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S. Ramasesha

Publications and source records attributed to S. Ramasesha.

At least 55 records · Page 3Linked to original sources
arXiv2010

Modified DMRG algorithm for the zigzag spin-1/2 chain with frustrated antiferromagnetic exchange: Comparison with field theory at large $J_2/J_1$

A modified density matrix renormalization group (DMRG) algorithm is applied to the zigzag spin-1/2 chain with frustrated antiferromagnetic exchange $J_1$, $J_2$ between first and second neighbors. The modified algorithm yields accurate results up to $J_2/J_1 \approx 4$ for the magnetic gap $Δ$ to the lowest triplet state, the amplitude $B$ of the bond order wave (BOW) phase, the wavelength $λ$ of the spiral phase, and the spin correlation length $ξ$. The $J_2/J_1$ dependences of $Δ$, $B$, $λ$ and $ξ$ provide multiple comparisons to field theories of the zigzag chain. The twist angle of the spiral phase and the spin structure factor yield additional comparisons between DMRG and field theory. Attention is given to the numerical accuracy required to obtain exponentially small gaps or exponentially long correlations near a quantum phase transition.

cond-mat.str-el↗
arXiv2009

Quantum interference in coherent molecular conductance

Coherent electronic transport through individual molecules is crucially sensitive to quantum interference. Using exact diagonalization techniques, we investigate the zero-bias and zero-temperature conductance through $π$-conjugated annulene molecules (modeled by the Pariser-Parr-Pople and Hubbard Hamiltonians) weakly coupled to two leads. We analyze the conductance for different source-drain configurations, finding an important reduction for certain transmission channels and for particular geometries as a consequence of destructive quantum interference between states with definite momenta. When translational symmetry is broken by an external perturbation we find an abrupt increase of the conductance through those channels. Previous studies concentrated on the effect at the Fermi energy, where this effect is very small. By analysing the effect of symmetry breaking on the main transmission channels we find a much larger response thus leading to the possibility of a larger switching of the conductance through single molecules.

cond-mat.str-el↗
arXiv2009

The role of triplet states in the emission mechanism of polymer light-emitting diodes

The blue emission of polyfluorene (PF) based light-emitting diodes (LEDs) is known to degrade due to a low energy green emission, which hitherto has been attributed to oxidative defects. By studying the electroluminescence from ethyl-hexyl substituted PF LEDs in the presence of oxygen and in an inert atmosphere, and by using trace quantities of paramagnetic impurities (PM) in the polymer, we show that the triplet states play a major role in the low energy emission mechanism. Our time-dependent many-body studies show that there is a large cross-section for the triplet formation in the electron-hole recombination process in presence of PM, and intersystem crossing from excited singlet to triplet states.

cond-mat.soft↗
arXiv2008

Quantum Phases of Long Range 1-D Bose-Hubbard Model: Field Theoretic and DMRG Study at Different Densities

We use Abelian Bosonization and density matrix renormalization group method to study the effect of density on quantum phases of long range 1-D Bose-Hubbard model. We predict the existence of supersolid phase and also other quantum phases for this system. We have analyzed the role of long range interaction parameter on solitonic phase near half filling. We discuss the effect of dimerization in nearest neighbor hopping and interaction terms on the plateau phase at the half filling.

cond-mat.stat-mech↗
arXiv2008

Tuning the bond order wave (BOW) phase of half-filled extended Hubbard models

Theoretical and computational studies of the quantum phase diagram of the one-dimensional half-filled extended Hubbard model (EHM) indicate a narrow bond order wave (BOW) phase with finite magnetic gap $E_m$ for on-site repulsion $U < U^*$, the critical point, and nearest neighbor interaction $V_c \approx U/2$ near the boundary of the charge density wave (CDW) phase. Potentials with more extended interactions that retain the EHM symmetry are shown to have a less cooperative CDW transition with higher $U^*$ and wider BOW phase. Density matrix renormalization group (DMRG) is used to obtain $E_m$ directly as the singlet-triplet gap, with finite $E_m$ marking the BOW boundary $V_s(U)$. The BOW/CDW boundary $V_c(U)$ is obtained from exact finite-size calculations that are consistent with previous EHM determinations. The kinetic energy or bond order provides a convenient new estimate of $U^*$ based on a metallic point at $V_c(U)$ for $U < U^*$. Tuning the BOW phase of half-filled Hubbard models with different intersite potentials indicates a ground state with large charge fluctuations and magnetic frustration. The possibility of physical realizations of a BOW phase is raised for Coulomb interactions.

