Ex 3

INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z=
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Al, Ge, Sb): A FIRST PRINCIPLE STUDY
Said Mohd Al Azar Supervisor: Prof. Dr. Jamil Khalifeh Co-supervisor: Dr. Bothina Hamad
August 5, 2011
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Outline
1 2 3 4 5
Overview Half-Metallicity Heusler Alloy Density Functional Theory (DFT) Full-Potential Linearized Augmented Plane-wave (FP-LAPW) Method Formalism WIEN2k Package Results and Discussion Stoichiometric Fe3x Mnx Z (Z= Al, Ge, Sb) Systems Non-Stoichiometric Fe3x Mnx Z (Z= Al, Ge, Sb) Systems Conclution and Open issue
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Overview
The Goal The goal of this work is to study, with ab initio accuracy over a wide concentration range, the eect of the main-group elements on the electronic and magnetic structures of bulk Fe3x Mnx Z(Z=Al, Ge, Sb) alloys. Manganese concentration and the main-group elements (Z) play an important role in the electronic and magnetic structures of these alloys. Furthermore, the half-metallic behavior is investigated.
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Overview
The Goal The goal of this work is to study, with ab initio accuracy over a wide concentration range, the eect of the main-group elements on the electronic and magnetic structures of bulk Fe3x Mnx Z(Z=Al, Ge, Sb) alloys. Manganese concentration and the main-group elements (Z) play an important role in the electronic and magnetic structures of these alloys. Furthermore, the half-metallic behavior is investigated. Motivation 1 Fe MnZ and Mn FeZ have been proposed theoretically to 2 2 show half-metallicity.
2 3
An upsurge of interest in the ordered compound containing Fe. Perspectives to use them in spintronics applications as spin-injection devices , spin-lters , tunnel junctions , GMR CMR and TMR devices.
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Half-Metallicity
What is Half-metallicity?
Denition A half-metal is any materials that acts as a conductor to electrons of one spin orientation, but as an insulator or semiconductor to those of the opposite orientation. Such materials exhibit nearly fully spin polarized conduction electrons.
What is Half-metallicity?
Denition A half-metal is any materials that acts as a conductor to electrons of one spin orientation, but as an insulator or semiconductor to those of the opposite orientation. Such materials exhibit nearly fully spin polarized conduction electrons. Half-Metallicity Rules Obey Slater-Pauling rule (integer total magnetic moment). Kbler rule Mn atom have a high, localized magnetic moment. u Normally possible for alloys, typically 2 - 4 components.
Classifecation of half-metals after Coey and Venkatesan (2002)
Type IA IB IIA IIB IIIA IIIB IVA IVB VA VB
DOS half-metal half-metal half-metal half-metal metal metal semimetal semimetal semiconductor semiconductor
Conductivity metallic metallic nonmetallic nonmetallic metallic metallic metallic metallic semiconducting semiconducting
Spin up electrons at EF itinerant none localized none itinerant localized itinerant localized few, itinerant none
Spin down electrons at EF none itinerant none localized localized itinerant localized itinerant none few, itinerant
Example CrO2 or NiMnSb Mn2 VAl Fe3 O4 (La0.7 Sr0.3 )MnO3
Tl2 Mn2 O7 GaAs
Example Two types of Heusler Some oxides Manganites Double perovskites
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Heusler Alloy
Full and Half Heusler alloys structure and their Wycko positions.
Wycko positions For X2 YZ (AlCu2 Mn-type) 1 1 1 X at 8c ( 4 , 4 , 4 ) Y and Z atoms at 1 1 4a (0,0,0) and 4b ( 2 , 1 , 2 ) 2 For XYZ 1 1 X at 4a ( 4 , 1 , 4 ) 4 Y and Z atoms at 4b (0,0,0) and 4c ( 1 , 1 , 1 ) 2 2 2
11111 00000 11111 00000 11111 00000 11111 00000 11111 00000 11111 00000 11111 00000 11111 00000
Full-Heusler X2YZ [L21]

X X
1111 0000 1111 0000 1111 0000 1111 0000 1111 0000
Y Z
11111 00000 11111 00000 11111 00000 11111 00000 1111 0000 1111 0000 1111 0000 1111 0000
Half-Heusler XYZ [C1b]

