arXiv subjects

S. Ramasesha

Publications and source records attributed to S. Ramasesha.

At least 73 records · Page 4Linked to original sources

arXiv2002

Study of Low-energy States of Clusters of Spin-1/2 and Spin-1 Triangles with Kagome-like Geometries

We study the low-energy properties of Heisenberg antiferromagnetic spin-1/2 and spin-1 systems on various clusters made up of triangles. Some of the clusters have a geometry similar to representative pieces of the Kagome lattice, while others have the geometry of a sawtooth chain. While the ground state always has the lowest possible spin (0 or 1/2), the nature of the low-energy excitations depends on the geometry and the site spin. For the Kagome clusters with spin-1 sites, the lowest excitations are gapped, with singlet and triplet excitations having similar gaps. This is in contrast to Kagome clusters with spin-1/2 sites where there are several low-energy singlet excitations (possibly gapless in the thermodynamic limit), while triplet excitations have a gap. For the sawtooth chain with spin-1 sites, the lowest excitations are triplets with a gap; the gap to singlet excitations is about twice the triplet gap.

cond-mat.str-el↗

arXiv2002

Electron correlation effects in electron-hole recombination in organic light-emitting diodes

We develop a general theory of electron--hole recombination in organic light emitting diodes that leads to formation of emissive singlet excitons and nonemissive triplet excitons. We briefly review other existing theories and show how our approach is substantively different from these theories. Using an exact time-dependent approach to the interchain/intermolecular charge-transfer within a long-range interacting model we find that, (i) the relative yield of the singlet exciton in polymers is considerably larger than the 25% predicted from statistical considerations, (ii) the singlet exciton yield increases with chain length in oligomers, and, (iii) in small molecules containing nitrogen heteroatoms, the relative yield of the singlet exciton is considerably smaller and may be even close to 25%. The above results are independent of whether or not the bond-charge repulsion, X_perp, is included in the interchain part of the Hamiltonian for the two-chain system. The larger (smaller) yield of the singlet (triplet) exciton in carbon-based long-chain polymers is a consequence of both its ionic (covalent) nature and smaller (larger) binding energy. In nitrogen containing monomers, wavefunctions are closer to the noninteracting limit, and this decreases (increases) the relative yield of the singlet (triplet) exciton. Our results are in qualitative agreement with electroluminescence experiments involving both molecular and polymeric light emitters. The time-dependent approach developed here for describing intermolecular charge-transfer processes is completely general and may be applied to many other such processes.

cond-mat.mtrl-sci↗

arXiv2002

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 145 million for M$_s$=0 subspace. Our calculated gaps from the singlet ground state to the excited triplet state agrees well with the experimentally measured values. Study of the static structure factor shows that the ground state is spontaneously dimerized for ferric wheels. Spin states of ferric wheels can be viewed as quantized states of a rigid rotor with the gap between the ground and the first excited state defining the inverse of 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 Schrödinger 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 magnetization which is dependent on the amplitude of the {\it ac} field. We have also studied the torque response of Fe$_{12}$ as a function of magnetic field, which clearly shows spin-state crossover.

cond-mat.mes-hall↗

arXiv2001

Exchange Interaction in Binuclear Complexes with Rare Earth and Copper Ions: A Many-Body Model Study

We have used a many-body model Hamiltonian to study the nature of the magnetic ground state of hetero-binuclear complexes involving rare-earth and copper ions. We have taken into account all diagonal repulsions involving the rare-earth 4f and 5d orbitals and the copper 3d orbital. Besides, we have included direct exchange interaction, crystal field splitting of the rare-earth atomic levels and spin-orbit interaction in the 4f orbitals. We have identified the inter-orbital $4f$ repulsion, U$_{ff}$ and crystal field parameter, $Δ_f$ as the key parameters involved in controlling the type of exchange interaction between the rare earth $4f$ and copper 3d spins. We have explored the nature of the ground state in the parameter space of U$_{ff}$, $Δ_f$, spin-orbit interaction strength $λ$ and the $4f$ filling n$_f$. We find that these systems show low-spin or high-spin ground state depending on the filling of the $4f$ levels of the rare-earth ion and ground state spin is critically dependent on U$_{ff}$ and $Δ_f$. In case of half-filling (Gd(III)) we find a reentrant low-spin state as U$_{ff}$ is increased, for small values of $Δ_f$, which explains the recently reported apparent anomalous anti-ferromagnetic behaviour of Gd(III)-radical complexes. By varying U$_{ff}$ we also observe a switch over in the ground state spin for other fillings . We have introduced a spin-orbit coupling scheme which goes beyond L-S or j-j coupling scheme and we find that spin-orbit coupling does not significantly alter the basic picture.

