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Phase diagram, ferromagnetic martensitic

transformation and magnetoresponsive
properties of Fe-doped MnCoGe alloys

Article in Journal of Magnetism and Magnetic Materials · November 2012

DOI: 10.1016/j.jmmm.2012.12.001 · Source: arXiv

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1 Contents lists available at SciVerse ScienceDirect

2
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4 Journal of Magnetism and Magnetic Materials
5
6
journal homepage: www.elsevier.com/locate/jmmm
7
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Phase diagram, ferromagnetic martensitic transformation and
13 magnetoresponsive properties of Fe-doped MnCoGe alloys
14
15 Q1 G.J. Li a, E.K. Liu a, H.G. Zhang a, Y.J Zhang a, J.L. Chen a, W.H Wang a, H.W. Zhang a, G.H. Wu a,n, S.Y. Yu b
16
a
17 Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Science, Beijing 100190, People’s Republic of China
b
School of Physics, Shandong University, Jinan 250100, People’s Republic of China
18
19
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21 a r t i c l e i n f o abstract
22
Article history: The crystal structure and magnetoresponsive properties of Fe-doped MnCoGe alloys have been
23
Received 11 March 2012 investigated using x-ray diffraction (XRD) and magnetic measurements. By alloying the Fe-
24 Received in revised form containing isostructure compounds into MnCoGe, a magnetostructural transition from paramagnetic
25 30 November 2012
austenite to ferromagnetic martensite with large magnetization difference can be realized in a
26 temperature window between the Curie temperatures of the austenite and martensite, resulting in a
27 Keywords: magnetic-field-induced martensitic transformation and large magnetic-entropy changes. A structural
28 Isostructural alloying and magnetic phase diagram of Fe-doped MnCoGe alloys is presented.
29 Ferromagnetic martensitic transformation & 2012 Elsevier B.V. All rights reserved.
Magnetoresponsive property
30
Fe-doped MnCoGe alloy
31
67
32
1. Introduction vacancy [17], the fourth elements [18,19,21,22,24,25] or pressure 68
33
[26–28] in MnCo(Ni)Ge alloys. Thus, a strong magnetostructural 69
34
Ferromagnetic (FM) martensitic-transition materials have coupling with large magnetization difference can be realized. The 70
35
attracted increasing attention due to their magnetoresponsive previous reports indicate that the doping of Fe in Heusler alloys 71
36
effects, including magnetic-field-induced martensitic transforma- [29–31], Ru-based [32] alloys or Gd5Ge2Si2 [33] can suppress the 72
37
tion/strain effect [1–3], magnetoresistance [4,5] and magnetocaloric martensitic transition and stabilize the parent phases. Recently, 73
38
effect [6,7], etc. For these properties, the magnetostructural coupling chemically alloying the Fe-containing isostructure MnFeGe or 74
39
between structural and magnetic transition plays a crucial role. FeNiGe alloy to Ni2In-type MnNiGe is proved to be an effective 75
40
Thus, exploring materials with magnetostructural transition is of method to manipulate the first-order martensitic transformation 76
41
Q2 importance for fundamental science and technology application. in a temperature window [18]. Another study has reported the 77
42
The magnetic equiatomic MM’X (M, M’¼transition metals, magnetocaloric effect based on a second-order magnetic transi- 78
43
X¼Si, Ge, Sn) compounds [8–11] have become interesting tion at TC in MnCo1  xFexGe alloys (x¼ 0  1.00) [34]. However, the 79
44
research objects due to their remarkable magnetoresponsive study of the first-order martensitic transformation based on the 80
45
properties [12–25]. As one of the important MM’X compounds, coupling of magnetic and structural transitions, and their mag- 81
46
the stoichiometric MnCoGe alloy transforms from the Ni2In-type netoresponsive properties of MnCo1  xFexGe(xo0.10) are still 82
47
hexagonal structure (space group p63/mmc, 194) to the TiNiSi- absent up to now. 83
48
type orthorhombic structure (space group pnma,62) via the In this work, based on the isostructural alloying method, the 84
49
martensitic transformation at about 420 K, i.e. martensitic trans- MnCo1  xFexGe and Mn1  xFexCoGe alloys were prepared. The 85
50
formation temperature (T m ). The Curie temperatures of hexagonal study on the first-order FM martensitic transformation in Fe- 86
51
austenite and orthorhombic martensite are 276 K (T AC ) and 355 K doped MnCoGe alloys was carried out. By Fe substitution, a 87
52
(T M M
temperature window between T AC and T M 88
53 C ), respectively [9–11]. It can be seen that T C is about 80 K C and therein a martensi-
A M
higher than T C . Because T m is higher than T C , the martensitic tic transformation from PM austenite to FM martensite with large 89
54
transformation occurs in the paramagnetic (PM) state without a magnetization difference was realized. The magnetic-field- 90
55
magnetostructural coupling. If lowering the T m below T M 91
56 C , a induced martensitic transformations and magnetocaloric effects
magnetostructural transition can occur in the magnetic region. were also investigated. 92
57
In previous studies, a martensitic transformation between PM 93
58
Ni2In-type structure and FM TiNiSi-type structure can be obtained 94
59
in a temperature window between T AC and T M 2. Experimental method 95
60 C by introducing the
96
61
Polycrystalline ingots of MnCo1 xFexGe(x¼0 0.15) and 97
62
n
Corresponding author. Mn1 xFexCoGe(x¼00.10) alloys were prepared by arc-melting 98
63
E-mail address: ghwu@iphy.ac.cn (G.H. Wu). high-purity metal Mn, Co, Ge and Fe with purity of 99.99% and 99
64
100
65 0304-8853/$ - see front matter & 2012 Elsevier B.V. All rights reserved. 101
66 http://dx.doi.org/10.1016/j.jmmm.2012.12.001

