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Contents lists available at ScienceDirect

Energy and Built Environment

journal homepage: http://www.keaipublishing.com/en/journals/energy-and-built-environment/

Design and optimization of graphene quantum dot-based luminescent solar

concentrator using Monte-Carlo simulation
Milad Rastkar Mirzaei a,b,d,∗, Ali Rostami b,c, Samiye Matloub d, Masoumeh Nazari b,d
a
ECE Department, University of Oklahoma, Norman, Oklahoma, 73019, United States
b
Photonics and Nanocrystals Research Lab (PNRL), University of Tabriz, Tabriz, 5166614761, Iran
c
SP-EPT Lab, ASEPE Company, Industrial Park of Advanced Technologies, Tabriz, Iran
d
Quantum Photonics Research Lab (QPRL), University of Tabriz, Tabriz, 5166614761, Iran

a r t i c l e i n f o a b s t r a c t

Keywords: The demand for green energy is growing these days as a result of the world energy crisis, as well as global warm-
Luminescent solar concentrator ing. Solar cells are in great interest due to the fact that solar energy can be easily converted to electricity, if
Solar cell the photovoltaic cell’s cost can be lowered. One of the methods to make low-cost energy is using Luminescent
Quantum dot
solar concentrators. They have the advantage of directly integrating solar cells to dense urban areas as well as
Graphene
skyscrapers. Different materials and waveguide sizes have been investigated for use in luminescent solar concen-
Energy-efficient building
Monte Carlo trators. However, the optimized waveguide geometry and quantum dots concentrators have not been thoroughly
studied. In this paper, we have simulated graphene quantum dots using density function theory. A Monte-Carlo
ray-tracing simulation was developed to model our device. We have optimized the luminescent solar concentrator
geometry by Monte-Carlo simulation. The optimization results show a 99% enhancement in the energy flux gain
of the final device. Besides, we have calculated and analyzed the fate of all photons.

1. Introduction concentrates light on photovoltaic devices. Different fluorophores have

been used for LSC applications such as organic dyes [19–22], lanthanide
Global warming, along with the financial crisis, has intensified the complex hybrids [23,24], perovskites [25,26], and quantum dots (QDs)
necessity of developing low-cost, extensive, and energy-efficient tech- [27–30]. Among these, QD LSCs have some significant advantages over
nologies to save sustainable energies [1]. Solar cells are one of the best others, such as stability, tunable absorption, and emission spectra, large
technologies to convert solar energy to electricity directly [2,3]. How- absorption cross-section, and high quantum yield (QY) [31–34]. How-
ever, the price of solar cells should be decreased 2-5 times to make ever, commercializing LSCs have been impeded by some loss mecha-
power from photovoltaics competitive with fossil fuels. The material nism,
and processing cost of silicon solar cells is the reason for their high The loss mechanism owing to luminescent materials can be classi-
price [4]. Luminescent solar concentrators (LSCs) can reduce the cost of fied into three main groups. First, only a fraction of the solar spectrum
solar power by reducing the amount of expensive solar panels needed is absorbed by QD because of its wide bandgap. Second, not all ab-
[5,6]. sorbed photons are radiated (non-unity QY). Third, re-absorption due to
LSCs can be produced in different sizes, shapes, and colors which overlap between absorption and photoluminescence spectra, followed
make them a suitable option to be used as windows and building facades, by non-radiative decay. Several methods have been proposed to miti-
turning them into power-generating objects [7–13]. Unlike other solar gate re-absorption losses by ’Stokes-shift engineering’ including hetero-
concentrating systems, LSCs do not need any cooling system. Besides, structuring [35–39], exploiting ternary semiconductor QDs with native
they can concentrate both direct and diffuse light, so they do not need intragap defects [40–43], utilizing indirect-bandgap QDs [44], impurity
any tracking systems [14,15]. An LSC consists of a thin flat plastic sheet doping [10,45,46], and using Föster energy transfer between QDs and
doped with fluorophores and edge-mounted solar cells. Fluorophores ab- dyes [47]. Some of the most prominent ones are going to be mentioned
sorb solar irradiance then re-emit photons at a lower frequency. These in the next paragraphs.
newly-generated photons are trapped in the plastic waveguide, which One of the common methods to tackle re-absorption loss is hetero-
guides them to the edge-mounted solar cell, converting solar energy to structuring. QDs may be classified according to their band structure into
electricity [16–18]. LSC is a purely photonic system that gathers and type I and type II. The key point of using type I hetero-structured QDs is

