Full spin and spatial symmetry adapted technique for correlated electronic hamiltonians: Application to an icosahedral cluster

One of the long standing problems in quantum chemistry had been the inability to exploit full spatial and spin symmetry of an electronic Hamiltonian belonging to a non-Abelian point group. Here, we present a general technique which can utilize all the symmetries of an electronic (magnetic) Hamiltonian to obtain its full eigenvalue spectrum. This is a hybrid method based on Valence Bond basis and the basis of constant z-component of the total spin. This technique is applicable to systems with any point group symmetry and is easy to implement on a computer. We illustrate the power of the method by applying it to a model icosahedral half-filled electronic system. This model spans a huge Hilbert space (dimension 1,778,966) and in the largest non-Abelian point group. The C60 molecule has this symmetry and hence our calculation throw light on the higher energy excited states of the bucky ball. This method can also be utilized to study finite temperature properties of strongly correlated systems within an exact diagonalization approach. (C) 2011 Wiley Periodicals, Inc. Int J Quantum Chem, 2012

Universal jellium BCS picture for Peierls and spin-Peierls phase transitions

Both metal-insulator Peierls and antiferromagnetic spin-Peierls dimerized phase transitions are observed to have a BCS electron-phonon interaction parameter which is compatible with the jellium value λ = 2/3π ≈ 0.21.

Temperature- and pressure-dependent study of Cl-35 NQR frequency and spin lattice relaxation time in 2,3-dichloroanisole

The temperature and pressure dependence of Cl-35 NQR frequency and spin lattice relaxation time (T-1) were investigated in 2,3-dichloroanisole. Two NQR signals were observed throughout the temperature and pressure range studied. T-1 were measured in the temperature range from 77 to 300 K and from atmospheric pressure to 5 kbar. Relaxation was found to be due to the torsional motion of the molecule and also reorientation f motion of the CH3 group. T-1 versus temperature data were analyzed on the basis of Woessner and Gutowsky model, and the activation energy for the reorientation of the CH3 group was estimated. The temperature dependence of the average torsional lifetimes of the molecules and the transition probabilities were also obtained. NQR frequency shows a nonlinear behavior with pressure, indicating both dynamic and static effects of pressure. The pressure coefficients were observed to be positive for both the lines. A thermodynamic analysis of the data was carried out to determine the constant volume temperature coefficients of the NQR frequency. The variation of spin lattice time with pressure was very small, showing that the relaxation is mainly due to the torsional motions of the molecules. Copyright (C) 2010 John Wiley & Sons, Ltd.

Influence of lattice distortion on the Curie temperature and spin-phonon coupling in LaMn0.5Co0.5O3

Two distinct ferromagnetic phases of LaMn0.5Co0.5O3 having monoclinic structure with distinct physical properties have been studied. The ferromagnetic ordering temperature T-c is found to be different for both the phases. The origin of such contrasting characteristics is assigned to the changes in the distance(s) and angle(s) between Mn-O-Co resulting from distortions observed from neutron diffraction studies. Investigations on the temperature dependent Raman spectroscopy provide evidence for such structural characteristics, which affects the exchange interaction. The difference in B-site ordering which is evident from the neutron diffraction is also responsible for the difference in T-c. Raman scattering suggests the presence of spin-phonon coupling for both the phases around the T-c. Electrical transport properties of both the phases have been investigated based on the lattice distortion.

Crystal structures of fluorinated aryl biscarbonates and a biscarbamate: a counterpoise between weak intermolecular interactions and molecular symmetry

Conformational features and supramolecular structural organization in three aryl biscarbonates and an aryl biscarbamate with rigid acetylenic unit providing variable spacer lengths have been probed to gain insights into the packing features associated with molecular symmetry and the intermolecular interactions involving `organic' fluorine. Four structures but-2-yne-1,4-diyl bis(2,3,4,5,6-pentafluorophenylcarbonate), 1; but-2-yne-1,4-diyl bis(4-fluorophenylcarbonate), 2; but-2-yne-1,4-diyl bis(2,3,4,5,6-pentafluorophenylcarbamate), 3 and hexa-2,4-diyne-1,6-diyl bis(2,3,4,5,6-pentafluorophenylcarbonate), 4 have been analyzed in this context. Compound 1 adopts a non-centrosymmetric ``twisted'' (syn) conformation, whereas 2, 3 and 4 acquire a centrosymmetric ``extended'' (anti) conformation. Weak intermolecular interactions and in particular those involving fluorine are found to dictate this conformational variation in the crystal structure of 1. A single-crystal neutron diffraction study at 90 K was performed on 1 to obtain further insights into these interactions involving `organic' fluorine.

