RESEARCH ARTICLE
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Oriented Growth for Efficient and Scalable Perovskite Solar
Cells by Vapor–Solid Reaction
Changyu Duan, Jialing Zhong, Shenghan Hu, Yichen Dou, Jianfeng Lu, Yi-Bing Cheng,
and Zhiliang Ku*
The precise control and understanding of crystal orientation in perovskite
polycrystalline films are crucial for the development of efficient and stable
devices. However, achieving this control remains a significant challenge.
Herein, a PbI2 oriented growth strategy is developed, combined with in situ
vapor–solid reaction transformations, to achieve oriented growth of
full-vacuum perovskite films. Grazing-incidence wide-angle X-ray scattering
(GIWAXS) analysis revealed the general pattern of PbI2 oriented vapor growth
and in situ vapor–solid reaction transformation in this two-step process. The
resulting preferred orientation has effectively reduced trap state density,
optimizing the carrier dynamics. As a result, champion efficiencies of 22.11%
(0.148 cm2 ), 20.60% (1 cm2 ), and 19.41% (5 × 5 cm2 mini-modules) are
achieved, which are the highest value for perovskite based on vapor–solid
reaction. Additionally, the oriented growth method is applicable to a variety of
guide layers and is extended to 30 × 30 cm2 film, demonstrating the
universality and scalability of the method.
1. Introduction
Perovskite solar cells have garnered significant attention in re-
search due to their rapidly increasing efficiency and promising
potential for commercialization.[1] Numerous efforts have been
focused on enhancing the efficiency of perovskite solar cells,
such as additive doping,[2] solvent engineering,[3] and interface
modification,[4] which reduces carrier recombination by passivat-
ing bulk and interface defects, or enhances carrier extraction. The
underlying principle of these strategies is to manage the carrier
behavior within the device to improve the power output. There-
fore, precisely controlled crystal growth of perovskite thin films,
which can fundamentally improve the film quality to optimize
C. Duan, J. Zhong, S. Hu, Y. Dou, Y.-B. Cheng, Z. Ku
State Key Laboratory of Advanced Technology for Materials Synthesis and
Processing
Wuhan University of Technology
Wuhan 430070, China
E-mail: zhiliang.ku@whut.edu.cn
J. Lu
State Key Laboratory of Silicate Materials for Architectures
Wuhan University of Technology
Wuhan 430070, China
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adfm.202313435
DOI: 10.1002/adfm.202313435
Adv. Funct. Mater. 2024, 34, 2313435 2313435 (1 of 11)
the carrier dynamics, is crucial to further
enhance device performance.
Oriented growth has emerged as a highly
effective strategy for enhancing the qual-
ity and stability of perovskite films. This
is due to the close relationship between
carrier transport, trap state density, and
the crystal plane orientation, which is
known as the anisotropy of perovskite
optoelectronic properties.[5] For example,
the use of photoconductive atomic force
microscopy has revealed spatially corre-
lated heterogeneity in short-circuit cur-
rent and open-circuit voltage, which is
attributed to a facet-dependent density
of trap states.[6] Additionally, anisotropy
in all-inorganic single-crystal perovskites
has been observed, with surface-dependent
electronic structures, defect formation ener-
gies, and carrier mobility being compared
in CsPbBr3 -based optoelectronic devices
using (110) cubes and (111) tetrahedrons.[7] Both theoretical cal-
culations and experimental studies have further demonstrated
the anisotropy of carrier behavior and charge extraction in per-
ovskite crystals.[8] Based on these findings, considerable research
efforts have focused on manipulating the plane orientation of per-
ovskite crystals. Various approaches have been explored, includ-
ing the introduction of crystal seeds,[9] cation doping,[10] bottom-
up epitaxial growth,[11] and intermolecular exchange.[12] For in-
stance, cation doping has been shown to manipulate the crys-
tal facet orientation upon crystallographic plane stacking, result-
ing in absorbers with preferred facet orientation that exhibit
higher carrier mobility and photocurrent in the corresponding
devices.[10] Recent studies have reported the controlled formation
of perovskite polyhedral single crystals with well-defined crystal
planes, aiming to identify the top-performing perovskite crystal
planes for photovoltaic applications.[5b] It has been found that the
(100) and (111) planes demonstrate more n-type characteristics
and higher carrier mobility compared to the (110) planes. Ad-
ditionally, a solution-processed bottom-up quasi-epitaxial growth
method has been employed to manipulate the crystal orientation
of 𝛼-FAPbI3 films, resulting in a significant reduction in open-
circuit voltage (Voc ) loss and an enhanced power conversion effi-
ciency (PCE).[11]
Despite the extensive efforts mentioned, the fast crystalliza-
tion rate and unpredictable nucleation and growth of perovskite
in solution processes continue to hinder the control and mech-
anistic understanding of oriented growth.[13] Moreover, these
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solution methods, typically employed in small-area spin-coating,
face challenges when it comes to scaling up for large-area
fabrication, limiting their scalability. In contrast, vapor deposi-
tion is a well-established industrial method that offers precise
control over crystal growth at a slower rate, making it suitable
for large-scale production. However, vapor deposition growth
necessitates demanding conditions such as high vacuum, com-
plex equipment, or single crystal substrates. Consequently, the
oriented growth of perovskite films using the vapor deposition
method is still lacking.
