Short-range chemical order (SRO) has been recently demonstrated to play a decisive role in modulating a wide range of physical properties in medium-entropy alloy (MEA) and high-entropy alloy (HEA). The enormous configurational space of these alloys implies multiple forms of SRO are likely to develop concurrently but such structural diversity has not been reported. Here we show, through extensive {\em ab initio}-based sampling study, that SiGeSn medium-entropy alloys spontaneously develop two distinct forms of SRO. Remarkably, the two types of SROs, which carry different energies, distinct degrees of local ordering, and dissimilar electronic structures, are found to co-exist in a wide range of compositions of SiGeSn alloys. The co-existence of two SROs is rationalized through their virtual degeneracy of thermodynamic stability, due to the subtle balance in the change of enthalpy and configurational entropy upon the transformation between the two SROs. Such co-existence of SROs thus suggests an inherent structural heterogeneity, a diffuse electronic structure, and a new route for band engineering in SiGeSn MEA. More generally, our finding indicates the possible ubiquity of the co-existence of multiple forms of SRO in a broad range of MEAs and HEAs, which has profound implications on their diverse physical properties.
High-entropy alloys (HEAs), which have been intensely studied due to their excellent mechanical properties, generally refer to alloys with multiple equimolar or nearly equimolar elements. According to this definition, Si-Ge-Sn alloys with equal or comparable concentrations of the three Group IV elements belong to the category of HEAs. As a result, the equimolar elements of Si-Ge-Sn alloys likely cause their atomic structures to exhibit the same core effects of metallic HEAs such as lattice distortion. Here we apply density functional theory (DFT) calculations to show that the SiGeSn HEA indeed…
We provide strong numerical evidence for a hidden multihyperuniform long-range order (MHLRO) in SiGeSn medium-entropy alloys (MEAs), in which the normalized infinite-wavelength composition fluctuations for all three atomic species are completely suppressed as in a perfect crystalline state. We show this MHLRO naturally leads to the emergence of short-range order (SRO) recently discovered in MEAs, which results in stable lower-energy states compared to alloy models with random or special quasi-random structures (SQSs) possessing no atomic SROs. The MHLRO MEAs approximately realize the Vegard's …
The mechanism of spontaneous exchange bias (SEB) and the dominant factor of its blocking temperature are still unclear in Heusler alloys. Here, the related investigations are performed in Mn2Ni1.5Al0.5 Heusler alloys with SEB. The results of both magnetic measurements and first-principles calculations confirmed that spin frustrated and unfrustrated antiferromagnetic (AFM) states coexist there and they have different magnetic anisotropies, which are essential for SEB. Based on a series of measurement strategies, we demonstrate that the frustrated AFM state undergoes a first-order magnetic trans…
Sn-containing Si and Ge alloys belong to an emerging family of semiconductors with the potential to impact group IV semiconductor devices. Indeed, the ability to independently engineer both lattice parameter and band gap holds the premise to develop enhanced or novel photonic, optoelectronic, and electronic devices. With this perspective, we present detailed investigations of the influence of Ge1-y-xSixSny layers on the optical properties of Si- and Ge-based heterostructures and nanowires. We found that adding a thin Ge1-x-ySixSny capping layer on Si or Ge greatly enhances light absorption esp…
First order ferromagnetic (FM) to antiferromagnetic (AFM) phase transition in doped-CeFe$_2$ alloys is studied with micro-Hall probe technique. Clear visual evidence of magnetic phase-coexistence on micrometer scales and the evolution of this phase-coexistence as a function of temperature, magnetic field and time across the first order FM-AFM transition is presented. Such phase-coexistence and metastability arise as natural consequence of an intrinsic disorder-influenced first order transition. Generality of this phenomena involving other classes of materials is discussed.
Using first-principles calculations based on density functional theory, we have studied the mechanical, electronic, and magnetic properties of Heusler alloys, namely, Ni$_{2}BC$ and Co$_{2}BC$ ($B$ = Sc, Ti, V, Cr and Mn as well as Y, Zr, Nb, Mo and Tc; $C$ = Ga and Sn). On the basis of electronic structure (density of states) and mechanical properties (tetragonal shear constant), as well as magnetic interactions (Heisenberg exchange coupling parameters), we probe the properties of these materials in detail. We calculate the formation energy of these alloys in the (face-centered) cubic austeni…
The coexistence of two phases within a particle requires an interface with a significant capillary energy. We show that this entails changes in the nature of alloy phase equilibria at small size. Most notably, the eutectic points in alloy phase diagrams degenerate into intervals of composition where the alloy melts discontinuously.
Current theoretical studies on structural and magnetic properties of functional Ni-Mn-Z (Z = Ga, In, Sn) Heusler alloys address the origin of the structural transition from the austenite to martensite, and also address the dominant contribution to the latent heat associated with this magneto-structural transition. This should help understand the origin of kinetic arrest of 1st order magnetic transitions.
