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Procedia Engineering 36 (2012) 226 – 234

IUMRS-ICA 2011

Alloy Design for High-Entropy Bulk Glassy Alloys

A. Takeuchia,*, N. Chena, T. Wadab, W. Zhangb,
Y. Yokoyamab, A. Inoue a and J.-W. Yehc
a
World Premier International Research Center (WPI), Tohoku University, Sendai 980-8577, Japan
b
Institute for Materials Research, Tohoku University, Sendai 980-8577, Japan
c
Department of Materials Science and Engineering, National Tsing Hua University, Hsinchu 300, Taiwan, ROC.

Abstract

An efficient alloy design for bulk metallic glasses (BMGs) assisted by a composition–configurational entropy (C-CE)
diagram has been proposed by introducing a feature of high-entropy (HE) alloys that are defined by an equi-atomic
alloy with five or more elements. The proposed alloy design compensated for a shortcoming in determining the
compositions of BMGs and led to success in forming a Pd20Pt20Cu20Ni20P20 HE-BMG with a maximum diameter of
10 mm. The C-CE diagram demonstrates the equi-atomicity of alloys, providing candidates for HE-BMGs. The alloy
design for HE-BMG will promise opening up the new cutting-edge in both HE alloys and BMGs.

© 2011 Published by Elsevier Ltd. Selection and/or peer-review under responsibility of MRS-Taiwan
Open access under CC BY-NC-ND license.
Keywords: Bulk metallic glass; high-entropy alloy; alloy design

1. Introduction

Recently, bulk metallic glasses (BMGs) [1,2] and high-entropy (HE) alloys [3,4] have been
accumulating unprecedented academic and engineering interest in a field of advanced metallic materials.
The recent increasing interest for BMGs and HE alloys is due to their unique structures and resultant
superior properties than those of conventional crystalline alloys. Here, BMGs are defined as a subset of
metallic glasses formed with a critical diameter (dc) of a couple of millimeters or more. The superior
properties of BMGs as well as metallic glasses against conventional crystalline alloys are principally due
to features of metallic glasses, such as the glass transition in temperature and resultant supercooled liquid

*A. Takeuchi. Tel.: +81-22-217-5956; Fax: +81-22-217-5956.

E-mail address: takeuchi@wpi-aimr.tohoku.ac.jp

1877-7058 © 2012 Published by Elsevier Ltd. Open access under CC BY-NC-ND license.
doi:10.1016/j.proeng.2012.03.035
 A. Takeuchi et al. / Procedia Engineering 36 (2012) 226 – 234 227

range, and a non-crystalline amorphous/glassy structure. On the other hand, HE alloys are defined as
multicomponent alloys comprising five or more elements with perfect as well as partially-imperfect equi-
atomic composition where the former and the latter were categorized as HE alloys of narrow and wide
senses, respectively, by Takeuchi et al [4]. The HE alloys also exhibits superior properties than
conventional crystalline alloy owing to their unique structures, which prevent the complicated
intermetallic compounds from forming. Specifically, HE alloys are principally composed of a simple
crystalline structure of fcc or bcc or their mixture as well as a rarely formed amorphous structure in a
shape of thin film [3, 4] for systems with metalloid elements. An example of the superior properties of HE
alloys includes increase in mechanical properties than the conventional crystalline alloys [3, 4]. Thus, the
BMGs with amorphous structure and HE alloys comprising principally crystalline structures are thought
to be different advance metallic materials. However, recent reports on Pd20Pt20Cu20Ni20P20 [5] and
Zn20Ca20Sr20Yb20(Li0.55Mg0.45)20 [6] alloys revealed that new BMGs with a characteristic of HE alloys
have begun to be found as HE-BMGs in multicomponent systems.
Very recently, the authors have reported [5] that a Pd20Pt20Cu20Ni20P20 HE alloy can be produced as a
BMG with a critical diameter of 10 mm by referring to a ternary prototype of Pd40Ni40P20 BMG [7]. This
HE-BMG is the first success in merging HE alloys of narrow sense and BMGs. In addition, this alloy is
the first success in HE-BMGs in Metal-Metalloid type, which includes metalloid elements from B, C, Si,
P and Ge. The success in fabricating HE-BMG is considerably important when considering the mutual
progress in the development of both BMGs and HE alloys. However, there remain a plenty of unknown
features of HE-BMGs, since the history of HE-BMGs has just started. For instance, unknown features of
HE-BMGs include that the Pd20Pt20Cu20Ni20P20 HE-BMG has not yet optimized for the components as
HE-BMGs of narrow sense and that HE-BMGs of narrow sense in Metal–Metal type comprising metallic
elements solely have yet been discovered to date. To make matters worth, one cannot avoid searching for
new BMGs in multicomponent systems with elements more than four because of the saturating number of
BMGs found to date up to quaternary alloys. Hence, it is important to consider efficient alloy design for
BMGs to shorten consuming time and to reduce manual labor for the development of new BMGs.
The present study aims to develop Metal–Metalloid type of HE-BMG of narrow sense, to analyze the
compositional features of these HE-BMGs and to assess the efficiency of the alloy design for HE-BMG.

