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Quantum Transport of Transport of Quantum Transport of Quantum - - PowerPoint PPT Presentation

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Quantum Transport of Transport of Quantum Transport of Quantum Carbon Nanotube Nanotube & & Carbon Bio Sensor Applications Bio Sensor Applications Kazuhiko Matsumoto Osaka University Japan 2.3E-8 4 Drain Voltage (mV) 1.15E-8

slide-1
SLIDE 1

Quantum Transport of Quantum Quantum Transport of Transport of

0.0 0.2 0.4 0.6 0.8 1.0

  • 4
  • 2

2 4 Gate Voltage (V) Drain Voltage (mV)

  • 2.3E-8
  • 1.15E-8

1.15E-8 2.3E-8

Kazuhiko Matsumoto Osaka University Japan

Carbon Carbon Nanotube Nanotube & & Bio Sensor Applications Bio Sensor Applications

slide-2
SLIDE 2

1) Carbon Nanotube Quantum Devices

  • 1. Seamless Transition of Coulomb Blockade

Transport to Coherent Transport 2) Application of FET Type Bio sensor

  • 1. Top Gate FET type Bio Sensor
  • 2. Direct modification type Bio-Sensor

3) Conclusions

15 20 25 30 35 40 45 50

  • 25
  • 20
  • 15
  • 10
  • 5

Gate Voltage (V)

Carbon Nanoatube Source Drain 73nm 1~2 nm ~3 nm Si Aptamer Aptamer SiO2 Deby Deby Length Length IgE IgE

  • 25
  • 24
  • 23
  • 22
  • 21
  • 20
  • 150
  • 100
  • 50

50 100 150 Gate Voltage (V) Drain Voltage (mV)

  • 1E-5
  • 5E-6

5E-6 1E-5

d2ID/dVD

2

Back gate n+-Si SiO2 SiNx CNT Source Drain Catal yst Water proof resist

Contents

  • 20
  • 19
  • 18
  • 17
  • 16
  • 15
  • 100
  • 80
  • 60
  • 40
  • 20

20 40 60 80 100 dID/dVD (S) Gate Voltage (V) Drain Voltage (mV)

  • 1E-7

4E-7 9E-7 1.4E-6 1.9E-6 2.4E-6 2.9E-6 3.4E-6 3.9E-6 4E-6

slide-3
SLIDE 3

Carbon Nanoatube Drain Source 73nm h+ Drain Source

Back Gate Si Sub. SiO2 Drain Source Back Gate Si Sub. SiO2 Drain

73nm Carbon Nanotube

Drain EF Source CNT h+ e/C EF

Quantum Well

Carbon Nanotube Quantum Device Carbon Nanotube Quantum Device Carbon Nanotube Quantum Device Carbon Nanotube Quantum Device

slide-4
SLIDE 4

Back Gate Si Sub. SiO2 Drain Source Back Gate Si Sub. SiO2 Drain

VG A VD=11 mV ID

Period of peaks

Drain

EF

Source CNT

h+

e/C

EF

Carbon Nanoatube Drain Source 73nm

Gate Voltage VG (V) 10 20 30 40 50

  • 10

10 20 7.3 K VD=11 mV

ΔVG=3V

VG~ 0V

Coulomb Blockade Transport : Coulomb Oscillation Coulomb Blockade Transport : Coulomb Oscillation

