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Long-range ferromagnetism and magnetocaloric effects in rapidly quenched Ni50-xCoxMn50-yAly ribbons

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Despite some previous efforts [7,16 e18] , a clear understanding of the magneto- caloric effect and its association with the magnetic phase transition and magnetic interactions character[r]

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Nguyen Thi Maia,b, Nguyen Hai Yenc, Pham Thi Thanhc, Tran Dang Thanhc,

a The College of Printing Industry, Phuc Dien, Bac Tu Liem, Ha Noi, Viet Nam

b Hanoi University of Science, Vietnam National University, 334 Nguyen Trai, Thanh Xuan, Ha Noi, Viet Nam

c Institute of Material Science, Vietnam Academy of Science and Technology, 18 Hoang Quoc Viet, Cau Giay, Ha Noi, Viet Nam

d Hanoi Pedagogical University, No 2, 32 Nguyen Van Linh, Phuc Yen, Vinh Phuc, Viet Nam

e Hong Duc University, 565 Quang Trung, Dong Ve, Thanh Hoa, Viet Nam

f Quang Ninh University of Industry, Yen Tho, Dong Trieu, Quang Ninh, Viet Nam

a r t i c l e i n f o

Article history:

Received 15 February 2017

Received in revised form

17 February 2017

Accepted 19 February 2017

Available online 27 February 2017

Keywords:

Magnetocaloric effect

Magnetic phase transition

Heusler alloy

Critical parameter

Melt-spinning method

a b s t r a c t

Ni50xCoxMn50yAly(x¼ 7 and 9; y ¼ 17, 18 and 19) alloy ribbons were prepared by melt-spinning with a tangential velocity of copper wheel of 40 m s1 X-ray diffraction patterns reveal multi-crystalline phase behavior in the fabricated ribbons The shape of thermomagnetization curves clearly depends on Co and

Al concentrations The Curie temperatures (TC) of the alloy ribbons strongly increase with increasing the

Co concentration and slightly decrease with increasing the Al concentration The martensitic-austenitic phase transition in the alloy ribbons can be manipulated by tuning Co and Al concentrations The maximum magnetic entropy changejDSmjmaxof about 0.75 J kg1K1for afield change of 12 kOe at

TCz 364 K was achieved for the Ni43Co7Mn32Al18ribbon Critical analysis using the Arrott-Noaks and KouveleFisher methods demonstrates the existence of a long-range ferromagnetic order in this ribbon

© 2017 The Authors Publishing services by Elsevier B.V on behalf of Vietnam National University, Hanoi This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/)

1 Introduction

The magnetocaloric effect (MCE) is defined as the heating or

cooling of a magnetic material when a magneticfield is applied The

MCE occurs in a magnetic solid as a result of the entropy variation

due to the coupling of the magnetic spin system with the magnetic

field Since the discovery of the MCE, it has been widely utilized in

magnetic materials to reach low temperatures Nowadays, there is a

great deal of interest in using the MCE as an alternative technology

for refrigeration The magnetic refrigeration offers the prospect of

an energy-efficient and environmentally friendly alternative to the

common vapor cycle refrigeration technology used today[1e5]

Among magnetocaloric materials, NieMn-based Heusler alloys

are emerging as a promising candidate[6] Recently, Ni-Mn-based

alloys have been reported to exhibit the large magnetocaloric ef-fects, including both the conventional and inverse magnetocaloric effects [7e9] Besides that, the shape memory effect and other interesting properties have also been observed[10e12] In the Ni-Mn-Al Heusler alloys, the Neel temperature TN z 300 K was found to be virtually independent of composition[13] The

Ni-Mn-Al alloys with their relatively low cost and high ductility are a potentially attractive candidate material as a magnetic refrigerant The partial substitution of Co for Ni in these alloys has been re-ported to have a strong effect on the martensitic-austenitic trans-formation which greatly enhanced the MCE[14e16] Despite some previous efforts[7,16e18], a clear understanding of the magneto-caloric effect and its association with the magnetic phase transition and magnetic interactions characterized by critical exponents in Ni-Co-Mn-Al alloys has not been reached

To address this, we have systematically investigated the mag-netic, magnetocaloric and critical properties of Ni50 xCoxMn50 yAly

(x¼ 7 and 9; y ¼ 17, 18 and 19) rapidly quenched ribbons

* Corresponding author.

E-mail address: dannh@ims.vast.ac.vn (N.H Dan).

