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TiC2: a new two-dimensional sheet beyond MXenes
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High efficiency MAPbI3-xClx perovskite solar cell via interfacial
passivation
Received 00th January 20xx, + +
Accepted 00th January 20xx Sijian Yuan , Jiao Wang , Kunlong Yang , Pengfei Wang , Xin Zhang , Yiqiang Zhan * and Lirong
+&
Zheng *
DOI: 10.1039/x0xx00000x
www.rsc.org/
The trap states at the interface between perovskite and charge
transport layer have a great influence on the performance of
perovskite solar cell. Here, a high efficiency MAPbI3-xClx perovskite
solar cell has been demonstrated, by introducing a thin layer of LiF
or PbF2 between the SnO2/perovskite. The improved charge
collection and reduced interfacial charge recombination are
realized, leading to the remarkable raises of both open-circuit
voltage (Voc) and a short-circuit current (Jsc).The successful
interfacial passivation paved a new way to fabricate high
performance perovskite solar cell especially with large Voc.
Perovskite solar cells (PVSC) have attracted enormous
attention in the past few years for its more and more exciting
progress in power conversion efficiencies (PCE).1,2 Its PCE jumps
rapidly from 3.8% (2009) to 23.2% (2018), benefited from the
perovskite’s extraordinary optoelectronic properties, such as the
large absorption coefficient, long carrier lifetime, high tolerance
for trap states.3,4,5 Among these study, plenty of efforts has been
devoted to enhance the quality of perovskite film by cation
exchanging, additives, solvent engineering and so on.6,7,8,9
Besides achieving high quality perovskite films, novel electron-
transport layers (ETL) and hole-transport layers (HTL) were also
treated as an important issue for the PCE enhancement10–13. For
example, charge transport materials with well-aligned band
structure and high mobility such as SnO2 and PTAA were
employed to the perovskite solar cell to improve the PVSC’s
PCE.14,15,16
Although the perovskite layer itself has been dramatically
improved, as lack of study, the knowledge of the interfaces
between perovskite and HTL/ETL are still insufficient. According
to reported results, once the long carrier diffusion length was
achieved in perovskite, the loss at the interface became a main
factor for further PCE improvement.13,14 The interface PCE loss
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Nanoscale Accepted Manuscript
was usually caused by the deep trap states presented at the
interface between perovskite and change transport layers.13
From theoretic simulation, a 109-1010 cm-2 interface trap states
could largely reduce the solar cells’ fill factor (FF), open-circuit
voltage (Voc), short-circuit current (Jsc) and PCE.17 These
interface trap states could be caused by several reasons such as
the layer-by-layer fabricating process and the lattice
mismatching between the perovskite and change transport
layers.7,18
Recently a few attempts have been made to eliminate these
interface trap states. By introducing chlorine-capped layer on the
TiO2 and introducing an organic buffer layer on PEDOT: PSS, the
performances of solar cells have been successfully improved.18,19
The surface passivation has been regarded as an efficient method
in both papers. It is also worth to mention that the interface
defects presented at the light propagated side were more
harmful to the PVSC’s PCE.17 Although these attempts only
scraped the tip of the iceberg, the importance of
perovskite/charge transfer layer interface has already been
demonstrated. To fully understand the interface, obviously more
systematical studies are still highly demanded.
In this work, we have found that the LiF can function as a
highly efficient interfacial passivation layer for the
SnO2/perovskite interface, which is widely used.20-21 With this
LiF layer, the best Voc increases from 1.06 to 1.16 V, which is very
close to the recently reported highest Voc(1.18 V)22. And the Jsc
increases from 20.4 to 21.6 mA·cm-2. The best solar cell’s PCE is
18.3%, which is 22% higher than the reference device. The
further investigation of light dependent Voc and impedance
spectrum, were conducted. It gave solid evidences that the LiF
had suppressed the surface trap states and reduced the
interfacial charge recombination. Our research highlights a
possibility of opening a new way for suppressing the
SnO2/Perovskite interface trap states, which is of great interest
for efficient perovskite solar cells.
Results and Discussion
Perovskites solar cell fabrication. Fig. 1a shows a schematic of
our perovskite solar cell. A 30 nm thick SnO2 film was spin-
coated on the ITO substrate with a 1% SnO2 colloidal dispersion
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Table 1. The performance of the PVSC with different modified layers.
Voc (V) Jsc (mA∙cm-2) FF (%) Eff (%)
DeviceA-0nm LiF (best) 1.08 20.40 71.1 15.6
DeviceA-0nm LiF 1.06±0.019 19.7±0.84 68.10±1.38 14.3±0.81
DeviceB1-0.4nm LiF(best) 1.12 21.10 72.2 17.08
deviceB1-0.4nm LiF 1.12±0.016 20.22±1.04 69.1±3.36 15.6±1.49
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deviceB2-0.7nm LiF(best) 1.15 21.62 73.7 18.33

