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First-principles calculation has become one of the most reliable approaches in predicting structural, electronic, and magnetic properties for material applications. Alloys in Heusler structures have also attracted much attention recently since they can be easily synthesized and provide interesting properties for future spintronic applications. In this work, we investigate a series of Fe-based Heusler compounds Fe3−xYxZ (x = 0, 1, 2, 3; Y= Cr, Mn, Co; Z= Al, Ga, Si) with L21- and XA-type structures using first-principles calculations based on density functional theory. According to formation energy calculations and mechanical property analysis, most of the studied Heusler compounds are thermodynamically stable and could be synthesized experimentally. The Co substitution leads Fe3−xCoxZ to a ferromagnetic ground state like Fe3Z with a strong magnetization ranging from 4 to 6 μB/f. u. While replacing Fe with Cr or Mn, the exchange coupling between Cr (Mn) and its neighboring atoms generally tend to be anti-parallel. Among the antiferromagnetic compounds, Mn3Al and Mn3Ga are antiferromagnetic half metal while Mn3Si is ferrimagnetic half metal. These rarely found type of half metals with low magnetic moment and high spin polarization at the Fermi level are important for low energy consumption spintronic applications. The estimated Curie temperatures for Mn3Al, and Mn3Si and Co2FeSi (XA) are in good agreement with previously theoretical values, while for Fe3Al and Fe3Si, they are in good agreement with previous experimental results. The good consistency in Curie temperature demonstrates high reliability of our predictions based on first-principles calculations. As for the topological property aspect, we predict Fe2CrAl and Fe2MnAl as the 3-dimensional Weyl semimetal. Furthermore, Fe2CrSi is predicted to be the magnetic nodal-line semimetal. Interestingly, our mechanical property analysis demonstrates that Co3Si and Fe2CoSi (L21) exhibit ultraelastic metal behavior, which is of high potential in advanced mechanical industry. This work suggests that Heusler compounds are excellent candidates for future spintronics as well as for high-performance ultraelastic metals.

Based on density functional theory, we studied the electronic, magnetic, and mechanical properties of Co3−xCrxAl (x = 0, 1, 2, 3) Heusler compounds with the generalized gradient approximation (GGA) for the exchange-correlation potential. In this study, we report two principal spin-related phenomena, namely, the anomalous Hall effect and current spin polarization of the Co3−xCrxAl Heusler compounds in the L21 crystal structure. Heusler compounds, both ideally and inversely ordered, were considered. We found that the calculated magnetic moment of Co3−xCrxAl decreased with an increase in the Cr concentration for both ideally and inversely ordered structures, except for Cr3Al. We also found that the spin polarization for all Co3−xCrxAl was larger than 50%, except for Cr2CoAl in the inverse structure. All the considered Heusler compounds were mechanically stable except for the regular Cr2CoAl. The Hall current spin polarization was also calculated. We found that Co2CrAl in the XA structure had the largest spin Hall conductivity of 370 (ℏS/e cm), and the spin polarization of the induced Hall current was high.

Using the frameworks of density functional theory, we found a new class of three-dimensional (3D) topological insulators (TIs) in Pb2BiBrO6 and Pb2SeTeO6 double perovskites. Our ab initio theoretical calculations show that Pb2BiBrO6 and Pb2SeTeO6 are Z2 nontrivial, and their bandgaps are 0.390 eV and 0.181 eV, respectively. The topology comes from two mechanisms. Firstly, the band inversion occurs at Γ point in the absence of spin-orbit interactions and secondly, the bandgap is induced by the SOC. This results in a larger bandgap for this new class of topological insulators than conventional TI. In Pb2BiBrO6 double perovskites, our slab calculations confirm that the topology-protected surface metallic bands come from the BiBrO4 surface which means that one can build a transport device using Pb2BiBrO6 double perovskites with a PbO layer as an outmost protection layer. The mechanical stabilities such as bulk, shear, Young’s moduli, Poisson’s and Pugh’s ratio, longitudinal, transverse, and average sound velocity, together with Debye temperature are also studied. Our results show that these Pb2AA’O6 (A = Sb and Bi; A’ = Br and I) and Pb2SeTeO6 are mechanically stable.

