Nano Today 37 (2021) 101062

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Review

Photoferroelectric perovskite solar cells: Principles, advances and

insights ]]
]]]]]]
]]

⁎
Huilin Li a, Fumin Li a, Zhitao Shen a, Su-Ting Han d, Junwei Chen b, Chao Dong b, Chong Chen a, ,1,
⁎ ⁎
Ye Zhou c, ,2, Mingtai Wang b, ,3
a
Henan Key Laboratory of Photovoltaic Materials, Henan University, Kaifeng 475004, PR China
b
Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, PR China
c
Institute for Advanced Study, Shenzhen University, Shenzhen 518060, PR China
d
Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen 518060, PR China

a r t i cl e i nfo a bstr ac t

Article history: Increasing environmental crises caused by exploring and using fossil fuels have compelled human being to
Received 31 July 2020 develop innovative technologies to utilize renewable and sustainable energy sources. For this purpose,
Received in revised form 8 December 2020 photovoltaic conversion of solar energy into electricity with solar cells is a promising and attracting way in
Accepted 20 December 2020
that solar energy is clean and inexhaustible. Nowadays, the bottleneck in the application of solar cells on a
Available online 13 January 2021
large scale to sustainable energy generation still lies in lacking an efficient, stable and low-cost materials
system for photon-to-electricity conversion. Perovskite materials are a class of materials widely applied in
Keywords:
Solar cells solar cells. Many evidences showed that the perovskite materials have both ferroelectric and photovoltaic
Perovskite properties, offering a special system called photoferroelectric materials. A built-in electric field established
Photovoltaic in these materials due to the ferroelectric property is more helpful for the separation of e-h pairs and
Ferroelectric enhancing the power conversion efficiency during photovoltaic process in solar cells. Here, we review the
Photoferroelectric recent photoferroelectric perovskite solar cells (PPSCs). After giving a brief description of the structure and
property of photoferroelectric perovskite materials, the device structures, working principles and char­
acterization of PPSCs are introduced, followed by the state-of-the-art advances and the insights for the
PPSCs based on oxide and halide perovskite materials. Finally, the main challenges in developing efficient
PPSCs are discussed.
© 2020 The Author(s). Published by Elsevier Ltd.
CC_BY_NC_ND_4.0

Contents

. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
. Perovskite materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
. Basic aspects of PPSCs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
. Device structure and working principle of PPSCs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
. Photovoltaic parameters of PPSCs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
. Recent advances in PPSCs. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
. Oxide PPSCs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
. Halide PPSCs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
. Hybrid halide photoferroelectric perovskites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
. Inorganic halide photoferroelectric perovskites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
. Challenges, prospects and conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13

⁎
Corresponding authors.
E-mail addresses: chongchen@henu.edu.cn (C. Chen), yezhou@szu.edu.cn (Y. Zhou), mtwang@ipp.ac.cn (M. Wang).
1
ORCID: 0000-0003-2940-2030.
2
ORCID: 0000-0002-0273-007X.
3
ORCID: 0000-0002-5038-5020.

https://doi.org/10.1016/j.nantod.2020.101062
1748-0132/© 2020 The Author(s). Published by Elsevier Ltd.
CC_BY_NC_ND_4.0
H. Li, F. Li, Z. Shen et al. Nano Today 37 (2021) 101062

. Challenges . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
. Solution-processed stable photoferroelectric layer . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
. Characterization norm . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
. Physical insights . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
. Prospects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
. Molecule engineering to enhance ferroelectricity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
. Combination of halide and oxide perovskites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
. Multi-effects to increase the efficiency of PPSCs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
. CRediT authorship contribution statement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
. Declaration of Competing Interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
. Acknowledgments. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
. References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16

Introduction 26 meV, where kB is the Boltzmann constant and T is the tempera­

ture), resulting in the unfavorable geminate recombination of
The global energy is still mainly produced from fossil fuels. charge-transfer excitons [19,20]. A promising method to improve the
Facing the exhaustible fossil fuels and the catastrophic destroy and Ebi field in PSCs is to create an additional electric field using ferro­
pollution to environment resulting from mining and using them, electric materials. The polarization-induced electric field strength in
human being has to develop the technologies for the utility of re­ a ferroelectric material is approximately one to two orders of mag­
newable and clean energy. The sun is the most fundamental energy nitude higher than that in a semiconductor p-n junction [21], and
to the earth, and can provide inexhaustible and clean energy. Solar the field width spans the whole ferroelectric material [22], which
cells, which directly convert absorbed sunlight into electricity, are facilitates the separation of e-h pairs. Nalwa et al. reported that
the most promising photovoltaic devices to solve these serious en­ doping with ferroelectrics leads to localized enhancements of elec­
vironmental and energy problems caused by using fossil fuels. To tric field in photovoltaic active-layer with a resulting internal
date, crystalline silicon (Si) solar cells dominate the commercial quantum efficiencies of ca. 100%, and the PCE of the solar cell is
markets because of their superior stability and high power conver­ consequently increased by nearly 50%, indicating a much more ef­
sion efficiency (PCE). However, the expensive availability of high- ficient dissociation of singlet-excitons and charge-transfer-excitons
purity Si sources for photovoltaics and the costly fabrication of de­ as the result of the enhanced electric field [23]. Similarly, it has been
vices due to the high melting point of silicon (~ 1414 °C) limits the demonstrated that an enhanced the build-electric field by ferro­
application of crystalline Si solar cells to the terrestrial power gen­ electrics did make more charges separate in solar cells and sig­
eration by photovoltaics on a large scale [1]. nificantly improve the device PCE [24].
Oxide/halide perovskite solar cells (PSCs) are prepared at a lower In fact, many perovskite materials have a good ferroelectricity,
temperature (< 1000 °C for oxides but < 200 °C for halides) compared such as BaTiO3 [25], BiFeO3 [26] and CH3NH3PbI3 [27]. Ferroelectric
with crystalline Si solar cells. In particular, halide PSCs are solution- materials can display a spontaneous polarization due to the non­
processible at low cost and have achieved a fast improvement in PCE centrosymmetry of crystallographic unit cell, and have been used
from 3.8% in 2009 to 25.2% in 2020 [2,3]. Generally, during a pho­ widely in the fields including field effect transistors [28,29], non-
tovoltaic process, weakly bound electron-hole (e-h) pairs with a volatile memories [30–32], memristors and synapses [33–35]. The
small binding energy (Eb) are generated by photons absorption, and coupling of ferroelectricity and photovoltaic effect was envisioned
separated by a built-in electric field to form net electric current flow 41 years ago by Fridkin, who imagined a “photoferroelectric crystal”
[4]. In order to increase the PCE of solar cells, one effective way is to for a potential solar cell [36]. Since then, the photoferroelectric de­
use low bandgap materials to absorb lower energy photons for the vices have attracted the attention of academics. Therefore, photo­
generation of more e-h pairs because approximately 50% of the ra­ ferroelectric devices were mostly developed using perovskite
diant energy from the sun is in the infrared range (> 760 nm); an­ materials.
other way is to reduce the recombination of photogenerated e-h In this review, we refer to the solar cells based on both ferro­
pairs, caused by intrinsic point defects [5–8], impurities [9,10], sur­ electric and photovoltaic effects of photoferroelectric perovskites as
face defects [11], grain boundaries [12] and clusters [13,14], to en­ the photoferroelectric perovskite solar cells (PPSCs), and summarize
hance the collection efficiency of photogenerated charge carriers. the recent advances in the state-of-the-art technologies for devel­
Many researchers have concentrated on the passivation of defects in oping PPSCs. The outline of this paper is as follows: (1) The structure
PSCs to reduce charge recombination for an increased device PCE and property of ferroelectric perovskite are introduced to provide a
[15–18]. Zhao et al. reported a surface treating method with choline basic knowledge for understanding the PPSCs. (2) Basic aspects of
iodide in the β-CsPbI3-based PSCs, by which the charge-carrier life­ PPSCs are described including the device architecture, working
time was increased significantly and the PCE increased to 18.4% from principle and characterization. (3) The recent advances in PPSCs are
15.1% [15]. Yan et al. showed a method that can oxidize selectively discussed, focusing on oxide and halide perovskite materials. (4)
Pb0 and reduce I0 defects simultaneously with the europium ion pair Some strategies are envisioned for developing efficient PPSCs.
(Eu3+-Eu2+) in the CH3NH3PbI3-based PSCs, and the PCE was pro­ Notably, there are several review articles that describe the basic
moted to 21.52% with a substantially improved long-term dur­ knowledge and physics mechanism of photoferroelectric perovskite
ability [16]. materials and photovoltaics devices [37–41].
However, it is still not enough to improve the PCE only by pas­
sivating of defects. The separation of weakly bound e-h pairs is
Perovskite materials
normally driven by the built-in electric field (Ebi) due to the for­
mation of a space-charge region (i.e., depletion zone) across the p-n
In general, perovskite materials have a general structure of ABX3,
junction, but it is generally too weak to efficiently separate the
where six X-site anions coordinated to a B-site cation form a BX6
tightly bound e-h pairs (i.e. excitons) that have an Eb much larger
octahedral framework and twelve A-site cations occupy the centers
than the thermal energy at ambient temperature (i.e., Eb > > kBT ~
of four BX6 octahedra (seeing Fig. 1a). Each of the A, B and X sites can

