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1.
Nano Lett ; 24(37): 11722-11729, 2024 Sep 18.
Artículo en Inglés | MEDLINE | ID: mdl-39248378

RESUMEN

Graphene quantum dots (GQDs) commonly suffer from the fluorescence problem of aggregation-caused quenching under high-concentration loading or in the solid state, which seriously hinders the application. Here we report a type of GQDs with red aggregation-induced enhanced emission (AIEE). It is confirmed that the aggregation state of the AIEE GQDs is a J-aggregate. The GQDs/poly(methyl methacrylate) film presented a photoluminescence quantum yield as high as 60.81%, and the record-high performance of luminescent solar concentrators (LSCs) was achieved. The power conversion efficiency (ηPCE) is up to 8.35% and the external optical efficiency (ηext) is ∼8.99% for the GQD-based LSCs (45 mW/cm2). Even under one sun illumination (100 mW/cm2), the corresponding ηPCE and ηext values are 3.12% and 4.52%, respectively. The internal photon efficiency (ηint) of an LSC device is about 5.02%. The synthesis of AIEE GQDs bridges the research gap in the emission mechanism of AIEE in GQDs.

2.
Adv Sci (Weinh) ; 11(35): e2400540, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-39010670

RESUMEN

The growing prevalence of Internet of Things (IoT) devices hinges on resolving the challenge of powering sensors and transmitters. Addressing this, supply-less IoT devices are gaining traction by integrating energy harvesters. This study introduces a temperature sensor devoid of external power sources, achieved through a novel luminescent solar concentrator (LSC) device based on a stretchable, adhesive elastomer. Leveraging a lanthanide-doped styrene-ethylene-butylene-styrene matrix, the LSC yielded 0.09% device efficiency. The resultant temperature sensor exhibits a thermal sensitivity of 2.1%°C-1 and a 0.06 °C temperature uncertainty, autonomously transmitting real-time data to a server for user visualization via smartphones. Additionally, the integration of LED-based lighting enables functionality in low-light conditions, ensuring 24 h cycle operation and the possibility of having four distinct thermometric parameters without changing the device configuration, stating remarkable robustness and reliability of the system.

3.
ACS Appl Mater Interfaces ; 16(21): 27587-27595, 2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38748924

RESUMEN

Optimizing the photon spectrum for photosynthesis concurrently with improving crop yields presents an efficient and sustainable pathway to alleviate global food shortages. Luminescent solar concentrators (LSCs), consisting of transparent host matrices doped with fluorophores, show excellent promise to achieve the desired spectral tailoring. However, conventional LSCs are predominantly engineered for photon concentration, which results in a limited outcoupling efficiency of converted photons. Here, we introduce a scheme to implement LSCs into horticulture (HLSC) by enhancing light extraction. The symmetry of the device is disrupted by incorporating microcone arrays on the bottom surface to mitigate total internal reflection. Both Monte Carlo ray tracing simulations and experimental results have verified that the greatest enhancements in converted light extraction, relative to planar LSCs, are achieved using microcone arrays (base width 50 µm, aspect ratio 1.2) with extruded and protruded profiles (85.15 and 66.55% improvement, respectively). Angularly resolved transmission measurements show that the HLSC device exhibits a broad angular radiation distribution. This characteristic indicates that the HLSC device emits diffuse light, which is conducive to optimal plant growth.

4.
ACS Appl Mater Interfaces ; 16(11): 14072-14081, 2024 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-38442356

RESUMEN

Conventional luminescent solar concentrators (LSCs) usually only have the ability to absorb solar energy and convert it to electricity but are not able to regulate the transmitted light. Herein, a multistate thermoresponsive smart window (SW) based on LSC has been fabricated, in which the stimuli-responsive host layer consists of polydimethylsiloxane (PDMS) and ethylene glycol solution (EGS) microdroplets stacking with LSC layer-based on near-infrared (NIR) CuInSe2-xSx/ZnS core/shell quantum dots (QDs) and PDMS matrix. As-synthesized CISSe/ZnS QDs with broad NIR absorption in LSC exhibit controllable emission spectra over 833-1088 nm and high photoluminescence (PL) quantum yield from 45 to 83%. Coupling with Si solar cells as a reference, optimized LSC-SW devices with dimensions of 5 × 5 × 0.9 cm3 exhibit higher power conversion efficiency (PCE) of 1.19-1.36% with increased temperature from 0 to 50 °C than those of sole LSC and SW devices. The corresponding visible light transmissions are regulated from 75.1 to 48.1% accordingly. The improvement of PCEs in an opaque state is mainly due to enhanced absorption of QDs originating from rescattered photons from the EGS/PDMS layer, leading to more emitted photons reaching photovoltaics. This work is expected to bring up new opportunities for applications in greenhouses, building facades, and energy-efficient smart windows.

