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Molecular helium represents a benchmark system for testing $\textit{ab initio}$ calculations on few-electron molecules. We report on the determination of the adiabatic ionization energy of the $a\,^3\Sigma_u^+$ state of He$_2$, corresponding to the energy interval between the $a\,^3\Sigma_u^+$ ($v''=0$, $N''=1$) state of He$_2$ and the $X^+\,^2\Sigma_u^+$ ($v^+=0$, $N^+=1$) state of He${_2}^+$, and of the lowest rotational interval of He${_2}^+$. These measurements rely on the excitation of metastable He$_2$ molecules to high Rydberg states using frequency-comb-calibrated continuous-wave UV radiation in a counter-propagating-laser-beam setup. The observed Rydberg states were extrapolated to their series limit using multichannel quantum-defect theory. The ionization energy of He$_2$ ($a\,^3\Sigma_u^+$) and the lowest rotational interval of He${_2}^+$ ($X^+\,^2\Sigma_u^+$) are 34301.207002(23)$\pm 0.000037_{\mathrm{sys}}$ cm$^{-1}$ and 70.937589(23)$\pm 0.000060_{\mathrm{sys}}$ cm$^{-1}$, respectively.

The term values of all rotational levels of the $^4$He${_2}^+\,X^+\,^2\Sigma_u^+\,(\nu^+=0)$ ground vibronic state with rotational quantum number $N^+\le 19$ have been determined with an accuracy of 8 x 10$^{-4}$ cm$^{-1}$ ($\sim{25}$ MHz) by MQDT-assisted Rydberg spectroscopy of metastable He$_2^*$. Comparison of these term values with term values recently calculated ab initio by Tung et al. [J. Chem. Phys. 136, 104309 (2012)] reveal discrepancies that rapidly increase with increasing rotational quantum number and reach values of 0.07 cm$^{-1}$ ($\sim{2.1}$ GHz) at $N^+=19$., Comment: 11 pages, 6 figures

Recently, high-resolution spectroscopy of slow beams of metastable helium molecules (He$_2^*$) generated by multistage Zeeman deceleration was used in combination with Rydberg-series extrapolation techniques to obtain the lowest rotational interval in the molecular helium ion at a precision of 18 MHz [Jansen et al. Phys. Rev. Lett. 115 (13) (2015) 133202], limited by the temporal width of the Fourier-transform-limited laser pulses used to record the spectra. We present here an extension of these measurements in which we have (1) measured higher rotational intervals of He${_2}^+$, (2) replaced the pulsed UV laser by a cw UV laser and improved the resolution of the spectra by a factor of more than five, and (3) studied $M_J$ redistribution processes in regions of low magnetic fields of the Zeeman decelerator and shown how these processes can be exploited to assign transitions originating from specific spin-rotational levels ($N^{\prime\prime},J^{\prime\prime}$) of He$_2^*$., Comment: 28 pages, 8 figures