Vibrational dynamics in the undercooled liquid of ultra-fragile metallic glasses

Hillary L. Smith; Claire N. Saunders; Camille Bernal-Choban; Stefan H. Lohaus; Colby J. Stoddard; Lucy K. Decker; J. Y.Y. Lin; Jennifer L. Niedziela; D. L. Abernathy; Jong Hyun Na; Marios D. Demetriou; B. Fultz

doi:10.1016/j.mtla.2023.101710

Vibrational dynamics in the undercooled liquid of ultra-fragile metallic glasses

Hillary L. Smith, Claire N. Saunders, Camille Bernal-Choban, Stefan H. Lohaus, Colby J. Stoddard, Lucy K. Decker, J. Y.Y. Lin, Jennifer L. Niedziela, D. L. Abernathy, Jong Hyun Na, Marios D. Demetriou, B. Fultz

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

Abstract

The lattice vibrational dynamics in ultra-fragile Pt₅₇Cu₂₃P₂₀ and Pt₆₀Cu₂₀P₂₀ glasses were investigated using in situ inelastic neutron scattering to measure the evolution of the phonon density of states (DOS) through the glass transition, into the undercooled liquid phase, and through crystallization. The phonon DOS curves are remarkably similar for the undercooled liquids and the amorphous solids. The vibrational entropy was obtained with these phonon DOS curves, and changes in vibrational entropy caused by the glass transition are less than 0.05 k_B/atom. For these highly fragile metal/metalloid glasses, the excess vibrational entropy of the undercooled liquid is about 0.5–1.5 J mol⁻¹ K⁻¹, compared to 0.1 J mol⁻¹ K⁻¹ reported earlier for stronger Cu–Zr glasses. Our work suggests that, consistent with our previous report for less fragile metallic glasses, the fraction of the total excess entropy that is vibrational is small, and the discontinuity in excess entropy at the glass transition is mainly due to configurational entropy.

Original language	English
Article number	101710
Journal	Materialia
Volume	27
DOIs	https://doi.org/10.1016/j.mtla.2023.101710
State	Published - Mar 2023

Funding

Neutron scattering data collection was supported the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award No. DE-FG02-03ER46055. The use of Oak Ridge National Laboratory's Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. DOE. Support for calorimetry experiments and neutron scattering data analysis were provided by the American Chemical Society Petroleum Research Fund No. 62045-UNI10. Neutron scattering data collection was supported the U.S. Department of Energy, Office of Science, Basic Energy Sciences , under Award No. DE-FG02-03ER46055 . The use of Oak Ridge National Laboratory’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division , Office of Basic Energy Sciences, U.S. DOE. Support for calorimetry experiments and neutron scattering data analysis were provided by the American Chemical Society Petroleum Research Fund No. 62045-UNI10 .

Funders	Funder number
Scientific User Facilities Division
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-FG02-03ER46055
Oak Ridge National Laboratory
American Chemical Society Petroleum Research Fund	62045-UNI10

Keywords

Glass
Glass transition
Liquids
Metallic glasses
Neutron scattering

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10.1016/j.mtla.2023.101710

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title = "Vibrational dynamics in the undercooled liquid of ultra-fragile metallic glasses",

abstract = "The lattice vibrational dynamics in ultra-fragile Pt57Cu23P20 and Pt60Cu20P20 glasses were investigated using in situ inelastic neutron scattering to measure the evolution of the phonon density of states (DOS) through the glass transition, into the undercooled liquid phase, and through crystallization. The phonon DOS curves are remarkably similar for the undercooled liquids and the amorphous solids. The vibrational entropy was obtained with these phonon DOS curves, and changes in vibrational entropy caused by the glass transition are less than 0.05 kB/atom. For these highly fragile metal/metalloid glasses, the excess vibrational entropy of the undercooled liquid is about 0.5–1.5 J mol−1 K−1, compared to 0.1 J mol−1 K−1 reported earlier for stronger Cu–Zr glasses. Our work suggests that, consistent with our previous report for less fragile metallic glasses, the fraction of the total excess entropy that is vibrational is small, and the discontinuity in excess entropy at the glass transition is mainly due to configurational entropy.",

keywords = "Glass, Glass transition, Liquids, Metallic glasses, Neutron scattering",

author = "Smith, {Hillary L.} and Saunders, {Claire N.} and Camille Bernal-Choban and Lohaus, {Stefan H.} and Stoddard, {Colby J.} and Decker, {Lucy K.} and Lin, {J. Y.Y.} and Niedziela, {Jennifer L.} and Abernathy, {D. L.} and Na, {Jong Hyun} and Demetriou, {Marios D.} and B. Fultz",

note = "Publisher Copyright: {\textcopyright} 2023 Acta Materialia Inc.",

year = "2023",

month = mar,

doi = "10.1016/j.mtla.2023.101710",

language = "English",

volume = "27",

journal = "Materialia",

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AU - Smith, Hillary L.

AU - Saunders, Claire N.

AU - Bernal-Choban, Camille

AU - Lohaus, Stefan H.

AU - Stoddard, Colby J.

AU - Decker, Lucy K.

AU - Lin, J. Y.Y.

AU - Niedziela, Jennifer L.

AU - Abernathy, D. L.

AU - Na, Jong Hyun

AU - Demetriou, Marios D.

AU - Fultz, B.

PY - 2023/3

Y1 - 2023/3

N2 - The lattice vibrational dynamics in ultra-fragile Pt57Cu23P20 and Pt60Cu20P20 glasses were investigated using in situ inelastic neutron scattering to measure the evolution of the phonon density of states (DOS) through the glass transition, into the undercooled liquid phase, and through crystallization. The phonon DOS curves are remarkably similar for the undercooled liquids and the amorphous solids. The vibrational entropy was obtained with these phonon DOS curves, and changes in vibrational entropy caused by the glass transition are less than 0.05 kB/atom. For these highly fragile metal/metalloid glasses, the excess vibrational entropy of the undercooled liquid is about 0.5–1.5 J mol−1 K−1, compared to 0.1 J mol−1 K−1 reported earlier for stronger Cu–Zr glasses. Our work suggests that, consistent with our previous report for less fragile metallic glasses, the fraction of the total excess entropy that is vibrational is small, and the discontinuity in excess entropy at the glass transition is mainly due to configurational entropy.

AB - The lattice vibrational dynamics in ultra-fragile Pt57Cu23P20 and Pt60Cu20P20 glasses were investigated using in situ inelastic neutron scattering to measure the evolution of the phonon density of states (DOS) through the glass transition, into the undercooled liquid phase, and through crystallization. The phonon DOS curves are remarkably similar for the undercooled liquids and the amorphous solids. The vibrational entropy was obtained with these phonon DOS curves, and changes in vibrational entropy caused by the glass transition are less than 0.05 kB/atom. For these highly fragile metal/metalloid glasses, the excess vibrational entropy of the undercooled liquid is about 0.5–1.5 J mol−1 K−1, compared to 0.1 J mol−1 K−1 reported earlier for stronger Cu–Zr glasses. Our work suggests that, consistent with our previous report for less fragile metallic glasses, the fraction of the total excess entropy that is vibrational is small, and the discontinuity in excess entropy at the glass transition is mainly due to configurational entropy.

KW - Glass

KW - Glass transition

KW - Liquids

KW - Metallic glasses

KW - Neutron scattering

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Vibrational dynamics in the undercooled liquid of ultra-fragile metallic glasses

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