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We consider reheating driven by volume modulus decays in the LARGE Volume Scenario. Such reheating always generates non-zero dark radiation through the decays to the axion partner, while the only competitive visible sector decays are Higgs pairs via the Giudice-Masiero term. In the framework of sequestered models where the cosmological moduli problem is absent, the simplest model with a shift-symmetric Higgs sector generates 1.56 < N_{eff} - N_{eff,SM} < 1.74. For more general cases, the known experimental bounds on N_{eff} strongly constrain the parameters and matter content of the models.

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