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Laser Induced Breakdown Spectroscopy (LIBS) in the Ultra Violet/Visible/Near-IR (UVN) spectral range is a powerful analytical tool that facilitates the interpretation of Raman spectroscopic data by providing additional details in elemental chemistry. To acquire the complete information of molecular vibrations for more accurate and precise chemical bonding and structural analysis, an ideal in situ optical sensing facility should be able to rapidly probe the broad vibrational dipole and polarizability responses of molecules by acquiring both Raman scattering and mid-IR emission spectroscopic signatures. Recently, the research team at Brimrose has developed a novel optical technology, Long-Wave IR (LWIR) LIBS. Critical experimental approaches were made to capture the infrared molecular emission signatures from vibrationally excited intact samples excited by laser-induced plasma in a LIBS event. LWIR LIBS is the only fieldable mid-IR emission spectroscopic technique to-date that that offers the same instrumental and analytical advantages of both UVN LIBS and Raman spectroscopy in in-situ stand-off field applications and can perform rapid and comprehensive molecular structure analysis without any sample-preparation.•A single excitation laser pulse is used to trigger both UVN and LWIR spectrometers simultaneously.•Time-resolved UVN-LWIR LIBS measurements showed the evolution of both atomic and molecular signature emissions of target compounds in the laser-induced plasma.•The technique was applied to the characterization of mineral and organic compounds in planetary analog samples., Competing Interests: The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (© 2022 The Authors.)