cond-mat.str-el↗

arXiv2001

Structural and Electronic Instabilities in Polyacenes: Density Matrix Renormalization Group Study of a Long--Range Interacting Model

We have carried out Density Matrix Renormalization Group (DMRG) calculations on the ground state of long polyacene oligomers within a Pariser-Parr-Pople (PPP) Hamiltonian. The PPP model includes long-range electron correlations which are required for physically realistic modeling of conjugated polymers. We have obtained the ground state energy as a function of the dimerization $δ$ and various correlation functions and structure factors for $δ=0$. From energetics, we find that while the nature of the Peierls' instabilityin polyacene is conditional and strong electron correlations enhance the dimerization. The {\it cis} form of the distortion is favoured over the {\it trans} form. However, from the analysis of correlation functions and associated structure factors, we find that polyacene is not susceptible to the formation of a bond order wave (BOW), spin density wave (SDW) or a charge density wave (CDW) in the ground state.

cond-mat.str-el↗

arXiv2001

Exact and Approximate Theoretical Techniques for Quantum Magnetism in Low Dimensions

Quantum magnetism in low dimensions has been one of the central areas of theoretical research for many decades now. One of the key reasons for the long standing interest in this field has been the existence of simplified models, which serve as paradigms for understanding the role of strong interactions in many-electron systems. Although simple, these models quite often can not be solved exactly. In this review, we discuss a variety of analytical and numerical methods, which treat the system in a systematic and controlled manner. The central method employed in all the studies is the density matrix renormalization group (DMRG) method. This is supported by small scale numerical exact calculations, and by analytical methods using field theoretic techniques. We have considered a number of magnetic systems, from magnetic clusters to extended lattices, and have found some novel quantum ground states and low-energy elementary excitations. In some cases, we have also employed the finite-temperature DMRG method to accurately compute the low-temperature thermodynamic properties such as specific heat and magnetic susceptibility.

cond-mat.str-el↗

arXiv2001

Dynamic Oscillations of Magnetization in High Spin Magnetic Clusters

We have studied the time evolution of magnetization of a high spin magnetic cluster in the ground state, in the presence of a sinusoidal axial magnetic field and a static transverse field by explicitly solving time dependent schrödinger equation. We observe oscillations of magnetization in the plateau region which has all the characteristics reminiscent of the oscillation of probability of occupation of a state in a two level lattice in the presence of an oscillating electric field. The high spin of the ground state leads to a large but finite two-level pseudo-lattice. The oscillations in magnetization occur at amplitude of magnetic fields achievable in a laboratory and they also persist for a wide range of spin-dipolar interactions. Thus, our study provides a magnetic analog of the optical two-level lattice.

cond-mat.mes-hall↗

arXiv2000

An alternate model for magnetization plateaus in the molecular magnet V_15

Starting from an antiferromagnetic Heisenberg Hamiltonian for the fifteen spin-1/2 ions in V_15, we construct an effective spin Hamiltonian involving eight low-lying states (spin-1/2 and spin-3/2) coupled to a phonon bath. We numerically solve the time-dependent Schrodinger equation of this system, and obtain the magnetization as a function of temperature in a time-dependent magnetic field. The magnetization exhibits unusual patterns of hysteresis and plateaus as the field sweep rate and temperature are varied. The observed plateaus are not due to quantum tunneling but are a result of thermal averaging. Our results are in good agreement with recent experimental observations.

cond-mat.mes-hall↗

arXiv2000

Magnetization of Mn_12 Ac in a slowly varying magnetic field: an ab initio study

Beginning with a Heisenberg spin Hamiltonian for the manganese ions in the Mn_12 Ac molecule, we find a number of low-energy states of the system. We use these states to solve the time-dependent Schrodinger equation and find the magnetization of the molecule in the presence of a slowly varying magnetic field. We study the effects of the field sweep rate, fourth order anisotropic spin interactions and a transverse field on the weights of the different states as well as the magnetization steps which are known to occur in the hysteresis plots in this system. We find that the fourth order term and a slow field sweep rate are crucial for obtaining prominent steps in magnetization in the hysteresis plots.

cond-mat.mes-hall↗

arXiv2000

Evaluation of low-energy effective Hamiltonian techniques for coupled spin triangles

