“…Halide perovskites have shown great promise for applications in photovoltaic and optoelectronic devices, which is attributed to their unique and prominent photoelectric properties like long carrier lifetime/diffusion length, high defect tolerance, strong light absorption, etc. Recently, there are also growing interests in the nonlinear optical properties of perovskites, [ 1–3 ] e.g., second harmonic generation, [ 4,5 ] two‐photon absorption (TPA), [ 6 ] higher‐order harmonic generation, [ 7 ] and multiphoton absorption, etc. For instance, methylammonium lead bromide (MAPbBr 3 , hereafter denoted as MAPB) single crystal has been demonstrated to possess strong TPA coefficients of around 8 cm GW −1 , [ 6,8 ] which make them potential candidates for many nonlinear optical applications such as nonlinear photodetector, [ 6 ] optical modulator, [ 9 ] bio‐imaging, [ 10 ] and two‐photon pumped laser, [ 11,12 ] etc.…”