arXiv subjects

Z. G. Soos

Publications and source records attributed to Z. G. Soos.

15 recordsLinked to original sources

arXiv2020

Intriguing relaxor ferroelectricity in a polar CT crystal at the neutral-ionic interface

We investigated the mixed-stack charge-transfer crystal, N,N'-dimethylphenazine-TCNQ (M$_2$P-TCNQ), which is polar at room temperature and just at the neutral-to-ionic interface (ionicity $ρ\approx 0.5$). We detect the typical dielectric signature of a relaxor ferroelectric and an asymmetric positive-up-negative-down behavior. While relaxor ferroelectricity is usually ascribed to disorder in the crystal, we find no evidence for structural disorder in the investigated crystals. To elucidate the origin of M$_2$P-TCNQ's dielectric properties we perform parallel structural and spectroscopic measurements, associated with theoretical modeling and quantum-mechanical calculations. Our combined effort points to a highly polarizable electronic system that is strongly coupled to lattice vibrations. The found indications for polarization reversal imply flipping of the bent conformation of the M$_2$P molecule with an associated energy barrier of a few tens of an eV, broadly consistent with an Arrhenius fit of the dielectric relaxation times. While the polarization is mostly of electronic origin, its possible reversal implies slow collective motions that are affected by solid-state intermolecular interactions.

cond-mat.str-el↗

arXiv2015

Efficient Density Matrix Renormalization Group algorithm to study Y-Junctions with integer and half-integer spin

An efficient density matrix renormalization group (DMRG) algorithm is presented and applied to Y-junctions, systems with three arms of $n$ sites that meet at a central site. The accuracy is comparable to DMRG of chains. As in chains, new sites are always bonded to the most recently added sites and the superblock Hamiltonian contains only new or once renormalized operators. Junctions of up to $N = 3n + 1 \approx 500$ sites are studied with antiferromagnetic (AF) Heisenberg exchange $J$ between nearest-neighbor spins $S$ or electron transfer $t$ between nearest neighbors in half-filled Hubbard models. Exchange or electron transfer is exclusively between sites in two sublattices with $N_A \ne N_B$. The ground state (GS) and spin densities $ ρ_r = $ at site $r$ are quite different for junctions with $S$ = 1/2, 1, 3/2 and 2. The GS has finite total spin $S_G = 2S (S)$ for even (odd) $N$ and for $M_G =S_G$ in the $S_G$ spin manifold, $ρ_r > 0 (< 0)$ at sites of the larger (smaller) sublattice. $S$ = 1/2 junctions have delocalized states and decreasing spin densities with increasing $N$. $S$ = 1 junctions have four localized $S_z = 1/2$ states at the end of each arm and centered on the junction, consistent with localized states in $S$ = 1 chains with finite Haldane gap. The GS of $S$ = 3/2 or 2 junctions of up to 500 spins is a spin density wave (SDW) with increased amplitude at the ends of arms or near the junction. Quantum fluctuations completely suppress AF order in $S$ = 1/2 or 1 junctions, as well as in half-filled Hubbard junctions, but reduce rather than suppress AF order in $S$ = 3/2 or 2 junctions.

cond-mat.str-el↗

arXiv2014

Spin structure factor and quantum phases of frustrated spin-1/2 chains

The static structure factor S(q) of frustrated spin-1/2 chains with isotropic exchange and a singlet ground state (GS) diverges at wave vector q_m when the GS has quasi-long-range order (QLRO) with periodicity 2π/q_m but S(q_m) is finite in bond-order-wave (BOW) phases with finite-range spin correlations. Exact diagonalization and density matrix renormalization group (DMRG) calculations of S(q) indicate a decoupled phase with QLRO and q_m = π/2 in chains with large antiferromagnetic exchange between second neighbors. S(q_m) identifies quantum phase transitions based on GS spin correlations.

cond-mat.str-el↗

arXiv2013

Decoupled phase of frustrated spin-1/2 antiferromagnetic chains with and without long range order in the ground state

The quantum phases of one-dimensional spin $s= 1/2$ chains are discussed for models with two parameters, frustrating exchange $g = J_2 > 0$ between second neighbors and normalized nonfrustrating power-law exchange with exponent $α$ and distance dependence $r^{-α}$. The ground state (GS) at $g = 0$ has long-range order (LRO) for $α< 2$, long-range spin fluctuations for $α> 2$. The models conserve total spin $S = S_A + S_B$, have singlet GS for any $g$, $α\ge 0$ and decouple at $1/g = 0$ to linear Heisenberg antiferromagnets on sublattices $A$ and $B$ of odd and even-numbered sites. Exact diagonalization of finite chains gives the sublattice spin $ \ < S^2_A \ >$, the magnetic gap $E_m$ to the lowest triplet state and the excitation $E_σ$ to the lowest singlet with opposite inversion symmetry to the GS. An analytical model that conserves sublattice spin has a first order quantum transition at $g_c = 1/4{\rm ln2}$ from a GS with perfect LRO to a decoupled phase with $S_A = S_B = 0$ for $g \ge 4/π^2$ and no correlation between spins in different sublattices. The model with $α= 1$ has a first order transition to a decoupled phase that closely resembles the analytical model. The bond order wave (BOW) phase and continuous quantum phase transitions of finite models with $α\ge 2$ are discussed in terms of GS degeneracy where $E_σ(g) = 0$, excited state degeneracy where $E_σ(g) = E_m(g)$, and $\ < S^2_A \ >$. The decoupled phase at large frustration has nondegenerate GS for any exponent $α$ and excited states related to sublattice excitations.