In this study, we present an oriented growth approach of
vapor-deposited perovskite films using a 2D-guided PbI2 oriented
growth strategy coupled with in situ transformation of vapor–
solid reactions. By employing the Grazing-incidence wide-angle
X-ray scattering (GIWAXS) technique, we meticulously investi-
gated the stepwise process of the oriented growth of PbI2 films
and their transformation process toward perovskite. Our results
show that the 2D layers can act as a guide to induce the oriented
growth of the PbI2 (001) crystal plane along the direction per-
pendicular to the substrate. These oriented features are retained
during the subsequent in situ transformation, resulting in per-
ovskite films with well-aligned crystal orientations. The oriented
growth perovskites exhibit superior carrier dynamics due to re-
duced trap state density and better carrier mobility along specific
crystal planes. As a result, the corresponding devices based on
these oriented-growth perovskites exhibited enhanced PCE and
long-term stability, which are the highest value for perovskite
based on vapor–solid reaction. In addition, this oriented growing
technique can easily be extended to large-area fabrication (30 × 30
cm2 ), benefiting from the advantages of its vapor processing. Fur-
thermore, the universality of this approach is validated by effec-
tively inducing oriented growth with several common 2D per-
ovskites (PEA, PMA, BA, and HA-based). Our research confirms
the feasibility of oriented growth of perovskite by vapor-based
methods and provides an important route for commercial pro-
duction of large-area high-quality perovskite thin films.
2. Results and Discussion
2.1. The Guided-Oriented Growth Method and Orientation
Characterization
Herein, one of the most common 2D perovskites, PEA-based per-
ovskites, was used as an example to describe the oriented growth
method. The fabrication process of the 2D guide layer was stud-
ied first. Initially, a 10 nm PbI2 film was deposited on the sub-
strate by thermal evaporation, and then, reacted with PEAI vapor
to fabricate the 2D guide layer (Figures S1A,S2,S3 Note S1, Sup-
porting Information). Prior to reacting with the PEAI vapor, the
diffraction peak (12.6°) of the PbI2 (001) crystal plane was very
weak due to its thin thickness (Figure S1B, Supporting Infor-
mation). However, after the reaction, the diffraction peak (5.4°)
of the 2D guide layer, corresponding to (002) crystal plane of
PEA2 PbI4 perovskite (n = 1), showed a significant enhancement,
indicating superior high crystallinity. It is well known from pre-
vious reports that 2D perovskite with n = 1 exhibits a strong
preferred orientation.[14] From the scanning electron microscope
(SEM) image (Figure S1, Supporting Information), it can be ob-
served that the 2D guide layer completely and uniformly covered
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the substrate. In order to further investigate the vapor–solid re-
action that generates the 2D guide layer, PbI2 was exposed to a
PEAI atmosphere for 5, 10, 15, and 20 min, respectively (Figure
S4A, Supporting Information). These samples of 2D guide layer
with reaction times of 5, 10, 15, and 20 min were labeled as 2D-
5, 2D-10, 2D-15, and 2D-20. The X-ray diffraction (XRD) results
indicate that the intensity for the 2D guide layer continuously in-
creased as the reaction time, until reaching saturation at 15 min,
after which it slightly decreases (Figure 1B). This decrease may be
attributed to overreaction. The UV–vis and PL spectra (Figure S4,
Supporting Information) also exhibit the strongest absorption or
excitation peak at 15 min, similar to the XRD findings.
