Graphene electronics

‐ Wei‐Li Lee  IoP, Academia Sinica

OUTLINE
• Review on recent progress in graphene
• Device fabrication – mechanical exfoliation v tv t v
j = σE + α (−∇T )
• QHE and Thermopower in high magnetic field
• Novel phase near CNP in spin-polarized QH system e2
σ xy = n α xy = ?
• Conclusion h
 honeycomb

Single atomic layer of carbon sheet 

Each 12C  :  (He) 2s22p2 Chicken wire 

3 x sp2 hybridized orbitals + one π electron  

 Electronic Structure : Tight Binding Model
• Hamiltonian :

B
H int = −t ∑ [a
<i , j > ,σ
+
iσ b jσ + H .C. ]
e‐
A
− t' ∑ [(a
<<i , j >> ,σ
+
iσ ]
a jσ + b + iσ b jσ ) + H .C. + H imp.

• Eigen energy Ek ( neglect t ’ and Himp):
Ek =
1/ 2
⎡ 3a 3a 3a ⎤
t : nearest neighbour Hopping amplitude  ± t ⎢1 + 4 cos( 2 k x ) cos( 2 k y ) + 4 cos ( 2 k x )⎥
2

⎣ ⎦

r r
Bandstructure of Graphene

E (q = K ) = 0
1

0.8 3
0.6 2.5
2
Dirac points
0.4
1.5
0.2
1
kya/π

0
0.5
-0.2 0
-0.4 In a perfect graphene 
-0.6 sheet μ crosses the 
sheet μ crosses the
-0.8
Dirac points
-1
-1 -0.8 -0.6 -0.4 -0.2 0 0.2 0.4 0.6 0.8 1
kxa/π
• Low energy Hamiltonian : expand around the Dirac point 
K→K1+k ( K1 is one of the 6 Dirac points or vertices)
• Dirac’s (relativistic) equation with zero mass

v v ⎛ 0 k x − ik y ⎞ ⎛ψ ⎞ ⎛ψ ⎞
⎜
Η = hυ Fσ ⋅ k = hυ F ⎜ ⎟ , Η ⎜⎜ A ⎟⎟ = E ⎜⎜ A ⎟⎟
⎝ k x + ik y 0 ⎠⎟ ⎝ψ B ⎠ ⎝ψ B ⎠

Pauli “spin” matrices  “Pseudospin” state 
v v
E (k ) = ±υ F h k , υ F ≈ 10 6 ms −1 Massless quasiparticle !

• Two Well
Two Well‐defined
defined chirality : 
chirality :
Positive for electron and negative for hole (positron) 
 Zhou, et al., Nat. Phys. 06’

υ F = 9.1×105 m/sec
Graphene electronics
Energy Dispersion in a Bi-layer Graphene : Tight-Binding Model
• Hamiltonian :
Bernal stacking [
H int = −γ 0 ∑ a + m ,i ,σ bm , j ,σ + H .C. ]
<i , j > , m ,σ

v
[ ] [
− γ 1 ∑ a1+, j ,σ a2, jσ + H .C. − γ 3 ∑ b1+, j ,σ b2, jσ + H .C. ]
j ,σ j ,σ
E v
+ O(γ 4 ) + V ( E ) + H impp.
o
a = 2.46 A SWM parameters :
γ0 ~ 3 eV, γ1 ~ 0.4 eV, γ3 ~ 0.3 eV, γ4 ~ 0.04 eV
‐‐ Castro Neto, et. al., Rev. Mod. Phys. 09’
, , y
• Low energy dispersion relation εk (neglect γ3, γ4 and Himp):
V2 γ 12
γ 14 3aγ 0
ε (V ) = ± h υ k + +
±±
k
2 2
F
2
± + (γ 12 + V 2 )h 2υ F2 k 2 , υ F ≡ ≈ 1× 10 6 m/s.
2 4 4 2h
εk(eV) εk(eV)
V=0 h 2υ F2 k 2 VK0
εk → ± ,
small k γ1 Δg ≈ V
V <<γ 1
h 2υ F2 k 2 Δg
+ γ1 ,
γ1
γ h 2υ F2 k 2
m = 12 ≈ 0.035me
* − − γ1
2υ F γ1
Graphene electronics
Chiral Fermionic Excitations in Graphene
• Effective low‐energy Hamiltonian : Pseudo‐spin state

