Microscopic theory of cooperative spin crossover: Interaction of molecular modes with phonons

In this article, we present a new microscopic theoretical approach to the description of spin crossover in molecular crystals. The spin crossover crystals under consideration are composed of molecular fragments formed by the spin-crossover metal ion and its nearest ligand surrounding and exhibiting well defined localized (molecular) vibrations. As distinguished from the previous models of this phenomenon, the developed approach takes into account the interaction of spin-crossover ions not only with the phonons but also a strong coupling of the electronic shells with molecular modes. This leads to an effective coupling of the local modes with phonons which is shown to be responsible for the cooperative spin transition accompanied by the structural reorganization. The transition is characterized by the two order parameters representing the mean values of the products of electronic diagonal matrices and the coordinates of the local modes for the high- and low-spin states of the spin crossover complex. Finally, we demonstrate that the approach provides a reasonable explanation of the observed spin transition in the [Fe(ptz)6](BF4)2 crystal. The theory well reproduces the observed abrupt low-spin → high-spin transition and the temperature dependence of the high-spin fraction in a wide temperature range as well as the pronounced hysteresis loop. At the same time within the limiting approximations adopted in the developed model, the evaluated high-spin fraction vs. T shows that the cooperative spin-lattice transition proves to be incomplete in the sense that the high-spin fraction does not reach its maximum value at high temperature.

A gauge theory for continuous spin particles

In this dissertation we explore the features of a Gauge Field Theory formulation for continuous spin particles (CSP). To make our discussion as self-contained as possible, we begin by introducing all the basics of Group Theory - and representation theory - which are necessary to understand where the CSP come from. We then apply what we learn from Group Theory to the study of the Lorentz and Poincaré groups, to the point where we are able to construct the CSP representation. Finally, after a brief review of the Higher-Spin formalism, through the Schwinger-Fronsdal actions, we enter the realm of CSP Field Theory. We study and explore all the local symmetries of the CSP action, as well as all of the nuances associated with the introduction of an enlarged spacetime, which is used to formulate the CSP action. We end our discussion by showing that the physical contents of the CSP action are precisely what we expected them to be, in comparison to our Group Theoretical approach.

Cotunneling theory of atomic spin inelastic electron tunneling spectroscopy

We propose cotunneling as the microscopic mechanism that makes possible inelastic electron tunneling spectroscopy of magnetic atoms in surfaces for a wide range of systems, including single magnetic adatoms, molecules, and molecular stacks. We describe electronic transport between the scanning tip and the conducting surface through the magnetic system (MS) with a generalized Anderson model, without making use of effective spin models. Transport and spin dynamics are described with an effective cotunneling Hamiltonian in which the correlations in the magnetic system are calculated exactly and the coupling to the electrodes is included up to second order in the tip MS and MS substrate. In the adequate limit our approach is equivalent to the phenomenological Kondo exchange model that successfully describes the experiments. We apply our method to study in detail inelastic transport in two systems, stacks of cobalt phthalocyanines and a single Mn atom on Cu2N. Our method accounts for both the large contribution of the inelastic spin exchange events to the conductance and the observed conductance asymmetry.

Theory of single-spin inelastic tunneling spectroscopy

I show that recent experiments of inelastic scanning tunneling spectroscopy of single and a few magnetic atoms are modeled with a phenomenological spin-assisted tunneling Hamiltonian so that the inelastic dI/dV line shape is related to the spin spectral weight of the magnetic atom. This accounts for the spin selection rules and dI/dV spectra observed experimentally for single Fe and Mn atoms deposited on Cu2N. In the case of chains of Mn atoms it is found necessary to include both first and second-neighbor exchange interactions as well as single-ion anisotropy.

Quantum theory of spin waves in finite chiral spin chains

We calculate the effect of spin waves on the properties of finite-size spin chains with a chiral spin ground state observed on biatomic Fe chains deposited on iridium(001). The system is described with a Heisenberg model supplemented with a Dzyaloshinskii-Moriya coupling and a uniaxial single ion anisotropy that presents a chiral spin ground state. Spin waves are studied using the Holstein-Primakoff boson representation of spin operators. Both the renormalized ground state and the elementary excitations are found by means of Bogoliubov transformation, as a function of the two variables that can be controlled experimentally, the applied magnetic field and the chain length. Three main results are found. First, because of the noncollinear nature of the classical ground state, there is a significant zero-point reduction of the ground-state magnetization of the spin spiral. Second, there is a critical external field from which the ground state changes from chiral spin ground state to collinear ferromagnetic order. The character of the two lowest-energy spin waves changes from edge modes to confined bulk modes over this critical field. Third, in the spin-spiral state, the spin-wave spectrum exhibits oscillatory behavior as function of the chain length with the same period of the spin helix.

