Applied Nanoscience

https://doi.org/10.1007/s13204-020-01494-9

ORIGINAL ARTICLE

Deformational and magnetic effects in Cu–Al–Mn alloys

A. Titenko1 · L. Demchenko2 · A. Perekos3 · M. Babanli4 · S. Huseynov4 · T.‑Z. Ren5

Received: 14 December 2019 / Accepted: 22 June 2020

© King Abdulaziz City for Science and Technology 2020

Abstract
A comparative analysis of the magnetic, size and deformation effects of martensitic transformation in aged Cu–Al–Mn alloys
with a minimum width of the temperature hysteresis was performed. According to the experimental studies of the behav-
ior of alloys during martensitic transformations, the changes in temperature dependences of thermal expansion, magnetic
susceptibility and electrical resistance, depending on preliminary thermomagnetic treatment of alloys, were found. The
thermomagnetic treatment contributes to a change in the magnitude of volume effect of martensitic transformation. Using
magnetic analysis, the state and distribution of precipitated particles, affecting both the magnetic characteristics and the
volume effects of martensitic transformation in the alloys, were determined.

Keywords Cu–Al–Mn shape memory alloys · Aging in magnetic field · Martensitic transformation · Thermal expansion ·
Volume effect · Magnetic properties · Dimensional and magnetic parameters of nanoparticles

Abbreviations the possibilities and mechanisms for controlling these char-

SMAs Shape memory alloys acteristics. Among copper-based SMAs, the Cu–Al–Mn
MT Martensitic transformation alloys are the most attractive due to their good mechanical
TMT Thermomagnetic treatment and magnetic properties that can be controlled by chemical,
SE Superelastic mechanical, and magnetic treatments, or by the combined
action of these factors (Warlimont and Delay 1974; Kainuma
et al. 1996; Bubley et al. 1996; Omori et al. 2006; Sutou
Introduction et al. 2008). The SMA functional properties have a special
role in connection with the deformation effects which occur
The starting point in the creation of shape memory alloys therein when exposed to the temperature, magnetic field and/
(SMAs) was the discovery of thermoelastic equilibrium or mechanical load. The deformation effects make it possible
during phase transformation in Cu–Al alloy (Kurdyumov to use SMAs as sensors sensitive to external influences, or
and Handros 1949). Further systematic studies have shown as actuators that cause an appropriate response of the sizes
and shapes of materials when a control signal is applied.
* L. Demchenko The prospect of using copper-based SMAs is primarily
lesyademch@gmail.com associated with their cost and a set of optimal mechanical
characteristics, which are achieved by thermomechanical
1
Institute of Magnetism, NAS and MES of Ukraine, 36‑b treatment, consisting usually of preliminary deformation
Akademika Vernadskoho Blvd, Kyiv 03142, Ukraine
and annealing (Kainuma et al. 1996; Omori et al. 2006;
2
National Technical University of Ukraine “Igor Sikorsky Sutou et al. 2008). For the textured C ­ u71.5Al17.5Mn11 alloy,
Kyiv Polytechnic Institute”, 37 Peremohy Ave, Kyiv 03056,
Ukraine
the maximum superelastic (SE) deformation was obtained
3
greater than 11% (Sheng et al. 2017). Highly alloyed
G. V. Kurdyumov Institute for Metal Physics of the National
Academy of Sciences of Ukraine, 36 Akademika
­CuAl21Mn21 alloys have wide practical possibilities as light
Vernadskoho Blvd, Kyiv 03680, Ukraine with respect to steels, wear-resistant and high-temperature
4
Azerbaijan State University of Oil and Industry, 20 Azadliq
materials (Altenberger et al. 2017).
Ave, AZ1010 Baku, Azerbaijan Moreover, such functional SMAs have high technical
5
School of Chemical Engineering, Hebei University
characteristics for their application, for example, in medicine
of Technology, Guangrong Road 8, Tianjin,
Hongqiao district, China

