Spin-spiral calculations of the magnetic properties of Fe-based superconductors

Alexander Yaresko Max Planck Institute for Solid State Research, Stuttgart, Germany
FESC 2010 May 11, 2010

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in collaboration with

Guo-Qiang Liu, Viktor Antonov, and Ole Andersen MPI FKF

special thanks to: Lilia Boeri, George Jackeli, Wei Ku for helpful discussions

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overview

band structure, nesting, and susceptibility q-dependence of the total energy from spin-spiral calculations effect of electron and hole doping applicability of the Heisenberg model interlayer coupling conclusions

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new class of unconventional superonductors

150

T
120

90

T(K)

60

SDW
T
C

30

SC
0 0.0 0.2

x in Ba

0.4

1-

x x

Fe As
2

0.6

0.8

1.0

H.Luetkens,et al Nature Mat.8, 305 (2009)

H. Chen, et al, EPL 85, 17006 (2008)

undoped compounds: orthorombic distortions + AFM order when doping or pressure suppress magnetic order, superconductivity
comes into play (TC >50K) LiFeAs: nonmagnetic with (TC 18K) J. Tapp, et al, PRB 78, 060505 (2008) electron-phonon coupling seems to be too weak to explain high TC
L. Boeri, et al, PRL 101, 026403 (2008)

it is important to understand magnetic properties!

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crystal structure
MFe2 As2 M=Sr,Ba I4/mmm (122) LiFeAs P4/nmm (111)
La Fe As O
Ba Fe As

LaFeAsO P4/nmm (1111)

Li Fe As

Fe is surrounded by slightly distorted As4 tetrahedra Fe ions form a square lattice FeAs layers are separated by a LaO, M or Li layer(s)
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two limits
weak magnetic perturbation strong magnetic perturbation

noninteracting susceptibility

self-consistent calculations for spin spirals

0 (q, )
? ? ? ? ?

do the two limits always lead to the same conclusions how electron and hole doping affect the magnetic properties is stripe AFM order the ground state for doped compounds can the j1 j2 Heisenberg model describe the calculated E(q) similarities and differences between various families compounds

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two limits
weak magnetic perturbation strong magnetic perturbation

noninteracting susceptibility

self-consistent calculations for spin spirals

0 (q, )
? ? ? ? ?

do the two limits always lead to the same conclusions how electron and hole doping affect the magnetic properties is stripe AFM order the ground state for doped compounds can the j1 j2 Heisenberg model describe the calculated E(q) similarities and differences between various families compounds

details: L(S)DA calculations were performed using the LMTO method for experimental high-temperature tetragonal crystal structures orthorhombic distortions were neglected electron ( > 0) or hole ( < 0) doping per Fe ion was simulated by using the virtual crystal approximation
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t2 bands for BaFe2 As2

xy

yz,xz
N P X

M T

0
Energy (eV)

-1
T N

-2 T N P T M

three (2dyz,zx ; 1dxy ) hole-like pokets around and two electron-like (2dyz,zx +dxy ) pokets around X

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and for LiFeAs

xy yz,xz
Z A X M

0
Energy (eV)

-1
X

-2 M X Z

similar hole-like and electron-like pockets the size of the dxy FS is larger than dyz,zx ones less effective nesting the width of dxy and dyz,zx bands is larger than in BaFe2 As2
(dFe-Fe =2.67 A vs. 2.80 A)?
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noninteracting susceptibility for LaFeAsO

Im ( 0)/ (arb. units)

50 40 30

peak at X due to FS nesting

20 10

M=X

0
Re (0) (arb. units)

90 80 70 60 50
_ _

=0

J. Dong, et al, EPL 83, 27006 (2008), I. Mazin, et al, PRL 101,
X M

057003 (2008). . .
9

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noninteracting susceptibility for LaFeAsO

Im ( 0)/ (arb. units)

50 40 30

peak at X due to FS nesting

20 10

M=X

0
Re (0) (arb. units)

90 80 70 60 50
_ _

=0

J. Dong, et al, EPL 83, 27006 (2008), I. Mazin, et al, PRL 101,
X M

057003 (2008). . .
9

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for LaFeAsO1x Fx
doping sup presses the X peak maximum shifts to an incommensurate q

electron

Im ( 0)/ (arb. units)

50 40 30 20 10 0

=0.2 (x=0.2)

Re (0) (arb. units)

90 80 70 60 50
_ _

=0 =0.1 =0.2

M=X

10

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for LaFeAsO1x Fx
doping sup presses the X peak maximum shifts to an incommensurate q at which FS touch

electron

Im ( 0)/ (arb. units)

50 40 30 20 10 0

=0.2 (x=0.2)

Re (0) (arb. units)

90 80 70 60 50
_ _

=0 =0.1 =0.2

M=X

10

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. . . BaFe2 As2
30
Im ( 0)/ (arb. units)
_

