Machine learning-based inverse design for

single-phase high entropy alloys

Cite as: APL Mater. 10, 101104 (2022); https://doi.org/10.1063/5.0109491
Submitted: 13 July 2022 • Accepted: 12 September 2022 • Published Online: 20 October 2022

Yingzhi Zeng, Mengren Man, Chee Koon Ng, et al.

COLLECTIONS

Paper published as part of the special topic on Design and Development of High Entropy Materials

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APL Mater. 10, 101104 (2022); https://doi.org/10.1063/5.0109491 10, 101104

© 2022 Author(s).
 APL Materials ARTICLE scitation.org/journal/apm

Machine learning-based inverse design

for single-phase high entropy alloys
Cite as: APL Mater. 10, 101104 (2022); doi: 10.1063/5.0109491
Submitted: 13 July 2022 • Accepted: 12 September 2022 •
Published Online: 20 October 2022

Yingzhi Zeng,1 Mengren Man,1 Chee Koon Ng,2,a) Delvin Wuu,2 Jing Jun Lee,2 Fengxia Wei,2
2,3 1,a) 2
Pei Wang, Kewu Bai, Dennis Cheng Cheh Tan, and Yong-Wei Zhang1,a)

AFFILIATIONS
1
Institute of High Performance Computing, Agency for Science, Technology and Research, Singapore, 1 Fusionopolis Way,
No. 16-16 Connexis, Singapore 138632, Republic of Singapore
2
Institute of Materials Research and Engineering, Agency for Science Technology and Research, 2 Fusionopolis Way,
No. 08-03 Innovis, Singapore 138634, Republic of Singapore
3
Engineering Cluster, Singapore Institute of Technology, Singapore 519961, Republic of Singapore

Note: This paper is part of the Special Topic on Design and Development of High Entropy Materials.
a)
Authors to whom correspondence should be addressed: ng_chee_koon@imre.a-star.edu.sg; baikw@ihpc.a-star.edu.sg;
and zhangyw@ihpc.a-star.edu.sg

ABSTRACT
In this work, we develop an inverse design framework to search for single-phase high entropy alloys (HEAs) subjected to specified phase
targets and constraints. This framework is based on the fast grid search in the composition–temperature space, enabled by a highly accurate
and efficient machine learning model trained by a huge amount of data. Using the framework, we search through the entire quaternary,
quinary, and senary alloy systems, formed by Al, Co, Cr, Cu, Fe, Mn, Ni, and Ti, to identify three types of HEAs: (1) the single-phase FCC
HEA with the highest Al content; (2) the single-phase FCC HEA with lower equilibrium temperatures; and (3) single-phase BCC HEAs with
Al as the principal element. For the first time, we reveal that the highest Al content in single-phase FCC HEAs is 0.15 in mole fraction, which
is higher than the Al contents in all reported single-phase FCC HEAs. The identified HEAs for the quaternary, quinary, and senary groups are
Al0.15 Co0.34 Cr0.16 Ni0.35 , Al0.15 Co0.35 Cr0.1 Fe0.05 Ni0.35 , and Al0.15 Co0.36 Cr0.06 Fe0.06 Mn0.01 Ni0.36 , respectively. All the designed HEAs are verified
by the equilibrium calculations with Thermo-Calc software and the TCHEA3 database. We further conduct Scheil–Gulliver calculations and
experimental fabrications and characterizations for the designed HEAs, to verify the formation of the targeted phases at non-equilibrium
conditions. This work demonstrates a viable approach to design HEAs with specified phase targets and constraints.
© 2022 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license
(http://creativecommons.org/licenses/by/4.0/). https://doi.org/10.1063/5.0109491

I. INTRODUCTION first-principles calculations,7,8 CALPHAD methods,9–11 and

High entropy alloys (HEAs) have drawn significant interest
in the materials research community owing to their remarkable
physical, chemical, and mechanical properties, as well as the great
possibilities to tune their properties due to the large composition
space. However, the large composition space also poses a significant
challenge for designing novel HEAs with desirable properties or
functionalities. Because of a large number of possible combinations,
intuitive and empirical approaches generally lead to a low success
rate even though considerable time and cost have been spent.1,2
Various computational methods, such as empirical methods,3–6
machine learning (ML) methods,1,12–18 have been developed to dis-
cover and design promising HEAs. While these “forward prediction”
methods are successful in predicting new HEAs, they alone are often
unable to efficiently discover HEAs with desirable compositions
and specified phases due to the vast high-dimensional composition
space in HEAs; this problem calls for the need for inverse design
methods.
Inverse design or solving inverse problems in material dis-
covery takes the required functionality or property as an input
and outputs the materials or configurations with this function-
ality or property.19 Various inverse design methods have been

