Conformational Modulation of Efficient Macrocyclic Emitters Featuring Delayed Fluorescence by Conjugation Length and Cavity Dimensions DOI
Jingping Xiao, Denghui Liu, Yu Fu

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Окт. 19, 2024

Abstract The π‐conjugated macrocyclic emitters with thermally activated delayed fluorescence (TADF) characteristics have attracted widespread attention in the field of organic electroluminescence (EL) materials due to their unique geometries and excellent luminescence performance. Despite significant impact conjugation length cavity dimensions on molecular conformation, influence these factors excited‐state properties remains understudied. Herein, we formulated a strategy aimed at modulating conformation TADF molecules containing aniline as donor (D) unit, triazine acceptor (A), linked D−A D‐π‐A alternative construction ( MC‐TNT MC‐TST ). Corroborated by experimental theoretical analyses, compact conformationally twisted exhibits efficient blue crystalline state, facilitating EL high doping concentrations maximum external quantum efficiency (EQE max ) 13.9 %, leading emitters. Notably, π‐bridge flat demonstrates diminished Coulombic repulsion, achieving nearly 100 % photoluminescence yield superior horizontal dipole orientation 85 5 wt doped films, corresponding device‘s EQE reaches record‐high 32.7 within domain.

Язык: Английский

Versatile Thermally Activated Delayed Fluorescence Material Enabling High Efficiencies in both Photodynamic Therapy and Deep-Red/NIR Electroluminescence DOI
Hui Wang,

Yijian Gao,

Jia‐Xiong Chen

и другие.

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Янв. 9, 2025

Thermally activated delayed fluorescence (TADF) materials have received increasing attention from organic electronics to other related fields, such as bioapplications and photocatalysts. However, it remains a challenging task for TADF emitters showcase the versatility concurrent with high performance in multiple applications. Herein, we first present proof-of-concept material, namely, QCN-SAC, through strategically manipulating exciton dynamics. On one hand, QCN-SAC displays obvious aggregate-induced deep-red/near-infrared emission radiative rate beyond 107 s–1, thereby demonstrating nearly 100% utilization under oxygen-free conditions. In QCN-SAC-based nondoped light-emitting diode (OLED), superb external quantum efficiency of 16.4% can be reached peak at 708 nm. also exhibits intersystem crossing over 108 s–1 without leveraging heavy-atom effect, which makes nanoparticles perform well boosting reactive oxygen species generation imaging-guided photodynamic therapy (PDT). This work presents fundamental principle designing high-performance all-in-one molecules OLED PDT discovery holds promise advancing development versatile range uses near future.

Язык: Английский

Процитировано

1
Catalyst-Free Regio- and Stereoselective C(sp2)–H Chlorination of Enamides at Room Temperature DOI

Min‐Zhi Deng,

M. N. SHENG,

Xueqing Wen

и другие.

Organic Letters, Год журнала: 2025, Номер unknown

Опубликована: Апрель 29, 2025

We disclose herein a catalyst-free, room-temperature protocol for the highly regio- and stereoselective alkenyl C(sp2)-H chlorination of diverse enamides with commercially available, inexpensive N-chlorosuccinimide (NCS) as electrophilic chlorinating reagent under exceedingly mild conditions. This operationally simple approach features remarkably broad substrate scope accommodates excellent functional group tolerance, affording range synthetically valuable geometrically defined β-chlorinated in high yields an exclusive E configuration.

Язык: Английский

Процитировано

1
High‐Efficiency Solution‐Processed Organic Light‐Emitting Diodes Utilizing Multiple‐Resonance Emitters Incorporating Thiocarbazole Unit DOI Open Access
Shihua Li,

Maoqiu Li,

Yanru Li

и другие.

