This data set contains Level 1 spectral radiance data collected using the Fourier Transform Spectrometer (FTS) during airborne campaigns over the Alaskan and Canadian Arctic for the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE). Flight campaigns took place from 2012 to 2015 between the months of March and November to enable investigation of both seasonal and inter-annual variability in atmospheric gas content. The measurements included in this data set are crucial for understanding changes in Arctic carbon cycling and the potential threats posed by thawing of Arctic permafrost.