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deployed to predict alloys with desirable mechanical properties.
For example, Ikeda conducted an inverse design for nickel-based
super alloys using genetic algorithm (GA) and molecular dynam-
ics simulations.20 Ganguly et al.21 applied a non-dominated sorting
genetic algorithm (NSGA II)22 to determine the composition and
processing parameters that yield the strength–ductility balance of
thermo-mechanically processed multiphase steels. To obtain desir-
able yield strength and high-temperature creep rupture life of ultra-
supercritical alloys, Hu et al.23 developed an artificial neural network
(ANN) model using 580 data points collected from the literature and
experiments. Artrith et al.24 reported an inverse design methodol-
ogy to search for low-energy atomic configurations of amorphous
LiSi alloy. Their method was based on a potential model trained by
an ANN with 1000 first-principles calculations and a GA framework
serving as the search algorithm. Lee et al.25 set up an integrated ML
platform consisting of 16 ML algorithms to predict the yield strength
(YS) and ultimate tensile strength (UTS) based on 16 descriptors
and 5473 thermo-mechanically controlled processed steel alloys.
The authors fully trained seven non-linear ML models to ensure the
“inverse design” based on NSGA-II that enabled predicting desirable
YS/UTS values.
It is noted that the majority of reported studies of alloy inverse
designs focused on the prediction of material properties; only a few
investigations demonstrated the effective inverse design of mate-
rial structures. It is known that the excellent properties of HEAs
are largely attributed to the formation of solid solution phases
with unique microstructures. In the exploration of the HEA phase
domains in the composition–temperature space that satisfy the
desired phase constitution requirements, Abu-Odeh et al.11 pointed
out that the standard phase stability calculations/predictions are
the forward phase stability problems, whereas the targeted explo-
ration of a potentially high-dimensional thermodynamic space can
be constructed as an inverse phase stability problem. Since the
phase-stability space has non-analytical phase boundaries represent-
ing abrupt transitions between the presence and absence of specific
phases, they framed the inverse problem as a continuous constraint
satisfaction problem and solved it using a constraint satisfaction
algorithm. Lee et al.2 reported a deep learning classification model
trained by using more than 900 experimental data points to predict
solid solutions, intermetallic compounds, and amorphous phases. It
is worth noting that in their study, data augmentation was carried
out by inverse design of various phases using a generative adversarial
network.
Among the various types of HEAs, Al-containing FCC alloys
are particularly interesting because of their excellent high strength
and fabrication via 3D printing. It was shown that the Al content
could significantly affect the microstructures and, consequently, the
mechanical properties of HEAs.26 To our best knowledge, only a
few Al-containing single-phase FCC structures with Al mole fraction
greater than 0.1 were reported, as shown in the Appendix acquired
from various publications,1,27–33 where large datasets of HEAs are
compiled. The highest Al content of the reported single-phase FCC
was found to be 0.2 (mole fractions) in AlLiMg0.5 ScTi1.5 , 29 followed
by 0.13 in Al0.4 CoCrNi, 34 and 0.125 in AlCo3.5 CrCu0.5 FeNi.29 Our
equilibrium calculation by Thermo-Calc shows no single-phase FCC
in AlLiMg0.5 ScTi1.5 in the temperature ranging from 300 to 1700 K.
This is consistent with the original literature35 cited by Ref. 29,
in which it was stated that the single-phase FCC structure of
APL Mater. 10, 101104 (2022); doi: 10.1063/5.0109491
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AlLiMg0.5 ScTi1.5 was obtained during ball milling and transformed
to single-phase HCP upon annealing. The equilibrium calculation
of AlCo3.5 CrCu0.5 FeNi reveals that no single-phase FCC is found
within the temperature range 300–1700 K either. Instead, a mixture
of FCC and other phases is present. On the other hand, the equilib-
rium calculation confirms the existence of the single-phase FCC in
quaternary Al0.4 CoCrNi. Thus, an interesting question arises: What
is the highest Al content in single-phase FCC HEAs? Answer to this
question is of great importance to the design of lightweight, high
strength, high ductility, 3D printable, Al-based HEAs. In addition,
it is also highly desirable to obtain single-phase FCC HEAs that are
stable at lower temperatures, as such HEAs would enable a wider
processing window. Furthermore, single-phase BCC HEAs with Al
as the principal element are of great interest, but much less studied
compared to their FCC counterparts. Thus, it is also interesting to
design such types of HEAs.
However, it is highly challenging to design the above-
mentioned three categories of HEAs by experiments or by forward
prediction alone using Thermo-Calc calculations, as these methods
are inefficient. In the present work, we address the aforemen-
tioned issues by developing an inverse design framework to predict
HEAs with specific single-phase and constraints. This framework
is based on the fast grid search in the composition–temperature
space, enabled by a highly accurate and efficient machine learn-
ing model that was initially trained by 355 320 evenly-spaced data
points at the equilibrium computed from Thermo-Calc calculations
and further improved by nine rounds of active learning, with a total
of 654 757 data points.18 To demonstrate the effectiveness of the
framework, we study all the quaternary, quinary, and senary alloy
systems formed by Al, Co, Cr, Cu, Fe, Mn, Ni, and Ti. Remark-
ably, all the predictions of HEAs by the inverse design are verified