After the preparation of 2D guide layers, to examine the in-
fluence of 2D guide layers on PbI2 , 350 nm PbI2 films were de-
posited on 2D guide layers with varying reaction times through
thermal evaporation (Figure 1A). The PbI2 samples deposited on
2D guide layers with reaction times of 5, 10, 15, and 20 min were
denoted as PbI2 @ 2D-5, PbI2 @ 2D-10, PbI2 @ 2D-15 and PbI2
@ 2D-20, collectively referred to as guided PbI2 . As depicted in
Figure 1C, there is a strong correlation between the diffraction
intensity of the guided PbI2 films and the intensity of the 2D
guide layers. When the peaks of the 2D guide layer were inten-
sified, the diffraction peaks of the PbI2 films deposited on them
also increased. Notably, the diffraction intensity of the 2D guide
layer (2D-15) reached its maximum, coinciding with the maxi-
mum diffraction intensity of PbI2 (PbI2 @ 2D-15). This provides
compelling evidence that the 2D guide layers exert a notable in-
fluence on the crystalline growth of PbI2 films.
Next, a series of guided PbI2 films were transformed into FA-
based 3D perovskite films through an in situ vapor–solid reac-
tion with a mixture atmosphere of FAI and FACl (Figure 1A).
These perovskite samples were named PVK @ 2D-5, PVK @
2D-10, PVK @ 2D-15, and PVK @ 2D-20, collectively referred
to as guided perovskites. Figure 1D illustrates that the diffrac-
tion intensity of the perovskite films strongly correlates with the
intensity of the guided PbI2 films (Figure S5, Supporting Infor-
mation), indicating that the crystallographic modulation of PbI2
is retained in the perovskite films during the vapor–solid reac-
tion. This suggests that the 2D guide layer can manipulate the
crystallization of PbI2 films, thus achieving control over the crys-
tallization of the perovskite.
To further investigate the factors influencing the diffraction
enhancement of PbI2 and perovskite films (Figure 1B,C), pow-
ders were scraped from the PbI2 (control PbI2 and PbI2 @ 2D-
15) and perovskite (control PVK and PVK @ 2D-15) films, re-
spectively, and were tested by powder XRD (Figure S6, Support-
ing Information), and it was found that both PbI2 powders and
both perovskite powders exhibited comparable diffraction inten-
sities. Further, XRD pole figure analysis (Figure 1E–I) was con-
ducted on the (001) planes of the perovskite-based on 2D guide
layers with varying reaction times. It was observed that the (001)
plane of the control sample exhibited a relatively random orien-
tation, whereas the pole figure of guided perovskites displayed a
more concentrated diffraction signal at the center. These results
suggest that the diffraction enhancement in conventional XRD
comes from vertical orientation rather than crystallinity changes.
A vertical orientation of the perovskite (001) plane has been re-
ported to facilitate carrier transport.[5b,7,9,11,15] Furthermore, the
diffraction signal of the modified sample became increasingly
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Figure 1. Perovskite film processing and X-ray diffraction analysis. A) Schematic diagram of the preparation process of 2D guided oriented growth
method. B–D) Conventional XRD of 2D guide layer B), PbI2 C) films, and perovskite D) films. E–I) XRD pole figure along (001) orientation of control
PVK E), PVK @ 2D-5 F), PVK @ 2D-10 G), PVK @ 2D-15 H) and PVK @ 2D-20 I). J) XRD rocking curves of PVK @ 2D-15 and control perovskite films.

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Figure 2. Stepwise GIWAXS analysis to reveal the oriented growth mechanism. A) GIWAXS analysis of control sample and 2D guide layer. B) GIWAXS
analysis of control and oriented PbI2 (PbI2 @ 2D) films. C) GIWAXS analysis of control and oriented perovskite (PVK @ 2D) films.
localized as the reaction time of the 2D guide layer increased,
reaching a maximum in 15 min. This observation aligns with
the conventional XRD results, further confirming the inheri-
tability of orientation in our method. XRD rocking curves addi-
tionally demonstrated the vertical orientation of the (001) plane
(Figure 1J).