Spin and spatial dynamics in electron-impact scattering off S-wave He using R-matrix with Time-Dependence theory

R-matrix with time-dependence theory is applied to electron-impact ionisation processes for He in the S-wave model. Cross sections for electron-impact excitation, ionisation and ionisation with excitation for impact energies between 25 and 225 eV are in excellent agreement with benchmark cross sections. Ultra-fast dynamics induced by a scattering event is observed through time-dependent signatures associated with autoionisation from doubly excited states. Further insight into dynamics can be obtained through examination of the spin components of the time-dependent wavefunction.

Anomalous thermodynamic properties in ferropericlase throughout its spin crossover transition

The thermodynamics properties of ferropericlase (Mg(1-x)Fe(x)O where x=0.1875) (Fp) throughout its spin crossover were investigated by first principles. Fp was treated as an ideal solid solution of pure high-spin and low-spin states. The Gibbs free energies of the pure states were addressed using the LDA+U method. A vibrational virtual-crystal model was developed to address the vibrational properties of the pure spin cases and used in conjunction with quasiharmonic theory to compute their vibrational free energies. The thermodynamics properties of Fp display significant anomalies that should be typical of spin crossover systems in general. In Fp, in particular, they are fundamental for understanding the state of earth's interior, where the pressure and temperature conditions of the crossover are realized.

Gluon-Spin Contribution to the Proton Spin from the Double-Helicity Asymmetry in Inclusive pi(0) Production in Polarized p plus p Collisions at root s=200 GeV

The double helicity asymmetry in neutral pion production for p(T) = 1 to 12 GeV/c was measured with the PHENIX experiment to access the gluon-spin contribution, Delta G, to the proton spin. Measured asymmetries are consistent with zero, and at a theory scale of mu 2 = 4 GeV(2) a next to leading order QCD analysis gives Delta G([0.02,0.3]) = 0.2, with a constraint of -0.7 < Delta G([0.02,0.3]) < 0.5 at Delta chi(2) = 9 (similar to 3 sigma) for the sampled gluon momentum fraction (x) range, 0.02 to 0.3. The results are obtained using predictions for the measured asymmetries generated from four representative fits to polarized deep inelastic scattering data. We also consider the dependence of the Delta G constraint on the choice of the theoretical scale, a dominant uncertainty in these predictions.

Noncommutativity due to spin

Using the Berezin-Marinov pseudoclassical formulation of the spin particle we propose a classical model of spin noncommutativity. In the nonrelativistic case, the Poisson brackets between the coordinates are proportional to the spin angular momentum. The quantization of the model leads to the noncommutativity with mixed spatial and spin degrees of freedom. A modified Pauli equation, describing a spin half particle in an external electromagnetic field is obtained. We show that nonlocality caused by the spin noncommutativity depends on the spin of the particle; for spin zero, nonlocality does not appear, for spin half, Delta x Delta y >= theta(2)/2, etc. In the relativistic case the noncommutative Dirac equation was derived. For that we introduce a new star product. The advantage of our model is that in spite of the presence of noncommutativity and nonlocality, it is Lorentz invariant. Also, in the quasiclassical approximation it gives noncommutativity with a nilpotent parameter.

Determination of the spin of new resonances in electroweak gauge boson pair production at the LHC

The appearance of spin-1 resonances associated with the electroweak symmetry breaking sector is expected in many extensions of the standard model. We analyze the CERN Large Hadron Collider potential to probe the spin of possible new charged and neutral vector resonances through the purely leptonic processes pp -> Z' -> l(+) l'(-) E(T), and pp -> W' -> l'(+/-) l(+) l(-) E(T), with l, l' = e or mu. We perform a model-independent analysis and demonstrate that the spin of the new states can be determined with 99% C. L. in a large fraction of the parameter space where these resonances can be observed with 100 fb(-1). We show that the best sensitivity to the spin is obtained by directly studying correlations between the final state leptons, without the need of reconstructing the events in their center-of-mass frames.

Spin-Orbit Coupling in n-Type PbTe/PbEuTe Quantum Wells

Magnetoresistance measurements were performed on an n-type PbTe/PbEuTe quantum well and weak antilocalization effects were observed. This indicates the presence of spin orbit coupling phenomena and we showed that the Rashba effect is the main mechanism responsible for this spin orbit coupling. Using the model developed by Iordanskii et al., we fitted the experimental curves and obtained the inelastic and spin orbit scattering times. Thus we could compare the zero field energy spin-splitting predicted by the Rashba theory with the energy spin-splitting obtained from the analysis of the experimental curves. The final result confirms the theoretical prediction of strong Rashba effect on IV-VI based quantum wells.