Motivated by recent work on Heisenberg antiferromagnetic spin systems on various lattices made up of triangles, we examine the low-energy properties of a chain of antiferromagnetically coupled triangles of half-odd-integer spins. We derive the low-energy effective Hamiltonian to second order in the ratio of the coupling J_2 between triangles to the coupling J_1 within each triangle. The effective Hamiltonian contains four states for each triangle which are given by the products of spin-1/2 states with the states of a pseudospin-1/2. We compare the results obtained by exact diagonalization of the effective Hamiltonian with those obtained for the full Hamiltonian using exact diagonalization and the density-matrix renormalization group method. It is found that the effective Hamiltonian is accurate only for the ground state for rather low values of the ratio J_2 / J_1 and that too for the spin-1/2 case with linear topology. The chain of spin-1/2 triangles shows interesting properties like spontaneous dimerization and several singlet and triplet excited states lying close to the ground state.

cond-mat.str-el↗

arXiv1999

Magnetization Properties of Some Quantum Spin Ladders

The experimental realization of various spin ladder systems has prompted their detailed theoretical investigations. Here we study the evolution of ground state magnetization with an external magnetic field for two different antiferromagnetic systems: a three-legged spin-1/2 ladder, and a two-legged spin-1/2 ladder with an additional diagonal interaction. The finite system density-matrix renormalization group method is employed for numerical studies of the three-chain system, and an effective low-energy Hamiltonian is used in the limit of strong interchain coupling to study the two- and three-chain systems. The three-chain system has a magnetization plateau at one-third of the saturation magnetization. The two-chain system has a plateau at zero magnetization due to a gap above the singlet ground state. It also has a plateau at half of the saturation magnetization for a certain range of values of the couplings. We study the regions of transitions between plateaus numerically and analytically, and find that they are described, at first order in a strong-coupling expansion, by an XXZ spin-1/2 chain in a magnetic field; the second order terms give corrections to the XXZ model. We also study numerically some low-temperature properties of the three-chain system, such as the magnetization, magnetic susceptibility and specific heat.

cond-mat.str-el↗

arXiv1998

Theory of Coexisting Charge and Spin-Density Waves in (TMTTF)_2Br, (TMTSF)_2PF_6 and alpha-(BEDT-TTF)_2MHg(SCN)_4

Recent experiments indicate that the spin-density waves (SDWs) in (TMTTF)_2Br, (TMTSF)_2PF_6 and alpha-(BEDT-TTF)_2MHg(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 bandfilling within the starting Hamiltonian.

cond-mat.str-el↗

arXiv1997

A DMRG Study of Low-Energy Excitations and Low-Temperature Properties of Alternating Spin Systems

We use the density matrix renormalization group (DMRG) method to study the ground and low-lying excited states of three kinds of uniform and dimerized alternating spin chains. The DMRG procedure is also employed to obtain low-temperature thermodynamic properties of these systems. We consider a 2N site system with spins $s_1$ and $s_2$ alternating from site to site and interacting via a Heisenberg antiferromagnetic exchange. The three systems studied correspond to $(s_1 ,s_2 )$ being equal to $(1,1/2),(3/2,1/2)$ and $(3/2,1)$; all of them have very similar properties. The ground state is found to be ferrimagnetic with total spin $s_G =N(s_1 - s_2)$. We find that there is a gapless excitation to a state with spin $s_G -1$, and a gapped excitation to a state with spin $s_G +1$. Surprisingly, the correlation length in the ground state is found to be very small for this gapless system. The DMRG analysis shows that the chain is susceptible to a conditional spin-Peierls instability. Furthermore, our studies of the magnetization, magnetic susceptibility $χ$ and specific heat show strong magnetic-field dependences. The product $χT$ shows a minimum as a function of temperature T at low magnetic fields; the minimum vanishes at high magnetic fields. This low-field behavior is in agreement with earlier experimental observations. The specific heat shows a maximum as a function of temperature, and the height of the maximum increases sharply at high magnetic fields. Although all the three systems show qualitatively similar behavior, there are some notable quantitative differences between the systems in which the site spin difference, $|s_1 - s_2|$, is large and small respectively.

cond-mat.str-el↗

arXiv1997

Quantum confinement effects on the ordering of the lowest-lying excited states in conjugated chains