We performed first-principles calculations to study the adsorption of the CO molecules on both clean and Pd-doped ZnGa2O4(111) surfaces. The adsorption reaction and work function of the CO adsorption models were examined. The CO molecules on the clean and Pd-doped ZnGa2O4(111) surfaces exhibit maximum work function changes of −0.55 eV and −0.79 eV, respectively. The work function change of Pd-doped ZnGa2O4(111) for detecting CO is 1.43 times higher than that of the clean ZnGa2O4(111). In addition, the adsorption energy is also significantly reduced from −1.88 eV to −3.36 eV without and with Pd atoms, respectively. The results demonstrate ZnGa2O4-based gas sensors doped by palladium can improve the sensitivity of detecting CO molecules.

Nickel-based Ni2XAl (X ​= ​V, Cr, Mn, Fe, and Co) Heusler alloys for both L21 and L10 crystal structures are studied by using the density functional theory. The magnetization energy and formation energy of Ni2XAl Heusler alloys are calculated. We found that in the ideal L21 structure, ferromagnetic (FM) state is more stable than nonmagnetic (NM) and antiferromagnetic (AF) states, except Ni2VAl. The ground state for Ni2VAl is the nonmagnetic state. The so-called Bain paths method is applied to study the stability of Ni2XAl alloys under tetragonal distortion. We found that Ni2FeAl and Ni2CoAl are possible ferromagnetic shape materials (FSMs). We also found that Ni2CrAl and Ni2CoAl are energetically favorable in the antiferromagnetic state in the L10 structure. To study the stability between L21 and L10 crystal structure, we calculate the cohesive energy for comparison. We also calculate the elastic constants, bulk modulus, shear modulus, and universal elastic anisotropy to study the mechanical stability in L21 and L10 crystal structure. The spin polarization for the L21 structure is calculated whilst the largest spin polarization is smaller than 80%.

The work function variations of NO2 and H2S molecules on Pd-adsorbed ZnGa2O4(111) were calculated using first-principle calculations. For the bonding of a nitrogen atom from a single NO2 molecule to a Pd atom, the maximum work function change was +1.37 eV, and for the bonding of two NO2 molecules to a Pd atom, the maximum work function change was +2.37 eV. For H2S adsorption, the maximum work function change was reduced from −0.90 eV to −1.82 eV for bonding sulfur atoms from a single and two H2S molecules to a Pd atom, respectively. Thus, for both NO2 and H2S, the work function change increased with an increase in gas concentration, showing that Pd-decorated ZnGa2O4(111) is a suitable material in NO2/H2S gas detectors.

First-principles density functional theory was used to determine the surface band structures of CsPbBrxI3−x (x = 0, 1, 2, and 3) perovskites. The equilibrium lattice constants of CsPbBrxI3−x were obtained from the minimum of the total energy as a function of the iodine concentration. We discovered that the band gaps of CsPbBrxI3−x decreased monotonically under pressure. The phase change from a normal insulator to a topological insulator was found at approximately 2–4 GPa. The Pbp- and Brs-orbitals inverted at the R symmetric point with and without spin–orbit coupling. Nontrivial Z2 topological numbers were obtained, and the surface conduction bands were demonstrated theoretically using a 1 × 1 × 10 supercell. We ascertained that CsPbBr2I has the largest electric polarization 0.025 C/m2 under a compression strain of 10%. We also observed that in the normal insulation phase, the band gap increases with a small displacement of the central Pb atom in the z-direction, but in the topological insulator phase, the band gap decreases with the movement of the Pb atom in the z-direction. Additionally, in the supercell structure, CsPbBrxI3−x is a ferroelectric topological insulator because the Pb atom leaves its own equilibrium position.

