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The structural properties of Co2(Cr1-xFex)Al annealed at various temperatures and prepared on heated substrates are demonstrated. The TMR properties of MTJs with the disordered Co2(Cr1-xFex)Al is also shown. Magnetoresistance measurement of the MTJs was performed by using a four-point probe technique. Film structures and oxidization at surfaces and interfaces were characterized by using X-ray diffraction (XRD) (Cu-Kα) and X-ray photoelectron spectroscopy (XPS) (Al-Kα), respectively.