Advanced Optical Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 5, 2025

Abstract Introducing heavy atoms to enhance spin‐orbit coupling represents an effective strategy for boosting the reverse intersystem crossing (RISC) rate constants of Multi‐resonance thermally activated delayed fluorescence (MR‐TADF) emitters. Nevertheless, restricted diversity molecular structures obstructs a thorough investigation structure‐property relationships, thereby limiting improvement device performance, especially in case solution‐processed devices. Herein, alkylthio‐substituted carbazole building block is designed and developed two new MR‐TADF emitters, namely BNCz‐2S BNCz‐4S. Quantum simulations photophysical studies have revealed that as number sulfur increases, BNCz‐4S exhibits higher photoluminescence quantum yield (PLQY), smaller singlet‐triplet energy gap (Δ E ST ) reorganization energy, along with larger (SOC) constant ( k RISC compared BNCz‐2S. Consequently, solution‐processing devices based on exhibit external efficiency (EQE) 24.06%, which first tier reported organic light‐emitting diodes (OLED) date.

Язык: Английский

Процитировано

0
Synthesis of Polycyclic Heteroarenes via Rh(III)-Catalyzed Twofold C-H Activation of 3-Aryl-2H-benzo[b][1,4]oxazines and Annulation with α-Diazo-β-ketoesters DOI

Yiyue Li,

Li Song,

Haokang Du

и другие.

The Journal of Organic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Март 14, 2025

An efficient Rh(III)-catalyzed annulation between 3-aryl-2H-benzo[b][1,4]oxazines and α-diazo-β-ketoesters was developed, affording a series of polycyclic heteroarenes in moderate to excellent yields with good functional group compatibility. The procedure featured high efficiency, redox neutrality, twofold ortho-C-H activation, dual [4 + 2] annulation. Moreover, several important intermediates products have been isolated as powerful evidence for the proposed reaction mechanism.

Язык: Английский

Процитировано

0
High‐Performance Solution Processable Red TADF‐OLED with External Quantum Efficiency Exceeding 28% Using a Multi‐Resonance Emitter Host DOI
Xiaolong Liu,

Lei Hua,

Xiaoyi Lai

и другие.

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Апрель 7, 2025

Abstract Achieving high‐efficiency soluble red thermally activated delayed fluorescence (TADF) emitters remains a substantial challenge owing to the constraints imposed by energy‐gap law. In this study, an asymmetric pyrene‐azaacene derivative, named PBCNT, is prepared and characterized, featuring strong electron‐donating tert ‐butyl diphenylamine moiety electron‐withdrawing cyano group. PBCNT exhibits intense emission with peak wavelength of 664 nm in toluene solution. It demonstrates evident TADF character solid state, attributed small energy difference 0.04 eV between its lowest singlet triplet states. By employing multi resonance‐type molecule as host matrix, solution‐processed organic light‐emitting diode (OLED) based on achieved record‐high maximum external quantum efficiency (EQE) 28.5%, at 608 nm, facilitated effective Förster transfer, good horizontal emitting dipole orientation managed intermolecular interactions dopant. This represents one highest EQE values reported among OLEDs electroluminescence wavelengths greater than 600 nm. paper introduces promising pathway for developing efficient that overcome limitations

Язык: Английский

Процитировано

0
A dark-state–dominated photochemical upconversion afterglow via triplet energy transfer relay DOI Creative Commons

Hang Yuan,

Kuangshi Sun,

Xianlong Su

и другие.

Science Advances, Год журнала: 2025, Номер 11(17)

Опубликована: Апрель 25, 2025

Photochemical afterglow materials have drawn considerable attention due to their attractive luminescent properties and great application potential. Considering the classical photochemical always exhibit poor luminescence, it is urgent gain fundamental understanding of main limiting factors. Here, we identified existence a dark-state triplet in process, an overwhelming percentage ~98.5% was revealed for this non-emissive state. Guided by these observations, proposed activate unprecedented energy transfer relay simultaneously harness singlet energy. Consequently, upconverted material constructed with amazing luminescence performance albeit its moderate fluorescence emission property. The generality strategy evidenced adaptation similar emitters varied wavelengths. optimized enabled time-gated upconversion bioimaging under ultralow-power excitation. This study not only reveals pathways but also paves way rational design bright ultralong lifetime.