2
H. Li, F. Li, Z. Shen et al.
Fig. 1. (a) Crystal structure of a typical ABX3 perovskite. (b) Schematic illustration of the hysteresis loop for electric displacement versus electric field. (c) Hysteresis loop of
PbZr0.5Ti0.5O3 at the temperature of 300 K. Reproduced with permission [48]. Copyright 2018, American Chemical Society. High-resolution (d) PFM and (e) pc-AFM images of a
typical MAPbI3(Cl) sample surface. Reproduced with permission [27]. Copyright 2017, Royal Society of Chemistry.
accommodate one or multiple elements. However, to form a stable
perovskite structure, the Goldschmidt tolerance factor (t) must be in
range of ~ 0.8–1.0, and the octahedral factor (μ) in ~ 0.4–0.9, which
the formulas are as follows [42]:
rA + rX
t=
2 (rB + rX )
rB
µ=
rX
where rA, rB and rX are ionic radii of A, B and X sites, respectively.
Normally, orthorhombic or rhombohedral structure is formed in
range of 0.7 ≤ t ≤ 0.9, and cubic structures will be formed when
0.9 < t < 1.0, but other structures (e.g., hexagonal and A4BX3-type)
are formed as t < 0.7 or t > 1.0 [43]. According to the X-site ele­
ments, perovskite materials can be divided into oxide and halide
perovskite materials. If X-site element is oxygen, it is called oxide
perovskite material and the structure is usually be expressed by
ABO3, for which A-site elements are often Li, Na, K, Ca, Sr, Ba, Bi and
Pb, and B-site elements are Zr, Ti, Nb, Fe, Mn and Ta [44,45]. If X-site
element is halogen (e.g., Cl, I, Br), this material is known as halide
perovskite material, where A-site elements can be some metallic
elements (e.g., Cs, Rb) for all-inorganic perovskites, or some organic
functional groups (e.g., CH3NH3, CH(NH2)2) for organic–inorganic
halide perovskites (also called hybrid halide perovskites), while B-
site elements are often Sn, Pb [46,47].
Nano Today 37 (2021) 101062
Ferroelectricity of a perovskite material is determined by the
structure and symmetry of its crystalline unit cell. The prerequisite
for ferroelectricity is to have non-centrosymmetric unit cell. In the
family of unit cells, 21 kinds have noncentrosymmetry, and 20
types are the piezoelectric crystals that can lead to a displacement
of charges under mechanical stress and vice versa. Among these 20
(1) types of unit cells, 10 of them exhibits a permanently polarized
state referred to as being pyroelectric. In the pyroelectric state, the
polarization can be reoriented under a certain external electrical
(2) bias, and this property is called ferroelectricity. Obviously, all fer­
roelectrics are both piezoelectrics and pyroelectrics. The resulting
polarization hysteresis is a simple and direct method to identify the
ferroelectricity. In the ferroelectric perovskites, a small area with
the same direction of polarization is called ferroelectric domain. As
shown in Fig. 1b, as the polarization directions of all the small areas
are random, the macroscopic polarization intensity of the material
(P) is zero. When an increasing electric field is applied, the polar­
izations of small areas will start to align toward the direction of the
polarization field; when all of the polarizations are in the same
direction, P reaches saturation at point A corresponding to the sa­
turated polarization (Ps) of the material. After that, the polariza­
tions will be nonlinearly changed along the road A → B → C→ D → E
→ F → A with changing the polarization field, exhibiting a hyster­
esis loop on which the coercive field (Ec) and remnant polarization
(Pr) are the key parameters for a ferroelectric material. Lead zir­
conate titanate (PZT) is a classic ferroelectric perovskite, and its
hysteresis loop at room temperature is characterized by the Ec of ca.
3
H. Li, F. Li, Z. Shen et al. Nano Today 37 (2021) 101062

Table 1
Summary of bandgaps in various perovskite materials exhibiting photovoltaic effects.

Materials Bandgap (Eg) Exciton binding energy (Eb)

Eg (eV) Ref. Eb (meV) Ref.

Oxide perovskites
KNbO3 >4 [57] 500 [58]
LiNbO3 3.78 [59] / /
Pb(Zr,Ti)O3 3.6 [60] / /
NaNbO3 3.5 [61] / /
CaTiO3 3.45 [62] / /
BaTiO3 3.3 [38] / /
PbTiO3 3.25 [63] / /
SrTiO3 2.96 [64] 220 [65]
BiFeO3 2.67 [51] / /
Bi2FeCrO6 1.4 [66] / /
BiMnO3 1.1 [51] / /
Halide perovskites
Organic–inorganic hybrid
MASnCl3 3.61 [67] 257 [68]
MAPbCl3 3.02 [69] 69 [70]
FASnBr3 2.4 [71] 95 [68]
FAPbBr3 2.27 [72] 149 [73]
MAPbBr3 2.22 [74] 64 [70]
MASnBr3 2.2 [75] 33 [76]
MAPbI3 1.55 [77] 16 [78]
FAPbI3 1.43 [79] 58 [73]
FASnI3 1.3 [80] 31 [68]
MASnI3 1.21 [81] 29 [68]
Inorganic
CsGeCl3 3.67 [82] / /
CsSnCl3 2.8 [83] 37 [84]
CsPbF3 2.55 [81] / /
CsPbBr3 2.35 [85] 40 [86]
CsGeBr3 2.32 [82] / /
CsPbCl3 2.1 [81] 75 [86]
CsSnBr3 1.75 [87] 19.6 [76]
CsPbI3 1.73 [88] 20 [86]
CsGeI3 1.51 [81] / /
CsSnI3 1.3 [89] 12.2 [84]

0.6 kV/mm and the Pr of 36 μC/cm2 (Fig. 1c) [48]. Moreover, another
method to identify the ferroelectricity is to measure the topo­
graphy of ferroelectric domain. Roehm et al. observed ferroelectric
domains in the organic–inorganic halide perovskite of MAPbI3(Cl)
by using piezoresponse force microscopy (PFM) and photo-con­
ductive atomic force microscopy (pc-AFM), and revealed the pat­
terns of highly ordered ferroelectric domains within different
polarizations (Fig. 1d, e) [27].
If a material absorbs photons with energies more than the bandgap
(hv ≥ Eg), the electrons will be excited from the valence band to the
condition band. This process will generate charge carriers including the
excitons for Eb > > kBT or the free charge carriers Eb ≈ kBT. The bandgaps
of common perovskite materials were listed in the Table 1. Most of
oxide perovskite materials are the good insulators with a wider
bandgap above 3.0 eV, which only generate charge carriers under ul­
traviolet (UV) light. In contrast, halide perovskites are almost semi­
conductor materials. Actually, 93% of the sunlight energy is within the
visible and infrared range of ~ 390–4000 nm in wavelength (λ), corre­
sponding to the energy of ~ 0.31–3.18 eV [49]. For a solar cell, the ideal
bandgap is around 1.4 eV that matches well the maximum photon flux
of AM 1.5G solar spectrum [50,51]. Therefore, in order to prepare high-
performance PSCs, the perovskite materials normally have the small
bandgaps. The main method to tune the bandgap is to vary the com­
position of the A-, B- and/or X-sites [52–55]. For example, Das et al. [52]
exploited a strategy of substituting two Ti4+ ions in BaTiO3 by one Mn3+
ion and one Nb5+ ion to obtain a photoferroelectric perovskite material
with low band gap (Eb = 1.66 eV) and high ferroelectricity (Ps = 15.4 μC/
cm2). Moreover, photogenerated excitons, electrically neutral quasi­
particle comprising tightly and Coulombically bound e-h pairs, play an
important role in controlling the photophysical properties of materials.
Semiconductors with a low exciton binding energy are highly desirable
in solar cells, because of the easy dissociation of their excitons into free
carriers on sub-ps time scale [56]. Amongst the perovskite materials,
especially halide perovskites, those with a narrow bandgap generally
have a low Eb (Table 1).
Basic aspects of PPSCs
Device structure and working principle of PPSCs
The photoexcited charge carriers (e-h pairs), once generated, will
quickly decay back to the ground state, when they are not dis­
sociated and extracted into other material phases under open-circuit
condition for example. To obtain the photocurrent, it is essential to
for the charge carriers to effectively separate and be collected by
electrodes. In the early solar cells, a Schottky barrier formed by
placing a layer of selenium between two different metallic contacts
was used to separate the photon-generated charge carriers upon the
absorption of the selenium layer, and realize the photovoltaic effect
[90]. The p-n junction, prepared by doping different regions of a
single piece of silicon with phosphorous and boron, was found to be
effective for the charge generation under illumination in the 1950s
[37]. Up to date, the commercial crystalline Si solar cells continue to
follow the p-n junction architecture (Fig. 2a). In the p-n junction
devices, a built-in electric field Ebi is rendered due to the formation
of space-charge region (or called depletion zone) across the p/n in­
terface to separate the photoexcited charge carriers in the p-type
absorbing layer, with photogenerated electrons being injected into
the n-type layer and photogenerated holes remaining in the p-type
layer; the spatially separated charge carriers are transported in the

