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Institut Mines‐Télécom
Interfacing with the brain using organic electronics
George Malliaras
Department of Bioelectronics, Microelectronics Center of Provence
Email: malliaras@emse.fr ; Twitter: @GeorgeMalliaras
Institut Mines‐Télécom
Our location
Department of Bioelectronics    – www.bel.emse.fr2
Microelectronics Center of Provence
Inaugurated 2008
La Timone Hospital
AMU Medical School
Institut Mines‐Télécom
Outline
 Introduction to neural interfacing
 Why organics?
 Conducting polymers yield new capabilities for neuroscience  
• Recording single neurons without penetrating the brain
• Recording brain activity with high signal‐to‐noise ratio
• Stopping seizures (in vitro) with localized drug delivery
 Ion transport in conducting polymers
 Materials challenges ahead
Department of Bioelectronics    – www.bel.emse.fr3
Institut Mines‐Télécom
Bioelectronics: Coupling biology and electronics
Department of Bioelectronics    – www.bel.emse.fr4
Mostly soft
Complex signaling
Dynamic
Hard
Electrons/holes
Static 
Sensing
Diagnosis
Actuation
Therapy
Institut Mines‐Télécom
Importance of neural interfacing
 100 billion neurons in the 
human brain, organized in 
networks
 Their communication holds 
the key for understanding 
how the brain works
 These networks can be 
rewired by diseases such as 
epilepsy, cancer, …
 Stimulation of these 
networks is increasingly 
being used as therapy
Department of Bioelectronics    – www.bel.emse.fr5
EEG ECoG sEEG
Institut Mines‐Télécom
Epilepsy
 Affects 1‐2% of world population
 Temporal lobe epilepsy (TLE) is     
most frequent form in adults
 TLE is often drug resistant
Department of Bioelectronics    – www.bel.emse.fr6
Key challenges:
 Improve electrode performance
 Make less invasive recordings
Institut Mines‐Télécom
Deep brain stimulation for Parkinson’s
Department of Bioelectronics    – www.bel.emse.fr7
Institut Mines‐Télécom
Brain/machine interfaces
Department of Bioelectronics    – www.bel.emse.fr8
L.R. Hochberg, D. Bacher, B. Jarosiewicz, N.Y. Masse, J.D. Simeral, J. Vogel, S. Haddadin, J. Liu, P. van der Smagt, and J.P. Donoghue, Nature 485, 372 (2012). 
Institut Mines‐Télécom
From discovery to therapy
Department of Bioelectronics    – www.bel.emse.fr9
Luigi Galvani
(1737 – 1798) 
Pacemaker circa 1957
Arne Larsson, first to receive implantable 
pacemaker in 1958. He received a total 
of 26 pacemakers and died at 86.
Nanostim
Leadless pacemaker
Institut Mines‐Télécom
Implantable electronic medical devices
Department of Bioelectronics    – www.bel.emse.fr10
Artificial limbs controlled by the brain
(Penn Center for Brain Injury and Repair)
Cochlear implant
(Cochlear)
Implantable defibrillator
(Medtronic)
 Approved devices:
• Heart pacemakers – 600,000 per year
• Cochlear implants (hearing) – 300,000 patients
• Spinal cord stimulators (pain relief) – 15,000 per year
• Deep brain stimulators (Parkinson’s)
• Phrenic nerve stimulators (assisted breathing)
• Sacral nerve stimulators (bladder control)
• Vagus nerve stimulators (epilepsy)
• Retinal implants (vision)
 In development:
• Functional electrical stimulation (standing and gait)
• Brain Computer Interfaces (control of robotic limbs)
• DBS (severe psychiatric conditions) 
• Vestibular prostheses (balance) 
• Vision prostheses (vision) 
• Cortical prostheses (epilepsy detection & suppression) 
Institut Mines‐Télécom
Medical technologies raise ethical questions
Department of Bioelectronics    – www.bel.emse.fr11
Young Frankenstein, 20th Century FOX  (1974)
