The Fundamental Vibrational Frequencies and Spectroscopic Constants of the Dicyanoamine Anion, NCNCN$^-$ (C$_2$N$_3^-$): Quantum Chemical Analysis for Astrophysical and Planetary Environments

英文摘要：

Detecting anions in space has relied on a strong collaboration between theoretical and laboratory analyses to measure rotational spectra and spectroscopic constants to high accuracy. The advent of improved quantum chemical tools operating at higher accuracy and reduced computational cost is a crucial solution for the fundamental characterization of astrophysically-relevant anions and their detection in the interstellar medium and planetary atmospheres. In this context, we have turned towards the quantum chemical analysis of the penta-atomic dicyanoamine anion NCNCN$^-$ (C$_2$N$_3^-$), a structurally bent and polar compound. We have performed high-level coupled cluster theory quartic force field (QFF) computations of C$_2$N$_3^-$ satisfying both computational cost and accuracy conditions. We provide for the first time accurate spectroscopic constants and vibrational frequencies for this ion. In addition to exhibiting various Fermi resonances, C$_2$N$_3^-$ displays a bright $ν$2 (2130.9 cm$^{-1}$) and a less intense $ν$1 (2190.7 cm$^{-1}$) fundamental vibrational frequency, making for strong markers for future infrared observations < 5$μ$m. We have also determined near-IR overtone and combination bands of the bright fundamentals for which the 2$ν$2 at 4312.1 cm$^{-1}$ (2.319 $μ$m) is the best candidate. C$_2$N$_3^-$ could potentially exist and be detected in nitrogen-rich environments of the ISM such as IRC +10216 and other carbon-rich circumstellar envelopes, or in the atmosphere of Saturn's moon Titan, where advanced N-based reactions may lead to its formation.