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Sub-Doppler slit jet infrared spectroscopy of astrochemically relevant cations: Symmetric (ν 1 ) and antisymmetric (ν 6 ) NH stretching modes in ND 2 H 2 .

Sub-Doppler infrared rovibrational transitions in the symmetric (v1 ) and antisymmetric (v6 ) NH stretch modes of the isotopomerically substituted ND2 H2 + ammonium cation are reported for the first time in a slit jet discharge supersonic expansion spectrometer. The partially H/D substituted cation is generated by selective isotopic exchange of ND3 with H2 O to form NHD2 , followed by protonation with H3 + formed in the NHD2 /H2 /Ne slit-jet discharge expansion environment. Rotational assignment for ND2 H2 + is confirmed rigorously by four line ground state combination differences, which agree to be within the sub-Doppler precision in the slit jet (∼9 MHz). Observation of both b-type (ν1 ) and c-type (ν6 ) bands enables high precision determination of the ground and vibrationally excited state rotational constants. From an asymmetric top Watson Hamiltonian analysis, the ground state constants are found to be A″ = 4.856 75(4) cm-1 , B″ = 3.968 29(4) cm-1 , and C″ = 3.446 67(6) cm-1 , with band origins at 3297.5440(1) and 3337.9050(1) cm-1 for the v1 and v6 modes, respectively. This work permits prediction of precision microwave/mm-wave transitions, which should be invaluable in facilitating ongoing spectroscopic searches for partially deuterated ammonium cations in interstellar clouds and star-forming regions of the interstellar medium.

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