Journal of Alloys and Compounds 823 (2020) 153765

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Journal of Alloys and Compounds

journal homepage: http://www.elsevier.com/locate/jalcom

Designing new quasicrystalline compositions in Al-based alloys

Witor Wolf a, Claudemiro Bolfarini b, Claudio S. Kiminami b, Walter J. Botta b, *
a ^nio Carlos, 6627, Belo Horizonte, MG, 31270-901,
Departamento de Engenharia Metalúrgica e de Materiais, Universidade Federal de Minas Gerais, Av. Anto
Brazil
b
Departamento de Engenharia de Materiais, Universidade Federal de Sa~o Carlos, Rod.Washington Luiz, Km 235, Sa ~o Carlos, SP, 13565-905, Brazil

a r t i c l e i n f o a b s t r a c t

Article history: In the present work, we present and discuss the most important results that were obtained in the past
Received 26 September 2019 few years related with the development of new quaternary quasicrystalline alloys and composites. We
Received in revised form present the alloy design strategies that we have used and that led to the discovery of over 60 new
18 December 2019
quasicrystalline compositions, 2 new quasicrystal-forming systems and 1 new Al-matrix composite. New
Accepted 8 January 2020
Available online 9 January 2020
results are also presented and discussed here. Results of interest discussed in this work include: reas-
sessment of quasicrystal and approximant phase formation on the AleCoeFeeCr system; influence of Cr
and Ni additions on the icosahedral AleCueFe quasicrystal stability; discovery of a decagonal AleNieCo
Keywords:
Quasicrystals
eCr quasicrystal; composition range of formation of the decagonal AleCueFeeCr quasicrystal using
Al alloys combinatorial strategies; fabrication of aluminum matrix composites reinforced with quasicrystals using
Alloy design conventional metallurgy fabrication methods.
Al-matrix composites © 2020 Elsevier B.V. All rights reserved.

1. Introduction performed full structural and microstructural characterization in

Quasicrystalline (QC) and approximant phases present distinct
physical and mechanical properties associated with the complexity
of their unit cell, typically containing large number of atoms [1].
Properties such as low thermal conductivity, low friction coefficient
and wear resistance (despite brittle behavior) attracted important
efforts in the development of alloys containing such phases for
protective coating applications [2e6]. One of the main challenges to
design, or discover, new QC-forming alloys are related to the nar-
row composition ranges, in which such phases form and/or are
stable [7]. In our group we have revisited different Al-based alloys,
known to form QC phases, to study the effects of alloying and
metastable processing on the formation of new QC or approximant
phases [2,8e12]. We have also designed Al-matrix composites
reinforced with QCs [13e15].
The systems we have studied are AleCueFe, AleCueFeeCr,
AleCueFeeNi, AleNieCo, AleNieCoeCr, AleNieCoeCu, AleFeeCr-
(M ¼ Ce,Ti,Mn,V) and AleCoeFeeCr. Processing routes that we have
approached includes melt-spinning, gas-atomization, HVOF spraying,
arc melting, powder metallurgy and magnetron sputtering. We have
several compositions, which led to discovery of over 60 new QC-
forming alloys and 2 new QC-forming metallic systems (Al-Cu-Fe-
Ni and AleNieCoeCr) [8,10,11]. We have also discovered the first
metallic system, AleCueFeeCr, forming QCs embedded in Al-FCC
matrix which can be fabricated by conventional metallurgical fabri-
cation processes [13]. In addition, functional properties such as fric-
tion coefficient, wear resistance and thermal conductivity were
assessed in coatings fabricated by HVOF [2]. Mechanical properties of
composites were evaluated as well [14,15]. We also suggested and
applied combinatorial strategies, involving magnetron co-sputtering
and high-throughput XRD and EDX analysis, to map and design new
QC compositions in the AleCueFe and AleCueFeeCr systems [11].
We present the rationale behind the alloy design strategies that we
have used in the development of new quaternary QC alloys. New re-
sults are also presented and discussed here, which includes QC phase
formation on arc-melted AleCueFeeCr and on melt-spun
AleNieCoeCu alloys. In addition we show the as-cast microstruc-
ture of the Al85Cu6.75Fe3.375Cr4.875 alloy, the first conventionally casted
alloy forming a composite microstructure containing QCs and Al-FCC
(such microstructure only forms after an appropriate annealing) [13].

