Incommensurate antiferromagnetic order in weakly frustrated two- dimensional van der Waals insulator CrPSe 3 Baithi Mallesh12 Ngoc Toan Dang34 Tuan Anh Tran5 Dinh Hoa Luong12 Krishna P.

2025-05-06 0 0 1.53MB 23 页 10玖币

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Incommensurate antiferromagnetic order in weakly frustrated two-

dimensional van der Waals insulator CrPSe3

Baithi Mallesh1,2, Ngoc Toan Dang3,4,*, Tuan Anh Tran5, Dinh Hoa Luong1,2, Krishna P.

Dhakal2, Duhee Yoon1, Anton V. Rutkauskas6, Sergei E. Kichanov6, Ivan Y. Zel6, Jeongyoung

Kim2, Denis P. Kozlenko6,*, Young Hee Lee1,2,7,*, Dinh Loc Duong1,2,*

1 Center for Integrated Nanostructure Physics, Institute for Basic Science, Suwon 16419,

Republic of Korea

2Department of Energy Science, Sungkyunkwan University, Suwon 16419, Republic of Korea

3Institute of Research and Development, Duy Tan University, 550000 Danang, Vietnam

4Faculty of Environmental and Natural Sciences, Duy Tan University, 550000 Danang, Vietnam

5Ho Chi Minh City University of Technology and Education, 700000 Ho Chi Minh, Vietnam

6Frank Laboratory of Neutron Physics, Joint Institute for Nuclear Research, 141980 Dubna,

Russia

7Department of Physics, Sungkyunkwan University, Suwon 16419, Republic of Korea

*Correspondence to: dangngoctoan1@duytan.edu.vn, denk@nf.jinr.ru, leeyoung@skku.edu,

l.duong1902@gmail.com

Abstract

Although the magnetic order is suppressed by a strong magnetic frustration, it is maintained but

appears in complex order forms such as a cycloid or spin density wave in weakly frustrated systems.

Herein, we report a weakly magnetic-frustrated two-dimensional van der Waals material CrPSe3.

Polycrystalline CrPSe3 was synthesized at an optimized temperature of 700 oC to avoid the

formation of any secondary phases (e.g., Cr2Se3). The antiferromagnetic transition appeared at TN

~ 126 K with a large Curie–Weiss temperature θCW ~ –371 K via magnetic susceptibility

measurements, indicating weak frustration in CrPSe3 with a frustration factor f (|

CW|/TN) ~ 3.

Evidently, the formation of long-range incommensurate spin-density wave antiferromagnetic order

with the propagation vector k = (0, 0.40, 0) was revealed by neutron diffraction measurements at

low temperatures (below 120 K). The monoclinic crystal structure of C2/m symmetry is preserved

over the studied temperature range down to 20 K, as confirmed by Raman spectroscopy

measurements. Our findings on the spin density wave antiferromagnetic order in two-dimensional

(2D) magnetic materials, not previously observed in the MPX3 family, are expected to enrich the

physics of magnetism at the 2D limit, thereby opening opportunities for their practical applications

in spintronics and quantum devices.

I. INTRODUCTION

Two-dimensional (2D) van der Waals (vdW) magnetic materials are increasingly being

recognized for their potential application in next-generation spintronic devices [1–5]. These

materials in atomically thin forms give rise to controlling magnetic order and physical properties

by gate bias, strain, and proximity effects [3–10]. To explore novel materials and the physics of

magnetism at the 2D limit, both intrinsic-magnetic and magnetic-doped 2D vdW materials have

been synthesized and investigated [5,11–19]. Whereas the latter class requires sophisticated efforts

in designing and investigation, the exploration of intrinsic 2D vdW magnetic materials relies on

the available bulk forms like ferromagnetic insulating CrBr3 [20] and CrI3 [16], semiconducting

CrGeTe3 [15], metallic Fe3GeTe2 [21], and antiferromagnetic insulating MPX3 (M = Fe, Mn, Ni,

X = S, Se) systems [14,22–24]. In the most of these materials, the long-range magnetic order is

retained in atomically thin forms, and in some cases like CrI3, the inter layer magnetic interactions

can be tuned from FM to AFM by mediating the layers number [16]. Furthermore, the

antiferromagnetic order in MPX3 can assist in the formation of coherent excitons [25,26],

indicating an appropriate family of materials to investigate the Bose-Einstein condensation of

excitons [26]. These materials are also suitable prototypes to search for high-TC superconductors

by doping or using pressure [27].