13
Vol.:(0123456789)
 Applied Nanoscience

(Omori et al. 2006), for damping various vibrations (Bocci-

olone et al. 2012) and other purposes.
In the context of the discussion of changes in volume effect,
it is important to note that using different heat, magnetic or
mechanical treatment it is possible to vary volume effect in
alloys. For example, a preliminary mechanical treatment of
Cu–Al–Mn alloy leads to a significant (in 2 ÷ 3 times) change
in volume effect, but the considerable alloy strengthening is
accompanied by degradation of MT, and as a result, volume
effect decreases (Sutou 2004).
Thus, for understanding the nature of deformational effects
which are accompanied by structural changes in Cu–Al–Mn
alloys under the aging in magnetic field (Titenko et al. 2014,
2016, 2017) and further controlling them, it is of scientific
interest to study the deformational and magnetic behavior of
these alloys under effect of mechanical stress and temperature Fig. 1  The temperature dependences of low-field magnetic suscep-
and summarize with existing data. tibility for alloy 1 (a) and alloy 2 (b) after the various preliminary
TMTs: aging in parallel magnetic field (green), perpendicular field
(red) and without a field (black); the temperature dependence of
Materials and methods inverse magnetic susceptibility (c) for determining the Curie tempera-
ture (Tc)
Two aged Cu–Al–Mn alloys of following composition (wt.%),
Alloy 1–Cu–12.6Al–5.2Mn; Alloy 2–Cu–13.5Al–4.7Mn, with
the smallest width of temperature hysteresis ΔT of MT, were
selected for the investigation. The alloys were melted in an
induction furnace in an argon atmosphere. The samples were
made in the form of parallelepipeds of size 20 × 4 × 4 mm3.
After a homogenizing annealing at 850 °C for 10 h, the sam-
ples were quenched in water from 850 °C. Then, for the alloys’
aging, the thermomagnetic treatment (TMT) consisted of
annealing at 200 °C for 3 h in an air atmosphere with apply-
ing a magnetic field of 1.5 kOe, parallel or perpendicular to
the sample main axis, as well as without field.
The aging of the alloys under optimal conditions leads to a
decrease in elastic energy as a result of changes in the degree
of tetragonality of the lattice (Kokorin 1987; Kozlova and
Titenko 2006).
The dilatometric analysis in a wide temperature range
with the registration using inductive displacement sensor was
performed with the measurement accuracy of ± 2 °C in zero Fig. 2  The temperature dependences of electrical resistance taken in
zero magnetic field for alloy 2 after the various preliminary TMTs:
magnetic field to estimate the volume effect of martensitic
aging in parallel magnetic field (green), perpendicular field (red) and
transformation. without a field (black)
A magnetometery with a vibrating method was used to
measure the static magnetization.
The characteristic temperatures of martensite transforma- Results and discussion
tion (MT) of the alloys after thermal treatment were deter-
mined from the temperature dependences of low-field mag- The characteristic temperatures
netic susceptibility.
The temperature dependences of the low-field magnetic
susceptibility and electrical resistance under the MT
induction in alloys after TMT show a number of features
(Figs. 1 and 2). Evidence of MT occurrence during the
cooling is a sharp decrease in χ/χmax and an increase in

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ρ/ρmax in the temperature range of MT. Such a change is Magnetic characteristics

due to the transformation of a high-symmetric (austen-
ite) structure into a low-symmetric (martensite) one. An
increase in the resistance of alloys in the martensitic state
is associated with a more imperfect crystalline structure
of martensite as compared with austenite.
The behavior of χ(T) is associated not only with the
structural transformation of the austenite matrix, but
also to a greater extent with the magnetic state and the
interaction of ferromagnetic C ­ u 2AlMn-particles. Under
the structure transformation, the matrix exerts a non-
hydrostatic pressure on the particles of ~ 1 GPa (Kokorin
et al. 1993). A change in the shape of the particles from
the action of non-hydrostatic pressure creates a stress-
induced magnetic anisotropy, which is 2 orders of mag-
nitude higher than the magnetocrystalline one, which is
reflected in the χ/χ max dependences. Comparing the χ/
χmax(T) dependences for the alloys after different TMTs,
a certain change in the χ/χmax amplitude should be noted,
namely, the maximum value of χ/χmax occurs for anneal-
ing without a field, while the minimum is observed for
annealing in parallel field.
The characteristic temperatures and the hysteresis
width of MT for the alloys after different TMTs, deter-
mined from the temperature dependences of low-field
magnetic susceptibility (Fig. 1) and electrical resistance
(Fig. 2), are summarized in Table 1. As seen from Figs. 1
and 2, the application of magnetic field during anneal-
ing does not affect the characteristic temperatures and
the hysteresis width of martensite transformation of the
alloys. After the different TMTs, these parameters are
almost the same, they differ within the measurement
error.
To understand the nature of deformational effects in the
studied alloys, a qualitative and quantitative estimation of
the precipitation phase was carried out in accordance with
the methodology described in detail in Bean et al. (1959)
and Kokorin (1987) and the calculated parameters are sum-
marized in Table 2. There is a known procedure for deter-
mining a size of superparamagnetic particles from the slope
of curves of the field dependence of magnetization in the
region of low fields.
Although real nanoparticles can have a complex (nonu-
niform) magnetic structure, as a rule, an ensemble of non-
interacting single-domain isotropic particles behaves like
classical paramagnetic matter with very high (~ 103 –104µB)
effective magnetic moment m per particle, where µB is Bohr
magneton. If we have this ensemble at temperature T in an
applied field H, and assume that it has achieved thermody-
namic equilibrium, there will be a Boltzmann distribution of
the orientations of m with respect to H. The magnetization
of the ensemble of superparamagnetic particles depending
on the strength of the applied magnetic field and temperature
is described by the Langevin function:
(1)
/
I I0 ≅ L(mH∕kT) = coth(mH∕kT) − kT∕mH
and the average ensemble moment in the direction of the
field is equal to < m >  = mL(mH/kT), where I = I(H, T) is
the intensity of magnetization of the sample in an applied
magnetic field H at temperature T; I0 is the saturation mag-
netization of an ensemble of superparamagnetic particles
in the sample at temperature T; m is a particle magnetic
moment; k is the Boltzmann’s constant; L is the Langevin
function.

