Interplay between band structure and Hund's correlation to increase T$_{c}$ in FeSe

TL;DR

This study uses advanced ab initio methods to explore how Hund's coupling and band structure modifications influence the superconducting transition temperature in FeSe, revealing key factors that can enhance $T_c$ in different forms.

Contribution

It demonstrates the direct impact of Hund's exchange parameter J and band structure tuning on $T_c$ in FeSe, providing a unified framework for understanding superconductivity in Hund's metals.

Findings

Small changes in J cause large variations in $T_c$.

Proximity of $d_{xy}$ to the Fermi level is crucial for high $T_c$.

Monolayer FeSe on SrTiO$_{3}$ exhibits enhanced $J$ and high $T_c$.

Abstract

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.