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…
We report on a novel material, namely two-dimensional (2D) V$_{1-x}$Pt$_x$Se$_2$ alloy, exhibiting simultaneously ferromagnetic order and Rashba spin-orbit coupling. While ferromagnetism is absent in 1T-VSe$_2$ due to the competition with the charge density wave phase, we demonstrate theoretically and experimentally that the substitution of vanadium by platinum in VSe$_2$ (10-50 %) to form an homogeneous 2D alloy restores ferromagnetic order with Curie temperatures of 6 K for 5 monolayers and 25 K for one monolayer of V$_{0.65}$Pt$_{0.35}$Se$_2$. Moreover, the presence of platinum atoms gives …
The random substitutional solid solution between the antiferromagnetic (AFM) full-Heusler alloy Ru$_2$MnSn and the ferromagnetic (FM) full-Heusler alloy Ru$_2$FeSn provides a rare opportunity to study FM-AFM phase competition in a near-lattice-matched, cubic system, with full solubility. At intermediate $x$ in Ru$_2$Mn$_{1-x}$Fe$_x$Sn this system displays suppressed magnetic ordering temperatures, spatially coexisting FM and AFM order, and strong coercivity enhancement, despite rigorous chemical homogeneity. Here, we construct the most detailed temperature- and $x$-dependent understanding of t…
Whereas exceptional mechanical and radiation performances have been found in the emergent medium- and high-entropy alloys (MEAs and HEAs), the importance of their complex atomic environment, reflecting diversity in atomic size and chemistry, to defect transport has been largely unexplored at the atomic level. Here we adopt a local structure approach based on the atomic pair distribution function measurements in combination with density functional theory calculations to investigate a series of body-centered cubic (BCC) MEAs and HEAs. Our results demonstrate that all alloys exhibit local lattice…
Multi-principal-element alloys, including high-entropy alloys, experience segregation or partially-ordering as they are cooled to lower temperatures. For Ti$_{0.25}$CrFeNiAl$_{x}$, experiments suggest a partially-ordered B2 phase, whereas CALculation of PHAse Diagrams (CALPHAD) predicts a region of L2$_{1}$+B2 coexistence. We employ first-principles density-functional theory (DFT) based electronic-structure approach to assess stability of phases of alloys with arbitrary compositions and Bravais lattices (A1/A2/A3). In addition, DFT-based linear-response theory has been utilized to predict Warr…
We present results of dc magnetisation study showing that the low temperature antiferromagnetic state in various CeFe$_2$-based pseudobinary alloys can be transformed into ferromagnetic state through a magnetic field induced phase transition. We highlight the presence of hysteresis and phase coexistence across this metamagnetic transition and argue that the observed phase transition is of first order in nature.
Weyl semimetals are playing a major role in condensed matter physics due to exotic topological properties, and their coexistence with ferromagnetism may lead to enhanced spin-related phenomena. Here, the inverse spin Hall effect (ISHE) in the ferromagnetic Weyl-semimetal Heusler alloy Co$_2$MnGa was investigated at room temperature by means of electrical spin injection in lateral spin valve structures. Spin transport properties such as spin polarization and spin diffusion length in this material were precisely extracted in order to estimate the spin Hall angle $θ_{\textrm{SH}}$, which was foun…
Topological interpretations of phonons facilitate a new platform for novel concepts in phonon physics. Though there are ubiquitous set of reports on topological electronic excitations, the same for phonons are extremely limited. Here, we propose a new candidate material, KMgBO 3 , which showcase the co-existence of several multifold and multidimensional topological phonon excitations, which are protected by spatial and non-spatial symmetries. This includes zero dimensional double, triple and quadratic Weyl phonon nodes, one dimensional nodal line/loop and two dimensional doubly degenerate noda…
We present small angle neutron scattering (SANS) data collected on polycrystalline Ni$_{1-x}$V$_x$ samples with $x\geq0.10$ with confirmed random atomic distribution. We aim to determine the relevant length scales of magnetic correlations in ferromagnetic samples with low critical temperatures $T_c$ that show signs of magnetic inhomogeneities in magnetization and $μ$SR data. The SANS study reveals signatures of long-range order and coexistence of short-range magnetic correlations in this randomly disordered ferromagnetic alloy. We show the advantages of a polarization analysis in identifying t…
We present a lattice model to study the equilibrium phase diagram of ordered alloys with one magnetic component that exhibits a low temperature phase separation between paramagnetic and ferromagnetic phases. The model is constructed from the experimental facts observed in Cu$_{3-x}$AlMn$_{x}$ and it includes coupling between configurational and magnetic degrees of freedom which are appropriated for reproducing the low temperature miscibility gap. The essential ingredient for the occurrence of such a coexistence region is the development of ferromagnetic order induced by the long-range atomic o…
We discuss the phenomenology of phase transitions studied with two control variables. Such measurements have become routine with magnetic field and temperature being varied for 1st order magnetic transitions with an ease not conceivable with pressure and temperature. Similar ease may be possible with electric field as the second control variable, as in current studies on multiferroics. We develop this phenomenology for broad 1st order transitions that occur over a range of the control variable, as is common in substitutional alloys with inherent quenched disorder, including the possibility of …
A continuous surface wetting transition, pinned to a solid/liquid/liquid/vapor tetra coexistence point, is studied by x-ray reflectivity in liquid Ga-Bi binary alloys. The short-range surface potential is determined from the measured temperature evolution of the wetting film. The thermal fluctuations are shown to be insufficient to induce a noticeable breakdown of mean-field behavior, expected in short-range-interacting systems due to their $d_u=3$ upper critical dimensionality.
Effect of substitution La by Mg on electrochemical and electronic properties in La$_{2-x}$Mg$_x$Ni$_7$ alloys: a combined experimental and ab initio studies