2. Methods

2.1. Sample preparation and analysis

We studied Pd20Pt20(TM1)20(TM2)20P20 alloys in nominal atomic percentages where TM1 and TM2 are
transition metals from Fe, Co, Ni and Cu. Specifically, we studied (TM1,TM2) = (Co,Cu), (Co,Fe),
(Fe,Cu) and (Cu,Ni), but we did not deal with (TM1,TM2) = (Fe,Ni), (Co,Ni). The latter results will be
reported somewhere else in near future. The specimens with diameters of 3 and 5 mm were prepared by
conventional copper mold casting method after master alloys from pure substances had been prepared in
advance by arc melting in an argon atmosphere. When a BMG is formed with copper mold casting, then,
water quenching with B2O3 flux treatment was tried to form a BMG with greater dimensions in a capsuled
quartz tube. Structural analysis of the samples was conducted using X-ray diffraction (XRD).

2.2. A Composition–Configurational Entropy (C-CE) Diagram

An especial composition diagram was created to analyze the relationships between the compositions
(C) and configurational entropy (Sconfig.:CE) for HE-BMGs, HE alloys, BMGs and conventional alloys.
Examples of the C-CE diagrams for ternary and quaternary alloys are shown in Figs. 1 and 2, respectively.
228 A. Takeuchi et al. / Procedia Engineering 36 (2012) 226 – 234

The composition diagram has plots in three-dimensional space (x,y,z), where the base (x,y,0) corresponds
to a composition diagram comprising a regular polyhedron depending on the number of constituent
elements (N). On the other hand, the vertical axis (z) expresses Sconfig./Sconfig.(ideal) value where the
Sconfig./Sconfig,(ideal) = ln N [3, 5]. In the C-CE diagram, the coordinates of vertices on the base to form a
polyhedron, which corresponds to those of pure constituent elements, are expressed by Eqs. (1) and (2).
xi = cos (2Si/N) (i = 0, 1, 2, …, N-1) (1)
yi = sin (2Si/N) (i = 0, 1, 2, …, N-1) (2)
Thus, the coordinates of the plot of an alloy (x,y) were calculated by summing up the components
expressed by Eqs. (1) and (2) separately after multiplying the fraction of the i-th element (ci). Specifically,
x and y are expressed by Eqs. (3) and (4),
x = 6 ci xi (3)
y = 6 ci yi (4)
On the other hand, the value of z can be calculated by Eq. (5),
z = Sconfig. (x,y)/ Sconfig.(ideal) (0,0)= (–6 ci ln ci )/ ln N (5)

Fig. 1 Composition–configurational entropy (C-CE) diagram for an A-B-C ternary system: (a) A conventional triangle (Gibbs)
composition diagram with contour lines for z values given by Eq. (5). There vertices (A, B, C) have a distance of unity from the
origin (O). The area surrounded by the triangle A-O-AB is the intrinsic composition in an AaBbCc alloy that satisfies a t b t c; (b)
Three-dimensional C-CE diagram where the distance DO is unity, forming a hemisphere with a radius of unity.

