The measurement of mechanical properties of high-temperature resistant materials at high temperatures is particularly critical, and laser ultrasonic non-destructive testing technology is a prospective approach for measuring mechanical properties in high-temperature environments. Laser ultrasonic propagation models are constructed by finite element analysis, which reveals the effects of different excitation mechanisms on acoustic velocity measurements. It is found that the shear wave in the main propagation direction is hardly detected, and the distinction between shear waves and surface waves in the time domain signal is difficult. Based on the conclusions, the relationships between surface waves, longitudinal waves, and mechanical properties of materials are established by theoretical derivation. According to the propagation characteristics of surface waves and longitudinal waves, the eccentricity detection scheme of the same side and the concentricity detection scheme of the opposite side are, respectively, designed. The velocities of surface waves and longitudinal waves are measured, considering the thermal expansion coefficient and density changes with temperature. The mechanical properties of materials at different temperatures (25–1000 °C) are successfully calculated, and the experimental results are well in accordance with the reference values. It gives a reliable basis for efficient measurement of mechanical properties of materials at high temperatures.
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