5.
Macromol Rapid Commun ; 45(12): e2300724, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38485136

RESUMEN

Luminescent solar concentrators (LSCs) are spectral conversion devices offering interesting opportunities for the integration of photovoltaics into the built environment and portable systems. The Förster-resonance energy transfer (FRET) process can boost the optical response of LSCs by reducing energy losses typically associated to non-radiative processes occurring within the device under operation. In this work, a new class of FRET-based thin-film LSC devices is presented, in which the synthetic versatility of linear polyurethanes (PU) is exploited to control the photophysical properties and the device performance of the resulting LSCs. A series of luminescent linear PUs are synthesized in the presence of two novel bis-hydroxyl-functionalized luminophores of suitable optical properties, used as chain extenders during the step-growth polyaddition reaction for the formation of the linear macromolecular network. By synthetically tuning their composition, the obtained luminescent PUs can achieve a high energy transfer efficiency (≈90%) between the covalently linked luminophores. The corresponding LSC devices exhibit excellent photonic response, with external and internal photon efficiencies as high as ≈4% and ≈37%, respectively. Furthermore, their optimized power conversion efficiency combined with their enhanced average visible-light transmittance highlight their suitability for potential use as transparent solar energy devices.


Asunto(s)
Transferencia de Energía , Transferencia Resonante de Energía de Fluorescencia , Poliuretanos , Energía Solar , Poliuretanos/química , Luminiscencia , Estructura Molecular
6.
Sci Rep ; 14(1): 4160, 2024 Feb 20.
Artículo en Inglés | MEDLINE | ID: mdl-38378849

RESUMEN

Building-integrated photovoltaics (BIPV) is an emerging technology in the solar energy field. It involves using luminescent solar concentrators to convert traditional windows into energy generators by utilizing light harvesting and conversion materials. This study investigates the application of machine learning (ML) to advance the fundamental understanding of optical material design. By leveraging accessible photoluminescent measurements, ML models estimate optical properties, streamlining the process of developing novel materials, offering a cost-effective and efficient alternative to traditional methods, and facilitating the selection of competitive materials. Regression and clustering methods were used to estimate the optical conversion efficiency and power conversion efficiency. The regression models achieved a Mean Absolute Error (MAE) of 10%, which demonstrates accuracy within a 10% range of possible values. Both regression and clustering models showed high agreement, with a minimal MAE of 7%, highlighting the efficacy of ML in predicting optical properties of luminescent materials for BIPV.

7.
Artículo en Inglés | MEDLINE | ID: mdl-37922121

RESUMEN

Reabsorption-free luminescent solar concentrators (LSCs) are crucial ingredients for photovoltaic windows. Atomically precise metal nanoclusters (NCs) with large Stokes-shifted photoluminescence (PL) hold great promise for applications in LSCs. However, a fundamental understanding of the PL mechanism, particularly on the excited-state interaction and exciton kinetics, is still lacking. Herein, we studied the exciton-phonon coupling and singlet/triplet exciton dynamics for gold-doped silver NCs in a solid matrix. Following photoexcitation, the excitons can be self-trapped via strong exciton-phonon coupling. Subsequently, rapid thermal equilibration between the singlet and triplet states occurs due to the coexistence of small energy splitting and spin-orbit coupling. Finally, broadband delayed fluorescence with a large Stokes shift can be generated, namely, self-trapped, thermally equilibrated delayed fluorescence (ST-TEDF). Benefiting from superior ST-TEDF, we demonstrated efficient LSCs with minimized reabsorption.