slide-5
SLIDE 5

R

T >>h/e2 =25.8kΩ≡ R Q

ΔE •Δt ≈ h

∴h/CR

T <<e2 /2C

ΔE ≈ h/Δt = h/CR

T

Where ΔE << EC C : Tunnel Capacitance RT : Tunnel Resistance

(Charging Energy) h+ Drain Source Tunnel Res. RT>> Quantum Res. RQ

10 20 30 40 50

  • 1 0

1 0 2 0 7.3 K VD=11 mV ΔVG=3V

CNT VG~ 0

E F Drain E F Source CNT h+ e/C

Coulomb Blockade Condition Coulomb Blockade Condition

Drain Source

Heisenberg Rule

Quantum Resistance

2e2=13kΩ=RQ

slide-6
SLIDE 6

h+ Drain Source Tunnel Res. RT>> Quantum Res. RQ

10 20 30 40 50

  • 1 0

1 0 2 0 7.3 K VD=11 mV ΔVG=3V

CNT

E F Drain E F Source CNT h+ e/C

Coulomb Blockade Condition Coulomb Blockade Condition

Drain Source

Large depletion layer at drain Large tunnel resistance RT >RQ

At VG~0V

Coulomb Confinement

slide-7
SLIDE 7

10 20 30 40 50

  • 40-30-20-10 0 10 20 30 40

Gate Voltage (V)

7.3 K VD=11 mV

Carbon Nanoatube Source Drain 73nm

Back Gate Si Sub. SiO2 Drain Source Back Gate Si Sub. SiO2 Drain

VG A VD=11 mV

EF

Drain

EF

Source CNT

h+

e/C

Period of peaks

ΔVG=3V

ID

Coexistence of Coulomb Blockade Transport & Coherent Transport Coexistence of Coulomb Blockade Transport & Coherent Transport

slide-8
SLIDE 8

Enlargement

10 20 30 40 50

  • 40-30-20-10 0 10 20 30 40

Gate Voltage (V)

7.3 K VD=11 mV ΔVG=3V

15 20 25 30 35 40 45 50

  • 25
  • 20
  • 15
  • 10
  • 5

Gate Voltage (V)

ΔVG=0.65 V

Coexistence of Coulomb Blockade Transport & Coherent Transport Coexistence of Coulomb Blockade Transport & Coherent Transport Period of peaks ΔVG=0.65V

slide-9
SLIDE 9

Coherent Transport = Resonant Tunneling of Hole

Gate Electrode

4μm

SiO2 Drain Source

ΔEQ Discrete Energy Level

Hole

ΔVG Quantum Energy Level

73nm

Coexistence of Coulomb Blockade Transport & Coherent Transport Coexistence of Coulomb Blockade Transport & Coherent Transport

15 20 25 30 35 40 45 50

  • 25
  • 20
  • 15
  • 10
  • 5

Gate Voltage (V)

ΔVG=0.65 V

Coulomb Oscillation Coherent Oscillation

slide-10
SLIDE 10

EF

Drain

EF

Source CNT

h+

e/C

Coulmb Gap Quantum Level

15 20 25 30 35 40 45 50

  • 25
  • 20
  • 15
  • 10
  • 5

Gate Voltage (V)

ΔVG=0.65 V

Coulomb Oscillation Coexistence of Coulomb Blockade Transport & Coherent Transport Coexistence of Coulomb Blockade Transport & Coherent Transport

ΔVG=0.65 V

Coherent Oscillation Coherent Transport = Resonant Tunneling of Hole

slide-11
SLIDE 11

0.05 0.1 0.15 0.2

  • 40
  • 20

20 40 Gate Voltage (V) 7.2 K

Drain current (nA) 7.3 K

0.04 0.06 0.08 0.1 0.12 0.14 0.16 0.18

  • 25
  • 24
  • 23
  • 22
  • 21
  • 20

Gate Voltage (V) 7.3 K Drain current (nA)

Period of peaks ΔVG=0.65V Coherent Transport of Hole : Quantum Interference Coherent Transport of Hole : Quantum Interference

Enlargement

slide-12
SLIDE 12

Coherent Transport of Hole : Quantum Interference Coherent Transport of Hole : Quantum Interference

