REVIEW

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Phase Selection, Lattice Distortions, and Mechanical

Properties in High-Entropy Alloys
Raymond Kwesi Nutor, Qingping Cao, Xiaodong Wang, Dongxian Zhang,
Yunzhang Fang, Yong Zhang, and Jian-Zhong Jiang*

strategy is mainly based on the “solute–

High-entropy alloys (HEAs) composed of multiprincipal elements with near- solvent” principle. However, another alloy
equiatomic ratio have gained numerous attention in recent years. The design design strategy based on multiprincipal
concept and unique microstructure make them exhibit a wide range of attractive elements in the near-equimolar ratio has
recently been developed. In this multiprin-
properties, promoting them suitable for most structural and functional appli-
cipal element system, it is difficult to
cations. HEAs have four core effects: severe lattice distortion, high entropy, distinguish between the solute and the
sluggish diffusion, and cocktail effects, which are all interconnected. Among solvent, and various atoms are supposed
these core effects, severe lattice distortion is seen as the most key factor in to be randomly distributed in the crystal lat-
determining the properties of HEAs. Recent findings prove that phase selection in tices (which has not been confirmed yet).
HEAs cannot be described by the maximized entropy theory alone. As such, the This strategy, proposed by Yeh[1] and
Cantor,[2] was based on the Boltzmann
phase formation principles in terms of single-phase and multiphase formation
hypothesis of the relationship between
criteria are summarized. Severe lattice distortion affecting the mechanical entropy and system complexity. They pro-
properties and polymorphism of HEAs is reviewed. Several strategies, which posed that the increased configurational
have recently been successfully applied in overcoming the “strength–ductility entropy of mixing in alloys with multiple
trade-off” in HEAs, are discussed. Some key unsolved questions concerning the alloying elements in near-equiatomic pro-
lattice distortion in HEAs which could be interesting research topics in the future portions would overcome the enthalpy of
compound formation, stabilizing solid sol-
are suggested.
utions (SS) at the expense of intermetallics
(IMs) during solidification. These multi-
principal element alloys are named “high
1. Introduction entropy alloys” (HEAs), although the exact values of entropy
in HEAs have not been experimentally measured yet.
Increasing demand for improved physical, chemical, and Since then, hundreds of HEAs with different combinations
mechanical properties led to the development of conventional have been developed based on transition metals, refractory
alloys from single elements. These conventional alloys are made metals, and compound forming elements.[2–20] Most of these
by selecting one or two major elements with desired properties, HEAs have been found to possess simple crystal structures such
and other minor components are added to tune the properties to as the face-centered cubic (fcc) Fe–Co–Cr–Mn–Ni HEAs,[2] body-
meet performance specifications. The conventional alloy design centered cubic (bcc) Al–Co–Cr–Fe–Ni HEAs,[18] and the hexago-
nal close-pack (hcp) Ho–Dy–Y–Gd–Tb HEAs[6] when solidified
from the melts. Experimental characterization techniques such
R. K. Nutor, Dr. Q. Cao, Dr. X. Wang, Prof. D. Zhang, Prof. J.-Z. Jiang as X-ray diffraction (XRD), scanning electron microscopy (SEM),
International Center for New-Structured Materials (ICNSM)
State Key Laboratory of Silicon Materials transmission electron microscopy (TEM), differential scanning
School of Materials Science and Engineering calorimetry (DSC), nanoindentation, tensile, wear- and corrosion-
Zhejiang University resistance tests have been used to study the microstructure-
Hangzhou 310027, P. R. China properties correlations of HEAs.[3–50] These studies have revealed
E-mail: jiangjz@zju.edu.cn
that HEAs possess superior properties, such as high hardness
Prof. Y. Fang
Institute of Condensed Matter Physics
and strength,[23–29] superior corrosion and wear resistance,[3,30–35]
Zhejiang Normal University good magnetic properties,[9,36–39,51] structural stability,[7,40,41]
Jinhua 321004, P. R. China attractive mechanical properties at extreme temperature
Prof. Y. Zhang conditions,[21,42–47] and good electronic properties.[48,49] Yeh[50]
State Key Laboratory for Advanced Metals and Materials proposed four core effects of HEAs, namely: 1) high-entropy
University of Science and Technology Beijing effect; 2) sluggish diffusion effect; 3) sever lattice distortion effect;
Beijing 100083, P. R. China
and 4) cocktail effect, in which the lattice distortion might be the
The ORCID identification number(s) for the author(s) of this article key factor affecting the properties of HEAs. Although a complete
can be found under https://doi.org/10.1002/adem.202000466. understanding of lattice distortions in HEAs is still not estab-
DOI: 10.1002/adem.202000466 lished yet, significant progress in HEAs has been made recently.

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Therefore, this work will mainly focus on the lattice distortion
issue of HEAs, besides the phase formation rules.
2. Four Core Effects and Phase Formation Rules
2.1. Four Core Effects
The four core effects as proposed by Yeh[50] were categorized in
terms of thermodynamics, kinetics, structure, and properties.
These four core effects are briefly discussed as follows.
2.1.1. High-Entropy Effect
The high-entropy effect is the basis on which HEAs were
designed. In thermodynamics, the stability of a system is
determined by Gibbs free energy, which is dependent on both
entropic and enthalpic contributions. Gibbs free energy (ΔGss )
of a SS is related to the entropy of mixing ðΔSmix Þ and enthalpy
of mixing ðΔH mix Þ by
ΔGss ¼ ΔH mix TΔSmix (1)
Takeuchi et al.[52] proposed a method of calculating ΔHmix
for atomic pairs based on Miedema’s P scheme. According to
Boltzmann’s hypothesis, ΔSmix ¼ R ci ln ci , where R is the
molar gas constant, ci is the atomic fraction of the ith element.
At the melting point of a metal, the entropic change in fusion is
empirically equal to R.[53] ΔSmix for equimolar alloys with 4, 5, 7,
9, 12, 15, and 20 elements is 1.39R, 1.61R, 1.95R, 2.2R, 2.48R,
2.71R, and 3R respectively, indicating that the configurational
entropy of mixing increases with the number of components.
This high ΔSmix renders the SS of multiprincipal elements
thermodynamically stable due to the significant lowering of
ΔGss.[53] However, recent studies[11,22,26] have shown that
regardless of the high ΔSx , the formation of secondary phases
such as IMs, which are the ordered phases with a lower configu-
rational entropy of mixing, is somewhat inevitable. As such,
several phase formation criteria have been proposed to predict
the stability conditions of various phases. Most of the criteria
are based on the Hume-Rothery rules[54] for the formation of
substitutional binary SS. We will discuss the different phase
formation criteria of HEAs in Section 3.
2.1.2. Sluggish Diffusion Effect
The sluggish diffusion effect is another core effect of HEAs.
Diffusion in HEAs can be pictured to be different as compared
with conventional alloys, as there are a variety of atoms occupying
each lattice site orderly or randomly in HEAs. In the kinetics of
phase transformation, Yeh et al.[1] revealed that the long-range
diffusion for phase separation is very sluggish due to the lack
of a single-element principal matrix in HEAs. This effect allows
for the formation of ultrafine crystallites and even amorphous
phases during solidification, as a result of the lower rates of
nucleation and growth. The higher number of elements
increases the packing density[55] of HEAs, and based on the prin-
ciple of confusion,[56] this should make diffusion more sluggish.
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Tsai et al.[57] reported that the diffusion coefficient in fcc
Fe–Co–Cr–Mn–Ni HEA was smaller compared with pure fcc
metals and the Fe–Cr–Ni(–Si) alloys, due to a larger lattice poten-
tial energy (LPE), which leads to an increased activation energy of
diffusion and thus, a lower diffusion rate. Beke et al.[58] also con-
firmed the sluggish diffusion in HEAs but attributed it to the
correlation effects rather than the enhanced activation energies.
Tsai et al.[59] successfully used the Al–Mo–Nb–Si–Ti–Ta–V–Zr
HEA film as an effective diffusion barrier for copper metalliza-
tion to prevent the copper–silicide formation at temperatures
close to 993 K. The resistance to the interdiffusion of Cu and
Si was also improved from 973 K up to 1073 K by incorporating
Ru into Al–Cr–Ta–Ti–Zr HEA.[60] The Nb–Si–Ta–Ti–Zr HEA
due to its thermal stability comparable with ceramics also served
successfully as a diffusion barrier for copper metallization.[61]
Later on, Tsai et al.[62] developed the first HEA nitrides
(HEAN). This HEAN was developed from the previous octonary
Al–Mo–Nb–Si–Ti–Ta–V–Zr HEA due to the ability of all
eight elements to form strong nitrides. This HEAN film
ðAlMoNbSiTiTaVZrÞ50 N50 prevented the reaction between Cu
and Si in a Cu=ðAlMoNbSiTiTaVZrÞ50 N50 =Si thin-film system at
temperatures close to 1173 K, due to the sluggish diffusion effect
and excellent thermal and structural stabilities of the HEAN.
Chang et al.[63] also developed a quinary (Al–Cr–Ti–Ta–Zr)N
HEAN, which served as an excellent diffusion barrier against
interdiffusion between Cu and Si with the formation of silicates
up to 1173 K, while remaining thermally stable due to its slow
diffusion kinetics and nanocomposite structure. The slow
diffusion kinetics have made HEAs and HEANs an attractive
alternative as diffusion barriers for Cu metallization in the micro-
electronics industry.
In as much as these findings verify the sluggish diffusion
hypotheses, Paul[64] raised several concerns—hinting at possible
errors in diffusion calculations presented by Tsai et al.[57] They
had estimated diffusion coefficients using conventional means
based on a quasibinary approach.[57] In their response, Tsai
et al.[65] pointed out that Paul’s idea[64] behind a similar diffusion
behavior in quasibinary and binary couples being identical was
flawed. They argued that minor nontarget element diffusion
exists in many alloy systems and thus, it is almost impossible
to have a single interdiffusion coefficient. They also claimed that
Paul’s idea stemmed from a forced “normalization” of the diffu-
sion behavior which ignores minor nontarget diffusion, leading
to a wrong diffusion interpretation. The approach used by Tsai
et al.[65] was found to be valid by Dabrowa et al.[66] recently.
However, as they observed a sluggish diffusion response in only
the Mn-prominent HEAs, they argued that the diffusion rate in
HEAs is highly compositional dependent; therefore, the so-called
sluggish diffusion effect cannot be generalized for all HEAs.[66]
As it stands now, sluggish diffusion is still seen as one of the core
effects of HEAs, and we believe further diffusion studies are
needed to deepen our understanding.
2.1.3. Severe Lattice Distortion Effect
Lattice distortion is thought to be severe in HEAs as compared
with conventional alloys, because different elements having dif-
ferent atomic sizes, bond configurations, and lattice potential
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energies might be located on the same lattice matrix randomly.
The degree of lattice distortion is strongly linked with atomic
size, chemical bonding, and electron distribution among compo-
nent elements.[67] Thus, lattice distortions in HEAs are of impor-
tance, ultimately playing a key role in affecting physical and
mechanical properties. Yeh et al.[68] found that under the same
XRD measurement conditions, the diffraction peak intensities of
HEAs were lower than those of the corresponding conventional
alloys like temperature-diffused scattering, due to the deviation
of atoms from their neutral positions. This was attributed to the
severe lattice distortion effect. However, it was later revealed that
the XRD peak intensities decreased further beyond the thermal
effects with increasing number of principal elements, as a result
of an increase in lattice distortion.[69] The uncertainty in atomic
positions in HEAs induces severe lattice distortion, the most
important core effect of HEAs as it directly affects the properties
of HEAs.[50,70] As such, there have been numerous efforts made
to quantify lattice distortion and explain its corresponding effects
on the properties of HEAs. Lattice distortion-quantifying
methods, which have been made so far, and the correlation of
lattice distortions and mechanical properties of HEAs will be
discussed in detail in Section 4.
2.1.4. Cocktail Effect
The “near-equiatomic concentrations of component elements”
design basis of HEAs make them unique, and a synergetic effect
of the component elements brings about the attractive properties
HEAs possess. Also, the cocktail effect can be described as a
combination of the high entropy, sluggish diffusion, and severe
lattice distortion core effects in defining and affecting the overall
properties of HEAs. For example, low-density HEAs are
designed based on low-density elements[22,71] and refractory
HEAs (RHEAs) are designed based on high-melting-point
elements.[72,73] Studies have shown that these RHEAs possess
intriguing oxidation resistance combined with their high-
temperature mechanical properties—as most commercial alloys
with refractory metals suffer from oxidation. Among them,
NbCrMo0.5 Ta0.5 TiZr was found to possess good combination oxi-
dation resistance and mechanical properties, which makes them
potentially better than commercial Nb alloys.[74] Gorr et al.[75]
studied a series of equimolar RHEAs and found that Ta–Mo–
Cr–Ti–Al exhibited a superior oxidation resistance at tempera-
tures above 1000  C due to the formation of a thin and compact
Al-rich layer which followed the parabolic rate law for oxide
growth. The observed oxidation resistance exhibited by this
RHEA was found to be comparable with Ni-based superalloys.[76]
Very recently, Waseem and Ryu[77] developed the novel
Al10 CrNbTiZr10 RHEAs with a high oxidation resistance which
was attributed to CrNbO4 , Al2 O3 , and AlTiO5 oxides, rendering it
a potential candidate for high-temperature applications. Another
interesting property of RHEAs is their biocompatibility.[78] Todai
et al.[79] developed the novel equiatomic Ti–Nb–Ta–Zr–Mo
RHEAs and conducted cell culture experiments for biocompati-
bility analyses. They observed dense osteoblasts (help in bone
matrix formation) with widespread morphology on the surfaces
of the as-cast and annealed TiNbTaZrMo, similar to the morphol-
ogy of the cells on commercially pure (CP) Ti, suggesting
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analogous biocompatibility between novel RHEAs and CP Ti.
Since then, several biocompatibility studies of RHEAs[79–85] have
been reported, which is beyond the scope of our Review.
In designing HEAs, unusual elements and microstructure com-
binations can be made as long as the chosen elements meet the
phase formation requirements.[86] Therefore, a wide range of
attractive results can be achieved. This makes the design flexibil-
ity of HEAs outstanding.
2.2. Phase Formation Rules
In the design of HEAs, it is always nice to predict possible phases
and microstructures before conducting experiments. Although
the earliest HEAs were designed generally based on a high
entropy of mixing, advances in research methods have led to
other design criteria to predict the stability of SS formed.
Several phase formation rules have been proposed using thermo-
dynamic approaches and structural parameters, most of which
are based on the classic and extended Hume-Rothery SS forma-
tion rules.[54]
2.2.1. Classic Hume-Rothery Rules
The Hume-Rothery rules, which were proposed mainly for
conventional alloy systems containing solute and solvent atoms,
are dependent on atomic-size difference, mixing enthalpy,
electronegativity difference, and valence electron concentration
difference.[54,87] Similarities in any of these parameters favor
the formation of simple SS. As for HEAs, where solute and
solvent atoms are not easily distinguishable, these parameters
still play an important role in predicting phase formations.
Zhang et al.,[88] using the Hume-Rothery perspectives, estab-
lished the correlation of the mixing enthalpy and entropy with
the atomic-size difference of HEAs.
n
X
ΔHmix ¼ 4ΔH mix
ij c i c j (2)
i¼1,i6¼j
where ΔH mix is the mixing enthalpy of a SS in HEAs, ΔHmix ij is
the enthalpy of mixing of binary liquid alloys, and ci and cj are the
atomic percentages of the ith and jth alloy components, respec-
tively. The atomic-size difference in HEAs is determined as
vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
u N
uX
δ¼t c i ð1 r i =r̄Þ2 (3)
i¼1
where N is the number of components in a multicomponent
alloy system, r i is the atomic radius of each element, and r̄ ¼
n c r is the average atomic size. The correlation between
P
i¼1 i i
the mixing enthalpy (ΔHmix ), the mixing entropy (ΔSmix ), and
the atomic-size difference (δ) as found by Zhang et al.[88] is
shown in Figure 1a. It was found that in the formation of simple
SS phases in HEAs, a small δ, a slightly positive or negative
ΔHmix , and a high ΔSmix are most favorable, whereas a large
δ, a more negative ΔHmix , and a relatively lower ΔSmix favor
the formation of amorphous and intermediate phases.[88]
Although this confirmed the notion that a higher ΔSmix favored
the formation of simple SS, Guo et al.[89] initially argued that the
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vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
u N
uX
Δχ ¼ t ci ðχ i χ̄Þ2 (4)
i¼1

