Invoking ultralong room temperature phosphorescence of purely organic compounds through H-aggregation engineering

Yuan, Jie; Wang, Shuang; Ji, Yu; Chen, Runfeng; Zhu, Qi; Wang, Yongrong; Zheng, Chao; Tao, Ye; Fan, Quli; Huang, Wei

doi:10.1039/c9mh00220k

Cited by 153 publications

(98 citation statements)

References 42 publications

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“…The distinct dual‐emissive Cu I ‐NHC complexes differ from traditional Cu I complexes. The two separate emission bands with vibronic features are quite similar with the fluorescence and RTP from solid carbazole or Cz derivatives, suggesting singlet and triplet carbazole‐based transitions in these two Cu I complexes . In addition, the two Cu I complexes are analogous to a Au I complex [Au(Me 2 ‐imy)(cbz)] (Me 2 ‐imy=1,3‐dimethylimidazol‐2‐ylidene, cbz=carbazolate) in literature, which exhibits emission in a high‐energy band (404 nm) and low‐energy band (584 nm) in the crystalline solid.…”

Section: Resultsmentioning

confidence: 68%

Two‐Coordinate Copper(I)/NHC Complexes: Dual Emission Properties and Ultralong Room‐Temperature Phosphorescence

et al. 2020

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As a kind of photoluminescent material, CuI complexes have many advantages such as adjustable emission, variable structures, and low cost, attracting attention in many fields. In this work, two novel two‐coordinate CuI‐N‐heterocyclic carbene complexes were synthesized, and they exhibit unique dual emission properties, fluorescence and phosphorescence. The crystal structure, packing mode, and photophysical properties under different conditions were systematically studied, proving the emissive mechanism to be the locally excited state of the carbazole group. Based on this mechanism, ultralong room‐temperature phosphorescence (RTP) with a lifetime of 140 ms is achieved by selective deuteration of the carbazole group. These results deepen the understanding of the luminescence mechanism and design strategy for two‐coordinate CuI complexes, and prove their potential in applications as ultralong RTP materials.

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Section: Resultsmentioning

confidence: 68%

Two‐Coordinate Copper(I)/NHC Complexes: Dual Emission Properties and Ultralong Room‐Temperature Phosphorescence

et al. 2020

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“…Therefore, the significantly improved CP‐OURTP performance should be ascribed to the photo‐enhanced aggregation coupling including H‐aggregation and intra/intermolecular interactions of the chiral molecules in solid state . H‐aggregation has been proved to be effective to stabilize the highly active triplet excitons by suppressing both the radiative and non‐radiative rates for OURTP (Figure c) . Indeed, significant numbers of H‐aggregation were observed in the pristine single‐crystal (Figure S21) with positive exciton splitting energies (Δ ϵ ) ranging from 2.65×10 −5 to 2.81×10 −3 eV (Figure d and Table S9).…”

Section: Resultsmentioning

confidence: 99%

“…[31] H-aggregation has been proved to be effective to stabilize the highly active triplet excitons by suppressing both the radiative and non-radiative rates for OURTP Figure 3c). [32] Indeed, significant numbers of H-aggregation were observed in the pristine single-crystal ( Figure S21) with positive exciton splitting energies (De)r anging from 2.65 10 À5 to 2.81 10 À3 eV (Figure 3d and Table S9). From photoactivated single crystals,s tronger H-aggregation with enlarged De value resulted after photo-activation ( Figure S22).…”

Section: Angewandte Chemiementioning

confidence: 98%

Stimuli‐Responsive Circularly Polarized Organic Ultralong Room Temperature Phosphorescence

et al. 2020

Angew Chem Int Ed

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258

176

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Purely organic materials showing room temperature phosphorescence (RTP) and ultralong RTP (OURTP) have recently attracted much attention. However, it is challenging to integrate circularly polarized luminescence (CPL) into RTP/OURTP. Here, we show a strategy to realize CPL‐active OURTP (CP‐OURTP) by binding an achiral phosphor group directly to the chiral center of an ester chain. Engineering of this flexible chiral chain enables efficient chirality transfer to carbazole aggregates, resulting in strong CP‐OURTP with a lifetime of over 0.6 s and dissymmetry factor of 2.3×10−3 after the conformation regulation upon photo‐activation. The realized CP‐OURTP is thus stable at room temperature but can be deactivated quickly at 50 °C to CP‐RTP with high CPL stability during the photo‐activation/thermal‐deactivation cycles. Based on this extraordinary photo/thermal‐responsive and highly reversible CP‐OURTP/RTP, a CPL‐featured lifetime‐encrypted combinational logic device has been successfully established.

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“…Accordingly, the phosphorescence of C-dots was detected when they were incorporated into solids, such as polymer films [324]. In H-aggregated molecular assemblies of organic dyes, a bright room-temperature phosphorescence was achieved in solid powders [325] and even in water solutions [326] due to the fact of their special design [327]. Meanwhile, the basic mechanism of their triplet exciton generation [321,328] remains unclear as well as in nanocarbon systems.…”

Section: Triplet State Generationmentioning

confidence: 99%

“…Their generation is favored in H-aggregates formed by the charge-transfer dyes [39]. It was observed that the duration of phosphorescence in H-aggregates may be much longer than that of constituting molecules, by several orders of magnitude, reaching the level of second [327,329].…”

Section: Triplet State Generationmentioning

confidence: 99%

Excitons in Carbonic Nanostructures

Demchenko

2019

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Unexpectedly bright photoluminescence emission can be observed in materials incorporating inorganic carbon when their size is reduced from macro–micro to nano. At present, there is no consensus in its understanding, and many suggested explanations are not consistent with the broad range of experimental data. In this Review, I discuss the possible role of collective excitations (excitons) generated by resonance electronic interactions among the chromophore elements within these nanoparticles. The Förster-type resonance energy transfer (FRET) mechanism of energy migration within nanoparticles operates when the composing fluorophores are the localized electronic systems interacting at a distance. Meanwhile, the resonance interactions among closely located fluorophores may lead to delocalization of the excited states over many molecules resulting in Frenkel excitons. The H-aggregate-type quantum coherence originating from strong coupling among the transition dipoles of adjacent chromophores in a co-facial stacking arrangement and exciton transport to emissive traps are the basis of the presented model. It can explain most of the hitherto known experimental observations and must stimulate the progress towards their versatile applications.

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Invoking ultralong room temperature phosphorescence of purely organic compounds through H-aggregation engineering

Abstract: Splitting energy (Δε)-controlled thermally activated reversed phase transformation from the low-lying dark state to the high-lying transition-allowed state of H-aggregation plays a key role in the organic ultralong room-temperature phosphorescence.

Cited by 153 publications

References 42 publications

Two‐Coordinate Copper(I)/NHC Complexes: Dual Emission Properties and Ultralong Room‐Temperature Phosphorescence

Two‐Coordinate Copper(I)/NHC Complexes: Dual Emission Properties and Ultralong Room‐Temperature Phosphorescence

Stimuli‐Responsive Circularly Polarized Organic Ultralong Room Temperature Phosphorescence

Excitons in Carbonic Nanostructures

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