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Title: Ultrafast intersystem crossings in Fe-Co Prussian blue analogues

Ultrafast spincrossover is studied in Fe-Co Prussian blue analogues using a dissipative quantum-mechanical model of a cobalt ion coupled to a breathing mode. All electronic interactions are treated on an equal footing. It is theoretically demonstrated that the divalent cobalt ion reaches 90% of the S = 3/2 value within 20 fs after photoexciting a low-spin Co 3+ ion by an iron-to-cobalt charge transfer. The doublet-to-quartet spin crossover is significantly faster than the oscillation period of the breathing mode. The system relaxes to the lowest manifold of divalent cobalt ( 4T 1) in 150-200 fs. In conclusion, strong oscillations in spin-orbit coupling and the involvement of higher-lying quartets are found.
Authors:
 [1]
  1. Northern Illinois Univ., DeKalb, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Materials Sciences and Engineering Division; Northern Illinois University, Institute for Nanoscience, Engineering and Technology
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1393194

van Veenendaal, Michel. Ultrafast intersystem crossings in Fe-Co Prussian blue analogues. United States: N. p., Web. doi:10.1038/s41598-017-06664-4.
van Veenendaal, Michel. Ultrafast intersystem crossings in Fe-Co Prussian blue analogues. United States. doi:10.1038/s41598-017-06664-4.
van Veenendaal, Michel. 2017. "Ultrafast intersystem crossings in Fe-Co Prussian blue analogues". United States. doi:10.1038/s41598-017-06664-4. https://www.osti.gov/servlets/purl/1393194.
@article{osti_1393194,
title = {Ultrafast intersystem crossings in Fe-Co Prussian blue analogues},
author = {van Veenendaal, Michel},
abstractNote = {Ultrafast spincrossover is studied in Fe-Co Prussian blue analogues using a dissipative quantum-mechanical model of a cobalt ion coupled to a breathing mode. All electronic interactions are treated on an equal footing. It is theoretically demonstrated that the divalent cobalt ion reaches 90% of the S = 3/2 value within 20 fs after photoexciting a low-spin Co3+ ion by an iron-to-cobalt charge transfer. The doublet-to-quartet spin crossover is significantly faster than the oscillation period of the breathing mode. The system relaxes to the lowest manifold of divalent cobalt (4T1) in 150-200 fs. In conclusion, strong oscillations in spin-orbit coupling and the involvement of higher-lying quartets are found.},
doi = {10.1038/s41598-017-06664-4},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {2017},
month = {7}
}