where
Pχ i is the Pauling electronegativity of the ith element and
χ̄ ¼ ni¼1 c i χ i is the average electronegativity difference of
component elements calculated by the rule of mixtures. The
valance electron concentration (VEC) is also defined as
n
X
VEC ¼ ci ðVECÞi (5)
i¼1

where ðVECÞi is the valence electron concentration of the ith

element. Most of the simple SS HEAs possess bcc or fcc
structures,[2,18,24,27,43] with a few of the rare-earth elements
(Sc, Sm, Gd, Tb, Dy, To, Er) based ones forming the hcp
structure.[6,91] Guo et al.[92] found that VEC was an important
factor in determining the stability of fcc or bcc SS. A VEC ≥ 8
stabilized the fcc phase, a VEC < 6.87 stabilized the bcc phase,
and a multiphase was stabilized at 6.87 ≤ VEC < 8.[92] The sum-
Figure 1. a) A correlation between ΔSmix , ΔHmix , and δ for HEAs and mary of their findings is shown in Figure 2. The VEC can also be
BMGs.[88] b) Effects of ΔSmix , ΔHmix , and δ on the phase stability in used to predict the formation of the hcp phase, i.e., a VEC ≤ 3
equiatomic HEAs and both equiatomic and nonequiatomic BMGs. favored the stability of the hcp phase.[93] Quite recently, Takeuchi
Data obtained from a previous study.[89]
et al.[94] suggested 7.5 ≤ VEC ≤ 8.4 to be included in the phase
selection criteria of hcp-structured HEAs. However, this criterion
work by Zhang et al.[88] was inconclusive as their comparison is valid for hcp-structured HEAs comprising 4d and 5d transition
was between equiatomic HEAs and only nonequiatomic bulk metals solidified from a melt. Also, the VEC has been used suc-
metallic glasses (BMGs). Thus, Guo et al.[89] compared the cessfully to predict the existence of sigma phase (σ), which is an
enthalpic, entropic, and atomic-size difference effects in IM phase frequently observed in aged HEAs.[95] The range of
equiatomic HEAs and both equiatomic and nonequiatomic stability of the σ phase was found to be 6.88 < VEC < 7.84.
BMGs, as shown in Figure 1b. Figure 1 shows that to form Apart from predicting the crystal structure of HEAs, the VEC also
simple SS phases, 0 ≤ δ ≤ 8.5, 11 ≤ ΔSmix ≤ 19.5 J Kmol 1 predicts the ductility or brittleness of RHEAs, which are mostly
and 22 ≤ ΔHmix ≤ 7 J Kmol 1 whereas the amorphous phase- bcc structured.[96] Ductile RHEAs have a VEC ≤ 4.4, whereas
stability region lies within δ ≥ 8.5, 7 ≤ ΔSmix ≤ 14 J Kmol 1 and brittle RHEAs have a VEC ≥ 4.6.[96]
35 ≤ ΔHmix ≤ 8.5 J Kmol 1 . Electronegativity is the ability of atoms to attract electrons to
These findings confirmed that in the selection of elements itself, as such, a low electronegativity mismatch ðΔχÞ is suitable
for HEA design, δ plays a critical role in determining the stability
of a SS or amorphous phase. As such, elements much closer to
each other on the periodic table with δ < 4 are recommended in
HEA design. ΔHmix also plays an important role in phase stabil-
ity, with a more negative mixing enthalpy favoring the stability of
the amorphous phase. However, competition is found between
amorphous phase stability and IM compound stability at inter-
mediate conditions in terms of ΔHmix , with the product between
temperature and mixing entropy ðT · ΔSmix Þ being the deter-
mining factor.[90] As the design basis of HEAs, the highest
ΔSmix values lead to the stability of simple SS. However, this high
ΔSmix does not always favor the formation of random SSs, as IM
compounds could also form. This has over the years cast doubts
on the HEA design strategy by just increasing the number of
component elements to increase the tendency of achieving
single-phase SS.[13]
The other parameters which Hume-Rothery considered in
phase formation are the valence and electronegativity differences
of the solute and solvent atoms.[54,87] The role of these two
parameters in the phase selection of HEAs was also studied
in recent years. The electronegativity difference in HEAs is Figure 2. Relationship between VEC and the crystalline structures. Data
defined as obtained from previous studies.[92,93]

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for different elements to attract electrons uniformly in a lattice to
attain a stable SS, whereas a large electronegativity mismatch,
coupled with a large atomic-size mismatch and a very negative
mixing enthalpy, favors the formation of the amorphous
structure.[97] Topologically close-packed (TCP) phases are often
observed in HEAs as secondary phases or IM compounds with
complex structures; as such, TCP phases fall within the VEC
multiphase range of 6.87 ≤ VEC < 8. TCP phases, such as σ
phase, μ phase, R phase, and Laves phase, affect the properties
of HEAs significantly. Dong et al.[98] suggested a correlation
between Δχ and the TCP phase stability, as shown in
Figure 3. Δχ < 0.117 favors the formation of single SS phases,
whereas the range 0.1176 < Δχ < 0.133 is mostly a combination
of SS and TCP phases.[98] Δχ > 0.133 favors the stability of
TCP phases except for some HEAs with high Al content.[98]
2.2.2. Extended Hume-Rothery Rules
In this section, we will discuss other phase formation design
parameters, which have been developed over the years using
thermodynamic and structural approaches and correlate with
the Hume–Rothery rules.[97,99–108] These parameters aim to
obtain more precise and concise phase formation rules for
HEAs and also possibly minimize the need to refer to multiple
parameters simultaneously.
The Ω Design: Ω is a thermodynamic parameter proposed by
Yang et al.,[99] defined as a ratio of the product of the mixing
entropy and the melting temperature to the absolute value of
mixing enthalpy of HEAs.
T m ΔSmix
Ω¼
jHmix j
The melting temperature T m is calculated by the rule of
mixtures as
Figure 3. Effects of electronegativity mismatch ðΔχÞon TCP phase stability
of HEAs. Data obtained from a previous study.[98]
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n
X
Tm ¼ ci ðT m Þi (7)
i¼1
where ðT m Þi is the melting temperature of the ith element. Ω
is taking into consideration both entropic and enthalpic effects.
As entropic effects increase with temperature, it was proposed
that T · ΔSmix could be used to evaluate the driving force for
SS formation.[99] However, as crystalline phase formation gener-
ally occurs close to the melting temperature, T m was adopted for
the entropy term. Therefore, Yang et al.[99] gave a Ω–δ phase
formation criterion, as shown in Figure 4. Because Ω takes into
consideration both entropic and enthalpic effects, if Ω ≥ 1, it
means that the entropic effects exceed the enthalpic effects for
the SS formation and if Ω < 1, the enthalpic contributions over-
come the entropic contributions.[99] As previously discussed in
Section 2.2.1, it is also seen from Figure 4 that a small δ favors
the stability of SS phases, whereas a large δ favors the stability of
amorphous phases. In the formation of entropy-stabilized SS
phases, Ω ≥ 1.1 and δ ≤ 6.6% are the required criteria for
HEAs. A more detailed plot revealing the combined effects of
enthalpy–entropy competition is shown in Figure 4b. This is
an improved phase formation criterion as compared with the
ΔSmix –ΔHmix –δ relationships, as shown in Figure 1, as the
proposed thermodynamic parameter, Ω, considers both enthalpy
and entropy effects.
The ϕ Design: ϕ, proposed by Ye et al.,[102] takes into account
the enthalpy of formation and the excessive ΔSmix arising from
dense atomic packing and atomic-size mismatch. The total con-
figurational entropy of mixing of an alloy is ST ¼ Sc þ SE , where
Sc is the configurational mixing entropy of an ideal gas and SE is
the excess mixing entropy.[100] The early equiatomic concept
(6)
behind attaining a maximized entropy in HEAs assumed that
Figure 4. Phase stability selection criterion based on a) Ω versus δ and
b) Ω versus δ versus ΔHmix in metallic materials. Data obtained from
previous studies.[99,101]
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the alloy atoms had an indistinguishable size and were loosely
packed like an ideal gas in which attaining a maximized entropy
is elemental position dependent.[102] Of course, as alloy constit-
uent elements have different sizes, this assumption has evolved
over the years and the equiatomic HEA restriction has since then
been relaxed. Even more so, the equiatomic fraction does not
guarantee a maximized entropy. The single dimensionless ther-
modynamic design parameter ϕ is expressed as
Sc SH
ϕ¼
jSE j
where SH ¼ jHmix j=T m is defined as the complementary entropy
derived from the enthalpy jHmix j. The ϕ phase selection criterion
in Figure 5 reveals two main phase zones, with a critical value of
ϕc ¼ 20 separating the single-phase HEAs from the multiphase
HEAs even at different Sc values.[102] This ϕ parameter is a better
phase selection criterion as compared with the Hume-Rothery
mixing entropy (ΔSmix ) criterion due to its effectiveness in dis-
tinguishing single-phase HEAs from multiphase HEAs, which
can be viewed as an entropy indicator for alloy selection.[102]
The ∧ Design: This ∧ parameter combines a thermodynamic
approach coupled with geometrical information (lattice configu-
ration plus atomic radius) and is defined as
ΔSmix
∧¼
δ2
The basis of this parameter was the idea that an increase in
ΔSmix and a low δ stabilize single-phase SS. In a perfect lattice,
δ could be seen as a measure of strain; as such, δ2 can be con-
ceived as a measure of strain energy.[103] It was, however, found
that single-phase HEAs were stabilized when ∧ > 0.96, multi-
phase SS stabilized when 0.24 < ∧ < 0.96, and mixtures of IM
compounds formed when ∧ < 0.24.[103] Singh et al.[103] suggested
that the ∧ phase selection criterion was better than the previous
Figure 5. Sc versus ϕ for the phase stability zones of HEAs. Data obtained
from a previous study.[102]
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ΔH mix , VEC, Δχ and the Ω δ phase selection criteria due to the
ability of a single value of ∧ to predict the formation of SS and
IM compounds formed in HEAs. However, two limitations for
the ∧ design were found: 1) to predict the crystal structures of the
SS, ∧ has to be used in conjunction with VEC and 2) the disso-
ciation of single-phase SS into two or more phases cannot be
solely determined by ∧.
The γ Design: The γ parameter was put forward by Wang
et al.,[104] who considered the atomic-size effect based on atomic
packing behavior. Due to the complicated nature of atomic
(8)
packing in HEAs, the solid angles of atomic packing for the
largest- and smallest-sized elements were chosen to describe
the atomic packing effect.[104] γ describes the atomic packing
instability and is defined as the ratio between the solid angles
of the smallest and largest atoms, as shown in Figure 6a,b.
ωS
γ¼ (10)
ωL
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi ffi
ðr s þr̄Þ2 r̄ 2
where ωS ¼ 1 ðr s þr̄Þ2
is the solid angle of the smallest atom,
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
2
ðr l þr̄Þ r̄ 2
ωL ¼ 1 ðr þr̄Þ2
is the solid angle of the largest atom,
l
r s and r l are the radii of the smallest and largest atoms, respec-
tively, and r̄ is the mean atomic radius. The phase selection cri-
teria between γ and δ in Figure 6c shows that SS phases are stable
when γ < 1.175, whereas IMs and metallic glasses are stable
(9) when γ > 1.175.[104] It was also found that HEAs could satisfy
the δ < 0.06 SS criterion but still have various atomic packing
parameters γ. Thus, the authors suggested that the atomic pack-
ing parameter (γ) is a more efficient phase selection parameter as
compared with the atomic-size mismatch parameter δ.[104]
The μ Design: In another thermodynamic approach, μ was
derived like the Ω parameter. μ is defined as the ratio of the melt-
ing point from the entropy and enthalpy contributions to the
critical temperature above which an alloy is stable P as a single
x ΔH i fusion
homogeneous phase,[105] i.e., μ ¼ TTSC
m
, where T m ¼ Pi xi ΔSfusion ,
i i i
ΔH fusion
i and ΔSfusion
i are the enthalpy and entropy of fusion of
the ith element, x i is the atomic ratio of the ith element, and T SC
is the critical point above which a single phase can exist. In the μ
design, it was seen that when μ > 1.5, SS phases and multiphase
alloys could be formed. However, in an attempt to determine the
fcc or bcc crystal structures formed, the μ design failed.
2.2.3. Lattice Strain Perspectives
The lattice structure in HEAs is inherently strained, as already
explained in previous sections by the lattice distortion core effect.
Some new parameters have been developed to assist in the
classification of multicomponent HEAs. In this section, we will
summarize some of the phase selection parameters which have
been proposed in HEAs, based on lattice strain.
sm and K m Design: Interatomic spacing mismatch, sm , was
developed from the interatomic spacing matrix, Sd , a parameter
proposed by Moreen et al.[106] to represent the mean interatomic
spacing between element i and j in a SS to quantify lattice dis-
tortion. Using a computational approach 1) The force applied
between elements i and j by their interaction and 2) the force
applied by the surrounding atoms of the lattice on these two
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Figure 6. Sketch of the atomic packing around an atom via a solid angle: a) around the largest atom; b) around the smallest atom; and c) relationship
between atomic packing parameter γ and atomic size mismatch δ. Adapted with permission.[104] Copyright 2014, Elsevier Ltd.

