Radiation induced optical centers in magnesium aluminate spinel ceramics
There were investigated the optical absorption centers formation in magnesium aluminate spinel ceramics under irradiation with UV-light, X-, and gamma-rays. The lithium fluoride doped ceramics were produced by using hot-pressing technology. It was revealed that generation by irradiation changes in o...
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| Zitieren: | Radiation induced optical centers in magnesium aluminate spinel ceramics / V.T. Gritsyna, Yu.G. Kazarinov, A.A. Moskvitin, I.E. Reimanis // Вопросы атомной науки и техники. — 2010. — № 1. — С. 28-31. — Бібліогр.: 5 назв. — англ. |
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| author | Gritsyna, V.T. Kazarinov, Yu.G. Moskvitin, A.A. Reimanis, I.E. |
| author_facet | Gritsyna, V.T. Kazarinov, Yu.G. Moskvitin, A.A. Reimanis, I.E. |
| citation_txt | Radiation induced optical centers in magnesium aluminate spinel ceramics / V.T. Gritsyna, Yu.G. Kazarinov, A.A. Moskvitin, I.E. Reimanis // Вопросы атомной науки и техники. — 2010. — № 1. — С. 28-31. — Бібліогр.: 5 назв. — англ. |
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| description | There were investigated the optical absorption centers formation in magnesium aluminate spinel ceramics under irradiation with UV-light, X-, and gamma-rays. The lithium fluoride doped ceramics were produced by using hot-pressing technology. It was revealed that generation by irradiation changes in optical absorption spectra can be used for detection of invisible point defects in prepared ceramics, their distribution through the bulk of spinel disk, and predict the behavior of ceramics in different radiation fields.
Исследовано образование оптических центров поглощения в керамике магнийалюминиевой шпинели при облучении УФ-светом, рентгеновскими или гамма-квантами. Керамика шпинели с добавками фторида лития была приготовлена с помощью технологии горячего прессования. Обнаружено, что вызванные облучением изменения в оптических центрах поглощения могут быть использованы для детектирования невидимых точечных дефектов в полученной керамике, их распределения по объему керамического диска, а также для предсказания поведения керамики в различных радиационных полях.
Досліджено утворення оптичних центрів поглинання в кераміці магнійалюмінієвої шпінелі під дією УФ-світла, рентгенівських та гама-квантів. Кераміка шпінелі з добавками фториду літію готувалась методом гарячого пресування. Знайдено, що зміни в спектрах оптичного поглинання, які виникли при опроміненні, можуть бути використані для виявлення невидимих точкових дефектів в кераміці, їх розподілу по об’єму керамічного диску, а також прогнозувати поведінку кераміки в різних радіаційних полях.
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UDC 535.3
RADIATION INDUCED OPTICAL CENTERS IN MAGNESIUM
ALUMINATE SPINEL CERAMICS
V.T. Gritsyna, Yu.G. Kazarinov*, A.A. Moskvitin, I.E. Reimanis**
V.N. Karazin Kharkiv National University, Kharkiv, Ukraine;
*National Science Center “Kharkоv Institute of Physics and Technology”, Kharkоv, Ukraine;
**Colorado School of Mines, Golden, CO 80401, USA
There were investigated the optical absorption centers formation in magnesium aluminate spinel ceramics under
irradiation with UV-light, X-, and gamma-rays. The lithium fluoride doped ceramics were produced by using hot-
pressing technology. It was revealed that generation by irradiation changes in optical absorption spectra can be used
for detection of invisible point defects in prepared ceramics, their distribution through the bulk of spinel disk, and
predict the behavior of ceramics in different radiation fields.
INTRODUCTION
Ceramic materials have important properties which
make them suitable for a number of applications in
fission and fusion reactors. Magnesium aluminate spinel
(MgAl2O4 or MgO·Al2O3) in particular has been shown
to be very resistant to radiation damage. Considerable
attention has been, therefore, directed to spinel, such as
for a host of inert matrix fuels in light water nuclear
reactors, and a transmutation target for minor actinides
and long life fission products. Under environment of
such nuclear applications MgAl2O4 will be exposed to
electronic excitation for a wide range of intensity with
electrons, gamma rays, ions and other fission products.