 1771: Galvani’s experiments
 1958: First implantable pacemaker
 Today: Implantable defibrillator
Institut Mines‐Télécom
Hype versus reality
Department of Bioelectronics    – www.bel.emse.fr12
Dr. Octopus in Spiderman 2
Boy hearing for the first time
Institut Mines‐Télécom
Organic electronics
Department of Bioelectronics    – www.bel.emse.fr13
Thin film transistors Photovoltaics
DuPont
Someya Lab
Light emitting diodes
Samsung
Astron FIAMM
Heliatek
Institut Mines‐Télécom
Typical organic semiconductors
Department of Bioelectronics    – www.bel.emse.fr14
NN
CH3 CH3
O
N
Al
3
TPD
Alq3
Pentacene
nn
S
O O
n
S n
PPP
PPV
PEDOT
P3HT
Institut Mines‐Télécom
Carbon as a semiconductor
Department of Bioelectronics    – www.bel.emse.fr15
R. Hoffman, C. Janiak, C. Kollmar, Macromolecules 24, 13, 3725‐3746, (1991).
EG  
ħ2p2
2maN
CH2=CH2
Hybridization: sp2 and pZ
Particle in a box:
Institut Mines‐Télécom
PEDOT doped with PSS
Department of Bioelectronics    – www.bel.emse.fr16
SO3
H SO3
H SO3
H SO3
H SO3
- SO3
H SO3
H SO3
H
S
O O
S
O O
S
O O
S
O O
S
O O
S
O O
S
O O
S
O O
+ *
p‐type doped material
Holes on PEDOT
Sulfonate ions on PSS
Holes in the form of polarons
Polyanion immobilizes dopants
σ = 1000 S/cm
Electrically neutral
Institut Mines‐Télécom
Conducting polymers match properties of tissue
Department of Bioelectronics    – www.bel.emse.fr17
Slide courtesy of Dave Martin (U. Delaware)
Institut Mines‐Télécom
Conducting polymers show mixed conductivity
Department of Bioelectronics    – www.bel.emse.fr18
J. Rivnay, R.M. Owens, and G.G. Malliaras, Chem. Mater. 26, 679 (2014).
Mixed conductivity leads to novel/state‐of‐the‐art devices
Institut Mines‐Télécom
Conducting polymer microelectrodes
record single neurons from brain surface
Department of Bioelectronics    – www.bel.emse.fr19
Institut Mines‐Télécom
Levels of neural interfacing
Department of Bioelectronics    – www.bel.emse.fr20
schalklab.org
Ultimate resolution
EEG: Network level (~ 1 cm)  
ECoG: Intermediate
sEEG: Single neuron (~ 10 µm)
It was not considered possible to obtain single neuron recordings
without penetrating the brain
Institut Mines‐Télécom
State‐of‐the‐art ECoG circa 2010
Department of Bioelectronics    – www.bel.emse.fr21
Rogers group (UIUC)
Institut Mines‐Télécom
Conducting polymers improve neural interfaces
Department of Bioelectronics    – www.bel.emse.fr22
Work of Martin, Wallace, Inganäs, …
Electrochemical growth 
on pre‐patterned metal 
electrodes
Institut Mines‐Télécom
Conducting polymers lower interfacial impedance
Department of Bioelectronics    – www.bel.emse.fr23
Different “nature” of capacitance across 
the electrode/electrolyte interface
+
+
+
+
+
-
-
-
-
-
Metal
Au
PEDOT:PSS
+
+
+
+
+
+
+
+
+
+
-
+
-
-
-
-
-
-
-
-
-
Polymer
SO3H SO3
H SO3H SO3H SO3
- SO3H SO3H SO3H
S
O O
S
O O
S
O O
S
O O
S
O O
S
O O
S
O O
S
O O
+ *
Similar roughness
Institut Mines‐Télécom
Ultra‐conformable PEDOT:PSS microelectrodes
Department of Bioelectronics    – www.bel.emse.fr24
D. Khodagholy, T. Doublet, M. Gurfinkel, P. Quilichini, E. Ismailova, P. Leleux, T. 
Herve, S. Sanaur, C. Bernard, and G.G. Malliaras, Adv. Mater. 36, H268 (2011).