Table 1  The characteristic temperatures and hysteresis width of MT of Cu–Al–Mn alloys after annealing using the different TMT regimes
Alloy composition, wt.% Ms,°C Mf,°C As,°C Af,°C Tc,°C ΔT,°C

Alloy 1 Cu–12.6Al–5.2Mn − 51 − 63 − 50 − 39 − 75 12
Alloy 2 Cu–13.5Al–4.7Mn 0 − 27 8 18 − 35 18

Ms and Mf are the start and finish temperatures of direct MT; As and Af are the start and finish temperatures of reverse MT; Tc is the Curie tem-
perature; ΔT = Af − Ms is the temperature hysteresis of MT

Table 2  Magnetic and dimensional parameters of nanoparticles for the Cu–Al–Mn alloys
Parameters Saturation magnetiza- Particle volume Particle diam- Particle magnetic Nubmer of particles per Volume
tion of sample (I0), G (V), ­sm3 eter (d), nm moment (m), µB unit volume (n), ­sm−3 fraction of
particles, %

Alloy 1 13.6 5.7 × 10–20 3.8 4.3 × 103 3.4 × 1017 0.03
Alloy 2 10 1.7 × 10–20 2.6 1.3 × 103 8.5 × 1017 0.02

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Since, in low fields H (≪ kT∕m

) , the Langevin function
can be approximated by L mH mH
≅ 3kT and the particle mag-
kT
netic moment is equal to m = IS V = 𝜌𝜎SF V , where IS is the
saturation magnetization of ferromagnetic material of parti-
cles at temperature T; V is the particle average volume; ρ and
𝜎SF are the density and the specific saturation magnetization
of ferromagnetic material of particles of the ­Cu2MnAl stoi-
chiometric composition, respectively, we can obtain
I mH I VH
≅ = S
I0 3kT 3kT
So, for spherical particles, considering that I = 𝜌𝜎H and
I = 𝜌𝜎S, where 𝜎H is the specific magnetization in applied
magnetic field H at temperature T and 𝜎S is the specific satu-
ration magnetization of the ensemble of superparamagnetic
particles in the sample at temperature T, the particles’ aver-
age volume and diameter can be determined by formulas,
respectively:
√
𝜎 3kT 18 𝜎H kT
V= H⋅ and d = 3
⋅ ⋅ .
𝜎S IS H 𝜋 𝜎S IS H
Using the known values of the saturation magnetization
of the sample and the particle magnetic moment, one can
determine the /number of particles per unit volume of the
sample: n = I0 m.
Using relations of the theory of superparamagnetism
(Bean et al. 1959; Kokorin 1987) and assuming that the
(2) specific magnetization of particles at room temperature is
IS = 560 G for the bulk Cu–Al–Mn alloy of ­Cu2MnAl com-
position (Michelutti et al. 1978), the magnetic and dimen-
sional parameters of nanoparticles for the alloys 1 and 2
were determined (Table 2). The data for the calculation were
taken from the curves of static magnetization at room tem-
perature in magnetic fields up to 20 kOe (Fig. 3), behavior
of which indicates a typical superparamagnetic state of the
alloy. From the position of magnetic behavior, the stud-
ied alloys behave as soft magnetic materials, as evidenced

a b

Fig. 3  The magnetization curves and magnetic hysteresis loops for the alloy 1 (a) and 2 (b) at room temperature; the extrapolation of the static
magnetization dependence in coordinates I = f(1/H) (c)

