Sensor Devices for Mobile and Wearable Applications...S. Shrivastava et al., Biosensors and Bioelectronics, 95 (2018) 8 But, typical target concentration in blood (sepsis) and food

Sensor Devices for Mobile and Wearable Applications

Nae-Eung Lee

School of Advanced Materials Sci. & Eng.

SAINT SKKU Advanced Institute of Nanotechnology

SAIHST Samsung Advanced Institute for Health Sciences and Technology

Sungkyunkwan University (SKKU) Korea

Personalized smart healthcare technology

2

Pulse

Temp.

pO2

Biomarkers

Pulse

pO2

Bio-potentials

Neuro-chemicals

Biomarkers

Biomarkers

Motion

Respiration

Mobile and wearable POCT (point-care-testing)

systems for personalized healthcare

accessary dressable

skin-attachable implantable

3

Standalone IOT Smartphone-integrated

U

N

O

B

T

R

U

S

I

V

E

m

P

O

C

T

w

P

O

C

T

4

iSTAT

Abbott Labs Coagucheck

Roche

Blood analyzer

Alere Stratus troponin

analyzer

Siemens

Accu-Check

Roche

Glucometer

iHealth

LFA reader

CELLMIC

Heart monitor(ECG)

Alivecor SAW biosensor

OJbio

Mobile point-of-care testing (mPOCT)

systems

Development of Tunable, Label-free and Imaging-based Quantitative aptasensor platform for Biomolecule detection

CMOS Image Sensor (CIS)

Fluorescence imaging-based high accuracy

biosensing for mPOCT

5

Spectrophotometer PMT

Smartphone

ELISA is a gold standard in immunoassays

Development of Tunable, Label-free and Imaging-based Quantitative aptasensor platform for Biomolecule detection

Signal to noise ratio ↑

Inte

ns

ity

Concentration

“Seesawed” fluorescence

Smartphone-based “seesawed” fluorescence

imaging for high accuracy apta-assay

W. Lee et al., Biosensors and Bioelectronics 94(2017) , 643 6

Split dAP-conjugated

fluorescent bead

Double strand

split cAP

Sybr Green I Released

cDNA

Target

(Estradiol) Metal-enhanced

fluorescence substrate

Development of Tunable, Label-free and Imaging-based Quantitative aptasensor platform for Biomolecule detection Smartphone-based “seesawed” fluorescence

imaging for high accuracy apta-assay

7

~15 times enhanced

r2=0.9888 r2=0.9842

10-2

10-1

100

101

102

103

104

105

106

107

0.0

0.2

0.4

0.6

0.8

1.0

F/F

0

17-Estradiol concentarion (pg/mL)

10-2

10-1

100

101

102

103

104

105

106

107

0

2

4

6

8

10

12

14

16

F/F

0

17-Estradiol concentarion (pg/mL)

0.0 0.2 0.4 0.6 0.8 1.0

0.0

0.2

0.4

0.6

0.8

1.0

Sen

sit

ivit

y

1-Specificity

ELISA

Portable device

Statistical

accuracy

test of target

analyte spiked

wastewater

Area

under

ROC

curve

ELISA 0.956

Mobile biosensor

0.922

M E F ( A g ) S N R Calibration curve for 17-estradiol

with smartphone fluorescence microscope

Prototyping of

using 3D printing

ROC curve

Development of Tunable, Label-free and Imaging-based Quantitative aptasensor platform for Biomolecule detection Smartphone-based fluorescence imaging of

pathogenic bacteria for on-the-spot detection

8 S. Shrivastava et al., Biosensors and Bioelectronics, 95 (2018)

But, typical target concentration in blood

(sepsis) and food safety: 1~10 CFU/mL

Sample volume: 100 L

10 CFU/mL (single bacterial cell in 100 L) detectable

Development of Tunable, Label-free and Imaging-based Quantitative aptasensor platform for Biomolecule detection Fluorescence imaging-based IOT-enabled

on-the-spot POCT system

9

Cartridge integrated with

MEF substrate

Bacteria

separator/concentrator

Fluorescence imaging

based biosensing

Probes for bacteria and toxin

IOT-enabled system

` Skin-attachable sensor patches for

wearable electronics

10

Biostamp MC10

S-patch Samsung

non-invasive and unobtrusive monitoring,

high SNR due to conformal contact with skin

Patch:

Accessary : non-invasive but limit in unobtrusive monitoring

11

What can be measured by

skin-attachable sensor patches?

