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Nitrogen positional isomerism in heteroaromatic systems enables predictable color-tunable organic room-temperature phosphorescence (RTP). This study reveals a molecular design principle for rainbow-like phosphorescent materials with ultralong lifetimes.

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Area of Science:

  • Organic Chemistry
  • Materials Science
  • Photophysics

Background:

  • Predictable color-tunable organic room-temperature phosphorescence (RTP) is challenging due to limited understanding of triplet-state regulation.
  • Heteroaromatic systems, specifically carbazole and benzindole isomers, offer a platform to study nitrogen positional isomerism's effect on triplet excitons.

Purpose of the Study:

  • To establish a unified comparative framework to investigate how nitrogen positional isomerism in carbazole and benzindole isomers governs triplet exciton behavior and emission energetics.
  • To develop a general molecular design principle for achieving full-spectrum RTP with tunable properties.

Main Methods:

  • Systematic investigation of carbazole and benzindole isomers (Bd[f], Bd[e], Bd[g]) using a unified comparative framework.
  • Mechanochemical solvent-free synthesis for scalable preparation of benzindole isomers.
  • Photophysical measurements, DFT/TD-DFT calculations, single-crystal analysis, and interaction region indicator theory.

Main Results:

  • Nitrogen-site modulation within the fused tricyclic skeleton generated distinct red, yellow, green, and blue phosphorescence.
  • Positional isomerism was found to control exciton localization, triplet stabilization, and nonradiative decay independently of the host matrix.
  • Isomer-regulated triplet dynamics enabled full-spectrum RTP, ultralong lifetimes (up to 4.23 s), and thermally stimulated FRET (TSFRET) behavior.

Conclusions:

  • Nitrogen positional isomerism is a key factor in regulating triplet dynamics for predictable color-tunable organic RTP.
  • The study establishes a general molecular design principle for creating rainbow-like organic phosphorescent materials.
  • The findings pave the way for matrix-universal, multifunctional phosphorescent materials with extended lifetimes.