* Corresponding author.
E-mail addresses: witorw@gmail.com (W. Wolf), cbolfa@ufscar.br (C. Bolfarini),
kiminami@ufscar.br (C.S. Kiminami), wjbotta@ufscar.br (W.J. Botta).

https://doi.org/10.1016/j.jallcom.2020.153765
0925-8388/© 2020 Elsevier B.V. All rights reserved.
2 W. Wolf et al. / Journal of Alloys and Compounds 823 (2020) 153765

2. Designing new quasicrystalline compositions
2.1. Revisiting QC forming systems
QCs were first reported by Daniel Shechtman in an AleMn melt-
spun alloy [16]. Although refuted at first, his discovery led to huge
efforts in the sense of understanding their atomic structure and
physical properties.
Since this first metallic QC-forming system, many others have
been discovered, most of them Al-based, such as AleCueFe,
AleCueFeeCr, AleNieCo, AleFeeCr-(M ¼ transition metal),
AlePdeMn, AleMneSi, AleLieCu among others [17e24]. Some QC
phases are considered thermodynamically stable while others can
only be obtained with metastable processing routes.
The interest on stable QCs is related to the ability to fabricate
them using conventional casting techniques. In the past few years,
our work has been focused on developing new QC alloys, based on
traditionally known QC forming systems by adding alloying ele-
ments on them. Table 1 shows the previously known QC systems
that we have revisited, the chemical compositions we fabricated,
processing routes used and the phases that were obtained. In this
table we did not add the AleCueFeeCr system because, although
this system was already known to form QCs, we have made an
extensive work on it to find its compositional range of formation
and thus it will be discussed in more detail in the sequence. The
references where phase formation, shown in Table 1, can be found
are in the Table’s 1 legend. XRD patterns of alloys that have not
been published yet are available in Supplemental Material.
Three ternary systems have been studied and formation of QC
was observed in all of them, as expected from previously published
studies. High energy ball milling to alloy Al, Cu and Fe requires
posterior annealing to form QCs. We confirm the influence of
cooling rates on the icosahedral phase formation from the
AleCueFe system, which is favored by high cooling rates, > 104  C/
s. In the supplemental material, three XRD patterns of an
Al65Cu22.5Fe12.5 alloy fabricated in three different processing con-
ditions (a 10 g arc-melted button, a melt-spun ribbon and a 1 mm
arc-melted thick plate sample that was Cu-quenched) are shown.
The cooling rates in each case were in the range of 102  C/s, 106  C/s
and 104  C/s respectively and it can be observed that the relative
peak intensity of the QC phase increases with increasing cooling
rates. This was expected as reported in previous studies [17,25].
These cooling rates values were calculated using the same pro-
cedure of reference [26]. The AlePdeMn alloy studied easily
formed a QC phase even for a sample which solidified with cooling
rates in the range of 102  C/s. However, the presence of high Pd
contents is a huge obstacle for applying this QC system due to its
cost. The AleNieCo alloy formed a decagonal QC with some AleNi
based intermetallic phases. High cooling rates did not prevent
formation of such phases, as opposed to what was observed in the
AleCueFe alloys. This can be observed by comparing the XRD
pattern of this ternary alloy fabricated by melt-spinning (see
Ref. [10]) and by arc-melting a 1 mm thick plate sample that was
Cu-quenched (see Supplemental Material).
The quaternary system AleCoeFeeCr was studied aiming ap-
plications as thermal barrier coatings. The literature information
about the most famous alloy of this system, Al71Co13Fe8Cr8, was
somewhat contradictory. We showed, by fabricating this alloy with
different processing routes, that the microstructure of as-cast
samples is always composed by a hexagonal, m-Al5Co2, and a
monoclinic Al13Co4 phases. Both are QC approximants and exhibit
interesting physical properties for application as protective coat-
ings. Aiming to find new QC compositions, two other alloys from
this system were fabricated by rapid solidification processes.
However, no QC phases were found. The chemical compositions
were selected based on the valence electron concentration (e/a)
which would be closer to the usually found on ternary QCs [27],
which however, was unsuccessful.
2.2. Designing new quaternary QC alloys based on AleCueFe and
AleNieCo systems
From the systems studied in Table 1, two were selected based on
the ability to form QCs and costs related to the alloying elements.
These systems were AleCueFe and AleNieCo. Based on selected
ternary compositions, we have systematically added Cr and Ni on
the AleCueFe system and Cr and Cu on the AleNieCo system
aiming to retain the QC atomic structure even after the alloying
additions. The choice of chemical composition of each alloy was
based on trying to increase the fourth element fraction and
selecting values of valence electron concentration (e/a) as close as
possible to the values found for AleCueFe and AleNieCo QCs.
Table 2 shows the quaternary alloys that were studied, including
the fabrication processes and the phases identified. The references
where details about phase formation, shown in Table 2, can be
found are in the Table’s 2 legend. XRD patterns of alloys that have
not been published yet are available in Supplemental Material.
Cr addition on the AleCueFe QC leads to a gradual change on

