An official website of the United States government
Luminescent solar concentrators (LSCs) can concentrate direct and diffuse solar radiation spatially and energetically to help reduce the overall area of solar cells needed to meet current energy demands. LSCs require luminophores that absorb large fractions of the solar spectrum, emit photons into a light-capture medium with high photoluminescence quantum yields (PLQYs), and do not absorb their own photoluminescence. Luminescent nanocrystals (NCs) with near or above unity PLQYs and Stokes shifts large enough to avoid self-absorption losses are well-suited to meet these needs. In this work, we describe LSCs based on quantum-cutting Yb 3+ :CsPb(Cl 1−x Br x ) 3 NCs that have documented PLQYs as high as ∼200%. Through a combination of solution-phase 1D LSC measurements and modeling, we demonstrate that Yb 3+ :CsPbCl 3 NC LSCs show negligible intrinsic reabsorption losses, and we use these data to model the performance of large-scale 2D LSCs based on these NCs. We further propose a new and unique monolithic bilayer LSC device architecture that contains a Yb 3+ :CsPb(Cl 1−x Br x ) 3 NC top layer above a second narrower-gap LSC bottom layer ( e.g. , based on CuInS 2 NCs), both within the same waveguide and interfaced with the same Si PV for conversion. We extend the modeling to predict the flux gains of such bilayer devices. Because of the exceptionally high PLQYs of Yb 3+ :CsPb(Cl 1−x Br x ) 3 NCs, the optimized bilayer device has a projected flux gain of 63 for dimensions of 70 × 70 × 0.1 cm 3 , representing performance enhancement of at least 19% over the optimized CuInS 2 LSC alone.
more »
« less
Integration of Highly Luminescent Lead Halide Perovskite Nanocrystals on Transparent Lead Halide Nanowire Waveguides through Morphological Transformation and Spontaneous Growth in Water
Abstract The integration of highly luminescent CsPbBr3quantum dots on nanowire waveguides has enormous potential applications in nanophotonics, optical sensing, and quantum communications. On the other hand, CsPb2Br5nanowires have also attracted a lot of attention due to their unique water stability and controversial luminescent property. Here, the growth of CsPbBr3nanocrystals on CsPb2Br5nanowires is reported first by simply immersing CsPbBr3powder into pure water, CsPbBr3−γ Xγ(X = Cl, I) nanocrystals on CsPb2Br5−γ Xγnanowires are then synthesized for tunable light sources. Systematic structure and morphology studies, including in situ monitoring, reveal that CsPbBr3powder is first converted to CsPb2Br5microplatelets in water, followed by morphological transformation from CsPb2Br5microplatelets to nanowires, which is a kinetic dissolution–recrystallization process controlled by electrolytic dissociation and supersaturation of CsPb2Br5. CsPbBr3nanocrystals are spontaneously formed on CsPb2Br5nanowires when nanowires are collected from the aqueous solution. Raman spectroscopy, combined photoluminescence, and SEM imaging confirm that the bright emission originates from CsPbBr3−γ Xγnanocrystals while CsPb2Br5−γ Xγnanowires are transparent waveguides. The intimate integration of nanoscale light sources with a nanowire waveguide is demonstrated through the observation of the wave guiding of light from nanocrystals and Fabry–Perot interference modes of the nanowire cavity.
more »
« less
- PAR ID:
- 10447375
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Small
- Volume:
- 18
- Issue:
- 11
- ISSN:
- 1613-6810
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract This study presents an eco-friendly mechanochemical synthesis of cesium lead bromide (CsPbBr3), eliminating the need of organic solvents and high temperatures. The synthesized CsPbBr3powder is used to fabricate poly(methyl methacrylate) (PMMA)-CsPbBr3films and CsPbBr3nanocrystals (NCs). The photoluminescence (PL) peaks of the emission light are centered at 541 nm, 538 nm, and 514 nm for the CsPbBr3powder, PMMA-CsPbBr3films, and CsPbBr3NCs, respectively, correlating with crystal sizes of 0.96, 0.56, and 0.12μm, respectively. The PL lifetime analysis reveals decay times ( ) of (4.18, 20.08), (5.7, 46.99), and (5.81, 23.14) in the units (ns, ns) for the CsPbBr3powder, PMMA-CsPbBr3films, and CsPbBr3NCs, respectively. The PL quantum yield of the CsPbBr3NCs in toluene is 61.3%. Thermal activation energies for thermal quenching are 217.48 meV (films) and 178.15 meV (powder), indicating improved thermal stability with the PMMA encapsulation. The analysis of the PL intensity decay from water diffusion in the PMMA-CsPbBr3films yields 1.70 × 10−12m2s−1for the diffusion coefficient of water, comparable to that for water diffusion in pure PMMA. This work demonstrates a scalable, sustainable strategy for CsPbBr3synthesis and stability enhancement for optoelectronic applications.more » « less
-
