High-pressure structural behavior and elastic properties of U3Si5: A combined synchrotron XRD and DFT study

Jason L. Baker; Gaoxue Wang; Tashiema Ulrich; Josh T. White; Enrique R. Batista; Ping Yang; Robert C. Roback; Changyong Park; Hongwu Xu

doi:10.1016/j.jnucmat.2020.152373

High-pressure structural behavior and elastic properties of U₃Si₅: A combined synchrotron XRD and DFT study

Jason L. Baker, Gaoxue Wang, Tashiema Ulrich, Josh T. White, Enrique R. Batista, Ping Yang, Robert C. Roback, Changyong Park, Hongwu Xu

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

We present an integrated experimental and theoretical study of the structural behavior of U₃Si₅ at high-pressure conditions using angle-dispersive synchrotron X-ray diffraction (XRD) in a diamond anvil cell (DAC) and density functional theory (DFT) calculations. On increasing pressure, the ambient hexagonal structure of U₃Si₅ with space group P6/mmm remains stable up to 16.7 GPa, the maximum pressure tested with DAC. The bulk modulus and the a- and c-axial moduli of U₃Si₅ were experimentally determined to be 126 ± 4 GPa, 173 ± 8 GPa and 79.7 ± 4.3 GPa, respectively. Thus an anisotropy in the axial compressibility of U₃Si₅ is observed with its c-axis being more compressible than the a-axis. Our DFT calculation results are in general agreement with the experimental values, including reproducing the compressibility anisotropy. A comparison of the bulk modulus of U₃Si₅ to those of other U–Si compounds reveals a general trend that the bulk modulus of U–Si decreases with increasing U/(U + Si) ratio.

Original language	English
Article number	152373
Journal	Journal of Nuclear Materials
Volume	540
DOIs	https://doi.org/10.1016/j.jnucmat.2020.152373
State	Published - Nov 2020
Externally published	Yes

Funding

Research presented in this article was supported by the Laboratory Directed Research and Development (LDRD) program at Los Alamos National Laboratory (LANL) under project number 20180007. JLB acknowledges the support of the Seaborg Institute through a LANL Seaborg postdoctoral fellowship. The authors would like to thank Andrew J. Gaunt for useful discussions and comments. LANL, an affirmative action/equal opportunity employer, is managed by Triad National Security Administration of the U.S. Department of Energy under contract number 89233218CNA000001. High-P synchrotron XRD experiments were performed at HPCAT (Sector 16), Advanced Photon Source (APS), Argonne National Laboratory. HPCAT operations are supported by DOE-NNSA's Office of Experimental Sciences. The Advanced Photon Source is a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Research presented in this article was supported by the Laboratory Directed Research and Development (LDRD) program at Los Alamos National Laboratory (LANL) under project number 20180007 . JLB acknowledges the support of the Seaborg Institute through a LANL Seaborg postdoctoral fellowship . The authors would like to thank Andrew J. Gaunt for useful discussions and comments. LANL, an affirmative action/equal opportunity employer, is managed by Triad National Security Administration of the U.S. Department of Energy under contract number 89233218CNA000001 . High-P synchrotron XRD experiments were performed at HPCAT (Sector 16), Advanced Photon Source (APS), Argonne National Laboratory. HPCAT operations are supported by DOE-NNSA’s Office of Experimental Sciences. The Advanced Photon Source is a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357 .

Funders	Funder number
DOE Office of Science
DOE-NNSA's Office of Experimental Sciences
DOE-NNSA’s Office of Experimental Sciences
Seaborg Institute
U.S. Department of Energy	89233218CNA000001
Office of Science
Argonne National Laboratory	DE-AC02-06CH11357
Laboratory Directed Research and Development
Los Alamos National Laboratory	20180007

Keywords

Bulk modulus
Crystal structure
Density functional theory
Diamond anvil cell
High pressure
Synchrotron X-ray diffraction
Uranium silicide

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10.1016/j.jnucmat.2020.152373

