arXiv subjects

D. L. Cox

Publications and source records attributed to D. L. Cox.

At least 19 recordsLinked to original sources

arXiv2006

Influence of Correlated Hybridization on the Conductance of Molecular Transistors

We study the spin-1/2 single-channel Anderson impurity model with correlated (occupancy dependent) hybridization for molecular transistors using the numerical renormalization-group method. Correlated hybridization can induce nonuniversal deviations in the normalized zero-bias conductance and, for some parameters, modestly enhance the spin polarization of currents in applied magnetic field. Correlated hybridization can also explain a gate-voltage dependence to the Kondo scale similar to what has been observed in recent experiments.

cond-mat.str-el↗

arXiv2006

Correlated hybridization in transition metal complexes

We apply local orbital basis density functional theory (using SIESTA) coupled with a mapping to the Anderson impurity model to estimate the Coulomb assisted or correlated hybridization between transition metal d-orbitals and ligand sp-orbitals for a number of molecular complexes. We find remarkably high values which can have several physical implications including: (i) renormalization of effective single band or multiband Hubbard model parameters for the cuprates and, potentially, elemental iron, and (ii) spin polarizing molecular transistors.

cond-mat.str-el↗

arXiv2005

Optical conductivity of wet DNA

Motivated by recent experiments we have studied the optical conductivity of DNA in its natural environment containing water molecules and counter ions. Our density functional theory calculations (using SIESTA) for four base pair B-DNA with order 250 surrounding water molecules suggest a thermally activated doping of the DNA by water states which generically leads to an electronic contribution to low-frequency absorption. The main contributions to the doping result from water near DNA ends, breaks, or nicks and are thus potentially associated with temporal or structural defects in the DNA.

cond-mat.soft↗

arXiv2005

Phase diagram of the one-dimensional, two-channel Kondo lattice model

Employing the density matrix renormalization group method and strong-coupling perturbation theory, we study the phase diagram of the SU(2)xSU(2) Kondo lattice model in one dimension. We show that, at quarter filling, the system can exist in two phases depending on the coupling strength. The weak-coupling phase is dominated by RKKY exchange correlations while the strong-coupling phase is characterized by strong antiferromagnetic correlations of the channel degree of freedom. These two phases are separated by a quantum critical point. For conduction-band fillings of less than one quarter, we find a paramagnetic metallic phase at weak coupling and a ferromagnetic phase at moderate to strong coupling.

cond-mat.str-el↗

arXiv2004

An Anderson Impurity Model for Efficient Sampling of Adiabatic Potential Energy Surfaces of Transition Metal Complexes

We present a model intended for rapid sampling of ground and excited state potential energy surfaces for first-row transition metal active sites. The method is computationally inexpensive and is suited for dynamics simulations where (1) adiabatic states are required "on-the-fly" and (2) the primary source of the electronic coupling between the diabatic states is the perturbative spin-orbit interaction among the 3d electrons. The model Hamiltonian we develop is a variant of the Anderson impurity model and achieves efficiency through a physically motivated basis set reduction based on the large value of the d-d Coulomb interaction U_{d} and a Lanczos matrix diagonalization routine to solve for eigenvalues. The model parameters are constrained by fits to the partial density of states (PDOS) obtained from ab initio density functional theory calculations. For a particular application of our model we focus on electron-transfer occuring between cobalt ions solvated by ammonium, incorporating configuration interaction between multiplet states for both metal ions. We demonstrate the capability of the method to efficiently calculate adiabatic potential energy surfaces and the electronic coupling factor we have calculated compares well to previous calculations and experiment.

physics.chem-ph↗

arXiv2002

Theory of adiabatic Hexaamminecobalt-Self-Exchange

We have reexamined the thermally induced Co(NH_3)_6^{2+/3+} [Co(II/III)] redox reaction using the first principles density-functional-theory method, semiclassical Marcus theory, and known charge transfer parameters. We confirm a previously suggested mechanism involving excited state (^2E_g) of Co(II) which becomes lower than the ground state (^4T_1g) in the transition state region. This lowers the transition state barrier considerably by about 6.9 kcal/mol and leads to a spin-allowed and adiabatic electron exchange process. Our calculations are consistent with previous experimental results regarding the spin-excitation energy (^3T_1g) of Co(III), and the fact that an optical absorption peak (^2E_g) of the Co(II) species could not be found experimentally. Our rate is of order 6 10^{-3} 1/Ms and hence 2 orders of magnitude faster than determined previously by experiments.

physics.chem-ph↗

arXiv2002

Electronic properties of DNA: structural and chemical influence on the quest for high conductance and charge transfer

