The results of the lowest frequency spectral survey carried out toward a molecular cloud and sensitive observations at selected frequencies are presented. The entire Arecibo C-band (4--6 GHz) was observed towards the cyanopolyyne peak of TMC-1 with an rms sensitivity of about 17--18 mK (about 2--2.5 mJy). In addition, a number of selected frequency ranges within the C-band and X-band (8--10 GHz) were observed with longer integration times and rms sensitivities 7--8 mK (about 2 mJy) or higher. In the spectral scan itself, already--known H2CO and HC5N lines were detected. However, in more sensitive observations at selected frequencies, lines of C2S, C3S, C4H, C4H2, HC3N and its 13C substituted isotopic species, HC5N, HC7N, and HC9N were found, about half of them detected for the first time. The rotational temperatures of the detected molecules fall in the range 4--9 K. Cyanopolyyne column densities vary from 5.6x10^{13} cm^{-2} for HC5N to 2.7x10^{12} cm^{-2} for HC9N. Our results show that for molecular observations at low frequencies (4--10 GHz) to be useful for studying dark clouds, the sensitivity must be of the order of 5--10 mK or better. To date, observations at around 10 GHz have been more productive than those at lower frequencies.
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