Interface constitutes a significant volume fraction in nanocomposites, and it requires the ability to tune and tailor interfaces to tap the full potential of nanocomposites. However, the development and optimization of nanocomposites is currently restricted by the limited exploration and utilization of interfaces at different length scales. In this research, we have designed and introduced a relatively large-scale vertical interphase into carbon nanocomposites, in which the dielectric response and dispersion features in microwave frequency range are successfully adjusted. A remarkable relaxation process has been observed in vertical-interphase nanocomposites, showing sensitivity to both filler loading and the discrepancy in polarization ability across the interphase. Together with our analyses on dielectric spectra and relaxation processes, it is suggested that the intrinsic effect of vertical interphase lies in its ability to constrain and localize heterogeneous charges under external fields. Following this logic, systematic research is presented in this article affording to realize tunable frequency-dependent dielectric functionality by means of vertical interphase engineering. Overall, this study provides a novel method to utilize interfacial effects rationally. The research approach demonstrated here has great potential in developing microwave dielectric nanocomposites and devices with targeted or unique performance such as tunable broadband absorbers.
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