arXiv subjects

S. Mazumdar

Publications and source records attributed to S. Mazumdar.

At least 37 records · Page 2Linked to original sources

arXiv2011

The Paired Electron Crystal: order from frustration in the quarter-filled band

We present a study of the effects of simultaneous charge- and spin-frustration on the two-dimensional strongly correlated quarter-filled band on an anisotropic triangular lattice. The broken-symmetry states that dominate in the weakly frustrated region near the rectangular lattice limit are the well known antiferromagnetic state with in-phase lattice dimerization along one direction, and the Wigner crystal state with the checkerboard charge order. For moderate to strong frustration, however, the dominant phase is a novel spin-singlet paired-electron crystal (PEC), consisting of pairs of charge-rich sites separated by pairs of charge-poor sites. The PEC, with coexisting charge-order and spin-gap in two dimension, is the quarter-filled band equivalent of the valence bond solid (VBS) that can appear in the frustrated half-filled band within antiferromagnetic spin Hamiltonians. We discuss the phase diagram as a function of on-site and intersite Coulomb interactions as well as electron-phonon coupling strength. We speculate that the spin-bonded pairs of the PEC can become mobile for even stronger frustration, giving rise to a paired-electron liquid. We discuss the implications of the PEC concept for understanding several classes of quarter-filled band materials that display unconventional superconductivity, focusing in particular on organic charge transfer solids. Our work points out the need to go beyond quantum spin liquid (QSL) concepts for highly frustrated organic charge-transfer solids such as kappa-(BEDT-TTF)_2Cu_2(CN)_3 and EtMe_3Sb[Pd(dmit)_2]_2, which we believe show frustration-induced charge disproportionation at low temperatures. We discuss possible application to layered cobaltates and 1/4-filled band spinels.

cond-mat.str-el↗

arXiv2010

Cooperative orbital ordering and Peierls instability in the checkerboard lattice with doubly degenerate orbitals

It has been suggested that the metal-insulator transitions in a number of spinel materials with partially-filled t_2g d-orbitals can be explained as orbitally-driven Peierls instabilities. Motivated by these suggestions, we examine theoretically the possibility of formation of such orbitally-driven states within a simplified theoretical model, a two-dimensional checkerboard lattice with two directional metal orbitals per atomic site. We include orbital ordering and inter-atom electron-phonon interactions self-consistently within a semi-classical approximation, and onsite intra- and inter-orbital electron-electron interactions at the Hartree-Fock level. We find a stable, orbitally-induced Peierls bond-dimerized state for carrier concentration of one electron per atom. The Peierls bond distortion pattern continues to be period 2 bond-dimerization even when the charge density in the orbitals forming the one-dimensional band is significantly smaller than 1. In contrast, for carrier density of half an electron per atom the Peierls instability is absent within one-electron theory as well as mean-field theory of electron-electron interactions, even for nearly complete orbital ordering. We discuss the implications of our results in relation to complex charge, bond, and orbital-ordering found in spinels.

cond-mat.str-el↗

arXiv2010

The Paired-Electron Crystal in the Two-Dimensional Frustrated Quarter-Filled Band

The competition between antiferromagnetic and spin-singlet ground states within quantum spin models and the 1/2-filled band Hubbard model has received intense scrutiny. Here we demonstrate a frustration-induced transition from Néel antiferromagnetism to spin-singlet in the interacting 1/4-filled band on an anisotropic triangular lattice. While the antiferromagnetic state has equal charge densities 0.5 on all sites, the spin-singlet state is a paired-electron crystal, with pairs of charge-rich sites separated by pairs of charge-poor sites. The paired-electron crystal provides a natural description of the spin-gapped state proximate to superconductivity in many organic charge-transfer solids. Pressure-induced superconductivity in these correlated-electron systems is likely a transition from the 1/4-filled band valence bond solid to a valence bond liquid.

cond-mat.str-el↗

arXiv2010

Theory of interfacial charge-transfer complex photophysics in $π$-conjugated polymer-fullerene blends