0.04 0.06 0.08 0.1 0.12 0.14 0.16 0.18

  • 25
  • 24
  • 23
  • 22
  • 21
  • 20

Gate Voltage (V) 7.3 K Drain current (nA) Gate Electrode

4μm

SiO2 Drain Source

ΔEQ Discrete Energy Level

Hole

ΔVG Quantum Energy Level

73nm

Le h E

F Q

2 ν = Δ

ΔVG

L=73nm

SEM Observation

L=55nm

Calculated

ΔVG=0.65V α Coherent Oscillation

slide-13
SLIDE 13

h+ Drain Source

0.04 0.06 0.08 0.1 0.12 0.14 0.16 0.18

  • 25
  • 24
  • 23
  • 22
  • 21
  • 20

Gate Voltage (V) 7.3 K

VG~ -20 CNT

Tunnel Res. RT<< Quantum Res. RQ

EF EF

Drain CNT

h +

Source

VG~ -22V

Drain Source

Quite thin depletion layer at drain Quite small tunnel resistance RT ~ RQ

Why NO Coulomb oscillation

No Coulomb Confinement

Coherent Transport only

slide-14
SLIDE 14

G : Conductance of Barrier

( ) ( )

ε π ε π

2 2 2 2

4 T e e G

R L R L

h h = Γ + Γ + Γ Γ =

h h

E F E F Drain CNT h+ Source

R L Γ

+ Γ = Γ

I V T0(ε) : Tunneling Probability Γ : Transfer Probability

Resonant Peak FWHM

( )

ν ν φ φ h h L T T T T L d dk dk dE

R L R L

2 2 Γ = + + = = Γ

h

Γ= ΓL+ ΓR = T0(ε) = TL+TR = Γ 2L

h v

Conductance of Barrier G Conductance of Barrier G

Γ= ΓL+ ΓR T0(ε)

G

slide-15
SLIDE 15

For Low Vg

E F E F Drain CNT h+ Source

R L Γ

+ Γ = Γ

I V T0(ε) : Tunneling Probability

Resonant Peak FWHM

Conductance of Barrier G Conductance of Barrier G

Γ= ΓL+ ΓR = 20mV

20mV

T0(ε) = 2L

h vF

(ΓL+ ΓR ) = 1.53x10-1 T0(ε) = 11.8μS e2

h

π G = R = 1/G = 85 kΩ >> R0 = 13 kΩ G : Conductance of Barrier R : Tunneling Resistance vF=3x107m/sec

slide-16
SLIDE 16

For Low Vg Tunneling Resistance R by Different VG Tunneling Resistance R by Different VG

R = 85 kΩ ~ 7 R0 >> R0 = 13 kΩ

R : Tunneling Resistance

For High Vg

R = 42 kΩ ~ 3 R0 ~ R0 = 13 kΩ

R : Tunneling Resistance

Drain Source

h+ Drain Source

h+ Drain Source CNT CNT

Coulomb confinement Coulomb Oscillation NO Coulomb confinement Coherent Oscillation

slide-17
SLIDE 17

h+ Drain Source

0.04 0.06 0.08 0.1 0.12 0.14 0.16 0.18

  • 25
  • 24
  • 23
  • 22
  • 21
  • 20

Gate Voltage (V) 7.3 K

VG~ -20 CNT

Tunnel Res. RT<< Quantum Res. RQ

EF EF

Drain CNT

h +

Source

h+ Drain Source

h+ Drain Source

Tunnel Res. RT>> Quantum Res. RQ

15 20 25 30 35 40 45 50

  • 25
  • 20
  • 15
  • 10
  • 5

Gate Voltage (V)

10 20 30 40 50

  • 1 0

1 0 2 0 7.3 K VD=11 mV ΔVG=3V

VG~ 0 VG~ -10 CNT CNT

Tunnel Res. RT ~ Quantum Res. RQ

E F Drain E F Sourc e CNT h+ e/C E F Drain E F Source CNT h+ e/C

slide-18
SLIDE 18

1) Carbon Nanotube Quantum Devices

  • 1. Seamless Transition of Coulomb Blockade

Transport to Coherent Transport 2) Application of FET Type Bio sensor

  • 1. Top Gate FET type Bio Sensor
  • 2. Direct modification type Bio-Sensor

3) Conclusions

15 20 25 30 35 40 45 50

  • 25
  • 20
  • 15
  • 10
  • 5

Gate Voltage (V)