Table 1
Previously known QC-forming systems that we have revisited with their chemical compositions, processing routes used, and the phases obtained. Results taken from ref-
erences: [2,9,10,12,15].

Metallic system Alloy Processing route Phases

AleCueFe Al65Cu20Fe15 High energy ball milling Al, Cu, Fe, q-Al2Cu
Arc-melting þ annealing at 700  C i-QC
Al65Cu22.5Fe12.5 Arc-melting i-QC þ b-AlCu(Fe) þ l-Al13Fe4 þ Al2Cu
Melt-spinning i-QC þ t-AlCu(Fe)
1 mm plate - Cu-quenched i-QC þ t-AlCu(Fe)
AlePdeMn Al70.5Pd21Mn8.5 Arc-melting i-QC
AleCoeFeeCr Al71Co13Fe8Cr8 1 mm plate - Cu-quenched m-Al5Co2 þ M  Al13Co4 þ Cr-rich-unknown
Melt-spinning m-Al5Co2 þ M-Al13Co4
Gas-atomization m-Al5Co2 þ M-Al13Co4
Gas-atomization þ annealing at 1000  C m-Al5Co2
HVOF m-Al5Co2 þ M-Al13Co4
Al77Co11Fe6Cr6 1 mm plate - Cu-quenched M  Al13Co4 þ OeAl13Co4
Melt-spinning M  Al13Co4 þ OeAl13Co4 þ YeAl13Co4
Al76Co19Fe4Cr1 1 mm plate - Cu-quenched M  Al13Co4 þ Al9Co2
Melt-spinning M-Al13Co4
AleNieCo Al71Ni20Co9 Melt-spinning d-QC þ Al3Ni(Co) Al3Ni2(Co)
1 mm plate - Cu-quenched d-QC þ Al3Ni(Co) Al3Ni2(Co)
 W. Wolf et al. / Journal of Alloys and Compounds 823 (2020) 153765
Table 2
New quaternary alloys that were studied, including the fabrication processes used and the phases observed [8,10,11].
Metallic system Alloy
AleCueFeeCr Al65Cu22Fe10Cr3
Al67Cu20Fe5Cr8
AleCueFeeNi Al63Cu18Fe10Ni3
Al64Cu20Fe13Ni9
AleNieCoeCr Al72Ni19Co7Cr2
Al72Ni20Co5Cr3
AleNieCoeCu Al71Ni20Co7Cu2
Al70Ni20Co5Cu5
the atomic structure of the QC phase. Small additions, ~3 at. % Cr
results in the coexistence of the icosahedral and decagonal QCs,
with some presence of the cubic t-AlCu phase when the alloy is
fabricated using lower cooling rates, as shown in the XRD pattern in
Supplemental Material. Fig. 1 shows an energy dispersive X-ray
spectroscopy (EDX) mapping of a melt-spun Al65Cu22Fe10Cr3 alloy,
which forms an icosahedral QC with small amounts of the deca-
gonal QC (Cr-enriched). More details of this alloy’s phase formation
and characterization can be found in Ref. [8].
Increasing Cr content above a certain limit leads to only one QC
phase, with decagonal structure. The Al67Cu20Fe5Cr8 alloy was
processed by fast and low solidification methods and in all the
experiments, a decagonal phase co-existed with a cubic phase, with
the same structure of the t-AlCu(Fe) phase forming in ternary rapid
solidified AleCueFe QC forming alloys. The same cubic phase was
observed in Ref. [28]. Fig. 2a shows an EDX mapping of a melt-spun
Al67Cu20Fe5Cr8 alloy, which is formed by a decagonal QC matrix
with the presence of the t-AlCu(Fe) phase (phase enriched in Cu)
forming at the grain boundaries. Details of this alloy’s phase for-
mation can be found in Ref. [8]. In Fig. 2b, the same EDX mapping
analysis-type was performed in the ternary melt-spu-
nAl65Cu22.5Fe12.5 alloy which has an icosahedral QC matrix but also
forms the t-AlCu(Fe) phase, in the same way observed in the
quaternary alloy. Fig. 2c shows a TEM bright-field micrograph and
the selected area electron diffraction pattern (SAED) of this t-
AlCu(Fe) phase taken along the [111] zone axis, from the ternary
alloy. This phase is cubic with a CsCl-type structure and lattice
parameter a ¼ 2.94 Å. Fig. 2d shows the icosahedral QC phase, with
the respective SAED, taken along the 5-fold axis of rotational
Fig. 1. STEM EDX mapping from the Al65Cu22Fe10Cr3alloy. The matrix is the icosahedral
QC and the Cr-rich phase is the decagonal QC. Details of the phase formation in this
alloy can be found elsewhere [8].
3
Processing route Phases
Melt-spinning i-QC þ d-QC
1 mm plate - Cu-quenched i-QC þ d-QC þ t-AlCu(Fe)
Arc-melting þ annealing at 600  C d-QC þ t-AlCu(Fe)
Melt-spinning d-QC þ t-AlCu(Fe)
Melt-spinning i-QC þ 2 B2 cubic phases þ l-Al13Fe4
Melt-spinning i-QC þ 2 B2 cubic phases
Melt-spinning d-QC þ d-QC(Cr-rich) þ Al3Ni(Co) Al3Ni2(Co)
