<p>Complex <i>cis</i>-[Ru(bpy)<sub>2</sub>(NH<sub>3</sub>)<sub>2</sub>]<sup>2+</sup> (<b>1</b>) is a promising photo-activated chemotherapy (PACT) agent; however, its photophysical and photochemical properties have been poorly studied. In this work photoreactions of complex <b>1</b> in aqueous solutions were studied by means of steady-state photolysis, nanosecond laser flash photolysis, and ultrafast transient absorption spectroscopy. Excitation of <b>1</b> in the wavelength range of 254–505 nm results in substitution of two ammonia ligands by water molecules followed by partial dissociation with the formation of complexes <i>cis</i>-[Ru(bpy)<sub>2</sub>(H<sub>2</sub>O)<sub>2</sub>]<sup>2+</sup> (<b>2</b>) and <i>cis</i>-[Ru(bpy)<sub>2</sub>(H<sub>2</sub>O)(OH)]<sup>+</sup> (<b>3</b>), which exist in equilibrium. The quantum yield of photo-aquation is rather low (about 1%) and decreases on going from the UV to visible spectral range. Excitation of complex <b>1</b> in the region of the intra-ligand transition (350 nm) results in the formation of vibrationally hot, triplet excited metal-to-ligand charge transfer (<sup>3</sup>MLCT) state with a characteristic time shorter than 100 fs. The vibrational cooling time was about 3 ps. The thermally equilibrated <sup>3</sup>MLCT state decays within 120 ns in two parallel processes, <i>viz.</i>, intersystem crossing to the ground state and exchange of NH<sub>3</sub> ligand with a water molecule to give the complex <i>cis</i>-[Ru(bpy)<sub>2</sub>(NH<sub>3</sub>)(H<sub>2</sub>O)]<sup>2+</sup> (<b>4</b>). Possible reactions of complex <b>4</b> include the inverse substitution of water molecule by the ammonia ligand with the restoration of the initial structure of the complex and the exchange of the second NH<sub>3</sub> ligand with a water molecule with the formation of reaction products, <i>viz.</i>, complexes <b>2</b> and <b>3</b>. The photochemical properties of complex <b>1</b> are independent of the presence of dissolved oxygen in solution, which is favorable for the PACT applications.</p>

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Photochemistry of cis-[Ru(bpy)2(NH3)2]2+ complex, a promising light-activated anticancer agent

  • A. A. Kokorenko,
  • V. P. Grivin,
  • I. P. Pozdnyakov,
  • A. V. Mikheylis,
  • Yu. A. Belikov,
  • A. A. Melnikov,
  • S. V. Chekalin,
  • D. B. Vasilchenko,
  • E. M. Glebov

摘要

Complex cis-[Ru(bpy)2(NH3)2]2+ (1) is a promising photo-activated chemotherapy (PACT) agent; however, its photophysical and photochemical properties have been poorly studied. In this work photoreactions of complex 1 in aqueous solutions were studied by means of steady-state photolysis, nanosecond laser flash photolysis, and ultrafast transient absorption spectroscopy. Excitation of 1 in the wavelength range of 254–505 nm results in substitution of two ammonia ligands by water molecules followed by partial dissociation with the formation of complexes cis-[Ru(bpy)2(H2O)2]2+ (2) and cis-[Ru(bpy)2(H2O)(OH)]+ (3), which exist in equilibrium. The quantum yield of photo-aquation is rather low (about 1%) and decreases on going from the UV to visible spectral range. Excitation of complex 1 in the region of the intra-ligand transition (350 nm) results in the formation of vibrationally hot, triplet excited metal-to-ligand charge transfer (3MLCT) state with a characteristic time shorter than 100 fs. The vibrational cooling time was about 3 ps. The thermally equilibrated 3MLCT state decays within 120 ns in two parallel processes, viz., intersystem crossing to the ground state and exchange of NH3 ligand with a water molecule to give the complex cis-[Ru(bpy)2(NH3)(H2O)]2+ (4). Possible reactions of complex 4 include the inverse substitution of water molecule by the ammonia ligand with the restoration of the initial structure of the complex and the exchange of the second NH3 ligand with a water molecule with the formation of reaction products, viz., complexes 2 and 3. The photochemical properties of complex 1 are independent of the presence of dissolved oxygen in solution, which is favorable for the PACT applications.