X Void
11111 00000 11111 00000 11111 00000 11111 00000
Y Z
For X2 YZ (CuHg2 Ti-type) 1 X at 4a (0,0,0) and 4c ( 4 , 1 , 1 ) 4 4 1 Y and Z atoms at 4b ( 2 , 1 , 1 ) and 2 2 3 4d ( 4 , 3 , 3 ) 4 4
Heusler alloys that can be formed by combination of dierent elements in periodic table
Hybridization and the origin of band gap and spin gap in full-Heusler alloys
C.B Eg ES V.B
EF
d d hybridization Determined by the X-X interaction only ( t1u - eu splitting)
The Slater-Pauling behavior of Heusler alloys
HalfHeusler Alloys
6 5 4 7
FullHeusler Alloys
6
Total spin moment: Mt ()
NiMnTe CoFeSb RhMnSb NiFeSb
Total spin moment: Mt ()
NiMnSb PdMnSb PtMnSb
NiMnSe
5 4 3 2 1 0 1 2 3
Co2CrAl Fe2MnSi Ru2MnSi Ru2MnGe Ru2MnSn
Co2MnSi Co2MnGe Co2MnSn
Co2MnAs Rh2MnIn Rh2MnTl
Co2MnSb Co2FeSi Co2FeAl Ni2MnAl
3 2 1 0 1
Co2VAl Fe2MnAl
=Z
=Z
CoTiSb
Mn2VAl
22 23 24 25 26 27
16
17
18
19
20
21
22
23
24
25
20
21
FeMnSb CoCrSb NiVSb CoVSb
CoMnSb IrMnSb NiCrSb
Co2TiSn
Rh2MnGe Rh2MnSn Rh2MnPb Co2MnAl Co2MnGa Rh2MnAl Rh2MnGa Ru2MnSb
Fe2CrAl Co2TiAl Fe2VAl Mn2VGe
28
29
30
31
32
Number of valence electrons: Zt
Number of valence electrons: Zt
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Density Functional Theory (DFT)
The Hohenberg-Kohn Theorems

Theorem (1) It states that once you know the ground state electron density in position space any ground state property is uniquely dened.

Theorem (1) It states that once you know the ground state electron density in position space any ground state property is uniquely dened. Theorem (2) It states that once the functional that relates the electron density in position space with the total electronic energy is known, one may calculate it approximately by inserting approximate densities . Furthermore, just as for the variational method for wavefunctions, one may improve any actual calculation by minimizing Ee [ ].

Theorem (1) It states that once you know the ground state electron density in position space any ground state property is uniquely dened. Theorem (2) It states that once the functional that relates the electron density in position space with the total electronic energy is known, one may calculate it approximately by inserting approximate densities . Furthermore, just as for the variational method for wavefunctions, one may improve any actual calculation by minimizing Ee [ ]. The proof proceeds by reductio ad absurdum
Schematic representation of Hohenberg-Kohn theorems. HK Vext (r) n0 (r)
i ({r})
0 ({r})
Schematic representation of Kohn-Sham ansatz. HK0 HK KS Vext (r) n0 (r) n0 (r) VKS (r)
i ({r})
0 ({r})
i =1,Ne ({r})
i ({r})
The spin-polarized Kohn-Sham equations

(HKS )i (r) = 0, i
(1)
where
1 HKS (r) = 2 + VKS (r), (2) 2 the spin-polarized Kohn-Sham potential V could be wirte by two KS terms (r ) dr , (3) (r) = Vext (r) + |r r | and Exc [] = ( xc ( ))/ (4) () = xc (r, ) where is the spin-polarized exchange-correlation and the density given by
N
(r) =
(r, ) =
i =1
|i (r)|2 ,
(5)
Exchange-correlation energy(Exc )
Denition It is the dierent between the exact interacting many-body energy and the non-interacting one. Exc [n(r )] = F [n(r )] (Ts + EHartree ) = (Texact Ts ) + (Eint EHartree )
1 2 3 4
(6)
It is divided to Exc [n(r )] = Ex + Ec Ec smaller in size relative to Ex increase the Ex magnitude lower the Etot decrease the Ec magnitude increase Etot
LSDA versus GGA

Local Spin Density Approximation (LSDA)
1 2 3
Generalized Gradient Approximation (GGA)

1 2 3
Exc functional for only Favors density homogeneity von Barth and Hedin parametrization Desgined for slowly varying densities! Orbital independent Not self-interaction free Dispertion interaction is not included
Exc functional for and Favors density inhomogeneity Perdew, Burke and Ernzerhof (PBE96) parametrization Orbital independent Not self-interaction free Dispertion interaction is not included
4 5 6
5 6 7
Schematic ow-chart for self consistent functional calculations
Compute VKS (r) Solve Single Particle Eqns. Determine EF Calculate out (r)
Mix out (r), in (r)
Converged?
Done
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Full-Potential Linearized Augmented Plane-wave (FP-LAPW) Method Formalism
The historical progress of the FP-LAPW method ow chart

