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. 2023 Jan 5;3(1):25–35. doi: 10.1021/jacsau.2c00504

Achieving High-Efficiency Large-Area Luminescent Solar Concentrators

Mengyan Cao †, Xiujian Zhao †, Xiao Gong †,*
PMCID: PMC9875231  PMID: 36711087

Abstract

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Luminescent solar concentrators (LSCs) are semitransparent windows that are able to generate electricity from sunlight absorption. LSCs have shown huge promise for realizing building-integrated photovoltaics (BIPV). Unfortunately, to date, the power conversion efficiency (PCE) of LSCs is still very low which dramatically hampers their practical applications. In this Perspective, We summarize and review the latest developments of LSCs by looking at different structures. Among others, we focus more on the next developments in the field of LSCs, i.e., the possibility of high PCE, large area, mass production, and durability needed for future industrial development. We hope to promote the application of uniform testing standards and to draw attention to industrial development, toxicity, and durability. Then, we will provide a critical assessment of the field of LSCs. Finally, the challenge and solution will be discussed.

Keywords: Luminescent solar concentrators, Building-integrated photovoltaics, Large area, High efficiency, Different structures, Luminophores

1. Introduction

Since the Industrial Revolution, energy demand and economic growth have taken off simultaneously.1,2 Numerous renewable energy sources are being researched by various countries to meet the demand for energy.3−8 Research on common clean energy sources such as nuclear, wind, biomass, ocean, and solar energy is being conducted rapidly.9−14 The concept of building-integrated photovoltaics (BIPV) solves the problem that photovoltaics systems cannot be compatible with cities, and can be used for solar power generation while serving as the outer structure of a building.15 As a new type of solar photovoltaics device, the luminescent solar concentrators (LSCs) collector demonstrates the excellent potential to become a photovoltaic conversion device in BIPV.16

LSCs are mainly composed of three parts: light waveguide medium, luminophores, and solar cell.17 The light waveguide medium is mainly made of transparent glass or polymers (e.g., poly(methyl methacrylate) (PMMA), polyvinylpyrrolidone (PVP), and epoxy resin).18,19 Materials such as perovskite quantum dots, organic dyes, carbon quantum dots, and copper iodide based hybrid nanoparticles are often used as luminophores for LSCs.20,21 In contrast, monocrystalline silicon solar cells and gallium arsenide solar cells are commonly used for solar cells.22 After the luminophores in the LSCs are excited by sunlight, photoluminescence occurs, and the fluorescence emitted by the luminophores is transmitted through the medium of the optical waveguide and is totally reflected to the side-coupled solar cell, thereby realizing the final photoelectric conversion process.23,24 For LSCs, a complex sunlight tracking system is not required, and due to the nature of the flat panel structure, it can itself receive a wide range of sunlight.25,26 And the low cost of corresponding polymers and luminophores can effectively reduce the cost of the whole LSCs system. The low sensitivity to irradiation angle allows the device to achieve higher efficiency under conditions such as diffuse light reflection. Another very important advantage is the relatively simple preparation means and the absence of a cooling system. LSCs are considered to be a very potential technology that can concentrate large-area light onto small-area solar cells on the side, thereby realizing more efficient utilization of sunlight.

In recent years, some review articles on LSCs have been published, most of which take the important fluorescent molecules in them as the main thread, and the principles and characteristics of LSCs based on different luminophores are specifically reviewed.27,28 However, monolayer LSCs demonstrate relatively low optical efficiency due to their extensive nonradiative recombination loss, transmission loss, reabsorption loss, etc., which is quite significantly different from the currently calculated limiting efficiency.19 In order to achieve higher optical efficiency, tandem LSCs composed of different fluorescent molecules have been chosen to solve the problem of insufficient light utilization in some single-layer LSCs. LSCs with a tandem structure are composed of multiple single-layer LSCs, which have significant advantages compared with single-layer LSCs.29 Since each layer of LSCs is doped with different types of fluorescent nanoparticles, the range of sunlight absorbed by different types of fluorescent nanoparticles is different, thus widening the utilization of sunlight to a large extent, which can maximize the utilization of sunlight and thus effectively improve the photoelectric conversion efficiency of LSCs. Thus, the structural design of LSCs can solve the problem that the low efficiency of single-layer LSCs cannot meet a wide range of applications.

