping together with the inverse spin Hall effect in ferromagnet-platinum bilayer films. In all our samples, comprising ferromagnetic 3d transition metals, Heusler compounds, ferrite spinel oxides, and magnetic semiconductors, VISH invariably has the same polarity, and scales with the magnetization precession cone angle. These findings, together with the spin mixing conductance derived from the experimental data, quantitatively corroborate the present theoretical understanding of spin pumping in combination with the inverse spin Hall effect.

Magnetic hierarchical deposition

NASA Astrophysics Data System (ADS)

Posazhennikova, Anna I.; Indekeu, Joseph O.

2014-11-01

We consider random deposition of debris or blocks on a line, with block sizes following a rigorous hierarchy: the linear size equals 1/λn in generation n, in terms of a rescaling factor λ. Without interactions between the blocks, this model is described by a logarithmic fractal, studied previously, which is characterized by a constant increment of the length, area or volume upon proliferation. We study to what extent the logarithmic fractality survives, if each block is equipped with an Ising (pseudo-)spin s=±1 and the interactions between those spins are switched on (ranging from antiferromagnetic to ferromagnetic). It turns out that the dependence of the surface topology on the interaction sign and strength is not trivial. For instance, deep in the ferromagnetic regime, our numerical experiments and analytical results reveal a sharp crossover from a Euclidean transient, consisting of aggregated domains of aligned spins, to an asymptotic logarithmic fractal growth. In contrast, deep into the antiferromagnetic regime the surface roughness is important and is shown analytically to be controlled by vacancies induced by frustrated spins. Finally, in the weak interaction regime, we demonstrate that the non-interacting model is extremal in the sense that the effect of the introduction of interactions is only quadratic in the magnetic coupling strength. In all regimes, we demonstrate the adequacy of a mean-field approximation whenever vacancies are rare. In sum, the logarithmic fractal character is robust with respect to the introduction of spatial correlations in the hierarchical deposition process.

Modulation of magnetism in transition-metal-doped two-dimensional GeS

NASA Astrophysics Data System (ADS)

Zhang, Chunxiao; Yang, Baoyong; Tang, Chao; He, Chaoyu; Li, Jin; Ouyang, Tao; Zhong, Jianxin

2018-06-01

Two-dimensional (2D) germanium monosulfide (GeS) is a promising nanoelectronic material with a desirable band gap, high carrier mobility, and anisotropic structures. In this work, we present a density functional theory study on the magnetism of 3d TM (TM  =  Fe, Co and Ni)-doped 2D GeS. We find that the TM atoms strongly bond to the GeS sheet with quite sizable binding energies due to the sp 3-like hybridization of 2D GeS. The Fe- and Co-doped GeS show nonzero magnetic ground states. Hubbard parameter U hardly affects the magnetic moment when U is no more than 6 eV. In particular, substitutional Fe (Fe@GeS) and substitutional Co (Co@GeS) present high-spin states with 4 μ B and 3 μ B. The magnetism of TM-doped 2D GeS mainly arises from the crystal field splitting and spin exchange splitting of TM-3d orbitals. The magnetic and electronic properties of the Fe@GeS and Co@GeS systems can be easily controlled in a small vertical external electric field (E ext). The underlying mechanism of spin crossover is that E ext affects the crystal field splitting and then shifts the relative positions of 3d orbitals, which tunes the spin configurations. These results render monolayer GeS a promising 2D material for applications in future spintronics.

Strongly Interacting Fermi Gases: Non-Equilibrium Dynamics and Dimensional Crossover

NASA Astrophysics Data System (ADS)

Sommer, Ariel

2015-05-01

Strongly interacting atomic Fermi gases near Feshbach resonances give access to a rich variety of phenomena in many-fermion physics and superfluidity. This flexible and microscopically well-characterized system provides a pristine platform in which to benchmark many-body theories. I will describe three experiments on gases of fermionic 6Li atoms. In the first experiment, we study spin transport in the return to equilibrium after a spin excitation. From the dynamics near equilibrium, we obtain spin transport coefficients over a range of temperatures and interaction strengths, and observe quantum-limited spin diffusion at unitarity. In separate experiments, we study the effect of dimensionality on the binding of pairs of fermions. We tune the system from three to two dimensions by adjusting the strength of a one-dimensional optical lattice, and measure the binding energy of fermion pairs using radio-frequency spectroscopy. In a third set of experiments, we study nonlinear excitations of a fermionic superfluid. Imprinting a phase jump on the superfluid order parameter causes a long-lived, localized density depletion that oscillates through the cloud. We measure the oscillation period and find that it corresponds to an emergent particle with an effective mass of up to several hundred times the bare mass. This excitation has been identified as a solitonic vortex that results from the decay of a planar soliton. This work was performed at the Massachusetts Institute of Technology under the supervision of Prof. Martin Zwierlein.

Universal Behavior of Quantum Spin Liquid and Optical Conductivity in the Insulator Herbertsmithite

NASA Astrophysics Data System (ADS)

Shaginyan, V. R.; Msezane, A. Z.; Stephanovich, V. A.; Popov, K. G.; Japaridze, G. S.

2018-04-01

We analyze optical conductivity with the goal to demonstrate experimental manifestation of a new state of matter, the so-called fermion condensate. Fermion condensates are realized in quantum spin liquids, exhibiting typical behavior of heavy-fermion metals. Measurements of the low-frequency optical conductivity collected on the geometrically frustrated insulator herbertsmithite provide important experimental evidence of the nature of its quantum spin liquid composed of spinons. To analyze recent measurements of the herbertsmithite optical conductivity at different temperatures, we employ a model of strongly correlated quantum spin liquid located near the fermion condensation phase transition. Our theoretical analysis of the optical conductivity allows us to expose the physical mechanism of its temperature dependence. We also predict a dependence of the optical conductivity on a magnetic field. We consider an experimental manifestation (optical conductivity) of a new state of matter (so-called fermion condensate) realized in quantum spin liquids, for, in many ways, they exhibit typical behavior of heavy-fermion metals. Measurements of the low-frequency optical conductivity collected on the geometrically frustrated insulator herbertsmithite produce important experimental evidence of the nature of its quantum spin liquid composed of spinons. To analyze recent measurements of the herbertsmithite optical conductivity at different temperatures, we employ a model of a strongly correlated quantum spin liquid located near the fermion condensation phase transition. Our theoretical analysis of the optical conductivity allows us to reveal the physical mechanism of its temperature dependence. We also predict a dependence of the optical conductivity on a magnetic field.

Compressed exponential relaxation in liquid silicon: Universal feature of the crossover from ballistic to diffusive behavior in single-particle dynamics

NASA Astrophysics Data System (ADS)

Morishita, Tetsuya

2012-07-01

We report a first-principles molecular-dynamics study of the relaxation dynamics in liquid silicon (l-Si) over a wide temperature range (1000-2200 K). We find that the intermediate scattering function for l-Si exhibits a compressed exponential decay above 1200 K including the supercooled regime, which is in stark contrast to that for normal "dense" liquids which typically show stretched exponential decay in the supercooled regime. The coexistence of particles having ballistic-like motion and those having diffusive-like motion is demonstrated, which accounts for the compressed exponential decay in l-Si. An attempt to elucidate the crossover from the ballistic to the diffusive regime in the "time-dependent" diffusion coefficient is made and the temperature-independent universal feature of the crossover is disclosed.

