4.8 Article

Probing electronic structure in berkelium and californium via an electron microscopy nanosampling approach

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NATURE COMMUNICATIONS
卷 12, 期 1, 页码 -

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NATURE RESEARCH
DOI: 10.1038/s41467-021-21189-1

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  1. U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-AC02-05CH11231]
  2. DOE, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division at LBNL [DE-AC02-05CH11231]
  3. STROBE, a Science and Technology Center - National Science Foundation

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In this work, the authors utilize transmission electron microscopy to characterize highly-radioactive compounds of berkelium and californium, requiring only small amounts of the elements. They find that berkelium exhibits unexpectedly weak spin-orbit coupling, while californium follows a jj coupling scheme.
Due to their rarity and radioactive nature, comparatively little is known about the actinides, particularly those with atomic numbers higher than that of plutonium, and their compounds. In this work, we describe how transmission electron microscopy can provide comprehensive, safe, and cost-effective characterization using only single nanogram amounts of highly-radioactive, solid compounds. Chlorides of the rare elements berkelium and californium are dropcast and then converted in situ to oxides using the electron beam. The f-band occupancies are probed using electron energy loss spectroscopy and an unexpectedly weak spin-orbit-coupling is identified for berkelium. In contrast, californium follows a jj coupling scheme. These results have important implications for the chemistries of these elements and solidify the status of californium as a transitional element in the actinide series. The obtention and study of actinide elements is challenging due to various factors including their radioactivity and scarcity. Herein, the authors characterize the atomic and electronic structure of Am, Cm, Bk, and Cf compounds using a transmission electron microscopy-based workflow that only requires nanogram amounts of the actinide element.

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