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by the absence of magnetic hysteresis. Moreover, for the in a Cu–Mn–Al alloy, antiferromagnetic and ferromagnetic
alloys 1 and 2, the anisotropy field (the inflection point on clusters of Mn atoms coexist without long-range order.
the magnetization curves) practically coincides and is at the
level of 2 kOe, while the specific saturation magnetization Thermal properties
for the alloy 1 is 3 times higher than that for the alloy 2:
σs(1) = 0.78 emu/g vs σs(2) = 0.25 emu/g. Thermally induced deformation in SMAs is most clearly
During magnetization, the mechanism of rotation of mag- manifested in volume effects in MT interval. The measure-
netic moments of particles in the direction of the external ment of thermal expansion of alloys and estimation of vol-
magnetic field is mainly realized, and the magnetic anisot- ume effect of MT was performed in zero magnetic field for
ropy energy required for this can be calculated from the rela- alloys preliminary aged in parallel and perpendicular mag-
tion: K≈IS⋅HA = ½⋅2⋅103 Oe⋅560 emu/sm3 = 5.6⋅103 erg/sm3 netic field and without a field. According to the data of Δl/
at T = 300 К, where K is the constant of magnetic anisot- l0 = f(T), the samples’ size increases at cooling when tem-
ropy energy, which is expended on the rotation of magnetic perature starts equal ­Ms. The dilatational behavior of alloys 1
moments of particles in the direction of the external mag- and 2 depending on the TMT regimes is shown in Fig. 4, and
netic field; H
­ A is the magnetic anisotropy field; IS value was their features are directly related to sizes and distributions of
taken for bulk samples of ­Cu2MnAl phase from Michelutti precipitated particles. As a result of the Cu–Al–Mn alloys
et al. (1978). aging at TMT, the system of equiaxed particles (the dilata-
Thus, the main magnetic and dimensional parameters of tion centers) is formed in the alloy matrix (Kokorin 1987;
superparamagnetic nanoparticles were estimated from the Kozlova and Titenko 2006). For alloy 2, the magnitude of
magnetization curves (Table 2). volume effect of MT is smaller than that for alloy 1 due to a
Based on the data presented in Table 2, the difference in decrease in particle size (see Table 2).
magnetic behavior of the alloys is due to both the size of
precipitated particles and their distribution and interaction
in the non-ferromagnetic matrix. Thus, the diameter and vol-
ume fraction of nanoparticles in alloy 1 are 1.5 times higher,
and the magnetic moment of a particle in alloy 1 is 3 times a
higher than the corresponding parameters in alloy 2, but the
number of particles per unit volume in alloy 1 is 2.5 times
less than that in alloy 2.
The observed effects of magnetic ordering are associated
with the existence of magnetic clusters with ­Cu2MnAl struc-
ture, which do not undergo MT upon cooling. This is clearly
seen in the behavior of magnetic susceptibility (Fig. 1),
when, at paramagnetic Curie temperature, a decrease in sus-
ceptibility is observed due to the presence of concentration
inhomogeneities of alloys. Moreover, the change in magnetic
characteristics of the alloys is associated precisely with the
shape and size of the precipitated particles themselves, inter- b
acting in a magnetic field. Such change in magnetic charac-
teristics of the alloys during the induction of MT is due to
the fact that the crystal lattice of particles undergoes elastic
deformation resulting from the conjugation conditions of a
particle and the alloy matrix during the growth of martensite
crystals. This leads to an asymmetry in shape of ferromag-
netic particles embedded in a non-ferromagnetic matrix. The
magnetic characteristics of alloy 1 prevail the same charac-
teristics for alloy 2 as a consequence of a higher concen-
tration of magnetic carrier in alloy 1, despite the fact that
only 35% of manganese atoms are involved in the formation
of ferromagnetic phase (Takzey et al. 1999). The complex
nature of the interaction in ribbons of a similar composition Fig. 4  The thermal expansion curves (dilatograms) taken in zero
magnetic field for the alloy 1 (a) and 2 (b) after the various prelimi-
can be judged by the results of Hudak et al. (2018), which nary TMTs: aging in parallel magnetic field (green), perpendicular
indicate that, when measuring nuclear magnetic resonance field (red) and without a field (black)

