Separating the configurational and vibrational entropy contributions in metallic glasses

Smith, Hillary L.; Li, Chen W.; Hoff, Andrew; Garrett, Glenn R.; Kim, Dennis S.; Yang, Fred C.; Lucas, Matthew S.; Swan-Wood, Tabitha; Lin, Jiao Y.  Y.; Stone, Matthew B.; Abernathy, Douglas L.; Demetriou, Marios D.; Fultz, B.

doi:10.1038/nphys4142

Title: Separating the configurational and vibrational entropy contributions in metallic glasses

Journal Article · Mon May 29 00:00:00 EDT 2017 · Nature Physics

DOI:https://doi.org/10.1038/nphys4142· OSTI ID:1471839

Smith, Hillary L. ^[1]; Li, Chen W. ^[2]; Hoff, Andrew ^[1]; Garrett, Glenn R. ^[1];

^[1];

^[3]; Swan-Wood, Tabitha ^[4];

^[5]; Stone, Matthew B. ^[6];

^[6]; Demetriou, Marios D. ^[1]; Fultz, B. ^[1]

California Inst. of Technology (CalTech), Pasadena, CA (United States. Dept. of Applied Physics and Materials Science
Univ. of California, Riverside, CA (United States). Dept. of Mechanical Engineering
Air Force Research Lab. (AFRL), Wright-Patterson AFB, OH (United States)
California State Univ. Channel Islands (CI), Camarillo, CA (United States). Dept. of Applied Physics
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Data Analysis and Visualization Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division

Glassy materials exist in nature and play a critical role in technology, but key differences between the glass, liquid and crystalline phases are not well understood. Over several decades there has been controversy about the specific heat absorbed as a glass transforms to a liquid—does this originate from vibrational entropy or configurational entropy? We report direct in situ measurements of the vibrational spectra of strong and fragile metallic glasses in the glass, liquid and crystalline phases. For both types of material, the measured vibrational entropies of the glass and liquid show a tiny excess over the crystal, representing less than 5% of the total excess entropy measured with step calorimetry. These results reveal that the excess entropy of metallic glasses is almost entirely configurational in origin, consistent with the early theories of Gibbs and co-workers describing the glass transition as a purely configurational transition.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725; FG02-03ER46055; DMR-0520547

OSTI ID:: 1471839

Journal Information:: Nature Physics, Vol. 13, Issue 9; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 41 works

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Polytetrahedral structure and glass-forming ability of simulated Ni–Zr alloys Klumov, B. A.; Ryltsev, R. E.; Chtchelkatchev, N. M. The Journal of Chemical Physics, Vol. 149, Issue 13 https://doi.org/10.1063/1.5041325	journal	October 2018
Configurational entropy of glass-forming liquids Berthier, Ludovic; Ozawa, Misaki; Scalliet, Camille The Journal of Chemical Physics, Vol. 150, Issue 16 https://doi.org/10.1063/1.5091961	journal	April 2019
Does the Adam-Gibbs relation hold in simulated supercooled liquids? Ozawa, Misaki; Scalliet, Camille; Ninarello, Andrea The Journal of Chemical Physics, Vol. 151, Issue 8 https://doi.org/10.1063/1.5113477	journal	August 2019
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Does the Adam-Gibbs relation hold in simulated supercooled liquids? Ozawa, Misaki; Scalliet, Camille; Ninarello, Andrea arXiv https://doi.org/10.48550/arxiv.1905.08179	text	January 2019
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