T.Q. Trung and N.-E. Lee,

Adv. Mater. 29 (2017), 1521;

J. Mater. Chem. C, 5 (2017), 2202

Engineering of skin-attachable

sesnor patches

Stretchable

materials

Devices

Sensing materials, electrodes, electrochemical electrodes, dry biopotential electrodes

Substrate, dry adhesives, interconnect, encapsulation

Stretchable sensors, energy harvesters, energy storage devices

Packaging

Sensor-integrated systems

Signal acquisition, power management , data handling

Applications, big data, AI

New applications, clinical evaluation, services

Circuits

S/W

Clinical

Stretchable materials & devices

Chemical sensor

Substrate

Stretchable interconnect

Encapsulation

Selective membrane Dry adhesive

12

Stretchable physical sensors

for skin-attachable patches

13

` Approaches for stretchability

Materials Strategies Designs Process methods Stretchable

direction

Intrinsically

stretchable

components

Using intrinsically

stretchable

materials

Elastomeric

nanocomposites

Spin-coating, printing, spraying,

electropsinning Omni-direction

Geometric engineering of compliant

materials

In-plane, geometric

engineering Serpentine routing Patterning Uniaxial

Out-of-plane,

geometric

engineering

Wavy structure Pre-stretching and release Uniaxial,

Biaxial

Island-bridge Transfer printing Biaxial

Imperceptible Transfer on pre-strained

ultrathin substrate Unixial

Out-of-plane,

3D structuring

Bio-mimicking Soft lithography

Multi-direction,

but not fully

stretchable

Microstructrured

pattern

Soft lithography

spin coating, printing, spraying Omni-direction

Appl. Phys. Lett. 2014, 104, 021908

J. Vac. Sci. Technol. A 2009, 27, L9

IEEE Trans. Compon. Packag. Manuf. Technol.

2015, PP, 1

Adv. Mater. 2015, 27, 34

Adv. Sci. 2015, 2, n/a

ACS Nano 2015, 9, 6252

14

Approach 1: Intrinsically stretchable

elastomeric nanocomposites

Elastomer

Transparent

Stretchable

piezoelectric

pyroelectric

piezoresitive

chemresistive

thermoresistive

photoresponsive

electroactive

15

Nanomaterials

Thin films Sheets Nanofibers Microfibers

Stretchable, transparent and ultrasensitive

strain sensor for emotion detection

PU-PEDOT:PSS(top)

SWCNT

PU-PEDOT:PSS(bottom)

PDMS

400 500 600 700 8000

20

40

60

80

100

Tra

nsm

itta

nce

(%)

Wavelength(nm)

0 100 200

0

50

100

150

200

250 Bending mode

Resi

stance

change,

R/R

0(%

)

Time(sec)

1.6% 2.1% 2.5% 3.6%

10 20 30 40 50 60 70 80 90 10010

1

102

103

104

105

Stretching mode

Re

sist

an

ce c

ha

ng

e,

R/R

0(%

)

Strain(%)

1.5 2.0 2.5 3.0 3.5

101

102

8.7

18.6

62.3

50.8

9.2

13.7

35.349.7

Before cyclic stretching

After cyclic stretching

Ga

ug

e F

act

or(

GF

)

Strain(%)

1000cycles, up to 20%

Roh et al., ACS Nano 11 (2015) 6252 16

(b) near

the mouth

(a) forehead

0 5-0.2

0.0

0.2

0.4

0.6

0.8

1.0 Laughing

Re

sist

an

ce c

ha

ng

e,

R/R

0(%

)

Time(sec)

Start↓ ↓ Stop

Start↓

↓Stop

Start↓

↓Stop

0 5 10

0

100

200

300 Crying

Resi

stance

chan

ge,

R/R

0(%

)

Time(sec)

Start ↓ ↓ Stop Start↓ ↓Stop

Start↓ ↓Stop

Start↓ ↓ Stop

Start↓ ↓Stop

Start↓ ↓Stop

0 5 10-40

0

40

80 Laughing

Resi

stance

chan

ge,

R/R

0(%

)