8.
ACS Nano ; 17(23): 23512-23523, 2023 Dec 12.
Artículo en Inglés | MEDLINE | ID: mdl-37815407

RESUMEN

Luminescent solar concentrators (LSCs) have proven to be highly effective in enhancing the conversion efficiency of photovoltaic (PV) cells. However, the traditional LSCs always suffer from self-absorption and escape the losses of luminescence. To these challenges, this study presents an ingenious all-wood-based LSC (W-LSC) with directional light-concentrating capabilities. By converting lignin into fluorescent carbon quantum dots (CQDs) and integrating them into transparent cellulose channels in delignified wood, we achieved efficient directional luminescence transmission in the W-LSC is achieved. The synthesized lignin-based CQDs (L-CQDs) exhibited a large Stokes shift (0.63 eV) and a bright yellow emission (540 nm). The prepared W-LSC possessed an external optical efficiency (ηopt) along the longitudinal (L) direction of 4.60% under a low irradiation intensity (40 mW·cm-2). Besides, contributed to the low thermal conductivity (0.300 W·m-1·K-1) of wood, the W-LSC maintained an ηopt of 4.03% at a temperature of 65 °C. Furthermore, the W-LSC demonstrated high tensile strength (424 MPa) and light transmission (85%). By leveraging the advantages of wood, this approach provides a different solution for enhancing solar energy utilization and advancing sustainable building.

9.
Nanomaterials (Basel) ; 13(17)2023 Sep 02.
Artículo en Inglés | MEDLINE | ID: mdl-37686987

RESUMEN

Luminescent solar concentrators (LSCs) have become an attractive way to produce green energy via their integration into buildings as photovoltaic windows. Recently, carbon quantum dots (C-QDs) have become the most studied luminescent material for the manufacture of luminescent solar concentrators due to their advantages, such as low toxicity, sustainability, and low cost. Despite the advantages of carbon quantum dots, they remain a low-efficiency material, and it is difficult to fabricate LSCs with a good performance. To address this problem, some of the research has used SiO2 nanoparticles (Nps) to produce a light-scattering effect that helps to improve the system performance. However, these studies are limited and have not been discussed in detail. In this regard, this research work was designed to evaluate the contribution of the scattering effect in different systems of carbon quantum dots used in a possible luminescent solar concentrator. To carry out this study, C-QDs and SiO2 Nps were synthesized by hydrothermal methods and the Stober method, respectively. We used different concentrations of both materials to fabricate film LSCs (10 × 10 cm2). The results show that the light scattered by the SiO2 Nps has a double contribution, in terms of light redirected towards the edges of the window and as a secondary source of excitation for the C-QDs; thus, an improvement in the performance of the LSC is achieved. The best improvement in photoluminescence is achieved when the films are composed of 20% wt carbon quantum dots and 10% wt SiO2 Nps, reaching a gain of 16% of the intensity of the light incident on the edges of the window with respect to the LSCs where only C-QDs were used.

10.
Nano Lett ; 23(10): 4367-4374, 2023 May 24.
Artículo en Inglés | MEDLINE | ID: mdl-37141490

RESUMEN

Space-based solar power harvesting systems with high levels of specific power (the power produced per mass of the mounted photovoltaic cell) are highly desired. In this study, we synthesized high quality lead-free Cs3Cu2Cl5 perovskite nanodisks with efficient ultraviolet (UV) photon absorption, high photoluminescence quantum yields, and a large Stokes shift, which are suitable to serve as photon energy downshifting emitters in the applications of photon-managing devices especially for space solar power harvesting. To demonstrate this possibility, we have fabricated two types of photon-managing devices, i.e., luminescent solar concentrators (LSCs) and luminescent downshifting (LDS) layers. Both experimental results and simulation analyses show that the fabricated LSC and LDS devices exhibit high visible light transmission, low photon scattering and reabsorption energy loss, high UV photon harvesting, and energy conversion after integrating with silicon-based photovoltaic cells. Our research presents a new avenue for utilizing lead-free perovskite nanomaterials in space applications.