Onset of a Propagating Self-Sustained Spin Reversal Front in a Magnetic System

NASA Astrophysics Data System (ADS)

Kent, Andrew D.

2014-03-01

The energy released in a magnetic material by reversing spins as they relax toward equilibrium can lead to a dynamical magnetic instability in which all the spins in a sample rapidly reverse in a run-away process known as magnetic deflagration. A well-defined front separating reversed and un-reversed spins develops that propagates at a constant speed. This process is akin to a chemical reaction in which a flammable substance ignites and the resulting exothermic reaction leads via thermal conduction to increases in the temperature of an adjacent unburned substance that ignites it. In a magnetic system the reaction is the reversal of spins that releases Zeeman energy and the magnetic anisotropy barrier is the reaction's activation energy. An interesting aspect of magnetic systems is that these key energies-the activation energy and the energy released-can be independently controlled by applied magnetic fields enabling systematic studies of these magnetic instabilities. We have studied the instability that leads to the ignition of magnetic deflagration in a thermally driven Mn12-Ac molecular magnet single crystal. Each Mn12-ac molecule is a uniaxial nanomagnet with spin 10 and energy barrier of 60 K. We use a longitudinal field (a field parallel to the easy axis) to set the energy released and a transverse field to control the activation energy. A heat pulse is applied to one end of the crystal to initiate the process. We study the crossover between slow magnetic relaxation and rapid, self-sustained magnetic deflagration as a function of these fields at low temperature (0.5 K). An array of Hall sensors adjacent to a single crystal is used to detect and measure the speed of the spin-reversal front. I will describe a simple model we developed based on a reaction-diffusion process that describes our experimental findings. I will also discuss prospects for observing spin-fronts driven by magnetic dipole interactions between molecules that can be sonic, i.e. travel near the speed of sound (~ 1000 m/s). In collaboration with P. Subedi, S. Velez, F. Macià, S. Li, M. P. Sarachik, J. Tejada, S. Mukherjee and G. Christou. Supported by NSF-DMR-1006575.

Effects of Risperidone on Cognitive-Motor Performance and Motor Movements in Chronically Medicated Children

ERIC Educational Resources Information Center

Aman, Michael G.; Hollway, Jill A.; Leone, Sarah; Masty, Jessica; Lindsay, Ronald; Nash, Patricia; Arnold, L. Eugene

2009-01-01

This study was designed to explore the placebo-controlled effects of risperidone on cognitive-motor processes, dyskinetic movements, and behavior in children receiving maintenance risperidone therapy. Sixteen children aged 4-14 years with disruptive behavior were randomly assigned to drug order in a crossover study of risperidone and placebo for 2…

Investigations of the effect of nonmagnetic Ca substitution for magnetic Dy on spin-freezing in Dy₂Ti₂O₇.

PubMed

Anand, V K; Tennant, D A; Lake, B

2015-11-04

Physical properties of partially Ca substituted hole-doped Dy2Ti2O7 have been investigated by ac magnetic susceptibility χ(ac)(T), dc magnetic susceptibility χ(T), isothermal magnetization M(H) and heat capacity C(p)(T) measurements on Dy1.8Ca0.2Ti2O7. The spin-ice system Dy2Ti2O7 exhibits a spin-glass type freezing behavior near 16 K. Our frequency dependent χ(ac)(T) data of Dy1.8Ca0.2Ti2O7 show that the spin-freezing behavior is significantly influenced by Ca substitution. The effect of partial nonmagnetic Ca(2+) substitution for magnetic Dy(3+) is similar to the previous study on nonmagnetic isovalent Y(3+) substituted Dy(2-x)Y(x) Ti2O7 (for low levels of dilution), however the suppression of spin-freezing behavior is substantially stronger for Ca than Y. The Cole-Cole plot analysis reveals semicircular character and a single relaxation mode in Dy1.8Ca0.2Ti2O7 as for Dy2Ti2O7. No noticeable change in the insulating behavior of Dy2Ti2O7 results from the holes produced by 10% Ca(2+) substitution for Dy(3+) ions.

Self-Organized Critical Behavior:. the Evolution of Frozen Spin Networks Model in Quantum Gravity

NASA Astrophysics Data System (ADS)

Chen, Jian-Zhen; Zhu, Jian-Yang

In quantum gravity, we study the evolution of a two-dimensional planar open frozen spin network, in which the color (i.e. the twice spin of an edge) labeling edge changes but the underlying graph remains fixed. The mainly considered evolution rule, the random edge model, is depending on choosing an edge randomly and changing the color of it by an even integer. Since the change of color generally violate the gauge invariance conditions imposed on the system, detailed propagation rule is needed and it can be defined in many ways. Here, we provided one new propagation rule, in which the involved even integer is not a constant one as in previous works, but changeable with certain probability. In random edge model, we do find the evolution of the system under the propagation rule exhibits power-law behavior, which is suggestive of the self-organized criticality (SOC), and it is the first time to verify the SOC behavior in such evolution model for the frozen spin network. Furthermore, the increase of the average color of the spin network in time can show the nature of inflation for the universe.

Field-induced negative differential spin lifetime in silicon.

PubMed

Li, Jing; Qing, Lan; Dery, Hanan; Appelbaum, Ian

2012-04-13

We show that the electric-field-induced thermal asymmetry between the electron and lattice systems in pure silicon substantially impacts the identity of the dominant spin relaxation mechanism. Comparison of empirical results from long-distance spin transport devices with detailed Monte Carlo simulations confirms a strong spin depolarization beyond what is expected from the standard Elliott-Yafet theory even at low temperatures. The enhanced spin-flip mechanism is attributed to phonon emission processes during which electrons are scattered between conduction band valleys that reside on different crystal axes. This leads to anomalous behavior, where (beyond a critical field) reduction of the transit time between spin-injector and spin-detector is accompanied by a counterintuitive reduction in spin polarization and an apparent negative spin lifetime.

Probing the dynamics of 3He atoms adsorbed on MCM-41 with pulsed NMR

NASA Astrophysics Data System (ADS)

Huan, C.; Masuhara, N.; Adams, J.; Lewkowitz, M.; Sullivan, N. S.

2018-03-01

We report measurements of the nuclear spin-spin and spin-lattice relaxation times for 3He adsorbed on MCM-41 for temperatures 0.08 < T < 1.2 K. Deviations from Curie behavior are observed at low temperatures. The relaxation times exhibit a two-component behavior representing the differing dynamics of the mobile quasi-free molecules in the center of the tubes compared to the adsorbed layer on the walls. The amplitudes of the two components provide an accurate measure of the number of fluid-like molecules traveling in the center of the nanotubes.

Spin-glass behaviors in carrier polarity controlled Fe{sub 3−x}Ti{sub x}O{sub 4} semiconductor thin films

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yamahara, H., E-mail: yamahara@bioxide.t.u-tokyo.ac.jp; Seki, M.; Adachi, M.

