Atomically Polarization Regulation in Molybdenum Disulfide Nanosheets via Phase Transition Engineering for Superior Electromagnetic Wave Dissipation

Disentangling the limitations of dipole activity at the atomic scale in the dielectric materials is key to boosting the intrinsic polarization ability and electromagnetic (EM) energy dissipation. Herein, an atomic structure regulation in molybdenum disulfide (MoS2) nanosheets (NSs) connected by multi‐wall carbon nanotubes (MoS2‐MWCNTs) is studied to explore the correlation between the local atomic structure and polarization properties at the atomic scale. Induced by the phase transition engineering, 1T‐phase dominated MoS2 NSs with centrosymmetric D3d point groups are evolved from the 2H‐phase structure. Atomic‐scale and visualized electric field distribution in the MoS2 NSs are verified by the advanced integrated differential phase contrast technology and related scanning transmission electron microscopy (iDPC‐STEM) imaging. Periodic atomic structure in the 1T‐phase MoS2 is constructed to enhance symmetrical electric field distribution and those phase interlaced regions promoted a significant increase in dielectric relaxation. Benefiting the boosted dielectric ability and polarization behaviors, 1T‐phase dominated MoS2@MWCNTs (TMC) exhibit superior EM wave energy dissipation with the minimum reflection loss (RLmin) value of −74.3 dB at only 1.7 mm thickness. Changes in atomic structure and electric field study in the MoS2 NSs help to further elucidate their polarization mechanism and to explore the for studying the mixed‐phase 2D functional nanosheets.