Unit cell divided into two regions i) MT sphere ii) Interstitial region Plane-wave bases sets The energy dependence of the radial functions inside each sphere is linearized
APW (Slater 1937)
LAPW (Andersen 1975)
FP-LAPW (Wimmer et al. 1981)
No potential shape approximation
All-ellectron FP-LAPW (Weinert et al. 1982)
The explicit algebraic cancellation of the nuclear Coulomb singularities in the Kinetic and potential energy terms which leads to good numerical stability Introduced local orbitals (LOs) to augment the LAPW basis set for certain l values Where APWs are evaluated at a xed energy and exibility is added by including a type of local orbitals ( los) combining a u and u
LAPW + LO (Singh 1991)
APW +lo (Sjstedt et al. 2000) o
1 2 3
No shape approximations in charge density or potential includes core orbitals most precise method available
The FP-LAPW method enhanced the potential in LAPW and expand it in the form: Ve (r) =
|K | K pot Ve (K)e i K.r K lmax lm (r )Y (r ) lm lm Ve
rI rS
(7)
where Kpot and l max determine the highest reciprocal lattice vectors included in the sum.
LAPW assumptions
1 2
APW assumptions ul is expanded by a Taylor expansion around l Basis has more exibility inside sphere No asymptote problem
Interstitial Sphere
(r), V(r) : Lattice Harmonics (r) : Atomic-like function
(r), V(r) : Stars (r) : Planewave
APW and LAPW basis sets
The APW basis sets (r) = The LAPW basis sets (r) = 2 rI [Alm ul (r ) + Blm ul (r )] r S lm
1
G cG e
i (G+K).r
lm Alm ul (r )
rI rS
(8)
G cG e
i (G+K).r
(9)
LAPW+LO and APW+lo methods
The local orbitals basis sets in LAPW+LO method: 0 rI ,LO ,LO ,LO (aL u1l (r ) + bL u1l (r ) + cL u2l (r ))YL () r S r (10) The local orbitals basis sets in APW+lo method: (r)LO = (r)lo = 0 rI ,lo ,lo (aL u1l (r ) + bL u1l (r ))YL () r S r (11)
The pseudo-charge method for solving the Poisson equation
Calculate multipoles of the sphere charge Construct the pseudocharge Calculate VPW Synthesize VPW on the sphere boundaries Integrate Poissons Eqn. in the spheres
Calculate planewave charge multipoles
The total energy per unit cell is

E =
i
1 2
Vc (r )[ (r ) + (r )]dr +
1 r
[ (r) + (r )]
xc (r )[ (r ) + (r )]dr
2 Rn u
[R S0 (R ) + Z Q ] (12)
+Exc [ , ].
where Vc is the Coulomb potential, EXC is exchange-correlation energy, xc is the exchange-correlation energy density per atom
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Full-Potential Linearized Augmented Plane-wave (FP-LAPW) Method WIEN2k Package
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Results and Discussion Stoichiometric Fe3x Mnx Z (Z= Al, Ge, Sb) Systems
0.4
0.2
Fe3Al
0.3
Fe2MnAl
0.15
Total energy (eV)
Total energy (eV)

