4.8 Article

Thermodynamic equilibrium between locally excited and charge-transfer states through thermally activated charge transfer in 1-(pyren-2′-yl)-o-carborane

期刊

CHEMICAL SCIENCE
卷 13, 期 18, 页码 5205-5219

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1sc06867a

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资金

  1. Julius-Maximilians-Universitat Wurzburg
  2. Bavarian State Ministry of Science, Research, and the Arts (Collaborative Research Network Solar Technologies Go Hybrid)
  3. Deutsche Forschungsgemeinschaft [GRK 2112]
  4. Natural Science Foundation of China [62174137]
  5. Natural Science Foundation of Shaanxi Province [2020GXLH-Z-022]
  6. Fundamental Research Funds for the Central Universities
  7. DFG [NI1737/2-1]
  8. Diamond Light Source, UK

向作者/读者索取更多资源

Reversible conversion between excited states is crucial in various photophysical phenomena. By conducting experiments and calculations, we discovered that the energy gaps and barriers among the locally-excited and charge-transfer states in 1-(pyren-2'-yl)-o-carborane are negligible, making all three states accessible at room temperature. Furthermore, the internal-conversion and reverse internal-conversion processes occur much faster than radiative decay, resulting in the same lifetimes and thermodynamic equilibrium of the two states.
Reversible conversion between excited-states plays an important role in many photophysical phenomena. Using 1-(pyren-2 '-yl)-o-carborane as a model, we studied the photoinduced reversible charge-transfer (CT) process and the thermodynamic equilibrium between the locally-excited (LE) state and CT state, by combining steady state, time-resolved, and temperature-dependent fluorescence spectroscopy, fs- and ns-transient absorption, and DFT and LR-TDDFT calculations. Our results show that the energy gaps and energy barriers between the LE, CT, and a non-emissive 'mixed' state of 1-(pyren-2 '-yl)-o-carborane are very small, and all three excited states are accessible at room temperature. The internal-conversion and reverse internal-conversion between LE and CT states are significantly faster than the radiative decay, and the two states have the same lifetimes and are in thermodynamic equilibrium.

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