Optical Materials 127 (2022) 112348

Contents lists available at ScienceDirect

Optical Materials
journal homepage: www.elsevier.com/locate/optmat

Lithium chloride-based interface engineering at electron transport and

perovskite layers to boost the performance of perovskite photovoltaics
Mustafa K.A. Mohammed a, *, Haider G. Abdulzahraa b, Sangeeta Singh c, P. Sasikumar d,
Majid S. Jabir e
a
Radiology Techniques Department, Dijlah University College, Al-Masafi Street, Baghdad, 00964, Iraq
b
Department of Prosthodontic, Dijlah University College, Al-Masafi Street, Baghdad, 00964, Iraq
c
Microelectronics Lab, National Institute of Technology, Patna, 800005, India
d
Department of Physics, Periyar University, P.G Extension Center, Dharmapuri, Tamil Nadu, India
e
Applied Science Department, University of Technology, Iraq

A R T I C L E I N F O A B S T R A C T

Keywords: During the past decade in the perovskite solar cells (PSCs) field, mesoporous titanium oxide (mp-TiO2) has been
Perovskite widely used as electron transport layers (ETLs) to promote the electron extraction process and also as a scaffold
Lithium chloride for the perovskite layer (PSK) to gain better PSC performance. Usually, the interface between the mp-TiO2 layer
Electron transport layer
and PSK needs a modification process to boost the performance of mp-TiO2-based PSCs. Here, lithium chloride
Interface engineering
(LiCl) was used to modify the ETL/PSK interface. Results showed that a simple interface engineering based on
LiCl could improve the morphology and crystalline properties of the PSK film, and motivate charge transport
processes at the ETL/PSK interface and within PSK due to lower grain boundaries in PSK. Overall, ETL interface
engineering with a 0.03 M LiCl solution leads to an efficiency of 11.24% for PSCs, higher than that of 7.42% for
control devices. In addition, the modified PSCs compared to control PSCs were more stable in an environment
with a humidity of 25%. The improved stability is caused by reduced GBs and a suppressed lead iodide (PbI2)
surplus in the modified PSK.

1. Introduction outstanding stability, essentially under moisture condition, which is

Solid-state organometallic PSCs are one of the promising optoelec­
tronic device technologies [1–4]. In the last decade, PSCs have yielded
PCE close to or even better than those of accomplished traditional
silicon-based solar cells, from 3.8% up to a PCE of 25% with a n-i-p
structure, making it an outstanding and emerging candidate for future
photovoltaic commercialization [5–9]. Nevertheless, their intrinsic
features and the most utilized solution-processing method result in a
number of defects at grain boundaries (GBs) and interfaces of functional
layers [10–12]. The produced trap states can cause unappropriated
hysteresis effects, decline PCE, and increase instability, which prevent
perovskite materials from being scaled up in the photovoltaic market
[13–18]. For this content, many attempts by researchers have been re­
ported to tackle these problems, for instance, using passivation agents,
additive engineering, or solvent engineering to enhance the photovol­
taic parameters and reduce the instability [19–22]. Among these,
interfacial passivation is commonly used approach thanks to their
important in scaling-up the PSCs, and suitable optoelectronic properties
[5,20,23,24].
Perovskite solar cells are already attaining such consistently high
levels of efficiency that scalable, low-cost production is becoming
crucial. However, due to the high cost of hole-transporting materials and
the problems involved with scalable deposition of additional functional
layers, this remains a challenge. Different approaches are used to
construct hole-transport-layer (HTL)-free PSCs with increased photo­
voltaic performance by simplifying the device design [22,24–26]. By
reducing one step of the standard coating process, at least one third of
the manufacture cost and time can be saved, in addition to savings of
material cost for the HTL. The reported ambipolar charge transfer fea­
tures of hybrid perovskites endow them with considerable potential to
construct PSCs with simplified device structure, such as HTL-free PSCs
with either conventional or inverted structure due to the perovskite can
acts as light absorber as well as a hole carrier, fulfilling high PCE [27].
This structure helps the PSC structure, improves the stability of PSC, and

* Corresponding author.
E-mail address: mustafa_kareem97@yahoo.com (M.K.A. Mohammed).