2015-08-14

Carrier-type control of spin-glass (cluster spin-glass) is studied in order to engineer basic magnetic semiconductor elements using the memory functions of spin-glass. A key of carrier-polarity control in magnetite is the valence engineering between Fe(II) and Fe(III) that is achieved by Ti(IV) substitution. Single phases of (001)-oriented Fe{sub 3−x}Ti{sub x}O{sub 4} thin films have been obtained on spinel MgAl{sub 2}O{sub 4} substrates by pulsed laser deposition. Thermoelectric power measurements reveal that Ti-rich films (x = 0.8) show p-type conduction, while Ti-poor films (x = 0.6–0.75) show n-type conduction. The systematic Fe(III) reduction to Fe(II) followed by Ti(IV) substitution in the octahedral sublattice is confirmedmore » by the X-ray absorption spectra. All of the Fe{sub 3−x}Ti{sub x}O{sub 4} films (x = 0.6–0.8) exhibit ferrimagnetism above room temperature. Next, the spin-glass behaviors of Ti-rich Fe{sub 2.2}Ti{sub 0.8}O{sub 4} film are studied, since this magnetically diluted system is expected to exhibit the spin-glass behaviors. The DC magnetization and AC susceptibility measurements for the Ti-rich Fe{sub 2.2}Ti{sub 0.8}O{sub 4} film reveal the presence of the spin glass phase. Thermal- and magnetic-field-history memory effects are observed and are attributed to the long time-decay nature of remanent magnetization. The detailed analysis of the time-dependent thermoremanent magnetization reveals the presence of the cluster spin glass state.« less

NMR signal analysis to attribute the components to the solid/liquid phases present in mixes and ice creams.

PubMed

Mariette, François; Lucas, Tiphaine

2005-03-09

The NMR relaxation signals from complex products such as ice cream are hard to interpret because of the multiexponential behavior of the relaxation signal and the difficulty of attributing the NMR relaxation components to specific molecule fractions. An attribution of the NMR relaxation parameters is proposed, however, based on an approach that combines quantitative analysis of the spin-spin and spin-lattice relaxation times and the signal intensities with characterization of the ice cream components. We have been able to show that NMR can be used to describe the crystallized and liquid phases separately. The first component of the spin-spin and spin-lattice relaxation describes the behavior of the protons of the crystallized fat in the mix. The amount of fat crystals can then be estimated. In the case of ice cream, only the spin-lattice relaxation signal from the crystallized fraction is relevant. However, it enables the ice protons and the protons of the crystallized fat to be distinguished. The spin-lattice relaxation time can be used to describe the mobility of the protons in the different crystallized phases and also to quantify the amount of ice crystals and fat crystals in the ice cream. The NMR relaxation of the liquid phase of the mix has a biexponential behavior. A first component is attributable to the liquid fraction of the fat and to the sugars, while a second component is attributable to the aqueous phase. Overall, the study shows that despite the complexity of the NMR signal from ice cream, a number of relevant parameters can be extracted to study the influence of the formulation and of the process stages on the ice fraction, the crystallized fat fraction, and the liquid aqueous fraction.

Heat-driven spin torques in antiferromagnets

NASA Astrophysics Data System (ADS)

Białek, Marcin; Bréchet, Sylvain; Ansermet, Jean-Philippe

2018-04-01

Heat-driven magnetization damping, which is a linear function of a temperature gradient, is predicted in antiferromagnets by considering the sublattice dynamics subjected to a heat-driven spin torque. This points to the possibility of achieving spin torque oscillator behavior. The model is based on the magnetic Seebeck effect acting on sublattices which are exchange coupled. The heat-driven spin torque is estimated and the feasibility of detecting this effect is discussed.

Domino model for geomagnetic field reversals.

PubMed

Mori, N; Schmitt, D; Wicht, J; Ferriz-Mas, A; Mouri, H; Nakamichi, A; Morikawa, M

2013-01-01

We solve the equations of motion of a one-dimensional planar Heisenberg (or Vaks-Larkin) model consisting of a system of interacting macrospins aligned along a ring. Each spin has unit length and is described by its angle with respect to the rotational axis. The orientation of the spins can vary in time due to spin-spin interaction and random forcing. We statistically describe the behavior of the sum of all spins for different parameters. The term "domino model" in the title refers to the interaction among the spins. We compare the model results with geomagnetic field reversals and dynamo simulations and find strikingly similar behavior. The aggregate of all spins keeps the same direction for a long time and, once in a while, begins flipping to change the orientation by almost 180 degrees (mimicking a geomagnetic reversal) or to move back to the original direction (mimicking an excursion). Most of the time the spins are aligned or antialigned and deviate only slightly with respect to the rotational axis (mimicking the secular variation of the geomagnetic pole with respect to the geographic pole). Reversals are fast compared to the times in between and they occur at random times, both in the model and in the case of the Earth's magnetic field.

Spin-glass-like freezing of inner and outer surface layers in hollow γ-Fe 2O 3 nanoparticles

DOE PAGES

Khurshid, Hafsa; Lampen-Kelley, Paula; Iglesias, Òscar; ...

2015-10-27

Disorder among surface spins largely dominates the magnetic response of ultrafine magnetic particle systems. In this work, we examine time-dependent magnetization in high-quality, monodisperse hollow maghemite nanoparticles (NPs) with a 14.8±0.5 nm outer diameter and enhanced surface-to-volume ratio. The nanoparticle ensemble exhibits spin-glass-like signatures in dc magnetic aging and memory protocols and ac magnetic susceptibility. The dynamics of the system slow near 50 K, and becomes frozen on experimental time scales below 20 K. Remanence curves indicate the development of magnetic irreversibility concurrent with the freezing of the spin dynamics. A strong exchange-bias effect and its training behavior point tomore » highly frustrated surface spins that rearrange much more slowly than interior spins with bulk coordination. Monte Carlo simulations of a hollow particle reproducing the experimental morphology corroborate strongly disordered surface layers with complex energy landscapes that underlie both glass-like dynamics and magnetic irreversibility. Calculated hysteresis loops reveal that magnetic behavior is not identical at the inner and outer surfaces, with spins at the outer surface layer of the 15 nm hollow particles exhibiting a higher degree of frustration. Lastly, our combined experimental and simulated results shed light on the origin of spin-glass-like phenomena and the important role played by the surface spins in magnetic hollow nanostructures.« less

Spin-glass-like freezing of inner and outer surface layers in hollow γ-Fe2O3 nanoparticles

PubMed Central

Khurshid, Hafsa; Lampen-Kelley, Paula; Iglesias, Òscar; Alonso, Javier; Phan, Manh-Huong; Sun, Cheng-Jun; Saboungi, Marie-Louise; Srikanth, Hariharan

