@article{0456119a65b0488fb485f91b7eeae9b2,
title = "Fluctuation cepstral scanning transmission electron microscopy of mixed-phase amorphous materials",
abstract = "Four-dimensional scanning transmission electron microscopy (4D-STEM) is a versatile analytical tool for characterizing materials structural properties. However, extending such analysis to disordered materials is challenging, especially in technologically important samples with mixed ordered and disordered phases. Here, we present a new 4D-STEM method, called fluctuation cepstral STEM (FC-STEM), based on the fluctuation analysis of cepstral transform of diffraction patterns. The peaks in the associated transformation relate to inter-atomic distances in a thin sample. By varying the real-space range over which fluctuations are calculated, distinct ordered and disordered phases can be mapped in a diffractive image reconstruction. We demonstrate the principles of FC-STEM by characterizing a silicon anode, harvested from a cycled lithium-ion battery. A mixture of amorphous and nanocrystalline silicon, graphitic carbon, and electrolyte by-products is identified and mapped. Comparisons with conventional electron imaging and energy-dispersive X-ray spectroscopy show that FC-STEM is highly effective for the structure determination of mixed-phase amorphous materials.",
keywords = "4D-STEM, Amorphous silicon, Disordered materials, Electron diffractiion cepstrum, Electron nanodiffraction, Fluctuation electron microscopy, Lithium-ion battery",
author = "Saran Pidaparthy and Haoyang Ni and Hanyu Hou and Abraham, {Daniel P.} and Zuo, {Jian Min}",
note = "SP acknowledges support from the U.S. Department of Energy (DOE) Graduate Student Research (SCGSR) program. The SCGSR program is administered by the Oak Ridge Institute for Science and Education for DOE under contract number DE-SC0014664. DA is grateful for support from DOE's Vehicle Technologies Office (VTO). JMZ is supported by the U.S. DOE, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under contract No.DE-SC0022060. This work was carried out in part at the Materials Research Laboratory Central Research Facilities, University of Illinois. The silicon electrodes used in this article are from Argonne's Cell Analysis, Modeling and Prototyping (CAMP) Facility. We are grateful to Marco Rodrigues, Steve Trask and Andy Jansen for their assistance during the course of this research. Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02–06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. SP acknowledges support from the U.S. Department of Energy (DOE) Graduate Student Research (SCGSR) program. The SCGSR program is administered by the Oak Ridge Institute for Science and Education for DOE under contract number DE‐SC0014664. DA is grateful for support from DOE's Vehicle Technologies Office (VTO). JMZ is supported by the U.S. DOE, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under contract No.DE-SC0022060. This work was carried out in part at the Materials Research Laboratory Central Research Facilities, University of Illinois. The silicon electrodes used in this article are from Argonne's Cell Analysis, Modeling and Prototyping (CAMP) Facility. We are grateful to Marco Rodrigues, Steve Trask and Andy Jansen for their assistance during the course of this research. Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02–06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government.",
year = "2023",
month = jun,
doi = "10.1016/j.ultramic.2023.113718",
language = "English (US)",
volume = "248",
journal = "Ultramicroscopy",
issn = "0304-3991",
publisher = "Elsevier B.V.",
}