Forschungszentrum Jlich

Combining Ferroelectricity, Magnetism, and Superconductivity Supe co duct ty in Tunnel u e Junctions Ju ct o s

H. Kohlstedt1, N. A. Pertsev2, A. Petraru1, U. Poppe1, and R. Waser1
1CNI

Center of Nanoelectronic Systems y for Information Technology (IFF-IEM) 2A.F. Ioffe Physico-Technical Institute, Russian Academy of Sciences, 194021, St. Petersburg, Russia

Arusha, Tansania August 2007

Layer Sequence of a Tunnel Junction

Tunnel Barrier (1 nm 3 nm) Dielectric

Top electrode (50 nm)

Substrate Bottom B tt Electrode (50 nm)

Outline

Electron Tunneling and Junctions (Overview) F Ferroelectric l ti T Tunnel lJ Junctions ti Size Effects and Boundary Conditions Tunnel Junction: An Interfacial Device A novel zoo of Tunnel Junctions

Electron Tunneling and Junctions

Quantum Mechanical Electron Tunneling

E

kx real
A

e
kx
imaginary

kx

real

C
x

B
Transmission coefficient
t 2 = T C exp 2m ( x) dx h 0

Frenkel, Phys. Rev. 36 (1930).; A. Sommerfeld and H. Bethe, Handbuch der Physik, Springer 1933, XXIV, p.450 R. Holm and W. Meissner, Z. Phys. 74, 715 (1932).

Tunnel Junctions: A short Survey y

Me I Me Su I Su Mag I Mag Semic I Me

Eg

R/R

V
Sommerfeld/Frenkel/Holm

Giaever/Josephson

Jullier/Moodera/Parkin/ (Sun/Fert for oxides)

Esaki

Superconducting -, Magnetic-, and Ferroelectric Tunnel Junctions

Dielectric barrier

Density of states effects

Superconductor

Superconductor

Magnet

Magnet

I (V ) =

2 e A h

T ( E ) n1 ( E eV ) n2 ( E ) [f ( E eV ) f ( E )]dE
Ferroelectric tunnel junction:
Metal Metal

Cooperative phenomenon located in the barrier !

Ferroelectric Barrier

Ferroelectric Tunnel Junctions

Ferroelectric Tunnel Junction

Kohlstedt, Pertsev, Waser, Ferroelectric Thin Films X, Vol. 688 (M t i l R (Material Research hS Society) i t ) 2002 2002, p. 161 161. European Patent: 0 657936 A1, A1 1994 R. M. Wolf and P. W. M. Blom, Philips p Electronics, , Eindhoven (NL).

IBM Technical Disclosure Bulletin 13, 2161 (1971).

Patent Experiment

Ferroelectric Tunnel Junction

High-Resolution TEM, C. Jia, Jlich

SrRuO3

e-

++++++++++++++++++++++++

10 unit cells PZT

---------------------------------4 nm

SrRuO3

x1 2 = T C exp e p 2m ( x ) dx d x0 h

Tunneling matrix element:

Quantum Mechanical Electron Tunneling

Polarization State of PZT

Current-Voltage Curve?

Possible Effects: Tunnel Current vs. Polarization

H. Kohlstedt et al., Phys. Rev. B 72, 125341 (2005).

Strain: Barrier Effects

a. Variation of barrier thickness
t -t 0

t = to + d 33 V

-VC

VC
Voltage

b. Shift of the conduction and valence band edges * t 2 m 0 T = C exp 4 E Ez dz h 0 2 2 2 = + k k z k

C

h 0 + 3 S 33 EC = EC

k z2 =

2m *
2

0 EC Ez

)
3
Deformation Potential: Brooks 1955, Herring 1956, Kane 1970

c Change of the electron effective mass c. a: lattice parameter, Tight binding approx. 2h * m = 2 ,k =0 * * * m d 33 V * * m a EC m = m0 + S33 = m0 + S33 S 33 t0

Interfacial Effect
Symmetric barrier structure I t t`

1 1 2

2 1

Electrode

Ferroelectric Electrode

S Symmetric t i I-V IV
I

Asymmetric barrier structure

a = (1 + 2 )/2

variable fixed

b = (1 + 2 ) / 2

2
V

Asymmetric I-V

Origin of Giant Electroresistance (from E. Tsymbal, U Lincoln, Nebraska)

Metal

+ + + +

FE
P

Metal

Metal
+ + + +

FE
P

Metal

Electrostatic Potential

Tunneling Potential

EF

EF

Different potential (and barrier width) for transport electrons

M.Ye. Zhuravlev R. F. Sabirianov S. S. Jaswal and E.Y. Tsymbal, PRL 94, 246802 (2005)