4
H. Li, F. Li, Z. Shen et al.
Fig. 2. Schematic illustration of the typical device architectures for solar cells. (a) p-n junction architecture for crystalline silicon solar cells, (b) p-i-n architecture for conventional
PSCs, (c) single-layer and (d) p-i-n architectures for PPSCs. The green arrows in (c) and (d) represent the polarization origin from the ferroelectricity of perovskite materials.
different material phases toward their respective collection elec­
trodes.
Most of PSCs adopt the p-i-n architecture (or its variants: n-i-p,
mesoporous n-i-p and mesoporous p-i-n ones) (Fig. 2c), where the p,
i and n layers are usually referred to as p-type hole-transporting
layer (HTL), intrinsic perovskite layer, and n-type electron-trans­
porting layer (ETL), respectively [91–93]. Similar to the p-n junction
architecture, local electric fields in the p-i-n devices can be rendered
across the HTL/perovskite and ETL/perovskite interfaces as the result
of depletion zone formation [91,94]; the photoexcited charge carries
generated in the perovskite under illumination are spatially sepa­
rated and injected into the ETL and HTL layers, followed by the
collection at their respective electrodes.
However, the device architectures for PPSCs can be regarded as
the updated versions of p-n and p-i-n ones (Fig. 2b, d). The single-
layer architecture, with a photoferroelectric perovskite layer sand­
wiched between two electrodes, is very simple (Fig. 2b), the per­
ovskite layer therein acts as photoactive layer to harvest photons for
the generation of excited charge carriers [95,96]. Moreover, the p-i-n
structure is also often used in PPSCs, featuring an intrinsic photo­
ferroelectric perovskite layer sandwiched between n-type ETL and p-
type HTL layers (Fig. 2d) [97,98]. Obviously, PPSCs and conventional
PSCs have essentially the same device architectures. However, PPSCs
and conventional PSCs are actually distinct from each other in
photovoltaic process, that is, PPSCs convert photons into electricity
mainly under the combinational effects of the built-in electric field
Ebi and the ferroelectric polarization, while PSCs mainly works under
the Ebi contribution.
The physics mechanism for the photovoltaic devices of photo­
ferroelectric perovskite materials have been described previously,
including bulk photovoltaic effect, depolarization field driven pho­
tovoltaic effect, domain wall theory, Schottky barrier effect and so on
[37,39,99,100]. For simplicity, we here mainly introduce the polar­
ization field model based on Schottky barrier effect and depolar­
ization field driven photovoltaic effect. The work principle of PPSCs
5
Nano Today 37 (2021) 101062
is schematically illustrated in Fig. 3. In the pristine state, the per­
ovskite does not exhibit a macroscopic polarization intensity due to
the random orientation of ferroelectric domains, but there may exist
some local polarization (Fig. 3a); the main effects on PPSCs are from
the intrinsic built-in electric fields of Ebi-1 and Ebi-2 that locate ETL/
perovskite and perovskite/HTL interfaces, respectively (Fig. 3d).
When the domains are toward one direction after adding a polar­
ization voltage, the polarization charges distributed at the two se­
parated surfaces of the perovskite layer are not screened. As a result,
a depolarization field (Edp) is formed, which intrinsically origins
from the polarization but has opposite vector direction, and the
electrons and holes will move in the opposite direction under Edp, as
shown in Fig. 3b and c. If Edp and Ebi (Ebi−1 and Ebi−2) are in the same
direction, Edp is helpful to extend the depletion region and increase
Ebi, resulting in a larger Ebi to drive more electrons and holes to
transport to ETL and HTL, respectively. In this case, the photovoltaic
properties of PPSCs can get a promotion due the combinational ef­
fects of Edp and Ebi, as shown in Fig. 3e. On the contrary, as Edp and Ebi
(Ebi−1 and Ebi−2) are in the opposite directions after adding a reverse
polarization voltage, the Edp restrains the depletion region and re­
duces the Ebi, and consequently more electrons and holes cannot be
transported to ETL and HTL and recombine with each other to de­
teriorate the device performance (Fig. 3f). In short, the ferroelectric
polarization, including local and global polarization (global polar­
ization imposes a much larger effect), is the more crucial than the
build-in electric filed in PPSCs. However, photoferroelectric per­
ovskite material is such a complex system that the behaviors of
photons and electrons (holes) still remain many unknowns in PPSCs,
for which more complete and sound theories are being required.
Due to the ferroelectric polarization, the photovoltaic properties
of PPSCs are different from ones of traditional solar cells. From above
discussion, the current and voltage are regulated both by the po­
larization-electric field and the intrinsic built-in electric field (Ebi) in
the PPSCs [101,102]:
J = Jbi ± Jp (3)
H. Li, F. Li, Z. Shen et al. Nano Today 37 (2021) 101062

Fig. 3. Schematic illustration of the polarization changes and their corresponding band structures in the PPSCs during photovoltaic process.

V = Vbi ± Vp (4) and Jph when discussing the current property of solar cells.
Moreover, the Voc is the maximum voltage biased across the device
where Jbi and Vbi are the components due to the overall band
at which the opposite contributions from Jph and Jd balance each
bending potential, and Jp and Vp come from the switchable polar­
other, resulting no current flow (Ji = 0) through the device under
ization components.
illumination and Voc = V(Ji = 0).
Moreover, a theory model of bulk photovoltaic effect describes
Except for the additional effects from the ferroelectric polariza­
the photocurrent generation in PPSCs by using the rank three tensor
tion on the transport dynamics of photogenerated charge carriers,
βjik [37,99]:
the photovoltaic process in PSSCs proceeds in a way similar to the
J = Pj Pl* ijk I0 (5) conventional solar cells. Up to now, the performance of PPSCs is
normally characterized by the techniques used for the conventional
ijk solar cells; however, different from the conventional solar cells,
PCE = ×J
pv (6) PPSCs are pre-polarized prior to the characterizations.
From the measured J–V curve of solar cells, the photovoltaic
where Pn (Pj, Pl*) is the polarization of the medium in direction n, I0 parameters are obtained, including Voc, Jsc, fill factor (FF) and PCE.
is the intensity of the absorbed light, σpv is the photo-conductivity. The parameter PCE is defined as the ratio of the maximum power
output (Pout) to the incident light power (Pin), and is calculated from
Photovoltaic parameters of PPSCs the measured Voc, Jsc and FF as follows:

The J–V characterizations of solar cells is crucially important to Pout Voc × Jsc × FF
PCE = =
evaluate the photon-to-electricity conversion property of materials Pin Pi n (8)
system and the device. Normally, the J–V curve of a solar cell is
measured under AM 1.5 illumination with an incident intensity of Pin Vmpp × Jmpp
FF =
= 100 mW/cm2 at 25 °C. For conventional solar cells, the measured Voc × Jsc (9)
total current under illumination (Ji) consists of the photogenerated
current due to absorption of photons (Jph) and the dark current in­ where Vmpp and Jmpp are the voltage and the current density at the
jected from device electrodes (Jd) by a biased voltage (V), and both of maximum power point on the J–V curve. Moreover, the parasitic
Jph and Jd are in opposite signs. The relationship amongst those resistances in the solar cell, i.e., series resistance (Rs) and shunt re­
currents is as follows [103,104]: sistance (Rsh). The Rs is the resistance related to the materials con­
ductivity and the interfacial contacts, while the Rsh is resulted from
Ji (V ) = Jph (V ) + Jd (V ) (7) for the leakage current due to the interfacial charge recombination
The short-circuit current (Jsc) is the maximum photocurrent of a and the structural defects in materials. They are expressed as[105]:
solar cell under short-circuit condition, that is, Jsc = Ji(V = 0) ≈ Jph(V =
1 dI
0) and actually measures the collected number of charge carriers by Rs =
dV I=0 (10)
electrodes. No consideration is made to deliberately distinguish Jsc

6
H. Li, F. Li, Z. Shen et al. Nano Today 37 (2021) 101062

Fig. 4. (a) Crystal structure and ferroelectric polarization direction of BFO. Reproduced with permission [112]. Copyright 2020, Taylor and Francis. (b) Hysteresis loop of BFO, (c)
The photocurrent-voltage curves of Pt/BFO/FTO at different polarization states (the inset shows its JSC and VOC). Reproduced with permission [141]. Copyright 2017, ScienceDirect.
Four typical structures of BFO SCs: (d) doping BFO. Reproduced with permission [142]. Copyright 2015, AIP Publishing. (e) plasma-enhance. Reproduced with permission [143].
Copyright 2017, Royal Society of Chemistry. (f) added charge transporting layer. Reproduced with permission [144]. Copyright 2017, American Chemical Society (g) superlattice
structure. Reproduced with permission [145]. Copyright 2015, AIP Publishing.

1 dI Recent advances in PPSCs

Rsh =
dV V =0 (11)
Oxide PPSCs
On the other hand, the external quantum efficiency (EQE) is an­
other important parameter to characterization the photocurrent Oxide perovskites have usually two or more ferroic orders in­
generation related to the materials structure and the device archi­ cluding ferroelectricity, ferromagnetism, ferroelasticity and ferro­
tecture in solar cells. EQE is defined as the ratio of the number of toroidicity. Most of oxide perovskites with a wide bandgap of > 3 eV
output electrons to the one of incident photons at a specified wa­ (Table 1) are insulators, and they, for example, BaTiO3 (BTO)
velength. The factors affecting EQE includes the photon absorption [106,107], PZT [108,109], only exhibit a poor photovoltaic effect
efficiency (ηa), exciton diffusion efficiency (ηdiff), exciton dissociation under the illumination of photon in UV region. Nowadays, the oxide
efficiency (ηtc), electron transporting efficiency (ηtr), electron col­ perovskites with a bandgap of < 3 eV, such as BiFeO3 [51], BiMnO3
lection efficiency at electrode (ηcc) in solar cells. [51] and Bi2FeCrO6 [66], have attracted lots of attention for the de­
velopment of stable and new PPSCs; in particular, BiFeO3-based
EQE = a × diff × tc × tr × cc (12) materials have been extensively investigated.
BiFeO3 (BFO) is a single-phase ABO3-type perovskite compound
EQE is also described as incident photon-to-current efficiency
(t ≈ 0.88) and was first synthesized in the late 1950s [110]. BFO ex­
(IPCE). EQE or IPCE is simply defined by the following equation
hibits a rhombohedrally R3c space group (R phase) with the lattice
under a monochromatic light illumination:
parameter of arh = 3.965 Å and αrh = 89.3–89.4°, and a ferroelectric
1240 Jsc polarization along [111]pseudocubic at room temperature (Fig. 4a)
EQE( ) = IPCE( ) = [111,112]. At a high temperature (~ 1000 K), BFO occurs the first-
P in (13)
order phase transition from R3c to GdFeO3-like Pbnm phase and
2 probable orthorhombic γ phase [113–116]. The BFO unit cell is also
where λ (nm) is the wavelength of incident photon, Jsc (µA/cm ) is
the photocurrent of device, and Pin (W/m2) is the intensity of in­ described by a hexagonal structure with the lattice parameter of ahex
cident light. = 3.58 Å and αhex = 13.90°, and a ferroelectric polarization direction

7
H. Li, F. Li, Z. Shen et al. Nano Today 37 (2021) 101062

Table 2
Summary of the performances of BFO-based PPSCs. ITO: (Sn:In2O3), FTO: (SnO2:F), STO: SrTiO3, LAO: LaAlO3, LSMO: LaSrMnO3, BTO: BaTiO3, CRO: CaRuO3, BCO: BiCrO3, NPs:
nanorods, NPs: nanoparticles, (PEDOT:PSS): polystyrenesulfonate. 1: substitution for Bi or Fe site, 2: plasma enhance, 3: added charge transporting layer, 4: multilayered su­
perstrate structure.

Structure VOC (V) JSC (mA/cm2) Efficiency (%) FF (%) Light Intensity (mW cm−2) Light wavelength (nm) Ref.