) ⎛ψ ( A) ⎞ ⎛ψ ( A) ⎞
H J = ε J ( p ) σ ⋅ nJ (φ ), H J ⎜⎜ ~ ⎟⎟ = ε J ( p )⎜⎜ ~ ⎟⎟
⎝ψ ( B ) ⎠ ⎝ψ ( B ) ⎠
σ : Pauli spin matrices
) v
n J ≡ (− cos(( Jφ ), )) P = p eiφ
i ( Jφ )),
) − sin(
ε J ( p) = C J P J , C1 = υ F and C 2 = 1 / 2m*
• Two well‐defined Chirality (helicity) =  +1 or ‐1. 
)
σ ⋅ p = ±1
c.f. Helicity  :                       only for massless  ‐‐ McCann, et. al., PRL 06’
particles
• Chiral fermions with Berry’s phase Jπ.
Berry'
y s pphase acquired
q along
g p
path C v
~ r 1 k k‐space
γ ( C) = − ∫∫ B ⋅ dS = − Ω (C ) = − Jπ
C 2 v v Loop C
Pseudospin state ψ ∝ k J
 Laughlin’s Picture on Quantized Hall Conductivity in 2D

circumference L • Model system: a 2DEG system on a cylindrical surface

• Relate Ι to ΔV:
∂U ∂U
I= = ,
∂Φ L∂A
U : internal energy, Φ : total flux, and A : vector potential

• Require phase coherent, gauge invariance and single value

of wave function around the loop:
v
P → P − eA, and ψ (0) = ψ ( L)
nh h
⇒ A= or LΔA = (flux quanta, Φ 0 ), n : integer
eL e
• An increase of flux quanta h/e causing a transfer of n
electrons from one edge to the other.
‐‐ Laughlin, Phys. Rev. B 81’
neVH ne 2VH I e2
I= = ⇒ σ xyy = = n , n : integer.
Φ0 h VH h

Quantized Hall resistance
What about system with finite size ?
Graphene electronics
Ideal 2DEG with finite system size
Edge Current Model for QHE
Under high magnetic field
Under high magnetic field
Ιedge4
z x

y
v
B

Ιedge1
Ιedge3
e‐

‐‐ Halperin, PRB 82’ 
Ιedge2 Girvin, et. al., PRB 84’
• Incompressible when EF falls in the gap b/w LLs v tv t v
- ρxx=σxx = 0 and σxy = ne2/h j = σE + α (−∇T )
• In the absence of external bias, no net Ιedge
• When
Wh th there is a potential
t t ld difference
ff δV δΙy= Ιedge1-ΙΙedge3, is quantized.
δVx, t d
δI y = ne 2 / hδV → σ xy = ne 2 / h
Similarly for a temperature difference δTx,
• Similarly, δTx universal value in αxy ?
α xy ≡ J y /( −∇ xT ) = (k B e / h ) ln 2 ≈ 2.32 nA/K
‐‐ Checkelsky, et. al. PRB 09’
 Novoselov, et al., Nat. Phy. 06’

2‐DEG ge 2 Single‐layer graphene  Bilayer graphene 

free‐Fermion, σ xy = n 1 ge2
h y ,σ xy = (n + )
Berry’s Phase π, Berry’s phase 2π
2 h

• For a given B, D.O.S. at each Landau level = gB/Φ0
• Anomaly at N=0 Landau level in graphene
• Both N=0 and 1 are zero energy LLs in bilayer graphene  
Quantum Hall Effect at Room Temperature !

hυ F k BT
<< 1
En = sign
i (n)(2n) 1/ 2
ΔE
lB
For B = 29 Tesla, E1 − E 0 = 0.196eV = 2271K !!
1
cf : En = (n + )hωC , ΔE = hωC = 3.36meV = 39 K
2
 Thermopower in 2DES in Quantum Hall Regime
• Thermopower in 2DES GaAs/Ga
Thermopower in 2DES GaAs/Ga0.68Al0.32As 
As
mobility  > 105 cm2/V‐sec

• Unusual large S
Unusual large Sxx ~ 1 mV/K ! 
1 mV/K !
Theory 
k B ln 2 60 μVK −1
S xx = − =− .
e n +1/ 2 n +1/ 2
• Inconclusive results due to dominant 
Phonon‐drag effect even at low T.