cond-mat.str-el↗
arXiv2008

Fully Symmetrized VB Based Technique for Solving Exchange Hamiltonians of Molecular Magnets

Generally, the first step in modeling molecular magnets involves obtaining the low-lying eigenstates of a Heisenberg exchange Hamiltonian which conserves total spin and belongs usually to a non-Abelian point group. In quantum chemistry, it has been a long standing problem to target a state which has definite total spin and also belongs to a definite irreducible representation of the point group. Many attempts have been made over years, but unfortunately these have not resulted in methods that are easy to implement, or even applicable to all point groups. Here we present a general technique which is a hybrid method based on VB basis and constant Ms basis, which is applicable to all types of point groups, easy to implement on computer. We illustrate the power of the method by applying it to the molecular magnetic system, Cu6Fe8, with cubic symmetry. We emphasize that our method is applicable to spin clusters with arbitrary site spins and is easily extended to Fermionic systems.

physics.chem-ph↗
arXiv2008

A Theoretical Approach for Computing Magnetic Anisotropy in Single Molecule Magnets

We present a theoretical approach to calculate the molecular magnetic anisotropy parameters, $D_M$ and $E_M$ for single molecule magnets in any eigenstate of the exchange Hamiltonian, treating the anisotropy Hamiltonian as a perturbation. Neglecting inter-site dipolar interactions, we calculate molecular magnetic anisotropy in a given total spin state from the known single-ion anisotropies of the transition metal centers. The method is applied to $Mn_{12}Ac$ and $Fe_8$ in their ground and first few excited eigenstates, as an illustration. We have also studied the effect of orientation of local anisotropies on the molecular anisotropy in various eigenstates of the exchange Hamiltonian. We find that, in case of $Mn_{12}Ac$, the molecular anisotropy depends strongly on the orientation of the local anisotropies and the spin of the state. The $D_M$ value of $Mn_{12}Ac$ is almost independent of the orientation of the local anisotropy of the core $Mn(IV)$ ions. In the case of $Fe_8$, the dependence of molecular anisotropy on the spin of the state in question is weaker.

cond-mat.str-el↗
arXiv2008

Quantum Phase Analysis of Extended Bose-Hubbard Model

We have obtained the quantum phase diagram of one dimensional extended Bose-Hubbard model using the density-matrix renormalization group and Abelian bosonization methods for different commensurabilities. We describe the nature of different quantum phases at the charge degeneracy point. We find a direct phase transition from Mott insulating phase to superconducting phase for integer band fillings of bosons. We predict explicitly the presence of two kinds of repulsive Luttinger liquid phases, apart from the charge density wave and superconducting phases for half-integer band fillings. Our study reveals that extended range interactions are necessary to get the correct phase boundary of an one-dimensional interacting bosons system.

cond-mat.supr-con↗
arXiv2007

A Kinetic Model for Photoswitching of magnetism in the High Spin Molecule [Mo(IV)(CN)2(CN-Cu(II)(tren))6](ClO4)8

The heptanuclear complex [Mo(IV)(CN)2(CN-CuL)6]8+ exhibits photomagnetism. An earlier microscopic model showed that the transition dipole moments for excitation in different spin manifolds are similar in magnitude. In this paper, we attribute photomagnetism to the long lived S=3 charge transfer excited state for which there appears to be sufficient experimental evidence. We model the photomagnetism by employing a kinetic model which includes internal conversions and intersystem crossings. The key feature of the model is assumption of the existence of two kinds of S=3 states: one which has no direct pathway for internal conversion and the other characterized by slow kinetics for internal conversion to the low-energy states. The trapped S=3 state can decay via a thermally activated barrier to the other S=3 state. The experimental temperature dependence of magnetization plot is fitted using rate constants with Arrhenius dependence. The two different experimental cMT vs. T curves obtained with different irradiation times are fitted with our model. Our studies show that the photomagnetism in these systems is governed by kinetics and not due to differences in oscillator strengths for excitation of the different spin states.

