Li(NH(3))(4) has been proposed as a key entity in lithium-ammonia solutions, but its spectral signature has so far proved impossible to distinguish from other species in these solutions. Here we report the first electronic spectrum of Li(NH(3))(4) in the gas phase, which was recorded using mass-selective depletion spectroscopy. Strong absorption is observed in the near-infrared and the band system is assigned to the A (2)T(2)-X (2)A(1) transition in a nominally tetrahedral complex. However, the vibrational structure is indicative of a substantial Jahn-Teller effect in the excited electronic state. The broad and structured spectrum confirms a recent theoretical prediction that the electronic spectrum of Li(NH(3))(4) will strongly overlap with the spectrum of the solvated electron in lithium-ammonia solutions.
Electronic spectra of LiNH 3 and its partially and fully deuterated analogues are reported for the first time. The spectra have been recorded in the near-infrared and are consistent with two electronic transitions in close proximity, theà 2 E−X 2 A 1 andB 2 A 1 −X 2 A 1 systems. Vibrational structure is seen in both systems, with the Li-N-H bending vibration (ν 6 ) dominant in theà 2 E−X 2 A 1 system and the Li-N stretch (ν 3 ) in theB 2 A 1 −X 2 A 1 system. The prominence of the 6 1 0 band in theà 2 E−X 2 A 1 spectrum is attributed to Herzberg-Teller coupling. The proximity of theB 2 A 1 state, which lies a little more than 200 cm −1 above theà 2 E state, is likely to be the primary contributor to this strong vibronic coupling.
We report the first spectroscopic study of a complex consisting of a rare earth atom in combination with ammonia. Using two-color resonance-enhanced multiphoton ionization (REMPI) spectroscopy, the lowest energy electronic transition of YbNH 3 has been found in the near-infrared. The spectrum arises from a spin-forbidden transition between the 1 A 1 ground electronic state and the lowest 3 E excited electronic state. The transition is metal centered and approximately correlates with the Yb 6s6p 3 P ← 6s 2 1 S transition. The observation of clear spin-orbit structure in the spectrum confirms the C 3v symmetry of YbNH 3 . Vibrational structure is also observed in the REMPI spectrum, which is dominated by excitation of the Yb-N stretching vibration.
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