Pt/BFO/Au 1.3 0.105 0.0242 / 100 Sun light [165]

ZnO:Al/BLaFTaO/Pt 0.3 1.35 / / 100 Visible [142] 1
FTO/BFO/Au 0.35 3 × 10−4 3 × 10−4 / 100 Sun light [166]
FTO/BCaFO/Au 0.5 3 0.22 0.24
FTO/BCaFTiO/Au 0.3 3 0.12 0.4
ITO/BFO/Au 0.58 5 0.005–0.16 / 10 405 [167]
ITO/BSmFO/Au 0.7 94 × 10−3 0.25–3
ITO/BFO/Au 0.05 4 × 10−3 / 18 160 405 [168]
ITO/BFMnO/Au 0.1 11 × 10−3 / 22
ITO/BCeFO/Au 0.15 28 × 10−3 / 29
ITO/BCeFMnO/Au 0.25 36 × 10−3 / 34
STO/BFO 0.6 1.3 × 10−3 / / 2500 515 [150]
STO/BMnFO 3.1 15 × 10−3 / /
ITO/BFO/Pt 0.45 2.56 / 52.92 100 Sun light [169] 1&2
ITO/BFCrO/Pt 0.47 3.73 / 60.29
ITO/rGO/Au NRs/BFCrO/Pt 0.63 2.56 / 73.4
FTO/BFO/ITO 3.6 × 10−3 / / 100 Sun light [143]
FTO/BLaFO/ITO 0.2 5.3 × 10−3 / /
FTO/Au NPs/BLaFO/ITO 0.3 18.5 × 10−3 / /
FTO/p-TiO2/BFO/NiO/Au 0.28 0.13 9.5 × 10−3 25 100 Sun light [170] 3
FTO/m-TiO2/BFO/NiO/Au 0.67 0.51 0.19 55
FTO/BFO/Pt 0.5 0.02 / / 30 330–780 [141]
FTO/TiO2/BFO/BTO/Pt 0.73 0.17 / /
LAO/LSMO/BFO/Cr/Au 0.09 1.05 / / 200 365 [144]
ITO/BFO/Pt 0.37 1.6 × 10−3 0.005 / 22.3 435 [4]
ITO/ZnO/BFO/Pt 0.225 0.34 0.33 /
FTO/BFO/PEDOT:PSS/Au 0.17 16.8 × 10−3 0.00064 / 100 Sun light [171]
FTO/BFO/ZnO NR/PEDOT:PSS/Au 0.32 1.08 0.086 25
Pt/Ti/BFO/Au 0.33 0.13 / / 160 405 [145] 4
Pt/Ti/BTO/BFO/BTO/BFO/BTO/Au 1.25 0.32 0.067 /
Pt/Ti/BTO/BFO/BTO/BFO/Au 1.43 12.65 × 10−3 / / 160 405 [172]
LAO/CRO/BCO/BFO/BCO/BFO/ BCO/BFO/ITO 1.2 13 × 10−3 0.01 31 100 Sun light [173]

along [001]hexagonal (Fig. 4a) [112]. However, the BFO thin films
grown on different substrates show different crystal structures due
to the varied strains between the substrate and crystals, e.g.
monoclinic [117,118], tetragonal or tetragonal-like [119–121], rhom­
bohedral [122–124], orthorhombic [125,126] and triclinic [127]
structures. As the result of the off-center structural distortions in cell
lattice, BFO thin films shows an enhanced remnant polarization.
After the finding of spontaneous polarization (Ps = 3.5 μC/cm2) for
BFO in 1970 [128], the BFO-based materials with large spontaneous
polarization values have been reported [123,129–137]. The polar­
ization (Pr) has reached 100 μC/cm2 in R3c-structured BFO [129],
while the Pr up to ~ 230 μC/cm2 was found in super-tetragonal BFO
[132,135]. In the BFO-based materials, the origin of the polarization
is deemed to be the large ionic Bi displacement induced by stereo­
chemically active 6s lone pairs [138]. Some factors, such as the
oxygen vacancy defects (Eq. (14)) and the valence change from Fe3+
to Fe2+ (Eq. (15)), can generate the high leakage current and dete­
riorate the ferroelectricity of BFO [139]. The ferroelectric properties
of BFO-based materials can be improved by the substitution for Bi or
Fe site, and/or the addition of other ABO3 compounds [140].
2Bi3 + + 3O2 Bi2 O3 + 2VBi3 + 3VO2+
2Fe3 + + O2 2Fe2 + + 0.5O2 + VO2+
It was reported that BFO has a direct bandgap of 2.01–3.12 eV [146].
Moreover, the presence of an indirect bandgap of 0.4–1.0 eV in BFO has
also been confirmed, of which the absorption is very weak and often
ignored [22,147,148]. Therefore, the BFO absorption of sunlight is nor­
mally in the blue region of visible range that occupies about 25% energy
of AM 1.5G solar spectrum [112]. In order to improve the absorbance of
BFO, an method is the substitution of Mn and/or Cr for Fe [149,150]. It is
worth noting that the optical bandgap of BFO is susceptible to tem­
perature and pressure. For example, the BFO has an insulator-metal (I-
M) transition driven by either temperature or pressure, and its optical
bandgap may disappear abruptly as temperature or pressure increases
[151,152]. Although the BFO after the I-M transition is not strictly a
conventional metal with a half-filled band, its physical properties will
also change as a consequence, e.g., magnetism disappears, resistivity
reduces significantly, and reflectivity increases abruptly [153].
BFO materials can be prepared into powder and film forms, of
which both may consist of bulk grains or nanocrystals (e.g., spherical
nanoparticles, nanocubes, nanotubes, nanowires, nanodots, na­
nosheet, nanoplate and nanoislands) [140]. Normally, BFO thin films
are used in PPSCs, because a high-quality thin film is easily fabri­
cated by different deposition techniques, including pulsed laser de­
position (PLD) [154,155], chemical vapor deposition (CVD) [156,157],
chemical both deposition (CBD) [158,159] and sol-gel process
[160,161]. The simplest way to prepare BFO-based PPSCs is to
sandwich the BFO films between two electrodes, and the photo­
voltaic characteristics of the PPSCs can be adjusted by polarization
voltages [141,144,162–164]. Zhang et al. found that the Voc and Jsc of
Pt/BFO/FTO device increased to 0.5 V and 21.01 μA/cm2 at a negative
(14) polarization state from 0.39 V and 7.88 μA/cm2 at the initial state
(Fig. 4b and c) [141]. It is no doubt that the separation of e-h pairs in
(15)
PPSCs can be enhanced by ferroelectric polarization. On the other
hand, the photovoltaic characteristics of PPSCs also can be improved
by changing the material and/or device structure.
Table 2 summarizes the photovoltaic performances of BFO-based
materials reported recently. Obviously, there are mainly four
methods to enhance the photovoltaic performance of BFO-based
PPSCs, for which some typical structures used are displayed in
Fig. 4d–g. First, a popular method is ion substitution, such as, to

8
H. Li, F. Li, Z. Shen et al. Nano Today 37 (2021) 101062

substitute Mn, Cr, Ca, Ta, Ti for Fe, and/or Sm, Ce, La for Bi. As pointed
out above, the ion substitution will increase the photovoltaic per­
formance by reducing the bandgap and increase the absorbance of
BFO material. The presence of mid gap states (e.g., defects) will bring
forth a serious charge recombination in the solar cells. In the co-
substitution of Ca and Ti for Fe, the mid gap states is greatly reduced
or even eliminated, resulting in the device photocurrent enhanced
by four orders [166]. Zhang et al. reported that La3+ doping can re­
duce the bandgap of BFO, and the red-shift of absorption band can
enhance the absorption and utilization of visible light, which even­
tually improve the photoelectric conversion efficiency [174]. Second,
the plasmon effect of metal nanostructures can help to increase the
photovoltaic performance of solar cells. Nanometals, especially Au
nanomaterials, exhibit a strong absorption in the visible and near-
infrared range of solar spectrum due to their local surface plasmon
resonance (LSPR) effect. Thus, Au nanomaterials, such as Au na­
norods [169], Au spherical nanoparticles [143], have been used to
improve the performance of BFO-based solar cells. Not only BFO, but
other systems can also apply the plasmon effect to improve the
device performance of organic dye-sensitized and PbS solar cells for
example [175,176]. Third, to use the interfacial layers for selective
extraction of charge carriers for improving the collection efficiency
of photogenerated charge carriers. BFO has a high resistivity ex­
ceeding 1010 Ω cm, which deteriorates the transport and collection of
photogenerated char carriers. Fan et al. inserted a ZnO interface
between electrode and BFO film to prepare ITO/ZnO/BFO/Pt solar
cell, and found that ZnO layer can improve Jsc and PCE to 0.35 mA/
cm2 and 0.33% from 1.6 × 10−3 mA/cm2 and 0.005% of the counterpart
device without ZnO interfacial layer [4]. Wu et al. combined the
mesostructured carrier transporters TiO2 and NiO with BFO, and
demonstrated that the transporters layers could efficiently extract
the photocarriers generated in BFO leading to a better PV perfor­
mance than conventional devices [170]. Finally, multilayered su­
perstrate structure can overcome the deficiency of BFO single layer
to enhance the polarization in PPSCs for an increased photovoltaic
performance. Multilayered superstrate structure is usually realized
by multiple stacking BFO and other ABO3 layers sequentially on the
top of each other. Sharma et al. designed the Pt/Ti/BTO/ BFO/BTO/
BFO/BTO/Au solar cell with a multilayered structure of BTO by PLD
on platinum coated silicon substrate, and they found that the mul­
tilayered device has the Voc of 1.25 V and Jsc of 0.32 mA/cm2, much
higher than those of Voc = 0.33 V and Jsc = 0.13 mA/cm2 for the
counterpart device with only a single BFO layer [145]. A similar study
can be found in the devices of a multilayered structure of BFO and
BCO [173].
The recent studies of PPSCs based on other oxide perovskite
materials are summarized in Table 3. Among these materials,
Bi2FeCrO6 (BFCO) is the most promising candidate material. Similar
to BFO, BFCO has a rhombohedral structure with lattice parameter of
arh = 5.47 Å and αrh = 60.09°, and the ferroelectricity is also due to the
6s2 lone pair on Bi3+ ions, where atoms move off center to form the
electric dipole moment [177–179]. Moreover, metastable BFCO is
expected to adopt a double perovskite structure with a random oc­
cupancy of Fe3+ and Cr3+ on the B-site due to similar ionic radii of
Fe3+ (r = 0.654 Å) and Cr3+ (r = 0.615 Å), which reduced the symmetry
of the space group to R3 as compared with BFO [178,179]. BFCO was
predicted by Baettig and Spaldin using first-principles density
functional theory to have a large ferroelectric polarization of Pr ~
80 μC/cm2 [180]. Since then, experimental measurements revealed
the polarization up to Pr ~ 60 μC/cm2 for BFCO and also confirmed its
photovoltaic effect [181–185].
Until now, the highest PCE of BFCO-based PPSCs was achieved by
Nechache et al. through engineering the cationic ordering for the
case of BFCO, controlling the number of BFCO layer and changing the
polarization direction, as shown in Fig. 5 [66]. In their BFCO-based
PPSCs, the single layer of BFOC (S1, S2 and S3) is prepared by tai­
loring parameters of cationic ordering (Fig. 5b and c), the multilayer
is obtained by controlling the deposition rate (from 2 Hz to 8 Hz and
finally to 14 Hz) and grown temperatures (M1–580 °C and
M2–720 °C), the Schottky barriers and photovoltaic properties are
showing a good tunability (Fig. 5d–i). Therein, energy band structure
is adjusted by the ferroelectricity of BFCO during photovoltaic pro­
cess (Fig. 5f and g). Especially, J–V curves varies with the polarization
voltage, and high Voc and Jsc are obtained with an appropriate po­
larization voltage. As a result, the highest PCE is about 8.1% in M1
device after a +25 V polarization voltage. This is a further demon­
stration of the enormous potential to develop high property oxide
PPSCs. Very interestingly, the bandgap of BFCO is easily adjusted in
the range of 0.78–2.4 eV by controlling the molar ratio of Fe/Cr
[66,196–198].
Although lots of efforts have been attempted to develop oxide
PPSCs, the PCEs of these devices are still too low for practical

