hv

photonics

Article
Enhancing the Overall Performance of Perovskite Solar Cells
with a Nano-Pyramid Anti-Reflective Layer
Li Liu 1, *, Wenfeng Liu 2 , Wenfeng Fu 1 , Zao Yi 1,3, * , Yougen Yi 2 , Jianguo Zhang 4 , Chaojun Tang 5 ,
Tangyou Sun 6 , Qingdong Zeng 7 and Pinghui Wu 8

1 Joint Laboratory for Extreme Conditions Matter Properties, Key Laboratory of Manufacturing Process Testing
Technology of Ministry of Education, State Key Laboratory of Environment-Friendly Energy Materials,
Southwest University of Science and Technology, Mianyang 621010, China; fuwenfeng2021@[Link]
2 School of Energy Science and Engineering, College of Physics, Central South University,
Changsha 410083, China; 193902015@[Link] (W.L.); yougenyi@[Link] (Y.Y.)
3 School of Chemistry and Chemical Engineering, Jishou University, Jishou 416000, China
4 Department of Physics, Jinzhong University, Jinzhong 030619, China; [Link]@[Link]
5 College of Science, Zhejiang University of Technology, Hangzhou 310023, China; chaojuntang@[Link]
6 Guangxi Key Laboratory of Precision Navigation Technology and Application, Guilin University of Electronic
Technology, Guilin 541004, China; suntangyou@[Link]
7 School of Physics and Electronic-information Engineering, Hubei Engineering University,
Xiaogan 432000, China; zengqingdong2005@[Link]
8 Office of Science and Technology, Quanzhou Normal University, Quanzhou 362000, China; phwu@[Link]
* Correspondence: liuli_phy@[Link] (L.L.); yizaomy@[Link] (Z.Y.); Tel.: +86-0816-2480830 (Z.Y.);
Fax: +86-0816-2480830 (Z.Y.)

Abstract: Perovskite solar cells (PSCs) still suffer from varying degrees of optical and electrical losses.
To enhance the light decoupling and capture ability of Planar PSCs, an ultra-thin PSC structure with an
Al2 O3 pyramid anti-reflection layer (Al2 O3 PARL) is proposed. The effect of the structure of the Al2 O3
PARL on the photoelectric performance of PSCs was investigated by changing various parameters.
Under the AM1.5 solar spectrum (300–800 nm), the average light absorption rates and quantum
efficiency (QE) of PSCs containing pyramid-array textured rear layers (PARLs) were significantly
higher than those of planar PSCs. The Al2 O3 PARL-based PSCs achieved a light absorption rate of
96.05%. Additionally, electrical simulations were performed using the finite element method (FEM)
Citation: Liu, L.; Liu, W.; Fu, W.; to calculate the short-circuit current density (JSC ), open-circuit voltage (VOC ), and maximum power
Yi, Z.; Yi, Y.; Zhang, J.; Tang, C.; (Pmax). Based on the maximum value of the average light absorbance, the geometric structure of
Sun, T.; Zeng, Q.; Wu, P. Enhancing the Al2 O3 pyramid PSCs was optimized, and the optimization results coincided with the JSC and QE
the Overall Performance of Perovskite results. The results of the electrical simulation indicated that the maximum JSC was 23.54 mA/cm2 .
Solar Cells with a Nano-Pyramid Additionally, the JSC of the Al2 O3 pyramid PSCs was 22.73% higher than that of planar PSCs, resulting
Anti-Reflective Layer. Photonics 2024, in a photoelectric conversion efficiency (PCE) of 24.34%. As a result, the photoelectric conversion
11, 715. [Link]
rate of the solar cells increased from 14.01% to 17.19%. These findings suggest that the presence
photonics11080715
of the Al2 O3 PARL enhanced photon absorption, leading to an increase in electron–hole pairs and
Received: 30 May 2024 ultimately improving the photocurrent of the solar cells.
Revised: 27 July 2024
Accepted: 28 July 2024 Keywords: perovskite solar cells; pyramid structure; photoelectric conversion efficiency; solar
Published: 31 July 2024 energy absorption

Copyright: © 2024 by the authors.

1. Introduction
Licensee MDPI, Basel, Switzerland.
This article is an open access article Perovskite materials are different from other common semiconductor materials; they
distributed under the terms and have stronger optoelectronic performance, with advantages including a high light absorp-
conditions of the Creative Commons tion coefficient, adjustable diffusion length, low processing cost, and so on, attracting a lot
Attribution (CC BY) license (https:// of photovoltaic field scholars’ and industrial researchers’ attention [1–6]. However, when
[Link]/licenses/by/ sunlight enters from one medium into another medium, according to the Fresnel reflection
4.0/). principle, a reflection occurs at the interface between the two media, and the greater the

Photonics 2024, 11, 715. [Link] [Link]

