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Supplementary Information
Defect passivation in hybrid perovskite solar cellsusing quaternary ammonium halide
anions and cations
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SUPPLEMENTARY INFORMATIONVOLUME: 2 | ARTICLE NUMBER: 17102
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 1
Supplementary Figure 1: Photocurrent hysteresis and stabilized measurement for devices
with L-α-Phosphatidylcholine passivation. a, Current density-voltage (J-V) characteristics of
two-step processed MAPbI3 devices with different L-α-Phosphatidylcholine thickness. b, J-V
curves for the MAPbI3 device passivated by L-α-Phosphatidylcholine measured by forward and
reverse scans. c, Steady-state measurement of JSC and PCE for MAPbI3 device with L-α-
Phosphatidylcholine layers.
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 2
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Supplementary Figure 2: SEM images for MAPbI3 film after quaternary ammonium
halides (QAHs) deposition. No obvious damage to the morphology of the film was observed.
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 3
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© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 4
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© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 5
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Supplementary Figure 3: Independent PCE certification of perovskite solar cells by an
accredited PV laboratory of Newport Corporation confirming a PCE of 20.59±0.45% with
negligible hysteresis, which is a record certified efficiency for planar structured perovskite
solar cells.
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 6
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Supplementary Figure 4: A summary of the photovoltaic parameters of
FA0.85MA0.15Pb(I0.85Br0.15)3 devices (20 cells) with different passivation treatments (10 cells
each).
20
22
24
J SC (m
A/cm
2 )
1.05
1.08
1.11
1.14
VO
C
18
19
20
21
Choline chloridePCBM
PCE
(%)
72
76
80
FF (%
)
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 7
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0.0 0.2 0.4 0.6 0.8 1.0 1.2
0
-5
-10
-15
-20
Cur
rent
den
sity
(mA
/cm
2 )
Voltage (V)
PCBM Choline chloride
on FA0.83MA0.17Pb(I0.6Br0.4)3
Supplementary Figure 5: Current density-voltage (J-V) characteristics of
FA0.83MA0.17Pb(I0.6Br0.4)3 devices with choline chloride passivation.
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 8
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0.0 0.2 0.4 0.6 0.8 1.0 1.25
0
-5
-10
-15
-20
-25
Cur
rent
den
sity
(mA/
cm2 )
Voltage (V)
PCBM Choline chloride
on FA1-xMAxPb(I1-xBrx)3
Supplementary Figure 6: Current density-voltage (J-V) characteristics of two-step
processed FAxMA1-xPb(Br1-xIx)3 devices with choline chloride layers.
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 9
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-0.2 0.0 0.2 0.4 0.6 0.8 1.0-25
-20
-15
-10
-5
0
5
Cur
rent
den
sity
(mA
/cm
2 )
Voltage (V)
0.1% 0.01%
Blending with choline cloridewt%
Supplementary Figure 7: Current density-voltage (J-V) characteristics of
FA0.83MA0.17Pb(I0.83Br0.17)3 devices with choline chloride blending.
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 10
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Supplementary Figure 8: Steady-state photoluminescence (PL) spectra for the perovskite
thin films without (control) and with choline chloride.
650 700 750 800 850 900
PL
inte
nsity
(a.u
.)
Wavelength (nm)
Prinstine With Choline chloride
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 11
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Supplementary Figure 9: The isosurface plot (yellow area) of the highest occupied band of
the PbI2 surface with Pb-I antisite defect (a) without choline chloride and (b) with choline
chloride. Purple, grey, light blue, brown, light red and green spheres represent I, Pb, N, C, H
and Cl atoms, respectively (same for the following figures).
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NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 12
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Supplementary Figure 10: The isosurface plot of (a) the highest occupied band and (b)
lowest unoccupied band of the MAI surface with Pb cluster without choline chloride.
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
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Supplementary Figure 11: The isosurface plot of (a) the highest occupied band and (b)
lowest unoccupied band of the PbI2 surface with Pb-I antisite defect without choline chloride.
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 14
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Supplementary Figure 12: The local structure of MAI surface with Pb cluster (a) without
and (b) with choline chloride. Pb1 denotes the Pb cluster, and I1 and I2 are the two
neighboring I sites of Pb1.
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 15
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Supplementary Figure 13: The local structure of PbI2 surface with Pb-I antisite defect after
choline chloride passivation and a schematic draw of the evolution of antisite I. The red dotted
line denotes the immigration of I from its defected site (red dotted circle) to its position after
passivation.
© 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.
NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 16
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Supplementary Figure 14: Identification of the composition of the degraded perovskite film
by the evolution XRD patterns. XRD patterns of OIHP films without passivation layer
(control), with L-α-Phosphatidylcholine, and with choline chloride, respectively, before and
after exposure to humidity of 90 ± 5% for 2.5 h.
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NATURE ENERGY | DOI: 10.1038/nenergy.2017.102 | www.nature.com/natureenergy 17
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