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Curie Temperature and Density of States at the Fermi Level for Al Cu

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Curie Temperature and Density of States at the Fermi Level for Al Cu Vol. 126 (2014) ACTA PHYSICA POLONICA A No. 2 Proceedings of the 12th International Conference on Quasicrystals (ICQ12) Curie Temperature and Density of States at the Fermi Level for AlCuFe Phases: β-Solid State SolutionApproximantsIcosahedral Quasicrystals E.V. Shalaevaa;b, A.F. Prekulc, N.I. Shchegolikhinac and N.I. Medvedevaa aInstitute of Solid State Chemistry, Ural Branch RAS, Ekaterinburg, Russia bUral Federal University, Ekaterinburg, Russia cInstitute of Metal Physics, Ural Branch RAS, Ekaterinburg, Russia A consistent reduction in the absolute value of the negative paramagnetic Curie temperature was found in a series of AlCuFe phases: β(CsCl)-solid state solution, noncanonical approximant (η-AlCu(Fe) phase), rational approximants (P1+P2-pentagonal phases) and icosahedral quasicrystal. For these AlCuFe phases, the decrease in the Curie temperature correlates with a reduction of the density of states at the Fermi level which was estimated from the low-temperature heat capacity measurements and rst-principles calculations. The observed correlation was related to the antiferromagnetic indirect exchange interaction (RudermanKittelKasuyaYosida interaction) between the localized magnetic moments on Fe induced by the intrinsic structural defects in the AlCuFe phases. The weakening of Fe 3dAl s; p hybridization owing to the intrinsic structural defects such as vacancies, antisite defects and distortions of coordination polyhedrons is suggested to be the main mechanism of appearance of localized magnetic moments on Fe atoms. DOI: 10.12693/APhysPolA.126.572 PACS: 75.20.g, 71.23.Ft, 71.20.b, 61.66.Dk 1. Introduction structure decays, the diamagnetic contribution decreases Since the discovery of 3D-aperiodic quasicrystals and [9, 14]. At once, the CurieWeiss contribution rises ow- crystalline approximants in the AlCuFe system [15], ing to increased concentration of Fe ions with local mag- much attention has been devoted to the investigation netic moments [14]. Breaking of strong covalent inter- of their physical properties [611]. Structurally per- action is believed to reduce the diamagnetic term [18] and can be the cause of the magnetic state of Fe in the fect icosahedral (ι) quasicrystal and its canonical ap- proximants have been found to exhibit peculiar phys- AlCuFe icosahedral phase. A similar mechanism of ap- ical properties such as high electrical resistivity [6, 7], pearance of large local magnetic moments on Fe atoms diamagnetism [8, 9] and a pseudogap at the Fermi level was established by using rst-principles calculations for [10, 11]. These specic physical properties are consid- various structural defects in noncanonical approximants ered to be due to a complex cluster local structure with (β(CsCl)AlCuFe solid solution and β-based ordered -AlCu(Fe) phase) [19, 20]. Therefore, the study of Al s; pTm 3d covalent binding [7, 12, 13]. The β(CsCl) η Al(Cu,Fe) solid solution and non-canonical approximants the CurieWeiss paramagnetic contribution is of interest for characterization of the interaction between the local of the AlCuFe icosahedral phase such as β-based or- dered phases, for which the complex cluster local struc- magnetic moments induced by structural defects of the ture features are not pronounced, show neither anoma- AlCuFe ι-phase and its approximants. lous properties nor a pseudogap eect [1416]. At the The CurieWeiss term is known to have a negative same time, it is of special interest to investigate the Curie temperature for the AlCuFe icosahedral phase physical properties, whose behavior is directly aected [14, 17], which is indicative of an antiferromagnetic in- by structural defects, and to understand how these prop- teraction between localized magnetic moments. How- erties vary in the series of AlCuFe phases from β-solid ever, the type of the interaction between localized mo- solution to icosahedral phase. This is important for eluci- ments is still unclear for the AlCuFe approximants. It dation of electron and magnetic properties of defects and is even more intriguing to nd out whether the AlCuFe for characterization of chemical binding for these defects approximants exhibit an antiferromagnetic interaction in quasicrystal-forming systems. between the localized magnetic moments and how the At rst, it was supposed that the contribution of characteristics of this interaction, the Curie temperature low-temperature CurieWeiss paramagnetism character- in particular, can be varied in the series of AlCuFe izing the interaction between localized magnetic mo- phases noncanonical approximant, rational approx- ments points to magnetic impurities in the AlCuFe imant, icosahedral quasicrystal, where the density of icosahedral phase. However, weak CurieWeiss para- states at the Fermi level decreases. magnetism was later shown to be an intrinsic property In this work we study the parameters of the Curie of the AlCuFe icosahedral phase with superior qua- Weiss paramagnetic contribution, such as the Curie sicrystallinity [17]. As perfection of the icosahedral phase temperature and Curie constant, in the following se- (572) Curie Temperature and Density of States at the Fermi Level . 