by the Thermo-Calc calculations. We also conduct Scheil–Gulliver
calculations and experimental fabrications and characterizations
to further verify all the designed HEAs. This work demonstrates
a viable method to design HEAs with specified single-phase and
constraints.
II. INVERSE DESIGN BY MACHINE LEARNING
In this study, the targets are the alloy compositions that lead to
the phases of interest, namely, single-phase FCC and BCC in qua-
ternary, quinary, and senary alloys comprising the eight elements
Al, Co, Cr, Cu, Fe, Mn, Ni, and Ti. The corresponding forward
problem of phase prediction has been well studied and summa-
rized as follows: Thermo-Calc software with TCHEA3 database was
used for the equilibrium calculations. Among the 35 Al-containing
quinary alloy families, we chose 20 alloy families with high credi-
bility, namely, FAB (fractions of assessed end-binary) = 1 and FAT
(fractions of assessed end-ternary) > 0.7. We generated 355 320
data points on a uniform grid where the temperature range was
300–1700 K with step ΔT = 10 K and the composition (mole frac-
tion) step ΔX = 0.1. The equilibrium calculation results were labeled
the following four classes. Class-0: phases containing liquid; Class-
1: disordered single FCC phase with mole fraction >0.999; Class-2:
disordered single BCC phase with mole fraction >0.999; and Class-
3: the other phases. These data were used as the inputs to train the
initial machine learning model. Subsequently, we implemented an
iterative process known as active learning to improve the ML model
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 APL Materials
by predicting new FCC and BCC phases followed by CALPHAD ver-
ifications. A total of additional 299 437 data points were predicted
and verified and then incorporated as the ML inputs in nine rounds
of active learning.
As described earlier, both Thermo-Calc and its approxima-
tion by machine learning models allow predicting the alloy phases
under equilibrium. Either approach provides us with a forward pre-
diction model,which we denote by f . Making a forward prediction
essentially amounts to a function evaluation, f (Teq , XAl , . . . , XTi )
= y, where T eq is the equilibrium temperature, X i the mole frac-
tion of the i-th element, and the labels y = 0 for alloys containing
liquid, y = 1 for single-phase FCC, y = 2 for single-phase BCC, and
y = 3 for others. The function f is essentially a black box and does
not allow explicit inversion. To solve the inverse problem, we must
instead resort to querying the design space with the forward map
f to identify the inputs (Teq , XAl , . . . , XTi ) that are mapped to the
desired labels. The process potentially involves making a large num-
ber of function evaluations. In the given notation, the inverse design
problem for FCC, for instance, is stated as, find (Teq , XAl , . . . , XTi )
such that f (Teq , XAl , . . . , XTi ) = 1. Inverse design for single-phase
BCC can be stated similarly.
The design space of the inverse problem is the part of the
temperature–composition space between 300 and 1700 K. An opti-
mization algorithm can guide the choice of design points for evalu-
ation by the forward map, so that the sequence of evaluated design
points eventually converges into a solution to the inverse problem.
This approach requires a suitable loss function to measure the mis-
match between the predicted label and the target property, which
can then be minimized by the optimization algorithm. In the cases
where the forward model can make probabilistic predictions, the
mismatch can be measured with cross-entropy, Kullback–Leibler
divergence, or mutual information. Algorithms commonly used for
optimizing black-box functions include particle swarm and Bayesian
optimization. Alternatively, since the design space for our problem
is bounded, it can be covered by a uniform grid of design points,
with the forward map applied to make predictions over the entire
grid. The latter approach is commonly known as grid search. An
optimization algorithm takes advantage of queries that have already
been made in deciding the choice of new points for subsequent
evaluations. This could potentially lead to a saving in computa-
tion time. On the other hand, optimization of a black-box function,
especially with population methods such as particle swarm, can add
significantly to the computational cost. In the case of an extremely
efficient forward map, a naive grid search strategy can be benefi-
cial as it would not only be faster, but also affords a structured
view of the part of phase diagram covered by the grid. In a recent
publication,36 a similar framework was reported for electromagnetic
inverse design, and superb performance was shown over widely
used heuristic approaches, such as genetic algorithms or swarm
optimization.
Although thermodynamic simulation programs such as
Thermo-Calc are ideal for forward prediction, their computational
cost prohibits making a sufficiently large number of function evalua-
tions. Thermo-Calc is thus not suitable to be used directly for inverse
design. Instead, ML offers a viable solution as an efficient approx-
imation to Thermo-Calc. As reported in our previous studies,1,18
gradient boosting with decision trees implemented via the eXtreme
Gradient Boosting (XGBoost) library produces ML models that
APL Mater. 10, 101104 (2022); doi: 10.1063/5.0109491
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efficiently approximate Thermo-Calc in alloy phase prediction. The
details of the ML model training have been described in our pre-
vious work18 and have been summarized at the beginning of this
section.
Let us denote the XGBoost model by f̃ . We compared the
efficiencies of inverse design via (1) particle swarm optimization
guided queries by f̃ , and (2) grid search by f̃ . For approach (1),
finding 200 000 FCC inverse designs took ∼24 h, while finding
the same number of BCC inverse designs required a separate run