Photonics 2024, 11, 715 2 of 14

difference in refractive index between the two media, the stronger the reflection will be.
We know that there is a certain degree of optical loss in the existing perovskite solar cells
(PSCs), and the light absorption efficiency is low, seriously restricting the energy efficiency
improvement [7,8]. At the same time, due to the high optical loss, the perovskite light
absorption layer cannot absorb enough photons, thus cannot generate enough electron–
hole pairs, limiting the electrical performance. In existing research [9,10], many scholars
have added a high-performance anti-reflection film to the transparent substrate of PSCs.
The presence of the anti-reflection film enables solar cells to achieve broadband absorp-
tion, thus effectively improving the PCE. It also effectively isolates solar cells from the
external environment, reducing the impact of wind and rain on solar cells and minimizing
losses [11]. Al2 O3 material has a refractive index of about 1.62 in the visible light region,
and it is often used with MgF2 and ZrO2 to coat the visible light region of the anti-reflection
film. Generally, physical vapor deposition (PECVD) or solution-based methods are used to
prepare Al2 O3 thin films, ensuring the selection of high-purity precursor materials [12,13].
During PECVD, deposition temperature, gas flow rates, and deposition time were con-
trolled to achieve obtain uniform and dense Al2 O3 films. These methods can control the
thickness and morphology of the film to achieve optimal antireflection effects. Traditional
materials such as TiO2 and SnO2 exhibit good transparency in the visible light range, but
their electron transport properties are relatively poor. This can lead to recombination of
electron–hole pairs, thereby reducing solar cell efficiency. Additionally, some traditional
materials are sensitive to humidity and oxygen, which can lead to degradation and impact
solar cells’ lifespan. In summary, the Al2 O3 pyramid structure holds potential as a novel
antireflection coating material for solar cells, but further research and optimization are still
needed. Al2 O3 has excellent corrosion resistance, wear resistance, and heat resistance, with
both very high surface stability and excellent adhesion, and it can be closely combined with
glass substrate, giving it excellent optical performance, making it an ideal anti-reflection
film material. In addition, texturing the Al2 O3 anti-reflection film can further enhance light
capture efficiency, thereby improving light absorption. Texturing can involve a variety of
different nanostructures, including but not limited to nanowires [14,15], nanorods [16,17],
nanocones [18,19], nanoholes [19,20], and so on. Compared with the above nanostruc-
tures, nanopyramids have smaller surface recombination, more suitable for solar cells. The
nanopyramid Al2 O3 anti-reflection film significantly enhances light absorption in the solar
cell, thereby boosting energy conversion efficiency [21–23]. Incident light interacting with
different positions of the Al2 O3 pyramid structure experiences varying refractive indices,
known as the refractive index gradient effect. This effect enhances light capture efficiency
and accentuates the cone profile [24]. The side walls of the Al2 O3 pyramid structure create
multiple light-scattering effects, increasing the path length of photons within the active
layer, which enhances light capture. Based on this understanding of the anti-reflection
performance of the Al2 O3 pyramid structure, we integrated this structure into planar PSCs
to reduce optical losses and enhance light capture capability [25].
This paper proposes PSCs based on an Al2 O3 pyramid anti-reflection layer structure
(Al2 O3 PARLs). The change of the optoelectronic performance of the designed cells under
different geometric parameters of Al2 O3 PARLs was studied. When the Al2 O3 pyramid
height h = 200 nm, bottom length d = 200 nm, the performance of the solar cell was the best,
and its PCE increased to 17.19%. Comparing these structural parameters with the planar
PSCs, the comparison results revealed that the Al2 O3 pyramid PSCs on the surface had an
average light absorption of 96.05%, much higher than the planar PSCs. Al2 O3 PARLs had
the effect of reducing the reflectivity, improving the PSCs’ light absorption and quantum ef-
ficiency (QE). According to the calculated electric field intensity distribution map, the Al2 O3
pyramid structure had a strong light coupling effect, corresponding to its light absorption
results. Through electrical simulation, the maximum short-circuit current density of this
Al2 O3 pyramid PSCs was found to be 23.54 mA/cm2 , increasing by 4.36 mA/cm2 compared
with the planar PSCs’ short-circuit current density of 19.18 mA/cm2 , and the PCE increased
from 14.01% to 17.19%. The calculation results will be useful for developing and manufac-
Photonics 2024, 11, 715 3 of 14

turing the next generation of high-efficiency solar cells, providing detailed guidance for
PSCs with energy conversion efficiency.

2. Model Structure
Figure 1a shows the high-efficiency planar single-junction PSCs we designed. The
structure from top to bottom was a 200 nm thick FTO/glass substrate, a 150 nm thick TiO2
electron transport layer (ETL), and a 500 nm CH3 NH3 PbI3 perovskite active layer, placed
on a 250 nm Spiro-OMeTAD hole transport layer (HTL). Finally, 100 nm thick Au was
used as the electrode to complete this planar single-junction PSC. All geometric parameters
were optimized based on FDTD software (FDTD 8.15.736) [26–28]. Figure 1b illustrates
the energy band diagram of carrier transport in the designed PSC, wherein the contact
between each layer exhibits a gradient increasing band gap. This configuration ensured
favorable valence band matching, provided a nearly constant VOC , and enhanced the FF
by facilitating carrier transport and reducing the loss of carrier complexes in the absorber
layer. The planar PSC design shown in Figure 1a does not allow enough photons to be
absorbed in the active CH3 NH3 PbI3 layer, resulting in corresponding reflection losses. To
enhance the light decoupling and light capture capabilities of these planar PSCs, this paper
proposes PSCs with an Al2 O3 PARL structure based on the designed planar PSCs, as shown
in Figure 1c. Figure 1d shows a section of the designed model. In this design, the PSC
surface is textured with an Al2 O3 pyramid anti-reflection film with a length-to-width ratio
of 1(d = w) and a height of h, as shown in Figure 1e, using additional means to optimize
light decoupling and light capture, providing an effective structure for optimizing photon
management of single-junction PSCs. Since the metal oxide Al2 O3 has a refractive index
comparable with perovskite materials, when the incident light propagates from the air
medium to the solar cell, this Al2 O3 pyramid can serve as a refractive index gradient.
The incident light produces different refractive indices at different positions of the Al2 O3
pyramid structure. When the equivalent refractive index curve of the Al2 O3 pyramid
gradually increases from top to bottom, the gradient change of the refractive index with the
surrounding air gradually decreases, thereby reducing the reflectance of the incident light.
Using this gradient refractive index characteristic of the Al2 O3 pyramid, we can reduce the
reflectance of the PSCs in the wide band from 300 nm to 800 nm, thereby improving the light
absorption efficiency. In the optical simulation stage, we used the finite-difference time-
domain method (FDTD) to study the optical properties of the planar PSCs and the PSCs
with the Al2 O3 PARL structure. Due to its high accuracy and wideband frequency coverage,
Lumerical FDTD is one of the most suitable commercial software tools for detecting the
optical performance of optoelectronic devices [29,30]. The complex refractive index of the
material obtained from the experiment was used as the optical simulation parameter input
to the FDTD material library [31,32]. In FDTD, we set the wavelength range to between
300 nm and 800 nm, and the plane wave incident perpendicular to the PSCs surface. The
wave source was placed in the air, and periodic boundary conditions were set in the X-
axis and Y-axis directions, so that periodicity was established in the entire designed PSC
structure. To avoid parasitic emission and absorption of electromagnetic waves, we set the
boundary conditions along the Z-axis direction to be a perfect matching layer (PML). In all
simulation cases, the grid size was 5 nm. Through FDTD optical simulation, the generated
electron–hole pairs were used as optical inputs for finite element simulation, and then, the
photo-generated carrier rate was simulated via finite element method (FEM) technology
for electrical simulation [33,34]. For the electrical simulation, we calculated the electronic
parameters of the materials used from the literature [35,36].
Photonics 2024,
Photonics 2024,11,
11,715
x FOR PEER REVIEW 44 of 15
of 14