Peer review under responsibility of Vietnam National University, Hanoi.

http://dx.doi.org/10.1016/j.jsamd.2017.02.007

2468-2179/© 2017 The Authors Publishing services by Elsevier B.V on behalf of Vietnam National University, Hanoi This is an open access article under the CC BY license

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2 Experimental

Six alloy ingots with nominal compositions of Ni50x

-CoxMn50 yAly(x¼ 7 and 9; y ¼ 17, 18 and 19) were prepared from

pure elements (99.9%) of Ni, Co, Mn and Al using the arc-melting

method in Argon gas The melt-spinning method was then used

to fabricate the alloy ribbons with a tangential velocity of copper

wheel of 40 m s1 The structure of the alloys was investigated by

powder X-ray diffraction (XRD) technique using CuKa radiation

with measuring step of 0.02at room temperature The magnetic

properties and magnetocaloric effects of the alloys were

charac-terized on a vibrating sample magnetometer with temperature

range of 77e500 K and maximum magnetic field of 12 kOe

3 Results and discussion

The XRD patterns taken at room temperature (Fig 1) show that

crystalline phases of L10(face centered cubic), B2 (body centered

cubic) and 10M (orthorhombic) are formed in the ribbons Most of

the samples mainly contain B2 and L10 phases The 10M phase

appears in the ribbons with high concentrations of Al and Co The

change of the structure would probably affect magnetic and

mag-netocaloric properties of the alloys

The magnetic properties of the samples were characterized by

magnetization versus temperature (M-T) measurements (Fig 2a)

The results show that the shape of M-T curves clearly depends on Co

and Al concentrations For examples, the magnetization of the

sample with x¼ 7 increased from ~0.7 emu/g for y ¼ 17 to ~7.7 emu/g

for y¼ 19 The Curie temperatures of the alloy ribbons strongly increased with increasing the Co concentration and slightly decreased with increasing the Al concentration By increasing the Co concentration from 7 at.% to 9 at.%, the Curie temperature (TC) strongly increased from ~364 K (for x¼ 7 and y ¼ 18) to ~ 394 K (for

x¼ 9 and y ¼ 18) The magnetization of Ni50xCoxMn33Al17ribbons are also increased considerably with the substitution of Co for Ni The martensitic-austenitic phase transition in the alloy ribbons can

be tuned by adjusting Co and Al concentrations

In this series of samples, the Ni43Co7Mn32Al18ribbon shows two strong magnetic phase transitions near a room temperature region Therefore, it was chosen as a representative one for analyzing magnetic and magnetocaloric properties The magnetocaloric effect

in the ribbon was assessed by the magnetic entropy change (DSm)

as functions of temperature and magnetic field using Maxwell relationship:

DSm¼

ZH 2

H 1

 vM vT

 H

From a series of experimental curves M(T) (Fig 2b), the corre-sponding M(H) curves can be deduced (Fig 3a) Fig 3b shows

DSm(T) curves of the Ni43Co7Mn32Al18ribbon for different magnetic field changes (D ¼ 1, 4, 8, and 12 kOe) ForD ¼ 12 kOe, the maximum magnetic entropy changes (jDSmjmax) are determined to

be about 0.43 and0.74 J kg1K1for the conventional (negative) and inverse (positive) magnetocaloric effects, respectively As

Fig 1 XRD patterns of Ni50xCo x Mn50yAl y ribbons with x ¼ 7 (a) and x ¼ 9 (b).

Fig 2 Thermomagnetization curves of Ni 50x Co x Mn 50y Al y (x ¼ 7 and 9; y ¼ 17, 18 and 19) ribbons measured in a magnetic field of 100 Oe (a) and thermomagnetization curves of

fields (b).

N.T Mai et al / Journal of Science: Advanced Materials and Devices 2 (2017) 123e127 124

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expected, thejDSmjmaxincreases with increasing the magneticfield

(the inset ofFig 3b)

The temperature dependence ofDSmfor different appliedfield

changes for the second-order phase transition of materials can be

described by the so-called “universal master” curves [19e21]

Based on the DSm(T) curves, the DSm=DSmax versus q plots are

constructed Whiteqvalue is determined by the formula:



ðT  TCÞ=ðTr1 TCÞ; T  TC

ðT  TCÞ=ðTr2 TCÞ; T> TC (2)

where Tr1and Tr2are the temperatures of the two reference points

For the present study, they are selected as those corresponding to

DSmðTr1 ;2Þ ¼ k:DSmaxðk ¼ 0:5Þ This choice of k does not affect the

actual construction of the universal curve, as it implies only

pro-portionality constant.Fig 4a shows the universal master curve of

the Ni43Co7Mn32Al18ribbon AllDSm(T) data are well collapsed onto

a universal master curve, affirming the nature of second-order

magnetic transition of the material This is an interesting

prop-erty of second-order phase transition materials and is distinct from

first-order phase transition materials

It has been shown that the magnetic orders of materials

exhibiting in a second-order magnetic phase transition can be

assessed by the critical parameters using Arrott plots [22] The

Arrott plots, H/M versus M2(Fig 4b), were constructed from the

M(H) data It can be observed that the M2eH/M curves are

non-linear at low magnetic field and linear at high magnetic field

Values of the spontaneous magnetization (MS) and the inverse

initial susceptibility (c0 1) at different temperatures were derived

from Arrott plots The critical parameters ofb,gand TCrelate to the two above quantities via the following equations:

MSðTÞ ¼ M0ðεÞH ε < 0; (3)

c10 ðTÞ ¼H0

where M0, H0and D are the critical amplitudes andε ¼ ðT  TCÞ=TC

is the reduced temperature

The linear extrapolation from highfield to the intercepts with the M2 and H/M axes gives the values of MS(T) and c0 1(T),

respectively The critical parameters TC,bandgwere obtained from fitting MS(T) and c01(T) data (Fig 5a) following the according

formulas (3) and (4), whiledwas calculated by using the Widom scaling relation, equationd¼ 1 þg=b(5)[23] The Ni43Co7Mn32Al18

ribbon possesses TC ¼ 364.21 ± 0.61 K, b ¼ 0.469 ± 0.048,

g¼ 0.951 ± 0.035 anddz 3.027 The critical parameters can be obtained more accurately by the KouveleFisher method[25] Like Arrott-Noakes method, MS(T) andc10 ðTÞ are determined by plot-ting M1/bversus (H/M)1/gcurves The critical parameters ofbandg

relate to the two above quantities by these equations:

MS½dMS=dT1¼ ðT  TCÞ=b (6)

Fig 3 Magnetic field dependence of the magnetization at different temperatures (a) andDS m (D ¼ 1, 4, 8, and 12 kOe) versus temperature (inset shows the field dependence of

jDS m j max ) (b) of the Ni 43 Co 7 Mn 32 Al 18 ribbon.

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c10 ðTÞhdc10 ðTÞ.dTi1

The critical parameters TC,bandgobtained fromfitting MS(T)

andc0 1(T) data by using the accordingformulas (6) and (7).Fig 5b

shows the KouveleFisher curves of the Ni43Co7Mn32Al18 ribbon

withfitting results of TCz 364 K,bz 0.462 andgz 0.948 Based

on the Widom scaling relation, the dvalue was calculated to be

3.051 Clearly, the critical parameter values determined from the

KouveleFisher method are in good agreement with those obtained

by the Arrott-Noakesfittings These critical parameters are quite

close to those of the mean-field model (b¼ 0.5,g¼ 1 andd¼ 3)

characterizing materials with long-range ferromagnetic

in-teractions [24] In a previous study, it has been shown that

Ni50Mn50 xSnx(x¼ 13 and 14) alloy ribbons show a short-range

ferromagnetic order for x¼ 13 but a long-range ferromagnetic

or-der for x¼ 14 at temperatures just below Tc, indicating that that Sn

addition tends to drive the system, in the austenitic ferromagnetic

phase, from the short-range (x¼ 13) to long-range (x ¼ 14)

ferro-magnetic order[16] The long-range ferromagnetism has recently

been reported for Co50 xNixCr25Al25(x¼ 0 and 5) alloys[17] In the

present case, the presence of Co and Al seem to establish a

long-range ferromagnetic order in the Ni43Co7Mn32Al18ribbon, thus

fa-voring the conventional (negative) magnetocaloric effect rather

than the inverse (positive) magnetocaloric effect Nevertheless, a

systematic study on effects of various Co and Al contents on the

magnetic ordering and magnetocaloric effect in Ni50 xCoxMn33Al17

ribbons will be essential to fully understand their relationship

4 Conclusion

The rapidly quenched Ni50xCoxMn50yAly(x¼ 7 and 9; y ¼ 17,

18 and 19) ribbons exhibit multi-crystalline phases of the L10, B2

and 10M types The Curie temperature of the alloy ribbon strongly

increases with increasing the Co-concentration and slightly

de-creases with increasing the Al-concentration For afield change of

12 kOe, the maximum magnetic entropy change of the Ni43

C-o7Mn32Al18 ribbon is about 0.43 and 0.74 J kg1 K1 for the

negative and positive magnetocaloric effects, respectively This

sample exhibits a long-range ferromagnetic order at temperatures

just below the TC

Acknowledgments

This work was supported by the National Foundation for Science

and Technology Development (NAFOSTED) of Viet Nam under

Grant numbers of 103.02e2014.35 Part of the work was done in

Key Laboratory for Electronic Materials and Devices and Laboratory

of Magnetism and Superconductivity, IMS-VAST, Viet Nam

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Fig 5 Temperature dependence of spontaneous magnetization M S (T) and inverse initial susceptibilityc10 ðTÞ (a) and KouveleFisher plots (b) for the Ni 43 Co 7 Mn 32 Al 18 ribbon.

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