Therefore, investigation of nature and concentration of
defects and optical centers formed under ionizing
irradiation is issue of the present time.
The spinel crystal lattice has fcc structure of oxygen
ions with a lattice parameters of 0.808 nm. There are
eight molecules in its unit cell forming the 64
tetrahedral symmetry sites and 32 octahedral ones. In
natural spinel crystals magnesium ions (Mg2+) occupy 8
tetrahedral positions and aluminum ions (Al3+) occupy
16 octahedral sites. At non-equilibrium growth
conditions, for example, in ceramic technology at high
temperature and high pressure, there was observed the
partial cationic disordering, i.e. part of Al3+ ions occupy
tetrahedral position and equal part of Mg2+ ions occupy
octahedral sites, forming so called anti-site defects. As a
result, at the high concentration of different types of
point defects in crystal there are appeared complexes of
defects and it lost optical transparency. Also anti-site
defects play important role in radiation resistance of this
material because oppositely charged anti-site defects
form charge compensated clusters which serve as
recombination centers of radiation induced Frenkel pairs
[1, 2]. The main task of this research is to investigate
the spatial distribution of intrinsic defects in spinel
ceramics by using radiation induced processes of
formation and evolution of optically active centers.
In numerous papers there were investigated radiation
induced processes in nominally pure magnesium
aluminate spinel crystals and ceramics of different
origin and compositions [3-5].
EXPERIMENTAL DETAILS
In this paper we report the results of investigations
of optical center formation in spinel ceramics fabricated
by hot-pressing technique of spinel powder synthesized
with adding up to 1.0 wt. % LiF at Colorado School of
Mines, USA [6]. A uniaxial die pressure of 35 MPa was
applied at about 1550 °C to fabricate block of
transparent ceramics. Therefore, the non-equilibrium
conditions of spinel structure formation could lead to
different types of defects and their concentration to
compare with that in single crystals. Moreover, the
variation of technological parameters inside of spinel
disk (temperature, pressure, composition and so on)
causes the change of ceramic structure on microscopic
level [7]. Back scattered electron images of magnesium
aluminate spinel ceramics (MgAl2O4) disc obtained by
vacuum hot- pressing technique indicates that there
exists the variation of structure in cross-sections through
the ceramics plate surface area [8]. The difference in
structure on the microscopic level may indicate also
variation of point defects and atomic structure.
Samples for optical investigation were cut into slices
of 0.7 mm thickness across the disk of ceramics and
polished to optical finish. The optical absorption spectra
were measured in the wavelengths range of
185…1000 nm (6.7…1.2 eV) by using single beam
spectrophotometer SF-46. Irradiation with UV-light was
provided by using mercury lamp of quartz balloon, X-
ray irradiation by using X-ray tube of Cu-anode at
voltage of 35 keV, and current of 0.4 mA. Also
ceramics were irradiated with bremsstranglung gamma-
rays from energetic electrons of 7 MeV at linear
accelerator. The time for irradiation was chosen to reach
the saturation in the value of absorption density.
RESULTS AND DISCUSSION
At first we investigated the uniformity of optical
absorption through the disk of spinels prepared by hot-
pressing. The absorption spectra measured in pristine
samples cut from different places of disk demonstrate
no definite bands; also there is difference in absolute
values of optical density of samples. After subtraction
of absorption spectra of different samples we found the
additional information on the optical centers.
It turned out that in pristine samples cut from
different sites of disk in the difference spectra there
exist several absorption bands the main of which have
maxima at 2.8, 4.2 4.75, and 5.3 eV (Fig. 1). The
intensity of these bands varies from place to place
through plates indicating the variation of hot-pressing
28 Серия: Физика радиационных повреждений и радиационное материаловедение (95), с. 28-31.
