The neon dimers were prepared in a molecular beam under supersonic expansion of gaseous neon at a temperature of 60 K through a 5 µm nozzle (see Supplementary Figure 1 ). The nozzle temperature was stabilized within ±0.1 K by a continuous flow cryogenic cryostat (Model RC110 UHV, Cryo Industries of America, Inc.). The optimum dimer yield was found at a nozzle back pressure of 3 bar. Neon dimers were selected from the molecular beam by means of matter wave diffraction using a transmission grating with a period of 100 nm. The selection allowed increasing the relative yield of Ne2 from typically 2%12 (link) to 20% with respect to the monomer.
The neon dimers were singly ionized by a strong ultra-short laser field (40 fs -FWHM in intensity -, 780 nm, 8 kHz, Dragon KMLabs). The field intensities were 7.3×1014 W cm−2 (Keldysh parameter γ = 0.72) in case of circular polarization and 1.2×1015 W cm−2 (γ = 0.4) in the experiment with linearly polarized light. The 3D-momenta of the ion and the electron after ionization were measured by cold target recoil ion momentum spectroscopy (COLTRIMS). In the COLTRIMS spectrometer a homogeneous electric field of 16 V cm−1 for circularly polarized light, or 23 V cm−1 in case of linearly polarized laser field, guided the ions onto a time- and position-sensitive micro-channel plate detector with hexagonal delay-line position readout42 (link) and an active area of 80 mm. In order to achieve 4π solid angle detection of electrons with momenta up to 2.5 a.u., a magnetic field of 12.5 G was applied within the COLTRIMS spectrometer in the experiment with the circularly polarized laser field. In the case of linearly polarized light a magnetic field of 9 G was utilized. The ion and electron detectors were placed at 450 mm and 250 mm, respectively, away from the ionization region.
The neon dimers were singly ionized by a strong ultra-short laser field (40 fs -FWHM in intensity -, 780 nm, 8 kHz, Dragon KMLabs). The field intensities were 7.3×1014 W cm−2 (Keldysh parameter γ = 0.72) in case of circular polarization and 1.2×1015 W cm−2 (γ = 0.4) in the experiment with linearly polarized light. The 3D-momenta of the ion and the electron after ionization were measured by cold target recoil ion momentum spectroscopy (COLTRIMS). In the COLTRIMS spectrometer a homogeneous electric field of 16 V cm−1 for circularly polarized light, or 23 V cm−1 in case of linearly polarized laser field, guided the ions onto a time- and position-sensitive micro-channel plate detector with hexagonal delay-line position readout42 (link) and an active area of 80 mm. In order to achieve 4π solid angle detection of electrons with momenta up to 2.5 a.u., a magnetic field of 12.5 G was applied within the COLTRIMS spectrometer in the experiment with the circularly polarized laser field. In the case of linearly polarized light a magnetic field of 9 G was utilized. The ion and electron detectors were placed at 450 mm and 250 mm, respectively, away from the ionization region.