Motivated by the wide ranging experimental results on the conductivity of DNA, we have investigated extraordinary configurations and chemical environments in which DNA might become a true molecular wire, perticularly from enhanced electronic overlaps or from small activation energies. In particular, we examine A- vs B-DNA, the ribbon-like structures proposed to arise from molecular stretching, the potential role of counterions in hole doping the DNA orbitals, the possibility of backbone conduction, and the effects of water. We find that small activation gaps observed in conductivity experiments may arise in the presence of water and counter ions. We further discuss the role of harmonic vibration and twisting motion on electron tight binding matrix elements using ab initio density functional theory and model Koster-Slater theory calculations. We find that partial cancellation between pp-sigma and pp-pi interaction of Pz orbitals on adjacent base pairs, along with destructive interference of phase factors are needed to explain the weak conductance of A-DNA. Our results lead also to a physical interpretation of the angular dependence of inter-base pair tight binding matrix elements. Furthermore, we estimate Franck-Condon factors, reorganization energies and nuclear frequencies essential for charge transfer rates, and find our estimated hole transfer rates between base pairs to be in excellent agreement with recent picosecond dynamics data.

cond-mat.soft↗

arXiv2002

Theoretical modeling of prion disease incubation

We present a theory for the laboratory and epidemiological data for incubation times in infectious prion diseases. The central feature of our model is that slow growth of misfolded protein-aggregates from small initial seeds controls the `latent' or `lag' phase, whereas aggregate-fissioning and subsequent spreading leads to an exponential growth or doubling phase. Such a general framework can account for many features of prion diseases including the striking reproducibility of incubation times when high doses are inoculated into lab animals. Broad incubation time distributions arise for low infectious dose, while our calculated distributions narrow to sharply defined onset times with increased dose. We apply our distributions to epidemiological vCJD data and extract estimates of incubation times.

cond-mat↗

arXiv2002

Mediation of Long Range Charge Transfer by Kondo Bound States

We present a theory of non-equilibrium long range charge transfer between donor and acceptor centers in a model polymer mediated by magnetic exciton (Kondo) bound states. Our model produces electron tunneling lengths easily exceeding 10$Å$, as observed recently in DNA and organic charge transfer systems. This long ranged tunneling is effective for weak to intermediate donor-bridge coupling, and is enhanced both by weak to intermediate strength Coulomb hole-electron attraction (through the orthogonality catastrophe) and by coupling to local vibrational modes.

cond-mat.str-el↗

arXiv2002

Strong electron correlations in cobalt valence tautomers

We have examined cobalt based valence tautomer molecules such as Co(SQ)$_2$(phen) using density functional theory (DFT) and variational configuration interaction (VCI) approaches based upon a model Hamiltonian. Our DFT results extend earlier work by finding a reduced total energy gap (order 0.6 eV) between high temperature and low temperature states when we fully relax the coordinates (relative to experimental ones). Futhermore we demonstrate that the charge transfer picture based upon formal valence arguments succeeds qualitatively while failing quantitatively due to strong covalency between the Co 3$d$ orbitals and ligand $p$ orbitals. With the VCI approach, we argue that the high temperature, high spin phase is strongly mixed valent, with about 30 % admixture of Co(III) into the predominantly Co(II) ground state. We confirm this mixed valence through a fit to the XANES spectra. Moreover, the strong electron correlations of the mixed valent phase provide an energy lowering of about 0.2-0.3 eV of the high temperature phase relative to the low temperature one. Finally, we use the domain model to account for the extraordinarily large entropy and enthalpy values associated with the transition.

cond-mat↗

arXiv2001

On the statistical mechanics of prion diseases

We simulate a two-dimensional, lattice based, protein-level statistical mechanical model for prion diseases (e.g., Mad Cow disease) with concommitant prion protein misfolding and aggregation. Our simulations lead us to the hypothesis that the observed broad incubation time distribution in epidemiological data reflect fluctuation dominated growth seeded by a few nanometer scale aggregates, while much narrower incubation time distributions for innoculated lab animals arise from statistical self averaging. We model `species barriers' to prion infection and assess a related treatment protocol.

cond-mat.stat-mech↗

arXiv1999

Theory of "ferrisuperconductivity" in $U_{1-x}Th_xBe_{13}$

We construct a two component Ginzburg-Landau theory with coherent pair motion and incoherent quasiparticles for the phase diagram of $U_{1-x}Th_xBe_{13}$. The two staggered superconducting states live at the Brillouin zone center and the zone boundary, and coexist for temperatures $T\le T_{c2}$ at concentrations $x_{c1}\approx 0.02\le x \le x_{c2}\approx 0.04$. We predict below $T_{c2}$ appearance of a charge density wave (CDW) and Be-sublattice distortion. The distortion explains the $μ$SR relaxation anomaly, and Th-impurity mediated scattering of ultrasound to CDW fluctuations explains the attenuation peak.

