U8Al19Si6, A Uranium Aluminide Silicide with a Stuffed Supercell Grown from Aluminum Flux
Abstract
In this work, U8Al19Si6 is formed from the reaction of uranium oxide and silicon in aluminum flux. Growth of this material is dependent on the presence of surface hydroxyl groups on alumina in the crucible. The compound forms as large cuboid crystals with a complex new structure that is a cubic stuffed supercell of UAl3 (AuCu3 parent structure type). It features a 4-fold expansion of the unit cell axis and the addition of atoms on two extra positions resulting in Pm$$\bar{3n}$$ symmetry. The ordered distribution of aluminum and silicon was determined using single crystal neutron diffraction. The magnetic susceptibility shows temperature independent paramagnetic behavior, while heat capacity measurements are consistent with Fermi liquid characteristics at low temperatures where the Sommerfeld constant is enhanced in comparison to that of a conventional metal. Lastly, these bulk thermodynamic properties indicate that U8Al19Si6 is an itinerant electron Pauli paramagnet with moderately enhanced mass charge carrier quasiparticles.
- Authors:
-
[1]
- Florida State Univ., Tallahassee, FL (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Actinide Science & Technology (CAST); Florida State Univ., Tallahassee, FL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1566343
- Grant/Contract Number:
- SC0016568
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 30; Journal Issue: 11; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nuclear; defects; mechanical behavior; corrosion; charge transport; superconductivity; magnetism and spin physics; separations; geophysics/geochemistry; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (predictive); synthesis (scalable processing)
Citation Formats
Potter, Wesley M., Lai, You, Cao, Huibo, Baumbach, Ryan E., and Latturner, Susan E. U8Al19Si6, A Uranium Aluminide Silicide with a Stuffed Supercell Grown from Aluminum Flux. United States: N. p., 2018.
Web. doi:10.1021/acs.chemmater.8b00948.
Potter, Wesley M., Lai, You, Cao, Huibo, Baumbach, Ryan E., & Latturner, Susan E. U8Al19Si6, A Uranium Aluminide Silicide with a Stuffed Supercell Grown from Aluminum Flux. United States. https://doi.org/10.1021/acs.chemmater.8b00948
Potter, Wesley M., Lai, You, Cao, Huibo, Baumbach, Ryan E., and Latturner, Susan E. Thu .
"U8Al19Si6, A Uranium Aluminide Silicide with a Stuffed Supercell Grown from Aluminum Flux". United States. https://doi.org/10.1021/acs.chemmater.8b00948. https://www.osti.gov/servlets/purl/1566343.
@article{osti_1566343,
title = {U8Al19Si6, A Uranium Aluminide Silicide with a Stuffed Supercell Grown from Aluminum Flux},
author = {Potter, Wesley M. and Lai, You and Cao, Huibo and Baumbach, Ryan E. and Latturner, Susan E.},
abstractNote = {In this work, U8Al19Si6 is formed from the reaction of uranium oxide and silicon in aluminum flux. Growth of this material is dependent on the presence of surface hydroxyl groups on alumina in the crucible. The compound forms as large cuboid crystals with a complex new structure that is a cubic stuffed supercell of UAl3 (AuCu3 parent structure type). It features a 4-fold expansion of the unit cell axis and the addition of atoms on two extra positions resulting in Pm$\bar{3n}$ symmetry. The ordered distribution of aluminum and silicon was determined using single crystal neutron diffraction. The magnetic susceptibility shows temperature independent paramagnetic behavior, while heat capacity measurements are consistent with Fermi liquid characteristics at low temperatures where the Sommerfeld constant is enhanced in comparison to that of a conventional metal. Lastly, these bulk thermodynamic properties indicate that U8Al19Si6 is an itinerant electron Pauli paramagnet with moderately enhanced mass charge carrier quasiparticles.},
doi = {10.1021/acs.chemmater.8b00948},
journal = {Chemistry of Materials},
number = 11,
volume = 30,
place = {United States},
year = {2018},
month = {5}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 2 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
The effect of silicon on the interaction between metallic uranium and aluminum: A 50 year long diffusion experiment
journal, November 2008
- Leenaers, A.; Detavernier, C.; Van den Berghe, S.
