Tuning of topological properties in the strongly correlated antiferromagnet Mn 3Sn via Fe doping Achintya Low Susanta Ghosh Susmita Changdar Sayan Routh Shubham Purwar and S. Thirupathaiah Department of Condensed Matter and Materials Physics

2025-05-06 0 0 1.94MB 10 页 10玖币

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Tuning of topological properties in the strongly correlated antiferromagnet Mn3Sn via Fe doping

Achintya Low, Susanta Ghosh, Susmita Changdar, Sayan Routh, Shubham Purwar, and S. Thirupathaiah∗

Department of Condensed Matter and Materials Physics,

S. N. Bose National Centre for Basic Sciences, Kolkata, West Bengal-700106, India.

Magnetic topological materials, in which strong correlations between magnetic and electronic properties

of matter, give rise to various exotic phenomena such as anomalous Hall effect (AHE), topological Hall

effect (THE), and skyrmion lattice. Here, we report on the electronic, magnetic, and topological properties

of Mn3–xFexSn single crystals (x=0, 0.25, and 0.35). Low temperature magnetic properties have been

signiﬁcantly changed with Fe doping. Most importantly, we observe that large uniaxial magnetocrystalline

anisotropy that is induced by the Fe doping in combination with competing magnetic interactions at low

temperature produce nontrivial spin-texture, leading to large topological Hall effect in the doped systems at

low temperatures. Our studies further show that the topological properties of Mn3–xFexSn are very sensitive to

the Fe doping.

I. INTRODUCTION

Magnetic topological materials are the illustrations of an

interplay between magnetic and electronic states of matter,

providing an important stage for illuminating several exotic

phenomena such as the anomalous Hall effect (AHE) [1–

3], the topological Hall effect (THE) [4–6], the skyrmionic

lattice [7–9], and etc. On the other hand, the kagome

lattice in which atoms are arranged in star-like formation

anticipates a geometrical frustration, leading to noncollinear

antiferromagnetic (AFM) ordering [10–15]. So far, several

kagome intermetallics have been explored to a great extent

due to their potential magnetic topological properties. For

instance, Co3Sn2S2is a magnetic Weyl semimetal showing

giant AHE in addition to chiral anomaly [16,17], Mn3Sn(Ge)

are time-reversal symmetry broken Weyl semimetals, despite

being antiferromagnets, show large AHE induced by the

nonzero k-space Berry curvature [18–21], Fe3Sn2which

is a kagome ferromagnet generates skyrmionic bubbles in

addition to the giant AHE [22,23], YMn6Sn6is a rare

earth based kagome system showing several competing

magnetic orders and large THE [24], and Gd3Ru4Al12 posses

low temperature skyrmion lattice induced by the magnetic

frustration [25].

Skyrmions, the vortex-like spin texture formation in the

real space, are topologically protected and characterized by

their topological charge called the winding number [26].

The skymions pursuit futuristic technological applications

in the high-density data storage devices [27,28], ﬁne

current controlled devices [29], and information processing

devices [30]. There exist several systems showing skyrmion

lattice that is originated from different mechanisms. For

example, in noncentrosymmetric magnetic systems such

as MnSi [8], FeGe [31], and FeCoSi [7] the skyrmion

lattice formation was understood by the Dzyaloshinskii-

Moriya interaction (DMI) under the strong spin-orbit

coupling [32,33]. In the centrosymmetric magnetic

systems such as La1–xSrxMnO3[34] and Fe3Sn2[22]

the competition between magnetic dipole interactions

∗setti@bose.res.in

and uniaxial magnetocrystalline anisotropy stabilizes the

skyrmion lattice [35–37]. In addition, recent studies

show the existence of skyrmions in rare-earth based

intermetallics Gd2PdSi3and Gd3Ru4Al12 due to the magnetic

frustration [25,38].

