Module 3

EFFECTS OF NEUTRON
IRRADIATION
 NEUTRON INTERACTIONS

Elastic scattering:
• Neutron and nuclide collide and share part of their
kinetic energies.

• Neutron slows down. [thermalisation of neutrons in

thermal reactors].

• Elastic scattering in lighter nuclides more significant

than in heavier ones.

• ‘Energy loss’ of a neutron in elastic scattering gets

smaller as the nuclide becomes heavier.
 NEUTRON INTERACTIONS

Inelastic scattering:

• Energies are shared, but with the rebounding

nuclide left in an excited energy state.

• Energy loss of a neutron is much larger than in

elastic scattering, as a large portion of the initial
neutron energy is used in leaving the nucleus in
the excited state.

• Inelastic scattering is more significant in heavy

nuclides than in lighter ones.
 NEUTRON INTERACTIONS
Capture:
Neutron is absorbed by the target nucleus to form
the next higher isotope (of mass A+1), in an excited
state of energy. The new isotope de-excites by
emitting γ rays. The neutron is thus lost in this
reaction. This is known as ‘radiative capture’.

Fission:
A heavy nucleus, splits into two smaller nuclei,
called the fission fragments, mostly of unequal
masses, one often with nearly half the mass as
the other, and rarely of equal masses. This
reaction gives off a large amount of energy and
emits two or more neutrons, and gamma rays.
 TYPES &
GENERATION OF DEFECTS
 Defects in a Solid
Basics of Solids:

 A solid matter is constructed by the orderly

arrangement of atoms in space.

 Atoms arrange themselves in 14 different crystal

lattices, which fall into 7 crystal systems.

 Geometry and orientation of a crystal is decided by the

laws of thermodynamics – Minimum energy provides
maximum stability to the crystal lattice for any given
thermodynamic condition.

 For any given material, mechanical properties are

decided by crystal structure and the defects present.
 Defects in a Solid
Defects in a Crystal:

 A perfect crystal, with every atom of the same type in

the correct position, does not exist.

 All crystals have some defects. Defects contribute to

the mechanical properties of metals.

 In fact, the term “defect” is a misnomer since these

features are intentionally used to manipulate the
mechanical properties of a material.

 Defects may be produced by conditions such as high

temperature, high pressure and neutron radiation.
Defects in a crystal lattice - classifications
Point defects (Vacancy, Interstitials)
Line defects ( Dislocations)
Planar defect (Stacking fault, Twins, Grain boundary)
Volume defect (Precipitates, Voids and Bubbles)
 Generation of Defects

Neutron

Neutron

Energetic neutron strikes an atom in a crystal. Atom

gains energy & gets displaced. An atom displaced from
its site, may settle in an interstitial position forming
vacancy-interstitial pair.
 Displacement of atoms
Experimental values of minimum
(Ed, min) and average (Ed, av)
Neutron threshold energies.
Metal Ed, min(Ed,av) Ed ASTM
Ag 25 40
Al 16 25
Cu 19 (36) 30
Fe 17 40
Neutron Mo 33 60
W 41 90
Ni 23 40
SS 18 40

Minimum energy required is the ‘threshold displacement energy’

Ed. If the kinetic energy of the recoil atom is large enough it
leaves its site and, if deposited outside the recombination
volume, creates a Frenkel pair.
 Displacement Cascade

Displaced atom can knock other atoms leading to cascade of

displacements. Thus an initial displacement leads to a series of
subsequent displacements causing crystal defects, hence damage. A
neutron may cause multiple displacements.
DISLOCATION LOOPS
 Radiation Damage

Recombination
Defect Production
Vacancies & Supersaturation
Interstitials Clustering & Growth
Loss to Sinks

o Vacancies & interstitials produced in equal nos.

o Net vacancy flux to voids because of preferential
bias of interstitials to dislocations
 Radiation Damage

VOIDS
DISLOCATION
LOOPS

Radiation damage: Energetic radiation causes defects in a

crystal leading to ‘radiation damage’, affecting the mechanical
properties of the crystal.
 Helium bubble formation due to irradiation
Unirradiated

Coarse SiO2 ppts. along GB (marked 1) Low dislocation density + fine

ppts. rich in Fe, Mn, Cr, Si & Al (marked 2,3)
Irradiated

Helium bubbles along pre-existing dislocations and a denuded

zone of ~ 120nm along GB for large bubbles
Ref: D. Hamaguchi, Y. Dai / Journal of Nuclear Materials 329–333 (2004) 958–962
CONSEQUENCES ON PROPERTIES &
PERFORMANCE
 Irradiation Growth
Dimensional changes at constant volume of an
unstressed material under irradiation.

