Weak doping dependence of the antiferromagnetic coupling between nearest-neighbor Mn$^{2+}$ spins in (Ba$_{1-x}$K$_x$)(Zn$_{1-y}$Mn$_y$)$_2$As$_2$

TL;DR

This study investigates the magnetic interactions in a dilute magnetic semiconductor, revealing that hole doping minimally affects the antiferromagnetic coupling between nearest-neighbor Mn spins despite theoretical predictions of suppression.

Contribution

The paper provides experimental evidence showing weak doping dependence of Mn-Mn antiferromagnetic coupling, challenging previous first-principles predictions and highlighting the roles of superexchange and double-exchange interactions.

Findings

Localized magnetic excitation at ~13 meV observed

Hole doping broadens the excitation peak

Antiferromagnetic coupling remains nearly unchanged with doping

Abstract

Dilute magnetic semiconductors (DMS) are nonmagnetic semiconductors doped with magnetic transition metals. The recently discovered DMS material (Ba$_{1-x}$K$_{x}$)(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$ offers a unique and versatile control of the Curie temperature, $T_{\mathrm{C}}$, by decoupling the spin (Mn$^{2+}$, $S=5/2$) and charge (K$^{+}$) doping in different crystallographic layers. In an attempt to describe from first-principles calculations the role of hole doping in stabilizing ferromagnetic order, it was recently suggested that the antiferromagnetic exchange coupling $J$ between the nearest-neighbor Mn ions would experience a nearly twofold suppression upon doping 20\% of holes by potassium substitution. At the same time, further-neighbor interactions become increasingly ferromagnetic upon doping, leading to a rapid increase of $T_{\mathrm{C}}$. Using inelastic neutron scattering, we have observed a localized magnetic excitation at about 13 meV, associated with the destruction of the nearest-neighbor Mn-Mn singlet ground state. Hole doping results in a notable broadening of this peak, evidencing significant particle-hole damping, but with only a minor change in the peak position. We argue that this unexpected result can be explained by a combined effect of superexchange and double-exchange interactions.