2015-01-01

Disorder among surface spins is a dominant factor in the magnetic response of magnetic nanoparticle systems. In this work, we examine time-dependent magnetization in high-quality, monodisperse hollow maghemite nanoparticles (NPs) with a 14.8 ± 0.5 nm outer diameter and enhanced surface-to-volume ratio. The nanoparticle ensemble exhibits spin-glass-like signatures in dc magnetic aging and memory protocols and ac magnetic susceptibility. The dynamics of the system slow near 50 K, and become frozen on experimental time scales below 20 K. Remanence curves indicate the development of magnetic irreversibility concurrent with the freezing of the spin dynamics. A strong exchange-bias effect and its training behavior point to highly frustrated surface spins that rearrange much more slowly than interior spins. Monte Carlo simulations of a hollow particle corroborate strongly disordered surface layers with complex energy landscapes that underlie both glass-like dynamics and magnetic irreversibility. Calculated hysteresis loops reveal that magnetic behavior is not identical at the inner and outer surfaces, with spins at the outer surface layer of the 15 nm hollow particles exhibiting a higher degree of frustration. Our combined experimental and simulated results shed light on the origin of spin-glass-like phenomena and the important role played by the surface spins in magnetic hollow nanostructures. PMID:26503506

Discovery of room-temperature spin-glass behaviors in two-dimensional oriented attached single crystals

NASA Astrophysics Data System (ADS)

Ma, Ji; Chen, Kezheng

2016-05-01

In this study, room-temperature spin-glass behaviors were observed in flake-like oriented attached hematite (α-Fe2O3) and iron phosphate hydroxide hydrate (Fe5(PO4)4(OH)3·2H2O) single crystals. Remarkably, their coercivity (HC) values were found to be almost invariable at various given temperatures from 5 to 300 K. The spin topographic map in these flakes was assumed as superparamagnetic (SPM) "islands" isolated by spin glass (SG)-like "bridges". A spin-glass model was then proposed to demonstrate the spin frustration within these "bridges", which were formed by the staggered atomic planes in the uneven surfaces belonging to different attached nanoparticles. Under the spatial limitation and coupling shield of these "bridges", the SPM "islands" were found to be collectively frozen to form a superspin glass (SSG) state below 80 K in weak applied magnetic fields; whereas, when strong magnetic fields were applied, the magnetic coupling of these "islands" would become superferromagnetic (SFM) through tunneling superexchange, so that, these SFM spins could antiferromagnetically couple with the SG-like "bridges" to yield pronounced exchange bias (EB) effect.

Spin- and valley-dependent electronic band structure and electronic heat capacity of ferromagnetic silicene in the presence of strain, exchange field and Rashba spin-orbit coupling

NASA Astrophysics Data System (ADS)

Hoi, Bui Dinh; Yarmohammadi, Mohsen; Kazzaz, Houshang Araghi

2017-10-01

We studied how the strain, induced exchange field and extrinsic Rashba spin-orbit coupling (RSOC) enhance the electronic band structure (EBS) and electronic heat capacity (EHC) of ferromagnetic silicene in presence of external electric field (EF) by using the Kane-Mele Hamiltonian, Dirac cone approximation and the Green's function approach. Particular attention is paid to investigate the EHC of spin-up and spin-down bands at Dirac K and K‧ points. We have varied the EF, strain, exchange field and RSOC to tune the energy of inter-band transitions and consequently EHC, leading to very promising features for future applications. Evaluation of EF exhibits three phases: Topological insulator (TI), valley-spin polarized metal (VSPM) and band insulator (BI) at given aforementioned parameters. As a new finding, we have found a quantum anomalous Hall phase in BI regime at strong RSOCs. Interestingly, the effective mass of carriers changes with strain, resulting in EHC behaviors. Here, exchange field has the same behavior with EF. Finally, we have confirmed the reported and expected symmetry results for both Dirac points and spins with the study of valley-dependent EHC.

Exchange interactions in transition metal oxides: the role of oxygen spin polarization.

PubMed

Logemann, R; Rudenko, A N; Katsnelson, M I; Kirilyuk, A

2017-08-23

Magnetism of transition metal (TM) oxides is usually described in terms of the Heisenberg model, with orientation-independent interactions between the spins. However, the applicability of such a model is not fully justified for TM oxides because spin polarization of oxygen is usually ignored. In the conventional model based on the Anderson principle, oxygen effects are considered as a property of the TM ion and only TM interactions are relevant. Here, we perform a systematic comparison between two approaches for spin polarization on oxygen in typical TM oxides. To this end, we calculate the exchange interactions in NiO, MnO and hematite (Fe 2 O 3 ) for different magnetic configurations using the magnetic force theorem. We consider the full spin Hamiltonian including oxygen sites, and also derive an effective model where the spin polarization on oxygen renormalizes the exchange interactions between TM sites. Surprisingly, the exchange interactions in NiO depend on the magnetic state if spin polarization on oxygen is neglected, resulting in non-Heisenberg behavior. In contrast, the inclusion of spin polarization in NiO makes the Heisenberg model more applicable. Just the opposite, MnO behaves as a Heisenberg magnet when oxygen spin polarization is neglected, but shows strong non-Heisenberg effects when spin polarization on oxygen is included. In hematite, both models result in non-Heisenberg behavior. The general applicability of the magnetic force theorem as well as the Heisenberg model to TM oxides is discussed.

Competing spin fluctuations and trace of vortex dynamics in the two-dimensional triangular-lattice antiferromagnet AgCrS2

NASA Astrophysics Data System (ADS)

Gao, Wenshuai; Shi, Liran; Ouyang, Zhongwen; Xia, Zhengcai; Wang, Zhe; Liu, Bingjie; Li, Hexuan; Zou, Youming; Yu, Lu; Zhang, Lei; Pi, Li; Qu, Zhe; Zhang, Yuheng

2018-07-01

The spin dynamics of the two-dimensional triangular-lattice antiferromagnet AgCrS2 is investigated by electron spin resonance (ESR) spectroscopy. The g-factor is found to show an unusual non-monotonously temperature dependent behavior, which, along with the super-Curie behavior observed in the ESR intensity data, provides clear evidence for the competition between ferromagnetic and antiferromagnetic fluctuations at temperatures well above T N. On approaching the Néel temperature T N from above, the linewidth is found to diverge. Such a divergent behavior could be well described by the Kawamura–Miyashita model due to Z2 type magnetic vortex–antivortex pairing, which is consistent with the expectation for a 2D Heisenberg magnetic system.

Spin-ice behavior of three-dimensional inverse opal-like magnetic structures: Micromagnetic simulations

NASA Astrophysics Data System (ADS)

Dubitskiy, I. S.; Syromyatnikov, A. V.; Grigoryeva, N. A.; Mistonov, A. A.; Sapoletova, N. A.; Grigoriev, S. V.

2017-11-01

We perform micromagnetic simulations of the magnetization distribution in inverse opal-like structures (IOLS) made from ferromagnetic materials (nickel and cobalt). It is shown that the unit cell of these complex structures, whose characteristic length is approximately 700 nm, can be divided into a set of structural elements some of which behave like Ising-like objects. A spin-ice behavior of IOLS is observed in a broad range of external magnetic fields. Numerical results describe successfully the experimental hysteresis curves of the magnetization in Ni- and Co-based IOLS. We conclude that ferromagnetic IOLS can be considered as the first realization of three-dimensional artificial spin ice. The problem is discussed of optimal geometrical properties and material characteristics of IOLS for the spin-ice rule fulfillment.

A Two-Dimensional Manganese Gallium Nitride Surface Structure Showing Ferromagnetism at Room Temperature.

