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Materials physics in ferromagnetic semiconductors Materials physics in ferromagnetic semiconductors and AMR effects in and AMR effects in GaMnAs GaMnAs nanostructures nanostructures Tomáš Jungwirth Institute of Physics ASCR František Máca, Jan Mašek, Jan Kučera Josef Kudrnovský, Alexander Shick Karel Výborný, Jan Zemen, Vít Novák, Miroslav Cukr, Kamil Olejník, et al. University of Nottingham Bryan Gallagher, Tom Foxon, Richard Campion, Kevin Edmonds, Andrew Rushforth, Devin Giddings et al. Hitachi Cambridge UT & Texas A&M Würzburg SNS Pisa Jorg Wunderlich Allan MacDonald,Jairo Sinova Laurens Molenkamp, Marco Polini David Williams Quian Niu Charles Gold et al. in collaboration with
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Page 1: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Materials physics in ferromagnetic semiconductorsMaterials physics in ferromagnetic semiconductorsand AMR effects in and AMR effects in GaMnAsGaMnAs nanostructuresnanostructures

Tomáš Jungwirth

Institute of Physics ASCR

František Máca, Jan Mašek, Jan KučeraJosef Kudrnovský, Alexander Shick

Karel Výborný, Jan Zemen,Vít Novák, Miroslav Cukr, Kamil Olejník, et al.

University of Nottingham

Bryan Gallagher, Tom Foxon,Richard Campion, Kevin Edmonds,

Andrew Rushforth, Devin Giddings et al.

Hitachi Cambridge UT & Texas A&M Würzburg SNS Pisa

Jorg Wunderlich Allan MacDonald,Jairo Sinova Laurens Molenkamp, Marco PoliniDavid Williams Quian Niu Charles Gold et al.

in collaboration with

Page 2: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

11.. Introduction Introduction ((Ga,Mn)AsGa,Mn)As materialmaterial

intrinsic and extrinsic properties

22.. Other related diluted magnetic semiconductorsOther related diluted magnetic semiconductors

search for higher Curie temperature and p- and n-type FS

3. AMR effects in (Ga,Mn)As

spin-valves and SETs

Page 3: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

1. Introduction - (Ga,Mn)As material

Mn

As

Ga

5 d-electrons with L=0→ S=5/2 local moment

moderately shallow acceptor (110 meV)→ hole

Jungwirth, Sinova, Mašek, Kučera, MacDonald, Rev. Mod. Phys. (2006), http://unix12.fzu.cz/ms

- Mn local moments too dilute(near-neghbors cople AF)

- Holes don't polarizein pure GaAs

- Hole mediated Mn-Mn FM coupling

Page 4: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

• Tc linear in MnGa local moment concentration • Falls rapidly with decreasing hole density in more than

50% compensated samples• Nearly independent of hole density for compensation < 50%.

Intrinsic properties of Ga1-xMnxAs

As

GaMn

Mn Mn

super-exchange(anti-ferro)kinetic exchange

(RKKY)

hole density (nm-3) hole density / Mn density

room-Tcfor x=10%

Effective kinetic-exchange Hamiltonian, microscopic TBA or LDA+U

Page 5: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Extrinsic effects - covalent SC do not like doping→ self-compensation by interstitial Mn

Interstitial MnI is detrimental to magnetic order:

hcompensating double-donor – reduces carrier density

hattracted to substitutional MnGa acceptor and couples

antiferromagnetically to MnGa even at low compensation

Yu et al., PRB ’02; Blinowski PRB ‘03; Mašek, Máca PRB '03

MnGa

As

Ga

MnI

+

-

Page 6: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Theoretical linear dependence of MnGa on total Mn confirmed experimentally

Generation of MnI during growth

Mnsub

MnIntObtain Mnsub & MnInt assuming change in hole density due to

Mn out diffusion

I

Ga

Jungwirth, Wang, et al. PRB (2005)Total Mn doping

MnGa

As

Ga

MnI

+

-

no signs of saturation of MnGa

Page 7: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Tc in as-grown and annealed samples

0 1 2 3 4 5 6 7 8 9 100

20

40

60

80

100

120

140

160

180

T C(K

)

Mntotal(%)

-1 0 1-0.1

0.0

0.1T = 172 K8% (G a,M n)A s

M

[110

](T) /

MSa

t(5K

)

M agnetic F ie ld [ O e ]

Tc=173K

1.7% Mn2.2% Mn3.4% Mn4.5% Mn

6.7% Mn9% Mn

5.6% Mn6.7% Mn8% Mn

Open symbols as-grown. Closed symbols annealed

Total Mn doping (%)

Page 8: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

MnGa

As

Ga

MnI

+

-

Linear increase of Tc with effective Mn moment doping

Tc increases with Mneff when compensation is less than ~40%.