X=X

20
_

10

0
Re (0) (arb. units)

80

=0
_

P=X

70
_

60

50

11

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. . . Ba1x Kx Fe2 As2 (x = 2||)

30
Im ( 0)/ (arb. units)

20

10

hole doping also suppresses

0
Re (0) (arb. units)

the peak at X the maximum shifts

=0 =-0.1 =-0.2

80

70

60

The peak of Re(q) at X is suppressed by either electron or hole doping

50

12

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. . . LiFeAs
30
Im ( 0)/ (arb. units)

20

10

0
Re (0) (arb. units)

80

70

60

nesing is less effective (q) is lower the X peak is split already

in undoped LiFeAs

_ _

50

13

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response to nite AFM perturbation

BaFe2 As2
0.4
xy yz xz 3z2-r2 x2-y2 MFe/5

LiFeAs
0.4
xy yz xz 3z2-1 x2-y2 MFe/5

0.3

0.3

M (B)

0.2

M (B)

0.2

0.1 AFM || x; FM || y 0.0 0.0 0.2 0.4 0.6 0.8 =V -V (eV) 1.0 1.2 1.4

0.1 AFM || x; FM || y 0.0 0.0 0.2 0.4 0.6 0.8 =V -V (eV) 1.0 1.2 1.4

induced moment M vs. = V V

at small the moment is induced faster on obitals forming nested FS

BaFe2 As2 : dMdxy /d = 0.60 dMdx2 y2 /d = 0.18 LiFeAs: dMdxy /d = 0.45 dMdx2 y2 /d = 0.12 the degeneracy of dzx and dyz states is lifted at large nesting is less important: dMdxy /d=dMdx2 y2 /d=0.18 What happens when Fe moments are large?
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self-consistent calculations for spin spiral

X ;

q = (q, 0),

q =0.875

X M;

q = (1, q),

q =0.125

EH (j1 + 2j2 ) cos(q) + j1

EH (j1 2j2 ) cos(q) j1

EH is a monotonic function of q
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self-consistent calculations for spin spiral

X ;

q = (q, 0),

q =0.

X M;

q = (1, q),

q =1

EH (j1 + 2j2 ) cos(q) + j1

EH (j1 2j2 ) cos(q) j1

EH is a monotonic function of q
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 spin spirals along M

M;

q = (q, q),

q =0.125

EH 2j1 cos(q) + 2j2 cos2 (q)

a local minimum appears if j2 > j1 /2

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LaFeAsO

(0,0)

(,0)

(,)

(0,0)

1.5
MFe (B)

1.0

the E(q) minimum is at X

(stripe AFM order)

0.5

0.0 0
E(q)-E(0) (meV/Fe)

E(q) is reasonably well described

by the j1 j2 Heisenberg model

j1 =81 meV, j2 =57 meV, j2 /j1 =0.71

-50

nonmagnetic solution at small |q|

-100

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electron doping in LaFeAsO1x Fx (x = )

(0,0)

(,0)

(,)

(0,0)

deviation from the Heisenberg-like

behaviour increases with doping a new minimum at the XM line

1.5
MFe (B)

1.0 =0 =0.1 =0.2 =0.3

0.5

0.0 0
E(q)-E(0) (meV/Fe)

-50

-100

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electron doping in LaFeAsO1x Fx (x = )

(0,0)

(,0)

(,)

(0,0)

deviation from the Heisenberg-like

behaviour increases with doping a new minimum at the XM line

1.5
MFe (B)

1.0 =0 =0.1 =0.2 =0.3

0.5

stripe AFM order becomes unstable already at small

0.0 0
E(q)-E(0) (meV/Fe)

-50

-100

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band-structure effect?
LaFeAsO; =0
2
dyz dxz dxy

LaFeAsO1x Fx ; =0.1
20
q=(1,0.0)

DOS (1/eV/atom)

15
0 -1.5 -1.0 -0.5 0.0 0.5 Energy (eV) 1.0 1.5

DOS (states/eV)

10

1.5 1.0 0.5 0.0 -0.5 -1.0 -1.5

dyz dyz

Energy (eV)

0 -1.0
Y X

-0.5

0.0 0.5 Energy (eV)

1.0

1.5

a narrow Fe dyz DOS peak just above EF is lled when LaFeAsO is doped with electrons
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band-structure effect?
LaFeAsO; =0
2
dyz dxz dxy

LaFeAsO1x Fx ; =0.1
20
q=(1,0.0) q=(1,0.05) q=(1,0.10)

DOS (1/eV/atom)

15
0 -1.5 -1.0 -0.5 0.0 0.5 Energy (eV) 1.0 1.5

DOS (states/eV)

10

1.5 1.0 0.5 0.0 -0.5 -1.0 -1.5

dyz dyz

Energy (eV)

0 -1.0
Y X

-0.5

0.0 0.5 Energy (eV)

1.0

1.5

a narrow Fe dyz DOS peak just above EF is lled when LaFeAsO is doped with electrons The peak splits at incommensurate q
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BaFe2 As2

