Development of polar nematic fluids with giant-\k{appa} dielectric properties

Super-high-\k{appa} materials that exhibit exceptionally high dielectric permittivity are recognized as potential candidates for a wide range of next-generation photonic and electronic devices. Generally, the high dielectricity for achieving a high-\k{appa} state requires a low symmetry of materials so that most of the discovered high-\k{appa} materials are symmetry-broken crystals. There are scarce reports on fluidic high-\k{appa} dielectrics. Here we demonstrate a rational molecular design, supported by machine-learning analyses, that introduces high polarity to asymmetric molecules, successfully realizing super-high-\k{appa} fluid materials (dielectric permittivity, {\epsilon} > 104) and strong second harmonic generation with macroscopic spontaneous polar ordering. The polar structures are confirmed to be identical for all the synthesized materials. Our experiments and computational calculation reveal the unique orientational structures coupled with the emerging polarity. Furthermore, adopting this strategy to high-molecular-weight systems additionally extends the novel material category from monomer to polar polymer materials, creating polar soft matters with spontaneous symmetry breaking.