Fig. 2 Composition–configurational entropy (C-CE) diagram for a D-E-F-G quaternary system where the C-CE diagram is drawn to
inscribe a sphere with a radius of unity. The hatches in gray demonstrate the data for an A-B-C ternary system shown in Fig. 1 for
comparison. (a) A square composition diagram in which the intrinsic compositions of the DaEbFcGd alloy that satisfies a t b t c t d
are drawn in a quadrangle O-D-DE-H. (b) Three-dimensional C-CE diagram. Alloys with a composition in an area O-D-O-H have
smaller z-value than that for an A-B-C ternary system.
 A. Takeuchi et al. / Procedia Engineering 36 (2012) 226 – 234 229

In the C-CE diagram, all the HE alloy with perfect equi-atomicity are plotted at (x,y,z) = (0,0,1),
whereas the pure elements are plotted on the base at a vertex at a radius of unity from the origin. We
determined to arrange the constituent elements on the base as follows. The constituent element with the
greatest fraction in composition was set up at the vertex of (1,0,0). Then, the vertices located at the next in
anticlockwise direction were occupied in the order of decreasing fraction of the composition. This
arrangement of the constituent elements made the plots of alloys on the base at the first quadrant
principally. The distance between the plots traced on x-y plane and the origin exhibit the degree of equi-
atomicity of an alloy. Thus, the distance from the origin and the z-value identify the feature of alloys in
C-CE diagram.

3. Results and Discussion

3.1. HE-BMG

Figure 3 shows an outer surface and cross-sectional images and XRD diffraction pattern from the
cross-sectional area of the Pd20Pt20Ni20Cu20P20 alloy prepared by water-quenching with B2O3 flux
treatment [5]. As shown in Fig. 3(a), the cylindrical samples exhibit good metallic luster, indicating the
sample surfaces are neither oxidized and nor contaminated due to the effect of B2O3 on excluding
impurities other than the constituent elements. Furthermore, observations of the sample surfaces with
unaided eyes can explain the absence of a concave shape on the millimeters to sub-millimeter scales. The
XRD pattern in Fig. 3(b) taken from the cross-sectional area in Fig. 3(a) demonstrates the formation of a
glassy single phase in Pd20Pt20Cu20Ni20P20 alloy with a diameter of 10 mm [5].

Fig. 3 (a) Outer surface and cross-sectional images and (b) XRD pattern from a cross-sectional area of a Pd20Pt20Cu20Ni20P20 cylinder
with 10 mm in diameter prepared by water quenching with B2O3 fluxed treatment [5].

On the other hand, the XRD patterns shown in Fig. 4 revealed that Pd20Pt20(TM1)20(TM2)20P20 alloys
including TM1 and TM2 other than Cu and Ni shown as XRD profiles (a)–(f) are formed in a mixture
structure from fcc, bcc and monoclinic phases for specimens even in smaller diameters ranging 3–5 mm.
Thus, it was found that (TM1,TM2) = (Cu,Ni) shown as XRD profile (g) is the only possible
combinations for the alloy series to be formed in HE-BMG. The reason for the formation of BMGs
including an atomic pair of Cu-Ni is explained by the meat of mixing ('Hmix) [8, 9] summarized in Table
1 and the information of phase diagrams [10]. The Cu-Ni atomic pair has a positive value of 'Hmix = +4
kJmol-1, whereas Cu-Co and Cu-Fe atomic pairs have a greater positive 'Hmix values of + 6 kJmol-1 and
+13 kJmol-1, respectively. Besides, on the phase diagrams Cu-Ni exhibits solid solutions over an entire
composition, whereas Cu-Co and Cu-Fe exhibit immiscible composition region. Besides the alloys
studied in the present study, (TM1,TM2) = (Fe,Ni) and (Co,Ni) are expected as the candidates of HE-
230 A. Takeuchi et al. / Procedia Engineering 36 (2012) 226 – 234

BMGs because of their values of 'Hmix are –2 and 0 kJmol-1, respectively. In addition, both (TM1,TM2)
= (Fe,Ni) and (Co,Ni) exhibit entire formation of solid solutions on the phase diagram. These
considerations explain that the formation of HE-BMG for (TM1,TM2) = (Cu,Ni) is due to avoidance of
the phase separation tendencies of the atomic pair. Further researches for the alloys (TM1,TM2) = (Fe,Ni),
(Co,Ni) will be reported the results somewhere else in near future.