2.2. Understanding the Mechanism of the Guided-Oriented
Growth Method
Grazing-incidence wide-angle X-ray scattering (GIWAXS) is a
widely used technique in grazing-incidence X-ray scattering
(GIXS) that allows for the simultaneous collection of signals in
both in-plane and out-of-plane directions. This enables the di-
rect acquisition of orientation information from 2D patterns.[16]
Figure 2 displays the diffraction patterns of the 2D guide lay-
ers, guided PbI2 films (including control PbI2 ), and guided per-
ovskite films (including control perovskite). It is important to
note that the grazing incidence angle is dependent on the sam-
ple thickness. The 2D guide layer has a thickness of ≈50 nm,
corresponding to an angle of 0.2°, while the PbI2 and perovskite
films have thicknesses of several 100 nm, corresponding to an
angle of 0.5°. As shown in Figure 2A, for the control layer (thin
PbI2 film, precursor of the 2D guide layer), no visible diffrac-
tion signal was observed due to its extremely thin thickness and
poor crystallinity. For all the 2D guide layers, diffraction signals
were detected at q = 0.38, 0.77, and 1.15 Å−1 , which correspond to
the (002), (004), and (006) crystal planes with d-spacing values of
16.35, 8.18, and 5.45 Å, respectively.[17] These diffraction signals
are predominantly oriented in the out-of-plane direction and are
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most pronounced in the (002) crystal plane. This provides direct
evidence that the 2D guide layer possesses an out-of-plane orien-
tation, consistent with the characteristics of 2D perovskites.[16–18]
Furthermore, it is worth noting that the intensity of the diffrac-
tion signal increases with longer reaction times, suggesting that
reaction time is a crucial parameter for manipulating the ori-
entation. These findings align well with the conventional XRD
results.
Regarding the guided PbI2 films (Figure 2B), a diffraction sig-
nal is observed at q = 0.90 Å−1 , indicating an out-of-plane ori-
entation corresponding to the (001) crystal plane of PbI2 , with a
d-spacing value of 6.98 Å. The orientation of PbI2 closely aligns
with that of the 2D guide layer, and the degree of orientation
increases in tandem with the orientation of the 2D guide layer.
These findings provide compelling evidence that the 2D guide
layers induce oriented growth of PbI2 crystals along the out-of-
plane direction. The 2D guide layer plays a critical role in deter-
mining this oriented growth.
In the case of the perovskite films (Figure 2C), a diffrac-
tion signal at q ≈0.99 Å−1 corresponds to the perovskite (001)
plane, with a d-spacing value of 6.36 Å. Additionally, the refer-
ence perovskite exhibits homogeneous and continuous Debye-
Scherrer rings, indicating isotropic orientation. In contrast, the
(001) diffraction signal of the guided perovskite (PVK @ 2D) is
concentrated in the out-of-plane direction, demonstrating a desir-
able preferred orientation.[5b] Interestingly, the orientation level
of the perovskite aligns with that of PbI2 . This suggests that the
out-of-plane orientation has been inherited from PbI2 into the
perovskite during the in situ vapor–solid reaction. To gain a more
direct understanding of the preferred orientation, intensity az-
imuthal plots along the 2D perovskite (002) ring, the PbI2 (001)
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ring, and the perovskite (001) ring are depicted in Figure S7 (Sup-
porting Information), where the polar angle (𝜒) represents the
angle relative to the substrate normal.
Based on the aforementioned findings, the following conclu-
sions can be drawn. The 2D guide-oriented growth method en-
ables the manipulation of perovskite orientation by inducing
oriented growth of PbI2 through the 2D guide layer, followed
by an in situ transformation from oriented growth PbI2 to ori-
ented growth perovskite. Furthermore, we have discovered that
the 2D guided-oriented growth method is not restricted to a sin-
gle material. As illustrated in Figure S8 (Supporting Information,
PMAI, BAI, and HAI can all react with PbI2 to form 2D per-
ovskite, thereby facilitating guided oriented growth of PbI2 and
subsequent preparation of preferred orientation perovskite thin
films. These results strongly demonstrate the universality of our
method.