We present a theory of the electronic structure and photophysics of 1:1 blends of derivatives of polyparaphenylenevinylene and fullerenes. Within the same Coulomb-correlated Hamiltonian applied previously to interacting chains of single-component $π$-conjugated polymers, we find an exciplex state that occurs below the polymer's optical exciton. Weak absorption from the ground state occurs to the exciplex. We explain transient photoinduced absorptions in the blend, observed for both above-gap and below-gap photoexcitations, within our theory. Photoinduced absorptions for above-gap photoexcitation are from the optical exciton as well as the exciplex, while for below-gap photoexcitation induced absorptions are from the exciplex alone. In neither case are free polarons generated in the time scale of the experiment. Importantly, the photophysics of films of single-component $π$-conjugated polymers and blends can both be understood by extending Mulliken's theory of ground-state charge transfer to the case of excited-state charge transfer.

cond-mat.str-el↗

arXiv2009

Bipolaron Density-Wave Driven By Antiferromagnetic Correlations and Frustration in Organic Superconductors

We describe the Paired Electron Crystal (PEC) which occurs in the interacting frustrated two-dimensional 1/4-filled band. The PEC is a charge-ordered state with nearest-neighbor spin singlets separated by pairs of vacant sites, and can be thought of as a bipolaron density wave. The PEC has been experimentally observed in the insulating state proximate to superconductivity in the organic charge-transfer solids. Increased frustration drives a PEC-to-superconductor transition in these systems.

cond-mat.str-el↗

arXiv2009

Correlated-electron description of the photophysics of thin films of $π$-conjugated polymers

We extend Mulliken's theory of ground state charge transfer in a donor-acceptor complex to excited state charge transfer between pairs of identical $π$-conjugated oligomers, one of which is in the optically excited state and the other in the ground state, leading to the formation of a charge-transfer exciton. Within our theory, optical absorptions from the charge-transfer exciton should include a low energy intermolecular charge-transfer excitation, as well as distinct intramolecular excitations from both the neutral delocalized exciton component and the Coulombically bound polaron-pair component of the charge-transfer exciton. We report high order configuration-interaction calculations for pairs of oligomers of poly-paraphenylenevinylene (PPV) that go beyond our previous single configuration-interaction calculation and find all five excited state absorptions predicted using heuristic arguments based on the Mulliken concept. Our calculated excited state absorption spectrum exhibits strong qualitative agreement with the complete wavelength-dependent ultrafast photoinduced absorption in films of PPV derivatives, suggesting that a significant fraction of the photoinduced absorption here is from the charge-transfer exciton. We make detailed comparisons to experiments, and a testable experimental prediction.

cond-mat.mtrl-sci↗

arXiv2008

Local singlets, frustration, and unconventional superconductivity in the organic charge-transfer solids

We suggest that superconductivity (SC) in the organic charge transfer solids (CTS) is reached from a Bond-Charge Density Wave (BCDW). We discuss an effective model for the BCDW to SC transition, an attractive U extended Hubbard Hamiltonian with repulsive nearest neighbor interaction V. We discuss experimental consequences of the theory for different classes of CTS superconductors as well as related inorganic materials.

cond-mat.supr-con↗

arXiv2008

From valence bond solid to unconventional superconductivity in the organic charge-transfer solids

We show that superconductivity is absent within the 1/2-filled band triangular lattice repulsive Hubbard model that has been proposed for organic charge-transfer solids. We posit that organic superconductivity is rather reached from a Bond-Charge Density Wave that either constitutes the insulating state proximate to superconductivity, or is extremely close in energy to the antiferromagnetic state, and replaces the latter under pressure. The Bond-Charge Density Wave can be described within an effective attractive $U$ extended Hubbard Hamiltonian with repulsive nearest neighbor interaction $V$. A first-order transition from the insulating to the superconducting state occurs within the model with increasing frustration.