In this Perspective, we focus on summarizing the latest developments in single-layer and tandem LSCs. This includes a summary of the different luminophores used in LSCs for their optical efficiency and related parameters. Compared with the previous reviews focusing on the synthesis and mechanism of luminophores, this outlook is more focused on the very important next step in the field of studies on LSCs, which hopefully will lead to a more recent direction toward practical applications. For different structures and different luminophores, we are more interested in their future applicability for industrial use, also in terms of mass production or synthesis. Finally, we also paid special attention to durability and environmental toxicity in the corresponding literature, being relevant to future application possibilities. With this Perspective, we hope to promote the widespread use of uniformized test requirements and to draw attention to the issues of green high-volume synthesis and durability in order to facilitate LSCs devices further down the road to future commercialization.

2. Single-Layer LSCs

The variety of luminophores used for single-layer LSCs can be from the common fluorescent organic dyes and semiconductor quantum dots, to the newly developed perovskite quantum dots, carbon dots (CDs), silicon dots, etc., and all of them have been widely used in the field of LSCs with certain effects.30−32 We first discuss a little bit about perovskite quantum dots, which are very widely studied nowadays, and compare them with CDs and other eco-friendly quantum dots.33,34 Among them, we will discuss the real rigor in efficiency testing, the durability of the devices, and the possibility of scaling up production according to the properties of different materials. Finally, we discuss the challenges and limitations of the current development of monolayer LSCs and highlight the future directions and paths forward.

2.1. Perovskite Nanocrystals

Perovskite quantum dot have been widely used in the field of optoelectronics due to their excellent optoelectronic properties, ultrahigh photoluminescence quantum yield (PLQY), optical tunability, narrow-band emission, wide color gamut, and solution synthesizable advantages.35−38 Lead-based halide perovskite can achieve a modulating effect on the PL spectrum by changing the halogen species and ratio, which predicts relatively controllable optical properties and makes it easier for people to adjust the material’s corresponding absorption and emission spectra.39−43 The ease of doping in perovskite quantum dots gives them greater advantages such as enhanced stability, variable emission and absorption spectra, high PLQY, etc.44−46 Similarly, these excellent properties have led to the application of perovskites in the field of LSCs.

Zhao et al. reported in 2017 that the application of CsPb(BrxI1–x)3 nanocrystals in LSCs aims to reduce reabsorption losses, as shown in Figure 1a,b. Among them, the PLQY of CsPb(BrxI1–x)3 nanocrystals is ultrahigh (>60%) and the absorption spectrum is broad (300–650 nm), and the tunability of the PL spectrum across the visible spectrum can be achieved by the variation of the PbBr2/PbI2 placement ratio during preparation. With a G-factor of 45, they obtained large-size LSCs with an optical efficiency of about 2% and tested them for durability with 4 h of UV irradiation.47 However, the corresponding efficiency is still low, and a mere 4 h of UV irradiation is far from sufficient for a device like LSCs to indicate durability. There exists a continuing search for larger Stokes shifts and more commercially promising preparation methods. Meinardi et al. tried Mn ion-doped CsPbCl3 nanocrystals, resulting in the successful preparation of fluorescent emitters with almost no reabsorption, as shown in Figure 1c.48 Moreover, after Monte Carlo simulations and light propagation measurements, it was demonstrated that the doped nanocrystals had a very large Stokes shift and the corresponding fluorescence intensity was maintained up to 80% of the original one after a long transmission distance (25 cm), while the corresponding pure CsPbCl3 nanocrystals retained only 20% of the intensity. Based on the low reabsorption loss of CsPbCl3:Mn nanocrystals, the doped nanocrystals are also considered to be effective as suitable emitters for ideal large-area reabsorption-free LSCs. Some subsequent doped perovskite nanocrystals have also been widely explored for LSCs applications, for example, Cai et al. reported Mn2+/Yb3+ codoped CsPbCl3 nanocrystals prepared using the thermal injection method, which showed broad emission encompassing both visible and near-infrared regions and exhibited superior external optical efficiency compared to CsPbCl3:Mn2+ nanocrystals due to their high quantum yields (QY) and small reabsorption losses.49 The corresponding PL and absorption spectra of the nanocrystals demonstrating the larger Stokes shift and less reabsorption loss achieved due to the energy transfer from the host material to the doped ions after doping. Mn2+ ion-doped organic–inorganic hybrid perovskite quantum dots were also reported for the preparation of LSCs by Bhosale et al. to obtain optical efficiencies up to 8%.50 A special optical phenomenon, quantum cutting, is partially present in these doped lead-based halide perovskite nanocrystals. This phenomenon is manifested by the emission of two low-energy photons after the absorption of a high-energy photon by the nanocrystal, with a corresponding doubling of the QY in the ideal state. Luo et al. then reported Yb-doped CsPbCl3 nanocrystals with large Stokes shifts and ultrahigh QY of 164%.51 Among them, the main absorption peak of CsPbCl3:Yb nanocrystals located at 400 nm and the main emission peak located at 980 nm, showing a great Stokes shift, which is very favorable with minimal self-absorption effect in the transport. According to theoretical calculations, in larger size LSCs based on quantum cutting of energy conversion efficiency would be four times higher than that of conventional perovskite nanocrystals. The corresponding quantum cutting effects also appears in the Mn2+/Yb3+ codoped CsPbCl3 nanocrystals.49 These results suggest that the quantum cutting effect will open a new door for the LSCs field. And to address the unsuitability of the corresponding drop coating method for industrial production, Tong et al. prepared large-area flat LSCs using the scraping method, the most attractive of which was its maintenance at high temperature (60 °C) and high humidity (relative humidity = 90%) for 1000 h.52 To solve the toxicity problem of perovskite quantum dots, two methods usually exist, replacing toxic elements and encapsulating lead-based perovskite quantum dots in the device. The same Kment et al. reported very excellent results with an all-inorganic lead-free perovskite quantum dots as a nontoxic light emitter.53 The latter approach was chosen by Zhang et al. to encapsulate lead-based perovskite quantum dots in a glass matrix to protect the quantum dots and prevent the diffusion of toxic elements.54