ВОПРОСЫ АТОМНОЙ НАУКИ И ТЕХНИКИ. 2010. №1.
parameters during preparation (temperature and
pressure) and/or composition [8]. As a matter of fact
this optical data can be used for determination of
optimal conditions for preparation of optical ceramics of
the homogenous properties.
1 2 3 4 5 6
0,00
0,01
0,02
0,03
0,04
0,05
0,06
0,07
0,08
7
2-7
3-6
1-6
1-7
D
iff
er
en
ce
o
f o
pt
ic
al
d
en
si
ty
, a
rb
. u
n.
Photon energy, eV
4.75
4.2
2.8
5.3
Fig. 1. Examples of variation of optical absorption
spectra of samples cut in cross-sections through the
ceramics plate surface area (difference of absorption in
different samples)
The origin of initial absorption in pristine ceramics
samples could be explained by non-equilibrium process
of ceramics production. During the hot-pressing process
at elevated temperature (1550 °C) the formation of
lattice defects could be possible. At the high
temperature these charged defects can capture the
charge carriers of opposite signs forming residual
optical centers.
CENTERS IN UV-IRRADIATED CERAMICS
To activate the optical absorption in the samples
were irradiated with UV-light, X- and gamma-rays. The
UV-induced optical absorption spectra of three samples
cut from the different part of ceramic disc are shown in
Fig. 2. These spectra were obtained by subtraction of
initial spectra of pristine samples from that of the UV-
irradiated samples. The decomposition of these spectra
in elementary absorption bands gives several bands
related to different centers some of which was found in
irradiated single crystals with exception of band at
5.65 eV [5].
The UV-induced absorption bands are situated at
3.1 eV related to hole centers at cationic vacancies,
3.8 eV hole ascribed to centers at anti-site defects, and
band at 4.75 eV are related to F+-centers. Finally the
intensive absorption band at 5.65 eV was observed in
irradiated ceramics which is absent in spinel crystals.
The formation of optical absorption centers under UV-
irradiation could be explained in the next manner.
Because of UV-photons energy (Eph<6.7 eV) less than
energy gap of spinel (Eg~7.8 eV) the generation of free
charge carriers is unlikely. Therefore, under UV-
irradiation the charge carrier transfer happened between
near neighbor defects. From Fig. 2 one can see that
simultaneously formation of electron and hole centers
were happened, i.e. the direct transfer of electron from
one defect to another take place near neighbor defect.
Also, the change of charge states of already existing
optical centers also possible.
1 2 3 4 5 6
0,00
0,01
0,02
0,03
0,04
7
D
iff
er
en
ce
o
f o
pt
ic
al
d
en
si
ty
, a
rb
. u
n.
Photon energy, eV
#1
#2
#7
5.65
4.75
3.8
3.1
Fig. 2. UV-irradiation induced optical absorption
spectra of samples cut from different parts of spinel disc
Fig. 3 demonstrates the transformation of F-centers
in initial crystals (anion vacancy captured two electrons)
into F+-centers (anion vacancy captured one electron) by
taking off one electron under UV-irradiation.
1 2 3 4 5 6
-0,06
-0,05
-0,04
7 D
iff
er
en
ce
o
f o
pt
ic
al
a
bs
or
pt
io
n,
a
rb
. u
n.
Photon energy, eV
2-7 unirradiated
2-7 UV irradiated
Fig. 3. Difference of absorption spectra in two
pristine and UV-irradiated spinel samples
CENTERS IN X-IRRADIATED CERAMICS
Because the energy of X-rays much higher to
compare with energy gap of spinel we may expect
during the X-irradiation the generation of free charge
carriers in crystals which can be captured by the
existing lattice defects and impurities. Therefore, the
absolute value of X-ray induced optical absorption is
much higher to compare with UV-irradiation. Fig. 4
shows the difference in absorption spectra of two
samples cut from different parts of ceramic disc before
and after X-ray irradiation.
