When is an exact 2-form harmonic?

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Let $\alpha$ be an exact two-form, $\alpha=d\beta$ for some one-form $\beta$, when is $\alpha$ harmonic? By uniqueness of harmonic forms in cohomology classes, it cannot be harmonic?

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Yes, you answered your own question. If $\alpha=d\beta$, it is zero in cohomology, but harmonic forms represent nontrivial cohomology classes. Like you said, you can see this by uniqueness, since the 0 form also represents $0$ in cohomology.