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Negative piezoelectrics contract in the direction of applied electric field,which are opposite to normal piezoelectrics and rare in dielectric materials.The raising of low dimensional ferroelectrics, with unconventional mechanismsof polarity, opens a fertile branch for candidates with prominent negativepiezoelectricity. Here, the distorted $\alpha$-Bi monolayer, a newly-identifiedelementary ferroelectric with puckered black phosphorous-like structure [J.Guo, {\it et al}. Nature \textbf{617}, 67 (2023)], is computationally studied,which manifests a large negative in-plane piezoelectricity (with$d_{33}\sim-26$ pC/N). Its negative piezoelectricity originates from its uniquebuckling ferroelectric mechanism, namely the inter-column sliding.Consequently, a moderate tensile strain can significantly reduce itsferroelectric switching energy barrier, while the compressive strain cansignificantly enhance its prominent nonlinear optical response. The physicalmechanism of in-plane negative piezoelectricity also applies to otherelementary ferroeletric monolayers.

Large in-plane negative piezoelectricity and giant nonlinear optical susceptibility in elementary ferroelectric monolayers