Parylene C – 4 μm thickPEDOT:PSS
Institut Mines‐Télécom
Ultra‐conformable ECoG arrays
Department of Bioelectronics    – www.bel.emse.fr25
w/ Christophe Bernard (INSERM)
50 μm
d=2.2mm
Institut Mines‐Télécom
PEDOT:PSS electrodes outperform Au electrodes
Department of Bioelectronics    – www.bel.emse.fr26
w/ Christophe Bernard (INSERM)
D. Khodagholy, T. Doublet, M. Gurfinkel, P. Quilichini, E. Ismailova, P. Leleux, T. 
Herve, S. Sanaur, C. Bernard, and G.G. Malliaras, Adv. Mater. 36, H268 (2011).
Au
electrodes
PEDOT:PSS
electrodes
Institut Mines‐Télécom
Detection of single neurons from brain surface
Department of Bioelectronics    – www.bel.emse.fr27
w/ Dion Khodagholy, György Buzsáki (NYU)
D. Khodagholy, J.N. Gelinas, T. Thesen, W. Doyle, O. Devinsky, 
G.G. Malliaras and G. Buzsáki, Natrure Neurosci. 18, 310 (2015)
10 ms by 50 mV
Electrocorticography in rats
256 electrodes, 10 x 10 μm2 with 30 μm inter‐electrode spacing
Institut Mines‐Télécom
Translation to the clinic
Department of Bioelectronics    – www.bel.emse.fr28
w/ Dion Khodagholy, György Buzsáki (NYU)
D. Khodagholy, J.N. Gelinas, T. Thesen, W. Doyle, O. Devinsky, 
G.G. Malliaras and G. Buzsáki, Natrure Neurosci. 18, 310 (2015)
500 ms by 500 mV 
20 ms by 40 mV
Acute recordings in human patients
Institut Mines‐Télécom
Organic electrochemical transistors 
record brain activity with record‐high SNR
Department of Bioelectronics    – www.bel.emse.fr29
Institut Mines‐Télécom
Field‐effect transistors for neural recordings
Department of Bioelectronics    – www.bel.emse.fr30
Field‐effect transistor (FET)
C’max = 5 μF/cm2
M. Voelker and P. Fromherz, Small 1, 206 (2005).
SiO2
+++++
Vg
Id
Si
++++
- - - - - - - - -
Fromherz group, MPI
Institut Mines‐Télécom
The organic electrochemical transistor (OECT)
Department of Bioelectronics    – www.bel.emse.fr31
No insulator between channel and electrolyte
First OECT: H.S. White, G.P. Kittlesen, and M.S. Wrighton, J. Am. Chem. Soc. 106, 5375 (1984).
Institut Mines‐Télécom
Volumetric response of capacitance in PEDOT:PSS
Department of Bioelectronics    – www.bel.emse.fr32
For d=130 nm:
C’ = 500 μF/cm2
100× larger than 
double layer capacitance
C* = 39 F/cm3
J. Rivnay, P. Leleux, M. Ferro, M. Sessolo, A. Williamson, D.A. Koutsouras, 
D. Khodagholy, M. Ramuz, X. Strakosas, R.M. Owens, C. Benar, J.‐M. Badier, 
C. Bernard, and G.G. Malliaras, SCIENCE Advances 1, e1400251 (2015).
Institut Mines‐Télécom
Device model
Department of Bioelectronics    – www.bel.emse.fr33
dx
V(x)
Vg
cd W dx
Rs
......
