Fine-Tuning of β-Substitution to Modulate the Lowest Triplet Excited States: A Bioinspired Approach to Design Phosphorescent Metalloporphyrinoids

J Am Chem Soc. 2015 Aug 26;137(33):10745-52. doi: 10.1021/jacs.5b06332. Epub 2015 Aug 17.

Abstract

Learning nature's approach to modulate photophysical properties of NIR porphyrinoids by fine-tuning β-substituents including the number and position, in a manner similar to naturally occurring chlorophylls, has the potential to circumvent the disadvantages of traditional "extended π-conjugation" strategy such as stability, molecular size, solubility, and undesirable π-π stacking. Here we show that such subtle structural changes in Pt(II) or Pd(II) cis/trans-porphodilactones (termed by cis/trans-Pt/Pd) influence photophysical properties of the lowest triplet excited states including phosphorescence, Stokes shifts, and even photosensitization ability in triplet-triplet annihilation reactions with rubrene. Prominently, the overall upconversion capability (η, η = ε·Φ(UC)) of Pd or Pt trans-complex is 10(4) times higher than that of cis-analogue. Nanosecond time-resolved infrared (TR-IR) spectroscopy experiments showed larger frequency shift of ν(C═O) bands (ca. 10 cm(-1)) of cis-complexes than those of trans-complexes in the triplet excited states. These spectral features, combining with TD-DFT calculations, suggest the strong electronic coupling between the lactone moieties and the main porphyrin chromophores and thus the importance of precisely positioning β-substituents by mimicking chlorophylls, as an alternative to "extended π-conjugation", in designing NIR active porphyrinoids.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Biomimetics / methods*
  • Drug Design*
  • Luminescent Agents / chemistry*
  • Metalloporphyrins / chemistry*
  • Models, Molecular
  • Molecular Conformation
  • Palladium / chemistry
  • Photosensitizing Agents / chemistry
  • Platinum / chemistry
  • Stereoisomerism

Substances

  • Luminescent Agents
  • Metalloporphyrins
  • Photosensitizing Agents
  • Platinum
  • Palladium