We report measurements of circular polarization from the first two years of observation with the 40 GHz polarimeter of the Cosmology Large Angular Scale Surveyor (CLASS). CLASS is conducting a multi-frequency survey covering 75% of the sky from the Atacama Desert designed to measure the cosmic microwave background (CMB) linear E and B polarization on angular scales 1°  θ 90°, corresponding to a multipole range of 2 ℓ  200. The modulation technology enabling measurements of linear polarization at the largest angular scales from the ground, the Variable-delay Polarization Modulator, is uniquely designed to provide explicit sensitivity to circular polarization (Stokes V ). We present a first detection of circularly polarized atmospheric emission at 40 GHz that is well described by a dipole with an amplitude of 124 4 K  m when observed at an elevation of 45°, and discuss its potential impact on the recovery of linear polarization by CLASS. Filtering the atmospheric component, CLASS places a 95% confidence upper limit of 0.4 Km 2 to 13.5 Km 2 on ℓℓ C ( ) () + 1 2 ℓ p VV for 1 120  ℓ , representing an improvement by two orders of magnitude over previous CMB limits.