Table 3
Summary of performances of non-BFO-based PPSCs. NSTO: Nb-doped SrTiO3, SRO: SrRuO3, spiro-OMeTAD: 2,2′,7,7′-tetrakis (N, N′-di-p-methoxyphenylamine)-9,9′-spirobi­
fluorene.

Structure Voc (V) Jsc (mA/cm2) Efficiency (%) FF (%) Light Intensity (mW cm−2) Light wavelength (nm) Ref.
−3
FTO/(Pb,La)(Zr,Ti)O3/Au 0.73 2.11 × 10 / / / white-light [186]
ITO/Pb(Zr,Ti)O3/Au 0.18 3.35 × 10−3 / / / 200–400 [187]
ITO/Pb(Zr,Ti)O3/ZnO/Au 0.68 42.41 × 10−3 / /
ITO/PbTiO3/pn-Si/Ag 0.25 0.22 4.2 / 100 Sun light [188]
ITO/PbTiO3/Si/Ag 0.16 2.15 × 10−3 0.2 /
Ag/n-a-Si/Pb(Zr,Ti)O3/ITO 1.36 3.07 1.25 / 100 Sun light [108]
Ag/p-a-Si/Pb(Zr,Ti)O3/ITO 1.1 1.05 0.11 /
ITO/TiO2/(Na,Bi)FeO3/spiro-OMeTAD/Au 0.43 72.1 × 10−3 0.0075 24 100 Sun light [97]
Pt/Bi(Ti,Fe)O3/Au 0.58 0.5 × 10−3 / / / 300–1100 [189]
Pt/(Bi,Ho)(Ti,Fe)O3/Au 0.25 6 × 10−3 / /
ITO/YbFeO3/Pt/MgO 0.52 21 × 10−3 0.00312 28.6 100 Sun light [190]
ITO/YbFeO3/Pt/ZnO 0.46 10 × 10−3 0.00121 26.3
Pt/LuMnO3/ITO 0.71 0.52 0.11 30 100 Sun light [191]
Pt/YMnO3/ITO 0.66 0.55 0.11 30
Pt/(K,Na)NbO3/Au 0.72 3.31 × 10−3 / / / 300–1100 [192]
Pt/(K,Na)NbO3/BiMnO3/Au 1.3 25.4 × 10−3 / /
ITO/(Ba,Ca)TiO3-Ba(Zr,Ti)O3/ZnO/Pt 0.03 5.31 / / 100 Sun light [193]
ITO/ZnO/(Ba,Ca)TiO3-Ba(Zr,Ti)O3/Pt 2.5 × 10−3 3.4 × 10−3 / /
ITO/ZnO/(Ba,Ca)TiO3-Ba(Zr,Ti)O3/ZnO/Pt 0.11 52 × 10−3 / /
ITO/BFCO/NSTO 0.42 3.3 0.8 56 100 Sun light [194]
ITO/NiO/BFCO/NSTO 0.53 7.97 2 48
SRO/BFCO//ITO 0.52 13.8 2.65 38 100 Sun light [195]
STO/SRO/BFCO/ITO 0.84 20.6 8.1 47 100 Sun light [66]

9
H. Li, F. Li, Z. Shen et al. Nano Today 37 (2021) 101062

Fig. 5. (a) Schematic illustration of BFCO device. (b) Bulk phase diagram as a function of differences in formal valences (FV) and ionic radii (ri). (c) Schematic distribution diagram
of ordered domains with D size in disordered region of BFCO. J–V characteristics of BFCO devices under AM 1.5G illumination: (d) BFCO single layer and (e) BFCO multilayer.
Schematic of simplified energy band diagrams for BFCO SCs adjusting by the ferroelectric polarization (f) BFCO single layer and (g) BFCO multilayer. (e) Photovoltaic performances
of BFCO SCs. Reproduced with permission [66]. Copyright 2015, Nature.

application. Thus, “How to realize the oxide PPSCs with an efficiency
comparable to Si solar cells?” is eagerly waiting for answer. The wide
bandgap and poor conductivity are the two main efficiency-limiting
factors. It is urgent to overcome these deficiencies by optimizing the
function of these materials and the device structures. Of course, for
achieving efficient oxide PPSCs, it is necessary to combine the
fruitful breakthroughs in the fields of thin film technology, ferro­
electric community and photovoltaic engineering [22,112].
Halide PPSCs
Most of halide perovskites are good semiconductors and they are
of more interests in preparing low-cost solar cells than oxide per­
ovskites. Recently, many halide perovskites have been demonstrated
to have ferroelectric properties, offering the application of them to
halide PPSCs.
Hybrid halide photoferroelectric perovskites
In ABX3 (B = Sn, Pt, etc.; X = Cl, I, Br, etc.) halide perovskites, A-site
is generally occupied by organic functional groups of CH3NH3 (MA)
and CH(NH2)2 (FA) for example. Another molecular formula of (Aˊ)m
(A)nBnX3n+1 is also used to describe halide perovskites, in which Aˊ is
bulky organic cation that connects with inorganic (A)nBnX3n+1 two-
dimensional (2D) sheets [42,199,200]. The limit cases with n = ∞ to
three-dimensional (3D) perovskites, the ones with n = 1 represent
2D perovskites, and those with 1 < n < 5 is often known as quasi-2D
perovskites, as shown in Fig. 6a. Since the presence of organic ca­
tions imposes the properties of organic materials on the halide
perovskites, one normally refers to those perovskites with organic
groups at A sites as hybrid halide perovskites (i.e., hybrid ABX3). A
great advantage of hybrid halide perovskites is their versatile film-
processability at a low temperature. One-step and two-step solu­
tion-processing techniques are commonly use to prepare high-
quality hybrid halide perovskite films. The preparation processes of
the solution-processing methods and the morphology of resulting
films are depicted in Fig. 6b and c [201–204].
Hybrid halide perovskites are often direct-bandgap semi­
conductors with a large absorption coefficient up to ~ 105 cm−1 in the
UV–visible range [205]. The bandgap of these perovskites can be
tuned by chemical substitution in molecular formula. Similar to
oxide perovskites, three strategies are widely used to tune the op­
tical bandgap and charge transport properties of hybrid ABX3 as
shown in Table 1: organic cation substitution (A-site), metal cation
substitution (B-site), and anion substitution (X-site). In general, the