Figure 1.
Figure 1. (a) Diagram of planar PSCs; (b) energy band
band diagram
diagram of
of carrier
carrier transport
transport in
in the
the designed
designed
PSCs; (c) diagram of Al O pyramid PSCs; (d) part of the structure; (e) the dimensional details
PSCs; (c) diagram of Al2 O3 pyramid PSCs; (d) part of the structure; (e) the dimensional details of one
2 3 of
one pyramid of the Al2O3 PARL (d:w = 1:1).
pyramid of the Al2 O3 PARL (d:w = 1:1).

In the FDTD
FDTD simulation
simulationphase,
phase,we weused
used plane
planewaves
waveswith wavelengths
with wavelengths between
between300
nm and 800 nm incident on the solar cell surface in the negative
300 nm and 800 nm incident on the solar cell surface in the negative Z direction. Z direction. We used
used
periodic boundary
periodic boundary conditions
conditions in the the XX and
and YY directions
directions [37–39].
[37–39]. To
To eliminate
eliminate parasitic
parasitic
reflections and
reflections and absorption
absorption ofof electromagnetic
electromagnetic waves waves in the Z direction, we we used perfectly
suited layer
suited layer (PML) boundary
boundary conditions
conditions [40,41].
[40,41]. FDTD
FDTD cancan calculate
calculate the
the optical
optical power
power that
that
is absorbed
is absorbedon onaaper
perunit
unitvolume
volume basis
basis [42],
[42], which
which is defined
is defined by following
by the the following formula
formula [43]:
[43]:
Pabs = −0.5ω|E|2 Im{ε} (1)
Ρabs = −0.5ω|E| Im ε (1)
where
where EE isis the
the electric
electric field
field in
in the
the type,
type, the
the angular
angular frequency
frequency ofof the
the electromagnetic
electromagnetic wavewave
is the dielectric constant, and Im{ε} is the imaginary part of the dielectric constant. Under
is the dielectric constant, and Im{ε} is the imaginary part of the dielectric constant. Under
the AM1.5 solar spectrum, which was used to determine an important parameter of the
the AM1.5 solar spectrum, which was used to determine an important parameter of the
solar cells, namely JSC , the ideal JSC value can be calculated by the following formula under
solar cells, namely JSC, the ideal JSC value can be calculated by the following formula under
the assumption that every photon absorbed by the active layer generates an electron–hole
the assumption that every photon absorbed by the active layer generates an electron–hole
pair [44]:
pair [44]: Z 800nm
q
Jsc = λQE (λ)IAM1.5 λdλ (2)
2πh̄cq 300nm
J = λQ (λ) I . λd (2)
where Q is the charge of the electron, 2πℏc λ is the wavelength of the light source, C is the
speed
where ofQ islight
the in a vacuum,
charge QE (λ) is λthe
of the electron, QE wavelength
is the of the solar of
cells
thein thesource,
light formula,
C isand
the Ispeed
AM1.5
represents the solar irradiance under AM1.5. The following formula expresses
of light in a vacuum, QE(λ) is the QE of the solar cells in the formula, and IAM1.5 represents the amount
of
thephotogenerated
solar irradiancecarriers per unitThe
under AM1.5. volume [45]: formula expresses the amount of photo-
following
generated carriers per unit volume [45]:
Pabs 0.5Im{ε}
G= =− (3)
Pabs
2Πh̄ω 0.5Im
h̄ ε
G= =− (3)
2Πℏωand 2πω ℏis the corresponding frequency of
where h̄ is the reduced Planck’s constant
photon energy. G, the total number of photogenerated carriers [46], is integrated over the
Photonics 2024, 11, 715 5 of 14

entire range and depends on frequency and space. According to the relevant physical
theory expressed in the formula, we calculated the photogenerated charge carriers using
the FDTD software (FDTD 8.15.736) which were then imported into the Comsol software
(Comsol [Link]) for the electrical simulations. With the support of this theory, we obtained
the JSC , VOC , Pmax, and other electrical parameters of the solar cells.
In order to measure the actual photovoltaic performance of the solar cells, electrical
simulation of the designed solar cells was carried out using the finite element method to
determine the various electrical parameters of the calcium titanite solar cells, such as JSC ,
VOC , fill factor, and photovoltaic conversion efficiency. In the finite element method, a geo-
metrical model of the designed solar cells was first created, the material parameters of the
modeling region, boundary conditions, scanning voltages, and mesh size dimensions were
defined and finally, the simulation was run. Electrical simulations were performed using
the finite element method and the device characteristics were controlled by semiconductor
equations, including nonlinear Poisson, continuity, and drift-diffusion equations. Four
types of composite mechanisms were also considered in the electrical simulations [47]:
 
Rrad = B np − n2i (4)

 
RAug = nCn + pCp np − n2i (5)

np − n2i
RSRH = (6)
τp (n + nt ) + τn (p + pt )
np − n2i
RSurf = 1 1

(7)
Sp (n + nts ) + Sn p + ps

where Rrad is radiation recombination, RAug is non-radiative recombination, i.e., Auger

recombination, RSRH is Shockley–Read–Hall recombination, and RSurf is surface recombina-
tion, B is the radiation recombination coefficient, Cn is the electron Auger recombination
coefficient, CP is the hole Auger recombination coefficient, τn and τp are the lifetimes of
electrons and holes, respectively, Sn and Sp are the surface recombination velocities of elec-
trons and holes, respectively, and ni is the intrinsic carrier concentration. Through FDTD
optical simulation, the generated electron–hole pairs were used as optical inputs for the
finite element simulation, which was able to accurately simulate the electrical performance
of the solar cell devices. The generation rates of electrons and holes remained constant at
the total generation rate:
Gtotal = Gn = Gp (8)
In addition, the basic electronic properties of the materials were also used in the
calculations. Based on the above formulas, the electrical characteristics of the solar cells
were calculated using the finite element technology, and the light absorption curve, QE
curve, and various electrical simulation data of the PSCs were obtained.