cond-mat.supr-con↗

arXiv2008

Absence of superconductivity in the half-filled band Hubbard model on the anisotropic triangular lattice

We report exact calculations of magnetic and superconducting pair-pair correlations for the half-filled band Hubbard model on an anisotropic triangular lattice. Our results for the magnetic phases are similar to those obtained with other techniques. The superconducting pair-pair correlations at distances beyond nearest neighbor decrease monotonically with increasing Hubbard interaction U for all anisotropy, indicating the absence of frustration-driven superconductivity within the model.

cond-mat.str-el↗

arXiv2008

Quantum critical transition from charge-ordered to superconducting state in the triangular lattice negative-U extended Hubbard model

We demonstrate a robust frustration-driven charge-order to superconductivity transition in the half-filled negative-U extended Hubbard model. Superconductivity extends over a broad region of the parameter space. We argue that the model provides the correct insight to understanding unconventional superconductivity in the organic charge-transfer solids and other quarter-filled systems.

cond-mat.str-el↗

arXiv2007

Infrared Investigation of the Charge Ordering Pattern in the Organic Spin Ladder Candidate (DTTTF)2Cu(mnt)2

We measured the variable temperature infrared response of the spin ladder candidate (DTTTF)2Cu(mnt)2 in order to distinguish between two competing ladder models, rectangular versus zigzag, proposed for this family of materials. The distortion along the stack direction below 235 K is consistent with a doubling along b through the metal-insulator transition. While this would agree with either of the ladder models, the concomitant transverse distortion rules out the rectangular ladder model and supports the zigzag scenario. Intramolecular distortions within the DTTTF building block molecule also give rise to on-site charge asymmetry.

cond-mat.other↗

arXiv2007

Temperature-driven transition from the Wigner Crystal to the Bond-Charge-Density Wave in the Quasi-One-Dimensional Quarter-Filled band

It is known that within the interacting electron model Hamiltonian for the one-dimensional 1/4-filled band, the singlet ground state is a Wigner crystal only if the nearest neighbor electron-electron repulsion is larger than a critical value. We show that this critical nearest neighbor Coulomb interaction is different for each spin subspace, with the critical value decreasing with increasing spin. As a consequence, with the lowering of temperature, there can occur a transition from a Wigner crystal charge-ordered state to a spin-Peierls state that is a Bond-Charge-Density Wave with charge occupancies different from the Wigner crystal. This transition is possible because spin excitations from the spin-Peierls state in the 1/4-filled band are necessarily accompanied by changes in site charge densities. We apply our theory to the 1/4-filled band quasi-one-dimensional organic charge-transfer solids in general and to 2:1 tetramethyltetrathiafulvalene (TMTTF) and tetramethyltetraselenafulvalene (TMTSF) cationic salts in particular. We believe that many recent experiments strongly indicate the Wigner crystal to Bond-Charge-Density Wave transition in several members of the TMTTF family. We explain the occurrence of two different antiferromagnetic phases but a single spin-Peierls state in the generic phase diagram for the 2:1 cationic solids. The antiferromagnetic phases can have either the Wigner crystal or the Bond-Charge-Spin-Density Wave charge occupancies. The spin-Peierls state is always a Bond-Charge-Density Wave.

cond-mat.str-el↗

arXiv2007

Pinned Low Energy Electronic Excitation in Metal Exchanged Vanadium Oxide Nanoscrolls

We measured the optical properties of mixed valent vanadium oxide nanoscrolls and their metal exchanged derivatives in order to investigate the charge dynamics in these compounds. In contrast to the prediction of a metallic state for the metal exchanged derivatives within a rigid band model, we find that the injected charges in Mn$^{2+}$ exchanged vanadium oxide nanoscrolls are pinned. A low-energy electronic excitation associated with the pinned carriers appears in the far infrared and persists at low temperature, suggesting that the nanoscrolls are weak metals in their bulk form, dominated by inhomogeneous charge disproportionation and Madelung energy effects.