Melt-spinning d-QC þ d-QC(Cr-rich) þ Al3Ni(Co) Al3Ni2(Co)
Melt-spinning d-QC þ Al3Ni(Co) Al3Ni2(Co)
Melt-spinning d-QC þ Al3Ni(Co) Al3Ni2(Co)
symmetry. The bright-field micrograph was taken from the QC
phase oriented in the 5-fold symmetry axis.
In addition to the interesting results we obtained regarding the
relatively easiness of fabricating QCs in the quaternary
AleCueFeeCr system, formation of QC phases in this system has
also been reported by other authors and with a number of different
atomic compositions [6,29e35]. This motivated an extensive study
we performed using combinatorial strategies [11]. This included
fabrication of compositional libraries by magnetron co-sputtering
of Al, Cu, Fe and Cr targets on a Si wafer, which produced sam-
ples with gradient composition containing hundreds of alloys from
this system. The samples were than characterized by scanning X-
ray diffraction and EDX with fast data acquisition to identify phases
in the libraries. Using this strategy, we were able to screen the
decagonal QC range of formation on the AleCueFeeCr system for
Al atomic contents from 65 to 70%. We have studied over 300
different alloy compositions and found 59 new decagonal QC
dominant compositions. The QC composition range of formation
can be found in Wolf et al. [11].
On the other hand, Ni additions on the AleCueFe QC did not
lead to formation of a decagonal QC. We found that the icosahedral
QC can dissolve up to 4 at. % Ni in its atomic structure. However,
additions superior to that led to destabilization of the QC in favor of
a B2 cubic phase, which was the major phase in the higher Ni-
containing alloy, Al64Cu20Fe13Ni9.
It is also interesting to comment on the morphological differ-
ences that QC phases can be produced, which strongly depends on
the cooling rates applied during solidification and on the QC atomic
structure. For instance, the AleCueFe icosahedral QC can be formed
with a nanometric QC grain size, if fast cooling rates are applied
(Fig. 2d), or it can form an envelope-like and micrometric grain-
sized microstructure, which is a consequence of the peritectic re-
action that results in its formation under low cooling rates during
solidification [17]. The AleCueFeeCr decagonal QC also forms as
nanometric QC grains if fast cooling rates are applied (Fig. 2a) or it
forms as elongated micrometric-sized columnar grains if low
cooling rates are applied [11].
Cr addition on the AleNieCo decagonal QC led to discovery of a
new quaternary QC, also decagonal, which formed in two melt-spun
alloys. The composition of this phase was measured by EDX and it
was found to be Al78.2Ni8.7Cr10Co3.1. However, the alloys studied also
formed two AleNi based intermetallic phases, even when applying
rapid solidification processes. The thermal stability of this new QC
continues for future elucidation. Cu additions enhanced interme-
tallic phase formation in detriment of the QC phase. This can be seen
in the XRD patterns of melt spun Al71Ni20Co7Cu2 and Al70Ni20Co5Cu5
alloys, shown in the Supplemental Material. If compared to XRD
patterns of the AleNieCoeCr melt spun alloys (see Ref. [10]), the Cu-
containing alloys show significantly higher contents of Al3Ni and
Al3Ni2 phases. For this reason, this system was the less promising
one and was not further studied.
4 W. Wolf et al. / Journal of Alloys and Compounds 823 (2020) 153765
Fig. 2. (a) EDX mapping of a melt-spun Al67Cu20Fe5Cr8 alloy, showing the t-AlCu(Fe) phase, which is located in the Cu-rich regions. (b) EDX mapping from the ternary melt-spun
Al65Cu22.5Fe12.5 alloy also showing the t-AlCu(Fe) phase. (c) Bright-field TEM micrograph of the ternary alloy with a SAED pattern of the t-AlCu(Fe) phase taken along the [111] zone
axis. (d) Bright-field TEM micrograph of the ternary alloy showing the icosahedral QC and the SAED pattern taken along the 5-fold axis.