Carbon Nanoatube Source Drain 73nm 1~2 nm ~3 nm Si Aptamer Aptamer SiO2 Deby Deby Length Length IgE IgE

  • 25
  • 24
  • 23
  • 22
  • 21
  • 20
  • 150
  • 100
  • 50

50 100 150 Gate Voltage (V) Drain Voltage (mV)

  • 1E-5
  • 5E-6

5E-6 1E-5

d2ID/dVD

2

Back gate n+-Si SiO2 SiNx CNT Source Drain Catal yst Water proof resist

Contents

  • 20
  • 19
  • 18
  • 17
  • 16
  • 15
  • 100
  • 80
  • 60
  • 40
  • 20

20 40 60 80 100 dID/dVD (S) Gate Voltage (V) Drain Voltage (mV)

  • 1E-7

4E-7 9E-7 1.4E-6 1.9E-6 2.4E-6 2.9E-6 3.4E-6 3.9E-6 4E-6

slide-19
SLIDE 19

Antigen Antibody （抗体） Antigen is eaten.

Immune

Antigen/Antibody Selective Reaction

Antigen / Antibody Reaction : Immunoassay

抗原（例えばウイルス） （免疫） （免疫）

slide-20
SLIDE 20

Drain Source Top gate Catalyst

窓(100 μm×100 μm)

Back gate n+-Si SiO2 SiNx CNT Source Drain Catalyst Water proof resist

SEM image of top-gate

  • f CNT-FET with

immobilized a-PSA.

a-PSA 100 nm

Top-gate with a-PSA

106

Electrical Detection of Antigen-Antibody Reaction by Carbon Nanotube FET Electrical Detection of Antigen-Antibody Reaction by Carbon Nanotube FET

PSA： Pig Serum Albumin a-PSA Anti-Body Antigen （抗原） （抗体）

slide-21
SLIDE 21

Drain V (V)

  • Drain I (nA)

0.0 0.2 0.4 0.6 0.8 1.0 500 1000 1500

Antigen/Antibody Reaction Reduction of ΔID

Top Gate

Antibody

Electron Current

  • Electrical Detection of Antigen-Antibody Reaction

Ag/AgCl Gate

Back Gate Source Top Gate SiO2 n+-Si SiNx CNT Analyzer Drain Antibody a-PSA Antigen PSA

  • Antigen

PSA a-PSA CNT

ΔID

slide-22
SLIDE 22

30th, August, 2006 第67回応用物理学会学術講演会 30p-D-17

Drain Voltage: +1 V Top-gate Voltage: +1 V Back-gate Voltage: +5 V 2 10-9 4 10-9 6 10-9 8 10-9 1 10-8 1 10 100 1000 104 105

PSA Cons. [nmol/L]

  • Reduc. Of Drain Current [A]

ΔID vs. CPSA

1 10-7 1.5 10-7 2 10-7 0.5 0.75 1 Top-gate Voltage [V] Drain Current [A] 0 nmol/L

ID vs. Vg ΔID

(VD = 1V, VBG = +5 V)

PSA/a-PSA Sensing

Electrical Detection of Antigen-Antibody Reaction

200 nmol/L PSA

slide-23
SLIDE 23

15th, September, 2006 SSDM, C-8-2

1 10 1001000 104 105 ΔID [nA] 10 8 6 4 2

Langmuir Equation ΔIDsat

Ntotal ∝ ΔIDsat Na ∝ ΔID

ΔID vs. CPSA

Na / Ntotal = Keq CPSA / (1＋Keq CPSA )

Quantitative Analysis of PSA/a-PSA Sensing

Where

CPSA

PSA Cons.[nmol/L]

