Phase Stability, Magnetic Properties, and Martensitic Transformation of Ni2−xMn1+x+ySn1−y Heusler Alloy with Excess Mn by First-Principles Calculations

doi:10.1007/s40195-022-01468-6

Abstract

Abstract:

The phase stability, magnetic properties, martensitic transformation, and electronic properties of the Ni₂₋_xMn₁₊_x₊_ySn₁₋_y system with excess Mn have been systematically investigated by the first-principles calculations. Results indicate that the excess Mn atoms will directly occupy the sublattices of Ni (Mn_Ni) or Sn (Mn_Sn). The formation energy (E_f) of the austenite has a relationship with the Mn content: E_f = 135.27(1 + x + y) − 293.01, that is, the phase stability of the austenite decreases gradually with the increase in Mn content. According to the results of the formation energy of austenite, there is an antiparallel arrangement of the magnetic moment between the excess and normal Mn atoms in the Ni₂₋_xMn₁₊_x₊_ySn₁₋_y (x = 0 or y = 0) system, while the magnetic moment direction of the normal Mn atoms arranges antiparallel to that of Mn_Ni atoms and parallel to that of Mn_Sn atoms in the Ni₂₋_xMn₁₊_x₊_ySn₁₋_y (x, y ≠ 0) system. The martensitic transformation occurs in some Ni₂₋_xMn₁₊_x₊_ySn₁₋_y (x, y ≠ 0) alloys with large magnetic moments of ferrimagnetic austenite. Besides, the valence electrons tend to distribute around the Ni or Mn_Ni atoms and mainly bond with the normal Mn atoms. The results of this work can lay a theoretical foundation for further development of the Ni₂₋_xMn₁₊_x₊_ySn₁₋_y system as the potential ferromagnetic shape memory alloys.

Key words: Ni-Mn-Sn, First-principles calculations, Phase stability, Magnetic property, Martensitic transformation

Yu Zhang, Jing Bai, Ziqi Guan, Xinzeng Liang, Yansong Li, Jianglong Gu, Yudong Zhang, Claude Esling, Xiang Zhao, Liang Zuo. Phase Stability, Magnetic Properties, and Martensitic Transformation of Ni₂₋_xMn₁₊_x₊_ySn₁₋_y Heusler Alloy with Excess Mn by First-Principles Calculations[J]. Acta Metallurgica Sinica (English Letters), 2023, 36(3): 513-528.

Figures/Tables 14

Fig. 1 Crystal structures of a L21-type austenite for Ni2MnSn alloy, b XA-type austenite for Mn2NiSn alloy, c L21-C, d L21-D austenite for Ni1.5Mn1.5Sn (x = 0.5, y = 0) alloy

Fig. 2 a-d Four possible configurations of Ni1.75Mn1.5Sn0.75 (x, y = 0.25) alloy and formation energy Ef. Among them, a, b, c, and d display direct (D), indirect (ID), and mixed (Mix1 and Mix 2) site occupation, respectively. e Schematic diagram of atomic spin directions in FM, FIM1, FIM2, and FIM3 states

Fig. 3 Ni1.75Mn1.75Sn0.5 (x = 0.25, y = 0.5) alloy based on possible configurations of the two structures: XA and L21 types, and formation energies of different magnetic states

Fig. 4 Ef of austenite with possible site occupation and magnetic configuration in Ni2?xMn1+x+ySn1?y systems: a x = 0; b y = 0; c x = 0.25; d x = 0.5; and e x = 0.75. Ef = 0 meV/atom is marked with a dashed line. f A diagram of relationship between formation energy and Mn content. Red line represents linear fit to data points

Fig. 5 Lattice parameters of austenite versus composition for Ni2?xMn1+x+ySn1?y systems in all possible magnetic states: a x = 0, b y = 0, c x = 0.25, d x = 0.5, e x = 0.75. Experimental and theoretical data are quoted from references [18,26,50,51].

Table 1 Interatomic distance of possible magnetic configurations (FM, FIM, FIM1, FIM2, and FIM3) for austenite of Ni2Mn1.5Sn0.5 (x = 0, y = 0.5), Ni1.5Mn1.5Sn (x = 0.5, y = 0), and Ni1.75Mn1.75Sn0.5 (x = 0.25, y = 0.5) alloys.