• Graphene at 10 Tesla,  ΔE  ~ 700 K  single layer
ΔE  ~  630 K  bi‐layer  

‐‐ Fletcher, et. al., PRB 86’ and 88’
‐‐ Ruf, et al.,  PRB 88’
Graphene electronics

Mechanical Exfoliation of Graphite

“Seeing” a single atom thick graphene !

10 μm
10 μm
 Atomic Force Microscope Images
Atomic Force Microscope Images

3 layers 4 layers

Graphene
p ((single
g layer)
y )? 2 layers
y
Measured thickness ~ 0.8 nm > 0.34 nm
 Double Resonant Raman Process
‐ Ferrari, et al., PRL 06
Ferrari et al PRL 06

Single and sharp 2D peak in 
Single‐layer graphene  !!
 Raman Spectroscopy
Raman Spectroscopy
70
2D peak FWHM in Graphene
70 60

65
50

FWHM (cm-1)
60
55 40
-1
50 29.5(5) cm
M (cm )

30
-1

45
40
20
35
FWHM

30 10
25
20 0
0 1 2 3 4 5 6 7 8 9
15
Sample index
10
5
2D peak
k FWHM
0
0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16

Number of layers

Si l l
Single‐layer graphene  !!
h !!
Graphene electronics

Bi-layer Graphene Device for Thermopower

• Temp. modulation at f ~3 Hz,

δT~50-200mK
• Thermopower S detected at 2 f
by a lock-in amplifier
• Bottom Si substrate as gate
electrode

0.50
0.20
100K
Rt2 0.45
0.15

dT (K)
0.40

‐∇T 0.10

T ( Ω/K )
0.35
0.05
0.30
Rt1

Sens. dR/dT
0.00
0.25 0 5 10 15 20 25 30
2 2
I (mA)
heater 0.20

0.15

0.10

0.05 Rt1
Rt2

0.00
0 50 100 150 200 250 300

T (K)
Graphene electronics
Tuning the Chemical Potential
10 8
3.0
9 5K 6
8K 2.5

n (x 1 0 c m )
4

-2
8
20K 2
7
+Vg

12
0
2.0
-2
6
EF
-4
5 -6 1.5
4 -8
μ0H= 0T -4 0 -2 0 0 20
V g' ( V )
40
1.0 -Vg
3
Rxx (kΩ)

2 Vg

Ryx (kΩ)
0.5
1
0 0.0
-1 1T • Vg’=Vg-Vg0 (+10V)
-0.5
-2
-3
10 • R0 : sheet resistance Rxx at charge
-1.0
-4
8 neutral point(CNP)
R0 weak T d
dependence
p d below 20K
K
R0 (kΩ)

6
-5
5 15
-1.5
2
-6 4 μ ~ 3000 cm /V-sec
-7 2
-2.0 • Ambi-polar field effect device
-8 0
n0 < 1x1011 cm-2
-2.5
-9
0 5 10
T (K)
15 20 25
μ~ 3000 cm2/ V-secV
-10 -3.0
-40 -30 -20 -10 0 10 20 30 40

Vg ( V )
Graphene electronics

12
Quantum Hall Effect
Q
8
• Hall conductivity
4 σxy = ±n (4e2/h),
/h) n=1
n=1, 2,
2 3…
3
σxy ( e /h )

⇒signature for a bilayer graphene

2

0 20

15 15 T
• Landau Level energy
R0 ( k Ω )

-4
10

5
0T E N = ± hωc N ( N − 1)
-8
0
0 10 20 30 Double degeneracy N=0,1 at zero
-12
T(K)
energy
10 8K
15 K
μ0H = 15 T πˆ Jψ n < J = 0
20 K
8 25 K for J = 2, ψ 0 and ψ 1 both has zero eigen energy.
30 K
σxx ( e /h )

40 K • Minor drop of slope in σxy around CNP.

2

6 60 K
80 K
4 100 K
D.O.S.
2

0 − 2 hω c 0 + 2 hω c Energy
-30 -20 -10 0 10 20 30 40 50 60 70 80

Vg ( V ) N=2 N=0,1 N=2

Graphene electronics
8
20
μ0H=
7 Lifting of Spin Degeneracy
6
• Double peaks feature in Gxx for E0 state only !