Time(sec)0 5

-0.6

-0.3

0.0

0.3

0.6 Crying

Resi

stance

chan

ge,

R/R

0(%

)Time(sec)

↓ Start

Stop↓ ↓Start ↓Stop

↓Start ↓Stop

Laughing Crying

(a)

(b)

Start Stop Start Stop

Start Stop Start Stop

Stretchable, transparent and ultrasensitive

strain sensor for emotion detection

17

Stretchable, transparent, ultrasensitive,

self-powered strain sensor for activity monitoring

Strain : 100 %

Strain : 0 %

Evaluation

Hwang et al., ACS Nano 9 (2015)

8801, collaboration w/ prof. S.W. Kim 18

Hwang et al., ACS Nano (2015)

throat

0 20 40

0

5

10

15

20

10 % stretching

Time (s)

Resis

tan

ce c

han

ge,

ΔR

/ R

0 (

%)

-1.0 -0.5 0.0 0.5 1.0-60

-40

-20

0

20

40

60During stretching as 10% of strain

Vo

ltag

e (

V)

Time (s)

-1.0 -0.5 0.0 0.5 1.0-60

-40

-20

0

20

40

60Before stretching

Vo

lta

ge

(V

)Time (s)

-0.2 0.0 0.2 0.4 0.6 0.8-50

-25

0

25

50

75

100

125 Before stretching

During stretching as 10% of strain

Voltage (V)

Cu

rren

t (u

A/c

m2)

Strain sensor Supercapacitor

Triboelectric nanogenerator

Electrical performance of integrated devices

during stretching as 10% of strain

10k 100k 1M 10M 100M 1G

0.00

0.05

0.10

0.15

0.20

Pe

ak

po

we

r (m

W)

Resistance (Ohm)

-0.2 0.0 0.2 0.4 0.6 0.8-300

-200

-100

0

100

200

300

400

Cu

rre

nt

(uA

)

Voltage (V)

50 mV/s

100 mV/s

200 mV/s

500 mV/s

1000 mV/s

TENG

SC



19

throat

0 5 10 15-5

0

5

10

15

20

25

30

35

Re

sis

tan

ce c

ha

ng

e,

ΔR

/ R

0 (

%)

Time (s)

Index finger

0 5 10 15 20 25 30 35-2

-1

0

1

2

3

4

5

6

7

Clench one's fist

Resis

tan

ce c

han

ge,

ΔR

/ R

0 (

%)

Time (s)

0 5 10 15 20 25 30-6

-5

-4

-3

-2

-1

0

1

2

3

Turn wrist

Re

sis

tan

ce

ch

an

ge,

ΔR

/ R

0 (

%)

Time (s)0 5 10 15 20 25 30

-10

-8

-6

-4

-2

0

2

4

Move wrist

Re

sis

tan

ce

ch

an

ge,

ΔR

/ R

0 (

%)

Time (s)

0 5 10 15 20 25 30 35-2

-1

0

1

2

3

4

5

6

7

Clench one's fist

Clench

Spread

Resis

tan

ce c

han

ge,

ΔR

/ R

0 (

%)

Time (s)

forearm

throat



20

All-elastomeric transparent and stretchable

multi-sensors for activity monitoring

Trung et al., Adv. Mater., 28(2016) 502 21

Reduced graphene oxide-PU channel,

PU gate dielectric and

PEDOT:PSS-PU electrode

AgNWs/PEDOT:PSS-PU

resistor



Monitoring thermal distribution by FET temperature sensor array

Hot object

throat

Strain of 70 %

TS-FET array

1

2

3

4

1.0

1.1

1.2

B

C

D

E

4

2

3

Row

No

rm

ali

zed

cu

rren

t (I

DS/I

DS

0)

Column

1

1 2 3 4

1

2

3

4

Row

1

2

3

4

1.0

1.1

1.2

B

C

D

E

4

2

3

Row

No

rm

ali

zed

cu

rren

t (I

DS/I

DS

0)

Colum

n1

1 2 3 4

1

2

34

Row22

0 100 200 300 400 500

8.8x10-6

9.0x10-6

9.2x10-6

Dra

in c

urr

ent,

ID

S (

A)

Time (sec)

5.1x10-5

5.2x10-5

5.3x10-5

5.4x10-5

Tem

per

atu

re (

oC

)

