Highly Tunable Magnetic Phases in Transition-Metal Dichalcogenide Fe 1 / 3 + δ NbS 2

Wu, Shan; Xu, Zhijun; Haley, Shannon C.; Weber, Sophie F.; Acharya, Arani; Maniv, Eran; Qiu, Yiming; Aczel, A. A.; Settineri, Nicholas S.; Neaton, Jeffrey B.; Analytis, James G.; Birgeneau, Robert J.

doi:10.1103/PhysRevX.12.021003

Title: Highly Tunable Magnetic Phases in Transition-Metal Dichalcogenide ${Fe}_{1 / 3 + δ} {NbS}_{2}$

Journal Article · Tue Apr 05 00:00:00 EDT 2022 · Physical Review. X

DOI:https://doi.org/10.1103/PhysRevX.12.021003· OSTI ID:1861133

; Xu, Zhijun;

; Weber, Sophie F.;

; Maniv, Eran; Qiu, Yiming;

; Settineri, Nicholas S.; Neaton, Jeffrey B.; Analytis, James G.;

Layered transition-metal dichalcogenides (TMDCs) host a plethora of interesting physical phenomena ranging from charge order to superconductivity. By introducing magnetic ions into 2H-TA₂ (T=Nb, Ta; A=S, Se), the material forms a family of magnetic intercalated TMDCs M_xTA₂ (M=3d transition metal). Recently, Fe_1/3+δNbS₂ has been found to possess intriguing resistance switching and magnetic memory effects coupled to the Néel temperature of TN~45 K [Maniv et al., Nat. Phys. 17, 525 (2021); Sci. Adv. 7, eabd8452 (2021)]. We present comprehensive single crystal neutron diffraction measurements on underintercalated (δ~-0.01), stoichiometric, and overintercalated (δ~0.01) samples. Magnetic defects are usually considered to suppress magnetic correlations and, concomitantly, transition temperatures. Instead, we observe highly tunable magnetic long-ranged states as the Fe concentration is varied from underintercalated to overintercalated, that is, from Fe vacancies to Fe interstitials. The under- and overintercalated samples reveal distinct antiferromagnetic stripe and zigzag orders, associated with wave vectors k₁=(0.5,0,0) and k₂=(0.25,0.5,0), respectively. The stoichiometric sample shows two successive magnetic phase transitions for these two wave vectors with an unusual rise-and-fall feature in the intensities connected to k1. We ascribe this sensitive tunability to the competing next-nearest neighbor exchange interactions and the oscillatory nature of the Ruderman-Kittel-Kasuya-Yosida mechanism. We discuss experimental observations that relate to the observed intriguing switching resistance behaviors. Our discovery of a magnetic defect tuning of the magnetic structure in bulk crystals Fe_1/3+δNbS₂ provides a possible new avenue to implement controllable antiferromagnetic spintronic devices.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Novel Pathways to Quantum Coherence in Materials (NPQC); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). High Flux Isotope Reactor (HFIR)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Institute of Standards and Technology (NIST); National Science Foundation (NSF)

Grant/Contract Number:: AC02-05-CH11231; AC02-05CH11231; AC05-00OR22725

OSTI ID:: 1861133

Alternate ID(s):: OSTI ID: 1877044; OSTI ID: 1892423

Journal Information:: Physical Review. X, Journal Name: Physical Review. X Vol. 12 Journal Issue: 2; ISSN 2160-3308

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Highly Tunable Magnetic Phases in Transition-Metal Dichalcogenide Fe 1 / 3 + δ NbS 2

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Title: Highly Tunable Magnetic Phases in Transition-Metal Dichalcogenide ${Fe}_{1 / 3 + δ} {NbS}_{2}$