Liquid-liquid phase transition and chemical phase separation in Cu-Zr-Al-Y bulk glass-forming supercooled liquid

H. R. Jiang; M. Frey; N. Neuber; Q. Wang; W. F. Lu; L. M. Ruschel; G. Y. Sun; I. Gallino; B. Zhang; G. Wang; R. Busch; J. Shen; Y. Yang

doi:10.1016/j.actamat.2025.121090

Liquid-liquid phase transition and chemical phase separation in Cu-Zr-Al-Y bulk glass-forming supercooled liquid

H. R. Jiang, M. Frey, N. Neuber, Q. Wang, W. F. Lu, L. M. Ruschel, G. Y. Sun, I. Gallino, B. Zhang, G. Wang^*, R. Busch, J. Shen, Y. Yang

^*Corresponding author for this work

Department of Mechanical Engineering

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

Abstract

Anomalous exothermic peaks before crystallization in metallic supercooled liquids are commonly attributed to chemical phase separation (CPS) or structural changes due to polyamorphic liquid-liquid phase transition (LLPT). In this work, we present experimental evidence of the simultaneous occurrence of LLPT and CPS during the anomalous exothermic reaction in a supercooled Cu-Zr-Al-Y liquid. The CPS results from the positive enthalpy of mixing between Y and Zr, while LLPT, characterized by medium-range structural ordering, originates from the two-phase field (fragile and strong phases) centered around Cu₅₀Zr₅₀ in the Cu-Zr system. These two aspects interact with each other and are considered to be a key factor in stabilizing the supercooled liquid against crystallization. To describe the structural and chemical evolutions in the supercooled liquid, we propose schematic Gibbs free energy surfaces for the (Cu, Al)-(Zr, Al)-Y pseudo-ternary system that incorporate both the two-phase field of LLPT and the local maximum of the CPS in the Y direction. The results of this work not only enrich our understanding of anomalous thermophysical signals in the supercooled liquid but also offer insights into the development of bulk metallic glasses with superior glass-forming ability and thermal stability. © 2025 Acta Materialia Inc.

Original language	English
Article number	121090
Journal	Acta Materialia
Volume	293
Online published	2 May 2025
DOIs	https://doi.org/10.1016/j.actamat.2025.121090
Publication status	Published - 1 Jul 2025

Funding

This work is supported by the National Natural Science Foundation of China (Grant Nos. 52301209, U23A2065 and 51925103), the open research fund of Songshan Lake Materials Laboratory (Grant No 2023SLABFN13), Shanghai Rising-Star Program Yangfan Project (Grant No 23YF1411900), the Space Utilization System of China Manned Space Engineering (Grant No KJZ-YY-NCL08), the Innovation Program of Shanghai Science and Technology (No. 23520760700), and the Aviation Foundation (No. 2023Z0530S6004). The authors acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at PETRA III and we would like to thank Dr. M. Blankenburg and Dr. U. Lienert for their assistance in using beamline P21.2. We would like to thank S.S. Riegler and B. Adam for their assistance in conducting the HESXRD experiments.

Research Keywords

Bulk metallic glasses
Glass-forming ability
Liquid-liquid phase transition
Phase separation
Supercooled liquid

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title = "Liquid-liquid phase transition and chemical phase separation in Cu-Zr-Al-Y bulk glass-forming supercooled liquid",

abstract = "Anomalous exothermic peaks before crystallization in metallic supercooled liquids are commonly attributed to chemical phase separation (CPS) or structural changes due to polyamorphic liquid-liquid phase transition (LLPT). In this work, we present experimental evidence of the simultaneous occurrence of LLPT and CPS during the anomalous exothermic reaction in a supercooled Cu-Zr-Al-Y liquid. The CPS results from the positive enthalpy of mixing between Y and Zr, while LLPT, characterized by medium-range structural ordering, originates from the two-phase field (fragile and strong phases) centered around Cu50Zr50 in the Cu-Zr system. These two aspects interact with each other and are considered to be a key factor in stabilizing the supercooled liquid against crystallization. To describe the structural and chemical evolutions in the supercooled liquid, we propose schematic Gibbs free energy surfaces for the (Cu, Al)-(Zr, Al)-Y pseudo-ternary system that incorporate both the two-phase field of LLPT and the local maximum of the CPS in the Y direction. The results of this work not only enrich our understanding of anomalous thermophysical signals in the supercooled liquid but also offer insights into the development of bulk metallic glasses with superior glass-forming ability and thermal stability. {\textcopyright} 2025 Acta Materialia Inc.",