atoms were considered in the sm design.[97] The interatomic spac-

ing mismatch is defined as
n
n X sdij 
X  

sm ¼ x i x j 1  (11)
i j
s 
lat

where sdij is the mean interatomic distance between atoms i and j,

slat ¼ alat f , alat is the mean unit cell parameter, and f is the
atomic packing factor. sm δ was plotted in Figure 7a, whereas
sm and δ are comparable parameters having a similar order of
magnitude. The sm phase stability rule showed that SS phases
are formed at sm < 1% whereas BMGs are formed at
sm > 1%.[97] However, the alloys with 0.75 < sm < 1% possess
combinations of SS, IM, and amorphous phases.[97] sm was also
found to be in agreement well with the previous thermodynamic
and physical parameters such as μ, Ω, Δχ, and ΔHmix .
Like sm , the bulk modulus mismatch K m was developed from
the balance of force approach, as stated in the previous section.
It is worth mentioning that both sm and K m account for the vari-
ation of forces across the lattice of HEAs.[97] K m , defined as the
moduli distribution across a lattice, is expressed as Figure 7. a) Interatomic spacing mismatch versus atomic spacing
mismatch phase selection criteria in metallic materials and b) K m versus
X n
n X 
 K dij 
 sm phase stability diagram in metallic materials. Data obtained from a
Km ¼ x i x j 1  (12) previous study.[97]
i j
K  lat

where K dij is the mean bulk modulus of the HEA and K lat is the positions and elastic interactions is shown in Figure 7b. In this
bulk modulus of the lattice. Since sm and K m were developed phase selection criterion, SS phases are formed when sm < 1 and
simultaneously, the combined behavior of distortions in atomic K m < 8, whereas amorphous phases are formed when sm > 1

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Figure 8. The RMS residual strain versus elastic energy for phase selection
in metallic materials. Data obtained from a previous study.[107]
and K m > 8. K m , as a standalone parameter, was found to be able
to predict the stability of different crystal structures similar to the
Hume-Rothery VEC phase selection criteria.[92–94] The fcc HEAs
have a K m < 4 whereas bcc HEAs have 4 < K m < 8.
The Intrinsic Residual Strain Design: Ye et al.[107] developed a
geometric model which enabled them to calculate intrinsic
residual strain to predict phase stability in HEAs, based on
the average lattice constant, packing density, atomic size, and
atomic fraction. In their approach, a relationship between the
elastic energy stored in HEAs and the root mean square
(RMS) residual strain (εRMS ), which measures the degree of fluc-
tuation in the intrinsic residual strains from the mean value to
serve as the driving force for phase transition, was established
based on Lindemann’s criterion.[107,108] As shown in Figure 8,
an increase in elastic energy causes a large RMS residual strain,
which favors a multiphase structure or amorphous phase.
Figure 8 shows that a single-phase SS HEA would be formed
if εRMS < 0.05, a multiphase SS HEA if 0.05 < εRMS < 0.1,
and an amorphous phase HEA if εRMS > 0.1.
3. Lattice Distortion in HEAs
In Section 2, we discussed the core effects in HEAs and found
that the severe lattice distortion effect is probably the most
important one, which has been successfully used as a basis of
phase selection in HEAs. The roles of the severe lattice distor-
tions in various physical metallurgies in HEAs are suggested
in Figure 9. The role of lattice distortion in the mechanical prop-
erties of HEAs will be mainly focused on in this section.
3.1. Quantifying Lattice Distortion
To quantify lattice distortion in HEAs, the local atomic arrange-
ments should be first understood. By visualizing the atomic
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Figure 9. The relationship between physical metallurgy and the severe
lattice distortion effect in HEAs.
arrangements, their relative positions, coordination number,
and whether there exists short-range order (SRO) or disorder,
the degree of distortion in a material can be effectively revealed.
Although high-resolution TEM can be used to illustrate the
existence of local lattice distortion (LLD), it is still important
to quantify the average effect using physical parameters.
Average atomic local packing information is good for quantifying
the lattice distortion effect in HEAs, which have recently been
done. X-ray absorption spectroscopy (XAS) which includes of
extended X-ray absorption fine structure (EXAFS) and X-ray
near-edge spectroscopy (XANES) techniques can provide infor-
mation regarding the local structure around each elemental
species and thus, can provide information about the degree of
distortion in an alloy.[109] In X-ray spectroscopy, when the
X-ray exceeds the ionization energy of an electron in a shell,
the electron is ejected when the X-ray beam and atom interact.
EXAFS uses this theory by measuring the intensity change
before and after an X-ray beam interacts with a sample.[110]
In a comprehensive study by Cheng et al.,[67] EXAFS, which
reveals information about the local atomic configuration, was
used to examine the origin of lattice distortion in fcc
FeCoNiCrMn HEA. The degree of distortion in the HEA was
quantified from the Fourier transform of the EXAFS K-edge
spectra shown in Figure 10c as the deviation in peak positions
of the component elements of the HEA from Ni position in pure
fcc Ni, as shown in Table 1. Both positive and negative deviations
in peak positions are indicative of average lattice sites being dis-
torted as each atom has an offset from the lattice site of pure Ni.
Atomic-size mismatch generates lattice distortion in HEAs.
From a geometric viewpoint of single-phase SS, the large-sized
atoms push atoms around them away, whereas small-sized
atoms attract atoms around them. Zhao et al.[111] described
the lattice distortion in Ni-based fcc-structured HEA using the
atomic-size mismatch parameter, by defining the linear distor-
tion as α ¼ ðaHEA aNi Þ=aNi , where aHEA is the lattice constant
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Figure 10. a) The sketch of the random occupation of atoms with different atomic sizes in HEAs; b) the referenced ideal lattice for comparison,
¯ c) Fourier transforms of the EXAFS K-edge spectra of Ni, Co, Fe, Cr, and Mn
dotted circles represent the virtual atoms with average atomic size r;
in FeCoCrMnNi HEA compared with pure Ni. Adapted with permission.[67,112] Copyright 2017, 2015, Elsevier Ltd.

Table 1. Peak positions for Ni, Co, Fe, Cr, and Mn in FeCoNiCrMn alloy, and their deviations from Ni positions in percentage.[67]

Element Ni Co Cr Mn Fe

First peak 2.178 2.209 (þ1.4%) 2.178 (0%) 2.178 (0%) 2.178 (0%)
Third peak 4.111 4.080 ( 0.8%) 4.080 ( 0.8%) 4.142 (þ0.8%) 4.080 ( 0.8%)
Fourth peak 4.786 4.755 ( 0.7%) 4.755 ( 0.7%) 4.786 (0%) 4.817 (þ0.7%)

of the HEA and aNi is the lattice constant of pure fcc Ni. In this
method, it is assumed that pure fcc Ni is occupied with only Ni
atoms and by adding other atoms, some of the Ni atoms are
effectively substituted by other atoms, thus altering the bond
length. This method can only be envisioned in single-phase
HEAs and is far from ideal (i.e., either over- or under-estimated)
by assuming a uniform distortion. Based on the atomic-size
P c c jr þ r 2r̄j
mismatch, α2 ¼ nj≥1 i j i 2r̄ j , which is an optimal parameter
proposed by Wang et al.,[112] which effectively quantifies the
jr þ r 2r̄j
lattice distortion effect. i 2r̄j is the dimensionless displace-
ment between atomic pairs ci and cj of the ith and jth element
and their counterpart pairs. α2 was ideally developed by compar-
ing a multicomponent distorted lattice with an ideal counterpart,
as shown in Figure 10a,b. We believe this parameter presents a
better visualization of lattice distortion in HEAs as the interac-
tions between atomic pairs c i and cj and neighboring atoms
are considered.
The pair distribution function (PDF) technique uses informa-
tion obtained from synchrotron XRD and neutron diffraction
sources via Fourier transformation of both Bragg peaks and
diffuse scattering to reveal local atomic structure information
with high accuracy.[113] Using the PDF and the fluctuations in
LLDs in the Ni80 Pd20 binary alloy and the equiatomic
FeCoNiCrPd HEA, Tong et al.[114] quantitatively characterized
the mean LLD. The measured PDFs and their fits obtained from
the ideal fcc structure are shown in Figure 11a,b. The PDF
results revealed the existence of strongly localized LLD distrib-
uted over a long distance due to a large size mismatch, with
profound deviation in the FeCoNiCrPd HEA indicating a high
LLD as compared with NiPd alloy. These results were then used
to quantify the LLD as ε ¼ ða1st aavg Þ=aavg , where a1st is the
lattice parameter obtained from fitting the first peak of PDF
and aavg from the overall spectrum fitting. ε was found to be
0.79% for the FeCoNiCrPd HEA and 0.41% for the NiPd binary
alloy, suggesting a synergetic effect of chemical complexity on

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Figure 11. Experimentally observed PDFs and their fits based on the ideal fcc structures for a) Ni80 Pd20 and b) FeCoNiCrPd HEA. Two fitting approaches
were used. Upper panel: lattice constant as a free parameter. Lower panel: lattice constant predetermined by fitting only the first peak of PDF and then
fixed for the subsequent whole spectrum fitting. Adapted with permission.[114] Copyright 2018, Elsevier Ltd. Deviation of local lattice constant, a1st , from
the average lattice constant, aavg , for c) Ni powder sample and d) FeCoNiCrPd HEA. In the upper panels, the measured PDFs were fitted over the whole r
range, whereas in the lower panels, the first PDF peak was fitted to obtain a1st and then the fitting was extended to the whole r range but with lattice
constant parameter fixed as a1st . Adapted with permission.[116] Copyright 2018, Elsevier Ltd.

