Unraveling the magnetic ground-state in alkali-metal lanthanide oxide Na$_2$PrO$_3$

TL;DR

This study combines muon spin spectroscopy, neutron scattering, and theoretical modeling to elucidate the magnetic ground state of Na$_2$PrO$_3$, revealing antiferromagnetic order with a small static moment and complex excitation spectra.

Contribution

It provides a detailed experimental and theoretical analysis of Na$_2$PrO$_3$, showing the deviation of the Pr$^{4+}$ ground state from the Kitaev model and characterizing its magnetic interactions.

Findings

Na$_2$PrO$_3$ exhibits Néel antiferromagnetic order below 4.9 K.

The static magnetic moment is small, ≤ 0.22 μ_B per Pr.

Magnetic excitations are well described by an XY model with Heisenberg and anisotropic exchanges.

Abstract

A comprehensive set of muon spin spectroscopy and neutron scattering measurements supported by ab-initio and model Hamiltonian simulations have been used to investigate the magnetic ground state of Na$_2$PrO$_3$. $\mu$SR reveals N\'eel antiferromagnetic order below $T_{\rm N}\! \sim\! 4.9$ K, with a small static magnetic moment $m_{\rm static}\!\leq \! 0.22$~$\mu_{\rm B}/{\rm Pr}$ collinearly aligned along the $c-$axis. Inelastic neutron measurements reveal the full spectrum of crystal field excitations and confirm that the Pr$^{4+}$ ground state wave function deviates significantly from the $\Gamma_7$ limit relevant to the Kitaev model. Single and two magnon excitations are observed in the ordered state below $T_N=4.6$ K and are well described by non-linear spin wave theory from the N\'eel state using a magnetic Hamiltonian with Heisenberg exchange $J=1$ meV and symmetric anisotropic exchange $\Gamma/J=0.1$, corresponding to an XY model. Intense two magnon excitations are accounted for by $g$-factor anisotropy $g_\mathrm{z}/g_\pm = 1.29$. A fluctuating moment $\delta m^2 = 0.57(22)$ $\mu_{\rm B}^2/{\rm Pr}$ extracted from the energy and momentum integrated inelastic neutron signal is reduced from expectations for a local $J=1/2$ moment with average $g$-factor $g_{\rm avg}\approx 1.1$. Together, the results demonstrate that the small moment in Na$_2$PrO$_3$ arises from crystal field and covalency effects and that the material does not exhibit significant quantum fluctuations..