BaTiO3: 5nm
SrRuO3 BaTiO3 SrRuO3 SrTiO3

E (kV/cm) (kV/ ) 16 14
P (C C/cm )
2

E (KV/cm)
800 1200
30 20 10 0 -10 -20 -30 -1200 -800 -400 0 400 800 1200

-1200 -800 -400

400

@100 Hz H

12 pF) C (p 10 8 6 4 2 f=1000 Hz@ 300K -0,6 -0,4 -0,2 0,0 U (V) 0,2 0,4 0,6

-0.6

-0.4

-0.2

0.0

0.2

0.4

0.6

U (V)

Similar to: Y.S Kim et al., APL 86, 102907 (2005).

I-V curve of a SRO/BTO/SRO Junction

100
I (A)
2.9 nm BTO at 1 kHz

50 0 -50 -100 -1,0

2.9 nm BTO

-0,5

0,0
U (V)

0,5

1,0

Could not detect displacement current

Current Transport Measurements

Pt

Electric Field [kV/cm]

-2000 0.5 -1000 0
3

PbZr0.52Ti0.48O3 SrRuO3

1000

0.2

t [mA] Current

6 nm PZT
0.0
8 5

4 1

0.0

-0.2 -0.5 0.5

7 6

@300 K
-0.5 0.0 0.5

-0.4 1.0

-1.0

Voltage [V]

J. Rodriguez Contreras et al., APL 83, 83 4959 (2003) (2003).

No direct (elastic) tunnling Switching not caused by ferroelectricity! K. Szot et al., Nature Mat. 2006

Curre ent Density [kA/cm m]

SrTiO3

Size Effects and Boundary Conditions

1
12 1999
Tybell (PZT)

Numbe er of unit cells

10 2
Ghos sez and R Rabe (PT TO)

0 2000 2001 2002 2003 2004 2005 2006

Pertse ev (PTO)

4
Streiffer (P S PTO)

Ultra thin Ferroelectric Oxide Films

Year
0.4 nm

Junquera an nd Gh hosez (BT TO) Strei iffer (PTO O) Lichtenste L eiger (PTO O) Kim (BTO) an (PZT) Nagaraja Ra appe (PTO O) Gerr ra (BTO)

5 nm

Electro on direct tunneling regime

Strain enhanced Ferroelectricity

N.A. Pertsev, et al., Phys. Rev. Lett. 80, 1988 (1998) K. J. Choi, et al., Science, 306 1005 (2004).

Film

Substrate: side view

E h Enhancement of f P possible ibl

Sm = (b a0)/b
b = Substrate lattice parameter a0 = Equiv. cubic cell constant of free film, Prototypic cell

out-of-plane c b a in plane in-plane

Sm: Misfit strain

Electrical Boundary Conditions

Metal
_____________________
+++++++++++++++++++++

E ds = 0

ED 0
(only for

ED

perfect screening!!)

P. Wrfel and I. P. Batra , Ferroelectrics 12, 55 (1976). J. Juncquera and Ph. Ghosez, Nature 422, 506 (2003).

+++++++++++++++++++++

_____________________

Metal

Tunnel Junction: An Interfacial Device

Tunnel Junction: An interfacial device!

F Fermis i Golden G ld Rule R l Initial State Travel Final State

Tunneling g electrons are extremely y sensitive to barrier and interface properties!! examples? examples?

Tunneling electrons - coupling to excitations

(Inelastic) Electron Tunneling Spectroscopy Molecule and Phonon Spectroscopy

P. Balk, JAP 1991

Electron-Phonon C Coupling li 2 (,k) k)

E. L. Wolf, PRB 1985

Magnons
J. S. Moodera, PRL 1998

n-Si/SiO2/Al

Nb/MgO/Ag

Co/Al2O3/Ni80Fe20

Magnetic Oxide Tunnel Junctions

LSMO/SrTiO3/LSMO @4.2 K

3 nm SrTiO3 barrier
Y. Lu et al., PRB 54, R8357 (1996).

Interface Effect in Magnetic Tunnel Junctions

Spinpolarization influenced by Barrier Material J. M. De Teresa et al., Science 286, 507 (1999).

Tunneling Magneto Resistance An Interface Effect! Fe MgO Fe

Ch. Heiliger et al Ch al., Phys. Rev. B 73, 214441 2006 , G. Mathon J. S. Moodera, JMMM 200, 248 (1999).

First layer adjacent to tunnel barrier is essential!

