Role of nematicity in controlling spin fluctuations and superconducting Tc in bulk FeSe

Bulk FeSe superconducts inside a nematic phase, that sets in through an orthorhombic distortion of the high temperature tetragonal phase. Bulk non-alloy tetragonal superconducting FeSe does not exist as yet. This raises the question whether nematicity is fundamental to superconductivity. We employ an advanced ab-initio ability and show that bulk tetragonal FeSe can, in principle, superconduct at almost the same Tc as the orthorhombic phase had that been the ground state. Further, we perform rigorous benchmarking of our theoretical spin susceptibilities against experimentally observed data over all energies and relevant momentum direction. We show that susceptibilities computed in both the tetragonal and orthorhombic phases already have the correct momentum structure at all energies, but not the desired intensity. The enhanced nematicity that simulates the correct spin fluctuation intensity can only lead to a maximum 10-15% increment in the superconducting Tc . Our results suggest while nematicity may be intrinsic property of the bulk FeSe, is not the primary force driving the superconducting pairing.Comment: 5 page, 4 figure

First-Principles Correlated Approach to the Normal State of Strontium Ruthenate

The interplay between multiple bands, sizable multi-band electronic correlations and strong spin-orbit coupling may conspire in selecting a rather unusual unconventional pairing symmetry in layered Sr$_{2}$RuO$_{4}$. This mandates a detailed revisit of the normal state and, in particular, the $T$-dependent incoherence-coherence crossover. Using a modern first-principles correlated view, we study this issue in the actual structure of Sr$_{2}$RuO$_{4}$ and present a unified and quantitative description of a range of unusual physical responses in the normal state. Armed with these, we propose that a new and important element, that of dominant multi-orbital charge fluctuations in a Hund's metal, may be a primary pair glue for unconventional superconductivity. Thereby we establish a connection between the normal state responses and superconductivity in this system.Comment: 8 pages, 4 figure

Evening out the spin and charge parity to increase Tc_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.Comment: 30 pages, 9 figure, 2 table

Metal-insulator transition in copper oxides induced by apex displacements

High temperature superconductivity has been found in many kinds of compounds built from planes of Cu and O, separated by spacer layers. Understanding why critical temperatures are so high has been the subject of numerous investigations and extensive controversy. To realize high temperature superconductivity, parent compounds are either hole-doped, such as {La$_{2}$CuO$_4$} (LCO) with Sr (LSCO), or electron doped, such as {Nd$_{2}$CuO$_4$} (NCO) with Ce (NCCO). In the electron doped cuprates, the antiferromagnetic phase is much more robust than the superconducting phase. However, it was recently found that the reduction of residual out-of-plane apical oxygens dramatically affects the phase diagram, driving those compounds to a superconducting phase. Here we use a recently developed first principles method to explore how displacement of the apical oxygen (A-O) in LCO affects the optical gap, spin and charge susceptibilities, and superconducting order parameter. By combining quasiparticle self-consistent GW (QS\emph{GW}) and dynamical mean field theory (DMFT), that LCO is a Mott insulator; but small displacements of the apical oxygens drive the compound to a metallic state through a localization/delocalization transition, with a concomitant maximum $d$-wave order parameter at the transition. We address the question whether NCO can be seen as the limit of LCO with large apical displacements, and elucidate the deep physical reasons why the behaviour of NCO is so different than the hole doped materials. We shed new light on the recent correlation observed between T$_c$ and the charge transfer gap, while also providing a guide towards the design of optimized high-Tc superconductors. Further our results suggest that strong correlation, enough to induce Mott gap, may not be a prerequisite for high-Tc superconductivity

Controlling Tc_c through band structure and correlation engineering in collapsed and uncollapsed phases of iron arsenides

Recent observations of selective emergence (suppression) of superconductivity in the uncollapsed (collapsed) tetragonal phase of LaFe$_2$As$_2$ has rekindled interest in understanding what features of the band structure control the superconducting T$_c$. We show that the proximity of the narrow Fe-d$_{xy}$ state to the Fermi energy emerges as the primary factor. In the uncollapsed phase this state is at the Fermi energy, and is most strongly correlated and source of enhanced scattering in both single and two particle channels. The resulting intense and broad low energy spin fluctuations suppress magnetic ordering and simultaneously provide glue for Cooper pair formation. In the collapsed tetragonal phase, the d$_{xy}$ state is driven far below the Fermi energy, which suppresses the low-energy scattering and blocks superconductivity. A similar source of broad spin excitation appears in uncollapsed and collapsed phases of CaFe$_{2}$As$_{2}$. This suggests controlling coherence provides a way to engineer T$_c$ in unconventional superconductors primarily mediated through spin fluctuations

Interplay between band structure and Hund's correlation to increase Tc_{c} in FeSe

FeSe is classed as a Hund's metal, with a multiplicity of $d$ bands near the Fermi level. Correlations in Hund's metals mostly originate from the exchange parameter \emph{J}, which can drive a strong orbital selectivity in the correlations. The Fe-chalcogens are the most strongly correlated of the Fe-based superconductors, with $d_{xy}$ the most correlated orbital. Yet little is understood whether and how such correlations directly affect the superconducting instability in Hund's systems. By applying a recently developed high-fidelity \emph{ab initio} theory, we show explicitly the connections between correlations in $d_{xy}$ and the superconducting critical temperature $T_{c}$. Starting from the \emph{ab initio} results as a reference, we consider various kinds of excursions in parameter space around the reference to determine what controls $T_{c}$. We show small excursions in $J$ can cause colossal changes in $T_{c}$. Additionally we consider changes in hopping by varying the Fe-Se bond length in bulk, in the free standing monolayer M-FeSe, and M-FeSe on a SrTiO$_{3}$ substrate (M-FeSe/STO). The twin conditions of proximity of the $d_{xy}$ state to the Fermi energy, and the strength of $J$ emerge as the primary criteria for incoherent spectral response and enhanced single- and two-particle scattering that in turn controls $T_{c}$. Using constrained RPA, we show further that FeSe in monolayer form (M-FeSe) provides a natural mechanism to enhance $J$. We explain why M-FeSe/STO has a high $T_{c}$, whereas M-FeSe in isolation should not. Our study opens a paradigm for a unified understanding what controls $T_{c}$ in bulk, layers, and interfaces of Hund's metals by hole pocket and electron screening cloud engineering