Spin filtering and disorder-induced magnetoresistance in carbon nanotubes: Ab initio calculations

Nitrogen-doped carbon nanotubes can provide reactive sites on the porphyrin-like defects. It is well known that many porphyrins have transition-metal atoms, and we have explored transition-metal atoms bonded to those porphyrin-like defects inN-doped carbon nanotubes. The electronic structure and transport are analyzed by means of a combination of density functional theory and recursive Green's function methods. The results determined the heme B-like defect (an iron atom bonded to four nitrogens) is the most stable and has a higher polarization current for a single defect. With randomly positioned heme B defects in nanotubes a few hundred nanometers long, the polarization reaches near 100%, meaning they are effective spin filters. A disorder-induced magnetoresistance effect is also observed in those long nanotubes, and values as high as 20 000% are calculated with nonmagnectic eletrodes.

Measurement of the Parity-Violating Longitudinal Single-Spin Asymmetry for W(+/-) Boson Production in Polarized Proton-Proton Collisions at root s=500 GeV

We report the first measurement of the parity-violating single-spin asymmetries for midrapidity decay positrons and electrons from W(+) and W(-) boson production in longitudinally polarized proton-proton collisions at root s = 500 GeV by the STAR experiment at RHIC. The measured asymmetries, A(L)(W+) = -0.27 +/- 0.10(stat.) +/- 0.02(syst.) +/- 0.03(norm.) and A(L)(W-) = 0.14 +/- 0.19(stat.) +/- 0.02(syst.) +/- 0.01(norm.), are consistent with theory predictions, which are large and of opposite sign. These predictions are based on polarized quark and antiquark distribution functions constrained by polarized deep-inelastic scattering measurements.

Orbital multicriticality in spin-gapped quasi-one-dimensional antiferromagnets

Motivated by the quasi-one-dimensional antiferromagnet CaV(2)O(4), we explore spin-orbital systems in which the spin modes are gapped but orbitals are near a macroscopically degenerate classical transition. Within a simplified model we show that gapless orbital liquid phases possessing power-law correlations may occur without the strict condition of a continuous orbital symmetry. For the model proposed for CaV(2)O(4), we find that an orbital phase with coexisting order parameters emerges from a multicritical point. The effective orbital model consists of zigzag-coupled transverse field Ising chains. The corresponding global phase diagram is constructed using field theory methods and analyzed near the multicritical point with the aid of an exact solution of a zigzag XXZ model.

Structural models for yttrium aluminium borate laser glasses: NMR and EPR studies of the system (Y(2)O(3))(0.2)-(Al(2)O(3))(x)-(B(2)O(3))(0.8-x)

The structure of laser glasses in the system (Y(2)O(3))(0.2){(Al(2)O(3))(x))(B(2)O(3))(0.8-x)} (0.15 <= x <= 0.40) has been investigated by means of (11)B, (27)Al, and (89)Y solid state NMR as well as electron spin echo envelope modulation (ESEEM) of Yb-doped samples. The latter technique has been applied for the first time to an aluminoborate glass system. (11)B magic-angle spinning (MAS)-NMR spectra reveal that, while the majority of the boron atoms are three-coordinated over the entire composition region, the fraction of three-coordinated boron atoms increases significantly with increasing x. Charge balance considerations as well as (11)B NMR lineshape analyses suggest that the dominant borate species are predominantly singly charged metaborate (BO(2/2)O(-)), doubly charged pyroborate (BO(1/2)(O(-))(2)), and (at x = 0.40) triply charged orthoborate groups. As x increases along this series, the average anionic charge per trigonal borate group increases from 1.38 to 2.91. (27)Al MAS-NMR spectra show that the alumina species are present in the coordination states four, five and six, and the fraction of four-coordinated Al increases markedly with increasing x. All of the Al coordination states are in intimate contact with both the three-and the four-coordinate boron species and vice versa, as indicated by (11)B/(27)Al rotational echo double resonance (REDOR) data. These results are consistent with the formation of a homogeneous, non-segregated glass structure. (89)Y solid state NMR spectra show a significant chemical shift trend, reflecting that the second coordination sphere becomes increasingly ""aluminate-like'' with increasing x. This conclusion is supported by electron spin echo envelope modulation (ESEEM) data of Yb-doped glasses, which indicate that both borate and aluminate species participate in the medium range structure of the rare-earth ions, consistent with a random spatial distribution of the glass components.