Dra

in c

urr

ent,

ID

S (

A)

22

24

26

28

30

32

34

36

38

252 256 260

8.8x10-6

9.0x10-6

9.2x10-6

Cu

rren

t,

I (

A)

Time (sec)

Averaged

region

Before drinking hot water

Averaged

region

After drinking hot water

0 100 200 300 400 500

8.8x10-6

9.0x10-6

9.2x10-6

Drai

n cu

rren

t, I DS

(A)

Time (sec)

5.1x10-5

5.2x10-5

5.3x10-5

5.4x10-5

Tem

pera

ture

(o C)

Dra

in c

urre

nt, I

DS (A

)

22

24

26

28

30

32

34

36

38

252 256 260

8.8x10-6

9.0x10-6

9.2x10-6

Cu

rren

t, I

(A

)

Time (sec)

Averaged

region


Averaged

region


0 100 200 300 400 500

8.8x10-6

9.0x10-6

9.2x10-6

Dra

in cu

rren

t, I D

S (A)

Time (sec)

5.1x10-5

5.2x10-5

5.3x10-5

5.4x10-5

Tem

pera

ture

(o C)

Dra

in c

urre

nt, I

DS (A

)

22

24

26

28

30

32

34

36

38

252 256 260

8.8x10-6

9.0x10-6

9.2x10-6

Cu

rren

t, I

(A

)

Time (sec)

Averaged

region


Averaged

region


Simultaneous monitoring skin temperature and muscle movement during drinking hot water

Drinking Stop drinking Detaching

Attaching

Drinking Stop drinking



23

5.1x10-5

5.2x10-5

5.3x10-5

5.4x10-5

Dra

in c

urr

ent,

ID

S (

A)

22

24

26

28

30

32

34

36

38

Tem

per

atu

re (

o C)

0 100 200 300 400 500

8.0x10-6

9.0x10-6

1.0x10-5

1.1x10-5

Dra

in c

urr

ent,

ID

S (

A)

Time (sec)

122 124 126 128 130 132 1348.0x10

-6

9.0x10-6

1.0x10-5

Cu

rren

t I

, (A

)

Time (sec)

Averaged

region

Before work-out

Averaged

region

After work-out

Workout Stop workout

Detaching

Lift up

Release

Attaching



24

Simultaneous monitoring skin temperature and muscle movement during workout

` Approach 2: Mogul-patterned elastomeric

substrate for stress-relieving

A versatile substrate for stretchable electronics

H.B. Lee et al., Adv. Mater., 28 (2016) 3086

7

25

` Approach 2: Mogul-patterned elastomeric

substrate for stress-relieving

7

26

Optical image depending on stretching direction

Biaxial stretching Triaxial stretching

Without stretching Uniaxial stretching

- Omniaxially stretchable and stress of the layers are readily relived.

- Conventional processing (CVD, PVD, ALD, spin coating, spray coating,

printing etc) can be used to form the layers directly on the substrate

- Multi-layer stacking is possible by forming layers directly on the 3D micro-

pattern

` Omniaxially stretchable R-GO gas sensor on

mogul-patterned elastomeric substrate

Bump

Valley

10μm

Bump

Valley

10μm

Stability of Au electrode (70nm)

After 1,000 cycles of

stretching in x- and y-

directions at 50% strain

Structure

Electrode (Au)

Active Layer(R-GO)

27

` Omniaxially stretchable R-GO gas sensor on

mogul-patterned elastomeric substrate

28

0 50 100 150 200 250 300

0

10

20

30

40

50

60

70

40%

20%5%

50%

30%

R

/R0

Time (s)

Mogul, x-direction

Mogul, y-direction

Pre-strained, x-direction

Pre-strained, y-direction

10%

0 200 400 600 800 1000

0

1

2

3

4

5 Mogul, x-direction

Mogul, y-direction

Pre-strained, x-direction

Pre-strained, y-direction

R

/R0

Number of cycles

Investigatiion of electrical stability

Electrical stability of Au electrode [ Dynamic test ] [ Cyclic test ]

NO2 sesning

0 500 1000 1500 2000 2500

-20

0

20

40

60

80

No strain

30% strain

Resp

on

se,

I/I 0

(%

)