Interatomic distance (Å)	Ni₂Mn_1.5Sn_0.5		Ni_1.5Mn_1.5Sn		Ni_1.75Mn_1.75Sn_0.5
Interatomic distance (Å)	FM	FIM	FM	FIM	FIM1	FIM2	FIM3
Mn_Mn-Ni	2.521	2.525	2.623	2.635	2.518	2.522	2.515
Mn_Mn-Sn	2.975	2.964	3.028	3.043	2.994	2.998	2.952
Mn_Mn-Mn_Mn	4.207	4.192	4.309	4.307	4.167	4.214	4.176
Mn_Sn-Ni	2.521	2.525	-	-	2.539	2.524	2.513
Mn_Sn-Sn	4.207	4.192	-	-	4.292	4.249	4.167
Mn_Sn-Mn_Mn	2.975	2.964	-	-	3.139	2.993	2.952
Mn_Sn-Mn_Sn	5.950	5.929	-	-	5.939	5.958	5.911
Mn_Ni-Ni	-	-	3.028	3.043	2.972	2.981	2.956
Mn_Ni-Sn	-	-	2.639	2.689	2.683	2.739	2.657
Mn_Ni-Mn_Mn	-	-	2.644	2.631	2.523	2.474	2.480
Mn_Ni-Mn_Ni	-	-	3.028	3.043	-	-	-
Mn_Ni-Mn_Sn	-	-	-	-	2.598	2.477	2.452

Fig. 6 Variation of lattice parameter a of austenite with x-y of Ni2?xMn1+x+ySn1?y system (The same color means y is unchanged, and the same shape means x is unchanged.)

Fig. 7 Variation of total magnetic moment with x-y of the most stable austenitic configuration for each alloy composition in Ni2?xMn1+x+ySn1?y system

Fig. 8 Total and atomic magnetic moments for Ni2?xMn1+x+ySn1?y systems: a x = 0, b y = 0, c x = 0.25, d x = 0.5, e x = 0.75

Fig. 9 Variation of total energy (E-Ec/a=1) with tetragonality c/a ratio in Ni2?xMn1+x+ySn1?y systems: a x = 0, b y = 0, c x = 0.25, d x = 0.5, y = 0.25, 0.5 and x = 0.75, y = 0.25. Ec/a=1 is total energy of austenite with the most stable configuration of each alloy

Fig. 10 a Variation of total energy (E-Ec/a=1) with tetragonality c/a ratio in Ni1.75Mn1.75Sn0.5 (x = 0.25, y = 0.5) alloy with different site occupations and magnetic configurations (Ec/a=1 is the energy of austenite with D + FIM2 configuration), b crystal structures of L10 martensite for Ni2MnSn, c formation energy of austenite and NM martensite with most stable magnetic states for Ni2?xMn1+x+ySn1?y (x = 0, 0.25 and y = 0.5, 0.75) alloys

Fig. 11 Differential charge density map at 0.005 e/?3 isosurface for Mn-excess Ni2?xMn1+x+ySn1?y system

Table 2 Distance between different atoms of austenite in Ni2?xMn1+x+ySn1?y system

Interatomic distance (Å)	Ni-Mn_Mn-a	Ni-Mn_Mn-b	Mn_Ni-Sn	Mn_Ni-Mn_Mn-a	Mn_Ni-Mn_Mn-b
x = 0, y = 0.25	2.572	2.572	-	-	-
x = 0, y = 0.5	2.525	2.525	-	-	-
x = 0, y = 0.75	2.560	2.484	-	-	-
y = 0, x = 0.25	-	-	2.670	2.618	2.618
y = 0, x = 0.5	-	-	2.689	2.631	2.631
y = 0, x = 0.75	-	-	2.712	2.638	2.638
x = 0.25, y = 0.25	-	-	-	2.541	2.541
x = 0.25, y = 0.5	-	-	-	2.474	2.474
x = 0.25, y = 0.75	-	-	-	2.608	2.408
x = 0.5, y = 0.25	-	-	-	2.533	2.536
x = 0.5, y = 0.5	-	-	-	2.472	2.472
x = 0.5, y = 0.75	-	-	-	2.618	2.392
x = 0.75, y = 0.25	-	-	-	2.538	2.538
x = 0.75, y = 0.5	-	-	-	2.473	2.473
x = 0.75, y = 0.75	-	-	-	2.612	2.379

Fig. 12 DOS near (EF) of austenite with the lowest energy configuration in Ni2?xMn1+x+ySn1?y systems: a x = 0, b y = 0, c x = 0.25, d x = 0.5, e x = 0.75. Zero energy is regarded as EF and indicated by a vertical black dashed line. The enlarged view of the gray-white boxed area near EF is shown in the illustration

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Phase Stability, Magnetic Properties, and Martensitic Transformation of Ni₂₋_xMn₁₊_x₊_ySn₁₋_y Heusler Alloy with Excess Mn by First-Principles Calculations

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