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This paper proposes a new optical angle measurement method in the optical frequency domain based on second harmonic generation with a mode-locked femtosecond laser source by making use of the unique characteristic of the high peak power and wide spectral range of the femtosecond laser pulses. To get a wide measurable range of angle measurement, a theoretical calculation for several nonlinear optical crystals is performed. As a result, LiNbO3 crystal is employed in the proposed method. In the experiment, the validity of the use of a parabolic mirror is also demonstrated, where the chromatic aberration of the focusing beam caused the localization of second harmonic generation in our previous research. Moreover, an experimental demonstration is also carried out for the proposed angle measurement method. The measurable range of 10,000 arc-seconds is achieved.

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