Effect of sintering conditions on optical and mechanical

properties of MgAl2O4/Al2O3 laminated transparent

composite fabricated by spark-plasma-sintering (SPS)
processing
Lihong Liu, Koji Morita

I. Introduction
Over the past few decades, the transparent magnesium aluminate
(MgAl2O4) spinel polycrystal has attracted much attention and has been
extensively used as optical components due to its wide transparency,
The polycrystalline MgAl2O4 is expected to replace the sapphire single
crystal and polycrystalline AlON due to its isotropic cubic crystal
structure and relatively lower synthesis temperature. As compared to
Al2O3 and AlON, however, the mechanical properties of the
polycrystalline MgAl2O4 are relatively lower. Hence, for industrial
applications, the polycrystalline MgAl2O4 has been required to improve
its mechanical properties in addition to its optical properties. For the
MgAl2O4, the Al2O3 was chosen as the candidate laminating. By
combining the strong point of each phase, the MgAl2O4/Al2O3
laminated composite improved the hardness with maintaining the high
transparency. The obtained results indicate that since forming the Al2O3
layer on the MgAl2O4 is an effective method to simultaneously achieve
high optical and mechanical properties using the commercial powders, it
is possible to scale up the sample size using the relatively conventional
SPS processing.
II. Experimental procedure
1. Fabrication of MgAl2O4/Al2O3 laminated transparent composite
In order to fabricate the MgAl2O4/Al2O3 laminated transparent composite,
commercially- available MgAl2O4 powders were used as the starting materials.
The detailed experimental procedures were also described in our previous
paper. Briefly, as shown in Fig. 1, the MgAl2O4 and alumina powders were
individuallystacked in a sequence in a high-pressure sintering mold with an
inner diameter of 10 mm. The mold was surrounded by carbon felt to suppress
any heat losses from the mold surfaces. The stacked MgAl2O4 and Al2O3
powders were densified using an SPS machine to prepare the MgAl2O4/Al2O3
laminated transparent composites. The SPS processing was carried out at
temperatures of T = 1175- 1275 ◦C, heating rates of α= 5- 50 ◦C/min and dwell
timesof tD = 5- 30 min, under a constant uniaxial pressure of 300 MPa. For
comparison, the monolithic MgAl2O4 and Al2O3 were also fabricated at T =
1225 ◦C, α = 10 ◦C/min and tD = 10 min under a uniaxial pressure of 300 MPa.
During the sintering, the temperature was controlled by measuring the surface
temperature of the mold using an optical pyrometer through a hole made in
the carbon felt.

2. Characterization techniques
Using FE-SEM allows for the observation of the microstructure and lamellar
interface of the composite material. By counting the number of particles from
the SEM images, the particle size can be determined. Additionally, measuring
Tin and TIR enables the evaluation of the material's light transmittance within
the optical and infrared wavelength ranges.
The measurement of hardness (Hv) helps assess the mechanical properties of
the composite material. Measuring Hv, the material's hardness is determined
based on the formation of an indentation on the material's surface when a
load is applied.
Evaluating residual stress using X-ray diffraction method helps understand the
state of stress within the composite material. From the measured data, the
residual stress in the material can be calculated.

III. Results and discussion

1. Microstructural characteristics

- Photographs of the monolithic MgAl2O4 and the Al2O3/MgAl2O4 laminated

composite, which were sintered under the same conditions of T = 1225 C for t
= 10 min at α = 10 C/min, are shown in Fig. 2.
- Fig. 3(a) shows the low magnification cross- sectional SEM image of the
MgAl2O4/Al2O3 laminated transparent composite. This indicated that the
Al2O3 and MgAl2O4 phases were tightly bonded to each other without
forming any second phases (Fig. S1) and this microstructure agrees well with
the high transparency shown in Fig. 2.
- The EDS analysis data taken from the cross section are shown in Fig. 3(b–e).
The EDS spectrum shown in Fig. 3(b)
2. Sintering temperature

Fig. 4. Temperature dependent transmittance efficiencies, T and TIR, in the

wavelength range of (a) 0.2-1.6 μm and (b) 2.5-7 μm, respectively, for the
composites in sintered at several sintering temperatures; black:1175 C, red:
1225 C and blue: 1275 C.
3. Dwelling time tD dependence
Transmittance efficiencies of MgAl2O4/Al2O3 laminated composites sintered
at 1225°C were studied. For shorter wavelengths, the composite sintered for
30 minutes had slightly lower transmittance due to significant grain growth in
the Al2O3 phase. Increasing the sintering time improved transmittance. In the
infrared range, transmittance efficiency was consistent across all composites,
indicating that microstructural factors had little impact. Higher density
composites exhibited over 77% transmittance in the infrared range.
4. Heating rate α dependence
Transmittance of MgAl2O4/Al2O3 laminated composites decreased with
higher heating rates, resulting in lower values of Tin and TIR across the
wavelength range. Optimal microstructures with lower porosity and finer grain
size achieved higher transmittance in the visible range. The lowest heating rate
of 5°C/min yielded the highest Tin and TIR values. The decrease in
transmittance at higher heating rates was attributed to light scattering caused
by residual pores in the MgAl2O4 phase.
5. Mechanical property
Fig. 7. Sintering temperature T dependent Vickers hardness (Hv ) of the
MgAl2O4 and Al2O3 phases in the MgAl2O4/ Al2O3 laminated transparent
composites sintered at T = 1225 ◦C for tD = 10 min and α = 10 ◦C/min. For
comparison, Hv values of the monolithic MgAl2O4 and Al2O3, which were
sintered under the same SPS conditions, are also denoted by the closed square
and circle symbols.

Fig. 8. Lattice spacing d versus sin2ѱ for Al2O3 layer

Fig. 9. (a) Dwelling time tD and (b) heating rate α dependent Hv of the Al2O3
phase in the MgAl2O4/Al2O3 laminated transparent composites sintered at T =
1225 ◦C with α = 10 ◦C/min and at T = 1225 ◦C for tD = 10 min, respectively. (c)
Hall-Petch plot of the Al2O3 phase in the MgAl2O4/Al2O3 laminated
IV. Conclusions
1)The MgAl2O4/Al2O3 laminated composite fabricated by the optimum
SPS temperature, dwelling time and heating rate can successfully
attain the high and wide band transmittance, and mechanical
properties simultaneously.
2) At the optimum SPS condition, the laminated composite exhibits the
in-line transmission of Tin, 0.5= 50 % at a visible wavelength of λ =
0.5 μm and the IR transmission of TIR, 4 > 77 % at IR wavelength of λ
= 4 μm, which are similar to those of the monolithic MgAl2O4 with
the cubic crystal structure.
3) The Vickers hardness of the laminated composite exhibits 29 GPa,
which is higher than those of the monolithic Al2O3 (26.6 GPa) and
MgAl2O4 (17.2 GPa), with maintaining the high and wide band
transmittance.
4) It is found that the high optical and mechanical properties can be
ascribed to the smaller grain sizes and higher densities, which are
simultaneously attained in both the MgAl2O4 and Al2O3 phases in the
laminated composite. The necessary microstructural factors both for
the optical and mechanical properties can be realized by optimizing
the sintering conditions during the SPS processing.