Probing soft X-ray induced photoreduction of a model Mn-complex at cryogenic conditions

  • Kuntal Chatterjee
  • , Sang Jun Lee
  • , Li Cheng Kao
  • , Margaret D. Doyle
  • , Charles J. Titus
  • , Stephen R. Leone
  • , Junko Yano
  • , Vittal K. Yachandra
  • , Philippe Wernet
  • , Jan F. Kern

研究成果: Article同行評審

摘要

Soft X-ray absorption spectroscopy of first row transition elements at their respective L-edges provides important information about the oxidation and spin states of the metal centers. However, the associated sample damage in radiation-sensitive samples substantially alters the electronic and chemical structures of redox-active metal centers. Here, we measure the soft X-ray spectrum of the model MnIII(acac)3 complex containing a redox-active MnIII metal center in an octahedral environment with a superconducting transition-edge sensor detector. To reduce the secondary damage resulting primarily from the diffusion of radicals and electrons, the spectra are collected at 30 K and 80 K on solid samples. Starting from the first scan, we detect the contribution of X-ray induced sample damage leading to a change in the MnII intensity. However, at low temperatures, particularly at 30 K, we do not observe a gradual increase in the radiation damage with successive scans with the X-ray beam at the same spot. At our estimated dose of 90 kGy, we find 62% of MnIII(acac)3 is still intact at 30 K. However, at room temperature, we see a gradual increase in radiation damage with increasing numbers of scans at the same spot, which is consistent with the possibility of increased diffusion rates of secondary radicals and electrons as noted in other studies.

原文English
頁(從 - 到)399-407
頁數9
期刊Journal of Synchrotron Radiation
32
發行號Pt 2
DOIs
出版狀態Published - 2025 3月 1

All Science Journal Classification (ASJC) codes

  • 輻射
  • 核能與高能物理
  • 儀器

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