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Roser Valentí

Publications and source records attributed to Roser Valentí.

106 records · Page 6Linked to original sources

Unfolding of the electronic structure through the induced representations of space groups: Application to Fe-based superconductors

We revisit the problem that relevant parts of bandstructures for a given cell choice can reflect exact or approximate higher symmetries of subsystems in the cell and can therefore be significantly simplified by an unfolding procedure that recovers the higher symmetry. We show that bandstructure unfolding can be understood as projection onto induced irreducible representations of a group obtained by extending the original group of translations with a number of additional symmetry operations. The resulting framework allows us to define a generalized unfolding procedure which includes the point group operations and can be applied to any quantity in the reciprocal space. The unfolding of the Brillouin zone follows naturally from the properties of the induced irreducible representations. In this context, we also introduce a procedure to derive tight-binding models of reduced dimensionality by making use of point group symmetries. Further, we show that careful consideration of unfolding has important consequences on the interpretation of angle resolved photoemission experiments. Finally, we apply the unfolding procedure to various representative examples of Fe-based superconductor compounds and show that the one iron picture arises as an irreducible representation of the glide mirror group and we comment on the consequences for the interpretation of one-iron versus two-iron Brillouin zone representations.

cond-mat.str-el↗

One-dimensional spin liquid, collinear, and spiral phases from uncoupled chains to the triangular lattice

We investigate the Hubbard model on the anisotropic triangular lattice with two hopping parameters $t$ and $t^\prime$ in different spatial directions, interpolating between decoupled chains ($t=0$) and the isotropic triangular lattice ($t=t^\prime$). Variational wave functions that include both Jastrow and backflow terms are used to compare spin-liquid and magnetic phases with different pitch vectors describing both collinear and coplanar (spiral) order. For relatively large values of the on-site interaction $U/t^\prime \gtrsim 10$ and substantial frustration, i.e., $0.3\lesssim t/t^\prime \lesssim 0.8$, the spin-liquid state is clearly favored over magnetic states. Spiral magnetic order is only stable in the vicinity of the isotropic point, while collinear order is obtained in a wide range of inter-chain hoppings from small to intermediate frustration.

cond-mat.str-el↗

Phase diagram of the square lattice bilayer Hubbard model: a variational Monte Carlo study

We investigate the phase diagram of the square lattice bilayer Hubbard model at half filling with the variational Monte Carlo method for both the magnetic and the paramagnetic case as a function of interlayer hopping t_perp and on-site Coulomb repulsion U. With this study we resolve some discrepancies in previous calculations based on the dynamical mean field theory, and we are able to determine the nature of the phase transitions between metal, Mott insulator and band insulator. In the magnetic case we find only two phases: An antiferromagnetic Mott insulator at small t_perp for any value of U and a band insulator at large t_perp. At large U values we approach the Heisenberg limit. The paramagnetic phase diagram shows at small t_perp a metal to Mott insulator transition at moderate U values and a Mott to band insulator transition at larger U values. We also observe a reentrant Mott insulator to metal transition and metal to band insulator transition for increasing t_perp in the range of 5.5t < U < 7.5t. Finally, we discuss the obtained phase diagrams in relation to previous studies based on different many-body approaches.

cond-mat.str-el↗

Absence of metallicity in K-doped picene: Importance of electronic correlations

Potassium-doped picene (K$_x$picene) has recently been reported to be a superconductor at $x=3$ with critical temperatures up to 18 K. Here we study the electronic structure of K-doped picene films by photoelectron spectroscopy and {\it ab initio} density functional theory combined with dynamical mean-field theory (DFT+DMFT). Experimentally we observe that, except for spurious spectral weight due to the lack of a homogeneous chemical potential at low K-concentrations ($x \approx 1$), the spectra always display a finite energy gap. This result is supported by our DFT+DMFT calculations which provide clear evidence that K$_x$picene is a Mott insulator for integer doping concentrations $x=1$, 2, and 3. We discuss various scenarios to understand the discrepancies with previous reports of superconductivity and metallic behavior.

cond-mat.str-el↗

Electronic properties of Fabre charge-transfer salts under various temperature and pressure conditions

Using density functional theory, we determine parameters of tight-binding Hamiltonians for a variety of Fabre charge transfer salts, focusing in particular on the effects of temperature and pressure. Besides relying on previously published crystal structures, we experimentally determine two new sets of structures; (TMTTF)$_2$SbF$_6$ at different temperatures and (TMTTF)$_2$PF$_6$ at various pressures. We find that a few trends in the electronic behavior can be connected to the complex phase diagram shown by these materials. Decreasing temperature and increasing pressure cause the systems to become more two-dimensional. We analyze the importance of correlations by considering an extended Hubbard model parameterized using Wannier orbital overlaps and show that while charge order is strongly activated by the inter-site Coulomb interaction, the magnetic order is only weakly enhanced. Both orders are suppressed when the effective pressure is increased.