Figure 1.

Figure 1

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(a) PL and absorption spectra of CsPb(BrxI1–x)3 QDs (x = 0–1). (b) Photographs of the LSCs under one sun (left) and UV illumination (right). (Reproduced from ref (47), with permission from Copyright 2017, Elsevier.) (c) Photograph of the LSCs comprising CsPbCl3:Mn2+ QDs under ambient (left) and UV illumination (365 nm, right). (Reproduced from ref (48). Copyright 2017 American Chemical Society.)

Numerous studies have reported the rapid development of perovskite quantum dots on the surface, which has gained much popularity, but there are still many problems to be solved in the application of experimental perovskite quantum dots on LSCs. From the material itself, the first and foremost problem is the stability of perovskite quantum dots, whose stability to light, water, oxygen, heat, and other aspects are crucial and will become the primary issue for future industrialization. Although some of the current encapsulation and passivation solutions have significantly improved the corresponding stability problems, but for the development of the subsequent practical applications still seems to be a drop in the bucket. The second question by everyone is the toxicity of the problem, the element of lead for many systems in the human body will have a very serious impact, and can be directly through the skin into the body, and very difficult to discharge. Lead-free perovskite quantum dots have attracted interests, but their optical and electrical properties are generally worse than those of lead-based perovskite quantum dots. The solution to this problem needs to be studied in a combination of theory and practice. The problem of toxicity of the material itself is extremely limiting for subsequent applications, but in the case of environmentally friendly quantum dots, there is relatively no need to consider the issue of biological toxicity.

2.2. Carbon Dots

As a new type of carbon-based fluorescent nanomaterial, CDs have recently received extensive research attention for their diverse physicochemical properties, abundant surface groups (such as amino, carboxyl, and hydroxyl groups, etc.), environmental friendliness, and low cost.55−61 Among them, simple preparation methods, high PLQY, low toxicity, and tunable emission spectra are considered by researchers as the ideal luminophores in LSCs.62,63

