Overcoming the strength-ductility paradox of FCC materials by defect

healing (SPD)
A brief literature review and future work
Submitted by - AKASH KUMAR RAM (19106004)
M.Tech IIT KANPUR

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 Content
1. Abstract----------------------------------------------------------------------------------------------03

2. Introduction-----------------------------------------------------------------------------------------05

3. Severe Plastic Deformation (SPD) Processes-------------------------------------------------07

3.1 Constrained groove pressing (CGP)--------------------------------------------------------08

4. Properties of CGP Processed materials-------------------------------------------------------10

4.1 Mechanical properties-----------------------------------------------------------------------10

4.2 Microstructural change ----------------------------------------------------------------------12

5. Factors affecting the ductility of SPD processed materials--------------------------------

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6. Heat treatment process --------------------------------------------------------------------------15

6.1 Recovery and recrystallization--------------------------------------------------------------16

6.2 Effect of annealing on mechanical properties of CGP Processed materials----------17

6.3 Effect of annealing on microstructure of CGP Processed materials-------------------18

7. Conclusion ------------------------------------------------------------------------------------------19

8. Future Work----------------------------------------------------------------------------------------19

9. References-------------------------------------------------------------------------------------------20

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 1. Abstract

The paradox of strength and ductility is now well established and denotes the difficulty of
simultaneously achieving both high strength and high ductility. It is well known that any
conventional metal forming processes such as rolling, extrusion, drawing etc and SPD
can increase strength of metals with decrease in ductility.
Nanostructured metallic materials having Nano-crystalline and ultrafine-grained
structures show exceptional mechanical properties, e.g. superior strength, that are very
attractive for various applications. However, super strong metallic nanomaterials
typically have low ductility at ambient temperatures, which significantly limits their
applications. These two properties are generally mutually exclusive. In this survey we
will be dealing with SPD processed FCC materials. SPD methods produce ultra-fined
grain in materials.
UFG materials has excellent mechanical properties which are used in structural
applications. In this work we will try to demonstrate the possibility of tailoring the
microstructures of material by defect healing to obtain both high strength and high
ductility. Materials with such desirable mechanical properties are very attractive for
advanced structural applications. Here we will discuss about the factors affecting ductility
of SPD processed materials and some basic strategies to overcome the strength-ductility
paradox.

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Fig.1 Rank of the countries according to a the total number of publications in the field of SPD and b the
citations to the published articles during 2008–2018 based on different criteria

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 2. Introduction

SPD methods produce ultrafine-grained (UFG) structures demonstrate unique

mechanical, chemical and physical properties that are of utmost interest for a wide range
of applications. In particular, UFG in metallic materials typically show superior strength,
superior hardness and enhanced wear resistance due to the nanoscale and interface
effects.
Large severe plastic deformation mostly introduces high angle grain boundaries. In
addition to creating ultrafine grains, the SPD process also introduces high densities of
dislocations and internal elastic strains. The processing of metals through the application
of severe plastic deformation (SPD) has now become a major tool for producing bulk
solids with ultrafine grains (UFG), where these grains are within the sub-micrometer or
even the nanometer range.
The primary advantage of producing UFG materials is that, as a consequence of the Hall-
Petch relationship in which the yield stress varies inversely with the square root of the
grain size. The strength of the metal is increased when the grain size is reduced. But
conversely the overall ductilities or elongations to failure are generally very small in
UFG metals, thereby leading to the maxim that “materials may be strong or ductile, but
rarely both at once”.
The loss in ductility at small grain sizes is due to the low rate of strain hardening and the
low strain rate sensitivity, m. If the rate of strain hardening is high, dislocations are able
to accumulate within the grains so that, when combined also with a high value of m, the
onset of necking or localized deformation is delayed. However, in UFG metals, the very
small grains preclude a capability for storing dislocations and instead the dislocations
move through the grains and are absorbed at the grain boundaries. This leads to a low rate
of strain hardening so that the elongations to failure are very limited even for metals that
are inherently ductile when tested with conventional coarse grain sizes.

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Fig:2 The extraordinary combination of high strength and high ductility in metals processed by SPD

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 3. SPD Processes

Any method of metal forming under an extensive hydrostatic pressure that may be used
to impose a very high strain on a bulk solid without the introduction of any significant
change in the overall dimensions of the sample and having the ability to produce
exceptional grain refinement is called severe plastic deformation process (SPD). These
techniques became great popularity because of their ability to produce considerable grain
refinement in fully dense, bulk scale work pieces, thus giving more promise for structural
applications. There are many SPD process such as Equal channel angular pressing
(ECAP), High pressure torsion (HPT), Constrained groove pressing (CGP) etc.

