Journal of the Korean Physical Society, Vol. 34, No. 5, May 1999, pp.

434∼438

The Changes of the Structural, Magnetic, and Mechanical Properties

in a Reactor Pressure Vessel Steel Neutron-irradiated at 70 ◦ C

D. G. Park and J. H. Hong∗

Reactor Materials Department, Korea Atomic Energy Research Institute,
Taejon 305-600

K. S. Jang
Korea Electric Power Research Institute, Taejon 305-380

M. M. Jung
Korea Institute of Nuclear Safety, Taejon 305-338

G. M. Kim
Chungnam National University, Taejon 305-764

(Received 8 January 1999)

The irradiation embrittlement of reactor-pressure-vessel steel has been one of the main safety
concerns in nuclear power plants. In the present study, an SA508-3 RPV steel was irradiated by
neutrons with various fluences up to 1018 n/cm2 (E ≥ 1 MeV) at a temperature of approximately 70
◦
C. The irradiation responses of the structural, the magnetic, and the mechanical properties of the
steel were investigated by means of X-ray diffraction, Mössbauer spectoscopy, magnetic Barkhausen
noise, and micro-Vickers hardness measurements. The transitions of all of these parameters occurred
above a neutron dose of 1016 n/cm2 . The results of the X-ray and the Mössbauer experiments
revealed that neutron irradiation led to the possibility of partial amorphization in the investigated
RPV steel. The changes of the physical and the mechanical properties were discussed in terms of
irradiation-induced cascade damage of crystalline materials.

I. INTRODUCTION eral nanometers [3]. These defects should have a strong

Recently, non-destructive evaluation methods, such
as measurements of magnetic properties and Mössbauer
spectra, have been of growing interest as techniques for
evaluating radiation damage of nuclear reactor pressure
vessels (RPV). It has been shown that the degradation of
RPV steel is simultaneously accompanied by embrittle-
ment, hardening, and decrease in ductility [1,2], and this
degradation increases with increasing neutron dose. The
irradiation embrittlement is a limiting factor for some
technical applications, such as the lifetime of nuclear
power plants, so a better understanding of the relation-
ship between the microstructure and the observed mag-
netic and mechanical properties is very important. The
most important microstructural change under neutron
irradiation is atomic displacements which cause defects,
self-interstitial and vacancy clusters on the order of sev-
interaction with the magnetic domain walls [4]. However,
the underlying mechanism for the effects of neutron ir-
radiation on the magnetic characteristics is not under-
stood yet. Since the above-mentioned effects are the
characteristics for bombardments of amorphous, as well
as crystalline, alloys like RPV steel with high-energy par-
ticles, it would be interesting to evaluate the responses
of material parameters to the correlated microstructural
changes and to compare them in both structural states
[5]. For radiation-damage problems, nuclear hyperfine
interactions can be used to characterize the static and
the dynamic local configurations of both intrinsic and
extrinsic defects. In view of this fact, the present paper
is focused on the investigation of the irradiation-induced
changes in the structural, the magnetic, and the mechan-
ical properties of RPV steel as a function of the neutron
dose.

∗
E-mail: jhhong@nanum.kaeri.re.kr II. EXPERIMENTAL

-434-
The Changes of the Structural, Magnetic, and Mechanical Properties · · · – D. G. PARK et al. -435-

Fig. 2. Relative changes of Mössbauer spectra for various

neutron fluences (10n n/cm2 ).

Fig. 1. X-ray diffraction patterns for various neutron flu-

ences in units of 10n n/cm2 .
The sample was an SA508-3 Mn-Mo-Ni low alloy forg-
ing steel for nuclear pressure vessels; the alloy was pro-
duced by Korea Heavy Industries and Construction Co
(HANJUNG). Samples of 18 mm × 23 mm with a thick-
ness of 1 mm were irradiated by neutrons for various
numbers of cycles at full power (1.5 MW) in the TRIGA
MARK III reactor of Korea Atomic Energy Rearsech In-
stitute (KAERI) at a temperature of approximately 70
◦
C . The accumulated dose was 1012 to 1018 n/cm2 (E ≥
1 MeV) where iron wire was employed to determine the
neutron dose.

Table. 1. Changes of (a)isomer shift, (b)quadrupole splitting, (c)magnetic hyperfine field, and (d)absorption area and line
width.

