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Register a new userCoexistence of ferro- and antiferromagnetic order in Mn-doped Ni$_2$MnGa
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Ni-Mn-Ga is interesting as a prototype of a magnetic shape-memory alloy showing large magnetic field induced strains. We present here results for the magnetic ordering of Mn-rich Ni-Mn-Ga alloys based on both experiments and theory. Experimental trends for the composition dependence of the magnetization are measured by a vibrating sample magnetometer (VSM) in magnetic fields of up to several tesla and at low temperatures. The saturation magnetization has a maximum near the stoichiometric composition and it decreases with increasing Mn content. This unexpected behaviour is interpreted via first-principles calculations within the density-functional theory. We show that extra Mn atoms are antiferromagnetically aligned to the other moments, which explains the dependence of the magnetization on composition. In addition, the effect of Mn doping on the stabilization of the structural phases and on the magnetic anisotropy energy is demonstrated.
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The different crystal structures of ferromagnetic Ni$_2$MnGa have been calculated using density functional theory (DFT) with special emphasis on the modulated structures 10M and 14M. These are important for understanding the stability of Ni$_2$MnGa martensites and their functionality as shape-memory materials. The modulated structures have been optimized in the calculations and their properties are discussed in relation to the structures without modulation. The occurrence of the modulated structures is related to the soft TA$_2$ phonon mode observed in Ni$_2$MnGa. The latter is related to the specific nesting behavior of the Fermi surface in Ni$_2$MnGa. Particular shapes of the modulated structures are stabilized by the covalent interaction mediated by the textit{p}-orbitals of Ga and textit{d}-orbitals of Ni. The role of this interaction becomes clear seen when considering the phonon dispersion spectrum of Ni$_2$MnGa, where some characteristic anomalies occur in the coupling of acoustical vibrational modes and the optical modes of Ni.
Ultraviolet-photoemission (UPS) measurements and supporting specific-heat, thermal-expansion, resistivity and magnetic-moment measurements are reported for the magnetic shape-memory alloy Ni$_2$MnGa over the temperature range $100K < T < 250K$. All measurements detect clear signatures of the premartensitic transition ($T_mathrm{PM}sim 247K$) and the martensitic transition ($T_mathrm{M} sim 196K$). Temperature-dependent UPS shows a dramatic depletion of states (pseudogap) at $T_mathrm{PM}$ located 0.3eV below the Fermi energy. First-principles electronic structure calculations show that the peak observed at 0.3eV in the UPS spectra for $T > T_mathrm{PM}$ is due to the Ni-d minority-spin electrons. Below $T_mathrm{M}$ this peak disappears, resulting in an enhanced density of states at energies around 0.8eV. This enhancement reflects Ni-d and Mn-d electronic contributions to the majority-spin density of states and is accompanied by significant reconstruction of the Fermi surface.
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.
The stability of the nonmodulated martensitic phase, the austenitic Fermi surface and the phonon dispersion relations for ferromagnetic Ni$_2$MnGa are studied using density functional theory. Exchange-correlation effects are considered with various degrees of precision, starting from the simplest local spin density approximation (LSDA), then adding corrections within the generalized gradient approximation (GGA) and finally, including the meta-GGA corrections within the strongly constrained and appropriately normed (SCAN). We discuss a simple procedure to reduce a possible overestimation of magnetization and underestimation of nesting vector in SCAN by parametrically decreasing self-interaction corrections.
Mn$_2$Au is an important antiferromagnetic (AF) material for spintronics applications. Due to its very high Neel temperature of about 1500 K, some of the basic properties are difficult to explore, such as the AF susceptibility and the exchange constants. Experimental determination of these properties is further complicated in thin films by unavoidable presence of uncompensated and quasiloose spins on antisites and at interfaces. Using x-ray magnetic circular dichroism (XMCD), we have measured the spin and orbital contribution to the susceptibility in the direction perpendicular to the in-plane magnetic moments of a Mn$_2$Au(001) film and in fields up to 8 T. By performing these measurements at a low temperature of 7 K and at room temperature, we were able to separate the loose spin contribution from the susceptibility of AF coupled spins. The value of the AF exchange constant obtained with this method for a 10 nm thick Mn$_2$Au(001) film equals to (24 $pm$ 5) meV.
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