ECAP
Equal-channel angular pressing is the most highly developed SPD processing technique.
When the billet passes through the area where the two channels meet, there is an
introduction of a simple shear strain. The cross sectional dimension of the billet remains
constant. Therefore, the process permits repetitive pressing which leads to accumulation
of very large strains. There are some different variants of ECAP processes based on the
rotations of the billet about the pressing axis between the passes are generally leads to
different results in terms of the microstructure and texture produced.

HPT
High pressure torsion involves a combination of high pressure with torsional straining.A
main disadvantage of this method is that only small coin shaped samples can be
processed, which is typically 10–15 mm in diameter and 1 mm in thickness. The HPT
process is primarily used for research purposes due to size restriction. Another important
issue on HPT is non-uniformity in deformation.

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 3.1 Constrained Groove Pressing (CGP)
In this technique, the sheet sample is subjected to repetitive shear deformation via
alternant pressings by asymmetrically groove dies and flat dies. Thus, a large strain can
be uniformly accumulated throughout the whole sample without any significant change in
its dimensions. As a result, a relatively homogeneous UFG structure can be obtained.
There is a catch in the conditions involving the sample thickness and the dies used. The
gap between the upper and the lower die is similar to the sample thickness, which is
under processing, also the angle of the groove is kept at 45° but it can be altered
according to the aim and focus of the experiment.
This situation results in pure shear deformation at the inclined regions of the sample,
under plane strain condition. A small groove width and tight constraint indeed enhance
the strain accumulation. However, due to more severe plastic deformation induced under
this condition, initiation and propagation of micro-cracks occur much earlier, and
consequently, the effective pass number is limited. The pass number in this study is
increased by the reduction of either groove angle or friction coefficient.

Fig:3 Conventional Structure of grooved CGP die

There are primarily four steps involved in producing a single pass CGP processed metal
sheet sample. The first step involves pressing the work-piece between the symmetrical
grooved dies, which have a gap equal to the sample thickness and groove angles of 45°
(standard). If we look closely at the structure of the grooved dies, it can be observed that
there are inclined regions as well as flat regions in the teeth of the dies as seen in figure 3.
Every time a sample is pressed between the grooved dies, an effective strain of 0.58 is

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imposed on the inclined region, under plane strain condition. Meanwhile, the flat region
on the sample does not go under any kind of deformation. This generates a non-uniform
strain distribution in the sample as can be seen by the hatched region of figure 4(b). The
second step involves removing the sample from the grooved dies and placing it between
the flat dies while keeping the orientation similar to the previous press. The sample is
now pressed between the flat dies. This step results in adding an additional value of 0.58
effective strain in the opposite direction. Thus the total effective strain now after the
flattening step is 1.16 as shown in figure 4(c) (hatched regions).

Subsequently, after the straightening, the specimen now is turned by 180° about the axis
perpendicular to the plane of the sample. This step ensures that an overall strain of 1.16 is
attained in the undeformed (unhatched) region by further pressing of the sample using the
grooved die and then by the flat die (figure 4 (e)-(f)). An effective strain of 1.16 is
expected to be uniformly attained throughout the specimen. So a total of four steps are
involved in obtaining a uniform strain value throughout the sample as depicted in figure
4. This complete set of steps constitute a single pass of CGP process.

Fig:4 Schematic of constrained groove pressing (CGP)

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 4. Properties of CGP Processed materials

Constrained groove pressing or CGP has proven time and again to improve the
mechanical properties of the material under processing. The major properties affected by
this process are ultimate tensile strength (UTS), yield strength (YS), mean hardness, and
ductility of the material. Improvements have been reported in the properties like strength,
yield strength, and hardness for CGP processed materials. The major reasons behind
these improvements in properties have been explained by the increasing dislocation
density in the heavily deformed materials by this process .The increased dislocation
density is due to the increased the number of dislocation. As the number of dislocations
increase, their motion through the material gets restricted due to repulsion among
themselves and greater strength is required to perform further deformation. This trend of
increase in strength and hardness due to increase in dislocation density is consistent
across all SPD processes.

4.1 Mechanical Properties

Strength and ductility are the most primary parameter of a material, which will assign all
other mechanical characteristics. These properties are grain-size dependent because it is
more affected by SPD process than any other mechanical properties. Moreover, many
properties are directly governed by strength and ductility. Improving strength and
ductility at the same time is considered as a very challenging task.
According to Hall-Petch relation in which the yield stress varies inversely with the square
root of the grain size thus strength of the metal is increased when the grain size is
reduced.
While increase in strength there will be loss of ductility. Combination of high flow stress
and low strain-hardening capability is the main reason for loss of ductility.
CGP has been used in the study of many metals and alloys to further expand the
understanding on the improvements and revision of the mechanical properties.