10
H. Li, F. Li, Z. Shen et al.
Fig. 6. (a) Schematic comparing 2D and 3D halide perovskite structures. Reproduced with permission [42]. Copyright 2020, Royal Society of Chemistry. (b) One-step spin-coating
procedure for CH3NH3PbI3 and their topographic characteristics. Reproduced with permission [204]. Copyright 2015, American Chemical Society. (c) Two-step spin-coating
procedure for CH3NH3PbI3 and their topographic characteristics. Reproduced with permission [203]. Copyright 2014, Nature.
bandgap of hybrid ABX3 decreases with increased the radius of the
anion (Cl− < Br− < I−), which actually maps a direction to fabricate
perovskites with narrow bandgap. Moreover, it is also an effective
path to tune the bandgap of hybrid ABX3 by using mixed ions in one
perovskite. In 2014, Pellet et al. [206] reported the first mixed or­
ganic-organic cation perovskite MAxFA1−xPbI3 (0 ≤ x ≤ 1), where a
significant red shift from 776 nm (x = 1) to 803 nm (x = 0) was ob­
served in the absorption spectrum; they also found that the opti­
mized solar cell was obtained at x = 0.6, resulting in the Jsc, Voc, FF
and PCE of 21.2 mA/cm−2, 1.003 V, 70% and 14.9%, respectively.
Eperon et al. further found that the bandgap of MAxFA1-xPbI3 is
tunable between 1.57 eV and 1.48 eV [207]. Similarly, using mixed
ions in B- or C-site can also tune the bandgap and photovoltaic
properties of hybrid ABX3 [208–210]. For example, Ju et al. have
successfully obtained a series of centimeter-size MAPbxSn1−xBr3
single crystals, and the optical bandgaps of them were greatly de­
creased by formulating Sn2+ content [208].
However, the study on the ferroelectricity effects on the perfor­
mance of hybrid ABX3-based solar cell is not going well, perhaps two
existing controversial issues. One debate is whether hybrid ABX3
(e.g. MAPbI3) is ferroelectric. Some results demonstrated that
MAPbI3 is not ferroelectric [211–213], but others supported a con­
trary opinion that MAPbI3 should be ferroelectric [27,77,214–220].
Theoretically, Stroppa et al. used density functional theory in com­
bination symmetry mode analysis to study the ferroelectricity of
MAPbI3, and estimated that its polarization was about 4.42 μC/cm2 at
180 K, but only a few μC/cm2 at room temperature [214]. On the basis
of time-domain density functional theory and nonadiabatic mole­
cular dynamics, Qiao et al. found the long-range charge separation
and the slow charge recombination due to a ferroelectric reason in
MAPbI3-based solar cells [215]. The P–E hysteresis loops of hybrid
ABX3 have also been experimentally observed. Sewvandi et al. ob­
served the P–E hysteresis loops of MAPbI3−xClx that has the
11
Nano Today 37 (2021) 101062
polarization Pr of about 1.2 μC/cm2 [218]. Moreover, the ferroelectric
domains in MAPbI3(Cl) have been clearly imaged by PFM
[27,77,216,221]. Therefore, the accumulated evidences suggest that
MAPbI3 is indeed ferroelectric in nature. Another debate focuses on
whether the J–V hysteresis, also simply called current hysteresis, of
hybrid ABX3-based solar cells originates from the ferroelectric
characteristics. The J–V hysteresis is the current mismatch between
the forward scan (voltage biased from 0 V to Voc) and reverse scan
(voltage biased from Voc to 0 V) during J–V measurements [222]. One
opinion is that the hysteresis is attributed to the intrinsic ferro­
electric properties of hybrid ABX3. Cao et al. recorded the J–V hys­
teresis by applying a series of polarization voltages onto the MAPbI3-
based solar cells, and found that the polarization and depolarization
of electric dipoles of CH3NH3+ under the external electric field were
the origin of the hysteresis [223]. The ferroelectric mechanism of the
J–V hysteresis was also supported by other groups [224–230]. On the
other hand, however, the J–V hysteresis was believed to follow other
mechanisms, including ion migration [231–234], interface charge
accumulation [235–237], charge trapping and detrapping [238,239],
and even interfacial effect of compact layer [240]. Interestingly, the
J–V hysteresis can be affected by test parameters, such as scan rate
[241], scan range [226,242], and the delay time after each voltage
step before the measurement [243]. Kang and Park have published a
review article that discusses the origins and the removal methods of
the J–V hysteresis [222]; according to their opinion, the J–V hyster­
esis mainly depends on the composition of hybrid ABX3, and the ion
migration and charge recombination in the vicinity of interfaces play
a critical role in generating hysteresis, but the interfacial and bulk
engineering to passivate defects is the most promising approach to
eliminate the J–V hysteresis. In short, it is still an issue to clarify the
predominant factor leading to the presence of the J–V hysteresis.
The MAPbI3 crystal exhibits a tetragonal symmetry (space group
I4/mcm, Z = 4) at room temperature with the lattice parameter of atet
H. Li, F. Li, Z. Shen et al. Nano Today 37 (2021) 101062

Fig. 7. (a)–(c) Schematics of electronic band structure under different polarization conditions, (d) SEM image and (e) J–V plots for MAPbI3(Cl) based PPSCs. Reproduced with
permission [101]. Copyright 2015, Royal Society of Chemistry. (f) Difference (Δ) of Jsc and PCE with various polarization voltages in MAPbI3 based PPSCs. Reproduced with
permission [223]. Copyright 2016, American Chemical Society. (h) Device configuration of CH3NH3PbI3-based PPSCs with PVDF-based ferroelectric polymers, (i)-(l) J–V curves in
PVDF-based ferroelectric polymers doped perovskite PPSCs. Reproduced with permission [251]. Copyright 2019, Wiley-VCH.

= 8.8 Å and ctet = 12.685 Å, and change into an orthorhombic struc­
ture below 162.2 K and a cubic one above 327.4 K [244]. Generally,
the ferroelectricity of MAPbI3 originates from the three processes
taking place in MAPbI3 crystal [245–247]: ionic polarization by the
off-center shift of Pb in the PbI6 octahedral; ionic polarization by the
displacement of the positive charge center (MA+) from the negative
charge center (PbI3−); polarization from oriented MA+ dipoles. In
particular, the orientation of organic species leads to the charged
domain walls to reduce the bandgap of MAPbI3 material [248]. The
bandgap structure also is susceptible to direction of polarization,
Chen et al. [101] studied the polarization effects on the performance
of FTO/cp-TiO2/MAPbI3−xClx/Au solar cells at ± 2 V polarization vol­
tage (Fig. 7a–e). They found that, the positive polarization voltage at
2 V leads to a larger width of depletion region (W1+ and W2+) in
MAPbI3−xClx layer and enlarges the band bendings at both cp-TiO2/
MAPbI3-xClx and MAPbI3-xClx/Au interfaces, resulting in an increased
Voc due to the additional band bending and a higher Jsc as the result
of improved charge separation (Fig. 7b, e); in contrast, the negative
polarization voltage at −2 V produces the reduced band bendings at
the interfaces, with deteriorated Voc and Jsc in the device (Fig. 7c, e).
Moreover, another group has reported that a larger polarization
voltage is easier to get the better photovoltaic performances to a
certain extent (Fig. 7f) [223]. It is worth noting that light illumina­
tion can also induce ferroelectric switching in perovskite MAPbI3
[249,250]. Wang et al. observed that the spontaneous polarization
was switched by light when without an electric field because of the
ionic motions in combination with a photoelectric field [249].
The photovoltaic properties of some MAPbI3-based solar cells are
listed in Table 4. The PCEs of those halide perovskites are about 20%,
much greater than those of BFO or BFCO, inferring the application
potentials for PPSCs. Other ferroelectric materials were also used in
the MAPbI3-based PPSCs to enhance the device performances, in­
cluding oxide ferroelectric perovskites and ferroelectric polymers
[251,267–269]. Poly(vinylidene fluoride) (PVDF)-based ferroelectric

12
H. Li, F. Li, Z. Shen et al. Nano Today 37 (2021) 101062

Table 4
Summary of performances of MAPbI3-based perovskites. Ace: acetamidinium, IMS: 4-(1H-imidazol-3-ium-3-yl)butane-1-sulfonate, F-PDI: N, N′-bis-(1, 1, 1, 2, 2, 3, 3, 4, 4-
nonafluorododecan-6-yl)-perylenediimide, PCBB-3N-3I:, PCBM: phenyl-C61-butyric acid methyl ester, BCP: bathocuproine, PTAA: poly(triarylamine), PSCT-N: thiophene-based
polyelectrolyte, E2CA: ethyl 2-cyanoacrylate, π-PFE: π-extended phosphoniumfluorene. The tests were under standard AM 1.5G illumination.

Structure VOC (V) JSC (mA/cm2) Efficiency (%) FF (%) Ref.

ITO/SnO2/MAPbI3/PTAA/Ag 1.13 22.77 20.25 77 [252]

ITO/PEDOT:PSS/MAPbI3/PCBM/Al 1.04 22.63 18.9 80 [253]
FTO/TiO2/MAPbI3/spiro-OMeTAD/Au 1.08 22.7 19.51 80 [254]
FTO/SnO2/MAPbI3/spiro-OMeTAD/Ag 1.13 22.02 20.18 81 [255]
FTO/SnOx-Cl/MAPbI3/spiro-OMeTAD/Ag 1.19 22.52 20.32 76 [256]
ITO/NiOx/MAPbI3 + F-PDI/PCBM/BCP/Ag 1.02 22.05 18.28 81 [257]
ITO/TiO2/MAPbI3 + IMS/spiro-OMeTAD/Au 1.14 22.08 20.84 83 [258]
ITO/PTAA/MAPbI3/PCBB-3N-3I/PCBM/Al 1.11 23.46 21.1 81 [259]
ITO/ PEDOT:PSS/MAPbI3/PCBM/π-PFE/Ag 1.04 22.11 18.46 80 [260]
FTO/TiO2/MAPbI3 + EATZ/spiro-OMeTAD/Au 1.1 23.39 20.03 78 [261]
ITO/SnO2/AcexMA1−xPbI3/spiro-OMeTAD/Au 1.13 22.67 20.3 75 [262]
FTO/TiO2/FA0.15MA0.85PbI3/spiro-OMeTAD/Au 1.12 24.23 21.88 81 [263]
ITO/PSCT-N/MAPbI3-E2CA/PCBM/C60/BCP/Cu 1.12 23.02 21.03 81 [264]
FTO/SnO2/Al2O3/Cu:NiO/MAPbI3−xClx-Cu:NiO/Spiro-OMeTAD/Au 1.02 23.11 18.56 78 [265]
ITO/NiOx/MAPbBr3/MAPbIBr2/MAPbI2Br/MAPbI3/ICBA/PCBM/Al 5.29 5.35 21.33 75 [266]