3.7 3.65 lattice parameter a () 3.8
0.2
0.1
0.1
0.05
3.5
3.55
3.6
3.75
3.45
3.5
3.55 lattice parameter a ()
3.6
3.65
0.2
0.15
FeMn2Al
0.15
0.1
Mn3Al
Total energy (eV)
Total energy (eV)
0.1
0.05
0.05
3.5
3.55
3.6 3.65 lattice parameter a ()
3.7
3.75
3.5
3.55
3.6
3.7 3.65 lattice parameter a ()
3.75
3.8
compound Fe3 Al structure DO3 a(A ) 5.750 5.738 5.820(exp) 3.653 3.651 5.683 5.670 5.850(exp) 5.760 5.725 5.806 5.723 5.736 5.760(exp) 3.642 3.667(exp) 5.703 5.780(exp) 5.718 5.675 5.765 5.749 3.654 3.800(exp) 5.996 5.900(exp) 5.955 5.999 5.925 5.985 5.930 3.811 4.000(exp) B (GPa) 169.9 169.3 169.4 174.9 200.9 EV (max) (eV) EC (min) (eV) Eg (eV) ES (eV) P(%) 35 Ref. Lechermann et al. 02 Bansal et al. 94 Lechermann et al. 02 0.740 1.205 0.465 81 Fujii et al. 95 Vinesh et al. 09 150.2 143.9 167.7 179.6 Zhou et al. 95 217.6 214.4 197.2 170.5 Takizawa et al. 02 159.5 192.6 141.2 174.4 177.1 Yamashita et al. 03 0.979 0.731 0.768 1.668 1.127 1.375 0.689 0.396 0.607 28 Bansal et al. 94 0.063 0.043 82 100 Luo et al. 08 100 Fujii et al. 08 0.845 0.893 0.828 1.392 1.376 1.326 0.547 0.482 0.497 96 Rodriquez-Carvajal 93 87 Luo et al. 08 96 Fujii et al. 08 0.674 0.555 1.218 1.098 0.544 0.543 0.116 99 Luo et al. 08 100 Fujii et al. 08 20 Zhou et al. 95
L12 Fe2 MnAl L21 (Fm-3m)
Mn2 FeAl Mn3 Al Fe3 Ge
L21 (F-43m) DO3 DO3 L12
Fe2 MnGe Mn2 FeGe Mn3 Ge
L21 (Fm-3m) DO3 L21 (F-43m) DO3 L12
Fe3 Sb Fe2 MnSb Mn2 FeSb Mn3 Sb
DO3 L21 (Fm-3m) L21 (F-43m) DO3 L12
Total and atom-resolved DOS of the stoichiometric Fe3x Mnx Sb

10 5 0 -5 -10 3 DOS (states/eV) 0 -3 3 0 -3 1 0 -1 -4 -2 0 E-EF (eV) 2 4 Sb[D] Fe[B] Fe3Sb - total
Fe[A,C]

10 5 0 -5 -10 3 DOS (states/eV) 0 -3 3 0 -3 1 0 -1 -4 -2 0 E-EF (eV) 2 4 Sb[D] Fe[B] Fe3Sb - total Fe2MnSb -Total
Fe[A,C]
5 0 -5 -10 4 0 DOS (states/eV) -4 -8 4 2 0 -2 -4 2 1 0 -1 -2 -4 -2 0 E-EF (eV) 2
Fe[A,C]
Mn[B]
Sb[D]

Fe[A,C]
Fe[A,C]
Mn[B]
Sb[D]
8 4 0 -4 -8 3 0 -3 3 0 -3 3 0 -3 1 0 -1 -3 0 E-EF (eV)
Mn2FeSb - Total
Mn[A]
DOS (states/eV)
Mn[B]
Fe[C]
Sb[D]

Fe[A,C]
Fe[A,C]
Mn[B]
Sb[D]
8 4 0 -4 -8 3 0 -3 3 0 -3 3 0 -3 1 0 -1 -3 0 E-EF (eV)
Mn2FeSb - Total
5 0 -5
Mn3Sb-Total
Mn[A]
-10 5 0 -5 -10 5
Mn[A,C]
DOS (states/eV)
Mn[B]
Mn[B]
Fe[C]
0 -5 -10 1 Sb[D]
Sb[D]
0 -1
3
-4
-2
0 E-EF (eV)
The Fe[A,C] d-eg and d-t2g partial DOS
2 1 0 -1 -2 2 1 DOS[states/eV] 0 -1 2 -2 1 0 -1 2 -2 1 0 -1 -2 -3 -2 -1 0 E-EF(eV)
Fe[A,C] (d-eg) Fe3Al
Fe[A,C] (d-t2g)
Fe[A,C] (d-eg) Fe2MnAl
Fe[A,C] (d-t2g)
The bandstructure and DOS

Mn2FeSb up
5
Mn2FeSb down
5
E-EF (eV)
EF
EF
-5
-5
X WK
-10
-10 W
X WK
E-EF (eV)
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Results and Discussion Non-Stoichiometric Fe3x Mnx Z (Z= Al, Ge, Sb) Systems
Zooming DOS Figure Example
30
Majority
20
Fe0.5Mn2.5Ge
10 DOS[states/eV]
-10
-20
Minority
-4 -2 E - EF 0 2 4
-30
Zooming DOS Figure Example
10 DOS[states/eV]
-10
-20
Minority
Spin-polarised DOS for Fe3x Mnx Z with dierent Mn concentration

40 30 20 10 0 -10 -20 -30 30 20 10 0 -10 -20 30 -30 20 10 0 -10 -20 -30
Fe1.25Mn1.75Al
DOS [states/eV]
Majority Minority
Fe1.5Mn1.5Al
Fe1.75Mn1.25Al
-8
-4 E-EF (eV)

