ConspectusThe phosphorescence is produced by the radiative transition of the excited triplet state which is generated by the intersystem crossing (ISC) from the excited singlet state. Compared with fluorescence, it has a longer luminescence lifetime and larger Stokes shift, so phosphorescent materials have great application value in fields such as displays, anticounterfeiting, and imaging. But due to the low ISC rate of organic molecules, the slow radiative transition rate of the triplet state, and the large nonradiative energy loss caused by molecular vibration, pure organic room temperature phosphorescence (RTP) is usually difficult to obtain. Among the most widely used strategies including crystal assembly, polymerization, and host–guest encapsulation, the polymerization strategy based on rigid polymers has achieved great success and widespread attention due to their easy processing and excellent luminescence performance.The main function of polymers is to fix the luminophore into the matrix and suppress the energy loss of the triplet state caused by nonradiative transitions and oxygen quenching. That is, polymers provide a rigid microenvironment necessary for the RTP, although some polymers are flexible and stretchable. Conventional polymers have limited interaction with luminophores and do not have the function of promoting triplet states. Therefore, the high RTP quantum yield depends more on the structural design of luminophores. By modification of the structure, functionalized polymers can be endowed with the ability to regulate the singlet and triplet energy levels of luminophores, enhance ISC, and increase the quantum yield of RTP. The selection of functionalized polymers also enriches the diverse properties of RTP materials.This Account summarizes the latest research progress in the field of polymer-based RTP and RTP enhancement by functionalized polymers. Luminophores are used to construct RTP systems by doping, covalent linking, or supramolecular interactions with polymers such as PAA, PMMA, PVA, and PAM. To further strengthen polymer rigidity, secondary processing has been successfully employed to synergistically suppress nonradioactivation and enhance RTP performance, such as hydrogen bonding bridges, host–guest encapsulation, and cross-linking. The function of polymers is no longer limited to suppressing nonradiative transitions but also includes enhancing the yield of triplet states and generating special luminescence phenomena. A few functionalized polymers are specially designed to utilize external heavy atom effects, dipole–dipole interactions, and electrostatic and diffusion interactions with the luminophores to promote the ISC rate. Due to the diversification and functionalization of polymers, RTP systems were developed with various special luminescence phenomena such as photoactivation, excitation wavelength dependence, photochromism, circularly polarized RTP, and stimulus-response. We hope the summarized functions and development trends of polymers in RTP systems can provide helpful guidance for designing more high-performance RTP materials. 

Recent Advances of Pure Organic Room Temperature Phosphorescence Based on Functional Polymers

A rational molecular design strategy facilitates the development of a purely organic room‐temperature phosphorescence (RTP) material system with precisely regulated luminescence properties, which surely promotes its functional integration and intelligent application. Here, a functional unit combination strategy is proposed to design novel RTP molecules combining a folding unit with diverse luminescent cores. The different luminescent cores are mainly responsible for tunable RTP properties, while the folding unit contributes to the spin–orbit coupling (SOC) enhancement, which makes the RTP material design as workable as the building block principle. By this strategy, a series of color/lifetime‐tunable RTP materials is achieved with unique photo‐responsive RTP enhancement when subjected to UV irradiation, which expands their application scenarios in reusable privacy tags, advanced “4D” encryption, and phase separation analysis of blended polymers. This work suggests a simple and effective strategy to design purely organic RTP materials with tunable color and lifetime, and also provides new application options for photo‐responsive dynamic RTP materials.

Photo-Responsive Dynamic Organic Room-temperature Phosphorescence Materials Based on A Functional Unit Combination Strategy.

Triarylboranes-based pure organic room-temperature phosphorescence (RTP) materials are rarely investigated because of their large steric hindrance and the electron defect of the boron atom. As a result, creating functional triarylborane RTP materials is difficult. Herein, we report the first photo-activated RTP materials with lifetimes/quantum yields ≤0.18 s/6.83% based on donor (D)–π–acceptor (A) from methylene carbazole-functionalized aminoborane (BN)-doped polymethyl methacrylate (BN-o-Met-Cz@PMMA) under 365 nm UV irradiation (30 s). Incredibly, BN-o-Met-Cz@PMMA films exhibited unprecedented photo-activated RTP dual–response properties (e.g., air + 365 nm: τP = 0.18 s, ΦP = 6.83%; N2 + 365 nm: τP = 0.42 s, ΦP = 17.34%). Intriguingly, the BN (D–π–A) system demonstrated good versatility for photo-activated RTP whether the electron-donating group or electron-withdrawing group was placed in the ortho (meta)-position of the B atom. As a result, a series of photo-activated single-molecule organic RTP materials with multi-color emission, high quantum yields, and ultra-long lifetimes can be prepared rapidly. BN-X@PMMA films showed broad application prospects for information encryption, data erasure, anti-counterfeiting, and water resistance. Our method provides new strategies for the design, synthesis, and application of RTP materials, thereby enriching the types of organic RTP materials and facilitating further developments in this area.