3. Results and Analysis

The Al2 O3 PARLs were able to effectively reduce the reflection of solar energy and
increase the light transmission rate in the PSCs. According to the gradient refractive index
effect, different base and height ratios of the pyramid led to different anti-reflection effects,
and the light absorption in the PSCs was different [48]. In order to study the specific
optical properties of the PSCs with the Al2 O3 PARLs, we studied the changes in the optical
properties of the PSCs designed with different Al2 O3 PARLs. First, we fixed the bottom
width d = 200 nm of the Al2 O3 pyramid structure and explored the effect of different
heights h on the light absorption rate of the designed PSCs, as shown in Figure 2a. The light
absorption curve results showed that in the entire wavelength range we calculated, when
the height of the Al2 O3 pyramid was 100 nm, the light absorption rate of the designed
PSCs was the lowest. As the height of the Al2 O3 pyramid increased, the light absorption
 heights h on the light absorption rate of the designed PSCs, as shown in Figure 2a. The
Photonics 2024, 11, 715 light absorption curve results showed that in the entire wavelength range we calculated,
6 of 14
when the height of the Al2O3 pyramid was 100 nm, the light absorption rate of the de-
signed PSCs was the lowest. As the height of the Al2O3 pyramid increased, the light ab-
sorption of the PSCs gradually increased and stabilized. The light absorption rates of the
of the PSCs gradually increased and stabilized. The light absorption rates of the Al2 O3
Al2O3 pyramid at 200 nm, 300 nm, and 400 nm were not much different. This is because
pyramid at 200 nm, 300 nm, and 400 nm were not much different. This is because when
when the height of the Al2O3 pyramid increased to a certain level, the light absorption of
the height of the Al2 O3 pyramid increased to a certain level, the light absorption of the
the PSCs
PSCs reached
reached its limit,
its limit, andand
the the overly
overly high high
Al2Al
O23Opyramid
3 pyramid hindered a small part of the
hindered a small part of the
light absorption [49]. Figure 2b explores the average
light absorption [49]. Figure 2b explores the average light lightabsorption
absorptionof ofthe
thedesigned
designedPSCs
PSCs
calculated under different Al 2O3 pyramid structure heights h. In addition, it is apparent in
calculated under different Al2 O3 pyramid structure heights h. In addition, it is apparent
Figure
in Figure2b2b that from
that from 100
100nmnmto to
200 nm,
200 nm,as as
thethe
height
heightof of
thethe
Al2Al
O3 O
pyramid increased, the
2 3 pyramid increased,
average light absorption rate increased from 87.42%
the average light absorption rate increased from 87.42% to 96.05%, butto 96.05%, but when the height
when h of
the height
the Al 2O3 pyramid increased to 300 nm or 400 nm, the average light absorption of the solar
h of the Al2 O3 pyramid increased to 300 nm or 400 nm, the average light absorption of
cellsolar
the gradually began tobegan
cell gradually decrease. From Figure
to decrease. From2,Figure
we can2,conclude that when
we can conclude thewhen
that height
theh
of the Al 2 O 3 PARLs was 200 nm, the average light absorption rate of
height h of the Al2 O3 PARLs was 200 nm, the average light absorption rate of the solarthe solar cell was the
largest
cell wasatthe 96.05%.
largestThis shows that
at 96.05%. Thisasshows
the thickness
that as theof the Al2O3 pyramid
thickness of the Al2increased,
O3 pyramid the
light absorption
increased, the light ofabsorption
the solar cell increased
of the with
solar cell the increase
increased in thickness
with the and
increase in then gradu-
thickness and
ally decreased.
then gradually decreased.

[Link]
Figure Atdifferent
differentheights
heightsof
ofthe
theAlAl22O
O33 pyramid,
pyramid, (a)
(a) the
the absorption
absorption spectra
spectra of
of the
the designed
designed cells;
cells;
(b) the average light absorbance of the designed cells.
(b) the average light absorbance of the designed cells.

ToTofurther
furtherexplore
explore the
the optical
optical performance
performance of2Al
of Al O32O 3 pyramid
pyramid PSCs,
PSCs, we also
we also studied
studied the
effect of different bottom side lengths of the
the effect of different bottom side lengths of2 the Al O pyramids on the optical performance
3 Al2O3 pyramids on the optical perfor- of
the designed
mance of thePSCs. Figure
designed 3a shows
PSCs. Figurethat as the that
3a shows bottom side
as the lengthside
bottom d oflength
the Ald 2Oof3 pyramid
the Al2O3
increased from 40 nm
pyramid increased to 200
from nm,to
40 nm the200
light
nm,absorption of the solarofcell
the light absorption thegradually
solar cellincreased;
gradually
however,
increased;when
Photonics 2024, 11, x FOR PEER REVIEW
d increased
however, when dfrom 200 nm
increased to 280
from 200 nm,
nm to the280
light
nm,absorption of the solar
the light absorption cell15
7ofofthe
decreased. Figure 3b shows
solar cell decreased. Figure more clearly
3b shows morethatclearly
when the
thatbottom
when thesidebottom
lengthside
d of length
the Al2dOof 3
pyramid was 200 nm, the average light absorption of the solar cell was at
the Al2O3 pyramid was 200 nm, the average light absorption of the solar cell was at its its highest.
highest.

[Link]
Figure Atdifferent
differentbottom
bottomside
sidelengths
lengthsofofthe
theAl
Al2 O
2O33 pyramid,
pyramid, (a)
(a)the
theabsorption
absorptionspectra
spectraof
ofPSCs;
PSCs;
(b)
(b)the
theaverage
averagelight
lightabsorption
absorptionrate
rateofofthe
thePSCs.
PSCs.