LLD in HEAs. Tong et al.[115] quantified the lattice distortion
in NiCoCr, FeCoNiCr, and FeCoNiCrMn alloys based on
the PDFs obtained from synchrotron XRD and found ε in
NiCoCr ¼ 0.23%, FeCoNiCr ¼ 0.04%, and FeCoNiCrMn ¼ 0.24%.
These results also indicate that LLD does not simply depend on
chemical complexity in HEAs alone. It could have different ori-
gins, e.g., the size mismatch effect in FeCoNiCrMn alloy and
chemical SRO involving Ni–Cr and Co–Cr pairs in the
NiCoCr alloy. In another approach based on the PDF technique,
the mean LLD was effectively quantified in fcc-structured
FeCoNiCr, FeCoNiCrMn, and FeCoNiCrPd HEAs before and
after ion irradiation.[116] In the study, stripe samples of 150 μm
in thickness were irradiated with multiple energies of Ni ions
to 0.1, 0.3, and 1 dpa fluences by a raster ion beam to ensure
homogeneous irradiation. It was found that before irradiation
ε varied as FeCoNiCr < FeCoNiCrMn < FeCoNiCrPd, and the
variations in LLD extracted from the PDF peaks in Figure 11c,
LLD, as shown in Figure 12. In the three studied alloys, it was
found that with increasing radiation dose, the lattice constant
ðaavg Þ initially increases rapidly before reaching a steady state,
as shown in Figure 12a. However, in Figure 12b, ε exhibits a relax-
ation phenomenon in FeCoNiCr and FeCoNiCrMn at the initial
radiation stages before increasing at the later stage whereas
FeCoNiCrPd monotonically increases with radiation dose. The
initially large LLD in the pristine FeCoNiCrPd (0.74%) prevents
the relaxation behavior in FeCoNiCr and FeCoNiCrMn at the ini-
tial stages of radiation. This trend was attributed to a large atomic
size misfit induced from the large bond distance between Pd–Pd
pairs and the Pd atoms providing a strong Fleischer-type pinning
on dislocations.[116]
In the atomic structure modeling using the maximum entropy
principle which states that every particle strives for the maximum
free space in the system by Wang,[117] lattice distortions were
qffiffiffiffiffiffiffiffiffiffiffiffi
2

d revealed that the FeCoNiCrPd HEA possessed the largest measured by a lattice distortion parameter g ¼ d̄d2 1, where

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Figure 12. Ion irradiation effect on a) the lattice constant of the average
structure and b) the lattice distortion in the first atomic shell extracted
from the PDF fitting in ther range from 1.5 to 3 Å, covering only the first
atomic shell. Data obtained from a previous study.[116]
d is the lattice geometrical parameter of the structure which could
either be the interplanar spacing or the lattice constant and d̄ and
d2 are the mean and mean square values of the lattice geometrical
parameters, respectively.[118] The lattice distortions in the alloys
were as follows: fcc FeCoNiCrMn (0.0070) < fcc FoNiCr (0.0085)
< bcc AlCoCrCuFeNi (0.0150) < bcc AlCoCrFeNi (0.0210), sug-
gesting that the lattice distortions in bcc structures are of a larger
magnitude compared with fcc structures.[9,117] Feng et al.[119]
quantified the lattice distortion, Λ, as the RMS average of the
pffiffiffiffiffiffiffiffiffiffiffi
atomic displacements u from the ideal sites (Λ ¼ hjuji2 ) in
RHEAs (RHEAs). The lattice distortion at absolute zero temper-
ature was attributed to atomic-size effects. Wang et al.[120] studied
the impact of the atomic-scale lattice distortion on dislocation
activity in HEAs using molecular dynamics simulations. It
was reported that the magnitude of lattice distortion can be quan-
tified by the atomic-scale Mises strain ðεMises Þ which causes a
variation in dislocation dissociation width and introduces energy
barriers against dislocation motion, thus, acting as an effective
strengthening mechanism. The LLDs in RHEAs and 3d transi-
tion HEAs were studied by He et al.[121] by proposing a supercell
model with a similar local atomic environment combined with
ab initio calculations. It is revealed that the LLD is more signifi-
cant in RHEAs than in 3d transition HEAs, suggesting the
significance of lattice distortion in RHEAs with less-packed
bcc structures which have an atomic packing factor of 0.68, com-
pared with both closely packed fcc and hcp structures having an
atomic packing factor of 0.74. In addition, the atomic packing
density and the bonding strength are known to affect the lattice
structure. Tsai and Yeh[122] characterized typical phases in HEAs
based on the hardness range, as shown in Table 2. These
attempts offer a means to explain some deformation and
strengthening mechanisms and corresponding properties in
HEAs, which will be discussed in the following section.
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Table 2. Phases in HEAs as categorized by hardness. Data obtained from
a previous study.[122]
Type Examples Typical
hardness [HV]
Valence compounds Carbides, borides, 1000–4000
silicides
IM phases with nonsimple structures σ, Laves, η 650–1300
BCC and derivatives BCC, B2, Heusler 300–700
FCC and derivatives FCC, L12, L10 100–300
3.2. Influence of Lattice Distortion on Mechanical Properties
One of the main reasons why HEAs have gained significant
attention is their prospect as structural engineering alloys which
can operate at extreme conditions (elevated temperature and
cryogenic applications), with a good combination of strength
and ductility. These properties are dependent on the composition
and microstructure of these alloys, which are ultimately deter-
mined by the grain and twin boundaries, dislocation, and the
atomic-scale strain distribution. Figure 9 shows that lattice dis-
tortion as a core effect is related to the deformation theories and
strengthening mechanisms in HEAs. In this section, recent
studies of the correlation of lattice distortion with mechanical
properties of HEAs will be summarized. Judging by the notion
that lattice distortion is significant in less-packed structures com-
pared with densely packed structures, one should expect higher
strength and hardness values in the less-packed structures. This
should lead to questions like: 1) are deformation mechanisms
highly dependent on the degree of lattice distortions and 2) does
the precipitation of IMs in HEAs always suggest an enhanced
lattice distortion? As previously mentioned, the lattice distortion
effect is dependent on the crystal structure of the HEA; therefore,
we will discuss the impact of lattice distortion on fcc-, bcc-, and
hcp-structured HEAs, separately.
3.2.1. fcc HEAs
Although the phase formation rules play a role in HEA design,
there is still a freedom of choice with regard to the component
elements. For instance, the quaternary equiatomic FeCoNiCr
HEA is fcc structured and when Mn is added to make it a
quinary equiatomic FeCoNiCrMn, it remains fcc-structured
HEA, whereas Al addition makes it a bcc-structured quinary
AlCoCrFeNi HEA. Now, let us first look at the role of lattice
distortion playing in fcc-structured HEAs. The widely studied
fcc FeCoNiCrMn HEA, named as Cantor alloy, was found by
Gludovatz et al.[21] to be a fracture-resistant HEA with the
potential for cryogenic applications. The strength and ductility
of the single-phase fcc FeCoNiCrMn HEA increase with decreas-
ing temperature to 77 K with a fracture toughness up to
200 MPaΔm0.5 , as shown in Figure 13a. This behavior was attrib-
uted to a transition from a planar-slip dislocation activity at
ambient temperature to nanotwinning-dominated deformation
as the temperature decreased, resulting in continuous steady
strain hardening. The mechanical nanotwinning and continuous
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Figure 13. Temperature-dependent mechanical behavior of a) FeCoNiCrMn[21]
and b) FeCoNiCr HEAs. Adapted with permission.[21,124] Copyright 2018,
Science China Press and Springer-Verlag GmbH Germany, part of Springer
Nature.
strain hardening occur as a result of increased energy of the
distorted fcc lattice which decreases the stacking fault energy
(SFE).[13,21,44,123] In a very recent study,[124] the fcc-structured
FeCoNiCr HEA was found to possess a good combination of
tensile strength (1250 MPa) and ductility (62%) at liquid helium
temperatures (4.2 K) shown in Figure 13b. The excellent
mechanical properties of this alloy at extremely low temperatures
were attributed to a profuse formation of twins triggered by
the low SFE. The observed serration behavior (defined as the
visible stress and strain drops or zig zagging) was attributed
to a joint action between hcp plates and high-density deformation
twins. An investigation by Zhang et al.[125] using in situ TEM
revealed a synergetic combination of multiple deformation
mechanisms including easy motion of Shockley partials, their
interactions to form stacking-fault parallelepipeds, and arrest
at planar slip bands of undissociated dislocations to be the
origin of the exceptional combination between tensile strength
(1 GPa) and ductility (60–70%) of the fcc FeCoNiCrMn
HEA. The high fracture toughness was due to the delay in crack
propagation by twinned, nanoscale bridges that form between
the near-tip crack faces. Schuh et al.[126] also found that upon
subjecting the Cantor alloy to severe plastic deformation through
high-pressure torsion (HPT), a highly distorted fcc nanocrystal-
line structure is obtained with an enhanced tensile strength of
about 1950 MPa and a hardness of 520 HV. In addition, Qin
et al.[127] investigated the effect of Mo addition on the mechanical
properties of FeCoNiCrMn HEA. The single-phase fcc structure
was maintained up to 4 at% Mo content, above which sigma
phases were formed. Increasing Mo content up to 16 at%
enhanced the compressive yield strength from 216 to
765 MPa, as shown in Figure 14. The ductility decreases from
50% to 19% with increasing Mo content and the alloy exhibits
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Figure 14. Relationships between yield strength and volume fraction of
sigma phase with Mo content in the ðFeCoNiCrMnÞ100 x Mox HEA.
Data obtained from a previous study.[127]
the best combined compressive properties when Mo ¼ 11 at%,
with the yield strength, fracture strength, and fracture strain
as 547 MPa, 2762 MPa, and 44% respectively. This was attributed
to the SS strengthening effect via the enhanced lattice distortion,
and the sigma-phase precipitation strengthening effect.
Wu et al.[128] showed that grain refinement was induced by
HPT in the equiatomic fcc FeCoNiCr HEA via a four-stage con-
tinuous deformation process with increasing strain as follows:
1) formation of nanobands (NBs) and deformation twins at
strain ¼  0 0.25, 2) NB–NB, NB–twin, and twin–twin interac-
tions at strain ¼  0.25 0.3, 3) grain refinement by NB
interaction and formation of stacking faults (SFs) and nanotwins
at strain ¼  3 4, and 4) attaining equilibrium microstructure
at ε ¼ 4 6.5. Figure 15 shows the schematic diagram of
the grain refinement process and TEM images of the nanocrys-
talline grains containing SFs and nanotwins. Induced lattice
distortion from twin–twin interactions refines the grains
from 25 μm in the as-cast sample to 68 nm at the end of
the fourth deformation stage. This suggests an additional contri-
bution from grain-size strengthening to the enhanced mechani-
cal property of the fcc FeCoNiCr HEA. In an attempt to provide
insight into the deformation mechanisms in HEAs, Hu
et al.[129] studied the dislocation avalanche phenomenon in
slowly compressed fcc Al0.1 CoCrFeNi nanopillars, using direct
electron imaging and precise mechanical measurements.
Dislocation activities were monitored by quantifying the
dislocation line contrast in recorded images using a line
detection algorithm. An inhomogeneous strain field and
low-angle boundaries with nanometer-sized local clusters were
observed. Lattice distortion increased the lattice friction
stress against the motion of a dislocation line, with low-angle
grain boundaries also acting as strong dislocation barriers.
This together with a low SFE retards dislocation mobility,
results in dislocation pile-ups in front of dislocation bands,
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Figure 15. a–e) Schematic diagram of the HPT-induced grain refinement process f ) TEM image of the fcc FeCoNiCr HEA with nanocrystalline grains
containing SFs and nanotwins; g) HRTEM image of nanocrystalline grains in (f ). Redrawn from Ref. [128]
and thus, triggers an avalanche in the nanopillars, as shown
in Figure 16.
Fu et al.[130] fabricated an fcc-structured bulk nanocrystalline
Co25 Ni25 Fe25 Al7.5 Cu17.5 HEA by mechanical alloying followed
by spark plasma sintering. The nanostructured fcc HEA with
the severe lattice distortion effect enhances its yield strength
and hardness by 834.9% and 251.9%, respectively, as compared
with its as-cast coarse-grained counterpart. The main strengthen-
ing mechanisms in this nanocrystalline HEA were attributed to
both grain boundary and dislocation strengthening. The nano-
crystalline HEA was found to possess a low SFE, as such a high
dislocation density is seen as shown in TEM images in
Figure 17a,b. The mechanical properties of the bulk nanocrystal-
line and coarse-grained Co25 Ni25 Fe25 Al7.5 Cu17.5 HEAs with other
HEAs are shown in Figure 17c,d. Li et al.[131] studied the mechan-
ical behavior of the single-phase fcc Al0.3 CoCrFeNi HEA at low
and high strain rates. At high strain rates, the lattice distortion
effect reduces the SFE, thus inducing profuse mechanical
twins. This combined with SS hardening and dislocation hard-
ening leads to enhanced mechanical properties at high strain
rates. The high resistance to shear localization at high strain rates
of the fccAl0.3 CoCrFeNi HEA makes it a potential candidate for
ballistic applications.[131] In the senary fcc CoCrFeCuNiAl0.5 ,
Xu et al.[132] examined the atomic structure by combining scan-
ning transmission electron microscopy (STEM) and atom probe
tomography (APT). They found that Al induced nanoscale phase
separation between Cu-rich fcc domains and FeCrCoNi-rich
L12 -ordered phase, which was suggested to minimize lattice
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distortion, subsequently reducing the SS strengthening effects
in the fcc CoCrFeCuNiAl0.5 HEA.
It is worth mentioning that the fcc FeCoNiCrMn HEA also
shows an improvement in mechanical properties at high strain
rates and exhibits a serration behavior attributed to thermal soft-
ening and a collapse of grains in the deformation zone.[133]
Serration in materials originates from three possible sources:
1) martensitic transformation; 2) deformation twinning; and
3) dynamic strain aging (DSA) where there are interactions
between solute atoms and dislocation.[134] The strain rates and
deformation temperatures are also known factors that affect
the serration response of alloy systems. Serration is promi-
nent in Al-containing HEAs, e.g., CoCrFeNiAl0.5 ,[135]
CoCrFeCuNiAl0.5 , [136,137] and CoCrFeNiAl0.3 ,[138] originating
from DSA.[135-138] The DSA phenomenon is likely triggered
via interactions between the Al atoms and moving dislocations
in the distorted lattice of HEAs, resulting in enhanced frictional
stress on the dislocations.
3.2.2. bcc HEAs
Zhou et al.[139] observed an fcc-to-bcc phase transition in
the CoCrFeNiAlx Cu1 x HEA with increasing Al content. This
phase transformation was induced by an increase in lattice
distortion upon addition of the larger atomic-sized Al, which also
results in an enhancement of strength but a reduction in ductil-
ity, as shown in Figure 18a. A similar fcc-to-bcc transition
was also observed for the Ti0.5 CrFeCoNiAlx Cu1 x HEA by
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Figure 16. In situ nanomechanical measurement and TEM observation of slip avalanches in Al0.1 CoCrFeNi HEA a) show the measured stress–time curve
with color-coded deformation stages (I, II, and III). b–d) Two captured images at each stage, one is before and one is after a nanopillar slip. The images
are labeled from 1 to 6, and their recording time is labeled below the image. Regions of the images are highlighted by red and white arrows to mark the
dislocation band and the dislocation pileup. e) SEM image of the deformed nanopillar, which confirms the large crystal slips. 1–2 and 3–4 are two different
images between the images of 1 and 2, 3, and 4, respectively; they are displayed in color. The color bar marks a different intensity level in counts.
The design of the nanopillar compression experiment. f ) The nanopillar compression experiment as conducted in a TEM. The electron image of
the nanopillar and the stress (τ)–strain (γ) curve are simultaneously recorded as functions of time. g) BF image of an as-prepared HEA nanopillar,
on which the in situ TEM experiment was conducted (scale bar is 500 nm). The image contrast indicates a relatively uniform starting dislocation micro-
structure. h) Schematic of the nanopillar orientation and the activated slip system, ð11̄1Þ½011Š with a Frank–Read source under compression. Redrawn
from Ref. [129]