No saturation of Tc at high Mn concentrations

Closed symbols are annealed samples

0 1 2 3 4 5 6 70

20

40

60

80

100

120

140

160

180

T C(K

)

Mneff(%)

High compensation

Mneff = MnGa-MnI

Effective Mn doping (%)

Page 9: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Universal scaling of Tc per Mneff vs. hole per Mneff

hole density / Mneff density

theory theory expectationsexpectations

experimentexperiment

No signs of approaching an intrinsic Tc limit in current (Ga,Mn)As materials yet

Robust mean-fieldferromagnet

Page 10: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Prospects for higher Tc in (Ga,Mn)As

- Effective concentration of uncompensated MnGa moments has to increasebeyond 6.2% of the current record Tc=173K sample

- Charge compensation not so important unless > 40%

- Technology (precise control of growth-T, stoichiometry) is expectedto move Tc above 200K

- Tc above 400 K needed for widespread applications

Page 11: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

The central tension in dilute moment systems

- Keep the number of moments (local and band-electrons) large for large Tc

- Keep the number of moments low to retain semiconductor characteristics

The central question in dilute magnetic semiconductors materials

- Where to find the factor of ~2 Tc enhancement?

How far can we go (physics and technology wise) with doping andlocal-carrier moment coupling strength while still increasing Tc?

Which semiconductor host is optimal?

2. Other related diluted magnetic semiconductors2. Other related diluted magnetic semiconductors

Page 12: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Magnetism in systems with coupled dilute moments and delocalized band electrons

(Ga,Mn)As

coup

ling

stre

ngth

/ Fe

rmi e

nerg

y

band-electron density / local-moment density

Page 13: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

(III,Mn)V materials: Microscopic picture of Mn-hole coupling in (Ga,Mn)As

L

Mn

Ga

As

Ga s-orb.

As p-orb.

1 Mn0.1eV acceptor many Mn

d5 ↑

d5 ↓

As 4p - Mn 3d

hybridization

GaAs Mn

Page 14: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

d4

d

Internal reference rule

Weak hybrid. Delocalized holeslong-range coupl.

Strong hybrid.Impurity-band holesshort-range coupl.

d 5 → d 4 no holes

InSb, InAs, GaAsTc: 7 → 173 K

(GaN ?)

GaP Tc: 65 K

Mn d ↑ level

Mn acceptorlevel

Mn d ↓ level

Other III-V hosts

Scarpulla, et al. PRL (2005)

d5

Page 15: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Mn d ↑ level

Mn d ↓ level

Ed↓

Ed↑

|Vpd|2 ~ alc-7

Hole - local moment Kondo coupling:

Mixed (Al,Ga)As and Ga(As,P) hosts

1/|Ed↓| + 1/|Ed↑| ~ const.

=Mean-field Curie temperature:

4% in GaP and AlAs50% in GaP

Page 16: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Smaller lattice const. more importantfor enhancing p-d coupling than larger gap

↓Mixing P in GaAs more favorable

for increasing mean-field Tc than Al

No dramatic decrease in the LDA+Urange of Mn-Mn interactions

p-d coupling and Tc in mixed

(Al,Ga)As and Ga(As,P)

Mašek, et al. to be publishedMicroscopic TBA/CPA or LDA+U/CPA

Page 17: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

GaAs

Total concentration of Mn

MnGa

MnI

theory & exp.

Additional motivation for MBE research:Mixing P in GaAs might lead toeasier incorporation of MnGa

Mn formation energies in mixed Ga(As,P)

theory

III-V [(Ga,Al)(As,P)] based ferromagnetic semiconductors:

- adding few % of one type of dopand (Mn) in a common semiconductor

but the simplicity brings limitations

- Mn solubility limits; correlated local-moment and carrier densities;

p-type only

Page 18: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Kudrnovský, et al. to be published

III = I + II → Ga = Li + Zn

GaAs and LiZnAs are twin SC

- Band gaps 1.5 eV vs. 1.6 eV

- similar band dispersions

- similar GS charge densities

- similar phonon dispersions, ...

No solubility limit for MnZn

Wei, Zunger '86;Bacewicz, Ciszek '88;Kuriyama, et al. '87,'94;Wood, Strohmayer '05

Page 19: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Large electron densities in non-stoichiometric n-type Li(Zn,Mn)As

interstitial Li in

Ga tetrahedral

position +

5% Mn 12.5% Mn

Page 20: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

L

As p-orb.

Ga s-orb.As p-orb.