1 2 3 4 5 6
-0,11
-0,10
-0,09
-0,08
-0,07
-0,06
-0,05
-0,04
-0,03
-0,02
7
3.2
4.75
5.3
D
iff
er
en
ce
o
f o
pt
ic
al
d
en
si
ty
, a
rb
. u
n.
Photon energy, eV
#2 - #7 unirraiated
#2 - #7 X-irradiated
5.65
Fig. 4. Difference of absorption spectra in two pristine
and X-irradiated spinel samples
29
These spectra we can compare with that after UV-
irradiation shown in Fig. 3. Despite of very low net
difference in absorption of two pristine samples (low
intensity 5.3 and 5.65 eV bands) the net difference for
X-ray irradiated samples drastically changed. Therefore,
the existing defects in pristine samples captured electron
and holes under irradiation forming in one sample (#2)
larger concentration of F+-centers, in another (#7) – V-
type centers and unknown centers (5.65 eV).
From these data we conclude that in some samples
there exists large concentration of anionic vacancies
which can not be seen in pristine samples but under X-
irradiation the F+-centers can be formed leading to
absorption band at 4.75 eV. Analysis of reaction
between MgAl2O4 and LiF leads to conclusion on the
formation of oxygen vacancies due to the incorporation
of both Li and F ions into crystal lattice [9]:
2 4 2 23 2 3MgAl O
Mg Al O OLiF Li Li F V− − + +⎯⎯⎯⎯→ + + + .
The residual oxygen vacancies (VO
2+) under X-
irradiation can capture one or two electrons forming F+-
or F-centers and corresponding absorption bands. Other
product of this reaction the fluorine ions in oxygen site
(FO
+) serve also as electron traps forming electron
centers, transition in which may lead to absorption band
at 5.65 eV. Moreover, other products of this reaction Li
ion in Mg ( MgLi− ) or in Al sites ( ) could lead to
creation of optically active hole centers. The spectral
position of absorption band near 3 eV changes from
sample to sample in dependence on contribution of V-
type centers at isolated cationic vacancies or Li-
containing hole centers having slightly different spectral
position of individual absorption bands.
2
AlLi −
This is very striking example for demonstration of
possibility optical measurements of irradiated with
ionizing radiation ceramics (without formation of
additional lattice defects) for determination the nature
and concentration defects in ceramics prepared at
different technological conditions.
CENTERS IN GAMMA-IRRADIATED
CERAMICS
Irradiation with high energy gamma-rays causes the
strong change of initial absorption in spinel ceramics
leading to the optical absorption spectra containing
many overlapping bands (Fig. 5). The irradiation with
gammas of 7 MeV leads to generation of secondary
electrons (photo- or Compton-electrons) which may
create the free charge carriers and also lattice defects
and may form additional optical centers. Also, the
analysis of gamma induced spectra shows the existence
of already discussed bands of different intensity.
After irradiation with high energy gamma-rays the
intensity of absorption bands which related to hole
centers (bands at 3.2 and 3.8 eV) increases, but intensity
of bands ascribe to electron centers at anion vacancies
decreases, i.e. the radiation-induced absorption in
gamma-irradiated ceramics become negative.
The negative value of the 4.75 eV band along with
(specific for ceramics) band at 5.65 eV means that this
band could be related also to electron centers.
1 2 3 4 5 6 7
-0,2
-0,1
0,0
0,1
0,2
0,3
0,4
0,5
5.75
5.3
4.23.8
Initial
γ - irradiated
difference
O
pt
ic
al
d
en
si
ty
, a
rb
. u
n.
Photon energy, eV
3.2
7
Fig. 5. Absorption spectra of initial ceramic sample,
after gamma-irradiation and difference spectra of
irradiated and initial sample
To define the nature of optical centers formed by
gamma-irradiation we provided measurements of
absorption spectra after the subsequent UV- and gamma
irradiation of these samples (Fig. 6).
1 2 3 4 5 6
0,00
0,01
0,02
0,03
0,04
γ - irradiated
UV - irradiated
X - irradiated
Difference
D
iff
er
en
ce
o
f o
pt
ic
al
d
en
si
ty
, a
rb
. u
n.
