We present the first results of a survey of 220 starless cores selected primarily by their optical obscuration and observed in CS (2-1), N_2_H^+^ (1-0), and C^18^O (1-0) using the Northeast Radio Observatory Corporation (NEROC) Haystack 37 m telescope. We have detected 163 out of 196 sources observed in CS, 72 out of 142 in N_2_H^+^, and 30 out of 30 in C18O. In total, 69 sources were detected in both CS and N_2_H^+^. The isolated component of the N_2_H^+^ (1-0) spectrum (F_1_F = 0,1-1,2) usually shows a weak symmetric profile that is optically thin. In contrast, a significant fraction of the CS spectra show non-Gaussian shapes, which we interpret as arising from a combination of self-absorption due to lower excitation gas in the core front and kinematics in the core. The distribution of the normalized velocity difference ({delta}V_CS_) between the CS and N_2_H^+^ peaks appears significantly skewed to the blue (V_CS_ < 0), as was found in a similar study of dense cores with embedded young stellar objects (YSOs). The incidence of sources with blue asymmetry tends to increase as the total optical depth or the integrated intensity of the N_2_H^+^ line increases.
Cone search capability for table J/ApJ/526/788/table1 (Starless Cores Observed in CS, N_2_H^+^, and C^18^O)
Cone search capability for table J/ApJ/526/788/table2 (Parameters of starless cores observed in both CS and N_2_H^+^)