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X-ray-induced sample damage at the Mn L-edge: a case study for soft X-ray spectroscopy of transition metal complexes in solution
Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Berlin, Germany.
Lawrence Berkeley National Laboratory, Berkeley, USA.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Theoretical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Theoretical Chemistry.
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2018 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 20, no 24, p. 16817-16827Article in journal (Refereed) Published
Abstract [en]

X-ray induced sample damage can impede electronic and structural investigations of radiation-sensitive samples studied with X-rays. Here we quantify dose-dependent sample damage to the prototypical Mn-III(acac)(3) complex in solution and at room temperature for the soft X-ray range, using X-ray absorption spectroscopy at the Mn L-edge. We observe the appearance of a reduced Mn-II species as the X-ray dose is increased. We find a half-damage dose of 1.6 MGy and quantify a spectroscopically tolerable dose on the order of 0.3 MGy (1 Gy = 1 J kg(-1)), where 90% of Mn-III(acac)(3) are intact. Our dose-limit is around one order of magnitude lower than the Henderson limit (half-damage dose of 20 MGy) which is commonly employed for protein crystallography with hard X-rays. It is comparable, however, to the dose-limits obtained for collecting un-damaged Mn K-edge spectra of the photosystem II protein, using hard X-rays. The dose-dependent reduction of Mn-III observed here for solution samples occurs at a dose limit that is two to four orders of magnitude smaller than the dose limits previously reported for soft X-ray spectroscopy of iron samples in the solid phase. We compare our measured to calculated spectra from ab initio restricted active space (RAS) theory and discuss possible mechanisms for the observed dose-dependent damage of Mn-III(acac)(3) in solution. On the basis of our results, we assess the influence of sample damage in other experimental studies with soft X-rays from storage-ring synchrotron radiation sources and X-ray free-electron lasers.

Place, publisher, year, edition, pages
RSC Publishing, 2018. Vol. 20, no 24, p. 16817-16827
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Physical Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-357207DOI: 10.1039/c8cp03094dISI: 000436032900053OAI: oai:DiVA.org:uu-357207DiVA, id: diva2:1238497
Funder
Swedish Research Council, 2012-3924Knut and Alice Wallenberg Foundation, KAW-2013.0020Swedish National Infrastructure for Computing (SNIC), snic2016-1-464NIH (National Institute of Health), GM110501NIH (National Institute of Health), GM126289NIH (National Institute of Health), GM55302Available from: 2018-08-13 Created: 2018-08-13 Last updated: 2018-09-14Bibliographically approved

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Guo, MeiyuanKällman, ErikLundberg, Marcus

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