In 2017, Li et al. first introduced N-doped CDs into the preparation of LSCs with composite PMMA as a film-forming agent (Figure 2a), demonstrating a very promising efficiency of 3.94%, which is very high as the first utilization.64 However, where the size of LSCs is relatively small, its corresponding test conditions are relatively unclear. Limited by the development of CDs, most of the CDs long used for LSCs until 2020 exhibit properties of emission at short wavelengths, for example, the CDs reported by Gong et al. in 2018 demonstrate emission with a peak located at 435 nm and absorption mainly in the UV region, accompanied by a corresponding efficiency of 2.63%.65 In the same year, CDs in LSCs reported by Wang et al. exhibited emission with a peak located at 420 nm accompanied by excitation-dependent phenomena (Figure 2b), possessing a conversion efficiency of 4.97%.66 Meanwhile, the size of the corresponding LSCs is relatively small and the tested efficiency is relatively not decisive for future commercialization progress. With the development of time, researchers have continued to broaden the scope of their studies, and larger size, longer emission wavelength CDs were used in the preparation of LSCs. In 2018, Zhou et al. reported CDs with emission centered at 540 nm and possessing the QY of nearly 30% for LSCs luminescence. The optical efficiency of their corresponding LSCs was 1.2%, accompanied by a corresponding geometric (G) factor of 10.67 The LSCs reported by Zhao et al. in 2019 demonstrated a larger size (10 × 10 × 0.9 cm3), accompanied by an optical conversion efficiency of 1.6%. where the absorption of the CDs broadens to the visible region (300–550 nm), accompanied by a QY of nearly 50% in ethanol solution.68 However, the corresponding efficiency is still not satisfactory, and the drop coating method cannot guarantee the corresponding reproducibility to demonstrate future industrialization possibilities. More researchers have put efforts on the QY and Stokes shift of CDs, for example, in 2020, Huang et al. reported aminosilane-functionalized CDs (Si-CDs) with high QY (>60%) and very large Stokes shift (>200 nm), obtaining a very high optical efficiency of 4.4%.69 The corresponding PL spectra of the correlated emission of LSCs are shown in Figure 2c. Demonstrating their breakthrough in the corresponding direction, Maria et al. loaded CDs with the QY up to 94% into a silicone matrix to obtain LSCs with high transparency and high loading, achieving with an external efficiencies of nearly 3.9% at a size of 3 × 3 × 0.3 cm3 (Figure 2d).70 The smaller size may be the reason for the corresponding higher efficiency, but the application of the high transparency in BIPV is very promising, but the emission, which is only located around 450 nm, will greatly limit its subsequent industrialization.

Figure 2.

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(a) Schematic of LSCs structure consisting of carbon dots based on PMMA substrate. (Reproduced from ref (64), with permission from Copyright 2017, Royal Society of Chemistry.) (b) Photographs of the N-CDs based LSCs under UV illumination. (Reproduced from ref (66), with permission from Copyright 2017, Elsevier.) (c) PL spectra collected based on the whole LSCs, the LSCs surface, and the LSCs edge. (Reproduced from ref (69), with permission from Copyright 2020, Royal Society of Chemistry.) (d) Absorption and emission spectra of LSCs based on silicon CDs, inset is the physical image obtained under UV light irradiation. (Reproduced from ref (32). Copyright 2020 American Chemical Society.).

Afterward, researchers have provided more ideas to enhance the efficiency of the corresponding LSCs, such as using plasma enhancement and high carbon dot loading rate.71,72 However, the corresponding efficiency is still unsatisfactory, while the reduction of QY at higher loading rates, the loss of scattering and reabsorption, and stability are still some problems to be solved. Zhao et al. then reported a step further along the road toward industrialization through another aspect of enhancement. A space-constrained vacuum heating method was reported to prepare large batches of CDs while retaining a high QY (65%), where a thin-film type large-size LSCs (15 × 15 × 0.5 cm3) fabricated on a PVP substrate showed an external optical efficiency up to 2.2%. This large area of efficient LSCs is due to the prepared CDs with a large Stokes shift, which suppresses the reabsorption loss during light collection.73 This report provides new ideas for the industrial development of LSCs, and we all need to explore equally simple and easy mass production methods in synthesis while considering the corresponding efficiency improvement. Cai et al., on the other hand, reported two-dimensional self-assembled CDs that could be induced by solvent, showing tunable PLQY, while also containing ultrahigh QY (90%) in a polystyrene matrix, and the correspondingly prepared LSCs with large dimensions (100 × 100 × 6.3 mm3) showed a power conversion efficiency of 1.4%.74 The ordered self-assembly in which can be achieved by the synergistic effect of stacking and lateral hydrogen bonding in planes is very novel, while the atomic force microscopy (AFM) images in Figure 3a also confirm the existence of a two-dimensional sheet structure. The high quality optical properties possessed by this carbon dot, including a broad absorption spectrum with high QY and long wavelength emission (better matching with the response region of the solar cell), are well suited for LSCs devices. And the authors also mentioned that as there is a certain overlap between absorption and emission spectra, combined with the high QY and very large absorption rate there is a possible behavior of photon recycling, where the reabsorbed photons can be effectively re-emitted, thus mitigating the effect of reabsorption on the efficiency.75 This seems to demonstrate new ways of mitigating the effects of reabsorption. Gong et al. recently reported high QY silicon doped CDs for efficient preparation of large area LSCs. The Si-doped CDs were encapsulated in PVP and obtained an energy conversion efficiency of 4.36% at a size of 5 × 5 cm2, and further LSCs with a size of 15 × 15 cm2 were prepared using the drop coating method (Figure 3b), accompanied by a conversion efficiency of 2.06%.76 The corresponding large size is very rare in the reports, but the conversion efficiency of less than 3% is unsatisfactory for all and is not applicable for future industrialization. Among them, the 4-week optical durability test is very effective to prove the stability of the material, but the stability of light alone is also not enough to illustrate the problem of antiaging in industrialization, stable working time and service life should be reflected in the subsequent work. These long wavelength CDs with high QY and CDs with self-assembly properties have been reported by researchers to be applied in the field of large size LSCs, and both have achieved some results.77,78 Similarly, we believe that the issue of durability has been put aside in the preparation and testing, and as a thin film LSCs, the aging data generated when subjected to long-term light radiation under outdoor environment needs to be provided by everyone in order to move further toward industrialization.