In the study of CGP for sheet metals, the literature by Amit et al. [1] explained the
improvements in the mechanical properties namely - tensile strength, yield strength, and
hardness by showing results for metals like aluminium, copper, low carbon steel, nickel,
and titanium.
It was also observed that these properties showed a very minor increase in the values
when the specimens were subjected to a second pass and subsequent passes resulted in
decreasing the YS and UTS [1]. The improvement in the first and second pass was due to
the refinement of the microstructure. All the observations in this study showed a drastic
decrease in the elongation property of the material under processing. The reason behind
this decrease in ductility can be attributed to the insufficiency in the movement of the
dislocations and decreasing strain hardenability in the material [1]. CGP also introduces
micro-cracks and voids in the material while processing and when the processed samples
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are introduced to further load, these cracks and voids start to expand and result in pre-
mature failure leading to decreased ductility of the material.

Fig:5 The diagram showing the strength–ductility paradox

Fatigue and creep behavior

Fatigue strength of UFG materials are very high as crack propagation become very
difficult by large number of grain boundaries. It is noticed that the creep behavior
strongly depends on number of passes, a decrease in the creep resistance on every
successive pass. It is due to the number of factors including microstructural changes,
homogenization of the microstructure and Nano-porosity induced by ECAP.

Thermal stability
In most of the cases, thermal stability is a vulnerable point of many SPD-treated
materials. For example, SPD processed pure oxygen-free copper provides poor thermal
stability. It has a tendency to recover during storage even at room temperature because
during severe straining, annihilation of excess dislocations accumulated.

Corrosion resistance
Corrosion in single-phase polycrystalline metals is mainly depending upon grain size and
SPD processed strengthening mechanism should deteriorate the corrosion behavior.
Investigations carried out on only ECAP-processed copper based on these aspects. In this
investigation, SPD process as a better conclusion. While increasing the mechanical

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characteristics does not compromise the overall corrosion resistance and improves the
SCC and corrosion fatigue resistance also.
4.2 Microstructural change

CGP processed samples have shown improvements in some mechanical properties while
deterioration in other properties of the materials and all of these can be related to the
effect and changes in the microstructure of the material under processing. The change in
the microstructure is the major reason that contributes in the change of properties.
Generally the starting material i.e. before the material has been processed by CGP, has a
coarse microstructure. The coarse structured materials show very high ductility with
ordinary strength and hardness values when compared to that of materials processed by
SPD techniques. CGP has shown promising results in refining the grain structure of the
sheet metals. The resultant grain sizes of CGP processed material are typically in the sub-
micro-meter range and in some cases even up to Nano-meter range. Microstructure and
grain size can also be altered by heat treatment or annealing the post processed materials
and will be discussed in the later sections.

As suggested in the literature by Amit et al. [1] significant grain refinement was observed
in the initial stages of pressing for all the sample by the dies. It was also noticed that as
the number of passes increased, the grain size decreased with each pass. The rate of
increase of deformation and dislocation density was high during the initial passes but
decreased in the subsequent passes [1]. As stated earlier, the grain size is inversely
proportional to deformation strain and the ensuing dislocation density. Thus a faster rate
of grain refinement was observed in the introductory stages of pressing and straining, also
very nominal grain refinement was observed at higher values of strain when the
dislocation density start to saturate. The grain refinement is expected to be uniform
during straining due to the increase in the dislocation density, but as the dislocation
density increases, the dynamic recovery also becomes more prominent. The rate of
dynamic recovery is directly proportional to the dislocation density which in turn is
directly proportional to the strain induced in the specimen.
Dynamic recovery results in the dislocation annihilation. Also the grain refinement is
prevented by the dynamic recovery as the grains try to lower their energy. As the strain
increases, dislocation density increases which boosts the rate of dynamic recovery and
this leads to the dislocation annihilation, which in turn, slows the rate of grain refinement
at higher strains [1]. Thus when the dislocation density and strain reaches a saturation
value the grain refinement and grain size also saturates as a balance between the
generation of dislocations and their annihilation due to dynamic recovery.