https://doi.org/10.1016/j.optmat.2022.112348
Received 10 February 2022; Received in revised form 29 March 2022; Accepted 7 April 2022
Available online 11 April 2022
0925-3467/© 2022 Elsevier B.V. All rights reserved.
M.K.A. Mohammed et al.
removes the use of HTL that decreases the device price. Also, HTL-free
PSCs have been reported in literature aimed to improve the perfor­
mance perovskite solar cells without using HTL. The electron transport
layer (ETL) performs a functional role in the structure of PSCs. The
additives have been used in the mesoporous TiO2 precursor solution to
improve the ETL and the performance of PSCs. It found that this additive
treatment increased the performance and stability of HTL-free PSCs.
Also, the use of additives with excellent properties in the electron
transfer layer ensures facilitating electron transfer and improving the
surface of the perovskite layer [17,26].
Different interfacial modifiers have been used in the PSCs, such as
carbon nanomaterials [11,15,28], ammonium fluoride [29], poly­
ethylenimine [30], and so on. Shaoxi and co-workers have used lithium
(Li) and cobalt (Co) to improve the collection of photo-generated car­
riers in inverted planar PSCs. Compared to the pristine devices, loading
an optimal content of Li and Co can improve optical absorption, elec­
trical conductivity, and charge mobility of the PSCs, yielded a power
conversion efficiency (PCE) of 18.7% [31]. Minjin and co-workers re­
ported Li-salt doping in mp-TiO2 ETL for perovskite devices. The Li2CO3
salt doping of mp-TiO2 resulted in conduction bands deeper than those
of unmodified films, which led to the certified PCE of 24.68% (Newport)
[32]. Xianhua and co-workers used Li dopant to enhance the quality of
inorganic CsPbIBr2 perovskite films. Also, the Li doping approach helped
promoted the morphological, optical, and optoelectronic merits of the
solution-processed CsPbIBr2 layers. The trap-state defects in the modi­
fied layer have been suppressed while the charge lifetimes are elongated
by Li incorporating them, resulting in less energy loss and a higher PCE
(9.25%) [33]. A salt of LiCl has been added to tin oxide (SnO2) ETLs for
planar PSCs. As shown by their work, using LiCl could improve the
charge transfer in the SnO2 layer and improve the optical stability.
Modified PSCs recorded a high and steady-state PCE of 18.3% with
prominent stability [34].
In this paper, we report the method of passivation at mesoporous-
TiO2/perovskite interfaces by using LiCl salt. We found that the modifier
layer exhibits enhanced properties at the ETL/perovskite interface, and
as a result, the overall device performance is higher in the case of LiCl
devices. Our results reveal that the addition of LiCl not only passivates
the surface of TiO2, but also suppresses recombination at the interfaces.
This leads to improved PCE in the case of LiCl modified PSCs.
2. Experimental details
2.1. Materials and chemicals
Unless otherwise stated, all materials were provided from Sigma-
Aldrich. Methylammonium iodide (MAI) and PbI2 were bought from
LumTec. Commercial TiO2 paste (30 NR-D) was obtained from Dyesol.
lithium chloride (LiCl) was provided from AlfaAser.
2.2. Solution synthesis
In brief, 1.42 M of PbI2 was dissolved in a mixed solution of N,N-
dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) (9:1 v/v).
The produced solutions were stirred at 70 ◦ C for 40 min. Finally, 159 mg
of MAI was added into the cooled PbI2 solution and stirrer for 15 min at
room temperature to prepare MAPbI3 solution. The TiO2 was mixed in
ethanol (EtOH) (1:6 wt%) and stirred for one day at room temperature to
attain a mesoporous TiO2 (mp-TiO2) precursor. To prepare LiCl solu­
tions, different amounts of it were dissolved in deionized water and
sonicate for 30 min.
2.3. Solar cells preparation
The patterned fluorine-doped tin oxide (FTO, 6 Ω/sq, 15 ╳20 mm2)
substrates were washed using ultrasonic device with deionized water,
ethanol, and methanol for 15 min in successive manner. A compact TiO2
2
Optical Materials 127 (2022) 112348
(c-TiO2) films were deposited on substrates at 5000 rpm and baked at