Remarkably, no characteristic signals of 2D perovskites were
observed in the final perovskite films, leading to speculation that
the 2D guide layers underwent conversion to FA-based 3D per-
ovskites in an FAI/FACl mixture atmosphere during the in situ
vapor–solid reaction. To verify this hypothesis, a pure 2D film
with the same components as the 2D guide layer but with a
greater thickness was exposed to an FAI/FACl mixture atmo-
sphere at 160 °C and 100 Pa for 5 min. XRD and SEM anal-
yses were performed at the first, third, and fifth-minute inter-
vals. Figures S9,S10 (Supporting Information) clearly demon-
strate the transformation process from 2D perovskite to 3D per-
ovskite through the XRD patterns and SEM images. The pro-
cess can be summarized as follows: Initially, FA+ infiltrates the
lattice of the 2D perovskite film and replaces PEA+ , converting
the 2D PEA2 PbI4 (n = 1) perovskite to 2D PEA2 FAPb2 I7 per-
ovskite (n = 2). As the reaction proceeds, FA+ continues to
enter while PEA+ gradually escapes as PEAI vapor. Eventually,
the film is completely saturated and completely converted to 3D
perovskite. The relevant reaction equation is shown in Note S2
(Supporting Information). To further substantiate the absence
of 2D perovskite residues in the final films, a comparison was
made between the reference perovskite and the guided perovskite
using Fourier transform infrared (FTIR) spectroscopy and UV–
vis analysis (Figures S11,S12, Supporting Information). The ab-
sorption peaks associated with benzene rings (≈3050 cm−1 for
C─H stretch and 1600–1450 cm−1 for C = C stretch) were not de-
tected in either the reference perovskite or the guided perovskite
films.[19] Additionally, the UV–vis absorption edges of both per-
ovskites showed no shift. These results indicate the absence of
2D perovskite residues in the final guided 3D perovskite films
and exclude the possibility of potential carrier hindrances caused
by 2D perovskite remnants.[20]
Observation of microscopic morphology promotes further un-
derstanding of the mechanism of oriented growth. SEM analy-
sis was conducted to examine the morphology of PbI2 (prior to
the in situ vapor–solid reaction) and perovskite (following the
in situ vapor–solid reaction). From the SEM top view images
(Figure 3B,D), it is evident that PbI2 exhibits typical sheet-like
crystal structures in both the reference and guided samples.[21]
The reference PbI2 sheet crystals are randomly distributed on
the substrate, exhibiting both vertical and horizontal orienta-
tions. In contrast, the guided PbI2 sheet-like crystals predom-
inantly display a horizontal morphology, with only a few verti-
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cal structures. Upon transformation of PbI2 into perovskite, the
guided perovskite demonstrates a smoother surface with fewer
pores compared to the reference perovskite (Figure 3C,E). To
further investigate the mechanism of oriented growth, cross-
sectional SEM images were analyzed (Figure 3J–M). It can be
observed that the sheet-like PbI2 crystals undergo a transition
from chaotic and vertical arrangements to ordered and paral-
lel structures with the guided-oriented growth approach. Impor-
tantly, as PbI2 undergoes oriented growth, the perovskite also
transfers into a vertical and thorough structure, which is be-
lieved to contribute to enhanced performance.[16a,22] The large-
scale SEM cross-section is shown in Figure S13 (Supporting
Information).
AFM (Atomic Force Microscopy) was utilized to examine the
micromorphology of PbI2 and perovskite films, providing addi-
tional evidence for the proposed mechanism (Figure 3F–I). Con-
sistent with the SEM findings, AFM images demonstrate that the
reference PbI2 crystals exhibit a random arrangement and are in-
clined to the substrate, while the guided PbI2 sheet crystals align
approximately parallel to the substrate. Furthermore, AFM was
employed to evaluate surface roughness, yielding a root mean
square roughness (Rq ) of 17.4 nm for the control PbI2 films and
11.9 nm for the guided PbI2 films. This indicates that the ori-
ented growth of PbI2 results in a smoother surface. Similarly, the
Rq value for the control perovskite films was 24.1 nm compared
to 9.4 nm for the guided perovskite films, which is in agreement
with the SEM observations. These findings provide further con-
firmation of the proposed mechanism.
The mechanism of the 2D layer-guided oriented growth of
PbI2 can be explained by lattice matching (Note S3, Support-
ing Information).[23] As shown in Figure S14 (Supporting Infor-
mation), lattice matches between the three most dominant PbI2
(001), (011), and (012) planes (according to the standard powder
diffraction file) and the 2D perovskite (001) planes were com-
puted. The results are shown in Figure S15 and Table S1 (Sup-
porting Information), the PbI2 (001) plane has the smallest lat-
tice mismatch of 7.0% compared to the (011) and (012) planes
(44.4% and 13%). This indicates that PbI2 is more likely to grow
vertically with the (001) plane oriented when deposited on the 2D
(001) plane.
Based on the above results, we propose the following mech-
anism (schematically represented in Figure 3A): i) In the case
of the control PbI2 films, the crystal orientation is random, as
confirmed by GIWAXS analysis. ii) In the guided PbI2 films, the
highly oriented 2D guide layers serve as guides for the oriented
growth of PbI2 during vapor deposition, explained by the lattice
match. iii) The orientation characteristic is preserved during the
transformation of PbI2 to perovskite through the vapor–solid re-
action. This preservation occurs due to the in situ crystal growth
of perovskite, which differs from the dissolution and recrystal-
lization process in a solvent environment.