Mn3Sn is a kagome itinerant antiferromagnet with a N´

eel

temperature of 420 K, has hexagonal crystal structure with

a space group of P63/mmc [18,39]. Here, the Mn atoms

form kagome network in the ab plane of the crystal, showing

chiral 120◦inverse triangular spin structure stabilized by

the DM interaction [14,40]. Due to a slight distortion in

kagome lattice and as well off-stoichiometry of the system,

usually, weak-ferromagnetism is present in this system [15,

18]. Moreover, low-temperature magnetic structure depends

on the elemental ratio of Mn and Sn, annealing temperature,

and crystal growth techniques. Thus, some studies report

helical spin structure in Mn3Sn at low temperatures [41,42]

while the other studies realized spin-glass state below 50

K [43,44]. At room temperature, Mn3Sn shows noncollinear

antiferromagnetic ordering with 1200inverse triangular spin

structure [14,15,18,40] leading to large anomalous Hall

effect. Particularly, Mn3Sn is of great research interest as

the triangular-coplanar magnetic order reshapes into a spiral-

noncoplanar magnetic ordering with a ﬁnite net magnetization

along the c-axis at a critical spin-reorientation transition

temperature (TSR ≈260 K) [14,18,40] which is not found in

Mn3Ge [45]. As a result, the large AHE is suppressed below

TSR in Mn3Sn but not in Mn3Ge [46].

Theoretically, Mn3Sn is not expected to show topological

Hall effect (THE) as the stoichiometric Mn3Sn does not

possess chiral-spin texture. However, there are few

reports claiming the observation of a small topological Hall

resistivity due to the ﬁeld induced chiral-spin texture in

polycrystalline Mn3Sn [47] at low temperature and due to

domain wall formation in the single crystalline Mn3Sn at

room temperature [48,49]. On the other hand, Fe3Sn sharing

similar crystal structure of Mn3Sn is a ferromagnetic metal

with an easy axis of magnetization in the ab plane that can

be shifted to the c-axis with doping [50,51]. Motivated

from the polymorphic magnetic properties of Mn3Sn and

ﬂexibility of manipulating the easy axis in Fe3Sn, we have

substituted Fe atoms at Mn sites of Mn3Sn to enhance the

topological properties of Mn3Sn as Fe substitution introduces

arXiv:2210.14150v1 [cond-mat.mtrl-sci] 25 Oct 2022

ferromagnetism to the system.

In this work, single crystals of Mn3–xFexSn (x=0, 0.25,

and 0.35) were systematically studied for their electrical

resistivity, magnetic, and topological properties. While

Mn3Sn is found to be metallic in nature up to room

temperature with a spin-reorientation driven kink at 260 K,

with Fe doping the system shows magnetism induced metal-

insulator (MI) transition at 240 K for x=0.25 and 150 K

for x=0.35. In addition to MI transition, x=0.35 system

shows disorder induced resistivity upturn with a minima

at Tm=50 K. As for the magnetic properties, Mn3Sn is

found to show a sudden drop in magnetization at a spin-

reorientation transition temperature of 260 K and spin-glass-

like transition below 40 K. On the other hand, with Fe doping

ferromagnetic transition has been introduced alongside with

enhanced magnetic anisotropy. Also, anisotropic anomalous

Hall resistivity has been induced at low temperatures with Fe

doping. Particularly, the out-of-plane Hall resistivity (ρzx)

increases with decreasing temperature for all the compositions

from 300 K down to their respective magnetic transition

temperatures where a sudden change in Hall resistivity is

noticed. Though not much change in out-of-plane Hall

resistivity is noticed with Fe doping at 2 K, the in-plane Hall

resistivity (ρxy) is gigantically enhanced from -0.25 µΩ-cm

to 48 µΩ-cm in going from x=0 to x=0.35. Along with the

anomalous Hall resistivity, a large topological Hall resistivity

also is observed for both Fe doped systems at 2 K.

II. EXPERIMENTAL DETAILS

Single crystals of Mn3–xFexSn (x=0, 0.25, and 0.35)

were prepared by self ﬂux method [52–54]. First, Mn

(Alfa Aesar 99.995%), Fe (Alfa Aesar, 99.99%), and Sn

(Alfa Aesar 99.998%) powders were taken with a ratio of

(7-x) : x: 3, mixed thoroughly before inserting into

a preheated quartz tube, and sealed under partial Argon

pressure. The mixture was then heated up to 1000oC,

slowly cooled down to 900oC, and then was air quenched to

room temperature by taking out the ampoule from furnace.

