B-Site Nanoscale-Ordered Structure Enables Ultra-High Tunable Performance.

Tunable devices constructed by ferroelectric thin films are often desired to possess a low dielectric loss while maintainging a high dielectric tunability over a broad operating temperature range in applications, for example, resonators, filters, or phase shifters. However, it is difficult to simultaneously achieve these characteristics by traditional strategies, such as doping and strain modifying. Here, we demonstrate that the dielectric tunability of the sol-gel-prepared Pb(Sc_1/2Nb_1/2)_0.9(Mg_1/3Nb_2/3)_0.1O₃ (PSNMN) thin film can be almost doubled from ~47% to ~80.0% (at 10 kHz) at a low electric field (~530 kV/cm), and the dielectric loss can be sharply reduced by more than an order of magnitude, from ~0.50 to ~0.037 (at 1 kHz) when the thin film was annealed in air at 650°C for 15 h under the help of an atmosphere-compensating-block (ACB) made from the proto-PSNMN gel. Moreover, the PSNMN thin film annealed with ACB also exhibited an extremely high thermally-stable dielectric tunability in an ultrabroad temperature range (>130 K), which could be attributed to the Maxwell-Wagner (MW) effect generated by the interface between the PSNMN disordered matrix and the B-site nanoscale-ordered structure formed during the long-term annealing process. The reduced dielectric loss is mainly benefited from the reduced concentration of oxygen vacancy and the possible MW effects, and the enhanced dielectric tunability could be ascribed to the weaker domain-pinning effect by oxygen vacancy. The breakthrough provides a new universal strategy to achieve utrahigh tunable performance in A(B'_1/2B"_1/2)O₃ ferroelectric thin films with a B-site nanoscale-ordered structure, meanwhile it paves the way for ultraintergrated tunable thin-film-devices with great phase shifter performance in practical applications.