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Femtosecond ͑fs͒ dynamics of reactions of cyclic ethers, symmetric and asymmetric structures, are reported. The diradical intermediates and their ␤-cleavages, which involve simultaneous C-C, C-H -bond breakage and C-O, C-C -bond formation, are observed and studied by fs-resolved mass spectrometry. To compare with experiments, we present density functional theory calculations of the potential energy surface and microcanonical rates and product distributions.

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