Probing the formation of ultrastable metallic glass from structural heterogeneity

doi:10.1016/j.jmst.2021.06.059

Abstract

Abstract:

Ultrastable metallic glasses (SMGs) exhibit enhanced stability comparable to those of conventional glasses aged for thousands of years. The ability to understand why certain alloy compositions and processing conditions generate an SMG is an emerging challenge. Herein, amplitude-modulation dynamic atomic force microscopy was utilized for tracking the structure of Zr₅₀Cu₅₀, Zr₅₀Cu_44.5Al_5.5 and Zr₅₀Cu_41.5Al_5.5Mo₃ thin film metallic glasses (TFMGs) that were produced by direct current magnetron sputtering at room temperature with the rate of deposition being the only variable. The transition in stability from bulk-to SMG-like behavior resides in the change of relaxation mechanism as the deposition rate is decreased. The formation of SMGs is directly linked with the degree of structural heterogeneity, whereby MGs with greater heterogeneity have a higher potential to form SMGs with more significant enhancement in stability. Slower deposition rates, however, are required to yield the more homogenous structure and lower energy state underlying the ultrastability. Ultrastability is closely linked with the geometric shape and distribution of loosely packed phases, whereby SMGs containing more slender loosely packed phases with a more skewed distribution achieve more significant improvements in stability. This work not only provides direct evidence of the structure of SMGs, but also opens new horizons for the design of SMGs.

Key words: Ultrastable metallic glass, Structural heterogeneity, Relaxation dynamics, Amplitude-modulation dynamic atomic force microscopy

Qijing Sun, David M Miskovic, Michael Ferry. Probing the formation of ultrastable metallic glass from structural heterogeneity[J]. J. Mater. Sci. Technol., 2022, 104: 214-223.

Figures/Tables 7

Fig. 1. DSC traces at a heating rate of 20 K/min. (a-c) DSC for TFMGs deposited at different rates. The glass transition temperature (Tg), which is defined from the onset of the transformation, is indicated by the intersection of the purple lines [24]. (d)-(f) Comparison of TFMGs with different compositions deposited at similar rates.

Fig. 2. The effect of deposition rate on MG stability and structural heterogeneity. (a) ΔTg as a function of deposition rate. The inset in (a) provides greater detail of the highlighted blue section with linear fits applied to the data for deposition rates ranging from ~20 nm/min to ~10 nm/min and the maximum values for ΔTg. The critical deposition rate for an SMG is defined as the tangential intersection of the linear fits and highlighted in the inset by pink arrows. (b) Correlation length ξ as a function of deposition rate.

Table 1 Characteristic parameters for TFMGs. $\text{ }\!\!\Delta\!\!\text{ }{{\xi }_{\text{SMG}}}={{\xi }_{\text{SMG}}}-{{\xi }_{\text{BMG}}}$.$\text{ }\!\!\Delta\!\!\text{ }{{T}_{\text{g},\text{SMG}}}={{T}_{\text{g},\text{SMG}}}-{{T}_{\text{g},\text{BMG}}}$. ${{\xi }_{\text{SMG}}}$ and ${{T}_{\text{g},\text{SMG}}}$ are the average values for TFMGs deposited at rates lower than the critical deposition rates. ${{\xi }_{\text{BMG}}}$ and ${{T}_{\text{g},\text{BMG}}}$ are the correlation length and glass transition temperature for BMGs.

Composition	ZrCu	ZrCuAl	ZrCuAlMo
ξ_BMG (nm)	10.4±0.67	7.28±0.54	9.85±1.0
ξ_SMG (nm)	3.78±0.22	3.61±0.30	3.75±0.40
Δξ_SMG/ξ_BMG	-63.7%±2.7%	-50.4%±4.8%	-61.9%±4.9%
T_g,BMG (K)	670±2	699±1	703±2
T_g,SMG (K)	755±1	768±1	777±1
ΔT_g,SMG/T_g,BMG	12.7%±0.4%	9.87%±0.3%	10.5%±0.4%
Critical deposition rate (nm/min)	8.7±0.3	14.3±0.5	12.8±0.4
Slow β relaxation	Hump [41]	Excess wing [40]	Hump [40]

Fig. 3. Statistical and geometrical analyses of AM-AFM images. (a) and (b) Typical AM-AFM height and phase shift images for ZrCuAlMo TFMG deposited at ~242 nm/min; (c) Roughness as a function of deposition rate; (d) and (e) Edis maps calculated from (b). The HDRs are shown in green in (d), whereas the LDRs are shown in blue in (e); (f) Distribution spectrum for Edis map shown in (d) and (e); (g) and (h) The influence of deposition rate on Dmax/Dmin and Req.

Fig. 4. The frequency distributions of Req. (a, b) Effect of deposition rate on the distribution of Req for ZrCuAlMo TFMGs; (c)-(e) Comparison of Req distribution for TFMGs of different compositions deposited at similar rates. The curves were fitted to a lognormal distribution function (Adj. R2 > 0.90).

Fig. 5. LDR behavior in TFMGs. (a)-(c) Influence of deposition rate on the accumulated size distributions of LDRs for ZrCu, ZrCuAl and ZrCuAlMo; (d)-(f) Edis maps for ZrCuAlMo TFMGs deposited at ~242 nm/min, ~21.1 nm/min and ~6.90 nm/min, respectively. The images are rendered with the same color bar. LDRs are shown in blue; (g)-(i) Comparisons of LDRs for TFMGs of different compositions deposited at similar rates.

Table 2 Simultaneous efficiently geometrically packed clusters for the different compositions.

Composition	ZrCu			ZrCuAl \| ZrCuAlMo
Cluster centre	Cu	Cu	Zr	Cu	Cu	Al/Mo	Zr
Coordination number	10	11	16	11	12	13	15
Packing efficiency (%)	98.6-100	101.6	99.5-101	100	102	99.4	100.6-100.9

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