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Spin-charge interplay in the diluted magnetic semiconductor Na(Zn,Mn)Sb studied by multiprobe measurements and simulations

Guoqiang Zhao1,2,3,*,†, Xiang Li1,*, Shuang Yu2, Hui Chen2, Yong Hu2,4, Yipeng Cai3,5, Shengli Guo6,7, Bo Gu1,8,‡, Fanlong Ning3,6,7 et al.

Kenji M. Kojima5, Zheng Deng2,8, Yuqing Xing2, Hong-Jun Gao2,8, Xingjiang Zhou2, Gang Su1,9, S. Maekawa1,10,11, Changqing Jin2,8, and Yasutomo J. Uemura3,§

  • *These authors contributed equally to this work.
  • †Contact author: g.q.zhao@iphy.ac.cn
  • ‡Contact author: gubo@ucas.ac.cn
  • §Contact author: yu2@columbia.edu

Phys. Rev. B 112, 075104 – Published 4 August, 2025

DOI: https://doi.org/10.1103/myxg-tt85

Abstract

Diluted magnetic semiconductor (DMS) systems have been extensively studied in recent decades. DMSs provides a platform where charge transport and magnetic ordering phenomena exhibit unique interplays, together with possible applications to spin-dependent electronics (spintronics) devices. Initial development of ferromagnetic (FM) DMS systems centered around III-V semiconductors doped with dilute transition metals, such as (Ga,Mn)As, obtained by co-doping of spin and charge. More recently, independent spin and charge doping was first achieved in Li(Zn,Mn)As, a DMS system based on I-II-V semiconductor, with charge doping via variable Li concentrations and spin doping via iso-valent (Zn,Mn) substitutions. Although more than 30 new DMS systems with independent spin and charge doping have been synthesized since then, the main research emphasis has been put on development and characterization of systems with higher FM Curie temperature (TC) and different crystal structures suitable for possible formation of heterostructure devices. This article focuses on a new DMS material Na(Zn,Mn)Sb, which exhibits a spin glass (SG) ordering, together with metal-insulator transition (MIT) and colossal negative magnetoresistance (CMR) as a function of independent spin and charge doping and application of external magnetic fields. MIT and CMR phenomena are elucidated by magneto transport, magnetization, angle resolved photoemission spectroscopy (ARPES), and scanning tunneling microscopy (STM) measurements, and by band calculations which demonstrate development and disappearance of energy gap. Magnetic order and dynamic spin fluctuations are probed with muon spin relaxation (µSR) and magnetization, and the results for Na(Zn,Mn)Sb are compared to those from FM DMS systems Li(Zn,Mn)As, Li(Zn,Mn)P, and Li(Zn,Mn,Cu)As. First-principles calculations are performed for Na(Zn,Mn)Sb, (Ga,Mn)As and Li(Zn,Mn)P to highlight the roles of charge and spin doping on exchange interactions mediated by nearest neighbor super-exchange coupling and oscillatory Ruderman-Kittel-Kasuya-Yosida (RKKY) coupling via conduction electrons. These studies reveal (1) MIT and CMR of Na(Zn,Mn)Sb manifest as a response to spin configurations as spin-driven transport phenomena; (2) a dynamic critical behavior is observed in SG transition of Na(Zn,Mn)Sb, in contrast to more first-order-like magnetic evolutions in other FM DMS systems; (3) charge doping supports FM coupling additive to direct AFM exchange interaction between nearest-neighbor Mn pairs; and (4) a widely different coercive fields seen in different families of FM and SG DMS systems can be explained by geometrical frustration of AFM interaction in underlying lattice for Mn spin network.

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