2.3. Charge Carrier Dynamics
The guided-oriented growth method employed in this study
induces the orientational crystallization of perovskite films,
which prompted us to investigate its positive effects on carrier
dynamics.[5b,7] Initially, the steady-state photoluminescence (PL)
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Figure 3. Microstructure analysis to reveal the oriented growth mechanism. A) Schematic diagram of the oriented growth mechanism. B–E) Top-view
SEM images of oriented PbI2 (PbI2 @ 2D-15) films B), oriented perovskite (PVK @ 2D-15) films C), control PbI2 films D) and control perovskite films
E). F–I) 3D AFM images of control PbI2 films F), oriented PbI2 (PbI2 @ 2D-15) films G), control perovskite films H), and oriented perovskite (PVK @
2D-15) films I). J–M) Cross-sectional SEM image of control PbI2 films J), oriented PbI2 (PbI2 @ 2D-15) films K), control perovskite films L) and oriented
perovskite (PVK @ 2D-15) films M). The scale bar is 1 μm.

spectrum was utilized to assess the non-radiative recombination
of carriers (Figure 4A). All perovskite films were fabricated on
glass substrates. In comparison to the control films, the guided
perovskite films exhibited significantly higher PL peak intensi-
ties, which increased progressively with reaction time. The peak
intensity reached its maximum at 15 min, corresponding to the
point where the orientation is most concentrated (Figure S16,
Supporting Information). This observation suggests that the ori-
ented growth of perovskite films leads to reduced nonradiative
recombination losses and improved film quality.[24] Further, car-
rier recombination was quantified using the time-resolved pho-
toluminescence (TRPL) spectrum (Figure 4D). The decay curves
were fitted with a bi-exponential equation:
I (t) = A1 e−t∕𝜏1 + A2 e−t∕𝜏2
The average carrier lifetime was evaluated by the following
equation:
( ) ( )
𝜏avg = A1 𝜏12 + A2 𝜏22 ∕ A2 𝜏2 + A2 𝜏2 (2)
The average carrier lifetimes of the guided-oriented perovskite
films increased to 223.05, 309.07, and 350.23 ns, corresponding
to 5, 10, and 15 min of reaction time, respectively. In contrast,
the average carrier lifetime of the reference films was measured
at 92.3 ns (Figure S17, Table S2, Supporting Information). To fur-
ther assess the charge carrier dynamics of the perovskite films,
time-resolved confocal photoluminescence microscopy measure-
ments were conducted (Figure 4B,C).[25] The results revealed that
the oriented perovskite films exhibited a longer PL lifetime, as
they were distributed in the green region. On the other hand, the
(1) control perovskite films showed a shorter PL lifetime and were

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Figure 4. The Carrier dynamics characterization of oriented growth perovskite. A) Steady-state photoluminescence spectrum of perovskite films. B,C)
Time-resolved confocal photoluminescence microscopy images of control perovskite films and oriented perovskite films. D) TRPL of perovskite films
deposited on glass. E,F) SCLC measurements based on electron-only devices for control E) and oriented (PVK @ 2D-15) perovskite F). G) Dark J–V
curves of control and oriented (PVK @ 2D-15) PSCs. H) Mott-Schottky curves of control and oriented (PVK @ 2D-15) PSCs. I) Nyquist plots of control
and oriented (PVK @ 2D-15) PSCs.

predominantly distributed in the blue region. This observation
indicates that the guided-oriented perovskite films effectively in-
hibit trap-induced or nonradiative recombination.
The space charge limited current (SCLC) technique was ap-
plied to quantify the trap state density.[7] The electron-only de-
vices were fabricated as FTO|SnO2 |PVK|PCBM|Ag for testing. As
shown in Figure 4E,F, according to the different current–voltage
characteristics, the curve is divided into three regions, which are
defined as the ohmic region, the trap-filling limit (TFL) region,
and the SCLC region respectively. The inflection point between
the ohmic and TFL regions is defined as the VTFL , which is often
used to evaluate the trap state density according to the following
equation:
Ntrap = 2𝜀𝜀0 VTFL ∕eL2 (3)
where Ntrap is trap states density, 𝜖 is the relative permittivity of
perovskite, 𝜖 0 denotes permittivity of vacuum, e is the elementary
charge, L is the thickness of perovskite film. The trap state den-
sities were calculated to be 4.81 × 1015 and 3.65 × 1015 cm−3 for
oriented perovskite and control perovskite, respectively.