that took substantially longer. For approach (2), we covered the
design space with a fine grid having ΔT = 1 K and ΔX = 0.01
for 35 Al-containing quinary alloy families; the entire grid search
procedure finished in about 7 h, producing both FCC and BCC
inverse designs that number in tens of millions. This is an indica-
tion that the ML model f̃ is extremely efficient, whereas running
an optimization algorithm to guide function evaluations introduces
a bottleneck. For this reason, we adopt the grid search approach
with the ML model f̃ for inverse design of single-phase FCC
and BCC.
The flowchart for the design of new HEAs is shown in Fig. 1.
The conditions of the design and the verifications of the inverse
design are described in Secs. III and IV.
III. PREDICTION RESULTS BY INVERSE DESIGN
As mentioned previously, it is often difficult to find new HEAs
by intuition and experience or even by forward CALPHAD cal-
culations. Therefore, in the present work, we employ the inverse
design by ML to search for new HEAs. In particular, we study the
quaternary, quinary, and senary alloy systems containing the eight
elements of Al, Co, Cr, Cu, Fe, Mn, Ni, and Ti, and search for
the following three groups of new HEAs satisfying the specified
conditions:
(1) High Al single-phase FCC structures:
● single-phase FCC with Al mole fraction greater than
0.10,
● the mole fraction of each element in the range
0.05–0.35 for quaternary and quinary systems,
● the mole fraction of at least five atoms in the range
0.05–0.36 for senary systems.
(2) Single-phase FCC structures stable at lower equilibrium
temperatures:
● the mole fraction of each element in the range
0.05–0.35 for quinary systems,
● the equilibrium temperature lower than 1000 K.
(3) High Al single-phase BCC structures:
● single-phase BCC with Al mole fraction greater than
0.10,
● the mole fraction of each element in the range
0.05–0.35 for quinary systems.
We obtain a set of 18 entries satisfying the conditions men-
tioned earlier by the inverse design. The predicted compositions
(in mole fraction) of the three groups of HEAs are shown in the
10, 101104-3
 APL Materials
three parts of Table I. These predicted compositions are first veri-
fied by the equilibrium calculations with Thermo-Cal software and
TCHEA3 database.37
As shown in the first part of Table I, one quinary Al0.15 Co0.35
Cr0.1 Fe0.05 Ni0.35 (No. 1) and one senary Al0.15 Co0.36 Cr0.06 Fe0.06
Mn0.01 Ni0.36 (No. 2) have the Al mole fraction 0.15, which is clearly
higher than all the reported quinary and senary HEAs of single-
phase FCC structures listed in the Appendix. Furthermore, a set
of predicted Al–Co–Cr–Ni quaternary systems is found to have an
Al mole fraction higher than that of the highest Al mole fraction
(0.13) in Al0.4 CoCrNi reported in Ref. 34. In Table I, we list one
of the predicted quaternary systems, Al0.15 Co0.34 Cr0.16 Ni0.35 (No. 3),
which has the highest Al mole fraction. We also obtain other quinary
single-phase FCC compositions and temperatures with Al mole frac-
tion close to 0.1 and list these entries with the lowest equilibrium
temperatures in Table I.
To examine whether there exist single-phase FCC struc-
tures with the Al mole fraction higher than 0.15, i.e., the Al
mole fractions of Al0.15 Co0.35 Cr0.1 Fe0.05 Ni0.35 (No. 1), Al0.15 Co0.36
Cr0.06 Fe0.06 Mn0.01 Ni0.36 (No. 2), and Al0.15 Co0.34 Cr0.16 Ni0.35 (No. 3),
we conduct the calculations of the pseudo-binary phase diagram
by varying the compositions of Al and another element, while
keeping the compositions of the rest of the atoms the same as
in the original formulas. In Al0.15 Co0.35 Cr0.1 Fe0.05 Ni0.35 (No. 1),
the following four pseudo-binary phase diagrams are generated,
Al–Co, Al–Ni, Al–Fe, and Al–Cr, as shown in Fig. 2. Similarly,
in Al0.15 Co0.36 Cr0.06 Fe0.06 Mn0.01 Ni0.36 (No. 2), the following four
APL Mater. 10, 101104 (2022); doi: 10.1063/5.0109491
© Author(s) 2022
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FIG. 1. The workflow for the inverse
design of HEAs.
pseudo-binary phase diagrams Al–Co, Al–Ni, Al–Fe, and Al–Cr are
generated and shown in Fig. 3. It is noted that since the composition
of Mn is 0.01, the minimum value of the current study, we do not
generate the Al–Mn pseudo-binary phase diagram. Furthermore,
in Al0.15 Co0.34 Cr0.16 Ni0.35 (No. 3), the three pseudo-binary phase
diagrams of Al–Co, Al–Cr, and Al–Ni are generated and shown
in Fig. 4.
As can be seen in Figs. 2–4, the highest Al mole fractions in the
phase diagrams are completely overlapped with the inverse design
results (shown by the magenta stars) in all the plots, indicating that
no higher Al compositions can be found in the single-phase FCC
regions. These results demonstrate that the inverse design method is
successful in searching for the alloys with the highest Al contents.
To further demonstrate the performance of the inverse design
framework, we add the temperature constraints in the conditions
of Figs. 2(a) and 2(b), respectively. The objective is to search for
the maximum Al composition in the single-phase FCC regions at
temperatures 1300, 1400, 1500, and 1600 K, respectively. The red
triangles in Figs. 5(a) and 5(b) show the maximum Al mole fractions
at the four temperatures predicted by the inverse design. Clearly, the
predicted entries are well located near the boundaries of the FCC
single-phase regions in which the maximum Al contents are present
at the corresponding temperatures.
A series of HEAs with the chemical formula Alx CoCrFeMn
have been extensively studied.32,33,38 Among these studies, it was
reported that single-phase FCC structures are present when x
< 0.375, which is equivalent to Al mole fraction 0.086. To explore if
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TABLE I. Chemical compositions (mole fraction) and the equilibrium temperatures of the single-phase FCC and BCC
predicted by the inverse design and Scheil–Gulliver (S–G) calculations.