PubMed

Ma, Yingqiao; Chinchore, Abhijit V; Smith, Arthur R; Barral, María Andrea; Ferrari, Valeria

2018-01-10

Practical applications of semiconductor spintronic devices necessitate ferromagnetic behavior at or above room temperature. In this paper, we demonstrate a two-dimensional manganese gallium nitride surface structure (MnGaN-2D) which is atomically thin and shows ferromagnetic domain structure at room temperature as measured by spin-resolved scanning tunneling microscopy and spectroscopy. Application of small magnetic fields proves that the observed magnetic domains follow a hysteretic behavior. Two initially oppositely oriented MnGaN-2D domains are rotated into alignment with only 120 mT and remain mostly in alignment at remanence. The measurements are further supported by first-principles theoretical calculations which reveal highly spin-polarized and spin-split surface states with spin polarization of up to 95% for manganese local density of states.

Modulating the spin transport behaviors in ZBNCNRs by edge hydrogenation and position of BN chain

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ouyang, Jun; Long, Mengqiu, E-mail: mqlong@csu.edu.cn, E-mail: ygao@csu.edu.cn; Zhang, Dan

2016-03-15

Using the density functional theory and the nonequilibrium Green’s function method, we study the spin transport behaviors in zigzag boron-nitrogen-carbon nanoribbons (ZBNCNRs) by modulating the edge hydrogenation and the position of B-N nanoribbons (BNNRs) chain. The different edge hydrogenations of the ZBNCNRs and the different position relationships of the BNNRs have been considered systematically. Our results show that the metallic, semimetallic and semiconductive properties of the ZBNCNRs can be modulated by the different edge hydrogenations and different position relationships of BN chains. And our proposaled ZBNCNRs devices act as perfect spin-filters with nearly 100% spin polarization. These effects would havemore » potential applications for boron-nitrogen-carbon-based nanomaterials in spintronics nano-devices.« less

Velocity-dependent quantum phase slips in 1D atomic superfluids.

PubMed

Tanzi, Luca; Scaffidi Abbate, Simona; Cataldini, Federica; Gori, Lorenzo; Lucioni, Eleonora; Inguscio, Massimo; Modugno, Giovanni; D'Errico, Chiara

2016-05-18

Quantum phase slips are the primary excitations in one-dimensional superfluids and superconductors at low temperatures but their existence in ultracold quantum gases has not been demonstrated yet. We now study experimentally the nucleation rate of phase slips in one-dimensional superfluids realized with ultracold quantum gases, flowing along a periodic potential. We observe a crossover between a regime of temperature-dependent dissipation at small velocity and interaction and a second regime of velocity-dependent dissipation at larger velocity and interaction. This behavior is consistent with the predicted crossover from thermally-assisted quantum phase slips to purely quantum phase slips.

Neurobehavioral toxicity of cadmium sulfate to the planarian Dugesia dorotocephala

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grebe, E.; Schaeffer, D.J.

1991-05-01

The authors are developing bioassays which use planarians (free-living platyhelminthes) for the rapid determination of various types of toxicity, including acute mortality, tumorigenicity, and short-term neurobehavioral responses. Their motivation for using these animals is due to their importance as components of the aquatic ecology of unpolluted streams their sensitivity to low concentrations of environmental toxicants and the presence of a sensitive neurological system with a true brain which allows for complex social behavior. A previous paper described the results of a neurobehavioral bioassay using phenol in a crossover study. This paper reports a similar crossover study using cadmium sulfate.

Choosing an Appropriate Physical Exercise to Reduce Stereotypic Behavior in Children with Autism Spectrum Disorders: A Non-Randomized Crossover Study

ERIC Educational Resources Information Center

Tse, C. Y. Andy; Pang, C. L.; Lee, Paul H.

2018-01-01

Considerable evidence has shown that physical exercise could be an effective treatment in reducing stereotypical autism spectrum disorder (ASD) behaviors in children. The present study seeks to examine the underlying mechanism by considering the theoretical operant nature of stereotypy. Children with ASD (n = 30) who exhibited hand-flapping and…

Increased Erythrocyte Eicosapentaenoic Acid and Docosahexaenoic Acid Are Associated With Improved Attention and Behavior in Children With ADHD in a Randomized Controlled Three-Way Crossover Trial.

PubMed

Milte, Catherine M; Parletta, Natalie; Buckley, Jonathan D; Coates, Alison M; Young, Ross M; Howe, Peter R C

2015-11-01

To investigate effects of omega-3 polyunsaturated fatty acids (n-3 PUFA) docosahexaenoic acid (DHA) and eicosapentaenoic acid (EPA) on attention, literacy, and behavior in children with ADHD. Ninety children were randomized to consume supplements high in EPA, DHA, or linoleic acid (control) for 4 months each in a crossover design. Erythrocyte fatty acids, attention, cognition, literacy, and Conners' Parent Rating Scales (CPRS) were measured at 0, 4, 8, 12 months. Fifty-three children completed the treatment. Outcome measures showed no significant differences between the three treatments. However, in children with blood samples (n = 76-46), increased erythrocyte EPA + DHA was associated with improved spelling (r = .365, p < .001) and attention (r = -.540, p < .001) and reduced oppositional behavior (r = -.301, p < .003), hyperactivity (r = -.310, p < .001), cognitive problems (r = -.326, p < .001), Diagnostic and Statistical Manual of Mental Disorders (4th ed.; DSM-IV) hyperactivity (r = -.270, p = .002) and DSM-IV inattention (r = -.343, p < .001). Increasing erythrocyte DHA and EPA via dietary supplementation may improve behavior, attention, and literacy in children with ADHD. © The Author(s) 2013.

The Widom line and dynamical crossover in supercritical water: Popular water models versus experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Corradini, D.; Rovere, M.; Gallo, P., E-mail: gallop@fis.uniroma3.it

2015-09-21

In a previous study [Gallo et al., Nat. Commun. 5, 5806 (2014)], we have shown an important connection between thermodynamic and dynamical properties of water in the supercritical region. In particular, by analyzing the experimental viscosity and the diffusion coefficient obtained in simulations performed using the TIP4P/2005 model, we have found that the line of response function maxima in the one phase region, the Widom line, is connected to a crossover from a liquid-like to a gas-like behavior of the transport coefficients. This is in agreement with recent experiments concerning the dynamics of supercritical simple fluids. We here show howmore » different popular water models (TIP4P/2005, TIP4P, SPC/E, TIP5P, and TIP3P) perform in reproducing thermodynamic and dynamic experimental properties in the supercritical region. In particular, the comparison with experiments shows that all the analyzed models are able to qualitatively predict the dynamical crossover from a liquid-like to a gas-like behavior upon crossing the Widom line. Some of the models perform better in reproducing the pressure-temperature slope of the Widom line of supercritical water once a rigid shift of the phase diagram is applied to bring the critical points to coincide with the experimental ones.« less

Spin Hall effects in metallic antiferromagnets – perspectives for future spin-orbitronics

DOE PAGES

Sklenar, Joseph; Zhang, Wei; Jungfleisch, Matthias B.; ...