The dark current density–voltage (J–V) characteristics of the
perovskite solar cells (PSCs) are presented in Figure 4G. The
device with the preferred orientation demonstrates a leakage
current density that is one order of magnitude lower compared to
the reference device. Notably, in the high voltage range of the J–V
curve, the preferred orientation device exhibits a steeper slope
than the reference device, indicating a lower series resistance
(Rs ). Mott–Schottky analysis was performed to investigate the
built-in potential (Vbi ) and carrier behavior in the devices,[26] as
depicted in Figure 4H. The Vbi increases from 0.97 V for the

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Figure 5. The Device efficiency and stability characterization. A,B) Schematic diagram of devices and charge carrier transport. C) Reverse J–V curves
of champion control and oriented devices. D) External quantum efficiency (EQE) spectra of control and oriented devices. E) Steady-state power output
(SPO) of control and oriented devices. F) Histogram of devices PCE for control and oriented perovskites. G) Long-term stability at 25 ± 5 °C, 15 ± 10%
RH of the unencapsulated devices. H) Thermal stability at 70 ± 5 °C, 25 ± 10% RH of the unencapsulated devices.

reference devices to 1.01 V for the preferred orientation devices.
This enhancement in Vbi facilitates carrier extraction, sup-
presses carrier complexation, and enhances the Voc (open-circuit
voltage).[27]
To gain further insights into the influence of preferred orien-
tation on carrier transport and recombination processes, Elec-
trochemical Impedance Spectroscopy (EIS) measurements were
conducted. The recombination resistance (Rrec ) was evaluated by
fitting an equivalent circuit model, showing that the oriented
growth PSCs have a greater Rrec (1108 Ω) compared to the ref-
erence PSCs (658 Ω), indicating a suppression of charge re-
combination (Figure 4I).[28] Additionally, the conductive Atomic
Force Microscopy (c-AFM) characterization demonstrates higher
currents for the oriented perovskite, further supporting the
optimized carrier dynamics (Figure S18, Supporting Informa-
tion). Thus, the guided-oriented growth method proves to be
highly effective in enhancing the quality of perovskite films at
the carrier kinetic level, as confirmed by the aforementioned
results.[29]
2.4. Photovoltaic Performance and Stability of Devices
After characterizing the carrier dynamics, we proceeded to
fabricate solar cell devices to evaluate the impact of the oriented
growth method on photovoltaic performance. The schematic di-
agram illustrating carrier transport within the device is depicted
in Figure 5A,B. Benefiting from the optimization of carrier
dynamics, the oriented growth PSCs demonstrate a champion
power conversion efficiency (PCE) of 22.11%. This notable PCE
is accompanied by a Voc of 1.163 V, a Jsc of 24.00 mA cm−2 , and
a fill factor (FF) of 0.792. In comparison, the highest efficiency
achieved by the control PSCs was a mere 20.42%, featuring a Voc
of 1.126 V, a Jsc of 23.40 mA cm−2 , and an FF of 0.775 (Figure 5C;
Figures S19,S20, Supporting Information). It represents the
highest value for PSCs via vapor–solid reaction (Figure S21,
Table S3, Supporting Information). To verify the reproducibility
of the oriented growth strategy in enhancing device PCE, the
PCE distributions of the oriented growth devices and control
devices are presented in Figure 5F. The PCE distribution of the

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Figure 6. The large area of perovskite devices and films. A) Reverse J–V curves of champion 1 × 1 cm2 devices. B) Reverse J–V curves of champion
5 × 5 cm2 modules. C) Photograph of 30 × 30 cm2 perovskite films.
control devices ranges from 19.1% to 20.3%, while the oriented
growth devices exhibit an improvement of 20.7% to 21.8%.
Figure 5D illustrates the external quantum efficiency (EQE)
spectra and corresponding integrated current densities of the
oriented device and the control device. The results indicate that
the oriented growth devices achieve higher EQE and a signifi-
cant increase in integrated current density, from 23.05 mA cm−2
(control device) to 23.58 mA cm−2 (oriented growth device),
consistent with the short-circuit current densities derived from
the J–V measurements. To assess the operational stability of the
control and oriented growth devices, steady-state power output
was recorded for 600 s at the maximum power point (MPP)
derived from J–V curves (Figure 5E). During the 600 s steady-
state output, the average efficiency of the oriented growth device
remained at 20.98%, experiencing only a 2.5% drop compared to
the initial value. In contrast, the average efficiency of the control
device was a mere 18.75%, with a final efficiency decrease of 4%
compared to the initial value.