Single-phase FCC, X(Al) ≥ 0.1

Number Temp (K) Al Co Cr Fe Mn Ni FCC mole fraction by S–G
1 1660 0.15 0.35 0.1 0.05 0.35 0.903
2 1640 0.15 0.36 0.06 0.06 0.01 0.36 0.910
3 1660 0.15 0.34 0.16 0.35 0.914
4 1464.7 0.1 0.34 0.11 0.1 0.35 0.990
5 1483.6 0.1 0.33 0.06 0.16 0.35 0.990
6 1491 0.1 0.26 0.21 0.08 0.35 0.990
7 1491.6 0.1 0.35 0.19 0.05 0.31 0.990
8 1504.8 0.1 0.27 0.11 0.17 0.35 0.990

Single-phase FCC, lower temperature

Number Temp (K) Co Cr Cu Fe Mn Ni FCC mole fraction by S–G
9 955 0.13 0.08 0.35 0.09 0.35 0.990
10 703.1 0.35 0.07 0.06 0.18 0.34 0.990
11 910.8 0.22 0.07 0.35 0.07 0.29 0.990
12 792 0.35 0.07 0.11 0.19 0.28 0.990
13 972.5 0.26 0.21 0.08 0.12 0.33 0.990
14 988.9 0.2 0.19 0.11 0.17 0.33 0.990
15 883.5 0.22 0.1 0.28 0.13 0.27 0.990

Single-phase BCC
Number Temp (K) Al Co Cr Fe Mn BCC mole fraction by S–G
16 1200 0.12 0.05 0.35 0.14 0.34 0.990
17 1363.5 0.12 0.05 0.35 0.35 0.13 0.990
18 1400 0.10 0.11 0.35 0.35 0.09 0.990

a higher Al content can be achieved in the single-phase FCC region,
we conduct inverse design for Alx CoCrFeMn and reveal that at tem-
perature range 1580–1610 K, the Al ratio x can be reached up to
0.45, which is equivalent to Al mole fraction 0.10. We further gener-
ate the phase diagram and confirm that the highest Al mole fraction
is 0.10 at temperature 1600 K, as indicated by the magenta star in
Fig. 6, where the x-axis is the Al ratio in Alx CoCrFeMn. This result
shows that the Al mole fraction in Alx CoCrFeMn cannot be higher
than 0.15, which is the highest Al content found in this work by the
inverse design.
In order to examine the possibility of fabricating the predicted
HEAs by experiments, we conduct the Scheil–Gulliver calculations
for all the 18 entries listed in Table I. The mole fractions of the single-
phase FCC or BCC at the solidification temperatures are listed in the
last column of Table I. As can be seen, the phase fractions of FCC in
the first three alloys (with Al mole fraction = 0.15) are slightly greater
than 0.9, whereas the FCC or BCC mole fractions of the other alloys
are larger than 0.99. These results imply that in comparison with the
other predicted HEAs, lower single-phase fractions will be observed
in alloys 1–3 in the experiments.
IV. EXPERIMENTAL VERIFICATION
A. Experimental Procedures
All the alloy ingots (each about 20 g) are prepared by arc
melting and are re-melted at least five times in a hemispherical
water-cooled Cu mold to ensure the microstructure homogeneity.
The as-cast samples are about 25 mm in diameter and 10 mm in
height. The purity of all the raw materials used for the melting
is higher than 99.9% (wt %). The phase constitution is analyzed
by x-ray diffraction (XRD) analysis on an x-ray diffractometer
(Bruker D8 Advance) using Cu Kα radiation scanning from 20○
to 100○ with a scanning speed of 6○ /min. The cylindrical ingot
is mechanically grinded and polished utilizing conventional met-
allurgical procedures down to 0.3 μm colloidal silica suspension
followed by vibratory polishing (VibroMet 2) to prepare them
for microstructure analysis under an optical microscope (Olympus
BX53M), field-emission scanning electron microscope (SEM, JSM-
7600F) with energy dispersive x-ray spectroscopy (EDS), and
electron backscattered diffraction (EBSD) (JSM-IT500HR).
B. Experimental Results
The predicted compositions in Table I are used to fabricate
HEAs via arc melting. Table II shows the actual experimental chem-
ical compositions of the alloys verified by SEM–EDS. The majority
of the experimental compositions match the predicted compositions
with the exception of aluminum, which has relatively low melting
and boiling points. Hence, some of the aluminum would have vapor-
ized during the arc melting process, accounting for the reduction in
atomic concentration for the Al-containing alloys. Figure 7 shows
the XRD data for all the single-phase FCC and BCC alloys, which

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FIG. 2. Pseudo binary phase diagrams based on (No. 1). (a) Al–Co for
Alx Co(0.5−x) Cr0.1 Fe0.05 Ni0.35 , (b) Al–Ni for Alx Co0.35 Cr0.1 Fe0.05 Ni(0.5−x) , (c) Al–Fe
for Alx Co0.35 Cr0.1 Fe(0.2−x) Ni0.35 , and (d) Al–Cr for Alx Co0.35 Cr(0.25−x) Fe0.05 Ni0.35 .
The magenta stars indicate the compositions of the inverse design.
FIG. 3. Pseudo binary phase diagrams based on (No. 2). (a) Al–Co for
Alx Co(0.51−x) Cr0.06 Fe0.06 Mn0.01 Ni0.36 , (b) Al–Ni for Alx Co0.36 Cr0.06 Fe0.06 Mn0.01
Ni(0.51−x) , (c) Al–Fe for Alx Co0.36 Cr0.06 Fe(0.21−x) Mn0.01 Ni0.36 , and (d) Al–Cr for
Alx Co0.36 Cr(0.21−x) Fe0.06 Mn0.01 Ni0.36 . The magenta stars indicate the compositions
of the inverse design.