cond-mat.str-el↗
arXiv2007

DMRG study of scaling exponents in spin-1/2 Heisenberg chains with dimerization and frustration

In conformal field theory, key properties of spin-1/2 chains, such as the ground state energy per site and the excitation gap scale with dimerization delta as delta^alpha with known exponents alpha and logarithmic corrections. The logarithmic corrections vanish in a spin chain with nearest (J=1) and next nearest neighbor interactions (J_2), for J_2c=0.2411. DMRG analysis of a frustrated spin chain with no logarithmic corrections yields the field theoretic values of alpha, and the scaling relation is valid up to the physically realized range, delta ~ 0.1. However, chains with logarithmic corrections (J_2<0.2411 J) are more accurately fit by simple power laws with different exponents for physically realized dimerizations. We show the exponents decreasing from approximately 3/4 to 2/3 for the spin gap and from approximately 3/2 to 4/3 for the energy per site and error bars in the exponent also decrease as J_2 approaches to J_2c.

cond-mat.str-el↗
arXiv2006

Dimerization-induced enhancement of the spin gap in the quarter-filled two-leg rectangular ladder

We report density-matrix renormalization group calculations of spin gaps in the quarter-filled correlated two-leg rectangular ladder with bond-dimerization along the legs of the ladder. In the small rung-coupling region, dimerization along the leg bonds can lead to large enhancement of the spin gap. Electron-electron interactions further enhance the spin gap, which is nonzero for all values of the rung electron hopping and for arbitrarily small bond-dimerization. Very large spin gaps, as are found experimentally in quarter-filled band organic charge-transfer solids with coupled pairs of quasi-one-dimensional stacks, however, occur within the model only for large dimerization and rung electron hopping that are nearly equal to the hopping along the legs. Coexistence of charge order and spin gap is also possible within the model for not too large intersite Coulomb interaction.

cond-mat.str-el↗
arXiv2005

Microscopic Model for High-spin vs. Low-spin ground state in $[Ni_2{M(CN)_8]}$ ($M=Mo^V, W^V, Nb^{IV}$) magnetic clusters

Conventional superexchange rules predict ferromagnetic exchange interaction between Ni(II) and M (M=Mo(V), W(V), Nb(IV)). Recent experiments show that in some systems this superexchange is antiferromagnetic. To understand this feature, in this paper we develop a microscopic model for Ni(II)-M systems and solve it exactly using a valence bond approach. We identify the direct exchange coupling, the splitting of the magnetic orbitals and the inter-orbital electron repulsions, on the M site as the parameters which control the ground state spin of various clusters of the Ni(II)-M system. We present quantum phase diagrams which delineate the high-spin and low-spin ground states in the parameter space. We fit the spin gap to a spin Hamiltonian and extract the effective exchange constant within the experimentally observed range, for reasonable parameter values. We also find a region in the parameter space where an intermediate spin state is the ground state. These results indicate that the spin spectrum of the microscopic model cannot be reproduced by a simple Heisenberg exchange Hamiltonian.

cond-mat.str-el↗
arXiv2005

Microscopic Model for Photoinduced Magnetism in the Molecular Complex $[Mo(IV)(CN)_2(CN-CuL)_6]^{8+}$ Perchlorate

A theoretical model for understanding photomagnetism in the heptanuclear complex $[Mo(IV)(CN)_2(CN-CuL)_6]^{8+}$ perchlorate is developed. It is a many-body model involving the active orbitals on the transition metal ions. The model is exactly solved using a valence bond approach. The ground state solution of the model is highly degenerate and is spanned by five S=0 states, nine S=1 states, five S=2 states and one S=3 state. The orbital occupancies in all these states correspond to six $Cu(II)$ ions and one diamagnetic $Mo(IV)$ ion. The optically excited charge-transfer (CT) state in each spin sector occur at nearly the same excitation energy of 2.993 eV for the physically reasonable parameter values. The degeneracy of the CT states is largest in the S=3 sector and so is the transition dipole moment from the ground state to these excited states. Thus laser irradiation with light of this energy results in most intense absorption in the S=3 sector. The life-time of the S=3 excited states is also expected to be the largest as the number of states below that energy is very sparse in this spin sector when compared to other spin sectors. These twin features of our model explain the observed photomagnetism in the $[Mo(IV)(CN)_2(CN-CuL)_6]^{8+}$ complex.

