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Separating the configurational and vibrational entropy contributions in metallic glasses

Smith, Hillary L. and Li, Chen W. and Hoff, Andrew and Garrett, Glenn R. and Kim, Dennis S. and Yang, Fred C. and Lucas, Matthew S. and Swan-Wood, Tabitha and Lin, J. Y. Y. and Stone, M. B. and Abernathy, D. L. and Demetriou, Marios D. and Fultz, B. (2017) Separating the configurational and vibrational entropy contributions in metallic glasses. Nature Physics, 13 (9). pp. 900-905. ISSN 1745-2473. https://resolver.caltech.edu/CaltechAUTHORS:20170411-135835964

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Abstract

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? Here 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.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://dx.doi.org/10.1038/nphys4142DOIArticle
http://rdcu.be/s61uPublisherFree ReadCube access
ORCID:
AuthorORCID
Li, Chen W.0000-0002-0758-5334
Kim, Dennis S.0000-0002-5707-2609
Yang, Fred C. 0000-0002-5615-5170
Lin, J. Y. Y.0000-0001-9233-0100
Stone, M. B.0000-0001-7884-9715
Abernathy, D. L.0000-0002-3533-003X
Fultz, B.0000-0002-6364-8782
Additional Information:© 2017 Macmillan Publishers Limited. Received 30 October 2016. Accepted 18 April 2017. Published online 29 May 2017. The authors would like to acknowledge S. Randolph for her help with data collection. A portion of this research at Oak Ridge National Laboratory’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. This work benefited from DANSE software developed under NSF Grant No. DMR-0520547. This work was supported by DOE BES under contract DE-FG02-03ER46055. Author Contributions: Samples were prepared by H.L.S., A.H., G.R.G., D.S.K. and M.D.D. Neutron data collection was performed by H.L.S., D.L.A., M.B.S., C.W.L., A.H., G.R.G., F.C.Y., M.S.L., T.S.-W. and B.F. Heat capacity measurements were carried out by H.L.S., A.H., G.R.G. and M.D.D. Data analysis was performed by H.L.S., C.W.L., D.S.K., J.Y.Y.L., M.D.D. and B.F. The manuscript was written by H.L.S., C.W.L. M.D.D. and B.F. All authors discussed the results and provided input on the paper. Data availability. The data that support the plots within this paper and other findings of this study are available from the corresponding author on reasonable request. The authors declare no competing financial interests.
Funders:
Funding AgencyGrant Number
NSFDMR-0520547
Department of Energy (DOE)DE-FG02-03ER46055
Issue or Number:9
Record Number:CaltechAUTHORS:20170411-135835964
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170411-135835964
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:76518
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:30 May 2017 18:18
Last Modified:16 Mar 2020 18:44

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