Wang et al.,[140] as shown in Figure 18b. Consequently, the bcc-
structured HEAs lost ductility and enhanced the strength.[139,140]
This is in agreement with He et al.[121] suggesting that lattice
distortion is larger in bcc-structured HEAs as compared with
fcc-structured HEAs. Next, we will discuss primarily the role
of lattice distortion in bcc-structured HEAs. Similar to the
CoCrFeNiAlx Cu1 x HEA, alloying with Al in the Alx CoCrFeNi
system leads to an fcc-to-bcc phase transition.[141–147] It is
found that the Alð0 0.5Þ CoCrFeNi HEAs are fcc structured,
Alð0.6 0.9Þ CoCrFeNi are fcc þ bcc structured, and
Alð1.0 3.0Þ CoCrFeNi are bcc structured.[141–147] Increasing Al
content enhances the lattice distortion effect and bond strength
between larger-sized Al and other elements, which leads to an
increase in the hardness of Alx CoCrFeNi with increasing Al
content, as shown in Figure 18c.
Qiao et al.[148] studied the mechanical and microstructural
characteristics of the equiatomic bcc AlCoCrFeNi HEA at
ambient and cryogenic temperatures. The yield and fracture
strengths increased by 29.7% and 19.9%, respectively, at cryo-
genic temperature as compared with ambient temperature.
These results are linked with the lattice distortion, which, most
likely, increases the energy barriers for dislocation motion. There
was a transition from an intergranular fracture mode at 298 K to
a transgranular fracture mode at 77 K. Dong et al.[149] found that
the bcc structure of AlCoCrFeNi was mainly maintained upon
alloying with V, even though a ferromagnetic-to-paramagnetic
transition was induced. Fe–Cr and Al–Ni segregation effects
were reduced, signifying an enhancement in lattice distortion
resulting in a high compressive strength of 3.29 GPa and a plastic
strain of 26.8% for AlCoCrFeNiV0.2 Chen et al.[150] observed two

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Figure 17. a) Dislocations in the 49 h-milled Co25 Ni25 Fe25 Al7.5 Cu17.5 HEA powders, b) dislocations in the bulk nanocrystalline Co25 Ni25 Fe25 Al7.5 Cu17.5 ,
arrows indicate dislocations, c) representative engineering stress–strain curves of the bulk nanocrystalline (nc) and CG Co25 Ni25 Fe25 Al7.5 Cu17.5 samples
after spark plasma sintering and casting in compression, respectively. d) compressive yield strength versus strain for the bulk nanocrystalline
Co25 Ni25 Fe25 Al7.5 Cu17.5 HEA in comparison with those of fcc-structured HEAs in the literature. #1 and #2 represent the bulk nanocrystalline
and CG Co25 Ni25 Fe25 Al7.5 Cu17.5 , respectively; #3–#9 correspond to as-cast CG Co20 Ni20 Fe20 Cr20 Cu20 , Co18.2 Ni18.2 Fe18.2 Cr18.2 Ti9.0 Cu18.2 ,
Co18.2 Ni18.2 Fe18.2 Cr18.2 Al9.0 Cu18.2 , Co25 Ni25 Fe25 Cr25 , Co23.25 Ni23.25 Fe23.25 Cr23.25 Mo7.0 , Co23.25 Ni23.25 Fe23.25 Cr23.25 Ti7.0 , and Co29.41 Ni29.41 Fe29.42 Al5.88 Si5.88 ,
respectively. #2, #3, #5, and #9 alloys were not fractured during compression tests. Adapted with permission.[130] Copyright 2016, Elsevier Ltd.

types of microstructures upon alloying AlCoCrFeNi with Zr:
1) a periodic structure of ordered bcc phase and a bcc SS phase
and 2) a mixture of ordered bcc phase and Laves phase, which
significantly affect the mechanical properties. AlCoCrFeNiZr0.008
was found to exhibit the best mechanical properties, possessing a
yield strength of 1560 MPa, fracture strength of 3510 MPa, and
plastic strain of 29.5%, which increase by 240 MPa, 843 MPa, and
7% as compared with the AlCoCrFeNi alloy, respectively.
The significant improvement in mechanical properties exhibited
by AlCoCrFeNiV0.2 and AlCoCrFeNiZr0.008 was attributed to
the fine nanoscale spinodal decomposition within the bcc
matrix.[149,150] Zhu et al.[151] studied the effects of Mo addition
on the microstructure and compressive properties of
AlCoCrFeNiMox HEAs. When Mo ¼ 0, 0.1, the alloy possessed
a single-phase bcc structure which transformed to a lamellar
eutectic structure with Mo ¼ 0.2–0.5. On the one hand, the yield
strength increased from 1051 to 2757 MPa with increasing
Mo content as a result of an increase in lattice distortion energy,
as the Mo atom occupied the lattice sites, enhancing the SS
strengthening effect. On the other hand, the ductility decreased
from 9.1% to 2.5% with increasing Mo due to the limited num-
ber of slip systems in the lamellar structure as compared with the
bcc structure. The back-scattering images of the AlCoCrFeNiZrx
and AlCoCrFeNiMox HEAs are shown in Figure 19. Zhu
et al.[152] found that the AlCoCrFeNiSix HEA is mainly bcc
structured, with a precipitation of a nanoscale cellular structure
when Si > 0.4. The precipitation of this nanoscale cellular struc-
ture in the bcc matrix makes AlCoCrFeNiSi0.4 possess excellent
comprehensive mechanical properties i.e., yield strength of
1481 MPa, fracture strength of 2444 MPa, and plastic strain of
13.4%. Alloying with Si increases the lattice distortion energy,
thus, enhancing SS strengthening effects while decreasing
ductility. The precipitation of the nanoscale cellular structure
at the grain boundary results in a transition from ductile to brittle
fracture. However, the mechanical properties of AlCoCrFeNi
rapidly deteriorated upon alloying with C due to an inhomoge-
neous distribution of graphite and ε phase, rendering
AlCoCrFeNiCx very brittle.[153] Zhou et al.[154,155] studied the
microstructure and mechanical properties of AlCoCrFeNiTix
alloy. This alloy series is composed mainly of a bcc phase that

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Figure 18. a) Compressive true stress–strain curves of as-cast CoCrFeNiAlx Cu1 x (x ¼ 0, 0.25, 0.5, 0.75, and 1), i.e., SCA1, SCA2, SCA3, SCA4, and SCA5
alloy samples. Adapted with permission.[139] 2008, American Insitute of Physics. b) Compressive test results for the Ti0.5 CrFeCoNiAlx Cu1 x (x ¼ 0–1)
HEAs. Adapted with permission.[140] Copyright 2008, Elsevier B.V. c) Lattice constant and hardness of the Alx CoCrFeNi alloys as functions of Al content.
Symbol (▴) and symbol (▪) denote lattice constants of fcc and bcc phases, respectively. Symbol ( ) denotes hardness. Adapted with permission.[146]
•
Copyright 2012, Elsevier Ltd.

possesses excellent room-temperature mechanical properties
with AlCoCrFeNiTi0.5 exhibiting the highest yield strength
(2.26 GPa), plastic strain (23.3%), and fracture strength
(3.14 GPa). The presence of Al and Ti with large atomic radii
compared with the other elements occupying the lattice sites
enhances the lattice distortion effects by increasing the lattice dis-
tortion energy and enhancing SS strengthening. The mechanical
properties of the AlCoCrFeNiMox , AlCoCrFeNiSix , AlCoCrFeNiCx ,
and AlCoCrFeNiTix HEAs are shown in Figure 20.
RHEAs are a class of HEAs that are based on several refractory
elements and are mostly bcc structured. The Nb25 Ti25 Zr25 Hf 25
RHEA studied by Wu et al.[41] and was found to be structurally
stable by maintaining its single-phase bcc phase even after
homogenization at 1573 K for 6 h. The alloy possessed yield
strength, ultimate tensile strength, elastic, and plastic deforma-
tion values of about 879 MPa, 969 MPa, 0.9%, and 14.9%, respec-
tively, and also a relatively higher fracture strength, as shown in
Figure 21. This was attributed to a strong bonding of the refrac-
tory elements combined with a large lattice distortion effect in
the bcc structure enhancing the dislocation strengthening
effect. Further studies by Wu et al.[156] on the Al alloying effect
on the microstructure and mechanical properties of the
Alx ðNbTiZrHf Þ100 x HEA revealed that below 7% Al content,
the bcc structure was maintained, whereas an Al–Zr-rich hexag-
onal phase was precipitated above 7% Al content upon aging at
873 K, as shown in Figure 22a–f. The overall mechanical prop-
erties of Alx ðNbTiZrHf Þ100 x are attractive due to SS strengthen-
ing and the lattice distortion effect upon Al addition. However,
the work-hardening effect and ductility are reduced upon the
precipitation of the Al–Zr rich secondary phase, as shown in
Figure 22g–h. Another ductile bcc-structured RHEA is the equia-
tomic NbTaTiV alloy, as studied by Lee et al.[157] This NbTaTiV
RHEA was found to possess a severely distorted lattice over a
long range, which was further optimized upon homogenization,
leading to an improvement in mechanical properties at ambient
and high temperatures. The optimization in lattice distortion via
homogenization was attributed to the reduction in chemical
segregation effects, confirmed by first-principle calculations.
It is also worth mentioning that ductile NbTaTiV RHEA was suc-
cessfully prepared via powder metallurgy,[26] and upon alloying
with Al, it still maintains a single-phase bcc structure possessing
about >50% compressive ductility.[158]
Similar to the situations in conventional alloys, hot-, cold-
working, and heat-treatment processes can be used to further
improve the mechanical properties in HEAs. Soni et al.[159] devel-
oped a method for improving the ductility of brittle RHEAs by

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Figure 19. a–k) Back-scattering images of as-cast AlCoCrFeNiZrx and l–q) AlCoCrFeNiMox HEAs showing the transition from single bcc structure to a
lamellar eutectic structure. Adapted from previous studies. Adapted with permission.[150,151] Copyright 2016, 2010, Elsevier Ltd., Elsevier B.V.

microstructure modification. The Al0.5 NbTa0.8 Ti1.5 V0.2 Zr RHEA
was subjected to three treatment conditions: 1) Cast þ hot
isostatically pressed þ homogenized at 1200  C for 24 h þ slow
cooling (10  C min 1), 2) Condition 1 þ solutionized at 1400  C
for 20 min þ water quenching, and 3) Condition 2 þ annealed
at 600  C for 120 h þ water quenched. Figure 23 shows the
room-temperature yield strength as follows: Condition 2
(1065 MPa) < Condition 3 (1345 MPa) < Condition 1 (2032 MPa)
and the high-temperature yield strength also as follows:
Condition 2 (975 MPa) < Condition 3 (1423 MPa) < Condition 1
(1774 MPa). The room-temperature compressive ductility is as
follows: Condition 1 (3.5%) < Condition 3 (16.9%) < Condition 2
(38%), whereas the high-temperature compressive ductility is also
as follows: Condition 1 (2.8%) < Condition 3 (16.2%) < Condition 2
(63%). Thus, the sample subjected to Condition 3 treatment
exhibits a good balance between ductility and yield strength both
at room temperature and at 600  C. These results were attributed
to the microstructural transformation from a B2 (ordered) matrix
with bcc precipitates in Condition 1 to a disordered continuous
bcc matrix with a higher fraction of coarse B2 precipitates, as
shown in Figure 23. The inversion from an ordered B2 matrix
to a rather disordered bcc matrix can be used to reduce the chemi-
cal segregation effect, which was suggested to enhance lattice dis-
tortion. This combined with the precipitation strengthening effect
of the B2 phase in Condition 3 gives a good balance between the
yield strength and ductility at room and elevated temperatures.
Senkov et al.[45] studied the mechanical properties of the
bcc-structured Nb25 Ta25 Mo25 W25 and V20 Nb20 Ta20 Mo20 W20
RHEAs. The room-temperature and high-temperature yield
strengths of these two alloys were found to compare favorably
with those of the “Inconel 718”[160] and “Haynes 230”[161] super-
alloys, as shown in Figure 24g. The attractive mechanical prop-
erties and phase stability were attributed to the severe lattice
distortion effect combined with high configurational entropy,
which retards the diffusion of the constituent elements for grain
boundary sliding accommodation. Zou et al.[72] studied the
size dependence of plasticity for the Nb25 Ta25 Mo25 W25 RHEA.
The RHEA pillar samples reached a high tensile strength value
of about 4.5 GPa, independent on size, which originated from
increased lattice friction caused by LLD at atomic length scales
observed by high-resolution TEM images, as shown in
Figure 24a–f.