polymers are the suitable materials due to their superior solution-
processed film-formation property and good compatibility with
MAPbI3 precursors in solutions. Zhang et al. [251] developed a
simple and effective strategy to improve the device performances of
MAPbI3-based PPSCs by using PVDF-based polymers in the forms of
dopant (mixed with MAPbI3), interlayer (between MAPbI3 and
charge transporting layer), and integrated (both dopant and inter­
layer) (Fig. 7h–l). They first used the ferroelectricity of MAPbI3 to
improve PCE from 17.21% to 19.18%, and further up to 21.38% (Voc =
1.14 V, Jsc = 24.10 mA/cm2, FF = 78%) after the formation of double-
ferroelectricity in the corporation of poly(vinylidene fluoride-tri­
fluoroethylene) [P(VDF-TrFE)]. Jia et al. also used P(VDF-TrFE) doped
MAPbI3 to obtain efficient PPSCs [267]. Due to the different pre­
paration methods, oxide ferroelectric perovskites are generally ap­
plied in the form of interlayer to the MAPbI3-based PPSCs. Wang
et al. reported the PPSCs with a structure of FTO/PbTiO3/MAPbI3/
spiro-OMeTAD/Au, in which the ferroelectric perovskite PbTiO3 layer
acted as an electron transporting interlayer, and the PCE was in­
creased by nearly 30% in comparison to the counterpart device
without the PbTiO3 layer [269].
Inorganic halide photoferroelectric perovskites
Although hybrid halide perovskites (i.e., hybrid ABX3) exhibit
superior photovoltaic performances, poor stability is still challenge
to their practical applications. The instability of hybrid halide ABX3 is
normally caused by the volatile and hygroscopic nature of organic
components when exposed to oxygen, moisture, heat and illumi­
nation. In contrast, inorganic halide perovskites (inorganic ABX3)
have a high stability thanks to the replacement of organic cations by
inorganic cations (e.g. Cs+) (i.e., A = Cs+). Similar to hybrid halide
perovskites, the bandgap of the inorganic halide perovskites also
shows a lower shift trend along the changing a map of Cl → Br → I
(Table 1). Compared to Pb-based perovskites (B = Pb2+), Sn-based
perovskites (B = Sn2+) have a smaller bandgap and are of great in­
terests in preparing environmental-friendly PSCs without toxic lead.
Moreover, inorganic halide perovskites are also easily solution-pro­
cessible, similar to hybrid ones [270–272].
The recent performances of some efficient solar cells based on
inorganic ABX3 are summarized in Table 5. Obviously, Pb-based in­
organic ABX3 materials, especially CsPbI3, dominated the previous
studies of PCE up to 18%, which also infers the application potentials
for PPSCs similar to the organic one. CsPbI3 has a relatively low
bandgap of 1.7 eV close to MAPbI3 (Table 1). However, CsPbI3 is non-
perovskite orthorhombic structure (Pnma) due to the lower toler­
ance factor (t = 0.807) at the room temperature [1]. When heated to
above 360 °C, CsPbI3 is transformed into cubic phase (Pm3m); upon
cooling, it converts to tetragonal phase (P4/mbm) at 260 °C, and to
perovskite orthorhombic phase (Pbnm) at 175 °C that easily con­
verted to non-perovskite structure again after few days [288,289].
The ferroelectricity of inorganic ABX3 perovskites is mainly theore­
tically investigated on the basis of first-principle calculations
[290–293]. Sadok et al. predicted that the inorganic ABX3 with A = Cs
and Rb have spontaneous polarization to a certain extent, and ob­
tained the calculated spontaneous polarization for CsPbI3 (~ 5.36 μC/
cm2), CsPbBr3 (Ps ~ 3.72 μC/cm2), CsPbCl3 (~ 3.11 μC/cm2), CsSnCl3 (~
−1.11 μC/cm2) and RbPbI3 (~ −12.25 μC/cm2) [290]. Song et al. theo­
retically showed that the polarization (Ps) of CsSnI3 is up to several
μC/cm2 [293]. However, there are only a few articles that in­
vestigated experimentally the ferroelectricity of inorganic ABX3
perovskites [294–296]. Li et al. observed that CsPbBr3 displayed Ps
values of 0.25 μC/cm2 and 0.018 μC/cm2 at 77 K and 293 K, respec­
tively [296]. However, it still requires further studies for the fer­
roelectricity of inorganic ABX3 perovskites both theoretically and
experimentally.
Moreover, other kinds of halide perovskites from 3D to 1D have
been found to have photoferroelectric properties [297–302]. Luo
et al. [297] reported that bis(cyclohexylaminium) tetrabromo lead
(1) is a layered perovskite-type photoferroelectric material, and ex­
hibits quite a good bulk photovoltaic effect along with exceptional
anisotropy which is dominated by ferroelectric polarization. Park
et al. [300] fabricated the 3D organic–inorganic hybrid perovskite
that featured an out-of-plane polarization and a saturated polar­
ization (Ps) value of 3.7 μC/cm2, and showed a long carrier lifetime
and absorption edge. Shi et al. [302] theoretically designed and ex­
perimentally synthesized an electrically switchable, chiral spin-orbit
ferroelectric 1D hybrid halide perovskite material by using chiral
(R)-(-)-1-cyclohexylethylamine (R-CYHEA, C8H15NH2) or (S)-(+)-1-
cyclohexylethylamine (S-CYHEA, C8H15NH2) for the organic group.
Furthers efforts from materials to devices need intensive attempts.
Challenges, prospects and conclusions
Challenges
The PPSCs based on both ferroelectric and photovoltaic effects of
photoferroelectric perovskites are novel photovoltaic devices.
However, many issues concerning the material preparation, device
characterization and insights in to the physical principles behind
need external and internal investigations. Here we highlight the
challenges in developing highly efficient PPSCs.
Solution-processed stable photoferroelectric layer
It is well accepted that solution-processing strategy, featuring a
film matrix formation by simple solution-processing technologies

13
H. Li, F. Li, Z. Shen et al. Nano Today 37 (2021) 101062

(e.g., spin-coating, doctor blading, screen printing, inkjet printing)
and a followed post-annealing at a given annealing temperature (Ta),
is an effective to fabricate low-cost and efficient solar cells. Halide
hybrid photoferroelectric perovskite layers are generally solution-
processed with Ta < 200 °C. However, the films of oxide perovskites
are normally prepared using epitaxy technology at high tempera­
tures (~ 1000 °C), how to get solution-processed oxide photoferro­
electric perovskite layers at a low temperature of Ta < 550 °C for
example is still a challenging technology.
Characterization norm
The J–V characterization is crucially important to evaluate the
performance of solar cells. Presently, the J–V property of PPSCs is
normally measured by the way similar to the conventional solar cells
after the PPSCs have been polarized by the polarization voltage Vp
before the J–V characterizations. The characterization norm is re­
quired. Up to now, during the J–V measurement, an external electric
field is imposed onto the device by a biased voltage (V) on the two
electrodes of the PPSCs. It is still not clear that how the biased
voltage V affects the polarization preformed in the device, and
whether the time gap due to the switch from the Vp state for po­
larization to the V one imposes effects on the J–V measurement.
Moreover, whether it is possible to use the biased voltage V to di­
rectly induce the polarization in PPSCs during the J–V measurement,
from which the YES answer will imply the practical application of
efficient PPSCs with a suitable biased voltage V to provide a con­
tinuing polarization during photovoltaic process.
Physical insights
The correlations between the polarization voltage Vp (or V) or the
polarization electric field Ep and the photovoltaic parameters (Voc,
Jsc, FF, PCE and EQE) are very important. Unfortunately, we are still
lacking the deep insights into the relationship between the materials
ferroelectricity and photovoltaic behaviors. In particular, the physical
bases of the photovoltaic process in PPSCs are rarely known, for
examples, we are still lacking the detailed dynamics of the charge
generation and interfacial injection governed by the photoferro­
electrics property in solar cells, the physical model for the defect-
related charge generation and transport inside the bulk photo­
ferroelectrics perovskite layer, and the comprehensive model to
describe the whole photovoltaic process of PSSCs.
Prospects
The present research and developing tendency of PPSCs is de­
picted by Fig. 8. Oxide perovskites usually have a strong ferroelec­
tricity and their photoelectricity is of increasing interests. In
contrast, the attentions on halide perovskites, are changing from
photoelectricity to ferroelectricity. As a result, both oxide and halide
perovskites are extending their applications photoferroelectrics.
Here we envision some promising methods for achieving efficient
PPSCs.
Molecule engineering to enhance ferroelectricity
Molecular engineering is an effective method to increase the
ferroelectricity or P–E field in the halide perovskites for PPSCs. Hua
et al. reported a precise molecular modification approach to prepare
the [(CH3)3NCH2I]PbI3 perovskite from MAPbI3 by using [(CH3)4N]
PbI3 to increase the ferroelectricity at the room temperature [303].
We also have got the similar findings [304–306]: the electrons on
the oleic acid (OA) molecular chains and the holes on the Pb atoms of
MAPbI3 at the MAPbI3/OA interface form an interfacial electric field
[304]. Moreover, it was found that titanium diisopropoxide bis
(acetylacetonate) (TIPD) can not only effectively passivate the defect
states in MAPbI3 perovskite crystals but also make MA-molecules in
the perovskite crystals preferentially orientated, resulting in an en­
hanced built-in electric field in solar cell [305].
Combination of halide and oxide perovskites
To avoid the toxic Pb element, Sn-based halide perovskite
(ASnX3) is of great interest [43,307,308]. However, the poor photo­
voltaic property and ferroelectricity of ASnX3 are the main factors
limiting the performance of ASnX3-based PPSCs. In order to increase
the ferroelectricity and photovoltaic performance in the solar cell, a
possible approach is to blend the oxide perovskite nanocrystals in
the Sn-based halide perovskite matrix, which brings together the
good film formation property of halides and the strong ferroelec­
tricity of oxides.
Multi-effects to increase the efficiency of PPSCs
Now the PPSCs are mainly based on the dual-effects of ferro­
electrics and photovoltaics. Since all of the ferroelectric materials are
also piezoelectric and pyroelectric ones. Meanwhile, ferroelectricity
is closely associated with ferromagnetism, and sometimes they co­
exist in one material. Therefore, the appropriate integration of these
properties may also enhance the PCE of PPSCs. For example, MAPbI3
was confirmed with both photoferroelectric and photopiezoelectric
properties through density functional theory by Rappe et al. [309],
which could utilize the photopiezoelectric property into PPSCs. A
high proportion of the absorbed sunlight in solar cells is converted to
heat that is detrimental to photovoltaic process, whereas the heat, if
absorbed in situ, can be changed into electricity to increase the PCE
due to the pyroelectric effect. Moreover, in the cases of many flexible
devices, the stress of the flexible substrates will help the

Table 5
Summary of performances of inorganic halide perovskites. BCA: butyl cyanoacetate, NGBr: steric neostigmine bromide, 4AMPI2: (aminomethyl)piperidinium diiodide, PN4N:
amino-functionalized polymer, AZO: Al-doped ZnO. The tests were under standard AM 1.5G illumination.

