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Title: Surface-Engineered MXenes: Electric Field Control of Magnetism and Enhanced Magnetic Anisotropy

Abstract

Controlling magnetism in two-dimensional (2D) materials via electric fields and doping enables robust long-range order by providing an external mechanism to modulate magnetic exchange interactions and anisotropy. Here in this report, we predict that transition metal carbide and nitride MXenes are promising candidates for controllable magnetic 2D materials. The surface terminations introduced during synthesis act as chemical dopants that influence the electronic structure, enabling controllable magnetic order. We show ground-state magnetic ordering in Janus M2XOxF2–x (M is an early transition metal, X is carbon or nitrogen, and x = 0.5, 1, or 1.5) with asymmetric surface functionalization, where local structural and chemical disorder induces magnetic ordering in some systems that are nonmagnetic or weakly magnetic in their pristine form. The resulting magnetic states of these noncentrosymmetric structures can be robustly switched and stabilized by tuning the interlayer exchange couplings with small applied electric fields. Furthermore, bond directionality is enhanced by Janus functionalization, resulting in improved magnetic anisotropy, which is essential to stable 2D magnetic ordering. The mixed termination-induced anisotropy leads to robust Ising ferromagnetism with an out-of-plane easy axis over the full range of relevant termination compositions for Janus Mn2N. Janus Cr2C, V2C, and Ti2C were found to be robustlymore » antiferromagnetic. Our results provide a strategy for exploiting asymmetric surface functionalization to achieve room-temperature nanoscale magnetism under ambient conditions in MXenes with currently available synthesis techniques.« less

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [2];  [2];  [1]
  1. Univ. of Pennsylvania, Philadelphia, PA (United States)
  2. Drexel Univ., Philadelphia, PA (United States). A. J. Drexel Nanotechnology Inst.
Publication Date:
Research Org.:
Drexel Univ., Philadelphia, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Army Research Office (ARO); National Science Foundation (NSF)
OSTI Identifier:
1774202
Grant/Contract Number:  
SC0018618; W911NF-16-1-0447; CMMI-1727717; EFMA-542879
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 13; Journal Issue: 3; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 2D materials; MXene; ferromagnetism; magnetic anisotropy; electrical control; Janus; DFT

Citation Formats

Frey, Nathan C., Bandyopadhyay, Arkamita, Kumar, Hemant, Anasori, Babak, Gogotsi, Yury, and Shenoy, Vivek B. Surface-Engineered MXenes: Electric Field Control of Magnetism and Enhanced Magnetic Anisotropy. United States: N. p., 2019. Web. doi:10.1021/acsnano.8b09201.
Frey, Nathan C., Bandyopadhyay, Arkamita, Kumar, Hemant, Anasori, Babak, Gogotsi, Yury, & Shenoy, Vivek B. Surface-Engineered MXenes: Electric Field Control of Magnetism and Enhanced Magnetic Anisotropy. United States. https://doi.org/10.1021/acsnano.8b09201
Frey, Nathan C., Bandyopadhyay, Arkamita, Kumar, Hemant, Anasori, Babak, Gogotsi, Yury, and Shenoy, Vivek B. Thu . "Surface-Engineered MXenes: Electric Field Control of Magnetism and Enhanced Magnetic Anisotropy". United States. https://doi.org/10.1021/acsnano.8b09201. https://www.osti.gov/servlets/purl/1774202.
@article{osti_1774202,
title = {Surface-Engineered MXenes: Electric Field Control of Magnetism and Enhanced Magnetic Anisotropy},
author = {Frey, Nathan C. and Bandyopadhyay, Arkamita and Kumar, Hemant and Anasori, Babak and Gogotsi, Yury and Shenoy, Vivek B.},
abstractNote = {Controlling magnetism in two-dimensional (2D) materials via electric fields and doping enables robust long-range order by providing an external mechanism to modulate magnetic exchange interactions and anisotropy. Here in this report, we predict that transition metal carbide and nitride MXenes are promising candidates for controllable magnetic 2D materials. The surface terminations introduced during synthesis act as chemical dopants that influence the electronic structure, enabling controllable magnetic order. We show ground-state magnetic ordering in Janus M2XOxF2–x (M is an early transition metal, X is carbon or nitrogen, and x = 0.5, 1, or 1.5) with asymmetric surface functionalization, where local structural and chemical disorder induces magnetic ordering in some systems that are nonmagnetic or weakly magnetic in their pristine form. The resulting magnetic states of these noncentrosymmetric structures can be robustly switched and stabilized by tuning the interlayer exchange couplings with small applied electric fields. Furthermore, bond directionality is enhanced by Janus functionalization, resulting in improved magnetic anisotropy, which is essential to stable 2D magnetic ordering. The mixed termination-induced anisotropy leads to robust Ising ferromagnetism with an out-of-plane easy axis over the full range of relevant termination compositions for Janus Mn2N. Janus Cr2C, V2C, and Ti2C were found to be robustly antiferromagnetic. Our results provide a strategy for exploiting asymmetric surface functionalization to achieve room-temperature nanoscale magnetism under ambient conditions in MXenes with currently available synthesis techniques.},
doi = {10.1021/acsnano.8b09201},
journal = {ACS Nano},
number = 3,
volume = 13,
place = {United States},
year = {Thu Jan 17 00:00:00 EST 2019},
month = {Thu Jan 17 00:00:00 EST 2019}
}

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