Energy and Electron Transfer MMP+ discussion Chapter 7 first half December 17, 2002 Zhiqiang Liu.

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Presentation transcript:

Energy and Electron Transfer MMP+ discussion Chapter 7 first half December 17, 2002 Zhiqiang Liu

Transfer

Competing Processes upon encountering

Trivial Mechanism for energy transfer

Spectral Overlap Integral

Trivial Mechanism for electron transfer

Non-trivial energy transfer

Forster Theory of Coulombic Energy Transfer  2 : orientation. Alignment factor J: overlap. Energy match of donor and acceptor R: distance between dipoles dipole-dipole interaction

Energy transfer by electron exchange Dexter:

Comparison: Forster v. Dexter Dexter: Forster: 1.Dependence on separation. Dexter much stronger than Forster. 2.Forster depends on oscillator strength. 3.Both dependent on J. 4.Dexter involves excited states

Generating D and A*

Triplet Triplet Annihilation. Energy transfer via electron exchange

Electron Transfer

Excited states: better oxidizing and reducing agents

Free energy for gas phase electron transfer

Free energy in solution phase GG Gas phase results + terms for solution Electrochemical potential in solution

Coulombic term in free energy of electron transfer

Libby vs. Marcus theory Three events: 1.Electron transfer 2.Molecular reorientation 3.Solvent reorientation Libby: Molecular and solvent after Electron. Marcus: Assumptions: 1. Loose bonding between molecules for classical phys/chem analysis 2. Geometrical and solvent reorientation to provide energy for the e jump Frank-Condon e Jump

Libby vs. Marcus theory

Marcus for non zero free energy difference

Experimental evidence for Marcus Inverted Region