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- W2022687089 abstract "An electric‐resonance optothermal spectrometer and phase‐locked backward‐wave oscillators are used to investigate the b type, ΔK=±1, Δm=0 spectrum of the hydrogen‐bonded HSH‐‐NH3 and H34SH‐‐NH3 complexes near 300 GHz. The spectrum is characterized by nearly free internal rotation of the NH3 subunit against the H2S, as initially concluded from Stark‐effect measurements by Herbine et al. [J. Chem. Phys. 93, 5485 (1990)]. Transitions are observed for the K=1←0, m=0, A symmetry and the K=0←±1 and K=±2←±1, m=±1, Km≳0, E‐symmetry subbands. The transitions are split into doublets with a 3:1 relative intensity ratio indicative of tunneling interchange of the two H2S protons. The observed selection rules, symmetric ↔ antisymmetric in the tunneling state, indicate that the tunneling motion reverses the sign of the molecular electric dipole moment component along the b inertial axis. The most likely interchange motion consists of a partial internal rotation of the H2S unit about its c inertial axis, through a bifurcated, doubly hydrogen‐bonded transition state. The proton interchange tunneling splittings of 859–864 MHz vary little between K and m states, indicating that the interchange motion is only weakly coupled to the internal rotation. The barrier to proton interchange is determined to be 510(3) cm−1, which can be compared to the ∼700 cm−1 barrier estimated from the 57 MHz tunneling splittings associated with the H2O proton interchange in the related HOH‐‐NH3 complex. The observation of dissociation of HSH‐‐NH3 following excitation of the NH3 umbrella mode with a line‐tunable CO2 laser places an upper bound of 992 cm−1 on the hydrogen‐bond zero‐point dissociation energy. The band origin for the umbrella vibration of 992.5(10) cm−1 is blueshifted by 43 cm−1 from the hypothetical inversion‐free band origin of uncomplexed NH3. Previous studies have shown that the HOH‐‐NH3 binding energy is greater than 1021 cm−1." @default.
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- W2022687089 date "1995-03-15" @default.
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- W2022687089 title "Proton interchange tunneling and internal rotation in HSH–NH<sub>3</sub>" @default.
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- W2022687089 doi "https://doi.org/10.1063/1.469480" @default.
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