Cite this

@article{c1562a82125041b7b93be71537ae680c,

title = "High-pressure structural behavior and elastic properties of U3Si5: A combined synchrotron XRD and DFT study",

abstract = "We present an integrated experimental and theoretical study of the structural behavior of U3Si5 at high-pressure conditions using angle-dispersive synchrotron X-ray diffraction (XRD) in a diamond anvil cell (DAC) and density functional theory (DFT) calculations. On increasing pressure, the ambient hexagonal structure of U3Si5 with space group P6/mmm remains stable up to 16.7 GPa, the maximum pressure tested with DAC. The bulk modulus and the a- and c-axial moduli of U3Si5 were experimentally determined to be 126 ± 4 GPa, 173 ± 8 GPa and 79.7 ± 4.3 GPa, respectively. Thus an anisotropy in the axial compressibility of U3Si5 is observed with its c-axis being more compressible than the a-axis. Our DFT calculation results are in general agreement with the experimental values, including reproducing the compressibility anisotropy. A comparison of the bulk modulus of U3Si5 to those of other U–Si compounds reveals a general trend that the bulk modulus of U–Si decreases with increasing U/(U + Si) ratio.",

keywords = "Bulk modulus, Crystal structure, Density functional theory, Diamond anvil cell, High pressure, Synchrotron X-ray diffraction, Uranium silicide",

author = "Baker, {Jason L.} and Gaoxue Wang and Tashiema Ulrich and White, {Josh T.} and Batista, {Enrique R.} and Ping Yang and Roback, {Robert C.} and Changyong Park and Hongwu Xu",

note = "Publisher Copyright: {\textcopyright} 2020 Elsevier B.V.",

year = "2020",

month = nov,

doi = "10.1016/j.jnucmat.2020.152373",

language = "English",

volume = "540",

journal = "Journal of Nuclear Materials",

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T1 - High-pressure structural behavior and elastic properties of U3Si5

T2 - A combined synchrotron XRD and DFT study

AU - Baker, Jason L.

AU - Wang, Gaoxue

AU - Ulrich, Tashiema

AU - White, Josh T.

AU - Batista, Enrique R.

AU - Yang, Ping

AU - Roback, Robert C.

AU - Park, Changyong

AU - Xu, Hongwu

PY - 2020/11

Y1 - 2020/11

N2 - We present an integrated experimental and theoretical study of the structural behavior of U3Si5 at high-pressure conditions using angle-dispersive synchrotron X-ray diffraction (XRD) in a diamond anvil cell (DAC) and density functional theory (DFT) calculations. On increasing pressure, the ambient hexagonal structure of U3Si5 with space group P6/mmm remains stable up to 16.7 GPa, the maximum pressure tested with DAC. The bulk modulus and the a- and c-axial moduli of U3Si5 were experimentally determined to be 126 ± 4 GPa, 173 ± 8 GPa and 79.7 ± 4.3 GPa, respectively. Thus an anisotropy in the axial compressibility of U3Si5 is observed with its c-axis being more compressible than the a-axis. Our DFT calculation results are in general agreement with the experimental values, including reproducing the compressibility anisotropy. A comparison of the bulk modulus of U3Si5 to those of other U–Si compounds reveals a general trend that the bulk modulus of U–Si decreases with increasing U/(U + Si) ratio.

AB - We present an integrated experimental and theoretical study of the structural behavior of U3Si5 at high-pressure conditions using angle-dispersive synchrotron X-ray diffraction (XRD) in a diamond anvil cell (DAC) and density functional theory (DFT) calculations. On increasing pressure, the ambient hexagonal structure of U3Si5 with space group P6/mmm remains stable up to 16.7 GPa, the maximum pressure tested with DAC. The bulk modulus and the a- and c-axial moduli of U3Si5 were experimentally determined to be 126 ± 4 GPa, 173 ± 8 GPa and 79.7 ± 4.3 GPa, respectively. Thus an anisotropy in the axial compressibility of U3Si5 is observed with its c-axis being more compressible than the a-axis. Our DFT calculation results are in general agreement with the experimental values, including reproducing the compressibility anisotropy. A comparison of the bulk modulus of U3Si5 to those of other U–Si compounds reveals a general trend that the bulk modulus of U–Si decreases with increasing U/(U + Si) ratio.

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KW - Crystal structure

KW - Density functional theory

KW - Diamond anvil cell

KW - High pressure

KW - Synchrotron X-ray diffraction

KW - Uranium silicide

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