cond-mat.mtrl-sci↗

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

Controlling quantum transport through a single molecule

We investigate multi-terminal quantum transport through single monocyclic aromatic annulene molecules, and their derivatives, using the nonequilibrium Green function approach in the self-consistent Hartree-Fock approximation. A new device concept, the Quantum Interference Effect Transistor (QuIET) is proposed, exploiting perfect destructive interference stemming from molecular symmetry, and controlling current flow by introducing decoherence and/or elastic scattering that break the symmetry. This approach overcomes the fundamental problems of power dissipation and environmental sensitivity that beset many nanoscale device proposals.

cond-mat.mes-hall↗

arXiv2005

Density matrix renormalization group study of conjugated polymers with transverse pi-conjugation

We report accurate numerical studies of excited state orderings in long hypothetical pi-conjugated oligomers in which the hydrogen atoms of trans-polyacetylene are replaced with conjugated sidegroups, within modified Hubbard models. There exists a range of the bare Coulomb repulsion for which the excited state ordering is conducive to photoluminescence in the substituted systems, even as this ordering is opposite in the unsubstituted polyenes of the same lengths. Our work provides motivation to study real pi-conjugated polymers with transverse conjugation and small optical gaps.

cond-mat.str-el↗

arXiv2005

Universal properties of quasi-one-dimensional excitons in semiconducting single-walled carbon nanotubes and $π$-conjugated polymers

The nature of the primary photoexcitations in semiconducting single-walled carbon nanotubes (S-SWCNTs) is of strong current interest. We have studied the emission spectra of S-SWCNTs and two different $π$-conjugated polymers in solutions and films, and have also performed ultrafast pump-probe spectroscopy on these systems. The emission spectra relative to the absorption bands are very similar in S-SWCNTs and polymers, with redshifted photoluminescence in films showing exciton migration. The transient photoinduced absorptions (PAs) in SWCNTs and $π$-conjugated polymers are also remarkably similar, with a low energy PA$_1$ and a higher energy PA$_2$ in all cases. Theoretical calculations of excited state absorptions within a correlated $π$-electron Hamiltonian find the same excitonic energy spectrum for S-SWCNTs and $π$-conjugated polymers, illustrating the universal features of quasi-one-dimensional excitons in carbon-based $π$-conjugated systems. In both cases PA$_1$ is an excited state absorption from the optically allowed exciton to a two-photon exciton that occurs below the continuum band threshold. PA$_1$ therefore gives the lower limit of the binding energy of the lowest optical exciton. The binding energy of lowest exciton belonging to the widest S-SWCNTs with diameters $\geq$ 1 nm in films is 0.3--0.4 eV, as determined by both experimental and theoretical methods.

cond-mat.mtrl-sci↗

arXiv2005

Electroabsorption spectroscopy of single walled nanotubes

We have measured the electric field modulated absorption of a sample of single-walled nanotubes (SWNT) suspended in a solid polyvinyl alcohol matrix. The electroabsorption (EA) spectrum roughly follows the first derivative of the absorption with respect to photon energy, scales quadratically with the electric field strength, and shows a pronounced anisotropy of light polarization with respect to the applied electric field direction. These findings indicate a quadratic Stark effect caused by a change in the polarizability of the excited states, which is common to quasi-one dimensional (1D) excitons in organic semiconductors. The EA spectrum is well described by calculations involving electron-electron interaction in the model Hamiltonian of both zigzag and chiral nanotubes. We have calculated the EA spectra for both zigzag and chiral nanotubes within a model Hamiltonian that includes electron-electron interactions. The calculations reproduce the observed quadratic Stark shift of the lowest optical exciton, as well as the more complicated behavior of the EA spectrum in the energy region that corresponds to the next higher exciton. Our findings show that the low-lying absorption bands in semiconducting SWNT are excitonic in origin, in agreement with transient optical measurements that identify the primary photoexcitations in SWNT as quasi-1D excitons with a substantial binding energy.

cond-mat.mtrl-sci↗