11.
ACS Appl Mater Interfaces ; 15(14): 17914-17921, 2023 Apr 12.
Artículo en Inglés | MEDLINE | ID: mdl-36975316

RESUMEN

Luminescent solar concentrators (LSCs) concentrate light via luminescence within a planar-waveguide and have potential use for building-integrated photovoltaics. However, their commercialization and potential applications are currently hindered greatly by photon reabsorption, where emitted waveguided light is parasitically reabsorbed by a luminophore. Nanotetrapod semiconductor materials have been theorized to be excellent luminophores for LSCs owing to their inherently large Stokes shifts. Here we present the first nanotetrapod-based LSCs (5 × 5 × 0.3 cm3) reported in the literature. External quantum efficiencies as high as 4.9 ± 0.5% were achieved under AM1.5G conditions. We also perform an in-depth investigation by optical characterization of the different operational metrics of our nanotetrapod-based LSCs and show reabsorption to be eliminated (mean number of average reabsorption events per photon equal to 0.00) in our most extended nanotetrapod devices.

12.
ACS Appl Mater Interfaces ; 15(6): 8377-8386, 2023 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-36722461

RESUMEN

Photon upconversion (UC) based on triplet-triplet annihilation is a very promising phenomenon with potential application in several areas, though, due to the intrinsic mechanism, the achievement of diffusion-limited solid materials with air-stable UC is still a challenge. Herein, we report UC coordination polymer nanoparticles (CPNs) combining sensitizer and emitter molecules especially designed with alkyl spacers that promote the amorphous character. Beyond the characteristic constraints of crystalline MOFs, amorphous CPNs facilitate high dye density and flexible ratio tunability. To show the universality of the approach, two types of UC-CPNs are reported, exhibiting highly photostable UC in two different visible spectral regions. Given their nanoscale, narrow size distribution, and good chemical/colloidal stability in water, the CPNs were also successfully printed as anticounterfeiting patterns and used to make highly transparent and photostable films for luminescent solar concentrators, both showing air-stable UC.

13.
Materials (Basel) ; 16(2)2023 Jan 10.
Artículo en Inglés | MEDLINE | ID: mdl-36676393

RESUMEN

Luminescent solar concentrators (LSCs) have been extensively studied as they offer a practical solution to increase the efficiency of silicon-based photovoltaics (PVs). In this context, the use of natural and organic luminescent materials is desirable in order to obtain sustainable and environmentally friendly devices. Moreover, solution-processable organic host-guest systems based on Foerster Resonant Energy Transfer (FRET) processes offer the possibility to exploit a low-cost technique to obtain an efficient energy downshift from the UV-visible to red or deep red emissions in order to concentrate the radiation in the area of maximum efficiency of the PV device. Nevertheless, organic materials are subjected to photodegradation that reduces their optical properties when exposed to UV light and oxygen. In this work, we incorporated two different antioxidant molecules (i.e., octadecyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate (Octa) and L-ascorbic acid (L-Asc)) in a three-dye host-guest system and studied the corresponding optical properties after prolonged irradiation times in air. It was found that the presence of the antioxidants, especially L-Asc, slowed the system's photodegradation down whilst at the same time retaining high emission efficiencies and without interfering with the cascade Resonant Energy Transfer processes among the dyes inserted in the nanochannels of the host.

14.
ACS Photonics ; 10(9): 3195-3202, 2023 Sep 20.
Artículo en Inglés | MEDLINE | ID: mdl-39071812

RESUMEN

Organic luminophores offer great potential for energy harvesting and light emission due to tunable spectral properties, strong luminescence, high solubility, and excellent wavelength-selectivity. To realize their full potential, the lifetimes of luminophores must extend to many years under illumination. Many organic luminophores, however, have a tendency to degrade and undergo rapid photobleaching, leading to the perception of intrinsic instability of organic molecules. In this work we demonstrate that by exchanging the counterion of a heptamethine cyanine salt the photostability and corresponding lifetime of dilute cyanine salts can be enhanced by orders of magnitude from 10 hours to an extrapolated lifetime of greater than 65,000 hours under illumination. To help correlate and comprehend the underlying mechanism behind this phenomenon, the water contact angle and binding energy of each pairing were measured and calculated. We find that increased water contact angle, and therefore increasing hydrophobicity, generally correlate to improved lifetimes. Similarly, a lower absolute binding energy between cation and anion correlates to increased lifetimes. Utilizing the binding energy formalism, we predict the stability of a new anion and experimentally verify with good consistency. Moving forward, these factors could be used to rapidly screen and identify highly photostable organic luminophore salt systems for a range of energy harvesting and light emitting applications.

