Nanometer interatomic distances in Rydberg Matter clusters confirmed by phase-delay spectroscopy

Recently, rotational spectroscopy in the radio frequency range was used to determine the bond lengths in several types of potassium Rydberg Matter (RM) clusters with high precision (Mol Phy 105: 933–939, 2007). Due to the large bond lengths of a few nm and well-ordered structure of such clusters, it is expected that light scattering can be used to determine their dimensions. A weak carbon dioxide laser beam is introduced collinearly into a tunable RM cavity. When RM is formed, a very pronounced fringe structure with several hundred fringes is observed at the detector as a function of the grating position. These fringes show a phase delay of the carbon dioxide laser light caused by reflections within the RM clusters. The delay lengths derived from the fringe structure give distances between the rows of atoms in the clusters. The excitation level of the most easily observed clusters is n = 5. Clusters with n = 6, 7, and 8 are also commonly detected. The bond distance for n = 5 is found to be 3.804 ± 0.015 nm, while that for n = 6 is 5.525 ± 0.014 nm, in accurate agreement with values from rotational spectroscopy.