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1938-8
Workshop on Nanoscience for Solar Energy Conversion
Emilio PALOMARES
27 - 29 October 2008
Institute of Chemical Research of CataloniaAvinguda Paisos Catalans 16
43007 TarragonaSpain
Charge Recombination Studies in Hybrid Molecular Photovoltaic Devices
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Charge Recombination Dynamics in
Molecular Photovoltaic Devices.
Dr. Emilio Palomares. ICREA Research Professor
Institute of Chemical Research of Catalonia (ICIQ).
e-mail: [email protected]
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Always Different Interfaces
Molecular Solar Cells
Photons in....Electrons Out
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Always Different Interfaces
Molecular Solar Cells
Photons in....Electrons Out
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Always Different Interfaces
Molecular Solar Cells
Photons in....Electrons Out
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Always Different Interfaces
Molecular Solar Cells
Photons in....Electrons Out
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Always Different Interfaces
Molecular Solar Cells
Photons in....Electrons Out
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Dye Sensitised Solar Cells
"Blend" Solar Cells
Two different approaches
Different Photovoltaic Devices
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HTM/ DYE+ Regeneration
ETIO2/ DYE Injection
ETIO2/ HTM RECOMBINATION
ETIO2/ DYE+
RECOMBINATION
L-TAS
TCSPC
Charge Transfer Processes
TPV
![Page 10: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/10.jpg)
Charge Transfer Processes
E
HOMO
LUMO
ETIO2/ DYE+ injection
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Charge Transfer Processes
E
HOMO
LUMO
ETIO2/ DYE+ injection
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Charge Transfer Processes
E
HOMO
LUMO
ETIO2/ DYE+ injection
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Charge Transfer Processes
E
HOMO
LUMO
ETIO2/ DYE+ injection
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E
HOMO
LUMO
ETIO2/ DYE+ recombination
y = y0(�� /t )�
Fitting to KWW function
Charge Transfer Processes
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E
HOMO
LUMO
ETIO2/ DYE+ recombination
y = y0(�� /t )�
Fitting to KWW function
Charge Transfer Processes
![Page 16: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/16.jpg)
E
HOMO
LUMO
ETIO2/ DYE+ recombination
y = y0(�� /t )�
Fitting to KWW function
Charge Transfer Processes
![Page 17: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/17.jpg)
E
HOMO
LUMO
ETIO2/ DYE+ RECOMBINATION
Charge Transfer Processes
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E
HOMO
LUMO
ETIO2/ HTM RECOMBINATION
HTM
Charge Transfer Processes
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E
HOMO
LUMO
ETIO2/ HTM RECOMBINATION
HTM
Charge Transfer Processes
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E
HOMO
LUMO
ETIO2/ HTM RECOMBINATION
HTM
Charge Transfer Processes
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E
HOMO
LUMO
HTM
HTM/ DYE+ Regeneration
Charge Transfer Processes
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E
HOMO
LUMO
HTM
HTM/ DYE+ Regeneration
Charge Transfer Processes
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E
HOMO
LUMO
HTM
HTM/ DYE+ Regeneration
Charge Transfer Processes
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E
HOMO
LUMO
HTM
Overall charge transfer processes
Charge Transfer Processes
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E
HOMO
LUMO
HTM
Overall charge transfer processes
10-12-10-9s
Charge Transfer Processes
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E
HOMO
LUMO
HTM
Overall charge transfer processes
10-12-10-9s
10-4-10-6s
Charge Transfer Processes
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E
HOMO
LUMO
HTM
Overall charge transfer processes
10-12-10-9s
10-4-10-6s10-3-101 s
Charge Transfer Processes
![Page 28: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/28.jpg)
E
HOMO
LUMO
HTM
Overall charge transfer processes
10-12-10-9s
10-4-10-6s10-3-101 s
10-10-10-9 s
Charge Transfer Processes
![Page 29: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/29.jpg)
Device Characterisation
IPCE =Iph �1240
� � P0�100
�device = Isc �Voc � FF
Charge Transfer Processes
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Device Characterisation
IPCE =Iph �1240
� � P0�100
�device = Isc �Voc � FF
Charge Transfer Processes
![Page 31: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/31.jpg)
Device Characterisation
IPCE =Iph �1240
� � P0�100
�device = Isc �Voc � FF
Charge Transfer Processes
![Page 32: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/32.jpg)