Please cite this article as: G.J. Li, et al., Journal of Magnetism and Magnetic Materials (2012), http://dx.doi.org/10.1016/
j.jmmm.2012.12.001i
 2 G.J. Li et al. / Journal of Magnetism and Magnetic Materials ] (]]]]) ]]]–]]]

1 higher under argon atmosphere. The ingots were homogenized indicating a large lattice distortion. This large and positive volume 67
2 subsequently in evacuated quartz tubes with argon at 1123 K for expansion can result in significant difference of atomic surrounding 68
3 5 days and then quenched into ice water. The X-ray diffraction and crystal structure between Ni2In-type and TiNiSi-type structures. 69
4 (XRD) with Cu-Ka was employed to characterize the crystal struc- It is known that the radius of Fe (0.172 nm) is larger than that 70
5 tures. The magnetic measurements of the samples were carried out of Co atom (0.167 nm) while smaller than that of Mn atom 71
6 by a superconducting quantum interference device (SQUID). (0.179 nm) [35]. In Ni2In-type structure, however, the main peaks 72
7 of two series of alloys both shift to the large-angle direction with 73
8 the substitution of Fe for Mn or Co atoms, which means the unit- 74
9 3. Results and discussion cell sizes of the two series of alloys all decrease with the 75
10 increasing of Fe content. In MnCo1  xFexGe alloys, the newly 76
11 Fig. 1(a) and (b) shows the powder XRD patterns of MnCo1  x- introduced Fe atoms will occupy Co sites since MnCoGe and 77
12 FexGe and Mn1  xFexCoGe alloys measured at room temperature, MnFeGe are isostructural [10]. Thus the strong covalent effect 78
13 respectively. It can be seen that the crystal structure changes from between Fe and Ge atoms is formed. The reduction of lattice 79
14 the coexistence of TiNiSi-type and Ni2In-type structures to the parameter can be ascribed to this enhanced covalent effect, which 80
15 single Ni2In-type structure with the substitution of Fe for Co or Mn just like the case in Fe-doped MnNiGe alloys [18]. 81
16 atoms. This indicates the martensitic transformation temperatures The temperature dependence of magnetization for MnCo1 xFexGe 82
17 of the two series of alloys decrease from higher temperature down and Mn1 xFexCoGe alloys measured under a magnetic field of 100 Oe 83
18 to lower temperature. The substitution of Fe for Mn or Co can were shown in Fig. 2(a) and (b), respectively. It can be seen that the 84
19 effectively change the phase stability of MnCoGe alloys. martensitic transformation temperature decreases with the substitu- 85
20 Indexing the XRD pattern of the Mn0.97Fe0.03CoGe alloy (not tion of Fe for Co or Mn atoms, which means the doping of Fe atoms 86
21 shown in Fig. 1(b)), the lattice parameters of Ni2In-type hexagonal can realize the desired coupling of martensitic structural transition 87
22 austenitic and TiNiSi-type orthorhombic martensitic phase were and magnetic transition. This effect is very similar to the case in 88
23 obtained. For austenitic structure, the lattice parameters are isostructural Fe-doped MnNiGe alloys [18], in which the doping of Fe 89
24 a¼4.0812 Å, c¼5.2890 Å, and those of martensitic structure are for transition-metal atoms can also effectively decrease the marten- 90
25 a¼5.9074 Å, b¼3.8178 Å, c¼7.0445 Å, respectively. The unit-cell sitic transition temperature to magnetic ordering temperature. In 91
26 volume increases by 4.2% during the martensitic transformation, Mn1 xVxCoGe [21]and MnNi1 xCoxGe1.05 [23] alloys, the researchers 92
27 93
28 94
29 95
30 96
31 97
32 98
33 99
34 100
35 101
36 102
37 103
38 104
39 105
40 106
41 107
42 108
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44 110
45 Fig. 1. XRD patterns of MnCo1  xFexGe alloys (x ¼0.03, 0.06, 0.10, 0.12) (a) and Mn1  xFexCoGe alloys (x ¼0.02, 0.04, 0.06, 0.10) (b). Here h and o denote the Ni2In-type 111
46 hexagonal and TiNiSi-type orthorhombic structures, respectively. 112
47 113
48 114
49 115
50 116
51 117
52 118
53 119
54 120
55 121
56 122
57 123
58 124
59 125
60 126
61 127
62 128
63 129
64 Fig. 2. Temperature dependence of magnetization of MnCo1  xFexGe alloys (a) and Mn1  xFexCoGe alloys (b) measured under a magnetic field of 100 Oe. Insets of (a) and
130
65 (b) show the temperature dependence of magnetization of MnCo0.94Fe0.06Ge and Mn0.97Fe0.03CoGe alloys under a magnetic field of 50 kOe, respectively. Ms and Mf denote 131
66 the starting and finishing temperatures of the martensitic transformation; As and Af are the starting and finishing temperatures of the reverse transformation. 132

