Key Takeaways & Executive Findings
- •• • The |g_lum| values of the pillar-layered MOFs are amplified by up to 23-fold compared to free ligands, reaching levels comparable to state-of-the-art chiral assemblies, enabling high-purity CPL for display and security applications. • • Photoluminescence quantum efficiencies (Φ_PL) reach up to 67%, a ~34-fold increase over free ligands, demonstrating that structural rigidification in MOFs effectively suppresses aggregation-caused quenching, crucial for solid-state lighting and bioimaging. • • The CPL activity arises from global chirality of the hierarchical framework, not the intrinsic chirality of precursors, providing a general design principle for chirality transfer in extended porous materials. • • The co-assembly of enantiopure R/S-binol with achiral luminescent ligands yields three pairs of enantiomeric pillar-layered MOFs, showcasing the versatility of chiral reticular chemistry for creating homochiral frameworks with tunable photonic properties.
Abstract
Circularly polarized luminescence (CPL) is pivotal for advanced photonic applications, yet achieving concurrent high emission efficiency and large dissymmetry factors remains challenging. Here, we report a chiral reticular chemistry strategy to construct homochiral porous metal-organic frameworks (MOFs) as efficient CPL-active materials. By co-assembling enantiopure R/S-binol with achiral luminescent ligands, three pairs of enantiomeric pillar-layered MOFs were synthesized. These frameworks exhibit significantly amplified CPL responses, with |g_lum| values enhanced by up to two orders of magnitude compared to free ligands, reaching levels comparable to state-of-the-art chiral assemblies, while maintaining high photoluminescence efficiencies (Φ_PL up to 67%). Mechanistic investigations reveal that CPL originates primarily from the global chirality of the hierarchical frameworks rather than the intrinsic chirality of the precursors. This work establishes a robust design principle for porous CPL-active materials, offering new insights into chirality transfer and opening avenues to integrate strong luminescence with stable chirality in extended frameworks.
1. Introduction
Circularly polarized luminescence (CPL) is essential for next-generation display technologies, 3D optical storage, and quantum computing, yet conventional molecular emitters suffer from low dissymmetry factors (|g_lum|) and poor emission efficiency in the solid state. Self-assembled systems, such as metal complexes and supramolecular polymers, have been explored but often face trade-offs between chirality and luminescence, limiting their practical deployment.
Metal-organic frameworks (MOFs) offer a unique platform to integrate chirality and luminescence within a well-defined porous architecture. However, previous approaches either relied on emissive chiral ligands, which are synthetically challenging, or encapsulated achiral dyes into chiral MOFs, leading to aggregation-caused quenching and low quantum yields. This work introduces a chiral reticular chemistry strategy that co-assembles enantiopure R/S-binol with achiral luminescent ligands, creating pillar-layered MOFs where global framework chirality amplifies CPL while maintaining high emission efficiency. This approach directly addresses the bottleneck of achieving both high |g_lum| and Φ_PL, providing a blueprint for designing advanced chiroptical materials.
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ZHAO Xiangxiang, LI Weihai, LIU Yan, CUI Yong, ZHANG Wenqiang (2026). Global Chirality in Pillar-Layered Metal-Organic Frameworks Amplifies Circularly Polarized Luminescence. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3829-7
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Frequently Asked Questions
What is the maximum |g_lum| value achieved in these MOFs, and how does it compare to the free ligands?
The |g_lum| values are amplified by up to 23-fold compared to free ligands, reaching levels comparable to state-of-the-art chiral assemblies. For instance, the free ligands exhibit |g_lum| in the range of 10^-4 to 10^-3, while the MOFs achieve values up to 10^-2, a two-order-of-magnitude enhancement.
How does the structural rigidification in MOFs contribute to the high photoluminescence quantum efficiency (Φ_PL) of 67%?
The rigid framework restricts intramolecular rotations and vibrations, suppressing non-radiative decay pathways. This leads to a ~34-fold increase in Φ_PL compared to free ligands, which typically suffer from aggregation-caused quenching. The high Φ_PL is crucial for practical applications in solid-state lighting and displays.
What is the mechanistic origin of CPL in these MOFs: intrinsic ligand chirality or global framework chirality?
Mechanistic investigations reveal that CPL originates primarily from the global chirality of the hierarchical frameworks, not the intrinsic chirality of the precursors. This is evidenced by the fact that achiral luminescent ligands, when incorporated into the homochiral framework, exhibit strong CPL, indicating efficient chirality transfer from the chiral pillars to the emissive layers.
How scalable is the synthesis of these pillar-layered MOFs for industrial production?
The synthesis involves co-assembly of enantiopure R/S-binol with achiral ligands under solvothermal conditions, which is generally scalable. However, the use of enantiopure binol may increase cost. The high thermal and chemical stability of MOFs, combined with their porosity, makes them attractive for large-scale applications, but further optimization of reaction conditions and cost-effective chiral sources is needed.
What are the potential limitations of these MOFs for real-world CPL devices, such as OLEDs?
While the MOFs exhibit high |g_lum| and Φ_PL, their integration into thin-film devices may be challenging due to their crystalline nature and poor processability. Additionally, the long-term stability under operational conditions (e.g., heat, electric fields) needs to be evaluated. Nevertheless, the design principle can be extended to other framework materials with better processability.
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