R 0 ( kΩ )
18 15 T 5
13 T
4
10 T
7T 3 • Zeeman energy
16
Gaussian fit 2 gμBB ~ 9 K at 7 Tesla
1 Further enhanced by exchange inter.
14
0
0 5 10 15 20 25 30 spin gap ~ 450K at 10 Tesla*
12 T(K)
• Width of Disordered-broadened LL
σxxx (e /h)

WL ~ 180K < ΔE ~530K in bi-layer

2

10
• Edge channels contribution
EZeeman~300 K ⇒ Rxx at CNP not thermally activated
8
⇒ Double Gaussian fitting reveals excess Gxx
6 Spin‐polarized
Spin polarized
D.O.S.
4

2 − 2 hω c 0 + 2 hω c Energy
WL ~ 180K N=2 N=0,1 N=2
0
-40 -20 0 20 40

Vg ( V )
* Abanin, et. al., PRL 06’
 Graphene electronics
Bi-layer graphene
Bi-S37
120
|S m|
Bi-layer graphene |S| at V g = 80 V

100
100 fit curves
Thermo electric Power
Thermo-electric
80 1/2
~T

Sm| ( μ V/K )
80 60
• Particle-hole sym. w.r.t. CNP

|S
40
60 ~T
• Thermopower attends a maximum Sm at
40
20
n~2x1012 cm-2
0
0 50 100 150 200 250 300

• Away from CNP, S ~ 1/Vg .

S ( μ V/K )

T(K)
20
c.f. Free e model,
15 K
0 π 2 k B k BT 1
30
50 S≈− ( )∝
-20
1.0
80 2 e εF εF
120
0.5
160
200
-40 240 • Near CNP,, Sm scales as T1/2 ?
1/S

0.0
300 280
-60 120
-0.5 300
50
-80
-1.0
10

-80 -60 -40 -20 0 20 40 60 80

-100 Vg ( V )

-80 -60 -40 -20 0 20 40 60 80

Vg ( V )
Graphene electronics
Bi-layer graphene
30 30
Thermopower under High
25
μ0H = 15 T
Magnetic Field
T = 15 K
20 Syx 25
•Sxx (Syx) antisym. (sym.) w.r.t. CNP
15

10 20 • Syx (Sxx ) reaches minimum (maximum)

Gxx ( e /h )
whenever
h μ crosses the
th EN. Syx max =
S ( μ V/K )

5 20μV/K at CNP.

2
0 15
• More p physical
y insight
g to look at the
-5 Sxx Peltier conductivity α
J = σE + α (-∇T)
-10 10
• αyx = Jy/(-∇T)
/( ∇T)x : a d
directt measure off
-15
transverse current.
-20 5

-25

-30 0
-80 -60 -40 -20 0 20 40 60 80

Vg ( V )
Graphene electronics

Charge Current Driven by a -∇T : Peltier Conductivity

• Current density  Peltier conductivity

ji = σ ij E j + α ij (−∂ jT )
z //+B
v v
• In steady state, j=0, ∇
In steady state j=0 ∇yT=0 j , ((-∇T) y
⎧α xx = σ xx S xx − σ xy S yx x
⎨
⎩α xy = σ xy S xx + σ xx S yx
− Ex
S xx ≡ , th
thermopower.
| ∇T |
Ey
S yx ≡ , off - diagonal thermopower ( Nernst effect).
effect)
| ∇T |

