In this study, atomic-scale origin of the Invar effect, which is nearly-zero thermal expansion observed in the Invar alloy ${\mathrm{Fe}}_{65}{\mathrm{Ni}}_{35}$, was investigated by reverse Monte Carlo analysis using complementary data sets of extended x-ray absorption fine structure and x-ray diffraction. The interatomic distances of the nearest neighboring Fe-Fe atomic pairs were $\sim 0.02$ Å longer than those of the Fe-Ni and Ni-Ni pairs at the minimum pressure in this study (0.6 GPa). The elongation in the Fe-Fe pairs was suppressed with increasing pressure, and the distances of the three pairs were comparable under pressures above the magnetic transition from ferromagnetic to paramagnetic phase at $P_{\text{c}}\approx 7$ GPa. Therefore, the Fe-Fe pairs dominantly contribute to the volume expansion due to the magnetovolume effect. Because a similar magnitude of elongation was observed in the Fe-Fe pairs of a non-Invar Fe-Ni alloy, we conclude that the Invar effect originates from the delicate balance between the number of Fe-Fe pairs and their elongation depending on the magnetization.

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• Magnetoelastic effect
• Magnetostriction
• Pressure effects
• Structural properties
• Disordered alloys
• Transition metal alloys
• Monte Carlo methods
• X-ray absorption fine structure spectroscopy
• X-ray diffraction