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Yadav et al. [2] also studied the microstructural changes for single pass CGP deformed
copper samples. The undeformed sample was reported to have approximate equiaxed
grains throughout the microstructure. The deformed samples were reported to have large
fraction of elongated grains. Through orientation imaging microscopy it was also
observed that large residual strain existed in 1 pass deformed sample which was related to
high number of unindexed points in the microstructure. Decrease in grain size was also
reported for 1 pass sample when compared to as received sample. Fractography results
for deformed tensile samples revealed the presence of micro-cracks and micro-voids for
longitudinal and transverse direction. These defects were attributed to the pre-mature
failure of the single pass CGP deformed material.

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 5. Factors affecting the ductility of SPD processed materials

The key factors that determine the ductility of Nano-structured materials include:

1. Testing conditions such as temperature, strain rate, specimen geometry for small non-
standard samples.
2. Microstructures, which are determined primarily by processing history.

Under certain condition the SPD processed materials show superplasticity but here we are
talking about the microstructure/texture produced by SPD processes that affect the
ductility of materials.
SPD can also lead to unusual phase transformation such as a dissolution or formation of
second phases, disordering, amorphization, providing different nanostructures such as
Nano-twins, non-equilibrium GBs, dislocation cells, solute clusters and segregations.
Such changes in material structure can affect the mechanisms of deformation and
fundamentally modify the material properties.
Below we outline four key nanostructural attributes in SPD-processed metals which are
the basis for their remarkable mechanical and functional properties-
 Structure of grain boundaries (GBs) in SPD processed material
 Formation of nano-twins
 Segregations in nanostructured SPD-processed material
 Precipitations of second phases during and/or after SPD

UFG materials contain non-equilibrium GBs with strain-distorted structure, which have
excessive Gibbs free energy, enhanced free volume and enhanced stresses associated with
the distortions of near-boundary region due to high density of GB dislocations which
leads in nucleation of cracks at GBs and thus ductility decreases.
Indeed strain hardening mechanisms associated with the accumulation of dislocation may
not be effective in ultra-fine grains. The low strain hardening leads to low ductility in
UFG materials.

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 6. Heat Treatment

CGP introduces massive strain in the material which decreases the grain size and
increases the strength and hardness of the material. As stated earlier this increase in the
strength compromises the elongation property of the material and the material tends to
fail prematurely. This premature failure does not let the material use its complete work
hardening potential. The changes in the mechanical properties are accompanied by an
increase in the dislocations and microstructural defects i.e. micro-cracks and micro-voids
in the material. These dislocations and microstructural defects initiate at the highest stress
concentration sites i.e. the grooves of the die in contact with the specimen plate. When
the material is subjected to increasing strain the dislocations continue to increase in
number and get tangled with each other.
This entanglement of dislocations makes the movement of dislocations very difficult in
the material. The current dislocation arrangement requires a greater force for any further
movement. This phenomenon increases the strength of the material because the material
now requires greater external push to flow. When the stress on the material increases, the
defects i.e. the micro-cracks and voids introduced earlier during CGP get active and start
to increase in concentration and size. As the applied stress on the material increases
continuously, the material begins to deform permanently and in the end, fails under the
applied load by the contribution of the microstructural defects as stated earlier. This
premature failure of the material can be delayed by increasing the degree of softening
through reduction in the size and number of microstructural defects in the material. The
reduction can be combined to say that the material is being healed of these
microstructural defects.
The easiest way suggested for this ‘healing’ to occur is by annealing the already
deformed material at a higher temperature for a limited time period. Also the focus of the
work here is to use annealing to initiate controlled recrystallization which leads to
microstructural defect healing and softening of the material, thus improving the overall
properties.

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 6.1 Recovery and Recrystallization

To restore the ductility or electrical conductivity of cold worked materials with

simultaneous decrease in hardness and strength a heat treatment process is done which is
called annealing. In this process of heat treatment material is heated for a certain time at a
temperature higher than 0.3-0.5Tm (above recrystallization temp) and then slow cooling is
done. This procedure helps in improving the ductility while it reduces the strength and
hardness to some extent of the already deformed material. There are several form of
annealing process based on range of heating temperature but for relieving the internal
stress and strain recrystallization annealing is done. There are mainly three stages of the
annealing process which are the process of recovery, recrystallization and grain growth
.
Recovery is the first phenomena that occurs in the process of annealing at lower
temperature. In the processes of recovery the annihilation of dislocation takes place
without the movement of GBs.
“Recrystallization is the process of formation of new strain-free grains from deformed
grain in a solid body by the movement of high angle boundaries which occurs at higher
temperature.” the process of recrystallization depends on many parameters such as time
and temperature of annealing, initial grain size of the material, amount of deformation
and impurities present in the parent material.

