Vibrational Spectra and Isotope Effect of Dihydroxylammonium 5,5’-Bis(Tetrazole)-1,1’-Diolate under High Pressure
ZHAO Sheng-xiang1, SONG Xue-yan2, XING Xiao-ling1, LI Yan2, JU Xue-hai2*
1. Xi’an Modern Chemistry Research Institute, Xi’an 710065, China
2. School of Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
Abstract：Density functional theory calculations were performed on crystalline dihydroxylammonium 5,5’-bis(tetrazole)-1,1’-diolate (HATO) under high pressure up to 40 GPa. The GGA-PW91 method in combination with the ultrasoft pseudopotentials reproduced the experimental crystal structure of HATO and was thus employed for the optimizations of both molecular structure and cell parameters. The intermolecular O…H distances generally decrease with increasing pressures. However, the O—H and N—H bond lengths change irregularly upon pressure. Based on the optimized crystal structures at different pressures, the non-periodic calculations of frequencies with a scaling factor of 0.967 9 were used to predict both the IR and Raman spectra. The predicted strongest Raman peak at 1 580 cm-1, involving C—C stretching and NH2 symmetric deformation, is in agreement with the experiment. Although there is no hydrogen atom in the anion moiety of HATO, the deuteration in cation still affects the vibrational mode of anion. For O—H and O—D vibration modes, the Raman shifts decrease due to the strengthening intermolecular hydrogen bond as the pressure increases. Upon deuteration, the most characterized change of Raman shifts for ND2 is that the ν2 stretching mode increases dramatically with high pressure as compared to those of NH2, which leads to a coupling of ND2ν2/ν3 modes at high pressure. The calculated isotopic ratios, ν(NH2)/ν(ND2) for ν1 to ν3 modes, are in the range of 1.36～1.38, which are in consistent with the value from the reduced masses of these atoms. The couplings of vibrational modes change with both deuteration and pressure.
Key words：Dihydroxylammonium 5,5’-bis(tetrazole)-1,1’-diolate (HATO); IR and Raman; High pressure; H/D Isotope effect; Density functional theory
基金资助: National Natural Science Foundation of China (21207066)
通讯作者:
居学海
E-mail: xhju@njust.edu.cn
作者简介: ZHAO Sheng-xiang, (1963—), research fellow, Xi’an Modern Chemistry Research Institute
引用本文:
赵省向，宋雪燕，邢晓玲，李 燕，居学海. 高压下1,1’-二羟基-5,5’-联四唑二羟胺盐的振动光谱及同位素效应[J]. 光谱学与光谱分析, 2019, 39(09): 2946-2952.
ZHAO Sheng-xiang, SONG Xue-yan, XING Xiao-ling, LI Yan, JU Xue-hai. Vibrational Spectra and Isotope Effect of Dihydroxylammonium 5,5’-Bis(Tetrazole)-1,1’-Diolate under High Pressure. SPECTROSCOPY AND SPECTRAL ANALYSIS, 2019, 39(09): 2946-2952.
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