Electrical
Electricalperformance
performanceisisananimportant
importantindicator of of
indicator solar cells
solar [50,51].
cells In In
[50,51]. order to better
order to bet-
reveal the photoelectric performance of Al2 O 3 pyramid PSCs, we used the finite
ter reveal the photoelectric performance of Al2O3 pyramid PSCs, we used the finite ele- element
ment method (FEM) to simulate the electrical performance of cells with different Al2O3
PARL parameters. The specific electrical performance parameters of the solar cells at dif-
ferent Al2O3 pyramid heights are shown in Table 1, below. These results were consistent
with the absorption. As shown in Figure 4a, illustrating the J-V curves, we explored the
changes in JSC of the solar cells with different Al2O3 pyramid heights. In the figure, ‘Planar’
Photonics 2024, 11, 715 7 of 14

method (FEM) to simulate the electrical performance of cells with different Al2 O3 PARL
parameters. The specific electrical performance parameters of the solar cells at different
Al2 O3 pyramid heights are shown in Table 1, below. These results were consistent with the
absorption. As shown in Figure 4a, illustrating the J-V curves, we explored the changes in
Figure
JSC of the3. solar
At different bottom
cells with side lengths
different Al2 O3ofpyramid
the Al2O3heights.
pyramid,In(a) thefigure,
the absorption spectra
‘Planar’ of PSCs;
represents
a(b) the average
perovskite lightcell
solar absorption
withoutrate
Al2ofOthe
3
PSCs. From Figure 4a, it can be clearly seen that
PARLs.
the JSC of the PSCs without Al2 O3 PARLs was the lowest at 19.18 mA/cm2 . When the
heightElectrical
of the Alperformance is an important indicator of solar cells [50,51]. In order to bet-
2 O3 pyramid increased from 100 nm to 200 nm, the JSC increased from
ter reveal the 2 photoelectric
21.48 mA/cm to 23.54 mA/cm performance
2 , because asof Alheight
the 2O3 pyramid PSCs, we used the finite ele-
of the Al2 O3 pyramid increased, the
anti-reflection performance of the Al2 O3 pyramidperformance
ment method (FEM) to simulate the electrical also increased of [52].
cellsWhen
with different
the heights Al2ofO3
PARL parameters. The specific electrical performance parameters
the Al2 O3 pyramid were 200 nm, 300 nm, and 400 nm, the J-V curves of the solar cells almost of the solar cells at dif-
ferent Al2O
coincided, 3 pyramid heights are shown in Table 1, below. These results were consistent
indicating that as the height of the Al2 O3 pyramid increases, the JSC of the solar
with
cell nothe absorption.
longer increased. AsThe
shown in Figure
calculation 4a, showed
results illustrating
thatthe
whenJ-Vthecurves,
heightwe explored
h of the Al2 Othe
3
changes in J of the solar cells with different Al O pyramid
pyramid was 200 nm, the JSC of the designed cell was the largest, JSC = 23.54 mA/cm
SC 2 3 heights. In the figure, ‘Planar’
2 . As
represents
shown a perovskite
in Figure solarcurves
4b, the P-V cell without Al2O3 PARLs.
was basically the sameFrom Figure
as the 4a, it can
J-V curves be clearly
at different
seen that the J
Al2 O3 pyramid [Link] of the PSCs without Al 2O 3 PARLs was the lowest at 19.18 mA/cm 2. When

the height of the Al2O3 pyramid increased from 100 nm to 200 nm, the JSC increased from
[Link]/cm
Table to 23.54 mA/cm
Specific2 Electrical 2, because as the height of the Al2O3 pyramid increased, the
Performance Parameters of Cells with Different Al2O3 Pyramid Heights.
anti-reflection performance of the Al2O3 pyramid also increased [52]. When the heights of
2
the Al2H O3(nm)
pyramid were 200Vnm, OC (V)300 nm, and 400 nm, the )J-V curves ofPCE
JSC (mA/cm the(%)solar cells
almost Planar
coincided, indicating that 0.89as the height of the Al2O3 pyramid increases,
19.18 14.01 the JSC of
the solar100 cell no longer increased. 0.89 The calculation results 21.48 showed that when 15.50
the height h
200 0.90 23.54
of the Al2O3 pyramid was 200 nm, the JSC of the designed cell was the largest, 17.19 JSC = 23.54
300 0.90 23.41 17.06
mA/cm2. As shown in Figure 4b, the P-V curves was basically the same as the J-V curves
400 0.90 23.32 16.98
at different Al2O3 pyramid heights.

Figure4.4.(a,b)
(a,b)the
theJ-V
J-Vcurves
curvesand
andP-V
P-Vcurves
curvesofofthe
thedesigned
designedPSCs
PSCswith
withdifferent
different heights
heights ofof
AlAl2O 3
Figure 2 O3
pyramids, respectively (d = w = 200
pyramids, respectively (d = w = 200 nm). nm).

Table 1. Specific
Figure 5a,b,Electrical Performance
respectively, Parameters
show the of Cells
J-V curves andwith
P-VDifferent Al2O3
curves of Pyramid Heights.
the designed PSCs
when theHbottom
(nm) side length dV ofOCthe
(V)surface Al2 O3JSC
pyramid
(mA/cmwas
2) 40 nm, 120
PCEnm, 200 nm,
(%)
and 280 nm (the height of the Al2 O3 pyramid was fixed at 200 nm). The curve results
Planar 0.89 19.18 14.01
showed that under the Al2 O3 PARLs, when the bottom side length d = 200 nm, the max-
100 0.89 21.48 15.50
imum short-circuit current density was 23.54 mA/cm2 . When d = 40 nm, the minimum
200 0.90 23.54 2 17.19
short-circuit current density of the solar cell was 20.67 mA/cm . The corresponding P-V
curves and J-V curves showed that when d = 200 nm, the maximum electrical power of
the designed solar cell was 17.19 mW/cm2 . When the bottom side length of the Al2 O3
pyramid increased from 40 nm to 80 nm to 200 nm, the maximum electrical power showed
a tendency to increase and then decrease. From Tables 1 and 2, it can be seen that when the
Al2 O3 PARLs had dimensions of h = 200 nm, d = 200 nm, the JSC of the designed PSCs was
23.54 mA/cm2 and the electrical power was 17.19 mW/cm2 ; at this time, the photoelectric
performance of the solar cells was at its best, and the anti-reflection effect of the Al2 O3
structure was at its best.
 increased from 40 nm to 80 nm to 200 nm, the maximum electrical power showed a ten-
dency to increase and then decrease. From Tables 1 and 2, it can be seen that when the
Al2O3 PARLs had dimensions of h = 200 nm, d = 200 nm, the JSC of the designed PSCs was
23.54 mA/cm2 and the electrical power was 17.19 mW/cm2; at this time, the photoelectric
Photonics 2024, 11, 715
performance of the solar cells was at its best, and the anti-reflection effect of the 8Al
of 14
2O3

structure was at its best.