Fig. 4 XRD patters of Pd20Pt20(TM1)20(TM2)20P20 cylinders with 3 and 5 mm in diameter prepared by copper mold casting.
(TM1,TM2) = (Co,Cu), (Co,Fe), (Fe,Cu) and (Cu,Ni).

Table 1. Mixing enthalpy ('Hmix) in the units of kJmol-1 at binary equi-atomic compositions for atomic pairs [8, 9] for
Pd20Pt20(TM1)20(TM2)20P20 alloy where (TM1,TM2) = (Co,Cu), (Co,Fe), (Fe,Cu) and (Cu,Ni). Asterisk indicates the atomic pairs,
which were not studied in the present study.

'Hmix Pd Pt Ni Cu P Fe
Pd — +2 0 –14 –36.5 –4
Pt +2 — –5 –12 –34.5 –13
Ni 0 –5 — +4 –34.5 –2*
Cu –14 –12 +4 — –17.5 +13
P –36.5 –34.5 –34.5 –17.5 — –39.5

3.2. C-CE Diagram for HE-BMGs

Figure 5 shows the C-CE diagram for HE-BMGs and BMGs. Figure 5 contains plots of
Pd20Pt20Cu20Ni20P20 [5] with alloy No. 25 and Zn20Ca20Sr20Yb20(Li0.55Mg0.45)20 [6] with alloy No. 26 as
HE-BMGs of a narrow and wide senses, respectively. The other plots in Fig. 5 are BMGs with dc of half-
inch (~ 1.27 cm) or more with Nos. 1–18 [11–26] analyzed in our previous work [27], and other BMGs
with Nos. 19–23 [28–31]. The C-CE diagram clearly indicates that Pd20Pt20Ni20Cu20P20 alloy is plotted at
 A. Takeuchi et al. / Procedia Engineering 36 (2012) 226 – 234 231

(0,0,1), indicating that the Pd20Pt20Ni20Cu20P20 alloy is the HE-BMG of a narrow sense. On the other hand,
the Zn20Ca20Sr20Yb20(Li0.55Mg0.45)20 alloy with a high z-value of 0.98 ~ 1 is plotted near the origin in the
x-y plane, indicating that the Zn20Ca20Sr20Yb20(Li0.55Mg0.45)20 alloy is a HE-BMG of the wide sense.
Besides, the BMGs in the centimeter with dc of half-inch (~ 1.27 cm) with Nos. 1– 18 [11–26] are plotted
ranging 0.66 < z < 0.98. Among the alloys listed in Table 2, Pd- and Pt-based BMGs, such as Nos. 1, 3
and 8 tend to have high z value, whereas Zr- and La-based BMGs with Nos. 7, 11, 18, 21 and 22 has
lower z-values. The Be-containing Zr-based BMG (Vit1) with No. 2 has a high z-value of 0.9, but this
alloy is not plotted near the origin in x-z plane as the Pd- and Pt-based BMGs. This feature of Vit1
suggests that Vit1 cannot be a candidate of HE-BMG. On the other hand, it is noted that Y36Sc20Al24Co20
BMG with No. 9 has a high z-value of 0.98 and its position at x-y plane is as close to that of the
Zn20Ca20Sr20Yb20(Li0.55Mg0.45)20 HE-BMG of a wide sense. This feature of Y36Sc20Al24Co20 BMG
indicates that Metal-Metal type HE-BMG of a narrow sense will be found by modifying a composition
slightly from Y36Sc20Al24Co20 BMG. We will report the results of Metal-Metal type HE-BMG of a narrow
sense somewhere else in in near future. Thus, Fig. 5 indicates that a reason for the Pd20Pt20Cu20Ni20P20
formable as a HE-BMG is due to its prototype of Pd40Ni40P20 BMG, which is located at a nearest the
origin among the BMGs listed in Table 2. Thus, the C-CE diagram indicates the candidates of the future
HE-BMGs by its positions in the diagram.