∗
Corresponding author.
E-mail address: [email protected] (M. Rastkar Mirzaei).

https://doi.org/10.1016/j.enbenv.2021.10.002
Received 15 March 2021; Received in revised form 4 October 2021; Accepted 5 October 2021
Available online xxx
2666-1233/Copyright © 2021 Southwest Jiatong University. Publishing services by Elsevier B.V. on behalf of KeAi Communication Co. Ltd. This is an open access
article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/)
Please cite this article as: M. Rastkar Mirzaei, A. Rostami, S. Matloub et al., Design and optimization of graphene quantum dot-based luminescent
solar concentrator using Monte-Carlo simulation, Energy and Built Environment, https://doi.org/10.1016/j.enbenv.2021.10.002
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that a wide bandgap thick shell absorbs the photons with higher ener-
gies while the core re-emits the photon in a longer wavelength leading
to significant separation (typically 400 meV) between absorption and
emission spectra [38]. Whereas type II QDs enjoy the spatial separa-
tion of excitons, resulting in spatially indirect-bandgap material [36].
Typical structures of hetero-structured QDs for LSC applications are
CdS/PbS [39], CdSe/CdS [48], CdSe/ZnS [49] and CdTe/CdSe [36] to
mention but a few. Although they have great potential to reduce re-
absorption probability, they contain heavy metals, which make them
detrimental to the environment since their safe disposal is expensive
and difficult. Another class of QDs that have solved the shortcom-
ing mentioned above is ternary I-III-VI2 semiconductor QDs including
CuInSex S2-x [41,42], and AgInS2 [43] and their composites. The Stokes
shift in these QDs is attributed to the existence of intragap states associ-
ated with native defects. Light’s absorption is due to band-edge transi-
tions, while emission is chiefly due to transitions from the valence band
to the intragap native state, resulting in a large separation of absorption
and emission spectra. These QDs exhibit encouraging features such as
broad absorption spectrum, large Stokes shift, and realization of color-
less LSC thanks to near-infrared emission [40]. However, insufficient in-
dium resources will impede their large-scale production[4]. Perovskite
materials are another candidate for LSC applications that have recently
received much attention [25,26,50,51]. Perovskites may reach QY as
high as 0.9, which is excellent for LSCs [52]. Nevertheless, perovskites
suffer from a lack of stability when exposed to constant sunlight, radi- Fig. 1. Schematic of an LSC and the possible event that can be occurred in an
LSC.
ation, and moisture, and these conditions are inevitable [53–56]. The
degradation of Perovskite-based LSCs makes their mass production eco-
nomically inefficient. its size is denoted by X. Also, t shows the thickness of the LSC. Figure 1
Fluorescent graphene quantum dot (GQD), the state-of-the-art nano- exhibits a schematic of an LSC and the possible phenomenon that can
material of carbon Nano-hybrids, has potential to realize the large- be occurred in an LSC.
scale production of LSCs owing to its unique and distinctive character-
istics such as tunable photoluminescence [57], photo-stability [58,59], 3. Monte-Carlo ray tracing simulation
low toxicity [60,61], low cost [62,63], the abundance of raw material
[64–66], resistance against photobleaching [67,68] and biocompatibil- Monte Carlo ray tracing determines the ultimate fate of each photon
ity [69,70]. Based on the characteristics mentioned above of graphene according to physical phenomena such as absorption, reflection, trans-
quantum dots, carbon dots (CD) have been recently proposed as a mission, and emission, based on mathematical equations and empiri-
promising material to be used in LSCs [71]. In research, two types of cal data, such as the Beer-Lambert Law, Snell’s law, absorption spec-
CDs were synthesized with UV and visible absorption, having QY of 0.6 tra, emission spectra, quantum yield, and many other factors. Graphene
and 0.4, respectively. The optical efficiency of each LSC reached 0.4% quantum dots was simulated using density functional theory (DFT), and
and 0.9%; then, using them together in a tandem configuration resulted the real and imaginary part of the refractive index was obtained. Then
in the enhancement of optical efficiency to 1.1% [72]. In the most recent the absorption and the photoluminescence profile were extracted and
work, exploiting spin-coated carbon dot LSC and two perovskite LSCs in used as input for Monte-Carlo ray-tracing simulation. The Monte Carlo
the tandem structure was studied. Carbon dot LSC absorbing the ultra- simulation was previously used to simulate the LSC [74,75].
violet spectrum improved the stability of the perovskite films to some The flow chart used to develop the Monte-Carlo simulation is shown
extent. The optical efficiency of each layer was 0.3%, 1.1%, and 1.65% in Fig.2. To generate photons probability density function (PDF) of the
for carbon dot and perovskites emitting green and red, respectively. Uti- standard AM 1.5G solar spectrum is used, then the PDF is converted
lizing a three-layer tandem structure led the optical efficiency to reach to the cumulative distribution function (CDF) which the wavelength of
3.05% [73]. each photon is sampled from it using the inverse transform sampling
Many shortcomings have hindered the commercialization of the method. 10ˆ5 initial sampled photons used for the simulation. The pho-
LSCs, including low optical absorption, inappropriate LSC size and scale, tons are assumed to hit the LSC with a normal angle. According to Snell’s
low QY, and overlap between absorption and emission spectra. Most of law, some percent of photons are reflected from the top surface of the
the other works published earlier don’t have an authentic design process, LSC which those photons should be removed from the rest of the pro-
and they have been chosen with the favor of the author rather than an cess. Those photons are regarded as reflection loss, and their amount is
optimization flowchart. In this paper, we have simulated the absorption approximately four percent of total initial photons.
and photoluminescence spectra of GQDs using density function theory Then we should know that if the quantum dots absorbed the photons.
and simulated the LSC with Monte-Carlo ray-tracing simulation. Then, The Beer-Lambert law determines the probability of a photon being ab-
we have further optimized the LSC geometry using Monte-Carlo simu- sorbed after moving along a distance, Δ𝑑 (in cm),
lation. Also, we have calculated the photons loss percentage that every
event is responsible for. 𝑃 = 1 − 10−𝐴(𝜆)Δ𝑑 (1)

