Isoelectronic perturbations to $f$-$d$-electron hybridization and the enhancement of hidden order in URu$_2$Si$_2$

TL;DR

This study investigates how isoelectronic substitution of Os in URu2Si2 enhances hidden order and induces phase transitions, linking increased hybridization of U-5f and transition metal d-electrons to electronic instability and phase stability.

Contribution

It demonstrates that Os substitution enhances hidden order in URu2Si2 by increasing hybridization, providing new insights into the electronic mechanisms behind phase transitions in this material.

Findings

Os substitution expands the lattice and enhances hidden order.

Less external pressure is needed to induce phase transition with Os.

Hybridization between U-5f and transition metal d-electrons increases with Os substitution.

Abstract

Electrical resistivity measurements were performed on single crystals of URu$_2-x$Os$_x$Si$_2$ up to $x$ = 0.28 under hydrostatic pressure up to $P$ = 2 GPa. As the Os concentration, $x$ , is increased, (1) the lattice expands, creating an effective negative chemical pressure $P_{ch}$($x$), (2) the hidden order (HO) phase is enhanced and the system is driven toward a large-moment antiferromagnetic (LMAFM) phase, and (3) less external pressure $P_{c}$ is required to induce the HO to LMAFM phase transition. We compare the $T(x)$, $T(P)$ phase behavior reported here for the URu$_2-x$Os$_x$Si$_2$ system with previous reports of enhanced HO in URu$_2$Si$_2$ upon tuning with $P$, or similarly in URu$_2-x$Fe$_x$Si$_2$ upon tuning with positive $P_{ch}$($x$). It is noted that pressure, Fe substitution, and Os substitution are the only known perturbations that enhance the HO phase and induce the first order transition to the LMAFM phase in URu$_2$Si$_2$. We present a scenario in which the application of pressure or the isoelectronic substitution of Fe and Os ions for Ru results in an increase in the hybridization of the U-5$f$- and transition metal $d$-electron states which leads to electronic instability in the paramagnetic phase and a concurrent stability of HO (and LMAFM) in URu$_2$Si$_2$. Calculations in the tight binding approximation are included to determine the strength of hybridization between the U-5$f$ electrons and each of the isoelectronic transition metal $d$-electron states of Fe, Ru, and Os.