Anomalous atomic fluctuations in the local structure around Mn of 
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 thin films

Kizaki, Hidetoshi; Hayashi, Kouichi; Cong, Lin; Happo, Naohisa; Hosokawa, Shinya; Hidaka, S.; Hayashi, Shuhei; Suzuki, Motohiro; Uchitomi, Naotaka

doi:10.1103/physrevb.106.064434

Cited by 8 publications

(3 citation statements)

References 29 publications

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“…This is comparable with the average R-factors of the Mn atoms of the synchrotron radiation [B-factor $ 26 A ˚2 (Umena et al, 2011)] or XFEL [B-factor $ 24 A ˚2 (Suga et al, 2015)] structures, suggesting that, aside from dynamic fluctuations caused by thermal vibrations at 100 K, the atoms in the Mn 4 CaO 5 cluster also have large positional fluctuations within the crystal. Though we were only able to extract average isotropic fluctuations in this work, we expect that in future work, the radial and angular positional fluctuations of Mn atoms can be extracted from more accurate hologram patterns, as this has already been demonstrated in XFH experiments on inorganic samples and organic crystals (Hosokawa et al, 2013;Hayashi et al, 2014;Ang et al, 2021;Kizaki et al, 2022). Once this is realized, valuable information to help understand the mechanisms of the oxidation process in PSII will be obtainable.…”

Section: Discussionmentioning

confidence: 80%

Development of serial X-ray fluorescence holography for radiation-sensitive protein crystals

Ang¹,

Umena²,

Sato‐Tomita³

et al. 2023

J Synchrotron Radiat

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X-ray fluorescence holography (XFH) is a powerful atomic resolution technique capable of directly imaging the local atomic structure around atoms of a target element within a material. Although it is theoretically possible to use XFH to study the local structures of metal clusters in large protein crystals, the experiment has proven difficult to perform, especially on radiation-sensitive proteins. Here, the development of serial X-ray fluorescence holography to allow the direct recording of hologram patterns before the onset of radiation damage is reported. By combining a 2D hybrid detector and the serial data collection used in serial protein crystallography, the X-ray fluorescence hologram can be directly recorded in a fraction of the measurement time needed for conventional XFH measurements. This approach was demonstrated by obtaining the Mn Kα hologram pattern from the protein crystal Photosystem II without any X-ray-induced reduction of the Mn clusters. Furthermore, a method to interpret the fluorescence patterns as real-space projections of the atoms surrounding the Mn emitters has been developed, where the surrounding atoms produce large dark dips along the emitter–scatterer bond directions. This new technique paves the way for future experiments on protein crystals that aim to clarify the local atomic structures of their functional metal clusters, and for other related XFH experiments such as valence-selective XFH or time-resolved XFH.

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Section: Discussionmentioning

confidence: 80%

Development of serial X-ray fluorescence holography for radiation-sensitive protein crystals

Ang¹,

Umena²,

Sato‐Tomita³

et al. 2023

J Synchrotron Radiat

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“…Thermal fluctuations in pure Fe and Co can be calculated with Debye temperatures of 703 and 683 K, respectively [18]. The magnitudes of the calculated fluctuations u are u Fe = 0.064 nm and u Co = 0.065 nm at 100 K, and u Fe = 0.095 nm and u Co = 0.096 nm at 300 K. The relationship between fluctuations and atomic image intensity has been calculated in previous studies [16,19]. According to the relationship and the u values, the intensity ratio at 300 and 100 K is only about 0.9, which does not explain the changes of a.…”

Section: Resultsmentioning

confidence: 91%

Local Structures of Fe0.08Co0.92 Studied by X-ray Fluorescence Holography

Fukui,

Kanno,

Yamakawa

et al. 2023

e-J. Surf. Sci. Nanotechnol.

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At room temperature, pure Co has a hexagonal close-packed (HCP) structure. When several percent of Fe is doped into a Co crystal, it changes to the face-centered cubic (FCC) structure. However, it is not clear why the FCC structure in the Fe x Co 1−x system is so stable even with small amounts of Fe concentration. Therefore, we carried out X-ray fluorescence holography (XFH) on a Fe 0.08 Co 0.92 single crystal to visualize the three-dimensional atomic images around both Fe and Co atoms. The intensities of the reconstructed images by XFH around Fe atoms at both 100 and 300 K are inversely proportional to the distance from the Fe emitter, and those at 100 K were always higher than those at 300 K due to the suppression of the thermal vibrations of atoms. However, the image intensities around Co did not increase by cooling unlike those around Fe. In particular, the distance dependence of the atomic image intensities at 100 K are roughly constant up to 0.8 nm. This suggests that the lattice around Co, i.e., matrix crystal lattice of Fe 0.08 Co 0.92 , is more distorted than that around dopant Fe.

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“…X-ray fluorescence holography (XFH) is a promising method to elucidate the arrangement of the solute-elements in Mg-TM-RE alloy. XFH can visualize three-dimensional atomic arrangement around a specific element [18][19][20] , and has been applied to various structural and functional materials [21][22][23][24][25][26][27][28][29][30] , including Mg85Zn6Y9 and Mg75Zn10Y15 alloys 31,32) . In particular, XFH is applicable to dilute systems 33) , and thus local structures around solute-elements in dilute Mg99.2Zn0.2Y0.6 alloy are expected to be clarified by this technique.…”

Section: Introductionmentioning

confidence: 99%

Local Structural Analysis around Solute-Element in Annealed Mg99.2Zn0.2Y0.6 Alloy Using X-ray Fluorescence Holography

et al. 2023

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X-ray fluorescence holography was applied to dilute Mg99.2Zn0.2Y0.6 alloy annealed at 520 ℃ for 5 h to obtain atomic images around Zn atom. In spite of the extremely low concentration of the soluteelement, clear hologram patterns were obtained. The reconstructed atomic images revealed that the Zn atom in this annealed Mg99.2Zn0.2Y0.6 alloy mainly occupy the hcp Mg site. This finding is consistent with the transmission electron microscope image, where fcc-type stacking faults are hardly observed. These results are in contrast to the previous report that Zn and Y form short-range-ordered solute clusters at the fcc-type stacking fault in Mg-Zn-Y alloy. The effect of heat treatment on the atomic arrangement of solute-elements in this dilute alloy is discussed in relation to the previously reported mechanical properties.

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Anomalous atomic fluctuations in the local structure around Mn of (Zn,Sn,Mn)As2 thin films

Cited by 8 publications

References 29 publications

Development of serial X-ray fluorescence holography for radiation-sensitive protein crystals

Development of serial X-ray fluorescence holography for radiation-sensitive protein crystals

Local Structures of Fe<sub>0.08</sub>Co<sub>0.92</sub> Studied by X-ray Fluorescence Holography

Local Structural Analysis around Solute-Element in Annealed Mg<sub>99.2</sub>Zn<sub>0.2</sub>Y<sub>0.6</sub> Alloy Using X-ray Fluorescence Holography

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