Moreover,
2. LSC structure and possible phenomenon
1
Δ𝑑 = − log(𝑃 ) (2)
In our structure, the LSC is consists of the plastic waveguide embed- 𝐴(𝜆)
ded with graphene quantum dots. The four faces of it are covered by A is the absorbance which is measured from the absorption spec-
four solar cells on the edge of the film, and the light is incident on the trum of the graphene quantum dots. Its unit is 1/cm when multiplied
front surface. The device is assumed to have a square front surface, and by the LSC thickness (Δ𝑑); it would be a unitless number that is used

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Fig. 2. Flowchart of Monte-Carlo ray-tracing simula-

tion.

pass without absorption. Else, the photon is absorbed, and the position
of the photon is stored. In the next step, we should determine if the
quantum dot would emit the absorbed photon. It is done by the use of
QY, which is defined by the ratio of a number of the photon emitted
to the total number of photons absorbed. A random-generated number
(𝛽) which is between 0 and one, is compared by quantum yield. If the
𝛽 is smaller than the QY, the photon would be re-emitted. The emission
angle is randomly chosen, and its wavelength is chosen from the CDF
of the emission spectrum. The distance that photons cross after being
reabsorbed is given by equation 3.

1
Δ𝑑 = − log(𝛽) (3)
𝐴(𝜆)

The photon’s new position after propagating Δ𝑑is stored. Then, the
photon should be checked if it is inside the LSC. If yes, then it must have
been absorbed. If the answer is No, the photon must have an interaction
with LSC surfaces. The nest objective is to figure out with which surface
Fig. 3. Absorption and Photoluminescence spectra of graphene quantum dots. it has interaction. The photon reaches the solar cells if it hit the first four
surface (surfaces with solar cells). If the photon hits the up or bottom
surface of the LSC, two scenarios can be the outcome. First, the photon
in determining photon absorption probability in equation (1). In the escape from the surface, so the photon is lost. Second, the surface re-
simulation, absorption probability is generated by a random number. flects the photon because of total internal reflection and subsequently
Suppose the Δ𝑑found to be larger than the LSC thickness (t), the photon reabsorbed or reached the solar cells.