deviceB2-0.7nm LiF 1.14±0.017 20.93±1.59 70.6±2.31 16.7±1.57
deviceB3-1.0nm LiF(best) 1.16 20.20 73.5 17.23
deviceB3-1.0nm LiF 1.14±0.018 19.61±2.07 70.6±2.52 15.7±1.75
deviceB4-1.5nm LiF(best) 1.15 19.50 73.1 16.39

Nanoscale Accepted Manuscript

deviceB4-1.5nm LiF 1.14±0.017 20.1±1.70 68.1±3.2 15.4±1.81
deviceC-0.7nm PbF2(best) 1.14 19.05 71.4 15.5
deviceC-0.7nm PbF2 1.12±0.014 18.62±0.90 68.7±2.0 14.1±1.81
LiTFSI(best) 1.07 20.6 69.1 15.23
LiTFSI 1.07±0.016 19.6±0.90 68.2±2.0 14.3±0.85
(Alfa Aesar) and annealed at 180 oC for 1 hour in air. A LiF or the whole perovskite solar cell performance was enhanced. The
PbF2 film with different thickness was deposited on the SnO2 film LiF layer lead to a significant increase of devices’ Voc and PCE. As
via shown in Table 1, the best reference device A shows a PCE of
thermal evaporation under high vacuum (5
10-5 Pa). Based on 15.6%. By precisely controlling the thickness of LiF modified

Figure 1. Structure of the PVSC and the J-V of different modified PVSC. (A) Structure of the PVSC. (B) J-V of the devices.

the thickness of LiF or PbF2, the devices were noted as device A
(0 nm LiF), B1 (0.4 nm LiF), B2 (0.7 nm LiF), B3 (1 nm LiF), B4
(1.5 nm LiF), C (0.7 nm PbF2), respectively. Then, 50 μL
perovskite precursor solution was spin-coated at a speed of
4000 rpm for 30 s followed by dripping 400 μL methylbenzene
in one second on the rotating film. After that, the film was
annealed at 100  for 7 min in a N2 glove box. A doped Spiro-
OMeTAD (80 mg/mL) layer was spin-coated on the perovskite
film. Finally, a 50 nm gold anode was deposited in the vacuum
chamber with an active area of 0.06 cm2.
Characterization of LiF modified perovskite solar cell. By
applying a LiF layer between the SnO2 and the perovskite film,
layer, the 0.7 nm LiF perovskite solar cell shows a best PCE of
18.3% with a Voc of 1.15 V, a Jsc of 21.6 mA∙cm-2, and an FF of
73.7 % under reverse voltage scan. Compared to the device
without the LiF layer, the LiF cells’ average Voc is significantly
increased (from 1.08 to 1.13 V), as shown in Table 1. It is worth
to note that the best achieved Voc is 1.16, which is among the
highest Voc of recent reported SnO2 based PVSCs (listed in the
supporting material table S2x). For the Jsc, a thin LiF Layer (<1
nm) also lead to a higher Jsc comparing to the reference device,
while thicker LiF layer (1.5 nm) could reduce the Jsc because of
the additional resistance brought by LiF layer. And for the best
device, devices’ series resistance changed from 45.3 ohm to 59.3

