The structure of amorphous and deeply supercooled liquid alumina

Caijuan Shi; Oliver L.G. Alderman; Diana Berman; Jincheng Du; Joerg Neuefeind; Anthony Tamalonis; J. K.Richard Weber; Jinglin You; Chris J. Benmore

doi:10.3389/fmats.2019.00038

The structure of amorphous and deeply supercooled liquid alumina

Caijuan Shi, Oliver L.G. Alderman, Diana Berman, Jincheng Du, Joerg Neuefeind, Anthony Tamalonis, J. K.Richard Weber, Jinglin You, Chris J. Benmore

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Abstract

Liquid Al₂O₃ has been supercooled more than 500 K below its melting point (T_m = 2,327 K) using aerodynamic levitation and laser heating techniques. High energy synchrotron x-ray measurements were performed over a temperature range of 1,817 ≤ T (K) ≤ 2,700 and stroboscopic neutron diffraction at 1,984 and 2,587 K. The diffraction patterns have been fitted with Empirical Potential Structure Refinement (EPSR) models and compared to classical Molecular Dynamics (MD) simulation results. Both sets of models show similar trends, indicating the presence of high populations of AlO₄ and AlO₅ polyhedral units predominantly linked by triply shared oxygen atoms. EPSR reveals that the mean Al–O coordination number changes linearly with temperature with n_AlO = 4.41 – [1.25 × 10⁻⁴] (T – T_m), with a 2.5 Å cutoff. Both EPSR and MD simulations reveal a direction of the temperature dependence of the aluminate network structure which moves further away from the glass forming ideal (n_AlO = 3) during supercooling. Furthermore, we provide new experimental data and models for amorphous alumina grown by sequential infiltration synthesis of a polymer template. The amorphous solid form likely has a larger Al-O coordination number than the liquid, consistent with expectations for the hypothetical glass.

Original language	English
Article number	38
Journal	Frontiers in Materials
Volume	6
DOIs	https://doi.org/10.3389/fmats.2019.00038
State	Published - Mar 8 2019

Funding

CS gratefully acknowledges financial support from the China Scholarship Council (CSC No. 201706890053). This research used resources of the Advanced Photon Source, the 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 and by the Spallation Neutron Source, Oak Ridge National Laboratory under Contract No. DE-AC05-00OR22725. This work was partially funded under DOE grant number DE-SC0015241.

Funders	Funder number
U.S. Department of Energy
Office of Science
Argonne National Laboratory	DE-AC02-06CH11357
Oak Ridge National Laboratory	DE-AC05-00OR22725, DE-SC0015241
China Scholarship Council	201706890053

Keywords

Alumina
Amorphous
Glass forming ability
Structure
Supercooled liquid
X-ray diffraction

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10.3389/fmats.2019.00038

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title = "The structure of amorphous and deeply supercooled liquid alumina",

abstract = "Liquid Al2O3 has been supercooled more than 500 K below its melting point (Tm = 2,327 K) using aerodynamic levitation and laser heating techniques. High energy synchrotron x-ray measurements were performed over a temperature range of 1,817 ≤ T (K) ≤ 2,700 and stroboscopic neutron diffraction at 1,984 and 2,587 K. The diffraction patterns have been fitted with Empirical Potential Structure Refinement (EPSR) models and compared to classical Molecular Dynamics (MD) simulation results. Both sets of models show similar trends, indicating the presence of high populations of AlO4 and AlO5 polyhedral units predominantly linked by triply shared oxygen atoms. EPSR reveals that the mean Al–O coordination number changes linearly with temperature with nAlO = 4.41 – [1.25 × 10−4] (T – Tm), with a 2.5 {\AA} cutoff. Both EPSR and MD simulations reveal a direction of the temperature dependence of the aluminate network structure which moves further away from the glass forming ideal (nAlO = 3) during supercooling. Furthermore, we provide new experimental data and models for amorphous alumina grown by sequential infiltration synthesis of a polymer template. The amorphous solid form likely has a larger Al-O coordination number than the liquid, consistent with expectations for the hypothetical glass.",

keywords = "Alumina, Amorphous, Glass forming ability, Structure, Supercooled liquid, X-ray diffraction",

author = "Caijuan Shi and Alderman, {Oliver L.G.} and Diana Berman and Jincheng Du and Joerg Neuefeind and Anthony Tamalonis and Weber, {J. K.Richard} and Jinglin You and Benmore, {Chris J.}",

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AU - Alderman, Oliver L.G.

AU - Berman, Diana

AU - Du, Jincheng

AU - Neuefeind, Joerg

AU - Tamalonis, Anthony

AU - Weber, J. K.Richard

AU - You, Jinglin

AU - Benmore, Chris J.

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AB - Liquid Al2O3 has been supercooled more than 500 K below its melting point (Tm = 2,327 K) using aerodynamic levitation and laser heating techniques. High energy synchrotron x-ray measurements were performed over a temperature range of 1,817 ≤ T (K) ≤ 2,700 and stroboscopic neutron diffraction at 1,984 and 2,587 K. The diffraction patterns have been fitted with Empirical Potential Structure Refinement (EPSR) models and compared to classical Molecular Dynamics (MD) simulation results. Both sets of models show similar trends, indicating the presence of high populations of AlO4 and AlO5 polyhedral units predominantly linked by triply shared oxygen atoms. EPSR reveals that the mean Al–O coordination number changes linearly with temperature with nAlO = 4.41 – [1.25 × 10−4] (T – Tm), with a 2.5 Å cutoff. Both EPSR and MD simulations reveal a direction of the temperature dependence of the aluminate network structure which moves further away from the glass forming ideal (nAlO = 3) during supercooling. Furthermore, we provide new experimental data and models for amorphous alumina grown by sequential infiltration synthesis of a polymer template. The amorphous solid form likely has a larger Al-O coordination number than the liquid, consistent with expectations for the hypothetical glass.

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The structure of amorphous and deeply supercooled liquid alumina

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