Electrical manipulation of lattice, charge, and spin has been realized respectively by the piezoelectric effect, field-effect transistor, and electric field control of ferromagnetism, bringing about dramatic promotions both in fundamental research and industrial production. However, it is generally accepted that the orbital of materials are impossible to be altered once they have been made. Here we use electric-field to dynamically tune the electronic phase transition in (La,Sr)MnO3 films with different Mn^4+/(Mn^3+ + Mn^4+) ratios. The orbital occupancy and corresponding magnetic anisotropy of these thin films are manipulated by gate voltage in a reversible and quantitative manner. Positive gate voltage increases the proportion of occupancy of the orbital and magnetic anisotropy that were initially favored by strain (irrespective of tensile and compressive), while negative gate voltage reduces the concomitant preferential orbital occupancy and magnetic anisotropy. Besides its fundamental significance in orbital physics, our findings might advance the process towards practical oxide-electronics based on orbital.
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