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ohm when increased the LiF from 0 nm to 1.5 nm. (0 nm LiF:
45.3 ohm, 0.4 nm LiF: 55.9 ohm, 0.7 nm LiF: 57.5 ohm, 1.0 nm
LiF: 56.9 ohm, 1.0 nm LiF: 59.3 ohm)
Characterization of LiF modified perovskite films. To explore
the reason why the PVSC with LiF layer exhibiting an
outstanding performance, the effect of LiF to the perovskite bulk
properties should be performed. We investigated the perovskite
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film’s bulk properties by the scanning electron microscope
(SEM) and X-Ray diffraction (XRD). Firstly, SEM images of the
perovskite films on the SnO2 layers with different LiF thicknesses
are shown in Fig. 2. The different perovskite films show very
similar surface morphology. These films are very smooth and
formed by hundreds nanometer perovskite crystals without any
observable pinholes. The XRD patterns are shown in Fig. S1.
Different perovskite films have the same peaks at 14.1° and 28.6°
which are attributed to the (110) and (220) planes of perovskite.
On the other hand, there is a small peak at 12.7° in all the films,
which indicate the existence of a small amount of PbI2 on the
grain boundary. Moreover, these PbI2 can passivate the trap
states on the grain boundary which is helpful to the PVSC.23
Figure 2. SEM of the perovskite film on different modified layers.
The films were deposited on ITO/ SnO2(/LiF or PbF2) substrates,
which can be described as follows: (A) 0 nm, (B) 0.4 nm LiF, (C)
0.7 nm LiF, (D) 1nm LiF, (E) 1.5nm LiF, (F) 0.7nm PbF2. The scale
bars are 1 μm.
From all the above results, it is evident that the perovskite films
with or without LiF are very similar in their morphology and
crystal structures.24 It also suggests that the difference of
devices’ performance cannot be attributed to the perovskite
film’s quality.
In order to shed light on the effect of LiF layer on the
absorption of device performance, the UV-vis absorption spectra
of the PVSC were investigated (Figure 3A). From the Fig.3A, the
absorption spectra of those PVSC almost share the same
tendency and have little difference in the region between 300 nm
and 1000 nm. And the similar absorption edges are observed for
all the samples which indicates a unified perovskite band gap is
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formed. 23 So it can be deduced that the LiF layer makes no
difference in the devices’ light absorption.
Since the light absorption of each device was nearly the
same, the difference in devices’ PCE could only come from the
different photoelectric conversion efficiency. So the PVSC’s EQE
spectra tests were conducted to give us more details about the
role of LiF layer on photoelectric conversion efficiency.25 The
EQE results obtained for the devices with and without LiF are
depicted in Fig. 3B. Devices B1 (0.4 nm LiF) and B2 (0.7 nm LiF)
showed higher conversion efficiency than other devices. Those
Nanoscale Accepted Manuscript
Figure 3. The absorption spectrum and EQE of different
devices. (A) The absorption spectrum of the PVSC. (B) EQE of
the PVSC.
devices with LiF had a better EQE than the reference one. In
general, higher EQE means more efficient carrier migration and
collection.
Identify the interfacial passivation of LiF modified Layer. As
the SEM and XRD measurement confirms that the bulk
properties of the perovskites film are not the source of
performance enhancement, we then pay our attention to the
interface. As we know, the existence of trap states at
SnO2/Perovskite interface will cause a charge recombination
leading to a reduced carrier density and Voc.14 Furthermore, for a
solar cell, the Voc usually followed the function of Jsc,26 as:
  
  , ln EQE  , ∆, (1)

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Nanoscale Accepted Manuscript

Figure 4. The PVSC’s Voc curves as a function of illumination intensity. (A) The PVSC’s Voc curves of all the device. (B) The Voc curve of
device A. (C) The Voc curve of device B1. (D) The Voc curve of device B2. (E) The Voc curve of device B4. The devices with different
thickness of LiF layer is indicated by different colors as shown in legend.

