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We investigate the twistor space and the Grassmannian fibre bundle of a Lorentzian 4-space with natural almost optical structures and its induced CR-structures. The twistor spaces of the Lorentzian space forms $\R^4_1, \Di{S}^4_1\Di{H}^4_1$ are explicitly discussed. The given twistor construction is applied to surface theory in Lorentzian 4-spaces. Immersed spacelike surfaces in a Lorentzian 4-space with special geometric properties like semi-umbilic surfaces and surfaces that have mean curvature of vanishing lengths correspond to holomorphic curves in the Lorentzian twistor space. For the Lorentzian space forms and those surfaces are explicitly constructed and classified.

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