cond-mat.str-el↗

arXiv1998

Multi-Orbital Hubbard Model in Infinite Dimensions: Quantum Monte Carlo Calculation

Using Quantum Monte Carlo we compute thermodynamics and spectra for the orbitally degenerate Hubbard model in infinite spatial dimensions. With increasing orbital degeneracy we find in the one-particle spectra: broader Hubbard bands (consistent with increased kinetic energy), a narrowing Mott gap, and increasing quasi-particle spectral weight. In opposition, Hund's rule exchange coupling decreases the critical on-site Coulomb energy for the Mott transition. The metallic regime resistivity for two-fold degeneracy is quadratic-in-temperature at low temperatures.

cond-mat.str-el↗

arXiv1997

Exotic Kondo Effects in Metals: Magnetic Ions in a Crystalline Electric Field and Tunneling Centers

This review article provides an overview of the physics of the two-channel Kondo impurity model as manifested in two-level systems in metals and certain actinide/lanthanide ions in metals. Basic models are presented, followed by a discussion of the multiplicative renormalization group, numerical renormalization group, non-crossing approximation, conformal field theory, abelian bosonization, and Bethe-ansatz approaches to the models. An extensive discussion of experiment is presented for both classes of models, with critical attention paid to the relevance of the models to the data. Finally, a last section details other models which are related, approaches to the lattice via two impurity and infinite dimension models, and the connection of these models to exotic odd-frequency superconductivity. Also available at http://onsager.ucdavis.edu/~cox/REVIEW/drmpmain2.ps.gz

cond-mat.str-el↗

arXiv1997

Staggered Pairing Phenomenology for UPd_2Al_3 and UNi_2Al_3

We apply the staggered-pairing Ginzburg-Landau phenomenology to describe superconductivity in UPd_2Al_3 and UNi_2Al_3. The phenomenology was applied successfully to UPt_3 so it explains why these materials have qualitatively different superconducting phase diagrams although they have the same point-group symmetry. UPd_2Al_3 and UNi_2Al_3 have a two-component superconducting order parameter transforming as an H-point irreducible representation of the space group. Staggered superconductivity can induce charge-density waves characterized by new Bragg peaks suggesting experimental tests of the phenomenology.

cond-mat.supr-con↗

arXiv1997

Calculations of the Knight Shift Anomalies in Heavy Electron Materials

We have studied the Knight shift $K(\vec r, T)$ and magnetic susceptibility $χ(T)$ of heavy electron materials, modeled by the infinite U Anderson model with the NCA method. A systematic study of $K(\vec r, T)$ and $χ(T)$ for different Kondo temperatures $T_0$ (which depends on the hybridization width $Γ$) shows a low temperature anomaly (nonlinear relation between $K$ and $χ$) which increases as the Kondo temperature $T_0$ and distance $r$ increase. We carried out an incoherent lattice sum by adding the $K(\vec r)$ of a few hundred shells of rare earth atoms around a nucleus and compare the numerically calculated results with the experimental results. For CeSn_3, which is a concentrated heavy electron material, both the ^{119}Sn NMR Knight shift and positive muon Knight shift are studied. Also, lattice coherence effects by conduction electron scattering at every rare earth site are included using the average-T matrix approximation. Also NMR Knight shifts for YbCuAl and the proposed quadrupolar Kondo alloy Y_{0.8}U_{0.2}Pd_{3} are studied.

cond-mat.str-el↗

arXiv1996

Phase Diagram of the Two-Channel Kondo Lattice

The phase diagram of the two-channel Kondo lattice model is examined with a Quantum Monte Carlo simulation in the limit of infinite dimensions. Commensurate (and incommensurate) antiferromagnetic and superconducting states are found. The antiferromagnetic transition is very weak and continuous; whereas the superconducting transition is discontinuous to an odd-frequency channel-singlet and spin-singlet pairing state.

cond-mat↗

arXiv1996

Magneto-Resistance in the Two-Channel Anderson Lattice

The paramagnetic phase of the two channel Anderson Lattice model in the Kondo limit is investigated in infinite spatial dimensions using the non-crossing approximation. The resistivity exhibits a Kondo upturn with decreasing $T$, followed by a slow decrease to a finite value at $T=0$. The decrease reflects lattice coherence effects in concert with particle-hole symmetry breaking. The magneto-resistance obeys an approximate scaling relation, decreasing towards coherent Fermi liquid behavior with increasing field. The magnetic field induces a Drude peak in the optical conductivity.

cond-mat↗