Fig. 5 Composition–configurational entropy (C-CE) diagram for HE-BMGs and BMGs. The plots (pink) with alloy numbers in
Table 2 exhibit the (x,y,z) calculated by Eqs. (3)–(5). The dots (light green) on the x-z plane, which are drawn by tracing the plots,
are to show the z-value comprehensively. The Pd20Pt20Cu20Ni20P20 HE-BMG (Alloy No. 25) has a plot at (0,0,1). The distance of the
plots traced on the base (x-y plane) form the origin (0,0,0) indicates the degree of equi-atomicity of alloys.
232 A. Takeuchi et al. / Procedia Engineering 36 (2012) 226 – 234

Table 2 Bulk metallic glasses, their critical diameters (dc) and their references. Alloys with Nos. 1–18 are BMGs with dc of half-
inch (~ 1.27 cm) or more, which were analyzed in the authors’ previous study [27]. Alloys with Nos. 19–23 are newly added as dc
t half-inch in the present study and those with Nos. 25 and 26 are HE-BMGs. Alloy with No. 24 is the prototype of Alloy No. 14.

No Alloy dc / mm z Ref.
1 Pd40Cu30Ni10P20 72 0.92 [11]
2 Zr41.2Ti13.8Cu12.5Ni10Be22.5 (Vit1) >50 0.91 [12]
3 Pd35Pt15Cu30P20 30 0.96 [13]
4 Zr55Al10Ni5Cu30 30 0.77 [14]
5 Mg59.5Cu22.9Ag6.6Gd11 27 0.77 [15]
6 Mg54Cu26.5Ag8.5Gd11 25 0.82 [16]
7 Zr48Cu36Ag8Al8 25 0.81 [17]
8 Pd40Ni40P20 25 0.96 [18]
9 Y36Sc20Al24Co20 25 0.98 [19]
10 (La0.7Ce0.3)65Co25Al10 25 0.90 [20]
11 La62(Cu5/6Ag1/6)14Ni5Co5Al14 >20 0.68 [21]
12 Zr57Ti5Cu20Ni8Al10 20 0.76 [22]
13 Pt42.5Cu27Ni9.5P21 20 0.92 [23]
14 (Fe0.8Co0.2)48Cr15Mo14C15B6Tm2 16 0.87 [24]
15 Pt60Cu16Ni2P22 16 0.73 [23]
16 Mg54Cu28Ag7Y11 16 0.81 [16]
17 Ca65Mg15Zn20 >15 0.81 [25]
18 Zr58.5Nb2.8Cu15.6Ni12.8Al10.3 15 0.75 [26]
19 Ni50Pd30P20 21 0.94 [28]
20 Pd40Ni40Si4P16 20 0.83 [29]
21 Zr61Ti2Nb2Al7.5Ni10Cu17.5 20 0.66 [30]
22 Zr60Ti2Nb2Al7.5Ni10Cu18:5 20 0.67 [30]
23 Ti40Zr25Cu12Ni3Be20 14 0.87 [31]
24 Fe48Cr15Mo14Er2C15B6 12 0.81 [32]
25 Pd20Pt20Cu20Ni20P20 10 1 [5]
26 Zn20Ca20Sr20Yb20(Li0.55Mg0.45)20 >3 0.98 [6]

4. Conclusions

The Pd20Pt20(TM1)20(TM2)20P20 alloys where (TM1,TM2) = (Co,Cu), (Co,Fe), (Fe,Cu) and (Cu,Ni) in
Metal–Metalloid type were experimentally studied in the present work. The results revealed that
Pd20Pt20Cu20Ni20P20 is formed in HE-BMG with a critical diameter of 10 mm, but other alloys with atomic
pairs excepting for (TM1,TM2) = (Cu,Ni) were not formed in BMGs. The composition–configurational
entropy (C-CE) diagrams proposed in the present study efficiently express the degree of equi-atomicity,
 A. Takeuchi et al. / Procedia Engineering 36 (2012) 226 – 234 233

leading to suggesting candidates of HE-BMGs from BMGs found to date. The alloy design with a concept
of HE alloys accompanied by C-CE diagram is useful for the further development of HE-BMGs.

Acknowledgements

This work was supported by Grants-in-Aid for Scientific Research from Japan Society for the
Promotion of Science (JSPS). 1: Grant Program of Scientific Research (S) with a program title of
“Fabrication of Bulk Metallic Glasses in Centimeter Class and their Industrialization” (grant number
20226013) and 2: Grant Program of Scientific Research (C) with program title of “Clarification of Local
Atomic Arrangements of Metallic Glasses with Plastic Crystal Model and Fabrication of Novel Bulk
Metallic Glasses” (grant number 21560715).

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