40 30 20 10 0 -10 -20 -30 30 20 10 0 -10 -20 30 -30 20 10 0 -10 -20 -30
Fe1.25Mn1.75Al
DOS [states/eV]
DOS[states/eV]
Majority Minority
Fe1.5Mn1.5Al
Fe1.75Mn1.25Al
-8
-4 E-EF (eV)
30 20 10 0 -10 -20 -30 30 20 10 0 -10 -20 30 -30 20 10 0 -10 -20 -30 -12
Fe0.75Mn2.25Ge
Majority Minority
Fe0.5Mn2.5Ge
Fe0.25Mn2.75Ge
-8
-4 E-EF (eV)

40 30 20 10 0 -10 -20 -30 30 20 10 0 -10 -20 30 -30 20 10 0 -10 -20 -30
Fe1.25Mn1.75Al
DOS [states/eV]
DOS[states/eV]
Majority Minority
Fe1.5Mn1.5Al
Fe1.75Mn1.25Al
-8
-4 E-EF (eV)
30 20 10 0 -10 -20 -30 30 20 10 0 -10 -20 30 -30 20 10 0 -10 -20 -30 -12
Fe0.75Mn2.25Ge
Majority Minority
Fe0.5Mn2.5Ge
Fe0.25Mn2.75Ge
-8
-4 E-EF (eV)
40 20 0 -20 20 DOS [states/eV] 10 0 -10 40 20 0 -20 -40 -10 -5 E - EF (eV) 0
Fe2.75Mn0.25Sb
Majority Minority
Fe2.5Mn0.5Sb
Fe2.25Mn0.75Sb
Compound Fe2.75 Mn0.25 Al Fe2.5 Mn0.5 Al Fe2.25 Mn0.75 Al Fe1.75 Mn1.25 Al Fe1.5 Mn1.5 Al Fe1.25 Mn1.75 Al Fe0.75 Mn2.25 Al Fe0.5 Mn2.5 Al Fe0.25 Mn2.75 Al Fe2.75 Mn0.25 Ge Fe2.5 Mn0.5 Ge Fe2.25 Mn0.75 Ge Fe1.75 Mn1.25 Ge Fe1.5 Mn1.5 Ge Fe1.25 Mn1.75 Ge Fe0.75 Mn2.25 Ge Fe0.5 Mn2.5 Ge Fe0.25 Mn2.75 Ge Fe2.75 Mn0.25 Sb Fe2.5 Mn0.5 Sb Fe2.25 Mn0.75 Sb Fe1.75 Mn1.25 Sb Fe1.5 Mn1.5 Sb Fe1.25 Mn1.75 Sb Fe0.75 Mn2.25 Sb Fe0.5 Mn2.5 Sb Fe0.25 Mn2.75 Sb
Space group Pm (221) 3m P4/mmm (123) Pm (221) 3m P 43m (215) Pn (224) 3m P 43m (215) P 43m (215) P42 /nnm (134) P 43m (215) Pm (221) 3m P4/mmm (123) (221) Pm3m P 43m (215) Pn (224) 3m P 43m (215) P 43m (215) P42 /nnm (134) P 43m (215) Pm (221) 3m P4/mmm (123) Pm (221) 3m P 43m (215) Pn (224) 3m P 43m (215) P43m (215) P42 /nnm (134) P 43m (215)
a(A ) 5.741 4.059 5.726 5.694 5.698 5.731 5.726 5.696 5.708 5.724 4.026 5.701 5.697 5.703 5.715 5.729 5.751 5.748 5.985 4.228 5.978 5.949 5.981 6.01 5.992 5.975 5.988
B (GPa) 172.9 132.7 197.4 194.1 180.8 157.6 134.3 150.7 156.2 166.4 210.9 213.0 209.2 205.9 194.4 180.9 190.4 192.4 158.1 148.8 160.2 197.4 188.4 135.4 157.7 164.6 172.8
Eg (eV) 0.405 0.311 0.274 0.356 0.349 0.491 0.595 0.447 0.332 0.282 0.221 0.243 0.389 0.292 0.063 0.045 0.057 0.051 0.079 0.499 0.021
P(%) 38.5 40 100 88 100 98 100 100 100 22 62 100 90 95 94 90 94 100 24.4 28 88 85 86 99 95 100 100