Occurs in both single crystals and textured poly-

crystals of anisotropic metals and alloys.

Due to unequal distribution of interstitial and vacancy

loops on different crystallographic planes.

Occurs at relatively low temperatures in the vicinity of

0.2 Tm and is accompanied by irradiation hardening and
embrittlement.

Texture, grain size, dislocation density and alloy content

affect the growth rate, which also increases with
temperature.
 Irradiation Growth
Examples:
Irradiation growth in Zr alloys is significant for
the design and operation of PHWRs.

The texture in zircaloy cladding tubes causes

the axial length to increase and cladding
diameter and thickness to diminish.

This has an impact on design and safety, the

growth distortions setting operational burn up
limits.
 Radiation induced void formation
First observed by Cawthrone and Fulton (1967) in SS irradiated in the
Dounrey fast reactor

Material: Large Voids on GB in neutron

0.12C–18Cr–9Ni–Ti alloy irradiated 12X18H9T steel
(Austenitic)
Conditions
Fluence:0.35 x1026n/m2
Dose:0.64 dpa, T:350 C

Large super saturation of vacancies

High vacancy mobility and migration of vacancies to
voids

Implications:
Decrease in density of the material
Increase in physical size
 Radiation induced void formation

Swelling is a volumetric expansion caused by formation

of voids due to supersaturation of vacancies when the
structural materials are subjected to fast neutron
irradiation in the temperature range ~0.3 to 0.5T.

For stainless steels, these are the temperatures

in which the Fast Breeder reactor core operates
Above 0.5 Tm and the thermal vacancy concentration
exceeds that introduced by irradiation and there is no
supersaturation of vacancies to collapse to voids.
CONSEQUENCES OF SWELLING
 Evolution of dislocation loops under irradiation
Material: 0.12C–18Cr–9Ni–Ti alloy (Austenitic steel)
Conditions
Fluence:0.35 x1026n/m2 , Dose:0.64 dpa; T:350 C

unirradiated steel irradiated steel

Austenite grains with subgrain
Dislocation loops arrays along
boundaries, fine TiC
previously existing sub-grain
precipitates & dislocations
boundaries

Ref: S.I. Porollo et al. / J. Nucl. Mater. 359 (2006) 41–49

 Radiation induced defect production
Dose: 5 dpa Dose: 50 dpa

1& 2) Dislocation loops (BF & DF image) , 3) loops (dark field image)

Fine distribution of precipitates in

irradiated alloy (3)
Material: Alloy 800H
Particle: 5 MeV Ni ions
Irradiation conditions Suppression of dislocation loop growth
T:500C

Avoids void formation

J. Gan et al. / Journal of Nuclear Materials 351 (2006) 223–227
 Irradiation Hardening
The general effects of neutron irradiation on the
mechanical behaviour are

 increase in the yield strength (irradiation

hardening);
 increase in the ultimate tensile strength, which
is less than the increase in yield strength;
 decrease in the rate of work hardening
 reduction in the uniform and total elongations.
 Irradiation Hardening

(a) Stress-strain curves for polycrystalline copper

tested at 20  C after irradiation;
Embrittlement
 Irradiation Embrittlement
Transition from ductile to brittle behaviour as Temp. is ;
Below the transition temperature or nil-ductility transition
temperature (NDTT), fracture occurs by cleavage;
Energy required for fracturing a specimen in an impact test
is negligible.
Irradiation embrittlement and increase in NDTT are serious
engineering problems in nuclear reactors

Irradiation embrittlement – affects performance of many

reactor components. Loss of ductility depends on
•Irradiation temperature
•Pre-irradiation microstructure
•Fluence
 Irradiation Embrittlement

(b) Impact energy vs temperature curves for ASTM A 203 grade D steel.
A= Unirradiated;
B= Irradiated to a fluence of 3.5x1019 n cm-2;
C= irradiated to a fluence of 5x1018 n cm-2;
D= Annealed at 300C for 15 days after irradiation to a fluence of
3.5x1019 n cm-2.
 Irradiation Embrittlement
Irradiation embrittlement in bcc alloys:
Irradiation has two effects on BCC metals and alloys,
firstly it increases the NDTT or DBTT and secondly it
brings down the fracture energy of the material even in
the ductile region (called upper shelf).

shift of DBTT
with
irradiation
 Irradiation Embrittlement
At low temperatures: embrittlement is a
consequence of irradiation hardening by defects,
clustering of solute atoms and consequent short
and long-range dislocation barrier effects arising
from them, which manifest themselves as an
increase in ductile-brittle transition temperature
(DBTT) (in BCC alloys).