2016-03-07

In this paper, we investigate angular dependent spin-orbit torques from the spin Hall effect in a metallic antiferromagnet using the spin-torque ferromagnetic resonance technique. The large spin Hall effect exists in PtMn, a prototypical CuAu-I-type metallic antiferromagnet. By applying epitaxial growth, we previously reported an appreciable difference in spin-orbit torques for c- and a-axis orientated samples, implying anisotropic effects in magnetically ordered materials. In this work we demonstrate through bipolar-magnetic-field experiments a small but noticeable asymmetric behavior in the spin-transfer-torque that appears as a hysteresis effect. Finally, we also suggest that metallic antiferromagnets may be good candidates for the investigationmore » of various unidirectional effects related to novel spin-orbitronics phenomena.« less

Liquid-to-liquid crossover in the GaIn eutectic alloy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yu, Q.; Wang, X. D.; Su, Y.

Liquid-liquid crossover is promising and closely related to the atomic dynamics during heating and cooling processes. Here we reveal a reversible structural crossover in the liquid Ga85.8In14.2 eutectic alloys by using in situ synchrotron x-ray diffraction and ab initio molecular dynamics simulation. A kink always appears on the temperature dependent behaviors of density, ratio of the second peak position to the first in the pair correlation function, coordination number, heat capacity, free energy, and atomic diffusivity in the temperature range of about 400–550 K. It is likely ascribed to atomic rearrangements of Ga and In atoms from a relative randommore » packing at high temperatures to a relative nonuniform packing at low temperatures, in which In atoms prefer to have more In neighbors. This observation will promote more understanding of the liquid structure of eutectic alloys« less

A novel mechanism important for the alignment of microtubules.

PubMed

Wightman, Raymond; Turner, Simon R

2008-04-01

Using a live-cell imaging approach to study individual micro-tubules, we have compared microtubule behavior between net-like and aligned cortical arrays. In contrast to previous studies, a steep angled collision between the growing end of a microtubule and a preexisting microtubule was found to favor crossover. Frequencies of microtubule crossovers, bundling and catastrophes are similar regardless of whether the cell exhibited a net-like or aligned microtubule array. In the predominantly aligned array of petiole cells, severing occurs at the sites of microtubule crossovers and serves to remove unaligned microtubules and to increase microtubule density. Severing was observed to be rare in net-like arrays. Microtubule severing is carried out by the katanin enzyme. In this addendum, we present new insights into the possible mechanism of crossing over and preliminary data looking at organization of the array in a katanin mutant.

Spinon dynamics in quantum integrable antiferromagnets

NASA Astrophysics Data System (ADS)

Vlijm, R.; Caux, J.-S.

2016-05-01

The excitations of the Heisenberg antiferromagnetic spin chain in zero field are known as spinons. As pairwise-created fractionalized excitations, spinons are important in the understanding of inelastic neutron scattering experiments in (quasi-)one-dimensional materials. In the present paper, we consider the real space-time dynamics of spinons originating from a local spin flip on the antiferromagnetic ground state of the (an)isotropic Heisenberg spin-1/2 model and the Babujan-Takhtajan spin-1 model. By utilizing algebraic Bethe ansatz methods at finite system size to compute the expectation value of the local magnetization and spin-spin correlations, spinons are visualized as propagating domain walls in the antiferromagnetic spin ordering with anisotropy dependent behavior. The spin-spin correlation after the spin flip displays a light cone, satisfying the Lieb-Robinson bound for the propagation of correlations at the spinon velocity.

Spin wave nonreciprocity for logic device applications

NASA Astrophysics Data System (ADS)

Jamali, Mahdi; Kwon, Jae Hyun; Seo, Soo-Man; Lee, Kyung-Jin; Yang, Hyunsoo

2013-11-01

The utilization of spin waves as eigenmodes of the magnetization dynamics for information processing and communication has been widely explored recently due to its high operational speed with low power consumption and possible applications for quantum computations. Previous proposals of spin wave Mach-Zehnder devices were based on the spin wave phase, a delicate entity which can be easily disrupted. Here, we propose a complete logic system based on the spin wave amplitude utilizing the nonreciprocal spin wave behavior excited by microstrip antennas. The experimental data reveal that the nonreciprocity of magnetostatic surface spin wave can be tuned by the bias magnetic field. Furthermore, engineering of the device structure could result in a high nonreciprocity factor for spin wave logic applications.

Spin wave nonreciprocity for logic device applications

PubMed Central

Jamali, Mahdi; Kwon, Jae Hyun; Seo, Soo-Man; Lee, Kyung-Jin; Yang, Hyunsoo

2013-01-01

The utilization of spin waves as eigenmodes of the magnetization dynamics for information processing and communication has been widely explored recently due to its high operational speed with low power consumption and possible applications for quantum computations. Previous proposals of spin wave Mach-Zehnder devices were based on the spin wave phase, a delicate entity which can be easily disrupted. Here, we propose a complete logic system based on the spin wave amplitude utilizing the nonreciprocal spin wave behavior excited by microstrip antennas. The experimental data reveal that the nonreciprocity of magnetostatic surface spin wave can be tuned by the bias magnetic field. Furthermore, engineering of the device structure could result in a high nonreciprocity factor for spin wave logic applications. PMID:24196318

Thermally driven spin-Seebeck transport in chiral dsDNA-based molecular devices

NASA Astrophysics Data System (ADS)

Nian, L. L.; Zhang, Rong; Tang, F. R.; Tang, Jun; Bai, Long

2018-03-01

By employing the nonequilibrium Green's function technique, we study the thermal-induced spin-Seebeck transport through a chiral double-stranded DNA (dsDNA) connected to a normal-metal and a ferromagnetic lead. How the main parameters of the dsDNA-based system influence the spin-Seebeck transport is analyzed at length, and the thermally created charge (spin-related) current displays the rectification effect and the negative differential thermal conductance feature. More importantly, the spin current exhibits the rectification behavior of the spin-Seebeck effect; even the perfect spin-Seebeck effect can be obtained with the null charge current. Thus, the chiral dsDNA-based system can act as a spin(charge)-Seebeck diode, spin(charge)-Seebeck switch, and spin(charge)-Seebeck transistor. Our results provide new ways to design spin caloritronic devices based on dsDNA or other organic molecules.

The Effects of Caffeine on Hyperactive Children

ERIC Educational Resources Information Center

Firestone, Philip; And Others

1978-01-01

The psychological, physiological, and behavioral effects of a 2-week regimen of 300 mg of caffeine on 20 hyperactive males between the ages of 5 and 12 years were examined, using a double-blind crossover format. (Author)

Magnetoelectric Effect in a Spin-State Transition System

NASA Astrophysics Data System (ADS)

Naka, Makoto; Mizoguchi, Eriko; Nasu, Joji; Ishihara, Sumio

2018-06-01

Magnetic, dielectric, and magnetoelectric properties in a spin-state transition system are examined, motivated by the recent discovery of multiferroic behavior in a cobalt oxide. We construct an effective model Hamiltonian on the basis of the two-orbital Hubbard model, in which the spin-state degrees of freedom in magnetic ions couple with ferroelectric-type lattice distortions. A phase transition occurs from the high-temperature low-spin phase to the low-temperature high-spin ferroelectric phase with an accompanying increase in spin entropy. The calculated results are consistent with the experimental pressure-temperature phase diagram. We predict the magnetic-field induced electric polarization in the low-spin paraelectric phase near the ferroelectric phase boundary.