Keq CPSA 1 + Keq CPSA = ΔID ΔIDsat

Equilibrium Constant Keq = 1x107 [(mol/L)-1]

slide-24
SLIDE 24

15th, September, 2006 SSDM, C-8-2

ΔEad = -0.41 [eV / mol] ΔEad = -RT ln Keq

ΔEad

Binding Energy

Binding Energy of PSA/a-PSA Reaction

Equilibrium constant

Keq = 1x107 [(mol/L)-1]

Antigen Antibody

表面プラズモン法で求まる 値と一致 電気的に初めて求まる

ΔEad = -0.41 [eV / mol]

Coincide with the value by surface plasmon method First time obtained by Simple Electrical Method

slide-25
SLIDE 25

Source Drain Sensing Area 1.5 μm 6 μm

2 10-9 4 10-9 6 10-9 8 10-9 1 10-8 1.2 10-8

CPSA (nM) ΔI D (A)

0.1 10 103

Back-gate

n+-Si SiO2 SiNx CNT

Source

Drain

Resist

Langmuir Equation Na / Ntotal = Keq CPSA / (1＋Keq CPSA )

Antigen Antibody

Effect of gate metal for Protein Detection Effect of gate metal for Protein Detection

slide-26
SLIDE 26

ΔI D (nA)

PSA Conc. (nM) NO gate metal With gate metal

5 10 15 20 25 30 35 0.1 1 10 100 103 104

gm = 163.7 nS ΔIDsat = 30.96 nA gm = 62.0 nS ΔIDsat = 9.26 nA

VD = + 1 VTG = + 1 V VBG = + 5 V

Higher Sensitivity without Gate Metal

Comparison of Sensitivity with and without Gate Metal Comparison of Sensitivity with and without Gate Metal

slide-27
SLIDE 27

100 200 300 400 10 20 I DS(nA) Time (min) 0.25 nM 2.2 nM 18.5 nM 159 nM

Carbon Carbon Nanotube Nanotube

金属電極 金属電極

Protein Sensor by Aptamer Modified CNT FET Protein Sensor by Aptamer Modified CNT FET

1~2 nm ~3 nm Si Aptamer Aptamer SiO2 Deby Deby Length Length

IgE IgE

Electrical Detection of Protein:IgE by CNT FET

4μm

slide-28
SLIDE 28

CNT aptamer IgE

Aptamer- modified CNTFET

100 200 10 12 14 16 18 Time (min) ISD (nA) IgE VD = 0.2 V VG = 0 V

250 pM 250 pM 250 pM 250 250 pM pM 2.2 nM 2.2 nM .2 n 2.2 2.2 nM nM 18.5 nM 18.5 nM 18.5 18.5 nM nM

Arrows indicate the point of adding IgE IgE solutions.

Detection of IgE by CNT FET Detection of Detection of IgE IgE by CNT FET by CNT FET

slide-29
SLIDE 29

Binding Energy of Binding Energy of IgE IgE AB / AB / Aptamer Aptamer

Keq CIgE 1 + Keq CIgE = ΔID ΔIDsat Langmuir Eq. ΔEad = -RT ln Keq ΔEad

Binding Energy of Aptamer-IgE

] ) / [( 10 8 . 2 10 2 . 5

1 8 8 −

× ± × = L mol Keq

] [ 51 . eV Ead − = Δ

ΔID vs. CPSA Plot

50 100 150 5 10

ΔIDS (nA) IgE Concentration (nM)

V VDS

DS＝

＝200 mV 200 mV V VGS

GS＝

＝0 V 0 V

slide-30
SLIDE 30

IgE concentration dependence of electrical properties IgE IgE concentration dependence of electrical properties concentration dependence of electrical properties IgE with concentration as low as 250 pM solution can be effectively detected. IgE with concentration as low as 250 pM solution can be effectively detected.