(0,0)

(,0)

(,)

(0,0)

1.5

MFe (B)

1.0

0.5

0.0 0
E(q)-E(0) (meV/Fe)

the minimum is at X E(q) is Heisenberg-like j1 =95 meV; j2 =73 meV; j2 /j1 =0.77

-50

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hole doping in Ba1x Kx Fe2 As2 (x = 2||)

(0,0)

(,0)

(,)

(0,0)

1.5

the E(q) minimum stays at X up

to x =0.6 ( = 0.3) the stabilization energy

MFe (B)

1.0 =0 =-0.1 =-0.2 =-0.3

|E(X) E(0)|
decreases with doping

0.5

0.0 0
E(q)-E(0) (meV/Fe)

-50

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hole doping in Ba1x Kx Fe2 As2 (x = 2||)

(0,0)

(,0)

(,)

(0,0)

1.5

the E(q) minimum stays at X up

to x =0.6 ( = 0.3) the stabilization energy

MFe (B)

1.0 =0 =-0.1 =-0.2 =-0.3

|E(X) E(0)|
decreases with doping stripe AFM order is more stable
150

0.5

0.0 0
E(q)-E(0) (meV/Fe)

T
120

90

T(K)

60

SDW
T
C

-50

30

SC
0 0.0 0.2

x in Ba

0.4

1-

x x

Fe As
2

0.6

0.8

1.0

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hole vs. electron doping in MFe2 As2 (M=Ba, Sr)

hole doping ( < 0): M1x Kx Fe2 As2 (x = 2|| ) electron doping ( > 0): M(Fe1x Cox )2 As2 (x = )
0
E(q)-E(0) (meV/Fe)

-50
BaFe2As2

qz=
_ _

SrFe2As2

=-0.1 =0 =0.1
_ _

already weak electron doping ( < 0.1) destabilizes stripe AFM order magnetic transition in Ba(Fe1x Cox )2 As2 is suppressed at x 0.06
J. Chu, et al PRB 79, 014506 (2009)

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LiFeAs

(0,0)

(,0)

(,)

(0,0)

1.5

MFe (B)

1.0

0.5

Fe moment is much smaller magnetic solution exists in a

0.0 0
E(q)-E(0) (meV/Fe)

narrow range around X stabilization energy is only 12 meV/Fe

The loss of kinetic energy is higher because of compressed lattice?

-50

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does the Heisenberg model work for undoped compounds?

q=( ,0):
two decoupled AFM sublattices each Fe has two FM and two AFM nn

EH

= j1 [cos + cos( )] 2j2 = 2j2 = const.

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does the Heisenberg model work for undoped compounds?

q=( ,0):
two decoupled AFM sublattices each Fe has two FM and two AFM nn

EH

= j1 [cos + cos( )] 2j2 = 2j2 = const.

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does the Heisenberg model work for undoped compounds?

q=( ,0):
two decoupled AFM sublattices each Fe has two FM and two AFM nn

EH

= j1 [cos + cos( )] 2j2 = 2j2 = const.

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NO!
50 40
E()-E(0) (meV)

La =0 La =0.2

Ba =0 Ba =-0.2

30 20 10 0 0 45 90 (deg) 135 180

already LSDA prefers collinear stripe AFM order E() sin2 (Si Sj )2 energy variation is suppressed by doping, especially in BaFe2 As2
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orbital degrees of freedom?

variation of orbital occupations as a function of
0.8
yz zx xy yz zx xy

0.7
n

0.6

0.5 0 45 90 (deg) 135 180

stripe AFM order lifts the degeneracy of dyz and dzx orbitals (n 0.15)
is this the reason for anisotropic j1 and j1 ? ||

Z. Yin, et al PRL 101, 047001 (2008)

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interlayer exchange coupling

stripe AFM order in the ab-plane
E()-E(0) (meV/Fe)

0 -1 -2 -3 -4

Ba Fe As

BaFe2As2 LaFeAsO

90 (deg)

180

E(FMc ) E(AFMc ) 4 meV/Fe

strong AFM interlayer coupling in MFe2 As2

FMc : qz = 0, = 0 AFMc : qz = , = 180

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conclusions

In the undoped compounds the minimum of the total energy is found at

q=( ,0) corresponding to stripe AFM order LaFeAsO1x Fx ( > 0): the minimum shifts to incommensurate wave

vectors with doping and stripe AFM order becomes unstable M1x Kx Fe2 As2 ( < 0): stripe AFM order remains stable in a wide range of K concentrations. However, the stabilization energy decreases with doping M(Fe1x Cox )2 As2 ( > 0): stripe AFM order is rapidly destabilized when FeAs layer is doped with electrons LiFeAs: the Fe moment and the stabilization energy are much smaller strong dependence of the energy on shows that the magnetic interactions between Fe spins cannot be described by the simple j1 j2 Heisenberg model the interlayer coupling in MFe2 As2 is much stronger than in LaFeAsO

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