Mengjia Shi, Zirui Jia, Shuai Xu, Zhenguo Gao, Guanglei Wu
ABSTRACT Constructing heterogeneous structures to precisely regulate the interface characteristics and loss mechanisms of materials is the key to performance improvement. This study proposes a strategy of constructing the NiS 2 ‐CdS P‐N heterojunction with Porous carbon nanofibers (PCNFs) as the supporting skeleton, and deeply investigates the influence of the interface regulation mechanism of the P‐N heterojunction on the absorption performance. The study clarified the structural reconstruction information such as bond parameter distortion, atomic occupation deviation, and lattice disorder caused by the Built‐in electric field (BIEF) of the P‐N heterojunction through X‐Ray Diffraction (XRD) refinement. With the help of Density functional theory (DFT) calculation, the performance regulation mechanism of the heterojunction was revealed at the atomic/electronic scale. A carrier migration model between NiS 2 and CdS was constructed, and the absorption mechanism was analyzed. By utilizing the BIEF and space charge region formed by NiS 2 and CdS, the equivalent impedance is regulated. Ultimately, the cooperative optimization of material impedance matching and energy dissipation is achieved, providing new ideas and development of high‐performance electromagnetic wave (EMW) absorbing materials. This research provides theoretical support for the subsequent shift of absorbing materials from empirical synthesis to precise design.