Monitoring Ultrafast Spin Crossover Intermediates in an Iron(II) Complex by Broad Band Stimulated X-ray Raman Spectroscopy

Zhang, Yu; Bennett, Kochise; Mukamel, Shaul

doi:10.1021/acs.jpca.8b01762

Title: Monitoring Ultrafast Spin Crossover Intermediates in an Iron(II) Complex by Broad Band Stimulated X-ray Raman Spectroscopy

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Abstract

Here, the photoinduced spin crossover dynamics of transition metal complexes is of fundamental scientific importance and is used for sensor device applications and solar energy harvesting. Current X-ray and optical spectroscopy experiments for [Fe^II(bpy)₃], an archetypal earth-abundant metal complex, show conflicting spin dynamics. We have simulated the broad band transient X-ray absorption and hybrid (broad + narrow band) X-ray stimulated Raman signals at the N and Fe K-edges of the key excited state intermediates involved in the spin crossover process of this complex. We find that these signals are much more sensitive to electron and spin populations than transition absorption and may be useful in the design of photovoltaic and artificial photosynthetic systems.

Authors:

Zhang, Yu ^[1];

^[2];

^[3]

Univ. of California, Irvine, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Univ. of California, Irvine, CA (United States); Univ. of California, Berkeley, CA (United States)
Univ. of California, Irvine, CA (United States)

Publication Date:: 2018-06-26

Research Org.:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1476121

Grant/Contract Number:: AC02-76SF00515; CHE-1361516; FG02-04ER15571

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

Additional Journal Information:: Journal Volume: 122; Journal Issue: 32; Journal ID: ISSN 1089-5639

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Zhang, Yu, Bennett, Kochise, and Mukamel, Shaul. Monitoring Ultrafast Spin Crossover Intermediates in an Iron(II) Complex by Broad Band Stimulated X-ray Raman Spectroscopy.  United States: N. p., 2018. 
Web.  doi:10.1021/acs.jpca.8b01762.

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                    Zhang, Yu, Bennett, Kochise, & Mukamel, Shaul. Monitoring Ultrafast Spin Crossover Intermediates in an Iron(II) Complex by Broad Band Stimulated X-ray Raman Spectroscopy.  United States.  https://doi.org/10.1021/acs.jpca.8b01762

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                    Zhang, Yu, Bennett, Kochise, and Mukamel, Shaul. Tue .  
"Monitoring Ultrafast Spin Crossover Intermediates in an Iron(II) Complex by Broad Band Stimulated X-ray Raman Spectroscopy".  United States.  https://doi.org/10.1021/acs.jpca.8b01762.  https://www.osti.gov/servlets/purl/1476121.

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@article{osti_1476121,

  title        = {Monitoring Ultrafast Spin Crossover Intermediates in an Iron(II) Complex by Broad Band Stimulated X-ray Raman Spectroscopy},

  author       = {Zhang, Yu and Bennett, Kochise and Mukamel, Shaul},

  abstractNote = {Here, the photoinduced spin crossover dynamics of transition metal complexes is of fundamental scientific importance and is used for sensor device applications and solar energy harvesting. Current X-ray and optical spectroscopy experiments for [FeII(bpy)3], an archetypal earth-abundant metal complex, show conflicting spin dynamics. We have simulated the broad band transient X-ray absorption and hybrid (broad + narrow band) X-ray stimulated Raman signals at the N and Fe K-edges of the key excited state intermediates involved in the spin crossover process of this complex. We find that these signals are much more sensitive to electron and spin populations than transition absorption and may be useful in the design of photovoltaic and artificial photosynthetic systems.},

  doi          = {10.1021/acs.jpca.8b01762},

  journal      = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},

  number       = 32,

  volume       = 122,

  place        = {United States},

  year         = {2018},

  month        = {6}

}

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