At high temperatures (> 0.5 Tm): embrittlement

due to helium generated by (n,) reactions is
predominant (in FCC alloys).
 EMBRITTLEMENT

Comparison of shift of DBTT after irradiation

for the mod.9Cr-1Mo and HT9
CREEP – time dependent deformation under stress

• tendency of solid to slowly move or deform

permanently under the influence of stress.
• occurs as a result of long term exposure to
levels of stress that are below the yield
strength or ultimate strength of the material.
• more severe in materials that are subjected
to heat for long periods, and near the melting
point.
 CREEP – time dependent deformation under stress
Stages of creep
• Initial stage, or primary creep -
strain rate is high, but slows with
increasing time due to work
hardening.

• Strain rate reaches a minimum

and becomes near constant -
secondary or steady-state creep
due to the balance between work
hardening and annealing .

• "creep strain rate" refers to the

rate in this secondary stage.
Stress dependence of this rate • In tertiary creep, the strain rate
depends on the creep exponentially increases with
mechanism. strain due to necking phenomena.
Assessment of Creep:
Stress to Rupture Time to rupture at constant stress
 IRRADIATION CREEP

 Increased concentration of irradiation induced vacancies

brings down the temperature range where creep occurs.

 At low temp. below ~ 0.3 Tm - reduction in creep rate under

irradiation due to irradiation hardening.

 At higher temperature (0.3-0.5Tm) irradiation will increase

the creep rate due to excess concentration of vacancies.

 At very high temperatures >0.6 Tm - concentration of

vacancies produced by irradiation is small compared to
thermal equilibrium concentration of vacancies - irradiation
will not have any significant effect on creep - thermal creep
dominates
 IRRADIATION CREEP
Stress induced
preferential absorption
(SIPA) of point defects at
dislocations.

Stress-induced preferred
nucleation or alignment
of dislocation loops
(SIPN)
Formation or growth of
loops and absorption of
defects at existing
dislocations depending
upon their orientation
with respect to the
external stress, causes
a macroscopic
creep strain.
IRRADIATION CREEP
CREEP DAMAGE
 Phase Stability Under Irradiation
Radiation Induced Segregation and Precipitation

Point defects migrate to sinks such as grain boundaries,

other interfaces and surfaces during irradiation.
Persistent flux of point defects to sinks gives rise to the
phenomenon of radiation-induced segregation (RIS) - a non-
equilibrium segregation caused by coupling of solute atoms
to defect fluxes.

Eg: Segregation of Cr and Ni in austenitic SS, due to

difference in elemental diffusivities DCr > DFe > DNi.

Possibility of Austenite grains transforming into ferrite

during neutron irradiation, because localised regions get
enriched in either Cr or Ni, stabilizing either ferrite or
austenite at the respective locations.
 Radiation induced segregation

 Unequal participation of solutes

in the vacancy and interstitial
defect fluxes.
 Enrichment or depletion of an
element occurs according to
the relative interaction with the
defect flux.

Cr depletion at GB - Sensitisation

Material: Fe-20Cr-25Ni-0.75Nb-0.5Si
Particle: Electron (1MeV)
Dose conditions: 420C/ 7.2 dpa

Ref: M.A. Ashworth etal, JNM, 189 (1992) 289-302

 Phase Stability Under Irradiation
Radiation Induced Precipitation
One of the manifestations of RIS is the formation and growth of
precipitates. Phases that form during irradiation have been
classified as (i) radiation induced (ii) radiation enhanced and
(iii) radiation modified.

Radiation induced phases form as a result of radiation induced

segregation and normally not form under thermal conditions.

Eg: In SS316, formation of Ni3Si(γ'), Si may be replaced by Al,

Nb or Ti, G-phases M6Ni16Si7 (M = Cr or Mn) & phosphides.

Formation of such phases affect not only mechanical

properties of SS, but also onset of void swelling and irradiation
creep through removal of Ni and Si from the matrix.
 Phase Stability Under Irradiation

Radiation enhanced phases are those that form in the

alloy under normal thermal conditions but during
irradiation they are produced more rapidly, more
abundantly and at lower temperatures. The opposite
effect of retardation of a phase is also possible by
radiation; M6C is generally enhanced and M23C6 is
retarded due to irradiation (M=Cr, Fe, Mo, W).

