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Totally isotropic surfaces in are not necessarily Willmore surfaces. Therefore it is the first goal of this paper to derive a geometric characterization of totally isotropic Willmore two-spheres in . This will naturally yield to a description of such surfaces in terms of the loop group language. Moreover, applying the loop group method, we also obtain an algorithm to construct totally isotropic Willmore two-spheres in . As an application, a new, totally isotropic Willmore two-sphere which is not S-Willmore (i.e., has no dual surface) in is constructed, illustrating the theory of this paper.

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