- Journal of Nuclear Materials, Vol. 381, Issue 3
Literature review of thermal and radiation performance parameters for high-temperature, uranium dioxide fueled cermet materials
journal, July 2007
- Haertling, C.; Hanrahan, R. J.
- Journal of Nuclear Materials, Vol. 366, Issue 3
The Metal Flux: A Preparative Tool for the Exploration of Intermetallic Compounds
journal, November 2005
- Kanatzidis, Mercouri G.; Pöttgen, Rainer; Jeitschko, Wolfgang
- Angewandte Chemie International Edition, Vol. 44, Issue 43
Adventures in Crystal Growth: Synthesis and Characterization of Single Crystals of Complex Intermetallic Compounds
journal, December 2011
- Phelan, W. Adam; Menard, Melissa C.; Kangas, Michael J.
- Chemistry of Materials, Vol. 24, Issue 3
Clusters, Assemble: Growth of Intermetallic Compounds from Metal Flux Reactions
journal, December 2017
- Latturner, Susan E.
- Accounts of Chemical Research, Vol. 51, Issue 1
Use of frit-disc crucibles for routine and exploratory solution growth of single crystalline samples
journal, December 2015
- Canfield, Paul C.; Kong, Tai; Kaluarachchi, Udhara S.
- Philosophical Magazine, Vol. 96, Issue 1
Formation of Multinary Intermetallics from Reduction of Perovskites by Aluminum Flux: M 3 Au 6+ x Al 26 Ti (M = Ca, Sr, Yb), a Stuffed Variant of the BaHg 11 Type
journal, November 2003
- Latturner, Susan E.; Kanatzidis, Mercouri G.
- Inorganic Chemistry, Vol. 43, Issue 1
Competing Phases, Complex Structure, and Complementary Diffraction Studies of R 3-δ FeAl 4-x Mg x Tt 2 Intermetallics (R = Y, Dy, Er, Yb; Tt = Si or Ge; x < 0.5)
journal, August 2013
- Ma, Xiaowei; Whalen, Jeffrey B.; Cao, Huibo
- Chemistry of Materials, Vol. 25, Issue 16
REAu4Al8Si: the end member of a new homologous series of intermetallics featuring thick AuAl2 layersElectronic Supplementary Information (ESI) available: crystallographic data for all analogues (tables of atomic positions, thermal parameters, bond lengths) in the form of cif files. See http://www.rsc.org/suppdata/cc/b3/b306641j/.
journal, January 2003
- Latturner, Susan E.; Kanatzidis, Mercouri G.
- Chemical Communications, Issue 18
Synthesis and Properties of New Multinary Silicides R 5 Mg 5 Fe 4 Al x Si 18– x (R = Gd, Dy, Y, x ≈ 12) Grown in Mg/Al Flux
journal, May 2012
- Ma, Xiaowei; Chen, Banghao; Latturner, Susan E.
- Inorganic Chemistry, Vol. 51, Issue 11
Quaternary Intermetallics Grown from Molten Aluminum: The Homologous Series Th 2 (Au x Si 1 - x )[AuAl 2 ] n Si 2 ( n = 1, 2, 4)
journal, April 2002
- Latturner, S. E.; Bilc, D.; Mahanti, S. D.
- Chemistry of Materials, Vol. 14, Issue 4
Ordered U(Al, Si)3 phase: Structure and bonding
journal, January 2017
- Zenou, V. Y.; Rafailov, G.; Dahan, I.
- Journal of Alloys and Compounds, Vol. 690
New ordered phase in the quasi-binary UAl 3 –USi 3 system
journal, May 2014
- Rafailov, Gennady; Dahan, Isaac; Meshi, Louisa
- Acta Crystallographica Section B Structural Science, Crystal Engineering and Materials, Vol. 70, Issue 3
Electronic properties of Al, and Sn) compounds in high magnetic fields: Transport, specific heat, magnetization, and quantum oscillations
journal, June 1999
- Cornelius, A. L.; Arko, A. J.; Sarrao, J. L.
