“…[1][2][3] The interaction between lattice, charge, spin, and orbital degrees of freedom is found to play a direct and crucial role in the performance of electronic materials, displaying a rich spectrum of exotic phenomena. [4][5][6] The electric field effect with advantages of low power consumption and high controllability offers an effective and reversible route to confine the lattice, charge, and spin (as illustrated in Figure 1): (a) the piezoelectric effect in crystalline materials without inversion symmetry has bridged electric field and lattice for more than 130 years; [7] (b) the field-effect transistor (FET) provided a classic model for the manipulation of carrier density by electrical means, constituting the cornerstone of the semiconductor industry; [8] (c) the magnetization switching is driven reversibly by applied electric fields, which is expected to have a great technological impact on information storage. [9,10] However, electrical control of the missing member-orbital degree of freedom, whose small perturbations would lead to giant responses in the electric and magnetic properties, [11,12] has thus far remained an interesting concept lacking experimental insight.…”