/pdf/time-dependent-photo-activated-aminoborane-room-temperature-1ljoeswv.pdf

Time-dependent photo-activated aminoborane room-temperature phosphorescence materials with unprecedented properties: simple, versatile, multicolor-tuneable, water resistance, optical information writing/erasing, and multilevel data encryption

Abstract Dynamic organic room‐temperature phosphorescence (RTP) materials are highly promising for various applications. However, developing photo‐responsive RTP systems with simple fabrication, high reversibility, and visible‐light responsiveness presents a significant challenge. Herein, in situ embedding of boron‐doped carbon dots (B‐CDs) in amorphous polymer (pPBA) is achieved by a two‐step polymerization and carbonization process. Impressively, the B‐CDs@pPBA composite exhibits visible‐light‐activated ultralong RTP with full reversibility and a lifetime on–off ratio exceeding 280. By correlating photophysical properties with structural characterization results, it is concluded that photoinduced intensifying of the crosslinking between B‐CDs and pPBA is responsible for the dynamic RTP. More interestingly, the B‐CDs@pPBA film is found to display bending actuation and reversible deformable behavior upon light exposure. Finally, potential applications of such photo‐responsive systems in programmable information storage and encryption are demonstrated. This research may pave a new way for the development of dynamic RTP nanomaterials and promote their use in a wide range of promising applications. 

Visible‐Light Manipulated Reversible and Ultralong Phosphorescence of Carbon Dots Through Dynamic Cross‐Linking

Molecular emitters with multi-emissive properties are in high demand in numerous fields, while these properties basically depend on specific molecular conformation and packing. For amorphous systems, special molecular arrangement is unnecessary, but it remains challenging to achieve such luminescent behaviors. Herein, we present a general strategy that takes advantage of molecular rigidity and S1-T1 energy gap balance for emitter design, which enables fluorescence-phosphorescence dual-emission properties in various solid forms, whether crystalline or amorphous. Subsequently, the amorphism of the emitters based polymethyl methacrylate films endowed an in situ regulation of the dual-emissive characteristics. With the ratiometric regulation of phosphorescence by external stimuli and stable fluorescence as internal reference, highly controllable luminescent color tuning (yellow to blue including white emission) was achieved. There properties together with a persistent luminous behavior is of benefit for an irreplaceable set of optical information combination, featuring an ultrahigh-security anti-counterfeiting ability. Our research introduces a concept of eliminating the crystal-form and molecular-conformational dependence of complex luminescent properties through emitter molecular design. This has profound implications for the development of functional materials.

Engineering tunable ratiometric dual emission in single emitter-based amorphous systems.

As intelligent probes, dynamic and controllable molecular switches are useful tools for probing and intervening in life processes. However, the types and properties of molecular switches are still relatively single and often can only make two actions: "off" and "on". Therefore, the development of novel molecular switches with multiple colors and multiple instructions is very challenging. Herein, we propose a novel strategy based on the instability of the Lewis acid-base pair (boron (B) and nitrogen (N)), such as introducing the Schiff base (C═N) group into the aminoborane skeleton and preparing the novel molecular switches BN-HDZ and BN-HDZ-N. These two molecules were found to have good multicolor fluorescence switching capability for methanol. Surprisingly, the compound BN-HDZ-N shows unprecedented visual identification for the butanol isomers and could be made into a portable strip for simple and rapid visual identification of the four isomers of butanol, promising an alternative to conventional Lucas reagents. This provides a novel strategy for the design and fabrication of novel multicolor-tunable molecular switches with visual identification of isomers.

Multicolor Adjustable B-N Molecular Switches: Simple, Efficient, Portable, and Visual Identification of Butanol Isomers.

Triarylphosphine-based pure organic long persistent luminescence materials are rarely investigated because of their poor stability and low photoluminescence quantum yield. Herein, we demonstrate that the introduction of a methoxy group (TPP-o-3OMe) at the ortho position of triphenylphosphine (TPP) can essentially promote the n → π* transition and promote intersystem crossing to generate more triplet excitons. Simultaneously, generating abundant intramolecular and intermolecular hydrogen bonds to stable excited triplet excitons is beneficial, thereby causing high-efficiency phosphorescence emission (τp = 394.1 ms; Φp = 9.28%). Interestingly, it shows a good acid response to protonic acids and can often be cycled many times under the heating or ammonia fumigation conditions. This research provides a new idea for enriching the types of pure organic room-temperature phosphorescent materials, widening their applications in the fields of anticounterfeiting and smart response, and promotes the further development of this field.

Simple Stimulus-Responsive Organic Long Persistent Luminescence Systems Based on Methoxy-Functionalized Triphenylphosphine.

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Time-dependent photo-activated aminoborane room-temperature phosphorescence materials with unprecedented properties: simple, versatile, multicolor-tuneable, water resistance, optical information writing/erasing, and multilevel data encryption

Multicolor Adjustable B-N Molecular Switches: Simple, Efficient, Portable, and Visual Identification of Butanol Isomers.

Simple Stimulus-Responsive Organic Long Persistent Luminescence Systems Based on Methoxy-Functionalized Triphenylphosphine.