Figure 3.

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(a) AFM images of boric acid-functionalized graphene quantum dots. (Reproduced from ref (74). Copyright 2022 American Chemical Society.) (b) Photographs of the LSCs under sunlight, accompanied by dimensions of 15 × 15 × 0.5 cm3. (Reproduced from ref (76), with permission from Copyright 2022, Elsevier.) (c,d) Schematic illustration of the 3D structure unfolding (c) and cross-sectional views (d) of the Si-CDs based LSCs. (Reproduced from ref (87). Copyright 2020 American Chemical Society.)

As a nontoxic luminophore, CDs are becoming more and more popular for LSCs applications, and the diversity of synthesis methods for CDs determines the variety of its structures, which can eventually be tuned for optical properties is very interesting. However, how to synthesize CDs on a large scale using simple green synthesis methods is still a great challenge before industrialization. The long wavelength emission, high QY, and larger Stokes shift of CDs are still difficult to prepare, and the obvious overlap of absorption and emission spectra in CDs will lead to significant reabsorption effects in LSCs, which will ultimately result in lower optical conversion efficiency. Moreover, most of the current CDs are only located below 600 nm absorption wavelength, which has relatively little utilization of sunlight, while the near-infrared emitting CDs have the problem of low QY. In everyone’s report, it is difficult to compare the efficiency derived from different test methods of different sizes in a uniform way, which is very unfavorable to the overall development. We believe that unified test standards and complete durability tests are very much needed for the LSCs field. In terms of LSCs devices, carbon dot-based LSCs still show a low energy conversion efficiency, and there is an urgent need to find methods that can effectively improve the efficiency. The preparation, testing, and characterization of ultralarge area LSCs are relatively little reported to make clear their effective industrial significance, and the study of theoretical models for large area LSCs also needs to be improved. In the film-forming form of luminophores, a way of uniform and continuous film formation in large-area substrates needs to be sought for subsequent real applications.

2.3. Other QDs

Other environmentally friendly quantum dots such as ZnO quantum dots and silicon quantum dots are also widely used in the field of LSCs.79,80 Among them, silica quantum dots are ideal emitters for LSCs due to their large reserves on earth, nontoxicity, excellent ability to inhibit reabsorption, and excellent compatibility with polymers.81−83 ZnO quantum dots, on the other hand, are easy to prepare in solution, inexpensive, with good UV absorption and high stability, and show unique potential.84−86

In 2017, Meinardi et al. reported the combination of indirect bandgap silicon quantum dots into a poly(acrylic acid) matrix material, resulting in a high-quality optical waveguide that also guarantees a transmission rate of nearly 70% at a large size (144 cm2), achieving an efficiency of 2.85% for power conversion.80 The larger size is very advantageous, and the bright luminescence located at the edges demonstrates the excellent optical properties of the silicon dots. The overlap between the corresponding absorption spectrum and emission spectrum is not obvious, which may lead to less light loss due to the reabsorption effect, so as to achieve higher energy conversion efficiency. Moreover, the flexible devices were prepared and used to evaluate the effect of the bending angle on the waveguide performance of the LSCs, and based on the data from numerical simulations, they indicated that the bending angle does not affect the performance of the LSCs. These results are very meaningful, and the preparation of flexible devices broadens the scope of future LSCs integration applications, where long-wavelength emitting silicon quantum dots can be better matched to the response region of silicon solar cells. In 2020, Han et al. reported the use of liquid silicon quantum dots for a novel structure of LSCs (shown in Figure 3c,d), in which two thin glass plates sandwich a suspension of silicon quantum dots, while silicon solar cells are placed as window frames along the perimeter of the LSCs.87 The energy conversion efficiency of the LSCs reaches 2.47%, while the overall device (10 × 10 cm2) retains a transmittance of nearly 84%, which is perfectly suitable for daily light transmission purposes. Several low light scattering silicon quantum dot films and novel 3-layer glass structures have been explored and used in LSCs to pursue higher energy conversion efficiency and more practical features.88,89