Please cite this article as: G.J. Li, et al., Journal of Magnetism and Magnetic Materials (2012), http://dx.doi.org/10.1016/
j.jmmm.2012.12.001i
 G.J. Li et al. / Journal of Magnetism and Magnetic Materials ] (]]]]) ]]]–]]] 3

1 attributed this effect to the so-called ‘‘chemical pressure’’, originating Meanwhile, comparing the thermomagnetization curves of 67
2 from the different atomic radii during substitution. The ‘‘chemical MnCo0.94Fe0.06Ge with those of Mn0.97Fe0.03CoGe alloy under 68
3 pressure’’ works like the applied external hydrostatic pressure to tune 100 Oe and 50 kOe, we can find that their martensitic starting 69
4 the phase stability [26]. In this work, the substitution of Fe (0.172 nm) transition temperatures were pushed upward about 10 K by a 70
5 for Co (0.167 nm) or Mn (0.179 nm) atoms can give rise to the local magnetic field of 50 kOe, which implies a magnetic-field-induced 71
6 lattice distortion in MnCo1 xFexGe and Mn1 xFexCoGe alloys, conse- martensitic transformation occurs. This also suggests that the 72
7 quently imposing a similar ‘‘chemical pressure’’ effect and modifying stability of martensitic phase can be enhanced with the aid of 73
8 the relative stability between the austenitic and martensitic phases. applied external magnetic field. 74
9 In nature, the ‘‘chemical pressure’’ corresponds to the local chemical Collecting the magnetic measurement data, the structural and 75
10 bonding in these alloys. In Fe-doped MnCoGe alloys, as demonstrated magnetic phase diagrams for MnCo1  xFexGe and Mn1  xFexCoGe 76
11 in Fe-doped MnNiGe alloys [18], the strengthened covalent bonding alloys are both shown in Fig. 3. By alloying isostructural MnFeGe 77
12 between the nearest-neighbor Fe and Ge atoms with respect to the or FeCoGe compounds into MnCoGe, two interesting results can 78
13 nearest-neighbor Mn/Co and Ge atoms increases the stability of be observed as follows: (i) In the present change range of 79
14 Ni2In-type austenite structure and consequently decreases the mar- composition, the Curie temperatures of austenite phase (T AC ) and 80
15 tensitic transformation temperature. martensite phase (T M C ) remain almost constants and they are 81
16 The thermomagnetization curves of MnCo0.94Fe0.06Ge and basically at 276 K and 355 K, respectively, which are consistent 82
17 Mn0.97Fe0.03CoGe alloys in a magnetic field up to 50 kOe are with those of MnCoGe alloy [9,11,17]. (ii) The martensitic trans- 83
18 shown in the insets of Fig. 2(a) and (b), respectively. Due to the formation temperature is lowered, spanning over T AC and T M C . 84
19 PM/FM-type martensitic transformation, the magnetization dif- These two achievements subsequently result in a temperature 85
20 ference values for the two alloys are about 51 and 58 emu/g, window with an interval width of about 80 K between T AC and T M C . 86
21 respectively, which is closed to that of Mn1  xCoGe [17]. This In this temperature window, the martensitic transformations 87
22 magnetization difference may give rise to the magnetic-field- with large magnetization difference can occur in Mn1  xFexCoGe 88
23 induced martensitic transformation and large magnetic-entropy (x r0.05) and MnCo1  xFexGe(x r0.06) alloys. 89