450 ◦ C for 35 min. The mp-TiO2 layers were coated on the c-TiO2 at
4500 rpm for 30 s, then annealed at 500 ◦ C for 1 h. To modify mp-TiO2
layers, LiCl solutions were spin-coated over them with an annealing step
at 500 ◦ C for 30 min. To fabricate the perovskite layer, 50 μL of PSV
precursor was poured on the substrate and spin-coated at 1000 rpm for
8 s and then accelerated to 4500 rpm for 20 s. In the second stage, 100 μL
of chlorobenzene was pipeted onto the perovskite layer to assist crystal
growth of PSK films. The fabricated PSKs were annealed for 30 min at
100 ◦ C. Finally, an 85 nm gold contact was thermally deposited at the
rate of 2 Å/s on the PSV films.
2.4. Characterizations
The scanning electron microscope (SEM, TESCAN, MIR3) was uti­
lized to visualize the morphology of PSK films. The X-ray diffraction
(XRD) analyses of the PSK films were collected with a Bruker, D8
advance XRD spectrometer. The ultraviolet–visible spectroscopic mea­
surements of the PSK and ETL were studied by LAMBDA 1050 a spec­
trophotometer. The steady-state photoluminescence (PL) plots of PSKs
were collected with a HORIBA Fluorolog-III device. The J-V measure­
ments of the MAPbI3-based devices were characterized using a Keithley
Model 2400 under AM 1.5 light simulator. The Si reference cell was used
to calibrate the light simulator. The active area of perovskite solar cells
was 6 mm2.
3. Results and discussion
The PSK layer quality is essential for the final performance of the
perovskite devices, while the light absorbance, crystallinity, and
morphology of the PSK layers are the main indicators. For the purpose of
studying the impact of underlayer net ETL and modified ETLs on the
optical absorption and charge transportation of PSK film, we performed
UV–vis and steady-state PL measurements of PSK fabricated by the
antisolvent-assisted spin-coating approach. The PSK absorbance spectra
of pure and modified mp-TiO2 with different concentrations of LiCl are
shown in Fig. 1a. From the ultraviolet to the visible wavelength range,
the absorbance for all PSK layers is higher compared to the unmodified
film. The 0.03 M LiCl-based PSK film revealed a slightly stronger spec­
trum compared to the other modified layers because of the improved
PSK crystallization process due to LiCl treatment, which is in good
agreement with the XRD data [35]. The films showed the same ab­
sorption edges at 795 nm since the PSK energy bandgap was 1.55 eV.
Steady-state PL analyses were utilized to investigate the ability of car­
riers to transfer from PSK film to ETL [36–38]. In Fig. 1b, it is clearly
detected that the photoluminescence intensity of PSK is quenched with
LiCl doping in mp-TiO2 films. Furthermore, the high intensity of the PL
peak is highly suppressed with 0.03 M LiCl incorporated, indicating that
the salt loading can inhibit the recombination of photo-induced carriers
and promote electron transpiration rate from PSK to ETL film [39–41].
Fig. 1c displays the UV–vis transmission spectra of the pure mp-TiO2 and
LiCl-modified mp-TiO2 ETLs. As well-known by the bandgap of TiO2, it
showed low transparency in the range of 300–400 nm and high trans­
parency in the range of 450–900 nm. As expected, LiCl treatment could
influence the transmittance of TiO2 films, where the highest decrease in
the spectrum was observed for 0.04 M LiCl modified film in the range of
450–850 nm. This reduction could lead to a reduction in the photocur­
rent density of corresponding PSC devices.
As shown in SEM images (Fig. 2), the PSK layers demonstrate smooth
surfaces and dense polycrystalline particles. The PSK particle size is
more homogeneous with modified TiO2 ETLs than the pristine TiO2.
Moreover, compared to pure ETL-based PSK film (Fig. 2a), the modified
ETL based PSK layers show bigger grain sizes (Fig. 2b–d). The large size
of the crystallized PSK grain exhibits that the MAPbI3 morphology can
be enhanced by ETL treatment with LiCl doping, which is beneficial for
light absorption and charge transport [42]. ImageJ software was used to
M.K.A. Mohammed et al. Optical Materials 127 (2022) 112348