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Figure 20. Compressive stress–strain curves of as-cast a) AlCoCrFeNiMox (x ¼ 0, 0.1, 0.2, 0.3, 0.4, and 0.5) HEAs. Adapted with permission.[151]
Copyright 2010, Elsevier B.V. b) AlCoCrFeNiSix (x ¼ 0, 0.2, 0.4, 0.6, 0.8, and 1.0) HEAs. Adapted with permission.[152] Copyright 2010, Elsevier B.V.
c) AlCoCrFeNiCx (x ¼ 0, 0.1, 0.2, 0.3, 0.4, 0.5, 1, 1.5) HEAs. Adapted with permission.[153] Copyright 2011, Elsevier B.V. d) AlCoCrFeNiTix
(x ¼ 0, 0.5, 1, 1.5) HEAs. Adapted with permission.[154] Copyright 2007, American Institute of Physics.

Dirras et al.[162] investigated the microstructure evolution of
plastically deformed bcc Ti20 Zr20 Hf 20 Nb20 Ta20 by XRD and
TEM. The grain size was found to decrease whereas the disloca-
tion density increased during compression. The screw character
of the dislocations became stronger with increasing strain, as
shown by TEM images in Figure 25, and the yield strength
(890 MPa) of this alloy was found to be dependent on the dislo-
cation density and the lattice friction stress which correlates
linearly with lattice distortion.[111,162] In the extensive investiga-
tions of the microstructure and mechanical properties of the bcc
Hf 20 Nb20 Ta20 Ti20 Zr20 HEA,[28,46,163–165] it was found that even
after hot-isostatic pressing and annealing at 1473 K, the alloy
maintains its bcc structure. It possessed a high yield strength
and good ductility at room temperature. The alloy also exhibited
good high-temperature properties with a yield strength of about
92 MPa at 1473 K. The good mechanical properties of the bcc
Hf 20 Nb20 Ta20 Ti20 Zr20 HEA were attributed to its fully distorted
lattice, dislocation-patterned nanostructure, deformation twin-
ning, and recrystallization effects at room and high tempera-
tures, respectively, as shown in the SEM images in Figure 26.
Lin et al.[166] studied Al alloying effect on the refractory
Alx HfNbTaTiZr HEAs. The alloy maintained its dominant bcc
structure with increasing Al content, until the equiatomic senary
AlHfNbTaTiZr where minor precipitation of the Al–Hf–Zr rich
phase was observed. Al addition enhanced the strength but
reduced ductility due to a large solution hardening as a result
of the increase in lattice distortion. Juan et al.[167] found that
alloying HfNbTaTiZr with Mo improved the strength and hard-
ness by increasing the lattice distortion energy while maintaining
its bcc structure. For the HfMo0.75 NbTaTiZr RHEA, a yield
strength of 1373 MPa, Young’s modulus of 109 GPa, and a frac-
ture strain >50% were seen.
The effects of structural disorder on the mechanical properties
of equiatomic TaNbHfZr HEA after annealing at 2073 K up to
8 days were investigated by Maiti et al.[168] The alloy is mainly
composed of a single-phase bcc structure even after annealing
for 8 days. However, a short-range clustering (SRC) of Hf and Zr
enriched takes place perpendicular to the principal <110> axes
with increasing annealing time. The nature of this SRC was stud-
ied using HRTEM, as shown in Figure 27a–f. They suggested
the presence of a local structural disorder, due to asymmetric dif-
fuse intensities around the Bragg reflections in selected-area

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Figure 21. TEM BF images and the corresponding selected-area diffraction pattern of a) as-cast and b) tensile-tested Nb25 Ti25 Zr25 Hf 25 alloy.
c) Tensile true stress–strain curve of Nb25 Ti25 Zr25 Hf 25 alloy and d) SEM high-magnification image of the fracture surface. Adapted with permission.[41]
Copyright 2014, Elsevier B.V.
diffraction pattern (SAED) and the contrasts in the bright-field
(BF) images. The mechanical properties of the TaNbHfZr
HEA under different annealing conditions were also studied
in Figure 27g. The high hardness and strength exhibited by this
alloy in the as-cast condition were attributed to LLD and SS
strengthening effects while the further increase in strength
was explained by the minimization of local energy by the
SRCs. This is because the SRCs become highly interconnected
upon annealing and act as energy barriers against dislocation
motion upon deformation. The decrease in yield strength and
improvement in ductility after annealing for 4 days and above
were attributed to the clustering of Hf and Zr in the SRCs which
lead to the precipitation of a β phase which subsequently lowers
the internal stresses of the matrix.
3.2.3. hcp HEAs and Others
In single-phase hcp-structured HEAs, Zhao et al.[93] found that
the lattice distortion effect had an insignificant effect on the
mechanical properties of the hcp GdHoLaTbY HEA, by studying
the mechanical properties of the component elements and com-
paring them. The GdHoLaTbY HEA possessed a compressive
yield strength, fracture strength, and plastic strain of 108 MPa,
880 MPa, and 21.8%, respectively, obeying the rule of mixtures,
as shown in Figure 28a, and indicating the minor hardening
effect from high entropy and lattice strain.
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Apart from the single-phase fcc and bcc SS, other complex IM
phases are sometimes formed which can lead to deterioration in
mechanical properties. A typical example is a study by Zhuang
et al.[169] on the effects of elemental interaction on the micro-
structure and mechanical properties of FeCoNiCuAlX HEAs.
These HEAs exhibit typical dendrite microstructures of fcc
and bcc SS, which remain unchanged upon the addition of Si,
Ti, and Cr, but Zr and Nd alloying induce the formation of
IM compounds. The formation of IM proved to be detrimental
to the mechanical properties of these HEAs by inducing a
ductile-to-brittle transition, as shown in Figure 28b. These results
were explained in terms of the lattice distortion energy and the
SS strengthening mechanisms.
The severe lattice distortion effect plays an important role in
strengthening HEAs but it also leads to a significant loss in
ductility. As such, applications of single-phase HEAs could be
limited; therefore, a good balance in the lattice distortion effect
is necessary. This led to the proposal of eutectic high-entropy
alloys (EHEAs) by Lu et al.[42,170,171] Their concept was based
on the eutectic conventional alloy design. This EHEA concept
has gained significant attention in recent years,[172–181] with
some of the EHEAs possessing attractive mechanical properties
due to their carefully designed microstructures. Lu et al.[170]
found the eutectic AlCoCrFeNi2.1 to exhibit a good combination
of strength and ductility over a wide temperature range as
compared withits hypoeutectic AlCoCrFeNi2.0 and hypereutectic
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Figure 22. Backscattering SEM micrographs for Alx ðNbTiZrHf Þ100 x HEA SS treated at 1273 K followed by aging at 873 K specimens with different
Al concentrations. a) A-0, b) A-3, c) A-5, d) A-7, e) A-10, and f ) A-12, and the inset shows an enlarged image of the corresponding rectangle area.
Tensile true stress–strain curves of Alx ðNbTiZrHf Þ100 x HEAs subjected to g) SS treatment at 1273 K for 0.5 h and h) SS treatment at 1273 K for
0.5 h þ aging at 873 K for 100 h. Adapted with permission.[156] Copyright 2018, Elsevier B.V.

AlCoCrFeNi2.2 counterparts. The microstructure and mechanical
behaviors of AlCoCrFeNix alloys are shown in Figure 29.
The AlCoCrFeNix alloys exhibit the similar yield and fracture
strength of 545 and 1100 MPa, respectively, at room
temperature. At 70  C, AlCoCrFeNi2.1 exhibits a yield strength,
ductility, and fracture strength of 595 MPa, 15.8%, and
1168 MPa, respectively, compared with 580 MPa/10.5%/
1034 MPa and 570 MPa/18%/1143 MPa for AlCoCrFeNi2.0
and AlCoCrFeNi2.2 , respectively. At 196  C, all three alloys
exhibit an increase in yield strength (700 MPa), whereas
ductility decreases to 4%, 7%, and 9% for AlCoCrFeNi2.0 ,
AlCoCrFeNi2.1 , and AlCoCrFeNi2.2 , respectively. The relatively
high-strength and high-ductility combination of the
AlCoCrFeNi2.1 EHEAs was found by Gao et al.[172] to originate
from back stresses generated as a result of coupling between
the ductile fcc L12 phase and the brittle bcc B2 phase.
Yin et al.[174] found that Fe45 Ni25 Cr5 Mo25 EHEA combined a
hard trigonal μ phase with the relatively ductile lamellar eutectic
structure, achieving a high compressive strength of 1661 MPa
and a ductility of 17%. Fe20 Co20 Ni41 Al19 EHEA studied by Jin
et al.[175] exhibits a room-temperature tensile strength of
1103 MPa and a ductility of 18.7% due to its nano-lamellar eutec-
tic microstructure of B2 and L12 phase. He et al.[177] designed a
series of CoCrFeNiNbx EHEAs with a fine lamellar structure of
fcc and Laves phases, with CoCrFeNiNb0.25 possessing a com-
pressive fracture strength of 2024.6 MPa and a fracture strain
of 38.8%. In a similar manner, Huo et al.[179,180] developed
EHEAs with Laves and fcc phases by alloying the single-phase
fcc-structured CoCrFeNi with Ta and Zr, of which
CoCrFeNiTa0.3 showed a 2.5 GPa compressive strength and a
44% fracture strain whereas the fracture mode of the
CoCrFeNiZrx alloy series was converted from an the initial brittle
translamellar fracture at room temperature to a ductile fracture at
elevated temperatures. Ai et al.[181] found CoCrFeNiTa0.43 EHEA
to be composed of the fcc-structured and the hcp-structured
C14-type Laves phase, exhibiting a high strength of 2377 MPa
and a plastic strain of 17.5%. These results indicate that
EHEAs simultaneously possess high strength and plasticity,
which make them suitable candidates in overcoming the long-
standing “strength–toughness conflict.”[182] This dilemma
observed in most materials is further discussed in terms of
HEAs in Section 4. Finally, Komarasamy et al.[183] proposed a

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Figure 23. Mechanical behavior of Al0.5 NbTa0.8 Ti1.5 V0.2 Zr HEA at a) room temperature and c) 600  C after subjection to three heat-treatment processes.
b) TEM dark-field image showing the continuous channels of an ordered B2 phase (bright) and cuboidal precipitates of a disordered bcc phase (dark)
(<100> bcc SADP shown as inset) after Condition 1 and d) dark-field TEM image taken from a B2 superlattice spot in <001> bcc zone axis after
Condition 3 treatment. Redrawn from previous study.[159]

framework on enhancing the strength of HEAs by selecting
elements with large differences in atomic size and modulus to
optimize the lattice distortion effect and decrease the SFE of
these alloys, as shown in Figure 30.
In summary of this section, lattice distortion as a core effect
plays a major role in affecting the mechanical properties of
HEAs. Lattice distortion is of a large magnitude in bcc-structured
HEAs as compared with fcc-structured HEAs; as such, fcc-
structured HEAs exhibit low strength and high plasticity,
whereas bcc-structured HEAs exhibit high strength and low
plasticity.[184] Table S1, Supporting Information, shows a
summary of the mechanical properties of some HEAs which
have been studied so far. The lattice distortion effect combines
with other deformation mechanisms such as nano-twinning,
which makes the fracture toughness of the fcc-structured
FeCoNiCrMn HEA one of the highest of any existing material
till date. Therefore, a good combination in the understanding
of the deformation and strengthening mechanisms and quanti-
fying lattice distortion in HEAs is important. As such, even
though efforts are being made[185–194] in studying these
mechanisms, future work in terms of quantifying lattice
distortion will be useful to elucidate the outstanding properties
of HEAs.
3.3. Role of Lattice Distortion in Polymorphism in HEAs
Polymorphism in materials science is the ability of a material to
exist in more than one crystal structure with identical composi-
tion. Polymorphism has over the years been seen to be triggered
under different temperatures and pressure conditions and has
been observed in pure elements[195–198] and conventional
alloys.[199–201] As such, polymorphic studies have played a key
role in establishing the structure–property relationship in
materials science. Thus, it is important to study polymorphism
in HEAs, in an attempt to understand the phase stability of
these alloys. Although some of these HEAs exhibit excellent
structural stability under extreme conditions of temperature and
pressure,[7,40,41,156] polymorphic phase transitions have already
been observed.[8,202–209] As such, we will look at how lattice dis-
tortion induces or affects polymorphic transitions in this section.

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Figure 24. HRTEM images of Nb25 Ta25 Mo25 W25 homogenized at 1800  C for 7 days: a) a BF TEM image oriented in [100] zone axis and the correspond-
ing SAED, b) an inverse FFT image of area (a), c,e) enlarged images of the indicated boxes in (b), d,f ) lattice fringes which are traced for (c) and (f ),
respectively, to indicate the regions with lattice distortions. g) Temperature-dependent yield strength of bcc RHEAs and conventional superalloys.
Adapted with permission.[45,72] Copyright 2011, 2013, Elsevier Ltd.