573 ries of AlCuFe phases: β(CsCl)-solid state solution, melting the ingots were turned over. At all stages, the noncanonical approximant (η-AlCu(Fe) phase), rational weight of the ingots was controlled. Then 50100 mg of approximants (P1+P2-pentagonal phases), icosahedral the as-prepared material were melted in suspended drop −3 quasicrystal. For this series, in which the eects of the under helium atmosphere (PHe ≈ 10 mm Hg). The complex cluster local structure become more pronounced melt was quenched upon falling of the drop on a disc sur- from β-solid state solution to icosahedral quasicrystal, face cooled with water. The alloys of the compositions we estimate the density of states at the Fermi level (NF) Al50Cu33Fe17, Al50Cu44Fe6, Al62Cu25:7Fe12:3 were pre- using low-temperature heat capacity measurements and pared. Isothermal treatment was performed in He atmo- rst-principles calculations. We show that the density of sphere to prepare the desired phase composition. Local states at the Fermi level lowers and the absolute values of chemical analysis was carried out by electron probe X-ray the negative Curie temperature fall consistently in these microanalysis using a JSM9600LV instrument. The local series of AlCuFe phases. We consider the observed cor- composition was analyzed on the basis of JSM9600LV relations in terms of the antiferromagnetic Ruderman references using Phi-Pho-Z software. KittelKasuyaYosida (RKKY) interaction between the local magnetic moments on Fe induced by intrinsic struc- tural defects. The structure of the annealed AlCuFe alloys was 2. Experimental details investigated by transmission electron microscopy using 2.1. Preparation and structural characterization a JEM-200CX facility and by X-ray method. The ob- of AlCuFe alloys tained electron-diraction patterns conrmed the for- The AlCuFe alloys were melted from components mation of the following series of phases: β(CsCl) with purity not less than 99.9% in an arc furnace under Al50Cu33Fe17, η-Al50Cu44Fe6, P1+P2-Al62Cu25:7Fe12:3, very-high-purity helium atmosphere. For homogeniza- ι-Al62Cu25:7Fe12:3. Typical electron-diraction patterns tion, the ingots were re-melted ve times; each time upon are shown in Fig. 1. Fig. 1. Electron-diraction patterns of the AlCuFe alloys with structure: (a) β-solid solution, [111] zone axis; (b) β-based ordered η-AlCu(Fe), domains with orientations type of [301]η and [011]η; (c) P1+P2 pentagonal phases, (d) icosahedral phase, orientation along twofold symmetry axis [0/0 0/2 0/0]. The periodic reections of P1 and P2 phases are shown by the white and grey arrows. 2.2. Measurements of physical properties and Ernzerhof (PBE) for the exchange-correlation poten- tial [23]. We used a kinetic energy cut-o of 350 eV for the The magnetic susceptibility was measured in the tem- expansion of valence orbitals in plane waves and a 5×5×5 perature interval 2400 K in a magnetic eld of 50 kOe MonkhorstPack k-point mesh, which were sucient for using a Quantum Design MPMS-XL5 magnetometer. total energy calculations with convergence better than The heat capacity measurements were performed by the 0.01 eV/atom. All the calculations were spin-polarized. relaxation method on a Quantum Design PPMS device The β-alloys of the composition Al Cu Fe and in the temperature range 1.8400 K. 50 31:3 18:7 Al50Cu43:8Fe6:2 were simulated with a supercell contain- 2.3. Calculation technique and structural models ing eight unit cells (16 atoms) of the FeAl-phase with a CsCl-type structure (S.G. Pm3m). The η-alloy of the The electronic structure of the β(CsCl)AlCu(Fe) solid composition Al50Cu45Fe5 was simulated with one unit solution and β-based ordered η-AlCu(Fe) phase was stud- cell (20 atoms) of the low-temperature modication of η2- ied using the projector augmented waves (PAW) method AlCu phase (S.G. I12=m1) [24]. Copper and iron atoms as implemented in the Vienna ab initio simulation pack- were located in the same sublattice. age (VASP) [21, 22] and the generalized gradient approx- imation (GGA) technique introduced by Perdew, Burke, 574 E.V. Shalaeva et al. 3. Results and discussion the behavior of the CurieWeiss paramagnetic param- eters for the above series of AlCuFe phases. It can Figure 2 shows the temperature function of mag- be seen (Table) that the CurieWeiss terms of all the netic susceptibilities χ for the AlCuFe alloys having phases have negative values of the Curie temperature, the structures of β(CsCl)-solid solution, η-ordered phase and the absolute values of the Curie temperature fall (noncanonical approximant), P1+P2-pentagonal phases consistently in this series from β-solid state solution to (canonical rational approximants) and icosahedral phase. icosahedral phase. The reduction of the absolute values The magnetic susceptibility function for the AlCuFe of negative Curie temperatures means that the antifer- alloys is known to consist of three contributions: the romagnetic interactions of local magnetic moments de- low-temperature CurieWeiss paramagnetic term ( ), χCW crease in the series of AlCuFe phases [25].
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