In multifrequency atomic force microscopy (AFM) to simultaneously measure topography and material properties of specimens, it is highly desirable that the higher order resonance frequencies of the cantilever probe are assigned to be integer harmonics of the excitation frequency. The harmonic resonances are essential for significant enhancement of the probe's response at the specified harmonic frequencies. In this letter, a structural optimization technique is employed to design cantilever probes so that the ratios between one or more higher order resonance frequencies and the fundamental natural frequency are ensured to be equal to specified integers and, in the meantime, that the fundamental natural frequency is maximized. Width profile of the cantilever probe is the design variable in optimization. Thereafter, the probes were prepared by modifying a commercial probe through the focused ion beam (FIB) milling. The resonance frequencies of the FIB fabricated probes were measured with an AFM. Results of the measurement show that the optimal design of probe is as effective as design prediction.

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