The FeCoNiCrMn Cantor HEA was found to exhibit a
martensitic fcc-to-hcp polymorphic transition with pressure
>14 GPa at ambient or low temperatures.[8,202–204] The high
pressure increases lattice distortion in the alloy and as
FeCoNiCrMn possesses a low SFE,[210–212] with the energy dif-
ference between fcc and hcp phases being small, it induces a
transition from the ductile fcc-to-hard hcp phase. Although this
transition was initially thought to be irreversible, Yu et al.[205]
found a way to reverse this process, by compressing the sample
at 1073 K at 20 GPa. Figure 31a–b shows the fcc-to-hcp phase
transition of the FeCoNiCrMn HEA. In a similar manner,
Zhang et al.[206] observed a pressure-induced fcc-to-hcp transi-
tion in the equiatomic FeCoNiCr and FeCoNiCrPd HEAs, which
began at 13.5 GPa for FeCoNiCr and 74 GPa for FeCoNiCrPd.
The pressure acts as a driving force, combined with the lattice
strains and defects, resulting in the nucleation of the hcp phase.
In the senary CoCrCuFeNiPr HEA, Ma et al.[213] detected a
pressure-induced disordered fcc-to-ordered fcc phase transition
between 7.8 and 16 GPa, which was attributed to the presence of
local SRO structures. Cheng et al.[207] studied the pressure-
induced phase transition in the bcc-structured AlCoCrFeNi
HEA using in situ synchrotron radiation XRD. It is found that
under compression from ambient pressure to 40 GPa and
decompression back to ambient pressure, there is a transition
from the ordered B2 phase to a high-pressure-unknown disor-
dered phase above 17.6 GPa. This transition was confirmed by
TEM to be accompanied by an increase in the lattice distortion
effect. Wang et al.[208] found that the Al0.6 CoCrFeNi HEA exhib-
ited abundant polymorphic transitions under different pressure
and temperature conditions. A total of five polymorphs of the
Al0.6 CoCrFeNi HEA were found, which were explained using
the severe lattice distortion effect, as shown in Figure 31c.
The bcc-structured Hf 25 Nb25 Ti25 Zr25 RHEA exhibits exceptional
structural stability from ambient temperature and pressure to
1262 K and 80 GPa.[40]
In hcp-structured HEAs, the ReRuCoFe HEA was found by
Ahmad et al.[40] to maintain its hcp structure up to pressures
of about 80 GPa. However, the hcp-structured HoDyYGdTb
HEA displays a pressure-induced sequential polymorphic transi-
tion, as revealed by Yu et al.[209] The transformation proceeds
from the conventional hcp structure to a samarium type at
4.4 GPa, a double-hcp structure at 26.7 GPa, and then finally a
distorted fcc structure at 40.2 GPa. The transformation was
correlated with the s ! d electron charge transfer of the HEA.
The similarity in atomic packing of the fcc and hcp structures
makes the fcc-to-hcp phase transition a common one; however,
the core effects of HEAs render the kinetic barrier for this
transition very high. As such, polymorphism in HEAs is thus
induced under relatively extreme conditions of pressure and
temperature. These findings of the polymorphic transitions in
fcc-, bcc-, and hcp-structured HEAs reveal that these entropy-
stabilized SS alloys are somewhat “metastable.”[214]

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Figure 25. TEM micrographs showing the dislocations patterning in Ti20 Zr20 Hf 20 Nb20 Ta20 after compression test at room temperature for different
plastic strains: a) εp ¼ 1%; b) εp ¼ 3%; c) εp ¼ 10% d) Engineering stress versus engineering strain (red color) and true stress versus true strain (blue
color) plots of the as-processed HEA during room-temperature compression. Adapted with permission.[162] Copyright 2015, Elsevier Inc.

Figure 26. a) SEM backscattered images of the longitudinal cross section of TaZrHfNbTi alloy after 50% compression strain at 873 K showing a shear
band with a sharp crack, b) microstructure of a weakly deformed region showing deformation twins initiated from a grain boundary and ending inside the
grain, as well as microcracks at the grain boundary, c) SEM backscattered images from a longitudinal cross section of TaZrHfNbTi sheet after 65% cold
reduction showing heavily deformed grains and d) deformation bands inside the grains. Adapted with permission.[46,163] Copyright 2012, 2015, Springer
Science þ Business Media, LLC, Elsevier B.V.

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Figure 27. HRTEM images of TaNbHfZr annealed at 2073 K for 1 day a) TEM BF image along the [100] zone axis. SAED pattern in the inset shows an
asymmetric nature of streak-like diffuse scattering intensities indicated by small red arrows. b) BF HRTEM image revealing lattice fringes and LLDs at the
SRCs. The two boxed regions are enlarged in (c) and (e), showing a detailed view of local lattice relaxations/distortions due to SRCs. d,f ) the FFTs of (c)
and (e), respectively, revealing the directions of asymmetric diffuse scatterings perpendicular to the two different sets of SRCs. g) Engineering
stress–strain curves under compression for the different HEAs. Adapted with permission.[168] Copyright 2016, Elsevier Ltd.

4. Overcoming the “Strength–Ductility Trade-Off”
The increased strength of structural materials is usually
accompanied by a loss in ductility, a phenomenon called the
“strength–ductility trade-off.” Overcoming this conflict to attain
more damage-tolerant materials for applications has been the
focus of many research efforts. Due to the outstanding mechani-
cal properties of HEAs, one would think they would be immune
to this long-running conflict. However, regardless of their
intriguing core effects, HEAs also undergo this phenomenon,
as shown in Section 3. Thus, many research efforts[215–230]
have been made in terms of tuning the structure of HEAs to
overcome this “strength–ductility trade-off,” which will be sur-
veyed in this section.
Li et al.[215,216] proposed a metastability engineering tech-
nique, which decreases phase stability to achieve interfacial
and transformation-induced hardening as a means to overcome
the strength–ductility trade-off. As such, a transformation-induced
plasticity-assisted, dual-phase HEA (TRIP-DP-HEA) was devel-
oped by switching from the equiatomic Fe20 Co20 Cr20 Mn20 Ni20
to the nonequiatomic Fe50 Mn30 Co10 Cr10 by controlling the Mn
content in Fe80 x Mnx Co10 Cr10 . The as-cast alloys were then hot
rolled to 50% reduction in thickness at 900  C, homogenized at
1200  C for 2 h in Ar atmosphere, and water quenched.
Further grain refinement was achieved by cold rolling (to 60%
thickness reduction) and 3 min annealing at 900  C in an Ar atmo-
sphere. This nonequiatomic Fe50 Mn30 Co10 Cr10 alloy exhibits a
partial martensitic transformation from fcc-to-hcp phase upon
cooling, and by increasing the hcp phase fraction and decreasing
the grain size a simultaneous enhancement in strength and duc-
tility is achieved, as shown in Figure 32a. Sun et al.[223] successfully
designed a treatment process to obtain a good balance in strength
and ductility in the Fe20 Co20 Cr20 Mn20 Ni20 HEA. The as-cast
ingots were solution treated at 1100  C for 2 h and hot forged
at 1000  C to a rod with a final diameter of 30 mm. The rod
was further cold rolled to sheets with a final thickness of
1 mm. The cold-rolled sheets were then annealed at various tem-
peratures ranging from 650 to 1100  C for 30 min. This resulted in
the samples having various grain sizes ranging from the ultrafine
regime to the coarse-grain regime. The ultrafine-grained (UFG)
HEA possessed a 21% uniform elongation and a 984 MPa yield
strength, as shown in Figure 32b. In a subsequent study,
Sun et al.[224] modulated the prestrain history by subjecting the
UFG Fe20 Co20 Cr20 Mn20 Ni20 HEA to 10% engineering strain

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Figure 28. a) Compressive true stress–strain curves of the as-cast GdHoLaTbY alloy and its constituent elements. Adapted with permission.[93] Copyright
2016, Elsevier Ltd. b) Room temperature compressive true stress–strain curves of the as-cast FeCoNiCuAlX HEAs. Adapted with permission.[169]
Copyright 2012, Elsevier B.V.
at 293 and 77 K before conducting the tensile tests. It was found
that the samples prestrained at 77 K possessed a superior yield
strength (1.07 GPa) and ductility (15.3%), as compared with the
293 K prestrained samples with a yield strength and ductility
of 1 GPa and 10.3%, respectively, as shown in Figure 32c.
This was attributed to a uniform distribution of the high-density
dislocations in the 77 K prestrained samples as compared with the
293 K prestrained samples. Chen et al.[225] used the alloying
approach to simultaneously enhance the strength and ductility
of a HEA. In their method, the fcc-structured twinning-induced
plasticity (TWIP) Fe40 Mn40 Co10 Cr10 HEA was alloyed with
carbon. Their results, as shown in Figure 32d, revealed that the
strength and ductility are concurrently improved when up to
3.3 at% C is added. This was attributed to a room temperature
deformation-induced twinning upon dislocation pinning by the
interstitial carbon atoms, leading to improvement in toughness.
Similarly, interstitial carbon atoms are found to induce both
TWIP and TRIP in HEAs, leading to an improvement in strength
and ductility.[226]
However, Su et al.[227] very recently developed a method for
improving the mechanical properties of interstitially C-doped
HEAs. In their approach, the alloys are cold rolled, followed
by subsequent tempering and annealing to utilize a hierarchical
microstructure and attain a strength–ductility synergy. Details of
their procedure are shown in the schematic plot of Figure 33a.
These hierarchical bimodal- and trimodal-structured interstitial
HEAs exhibit a superior strength–ductility combination com-
pared with the previous carbon-doped HEA, as shown in
Figure 33b. By developing a heterogeneous structure through
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cold working followed by annealing at 923 K, Wu et al.[228] over-
came the strength–ductility trade-off in the Al0.1 CoCrFeNi HEA.
The heterogeneous structured alloy possessed a yield strength,
tensile strength, and an elongation of 711 MPa, 928 MPa, and
30.3%, respectively. This improvement in mechanical properties
is found to be due to a combination of the nonrecrystallized and
recrystallized grains in the heterogeneous microstructure.
Another system which utilizes a heterogeneous structure to over-
come the strength–ductility trade-off is the Fe29 Co28 Ni29 Cu7 Ti7
HEA.[229]
In groundbreaking research by Lei et al.,[230] oxygen which
usually renders materials brittle was used in the form of ordered
oxygen complexes, a state in between oxide particles and random
interstitials, to enhance the strength and ductility of HEAs. In
their work, the structurally stable bcc-structured TiNbZrHf [40,41]
HEA was used as a base alloy and then doped with oxygen and
nitrogen, respectively, as ðTiNbZrHf Þ98 O2 and ðTiNbZrHf Þ98 N2 .
Figure 34a shows the tensile stress–strain curves of the studied
alloys. The strength is enhanced by about 49% whereas the
ductility is also enhanced by about 95% in the ðTiNbZrHf Þ98 O2
HEA. Microstructural studies revealed the simultaneous
strength and ductility enhancement as a result of the nanoscale-
ordered (O, Zr, Ti)-rich atomic complexes optimizing
dislocation multiplication and a high strain-hardening rate.
Ultimately, the ordered interstitials trigger the deformation
mode from planar slip to wavy slip. Synchrotron radiation
XRD studies revealed that the TiNbZrHf HEA maintained
its single-phase bcc structure even after doping with O2 and
N2 , as shown in Figure 34b.
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Figure 29. SEM image showing the microstructure of the bulk AlCoCrFeNix (x ¼ 2.0, 2.1, and 2.2) alloys: a) hypoeutectic AlCoCrFeNi2.0 alloy; b) eutectic
AlCoCrFeNi2.1 alloy; and c) hypereutectic AlCoCrFeNi2.2 alloy. Engineering tensile stress–strain curves of AlCoCrFeNix (x ¼ 2.0, 2.1, and 2.2) alloys
d) at room temperature, e) at 70  C, f ) 196  C. Adapted with permission.[170] Copyright 2016, Elsevier Ltd.

Yang et al.[217] developed a strategy to break the strength–

Figure 30. The overall framework for the reduction in SFE via lattice
distortion core effect in HEAs. Redrawn from Ref. [183]
ductility trade-off by introducing high-density ductile multicom-
ponent intermetallic nanoparticles (MCINPs) in fcc-type HEAs.
The idea was to generate a nanocomposite structure by generat-
ing ductile-ordered MCINPs in a ductile disordered multicompo-
nent matrix, as shown in Figure 35b. This strategy enhances the
strengthening effect of the IM nanoparticles while maintaining a
high strain-hardening rate and plastic deformation stability. The
process was successfully achieved by alloying an equiatomic
FeCoNi base alloy with Al and Ti to control the order–disorder
phase transition and elemental partitioning. The as-cast alloys
were homogenized at 1423 K for 2 h followed by water quench-
ing, then cold rolled to 65% reduction, and recrystallized at
1423 K for 90 s. The stress–strain response for the
ðFeCoNiÞ86 Alx Tiy alloy series is shown in Figure 35a.
ðFeCoNiÞ86 Al8 Ti6 showed a large increase in yield strength
(1000 MPa) as compared with the FeCoNi base alloy
(200 MPa), whereas the ductility was maintained at 32%
for both alloys. ðFeCoNiÞ86 Al7 Ti7 showed a very large increase
in both yield strength (1500 MPa) and ductility (50%),
exhibiting its ability to successfully break the strength–ductility
trade-off.

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Figure 31. a,b) XRD patterns as a function of pressure obtained during compression and decompression of FeCoNiCrMn HEA.[8,202] c) the schematic
plot of the atomic structure and transition paths between the polymorphs of the Al0.6 CoCrFeNi HEA. bcc, body-centered cubic; bct, body-centered
tetragonal; fcc, face-centered cubic; hcp, hexagonal close packing. Adapted with permission.[208] Copyright 2018, Elsevier Ltd.

