A hierarchical shell locks and stabilizes perovskite nanocrystals with near-unity quantum yield.
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| Title: | A hierarchical shell locks and stabilizes perovskite nanocrystals with near-unity quantum yield. |
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| Authors: | Zeng, Qingsen (AUTHOR), Zhao, Yue (AUTHOR), Park, Sunghee (AUTHOR), Zhou, Huanyu (AUTHOR), Shim, Hyun-Joon (AUTHOR), Li, Tianshu (AUTHOR), Ryu, Jinseok (AUTHOR), Sung, Min-Jun (AUTHOR), Chua, Xian Wei (AUTHOR), Yoon, Eojin (AUTHOR), Lewis, Barney A. I. (AUTHOR), Woo, Seung-Je (AUTHOR), Forzatti, Michele (AUTHOR), Kim, Min Ju (AUTHOR), Kim, Eun A. (AUTHOR), Dai, Linjie (AUTHOR), Jang, Jinhyeong (AUTHOR), Tang, Yipeng (AUTHOR), Kweon, Jin Jung (AUTHOR), Chen, Hao (AUTHOR) |
| Source: | Science. 1/15/2026, Vol. 391 Issue 6782, p1-10. 10p. |
| Subjects: | Perovskite, Nanocrystals, Photoluminescence, Stability (Mechanics), Light emitting diodes, Quantum efficiency |
| Abstract: | Solid-state emitters have exhibited external quantum yields (EQYs) below 65%, with no system combining unity photoluminescence quantum yield (PLQY) and commercially viable stability. These limitations are most pronounced in colloidal perovskite nanocrystals (PeNCs), given their soft ionic lattices and labile surfaces. We introduce a hierarchical shell (HS) structure comprising interbonded PbSO4-SiO2-polymer multilayers that simultaneously locks and stabilizes soft lattices and labile interfaces. HS-CsPbBr3 PeNC films exhibit T90 (10% PLQY loss) = 3211 hours under accelerated 60°C, 90% relative humidity (RH) and T90 = 12,000 hours under blue-light exposure. HS strategy generalizes across PeNC compositions—including mixed-halide, mixed-cation, iodide, and hybrid PeNCs—and enables MAPbBr3 with extended T90 = 3900 hours (60°C, 90% RH) and T90 = 27,234 hours (blue light). Moreover, HS-MAPbBr3 films with 100.0% PLQY eliminate self-absorption losses and achieve an EQY of 91.4%, approaching the theoretical maximum. The HS barrier also prevents lead leakage for safety of large-area, high-resolution displays and bio-optoelectronics. Editor's summary: A hierarchical shell (HS) with lead sulfate, silica, and polymer layers realized both high photoluminescent quantum yields and long lifetimes from perovskite nanocrystals. Zeng et al. show that these interbonded shells locked the nanocrystal surface and suppressed lattice softening, ion migration, and interfacial reactions (see the Perspective by Wei and Yuan). Films of HS cesium lead bromide nanocrystal films had only a 10% photoluminescent quantum yield loss after about 3200 hours at 60°C and 90% relative humidity. The HS shells minimized self-adsorption loss, and methylammonium lead bromide films exhibited 100% photoluminescent quantum yield. —Phil Szuromi INTRODUCTION: Luminescent materials have powered advances in various applications, including displays, lighting, sensing, imaging, and optical communication. Solid-state light emitters must exhibit both strong absorption and high photoluminescence quantum yield (PLQY) to maximize light-conversion efficiency. However, almost all known emitters exhibit concentration-induced quenching and self-absorption when integrated into dense solid films, fundamentally limiting external quantum yield (EQY; PLQY × absorptance) and light-conversion efficiency. Consequently, more than 2000 terawatt-hours of electricity are wasted annually in lighting and display technologies because of suboptimal electro-optical conversion, corresponding to ~8% of global electricity consumption. Colloidal perovskite nanocrystals (PeNCs) possess high absorption coefficients and intrinsically high PLQY, making them promising light-conversion materials. Yet their soft ionic lattices and labile surfaces undergo light-, heat-, and moisture-induced structural and chemical degradation. Achieving near-unity PLQY with commercially viable stability remains a central challenge. RATIONALE: Recent findings in bulk perovskites indicated that photo- or thermal-induced lattice expansion softens the crystal lattice and accelerates defect formation. However, how this lattice-softening couples with surface reactions in colloidal PeNC solids has remained unclear. We identify that PeNC degradation proceeds through a lattice-interface interlinked pathway, in which lattice expansion weakens ionic bonding, enhances ion migration, and facilitates surface oxidation and hydration reactions. Therefore, a stabilization strategy must simultaneously lock the lattice and chemically stabilize the surface rather than act only as a passive barrier. RESULTS: We introduce a hierarchical shell (HS) composed of interbonded PbSO4-SiO2-siloxane layers. This