Abstract The all‐inorganic metal halide perovskite CsPbX3(X = Cl, Br, and I) has received extensive attention in the field of white light‐emitting diodes (WLEDs) due to its high luminous intensity and high color purity. However, the shortcoming of poor stability directly affects the luminous performance of the WLED devices and reduces their luminous efficiency, which has become an urgent problem to be solved. Here, three‐color lead halide perovskite phosphors (blue‐emitting CsPbBr3synthesized at 20 °C (CPB‐20), green‐emitting CsPbBr3‐80 (CPB‐80)/CsPbBr3:SCN−(CPB:SCN−), and red‐emitting PEA2PbBr4(PPB)/PEA2PbBr4:Mn2+(PPB:Mn2+)) with higher stability and luminous intensity are simultaneously prepared and applied in WLEDs. Density functional theory is used to optimize the structures of CsPbBr3and PEA2PbBr4, and to calculate the work function, optical properties, and charge density difference. Not only the WLED devices with three‐color lead halide perovskite phosphors are constructed, but also WLED devices from warm white to cold white are realized by tuning the ratio of the different emissions, and a superior color quality (color rendering index of 96) and ideal correlated color temperature (CCT of 9376 K) are achieved. This work will set the stage for exploring low‐cost, environmentally friendly, high‐performance WLEDs.more » « less
-
Yb 3+ -Doped lead-halide perovskites (Yb 3+ :CsPb(Cl 1−x Br x ) 3 ) have emerged as unique materials combining strong, tunable broadband absorption with near-infrared photoluminescence quantum yields (PLQYs) approaching 200% at ambient temperature. These remarkable properties make Yb 3+ :CsPb(Cl 1−x Br x ) 3 an extremely promising candidate for spectral shaping in high-efficiency photovoltaic devices. Previous theoretical assessments of such “downconversion” devices have predicted single-junction efficiencies up to 40%, but have been highly idealized. Real materials like Yb 3+ :CsPb(Cl 1−x Br x ) 3 have practical limitations such as constrained band-gap and PL energies, non-directional emission, and an excitation-power-dependent PLQY. Hence, it is unclear whether Yb 3+ :CsPb(Cl 1−x Br x ) 3 , or any other non-ideal quantum-cutting material, can indeed boost the efficiencies of real high-performance PV. Here, we examine the thermodynamic, detailed-balance efficiency limit of Yb 3+ :CsPb(Cl 1−x Br x ) 3 on different existing PV under real-world conditions. Among these, we identify silicon heterojunction technology as very promising for achieving significant performance gains when paired with Yb 3+ :CsPb(Cl 1−x Br x ) 3 , and we predict power-conversion efficiencies of up to 32% for this combination. Surprisingly, PL saturation does not negate the improved device performance. Calculations accounting for actual hourly incident solar photon fluxes show that Yb 3+ :CsPb(Cl 1−x Br x ) 3 boosts power-conversion efficiencies at all times of day and year in two representative geographic locations. Predicted annual energy yields are comparable to those of tandem perovskite-on-silicon technologies, but without the need for current matching, tracking, or additional electrodes and inverters. In addition, we show that band-gap optimization in real quantum cutters is inherently a function of their PLQY and the ability to capture that PL. These results provide key design rules needed for development of high-efficiency quantum-cutting photovoltaic devices based on Yb 3+ :CsPb(Cl 1−x Br x ) 3 .more » « less
-
Abstract The disproportionation of H2O into solar fuels H2and O2, or water splitting, is a promising strategy for clean energy harvesting and storage but requires the concerted action of absorption of photons, separation of excitons, charge diffusion to catalytic sites and catalysis of redox processes. It is increasingly evident that the rational design of photocatalysts for efficient water splitting must employ hybrid systems, where the different components perform light harvesting, charge separation and catalysis in tandem. In this topical review, we report on the recent development of a new class of hybrid photocatalysts that employs MxV2O5(M = p-block cation) nanowires in order to engineer efficient charge transfer from the photoactive chalcogenide quantum dots (QDs) to the water-splitting and hydrogen evolving catalysts. Herein, we summarize the oxygen-mediated lone pair mechanism used to modulate the energy level and orbital character of mid-gap states in the MxV2O5nanowires. The electronic structure of MxV2O5is discussed in terms of density functional theory and hard x-ray photoelectron spectroscopy (HAXPES) measurements. The principles of HAXPES are explained within the context of its unique sensitivity to metal 5(6)s orbitals and ability to non-destructively study buried interface alignments of quantum dot decorated nanowires i.e., MxV2O5/CdX (X = S, Se, Te). We illustrate with examples how the MxV2O5/CdX band alignments can be rationally engineered for ultra-fast charge-transfer of photogenerated holes from the quantum dot to the nanowires; thereby suppressing anodic photo-corrosion in the CdX QDs and enabling efficacious hydrogen evolution.more » « less