Photon energy, eV
Fig. 6. Difference of absorption spectra of the gamma-
irradiated and subsequent UV- and X-irradiation in
spinel ceramics
The additional UV irradiation leads to appear
absorption bands at 5.65 and 3.8 eV. As it was
discussed before the first high intensity band could be
related to electron centers at fluorine incorporated anion
vacancies captured electron ( ), the band at 3.8 eV is
related to hole centers at anti-site defects [5]. The
additional irradiation with X-rays leads to formation
whole spectrum of absorption bands related to electron
and hole optical centers. The difference between the X-
ray and UV-induced absorption in gamma-irradiated
samples show the main contribution of bands related to
hole centers of different origins leading to very wide
band in the spectral range of 2…5 eV.
OF +
30
CONCLUSIONS REFERENCES
1. L. Thomé, A. Gentils, J. Jagielski, F. Garrido,
T. Thomé. Radiation stability of ceramics: Test cases
of zirconia and spinel //Vacuum. 2007, v. 81, p. 1264–
1270.
There were investigated the radiation-induced
optical center in magnesium aluminate spinel ceramics
doped with LiF after different types of irradiation. After
irradiation with UV-light we registered some absorption
bands arising from charge exchange between nearest
neighbor defects or defects and impurities. Irradiation
with X-rays leads to generation of free charge carriers in
conduction band of this insulator and subsequent
capture them by different defects or impurities which
gives additional absorption bands. Gamma-rays
(maximal energy of Eγ~7 MeV) ensure also formation
of new lattice defects with subsequent formation of
optical centers by free charge carriers. The existence of
radiation induced absorption bands was identified which
were found in irradiated single crystals and identified
with F- (5.3 eV), F+- (4.75 eV), V-type (3.1 eV) centers.
Also there is indication on the presence of bands at 4.2
and 3.8 eV which were previously identified with
electron and hole centers at anti-site defects. In spinel
ceramics doped with LiF evidently there was observed
absorption band at 5.65 eV which absent in nominally
pure spinel crystals and tentatively was identified with
complex F-type centers consisting of anion vacancies
with incorporated fluorine ion (F-) and captured one
electron. It was revealed that disk of transparent spinel
ceramics prepared by hot-pressing technology has un-
uniformly distributed defects of different origin
indicating the existence of uncontrolled variation of
technological parameters or composition in pressing
technique. Results of this research evidently show the
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Cтатья поступила в редакцию 29.09.2008 г.
РАДИАЦИОННО-ИНДУЦИРОВАННЫЕ ОПТИЧЕСКИЕ ЦЕНТРЫ В КЕРАМИКЕ
МАГНИЙАЛЮМИНИЕВОЙ ШПИНЕЛИ
В.Т. Грицына, Ю.Г. Kазаринов, A.A. Moсквитин, И.E. Рейманис
Исследовано образование оптических центров поглощения в керамике магнийалюминиевой шпинели при
облучении УФ-светом, рентгеновскими или гамма-квантами. Керамика шпинели с добавками фторида лития была
приготовлена с помощью технологии горячего прессования. Обнаружено, что вызванные облучением изменения в
оптических центрах поглощения могут быть использованы для детектирования невидимых точечных дефектов в
полученной керамике, их распределения по объему керамического диска, а также для предсказания поведения керамики
в различных радиационных полях.
РАДІАЦІЙНО ІНДУКОВАНІ ОПТИЧНІ ЦЕНТРИ В КЕРАМІЦІ
МАГНІЙАЛЮМІНІЄВОЇ ШПІНЕЛІ
В.Т. Грицина, Ю.Г. Kазарінов, A.A. Moсквітін, І.Є. Рейманіс
Досліджено утворення оптичних центрів поглинання в кераміці магнійалюмінієвої шпінелі під дією УФ-світла,
рентгенівських та гама-квантів. Кераміка шпінелі з добавками фториду літію готувалась методом гарячого пресування.
