Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids

Jaiswal, Abhishek; Egami, Takeshi; Kelton, K. F.; Schweizer, Kenneth S.; Zhang, Yang

doi:10.1103/PhysRevLett.117.205701

Title: Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids

Journal Article · Thu Nov 10 00:00:00 EST 2016 · Physical Review Letters

DOI:https://doi.org/10.1103/PhysRevLett.117.205701· OSTI ID:1337816

Jaiswal, Abhishek ^[1]; Egami, Takeshi ^[2]; Kelton, K. F. ^[3]; Schweizer, Kenneth S. ^[4]; Zhang, Yang ^[5]

Univ. of Illinois, Urbana, IL (United States). Dept. of Nuclear, Plasma, and Radiological Engineering
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Washington Univ., St. Louis, MO (United States). Dept. of Physics. Inst. of Materials Science and Engineering
Univ. of Illinois, Urbana, IL (United States). Dept. of Materials Science and Engineering
Univ. of Illinois, Urbana, IL (United States). Dept. of Nuclear, Plasma, and Radiological Engineering. Dept. of Materials Science and Engineering

In this paper, we report the observation of a distinct correlation between the kinetic fragility index m and the reduced Arrhenius crossover temperature θ_A = T_A/T_g in various glass-forming liquids, identifying three distinguishable groups. In particular, for 11 glass-forming metallic liquids, we universally observe a crossover in the mean diffusion coefficient from high-temperature Arrhenius to low-temperature super-Arrhenius behavior at approximately θ_A ≈ 2 which is in the stable liquid phases. In contrast, for fragile molecular liquids, this crossover occurs at much lower θ_A ≈ 1.4 and usually in their supercooled states. The θ_A values for strong network liquids spans a wide range higher than 2. Intriguingly, the high-temperature activation barrier E_∞ is universally found to be ~11k_BT_g and uncorrelated with the fragility or the reduced crossover temperature θ_A for metallic and molecular liquids. Finally, these observations provide a way to estimate the low-temperature glassy characteristics (T_g and m) from the high-temperature liquid quantities (E_∞ and θ_A).

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Contributing Organization:: Univ. of Tennessee, Knoxville, TN (United States); Washington Univ., St. Louis, MO (United States)

Grant/Contract Number:: SC0014804; SC-0014804

OSTI ID:: 1337816

Alternate ID(s):: OSTI ID: 1331724

Journal Information:: Physical Review Letters, Vol. 117, Issue 20; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 61 works

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