Figure5.5.(a,b)
Figure (a,b)J-V
J-Vand
andP-V
P-Vofofthe
thedesigned
designedsolar
solarcells
cellsatatdifferent
differentbottom
bottomside
sidelengths
lengthsofofthe
theAlAl
2O2O
33
pyramid,respectively.
pyramid, respectively.

[Link]
Table Specificparameters
parametersof
ofthe
theelectrical
electricalperformance
performanceof
ofcells
cellswith
withdifferent
differentbottom
bottomedge
edgelengths
lengths
of Al2O3 pyramid.
of Al2 O3 pyramid.
d (nm) VOC (V) JSC (mA/cm2) PCE (%)
d (nm) VOC (V) JSC (mA/cm2 ) PCE (%)
Planar 0.89 19.18 14.01
Planar 0.89 19.18 14.01
40 0.89 20.68 14.67
40 0.89 20.68 14.67
120
120 0.89
0.89 21.42
21.42 15.44
15.44
200
200 0.90
0.90 23.54
23.54 17.19
17.19
280
280 0.90
0.90 22.81
22.81 16.52
16.52

We
Weknow
knowthat
thatthe
thePSCs
PSCsdesigned
designedwithwiththetheAlAl2 O
2O33 PARLs
PARLs had hadthe
thebest
bestphotoelectric
photoelectric
performance when the height h = 200 nm and the bottom side
performance when the height h = 200 nm and the bottom side length d = 200 length d = 200 [Link],
There-
under the parameters of h = 200 nm and d = 200 nm, we compared
fore, under the parameters of h = 200 nm and d = 200 nm, we compared the photoelectric the photoelectric
characteristics
characteristics of planar PSCs
of planar PSCsandandAlAl
2O23Opyramid
3 pyramid [Link]. In FDTD,
In FDTD, we calculated
we calculated the
the reflec-
reflection
tion (R) and(R)absorption
and absorption (A) spectra
(A) spectra of twoofdifferently
two differently structured
structured cells,
cells, as shownas shown in
in Figure
Figure 6a. These two structures are marked as the ‘planar structure’ and
6a. These two structures are marked as the ‘planar structure’ and ‘Al2O3 pyramid’ in Fig- ‘Al 2 O 3 pyramid’
in Figure
ure 6a. The
6a. The ‘planar
‘planar structure’
structure’ represents
represents a aplanar
planarPSCsPSCswithout
without AlAl22OO33 PARLs,
PARLs, andand the
the
‘Al 2 O 3 pyramid’ represents a perovskite solar cell with an Al 2 O 3 PARL
‘Al2O3 pyramid’ represents a perovskite solar cell with an Al2O3 PARL structure. Figurestructure. Figure 6a
indicates that the PSCs with the Al2 O3 PARLs significantly reduced the reflectivity within
6a indicates that the PSCs with the Al2O3 PARLs significantly reduced the reflectivity
the wavelength range of 300 nm to 800 nm, which in turn enhanced absorption; the Al2 O3
within the wavelength range of 300 nm to 800 nm, which in turn enhanced absorption; the
pyramid had an anti-reflection effect on the entire solar cell, and the overall light capture
Al2O3 pyramid had an anti-reflection effect on the entire solar cell, and the overall light
ability of the solar cell was greatly improved compared with the traditional ‘planar structure’
PSCs. It was observed that within the wavelength range of 300 nm to 800 nm, the light
absorption rate of the Al2 O3 pyramid was basically above 90%, while the light absorption of
the planar structure was basically below 90%. This is because the Al2 O3 pyramid structure
on the surface of the solar cell was able to significantly reduce the reflectivity of the solar cell,
enhance the light capture ability of the solar cell, and improve the light absorption of the
solar cell [53,54]. In order to further compare the optical performance of the two structures
of PSCs, we compared the light absorption efficiency of planar and Al2 O3 pyramid PSCs
under the AM 1.5 solar spectrum, as shown in Figure 6b. In Figure 6b, it can be seen
that in the entire region of 300–800 nm, the average absorption rate of the Al2 O3 pyramid
structure reached 96.05%, while the average absorption rate of the planar structured cell
was 87.41%, with the former increasing the average light absorption rate by 8.64%. The
spectral absorption curve of the Al2 O3 pyramid structure basically coincided with the solar
energy spectrum at AM 1.5, indicating that the Al2 O3 PARLs improved the light absorption
of the PSCs in the visible light band [55].
 ure 6b, it can be seen that in the entire region of 300–800 nm, the average absorption rate
of the Al2O3 pyramid structure reached 96.05%, while the average absorption rate of the
planar structured cell was 87.41%, with the former increasing the average light absorption
rate by 8.64%. The spectral absorption curve of the Al2O3 pyramid structure basically co-
Photonics 2024, 11, 715 incided with the solar energy spectrum at AM 1.5, indicating that the Al2O3 PARLs 9 ofim-
14
proved the light absorption of the PSCs in the visible light band [55].

Figure6.6.(a)
Figure (a)The
Theabsorption
absorptionand
andreflection spectra
reflection of of
spectra thethe
Al2Al
O23Opyramid; (b)(b)
3 pyramid; thethe
comparison
comparisonchart of
chart
of the
the absorption
absorption spectra
spectra of planar
of planar andand O32O
Al2Al 3 pyramid
pyramid structures
structures under
under thethe
AM AM1.51.5 solar
solar spectrum.
spectrum.