Fig. 1. (a,b) Absorption and photoluminescence spectra of perovskite layers on mesoporous titanium oxide (mp-TiO2) electron transport layers (ETLs) modified with
lithium chloride (LiCl) solution with different concentrations in deionized water. (c) Optical transmittance of different mp-TiO2 ETLs modified with LiCl solutions.

Fig. 2. Top-view FESEM images of fabricated perovskite layers on modified mesoporous titanium oxide (mp-TiO2) electron transport layers with lithium chloride
(LiCl) solutions with different concentration in deionized water: (a) 0.00 M (b) 0.02 M, (c) 0.03 M, and (d) 0.04 M. (e) Grain size distributions of perovskite layers
fabricated on modified ETLs with different LiCl solutions.

determine the average grain size of MAPbI3 films. In Fig. 2 e, the average
grain size was increased from 300 nm of pure PSK film to 380 nm, 510
nm, and 408 nm for modified PSK films with 0.02 M, 0.03 M, and 0.04
M, respectively. The enlarged grains have a positive effect on the
morphology of the MAPbI3 film, for example enhancing the crystalline
nature and photon light absorbance efficiency as well as decreasing the
trap defects in the GBs. The crystallinity improvement in the LiCl-based
perovskite layer is attributed to the assistant effects of Cl on perovskite
growth [43,44].
The crystalline nature of the PSK layers on pure and optimized ETLs
was characterized by an XRD test and the results are described in Fig. 3a.
Obviously, X-ray diffraction peaks cantered at 13.81◦ , 19.97◦ , 28.19◦ ,
31.67◦ , and 40.42◦ are detected, which are related to (110), (112),
(220), (310), and (224) facets of the MAPbI3 tetragonal polycrystalline
structure, respectively [45]. The PSK film spin-coated on modified ETL
shows significantly improved crystallinity, which has been verified via
FESEM measurements. Also, for the film modified with 0.03 M of LiCl,
the PbI2 signal (at 12.3◦ ) is vanished. The zoomed XRD areas at the main

3
M.K.A. Mohammed et al. Optical Materials 127 (2022) 112348

Fig. 3. (a) XRD patterns of perovskite layers based on modified mp-TiO2 layers with lithium chloride (LiCl) with concentration of 0.00 and 0.03 M. Zoomed XRD
patterns around 2θ = 13.8◦ to measure full width at half maximum (FWHM) of perovskite film fabricated on (b) 0.00 M-LiCl and (c) 0.03 M-based mp-TiO2 ETL.
Contact-angle of perovskite droplet on the (d) neat mp-TiO2 and (e) modified mp-TiO2 with LiCl.

(110) peak are present in Fig. 3a–b. These figures confirm our hypothesis
Table 1
for crystallinity improvement by showing the values of FWHM and peak
Photovoltaic parameters of PSC devices based on of modified mp-TiO2 films with
intensity, where the modified film revealed a decreased FWHM value
different amounts of LiCl.
and improved peak intensity.
The contact angle of perovskite precursor on different ETLs was ETL type Voc (V) Jsc (mA/cm2) FF (%) PCE (%)

monitored (Fig. 3d and e) to find how modification of ETL with LiCl 0.00 M Average 0.804 16.91 50.62 6.29
leads to the formation of a desirable perovskite layer without PbI2 sur­ Best 0.808 16.77 51.90 7.42
0.01 M Average 0.818 18.25 53.93 8.05
plus content. As can be seen, by incorporation of LiCl into the ETL, the
Best 0.834 19.03 56.70 8.99
contact angle value increased form from 15◦ to 30◦ , referring to the 0.02 M Average 0.843 19.90 55.48 9.34
increased non-wetting behavior of ETL. This phenomenon suppresses Best 0.859 20.12 56.00 9.94
heterogeneous nucleation sites and brings larger perovskite grains [46]. 0.03 M Average 0.885 20.46 59.18 10.69
Besides, by reducing nuclei centers and tending to homogeneous Best 0.910 20.39 60.60 11.24
0.04 M Average 0.856 18.65 52.95 8.46
nucleation, the interaction of MAI and PbI2 is prompted during the Best 0.859 20.12 54.20 9.36
growing of perovskite islands, and unreacted PbI2 in the perovskite layer
is reduced.
The regular n-i-p configuration of the HTL-free PSC is FTO/c-TiO2/ PSC degrades. The improved Jsc and FF may be associated with the
mp-TiO2/MAPbI3 PSK/Au and is schematically shown in Fig. 4a. The improved electrical features of the LiCl modified-ETLs and fabricated a
mp-TiO2 layers were modified with LiCl solvent with different contents. PSC film with better quality, which is beneficial for efficient charge
The single-cation MAPbI3 films were fabricated using the anti-solvent transfer and suppressed carrier recombination at the PSC/ETL in­
spin-coating method by chlorobenzene assistant. Fig. 4b illustrates the terfaces. Further characterization was conducted to deeply study the
best-performing J-V plots of the HTL-free PSCs modified with different performance improvement mechanism resulting from LiCl addition. The
amounts of LiCl solvent under an AM 1.5G solar simulator. The PV pa­ dark J-V measurements are shown in Fig. 4c. The J-V test reveals that the
rameters of different PSCs, including Jsc, Voc, FF and PCE, are summa­ modified PSC shows a lower leakage current than the unmodified de­
rized in Table 1. The PCE of the PSC with pure mp-TiO2 is 7.42% with a vice, indicating a larger shunting resistance. The higher leakage current
Voc of 0.808 V, a Jsc of 16.77 mA/cm2 and an FF of 51.9%. It’s worth of the pure MAPbI3 PSC can be assigned to the more defects and GBs
noting that the PSC properties are remarkably improved via using LiCl lying in the PSK layer, working as the current shunting routes. The
doped mp-TiO2 as ETLs. As shown, 0.03 M of LiCl enhances the per­ reduced current is beneficial for the improvement of the Jsc and fill
formance of MAPbI3 devices, resulting in a PCE of 11.24%, a Jsc of 20.39 factor [33,47].
mA/cm2, a Voc of 0.910 V, and an FF of 60.6%. Nevertheless, with Fig. 5 shows PV data measured from eight cells with each type of LiCl
further loading of LiCl solvent, the performance of the corresponding solvent concentration (0, 0.01 M, 0.02 M, 0.03 M, and 0.04 M). Clearly,