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Fig. 4. (a) Percent of absorbed photons concerning geometric gain, (b) Optical power efficiency and energy flux gain.

Fig. 5. (a) internal quantum efficiency, (b) optical power efficiency (orange arrows shows results for optimized device), and (c) energy flux gain efficiency (orange
arrows shows results for optimized device) concerning different lateral sizes.

To assess LSC performance, we define some relations. We define op- mula is optical power efficiency (OPE).
tical efficiency as,
𝜆
collected power ∫𝜆 emitted max 𝑛collected (𝜆) ∗ 𝜆1 𝑑𝜆
𝜂opt
′
= = 𝜆emitted min (5)
collected photons incident power ∫𝜆 incident max 𝑛incident (𝜆) ∗ 𝜆1 𝑑𝜆
𝜂opt = (4) incident min
incident photons
Until now, we have defined optical power efficiency. However, we
However, optical efficiency does not take the shift of energy between need another parameter to evaluate the concentration of the LSC. An-
absorption and emission into account. Therefore, a more convenient for- other parameter is geometric gain. The geometric gain is a measure of

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Fig. 6. Results of optimization stages as

well as LSC photo from the corresponding
stage.

the maximum possible photon flux concentration of an LSC with all

other factors are perfect.
𝐴𝐿𝑆𝐶
𝐺= (6)
𝐴𝑃 𝑉
Where 𝐴𝐿𝑆𝐶 is the area of the upper face of the LSC, and the 𝐴𝑃 𝑉 is
the area of the faces with solar cells attached. The multiply of geometric
gain and optical power efficiency gives the most important parameter
for the LSC, that is, energy flux gain.

𝐹 𝐺𝑜𝑝𝑡
′
= 𝐺 ∗ 𝜂𝑜𝑝𝑡
′
(7)

4. Results and discussion

Density function theory has been applied to study optical and atomic
properties of materials in general, and especially organic [76–79].
Therefore, the optical absorption and emission spectra of the graphene
quantum dots obtained from the DFT simulation are shown in Fig. 3.
Also, the quantum yield was found to be 0.3. The absorption spectrum of
the GQDs exhibits absorbance extended through the visible region, sug- Fig. 7. AM 1.5G Sampled and transmitted photons from LSC versus wavelength.
gesting excellent solar irradiance absorption. Also, an acceptable Stocks-
shift of 147 meV is apparent from the figure, which is desirable for LSC It is obvious from Fig. 4 that the optical power efficiency decreases
application. The Stokes shifts of traditional and commercially available with increasing G, and accordingly, the energy flux gain increases with
organic dyes utilized in LSCs are generally small (<20–30 nm) [80,81]. G. We have defined G the intersection of the two curves determines the
The quantum dots, on the other hand, have better stokes shift starting optimum G number, which is roughly 15.
from a hundred to couples of hundred meV [82–85]. In the next step of the geometric optimization of the LSC, we scale
The next task is the determination of geometric gain (G), which plays the device with selected geometric gain to find the optimum size of the
a significant role in LSC’s overall performance as it defines the aspect ra- LSC. Fig. 5(a) shows that internal quantum efficiency swept against the
tio of the device. The ultimate goal of the designing of an LSC is lowering lateral size of the LSC. A severe decrease in internal quantum efficiency
the cost of photovoltaic systems by cutting down the cost of generated is apparent with increasing the LSC’s lateral size due to the fact that
solar power by decreasing the required amount of expensive solar cells. photons should pass longer optical paths leading to high re-absorption
The objective can be achieved by higher geometric gains because the probability.
edge area on which solar cells attach would be far smaller than the front The optical power efficiency and energy flux gain of the device is
surface of the LSC. However, the absorption of the photons and subse- depicted in Fig. 5 (b) and (c), respectively. For small lateral sizes, we
quently output power directly depend on LSC thickness. The relation observe a low OPE and EFG, which is attributed to low absorption be-
between geometric gain and absorbed photons is presented in Fig. 4(a). cause of thin device thickness. Also, a steep increasing rate for larger
Hence, the tradeoff between energy flux gain and optical power effi- LSC sizes is obvious, ending in a flat peak. This increase is due to higher
ciency is mandatory. Fig. 4 (b) represents flux gain energy and optical absorption and optimal devise size. With the continuation of device size
power efficiency against the geometric gain. enlargement, the OPE and EFG start to diminish again. Although the de-