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arXiv2013

Spin-flop and antiferromagnetic phases of the ferromagnetic half-twist ladder compounds Ba3Cu3In4O12 and Ba3Cu3Sc4O12

The title compounds have dominant ferromagnetic (FM) exchange interactions within one-dimensional (1D) half-twist ladders of s =1/2 Cu2^{+} ions and antiferromagnetic(AFM) interactions between ladders, leading to ordered 3D phases at temperatures below 20K. Here we show that a microscopic 1D model of the paramagnetic (PM) phase combined with a phenomenological model based on sublattice magnetization describes the observed temperature and field dependent magnetism. The model identifies AFM, spin-flop (SF) and PM phases whose boundaries have sharp features in the experimental magnetization M(T,H) and specific heat CP(T,H). Exact diagonalization (ED) of the 1D model, possible for 24 spins due to special structural features of half-twist ladders, yields the magnetization and spin susceptibility of the PM phase. AFM interactions between ladders are included at the mean-field level using the field, HAF, obtained from modeling the ordered phases. Isotropic exchange J1 = -135K and g-tensor g = 2.1 within ladders, plus exchange and anisotropy fields HAF and HA, describe the ordered phases, and are almost quantitative for the PM phase.

cond-mat.str-el↗

arXiv2012

Quantum spin liquid in frustrated one dimensional LiCuSbO4

A quantum magnet, LiCuSbO4, with chains of edge-sharing S = 1/2 CuO6 octahedra is reported. While the Curie-Weiss constant is ferromagnetic, θ= 30 K, no phase transition or spin freezing occurs down to 100 mK. Specific heat indicates a distinct high field phase near the 12 T saturation field. Neutron scattering shows incommensurate spin correlations with q = 0.47\pm0.01π/a and places an upper limit of 70 \mueV on a potential spin gap. Exact diagonalization of easy plane S = 1/2 chains with competing ferro- and antiferromagnetic interactions (J1 = - 75 K, J2 = 34 K) accounts for the T > 2 K data.

cond-mat.str-el↗

arXiv2012

Dominant ferromagnetism in the spin-1/2 half-twist ladder 334 compounds, Ba3Cu3In4O12 and Ba3Cu3Sc4O12

The magnetic properties of polycrystalline samples of Ba3Cu3In4O12 (In-334) and Ba3Cu3Sc4O12 (Sc-334) are reported. Both 334 phases have a structure derived from perovskite, with CuO4 squares interconnected to form half-twist ladders along the c-axis. The Cu-O-Cu angles, ~ 90o, and the positive Weiss temperatures indicate the presence of significant ferromagnetic (FM) interactions along the Cu ladders. At low temperatures, T < 20 K, sharp transitions in the magnetic susceptibility and heat capacity measurements indicate three-dimensional (3D) antiferromagnetic (AFM) ordering at TN. TN is suppressed on application of a field and a complex magnetic phase diagram with three distinct magnetic regimes below the upper critical field can be inferred from our measurements. The magnetic interactions are discussed in relation to a modified spin-1/2 FM-AFM model and the 334 half-twist ladder is compared to other 2-rung ladder spin-1/2 systems.

cond-mat.str-el↗

arXiv2010

Bond-order wave phase, spin solitons and thermodynamics of a frustrated linear spin-1/2 Heisenberg antiferromagnet

The linear spin-1/2 Heisenberg antiferromagnet with exchanges $J_1$, $J_2$ between first and second neighbors has a bond-order wave (BOW) phase that starts at the fluid-dimer transition at $J_2/J_1 = 0.2411$ and is particularly simple at $J_2/J_1 = 1/2$. The BOW phase has a doubly degenerate singlet ground state, broken inversion symmetry and a finite energy gap $E_m$ to the lowest triplet state. The interval $0.4<J_2/J_1<1.0$ has large $E_m$ and small finite size corrections. Exact solutions are presented up to $N=28$ spins with either periodic or open boundary conditions and for thermodynamics up to $N=18$. The elementary excitations of the BOW phase with large $E_m$ are topological spin-1/2 solitons that separate BOWs with opposite phase in a regular array of spins. The molar spin susceptibility $χ_M(T)$ is exponentially small for $T \ll E_m$ and increases nearly linearly with $T$ to a broad maximum. $J_1$, $J_2$ spin chains approximate the magnetic properties of the BOW phase of Hubbard-type models and provide a starting point for modeling alkali-TCNQ salts.

