Imaging emergent exotic quasiparticle state in a frustrated transition metal oxide

TL;DR

This study uncovers a novel quantum state in the frustrated spinel oxide superconductor LiTi2O4, characterized by Fermi surface flattening below 150 K without typical symmetry-breaking, revealing complex interplay between orbital frustration and emergent electronic properties.

Contribution

It provides the first evidence of exotic Fermiology and a new quantum state in a frustrated transition metal oxide superconductor using ARPES and thin film techniques.

Findings

Abrupt flattening of near Fermi energy dispersion below 150 K

Absence of energy gap opening or lattice distortion across T*

Emergent negative thermal expansion indicating a distinct phase

Abstract

The existence of rich Fermiology in anomalous metal phase in exotic superconductors has attracted considerable interests, as exemplified in copper, iron-based, and intermetallic frustrated kagome-based compounds. A common feature in these cases is pseudo-gap opening or long-range lattice/electronic ordering above superconducting critical temperature Tc. As yet developed area is the potential existence of exotic Fermiology in superconducting transition metal oxides on a geometrically frustrated lattice. Here, we focus on the spinel oxide superconductor LiTi2O4, which can be viewed as the hole-doped side of the orbital ordered 3d1 Mott system on the Ti-derived pyrochlore frustrated network. By the in-situ combination of angle-resolved photoemission spectroscopy (ARPES) and epitaxial thin film growth, we discovered the abrupt flattening of near Fermi energy dispersion below the characteristic temperature T* ~ 150 K. While the emergent negative thermal expansion below T* strongly supports a distinct phase at low-temperature, absence of energy gap opening, splitting/folding of bands, nor long-range lattice distortion are seen across T*. We propose that the competition between growing instability towards orbital ordering and its inherent geometric frustration in the Ti-pyrochlore network results in a new quantum state of matter with robust high entropic nature below T*. Our findings collectively point to a unique Fermiology in frustrated three-dimensional transition metal oxides, and its connection to superconductivity below Tc is open as an interesting future challenge. Also, a potential guideline is unexpectedly provided for designing zero thermal expansion metal to develop future solid-state devices.