This review gives an authoritative, critical, and accessible overview of an emergent class of fluorescent materials termed “LG@MOF”, engineered from the nanoscale confinement of luminescent guests (LG) in a metal–organic framework (MOF) host, realizing a myriad of unconventional materials with fascinating photophysical and photochemical properties. We begin by summarizing the synthetic methodologies and design guidelines for representative LG@MOF systems, where the major types of fluorescent guest encompass organic dyes, metal ions, metal complexes, metal nanoclusters, quantum dots, and hybrid perovskites. Subsequently, we discuss the methods for characterizing the resultant guest–host structures, guest loading, photophysical properties, and review local-scale techniques recently employed to elucidate guest positions. A special emphasis is paid to the pros and cons of the various methods in the context of LG@MOF. In the following section, we provide a brief tutorial on the basic guest–host phenomena, focusing on the excited state events and nanoscale confinement effects underpinning the exceptional behavior of LG@MOF systems. The review finally culminates in the most striking applications of LG@MOF materials, particularly the “turn-on” type fluorochromic chemo- and mechano-sensors, noninvasive thermometry and optical pH sensors, electroluminescence, and innovative security devices. This review offers a comprehensive coverage of general interest to the multidisciplinary materials community to stimulate frontier research in the vibrant sector of light-emitting MOF composite systems.

Confinement of Luminescent Guests in Metal–Organic Frameworks: Understanding Pathways from Synthesis and Multimodal Characterization to Potential Applications of LG@MOF Systems

Pure organic emitters with full utilization of triplet excitons are in high demand for organic light-emitting diodes (OLEDs). Herein, through modulation of electron donors and introduction of phenyl rings as π spacers, we present three pure organic fluorophores (BCz, BTCz and BPTCz) with the hybridized local and charge-transfer (HLCT) excited state feature for OLED fabrication. Importantly, the introduction of π spacers in BPTCz not only enhances locally excited character with a fast radiative decay but also promotes intermolecular interactions to suppress non-radiative decays, contributing to a high solid-state fluorescence efficiency over 90%. Significantly, BPTCz not only endows its doped OLEDs with an external quantum efficiency (EQE) up to 19.5%, but also its non-doped OLED with a high EQE of 17.8%, and these outstanding efficiencies are the state-of-the-art performances of HLCT-based OLEDs.

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Hybridized local and charge-transfer excited state fluorophores enabling organic light-emitting diodes with record high efficiencies close to 20

Hybridized local and charge‐transfer (HLCT) excited‐state compounds that enable full exciton utilization through a reverse intersystem conversion (RISC) from a high‐lying triplet to a singlet state have attracted attention. Developing high‐performance ultraviolet (UV) and blue organic light‐emitting diodes (OLEDs) is challenging due to difficulties acquiring HLCT molecules with a large energy bandgap and a high photoluminescence. Herein, a new strategy for excellent‐performance UV to blue emitters based on high steric‐hindrance windmill‐type structure is proposed. These emitters exhibit good thermal, morphological, and electrochemical stabilities, as well as HLCT excited‐state characteristics. Results suggest that OLED using CTPPI efficiently emits UV light (396 nm, CIEx,y = 0.16, 0.04) with a maximum external quantum efficiency (EQE) of 7.9% and currently ranks third in UV OLEDs. The lights of these devices are well modulated from UV/deep‐blue to pure‐blue with EQEs greater than 5% by regulating the locally excited (LE) and charge‐transfer (CT) components. Experimental and theoretical investigations indicate that harvesting triplet excitons afford high electroluminescence efficiencies via HLCT excited states in the devices. This study provides an efficient strategy to achieve high‐performance UV and blue OLEDs and offers great flexibility for material design.

High Steric‐Hindrance Windmill‐Type Molecules for Efficient Ultraviolet to Pure‐Blue Organic Light‐Emitting Diodes via Hybridized Local and Charge‐Transfer Excited‐State

Donor engineered Deep-Blue emitters for tuning luminescence mechanism in Solution-Processed OLEDs

Bipolar Molecules with Hybridized Local and Charge-Transfer State for Highly Efficient Deep-Blue Organic Light-Emitting Diodes with EQE of 7.4% and CIEy ∼ 0.05

Growth mechanisms of intermetallic compounds and Bi-rich layer in ball grid array structure Cu/Sn-58Bi/Cu solder joints during solid–solid and liquid–solid electromigration

The role of aromatic π bridges (called π-linkers), which are used to connect multiple D and A groups in asymmetric thermally activated delayed fluorescence (TADF) emitters, remains a critical issue for the development of high-efficiency organic light-emitting diodes (OLEDs). In this work, based on our previous asymmetric TADF emitter (SCP) with electron donors carbazole (D) and phenothiazine (D′), we introduced different numbers of phenyl rings as π-linkers on both sides of SCP, leading to four D–A–D′ TADF emitters (PCz, 2PCz, PSz, and 2PSz) with different levels of conjugation. Experimental and theoretical results reveal that the π-linker distance has a significant effect on excited state regulation and thereby the optoelectronic properties. In comparison, the TADF emitters (PCz, and PSz) with shorter π-linkers exhibit higher photoluminescence quantum yields, due to effective suppression of conformation changes between ground state and excited state, and consequently higher device performance with external quantum efficiencies (EQEs) ranging from 20% to 30% achieved. This work provides an insight into the relationship between molecular design and optoelectronic properties of asymmetric TADF emitters.

Modulation of π-linkers in asymmetric thermally activated delayed fluorescence molecules enabling high performance OLEDs

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Hybridized local and charge-transfer excited state fluorophores enabling organic light-emitting diodes with record high efficiencies close to 20

Growth mechanisms of intermetallic compounds and Bi-rich layer in ball grid array structure Cu/Sn-58Bi/Cu solder joints during solid–solid and liquid–solid electromigration

Modulation of π-linkers in asymmetric thermally activated delayed fluorescence molecules enabling high performance OLEDs