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In this work, the polar tetrahedron [PN$_2$O$_2$] was revealed as a newdeep-ultraviolet (deep-UV) nonlinear optically active unit. Accordingly, athermodynamically stable compound (PNO) consisting of the polar [PN$_2$O$_2$]units was predicted and suggested as a promising candidate of deep-UV nonlinearoptical (NLO) material. Compared with other deep-UV materials known to date,PNO possesses the strongest second harmonic generation (SHG) coefficient (about6 times that of KH$_2$PO$_4$ (KDP)). Moreover, its three-dimensionalconnectivity endows it with good mechanical and thermal properties. Therefore,PNO should be a new option for non-$\pi$-conjugated deep-UV NLO materials.

PNO: A Promising Deep-UV Nonlinear Optical Material with Extremely High Second Harmonic Generation Effect