Q(x)
D.A. Bernards and G.G. Malliaras, 
Adv. Funct. Mater. 17, 3538 (2008)
Ionic circuit
(electrochemistry)
Electronic circuit
(solid state physics)
-- -
-
-
+
+
-
+
- -
-
+
+
Gate Electrode
+
-
+
+
++
+ + +
+
+
SO3H SO3H SO3H SO3
H SO3
- SO3H SO3H SO3
H
S
O O
S
O O
S
O O
S
O O
S
O O
S
O O
S
O O
S
O O
+ *
Institut Mines‐Télécom
Characteristics of OECTs
Department of Bioelectronics    – www.bel.emse.fr34
J. Rivnay, P. Leleux, M. Sessolo, D. Khodagholy, T. Hervé, M. Fiocchi, G. G. Malliaras, Adv. Mater. 25, 7010 (2013).
Institut Mines‐Télécom
High transconductance OECTs
Department of Bioelectronics    – www.bel.emse.fr35
D. Khodagholy, J. Rivnay, M. Sessolo, M. Gurfinkel, P. Leleux, L.H. Jimison, E. Stavrinidou, T. Herve, S. Sanaur, R.M. Owens, and G.G. Malliaras, Nature Comm. 4, 2133 (2013).
Institut Mines‐Télécom
In vivo recordings using transistors
Department of Bioelectronics    – www.bel.emse.fr36
w/ Christophe Bernard (INSERM)
Transistor
SNR = 52.7 dB
SNR = 30.2 dB
1 μA
10 mV
1 s
Electrode
D. Khodagholy, T. Doublet, P. Quilichini, M. Gurfinkel, P. Leleux, A. Ghestem, E. Ismailova, 
T. Herve, S. Sanaur, C. Bernard, and G.G. Malliaras , Nature Comm. 4, 1575 (2013).
Institut Mines‐Télécom
Transistors enable less invasive recordings
Department of Bioelectronics    – www.bel.emse.fr37
w/ Christophe Bernard (INSERM)
D. Khodagholy, T. Doublet, P. Quilichini, M. Gurfinkel, P. Leleux, A. Ghestem, E. Ismailova, 
T. Herve, S. Sanaur, C. Bernard, and G.G. Malliaras , Nature Comm. 4, 1575 (2013).
Transistor
Surface
electrode
Depth
electrode
Institut Mines‐Télécom
Model for OECT operation
Department of Bioelectronics    – www.bel.emse.fr38
SO3
-
SO3
-
SO3
- SO3
-
SO3
-
+
+
+
+
+
+SO3
-
M+
ID=W∙d∙e∙μ∙p(x)∙[dV(x)/dx]
ID
p(x)=SO3
‐ – M+(x)
M+(x)=(C*/e)∙[VG – V(x)]
Integrating Id over the length of the channel:
ID=(W∙d/L)∙μ∙C*∙[VT – VG + VD/2]∙VD ID
SAT=[W /(2∙L)] ∙d ∙μ∙C*∙[VT – VG]2
VT= e∙SO3
‐/C*
Institut Mines‐Télécom
Scaling with geometry
Department of Bioelectronics    – www.bel.emse.fr39
b
10
-5
10
-4
10
-3
10
-5
10
-4
10
-3
 (s)
RS
 C (s)
∙ ∙ ∙ ∗
∙
J. Rivnay, P. Leleux, M. Ferro, M. Sessolo, A. Williamson, D.A. Koutsouras, 
D. Khodagholy, M. Ramuz, X. Strakosas, R.M. Owens, C. Benar, J.‐M. Badier, 
C. Bernard, and G.G. Malliaras, SCIENCE Advances1, e1400251 (2015).
Institut Mines‐Télécom
High transconductance means high SNR
Department of Bioelectronics    – www.bel.emse.fr40
w/ Christian Benar, Jean‐Michel Badier Bernard (INSERM)