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Fig. 8. Ultimate photons fate.

Table 1
Summarized LSC output for different LSC the optimizations.

Opt. Stage LSC size [cmˆ3] G Optical Power Efficiency[%] Energy Flux Gain

Initial Guess 12∗ 12∗ 0.3 10 2.1 20.1

First Opt. Stage 12∗ 12∗ 0.2 15 1.8 27
Second Opt. Stage 48∗ 48∗ 0.8 15 2.71 40

vice absorption is high in that lateral sizes, the re-absorption losses be- vice. Furthermore, LSC geometry was optimized to be 48∗ 48∗ 0.8 [cmˆ3],
come significant, leading to degradation in overall device performance. which was initially 12∗ 12∗ 0.3 [cmˆ3]. The OPE and EFG were enhanced
The three-stage optimized results and LSC pictures for the device are from 2.1% to 2.71% and 20.1 to 40, respectively. Also, losses from each
listed in Fig. 6. The blue dots represent photons that reached the exit possible event were calculated in detail. We have found that increasing
aperture of the LSC, while the red ones are lost because of scape cone device absorption would increase efficiency. We can see that 99% of the
losses. Comparing the photo from the initial guess with the final device, absorbed photons are lost because of re-absorption losses. Hence, syn-
we can see more concentrated photons, which is the result of higher thesizing GQDs with higher QY and low absorption and photolumines-
energy flux gain. Table 1, is summarized LSC output for different LSC cence overlap would significantly increase the efficiency of the device.
optimizations.
The Transmittance or transparency figure for optimized LSC can give Data availability
information about the wavelengths that have been absorbed in LSC or re-
flected from it. Fig 7 shows the wavelength of 100000 sampled photons Data underlying the results presented in this paper are not publicly
from the AM1.5G solar spectrum, along with transmitted photons from available at this time but may be obtained from the authors upon rea-
the LSC. The transmitted photons have been calculated by subtracting sonable request.
reflected photons and absorbed photons from Sampled AM1.5G. There is
a significant dip in transmitted photons from 470 nm to 538 nm, which Credit author statement
is because of QD’s absorption. Thus, the photons transmitted through
LSC would lack the green portion of the spectrum. The total absorption Milad Rastkar Mirzaei conceptualize the idea, wrote the Monte Carlo
of optimized LSC is 12.13%. simulation code and composing manuscript. He also, did the density
Now we calculate the fate of photons for the optimized device with function theory simulation. The Monte Carlo code was written in MAT-
48∗ 48∗ 0.8 [cmˆ3] size. According to the Monte-Carlo simulation, 84.11 LAB software and evaluated by simulating other papers. Masoumeh
% of photons pass through LSC without absorption. 3.98(approximately Nazari post processed results, edited data and plotted the figures.
4)% of photons reflect from the top surface without entering the device, Also, she proofread and edited the manuscript.(equation 2, equation 3,
and 12.099% of the photons are absorbed by the quantum dots having equation 4, equation 5, equation 6, equation 7)
the possibility to reach the edge of the device, which is shown in Fig. 8.
However, not all of the absorbed photons find a way to the exit aperture. Declaration of Competing Interest
73.75% of these photons are lost due to re-absorption losses (e.g., non-
unity quantum yield). 6.86% of the absorbed photons are lost from the The authors declare no conflicts of interest.
scape cone, and only 19.39% of the absorbed photons reach the edge of
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