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The volume effect (ΔVA−ΔV M)/VA = 3Δl/l 0 of MT
reaches its minimum values after the alloys’ TMT in a
parallel magnetic field: 0.66 and 0.48% for alloy 1 and 2,
respectively. These values are 10% less than ΔV/V0 after
the same thermal treatment without a field: 0.74 and 0.52%
for alloy 1 and 2, respectively. Thus, annealing in a parallel
magnetic field leads to a small (~ 10%) decrease in volume
effect of MT as a result of greater similarity of crystal lat-
tices of austenitic and martensitic phases and dispersion
hardening at aging, which creates additional conditions
for reducing both shear deformation and hysteresis width
(ΔT) of MT. In turn, maximum of ΔV/V0 is realized for
the case of annealing without a field, in which the particle
size is bigger than that after annealing in a magnetic field
(Titenko et al. 2016), this is also indicated by χ/χmax (a
decrease in the susceptibility with decrease of the particle
size in Fig. 1).
Depending on applied treatment regimes, the MT volume
effect changes as well as the width of temperature hysteresis
of MT changes, while the transition temperatures of MT
practically do not change. The lattice deformation during
MT is, mainly, shear and leads to shear elastic deformation
of both the alloy matrix and the precipitated particles under
the influence of non-hydrostatic stresses (Bean et al. 1959;
Kokorin 1987). These factors, as well as the influence of
magnetic field during heat treatment, lead to a change in
shape and size of nanoparticles (Titenko et al. 2014, 2016,
2017).
Prerequisites for such deformational behavior of aged
alloys may be the changes in elastic constants (shear modu-
lus) of the material due to dispersion hardening depending
on TMT regimes and the degree of tetragonality (a/c) of the
martensite lattice at constant elastic energy. Annealing in
magnetic field creates an additional elastic anisotropy during
the aging due to a change in the shape and volume fraction
of the precipitated particles, placed in the matrix (Titenko
et al. 2016, 2017, 2020). This is reflected in a change in
both the MT deformation and the elastic modulus, at the
same time the elastic energy of MT remains unchanged. The
constancy of elastic energy of the alloys after different TMT
is confirmed by the constant values of Ms and ΔT of MT.
The difference in MT volume effect depending on TMT
regimes correlates also with the microhardness of alloys
of the similar composition and heat treatment (Titenko
et al. 2014). In this case, the microhardness increases due
to dispersion hardening at aging, resulting in a decrease
in shear deformation, that limits the MT volume effect.
The smaller value of ΔV/V0 after annealing in a parallel
magnetic field can be associated also with a decrease in
particle size and an increase in their number compared to
annealing without a field (Titenko et al. 2014, 2016, 2017,
2020). This also leads to a decrease in crystal lattice mis-
match of the matrix and a precipitated particle, which can
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result in reducing the elastic energy of thermoelastic MT
(Bean et al. 1959; Kokorin 1987).
Thus, TMT of Cu–Al–Mn alloys contributes to a
decrease in volume effect of MT, as a result of a decrease
in size of the participated particles during the aging.
Comparing the results of reversible deformation effects in
Cu–Al–Mn alloys as a result of the influence of external
uniaxial tension and temperature, we can state that the
microstructure and interaction of precipitated particles
are significant. Due to the smaller particle size in alloy
2 in comparison with alloy 1 (Table 2), additional condi-
tions are created for increasing the thermoelasticity of the
alloy (Kozlova and Titenko 2006; Sutou 2013), which is
reflected in a decrease of MT temperature hysteresis width
and is associated also with reducing of elastic energy dur-
ing the transformation.
Conclusions
In the process of studying the deformation and mag-
netic behavior of Cu–Al–Mn alloys with different ther-
momagnetic treatment, the following regularities were
established:
1. The temperature dependences of low-field magnetic sus-
ceptibility, electrical resistance and thermal expansion
show the characteristic features associated with the mar-
tensitic transformation of the alloys. Thermomagnetic
treatment leads to a marked change in these dependences
due to the change in magnetic characteristics of precipi-
tated particles, as evidenced by analytical calculation in
theory of superparamagnetism.
2. The changes in volume effect of MT after the heat treat-
ment, in which the alloys have the minimum width of
temperature hysteresis, are established. In this case, the
minimum volume effect of martensite transformation
takes place after TMT in a parallel magnetic field, which
is associated with dispersion hardening of the alloy,
accompanied by a decrease in precipitated ferromagnetic
particle size and an increase in particles number per unit
volume in relation to other TMT regimes.
Acknowledgements This research was supported by the laboratories
of the Institute of Magnetism, the National Technical University of
Ukraine “Igor Sikorsky Kyiv Polytechnic Institute” and Azerbaijan
State University of Oil and Industry.
Compliance with ethical standard
Conflict of interest The authors declare that none of the authors have
any competing interests in the manuscript. On behalf of all authors, the
corresponding author states that there is no conflict of interest.
Applied Nanoscience

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