Suppression of electron spin relaxation in Mn-doped GaAs.

PubMed

Astakhov, G V; Dzhioev, R I; Kavokin, K V; Korenev, V L; Lazarev, M V; Tkachuk, M N; Kusrayev, Yu G; Kiessling, T; Ossau, W; Molenkamp, L W

2008-08-15

We report a surprisingly long spin relaxation time of electrons in Mn-doped p-GaAs. The spin relaxation time scales with the optical pumping and increases from 12 ns in the dark to 160 ns upon saturation. This behavior is associated with the difference in spin relaxation rates of electrons precessing in the fluctuating fields of ionized or neutral Mn acceptors, respectively. For the latter, the antiferromagnetic exchange interaction between a Mn ion and a bound hole results in a partial compensation of these fluctuating fields, leading to the enhanced spin memory.

Suppression of Electron Spin Relaxation in Mn-Doped GaAs

NASA Astrophysics Data System (ADS)

Astakhov, G. V.; Dzhioev, R. I.; Kavokin, K. V.; Korenev, V. L.; Lazarev, M. V.; Tkachuk, M. N.; Kusrayev, Yu. G.; Kiessling, T.; Ossau, W.; Molenkamp, L. W.

2008-08-01

We report a surprisingly long spin relaxation time of electrons in Mn-doped p-GaAs. The spin relaxation time scales with the optical pumping and increases from 12 ns in the dark to 160 ns upon saturation. This behavior is associated with the difference in spin relaxation rates of electrons precessing in the fluctuating fields of ionized or neutral Mn acceptors, respectively. For the latter, the antiferromagnetic exchange interaction between a Mn ion and a bound hole results in a partial compensation of these fluctuating fields, leading to the enhanced spin memory.

Exploratory study of the effects of wing-leading-edge modifications on the stall/spin behavior of a light general aviation airplane

NASA Technical Reports Server (NTRS)

1979-01-01

Configurations with full-span and segmented leading-edge flaps and full-span and segmented leading-edge droop were tested. Studies were conducted with wind-tunnel models, with an outdoor radio-controlled model, and with a full-scale airplane. Results show that wing-leading-edge modifications can produce large effects on stall/spin characteristics, particularly on spin resistance. One outboard wing-leading-edge modification tested significantly improved lateral stability at stall, spin resistance, and developed spin characteristics.

What about the leader? Crossover of emotional exhaustion and work engagement from followers to leaders.

PubMed

Wirtz, Nina; Rigotti, Thomas; Otto, Kathleen; Loeb, Carina

2017-01-01

Although a growing body of research links leadership behavior to follower health, comparatively little is known about the health effects of being in the lead. This longitudinal study of 315 team members and 67 leaders examined the crossover of emotional exhaustion and work engagement from followers to leaders. Leader emotional self-efficacy was tested as a moderator in the crossover process. Multiple regression analyses revealed that followers' work engagement was positively related to leaders' work engagement eight months later, controlling for followers' tenure with the leader, leader gender, autonomy, workload, and work engagement at Time 1. Leaders' emotional self-efficacy did not moderate the crossover of work engagement. Followers' emotional exhaustion was not directly related to leaders' emotional exhaustion over time. We did find a significant interaction effect for follower emotional exhaustion and leader emotional self-efficacy. This study is the first to show that crossover of emotional exhaustion and work engagement can unfold over time from team members to leaders. Main theoretical implications lie in the finding that-in line with job demands-resources theory-followers' psychological states can pose a demand or resource for leaders, and influence their well-being. For practitioners, our results offer valuable insights regarding the design of organizational health interventions as well as leadership development measures. (PsycINFO Database Record (c) 2016 APA, all rights reserved).

Electronic evidence of an insulator-superconductor crossover in single-layer FeSe/SrTiO3 films.

PubMed

He, Junfeng; Liu, Xu; Zhang, Wenhao; Zhao, Lin; Liu, Defa; He, Shaolong; Mou, Daixiang; Li, Fangsen; Tang, Chenjia; Li, Zhi; Wang, Lili; Peng, Yingying; Liu, Yan; Chen, Chaoyu; Yu, Li; Liu, Guodong; Dong, Xiaoli; Zhang, Jun; Chen, Chuangtian; Xu, Zuyan; Chen, Xi; Ma, Xucun; Xue, Qikun; Zhou, X J

2014-12-30

In high-temperature cuprate superconductors, it is now generally agreed that superconductivity is realized by doping an antiferromagnetic Mott (charge transfer) insulator. The doping-induced insulator-to-superconductor transition has been widely observed in cuprates, which provides important information for understanding the superconductivity mechanism. In the iron-based superconductors, however, the parent compound is mostly antiferromagnetic bad metal, raising a debate on whether an appropriate starting point should go with an itinerant picture or a localized picture. No evidence of doping-induced insulator-superconductor transition (or crossover) has been reported in the iron-based compounds so far. Here, we report an electronic evidence of an insulator-superconductor crossover observed in the single-layer FeSe film grown on a SrTiO3 substrate. By taking angle-resolved photoemission measurements on the electronic structure and energy gap, we have identified a clear evolution of an insulator to a superconductor with increasing carrier concentration. In particular, the insulator-superconductor crossover in FeSe/SrTiO3 film exhibits similar behaviors to that observed in the cuprate superconductors. Our results suggest that the observed insulator-superconductor crossover may be associated with the two-dimensionality that enhances electron localization or correlation. The reduced dimensionality and the interfacial effect provide a new pathway in searching for new phenomena and novel superconductors with a high transition temperature.

Electronic evidence of an insulator–superconductor crossover in single-layer FeSe/SrTiO3 films

PubMed Central

He, Junfeng; Liu, Xu; Zhang, Wenhao; Zhao, Lin; Liu, Defa; He, Shaolong; Mou, Daixiang; Li, Fangsen; Tang, Chenjia; Li, Zhi; Wang, Lili; Peng, Yingying; Liu, Yan; Chen, Chaoyu; Yu, Li; Liu, Guodong; Dong, Xiaoli; Zhang, Jun; Chen, Chuangtian; Xu, Zuyan; Chen, Xi; Ma, Xucun; Xue, Qikun; Zhou, X. J.