The symmetrized density matrix renormalization group approach is applied within the extended Hubbard-Peierls model (with parameters U/t, V/t, and bond alternation δ) to study the ordering of the lowest one-photon (1^{1}B^{-}_u) and two-photon (2^{1}A^{+}_g) states in one- dimensional conjugated systems with chain lengths, N, up to N=80 sites. Three different types of crossovers are studied, as a function of U/t, δ, and N. The U-crossover emphasizes the larger ionic character of the 2A_g state compared to the lowest triplet excitation. The δcrossover shows strong dependence on both N and U/t. The N-crossover illustrates the more localized nature of the 2A_g excitation relative to the 1B_u excitation at intermediate correlation strengths.

cond-mat↗

arXiv1997

Structural Instability in Polyacene : A Projector Quantum Monte Carlo Study

We have studied polyacene within the Hubbard model to explore the effect of electron correlations on the Peierls' instability in a system marginally away from one-dimension. We employ the projector quantum Monte Carlo method to obtain ground state estimates of the energy and various correlation functions. We find strong similarities between polyacene and polyacetylene which can be rationalized from the real-space valence-bond arguments of Mazumdar and Dixit. Electron correlations tend to enhance the Peierls' instability in polyacene. This enhancement appears to attain a maximum at $U/t \sim 3.0$ and the maximum shifts to larger values when the alternation parameter is increased. The system shows no tendency to destroy the imposed bond-alternation pattern, as evidenced by the bond-bond correlations. The cis- distortion is seen to be favoured over the trans- distortion. The spin-spin correlations show that undistorted polyacene is susceptible to a SDW distortion for large interaction strength. The charge-charge correlations indicate the absence of a CDW distortion for the parameters studied.

cond-mat.str-el↗

arXiv1996

Symmetrized DMRG studies of the properties of Low-lying states of Poly-para-phenylene (PPP) system

We report the symmetrized density matrix renormalization group (DMRG) study of neutral and doped oligomers of PPP system within an extended Hubbard model. Model parameters are determined by comparing the existing results for interacting small system. We compute a number of properties in the ground state as well as in the one-photon, two-photon and triplet states to completely characterize these states. Based on the relative positions of the one-photon and two-photon states in long oligomers, we suggest that invoking interchain interactions is essential for explaining strong fluorescence in this system. Bond-order studies show that the lowest two-photon state corresponds to a localized excitation while one-photon and triplet excitations are extended in nature. The bipolaronic state shows clear evidence for charge separation and disproportionation into two polarons. We find that the extended nature of one-photon and triplet states of neutral system are very similar to those of the bipolaronic ground states.

cond-mat↗

arXiv1996

Low-Lying Excited States and Low-Temperature Properties of an Alternating Spin-1 / Spin-1/2 Chain : A DMRG study

We report spin wave and DMRG studies of the ground and low-lying excited states of uniform and dimerized alternating spin chains. The DMRG procedure is also employed to obtain low-temperature thermodynamic properties of the system. The ground state of a 2N spin system with spin-1 and spin-1/2 alternating from site to site and interacting via an antiferromagnetic exchange is found to be ferrimagnetic with total spin $s_G=N/2$ from both DMRG and spin wave analysis. Both the studies also show that there is a gapless excitation to a state with spin $s_G-1$ and a gapped excitation to a state with spin $s_G+1$. Surprisingly, the correlation length in the ground state is found to be very small from both the studies for this gapless system. For this very reason, we show that the ground state can be described by a variational ``ansatz'' of the product type. DMRG analysis shows that the chain is susceptible to a conditional spin-Peierls' instability. The DMRG studies of magnetization, magnetic susceptibility ($χ$) and specific heat show strong magnetic-field dependence. The product $χT$ shows a minimum as a function of temperature($T$) at low-magnetic fields and the minimum vanishes at high-magnetic fields. This low-field behaviour is in agreement with earlier experimental observations. The specific heat shows a maximum as a function of temperature and the height of the maximum increases sharply at high magnetic fields. It is hoped that these studies will motivate experimental studies at high-magnetic fields.

cond-mat↗

arXiv1996

Low-Lying Electronic Excitations and Nonlinear Optic Properties of Polymers via Symmetrized Density Matrix Renormalization Group Method

A symmetrized Density Matrix Renormalization Group procedure together with the correction vector approach is shown to be highly accurate for obtaining dynamic linear and third order polarizabilities of one-dimensional Hubbard and $U-V$ models. The $U-V$ model is seen to show characteristically different third harmonic generation response in the CDW and SDW phases. This can be rationalized from the excitation spectrum of the systems.

cond-mat↗