(a)
Fluence (n/cm2 )
100 1012 1013 1014 1015 1016 1017 1018
Parameter
Site A −0.01 −0.06 −0.02 −0.02 −0.02 −0.01 −0.03 −0.01
I.S.
Site B −0.02 −0.07 −0.02 −0.02 −0.02 −0.03 0.00 −0.02
(mm/sec)
Site C 0.21 0.18 0.21 0.18 0.21 0.17 0.32 0.33

(b)
Fluence (n/cm2 )
100 1012 1013 1014 1015 1016 1017 1018
Parameter
Site A −0.09 −0.08 −0.08 −0.08 −0.07 −0.09 −0.09 −0.08
Q.S.
Site B −0.02 −0.05 −0.08 −0.07 −0.08 −0.04 −0.05 −0.04
(mm/sec)
Site C 0.50 0.48 0.53 0.50 0.54 0.47 0.64 0.66

(c)
Fluence (n/cm2 )
100 1012 1013 1014 1015 1016 1017 1018
Parameter
H.F. Site A 330.6 329.0 330.5 327.1 328.5 328.3 327.3 326.9
(kOe) Site B 306.3 304.3 308.3 305.3 306.5 307.2 303.8 304.0

(d)
Fluence (n/cm2 )
100 1012 1013 1014 1015 1016 1017 1018
Parameter
Site A 68.0 62.8 62.3 59.2 58.1 61.9 63.0 56.6
Area
Site B 27.4 33.2 33.4 36.5 37.2 33.9 22.0 22.1
(%)
Site C 4.6 4.0 4.3 4.3 4.7 4.2 15.0 21.3
Line Width Site A 0.38 0.39 0.33 0.35 0.39 0.35 0.41 0.48
(mm/sec) Site B 0.43 0.37 0.34 0.33 0.40 0.38 0.53 0.75
-436-
Fig. 3. Relative change of BNA, BNE, and hardness as
functions of the neutron fluence.
The structural state of the sample was investigated
for various neutron doses by using X-ray diffractometry
and Mössbauer spectroscopy. The X-ray diffraction mea-
surements were made in a Philips PW-1710 diffractome-
ter using CuKα radiation. The 57 Fe Mössbauer spec-
tra were collected in a transmission geometry at room
temperature by using a standard constant-acceleration
spectrometer with a 57 Co(Rh) source.
The magnetic Barkhausen noise (BN) was measured
by using a specially designed magnetizing core and a si-
nusoidal current of 0.5∼5 Hz. The BN signal detected by
the same pick-up coil was amplified and passed through
a wide-band filter with a flat response from 500 Hz to 20
kHz. The B-H loop and the BN signal, including the
Barkhausen-noise energy (BNE) and the Barkhausen-
noise amplitude (BNA), where BNE is defined as the
time integration of the squared BN voltage for a magne-
tizing cycle, were measured as functions of the neutron
fluence.
III. RESULTS AND DISCUSSION
The X-ray diffractograms of the unirradiated and the
neutron-irradiated samples are shown in Fig. 1 various
neutron doses. A significant change occured in the X-ray
diffraction profile above a neutron dose of 1016 n/cm2 .
The X-ray diffraction patterns represented by Miller in-
dices show that these samples have the typical bcc struc-
ture. With an increase in the neutron dose, some crys-
talline peaks disappeared in the corresponding X-ray
diffractogram, revealing the possibility of partial amor-
phization in the investigated RPV steel which could re-
sult in a drastic deterioration of mechanical properties.
The intensities of the peaks observed below 30◦ at the
neutron dose of 1016 n/cm2 are very high compared with
Journal of the Korean Physical Society, Vol. 34, No. 5, May 1999
Fig. 4. The linear relations between BNA, BNE, and hard-
ness.
the main bcc-Fe peak (110). The interplanar spacing of
the unknown peak appearing at 17.54◦ is about 5.05 Å,
suggesting that a new phase with a large lattice param-
eter was produced by neutron irradiation. However, it
may also be a result of the photoelectric effect due to the
replacement of a low-energy X-ray photon by a gamma-
ray photon [6].
In order to shed more light on the currently unclear
character of irradiation-induced structural changes in the
neutron-irradiated RPV steel, Mössbauer experiments
were performed.
Figure 2 shows the dose dependence of the Mössbauer
spectra from neutron-irradiated samples. In order to
evaluate the corresponding hyperfine parameters, we
fitted the measured spectra with three sets of six
Lorentzians by using a least-squares computer program,
and the results are shown in Table 1. The hyperfine
parameters are nearly constant up to 1016 n/cm2 , after
which a rapid increase is seen with increasing neutron
dose. The Mössbauer spectra did not show large varia-
tions up to a neutron dose of 1016 n/cm2 , but significant
changes were observed in the Mössbauer spectra from
samples irradiated with a neutron dose of 1017 n/cm2 ,
and the bombardment changed the energy state of the
constitutent atoms associated with the nuclear or the
electron charge distribution, resulting in the correspond-
ing hyperfine parameters. The resonance absorption ar-
eas of A and B sites representing the Zeeman splitting [7]
decreased with increasing neutron dose, but no variation
was observed in the peak position. Trapped defects pro-
duce an electric field gradient at the site of the radioac-
tive probe atoms, which leads to a level splitting of the
