Ultrafast cascading theory of intersystem crossings in transition-metal complexes

Jun Chang, A. J. Fedro, and Michel van Veenendaal
Phys. Rev. B 82, 075124 – Published 12 August 2010

Abstract

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 Fe2+ 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.

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  • Received 17 May 2010

DOI:https://doi.org/10.1103/PhysRevB.82.075124

©2010 American Physical Society

Authors & Affiliations

Jun Chang, A. J. Fedro, and Michel van Veenendaal

  • Department of Physics, Northern Illinois University, De Kalb, Illinois 60115, USA and Advanced Photon Source, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, USA

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Issue

Vol. 82, Iss. 7 — 15 August 2010

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