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Py4CAtS (PYthon scripts for Computational ATmospheric Spectroscopy) implements the individual steps of an infrared or microwave radiative transfer computation in separate scripts (and corresponding functions) to extract lines of relevant molecules in the spectral range of interest, compute line-by-line cross sections for given pressure(s) and temperature(s), combine cross sections to absorption coefficients and optical depths, and integrate along the line-of-sight to transmission and radiance/intensity. The code is a Python re-implementation of the Fortran code GARLIC (Generic Atmospheric Radiation Line-by-line Code) and uses the Numeric/Scientific Python modules for computationally-intensive highly optimized array-processing. Py4CAtS can be used in the console/terminal, inside the (I)Python interpreter, and in Jupyter notebooks.