4.2 Article

Modulating Room Temperature Phosphorescence by Oxidation of Thianthrene to Achieve Pure Organic Single-Molecule White-Light Emission

Journal

CCS CHEMISTRY
Volume 3, Issue 7, Pages 1940-1948

Publisher

CHINESE CHEMICAL SOC
DOI: 10.31635/ccschem.020.202000433

Keywords

single-molecule white light; room temperature phosphorescence; thianthrene; lone pair electrons; spin-orbital coupling

Funding

  1. National Natural Science Foundation of China [51873077, 91833304, 51803071]
  2. National Basic Research Program of China [2016YFB0401001]
  3. Postdoctoral Innovation Talent Support Project [BX20180121]
  4. China Postdoctoral Science Foundation [2018M641767, 2019TD-33]

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By oxidizing thianthrene at different degrees, a pure organic single-molecule white-light emitter was developed, demonstrating the modulation effect of oxidation levels on room temperature phosphorescence emission.
In order to develop pure organic single-molecule white-light emitters (SMWLE), the oxidation of thianthrene (TA) was performed on sulfur atoms at different degrees to tune room temperature phosphorescence (RTP) emission. With increasing degrees of oxidation from 1OTA, 2OTA, 3OTA, to 4OTA, monomeric and aggregative RTP emission was gradually suppressed, due to the gradual disappearance of lone pair electrons on sulfur atoms. Among these compounds, monomers and aggregates of 1OTA demonstrated a better intensity match between fluorescence and RTP. Through partial oxidation of TA, 1OTA exhibited the simultaneous ternary emissions from the lowest singlet state (S-1), the lowest triplet state (T-1), and the high-lying triplet state (T-n) in doped film. The single-molecule white-light emission was achieved in 1OTA crystal with a photoluminescence quantum yield (PLQY) of 47.1%. This work not only reports the RTP behavior of TA with different degrees of oxidation, but also provides an example of excited-state modulation to harvest an efficient SMWLE material.

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