In the equation, Voc,rad is the radiative limit of Voc, EQEEL
describes the external quantum efficiency of
electroluminescence. According to this equation, the Voc is
affected by the carrier’s non-radiation combination. And the
surface trap states which can greatly promote the carrier’s non-
rad combination will reduce the Voc significantly. Here, we
investigated the PVSC’s Voc curves as a function of illumination
intensity to further explore the interfacial trap states suppressed
by the LiF layer.27 In this experiment two exciting light with the
wavelength of 427 nm and 575 nm were applied. Because of the
different absorption length (the blue light’s absorption length
(about 80 nm) is shorter than the red (about 300 nm), this
method can be applied to identify the carrier recombination near
the ETL/Perovskite interface.
As shown in the Fig. 4, the devices’ Voc were positive
correlated to the light intensity. Moreover, there is a big
difference between LiF modified PVSC and the reference cells,
especially in weak light intensity. All the devices with LiF layer
show a prefect linear dependence to the light intensity, while the
reference device A is not. In addition, device A’s Voc curves under
weak light are much smaller than the fitting curves deduced by
strong light condition. Secondly, device A always has a smaller
Voc than the LiF modified PVSC under different light intensity.
The 1 nm LiF device has the highest Voc which is coincide with
the device J-V test. Thus, we suggest a high non-radiation
combination is existing in the reference device A.26
On the other hand, the difference Voc curves between the
blue and red light of each device also gave us a hint where the
non-radiation combinations happened. For the device A, the red
light’s Voc were much higher than the blue light one. From the
equation (1), a smaller Voc indicates a more severe non-radiation
combination. Combined with the fact that the blue light’s
absorption length was shorter than the red one, the location of
these carrier non-radiation combination traps states can be
confirmed to be at the SnO2/perovskite interface. Furthermore,
for the device B1, B2, B3 the differences of Voc curves between
the blue and red were reduced and even eliminated. It suggested
that the LiF layer has successfully eliminated the surface trap
state.
The devices’ impedance spectra measurement can further
identify the effect of modified layers on the surface trap states
and charge collection.28 Fig. 5A illustrates a schematic diagram of
the Nyquist plot of the PVSC with/without LiF layers and the
equivalent circuit which will be useful in the EIS analysis.29 All
the device’s Nyquist plots show a typical shape as reported
perovskite Nyquist curve plot, which is a half circle at high
frequency and an arc at low frequency. The equivalent circuit
used to describe these two features comprises the charge
transport resistances Rs, recombination resistance (Rrec), the
selective contact capacitance (Ccon) owing to the charge buildup
at the interfaces of perovskite/contact layers, the dielectric
relaxation resistance (Rdr) and the dielectric relaxation
capacitance (Cdr) of the perovskite film. Among these parameters
deduced from the equivalent circuit, the charge transport
resistance Rs and the Ccon are the two most important
parameters to characterize the role of LiF layer. The Rs is
constituted of the resistances of FTO, SnO2, LiF, perovskite, HTL,

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device’s Voc from 1.06 to 1.14 V, while LiTFSI does not affect the
devices’ Voc. Therefore, the F- ion may be the main factor to the
device performance improvement. Recently, Zuo et al. has
demonstrated that the F- ion may change the interfacial chemical
interaction and suppress the surface trap states efficiently19, the
device improvement in this work could also be attributed to the
similar mechanism.
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Conclusions
A simple method of inserting LiF layer has increased the PCE of
the perovskite solar cell up to 18.3%, with a nearly 0.1 V
improvement in Voc. Without a doubt, the light dependent Voc
and impedance results have proved that LiF layer could

Nanoscale Accepted Manuscript

effectively passivate interface trap state between SnO2 and
Perovskite. The F- iron on the surface is suggested to play an
important role of adjusting the interfacial chemical interaction
which suppress the surface trap states efficiently. Our research
highlights a new way to passivate the SnO2/Perovskite interface
trap states, which is of great interest to the device researchers.

Acknowledgments

This work was supported by the Science and Technology

Commission of Shanghai Municipality, the Ministry of Science
and Technology of China, and National Natural Science
Foundation of China.

Figure 5. The Nyquist plot of the PVSC and the equivalent

circuit. (A) The Nyquist plot of the PVSC under 1 sun. (B) Notes and references
The simplified equivalent circuit diagram. (C) Table 2.
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The reference device A’s Ccon is the biggest, which is 11.1 nF. With
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Nanoscale Accepted Manuscript

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