The design strategies used here to produce new QC composi-
tions proved to be efficient and led to the discovery of more than 60
new QC-based alloys. The main idea behind this strategy is: define a
ternary QC to be used as a base alloy. Using empirical QC-forming
rules, such as the valence electron concentration, add a fourth
element in different proportions. Applying rapid solidification
fabrication processes is the most adequate way to produce the
quaternary alloys, because since QCs usually form around several
intermetallic phases, whose formation can be suppressed by fast
cooling rates. If this fourth element addition leads to QC formation,
then this quaternary system is a potential candidate for the second
step of the alloy design. This second step would be applying a
method, in which the fabrication and characterization of hundreds
of alloy compositions can be performed so that the compositional
range where the quaternary phase can be fabricated will be dis-
closed. This can be done by magnetron co-sputtering [36e38] or by
using diffusion multiples [39].
3. Al-matrix composites reinforced with quasicrystals
In addition to discovering new QC forming compositions, our
research has also focused on developing Al-matrix composites rein-
forced with QCs. Although QCs show remarkable functional physical
properties that could be used for tribological protection [40,41], their
inherent brittleness makes their use very limited. To overcome this
difficulty, QC phases must be embedded in a ductile matrix.
There are two traditional methods to produce such composites.
The first one involves rapid solidification techniques, such as melt-
spinning, Cu-mold quenching and gas-atomization [14,22,42e45]
and can lead to the fabrication of composites reinforced with
nanosized QCs, which is very interesting and can result in high
strength composites. The main drawbacks are related to the com-
plex fabrication processes needed and the fact that QCs forming in
these systems are metastable and usually transform to crystalline
phases after heating around 350e500  C. The second way to
fabricate these composites is based on powder metallurgy [15,46].
This process allows fabrication of composites reinforced with stable
QCs, however, nanosized QC particles embedded in the ductile
matrix are hard to be obtained.
Following the results obtained in our combinatorial studies of
the AleCueFeeCr system and from literature data regarding pre-
viously published AleCueFeeCr QC compositions, we have devel-
oped an Al-matrix composite reinforced with QCs by arc-melting an
Al85Cu6.75Fe3.375Cr4.875 alloy and subsequently annealing it at
600  C. The details of the annealed alloy’s microstructure and
fabrication can be found in Ref. [13]. This was the first time such
microstructure could be obtained by conventional fabrication
methods. Here we will show the details of the as-cast alloy, which
was the precursor of the QC composite. Fig. 3 shows the XRD
pattern and SEM micrograph of the Al85Cu6.75Fe3.375Cr4.875 arc-
melted alloy in the as-cast condition. The XRD pattern of the as-
cast sample is very different from the one of the annealed sam-
ple, from Ref. [13].
In the as-cast sample, the decagonal QC could not be identified
and intense peaks of the Al2Cu phase can be seen. The XRD pattern
also show some peaks of the Al7Cu2Fe phase. The Al-FCC phase can
be seen in the SEM micrograph (phase with the darker contrast)
and the Al2Cu is observed, forming an eutectic constituent with the
Al-FCC phase. In addition, a third phase (the one with intermediate
contrast) seems to solidify with acicular morphology. EDX analysis
was performed in this phase showing an average atomic compo-
sition of Al80.79±0.27Cu2.05±0.11Fe5.16±0.52Cr12.0±0.35. This is an
AleFeeCr-based phase and its atomic structure could not be
