Molecular clouds of gas and dust pervade our galaxy, and are the birthplaces of stars and planets. The temperature, density, and radiation conditions inside these clouds make them unique chemical laboratories for studying both fundamental reactions and the evolution of the molecular complexity that seeds primitive planets. We have recently discovered a new regime of unexpected low-temperature aromatic chemistry in these sources that has far-reaching implications on the lifecycle of carbon in the universe. These detections are demanding new analysis techniques to extract the maximum information content from increasingly large and complex datasets both observationally and in the laboratory. Here, I will discuss novel applications of signal processing and analysis in both arenas. Observationally, we are using Bayesian approaches combined with matched filtering techniques, while in the laboratory, we are conducting reaction screening analyses to try to understand the content and evolution of this new carbon chemistry in space. I will describe the results of our new observational analysis techniques, as well as outline several new methods we have developed for rapidly screening complex chemical mixtures in the laboratory using pump-probe rotational spectroscopy in a (semi-)automated fashion to enable new molecular discovery.