cond-mat.str-el↗

Spin-liquid versus spiral-order phases in the anisotropic triangular lattice

We study the competition between magnetic and spin-liquid phases in the Hubbard model on the anisotropic triangular lattice, which is described by two hopping parameters t and t' in different spatial directions and is relevant for layered organic charge-transfer salts. By using a variational approach that includes spiral magnetic order, we provide solid evidence that a spin-liquid phase is stabilized in the strongly-correlated regime and close to the isotropic limit t'/t=1. Otherwise, a magnetically ordered spiral state is found, connecting the (collinear) Néel and the (coplanar) 120° phases. The pitch vector of the spiral phase obtained from the unrestricted Hartree-Fock approximation is substantially renormalized in presence of electronic correlations, and the Néel phase is stabilized in a wide regime of the phase diagram, i.e., for t'/t < 0.75. We discuss these results in the context of organic charge-transfer salts.

cond-mat.str-el↗

Mott correlated states in the underdoped two-dimensional Hubbard model: variational Monte Carlo versus a dynamical cluster approximation

We investigate the properties of the frustrated underdoped Hubbard model on the square lattice using two complementary approaches, the dynamical cluster extension of dynamical mean field theory, and variational Monte Carlo simulations of Gutzwiller-Jastrow wavefunctions with backflow corrections. We compare and discuss data for the energy and the double occupancies, as obtained from both approaches. At small dopings, we observe a rapid crossover from a weakly correlated metal at low interaction strength U to a non-Fermi liquid correlated state with strong local spin correlations. Furthermore, we investigate the stability of the correlated state against phase separation. We observe phase separation only for large values of U or very large frustration. No phase separation is present for the parameter range relevant for the cuprates.

cond-mat.str-el↗

Pattern formation in the dipolar Ising model on a two-dimensional honeycomb lattice

We present Monte Carlo simulation results for a two-dimensional Ising model with ferromagnetic nearest-neighbor couplings and a competing long-range dipolar interaction on a honeycomb lattice. Both structural and thermodynamic properties are very similar to the case of a square lattice, with the exception that structures reflect the sixfold rotational symmetry of the underlying honeycomb lattice. To deal with the long-range nature of the dipolar interaction we also present a simple method of evaluating effective interaction coefficients, which can be regarded as a more straightforward alternative to the prevalent Ewald summation techniques.

cond-mat.stat-mech↗

Spontaneous Dissociation of Co2(CO)8 and Autocatalytic growth of Co on SiO2 : A Combined Experimental and Theoretical Investigation

We present experimental results and theoretical simulations of the adsorption behavior of the metal-organic precursor Co2(CO)8 on SiO2 surfaces after application of two different pre-treatment steps, namely by air plasma cleaning or a focused electron beam pre-irradiation. We observe a spontaneous dissociation of the precursor molecules as well as auto-deposition of cobalt on the pre-treated SiO2 surfaces. We also find that the differences in metal content and relative stability of these deposits depend on the pre-treatment conditions of the substrate. Transport measurements of these deposits are also presented. We are led to assume that the degree of passivation of the SiO2 surface by hydroxyl groups is an important controlling factor in the dissociation process. Our calculations of various slab settings using dispersion corrected density functional theory support this assumption. We observe physisorption of the precursor molecule on a fully hydroxylated SiO2 surface (untreated surface) and chemisorption on a partially hydroxylated SiO2 surface (pre-treated surface) with a spontaneous dissociation of the precursor molecule. In view of these calculations, we discuss the origin of this dissociation and the subsequent autocatalysis.

cond-mat.mtrl-sci↗

Interaction of W(CO)$_6$ with SiO$_2$ Surfaces -- A Density Functional Study

The interaction of tungsten hexacarbonyl W(CO)$_6$ precursor molecules with SiO$_2$ substrates is investigated by means of density functional theory calculations with and without inclusion of long range van der Waals interactions. We consider two different surface models, a fully hydroxylated and a partially hydroxylated SiO$_2$ surface, corresponding to substrates under different experimental conditions. For the fully hydroxylated surface we observe only a weak interaction between the precursor molecule and the substrate with physisorption of W(CO)$_6$. Inclusion of van der Waals corrections results in a stabilization of the molecules on this surface, but does not lead to significant changes in the chemical bonding. In contrast, we find a spontaneous dissociation of the precursor molecule on the partially hydroxylated SiO$_2$ surface where chemisorption of a W(CO)$_5$ fragment is observed upon removal of one of the CO ligands from the precursor molecule. Irrespective of the hydroxylation, the precursor molecule prefers binding of more than one of its CO ligands. In the light of these results, implications for the initial growth stage of tungsten nano-deposits on SiO$_2$ in an electron beam induced deposition process are discussed.

cond-mat.mtrl-sci↗

Multi-step approach to microscopic models for frustrated quantum magnets - the case of the natural mineral azurite