QE
QE isis another
another important
important parameter
parameter to to characterize
characterize the the optical
optical performance of PSCs.
We
Wealso
alsocalculated
calculatedthe theQEQEdiagrams
diagramsof ofthe
thetwotwostructures
structuresand andthe thecorresponding
corresponding integral
integral
currents.
currents. Figure
Figure 7a 7a provides
provides thetheQEQEcurves
curvesand andintegral
integralcurrents
currentsof ofthe
thePSCs
PSCswith
withAl Al2 O
2O33
pyramids in comparison with planar PSCs. It was observed
pyramids in comparison with planar PSCs. It was observed that the two structures that the two structures showed
substantial differences
showed substantial in QE andin
differences integral
QE and current.
integralThe QE of The
current. the planar structure
QE of the planarwas much
structure
lower than that of
was much lower than thatthe Al O pyramid structure. The integral current value
2 3of the Al2O3 pyramid structure. The integral current value of of the planar
structure
the planarwas also smaller
structure was alsothan that of
smaller thethat
than Al2 O pyramid
of3 the [Link].
Al2O3 pyramid This result
Thisfurther
result
verifies
further that the light
verifies that capture
the light ability
captureof the structure
ability of the with Al2 O3 pyramids
structure with Al2Owas greater than
3 pyramids was
that of the
greater planar
than that structure [56,57].
of the planar In order
structure to better
[56,57]. compare
In order the electrical
to better comparecharacteristics
the electrical
of the two structures of PSCs, we used the finite element
characteristics of the two structures of PSCs, we used the finite element method to method
performtoelectrical
perform
simulation on the designed
electrical simulation on thecells. As shown
designed cells. Asin the
shownJ-V curves
in2 the inJ-VFigure
curves7b,
inthe VOC7b,
Figure of the
the
planar structure was 0.89 V,
VOC of the planar structure was 0.89and its J was 19.18 mA/cm . The short-circuit
SC V, and its JSC was 19.18 mA/cm2. The short-circuit current of the
J-V and the
current integral
of the J-V andcurrent of the QE
the integral wereof
current foundthe QE to be
werein close
found proximity to one
to be in close another
proximity
and aligned with the QE results. The VOC of the Al2 O3 pyramid structure was 0.90 V, and
to one another and aligned with the QE results. The VOC of the Al2O3 pyramid structure
its JSC was 23.54 mA/cm2 . By establishing the surface Al2 O3 PARLs, the JSC of the solar
was 0.90 V, and its JSC was 23.54 mA/cm 2. By establishing the surface Al2O3 PARLs, the JSC
cell was increased by 4.36 mA/cm2 . The above data prove that the Al2 O3 pyramid PSCs
of the solar cell was increased by 4.36 mA/cm2. The above data prove that the Al2O3 pyra-
had greatly improved short-circuit current density due to their significant anti-reflection
mid PSCs had greatly improved short-circuit current density due to their significant anti-
benefits. In the P-V curve shown in Figure 7c, the Pmax of the planar structure PSCs is
reflection benefits. In the P-V curve shown in Figure 7c, the Pmax of the planar structure
14.01 mW/cm2 , and the Pmax of the Al O pyramid structure is 17.19 mW/cm2 . Therefore,
PSCs is 14.01 mW/cm2, and the Pmax2 of3 the Al2O3 pyramid structure is 17.19 mW/cm
Photonics 2024, 11, x FOR PEER REVIEW 10 of 152.
the PSCs with Al2 O3 pyramids had a higher short-circuit current density and higher Pmax
Therefore, the PSCs with Al2O3 pyramids had a higher short-circuit current density and
compared with the planar PSCs.
higher Pmax compared with the planar PSCs.

Figure 7.
Figure 7. Diagrams
Diagrams of
ofresults
resultsfor
forplanar
planarand
andAl
Al22O
O33 pyramid
pyramid structures:
structures: (a)
(a) QE
QE curves
curves and
and integral
integral
current;(b)
current; (b)J-V
J-Vcurves;
curves;(c)
(c)P-V
P-Vcurves.
curves.

Generally
Generally speaking, in inorder
ordertotobetter
betterinterpret
interpret thethe optical
optical properties
properties of aofdevice,
a device,
it is
itnecessary
is necessary to model
to model its associated
its associated electromagnetic
electromagnetic fields fields [58–60].
[58–60]. Here, in Here,
orderin to
order
under-to
understand more clearly
stand more clearly the propagation
the propagation of incident
of incident lightthe
light inside inside
solarthe solar
cells cells
before before
and after
and after the assembly
the assembly of the Al2O of3 PARLs,
the Al2 O 3 PARLs,
Figure 8a–fFigure 8a–f
illustrate illustrate
the the electric
electric field field
intensity inten-
distribu-
sity
tiondistribution
of solar cellsof solar
with andcells with Al
without and
2O3without
PARLs at Aldifferent
2 O3 PARLs at different
wavelengths (λ wavelengths
= 300 nm, 410
(λ
nm,= 300
andnm,
700410 nm,
nm). and 700
Among nm).Figure
them, Among them,
8a–c Figure the
represent 8a–cinternal
represent the internal
electric electric
field intensity
distribution of the planar PSCs. Figure 8d–f show the internal electric field intensity dis-
tribution of the Al2O3 pyramid PSCs. Comparing the electric field intensity distribution
between the two can indirectly explain the increase in the light absorption rate. For the
electric field intensity distribution diagram, we chose the middle position in the X–Z
plane. From Figure 8a–c, it can be seen that the planar PSCs induced the Fabry–Perot in-
Photonics 2024, 11, 715 10 of 14