The high crystal quality and low defects achieved through
favorable orientation not only enhance the optoelectronic
properties of PSCs but also contribute to their improved
stability.[5a,9,15,30] As depicted in Figure 5G, the unencapsulated
oriented growth PSCs retained 95% of their initial PCE after
1248 h of storage in dry air (25 ± 5 °C, 15 ± 5% RH) in the
dark, while the control devices decayed to 81% of their initial
PCE. Furthermore, the thermal stability of the devices was in-
vestigated (Figure 5H). After aging for 880 h at 70 °C in the air
(25 ± 5% RH), the unencapsulated oriented growth PSCs main-
tained ≈80% of their initial PCE, whereas the control devices ex-
perienced a decay to ≈50% of their initial value. In the MPP track-
ing test, the oriented growth device remained at 60% of the ini-
tial value after 750 h, while the control device decreased to 30% of
the initial value after 250 h (Figure S22, Supporting Information).
These significant improvements in stability can be attributed to
the high crystal quality, minimal defects,[31] and the hydrophobic
nature of the perovskite crystal surface (Figure S23, Supporting
Information).[32] The XRD and SEM results reveal that the ori-
ented perovskite films undergo less decomposition of PbI2 under
thermal stress compared to the control perovskite films, indicat-
ing the effectiveness of the oriented growth method in enhancing
film stability (Figure S24, Supporting Information). Similar re-
sults were obtained in the device thermal stability measurements
(Figure S25, Supporting Information).
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With the vapor process offering easy scalability, the oriented
growth method can be readily applied to large areas.[33] We suc-
cessfully fabricated 1 × 1 cm2 devices and 5 × 5 cm2 modules
using the oriented growth approach. As depicted in Figure 6,
the 1 × 1 cm2 device achieved an impressive PCE of 20.60%,
while the 5 × 5 cm2 module achieved a PCE of 19.41%. In
addition, the oriented growth method has been extended to
the manufacture of 30 × 30 cm2 perovskite films (Figure 6C;
Figure S26, Supporting Information). These results further un-
derscore the immense potential of our method for large-scale
production.
3. Conclusion
In this study, we have successfully demonstrated the effective-
ness of the 2D guided oriented growth strategy in promoting the
orientation control of vapor-deposited PbI2 and subsequent per-
ovskite films. Through stepwise GIWAXS analysis, we have con-
firmed the strong correlation between the orientation of 2D guide
layers, vapor-deposited PbI2 , and perovskite films. Microstruc-
ture characterization has provided insights into the mechanism
of orientation growth in vapor-deposited PbI2 . The optimized ori-
entation has led to enhanced carrier dynamics and stability in
perovskite devices. As a result, we achieved remarkable power
conversion efficiencies of 22.11% for a 0.148 cm2 device, 20.60%
for a 1 cm2 device, and 19.41% for a 5 × 5 cm2 mini-module, all
based on the 2D guided oriented growth strategy. Notably, the un-
encapsulated devices using oriented perovskite retained 95% of
their initial efficiency after 1248 h of storage. To the best of our
knowledge, these efficiencies and stability represent some of the
highest achieved in PSCs based on vapor–solid reactions. This
work presents a promising strategy for manipulating orientation
in large-scale production (30 × 30 cm2 ) and provides valuable in-
sights into the mechanism of crystal growth in vapor-deposited
perovskite. We believe that this study contributes significantly
to the understanding of crystal growth manipulation in vapor-
deposited perovskite materials.
4. Experimental Section
See experimental details in the Supporting Information.
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Supporting Information
Supporting Information is available from the Wiley Online Library or from
the author.
Acknowledgements
The authors acknowledge the financial support from the National Natu-
ral Science Foundation of China (Grant No. NSFC 51972251, 91963209).
Joint Foundation for Innovation and Development of Hubei Natural Sci-
ence Foundation (Grant No. 2023AFD032). Hubei Provincial Natural Sci-
ence Foundation of China (Grant No. 2023AFA010).
Conflict of Interest
The authors declare no conflict of interest.
Data Availability Statement
The data that support the findings of this study are available from the cor-
responding author upon reasonable request.
Keywords
large-area, oriented growth, perovskite solar cells, photoelectric
anisotropy, vapor deposition
Received: October 30, 2023
Revised: December 31, 2023
Published online: January 30, 2024
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