24 changes in the two series of alloys around room temperature. In what follows, the magnetoresponsive properties of MnCo1  x- 90
25 FexGe and Mn1  xFexCoGe alloys are presented. The isothermal 91
26 magnetization (M–H) curves of MnCo0.94Fe0.06Ge and Mn0.97 92
27 Fe0.03CoGe alloys were measured in the process of increasing and 93
28 decreasing magnetic field up to 50 kOe across the temperature 94
29 windows. These results are shown in Fig. 4(a) and (b), respectively. 95
30 For both alloys, their magnetizations show similar changes under 96
31 the applied magnetic field in the temperature windows. Above the 97
32 Tm, the magnetization linearly increases with the increase of 98
33 magnetic field, which indicates the PM ground state of Ni2In-type 99
34 structure. While below the Tm, the two alloys with TiNiSi-type 100
35 structure show typical FM behavior. Around the Tm, an S-shaped 101
36 metamagnetic transition with a hysteresis indicates the occurrence 102
37 of the remarkable magnetic-field-induced martensitic transforma- 103
38 tion from PM austenite to FM martensite. This is due to the larger 104
39 Zeeman energy in the FM martensite introduced by the applied 105
40 external magnetic field [3,4,17]. 106
41 Based on the isothermal magnetization curves, the magnetic- 107
42 entropy changes for MnCo0.94Fe0.06Ge and Mn0.97 Fe0.03CoGe 108
43 alloys were estimated by Maxwell relation [36], as shown below, 109
44 and shown in Fig. 5(a) and (b), respectively. 110
45 Z H  111
46 @M ðT,HÞ 112
Fig. 3. Structural and magnetic phase diagram of MnCo1 xFexGe (a) and Mn1 xFex- DSm ðT,HÞ ¼ dH ð1Þ
47 0 @T H 113
CoGe alloys (b).
48 114
49 115
50 116
51 117
52 118
53 119
54 120
55 121
56 122
57 123
58 124
59 125
60 126
61 127
62 128
63 129
64 130
65 Fig. 4. Isothermal magnetization curves of the MnCo0.94Fe0.06Ge (a) and Mn0.97Fe0.03CoGe (b) alloys at various temperatures across the martensitic transformation in a 131
66 magnetic field up to 50 kOe. 132

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j.jmmm.2012.12.001i
 4 G.J. Li et al. / Journal of Magnetism and Magnetic Materials ] (]]]]) ]]]–]]]

1 67
2 68
3 69
4 70
5 71
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9 75
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11 77
12 78
13 79
14 80
15 Fig. 5. Isothermal magnetic-entropy changes derived from isothermal magnetization curves of MnCo0.94Fe0.06Ge (a) and Mn0.97Fe0.03CoGe alloys (b). 81
16 82
17 83
18 84
19 For MnCo0.94Fe0.06Ge and Mn0.97 Fe0.03CoGe alloys, the largest Acknowledgment 85
20 magnetic-entropy changes (DSm) are about  27.5 and  10.6 J/ 86
21 Kg K under the applied magnetic field of 50 kOe around the This work is supported by the National Natural Science Founda- 87
22 martensitic transformation temperature, respectively. Appar- tion of China in Grant Nos. 11174352 and 50901043, National Basic 88
23 ently, compared with MnCo0.94Fe0.06Ge alloy, the Mn0.97Fe0.03- Research Program of China (973 Program, 2012CB619405). 89
24 CoGe alloy shows a relatively smaller magnetic-entropy change 90
25 in a wide temperature range. And the value of magnetic-entropy 91
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