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FIG. 5. The maximum Al mole fractions predicted by the inverse design at temper-
atures 1300, 1400, 1500, and 1600 K in comparison with the two pseudo-binary
phase diagrams of No. 1. (a) Al–Co for Alx Co(0.5−x) Cr0.1 Fe0.05 Ni0.35 and (b) Al–Ni
for Alx Co0.35 Cr0.1 Fe0.05 Ni(0.5−x) .

FIG. 4. Pseudo binary phase diagrams based on (No. 3) (a) Al–Co for
Alx Co(0.49−x) Cr0.16 Ni0.35 , (b) Al–Ni for Alx Co0.34 Cr0.16 Ni(0.5−x) , and (c) Al–Cr for
Alx Co0.34 Cr(0.31−x) Ni0.35 . The magenta stars indicate the compositions of the
inverse design.

show apparent FCC peaks for alloys 1–15, while alloys 16–18 con-
tain only BCC peaks in the XRD patterns. Upon detailed analysis,
the EBSD of alloys 1–3 (Fig. 8) shows that the solidification of the
alloys starts with the formation of the primary FCC phase in yellow
FIG. 6. Phase diagram of Alx CoCrFeMn showing the highest Al content is x = 0.45
and ends with a eutectic reaction yielding a eutectic microstruc- in FCC region.
ture of FCC + BCC (in red) with a small size. It is likely that the

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TABLE II. Experimental chemical compositions (in mole fraction) of the single-phase
FCC and BCC alloys fabricated by arc melting.

Single-phase FCC, X(Al) ≥ 0.1

Number Al Co Cr Fe Mn Ni
1 0.15 0.35 0.103 0.054 0.343
2 0.16 0.355 0.06 0.06 0.011 0.354
3 0.165 0.333 0.158 0.344
4 0.076 0.356 0.116 0.101 0.35
5 0.073 0.341 0.067 0.16 0.36
6 0.07 0.266 0.221 0.087 0.355
7 0.074 0.362 0.201 0.054 0.31
8 0.071 0.272 0.126 0.176 0.355

Single-phase FCC, lower equilibrium temperature

Number Co Cr Cu Fe Mn Ni
9 0.131 0.082 0.352 0.091 0.344
10 0.358 0.068 0.062 0.174 0.338
11 0.354 0.074 0.114 0.176 0.282
12 0.293 0.162 0.076 0.138 0.332
13 0.221 0.09 0.339 0.067 0.282
14 0.193 0.229 0.109 0.163 0.306
15 0.215 0.126 0.274 0.13 0.254

Single-phase BCC
Number Al Co Cr Fe Mn
16 0.082 0.052 0.41 0.137 0.32
17 0.077 0.054 0.39 0.363 0.115
18 0.065 0.114 0.375 0.357 0.089

crystallite sizes of the BCC phases are too small, which result in sig-
nificant broadening of the BCC XRD peaks in alloys 1–3, making
them difficult to be observed. The Rietveld refinement of the XRD
peaks for these alloys yields FCC mole fractions of 91.3%, 91.7%,
and 91.2%, respectively, which match closely the Scheil–Gulliver
calculations in Table I.

V. DISCUSSIONS
In solving typical inverse design problems for which the for-
ward model is available only in the form of a black-box, an opti-
mization algorithm is often employed to guide the choice of design
points for evaluating the model. While using an optimization algo-
rithm could potentially reduce the number of evaluations and lead to
a shorter overall computation time, executing an optimization algo-
rithm, especially population methods such as particle swarm, can
significantly increase the computational cost. Therefore, to decide
on an optimal strategy, it is necessary to compare the computational
costs of evaluating the forward model and running an optimization
algorithm.
In the present work, we apply an alternative strategy for the
inverse design, i.e., making the predictions on the entire grid by the
forward ML model. Our strategy is based on the fact that the design FIG. 7. The XRD spectra of the single-phase FCC Al alloys 1–8 (top panel),
single-phase FCC alloys 9–15 (center panel), and single-phase BCC alloys 16–18
space for our problem is bounded, and it can be covered by a uni- (bottom panel).
form grid of design points. More importantly, since our forward ML