structure Fe3 Al Fe2.75 Mn0.25 Al Fe2.5 Mn0.5 Al Fe2.25 Mn0.75 Al Fe2 MnAl Fe1.75 Mn1.25 Al Fe1.5 Mn1.5 Al Fe1.25 Mn1.75 Al FeMn2 Al Fe0.75 Mn2.25 Al Fe0.5 Mn2.5 Al Fe0.25 Mn2.75 Al Mn3 Al Fe3 Ge Fe2.75 Mn0.25 Ge Fe2.5 Mn0.5 Ge Fe2.25 Mn0.75 Ge Fe2 MnGe Fe1.75 Mn1.25 Ge Fe1.5 Mn1.5 Ge Fe1.25 Mn1.75 Ge FeMn2 Ge Fe0.75 Mn2.25 Ge Fe0.5 Mn2.5 Ge Fe0.25 Mn2.75 Ge Mn3 Ge Fe3 Sb Fe2.75 Mn0.25 Sb Fe2.5 Mn0.5 Sb Fe2.25 Mn0.75 Sb Fe2 MnSb Fe1.75 Mn1.25 Sb Fe1.5 Mn1.5 Sb Fe1.25 Mn1.75 Sb FeMn2 Sb Fe0.75 Mn2.25 Sb Fe0.5 Mn2.5 Sb Fe0.25 Mn2.75 Sb Mn3 Sb FM: M TOT (B ) ma (B ) 5.966 1.927 22.23 1.640Mn 10.72 2.420 9.00 2.62 2.003 -0.152 7.13 -0.04 5.99 -1.66 5.01 0.200 0.999 0.15Fe 2.99 -1.47 1.99 0.38Fe 2.99 1.42Fe 0.000 -1.415 5.624 1.624 19.9 2.34Mn 8.19 2.61 12.99 2.70 3.024 0.209 11.05 0.30 10.09 -0.96 9.01 0.003 2.013 0.506 7.12 -0.83 6.03 0.59Fe 4.99 2.47Fe 1.002 -0.918 6.116 1.789 23.83 2.83Mn 11.27 2.72 17.14 3.04 4.140 0.670 15.55 1.27 14.07 -1.46 13.01 0.02 3.000 1.164 10.96 3.05 10.00 0.91Fe 8.98 2.70Fe 2.000 -0.472 Ferromagnetic mb (B ) 2.422 -0.09 -0.07 0.000 2.32Mn -1.49Mn 2.429 -0.31 2.669 -1.64 0.00 -0.011 2.826 2.575 -0.04 -0.03 -0.02 2.626 -1.34Mn 2.54 2.41Fe 2.562 -1.19 -1.02 0.03 2.750 2.730 -0.02 -0.04 -0.03 2.875 -2.01Mn 2.78 2.81Fe 2.948 0.02 0.02 0.023 2.856 FM : mc (B ) 2.410 -0.07 -0.013 -0.04 -0.004 0.050 -1.798 0.30Fe 2.44 -2.56 md (B ) -0.087 -0.08 1.74Mn 2.39Mn -0.015 -0.24 -0.07Fe -1.71Mn -0.006 -1.55 -1.41 -0.005 -0.057 -0.06 2.26Mn 2.36Mn -0.012 0.29 0.28Fe 2.47 0.010 -1.14 mg ,e1 (B ) 1.810 -0.09 2.38Mn 0.00 2.49 1.16 0.012 1.32 0.88 0.44 2.60Mn 0.76Fe 2.63 0.03 -0.73 1.69 0.74 2.79Mn 1.29Fe 0.04 -0.29 AF: magnetic phase FM FM 1.760 FM FM FM -0.01 FM FM 2.54Mn FM FM -0.002 FM FM FM AF FM FM FM FM FM -0.004 FM FM -0.98 FM FM 0.02 FM 2.68 FM FM FM FM FM 1.52 FM FM FM -0.01 FM FM -0.94 FM FM FM FM FM FM Antiferromagnetic me2 (B )
2.59 -0.03 -0.02 0.26 0.007 0.01 -1.080 0.60Fe -1.02 2.66 0.04 0.044 -0.028 2.72 -0.04 -0.03 2.78Mn -0.02 2.90Mn -0.02 0.76 1.03 -0.003 0.96Fe 0.02 2.92 -1.141 0.017 0.03 2.65Fe 2.91 -0.62 2.78 0.025 0.028 Ferrimagnetic
Relation between spin magnetic moment and Mn concentration

12
10 Total magnetic moment (B)
Fe3-xMnxAl
Generalized Slater-Pauling rule Calculated total magnetic moment
0.5
2 1.5 Mn concentration
2.5

12
Fe3-xMnxAl
Total magnetic moment (B) Generalized Slater-Pauling rule Calculated total magnetic moment
16
Fe3-xMnxGe
Generalized Slater-Pauling rule calculated total magnetic moment
14
12
10
6 0 4 0 0.5 1 2 1.5 Mn concentration 2.5 3 0 0.5 1 2 1.5 Mn concentration 2.5 3