field intensity distribution of the planar PSCs. Figure 8d–f show the internal electric field
intensity distribution of the Al2 O3 pyramid PSCs. Comparing the electric field intensity
distribution between the two can indirectly explain the increase in the light absorption
rate. For the electric field intensity distribution diagram, we chose the middle position
in the X–Z plane. From Figure 8a–c, it can be seen that the planar PSCs induced the
Fabry–Perot interference effect, responding to the electric field intensity as a striped pattern
distributed along the Z-axis direction [61–63]. Compared with the planar PSCs, the Al2 O3
PARLs enhanced the electric field intensity inside the perovskite light-absorbing layer,
characterized by two bright local points at the edge of the model, as can be seen from
Figure 8d–f. At λ = 300 nm, the electric field distribution of the planar PSCs was completely
different from the electric field distribution of the perovskite solar cells with Al2 O3 PARLs.
Compared with the planar PSCs, the electric field intensity distribution on both sides and
the inside of the top Al2 O3 pyramid of the perovskite solar cells with Al2 O3 PARLs was
higher. There was no high electric field in the planar PSCs, and most of the spectral energy
was distributed in the FTO/glass layer at this wavelength. In addition, compared with
Figure 8b,e, under the Al2 O3 pyramid structure, part of the spectral energy penetrated into
the perovskite photosensitive layer. Comparing Figure 8c,f, in the Al2 O3 pyramid PSCs
in Figure 8f, except for the surroundings of the Al2 O3 pyramid structure, the stripe width
is almost the same as that in Figure 8c, but the electric field on both sides of the Al2 O3
pyramid structure is significantly enhanced. This shows that the Al2 O3 PARLs were able
to excite guided-mode resonance in the perovskite absorption layer, corresponding to the
periodic pattern of electric field intensity [64–66]. Therefore, due to the increase in the
number of quasi-guided mode couplings, the electric field intensity was enhanced. The
absorption of light is proportional to the electric field intensity, so the light absorption of
the Al2 O3 pyramid PSCs was higher, and the Al2 O3 pyramid greatly improved the light
absorption of the solar cells. In summary, the Al2 O3 pyramid structure can adjust light
coupling, has an anti-reflection effect, and has a good focusing effect on solar energy within
the visible light range [67–69]. The existence of the Al2 O3 pyramid structure enhances
Photonics 2024, 11, x FOR PEER REVIEW 11 of 15
photon absorption, thereby generating more electron–hole pairs, so with the final increase
in the photocurrent of solar cell, the overall performance of the solar cell is improved.

[Link]
Figure Fieldprofiles
profilesof
of|E|,
|E|, (a,d)
(a,d) planar
planarPSCs
PSCsand
andAl
Al22O
O33 pyramid
pyramid PSCs
PSCs at
at 300
300 nm;
nm; (b,e)
(b,e)planar
planar
PSCs and Al 2O3 pyramid PSCs at 410 nm; (c,f) planar PSCs and Al2O3 pyramid PSCs at 700 nm.
PSCs and Al2 O3 pyramid PSCs at 410 nm; (c,f) planar PSCs and Al2 O3 pyramid PSCs at 700 nm.

4.
4. Conclusions
Conclusions
In
Inthis
thispaper,
paper,wewepropose
proposeaaperovskite
perovskitesolar
solarcell
cellbased
basedon
onan
anAl
Al22O
O33 PARL
PARL structure,
structure,
with
withaatotal
totalthickness
thicknessofof1400
1400nm.
[Link]
analyzedthe theoptoelectronic
optoelectroniccharacteristics
characteristicsofofAl2O
Al 2O33
pyramid
pyramid PSCs
PSCs inin detail,
detail, and
and calculated
calculated the
the light
lightabsorption,
absorption, QE,
QE, and
andvarious
various electrical
electrical
parameters of the solar cells by changing various parameters of the Al2O3 PARLs, includ-
ing different heights and bottom lengths. Under the AM1.5 solar spectrum (300–800 nm),
the average light absorption rate of the optimized Al2O3 pyramid was 96.05%, which was
much higher than that of the planar structure. In addition, electrical simulation was car-
ried out using the finite element method, and the JSC, VOC, and Pmax were calculated.
Photonics 2024, 11, 715 11 of 14

parameters of the solar cells by changing various parameters of the Al2 O3 PARLs, including
different heights and bottom lengths. Under the AM1.5 solar spectrum (300–800 nm), the
average light absorption rate of the optimized Al2 O3 pyramid was 96.05%, which was
much higher than that of the planar structure. In addition, electrical simulation was carried
out using the finite element method, and the JSC , VOC , and Pmax were calculated. Based on
the maximum value of the average light absorbance, the geometric structure of the Al2 O3
pyramid PSCs was optimized. The electrical simulation results showed that the maximum
JSC was 23.54 mA/cm2 and the Jsc of the Al2 O3 pyramid structure was 22.73% higher than
that of the planar model, while the PCE of the solar cells increased from 14.01% to 17.19%.
These results indicate that the ARL array had a strong light coupling effect, highlighting the
great potential of Al2 O3 PARLs for solar absorption. This work provides valuable insights
for the structural design of PSCs and suggests that further exploration will lead to even
greater improvements in the PCE of PSCs.

Author Contributions: Conceptualization, L.L., W.L., W.F., Z.Y. and C.T.; data curation, L.L., W.L.,
W.F., Z.Y., T.S., Q.Z. and P.W.; formal analysis, L.L., W.L., W.F., Z.Y., T.S., Q.Z. and P.W.; methodology,
L.L., W.L., W.F., Z.Y. and T.S.; resources, Y.Y.; software, Y.Y., J.Z., C.T., T.S., T.S., Q.Z. and C.T.; data
curation, L.L. and W.L.; writing—original draft preparation, L.L. and W.L.; writing—review and
editing, L.L., W.L., W.F., Z.Y. and P.W. All authors have read and agreed to the published version of
the manuscript.
Funding: The authors are grateful to the support from the National Natural Science Foundation
of China (No. 51606158, 11604311, 12074151); the funding from the Natural Science Foundation of
Fujian Province (2022J011102, 2022H0048); the funding from the Guangxi Science and Technology
Base and Talent Special Project (No. AD21075009); the funding from the Sichuan Science and
Technology Program (No. 2021JDRC0022); the funding from the Open Fund of the Key Laboratory for
Metallurgical Equipment and Control Technology of the Ministry of Education in Wuhan University
of Science and Technology, China (No. MECOF2022B01; MECOF2023B04); the funding from the
project supported by Guangxi Key Laboratory of Precision Navigation Technology and Application,
Guilin University of Electronic Technology (No. DH202321); the funding from the Doctoral Fund of
Southwest University of Science and Technology (no. 21zx7111); the funding from the Postgraduate
Innovation Fund Project of Southwest University of Science and Technology (No. 24ycx1007).
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Publicly available datasets were analyzed in this study. This data can
be found here: [Link]
Conflicts of Interest: The authors declare no conflicts of interest.

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