Time (s)

2.5ppm

gas ON

Gas OFF

5ppm 10ppm 25ppm

0 500 1000 1500 2000

0.0

0.5

1.0

Number of cycles

R

/R0

30% strain

0 20 40 60 80 100 120 140 160 180 200

0

2

4

6

8

10

R

/R0

Time (s)

5% 10% 15%30%25%20%

[ Dynamic test ] [ Cyclic test ]

Under stretched condition

Electrical stability of chemical sensor

Stretchable pressure sensor on

mogul-patterned elastomeric substrate Omniaxially stretchable piezoresistive

pressure sensor on mogul-patterned substrate

29

Device Structure

Mogul-patterned

PDMS

PEDOT:PSS-

SWCNTs

Ag paste

0 1 2 3 4 5-0.10

-0.05

0.00

0.05

0.10

0.15

0.20

Resis

tance c

hange,

R/R

0

Time (sec)

Electrode

Sensing layer

0 to 30% (uniaxial)

0.0 0.5 1.0 1.5 2.0

-0.4

-0.2

0.0

0.2

0.4

1.0 1.5

-0.05

0.00

release

Re

sis

tan

ce

ch

an

ge

,

R/R

0

Time (sec)

stretch to

30% (uniaxial)

Stability under stretching Materials stability under

stretching

Device stability under

stretching

0 1 2 3-3

-2

-1

0

1

2

3

Resis

tance c

hange,

R

/R0 (

%)

Time (sec)

Dynamic mode

0 1 2 3 4 5 6-15

-10

-5

0

5

10

15

20

Time (sec)

Unstretched

0 1 2 3-3

-2

-1

0

1

2

3

Resis

tance c

hange,

R

/R0 (

%)

Time (sec)

Dynamic mode

0 1 2 3 4 5 6-15

-10

-5

0

5

10

15

20

Time (sec)

Static mode

Pressure responsivity

Unstretched state

Under 30% stretching state

E. Roh et al., Adv. Mater., 29 (2017) 1703004

Static mode


mogul-patterned elastomeric substrate Omniaxially stretchable piezoresistive

pressure sensor on mogul-patterned substrate

Demonstration : Tremor detection

Skin area

Demonstration setup

Experimental

mixer for vibration

Arm Forearm

8 9 10 11 12 13 14

0.0

0.5

1.0

1.5

Am

plit

ude

8 9 10 11 12 13 14

0.00

0.05

0.10

0.15

Frequency (Hz)

Vibration detection using

the device

-6

-4

-2

0

2

4

6

Re

sis

tan

ce

ch

an

ge

,

R

/R0 (

%)

0 1 2 3

-1.6

-0.8

0.0

0.8

1.6

Time (sec)

Arm

Forearm

FFT (fast Fourier transform)

Vibration detection using the accelerometer in smartphone

0 2 4 6 8 10

-2.5

-2.0

-1.5

-1.0

-0.5

0.0

0.5

1.0

1.5

Acce

lera

tio

n m

/s2

Time (sec)

8 9 10 11 12 13 14

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

Am

plit

ud

e

Frequency

FFT

30


mogul-patterned elastomeric substrate Omniaxially stretchable piezoresistive pressure

sensor on mogul-patterned substrate

Measurement scheme

Skin

Sensor

R

Time

R

Time

Relative skin elasticity

Ballistometer

Skin elasticity evaluation

Cutometer

31

Self-powered Sensor for Smart Shoes Omniaxially stretchable self-powered

piezoelectric sensor

3D micro-patterned

Substrate

Graphite electrodes Stacked piezoelectric

nanofibers Stretchable self-powered

sensor

-12

-9

-6

-3

0

3

6

9

12

Op

en

Cir

cu

it V

olt

ag

e-V

oc (

V)

Time (sec)

BT-PU

3 layers

6 layers

BT-PU 3 Layers 6 layers 9 layers0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

1.6

1.8

Po

we

r D

en

sit

y (

W.c

m-2)