In 2021, Gong et al.79 reported the loading of Eu-doped ZnO materials into PVP using a facile solution method, accompanied by a higher loading concentration and obtained an optical efficiency of nearly 4.36%. Among them, the Eu3+-doped ZnO material showed a large Stokes shift with almost no overlapping range in the emission and absorption profiles and exhibited both the 550 nm emission belonging to ZnO and the 614 nm emission of 5D0 → 7F2 attributed to Eu3+ ions. The nontoxic and simple preparation of ZnO quantum dots for LSCs applications is very novel and the stability of ZnO is excellent compared to other materials. However, the absorption of ZnO is mainly located in the UV region, but the UV component of sunlight is low, so it is very difficult to have a good improvement of the subsequent energy conversion efficiency if it only contains UV absorption, and it is also difficult to get the subsequent application. Moreover, the size of LSCs is small, and the smaller size will not allow many key issues to be clearly demonstrated, and the subsequent preparation of a large size is also very necessary.

3. Tandem LSCs

The power conversion efficiency of single-layer LSCs is far from the commercialization purpose at present, and people have explored the possibility of improving the photoelectric conversion efficiency from the structure in addition to using the optimization of the emitter to improve the efficiency.29,90,91 Among them, the advantage of stacked structure is very obvious, in different layers mixed with different types of fluorescent emitters, can absorb solar radiation in different areas, improve the utilization of sunlight, so as to effectively improve the photoelectric conversion efficiency of LSCs. At present, CDs, perovskite quantum dots, aggregation-induced emission (AIE) organic materials, etc. are utilized by researchers as fluorescent emitters to achieve the purpose of enhancing the photoelectric conversion efficiency.92

In 2018, Liu et al. reported that CdSe/CdS quantum dots and CDs were prepared as emitter materials in stacked LSCs of 10 × 10 cm2, respectively, showing a conversion efficiency of nearly 1.1%.93 Among them, the carbon-dot-based LSCs is used as the top layer for the purpose of absorbing UV light for the first step of the conversion process, while the stability of the underlying CdSe/CdS quantum dots under solar light (which loses part of the UV light portion) can be enhanced. In Figure 4a, it is shown that the CdSe/CdS quantum dots without carbon dot base protection have a significant reduction of PL intensity after 70 h of irradiation, and when there is a carbon dot layer protection, although there is still a certain reduction of intensity, there is a great improvement compared with the raw material, which also reflects the protective effect of carbon dot base as the top LSCs. The photostability of CdSe/CdS quantum dots is very worrying. After only 70 h of irradiation, the PL intensity of CdSe/CdS quantum dots is reduced to 43% of the original one, which cannot be used for the subsequent BIPV, and the durability of the material is not guaranteed. Moreover, the corresponding conversion efficiency is too low to reach the expected level. Therefore, subsequent research is often pursued in the direction of more stable quantum dot materials and higher conversion efficiencies. Zhao et al. then prepared a stacked structure of LSCs using CDs and perovskite quantum dots, accompanied by a size of 10 × 10 × 0.2 cm3 and an external optical efficiency of about 3% in daylight, which is a great improvement compared to the single-layer perovskite quantum dot LSCs.94 Among the CDs, CsPb(Br0.8Cl0.2)3 quantum dots and CsPb(Br0.2I0.8)3 quantum dots materials were utilized as luminophores for the 3-layer stacked LSCs, respectively, and the corresponding absorption and emission profiles are shown in Figure 4b. The corresponding stacked-layer structure not only expands the utilization of sunlight but also further enhances the overall external optical efficiency as the light emitted from the carbon dot layer by the escape cone can be effectively absorbed by the CsPb(Br0.8Cl0.2)3 quantum dots in the second layer. The strong absorption of UV light by the carbon dot layer also attenuates the effect of strong UV light on the lower layer of the perovskite quantum dots, which enhances the overall device optical stability. Meanwhile, since conventional emitters often exhibit concentration quenching, Ma et al. reported a stacked LSCs using blue CDs and AIE materials, the structure and physical diagram of which are shown in Figure 4c.95 The coupling of the two types of emitters, CDs and TPFE-Rho, allows the absorption of sunlight from 300 to 570 nm, thus achieving a conversion efficiency of nearly 4.06%. However, the reason for the high conversion efficiency is believed to be the small size of 2.5 × 2.0 × 0.2 cm3, resulting in losses such as reabsorption that are not clearly demonstrated. How to get better conversion efficiency in larger sizes of LSCs is still a very important topic. The exploration of stability and durability needs to be taken into account while obtaining higher performance, and the future progress of commercialization cannot be separated from the study of device lifetime.