cond-mat.str-el↗

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↗

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↗

arXiv2003

Charge fluctuations and electron-phonon coupling in organic charge-transfer salts with neutral-ionic and Peierls transitions

The first-order transition of the charge-transfer complex TTF-CA (tetrathiafulvalene-chloranil) is both a neutral-ionic and a Peierls transition. In related organic charge transfer complexes, cooling at ambient pressure increases the ionicity $ρ$ in strikingly different ways, and is sometimes accompanied by a dielectric peak, that we relate to lattice stiffness, to structural and energetic disorder, and to the softening of the Peierls mode in the far-IR. The position operator $P$ for systems with periodic boundary conditions makes possible a systematic treatment of electron-phonon interactions in extended donor-acceptor stacks in terms of correlated Peierls-Hubbard models. The IR intensity of the Peierls mode peaks at the Peierls transition at small $ρ< 1/2$ in soft lattices, where the dielectric constant also has a large peak. In dimerized stacks, the IR intensity of totally symmetric, Raman active, molecular vibrations is related to charge fluctuations that modulate site energies. Combination bands of molecular and Peierls modes are identified in regular TTF-CA stacks above Tc. Energetic disorder can suppress the Peierls transition and rationalize a continuous crossover from small to large $ρ$. The TTF-CA scenario of a neutral-regular to ionic-dimerized transition must be broadened considerably in view of charge transfer salts that dimerize on the neutral side, that become ionic without a structural change, or that show vibrational evidence for dimerization at constant $ρ< 1$.

cond-mat.str-el↗

arXiv2003

Electronic polarization in pentacene crystals and thin films

Electronic polarization is evaluated in pentacene crystals and in thin films on a metallic substrate using a self-consistent method for computing charge redistribution in non-overlapping molecules. The optical dielectric constant and its principal axes are reported for a neutral crystal. The polarization energies P+ and P- of a cation and anion at infinite separation are found for both molecules in the crystal's unit cell in the bulk, at the surface, and at the organic-metal interface of a film of N molecular layers. We find that a single pentacene layer with herring-bone packing provides a screening environment approaching the bulk. The polarization contribution to the transport gap P=(P+)+(P-), which is 2.01 eV in the bulk, decreases and increases by only ~ 10% at surfaces and interfaces, respectively. We also compute the polarization energy of charge-transfer (CT) states with fixed separation between anion and cation, and compare to electroabsorption data and to submolecular calculations. Electronic polarization of ~ 1 eV per charge has a major role for transport in organic molecular systems with limited overlap.

cond-mat↗

arXiv2002

Electronic polarization at surfaces and thin films of organic molecular crystals: PTCDA

The electronic polarization energies, P = (P+) + (P-), of a PTCDA (perylenetetracarboxylic acid dianhydride) cation and anion in a crystalline thin film on a metallic substrate are computed and compared with measurements of the PTCDA transport gap on gold and silver. Both experiments and theory show that P is 500 meV larger in a PTCDA monolayer than in 50 A films. Electronic polarization in systems with surfaces and interfaces are obtained self-consistently in terms of charge redistribution within molecules.

cond-mat↗

arXiv2001

Charge redistribution and polarization energy of organic molecular crystals

We present an approach to electronic polarization in molecular solids treated as a set of quantum systems interacting classically. Individual molecules are dealt with rigorously as quantum-mechanical systems subject to classical external fields created by all other molecules and, possibly, external sources. Self-consistent equations are derived for induced dipoles and for atomic charges whose redistribution in external fields is given explicitly by an atom-atom polarizability tensor. Electronic polarization is studied in two representative organic molecular crystals, anthracene and perylenetetracarboxylic acid dianhydride (PTCDA), and contrasted to previous results for systems of polarizable points. The stabilization energies of the neutral lattice, of isolated anions and cations, and of cation-anion pairs are found. Charge redistribution on ions is included. The dielectric tensors of crystals are successfully related to gas-phase properties and provide consistency checks on polarization energies. The procedure is generally applicable to organic crystals in the limit of no intermolecular overlap.

cond-mat↗

arXiv2001

Symmetry crossover and excitation thresholds at the neutral-ionic transition of the modified Hubbard model

Exact ground states, charge densities and excitation energies are found using valence bond methods for N-site modified Hubbard models with uniform spacing. At the neutral-ionic transition (NIT), the ground state has a symmetry crossover in 4n, 4n+2 rings with periodic and antiperiodic boundary conditions, respectively. The modified Hubbard model has a continuous NIT between a diamagnetic band insulator on the paired side and a paramagnetic Mott insulator on the covalent side. The singlet-triplet (ST), singlet-singlet (SS) and charge gaps for finite N indicate that the ST and SS gaps close at the NIT with increasing U and that the charge gap vanishes only there. Finite-N excitations constrain all singularities to about 0.1t of the symmetry crossover. The NIT is interpreted as a localized ground state (gs) with finite gaps on the paired side and an extended gs with vanishing ST and SS gaps on the covalent side. The charge gap and charge stiffness indicate a metallic gs at the transition that, however, is unconditionally unstable to dimerization.

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