arXiv subjects

K. Aryanpour

Publications and source records attributed to K. Aryanpour.

15 recordsLinked to original sources

arXiv2014

Electron Correlations and Two-Photon States in Polycyclic Aromatic Hydrocarbon Molecules: A Peculiar Role of Geometry

We present numerical studies of one- and two-photon excited states ordering in a number of polycyclic aromatic hydrocarbon molecules: coronene, hexa-peri-hexabenzocoronene and circumcoronene, all possessing $D_{6h}$ point group symmetry versus ovalene with $D_{2h}$ symmetry, within the Pariser-Parr-Pople model of interacting $π$-electrons. The calculated energies of the two-photon states as well as their relative two-photon absorption cross-sections within the interacting model are qualitatively different from single-particle descriptions. More remarkably, a peculiar role of molecular geometry is found. The consequence of electron correlations is far stronger for ovalene, where the lowest spin-singlet two-photon state is a quantum superposition of pairs of lowest spin triplet states, as in the linear polyenes. The same is not true for $D_{6h}$ group hydrocarbons. Our work indicates significant covalent character, in valence bond language, of the ground state, the lowest spin triplet state and a few of the lowest two-photon states in $D_{2h}$ ovalene but not in those with $D_{6h}$ symmetry.

cond-mat.str-el↗

arXiv2014

Subgap Two-Photon States in Polycyclic Aromatic Hydrocarbons: Evidence for Strong Electron Correlations

Strong electron correlation effects in the photophysics of quasi-one-dimensional $π$-conjugated organic systems such as polyenes, polyacetylenes, polydiacetylenes, etc., have been extensively studied. Far less is known on correlation effects in two-dimensional $π$-conjugated systems. Here we present theoretical and experimental evidence for moderate repulsive electron-electron interactions in a number of finite polycyclic aromatic hydrocarbon molecules with $D_{6h}$ symmetry. We show that the excited state orderings in these molecules are reversed relative to that expected within one-electron and mean-field theories. Our results reflect similarities as well as differences in the role and magnitude of electron correlation effects in these two-dimensional molecules compared to those in polyenes.

cond-mat.str-el↗

arXiv2013

Does Singlet Fission Enhance the Performance of Organic Solar Cells?

Singlet fission, in which the optical spin-singlet exciton dissociates into two low energy triplet excitons, has been proposed as a viable approach to enhance the quantum efficiency of organic solar cells. We show that even when singlet fission is occurring in the donor molecule, the electronic structure at the donor$-$acceptor interface must satisfy specific requirements for the solar cell performance to be enhanced by this process. We focus on the pentacene$-$C$_{60}$ solar cell, and on the basis of our calculations and available experimental data, we conclude that there is not enough evidence that these requirements are met by the donor$-$acceptor interface here. We propose experiments that can determine whether the minimal requirement for enhanced performance driven by singlet fission is met in this and other solar cells.

cond-mat.str-el↗

arXiv2012

Triplet excitations in carbon nanostructures

We show that the energy differences between the lowest optical singlet exciton and the lowest triplet exciton in semiconducting single-walled carbon nanotubes with diameter $\sim 1$ nm and graphene nanoribbons with widths $\sim 2$ nm are an order of magnitude smaller than in the $π$-conjugated polymer poly(para-phenylenevinylene). Our calculated energy gaps between the singlet and triplet excitons are in excellent agreement with the measured values in three different nanotubes with diameters close to 1 nm. The spatial extent of the triplet exciton is nearly the same as that of the singlet exciton in wide nanotubes and nanoribbons, in contrast to that in $π$-conjugated polymers, in which the triplet exciton exhibits strong spatial confinement. Weakly confined behavior of the triplet state begins in nanoribbons with widths as narrow as 2.5 times the graphene unit lattice vector. We discuss possible consequences of the small singlet-triplet energy difference in the carbon nanostructures on device applications.

cond-mat.mes-hall↗

arXiv2011

Evidence for Excimer Photoexcitations in an Ordered π-Conjugated Polymer Film

We report pressure-dependent transient picosecond and continuous-wave photomodulation studies of disordered and ordered films of 2-methoxy-5-(2-ethylhexyloxy) poly(para-phenylenevinylene). Photoinduced absorption (PA) bands in the disordered film exhibit very weak pressure dependence and are assigned to intrachain excitons and polarons. In contrast, the ordered film exhibits two additional transient PA bands in the midinfrared that blueshift dramatically with pressure. Based on high-order configuration interaction calculations we ascribe the PA bands in the ordered film to excimers. Our work brings insight to the exciton binding energy in ordered films versus disordered films and solutions. The reduced exciton binding energy in ordered films is due to new energy states appearing below the continuum band threshold of the single strand.

