Magnetic Isotropy/Anisotropy in Layered Metal Phosphorous Trichalcogenide MPS3 (M = Mn, Fe)Single Crystals

Abstract

Despite the fact that two-dimensional layered magnetic materials hold immense potential applications in the field of spintronic devices, tunable magnetism is still a challenge due to the lack of controllable synthesis. Herein, high-quality single crystals MPS3 (M= Mn, Fe) of millimeter size were synthesized through the chemical vapor transport method. After systemic structural characterizations, magnetic properties were studied on the bulk MPS3 layers through experiments, along with first principle theoretical calculations. The susceptibilities as well as the EPR results evidently revealed unique isotropic and anisotropic behavior in MnPS3 and FePS3 crystals, respectively. It is worth noting that both of these materials show antiferromagnetic states at measured temperatures. The estimated antiferromagnetic transition temperature is 78 K for bulk MnPS3 and 123 K for FePS3 crystals. The spin polarized density functional theory calculations confirmed that the band gap of the antiferromagnetic states could be generated owing to asymmetric response all over the energy range. The ferromagnetic state in MnPS3 and FePS3 is less stable as compared to the antiferromagnetic state, resulting in antiferromagnetic behavior. Additionally, frequency-dependent dielectric functions for parallel and perpendicular electric field component vectors, along with the absorption properties of MPS3, are thoroughly investigated.

Phonon and Thermal Properties of Quasi-Two-Dimensional FePS3 and MnPS3 Antiferromagnetic Semiconductors

“…Figure a,b shows the results of X-ray diffraction spectroscopy (XRD) of FePS 3 and MnPS 3 crystals, respectively. The XRD data reveals that both materials possess a pure single-crystal phase with major (001) and (002) crystallographic planes . The insets in Figure a,b illustrate the crystal structure of both material systems where the gray, yellow, gold, and violet spheres represent phosphorus (P), sulfur (S), iron (Fe), and manganese (Mn) atoms, respectively.…”

“…The optical phonon properties of FePS 3 and MnPS 3 bulk crystals have been studied extensively using Raman spectroscopy and infrared (IR) absorption techniques. − ,− The early Raman studies of bulk crystals suggested that the vibrational dynamics of both crystals can be pictured within the framework of a molecular approach, dividing the Raman spectrum into the high-frequency internal modes of P 2 S 6 , and the low-frequency modes where the interaction of the M element with phosphorus (P) and chalcogenides (X) becomes significant. A recent temperature-dependent polarized Raman study of bulk, few-, and monolayer FePS 3 revealed features in the spectra, emerging at the transition temperature, and suggested that a monolayer FePS 3 possesses an Ising-type AFM ordering .…”

Low‐Frequency Electronic Noise in Quasi‐2D van der Waals Antiferromagnetic Semiconductor FePS3—Signatures of Phase Transitions

“…[32] The Néel temperature, T N , for FePS 3 is reported to be around 118 K. [1,2,20] It shows strong magnetic anisotropy. [15,33,34] In the crystal, each Fe atom is ferromagnetically coupled with two of its neighbors but the layer is antiferromagnetically coupled with nearest layers making it a zigzag-AF (z-AF) material. [1] The semiconducting nature of FePS 3 , with the energy bandgap of 1.5 eV, and a possibility of the strain engineering of electron and phonon band-structure create additional means for the control of both electron and spin transport.…”

The emerging ferroic orderings in two dimensions

“…The results show that the NiPS 3 is antiferromagnetic and with a small anisotropy, which leads to the generation of dispersive magnons with a ∼7 meV gap. Rehman et al [94] synthesized the 2D layered MnPS 3 and FePS 3 materials by chemical vapor transport method. The magnetic properties of multilayer MnPS 3 and FePS 3 materials are investigated.…”

“…A list of known experimental 2D magnetic materials and their properties is shown in Table 2 [30,32,51,53,54,61,74,94,96,105,106,108,[110][111][112]. The properties, according to the to-date experimental progress, listed in Table 2 and are extracted from single layer materials.…”