⇒ αxx, α
αxy can be determined by measuring ρ
can be determined by measuring ρxx, ρ
ρyx, SSxx, SSyx . 
 Graphene electronics
Bi-layer graphene
30 Peltier conductivityy
6
μ0H = 15 T
• At CNP, αxx is zero and αxy exhibits a
T = 15 K broad peak feature as in Gxx
25
4
αxy • αxx (αyx) antisym. (sym.) w.r.t. CNP
20
2 • Peak values of αxyy ≅ 2.1-3.3 n A/K

h)
Gxx (e /h
α (nA/K)

2
• Universal value by edge current model ?
0 15
αxx gk Be
α xy max = ln 2 ≈ 9.1 n A / K
h
-2
10
δI y = I y ,hot − I y ,cold is quantized.
quantized
-4
Gxx 5
Hot cold
-6

0
-80 -60 -40 -20 0 20 40 60 80

Vg ( V )
‐‐ Checkelsky, et. al., PRB  09’
Graphene electronics
Bi-layer graphene
30
15 K μ0H = 15 T
0.4
0.4 20 K
25 K 15 K
25 20 K
25 K

NP ( n A/K )
0.3

2
0.2
20
αxy//T (nA/K )
2

α /T at CN
0.2

Gxx (e /h)
2

xy
0.0 15
0.1
k BT 25K
25 K
~ ~ 0.14
WL 180 K
10 0.0
-0.2
0.2 0 3 6 9 12 15

μ 0H ( T )
Gxx
5
-0.4
<0 2 αxy/T = 0.2n
• For kBT/WL<0.2, 0 2n A/K2
⇒Indep. of T, B and LL index N
0
-80 -60 -40 -20 0 20 40 60 80

Vg ( V )
 25 12
S45, S37
20
μ0H = 15 T 11 N = 0 (1)
T = 15 K N=2
Syx 4 x (ln2)kBe/h
S ( μ V/K ) 15 10 N=3
N=4
10
9
5
8

K)
0

αxyy, peak ( n A/K

7
-5 Sxx
16 6
10 Double Gaussian Fit 0.5
12 5 Brown 15 K
Blue 20 K
8

αxy, peak/T ( n A/K )

8 0.4 Red 25 K

2
σxx ( e /h )

σxy ( e /h )
4 x S37 after I anneal
4 0.3
2

2
6
0 3
0.2

4 -4
4
2 0.1
-8 αxy/T = 0.19 ± 0.03 n A/k
2

2 1 0.0
-12 6 9 12 15
μ0H ( T )
0 -16 0
4 0 10 20 30 40 50 60 70 80 90 100

3 αxy T(K)
2 • For kBT/WL>0.5 , αxy saturates to 4xkBe/h (ln2)
A/K )

1
α(nA

0 •For kBT/WL<0.2, αxy/T = 0.2n A/K2

-1 αxx ⇒Indep. of T, B and LL index N
-2 kBT
-3
LL
-80 -60 -40 -20 0 20 40 60 80
Vg ( V ) ‐‐ Lee et. al, PRL 04’; Zhu et. al., PRB 10’
 Semi classical Transport Equations (Mott Relation)
Semi-classical
• Current density in the presence of E and (‐∇T):
v v t v t ∂f 0 v ⎡ v ε − μ v ⎤
J = 2 ∫ eυ k g k dk , g k = (− )τυ k ⋅ ⎢eE + (−∇T )⎥
∂ε ⎣ T ⎦

• From definition:  J = σ E + α (‐∇T)

π 2 k B2T 1 ⎛ ∂ ln σ ⎞
S xx = ⎜ ⎟ ⇒ Mott relation
3 e σ ⎝ ∂ε ⎠ε = μ ‐‐ Cutler and Mott, PR 69’

⎧ Ey π 2 k B2T ⎛ ∂ tan θ H ⎞
⎪S yx ≡ = ⎜ ⎟
⎪ | ∇ T | 3 e ⎝ ∂ε ⎠ε = μ
⎨
⎪ α xyy ≡
Jy π 2
k 2
T ⎛ ∂σ xy ⎞
= B
⎜⎜ ⎟⎟
⎪
⎩ | ∇ T | 3 e ⎝ ∂ ε ⎠ε = μ
 Bi-layer graphene Bi-layer graphene
-1.2 35 -20
μ0H = 15 T μ0H = 15 T
-1.0 30
0.4 T = 15 K T = 15 K -15
25
-0.8
20
-0.6 -10
15

anΘH)/dVg (arb.)
0.2

dσxy/dVg (arb.)
-0.4
A/K )

