This dataset provides atmospheric concentrations of CO2, CH4, CO, and N2O measured by the Harvard Quantum Cascade Laser System (QCLS) instruments during airborne campaigns conducted by NASA's Atmospheric Tomography (ATom) mission. The QCLS (DUAL and CO2) instrument package contains two separate optical assemblies and calibration systems, and a common data system and power supply. The QCLS DUAL instrument simultaneously measures CO, CH4, and N2O concentrations, in situ, using two thermoelectrically cooled pulsed-quantum cascade lasers light sources, a multiple pass absorption cell, and two liquid nitrogen-cooled solid-state detectors. The QCLS CO2 instrument measures CO2 concentrations in situ using a thermoelectrically cooled pulsed-quantum cascade laser light source, gas cells, and liquid nitrogen cooled solid-state detectors. The CO2 mixing ratio of air flowing through the sample gas cell is determined by measuring absorption from a single infrared transition line at 4.32 microns relative to a reference gas of known concentration.