Mean-field Tc

theory

EF

Also, comparable LDA+U range of Mn-Mn interactions in n-type Li(Zn,Mn)As as in p-type (Ga,Mn)As

p-d hybridization quickly buildsup when moving from CB Γ-point

↓n-type DMS ferromagnetism

Li(Mn,Zn)As: similar to (Ga,Mn)As but lifts all the limitations of Mn solubility; correlated local-moment and carrier densities; p-type only

Page 21: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

3. AMR3. AMR (anisotropic magnetoresistance) effects in (Ga,Mn)As

Band structure depends on Band structure depends on MM→

Ferromagnetism: sensitivity to magnetic field

SO-coupling: transport coefficients depend onangle between magnetization and current (crystal axes)

M || <100>

M ||

<010

>

GaMnAs

ky

kx

Page 22: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Gould, Ruster, Jungwirth, et al., PRL '04, '05

[100]

[010]

[100]

[010]

[100]

[010]

((Ga,Mn)AsGa,Mn)As

AuAu

- no exchange-bias needed

- spin-valve with ritcher phenomenology than TMR

Tunneling AMR: anisotropic tunneling DOS due to SO-couplingMRAMMRAM

[010]

Φ

Magnetization[110]

[100]

[110][010]

θ

Current

Page 23: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Magnetisation in planey

x

jt

z

Wavevector dependent tunnelling probabilityT (ky, kz) in GaMnAsRed high T; blue low T.

xz

y

jt

constriction

Magnetization perp. to plane

Magnetization in-plane

Giddings, Khalid, Jungwirth, Wunderlich et al., PRL '05

thin film

Page 24: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

TAMR in metals

Bolotin,Kemmeth, Ralph, cond-mat/0602251

Shick, Maca, Masek, Jungwirth, PRB '06

NiFe TAMR TMR

TMR ~TAMR >>AMR

ab-initio calculations

Viret et al., cond-mat/0602298 Fe, Co break junctions TAMR >TMR

Page 25: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Coulomb blockade AMR

Spintronic transistor - magnetoresistance controlled by gate voltageSingle-electron FET

Narrow channel SETdots due to disorderpotential fluctuations

Strong dependenceon field angle→hints to AMR origin

Huge hysteretic low-field MR

Sign & magnitudetunable by smallgate valtages

spin-coherent (resonant)tunneling unlikely origin

CB oscillationslow Vsd → blockeddue to SE charging

Wunderlich, Jungwirth, Kaestner et al., cond-mat/0602608

Page 26: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

AMR nature of the effect

normal AMR Coulomb blockade AMR

Page 27: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

magnetization angle θ

CB oscillation shifts by magnetication rotations

At fixed Vg peak → valleyor valley → peak

MR comparable to CBnegative or positive MR(Vg)

Page 28: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

Microscopic origin

Source Drain

GateVG

VDQ

∫ =→==Q

0

2

D'

D'

C2QUC/QV&)Q(VdQU

ΣΣ

TkC2e

B

2

→→ Coulomb blockadeCoulomb blockade

•• VVgg = 0= 0

•• VVgg ≠≠ 00

GG0

20 VCQ&

C2)QQ(U =

+=

Σ

Q=Q=nene -- discretediscreteQQ00==CCggVVgg -- continuouscontinuous

QQ00==--nene →→ blockedblocked

QQ00==--(n+1/2)e(n+1/2)e →→ openopenn-1 n n+1 n+2n-1 n n+1 n+2

ΔEC

QQindind = = nnee

QQindind = (= (n+1/2)n+1/2)eeQ0

Q0

e2/2CΣ

Page 29: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

chemical potential depends on MrSpin-orbit coupling →→

If lead and dot differentIf lead and dot different(different carrier concentrations in our (Ga,Mn)As SET)

∫ −=+=Q

0DL

'D

' )M()M()M(&e

)M(Q)Q(VdQUrrr

r

μμμΔμΔ

GMMGG0

20

CC

e)M(V&)]M(VV[CQ&

C2)QQ(U Σ

Σ

μΔr

r=+=

+=

electric && magneticmagneticcontrol of Coulomb blockade oscillations

Page 30: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

•• CBAMR if change of |CBAMR if change of |ΔμΔμ((MM)| ~ )| ~ ee22//22CCΣΣ

occurs when anisotropy of band-structure derived parameter comparable to independent energy scale (single-electron charging) → distinct from all other AMRs

•• In (In (Ga,Mn)AsGa,Mn)As ~ ~ meVmeV (~ 10 Kelvin)(~ 10 Kelvin)

•• In roomIn room--T T ferromagnetferromagnet change of change of ||ΔμΔμ((MM)|~100K )|~100K

Page 31: Materials physics in ferromagnetic semiconductors and AMR ...online.itp.ucsb.edu/online/spintr06/jungwirth/pdf/Jungwirth_KITP.pdf · Materials physics in ferromagnetic semiconductors

• Combines electrical transitor actionwith permanent storage

• n-type or p-type FET characteristicswitched by magnetization rotation