10
2

-5

K)
S ( μ V/K
-0
0.2
2
αxy/T (nA

5
0.0 0.0 0 0

0.2 -5

d(ta
5
0.4 -10
-0.2
-15
0.6 10
-20
0.8
-25
-0.4 15
1.0
dσxy/dVg -30 d(tanθΗ)/dVg
12
1.2 -35
35 20
-80 -60 -40 -20 0 20 40 60 80 -80 -60 -40 -20 0 20 40 60 80
Vg ( V ) Vg ( V )
• Relatively smaller particle
particle-hole asym in thermotransport → hot spot shorting effect in σxy.
hole asym.
• Near CNP, deviation from the fitting of Semi-classical transport equations ( Mott relation)
Graphene electronics

Spin‐polarized  QH states 
Edge Current in QH System
• Large spin gap due to enhanced Zeeman splitting  
by exchange interaction ( ~450K
by exchange interaction (  450K at 10 Tesla)
at 10 Tesla)
Spin  up
• Gapless chiral edge states at N=0.
⇒ counter
counter‐propagating
propagating edge states carrying 
edge states carrying
Spin  down opposite spin ! 

• Key features for the edge transport  
y g p
¾ Double peaks in Gxx and tilted plateau in Gxy .
¾ Large peak in ρxx at CNP (ν=0)
¾ Short circuiting though bulk results in the 
decrease in ρxx at finite ν.   

‐‐ Abanin, et. al., PRL 06’ 07’
 Comparison to Thermopower in Single Layer Graphene

‐‐ Wei, et. al., PRL  09’
‐‐ Checkelsky, et. al., PRB  09’
1
• At high carrier density,   S xx ≈
Vg
• Unusual large Syx at CNP  and deviation from Mott relation

• N=0 LL, spin degeneracy is not lifted even at 14 Tesla  
Gxx does not show double peaks 
‐‐ Zuev, et. al., PRL  09’
Graphene electronics
Conclusion ‐‐ CR Wang, WS Lu and WL Lee, PRB 82, 121406(R) 2010
• Massive chiral fermion in bilayer graphene:
two zero energy state N=0,1 ⇒ 8e2/h step in the σxy at CNP

• In spin-polarized QH regime
⇒ Double
D bl peaks k in Gxx and
d excess Gxx att CNP
⇒ WL dictates the behavior of αxy:
• kBT/WL>0.5 , αxy ~ 4xkBe/h (ln2) universal value
>0 5 , αxy /T ~ 0
• kBT/WL>0.5 0.2
2 nA/K2
⇒ Deviation from the semi-classical theory at CNP

• Existence of counter-propagating gapless chiral edge states

carrying opposite spin ? ⇒ possible application in spin electronics
Strong backscattering
b l l t
by local gate Spin filtered from 1 to 2
Spin filtered from 1 to 2

X X X 

‐‐ Abanin, et. al., PRL 06’
Strain Induced Zero-Field QHE
‐‐ Guinea, et. al. Nat. Phys. 10’

• Uniform gauge field Bs induced by a 2D strain field

along three main crystallographic directions.

• Bs is opposite for two valleys K and K’

• Bs ~ 40 Tesla for strain Δm =10%

• Landau quantization due to Bs

Bs = 0 T
10 T

7 T

Strain Δm =1%
 Group Members
• Active members 
Manoj Thakur, HC Hsu (Post‐doc)
CR Wang, CT Hsieh and TH Chen (RAs)
CC Ho (TIGP Ph.D. student)
CP Lu ( NTU Ph.D. student)
Feng Lin, WS Lu, HS Kung
Lin, WS Lu, HS Kung (NTU master)
(NTU master)

* Support from IoP AS + AS nanocore facility + Taiwan NSC 

 Nanospin Lab Major facilities

UHV e-beam evaporation System

Dilution fridge
g system
y (15
( mK))
with 15/17 Tesla magnet
UHV Magnetron-Sputter and Ion
Mill System
y