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 6.2 Effect of annealing on mechanical properties of CGP Processed
materials

As we know CGP processed materials have high strength and hardness due to grain
refinement. But ductility decreases with increase in strength and hardness. To recover the
ductility without significant decrease in strength controlled recrystallization is done by
annealing. So generally strength and hardness decreases with slightly increase in ductility
by the means of annealing.

In the literature by Amit et al. [1] it was observed that up to 400°C the strength was
preserved but as the annealing temperature was increased there was a decrease in the
strength of the material. Hardness values followed a similar trend as strength in this
study. After a certain range of temperature, there was a decrease in the hardness values of
the material. As the number of passes were increased, the observed strength showed a
drop while keeping the annealing time and temperature constant. This is explained by the
fact that as the accumulated strain gets added in the material, the driving force of
recrystallization increases leading to higher rate of restoration in the deformed sample.
Also the ductility was observed to increase with the continuous increase in annealing
time and temperature. This increase in ductility as compared to the prematurely failed
materials is due to the recrystallization occurring in the material leading to defect healing.

In the work by Yadav et al. [2], the major focus was on the improvements in the
mechanical properties by annealing the deformed samples for a short period of time at a
constant temperature. Hardness values were observed and they showed an increase when
it was only subjected to single pass CGP. As the samples were annealed, significant
decrease in the hardness values were observed with the increase in treatment time period.
The as-deformed and heat treated sample for lower time period showed premature failure
because of presence of micro-cracks and voids. As the treatment time of the samples
increased a decrease in the values of ultimate tensile strength and yield strength was
observed. As the treatment time increased, the ductility also increased for the deformed
sample and became constant after a certain treatment time. Toughness values initially
showed improvements but attained a constant value after a certain treatment time period.

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 6.3 Effect of annealing on microstructure of CGP Processed
materials

As discussed earlier, the process of CGP alters the microstructure of the material from a
coarser microstructure to a much finer range. This change in the microstructure is one of
the major reason for the improvement in the properties like yield strength, ultimate tensile
strength and mean hardness but this also results in the depreciation of the
ductile/elongation properties of the material. In the previous section it was shown from
the literature that the heat treatment of the deformed samples facilitates ductility but it
also diminishes the strength and harness to a certain extent. The heat treatment of
deformed samples induces transformation in the microstructure, which in turn, leads to
change in its properties. The improvement in ductility can also be linked to the alteration
in the microstructure due to the annealing of the deformed samples.

In the literature by Amit et al. [1], it was stated that one of the reasons for the possible
loss of strength and hardness can be the abnormal grain growth in the microstructure
observed at higher annealing temperature. Dissimilar grain sizes were observed due to
inhomogeneous strain distribution which led to varied driving force for recrystallization
in the material in the material. As the annealing temperature was increased, the
phenomena of recrystallization became more prominent as it was seen by increased grain
size.

The study of short heat treatment on CGP processed Cu-Zn sheet by Yadav et al. [2]
revealed that the CGP actually led to inhomogeneity in the microstructure and the
properties. After the heat treatment the fraction of <1° grain orientation spread (GOS)
was observed to increase with increasing treatment temperature until it became consistent
with the as-received material. This continuous increase in GOS hints at the phenomena of
recrystallization which reduces the residual strain in the deformed material. During the
onset of recrystallization a decrease in the grain size was observed. As the treatment time
was further increased the phenomena of grain growth occurs predominantly. Also the
fraction of LAGBs increased after single pass CGP due to drastic increase in the
dislocation density. Post heat treatment the fraction of HAGBs increase with increasing
annealing time due to decrease in dislocation density by recrystallization. It was
concluded that recrystallization led to microstructural changes which was also reflected
in the changed mechanical properties for the annealed samples as stated in the previous
section.

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 Conclusion
During the last three decades, severe plastic deformation has progressed as a novel
method to achieve nano/ultrafine- grained structure in a wide range of metallic materials.
SPD processes are very popular for producing ultra-fine grained materials with superior
mechanical properties.
large severe plastic deformation mostly introduces high angle grain boundaries. In
addition to creating ultrafine grains, the SPD process also introduces high densities of
dislocations and internal elastic strains.
As material is deformed strength decreases but decrease in ductility is seen. To get a
optimal combination of strength-ductility we do some heat treatment as a result new
strain-free equiaxed grains are formed.

Future Work
 CGP Process is to be done of samples

 Heat treatment to be done to the samples for different time length and temperature.

 Hardness and tensile strength is to be measured.

 Microstructural analysis of the samples.

 Optimization of strength and ductility of CGP processed samples.

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