Язык: Английский

Процитировано

0
Donor–Acceptor Viologens with Through‐Space Conjugation for Enhanced Visible‐Light‐Driven Photocatalysis DOI Creative Commons
Yi Qiao, Liang Xu, Xiaoyang Liu

и другие.

Advanced Science, Год журнала: 2024, Номер 12(2)

Опубликована: Ноя. 21, 2024

Abstract A series of novel donor–acceptor (D–A) type viologens with through‐space conjugation (TSC) are synthesized. The synergistic effect D–A and TSC endow these compounds a narrower energy gap, excellent redox properties, strong absorption in the visible range (up to 450 nm), high efficiency intramolecular charge transfer (ICT). These also exhibit long‐lived separation state stable radical formation. Considering their impressive photophysical explored for visible‐light‐driven photocatalysis. As catalyst oxidative coupling reactions under light, compound 9 can achieve yield 94%, attributed its ICT effect. Additionally, hybridized into graphitic carbon nitride (g‐C₃N₄), enhances hydrogen production performance achieving an H 2 generation rate 4102 µmol h −1 g . This study highlights potential applications photocatalytic systems.

Язык: Английский

Процитировано

1
Conformational Modulation of Efficient Macrocyclic Emitters Featuring Delayed Fluorescence by Conjugation Length and Cavity Dimensions DOI
Jingping Xiao, Denghui Liu, Yu Fu

и другие.

Angewandte Chemie, Год журнала: 2024, Номер unknown

Опубликована: Окт. 19, 2024

Abstract The π‐conjugated macrocyclic emitters with thermally activated delayed fluorescence (TADF) characteristics have attracted widespread attention in the field of organic electroluminescence (EL) materials due to their unique geometries and excellent luminescence performance. Despite significant impact conjugation length cavity dimensions on molecular conformation, influence these factors excited‐state properties remains understudied. Herein, we formulated a strategy aimed at modulating conformation TADF molecules containing aniline as donor (D) unit, triazine acceptor (A), linked D−A D‐π‐A alternative construction ( MC‐TNT MC‐TST ). Corroborated by experimental theoretical analyses, compact conformationally twisted exhibits efficient blue crystalline state, facilitating EL high doping concentrations maximum external quantum efficiency (EQE max ) 13.9 %, leading emitters. Notably, π‐bridge flat demonstrates diminished Coulombic repulsion, achieving nearly 100 % photoluminescence yield superior horizontal dipole orientation 85 5 wt doped films, corresponding device‘s EQE reaches record‐high 32.7 within domain.

Язык: Английский

Процитировано

0
Conformational Modulation of Efficient Macrocyclic Emitters Featuring Delayed Fluorescence by Conjugation Length and Cavity Dimensions DOI
Jingping Xiao, Denghui Liu, Yu Fu

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Окт. 19, 2024

Abstract The π‐conjugated macrocyclic emitters with thermally activated delayed fluorescence (TADF) characteristics have attracted widespread attention in the field of organic electroluminescence (EL) materials due to their unique geometries and excellent luminescence performance. Despite significant impact conjugation length cavity dimensions on molecular conformation, influence these factors excited‐state properties remains understudied. Herein, we formulated a strategy aimed at modulating conformation TADF molecules containing aniline as donor (D) unit, triazine acceptor (A), linked D−A D‐π‐A alternative construction ( MC‐TNT MC‐TST ). Corroborated by experimental theoretical analyses, compact conformationally twisted exhibits efficient blue crystalline state, facilitating EL high doping concentrations maximum external quantum efficiency (EQE max ) 13.9 %, leading emitters. Notably, π‐bridge flat demonstrates diminished Coulombic repulsion, achieving nearly 100 % photoluminescence yield superior horizontal dipole orientation 85 5 wt doped films, corresponding device‘s EQE reaches record‐high 32.7 within domain.

Язык: Английский

Процитировано

0