12
Fe3-xMnxAl
Total magnetic moment (B) Generalized Slater-Pauling rule Calculated total magnetic moment
16
Fe3-xMnxGe
Generalized Slater-Pauling rule calculated total magnetic moment
14
12
10
6 0 4 0 0.5 1 2 1.5 Mn concentration 2.5 3 0 0.5 1 2 1.5 Mn concentration 2.5 3
20
Fe3-xMnxSb
18 Total magnetic moment (B) Generalized Slater-Pauling rule Calculated total magnetic moment
16
14
12
10
0.5
2 1.5 Mn concentration
2.5
Magnetic hyperne eld on Z atoms
600 550 500 Magnetic hyperfine field on Z (KG) 450 400 350 300 250 200 150 100 50 0 -50 0 0.5 1 1.5 Mn concentration (%) 2 2.5 3 Fe3-xMnxAl Fe3-xMnxGe Fe3-xMnxSb
Hyperne elds (contact + dipolar + orbitals contribution)
Magnetic hyperne eld on the B-site
HFF on B site (KGauss)
-100
-200
-300
Fe3-xMnxAl Fe3-xMnxGe Fe3-xMnxSb
-400
0.5
1.5 concentration x
2.5
INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z= Conclution and Open issue
Conclusion
Fe rich compounds are metallic and have low spin polarization.
Conclusion
Fe rich compounds are metallic and have low spin polarization. The metalloid atoms are not responsible for the origin of the band gap but lead to a shift in the fermi level.
Conclusion
Fe rich compounds are metallic and have low spin polarization. The metalloid atoms are not responsible for the origin of the band gap but lead to a shift in the fermi level. Compounds beyond x > 0.75 are strong candidates as half-metals with high spin polarization.
Conclusion
Fe rich compounds are metallic and have low spin polarization. The metalloid atoms are not responsible for the origin of the band gap but lead to a shift in the fermi level. Compounds beyond x > 0.75 are strong candidates as half-metals with high spin polarization. Direct band gaps for the non-stoichiometric alloys.
Conclusion
Fe rich compounds are metallic and have low spin polarization. The metalloid atoms are not responsible for the origin of the band gap but lead to a shift in the fermi level. Compounds beyond x > 0.75 are strong candidates as half-metals with high spin polarization. Direct band gaps for the non-stoichiometric alloys. Indirect band gaps along - X symmetry line for the stoichiometric alloys.
Conclusion
Fe rich compounds are metallic and have low spin polarization. The metalloid atoms are not responsible for the origin of the band gap but lead to a shift in the fermi level. Compounds beyond x > 0.75 are strong candidates as half-metals with high spin polarization. Direct band gaps for the non-stoichiometric alloys. Indirect band gaps along - X symmetry line for the stoichiometric alloys. Hyperne elds on transition atoms are decreasing in magnitude with increasing Mn concentration, while the oppsite for metaloids.
Open issue
1
Investigation of the eect of disorder on the electric and magnetic properties of Fe3x Mnx Z compounds.
Open issue
1
Investigation of the eect of disorder on the electric and magnetic properties of Fe3x Mnx Z compounds. The optical properties of the Fe3x Mnx Z Heusler alloys.
Open issue
1
2 3
Investigation of the eect of disorder on the electric and magnetic properties of Fe3x Mnx Z compounds. The optical properties of the Fe3x Mnx Z Heusler alloys. Elastic properties and magnetic shape memory alloy for Fe3x Mnx Z.
Open issue
1
2 3
Investigation of the eect of disorder on the electric and magnetic properties of Fe3x Mnx Z compounds. The optical properties of the Fe3x Mnx Z Heusler alloys. Elastic properties and magnetic shape memory alloy for Fe3x Mnx Z. The transport properties and half-metallicity at elevated temperature of Fe3x Mnx Z compounds.
Open issue
1
2 3
Investigation of the eect of disorder on the electric and magnetic properties of Fe3x Mnx Z compounds. The optical properties of the Fe3x Mnx Z Heusler alloys. Elastic properties and magnetic shape memory alloy for Fe3x Mnx Z. The transport properties and half-metallicity at elevated temperature of Fe3x Mnx Z compounds. The eect of lowering the dimension of Fe3x Mnx Z compounds may be studied. ( surfaces and interfaces) The electronic and magnetic properties of Mn2 FeAl1x Gex quaternary Heusler alloys could be investigated.
Open issue
1
2 3
Investigation of the eect of disorder on the electric and magnetic properties of Fe3x Mnx Z compounds. The optical properties of the Fe3x Mnx Z Heusler alloys. Elastic properties and magnetic shape memory alloy for Fe3x Mnx Z. The transport properties and half-metallicity at elevated temperature of Fe3x Mnx Z compounds. The eect of lowering the dimension of Fe3x Mnx Z compounds may be studied. ( surfaces and interfaces) The electronic and magnetic properties of Mn2 FeAl1x Gex quaternary Heusler alloys could be investigated. The half-metallicity search in Ti1+x FeSb Heusler alloys (x= 0, 0.25, 0.5, 0.75, 1).
Acknowledgement
My deepest acknowledgement to: My supervisor Dr. Jamil khalifeh and co-supervisor Dr. Bothina Hamad The examination committee My colleagues, co-workers and friends Audience
Thank You

