Liquid dynamics and glass formation of Gd55Co20Al25 metallic glass with minor Si addition

doi:10.1016/j.jmst.2020.11.024

Abstract

Abstract:

Liquid dynamics plays an essential role in glass formation. Here we observed a distinct change of liquid dynamics in Gd₅₅Co₂₀Al₂₅ metallic glass induced by microalloying Si element. In the equilibrium melt, minor Si (0.5 at.%) addition leads to a more fragile liquid behavior and a smaller strength of liquid-liquid transition with the transition strength (ΔF) decreasing from 0.76 to 0.35. However, in the supercooled liquid, Si-doped liquid exhibits a remarkable enhanced fragile-to-strong transition (FST), and the value of FST factor f increases sharply from 1.63 to 3.84, resulting in a stronger liquid behavior and more sluggish crystallization kinetics for Gd₅₅Co₂₀Al_24.5Si_0.5 metallic glass. Moreover, minor Si addition promotes the formation of a crystal-like structure with a size of 1-2 nm. The interactions between the crystal-like structures and other local favored clusters frustrate the further growth of crystal-like phases, thus stabilizes the amorphous structure. As a result, the glass-forming ability (GFA) was largely improved. The critical diameter of Gd₅₅Co₂₀Al₂₅ metallic glass increased from 2 to 7 mm with 0.5 at.% Si addition without deterioration of the magnetocaloric effect. This study provides valuable insight for understanding the distinct effect of microalloying on GFA of metallic glasses from the aspect of the evolution of the liquid.

Key words: Glass-forming ability, Liquid-liquid transition, Fragile-to-strong transition, Viscosity, Relaxation

Lin Xue, Liliang Shao, Qiang Luo, Lina Hu, Yunbo Zhao, Kuibo Yin, Mingyun Zhu, Litao Sun, Baolong Shen, Xiufang Bian. Liquid dynamics and glass formation of Gd₅₅Co₂₀Al₂₅ metallic glass with minor Si addition[J]. J. Mater. Sci. Technol., 2021, 77: 28-37.

Figures/Tables 10

Fig. 1. (a) XRD patterns of the as-cast Si0 rod with a diameter of 2 mm and Si0.5 rods with diameters from 3 to 7 mm. (b) DSC traces of the Si0 glassy rod with a diameter of 2 mm and the Si0.5 glassy rods with diameters of 2 and 7 mm, the inset picture shows the photo of the Si0.5 BMG with a diameter of 7 mm. The melting and solidification curves of Si0 and Si0.5 alloys at the rate of 10 K/min are exhibited in the inset, marked with melting temperature, Tm, liquid temperature, Tl and solidus temperature, Ts. (c) The HRTEM image and SAED pattern for the Si0.5 glassy rod with a diameter of 7 mm. (d) Magnetic entropy changes as a function of temperature for the Si0 and Si0.5 ribbon samples under maximum magnetic fields of 2 and 5 T, the inset shows the derivative of the temperature-dependent magnetization (dM/dT) curves measured under an applied field of 0.02 T.

Fig. 2. Crystallization fractions versus annealing times for the Si0 and Si0.5 BMG samples at temperatures of 620 and 623 K. The inset shows the Avrami plots.

Fig. 3. Changes of viscosities of superheated liquids as a function of temperature for the Si0 and Si0.5 melts. Red lines are Arrhenius fitting curves. ?, II, and III represent high-temperature liquid, transition region, and low-temperature liquid, respectively.

Fig. 4. SEM image and EDS spectrums at the vicinity of the interface between the Si0.5 alloy and crucible after the measurement of high-temperature viscosity. The inset shows the sectional view of the ingot after viscosity measurement.

Table 1. The data of fragilities of the high-temperature liquid (MH) and low-temperature liquid (ML) in superheated liquid, transition strength of LLT (ΔF), fragility factors of melting liquids (m') and supercooled liquids (m), transition magnitude (f=m'/m), FST temperature (Tfs), and optimized viscosity parameters using the extended MYEGA model for the Si0 and Si0.5 liquids.

MGs	M_H	M_L	ΔF	m'	m	f	T_fs(K)	logη_∞(Pa s)	C₁	C₂	W₁	W₂
Si0	2.34	9.88	0.76	64	39	1.63	960	-2.45	5077.29	653.75	0.0323	0.000322
Si0.5	0.81	0.60	0.35	123	32	3.84	893	-2.25	13945.91	720.93	1051.97	0.000386

Fig. 5. (a) Viscosity data and fitted curves for the Si0 and Si0.5 liquids. The data of strong SiO2, fragile OTP (orthoterphenyl) and the typical FST liquid water are also shown for comparison [17,45]. (b) Viscosity data and fitted curves versus Tg/T for the Si0 and Si0.5 liquids, the inset shows the Angell plot for the Si0.5 liquid.

Fig. 6. The heat flow versus temperature for the as-cast Si0 (a) and Si0.5 (b) BMG samples after annealing at various temperatures for 60 min. The insets show the Tonset versus annealing temperature Ta. (c) The excess enthalpies versus Ta for the Si0 and Si0.5 BMG samples.

Fig. 7. (a) Normalized loss modulus E" curves at 1 Hz for the Si0 and Si0.5 BMG samples, the inset shows the angles (∠?) exhibiting the extent of the curve line shifted from the peak of theβ-relaxation for both samples. Loss modulus E" curves for Si0 (b) and Si0.5 (c) BMGs obtained during isothermal DMA temperature scans with various measurement frequencies from 1 to 10 Hz. The insets of (b) and (c) show Arrhenius plots to obtain Eβ.

Fig. 8. HRTEM images and SAED patterns for the Si0 (a) and Si0.5 (b) BMG samples.

Fig. 9. The segmentation of the selected squares in Fig. 8(a) and (b) for auto-correlation analysis of the Si0 (a) and Si0.5 (b) BMG samples, respectively. The dimension of each segment or cell is 1.995 nm × 1.995 nm.

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Liquid dynamics and glass formation of Gd₅₅Co₂₀Al₂₅ metallic glass with minor Si addition

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