Fig. 4. (a) PSC device architecture with mesoscopic ETL. (b) Current density-voltage (J–V) curves of the best-performing perovskite solar cells based on different
electron transport layers (ETLs). (c) Dark J-V measurements of PSCs based on 0.00 M- and 0.03 M-modified ETLs with lithium chloride.

4
M.K.A. Mohammed et al.
Fig. 5. The statistical distribution of photovoltaics parameters of PSCs without and with different amounts of lithium chloride modified ETLs. (a) Voc, (b) Jsc, (c) FF
and (d) PCE. The parameters were measured from 8 cells per each concentration.
LiCl modification reveals a comprehensive enhancement in the Jsc, Voc
and FF, resulting in a higher PCE of the HTL-free PSCs. This demon­
strates a more efficient carrier extraction and mitigated recombination
process, resulting from the improved morphology and less trapped de­
fects of the LiCl-based PSK, as described above. The average efficiency of
the PSC is boosted from 6.26% to 10.69% by 0.03 M LiCl. From the box
charts, the reproducibility of the as-fabricated PSCs can be evaluated.
The PCEs of the unmodified cells are mainly distributed with a higher
standard deviation than the modified cells. The narrower PV distribu­
tion suggests improved reproducibility of the modified PSCs. This could
be related to the improved quality of the LiCl-modified MAPbI3 film.
The long-term stability of unsealed PSC devices is measured with a
relative humidity (RH%) of 25% under ambient air and dark conditions.
Fig. 6. Shelf stability test of the unsealed perovskite solar cells based on 0.00
M- and 0.03 M-modified mp-TiO2 electron transport layer (ETL) substrates with
lithium chloride, at room temperature stored in ambient air with a relative
humidity of ~25% in dark conditions.
5
Optical Materials 127 (2022) 112348
Fig. 6 demonstrates the measured PSC PCE as a function of aging time
during 35 days. Compared to control PSCs without treatment, the
longevity of cells with LiCl-modified ETLs is remarkably enhanced. For
instance, after 35 days, the unmodified cells only retained 23% of their
original performance with fast declining. Nevertheless, cells based on
LiCl-modified ETLs retain 83% of their original PCE values during the
same period. The enhanced longevity could be attributed to better ETLs/
PSK interface contact, which improves film crystallinity and quality of
the MAPbI3 photoactive material.
4. Conclusions
In summary, this work reports the introduction of LiCl salt as a facile
modifier in the mp-TiO2 layer to enhance the ETL/PSK interface,
improving both the device performance and stability of the HTL-free
PSC. The enhanced interface contact could improve the carrier trans­
port and alleviate the recombination rate, which could be verified by the
steady-state PL measurement. Upon loading LiCl solvent into the TiO2, a
highly crystallized and well-oriented PSK film is successfully developed.
The as-fabricated LiCl-modified film reveals a more uniformed topog­
raphy with bigger crystals and passivated GBs compared to the un­
modified film. The inserting of this solvent modifier enhances the
performance of devices, enabling high PCE over 11% and this PCE is
higher than that of the unmodified devices (7.42%). Air stability of the
modified devices has been measured under 35 days of storage, and PSCs
have shown their potential as promising stabilizers for HTL-free perov­
skite solar cells by securing air stability at 25◦ and 25% RH. This work
provides a simple and effective approach for ETL/PSK interface treat­
ment and improves the PV performance of HTL-free PSC further.
CRediT authorship contribution statement
Mustafa K.A. Mohammed: Writing – original draft, Writing – re­
view & editing. Haider G. Abdulzahraa: Writing – original draft,
Writing – review & editing. Sangeeta Singh: Writing – original draft,
M.K.A. Mohammed et al. Optical Materials 127 (2022) 112348

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