Spin Susceptibility of Ga-Stabilized delta-Pu Probed by {69}^Ga NMR

TL;DR

This study uses {69}^Ga NMR to investigate the spin susceptibility and electronic behavior of delta-phase Pu-Ga alloy, revealing localized 5f electrons, electronic instability near the Fermi level, and no static magnetic order down to 5K.

Contribution

First NMR investigation of spin susceptibility in delta-Pu-Ga alloy, showing localized 5f electrons and electronic instability near the Fermi energy.

Findings

Nonmonotonic temperature dependence of NMR shift with a maximum around 150 K.

Evidence of electronic instability and pseudogap-like behavior below 150 K.

Absence of static magnetic order down to 5 K.

Abstract

Spin susceptibility of stabilized \delta phase in the Pu-Ga alloy is studied by measuring {69,71}^Ga NMR spectra and nuclear spin-lattice relaxation rate {69}T_{1}^{-1} in the temperature range 5 - 350 K. The shift ({69}^K) of the {69,71}^Ga NMR line and {69}^T_{1}^{-1} are controlled correspondingly by the static and the fluctuating in time parts of local magnetic field arisen at nonmagnetic gallium due to transferred hyperfine coupling with the nearest f electron environment of the more magnetic Pu. The nonmonotonic with a maximum around 150 K behavior of {69}^K(T) \chi_{s,5f}(T) is attributed to the peculiarities in temperature dependence of the f electron spin susceptibility \chi_{s,5f}(T) in \delta phase of plutonium. The temperature reversibility being observed in {69}^K(T) data provides strong evidence for an electronic instability developed with T in f electron bands near the Fermi energy and accompanied with a pseudogap-like decrease of \chi_{s,5f}(T) at T<150 K. The NMR data at high temperature are in favor of the mainly localized character of 5f electrons in \delta phase of the alloy with characteristic spin-fluctuation energy \Gamma(T) T^{0.35(5)}, which is close to $\Gamma(T) T^{0.5} predicted by Cox et al. [J. Appl. Phys. 57, 3166 (1985)] for 3D Kondo-system above T_Kondo}. The dynamic spin correlations of 5f electrons become essential to consider for {69}^T_{1}^{-1}(T) only at T<100 K. However, no NMR evidences favoring formation of the static magnetic order in \delta-Pu were revealed down to 5K .