Controlling "Dark" Electron transfer Reaction
ICIQ's Research
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Controlling "Dark" Electron transfer Reaction
Dye absorption Kinetics
A = Amax (1� exp(�Kadst))
Lagergren's Equation
ICIQ's Research
![Page 34: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/34.jpg)
Controlling "Dark" Electron transfer Reaction
Dye Injection kinetics
y = y0(�� /t )�
Injection into TiO2 CB occurs before 100 ps
Injection on Devices is slower. Nonetheless still faster than 250 ps
ICIQ's Research
![Page 35: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/35.jpg)
Controlling "Dark" Electron transfer Reaction
Dye Injection kinetics
y = y0(�� /t )�
Injection into TiO2 CB occurs before 100 ps
Injection on Devices is slower. Nonetheless still faster than 250 ps
ICIQ's Research
![Page 36: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/36.jpg)
Controlling "Dark" Electron transfer Reaction
TiO2/Dye+ charge transfer kinetics
y = y0(�� /t )�
TiO2/dye+ recombination half-lifetime ~3 x 10-4 s.TTT
ICIQ's Research
![Page 37: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/37.jpg)
Controlling "Dark" Electron transfer Reaction
TiO2/Dye+ charge transfer kinetics
y = y0(�� /t )�
TiO2/dye+ recombination half-lifetime ~3 x 10-4 s.TTT
ICIQ's Research
![Page 38: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/38.jpg)
Controlling "Dark" Electron transfer Reaction
TiO2/Dye+ charge transfer kinetics
y = y0(�� /t )�
TiO2/dye+ recombination half-lifetime ~3 x 10-4 s.TTT
ICIQ's Research
![Page 39: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/39.jpg)
Controlling "Dark" Electron transfer Reaction
TiO2/Dye+ charge transfer kinetics
y = y0(�� /t )�
TiO2/dye+ recombination half-lifetime ~3 x 10-4 s.TTT
ICIQ's Research
![Page 40: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/40.jpg)
Controlling "Dark" Electron transfer Reaction
TiO2/electrolyte+ charge transfer kinetics
No TiO2 CB shift. No effect on the DOS by alkyl chains
Slow "dark" recombination dynamics
ICIQ's Research
![Page 41: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/41.jpg)
Controlling "Dark" Electron transfer Reaction
TiO2/electrolyte+ charge transfer kinetics
No TiO2 CB shift. No effect on the DOS by alkyl chains
Slow "dark" recombination dynamics
ICIQ's Research
![Page 42: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/42.jpg)
Enhanced device efficiency
DSSC Devices
Increase in Current
Increase in voltage
ICIQ's Research
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1
10
100
1000
10000
100000
0 5 10 15 20
PI1/Al2O
3
PI1/TiO2
Em
iss
ion
Co
un
ts (
a.u
.)
Time (ns)
Dye Sensitised Solar Cells
![Page 44: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/44.jpg)
Dye Sensitised Solar Cells
0
1
2
3
4
5
6
7
550 600 650 700 750 800
PI1/Al2O
3
PI1/TiO2
Em
iss
ion
In
ten
sit
y (
a.u
.)
Wavelength (nm)
![Page 45: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/45.jpg)
Dye Sensitised Solar Cells
0
1 10-4
2 10-4
3 10-4
4 10-4
5 10-4
10-6
10-5
10-4
10-3
10-2
10-1
15 minutes4 hours14 hours
� O
.D.
Time (s)
SAME WL
0
5 10-5
1 10-4
1.5 10-4
2 10-4
10-6
10-5
10-4
10-3
10-2
10-1
15 minutes4 hours14 hours
� O
.D.
Time (s)
SAME OD
![Page 46: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/46.jpg)
Dye Sensitised Solar Cells
0
2
4
6
8
10
0 0.1 0.2 0.3 0.4 0.5 0.6
1 hour
4 hours
5 hours
14 hours
Ph
oto
cu
rre
nt
(mA
)
Voltage (V)
0.01
0.1
1
0.2 0.25 0.3 0.35 0.4 0.45 0.5
1 hour
14 hours
5 hours
Reco
mb
inati
on
Lif
eti
me (
s)
Cell Voltage (V)
![Page 47: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/47.jpg)
ICIQ-Dyes
phenanthroline heteroleptic Ru(II) complexes
Dye Sensitised Solar Cells
![Page 48: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/48.jpg)
MO
Dye Sensitised Solar Cells
-2.0
-3.0
-4.0
-5.0
E(eV)
(1.67) (1.70) (1.68)
(1.29)
(-2.97)
(-4.64)
(-2.89)
(-4.59)
(-2.91)
(-4.59)
(-3.54)
(-4.83) ( )
( 2 97)(-2 89)
( )
(-((((((( 4
-2.919191919119991111991199119111)))))))))))))))))))))))))))))))))))))
83)
Phen Me-PhenNH2-Phen NO2-Phen
![Page 49: 1938-8 Workshop on Nanoscience for Solar Energy Conversion · Workshop on Nanoscience for Solar Energy Conversion Emilio PALOMARES 27 - 29 October 2008 ... HOMO LUMO E TIO 2/ DYE+](https://reader033.vdocuments.us/reader033/viewer/2022042400/5f0f319f7e708231d442f3a7/html5/thumbnails/49.jpg)
Electron Injection
Dye Sensitised Solar Cells
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Electron Injection
Dye Sensitised Solar Cells
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e--TiO2/Dye+ Recombination
Dye Sensitised Solar Cells
0
5 10-5
0,0001
0,00015
0,0002
0,00025
0,0003
0,00035
0,0004
10-6
10-5
0,0001 0,001 0,01 0,1
N719
AR20
AR24
AR25
AR27
�O
.D.