Friction stir processing (FSP), which has been recently sug-
gested to be a processing technique with synergetic control of
strain rate, strain, and temperature, has been successfully used
to overcome the strength–ductility trade-off.[218–220] Using the
metastability engineering approach, Nene et al.[218,219] can control
the transformation of γ-fcc grains and twinning in the ε-hcp matrix
of the Fe40 Mn20 Co20 Cr15 Si5 and Fe39 Mn20 Co20 Cr15 Si5 Al1 HEAs
to achieve simultaneous strength–ductility enhancement. In the
AlCoCrFeNi2.1 EHEA, FSP was used by Wang et al.[220] to alter
the bristly lamellar eutectic structure in the as-cast condition to
UFG fcc/L12 and refinement of bcc/B2, which increased the
ductility from 6.5% to 10% and the strength from 800 to 920 MPa,
as shown in Figure 36a. However, in the same AlCoCrFeNi2.1
EHEA, Bhattacharjee et al.[221] developed a hierarchical micro-
structure by subjecting the as-cast samples to cryorolling (90%
thickness reduction) followed by annealing at 1073 K for 1 h.
This resulted in a nanolamellar microstructure which resulted
in a simultaneous improvement in both yield strength
(1450 MPa) and ductility (14%), as shown in Figure 36b.
Juan et al.[222] reported that grain refinement simultaneously
enhances the strength and ductility of the bcc TaTiNbZrHf
RHEA. In their study, the as-cast TaTiNbZrHf samples were
subjected to 70% reduction cold rolling and followed by heat treat-
ment at 1473, 1523, 1573, and 1623 K in air. The alloy maintained
its single-phase bcc structure even after thermo–mechanical proc-
essing but with various grain sizes due to different heat-treatment
temperatures. Figure 36c shows that when the grain size
decreased from 128 to 38 μm, the strength and ductility increased
to 985 MPa and 20%, respectively. This suggests that the grain-size
strengthening, which is effective in conventional alloys, could also
be useful in HEAs. Conventionally, one might think at first glance
that HEAs should be immune to the strength–ductility trade-off
dilemma. However, just like their conventional counterparts, this
dilemma is somewhat universal. As such, we have looked at recent
advances which have been made in overcoming this trade-off.
Studies show that the metastability engineering approach is the
most used one in HEAs, efficiently achieving concurrent strength
and ductility enhancement. Other methods such as grain refine-
ment, cold rolling, and interstitial alloying techniques and
prestrain modulation also play a significant role.

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Figure 32. a) Mechanical behavior of TRIP-DP HEAs compared with other HEAs. Adapted with permission.[215] Copyright 2016, Macmillan Publishers
Limited. b) Tensile engineering stress–strain curves of the fully recrystallized FeCoNiCrMn HEA with different grain sizes. Adapted with permission.[223]
Copyright 2017, Elsevier Ltd. c) Engineering stress–strain curves of the prestrained HEAs to 10% at 293 K and 77 K, respectively. Adapted with
permission.[224] Copyright 2019, Elsevier Ltd. d) Engineering stress–strain curves of Fe40 Mn40 Co10 Cr10 HEA with different C contents. Adapted with
permission.[225] Copyright 2018, Elsevier B.V.

At cryogenic temperatures, the strength–ductility trade-off 5. Summary and Outlook

is a common phenomenon in most engineering materials.
This is seen in cases where ductile materials transition into
brittle materials as temperatures decrease from ambient to
cryogenic temperatures. This is also called the “ductile–brittle
transition”. This is a key engineering issue that makes the
materials available for cryogenic applications in the space
industry, superconductivity, nuclear reactors, etc. somewhat
limited.[124] To date, only some conventional alloys are viable
for liquid-helium-temperature applications, most of which are
fcc structured.[231-236] Just as in conventional alloys, some fcc-
structured HEAs[21,124,237,238] have shown great potential for
cryogenic applications. This is seen first hand in Figure 13,
where the FeCoNiCrMn and FeCoNiCr HEAs exhibit an
enhancement in their mechanical response with decreasing tem-
peratures. Figure 37 shows the ultimate tensile strength versus
elongation Ashby plot for different cryogenic materials at 4.2 K. It
is seen that the HEAs possess an excellent combination of strength
(1 GPa) and ductility (>50%) at liquid helium temperatures.
Over the past decade, HEAs have gained wide attention.[239–245]
From the fcc CrCoNi-based HEAs with the potential for
cryogenic applications to RHEAs with high-temperature and
oxidation-resistance properties, HEAs have the potential as struc-
tural and functional materials. This potential can further be real-
ized if a clearer picture of the relationship between the four core
effects is painted. As one of the four hypotheses of HEA, lattice
distortion is seen as the most important one due to its direct
influence on deformation mechanisms, thermodynamic stabil-
ity, and other properties. As such, we believe that a better under-
standing of this core effect will help answer some of the
longstanding questions regarding the wide range of properties
HEAs exhibit. Even though research efforts have been made
in describing and understanding lattice distortion in HEAs thus
far, some unsolved dilemmas remain. The following research
issues from our perspectives will go a long way toward improving
our understanding of lattice distortion in HEAs. 1) A bold step

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Figure 33. a) Schematic plot of producing hierarchical bimodal and trimodal microstructures. b) Engineering stress–strain curves of
Fe49.5 Mn30 Co10 Cr10 C0.5 heat treated at 400, 650, and 750  C for 3 and 10 min. The two dashed lines represent the stress–strain curves of the fully
recrystallized grain structures with average grain sizes of 4 and 160 μm. Adapted with permission.[227] Copyright 2018, Elsevier Ltd.

toward unraveling lattice distortion in HEAs will be understand-

Figure 34. a) Room-temperature tensile stress–strain curves for the
as-cast TiNbZrHf (denoted as a base alloy), ðTiNbZrHf Þ98 O2 (denoted
as O-2), and ðTiNbZrHf Þ98 N2 (denoted as N-2) HEAs. The inset
shows the corresponding strain-hardening response ðTiNbZrHf Þ98 O2 .
A higher work-hardening rate is observed for the O2 HEA variant
ðTiNbZrHf Þ98 O2 compared with the base HEA. b) Synchrotron high-
energy XRD results for the as-cast, O2 - and N2 -doped TiNbZrHf HEA.
Adapted with permission.[230] Copyright 2018, Springer Nature Limited.
ing the nature of elemental distribution during solidification in
HEAs. The question is whether the elements are
randomly distributed along the lattice in HEAs. If not, what
are atomic packings on short- and medium-range scales in
HEAs? To some extent, this question has been answered by
Santodonato et al.,[246] who demonstrated via complementary
experimental and theoretical techniques that elemental segrega-
tion, precipitation, chemical ordering, and spinodal decomposi-
tion do not eliminate the amount of disorder in HEAs. Even
though this established the fact that multiphase materials also
benefit from entropy-enhanced stability, the degree of distortions
in HEAs was still unanswered. In addition to this, although
HEAs form single-phase SS of fcc, bcc, and hcp structures,
are the atomic packing factors comparable with that of single-
crystalline materials? 2) The local atomic mismatch parameter
δ which quantifies the variations in atomic sizes or lattice
constants has been mostly used to also quantify the degree of
distortions in HEAs. However, this parameter alone is not
enough to quantify the distortions in HEAs as the degree of dis-
tortion is dependent on whether small-sized or large-sized atoms
exist on the first shell.[239] Another important point is that the
variation in lattice constant in HEAs has mostly been described
based on the hard-sphere conventional alloy model which is not
realistic. As such, the proposed framework by Wang et al.[247] via
combining high-precision quantitative XRD measurements and
the lattice constant variation model seems more realistic.

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Figure 35. a) Engineering stress–strain curves of ðFeCoNiÞ86 Al7 Ti7 and ðFeCoNiÞ86 Al8 Ti6 alloys compared with the FeCoNi base alloy, showing a signifi-
cant increase in strength without ductility reduction. ðFeCoNiÞ86 Al7 Ti7 exhibits ductile dimpled structures without macroscopic necking. b) Schematic of
the design concept of the MCINPs alloys in a multicomponent matrix. Adapted from a previous study.[217]

Figure 37. Ultimate tensile strength versus elongation Ashby map of cryo-
genic materials at 4.2 K. Adapted with permission.[124] Copyright 2018, Science
China Press and Springer-Verlag GmbH Germany, part of Springer Nature.

Figure 36. a) Stress–strain curves of as-cast and friction stir-processed

AlCoCrFeNi2.1 : Adapted with permission.[220] Copyright 2018, Elsevier
B.V. b) Engineering stress–strain plots of the EHEA in various heat-treated
conditions. The dimensions of the tensile specimen are shown in the inset
(all dimensions in mm). Adapted with permission.[221] c) Engineering
stress–strain curves of TaTiNbZrHf alloy with different grain sizes.
Adapted with permission.[222] Copyright 2016, Elsevier B.V.
Therefore, further studies in line with Wang et al.[247] and a the-
oretical model which takes into consideration the atomic size,
bulk modulus, lattice constant, lattice spacing, and other unit cell
parameters should be developed while considering the effects of
environmental parameters, i.e., temperature, pressure, and
stress changes on the degree of distortions. 3) The ability of

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HEAs to form SS means they also contain intrinsic defects such
as vacancies and interstitials which affect the thermodynamic
and kinetic properties of HEAs. Could these vacancy and inter-
stitial defects be seen as lattice distortions as LLD is also directly
related to the thermodynamic and kinetic properties of HEAs? If
yes, we think the approach used by Wang et al.,[248] which revealed
that the equilibrium vacancy concentrations and their clusters in
HEAs are one order magnitude larger than that of pure and
binary metals, could be used to describe the degree of distortions
in HEAs. We recommend further studies regarding vacancy and
cluster formations in HEAs. 4) Concerning the characterization
of lattice distortion in HEAs, apart from diffraction techniques
(X-ray, electron, neutron), a combination of various advanced
characterization techniques such as TEM, APT, XAFS, EBSD, etc.
is strongly recommended in the study of the complicated nature
of lattice distortion in HEAs. 5) First-principle methods based on
DFT are useful tools in investigating lattice distortion in conven-
tional alloys. However, the presence of multiple elements on
HEAs and the scarcity of reliable binary or ternary atomic poten-
tials make the description of the lattice distortion complex. Thus,
from the theoretical perspective, what kind of new theory could be
developed to describe lattice distortions in HEAs? Considerable
theoretical studies should be done to elucidate lattice distortion
in HEAs. 6) Lattice distortion plays an important role in the
mechanical properties of HEAs, even though no definite lattice
distortion parameter has been established. The consensus
suggests that a large lattice distortion reduces SFE. Low SFE
HEAs possess an attractive combination of strength and ductility.
Therefore, it would be very nice if, after an effective lattice distor-
tion parameter has been developed, a property tailoring scheme
would be designed like that of SFE.[210,249]
In conclusion, the near-equiatomic basis of HEA design is
gradually being tweaked by the development of phase selection
parameters and the search for not just single-solution phases but
property optimization. In this Review, the recent progress on the
phase selection criteria which have been proposed thus far based
on the classical Hume-Rothery rules and lattice strain perspecti-
veshas been briefly summarized. The lattice distortion effect is
probably the most important one of the core effects due to the
role it plays in affecting thermodynamic, kinetic, and deforma-
tion theories. We focused on the significant effects of lattice dis-
tortion on the mechanical properties of HEAs and the role it
plays in polymorphism. Although attempts have been made in
quantifying lattice distortion in HEAs, further work is still
needed to improve the understanding of polymorphism and
the strengthening and deformation mechanisms. The narrative
behind single-phase SS HEAs potentially exhibiting the “best
properties” is gradually shifting with the emergence of the
EHEAs and other multiphase HEAs possessing superior proper-
ties. The strength–ductility trade-off dilemma was also looked at
in this Review and the evidence suggests that a metastability engi-
neering approach is an effective tool in overcoming the trade-off
dilemma to make HEAs the next cutting-edge structural materials.
Supporting Information
Supporting Information is available from the Wiley Online Library or from
the author.
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Acknowledgements
Financial support from the National Natural Science Foundation of China
(U1832203, 11975202, 51671170, and 51671169), the National Key
Research and Development Program of China (nos. 2016YFB0701203,
2017YFA0403400, and 2016YFB0700201), the Natural Science
Foundation of Zhejiang Province (grant nos. Z1110196 and Y4110192),
and the Fundamental Research Funds for the Central Universities are
gratefully acknowledged.
Conflict of Interest
The authors declare no conflict of interest.
Keywords
high-entropy alloys, lattice distortions, phase selections, structure-
property correlations
Received: April 17, 2020
Revised: June 15, 2020
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Raymond Kwesi Nutor received his Master’s degree in Zhejiang Normal University, China. He is currently
a Ph.D. candidate at the Laboratory of New-Structured Materials, School of Materials Science and
Engineering in Zhejiang University, China. His current research focuses on the mechanical behavior of
high-entropy alloys and their potential applications as advanced structural materials.

Qingping Cao has been a university associate professor of Materials Science and Engineering at Zhejiang
University (ZJU) since 2010. His current research interests are the structure–property correlations in
metallic glass and high-entropy alloys.

Xiaodong Wang is an associate professor of Materials Science and Engineering at Zhejiang University.
His research interests are currently in the atomic-level structure, dynamics, and physical properties of
multicomponent alloys in the glassy and liquid states using advanced synchrotron X-ray techniques and
computational methods.

Dongxian Zhang has been a university professor of Optical Science and Engineering at the Zhejiang
University since 2009. She has published many papers exploring the properties of micro/nano structures
with metals especially the high-entropy multicomponent amorphous alloys.

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Yunzhang Fang has been a university professor from 1986 till date, engaging in teaching and research in
Zhejiang Normal University. He is mainly engaged in the preparation of amorphous soft magnetic alloy
and the research of performance and structure characterization technology and has presided over more
than ten scientific research projects above the provincial and ministerial level.

Yong Zhang has been a university professor of Materials Science at the USTB since 2004. He proposed
a balance parameter to evaluate the configurational entropy effect over the enthalpy effect at the liquid
state, it has been verified effective to predict the phase formation for the multicomponent materials.

Jian-Zhong Jiang has been a chair professor at the School of Materials Science and Engineering, Zhejiang
University, since 2004.. He developed 73-mm Zr-based, 35-mm La-based, and 28-mm CuZr-based high-
entropy amorphous alloys, discovered the existence of fcc Ce3Al solid solution, long-range ordering,
amorphous–amorphous transition, liquid–liquid transition in single-, binary-, and high-entropy multi-
component metallic alloys, intermediate temperature brittleness in high-entropy amorphous alloys, and
proposed dense atomic packing mechanism for the formation of high-entropy amorphous alloys.

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