Under the density functional theory framework, we have calculated the electronic and elastic properties of APoO3 (A = Be, Mg, Ca, Sr, Ba, and Ra) cubic perovskites. We found that CaPoO3, SrPoO3, BaPoO3, and RaPoO3 are topological insulators (TIs) with very large bandgaps of 0.861, 0.871, 0.820, and 0.810 eV, respectively. The nontrivial band topology together with the Z2 topological number of APoO3 perovskite are investigated. We also theoretically determine the three independent elastic constants C11, C12, and C44 of the APoO3 perovskite. The bulk modulus, shear modulus, Young’s modulus, Poisson’s ratio, and anisotropy factor are also calculated from the obtained elastic constants. We found that the Debye temperature for the APoO3 perovskite is around 330-370 K. In the bulk APoO3 perovskite, if the center Po atom is shifted 0.09Å away from the center, the induced electric polarization is quite large, being around 0.02 C/m2. In the surface band calculation, we found that both AO and PoO2 surfaces give rise to contributions to the conduction channel. If the Po atom moves both in-plane and out-of-plane, we show that both electric polarization and topologically protect surface conduction states exist in APoO3 perovskite, indicating that these oxide APoO3 perovskites are ferroelectric TIs and might be useful for spintronic applications.

We performed first-principles total-energy density functional calculations to study the reactions of NO2 and H2S molecules on Ga–Zn–O-terminated ZnGa2O4(111) surfaces. The adsorption reaction and work functions of eight NO2 and H2S adsorption models were examined. The bonding of the nitrogen atom from a single NO2 molecule to the Ga atom of the Ga–Zn–O-terminated ZnGa2O4(111) surfaces exhibited a maximum work function change of +0.97 eV. The bond joining the sulfur atom from a single H2S molecule and the Ga atom of Ga–Zn–O-terminated ZnGa2O4(111) surfaces exhibited a maximum work function change of −1.66 eV. Both results concur with previously reported experimental observations for ZnGa2O4-based gas sensors.

We present first-principles total-energy density functional calculations to study the intermediate band states of substitutional V2+, Cr2+, and Mn2+ ions in ZnTe alloys. The intermediate band states of substitutional transition metal defects of TM2+xZn1−xTe (TM = V, Cr, Mn) alloys are examined as their atomic, structural, and electronic analysis. Our findings show that the scissor-corrected transitions due to Jahn-Teller effects lead to the wavelengths 2530 nm and 2695 nm in the emission spectra. Our findings agree with previously reported experimental results.

The aim of this research is the study of hydrogen abstraction reactions and methyl adsorption reactions on the surfaces of (100), (110), and (111) oriented nitrogen-doped diamond through first-principles density-functional calculations. The three steps of the growth mechanism for diamond thin films are hydrogen abstraction from the diamond surface, methyl adsorption on the diamond surface, and hydrogen abstraction from the methylated diamond surface. The activation energies for hydrogen abstraction from the surface of nitrogen-undoped and nitrogen-doped diamond (111) films were −0.64 and −2.95 eV, respectively. The results revealed that nitrogen substitution was beneficial for hydrogen abstraction and the subsequent adsorption of methyl molecules on the diamond (111) surface. The adsorption energy for methyl molecules on the diamond surface was generated during the growth of (100)-, (110)-, and (111)-oriented diamond films. Compared with nitrogen-doped diamond (100) films, adsorption energies for methyl molecule adsorption were by 0.14 and 0.69 eV higher for diamond (111) and (110) films, respectively. Moreover, compared with methylated diamond (100), the activation energies for hydrogen abstraction were by 0.36 and 1.25 eV higher from the surfaces of diamond (111) and (110), respectively. Growth mechanism simulations confirmed that nitrogen-doped diamond (100) films were preferred, which was in agreement with the experimental and theoretical observations of diamond film growth.

Based on first principles density functional calculations of the intrinsic anomalous and spin Hall conductivities, we predict that the charge Hall current in Co-based full Heusler compounds Co _2 XZ (X = Cr and Mn; Z = Al, Si, Ga, Ge, In and Sn), except Co _2 CrGa, would be almost fully spin polarized, even though Co _2 MnAl, Co _2 MnGa, Co _2 MnIn and Co _2 MnSn do not have a half-metallic band structure. Furthermore, the ratio of the associated spin current to the charge Hall current is slightly larger than 1.0. This suggests that these Co-based Heusler compounds, especially Co _2 MnAl, Co _2 MnGa and Co _2 MnIn which are found to have large anomalous and spin Hall conductivities, might be called anomalous Hall half-metals and could have valuable applications in spintronics such as spin valves as well as magnetoresistive and spin-torque-driven nanodevices. These interesting findings are discussed in terms of the calculated electronic band structures, magnetic moments and also anomalous and spin Hall conductivities as a function of the Fermi level.