excited nuclear state. Therefore, the Zeeman splitting is
attributed to defect clusters attached to the 57 Fe isotope.
However, it is not possible to directly identify a trapped
defect by its characteristic parameters determined via
The Changes of the Structural, Magnetic, and Mechanical Properties · · · – D. G. PARK et al.
the hyperfine interaction at the radioactive probe. Until
now, theoretical models have not been able to reproduce
these values with sufficient accuracy.
Figure 3 shows the changes in the BNE, the BNA,
and the hardness as functions of the neutron fluence.
These parameters are characterized by three stages with
respect to neutron dose. A rapid decrease developed in
the BNE at the early stage of irradiation, which did not
show a considerable change up to a neutron fluence of
1016 n/cm2 ; a rapid decrease of 38 % compared with the
unirradiated sample, was observed at 1018 n/cm2 . The
change in the BNA showed a similar trend, but the rate
of change was less than that of the BNE. These stages
seem to be related with the behavior of irradiation-
induced defects due to radiation damage under an in-
creasing irradiation dose. The profound effects of irra-
diation on the BN signify a change of domain-wall mo-
tion from that at a dose of 1016 n/cm2 , in qualitative
agreement with the results for hardness in the same fig-
ure. The decrease in the BN is attributed to domain-
wall pinning and to an increase in the hardness due
to the hindrance of dislocation motion by irradiation-
induced defect clusters [3]. In spite of the dimensional
difference between dislocations and the domain wall, it
was anticipated that the increase in the density of de-
fect clusters with increasing irradiation dose would lead
to greater hardness which would cause lower magnetic
Barkhausen emissions because of an increased number
of defect-pinning centers which impede both the move-
ment of the magnetic domain walls and the dislocations.
The hardness difference between unirradiated and
1018 n/cm2 -irradiated specimens, ∆Hv = 80, was very
large, considering the fluence level, compared with that
of ∆Hv = 15 in SA508-3 steel irradiated with a dose of
9 × 1018 n/cm2 (E ≥ 1 MeV) at 290 ◦ C [8]. It is known
that the hardness decreases with increasing irradiation
temperature [9], but the SA508-3 steel was fairly insen-
sitive to higher temperatures [10]. The present study
suggests that the degradation is more pronounced for ir-
radiation at lower temperatures.
The relationship between the hardness and the BN
characteristic including the BNE and the BNA, gives
some insight into the relation between the mechanical
and the magnetic properties, as shown in Fig. 4. The
observed BNE and BNA showed linear relationships with
hardness in the magnetization region, and a similar re-
lationship between the Barkhausen parameter and the
hardness has been obtained by others [11,12]. The radi-
ation hardening is due to dislocation pinning by small de-
fect clusters whereas the BN is associated with domain-
wall pinning by defect clusters; thus, good correlation
is found. The relation suggests that radiation hard-
ening can be evaluated non-destructively by using the
Barkhausen noise parameter.
IV. CONCLUSIONS
-437-
The effects of irradiation on the structural, the mag-
netic, and the mechanical properties were investigated
by means of X-ray diffraction, Mössbauer spectroscopy,
magnetic Barkhausen noise, and micro-hardness mea-
surements in neutron-irradiated RPV steel. The results
of all of these experiments showed similar characteristic
trends with the neutron dose: nearly constant up to a
neutron dose of 1016 n/cm2 and rapidly changing above
this dose. The BNE and the BNA decreased and the
hardness increased with neutron dose, and all of these
parameters showed great changes above a neutron flu-
ence of 1016 n/cm2 . This dose level seems to correspond
to a condition where the density of radiation-induced de-
fects reaches an appreciable fraction. From the sensitive
change of BN and hardness, it seems that defect clusters
impede the movements of both magnetic domain walls
and dislocations. The linear relation between the hard-
ness and the BN parameters suggests that the degrada-
tion of mechanical properties by neutron irradiation can
be evaluated well by measurements of the BNE and the
BNA.
ACKNOWLEDGMENTS
This work has been carried out as a part of the Reactor
Pressure Boundary Materials Project under the Nuclear
R & D Program by the Ministry of Science and Technol-
ogy in Korea.
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