First-Principles Study on the Regulation of Martensitic Transformation and Magnetic and Mechanical Properties of Ni-Mn-Ti Alloy via Co and Si Codoping

doi:10.11900/0412.1961.2024.00163

Acta Metall Sin

2026, Vol. 62

Issue (7): 1310-1322 DOI: 10.11900/0412.1961.2024.00163

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First-Principles Study on the Regulation of Martensitic Transformation and Magnetic and Mechanical Properties of Ni-Mn-Ti Alloy via Co and Si Codoping

LIU Dan¹^,², BAI Jing¹^,²^,³(

), ZHANG Yu¹, GUO Keliang¹, LIU Xin², ZUO Liang¹

1 Key Laboratory for Anisotropy and Texture of Materials Ministry of Education, Northeastern University, Shenyang 110819, China
2 School of Resources and Materials, Northeastern University at Qinhuangdao, Qinhuangdao 066004, China
3 Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province, Northeastern University at Qinhuangdao, Qinhuangdao 066004, China

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LIU Dan, BAI Jing, ZHANG Yu, GUO Keliang, LIU Xin, ZUO Liang. First-Principles Study on the Regulation of Martensitic Transformation and Magnetic and Mechanical Properties of Ni-Mn-Ti Alloy via Co and Si Codoping. Acta Metall Sin, 2026, 62(7): 1310-1322.

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Abstract

The novel all-d-metal Ni-Mn-Ti Heusler alloys have various application prospects in the field of functional materials owing to their excellent elastocaloric effect and mechanical properties. However, the noteworthy magnetocaloric effect in conventional Ni-Mn-based Heusler alloys is not reflected in Ni-Mn-Ti alloys because of the weak magnetism of both its austenitic parent and martensitic phases. To overcome this limitation, this study explored the effect of Co and Si codoping on the martensitic transformation and magnetic and mechanical properties of Ni-Mn-Ti alloys based on first-principles calculation. The codoping of Co and Si effectively modulated the comprehensive properties of the Ni-Mn-Ti alloys. Specifically, Si atoms tended to directly occupy the Mn sublattice, whereas Co atoms tended to directly occupy the Ni sublattice. Further, the codoped Co and Si atoms exhibited a tendency of aggregated distribution in the alloy. In the Ni-(Co)-Mn-(Si)-Ti alloy, the austenite transformed from an antiferromagnetic state to a ferromagnetic state with increasing Co content. In contrast, the martensite remained in an antiferromagnetic state. This resulted in the observation of a magneto-structural transition at specific compositions, which facilitated the realization of a significant magnetocaloric effect. Furthermore, the Si-doped Ni-Mn-Ti alloy significantly increased its strength while decreasing its toughness. Whereas, the Co and Si-codoped Ni-Mn-Ti alloy exhibited better overall mechanical properties than the ternary. Finally, the study also explored the density of electronic states (DOS) of the alloys to elucidate the physical mechanisms underlying the experimentally observed martensitic transformation and the changes in the magnetic properties.

Key words: Heusler alloy Ni-Mn-Ti first-principles calculation martensitic transformation magnetic property

Received: 15 May 2024

ZTFLH:

TG146

Fund: National Natural Science Foundation of China(51771044);Fundamental Research Funds for the Central Universities(N2223025);Foundation of Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province(22567627H)

Corresponding Authors: BAI Jing, professor, Tel: (0335)8066415, E-mail: baijing@neuq.edu.cn

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	LIU Dan
	BAI Jing
	ZHANG Yu
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	LIU Xin
	ZUO Liang

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https://www.ams.org.cn/EN/10.11900/0412.1961.2024.00163 OR https://www.ams.org.cn/EN/Y2026/V62/I7/1310

Fig.1 Illustration of the crystal structures of Ni-Mn-Ti alloy^[41]
(a) austenite (b) non-modulated (NM) martensite
(c) schematic of atomic spin directions in ferromagnetic and antiferromagnetic states (↑ and ↓ represent spin direc-tion of atomic magnetic moment)

