Atmospheric carbon monoxide (CO) is an effective tracer for monitoring atmospheric transport processes and for detecting pollution sources of anthropogenic origin. However, very few observation systems exist that are capable of providing measurements with high spatial and temporal resolution to identify hotspots for emission control purposes. Here we introduce a mountain-top remote sensing observatory, the California Laboratory for Atmospheric Remote Sensing (CLARS), for mapping the enhancement of CO column-averaged mixing ratio (XCO) over the Los Angeles (LA) megacity. Compared to conventional observation network, CLARS is unique in the following ways: (1) it mimics a geostationary satellite observatory for LA with approximately hourly- and kilometer-scale mapping capability; (2) the free tropospheric background atmosphere is simultaneously measured; and (3) the measurements are highly sensitive to anthropogenic emissions due to the long light path along the planetary boundary layer (PBL). The CO slant column density and XCO are retrieved from reflected sunlight measurements in the 2.3 μm CO band and the 1.27 μm oxygen (O2) band. Data filtering and corrections for aerosol scattering and geometric effects are then implemented to derive the XCO enhancement, which is the XCO excess in the PBL compared to the background value. In the LA megacity, the XCO enhancement shows a distinctive diurnal cycle primarily driven by changes in anthropogenic emissions and sea-breeze circulation. Such diurnal patterns can be reproduced by the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). The enhancement also shows a significant weekly cycle resulting from the weekly pattern in anthropogenic CO emissions. On average, the XCO enhancements on Sunday and Saturday are 16.1% and 4.4%, respectively, lower than weekday values. The weekly XCO enhancement patterns also show high correlation with traffic counts. A seasonal pattern of XCO enhancement with high (low) spatial contrast in summer (winter), resulting from changing sea-breeze circulation, can be observed. These diurnal, weekly, and seasonal patterns of XCO enhancement serve as tracers of the atmospheric pulse of the LA megacity. The CLARS observatory can serve as a testbed for future geostationary missions to track anthropogenic emissions in cities. •A mountaintop remote sensing observatory for mapping XCO in LA is introduced;•Maps of XCO enhancement at hour- and kilometer-scales are generated;•The diurnal, weekly, and seasonal pulses of XCO enhancement are investigated;•WRF-Chem simulations reproduce the observed spatial XCO patterns;•The observatory is a testbed for future geostationary missions to track emissions.