2014-01-01

In high-temperature cuprate superconductors, it is now generally agreed that superconductivity is realized by doping an antiferromagnetic Mott (charge transfer) insulator. The doping-induced insulator-to-superconductor transition has been widely observed in cuprates, which provides important information for understanding the superconductivity mechanism. In the iron-based superconductors, however, the parent compound is mostly antiferromagnetic bad metal, raising a debate on whether an appropriate starting point should go with an itinerant picture or a localized picture. No evidence of doping-induced insulator–superconductor transition (or crossover) has been reported in the iron-based compounds so far. Here, we report an electronic evidence of an insulator–superconductor crossover observed in the single-layer FeSe film grown on a SrTiO3 substrate. By taking angle-resolved photoemission measurements on the electronic structure and energy gap, we have identified a clear evolution of an insulator to a superconductor with increasing carrier concentration. In particular, the insulator–superconductor crossover in FeSe/SrTiO3 film exhibits similar behaviors to that observed in the cuprate superconductors. Our results suggest that the observed insulator–superconductor crossover may be associated with the two-dimensionality that enhances electron localization or correlation. The reduced dimensionality and the interfacial effect provide a new pathway in searching for new phenomena and novel superconductors with a high transition temperature. PMID:25502774

Spin-Filtering Rectifying and Negative Differential Resistance Behaviors in Co(dmit)2 Molecular Devices with Monatomic (C, Fe, Au) Electrodes

NASA Astrophysics Data System (ADS)

Yan, Shenlang; Long, Mengqiu; Zhang, Xiaojiao; He, Jun; Xu, Hui; Gao, Yongli

2014-09-01

Using nonequilibrium Green's functions (NEGFs) combined with the density functional theory (DFT), we study the electronic transport properties of a single molecule magnet Co(dmit)2, which is sandwiched between two monatomic chain electrodes, and the different electrode materials carbon, iron and gold, have been considered. The results show that the electrodes play a crucial role in the spin-dependent transport of the Co(dmit)2 molecular device, and some interesting phenomenon, such as perfect spin-filtering effect, rectifying and negative differential resistance (NDR) can be observed. We demonstrated that the magnetic Fe electrode can lead to high spin-flittering effect, and the different hybridization and alignment of energy levels between the molecule and the electrodes may be responsible for the rectification performance, and the distributions (delocalization or localization) of the frontier molecular orbitals under different bias result in the NDR behaviors. These characteristics could be used in the study of spin physics and the realization of nanospintronic devices.

Frustrated magnetism in the spin–chain metal Yb 2Fe 12P 7

DOE PAGES

Baumbach, Ryan E.; Hamlin, James J.; Janoschek, Marc; ...

2016-01-08

Here, magnetization measurements for magnetic fieldsmore » $${{\\mu}_{0}}H$$ up to 60 T are reported for the noncentrosymmetric spin–chain metal Yb 2Fe 12P 7. These measurements reveal behavior that is consistent with Ising-like spin chain magnetism that produces pronounced spin degeneracy. In particular, we find that although a Brillouin field dependence is observed in M( H) for $$H\\bot ~c$$ with a saturation moment that is close to the expected value for free ions of Yb 3+, non-Brillouin-like behavior is seen for $$H~\\parallel ~c$$ with an initial saturation moment that is nearly half the free ion value. In addition, hysteretic behavior that extends above the ordering temperature $${{T}_{\\text{M}}}$$ is seen for $$H~\\parallel ~c$$ but not for $$H~\\bot ~c$$ , suggesting out-of-equilibrium physics. This point of view is strengthened by the observation of a spin reconfiguration in the ordered state for $$H~\\parallel ~c$$ which is only seen for $$T\\leqslant {{T}_{\\text{M}}}$$ and after polarizing the spins. Together with the heat capacity data, these results suggest that the anomalous low temperature phenomena that were previously reported are driven by spin degeneracy that is related to the Ising-like one dimensional chain-like configuration of the Yb ions.« less

Investigating electron spin resonance spectroscopy of a spin-½ compound in a home-built spectrometer

NASA Astrophysics Data System (ADS)

Sarkar, Jit; Roy, Subhadip; Singh, Jitendra Kumar; Singh, Sourabh; Chakraborty, Tanmoy; Mitra, Chiranjib

2018-05-01

In this work we report electron spin resonance (ESR) measurements performed on NH4CuPO4.H2O, a Heisenberg spin ½ dimer compound. We carried out the experiments both at room temperature and at 78 K, which are well above the antiferromagnetic ordering temperature of the system where the paramagnetic spins have a dominant role in determining its magnetic behavior. We performed the measurements in a home built custom designed continuous wave electron spin resonance (CW-ESR) spectrometer. By analyzing the experimental data, we were able to quantify the Landé g-factor and the ESR line-width of the sample.

Efficient spin-filter and negative differential resistance behaviors in FeN4 embedded graphene nanoribbon device

NASA Astrophysics Data System (ADS)

Liu, N.; Liu, J. B.; Yao, K. L.; Ni, Y.; Wang, S. L.

2016-03-01

In this paper, we propose a new device of spintronics by embedding two FeN4 molecules into armchair graphene nanoribbon and sandwiching them between N-doped graphene nanoribbon electrodes. Our first-principle quantum transport calculations show that the device is a perfect spin filter with high spin-polarizations both in parallel configuration (PC) and antiparallel configuration (APC). Moreover, negative differential resistance phenomena are obtained for the spin-down current in PC, and the spin-up and spin-down currents in APC. These transport properties are explained by the bias-dependent evolution of molecular orbitals and the transmission spectra.

Spin-dependent Electron Correlations of a System with Broken Spin Symmetry

NASA Astrophysics Data System (ADS)

Yi, K. S.; Kim, J. I.; Kim, J. S.

2001-04-01

The spin-dependent local field corrections Gσ, σ'/ (q, ω) of a spin-polarized electron gas(SPEG) are examined within a genralized RPA. Numerical results of Gσ, σ/ (q, 0) for both the majority and minority spin electrons of SPEG show a complicated but interesting behavior as one varies the spin polarization ζ of the SPEG. A pronounced maximum in Gσ, σ/ (q, 0) is observed and the location of the peaks are found to depend strongly on the values of ζ. We also show some numerical results of the mixed susceptibilities χem and χme, which are finite and not identical in SPEG.

Competition of information channels in the spreading of innovations

NASA Astrophysics Data System (ADS)

Kocsis, Gergely; Kun, Ferenc

2011-08-01

We study the spreading of information on technological developments in socioeconomic systems where the social contacts of agents are represented by a network of connections. In the model, agents get informed about the existence and advantages of new innovations through advertising activities of producers, which are then followed by an interagent information transfer. Computer simulations revealed that varying the strength of external driving and of interagent coupling, furthermore, the topology of social contacts, the model presents a complex behavior with interesting novel features: On the macrolevel the system exhibits logistic behavior typical for the diffusion of innovations. The time evolution can be described analytically by an integral equation that captures the nucleation and growth of clusters of informed agents. On the microlevel, small clusters are found to be compact with a crossover to fractal structures with increasing size. The distribution of cluster sizes has a power-law behavior with a crossover to a higher exponent when long-range social contacts are present in the system. Based on computer simulations we construct an approximate phase diagram of the model on a regular square lattice of agents.

Competition of information channels in the spreading of innovations.

PubMed

Kocsis, Gergely; Kun, Ferenc

2011-08-01

We study the spreading of information on technological developments in socioeconomic systems where the social contacts of agents are represented by a network of connections. In the model, agents get informed about the existence and advantages of new innovations through advertising activities of producers, which are then followed by an interagent information transfer. Computer simulations revealed that varying the strength of external driving and of interagent coupling, furthermore, the topology of social contacts, the model presents a complex behavior with interesting novel features: On the macrolevel the system exhibits logistic behavior typical for the diffusion of innovations. The time evolution can be described analytically by an integral equation that captures the nucleation and growth of clusters of informed agents. On the microlevel, small clusters are found to be compact with a crossover to fractal structures with increasing size. The distribution of cluster sizes has a power-law behavior with a crossover to a higher exponent when long-range social contacts are present in the system. Based on computer simulations we construct an approximate phase diagram of the model on a regular square lattice of agents.