Drastically change in TMR!!

Electrical Boundary Conditions: An endless story

Metal
_____________________
+++++++++++++++++++++

E ds = 0

ED 0
(only for

ED

perfect screening!!)

P. Wrfel and I. P. Batra , Ferroelectrics 12, 55 (1976). J. Juncquera and Ph. Ghosez, Nature 422, 506 (2003).

+++++++++++++++++++++

_____________________

Metal

Alternative Screening Mechanism Ionic Screening

Fong, et al., Phys. Rev. B 71, 144112 (2005).

Theoretically confirmed: G. Gerra et al., PRL (2006).

Alternative Screening Mechanism

metal ferroelectric

Thomas-Fermi Th F i screening i and d Kretschmer-Binder effect

CTF

CKB Bond B d charge h compensation ti b by f free carriers in the ferroelectric

Extension E t i of f the th ionic i i polarization l i ti into the metal; Ionic distortion also in the metal Sketch taken from G. Gerra et al., PRL 96. 107603 (2006). Fig.1

Magnetoelectric Interface Effect

Fe/BaTiO3
P P
Interface between a ferromagnet g and a ferroelectric
Top interface

Minority-spin charge density

DOS

Paraelectric BTO

Bottom interface

Ferroelectric BTO

C.-G. Duan, S.S. Jaswal and E. Y. Tsymbal, PRL 97, 047201 (2006).

EF

Interface without Ionic Screening

BaTiO3

SrRuO3

Interface with Ionic Screening

Local atomic rearrangement g at the interface

Ferroelectric

Magnet or S Superconductor d t

Variation of DOS at the interfaces Tunneling current modified by interface properties

TMR vs. P?

Josephson-Effects vs. P?

Magnetic and superconducting junctions with ferroelectric barrier

La0.33Sr0.67MnO3 BaTiO3 La0.33Sr0.67MnO3 P

LaxSr1-xCuO3 BaTiO3 LaxSr1 1-x xCuO3

The (ferroelectric) Th (f l t i ) polarization l i ti might i ht modify the spin polarization and superconducting order parameter ( 0.1 nm) (at the interfaces)

Tunneling magneto resistance as well as quasiparticle current and Josephson current should depend on P!

An optimistic Outlook: A novel zoo of tunnel junctions

Pyroelectric Piezoelectric Dielectric

Paramagnet (Anti)-Ferromagnet P, ,M S Superconductor d

+ + + -

Ferroelectric Anti-ferroelectric
Multiferroic (I (Insulator) l t ) (Tunnel Barrier)

+ + + -

Magnetic g Anti-ferromagnetic

Josephson-Junction Josephson Junction with a ferroelectric barrier dc and ac Josepson Effect vs. P? Magnetic Tunnel Junction Tunnel Magneto Resistance vs. P?
E. Y. Tsymbal and H. Kohlstedt, Science 2006

Multiferroic Tunnel Junctions

M. Gajek et al., Tunnel junctions with multiferroic barriers Nature Mat. 2007 Sheng Ju et al, PRB 75, 064419 2007

La: BiMnO3 4 bit Memory: 2 from Ferroelectricity 2 from Magnetism

More about Multiferroics: N A N. A. Spaldin and M M. Fiebig Fiebig, Science (2005). R. Ramesh et al R al. Phil Mag. Lett. (2007). W. Eerenstein, e e ste , N. D. Mathur, at u , J. F. Scott Nature (2006).

Conclusion
Quantum Mechanical Electron Tunneling and M ltif Multiferroic i Materials: M t i l of new tunnel junctions j New Functionalities Will propel exciting theoretical approaches Tunneling T li Electrons El will ill be b applied li d as an analytical l i l tool l Better understanding of multiferroic materials on the nm level Multiple size effects Challenge: Defect free/ideal ferroelectric tunnel barriers, I- V curves alone are not sufficient to extract I the underlying switching mechanism There is a gap between theory and experiment!
Development p

Center of Nanoelectronic Systems for Information Technology

Acknowledgement Sponsors:
Volkswagen-Foundation: N Nano-sized i df ferroelectric l ti h hybrids b id under d contract t t number b I/77 737 Joint NSF-DFG Project: University of Berkeley (Material Science Department) University of Aachen (RWTH) Research Center Juelich DFG: Displacive and Conductive Phenomena in Ferroelectric Thin Films: Scaling effects and switching properties properties Synchrotronstrahlungsexperimente zu Skalierungseffekten und ungewhnlichen g Phasen epitaktischer, p ,p perowskitscher Schichten