Ultrafast cascading theory of intersystem crossings in transition-metal complexes.

Journal Article · Sun Aug 01 04:00:00 EDT 2010 · Phys. Rev. B

DOI:https://doi.org/10.1103/PhysRevB.82.075124· OSTI ID:992396

van Veenendaal, M; Chang, J; Fedro, A J

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.

• Research Organization: Argonne National Laboratory (ANL)
• Sponsoring Organization: SC; Northern Illinois Univ. IInst. for Nanoscience, Engineering and Technology
• DOE Contract Number: AC02-06CH11357
• OSTI ID: 992396
• Report Number(s): ANL/XSD/JA-64707
• Journal Information: Phys. Rev. B, Journal Name: Phys. Rev. B Journal Issue: Aug. 2010 Vol. 82; ISSN 1098-0121
• Country of Publication: United States
• Language: ENGLISH

Related Subjects

36 MATERIALS SCIENCE
DECAY
ELECTRONS
IRON COMPLEXES
L-S COUPLING
PHONONS
QUANTUM MECHANICS
SELF-ENERGY