15.
ACS Appl Mater Interfaces ; 14(39): 44572-44580, 2022 Oct 05.
Artículo en Inglés | MEDLINE | ID: mdl-36125906

RESUMEN

Luminescent solar concentrators (LSCs) can be used as large-area sunlight collectors, which show great potential in the application of building-integrated photovoltaic areas. Achieving highly efficient LSCs requires the suppression of reabsorption losses while maintaining a high photoluminescence quantum yield (PLQY) and broad absorption. Perovskites as the superstar fluorophores have recently emerged as candidates for large-area LSCs. However, highly emissive perovskites with a large Stokes shift and broad absorption have not been obtained up to now. Here, we devised a facile synthetic route to obtain Mn-doped multiple quantum well (MQW) Br-based perovskites. The Br-based perovskite host ensures broad absorption. Efficient energy transfer from the exciton to the Mn dopant produces a large Stokes shift and high PLQY simultaneously. By further coating the perovskites with Al2O3, the stability and PLQY are greatly elevated. A large area of liquid LSC (40 cm × 40 cm × 0.5 cm) is fabricated, which possesses an internal quantum efficiency (ηint) of 47% and an optical conversion efficiency (ηopt) reaching 11 ± 1%, which shows the highest value for large-area LSCs.

16.
ACS Appl Mater Interfaces ; 14(36): 41013-41021, 2022 Sep 14.
Artículo en Inglés | MEDLINE | ID: mdl-36044296

RESUMEN

Luminescent solar concentrators (LSCs) are a class of wave-guiding devices that can harvest solar light and concentrate it to targeted smaller areas. When coupled with photovoltaic devices (PVs), LSCs hold the potential to be integrated into various application setups, especially for building facade integration toward net-zero-energy buildings. Developing reliable LSC fabrication methods with easy scalability, high adaptability, and device controllability has been an important research topic. In this work, we report an ultrasonic nebulization-assisted spray deposition technique to fabricate quantum dot (QD)-based LSCs (QD-LSCs). This method allows for the production of high-performance QD-LSCs with different device dimensions and geometries. In addition, the quality of the QD thin-film coating layer is relatively independent of the concentration and volume of the coating QD ink solution, allowing for deliberate programming and performance optimization of the resulting QD-LSC devices. We anticipate that this ultrasonic spray coating method can be widely applied to the manufacturing of high-quality LSC devices that are integrable to various applications.

17.
Nanomaterials (Basel) ; 12(10)2022 May 23.
Artículo en Inglés | MEDLINE | ID: mdl-35630995

RESUMEN

In recent years, rare-earth metals with triply oxidized state, lanthanide ions (Ln3+), have been demonstrated as dopants, which can efficiently improve the optical and electronic properties of metal halide perovskite materials. On the one hand, doping Ln3+ ions can convert near-infrared/ultraviolet light into visible light through the process of up-/down-conversion and then the absorption efficiency of solar spectrum by perovskite solar cells can be significantly increased, leading to high device power conversion efficiency. On the other hand, multi-color light emissions and white light emissions originated from perovskite nanocrystals can be realized via inserting Ln3+ ions into the perovskite crystal lattice, which functioned as quantum cutting. In addition, doping or co-doping Ln3+ ions in perovskite films or devices can effectively facilitate perovskite film growth, tailor the energy band alignment and passivate the defect states, resulting in improved charge carrier transport efficiency or reduced nonradiative recombination. Finally, Ln3+ ions have also been used in the fields of photodetectors and luminescent solar concentrators. These indicate the huge potential of rare-earth metals in improving the perovskite optoelectronic device performances.

