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We study the existence of left-invariant harmonic spinors on three-dimensional Lie groups equipped with a left-invariant pseudo-Riemannian metric. An existing formula for the spin Dirac operator acting on left-invariant spinors in the Riemannian setting is revised and specialised to our cases, in particular to almost Abelian Lie algebras. Focussing on dimension two and three, we find equivalent conditions for the Lie groups to admit left-invariant harmonic spinors in terms of constraints on the structure equations of the corresponding Lie algebras. We then identify those metrics (up to automorphism) carrying left-invariant harmonic spinors in each case.

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