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

Ferromagnetic Spin Coupling as the Origin of 0.7 Anomaly in Quantum Point Contacts

We study one-dimensional itinerant electron models with ferromagnetic coupling to investigate the origin of 0.7 anomaly in quantum point contacts. Linear conductance calculations from the quantum Monte Carlo technique for spin interactions of different spatial range suggest that $0.7(2e^{2}/h)$ anomaly results from a strong interaction of low-density conduction electrons to ferromagnetic fluctuations formed across the potential barrier. The conductance plateau appears due to the strong incoherent scattering at high temperature when the electron traversal time matches the time scale of dynamic ferromagnetic excitations.

cond-mat.mes-hall↗

arXiv2007

s-wave Superconductivity Phase Diagram in the Inhomogeneous Two-Dimensional Attractive Hubbard Model

We study s-wave superconductivity in the two-dimensional square lattice attractive Hubbard Hamiltonian for various inhomogeneous patterns of interacting sites. Using the Bogoliubov-de Gennes (BdG) mean field approximation, we obtain the phase diagram for inhomogeneous patterns in which the on-site attractive interaction U_i between the electrons takes on two values, U_i=0 and -U/(1-f) (with f the concentration of non-interacting sites) as a function of average electron occupation per site n, and study the evolution of the phase diagram as f varies. In certain regions of the phase diagram, inhomogeneity results in a larger zero temperature average pairing amplitude (order parameter) and also a higher superconducting (SC) critical temperature T_c, relative to a uniform system with the same mean interaction strength (U_i=-U on all sites). These effects are observed for stripes, checkerboard, and even random patterns of the attractive centers, suggesting that the pattern of inhomogeneity is unimportant. The phase diagrams also include regions where superconductivity is obliterated due to the formation of various charge ordered phases. The enhancement of T_{c} due to inhomogeneity is robust as long as the electron doping per site n is less than twice the fraction of interacting sites [2(1-f)] regardless of the pattern. We also show that for certain inhomogeneous patterns, when n = 2(1-f), increasing temperature can work against the stability of existing charge ordered phases for large f and as a result, enhance T_{c}.

cond-mat.supr-con↗

arXiv2006

Dynamical mean field study of the Mott transition in the half-filled Hubbard model on a triangular lattice

We employ dynamical mean field theory (DMFT) with a Quantum Monte Carlo (QMC) atomic solver to investigate the finite temperature Mott transition in the Hubbard model with the nearest neighbor hopping on a triangular lattice at half-filling. We estimate the value of the critical interaction to be $U_c=12.0 \pm 0.5$ in units of the hopping amplitude $t$ through the evolution of the magnetic moment, spectral function, internal energy and specific heat as the interaction $U$ and temperature $T$ are varied. This work also presents a comparison between DMFT and finite size determinant Quantum Monte Carlo (DQMC) and a discussion of the advantages and limitations of both methods.

cond-mat.str-el↗

arXiv2006

Effect of inhomogeneity on s-wave superconductivity in the attractive Hubbard model

Inhomogeneous s-wave superconductivity is studied in the two-dimensional, square lattice attractive Hubbard Hamiltonian using the Bogoliubov-de Gennes (BdG) mean field approximation. We find that at weak coupling, and for densities mainly below half-filling, an inhomogeneous interaction in which the on-site interaction $U_i$ takes on two values, $U_i=0, 2U$ results in a larger zero temperature pairing amplitude, and that the superconducting $T_c$ can also be significantly increased, relative to a uniform system with $U_i=U$ on all sites. These effects are observed for stripe, checkerboard, and even random patterns of the attractive centers, suggesting that the pattern of inhomogeneity is unimportant. Monte Carlo calculations which reintroduce some of the fluctuations neglected within the BdG approach see the same effect, both for the attractive Hubbard model and a Hamiltonian with d-wave pairing symmetry.

cond-mat.supr-con↗

arXiv2005

Dynamics of Impurity and Valence Bands in GaMnAs within the Dynamical Mean Field Approximation