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© Author(s) 2022
 APL Materials
FIG. 8. The EBSD phase maps of alloys No. 1–No. 3, which show the primary phase FCC in yellow, while the secondary BCC phase in red.
model is very efficient, it is very quick to obtain the desired results
even if the finer grid size is set. However, for higher order alloy
systems with number of elements ≥6, if the grid size is equal to or
smaller than 0.01 in mole fractions, it would take a much longer time
to obtain the results for the much larger grid. In the case of senary
alloy systems, grid search can still be accomplished in a reasonable
amount of time by reducing the grid size to 0.02 mol fractions, which
is nevertheless well within experimental accuracy.
It is worth noting that in the three alloys predicted by the
inverse design where the highest Al contents (i.e., 0.15 mol fraction)
emerge, namely, Al0.15 Co0.35 Cr0.1 Fe0.05 Ni0.35 (No. 1), Al0.15 Co0.36
Cr0.06 Fe0.06 Mn0.01 Ni0.36 (No. 2), and Al0.15 Co0.34 Cr0.16 Ni0.35 (No. 3),
the compositions of Co and Ni reach their upper limits. This behav-
ior can be attributed to the fact reported in our previous work,1
where Co and Ni are FCC stabilizers, whereas Al destabilizes FCC.
It is noted that the concept of the phase stabilizer can be associ-
ated with the well-known Hume-Rothery rules, which are based on
the differences in the atomic size, crystal structure, and electron
valence state of the solute and solvent. The overall effect of these
factors of the elements alloying on a specific phase region are gen-
erally described by the concept of the phase stabilizer. Since the
single-phase FCC structure is maximally destabilized by Al, it must
be simultaneously maximally stabilized by Co and Ni. These three
alloys (Nos. 1–3) are nearly at the corners of the FCC phase regions.
Any further increase in Al content or decrease in Co or Ni content
will result in a phase transition out of the single-phase FCC. This can
be seen by the precipitation of some fine BCC phases in the three
as-cast alloys during the fabrication process.
The size effect is mainly responsible for the FCC stability and
solubility limit,18 which can be simply explained by the elastic the-
ory, assuming that a misfitting solute atom, such as Al, is regarded
as an elastic sphere that is then compressed or expanded into a sol-
vent lattice site composing atoms, such as Co–Cr–Fe–Ni atoms.39
It can be inferred that in the HEA alloys, the maximum limit of
Al is highly correlated with the size differences of the FCC region
of its solvent composed of other elements. A wider region of the
single phase disordered FCC in the Co–Cr–Fe–Ni quaternary system
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© Author(s) 2022
ARTICLE scitation.org/journal/apm
has been found,40 which may be possibly owing to the small atom
size difference compared to other quaternary systems. Therefore, it
is not surprising that Co–Cr–Fe–Ni can accommodate highest Al,
while maintaining stable structure of the disordered FCC, which
explains the existence of Al0.15 Co0.35 Cr0.1 Fe0.05 Ni0.35 as reported in
this work.
As mentioned previously, the three groups of HEAs listed
in Table I are predicted by the current inverse design frame-
work, which is based on the ML model trained by the equilib-
rium data. Therefore, these designed compositions should lead to
the formation of the targeted phases at the equilibrium states.
To investigate whether the targeted phases can still exist via fab-
rication through non-equilibrium processes, such as casting or
arc melting, it is necessary to conduct the Scheil–Gulliver sim-
ulation on the designed HEAs. Our results show that although
there are minor discrepancies in the compositions from the inverse
design and the experiments, a predominant fraction (greater than
0.9 mol fractions) of the targeted FCC or BCC is observed in the
experiments, demonstrating the robustness of our inverse design
framework.
VI. CONCLUSIONS
In the present work, we demonstrate the effectiveness of our
inverse design framework based on machine learning in designing
HEAs with specific requirements. Our ML model was trained by
a huge number (654 757) of data points, mainly evenly spacing in
the temperature–compositions space of eight elements. Since the
design space for our problem is bounded, we take the naïve grid
search as the inverse design strategy, which is more efficient than
other strategies. For the first time, by inverse design we reveal the
highest Al content is 0.15 mol fraction in the single-phase FCC
structures in quaternary, quinary, and senary alloy groups formed
by the eight elements Al, Co, Cr, Cu, Fe, Mn, Ni, and Ti. Specif-
ically, the alloys with the highest Al content in the three groups
are Al0.15 Co0.35 Cr0.1 Fe0.05 Ni0.35 , Al0.15 Co0.36 Cr0.06 Fe0.06 Mn0.01 Ni0.36 ,
and Al0.15 Co0.34 Cr0.16 Ni0.35 . These results are verified by the equi-
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librium calculations, Scheil–Gulliver calculations, and experimen-
tal tests. Hence, the present work presents an efficient inverse
design strategy to search for HEAs with specific single-phase
under specific constraints, which shed light on the design of
lightweight HEAs.
ACKNOWLEDGMENTS
This work was supported by the RIE2020 AME Programmatic
Grant (AMDM; Grant No. A1898b0043) and the A∗ STAR Com-
putational Resource Centre and National Supercomputing Centre,
Singapore, through use of their high-performance computing facil-
ities. Y.W.Z. acknowledges the support of the Singapore A∗ STAR
SERC CRF Award.
AUTHOR DECLARATIONS
Conflict of Interest
The authors have no conflicts to disclose.
(equal); Writing – original draft (equal); Writing – review & editing
(equal). Delvin Wuu: Investigation (equal); Visualization (equal);
Writing – review & editing (equal). Jing Jun Lee: Investigation
(equal); Visualization (equal); Writing – review & editing (equal).
Fengxia Wei: Investigation (equal); Visualization (equal); Writing –
review & editing (equal). Pei Wang: Formal analysis (equal); Fund-
ing acquisition (equal); Investigation (equal); Resources (equal);
Validation (equal); Writing – review & editing (equal). Kewu Bai:
Conceptualization (equal); Formal analysis (equal); Investigation
(equal); Methodology (equal); Supervision (equal); Writing – orig-
inal draft (equal); Writing – review & editing (equal). Dennis
Cheng Cheh Tan: Formal analysis (equal); Investigation (support-
ing); Resources (equal); Supervision (equal); Validation (support-
ing); Writing – review & editing (equal). Yong-Wei Zhang: Con-
ceptualization (lead); Formal analysis (equal); Funding acquisition
(lead); Investigation (equal); Methodology (equal); Project admin-
istration (lead); Resources (equal); Writing – original draft (equal);
Writing – review & editing (equal).