Another important feature of the MPX3 vdW materials is a diversity of commensurate

antiferromagnetic orders, realized on structurally similar lattices with a hexagonal-like

arrangement of transition metal atoms in the vdW layers (Table I). The magnetic structures can be

Néel or zigzag with Heisenberg (MnPS3 [28–31]), XY (NiPS3 [32–35]), and Ising

(FePS3 [28,31,35–38]) types, which depend solely on the exchange coupling energies between

transition metal ions in the lattice. The magnetic structures and magnetic ordering temperatures

are mediated by the strength and correlation between the first-, second-, and third-neighbor

interactions of the in-plane metal atoms [28,29]. The interlayer exchange coupling, though

relatively weak, plays a crucial role in the formation of the magnetic order along the c axis [34].

Although the MPX3 family has diverse magnetic properties, none of the explored MPX3

materials exhibit spin frustration or incommensurate spin arrangements. In this report, for the first

time, we explore a weak spin frustration system in this family, CrPSe3. It crystallizes in the

monoclinic structure of C2/m symmetry and orders antiferromagnetically at the Néel temperature

TN ~ 126 K. The large frustration factor, f = |

CW|/TN (~3) implies that CrPSe3 has weak spin-

frustration. The modulated spin density wave and incommensurate AFM order in CrPSe3, revealed

by neutron diffraction experiments, bring novel prospects for further search of related compounds

for studies of magnetic frustration effects and their interplay with physical properties of the layered

2D vdW compounds.

II. EXPERIMENTAL PROCEDURE

As the first stage of synthesis procedure, a polycrystalline powder of CrPSe3 was synthesized

by a solid-state reaction. Reagents of Cr (powder, 200 mesh, Alfa Aesar, 99.99%), P (red, lumps,

Alfa Aesar, 99.99%), and Se (crushed granules, Alfa Aesar, 99.999%) were ground together under

ambient conditions. Approximately 2 g of materials with their stoichiometric ratio Cr:P:Se = 1:1:3

were pressed as a pellet at 0.1 MPa pressure, followed by sealing in a quartz ampule (22×25×100

mm) under high vacuum (<5×10-3 Torr). The sealed ampule was kept in a box furnace at 700 oC

with a ramp rate of 1.6 oC per min for a 10-day holding time, followed by furnace cooling. At the

second stage, the single crystals were prepared using this powder. This pre-reacted material (1 g)

was sealed in a quartz ampoule (22×25×230 mm) along with I2 (~50 mg) and was kept in a two-

zone furnace at 800–700 oC with a 10-day holding time. Small crystals of a few millimeters were

obtained in the cool zone.

Powder XRD measurements were conducted using a Rigaku Smart Lab diffractometer with

Cu Kα radiation (λ = 1.5418 Å). Le-Bail refinement analysis was carried out using Jana2006 [39].

XPS data were collected using a VG Microtech ESCA2000 X-ray photoelectron spectrometer

using a monochromatic Al-K

X-ray source with 1486.7 eV energy.

The magnetic susceptibility as function of temperature and magnetic field was measured using

the vibrational sample magnetometer of a Quantum Design Physical Properties Measurement

System. The sample loaded at room temperature was cooled to a low temperature (2 K) without

applying magnetic field (zero field cooling, ZFC). At 2 K, a field of 0.1 T was applied, and the

susceptibility was measured on heating up to 300 K. The same magnetic field was applied during

the second cooling process (field cooling, FC) and data were collected while heating to 300 K. The

magnetic moment versus field measurements were conducted at 2 K in the fields range from -14

to 14 T and vice versa.

The room temperature and temperature dependent Raman spectra were collected using Horiba

iHR 550 spectrometer with 514 nm wavelength laser and optical setup of own construction with

the 532 nm wavelength laser in the inverted mode [40], respectively. The Montana system

(Cryostation s50) was used to provide low temperatures in the range between 20 and 250 K. The

sample was illuminated by low laser power (~500 μW) to protect it from unintentional laser effects

and the Raman spectra were collected in reflected geometry. To acquire the Raman spectra, the

collected signals were guided to a 50-cm-long spectrometer equipped with a cooled charge-

coupled device (CCD) using an optical fiber with a core diameter of 150 μm.

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Incommensurateantiferromagneticorderinweaklyfrustratedtwo-dimensionalvanderWaalsinsulatorCrPSe3BaithiMallesh1,2,NgocToanDang3,4,*,TuanAnhTran5,DinhHoaLuong1,2,KrishnaP.Dhakal2,DuheeYoon1,AntonV.Rutkauskas6,SergeiE.Kichanov6,IvanY.Zel6,JeongyoungKim2,DenisP.Kozlenko6,*,YoungHeeLee1,2,7,*,DinhLocDuong...

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Incommensurate antiferromagnetic order in weakly frustrated two- dimensional van der Waals insulator CrPSe 3 Baithi Mallesh12 Ngoc Toan Dang34 Tuan Anh Tran5 Dinh Hoa Luong12 Krishna P.

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