J. Rivnay, P. Leleux, M. Ferro, M. Sessolo, A. Williamson, D.A. Koutsouras, 
D. Khodagholy, M. Ramuz, X. Strakosas, R.M. Owens, C. Benar, J.‐M. Badier, 
C. Bernard, and G.G. Malliaras, SCIENCE Advances 1, e1400251 (2015).
Institut Mines‐Télécom
Organic electronic ion pumps
control epileptiform activity
Department of Bioelectronics    – www.bel.emse.fr41
Institut Mines‐Télécom
The organic electronic ion pump
Department of Bioelectronics    – www.bel.emse.fr42
Work at Linkoping University and Karolinska Institute
D. T. Simon, S. Kurup, K. C. Larsson, R. Hori, K. Tybrandt, 
M. Goiny, E. H. Jager, M. Berggren, B. Canlon, and 
A. Richter‐Dahlfors, Nature Materials 8, 742 (2009).
Institut Mines‐Télécom
Ion pump operation
Department of Bioelectronics    – www.bel.emse.fr43
-- --
-
+
+
+
- -
+ ++++
++
- -
- -
- -
- -
-
-
--- +
+
+
+
+
+ +
+
+
+
PEDOT:PSS PEDOT:PSSPSS
Institut Mines‐Télécom
Ion pump for local delivery in neural networks
Department of Bioelectronics    – www.bel.emse.fr44
w/ Christophe Bernard (INSERM), Magnus Berggren (Linköping)
Institut Mines‐Télécom
Local delivery of GABA suppress seizure activity
Department of Bioelectronics    – www.bel.emse.fr45
w/ Christophe Bernard (INSERM), Magnus Berggren (Linköping)
Institut Mines‐Télécom
Local delivery of GABA suppress seizure activity
Department of Bioelectronics    – www.bel.emse.fr46
w/ Christophe Bernard (INSERM), Magnus Berggren (Linköping)
Institut Mines‐Télécom
Scaling with geometry
Department of Bioelectronics    – www.bel.emse.fr47
b
10
-5
10
-4
10
-3
10
-5
10
-4
10
-3
 (s)
RS
 C (s)
∙ ∙ ∙ ∗
∙
J. Rivnay, P. Leleux, M. Ferro, M. Sessolo, A. Williamson, D.A. Koutsouras, 
D. Khodagholy, M. Ramuz, X. Strakosas, R.M. Owens, C. Benar, J.‐M. Badier, 
C. Bernard, and G.G. Malliaras, SCIENCE Advances1, e1400251 (2015).
Institut Mines‐Télécom Department of Bioelectronics    – www.bel.emse.fr48
1 10 100 1000
0.01
0.1
1
10
e
 (cm
2
/Vs)
C* (F/cm
3
)
+EG,GOPS
PEDOT:PSS 
+EG,GOPS
P3HT‐SO
3‐
Recent New 
High‐performer
(Iain McCulloch, Imperial)
0% EG
50% EG
5‐10% EG
μC* as the materials figure of merit
S
SO
O
O
* n
-
(C4H9)4N+
P3HT‐SO3
‐
(+EG +GOPS)
μC* = 7.2 F/cmVs
μ = 0.05 cm2/Vs
C* = 144 F/cm3
w/ M. Thelakkat, 
U. Bayreuth
S. Inal, J. Rivnay, P. Leleux, M. Ferro, M. Ramuz, J.C. Brendel, M. Schmidt, 
M. Thelakkat, and G.G. Malliaras, Adv. Mater. 26, 7450 (2014).
PEDOT:PSS
(+EG, +GOPS)
