Ultrafast cascading theory of intersystem crossings in transition-metal complexes

Journal Article · Sun Aug 15 04:00:00 EDT 2010 · Physical Review. B, Condensed Matter and Materials Physics

DOI:https://doi.org/10.1103/PHYSREVB.82.075124· OSTI ID:21421394

Chang, Jun; Fedro, A J; Veenendaal, Michel van ^[1]

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1. Department of Physics, Northern Illinois University, De Kalb, Illinois 60115 (United States) and Advanced Photon Source, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439 (United States)

We investigate the cascade decay mechanism for ultrafast intersystem crossing mediated by the spin-orbit coupling in transition-metal complexes. A quantum-mechanical description of the cascading process that occurs after photoexcitation is presented. The conditions for ultrafast cascading are given, which relate the energy difference between the levels in the cascading process to the electron-phonon self energy. These limitations aid in the determination of the cascade path. For Fe{sup 2+} spin-crossover complexes, this leads to the conclusion that the ultrafast decay primarily occurs in the manifold of antibonding metal-to-ligand charge-transfer states. We also give an interpretation why some intermediate states are bypassed.

• OSTI ID: 21421394
• Journal Information: Physical Review. B, Condensed Matter and Materials Physics, Journal Name: Physical Review. B, Condensed Matter and Materials Physics Journal Issue: 7 Vol. 82; ISSN 1098-0121
• Country of Publication: United States
• Language: English

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
ANGULAR MOMENTUM
CASCADE THEORY
CHARGED PARTICLES
COMPLEXES
COUPLING
ELECTRONS
ELEMENTARY PARTICLES
ENERGY
FERMIONS
INTERMEDIATE COUPLING
INTERMEDIATE STATE
IONS
IRON IONS
L-S COUPLING
LEPTONS
LIGANDS
MECHANICS
PARTICLE PROPERTIES
PHONONS
QUANTUM MECHANICS
QUASI PARTICLES
SELF-ENERGY
SPIN
TRANSITION ELEMENT COMPLEXES