Author Contributions
Yingzhi Zeng: Data curation (lead); Formal analysis (equal); Inves-
tigation (equal); Methodology (equal); Validation (equal); Visual-
ization (equal); Writing – original draft (lead); Writing – review
& editing (equal). Mengren Man: Methodology (equal); Software
(equal); Writing – original draft (equal); Writing – review & edit-
ing (equal). Chee Koon Ng: Formal analysis (equal); Investigation
DATA AVAILABILITY
The data that support the findings of this study are available
from the corresponding author upon reasonable request.
APPENDIX: LIST OF CHEMICAL FORMULAS OF
SINGLE-PHASE FCC REPORTED IN THE LITERATURE

Al mole Reported Citation

No. Formula fraction phase in reference Reference
1 Al0.5 CoCrCuFeNiTi0.2 0.088 FCC 76 Ye (2016)27
2 Al0.3 CoCrFeNi 0.070 FCC 77 Ye (2016)27
3 Al0.5 CrCuFeNi2 0.091 FCC 78 Ye (2016)27
4 CoCrFeNiCuAl0.3 0.057 FCC 2 Yang (2012)28
5 CoCrFeNiCuAl0.5 0.091 FCC 2 Yang (2012)28
6 CoCrFeNiAl0.25 0.059 FCC 18 Yang (2012)28
7 CoCrFeNiAl0.375 0.086 FCC 18 Yang (2012)28
8 Ti0.1 CoCrFeNiAl0.3 0.068 FCC 26 Yang (2012)28
9 Al0.25 CoCrCu0.75 FeNi 0.050 FCC 7 Miracle (2016)29
10 Al0.3 CoCrCuFeNi 0.057 FCC 9 Miracle (2016)29
11 Al0.5 CoCrCu0.5 FeNi 0.100 FCC 2 Miracle (2016)29
12 Al0.5 CoCrCuFeNi 0.091 FCC 9 Miracle (2016)29
13 AlCo3.5 CrCu0.5 FeNi 0.125 FCC 2 Miracle (2016)29
14 Al0.25 CoCrCu0.75 FeNiTi0.5 0.046 FCC 33 Miracle (2016)29
15 Al0.5 CoCrCuFeNiTi0.2 0.088 FCC 15 Miracle (2016)29
16 Al0.5 CoCrCuFeNiV0.2 0.088 FCC 16 Miracle (2016)29
17 Al0.02 CoCrFeMnNi 0.004 FCC 36 Miracle (2016)29
18 Al0.03 CoCrFeMnNi 0.006 FCC 36 Miracle (2016)29
19 Al0.04 CoCrFeMnNi 0.008 FCC 36 Miracle (2016)29
20 Al0.08 CoCrFeMnNi 0.016 FCC 36 Miracle (2016)29
21 Al0.3 CoCrFeMo0.1 Ni 0.068 FCC 38 Miracle (2016)29
22 Al0.1 CoCrFeNi 0.024 FCC 46 Miracle (2016)29
23 Al0.25 CoCrFeNi 0.059 FCC 47 Miracle (2016)29
24 AlLiMg0.5 ScTi1.5 0.200 FCC 118 Miracle (2016)29
25 Al0.25 CoCrFeNi 0.059 FCC 1 Zeng (2021)1

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Al mole Reported Citation

No. Formula fraction phase in reference Reference
26 Al0.3 CoCrFeNi 0.070 FCC 1 Zeng (2021)1
27 Al0.3 CoCrCu0.3 FeNi 0.065 FCC 3 Zeng (2021)1
28 Al0.3 CoCrFeNi 0.070 FCC 3 Zeng (2021)1
29 Al0.5 CoCrFeMo0.3 Ni 0.104 FCC 7 Zeng (2021)1
30 Al0.5 CoCrFeMo0.4 Ni 0.102 FCC 7 Zeng (2021)1
31 Al0.5 CoCrFeMo0.5 Ni 0.100 FCC 7 Zeng (2021)1
32 Al0.3 CoCrFeNi 0.070 FCC 11 Zeng (2021)1
33 FeCoNiCrCuAl0.3 0.057 FCC 34 Ye (2015)30
34 FeCoNiCrCuAl0.5 0.091 FCC 34 Ye (2015)30
35 FeNi2 CrCuAl0.6 0.107 FCC 16 Ye (2015)30
36 Al0.5 CoCrCuFeNiTi0.2 0.088 FCC 35 Ye (2015)30
37 Al0.3 CoCrFeNi 0.070 FCC 36 Ye (2015)30
38 Al0.5 CrCuFeNi2 0.091 FCC 37 Ye (2015)30
39 Al6.0 Mo2.5 Co22.2 Cr25.6 Fe21.0 Ni22.7 0.060 FCC 35 Singh (2014)31
40 Al5.89 Co23.21 Cr24.49 Fe23.82 Ni22.59 0.059 FCC 28 Singh (2014)31
41 Al0.375 CoCrFeNi 0.086 FCC Kao (2009)32
42 Al0.3 CoCrFeNi 0.070 FCC Wang (2014)33
43 Al0.4CoCrNi 0.13 FCC Sun (2022)34

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