18.
Nanotechnology ; 33(30)2022 May 04.
Artículo en Inglés | MEDLINE | ID: mdl-35395655

RESUMEN

The enhancement of photoluminescence (PL) emission and waveguide play a key role in improving the optical efficiency of luminescent solar concentrators (LSCs). In this work, to boosting PL emission and waveguide simultaneously, one photonic crystal (PC) structure (crystalline colloid arrays (CCAs)) was introduced into carbon dots (CDs)-based polymer LSCs. A sandwich-structured CDs-based polymer photonic LSC, comprising glass/CDs-based polymer PC film/glass, was created. First, CDs-based colloidal crystal suspensions were prepared by co-assembly of monodispersed p(MMA-NIPAm) colloids and multicolor-emitting CDs in HEMA monomer induced by the evaporation-driven assembly. The obtained suspensions not only had uniform PL and structural colors, but showed enhanced PL emission. Second, the above suspensions were sandwiched between two glass sheets and finally a photonic polymer LSC with sandwiched structure (25 × 25 × 1.8 mm3) were formed via one-step photopolymerization technique. Remarkably, the optimal CDs-based polymer photonic LSCs with sandwiched structure not only had high transparence at visible range (>60%), but exhibited PL emission enhancement (at least 2 times). Furthermore, the maximum external optical efficiency (ηopt) of 5.84% could be achieved based on yellow-emitting CDs-based polymer photonic LSC. The high external optical efficiency was mainly attributed to the PL emission enhancement and good PC waveguide.

19.
ACS Nano ; 16(3): 3994-4003, 2022 Mar 22.
Artículo en Inglés | MEDLINE | ID: mdl-35234037

RESUMEN

Carbon-based nanomaterials hold promise for eco-friendly alternatives to heavy-metal-containing quantum dots (QDs) in optoelectronic applications. Here, boric acid-functionalized graphene quantum dots (B-GQDs) were prepared using bottom-up molecular fusion based on nitrated pyrenes and boric acid. Such B-GQDs with crystalline graphitic structures and hydrogen-bonding functionalities would be suitable model systems for unraveling the photoluminescence (PL) mechanism, while serving as versatile building blocks for supramolecular self-assembly. Unlike conventional GQDs with multiple emissive states, the B-GQDs exhibited excitation-wavelength-independent, vibronic-coupled excitonic emission. Interestingly, their PL spectra can be tuned without largely sacrificing the quantum yield (QY) due to two-dimensional self-assembly. In addition, such B-GQDs in a polystyrene matrix possessed an ultrahigh QY (∼90%) and large exciton binding energy (∼300 meV). Benefiting from broadband absorption, ultrahigh QY, and long-wavelength emission, efficient laminated luminescent solar concentrators (100 × 100 × 6.3 mm3) were fabricated, yielding a high power conversion efficiency (1.4%).

20.
Polymers (Basel) ; 14(3)2022 Jan 28.
Artículo en Inglés | MEDLINE | ID: mdl-35160519

RESUMEN

Light-harvesting concentrators have a high potential to make highly efficient but precious energy converters, such as multijunction photovoltaics, more affordable for everyday applications. They collect sunlight, including diffusively scattered light, on large areas and redirect it to much smaller areas of the highly efficiency solar cells. Among the best current concepts are pools of randomly oriented light-collecting donor molecules that transfer all excitons to few aligned acceptors reemitting the light in the direction of the photovoltaics. So far, this system has only been realized for the 350-550 nm wavelength range, suitable for AlGaInP photovoltaics. This was achieved by using acceptor molecules that aligned during mechanical stretching of polymers together with donors, that stay random in that very same material and procedure. However, until recently, very little was known about the factors that are responsible for the alignability of molecules in stretched polymers and therefore it was difficult to find suitable donors and acceptors, as well as for other spectral ranges. Recently, a structural parameter was introduced with a high predictivity for the alignability of molecules that contain rigid band-like structures or linear aromatic π-systems. However, for light concentrators in more red spectral ranges, molecular systems often contain larger and extended, planar-like π-systems for which the previously reported parameter is not directly applicable. Here, we present a refined prediction parameter also suitable for larger plane-like structures. The new parameter depends on the number of in-plane atoms divided by out-of-plane atoms as determined by computational geometry optimization and additionally the planar aspect ratio for molecules that contain only in-plane atoms. With the help of this parameter, we found a new system that can efficiently collect and redirect light for the second 500-700 nm AlGaAs layer of current world-record multijunction photovoltaics. Similarly, as the previously reported system for the blue-green layer, it has also overall absorption and re-directioning quantum efficiencies close to 80-100%. Both layers, together, already cover about 75% of the energy in the solar spectrum.

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