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Abstract
Nitrogen has five valence electrons and can form a maximum of three shared electron-pair bonds to complete its octet, which suggests that its maximum bond order is three. With a joint anion photoelectron spectroscopy and quantum chemistry investigation, we report herein that nitrogen presents a quadruple bonding interaction with thorium in ThN. The quadruple Th≣N bond consists of two electron-sharing Th-N π bonds formed between the Th-6dxz/6dyz and N 2px/2py orbitals, one dative Th←N σ bond and one weak Th←N σ bonding interaction formed between Th-6dz2 and N 2s/2pz orbitals. The ThC molecule has also been investigated and proven to have a similar bonding pattern as ThN. Nonetheless, due to one singly occupied σ-bond, ThC is assigned a bond order of 3.5. Moreover, ThC has a longer bond length as well as a lower vibrational frequency in comparison with ThN.
Nitrogen can form a maximum of three shared electron-pair bonds to complete its octet, suggesting the maximum bond order of nitrogen is three. Here, the authors report a joint photoelectron spectroscopy and quantum chemical study, showing a quadruple bond between nitrogen and thorium in thorium nitride.
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1 Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Key Laboratory of Interfacial Physics and Technology, Shanghai, China (GRID:grid.450275.1) (ISNI:0000 0000 9989 3072)
2 Tsinghua University, Department of Chemistry, Beijing, China (GRID:grid.12527.33) (ISNI:0000 0001 0662 3178); Beijing Forestry University, College of Science, Beijing, China (GRID:grid.66741.32) (ISNI:0000 0001 1456 856X)
3 Collaborative Innovation Center of Quantum Matter, Tsinghua University, Department of Physics, State Key Laboratory of Low Dimensional Quantum Physics, Beijing, China (GRID:grid.495569.2)
4 Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Key Laboratory of Interfacial Physics and Technology, Shanghai, China (GRID:grid.450275.1) (ISNI:0000 0000 9989 3072); University of Chinese Academy of Sciences, Beijing, China (GRID:grid.410726.6) (ISNI:0000 0004 1797 8419)
5 Tsinghua University, Department of Chemistry, Beijing, China (GRID:grid.12527.33) (ISNI:0000 0001 0662 3178)
6 Sun Yat-sen University, Sino-French Institute of Nuclear Engineering and Technology, Zhuhai, China (GRID:grid.12981.33) (ISNI:0000 0001 2360 039X)