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.
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Promoting solution-phase superlattices of CsPbBr 3 nanocrystals
We present a size-selective method for purifying and isolating perovskite CsPbBr 3 nanocrystals (NCs) that preserves their as-synthesized surface chemistry and extremely high photoluminescence quantum yields (PLQYs). The isolation procedure is based on the stepwise evaporation of nonpolar co-solvents with high vapor pressure to promote precipitation of a size-selected product. As the sample fractions become more uniform in size, we observe that the NCs self-assemble into colloidally stable, solution-phase superlattices (SLs). Small angle X-ray scattering (SAXS) and dynamic light scattering (DLS) studies show that the solution-phase SLs contain 1000s of NCs per supercrystal in a simple cubic, face-to-face packing arrangement. The SLs also display systematically faster radiative decay dynamics and improved PLQYs, as well as unique spectral absorption features likely resulting from inter-particle electronic coupling effects. This study is the first demonstration of solution-phase CsPbBr 3 SLs and highlights their potential for achieving collective optoelectronic phenomena previously observed from solid-state assemblies.
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- Award ID(s):
- 2131408
- PAR ID:
- 10436719
- Publisher / Repository:
- Nanoscale
- Date Published:
- Journal Name:
- Nanoscale
- Volume:
- 15
- Issue:
- 22
- ISSN:
- 2040-3364
- Page Range / eLocation ID:
- 9728 to 9737
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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