keywords = "Bulk metallic glasses, Glass-forming ability, Liquid-liquid phase transition, Phase separation, Supercooled liquid",

author = "Jiang, {H. R.} and M. Frey and N. Neuber and Q. Wang and Lu, {W. F.} and Ruschel, {L. M.} and Sun, {G. Y.} and I. Gallino and B. Zhang and G. Wang and R. Busch and J. Shen and Y. Yang",

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doi = "10.1016/j.actamat.2025.121090",

language = "English",

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TY - JOUR

T1 - Liquid-liquid phase transition and chemical phase separation in Cu-Zr-Al-Y bulk glass-forming supercooled liquid

AU - Jiang, H. R.

AU - Frey, M.

AU - Neuber, N.

AU - Wang, Q.

AU - Lu, W. F.

AU - Ruschel, L. M.

AU - Sun, G. Y.

AU - Gallino, I.

AU - Zhang, B.

AU - Wang, G.

AU - Busch, R.

AU - Shen, J.

AU - Yang, Y.

PY - 2025/7/1

Y1 - 2025/7/1

N2 - Anomalous exothermic peaks before crystallization in metallic supercooled liquids are commonly attributed to chemical phase separation (CPS) or structural changes due to polyamorphic liquid-liquid phase transition (LLPT). In this work, we present experimental evidence of the simultaneous occurrence of LLPT and CPS during the anomalous exothermic reaction in a supercooled Cu-Zr-Al-Y liquid. The CPS results from the positive enthalpy of mixing between Y and Zr, while LLPT, characterized by medium-range structural ordering, originates from the two-phase field (fragile and strong phases) centered around Cu50Zr50 in the Cu-Zr system. These two aspects interact with each other and are considered to be a key factor in stabilizing the supercooled liquid against crystallization. To describe the structural and chemical evolutions in the supercooled liquid, we propose schematic Gibbs free energy surfaces for the (Cu, Al)-(Zr, Al)-Y pseudo-ternary system that incorporate both the two-phase field of LLPT and the local maximum of the CPS in the Y direction. The results of this work not only enrich our understanding of anomalous thermophysical signals in the supercooled liquid but also offer insights into the development of bulk metallic glasses with superior glass-forming ability and thermal stability. © 2025 Acta Materialia Inc.

AB - Anomalous exothermic peaks before crystallization in metallic supercooled liquids are commonly attributed to chemical phase separation (CPS) or structural changes due to polyamorphic liquid-liquid phase transition (LLPT). In this work, we present experimental evidence of the simultaneous occurrence of LLPT and CPS during the anomalous exothermic reaction in a supercooled Cu-Zr-Al-Y liquid. The CPS results from the positive enthalpy of mixing between Y and Zr, while LLPT, characterized by medium-range structural ordering, originates from the two-phase field (fragile and strong phases) centered around Cu50Zr50 in the Cu-Zr system. These two aspects interact with each other and are considered to be a key factor in stabilizing the supercooled liquid against crystallization. To describe the structural and chemical evolutions in the supercooled liquid, we propose schematic Gibbs free energy surfaces for the (Cu, Al)-(Zr, Al)-Y pseudo-ternary system that incorporate both the two-phase field of LLPT and the local maximum of the CPS in the Y direction. The results of this work not only enrich our understanding of anomalous thermophysical signals in the supercooled liquid but also offer insights into the development of bulk metallic glasses with superior glass-forming ability and thermal stability. © 2025 Acta Materialia Inc.

KW - Bulk metallic glasses

KW - Glass-forming ability

KW - Liquid-liquid phase transition

KW - Phase separation

KW - Supercooled liquid

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DO - 10.1016/j.actamat.2025.121090

M3 - RGC 21 - Publication in refereed journal

SN - 1359-6454

VL - 293

JO - Acta Materialia

JF - Acta Materialia

M1 - 121090

ER -

Liquid-liquid phase transition and chemical phase separation in Cu-Zr-Al-Y bulk glass-forming supercooled liquid

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