Laser driven transitions from the metastable a3Σ+u state to the predissociating level v′=4 of the electronic state c3Σ+g of He2 are investigated by fast beam laser spectroscopy. For transitions to the rotational levels N′=8, 10, and 12 of the c3Σ+g state, the fine structure is resolved and the fine structure parameters of both electronic states can be determined. The fine structure in the rotational levels N″=7, 9, and 11 of v″=0 in the a3Σ+u state is measured to 20 kHz precision (3σ) using laser–radio frequency double‐resonance spectroscopy. These measurements are complementary to the previous radio frequency (rf) measurements for the levels N″=1, 3, and 5 by Lichten etal. The fine structure parameters are compared to theoretical calculations and simple models for the electronic interactions and the couplings between different electronic states.

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