Three-dimensional porous borocarbonitride composed of pentagonal motifs as a high-performance pyroelectric material

Pyroelectric materials have been attracting significant attention due to their intrinsic and permanent polarization, where the induced polarization is not associated with specific conditions, such as ferroelectric phase transition, strain gradient, dopants, and electric field. Thus, these materials have great potential for wide applications in energy conversion. Here, we propose a new 3D porous borocarbonitride termed PH-BCN, which is composed of pentagonal motifs with intrinsic polarization along the [0001] direction. Based on first-principles calculations, we show that PH-BCN possesses a record high longitudinal electromechanical coupling coefficient with the value of k₃₃ = 97.99%, a remarkably strong SHG response (χ(2)xzx(0) = χ(2)yzy(0) = χ(2)zxx(0) = χ(2)zyy(0) = -6.23 pm V^-1 and χ(2)zzz(0) = 21.21 pm V^-1), and a record high shift current value of 908.58 μA V^-2 due to the intrinsic vertical polarization. This study expands the family of pentagon-based materials, and may open a new frontier in the design of high-performance pyroelectric materials as well.