Magnetic and spin evolution of pulsars

We explore the consequences of the model of spin-down-induced flux expulsion for the magnetic field evolution in solitary as well as in binary neutron stars. The spin evolution of pulsars, allowing for their field evolution according to this model, is shown to be consistent with the existing observational constraints in both low- and high-mass X-ray binary systems. The contribution from pulsars recycled in massive binaries to the observed excess in the number of low-field (10(11)-10(12) G) solitary pulsars is argued to be negligible in comparison with that of normal pulsars undergoing a 'restricted' field decay predicted by the adopted field decay model. Magnetic fields of neutron stars born in close binaries with intermediate- or high-mass main-sequence companions are predicted to decay down to values as low as similar to 10(6) G, which would leave them unobservable as pulsars during most of their lifetimes. The post-recycling evolution of some of these systems can, however, account for the observed binary pulsars having neutron star or massive white dwarf companions. Pulsars recycled in the disc population low-mass binaries are expected to have residual fields greater than or similar to 10(8) G, while for those processed in globular clusters larger residual fields are predicted because of the lower field strength of the neutron star at the epoch of binary formation. A value of tau similar to 1-2 x 10(7) yr for the mean value of the Ohmic decay time-scale in the crusts of neutron stars is suggested, based on the consistency of the model predictions with the observed distribution of periods and magnetic fields in the single and binary pulsars.

Role of free valences and spin densities on the migrating atom in location of saddle points in radical-exchange reactions

The principle of the conservation of bond orders during radical-exchange reactions is examined using Mayer's definition of bond orders. This simple intuitive approximation is not valid in a quantitative sense. Ab initio results reveal that free valences (or spin densities) develop on the migrating atom during reactions. For several examples of hydrogen-transfer reactions, the sum of the reaction coordinate bond orders in the transition state was found to be 0.92 +/- 0.04 instead of the theoretical 1.00 because free valences (or spin densities) develop on the migrating atom during reactions. It is shown that free valence is almost equal to the square of the spin density on the migrating hydrogen atom and the maxima in the free valence (or spin density) profiles coincide (or nearly coincide) with the saddle points in the corresponding energy profiles.

Enhanced charge and spin currents in the one-dimensional disordered mesoscopic Hubbard ring

We consider a one-dimensional mesoscopic Hubbard ring with and without disorder and compute charge and spin stiffness as a measure of the permanent currents. For finite disorder we identify critical disorder strength beyond which the charge currents in a system with repulsive interactions are larger than those for a free system. The spin currents in the disordered repulsive Hubbard model are enhanced only for small U, where the magnetic state of the system corresponds to a charge-density wave pinned to the impurities. For large U, the state of the system corresponds to localized isolated spins and the spin currents are found to be suppressed. For the attractive Hubbard model we find that the charge currents are always suppressed compared to the free system at all length scales.

Raman evidence for the superconducting gap and spin-phonon coupling in the superconductor Ca( Fe0.95Co0.05)(2)As-2

Inelastic light scattering studies on a single crystal of electron-doped Ca(Fe0.95Co0.05)(2)As-2 superconductor, covering the tetragonal-to-orthorhombic structural transition as well as the magnetic transition at T-SM similar to 140 K and the superconducting transition temperature T-c similar to 23 K, reveal evidence for superconductivity-induced phonon renormalization. In particular, the phonon mode near 260 cm(-1) shows hardening below T-c, signaling its coupling with the superconducting gap. All three Raman active phonon modes show anomalous temperature dependence between room temperature and T-c, i.e. the phonon frequency decreases with lowering temperature. Further, the frequency of one of the modes shows a sudden change in temperature dependence at TSM. Using first-principles density functional theory based calculations, we show that the low temperature phase (T-c < T < T-SM) exhibits short-ranged stripe antiferromagnetic ordering, and estimate the spin-phonon couplings that are responsible for these phonon anomalies.

Temperature dependence study of chlorine NQR frequency and spin-lattice relaxation time in 2-amino,-3,5-dichloropyridine

Chlorine-35 NQR frequency and spin-lattice relaxation time measurements as a function of temperature in the range 77-300 K were carried out on 2-amino-3,5-dichloropyridine. Two NQR signals were observed and were assigned to the two chlorines present in the molecule using the additive model for substituent effects. The temperature dependence of the NQR frequency was analysed in terms of the torsional oscillations of the molecule and the torsional frequencies and their temperature dependence were calculated numerically using a two-mode approximation. The temperature dependence of the NQR spin-lattice relaxation time was found to be mainly due to the torsional oscillations of the molecule, with anharmonicity effects showing up at higher temperatures. Copyright (C) 1999 John Wiley & Sons, Ltd.