Знайдено, що зміни в спектрах оптичного поглинання, які виникли при опроміненні, можуть бути використані для
виявлення невидимих точкових дефектів в кераміці, їх розподілу по об’єму керамічного диску, а також прогнозувати
поведінку кераміки в різних радіаційних полях.
31
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| id | nasplib_isofts_kiev_ua-123456789-14946 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1562-6016 |
| language | English |
| last_indexed | 2025-12-07T16:49:04Z |
| publishDate | 2010 |
| publisher | Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| record_format | dspace |
| spelling | Gritsyna, V.T. Kazarinov, Yu.G. Moskvitin, A.A. Reimanis, I.E. 2010-12-29T18:36:21Z 2010-12-29T18:36:21Z 2010 Radiation induced optical centers in magnesium aluminate spinel ceramics / V.T. Gritsyna, Yu.G. Kazarinov, A.A. Moskvitin, I.E. Reimanis // Вопросы атомной науки и техники. — 2010. — № 1. — С. 28-31. — Бібліогр.: 5 назв. — англ. 1562-6016 https://nasplib.isofts.kiev.ua/handle/123456789/14946 535.3 There were investigated the optical absorption centers formation in magnesium aluminate spinel ceramics under irradiation with UV-light, X-, and gamma-rays. The lithium fluoride doped ceramics were produced by using hot-pressing technology. It was revealed that generation by irradiation changes in optical absorption spectra can be used for detection of invisible point defects in prepared ceramics, their distribution through the bulk of spinel disk, and predict the behavior of ceramics in different radiation fields. Исследовано образование оптических центров поглощения в керамике магнийалюминиевой шпинели при облучении УФ-светом, рентгеновскими или гамма-квантами. Керамика шпинели с добавками фторида лития была приготовлена с помощью технологии горячего прессования. Обнаружено, что вызванные облучением изменения в оптических центрах поглощения могут быть использованы для детектирования невидимых точечных дефектов в полученной керамике, их распределения по объему керамического диска, а также для предсказания поведения керамики в различных радиационных полях. Досліджено утворення оптичних центрів поглинання в кераміці магнійалюмінієвої шпінелі під дією УФ-світла, рентгенівських та гама-квантів. Кераміка шпінелі з добавками фториду літію готувалась методом гарячого пресування. Знайдено, що зміни в спектрах оптичного поглинання, які виникли при опроміненні, можуть бути використані для виявлення невидимих точкових дефектів в кераміці, їх розподілу по об’єму керамічного диску, а також прогнозувати поведінку кераміки в різних радіаційних полях. en Національний науковий центр «Харківський фізико-технічний інститут» НАН України Физика радиационных повреждений и явлений в твердых телах Radiation induced optical centers in magnesium aluminate spinel ceramics Радиационно-индуцированные оптические центры в керамике магнийалюминиевой шпинели Радіаційно індуковані оптичні центри в кераміці магнійалюмінієвої шпінелі Article published earlier |
| spellingShingle | Radiation induced optical centers in magnesium aluminate spinel ceramics Gritsyna, V.T. Kazarinov, Yu.G. Moskvitin, A.A. Reimanis, I.E. Физика радиационных повреждений и явлений в твердых телах |
| title | Radiation induced optical centers in magnesium aluminate spinel ceramics |
| title_alt | Радиационно-индуцированные оптические центры в керамике магнийалюминиевой шпинели Радіаційно індуковані оптичні центри в кераміці магнійалюмінієвої шпінелі |
| title_full | Radiation induced optical centers in magnesium aluminate spinel ceramics |
| title_fullStr | Radiation induced optical centers in magnesium aluminate spinel ceramics |
| title_full_unstemmed | Radiation induced optical centers in magnesium aluminate spinel ceramics |
| title_short | Radiation induced optical centers in magnesium aluminate spinel ceramics |
| title_sort | radiation induced optical centers in magnesium aluminate spinel ceramics |
| topic | Физика радиационных повреждений и явлений в твердых телах |
| topic_facet | Физика радиационных повреждений и явлений в твердых телах |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/14946 |
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