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INVESTIGATION OF HALF-METALLIC BEHAVIOR AND SPIN POLARIZATION FOR THE HEUSLER ALLOYS Fe3x Mnx Z (Z=

Classifecation of half-metals after Coey and Venkatesan (2002)

Type IA IB IIA IIB IIIA IIIB IVA IVB VA VB

Example CrO2 or NiMnSb Mn2 VAl Fe3 O4 (La0.7 Sr0.3 )MnO3

Tl2 Mn2 O7 GaAs

Example Two types of Heusler Some oxides Manganites Double perovskites

Full-Heusler X2YZ [L21]

Half-Heusler XYZ [C1b]

For X2 YZ (CuHg2 Ti-type) 1 X at 4a (0,0,0) and 4c ( 4 , 1 , 1 ) 4 4 1 Y and Z atoms at 4b ( 2 , 1 , 1 ) and 2 2 3 4d ( 4 , 3 , 3 ) 4 4

d d hybridization Determined by the X-X interaction only ( t1u - eu splitting)

The Slater-Pauling behavior of Heusler alloys

Total spin moment: Mt ()

NiMnTe CoFeSb RhMnSb NiFeSb

Total spin moment: Mt ()

NiMnSb PdMnSb PtMnSb

Co2CrAl Fe2MnSi Ru2MnSi Ru2MnGe Ru2MnSn

Co2MnSi Co2MnGe Co2MnSn

Co2MnAs Rh2MnIn Rh2MnTl

Co2MnSb Co2FeSi Co2FeAl Ni2MnAl

FeMnSb CoCrSb NiVSb CoVSb

CoMnSb IrMnSb NiCrSb

Rh2MnGe Rh2MnSn Rh2MnPb Co2MnAl Co2MnGa Rh2MnAl Rh2MnGa Ru2MnSb

Fe2CrAl Co2TiAl Fe2VAl Mn2VGe

Number of valence electrons: Zt

Number of valence electrons: Zt

The Hohenberg-Kohn Theorems

The Hohenberg-Kohn Theorems

The Hohenberg-Kohn Theorems

Schematic representation of Hohenberg-Kohn theorems. HK Vext (r) n0 (r)

The spin-polarized Kohn-Sham equations

LSDA versus GGA

Generalized Gradient Approximation (GGA)

Schematic ow-chart for self consistent functional calculations

Mix out (r), in (r)

The historical progress of the FP-LAPW method ow chart

APW (Slater 1937)

LAPW (Andersen 1975)

FP-LAPW (Wimmer et al. 1981)

No potential shape approximation

All-ellectron FP-LAPW (Weinert et al. 1982)

LAPW + LO (Singh 1991)

APW +lo (Sjstedt et al. 2000) o

(r), V(r) : Stars (r) : Planewave

APW and LAPW basis sets

LAPW+LO and APW+lo methods

The pseudo-charge method for solving the Poisson equation

Calculate planewave charge multipoles

The total energy per unit cell is

Total energy (eV)

Total energy (eV)

3.55 lattice parameter a ()

Total energy (eV)

Total energy (eV)

3.6 3.65 lattice parameter a ()

3.7 3.65 lattice parameter a ()

L12 Fe2 MnAl L21 (Fm-3m)

Mn2 FeAl Mn3 Al Fe3 Ge

L21 (F-43m) DO3 DO3 L12

Fe2 MnGe Mn2 FeGe Mn3 Ge

L21 (Fm-3m) DO3 L21 (F-43m) DO3 L12

Fe3 Sb Fe2 MnSb Mn2 FeSb Mn3 Sb

DO3 L21 (Fm-3m) L21 (F-43m) DO3 L12