Theory of ultrafast photoinduced low-to-high spin crossover in divalent iron systems

Baker, William; van Veenendaal, Michel

doi:10.1103/physrevb.104.014407

Theory of ultrafast photoinduced low-to-high spin crossover in divalent iron systems

Journal Article · Tue Jul 06 00:00:00 EDT 2021 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.104.014407· OSTI ID:1848058

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Northern Illinois Univ., DeKalb, IL (United States)
Northern Illinois Univ., DeKalb, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

Here a theory is developed for the ultrafast low-to-high spin transition in divalent iron. Following the photoinduced metal-to-ligand charge transfer (MLCT), the ¹A₁ MLCT state decays on a sub-100-fs timescale into the ⁵T₂ MLCT using a ³T¹ MLCT state as intermediary. Damping of nuclear motion is crucial in obtaining a full singlet-to-quintet transition mediated by the spin-orbit interaction. Destructive interference suppresses transitions to metal-centered (MC) states. The relaxation to the MC ⁵T₂ is a result of Coulomb scattering with the surroundings.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1848058

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 1 Vol. 104; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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