Figure 4.

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(a) PL spectra of CdSe/CdS QDs-based LSCs under initial conditions and after 70 h UV irradiation, in the absence and possession of a carbon-dot-based protective layer. (Reproduced from ref (93), with permission from Copyright 2018, Royal Society of Chemistry.) (b) Absorption and emission spectra of CDs, CsPb(BrxCl1–x)3 QDs and CsPb(BrxI1–x)3 QDs. (Reproduced from ref (94), with permission from Copyright 2018, Elsevier.) (c) Photographs of CDs and AIE material-based LSCs under UV-based illumination. (Reproduced from ref (95), with permission from Copyright 2019, Royal Society of Chemistry.).

With further research on carbon dot materials, Li et al. reported CDs with red and yellow emissions for stacked LSCs (10 × 10 cm2) and achieved an energy conversion efficiency of 3.8%.96 The corresponding J–V curves and the calculated external quantum efficiencies obtained are shown in Figure 5a,b. The application of the corresponding eco-friendly CDs greatly reduces the biotoxicity problem similar to that of perovskite quantum dots and has better photostability. However, the red CDs, which are the emitters of one of the LSCs layers, show a relatively low QY (17.6%), which may be the main reason limiting the further growth of their efficiency. Chen et al. instead reported Cu4I6(pr-ted)2 nanoparticles with a QY of 92.1% and yellow CDs containing QY of nearly 91.1% to prepare stacked LSCs with dimensions of 5 × 5 × 0.2 cm3, demonstrating a high external optical efficiency of 6.40%.97 Among them, the introduction of Cu4I6(pr-ted)2 nanoparticles with good dispersion, large Stokes shift, and high QY is very innovative. The absorption and emission spectra of two of these nanoparticles are shown in Figure 5c,d. It shows that the absorption spectrum of the stacked LSCs contains 300–550 nm, while the emission spectrum ranges from 400 to 650 nm, which is a good match for the silicon solar cell. In addition, they also conducted a 14-day stability test, where the efficiency of the LSCs remained essentially unchanged, and a temperature-dependent PL spectrum was also tested to investigate the fluorescence performance of the device at the actual operating temperature. The use of multiple emitters with high QY for stacked LSCs is very promising and can effectively improve the corresponding optical conversion efficiency. However, the paper does not mention whether the conversion efficiency of larger LSCs can remain relatively stable after preparation, and we believe that the 14-days stability test is not sufficient to illustrate the durability issue, but the temperature-dependent fluorescence mapping to illustrate the temperature range of the device is very useful for the future industrialization path.

Figure 5.

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(a) Calculated and tested external optical efficiency of LSCs based on yellow-emitting CDs and red-emitting CDs. (b) The J–V curves of yellow-emitting carbon dot based LSCs, red-emitting carbon dot based LSCs, and tandem LSCs under natural sunlight. (Reproduced from ref (96), with permission from Copyright 2021, Royal Society of Chemistry.) (c,d) Absorption, PL emission, and excitation spectra of CDs and copper iodide based hybrid nanoparticles. (Reproduced from ref (97), with permission from Copyright 2022, Royal Society of Chemistry.).

4. Challenges and Future Advancements

In conclusion, we have effectively sorted out and summarized the applications of nanocrystalline materials such as perovskite quantum dots and CDs on LSCs (Table 1), which are developing relatively fast. We believe that compared with the toxicity and instability problems of the perovskite materials themselves, the environment-friendly quantum dots will appear more promising in the future commercialization of LSCs. Although we describe some quantum dots with high PLQY, large Stokes shift, and easy film formation for LSCs preparation, the limited absorption range, reabsorption loss in fluorescent materials, escape cone loss, and compatibility of fluorescent emitters with different optical waveguide media have slowed down the commercialization process. Several very critical challenges remain in the current LSCs field, and we also present our vision for the future.