The natural mineral azurite Cu$_3$(CO$_3$)$_2$(OH)$_2$ is a frustrated magnet displaying unusual and controversially discussed magnetic behavior. Motivated by the lack of a unified description for this system, we perform a theoretical study based on density functional theory as well as state-of-the-art numerical many-body calculations. We propose an effective generalized spin-1/2 diamond chain model which provides a consistent description of experiments: low-temperature magnetization, inelastic neutron scattering, nuclear magnetic resonance measurements, magnetic susceptibility as well as new specific heat measurements. With this study we demonstrate that the balanced combination of first principles with powerful many-body methods successfully describes the behavior of this frustrated material.

cond-mat.str-el↗

Determination of effective microscopic models for the frustrated antiferromagnets Cs$_2$CuCl$_4$ and Cs$_2$CuBr$_4$ by density functional methods

We investigate the electronic and magnetic properties of the frustrated triangular-lattice antiferromagnets Cs$_2$CuCl$_4$ and Cs$_2$CuBr$_4$ in the framework of density functional theory. Analysis of the exchange couplings J and J' using the available X-ray structural data corroborates the values obtained from experimental results for Cs$_2$CuBr$_4$ but not for Cs$_2$CuCl$_4$. In order to understand this discrepancy, we perform a detailed study of the effect of structural optimization on the exchange couplings of Cs$_2$CuCl$_4$ employing different exchange-correlation functionals. We find that the exchange couplings depend on rather subtle details of the structural optimization and that only when the insulating state (mediated through spin polarization) is present in the structural optimization, we do have good agreement between the calculated and the experimentally determined exchange couplings. Finally, we discuss the effect of interlayer couplings as well as longer-ranged couplings in both systems.

cond-mat.str-el↗

Modulation of pairing interaction in Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ by an O dopant: a density functional theory study

Scanning tunneling spectroscopy measurements on the high temperature superconductor Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ have reported an enhanced spectral gap in the neighborhood of O dopant atoms. We calculate, within density functional theory (DFT), the change in electronic structure due to such a dopant. We then construct and discuss the validity of several tight binding (TB) fits to the DFT bands with and without an O dopant. With the doping-modulated TB parameters, we finally evaluate the spin susceptibility and pairing interaction within spin fluctuation theory. The d-wave pairing eigenvalues are enhanced above the pure system without O dopant, supporting the picture of enhanced local pairing around such a defect.

cond-mat.supr-con↗

Comparative study of FeCr2S4 and FeSc2S4: Spinels with orbitally active A site

Using first-principles density functional calculations, we perform a comparative study of two Fe based spinel compounds, FeCr2S4 and FeSc2S4. Though both systems contain an orbitally active A site with an Fe2+ ion, their properties are rather dissimilar. Our study unravels the microscopic origin of their behavior driven by the differences in hybridization of Fe d states with Cr/Sc d states and S p states in the two cases. This leads to important differences in the nature of the magnetic exchanges as well as the nearest versus next nearest neighbor exchange parameter ratios, resulting into significant frustration effects in FeSc2S4 which are absent in FeCr2S4.

cond-mat.str-el↗

Local moments and symmetry breaking in metallic PrMnSbO

We report a combined experimental and theoretical investigation of the layered antimonide PrMnSbO which is isostructural to the parent phase of the iron pnictide superconductors. We find linear resistivity near room temperature and Fermi liquid-like T^{2} behaviour below 150 K. Neutron powder diffraction shows that unfrustrated C-type Mn magnetic order develops below \sim 230 K, followed by a spin-flop coupled to induced Pr order. At T \sim 35 K, we find a tetragonal to orthorhombic (T-O) transition. First principles calculations show that the large magnetic moments observed in this metallic compound are of local origin. Our results are thus inconsistent with either the itinerant or frustrated models proposed for symmetry breaking in the iron pnictides. We show that PrMnSbO is instead a rare example of a metal where structural distortions are driven by f-electron degrees of freedom.

cond-mat.str-el↗

Ferromagnetism in Fe-substituted spinel semiconductor ZnGa$_2$O$_4$

Motivated by the recent experimental observation of long range ferromagnetic order at a relatively high temperature of 200K in the Fe-doped ZnGa$_2$O$_4$ semiconducting spinel, we propose a possible mechanism for the observed ferromagnetism in this system. We show, supported by band structure calculations, how a model similar to the double exchange model can be written down for this system and calculate the ground state phase diagram for the two cases where Fe is doped either at the tetrahedral position or at the octahedral position. We find that in both cases such a model can account for a stable ferromagnetic phase in a wide range of parameter space. We also argue that in the limit of high Fe$^{2+}$ concentration at the tetrahedral positions a description in terms of a two band model is essential. The two $e_g$ orbitals and the hopping between them play a crucial role in stabilizing the ferromagnetic phase in this limit. The case when Fe is doped simultaneously at both the tetrahedral and the octahedral position is also discussed.

cond-mat.str-el↗