structure forms a lattice-interface interlocking network that locks the ionic lattice and stabilizes surface chemistry. HS inorganic PeNC (HS-CsPbBr3) films show a time for 10% PLQY loss (T90) of 3211 hours at 60°C, 90% relative humidity (RH) and 12,000 hours under continuous blue-light illumination, indicating long-term stability relevant for potential commercial applications. The HS strategy is compositionally general and scalable, enabling stable emission across 409 to 783 nm, including mixed-halide and hybrid perovskite formulations. Furthermore, HS organic-inorganic hybrid PeNC (HS-MAPbBr3) showing pure-green emission, a composition that is typically highly vulnerable to moisture and heat, exhibits extended humid-thermal and photostability lifetimes, surpassing T90 = 3900 hours and estimated T90 = 27,234 hours, respectively. HS-MAPbBr3 PeNC films also achieve 100.0% PLQY (average 98.6%), turning self-absorption into efficient photon recycling. A 20 wt % HS-MAPbBr3 film achieves EQY = 91.4%, approaching the theoretical limit and surpassing previously reported solid-state emitters. The HS structure prevents lead leakage and supports roll-to-roll coating, inkjet printing, and >3500 pixels per inch photolithographic patterning for high-resolution display demonstrations. CONCLUSION: The HS provides an interbonded stabilization framework that locks the lattice and stabilizes the interface, suppressing the lattice-interface interlinked degradation pathway. This approach enables near-unity PLQY, converts reabsorption into photon recycling, and achieves photoluminescence stability compatible with commercial use. Owing to broad compositional compatibility and patterning scalability, HS-PeNCs are well-suited for large-area displays (such as 75-inch televisions), mid-size tablets (~10 inch), and high-resolution microdisplays for augmented- and virtual-reality systems, as well as for solid-state lighting and bio-optoelectronic modules (for example, photoplethysmography sensing). More broadly, the lattice-interface interlocking concept provides a generalizable stabilization strategy for halide perovskite materials and related optoelectronic devices. A HS enables lattice-interface interlocking, transforming colloidal perovskite nanocrystals into commercially viable solid-state emitters.: The interbonded PbSO4-SiO2-polymer layers confine lattice expansion and stabilize the surface, suppressing soft-lattice–driven degradation. As a result, HS-PeNC films maintain near-unity PLQY with efficient photon recycling and achieve an external quantum yield of 91.4%, alongside commercially viable stability (T90 > 3000 hours at 60°C, 90% RH; T90 > 27,000 hours under blue-light exposure). [ABSTRACT FROM AUTHOR] |
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| Database: | Psychology and Behavioral Sciences Collection |
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| Abstract: | Solid-state emitters have exhibited external quantum yields (EQYs) below 65%, with no system combining unity photoluminescence quantum yield (PLQY) and commercially viable stability. These limitations are most pronounced in colloidal perovskite nanocrystals (PeNCs), given their soft ionic lattices and labile surfaces. We introduce a hierarchical shell (HS) structure comprising interbonded PbSO4-SiO2-polymer multilayers that simultaneously locks and stabilizes soft lattices and labile interfaces. HS-CsPbBr3 PeNC films exhibit T90 (10% PLQY loss) = 3211 hours under accelerated 60°C, 90% relative humidity (RH) and T90 = 12,000 hours under blue-light exposure. HS strategy generalizes across PeNC compositions—including mixed-halide, mixed-cation, iodide, and hybrid PeNCs—and enables MAPbBr3 with extended T90 = 3900 hours (60°C, 90% RH) and T90 = 27,234 hours (blue light). Moreover, HS-MAPbBr3 films with 100.0% PLQY eliminate self-absorption losses and achieve an EQY of 91.4%, approaching the theoretical maximum. The HS barrier also prevents lead leakage for safety of large-area, high-resolution displays and bio-optoelectronics. Editor's summary: A hierarchical shell (HS) with lead sulfate, silica, and polymer layers realized both high photoluminescent quantum yields and long lifetimes from perovskite nanocrystals. Zeng et al. show that these interbonded shells locked the nanocrystal surface and suppressed lattice softening, ion migration, and interfacial reactions (see the Perspective by Wei and Yuan). Films of HS cesium lead bromide nanocrystal films had only a 10% photoluminescent quantum yield loss after about 3200 hours at 60°C and 90% relative humidity. The HS shells minimized self-adsorption loss, and methylammonium lead bromide films exhibited 100% photoluminescent quantum yield. —Phil Szuromi INTRODUCTION: Luminescent materials have powered advances in various applications, including displays, lighting, sensing, imaging, and optical communication. Solid-state light emitters must exhibit both strong absorption and high photoluminescence quantum yield (PLQY) to maximize light-conversion efficiency. However, almost all known emitters exhibit concentration-induced quenching and self-absorption when integrated into dense solid films, fundamentally limiting external quantum yield (EQY; PLQY × absorptance) and light-conversion efficiency. Consequently, more than 2000 terawatt-hours of electricity are wasted annually in lighting and display technologies because of suboptimal electro-optical conversion, corresponding to ~8% of global electricity consumption. Colloidal perovskite nanocrystals (PeNCs) possess high absorption coefficients and intrinsically high PLQY, making them promising light-conversion materials. Yet their soft ionic lattices and labile surfaces undergo light-, heat-, and moisture-induced structural and chemical degradation. Achieving near-unity PLQY with commercially viable stability remains a central challenge. RATIONALE: Recent findings in bulk perovskites indicated that photo- or thermal-induced lattice expansion softens the crystal lattice and accelerates defect formation. However, how this lattice-softening couples with surface reactions in colloidal PeNC solids has remained unclear. We identify that PeNC degradation proceeds through a lattice-interface interlinked pathway, in which lattice expansion weakens ionic bonding, enhances ion migration, and facilitates surface oxidation and hydration reactions. Therefore, a stabilization strategy must simultaneously lock the lattice and chemically stabilize the surface rather than act only as a passive barrier. RESULTS: We introduce a hierarchical shell (HS) composed of interbonded PbSO4-SiO2-siloxane layers. This structure forms a lattice-interface interlocking network that locks the ionic lattice and stabilizes surface chemistry. HS inorganic PeNC (HS-CsPbBr3) films show a time for 10% PLQY loss (T90) of 3211 hours at 60°C, 90% relative humidity (RH) and 12,000 hours under continuous blue-light illumination, indicating long-term stability relevant for potential commercial applications. The HS strategy is compositionally general and scalable, enabling stable emission across 409 to 783 nm, including mixed-halide and hybrid perovskite formulations. Furthermore, HS organic-inorganic hybrid PeNC (HS-MAPbBr3) showing pure-green emission, a composition that is typically highly vulnerable to moisture and heat, exhibits extended humid-thermal and photostability lifetimes, surpassing T90 = 3900 hours and estimated T90 = 27,234 hours, respectively. HS-MAPbBr3 PeNC films also achieve 100.0% PLQY (average 98.6%), turning self-absorption into efficient photon recycling. A 20 wt % HS-MAPbBr3 film achieves EQY = 91.4%, approaching the theoretical limit and surpassing previously reported solid-state emitters. The HS structure prevents lead leakage and supports roll-to-roll coating, inkjet printing, and >3500 pixels per inch photolithographic patterning for high-resolution display demonstrations. CONCLUSION: The HS provides an interbonded stabilization framework that locks the lattice and stabilizes the interface, suppressing the lattice-interface interlinked degradation pathway. This approach enables near-unity PLQY, converts reabsorption into photon recycling, and achieves photoluminescence stability compatible with commercial use. Owing to broad compositional compatibility and patterning scalability, HS-PeNCs are well-suited for large-area displays (such as 75-inch televisions), mid-size tablets (~10 inch), and high-resolution microdisplays for augmented- and virtual-reality systems, as well as for solid-state lighting and bio-optoelectronic modules (for example, photoplethysmography sensing). More broadly, the lattice-interface interlocking concept provides a generalizable stabilization strategy for halide perovskite materials and related optoelectronic devices. A HS enables lattice-interface interlocking, transforming colloidal perovskite nanocrystals into commercially viable solid-state emitters.: The interbonded PbSO4-SiO2-polymer layers confine lattice expansion and stabilize the surface, suppressing soft-lattice–driven degradation. As a result, HS-PeNC films maintain near-unity PLQY with efficient photon recycling and achieve an external quantum yield of 91.4%, alongside commercially viable stability (T90 > 3000 hours at 60°C, 90% RH; T90 > 27,000 hours under blue-light exposure). [ABSTRACT FROM AUTHOR] |
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| ISSN: | 00368075 |
| DOI: | 10.1126/science.ady1370 |