Radiation modified phases are those that form in the

alloy under thermal conditions but in which the
composition is altered as a result of radiation induced
segregation.
Radiation produced precipitation – Austenitic SS
Classes of radiation-produced
precipitate phases in 300-series
austenitic stainless steels

Radiation-enhanced - retarded
phases - M6C, Laves, M23C6, MC,
Laves, , (eg: M23C6 generally forms at HT at
low t’s. But on irradiation it forms even at low T)

Radiation-modified phases- M6C,

Laves, M2P (composition could be modified)

Radiation-induced phases-
M6Ni16Si7(G), Ni3Si ('), MP, M2P,
M 3P

S.J. Zinkle et al, /Journal of Nuclear Materials 206 (1993) 266-286

 Radiation induced Transmutation

Brittle material
He gas bubble in Mo after 40 keV helium ion irradiation at 500°C
 Radiation induced Amorphisation

Zr(Cr,Fe)2, Proton
irradiation, 5 dpa at 310C

Radiation-Induced Amorphization and Disordering

Increase in point defect concentration affects phase
stability of solids;
increase in internal energy due to accumulation of point
defects - destabilization of the crystalline phase resulting in
amorphization of certain intermetallics.
Studies in several intermetallics have shown the existence
of a critical dose of irradiation for amorphization.
 Radiation induced Amorphisation
Radiation-Induced Amorphization and Disordering
Alloys which show amorphization on irradiation are all
ordered intermetallic compounds which retain their
ordered structure up to their melting point. In ordered
alloys that disorder before their melting temperature,
radiation also induces disordering.
0.7 dpa
3.4 dpa

M23C6

Material: SS 304L, Particle: 800MeV protons

Irradiation Temp: 250C
 Operating Conditions in different reactors
Research Thermal FBR Fusion
Reactors Reactors Reactor
Temperature C <100 ~300 ~550 300-1000

Neutron Flux ~1012 ~1014 ~5 x 1015 ~5 x 1015

n/cm2s (14MeV)
Neutron ~1019 ~1022 ~3 x 1023 ~3 x 1023
Fluence n/cm2 (14MeV)

Atom ~10-13 ~10-8 ~10-6 ~10-6

Displacement
rate dpa/s
Dpa in 3 ~1 ~5-10 >100 >100
operating years
Fuel Burn Up ~1000 ~7000 150,000
MWd/t
He production OF NO CONSEQUENCE ~10 100-600
Appm/year
 Effect of Radiation Exposures on
Microstructure & Property
Point
defects
Voids Transmutation
Thermal Dissolution
Precipitation +
Irradiation
effects Amorphisation
Segregation
Grain & Precipitate
Dislocation
coarsening
loops
Microstructural
changes

PROPERTY CHANGES
MICROSTRUCTURAL CHANGES DUE TO IRRADIATION

<0.1

0.3

Thermal: Equilibrium concentration of defects

Radiation: Non equilibrium concentration of defects produced
 Study of Irradiation induced defects
Neutron – Radiation Ions (H, He, Ni, Ar etc.)
in-core Simulation

Why Ion Irradiation

Neutron irradiation experiments – 1 to 3 years of in core
exposure to reach appreciable fluence levels
Post irradiation experiments needs precautions, special
facilities and instrumentation required for handling
radioactive samples

Advantages
Heavy ions ~ high dose rates
- accumulation of high doses
in short times.
Dense cascades, similar to
those produced by neutrons
Disadvantages
• Higher ion irradiation
temperatures causes annealing
• Short penetration depth
• Varying dose rate over
penetration depth.
DEFINITIONS
 DEFINITIONS
Dislocations are line defects in a crystal structure. The
bonds surrounding the dislocation are already elastically
strained by the defect compared to the bonds between the
constituents of the regular crystal lattice. The strained
bonds around a dislocation are characterized by lattice
strain fields. Each dislocation is associated with a strain
field which contributes some small but finite amount to the
stored energy of the materials.

Slip
Plane

Compressive Field

Tensile Field
 DEFINITIONS
Work hardening - increase in hardness of a metal induced, deliberately or
accidentally, by hammering, rolling, drawing, or other physical processes. Although
the first few deformations by such treatment may weaken it, its strength is
increased by continued deformations. The reason lies in the crystalline structure of
metal. As stresses are exerted, the crystals slip against each other; but, because of
the complexity of the crystal structure, the more such slips are multiplied, the more
they tend to place obstacles in the way of further slippage, because the various
dislocation lines crisscross each other.

Work hardening, also known as strain hardening is the strengthening of a metal

by plastic deformation. This strengthening occurs because of dislocation
movements and dislocation generation within the crystal structure of the material.
Many non-brittle metals with a reasonably high melting point as well as several
polymers can be strengthened in this fashion. Alloys not amenable to heat
treatment, including low-carbon steel, are often work-hardened. Some materials
cannot be work-hardened at low temperatures, such as indium, however others can
only be strengthened via work hardening, such as pure copper and aluminum.
Work hardening may be desirable or undesirable depending on the context.