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      One/Two‐Photon‐Excited ESIPT‐Attributed Coordination Polymers with Wide Temperature Range and Color‐Tunable Long Persistent Luminescence

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          Abstract

          The multiple metastable excited states provided by excited‐state intramolecular proton transfer (ESIPT) molecules are beneficial to bring temperature‐dependent and color‐tunable long persistent luminescence (LPL). Meanwhile, ESIPT molecules are intrinsically suitable to be modulated as D‐π‐A structure to obtain both one/two‐photon excitation and LPL emission simultaneously. Herein, we report the rational design of a dynamic Cd II coordination polymer ( LIFM‐106) from ESIPT ligand to achieve the above goals. By comparing LIFM‐106 with the counterparts, we established a temperature‐regulated competitive relationship between singlet excimer and triplet LPL emission. The optimization of ligand aggregation mode effectively boost the competitiveness of the latter. In result, LIFM‐106 shows outstanding one/two‐photon excited LPL performance with wide temperature range (100–380 K) and tunable color (green to red). The multichannel radiation process was further elucidated by transient absorption and theoretical calculations, benefiting for the application in anti‐counterfeiting systems.

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          Stabilizing triplet excited states for ultralong organic phosphorescence.

          The control of the emission properties of synthetic organic molecules through molecular design has led to the development of high-performance optoelectronic devices with tunable emission colours, high quantum efficiencies and efficient energy/charge transfer processes. However, the task of generating excited states with long lifetimes has been met with limited success, owing to the ultrafast deactivation of the highly active excited states. Here, we present a design rule that can be used to tune the emission lifetime of a wide range of luminescent organic molecules, based on effective stabilization of triplet excited states through strong coupling in H-aggregated molecules. Our experimental data revealed that luminescence lifetimes up to 1.35 s, which are several orders of magnitude longer than those of conventional organic fluorophores, can be realized under ambient conditions. These results outline a fundamental principle to design organic molecules with extended lifetimes of excited states, providing a major step forward in expanding the scope of organic phosphorescence applications.
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            Room-temperature phosphorescence from organic aggregates

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              Activating efficient phosphorescence from purely organic materials by crystal design.

              Phosphorescence is among the many functional features that, in practice, divide pure organic compounds from organometallics and inorganics. Considered to be practically non-phosphorescent, purely organic compounds (metal-free) are very rarely explored as emitters in phosphor applications, despite the emerging demand in this field. To defy this paradigm, we describe novel design principles to create purely organic materials demonstrating phosphorescence that can be turned on by incorporating halogen bonding into their crystals. By designing chromophores to contain triplet-producing aromatic aldehydes and triplet-promoting bromine, crystal-state halogen bonding can be made to direct the heavy atom effect to produce surprisingly efficient solid-state phosphorescence. When this chromophore is diluted into the crystal of a bi-halogenated, non-carbonyl analogue, ambient phosphorescent quantum yields reach 55%. Here, using this design, a series of pure organic phosphors are colour-tuned to emit blue, green, yellow and orange. From this initial discovery, a directed heavy atom design principle is demonstrated that will allow for the development of bright and practical purely organic phosphors.
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                Author and article information

                Contributors
                Journal
                Angewandte Chemie International Edition
                Angew Chem Int Ed
                Wiley
                1433-7851
                1521-3773
                September 11 2023
                August 04 2023
                September 11 2023
                : 62
                : 37
                Affiliations
                [1 ] MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional Materials School of Chemistry Sun Yat-Sen University Guangzhou 510006 China
                Article
                10.1002/anie.202309172
                23bb92e8-9d07-421b-93ba-3f6ed7c11683
                © 2023

                http://onlinelibrary.wiley.com/termsAndConditions#vor

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