Table 1. Optical Efficiencies of the LSCs with Different Fluorophores and Type.

fluorophores type absorption range (nm) PLQY (%) ηopt (%) LSC area (cm2) ref
dye tandem 400–600   16.3 5 × 5 (29)
CDs
perovskite nanoplatelets single layer 300–550 69 0.87 10 × 10 (33)
perovskite nanoplatelets single layer 350–700 56 2.0 10 × 10 (34)
perovskite-nanocrystal single layer 300–500 79 6.4 5 × 5 (43)
perovskite QDs single layer 300–550 81 6.17 2 × 2 (54)
CDs single layer 300–600 - 3.94 2 × 2 (64)
CDs tandem 300–700 60 1.1 10 × 10 (67)
CDs 30
CDs single layer 300–550 50 1.6 10 × 10 (68)
CDs single layer 300–500 65 2.7 10 × 10 (73)
CDs single layer 300–550 92.3 4.45 5 × 5 (76)
CDs single layer 250–600 49 5.89 2.5 × 2.5 (78)
CDs tandem 300–610 43.6 2.3 8 × 8 (90)
CDs 50.1
CDs 50.1
CDs tandem 300–600 15.0 4.03 5 × 5 (91)
CDs 41.5
CDs 7.6
CDs tandem 300–400 50 3 10 × 10 (94)
perovskite QDs 70
perovskite QDs 60
CDs tandem 300–550 - 3.55 6.5 × 2.5 (95)
AIE molecules
CDs tandem 300–660 86.4 4.3 10 × 10 (96)
CDs 17.6
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As far as fluorescent emitters are concerned, it should be very urgent to explore nontoxic and green fluorescent materials. As far as CDs are concerned, although the current materials are composed of nontoxic elements, the synthesis process with a large number of organic precursors, toxic solvents, and higher reaction temperatures are not meeting the conditions for green synthesis. And we should try our best to promote promising materials from laboratory preparation to industrial production scale in the future. Therefore, it is very important to explore a general green large-scale synthesis method for the current quantum dots, but not at the cost of performance loss for the sake of scale up production. It is also important to design the performance of quantum dots through the selection of precursors, and the development of emitters with higher efficiency, less absorption-emission spectral overlap, and better optical, thermal, and aqueous stability is crucial.

At present, the conversion efficiency of LSCs based on quantum dot materials is not sufficient to meet the demand of BIPV. Therefore, the exploration of novel structures of LSCs and fluorescent emitters with higher optical properties is very urgent. Current LSCs with higher than 5% conversion efficiency usually possess a very small size, which is unrealistic for subsequent practical applications. The improvement of efficiency often requires the reduction of light scattering losses and the quest for higher optical performance. One of the sources of scattering may be caused by the aggregation generated when quantum dots are dispersed in the optical waveguide material. Therefore, the subsequent high quality dispersion of quantum dots in the optical waveguide material is very important, and in the preparation of thin film type LSCs, the fluorescent layer is required to be able to be prepared on a large scale, and a certain homogeneity needs to exist, which may be prepared by the scraping method, spray deposition method or ink jet printing method, etc. Therefore, the design of surface functionalization of quantum dots and optical waveguide materials may be very important. For improving the efficiency, choosing quantum dots with high quantum yield, such as those with quantum cutting effect, or designing multiple fluorescent materials to prepare stacked LSCs to better match the best response region of solar cells are feasible solutions.

Second, as one of the limitations of LSCs is the size, a currently commonly reported large size is only 10 × 10 cm2 and usually exhibits less than 5% optical conversion efficiency. However, future BIPV applications require LSCs with a size of at least 0.5 × 0.5 m2, and even larger areas are needed for some windows. In this case, the emitted photons need to travel a very long distance, and thus the very small overlap of absorption and emission spectra can lead to very serious reabsorption losses. Therefore, the current research on very large size LSCs is very important, not only in the preparation of LSCs devices, but also in the theoretical research is very urgent. At the same time, the durability test of LSCs devices is often lacking in the current research, and the common stability test only includes 2 weeks of daily light test, which is totally insufficient. For the working characteristics of LSCs, certain technical requirements are needed in order to meet its corresponding usage conditions. (1) LSCs need to ensure a certain mechanical strength to face the complex external environment. (2) The light stability should be excellent and be able to resist the UV aging process. (3) The working life needs to be long, keeping at least 5–10 years. Although this is still a bit far from the commercialization process of LSCs, the corresponding service life needs to be more rigorously tested and made available for research.

Acknowledgments

We thank the National Natural Science Foundation of China (Grant no. 21774098) and the “111” project (Grant no. B18038) for the financial support.

Author Contributions

CRediT: Mengyan Cao formal analysis, writing-original draft, writing-review & editing; Xiujian Zhao supervision, writing-review & editing; Xiao Gong conceptualization, project administration, resources, supervision, writing-review & editing.

The authors declare no competing financial interest.

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