- Physical Review B, Vol. 59, Issue 22
Superconductivity in uranium compounds with Au structure
journal, February 1985
- Ott, H. R.; Hulliger, F.; Rudigier, H.
- Physical Review B, Vol. 31, Issue 3
Four-circle single-crystal neutron diffractometer at the High Flux Isotope Reactor
journal, May 2011
- Chakoumakos, Bryan C.; Cao, Huibo; Ye, Feng
- Journal of Applied Crystallography, Vol. 44, Issue 3
Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993
- Rodríguez-Carvajal, Juan
- Physica B: Condensed Matter, Vol. 192, Issue 1-2
Flux growth utilizing the reaction between flux and crucible
journal, April 2015
- Yan, J. -Q.
- Journal of Crystal Growth, Vol. 416
Metal Nitrides Grown from Ca/Li Flux: Ca 6 Te 3 N 2 and New Nitridoferrate(I) Ca 6 (Li x Fe 1– x )Te 2 N 3
journal, August 2016
- Dickman, Matthew J.; Latturner, Susan E.
- Journal of the American Chemical Society, Vol. 138, Issue 33
Nd8Co4−Al Ge2C3: A case study in flux growth of lanthanide-rich intermetallics
journal, April 2016
- Zhou, Sixuan; Latturner, Susan E.
- Journal of Solid State Chemistry, Vol. 236
Morphology, Dispersion, and Stability of Cu Nanoclusters on Clean and Hydroxylated α-Al 2 O 3 (0001) Substrates
journal, October 2008
- Jensen, M. C. R.; Venkataramani, K.; Helveg, S.
- The Journal of Physical Chemistry C, Vol. 112, Issue 43
Towards Realistic Surface Science Models of Heterogeneous Catalysts: Influence of Support Hydroxylation and Catalyst Preparation Method
journal, March 2013
- Sterrer, Martin; Freund, Hans-Joachim
- Catalysis Letters, Vol. 143, Issue 5
Neutron scattering lengths and cross sections
journal, January 1992
- Sears, Varley F.
- Neutron News, Vol. 3, Issue 3
Filling in the Holes: Structural and Magnetic Properties of the Chemical Pressure Stabilized LnMn x Ga 3 (Ln = Ho–Tm; x < 0.15)
journal, December 2013
- Fulfer, Bradford W.; McAlpin, Jacob D.; Engelkemier, Joshua
- Chemistry of Materials, Vol. 26, Issue 2
Rare-earth chromium gallides RE4CrGa12 (RE=Tb–Tm)
journal, December 2012
- Slater, Brianna R.; Bie, Haiying; Stoyko, Stanislav S.
- Journal of Solid State Chemistry, Vol. 196
Development and Loss of Ferromagnetism Controlled by the Interplay of Ge Concentration and Mn Vacancies in Structurally Modulated Y 4 Mn 1− x Ga 12− y Ge y
journal, June 2010
- Francisco, Melanie C.; Malliakas, Christos D.; Piccoli, Paula M. B.
- Journal of the American Chemical Society, Vol. 132, Issue 26
DFT-Chemical Pressure Analysis: Visualizing the Role of Atomic Size in Shaping the Structures of Inorganic Materials
journal, March 2012
- Fredrickson, Daniel C.
- Journal of the American Chemical Society, Vol. 134, Issue 13
Fermi Surface Properties of the Enhanced Pauli Paramagnet UAl 3
journal, August 2000
- Aoki, Dai; Watanabe, Narumi; Inada, Yoshihiko
- Journal of the Physical Society of Japan, Vol. 69, Issue 8
Works referencing / citing this record:
Neutron Instruments for Research in Coordination Chemistry: Neutron Instruments for Research in Coordination Chemistry
journal, January 2019
- Xue, Zi-Ling; Ramirez-Cuesta, Anibal J.; Brown, Craig M.
- European Journal of Inorganic Chemistry, Vol. 2019, Issue 8