DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Observation of Giant Optical Linear Dichroism in a Zigzag Antiferromagnet FePS3

Journal Article · · Nano Letters
 [1]; ORCiD logo [2];  [3];  [2];  [2];  [4];  [3]; ORCiD logo [2]
  1. Univ. of Washington, Seattle, WA (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Univ. of Washington, Seattle, WA (United States)
  3. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States)

Direct optical probing of the antiferromagnetic order parameter in atomically thin samples is challenging, for example, via magneto-optical spectroscopy, due to the lack of net magnetization. Here, we report zigzag-antiferromagnetism (AFM) induced optical linear dichroism (LD) in layered transition-metal thiophosphate FePS3 down to the monolayer limit. The observed LD is giant despite having the optical wave vector parallel to the Neel vector. The LD is at least one order of magnitude larger than those reported in other antiferromagnetic systems, where the optical wave vector is orthogonal to the Neel vector. The large LD enables the probe of 60 degrees orientated zigzag-AFM domains. The optical anisotropy in FePS3 originates from an electronic anisotropy associated with the zigzag direction of the AFM order and is independent of the spin-pointing direction. Furthermore, our findings point to a new optical approach for the investigation and control of zigzag or stripe magnetic order in strongly correlated systems.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1835248
Journal Information:
Nano Letters, Journal Name: Nano Letters Journal Issue: 16 Vol. 21; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (35)

Magnetic interactions in the layer compounds MPX3 (M = Mn, Fe, Ni; X = S, Se) journal January 1982
Change of the optical birefringence associated with the antiferromagnetic ordering of MnF2, FeF2, CoF2, and NiF2 journal September 1971
The role of the local magnetic mode in the optical absorption spectra of antiferromagnets journal November 1978
Review on structural and chemical properties of transition metal phosphorous trisulfides MPS3 journal December 1986
FePS3: A first-order phase transition in a “2D” Ising antiferromagnet journal December 1984
Anyons in an exactly solved model and beyond journal January 2006
Ising-Type Magnetic Ordering in Atomically Thin FePS 3 journal November 2016
Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals journal April 2017
Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit journal June 2017
Ultrafast observation of critical nematic fluctuations and giant magnetoelastic coupling in iron pnictides journal February 2014
Optical determination of the Néel vector in a CuMnAs thin-film antiferromagnet journal January 2017
Emergent superconductivity in an iron-based honeycomb lattice initiated by pressure-driven spin-crossover journal May 2018
Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3 journal January 2019
Two-dimensional itinerant ferromagnetism in atomically thin Fe3GeTe2 journal August 2018
Three-state nematicity in the triangular lattice antiferromagnet Fe1/3NbS2 journal May 2020
Spin-induced linear polarization of photoluminescence in antiferromagnetic van der Waals crystals journal April 2021
Highly anisotropic excitons and multiple phonon bound states in a van der Waals antiferromagnetic insulator journal March 2021
Coherent many-body exciton in van der Waals antiferromagnet NiPS3 journal July 2020
Temperature dependence of the optical birefringence of Mn F 2 , Mg F 2 , and Zn F 2 journal March 1984
Optical-absorption spectra of the layered transition-metal thiophosphates M PS 3 ( M =Mn, Fe, and Ni) journal September 1992
Phase diagram of a frustrated Heisenberg antiferromagnet on the honeycomb lattice: The J 1 - J 2 - J 3 model journal October 2012
Spiral order in the honeycomb iridate Li 2 IrO 3 journal September 2014
Magnetic ground state of semiconducting transition-metal trichalcogenide monolayers journal June 2015
Magnetic structure of the quasi-two-dimensional antiferromagnet NiPS 3 journal December 2015
Magnetic structure and magnon dynamics of the quasi-two-dimensional antiferromagnet FePS 3 journal December 2016
Charge-Spin Correlation in van der Waals Antiferromagnet NiPS 3 journal March 2018
X-ray magnetic dichroism of antiferromagnet Fe 2 O 3 : The orientation of magnetic moments observed by Fe 2 p x-ray absorption spectroscopy journal March 1993
Observation of the X-Ray Magneto-Optical Voigt Effect journal July 2001
Observation of Giant Magnetic Linear Dichroism in ( Ga , Mn ) As journal June 2005
Magneto-optic response of the metallic antiferromagnet Fe 2 As to ultrafast temperature excursions journal December 2019
VESTA : a three-dimensional visualization system for electronic and structural analysis journal May 2008
Neutron Diffraction Study on MnPS 3 and FePS 3 journal November 1983
Magnetic X-Ray Dichroism Study of the Nearest-Neighbor Spin-Spin Correlation Function and Long-Range Magnetic Order Parameter in Antiferromagnetic NiO journal October 1995
Magnetic ordering induced Raman scattering in FePS3 and NiPS3 layered compounds journal January 1987
Magnetic linear dichroism of an antiferromagnetic MnF2 crystal: Oddness in two different antiferromagnetic states journal November 2007