Time (s)
0
6 10-5
0,00012
0,00018
0,00024
0,0003
600 650 700 750 800 850 900 950
100us
500us
�O
.D. (a
.u.)
Wavelength (nm)
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e--TiO2/Dye+ Recombination
Dye Sensitised Solar Cells
0
2 10-5
4 10-5
6 10-5
8 10-5
0,0001
10-6
10-5
10-4
10-3
10-2
10-1
N719
TiO2
Cell Dark
White Light 800
White Light 999
Time (s)
� O
.D.
0
4 10-5
8 10-5
0,00012
0,00016
0,0002
0,00024
0,00028
10-6
10-5
10-4
10-3
10-2
10-1
AR25/TiO2:l
probe=800 nm
AR25/DSSC:lprobe
=800 nm
AR25/DSSC:lprobe
=1000 nm
Time (s)
� O
.D.
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e--TiO2/Dye+ Recombination
Dye Sensitised Solar Cells
0
5 10-5
0,0001
0,00015
0,0002
10-6
10-5
10-4
10-3
10-2
10-1
AR24a/TiO2
:�probe
=800nm
AR24a/DSSC2
:�probe
=800nm
AR24a/DSSC2
:�probe
=1000nm
�O
.D.
Time (s)
0
4 10-5
8 10-5
0,00012
0,00016
0,0002
0,00024
0,00028
10-6
10-5
10-4
10-3
10-2
10-1
AR25/TiO2:l
probe=800 nm
AR25/DSSC:lprobe
=800 nm
AR25/DSSC:lprobe
=1000 nm
Time (s)
� O
.D.
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Cell Characterisation
Dye Sensitised Solar Cells
-2
0
2
4
6
8
10
12
14
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7
Jsc (
mA
/cm
2)
Voltage (V)
DSSC 208
�: 6,10 %
Voc: 0,66 V
Jsc: 13,55 mA/cm2
FF: 66,60 %
Device Area: 0,152 cm2
Dye: AR20
Electrolyte: AF04
Ligth: 100mW/cm2
Layers: TiO2 TiCl
4 (16+4) -2
-1
0
1
2
0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8
AR20
AR24-16
AR24-18
AR25
AR27-16
AR27-18
Ph
oto
cu
rre
nt
(mA
)
Voltage (V)
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Dye Sensitised Solar Cellse--TiO2/Electrolyte+ Recombination
0
5 10-5
0,0001
0,00015
0,0002
0 0,1 0,2 0,3 0,4 0,5 0,6 0,7 0,8
AR20
AR24a
AR24b
AR25
AR27b
AR27b
N719
Ch
arg
e (
C)
/cm
2
Voltage (V)
*
0
0,5
1
1,5
2
0 0,004 0,008 0,012 0,016 0,02
AR25
AR27
AR20
AR24
No
rma
lize
d I
nte
ns
ity
(a
.u.)
Time (s)
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Organic solar cells
-- -
+ +
-----
-
+ +++
+
+++ ++
+
+
++
++
+++
-----
--------------
+
+++ ++
+
-
+
HOMO HOMO
LUMO LUMO
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Organic solar cellsP3HT/PCBM d-TiO2/ P3HT/PCBM
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Organic solar cells P3HT/PCBM
10-5
0,0001
0,001
10-6
10-5
0,0001 0,001 0,01
1:07
1:0.5
1:1
� O
.D.
Time (s)
Charge recombination
dynamics
dependent on P3HT/PCBM
ratio
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Organic solar cellsITO/pentacene/C60/BCP/Al
-10
-5
0
5
-0.4 -0.2 0 0.2 0.4
0,1 Sun
1 Sun
dark
Js
c (
mA
/cm
2)
Voc (V)
FF=44.7%
�=0.54%
Voc=0.285
Isc=4.23mA/cm2
PENTACENE
ITO
4.8EV5.0EV C60
4.5EV
6.2EV
3.0EV
X.X
AL
BCP
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Organic solar cellsITO/C60: ZnPc/DINPB/NDP2-DiNPB/NDP2-ZnPc/Au/Ag/Au
0
2
4
6
8
10
12
0 0.1 0.2 0.3 0.4 0.5 0.6
0.1 sun
0.5 sun
1 sun
Jsc(m
A)
Voltage (V)
�=2.70%
�=3.85%
�=3.59%
1
10
5 1016
1 1017
1.5 1017
2 1017
2.5 1017
3 1017
tau teoric
��
n (
μs
)
n (cm-3
)
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Acknowledgments
Research Group Members and collaborators
Funding Agencies
Private Funding
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Acknowledgments
Research Group Members and collaborators
Funding Agencies
Private Funding
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Acknowledgments
Research Group Members and collaborators
Funding Agencies
Private Funding
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Acknowledgments
Research Group Members and collaborators
Funding Agencies
Private Funding