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Ladder diagrams are useful for evaluating equilibria involving metal-ligand complexes. The vertical scale of the ladder diagram represents the concentration of unreacted or free ligand, pL. The horizontal lines on the scale depict the log of stepwise formation constants for metal-ligand complexes and indicate the dominant species in all the regions.
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Amide Coupling Reaction for the Synthesis of Bispyridine-based Ligands and Their Complexation to Platinum as Dinuclear Anticancer Agents
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Intersystem Crossing in Diplatinum Complexes.

Yan Choi Lam1, Harry B Gray1, Jay R Winkler1

  • 1Beckman Institute, California Institute of Technology , Pasadena, California 91125, United States.

The Journal of Physical Chemistry. A
|September 27, 2016
PubMed
Summary
This summary is machine-generated.

Intersystem crossing (ISC) in the platinum complex Pt(pop-BF2) is surprisingly slow. A quantum mechanical model explains this by proposing two pathways, one temperature-independent and one thermally activated, involving specific molecular vibrations.

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Area of Science:

  • Photochemistry and Photophysics
  • Inorganic Chemistry
  • Quantum Mechanics

Background:

  • Intersystem crossing (ISC) is a crucial photophysical process in transition metal complexes.
  • The platinum complex Pt(pop-BF2) exhibits unusually slow ISC rates across a range of temperatures.
  • Previous studies utilized classical models to explain the temperature dependence of ISC in Pt(pop-BF2).

Purpose of the Study:

  • To investigate the slow intersystem crossing (ISC) in solid Pt(pop-BF2) using a quantum mechanical approach.
  • To develop and validate a two-channel model for ISC that accounts for the observed temperature dependence.
  • To compare the ISC mechanisms in Pt(pop-BF2) with related complexes like Pt(pop).

Main Methods:

  • Application of quantum mechanical expressions for multiphonon radiationless transitions to model ISC.
  • Development of a two-channel model incorporating temperature-independent and thermally activated pathways.
  • Fitting the model to experimental data to determine parameters for vibrational modes and energy gaps.

Main Results:

  • A two-channel quantum mechanical model successfully explains the temperature-dependent ISC rates of Pt(pop-BF2).
  • Channel 1 involves direct ISC to 3A2u via high-energy B-F or P-O vibrations, yielding temperature-independent rates.
  • Channel 2 involves ISC via a triplet deactivating state (3X) using Pt-Pt stretching, explaining thermally activated rates and observed differences with Pt(pop).

Conclusions:

  • The quantum mechanical multiphonon transition model provides a more accurate description of ISC in Pt(pop-BF2) than classical models.
  • The identified ISC pathways and vibrational modes offer insights into the factors governing radiationless decay in heavy metal complexes.
  • The study elucidates the role of specific vibrational modes (B-F, P-O, Pt-Pt) and energy gaps in controlling ISC efficiency.