arXiv subjects

Cédric Weber

Publications and source records attributed to Cédric Weber.

11 recordsLinked to original sources

arXiv2020

Electronic structure correspondence of singlet-triplet scale separation in strained Sr2RuO4

At a temperature of roughly 1\,K, \ce{Sr2RuO4} undergoes a transition from a normal Fermi liquid to a superconducting phase. Even while the former is relatively simple and well understood, the superconducting state is not even after 25 years of study. More recently it has been found that critical temperatures can be enhanced by application of uniaxial strain, up to a critical strain, after which it falls off. In this work, we take an `instability' approach and seek for divergences in susceptibilities. This provides an unbiased way to distinguish tendencies to competing ground states. We show that in the unstrained compound the singlet and triplet instabilities of the normal Fermi liquid phase are closely spaced. Under uniaxial strain electrons residing on all orbitals contributing to the Fermiology become more coherent while the electrons of Ru-$d_{xy}$ character become heavier and electrons of Ru-$d_{xz,yz}$ characters become lighter. In the process, Im\,$χ(\mathbf{q},ω)$ increases rapidly around the incommensurate vector $\mathbf{q}{=}(0.3,0.3,0)2π/a$ while it gets suppressed at all other commensurate vectors, in particular at $q{=}0$, which is essential for spin-triplet superconductivity. Thus the triplet superconducting instability remains the lagging instability of the system and the singlet instability enhances under strain, leading to a large energy-scale separation between these competing instabilities. At large strain an instability to a spin density wave overtakes the superconducting one. The analysis relies on a high-fidelity, \emph{ab initio} description of the one-particle properties and two-particle susceptibilities, based on the Quasiparticle Self-Consistent \emph{GW} approximation augmented by Dynamical Mean Field theory. This approach is described and its high fidelity confirmed by comparing to observed one- and two-particle properties.

cond-mat.str-el↗

arXiv2020

ONETEP + TOSCAM: uniting dynamical mean field theory and linear-scaling density functional theory

We introduce the unification of dynamical mean field theory (DMFT) and linear-scaling density functional theory (DFT), as recently implemented in ONETEP, a linear-scaling DFT package, and TOSCAM, a DMFT toolbox. This code can account for strongly correlated electronic behavior while simultaneously including the effects of the environment, making it ideally suited for studying complex and heterogeneous systems containing transition metals and lanthanides, such as metalloproteins. We systematically introduce the necessary formalism, which must account for the non-orthogonal basis set used by ONETEP. In order to demonstrate the capabilities of this code, we apply it to carbon monoxide-ligated iron porphyrin and explore the distinctly quantum-mechanical character of the iron $3d$ electrons during the process of photodissociation.

cond-mat.str-el↗

arXiv2019

Super-exchange mechanism and quantum many body excitations in the archetypal hemocyanin/tyrosinase di-Cu oxo-bridge

We perform first-principles quantum mechanical studies of dioxygen ligand binding to the hemocyanin protein. Electronic correlation effects in the functional site of hemocyanin are investigated using a state-of-the-art approach, treating the localised copper 3\emph{d} electrons with cluster dynamical mean field theory (DMFT) for the first time. This approach has enabled us to account for dynamical and multi-reference quantum mechanics, capturing valence and spin fluctuations of the 3\emph{d} electrons. Our approach explains the stabilisation of the experimentally observed di-Cu singlet for the butterflied Cu$_2$O$_2$ core, with localised charge and incoherent scattering processes across the oxo-bridge that prevent long-lived charge excitations, suggesting that the magnetic structure of hemocyanin is largely influenced by the many-body corrections. Our computational model is supported by agreement with experimental optical absorption data, and provides a revised understanding of the bonding of the peroxide to the di-Cu system \emph{in vivo}.

cond-mat.str-el↗

arXiv2019

Evening out the spin and charge parity to increase T$_c$ in unconventional superconductor Sr_{2}RuO_{4}

Unconventional superconductivity in Sr$_{2}$RuO$_{4}$ has been intensively studied for decades. The origin and nature of the pairing continues to be widely debated, in particular, the possibility of a triplet origin of Cooper pairs. However, complexity of Sr$_{2}$RuO$_{4}$ with multiple low-energy scales, involving subtle interplay among spin, charge and orbital degrees of freedom, calls for advanced theoretical approaches which treat on equal footing all electronic effects. Here we develop a novel approach, a detailed \emph{ab initio} theory, coupling quasiparticle self-consistent \emph{GW} approximation with dynamical mean field theory (DMFT), including both local and non-local correlations. We report that the superconducting instability has multiple triplet and singlet components. In the unstrained case the triplet eigenvalues are larger than the singlets. Under uniaxial strain, the triplet eigenvalues drop rapidly and the singlet components increase. This is concomitant with our observation of spin and charge fluctuations shifting closer to wave-vectors favoring singlet pairing in the Brillouin zone. We identify a complex mechanism where charge fluctuations and spin fluctuations co-operate in the even-parity channel under strain leading to increment in $T_c$, thus proposing a novel mechanism for pushing the frontier of $T_c$ in unconventional `triplet' superconductors.

cond-mat.str-el↗

arXiv2019

Possible phonon-induced electronic bi-stability in VO$_2$ for ultrafast memory at room temperature