Theory of coexisting charge and spin-density waves in (TMTTF)(2)Br, (TMTSF)(2)PF6 and alpha-(BEDT-TTF)(2)MHg(SCN)(4)

We discuss a recently formulated microscopic theory of the unusual coexistence of spin density waves (SDWs) and charge density waves (CDWs) that has been seen in recent experiments on (TMTTF)2Br, (TMTSF)2PF6 and α-(BEDT-TTF)2MHg(SCN)4.

Theory of coexisting charge and spin-density waves in (TMTTF)(2)Br, (TMTSF)(2)PF6, and alpha-(BEDT-TTF)(2)MHg(SCN)(4)

Recent experiments indicate that the spin-density waves (SDWs) in (TMTTF)(2)Br, (TMTSF)(2)PF6, and alpha-(BEDT-TTF)(2)MHg(SCN)(4) are highly unconventional and coexist with charge-density waves (CDWs). We present a microscopic theory of this unusual CDW-SDW coexistence. A complete understanding requires the explicit inclusion of strong Coulomb interactions, lattice discreteness, the anisotropic two-dimensional nature of the lattice, and the correct hand filling within the starting Hamiltonian. [S0031-9007(99)08498-7].

Model exact low-lying states and spin dynamics in ferric wheels: Fe-6 to Fe-12

Using an efficient numerical scheme that exploits spatial symmetries and spin parity, we have obtained the exact low-lying eigenstates of exchange Hamiltonians for ferric wheels up to Fe-12. The largest calculation involves the Fe-12 ring which spans a Hilbert space dimension of about 145x10(6) for the M-S=0 subspace. Our calculated gaps from the singlet ground state to the excited triplet state agree well with the experimentally measured values. Study of the static structure factor shows that the ground state is spontaneously dimerized for ferric wheels. The spin states of ferric wheels can be viewed as quantized states of a rigid rotor with the gap between the ground and first excited states defining the inverse of the moment of inertia. We have studied the quantum dynamics of Fe-10 as a representative of ferric wheels. We use the low-lying states of Fe-10 to solve exactly the time-dependent Schrodinger equation and find the magnetization of the molecule in the presence of an alternating magnetic field at zero temperature. We observe a nontrivial oscillation of the magnetization which is dependent on the amplitude of the ac field. We have also studied the torque response of Fe-12 as a function of a magnetic field, which clearly shows spin-state crossover.

Confinement-deconfinement transition and spin correlations in a generalized Kitaev model

We present a spin model, namely, the Kitaev model augmented by a loop term and perturbed by an Ising Hamiltonian, and show that it exhibits both confinement-deconfinement transitions from spin liquid to antiferromagnetic/spin-chain/ferromagnetic phases and topological quantum phase transitions between gapped and gapless spin-liquid phases. We develop a fermionic resonating-valence-bonds (RVB) mean-field theory to chart out the phase diagram of the model and estimate the stability of its spin-liquid phases, which might be relevant for attempts to realize the model in optical lattices and other spin systems. We present an analytical mean-field theory to study the confinement-deconfinement transition for large coefficient of the loop term and show that this transition is first order within such mean-field analysis in this limit. We also conjecture that in some other regimes, the confinement-deconfinement transitions in the model, predicted to be first order within the mean-field theory, may become second order via a defect condensation mechanism. Finally, we present a general classification of the perturbations to the Kitaev model on the basis of their effect on it's spin correlation functions and derive a necessary and sufficient condition, within the regime of validity of perturbation theory, for the spin correlators to exhibit a long-ranged power-law behavior in the presence of such perturbations. Our results reproduce those of Tikhonov et al. [Phys. Rev. Lett. 106, 067203 (2011)] as a special case.

Griffiths phase-like behavior and spin-phonon coupling in double perovskite Tb(2)NiMnO(6)

The Griffiths phase-like features and the spin-phonon coupling effects observed in Tb(2)NiMnO(6) are reported. The double perovskite compound crystallizes in monoclinic P2(1)/n space group and exhibits a magnetic phase transition at T(c) similar to 111 K as an abrupt change in magnetization. A negative deviation from ideal Curie-Weiss law exhibited by 1/chi(T) curves and less-than-unity susceptibility exponents from the power-law analysis of inverse susceptibility are reminiscent of Griffiths phase-like features. Arrott plots derived from magnetization isotherms support the inhomogeneous nature of magnetism in this material. The observed effects originate from antiferromagnetic interactions that arise from inherent disorder in the system. Raman scattering experiments display no magnetic-order-induced phonon renormalization below Tc in Tb(2)NiMnO(6), which is different from the results observed in other double perovskites and is correlated to the smaller size of the rare earth. The temperature evolution of full-width-at-half-maximum for the stretching mode at 645 cm(-1) presents an anomaly that coincides with the magnetic transition temperature and signals a close connection between magnetism and lattice in this material. (C) 2011 American Institute of Physics. [doi: 10.1063/1.3671674]