identified with the analysis performed in this work. The AleFeeCr
phase diagram [47] shows the formation of a significant number of
complex ternary phases around this composition and its proper
identification would require an extensive electron diffraction
analysis (which was not done for this work).
Fig. 4 shows the results from DSC analysis of the arc-melted
sample in the as-cast and after annealing (at 600  C, see Ref. [13])
conditions; both curves are shown in the same scale for compari-
son. It is interesting to note that in the as-cast condition, an intense
 W. Wolf et al. / Journal of Alloys and Compounds 823 (2020) 153765
Fig. 3. XRD pattern and SEM micrograph of the Al85Cu6.75Fe3.375Cr4.875 arc-melted alloy in the as-cast condition.
Fig. 4. DSC analysis of the as cast and annealed Al85Cu6.75Fe3.375Cr4.875 arc-melted
alloy.
endothermic peak around 550  C is found, which is due to the
eutectic AleAl2Cu reaction (see Fig. 3). This peak practically van-
ishes after an annealing at 600  C for 10 h. The microstructure of the
annealed sample is shown in Ref. [13]. In the annealed sample, no
eutectic constituent was observed, and the dominant phases are Al-
FCC and the decagonal QC. These results show that, during the
annealing of the Al85Cu6.75Fe3.375Cr4.875 arc-melted alloy, there was
liquid phase formation (from the eutectic constituent) which
reacted with the AleFeeCr-based phase (Fig. 3) leading to a Cu
enrichment of this phase and then resulting in the QC phase after
the completion of the reaction. The high-Cu content of this liquid
phase lead to formation of the Al7Cu2Fe after the QC phase reached
its maximum Cu solubility and this phase was formed at the in-
terfaces of the QC-Al-FCC phases (see Ref. [13] for further details).
Thus, such QC composite can now be fabricated using simple
fabrication processes that are low-cost and allow fabrication of
large volume ingots containing this microstructure, which previ-
ously was only possible using expensive and non-conventional
fabrication processes.
4. Conclusions
In this work we present and discuss a successful alloy design
5
approach that can be applied for the discovery of new QC alloys.
Among the studied QC forming systems, AleCueFeeCr was the
most promising one. QCs can be formed in this system over large
composition ranges, it forms under fast or slow solidification con-
ditions and has an equilibrium phase field with Al-FCC, which al-
lows the fabrication of composites containing both phases by
conventional casting.
Due to the large number of known ternary QC-forming systems,
future applications of the here proposed strategy for alloy design
will certainly lead to discovery of new Al-matrix composites rein-
forced with QCs that can be fabricated in the same way as the
AleCueFeeCr system.
Authors contribution statement
W.W., C.B., C.S.K and W.J.B designed the study. W.W. fabricated
and characterized the samples. All authors contributed on data
analysis, discussing and manuscript writing.
Declaration of competing interests
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgments
The authors are grateful for the financial support granted by
FAPESP (processes n 2016/19314e3, n 2015/09008e0 and n
2013/05987e8), Coordenaça ~o de Aperfeiçoamento de Pessoal de
Nível Superior - Brasil (CAPES) - Finance code 001 and CNPq. The
authors are also grateful for the technical assistance on TEM, SEM
analysis and sample preparation from Laboratory of Structure
Characterization of Federal University of Sa ~o Carlos (UFSCar). Au-
thors are also grateful for all the collaborators that were involved in
the course of this research and played an important role for its
success.
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.jallcom.2020.153765.
6 W. Wolf et al. / Journal of Alloys and Compounds 823 (2020) 153765

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