100 101 2 3 4 5 IgE concentration (nM) Δ ISD (nA)

250 pM 250 pM 250 pM 250 pM 250 pM 250 250 pM pM 2.2 nM 2.2 nM nM 2.2 2.2 nM nM 19 nM 19 nM 19 19 nM nM

CNT aptamer IgE

100 200 10 12 14 16 18 Time (min) ISD (nA) IgE VD = 0.2 V VG = 0 V

250 pM 250 250 pM pM 2.2 nM 2.2 2.2 nM nM 18.5 nM 18.5 18.5 nM nM

100 200 10 12 14 16 18 Time (min) ISD (nA) IgE VD = 0.2 V VG = 0 V

250 pM 250 250 pM pM 2.2 nM 2.2 2.2 nM nM 18.5 nM 18.5 18.5 nM nM

slide-31
SLIDE 31

Method Target IgE concentration Quartz Crystal 500 pmol/L

  • M. Liss et al., Anal. Chem.

2002, 74, 4488-4495

Luminescence 300 pmol/L

  • Y. Jiang et al., Anal. Chem.

2004, 76, 5230-5235

Fluorescence 350 pmol/L

  • G. Gokulrangan et al., Anal.
  • Chem. 2005, 77, 1963-1970

CNTFETs 250 pmol/L Our experiments

Biosensors for Biosensors for IgE IgE detection detection

slide-32
SLIDE 32

12

Back gate in Air 107 ~85 mV/dec ~210 mV/dec Top gate in Liquid 107 subthreshold slope

  • n/off比

transconductance ~100 μS/μm

(Vds=100 mV)

~700 μS/μm (Vds=100 mV)

  • 1000
  • 500

500 1000 1E-14 1E-13 1E-12 1E-11 1E-10 1E-9 1E-8 1E-7

drain current (A) gate voltage (mV)

Vd=100 mV

back gate in air top gate in PBS

Top gate Carbon Top gate Carbon Top gate Carbon Nanotube Nanotube Nanotube FET in Solution FET in Solution FET in Solution

Drain Source Reference top gate Si Substrate SiO2 CNT back gate Resist 10 mM PBS

slide-33
SLIDE 33

Dependence of Response Time on Channel Structure Dependence of Response Time on Channel Structure

Plane CNT Experiment

Detectable Concentration at 600 sec. Response time (s)

103 1 10-15 10-12 10-9 10-6 10-3 106

Antigen Concentration (mol/L)

ρ0

Plane : 5 nmol/L CNT(φ=2 nm): 0.1 pmol/L

ts ~ Ns

2

D 1 ρ0

2

ts ~ Nsa0 D 1 ρ0

5 nmol/L

0.1 pmol/L

slide-34
SLIDE 34

1) Carbon Nanotube Quantum Devices

  • 1. Seamless Transition of Coulomb Blockade

Transport to Coherent Transport 2) Application of FET Type Bio sensor

  • 1. Top Gate FET type Bio Sensor
  • 2. Direct modification type Bio-Sensor

15 20 25 30 35 40 45 50

  • 25
  • 20
  • 15
  • 10
  • 5

Gate Voltage (V)

Carbon Nanoatube Source Drain 73nm 1~2 nm ~3 nm Si Aptamer Aptamer SiO2 Deby Deby Length Length IgE IgE

  • 25
  • 24
  • 23
  • 22
  • 21
  • 20
  • 150
  • 100
  • 50

50 100 150 Gate Voltage (V) Drain Voltage (mV)

  • 1E-5
  • 5E-6

5E-6 1E-5

d2ID/dVD

2

Back gate n+-Si SiO2 SiNx CNT Source Drain Catal yst Water proof resist

Conclusions

  • 20
  • 19
  • 18
  • 17
  • 16
  • 15
  • 100
  • 80
  • 60
  • 40
  • 20

20 40 60 80 100 dID/dVD (S) Gate Voltage (V) Drain Voltage (mV)

  • 1E-7

4E-7 9E-7 1.4E-6 1.9E-6 2.4E-6 2.9E-6 3.4E-6 3.9E-6 4E-6