Valence Transition Theory of the Pressure-Induced Dimensionality Crossover in Superconducting Sr$_{14-x}$Ca$_x$Cu$_{24}$O$_{41}$

TL;DR

This paper proposes a valence transition theory to explain the pressure-induced dimensionality crossover in superconducting Sr$_{14-x}$Ca$_x$Cu$_{24}$O$_{41}$, challenging ladder-based models and linking it to charge transfer and valence changes.

Contribution

It introduces a valence transition mechanism involving Cu-ion charge transfer to explain the dimensionality crossover in SCCO, providing a unified view of charge carrier increase in cuprates.

Findings

Dimensionality crossover driven by Cu valence change, not hole concentration increase.

Charge transfer leads to negative charge-transfer gap and increased carrier density.

Proposes a testable experimental prediction to validate the valence transition theory.

Abstract

More than three decades after the discovery of superconductivity (SC) in the cuprates, the nature of the "normal" state and the mechanism of SC remain mysterious. One popular theoretical approach has been to treat the CuO$_2$ layer as coupled two-leg one-band Hubbard ladders. In the undoped two-leg ladder spin-singlets occupy ladder rungs, and doped ladders are characterized by superconducting correlations with quasi-long range order (quasi-LRO). Pressure-induced SC in Sr$_{14-x}$Ca$_x$Cu$_{24}$O$_{41}$ (SCCO) has long been explained within one-band ladder theories. The dramatic pressure-driven crossover from quasi one-to-two dimensional (1D-to-2D) transport and the simultaneous vanishing of the spin gap due to ladder singlets in the metallic state preceding SC however lie outside the scope of ladder-based theories. Recent demonstration of rapid decay of superconducting correlations with distance within a realistic multiband model of the cuprate ladder gives additional credence to this viewpoint. Here we show that the assumption of pressure-driven increase in hole concentration in the ladders cannot explain the dimensionality crossover. The dimensionality crossover is due to discrete change in Cu-ion ionicity accompanied by transfer of holes from the Cu to O-ions, leading to "negative charge-transfer gap". Our theory of valence transition driven dimensionality crossover in SCCO provides a generic explanation of the very large increase in charge carrier density at critical doping concentrations in both hole and electron doped layered cuprates We propose a falsifiable experimental test of our theory.