Structure VOC (V) JSC (mA/cm2) Efficiency (%) FF (%) Ref.

FTO/NiOx/CsPbI3/ZnO/ITO 1.09 18.28 16.04 81 [273]

ITO/PTAA/CsPbI3/C60/BCP/Cu 1.12 17.1 13.4 70 [274]
FTO//TiO2/CsPbI2Br/PTAA/Au 1.32 15.34 16.14 80 [275]
FTO/TiO2/CsPbI3/PTAA/MoO3/Ag 1.25 14.96 14.1 76 [276]
FTO/PTAA/CsPbI3/PCBM/BCP/Ag 1.12 15.81 13.32 75 [277]
FTO/NiOx/CsPbI2Br/ZnO@C60/Ag 1.23 15.87 15.19 78 [278]
ITO/ZnO/CsPbI2Br/Spiro-OMeTAD/Ag 1.21 14.98 14.78 81 [279]
FTO/NiOx/InCl3:CsPbI2Br/ZnO@C60/Ag 1.14 15.7 13.74 77 [280]
ITO/SnO2/CsPbI3/Spiro-OMeTAD/MoO3/Al 1 18.93 14.4 / [281]
FTO/TiO2/CsPbI3/spiro-OMeTAD/MoO3/Ag 1.18 15.21 13.3 74 [282]
ITO/SnO2/LiF/CsPbI3−xBrx/spiro-OMeTAD/Au 1.23 18.3 18.64 83 [283]
FTO/NiOx/CsPb0.6Sn0.4I3/4AMPI2/PCBM/BCP/Ag 0.77 25.87 13.37 67 [284]
FTO/SnO2/CsPbI2.5Br0.5/Spiro-OMeTAD/MoO3/Ag 1.3 17.67 17.1 74 [285]
PEDOT:PSS/AZO/CsPbI2Br/BCA/PTAA/MoO3/Ag 1.26 15.87 15.08 75 [286]
FTO/TiO2/NGBr-CsPbI3/spiro-OMeTAD/MoO3/Au 1.11 19.81 18.27 / [287]

14
H. Li, F. Li, Z. Shen et al.
Fig. 8. Schematic of some development trends for PPSCs.
photoferroelectric materials to generate the strong polarization for a
high PCE. Internal magnetism of photoferroelectric materials con­
duces to reduce the e-h pairs recombination due to Hall effect.
Conclusions
Photoferroelectric perovskite solar cells (PPSCs) integrate the
ferroelectric and photovoltaic effects of photoferroelectric per­
ovskites and offer a novel strategy to develop solar cells. With the
breakthrough at the technology of solution-processed oxide photo­
ferroelectric perovskite layers at a low temperature of Ta < 550 °C for
example, PPSCs are expected to contribute significantly to low-cost
and efficient solar cells. While the perovskite materials with the
dual-effects of ferroelectrics and photovoltaics and/or the multi-ef­
fects of ferroelectrics, piezoelectrics, pyroelectrics and photovoltaics
will find the great potentials in developing efficient PPSCs, more
collaborative efforts from multidisciplinary fields are required to
reveal the physical principles of the charge behaviors regulated by
the dual- and/or multi-effects of photoferroelectric materials in
order to get optimized and efficient devices. This review summarizes
the recent advances in the materials and devices of PPSCs, mainly
involving the oxide and halide perovskites. The major conclusions
from this review are summarized as follows to provide the ele­
mentary background knowledge of the recent PPSCs:
(i) Photoferroelectric oxide and halide perovskites are the main
photoactive materials in the present PPSCs. Amongst the oxide
perovskites, Bi-based materials (e.g., BiFeO3 and Bi2FeCrO6) are
the most efficient ones due to their narrower bandgaps.
However, the PPSCs of Bi-based materials are far behind in the
efficiency of commercialized crystalline silicon solar cells (PCE =
27.6%) [3].
15
Nano Today 37 (2021) 101062
For the halide perovskites, the efficiencies of MAPbI3- and
CsPbI3-based PSCs have been more than 21% [252,255] and 18%
[283,287], respectively, which are comparable to the commer­
cialized crystalline silicon solar cells. However, the development
of their PPSCs is still on the scratch line due to the controversial
issues about their ferroelectricity and its contribution to pho­
tovoltaic process.
(ii) The presence of depolarization electric field (Edp) due to the
ferroelectric polarization is more helpful for the separation and
transport of photogenerated charge carriers to enhance the
photovoltaic performance of the materials system in PPSCs. After
polarization, the resulting Edp is helpful to extend the depletion
region and increase built-in electric field (Ebi) leading to the
significant improvement on the Voc and Jsc of solar cells.
CRediT authorship contribution statement
All authors have discussed and contributed to finish this article.
Huilin Li: Writing - original draft, Writing - review & editing. Fumin
Li: Writing - original draft. Zhitao Shen: Software, Writing - original
draft. Su-Ting Han: Writing - review & editing. Junwei Chen:
Writing - original draft. Chao Dong: Writing - original draft. Chong
Chen: Writing - review & editing, Supervision. Ye Zhou: Writing -
review & editing, Supervision. Mingtai Wang: Conceptualization,
Project administration, Writing - review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing fi­
nancial interests or personal relationships that could have appeared
to influence the work reported in this paper.
H. Li, F. Li, Z. Shen et al.
Acknowledgments
This study was funded by National Science Foundation for Young
Scientists of China (Grant Nos. 61704048, 52003073 and 52002373),
National Natural Science Foundation of China (Grant Nos. 11474286
and 11974353), Program for Science & Technology Innovation Talents
in University of Henan Province (Grant No. 19HASTIT049), Seed Fund
of Young Scientific Research Talents of Henan University (Grant No.
CX0000A40540), Natural Science Foundation of Henan Province
(Grant No. 162300410021), Natural Science Foundation for Young
Scientists of Henan Province (Grant No. 202300410071),
Collaborative Innovation Program of Hefei Science Center, CAS
(Grant No. 2020HSC-CIP004), and the President Foundation of Hefei
Institutes of Physical Science (Grant No. YZJJZX202018).
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Huilin Li is currently an associate Professor in the Henan
Key Laboratory of Photovoltaic Materials at Henan
University. He received his Ph.D. from University of
Science and Technology of China in 2017. He worked as a
postdoctoral fellow in Shenzhen University from 2017 to
2019. He joined the Henan Key Laboratory of
Photovoltaic Materials, Henan University in 2019. His
current research interests include perovskite materials,
low-dimensional ferroelectric and ferromagnetic mate­
rials, and their application in solar cells and memory
devices.
Fumin Li is currently an associate Professor in the Henan
Key Laboratory of Photovoltaic Materials at Henan
University. He received his Ph.D. from College of
Electronic Science and Engineering of Jilin University,
China in 2011. He joined Henan University as a post­
doctoral fellow in 2012. His research focuses on the ap­
plication of nanoscale materials for perovskite, polymer
and quantum dots solar cells.
Zhitao Shen received his Ph.D. degree from Institute of
Chemistry, Chinese Academy of Sciences in 2015. From
2015–2017, he worked as a postdoctoral fellow in
National Chiao Tung University. He joined the Henan Key
Laboratory of Photovoltaic Materials, Henan University in
2017. His current research interests include energy-re­
lated materials simulation and theoretical sum-fre­
quency generation (SFG) spectroscopy.
H. Li, F. Li, Z. Shen et al.
Su-Ting Han is an associate professor at Shenzhen
University. She received her M.Sc. degree in Analytical
Chemistry from Hong Kong Baptist University and her
Ph.D. degree in Physics and Materials Science from City
University of Hong Kong. After graduation, she worked at
the City University of Hong Kong as a postdoctoral fellow.
Her research interests include functional electronic de­
vices and flexible, stretchable, and wearable electronics.
Junwei Chen received his Ph.D. degree in Materials
Physics and Chemistry from University of Science and
Technology of China in 2018. He is now a postdoc re­
search fellow in the Institute of Solid State Physics, Hefei
Institutes of Physical Science, Chinese Academy of
Sciences. His current research activities focus on the
synthesis of semiconductor nanostructures, the solar
cells based on solution-processed inorganic heterojunc­
tions and perovskite films.
Chao Dong received his M.S. degree from Anhui Normal
University in 2014 and Ph.D. degree in Materials Science
and Engineering from University of Science and
Technology of China in 2018. He is now a postdoc re­
search fellow in the Institute of Solid State Physics, Hefei
Institutes of Physical Science, Chinese Academy of
Sciences. His current research activities focus on the thin
film solar cells based on multinary metal chalcogenides
and perovskites.
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Nano Today 37 (2021) 101062
Chong Chen is now a distinguished professor of Henan
Key Laboratory of Photovoltaic Materials, Henan
University. He received Ph.D. from Institute of Plasma
Physics, Chinese Academy of Sciences (CAS) in 2009.
Subsequently he moved to Korea Advanced institute of
Science and technology (KAIST, South Korea) and South
Dakota State University (SDSU, USA), as a postdoctoral
fellow in 2010 and 2011, respectively. In 2012, he joined
Henan University. He worked at Pittsburgh of University,
USA, as a visiting scholar during 2017–2018. He is leading
a group that mainly studies perovskite solar cells,
quantum dot-sensitized solar cells, and polymer solar
cells.
Ye Zhou is an IAS Fellow in the Institute for Advanced
Study, Shenzhen University. His research interests in­
clude flexible and printed electronics, organic/inorganic
semiconductors, surface and interface physics, nanos­
tructured materials, and nano-scale devices for techno­
logical applications, such as logic circuits, data storage,
photonics and sensors.
Mingtai Wang received Ph.D. degree from University of
Science and Technology of China in 1997. After his
postdoctoral research at Institute of Solid State Physics
(ISSP), Chinese Academy of Sciences (CAS), he joined the
ISSP as associate professor in 1999. He worked at
Institute of Polymer Research Dresden, Germany as vis­
iting scientist and Alexander von Humboldt research
fellow during 2000–2003. He became a full professor of
Materials Physics and Chemistry in Hefei Institutes of
Physical Science, CAS under “100-talent Program” in
2004. He is leading a group that mainly studies the ma­
terials and device performance in low-cost solar cells.