Fig.2 Formation energy (E_f) of doped Si atom with different atomic occupations in Ni₂Mn_1.5Ti_0.5 alloy

Fig.3 Degree of aggregation of Co and Si atoms in Ni₂Mn_1.5Ti_0.5 alloy and E_f
(a) aggregated distribution
(b) discrete distribution
(c) E_f for different distribution states of Co and Si

Table 1 Equilibrium lattice constants of Ni_{2 -}_x Co _x Mn_{1.5 -}_y Si _y Ti_0.5 (0≤ x ≤ 0.625, y = 0.125 and 0.25) alloys

Fig.4 Volume change (ΔV) between austenite and martensite for Ni_{2 -}_x Co _x Mn_{1.5 -}_y Si _y Ti_0.5 (0 ≤ x ≤ 0.625, y = 0.125 and 0.25) alloys

Fig.5 Formation energies of austenite and martensite in Ni_{2 -}_x Co _x Mn_{1.5 -}_y Si _y Ti_0.5 (0≤ x ≤ 0.625) alloys (AFA—antiferromagnetic austenite, FM—ferro-magnetic martensite, AFM—antiferromagnetic martensite. Within the shaded region, ferromag-netic austenite has higher thermodynamic stability than antiferromagnetic austenite)
(a) y = 0.125 (Inset shows the locally enlarged view of the elliptical region)
(b) y = 0.25

Fig.6 Formation energy differences between austenite and martensite of Ni_{2 -}_x Co _x Mn_{1.5 -}_y Si _y Ti_0.5 (0≤ x ≤ 0.625) alloys (ΔE₁ and ΔE₂ represent the formation energy differences between austenite and martensite at y = 0.125 and 0.25, respectively)

Fig.7 Total magnetic moments of austenite (A) and martensite for Ni-Co-Mn-Si-Ti alloys (μ_B—Bohr magneton. The shaded region indicates the composition range where austenite transforms from an antiferromagnetic state to a ferromagnetic state)

Fig.8 Atomic magnetic moments of austenite for Ni_{2 -}_x Co _x Mn_1.25Si_0.25Ti_0.5 (0≤ x ≤ 0.625) alloys (The numbers 0-5 represent the contens of Co for 0, 0.125, 0.25, 0.375, 0.5, and 0.625, respectively; the same in Fig.9)
(a) Ni (b) Mn (c) Ti (d) Si (e) Co

Fig.9 Atomic magnetic moments of martensite for Ni_{2 -}_x Co _x Mn_1.25Si_0.25Ti_0.5 (0≤ x ≤ 0.625) alloys
(a) Ni (b) Mn (c) Ti (d) Si (e) Co

Table 2 Nearest Mn-Mn and Co-Mn distances of austenite and martensite for Ni_{2 -}_x Co _x Mn_1.25Si_0.25Ti_0.5 alloys

Fig.10 Total density of states (TDOS) of austenite and martensite for Ni₂Mn_{1.5 -}_y Si _y Ti_0.5 (0≤ y ≤ 0.25) alloys (The light blue shaded regions indicate the distribution of electronic density of states near Fermi level (E_F). Figs.10a2-c2 present zoom-in views of the shaded regions in Figs.10a1-c1, respectively)
(a1, a2) y = 0 (b1, b2) y = 0.125 (c1, c2) y = 0.25

Fig.11 Partial density of states (PDOS) of the austenite for Ni₂Mn_1.5Ti_0.5 and Ni₂Mn_1.25Si_0.25Ti_0.5 alloys

Table 3 Elastic properties for Ni-(Co)-Mn-(Si)-Ti alloys

Fig.12 TDOS of austenite and martensite for Ni_{2 -}_x Co _x -Mn_1.25Si_0.25Ti_0.5 (0≤ x ≤ 0.625) alloys

Fig.13 PDOS of the austenite and martensite for Ni_1.375Co_0.625Mn_1.25Si_0.25Ti_0.5 alloy

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