VO$_{2}$ is a model material system which exhibits a metal to insulator transition at 67$^\circ$C. This holds potential for future ultrafast switching in memory devices, but typically requires a purely electronic process to avoid the slow lattice response. The role of lattice vibrations is thus important, but it is not well understood and it has been a long-standing source of controversy. We use a combination of ultrafast spectroscopy and ab initio quantum calculations to unveil the mechanism responsible for the transition. We identify an atypical Peierls vibrational mode which acts as a trigger for the transition. This rules out the long standing paradigm of a purely electronic Mott transition in VO$_{2}$; however, we found a new electron-phonon pathway for a purely reversible electronic transition in a true bi-stable fashion under specific conditions. This transition is very atypical, as it involves purely charge-like excitations and requires only small nuclear displacement. Our findings will prompt the design of future ultrafast electro-resistive non-volatile memory devices.

cond-mat.str-el↗

arXiv2012

Scaling of the transition temperature of hole-doped cuprate superconductors with the charge-transfer energy

We use first-principles calculations to extract two essential microscopic parameters, the charge-transfer energy and the inter-cell oxygen-oxygen hopping, which correlate with the maximum superconducting transition temperature $\Tcmax$ across the cuprates. We explore the superconducting state in the three-band model of the copper-oxygen planes using cluster Dynamical Mean-Field Theory. We find that the variation in the charge-transfer energy largely accounts for the empirical trend in $\Tcmax$, resolving a long-standing contradiction with theoretical calculations.

cond-mat.str-el↗

arXiv2012

Anticollinear magnetic order induced by impurities in the frustrated Heisenberg model of pnictides

We present Monte Carlo simulations for a classical antiferromagnetic Heisenberg model with both nearest ($J_1$) and next-nearest ($J_2$) exchange couplings on the square lattice in the presence of non-magnetic impurities. We show that the order-by-disorder entropy selection, associated with the Ising-like phase transition that appears for $J_2/J_1>1/2$ in the pure spin model, is quenched at low temperature due to the presence of non-magnetic impurities. Evidences that a new competing order is stabilized around the impurities, and in turn induces a re-entrance phase transition are reported. Implications for local magnetic measurement of the parent compound of iron pnictides are briefly discussed.

cond-mat.str-el↗

arXiv2011

High frequency thermoelectric response in correlated electronic systems

We derive a general formalism for evaluating the high-frequency limit of the thermoelectric power of strongly correlated materials, which can be straightforwardly implemented in available first principles LDA+DMFT programs. We explore this formalism using model Hamiltonians and we investigate the validity of approximating the static thermoelectric power $S_0$, by its high-temperature limit, $S^*$. We point out that the behaviors of $S^*$ and $S_0$ are qualitatively different for a correlated Fermi liquid near the Mott transition, when the temperature is in the coherent regime. When the temperature is well above the coherent regime, e.g., when the transport is dominated by incoherent excitations, $S^*$ provides a good estimation of $S_0$.

cond-mat.str-el↗

arXiv2008

Optical Weights and Waterfalls in Doped Charge Transfer Insulators: an LDA+DMFTStudy of LSCO

We use the Local Density Approximation in combination with the Dynamical Mean Field Theory to investigate intermediate energy properties of the copper oxides. We identify coherent and incoherent spectral features that results from doping a charge transfer insulator, namely quasiparticles, Zhang-Rice singlet band, and the upper and lower Hubbard bands. Angle resolving these features, we identify a \emphasize{waterfall} like feature, between the quasiparticle part and the incoherent part of the Zhang-Rice band. We investigate the assymetry between particle and hole doping. On the hole doped side, there is a very rapid transfer of spectral weight upon doping in the one particle spectra. The optical spectral weight increases superlinearly on the hole doped side in agreement with experiments.

cond-mat.str-el↗

arXiv2008

Orbital currents in extended Hubbard models of high-T$_c$ cuprates

Motivated by the recent report of broken time-reversal symmetry and zero momentum magnetic scattering in underdoped cuprates, we investigate under which circumstances orbital currents circulating inside a unit cell might be stabilized in extended Hubbard models that explicitly include oxygen orbitals. Using Gutzwiller projected variational wave functions that treat on an equal footing all instabilities, we show that orbital currents indeed develop on finite clusters, and that they are stabilized in the thermodynamic limit if additional interactions, e.g. strong hybridization with apical oxygens, are included in the model.

cond-mat.str-el↗

arXiv2005

Magnetism and superconductivity of strongly correlated electrons on the triangular lattice

We investigate the phase diagram of the \tj Model on a triangular lattice using a Variational Monte-Carlo approach. We use an extended set of Gutzwiller projected fermionic trial wave-functions allowing for simultaneous magnetic and superconducting order parameters. We obtain energies at zero doping for the spin-1/2 Heisenberg model in very good agreement with the best estimates. Upon electron doping (with a hopping integral $t<0$) this phase is surprisingly stable variationally up to $n\approx 1.4$, while the $d_{x^{2}-y^{2}}+i d_{xy}$ order parameter is rather weak and disappears at $n\approx 1.1$. For hole doping however the coplanar magnetic state is almost immediately destroyed and $d_{x^{2}-y^{2}}+i d_{xy}$ superconductivity survives down to $n\approx 0.8$. For lower $n$, between 0.2 and 0.8, we find saturated ferromagnetism. Moreover, there is evidence for a narrow spin density wave phase around $n\approx 0.8$. Commensurate flux phases were also considered, but these turned out {\em not} to be competitive at finite doping.

cond-mat.supr-con↗