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Precursor of the premartensite in Ni2MnGa magnetic shape memory alloy: A pair distribution function study

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 Publication date 2021
  fields Physics
and research's language is English




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Precursor phenomena observed prior to the martensite phase transition plays a critical role towards the understanding of important technological properties of shape memory and magnetic shape memory alloys (MSMAs). The premartensite (PM) phase, considered as the precursor state of the martensite is proven to be a thermodynamically stable phase recently (Nature Commun. 8, 1006 (2017)), necessitates a critical investigation of precursor effects in these materials. We present here an evidence for the existence of a precursor state of the PM phase in Ni2MnGa MSMA using high energy synchrotron pair distribution function (PDF) study. The precursor state embedded within the austenite matrix in the short-range ordered (SRO) regime starting from far above the actual PM phase transition. The presence of such SRO precursor states of the PM phase produces strains which couple with the ferromagnetic (FM) order parameter around TC leading to first order character of the paramagnetic to FM phase transition.



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The premartensite phase of shape memory and magnetic shape memory alloys (MSMAs) is believed to be a precursor state of the martensite phase with preserved austenite phase symmetry. The thermodynamic stability of the premartensite phase and its relation to the martensitic phase is still an unresolved issue, even though it is critical to the understanding of the functional properties of MSMAs. We present here unambiguous evidence for macroscopic symmetry breaking leading to robust Bain distortion in the premartensite phase of 10% Pt substituted Ni2MnGa. We show that the robust Bain distorted premartensite (T2) phase results from another premartensite (T1) phase with preserved cubic-like symmetry through an isostructural phase transition. The T2 phase finally transforms to the martensite phase with additional Bain distortion on further cooling. Our results demonstrate that the premartensite phase should not be considered as a precursor state with the preserved symmetry of the cubic austenite phase.
An inelastic neutron scattering study of the lattice dynamics of the martensite phase of the ferromagnetic shape memory alloy, Ni2MnGa, reveals the presence of well-defined phasons associated with the charge density wave (CDW) resulting from Fermi surface (FS) nesting. The velocity and the temperature dependence of the phason are measured as well as the anomalous [110]-TA2 phonon.
The origin of incommensurate structural modulation in Ni-Mn based Heusler type magnetic shape memory alloys (MSMAs) is still an unresolved issue inspite of intense focus on this due to its role in the magnetic field induced ultra-high strains. In the archetypal MSMA Ni2MnGa, the observation of non-uniform displacement of atoms from their mean positions in the modulated martensite phase, premartensite phase and charge density wave as well as the presence of phason broadening of satellite peaks have been taken in support of the electronic instability model linked with a soft acoustic phonon. We present here results of a combined high resolution synchrotron x-ray powder diffraction (SXRPD) and neutron powder diffraction (NPD) study on Ni2Mn1.4In0.6 using (3+1)D superspace group approach, which reveal not only uniform atomic displacements in the modulated structure of the martensite phase with physically acceptable ordered magnetic moments in the antiferromagnetic phase at low temperatures but also the absence of any premartensite phase and phason broadening of the satellite peaks. Our HRTEM studies and first principles calculations of the ground state also support uniform atomic displacements predicted by powder diffraction studies. All these observations suggest that the structural modulation in the martensite phase of Ni2Mn1.4In0.6 MSMA can be explained in terms of the adaptive phase model. The present study underlines the importance of superspace group analysis using complimentary SXRPD and NPD in understanding the physics of the origin of modulation as well as the magnetic and the modulated ground states of the Heusler type MSMAs. Our work also highlights the fact that the mechanism responsible for the origin of modulated structure in different Ni-Mn based MSMAs may not be universal and it must be investigated thoroughly in different alloy compositions.
We predict the existence of a new ferromagnetic shape memory alloy Ga_2MnNi using density functional theory. The martensitic start temperature (T_M) is found to be approximately proportional to the stabilization energy of the martensitic phase (deltaE_tot) for different shape memory alloys. Experimental studies performed to verify the theoretical results show that Ga_2MnNi is ferromagnetic at room temperature and the T_M and T_C are 780K and 330K, respectively. Both from theory and experiment, the martensitic transition is found to be volume conserving that is indicative of shape memory behavior.
Magnetic shape memory Heusler alloys are multiferroics stabilized by the correlations between electronic, magnetic and structural order. To study these correlations we use time resolved x-ray diffraction and magneto-optical Kerr effect experiments to measure the laser induced dynamics in a Heusler alloy Ni$_2$MnGa film and reveal a set of timescales intrinsic to the system. We observe a coherent phonon which we identify as the amplitudon of the modulated structure and an ultrafast phase transition leading to a quenching of the incommensurate modulation within 300~fs with a recovery time of a few ps. The thermally driven martensitic transition to the high temperature cubic phase proceeds via nucleation within a few ps and domain growth limited by the speed of sound. The demagnetization time is 320~fs, which is comparable to the quenching of the structural modulation.
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