In this way, we obtained shiny hexagonal and rod shaped

single crystals with a typical size of 1.5 mm ×1 mm

×1 mm. X-ray diffraction (XRD) measurements were

done on different surfaces of the single crystals using

Rigaku SmartLab equipped with 9 kW Cu KαX-ray source.

Elemental compositions of the crystals were calculated to

be Mn2.97Sn1.03, Mn2.74Fe0.26Sn, and Mn2.64Fe0.36Sn using

energy dispersive X-ray spectroscopy (EDXS) technique.

For convenience we denote the compositions Mn2.97Sn1.03,

Mn2.74Fe0.26Sn, and Mn2.64Fe0.36Sn by x=0, x=0.25, and

x=0.35, respectively, wherever applicable.

Electrical resistivity measurements were carried out

in the linear four-probe method and Hall measurements

were done in the measuring geometry shown in the

schematic of Fig. 1(e). Magneto-transport and magnetization

measurements were performed in Physical Properties

Measurement System (9T PPMS, DynaCool, Quantum

Design) using ETO and VSM options, respectively. Hall

40 60 80

20 40 60 80

2θ(

)

2θ(

)

Intensity(a.u.)

Intensity(a.u.) (0002)

(0004)

(011



0) (022



(033



(044







[011

0]

[21

1

0]

[0001]

 

HǁzHǁy

(a) (c)

(d)

(b)

(e)

FIG. 1. (a) and (b) show typical XRD patterns of Mn3Sn single

crystal taken from two different orientations as shown in the inset

images. (c) Schematic hexagonal lattice of Mn3Sn in the ab plane

where Mn atoms form kagome geometry and Sn atoms sit in the

center of hexagon. In (d), x,y, and z-axes correspond to [2 ¯

110],

[01¯

10], and [0001] orientations, respectively. Magnetotransport

measuring geometry is shown in (e), where ρxy is measured with

current along the x-axis and external magnetic ﬁeld applied along

the z-axis to ﬁnd Hall voltage along the y-axis and ρzx is measured

with current along the z-axis and ﬁeld applied along the y-axis to

ﬁnd Hall voltage along the x-axis.

resistivity was measured for two different orientations as

shown in Fig. 1(e). ρxy stands for current along the x

direction and ﬁeld along the zdirection where Hall voltage

was measured along the ydirection. Similarly ρzx stands

for current along zdirection, ﬁeld along the ydirection,

and Hall voltage was measured along the xdirection. To

eliminate longitudinal voltage contribution due to any

possible misalignment of the probes, the Hall resistivity

was calculated by ρ(H)–ρ(–H)

2. Temperature dependent Hall

resistivity measurements were done using both positive (H)

and negative (-H) applied ﬁelds and then calculated using the

formula ρ(T,H)–ρ(T,–H)

III. RESULTS AND DISCUSSIONS

XRD patterns shown in Figs. 1(a) and 1(b) represent

intensity reﬂections of (0002) and (01¯

10) hexagonal planes,

respectively, taken from Mn3Sn single crystal. Figs. 2(a),

(c), and (e) depict zero-ﬁeld out-of-plane resistivity (ρzz)

measured between 2 and 300 K from Mn3Sn, Mn2.75Fe0.25Sn,

and Mn2.65Fe0.35Sn single crystals, respectively. Overall, a

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TuningoftopologicalpropertiesinthestronglycorrelatedantiferromagnetMn3SnviaFedopingAchintyaLow,SusantaGhosh,SusmitaChangdar,SayanRouth,ShubhamPurwar,andS.ThirupathaiahDepartmentofCondensedMatterandMaterialsPhysics,S.N.BoseNationalCentreforBasicSciences,Kolkata,WestBengal-700106,India.Magnetictopolo...

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Tuning of topological properties in the strongly correlated antiferromagnet Mn 3Sn via Fe doping Achintya Low Susanta Ghosh Susmita Changdar Sayan Routh Shubham Purwar and S. Thirupathaiah Department of Condensed Matter and Materials Physics.pdf

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Tuning of topological properties in the strongly correlated antiferromagnet Mn 3Sn via Fe doping Achintya Low Susanta Ghosh Susmita Changdar Sayan Routh Shubham Purwar and S. Thirupathaiah Department of Condensed Matter and Materials Physics

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