cond-mat.str-el↗
arXiv2004

Role of Electron--Electron Interactions on Spin Effects in Electron--Hole Recombination in Organic Light Emitting Diodes

We extend our theory of electron--hole recombination in organic light emitting diodes to investigate the possibility that high energy singlet and triplet excited states with large electron--hole separations are generated in such processes, over and above the lowest singlet and triplet excitons. Our approach involves a time-dependent calculation of the interchain / intermolecular charge--transfer within model Hamiltonians that explicitly include electron-electron interactions between the $π$-electrons. We show that the electron--hole recombination reaction can be viewed as a tunneling process whose cross section depends on both the matrix element of the interchain part of Hamiltonian and the energy difference between the initial polaron--pair state and the final neutral states. There occurs a bifurcation of the electron--hole recombination path in each of the two spin channels that leads to the generation of both the lowest energy exciton and a specific high energy charge-transfer state, with the matrix elements favoring the lowest energy exciton and the energy difference factor favoring the higher energy state. The overall effect of the electron--electron interactions is to enhance the singlet:triplet yield ratio over the value of 0.25 predicted from statistical considerations that are valid only within noninteracting models.

cond-mat.str-el↗
arXiv2004

Magnetic properties of a helical spin chain with alternating isotropic and anisotropic spins: magnetization plateaus and finite entropy

We study a model which could explain some of the unusual magnetic properties observed for the one-dimensional helical spin system Co(hfac)_2 NITPhOMe. One of the properties observed is that the magnetization shows plateaus near zero and near one-third of the saturation value if a magnetic field is applied along the helical axis, but not if the field is applied in the plane perpendicular to that axis. The system consists of a spin-1/2 chain in which cobalt ions (which are highly anisotropic with an easy axis e_i) and organic radicals (which are isotropic) alternate with each other. The easy axis of the cobalts e_i lie at an angle theta_i with respect to the helical axis, while the projection of e_{i+1} - e_i on the plane perpendicular to the helical axis is given by 2 pi /3. For temperatures and magnetic fields which are much smaller than the coupling between the nearest-neighbor cobalts and radicals, one can integrate out the radicals to obtain an Ising model for the cobalts; this enables one to compute the thermodynamic properties of the system using the transfer matrix approach. We consider a model in which the tilt angles theta_i are allowed to vary with i with period three; we find that for certain patterns of theta_i, the system shows the magnetization plateaus mentioned above. At the ends of the plateaus, the entropy is finite even at very low temperatures, while the magnetic susceptibility and specific heat also show some interesting features.

cond-mat.stat-mech↗
arXiv2003

Properties of low-lying states in some high-nuclearity Mn, Fe and V clusters: Exact studies of Heisenberg models

Using an efficient numerical scheme that exploits spatial symmetries and spin parity, we have obtained the exact low-lying eigenstates of exchange Hamiltonians for the high nuclearity spin clusters, Mn_{12}, Fe_8 and V_{15}. The largest calculation involves the Mn_{12} cluster which spans a Fock space of a hundred million. Our results show that the earlier estimates of the exchange constants need to be revised for the Mn_{12} cluster to explain the level ordering of low-lying eigenstates. In the case of the Fe_8 cluster, correct level ordering can be obtained which is consistent with the exchange constants for the already known clusters with butterfly structure. In the V_{15} cluster, we obtain an effective Hamiltonian that reproduces exactly, the eight low-lying eigenvalues of the full Hamiltonian.

cond-mat.mes-hall↗
arXiv2002

Characterization of the Energy Structure and Adiabatic Magnetization Process of V15

The energy structure of the V$_{15}$ is studied using exact diagonalization methods, and the adiabatic changes of the magnetization in the system with the sweeping field are investigated. We confirm that the Dzyaloshinskii-Moriya interaction leads to an energy gap which allows the adiabatic change of the magnetization which has been found experimentally by Chiorescu et al., and also predict novel dynamics of the magnetization due to this energy level structure.

cond-mat.mes-hall↗