We calculate the density-of-states and the spectral function of GaMnAs within the dynamical mean-field approximation. Our model includes the competing effects of the strong spin-orbit coupling on the J=3/2 GaAs hole bands and the exchange interaction between the magnetic ions and the itinerant holes. We study the quasi-particle and impurity bands in the paramagnetic and ferromagnetic phases for different values of impurity-hole coupling at the Mn doping of x=0.05. By analyzing the anisotropic angular distribution of the impurity band carriers at T=0, we conclude that the carrier polarization is optimal when the carriers move along the direction parallel to the average magnetization.

cond-mat.str-el↗

arXiv2005

The Dynamical Cluster Approximation (DCA) versus the Cellular Dynamical Mean Field Theory (CDMFT) in strongly correlated electrons systems

We are commenting on the article Phys. Rev. {\bf B 65}, 155112 (2002) by G. Biroli and G. Kotliar in which they make a comparison between two cluster techniques, the {\it Cellular Dynamical Mean Field Theory} (CDMFT) and the {\it Dynamical Cluster Approximation} (DCA). Based upon an incorrect implementation of the DCA technique in their work, they conclude that the CDMFT is a faster converging technique than the DCA. We present the correct DCA prescription for the particular model Hamiltonian studied in their article and conclude that the DCA, once implemented correctly, is a faster converging technique for the quantities averaged over the cluster. We also refer to their latest response to our comment where they argue that instead of averaging over the cluster, local observables should be calculated in the bulk of the cluster which indeed makes them converge much faster in the CDMFT than in the DCA. We however show that in their original work, the authors themselves use the cluster averaged quantities to draw their conclusions in favor of using the CDMFT over the DCA.

cond-mat.str-el↗

arXiv2004

Magnetism in semiconductors: A dynamical mean field study of ferromagnetism in Ga_{1-x}Mn_xAs

We employ the dynamical mean field approximation to perform a systematic study of magnetism in Ga_{1-x}Mn_xAs. Our model incorporates the effects of the strong spin-orbit coupling on the J=3/2 GaAs valence bands and of the exchange interaction between the randomly distributed magnetic ions and the itinerant holes. The ferromagnetic phase transition temperature T_c is obtained for different values of the impurity-hole coupling J_c and of the hole concentration n_h at the Mn doping of x=0.05. We also investigate the temperature dependence of the local magnetization and spin polarization of the holes. By comparing our results with those for a single band Hamiltonian in which the spin-orbit coupling is switched off, we conclude that the spin-orbit coupling in Ga_{1-x}Mn_xAs gives rise to frustration in the ferromagnetic order, strengthening recent findings by Zarand and Janko (Phys. Rev. Lett. 89, 047201 (2002)).

cond-mat.str-el↗

arXiv2002

Dynamical Cluster Approximation Employing FLEX as a Cluster Solver

We employ the Dynamical Cluster Approximation (DCA) in conjunction with the Fluctuation Exchange Approximation (FLEX) to study the Hubbard model. The DCA is a technique to systematically restore the momentum conservation at the internal vertices of Feynman diagrams relinquished in the Dynamical Mean Field Approximation (DMFA). FLEX is a perturbative diagrammatic approach in which classes of Feynman diagrams are summed over analytically using geometric series. The FLEX is used as a tool to investigate the complementarity of the DCA and the finite size lattice technique with periodic boundary conditions by comparing their results for the Hubbard model. We also study the microscopic theory underlying the DCA in terms of compact (skeletal) and non-compact diagrammatic contributions to the thermodynamic potential independent of a specific model. The significant advantages of the DCA implementation in momentum space suggests the development of the same formalism for the frequency space. However, we show that such a formalism for the Matsubara frequencies at finite temperatures leads to acausal results and is not viable. However, a real frequency approach is shown to be feasible.

cond-mat.str-el↗

arXiv2002

Analysis of the dynamical cluster approximation for the Hubbard model

We examine a central approximation of the recently introduced Dynamical Cluster Approximation (DCA) by example of the Hubbard model. By both analytical and numerical means we study non-compact and compact contributions to the thermodynamic potential. We show that approximating non-compact diagrams by their cluster analogs results in a larger systematic error as compared to the compact diagrams. Consequently, only the compact contributions should be taken from the cluster, whereas non-compact graphs should be inferred from the appropriate Dyson equation. The distinction between non-compact and compact diagrams persists even in the limit of infinite dimensions. Non-local corrections beyond the DCA exist for the non-compact diagrams, whereas they vanish for compact diagrams.

cond-mat.str-el↗