Piezoelectric Layer

Key Issues for Stretchable

Sensors

Low stretchability

Poor stability of electrode

under stretching

Complicated process

High cost

Stacked mat of BT NPs-PU nanocomposite and P(VDF-TrFE) nanofibers on stress-

relieving mogul-patterned elastomeric substrate

Output during stretching Output power at 40% stretching

S. Siddiqui et al., Adv. Energy. Mater. 8 (2018) 1701520

Self-powered Sensor for Smart Shoes Omniaxially stretchable self-powered

piezoelectric sensor

33

-150

-100

-50

0

50

100

150

200

250

Sh

ort

Cir

cu

it C

urr

en

t-Is

c (

nA

)

Time (sec)

1000 Cycles

3000 Cycles

5000 Cycles

7000 Cycles

9000 Cycles

Stability at 30% stretching strain

-15

-12

-9

-6

-3

0

3

6

9

12

15

Fast Movement

Op

en

Cir

cu

it V

olt

ag

e-V

oc (

V)

Slow Movement

(a) (b)

Walk

ing P

att

ern

Dete

ctio

n

Charg

e S

tora

ge d

uring

walk

ing

0 700 1400 2100 2800 3500

0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

Vo

lta

ge

(V

)

Time (sec)

Disposable stretchable biosensor patches

for wPOCT

Sweat, ISF

Wound fluid

• Electrochemical enzyme

biosensors

• Electrochemical and

optical immunosensors

34

Disposable stretchable label-free electrochemical

immunosensor for wound monitoring

35

• Differential pulse voltammograms of immunoreaction of TNF- protein under 0 %

(d) and 30 % (e) strain and calibration curve (f) in human serum

-0.4 -0.2 0.0 0.2 0.4 0.6

-0.08

-0.06

-0.04

-0.02

0.00

0.02

0.04

0.06

0.08

Cu

rren

t (m

A)

Potential (V)

before

during twisting

-0.4 -0.2 0.0 0.2 0.4 0.6

-0.08

-0.06

-0.04

-0.02

0.00

0.02

0.04

0.06

0.08

Cu

rren

t (m

A)

Potential (V)

before

after 1000 times

cyclic stretching

up to 30 %

-0.4 -0.2 0.0 0.2 0.4 0.6-0.08

-0.06

-0.04

-0.02

0.00

0.02

0.04

0.06C

urr

en

t (m

A)

Potential (V)

0 % strain

10 % strain

20 % strain

30 % strain

a) b) c)

-0.2 0.0 0.2 0.4-5

0

5

10

15

20

25

30

Cu

rren

t (

A)

Potential (V)

0 M

10 fM

100 fM

1 pM

10 pM

100 pM

1 nM

10 nM

100 nM

Human serum

-0.2 0.0 0.2 0.4-5

0

5

10

15

20

25

Cu

rren

t (

A)

Potential (V)

0 M

10 fM

100 fM

1 pM

10 pM

100 pM

1 nM

10 nM

100 nM

Human serumd) e) f)

10-15

10-14

10-13

10-12

10-11

10-10

10-9

10-8

10-7

10-6

0.0

0.1

0.2

0.3 0 % strain

30 % strain

I

Concentration of TNF- protein (C0, M)

Human serum

• Cyclic voltammograms of a device under a) a non-stretched and 10, 20, and 30%

stretched condition, b) without twisting and under twisting, and c) before cyclic

stretching and after cyclic stretching 1000 times at 30% strain

Perspectives

36

Efforts toward the improvement of stability and reliability of

the sensing nano-materials are required for real applications.

Sensor-integrated systems need to be developed by

considering the specific needs and service scenario.

Collaborative research is essential for success.

Circuits/tele-comm.

materials & devices

Biomedicine

Sensor-integrated stretchable electronics

software

Acknowledgments

Group members :

Dr. Tien Thanh Ngyuen, Dr. Tran Quang Trung, Dr. Sajal Shrivastava, Dr. Le

Thai Duy, Dr. Muhammad Saqib, Dr. Dang Vinh Quang, Do Il Kim, Il-Young

Sohn, Bo-Yeong Kim, Byung-Ung Hwang, Young-Min Son, Eun Roh, Han-

Byeol Lee, Won-il Lee, Ari Kim,

Sponsors :

National Research Foundation of Korea (NCRC, WCU, Basic Science

Research Programs)

Documents

Sensor Devices for Mobile and Wearable Applications...S. Shrivastava et al., Biosensors and Bioelectronics, 95 (2018) 8 But, typical target concentration in blood (sepsis) and food