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Overtone spectroscopy is used to observe the rovibrational spectra of the hydrogen isotopologues H2, HD, and D2 adsorbed in the metal–organic framework known as MOF-5. It is shown that the overtone spectrum facilitates the identification of hydrogen modes which are obscured in the fundamental region by the presence of MOF-5 features. Further, the overtone spectrum of H2 at the primary adsorption site...
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