Searching for the largest bound atoms in space
(abridged) Radio recombination lines (RRLs) at frequencies $ν$ < 250 MHz trace the cold, diffuse phase of the ISM. Next generation low frequency interferometers, such as LOFAR, MWA and the future SKA, with unprecedented sensitivity, resolution, and large fractional bandwidths, are enabling the exploration of the extragalactic RRL universe. We observed the radio quasar 3C 190 (z~1.2) with the LOFAR HBA. In reducing this data for spectroscopic analysis, we have placed special emphasis on bandpass calibration. We devised cross-correlation techniques to significantly identify the presence of RRLs in a low frequency spectrum. We demonstrate the utility of this method by applying it to existing low-frequency spectra of Cassiopeia A and M 82, and to the new observations of 3C 190. RRLs have been detected in the foreground of 3C 190 at z = 1.12355 (assuming a carbon origin), owing to the first detection of RRLs outside of the local universe (first reported in Emig et al. 2019). Towards the Galactic supernova remnant Cas A, we uncover three new detections: (1) C$ε$-transitions ($Δ$n = 5) for the first time at low radio frequencies, (2) H$α$-transitions at 64 MHz with a FWHM of 3.1 km/s, the most narrow and one of the lowest frequency detections of hydrogen to date, and (3) C$α$ at v$_{LSR}$ = 0 km/s in the frequency range 55-78 MHz for the first time. Additionally we recover C$α$, C$β$, C$γ$, and C$δ$ from the -47 km/s and -38 km/s components. In the nearby starburst galaxy, M 82, we do not find a significant feature. Our current searches for RRLs in LOFAR observations are limited to narrow (< 100 km/s) features, owing to the relatively small number of channels available for continuum estimation. Future strategies making use of larger contiguous frequency coverage would aid calibration to deeper sensitivities and broader features.