μC* = 128 F/cmVs
μ = 3.3 cm2/Vs
C* = 39 F/cm3
Such maps provide a way to 
compare materials as potential 
candidates in OECTs
Institut Mines‐Télécom Department of Bioelectronics – www.bel.emse.fr49
PEDOT:PSS as a champion material
 Phase separated morphology
 Hole transport in PEDOT‐rich domains, ion transport in PSS matrix
Institut Mines‐Télécom
“Moving front” measurements
Department of Bioelectronics    – www.bel.emse.fr50
K. Aoki, T. Aramoto and Y. Hoshino, Journal of Electroanalytical Chemistry 340, 127 (1992).
T. Johansson, N. K. Persson and O. Inganas, Journal of the Electrochemical Society 151, E119 (2004).
X. Wang and E. Smela, The Journal of Physical Chemistry C 113, 369 (2008).
holes
ions
2D geometry makes
analysis difficult
Institut Mines‐Télécom
A simple way to measure ion transport
Department of Bioelectronics    – www.bel.emse.fr51
Glass
Electrolyte PEDOT:PSS Au
Vappl
Dedoped Doped
Barrier
+‐
+
‐
+
+
+
+ SO3
-
SO3
-
SO3
-
SO3
-
SO3
-
SO3
-
SO3
-
SO3
-
SO3
-
SO3
-
+
+
+
+
+
+
E. Stavrinidou, P. Leleux, H. Rajaona, D. Khodagholy, J. Rivnay, M. Lindau, S. Sanaur, and G.G. Malliaras, Adv. Mater. 25, 4488 (2013).
RI RC
ℓ 	 ∙ ∙
	 ∙ 	 2 ∙ ∙
2
Institut Mines‐Télécom
Ions are highly mobile in PEDOT:PSS
Department of Bioelectronics    – www.bel.emse.fr52
E. Stavrinidou, P. Leleux, H. Rajaona, D. Khodagholy, J. Rivnay, M. Lindau, S. Sanaur, and G.G. Malliaras, Adv. Mater. 25, 4488 (2013).
K+ mobility in film 
( )
K+ density in film
(cm‐3)
PEDOT:PSS 1.4	 ∙ 10 5.9	 ∙ 10
PEDOT:PSS :GOPS 1.9	 ∙ 10 3.2	 ∙ 10
Institut Mines‐Télécom
Linking ion transport and electrode impedance
Department of Bioelectronics    – www.bel.emse.fr53
E. Stavrinidou, M. Sessolo, B. Winther‐Jensen, S. Sanaur, and G.G. Malliaras, AIP Advances 4, 017127 (2014).
Institut Mines‐Télécom
Open questions
We should leverage our understanding
of electronic processes in organics
 How do we envision ion injection
• Field‐dependence?
• Hydrophilicity, hydration?
• Connection to mechanical properties?
• Dependence on ion size?
 What is the optimal material
• Balance between crystalline and amorphous domains?
• Separate paths of ionic/electronic transport – copolymers?
 Characterization in aqueous media
Department of Bioelectronics    – www.bel.emse.fr54
metal polymer
+‐+
electrolyte
Institut Mines‐Télécom
Conclusions
 Organic bioelectronics represents an emerging research direction. 
 Conducting polymers are leading to new capabilities for 
neuroscience:
• Non‐invasive, high SNR recordings of brain activity in animal models 
and in the clinic
• Localized drug delivery that can stop seizure in in vitro model
 Mixed conductivity of organics a key advantage.
 We need to leverage advances in understanding electronic 
structure & transport to describe mixed conductivity and design 
better materials.
Department of Bioelectronics    – www.bel.emse.fr55
Institut Mines‐Télécom
Acknowledgements
 Neuroengineering team at BEL
Jonathan Rivnay, Sahika Inal, Mary Donahue, Marc Ferro, 
Dimitris Koutsouras, Thomas Lonjaret, Ilke Uguz, Eloise 
Bihar, Marcel Brändlein, Shahab Rezaei Mazinani, Jolien
Pas, Esma Ismailova
Colleagues @ BEL: Xenofon Strakosas, Roisin Owens
 Institute of Systems Neuroscience
Animal research: Adam Williamson, Attila Kaszas, 
Christophe Bernard 
Clinical: Jean‐Michel Badier, Christian Benar
 University of Linköping (Sweden)
Amanda Jonsson, Loig Kergoat, Daniel Simon, Magnus 
Berggren
 Microvitae Technologies
Pierre Leleux, Thierry Hervé
 Other Collaborators 
Dion Khodagholy, György Buzsáki (NYU), Michele Sessolo 
(Valencia), Seiichi Takamatsu (AIST), Marc Ramuz (EMSE).
Department of Bioelectronics    – www.bel.emse.fr56
For more information:
Department of Bioelectronics (BEL)

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