Tailoring Interfacial Charge Transfer for Optimizing Thermoelectric Performances of MnTe‐Sb 2 Te 3 Superlattice‐Like Films

Interfacial charge transfer has a vital role in tailoring the thermoelectric performance of superlattices (SLs), which, however, is rarely clarified by experiments. Herein, based on epitaxially grown p‐type (MnTe) x (Sb 2 Te 3 ) y superlattice‐like films, synergistically optimized thermoelectric parameters of carrier density, carrier mobility, and Seebeck coefficient are achieved by introducing interfacial charge transfer, in which effects of hole injection, modulation doping, and energy filtering are involved. Carrier transport measurements and angle‐resolved photoemission spectroscopy (ARPES) characterizations reveal a strong hole injection from the MnTe layer to the Sb 2 Te 3 layer in the SLs, originating from the work function difference between MnTe and Sb 2 Te 3 . By reducing the thickness of MnTe less than one monolayer, all electronic transport parameters are synergistically optimized in the quantum‐dots (MnTe) x (Sb 2 Te 3 ) 12 superlattice‐like films, leading to much improved thermoelectric power factors ( PF s). The (MnTe) 0.1 (Sb 2 Te 3 ) 12 obtains the highest room‐temperature PF of 2.50 mWm −1 K −2 , while the (MnTe) 0.25 (Sb 2 Te 3 ) 12 possesses the highest PF of 2.79 mWm −1 K −2 at 381 K, remarkably superior to the values acquired in binary MnTe and Sb 2 Te 3 films. This research provides valuable guidance on understanding and rationally tailoring the interfacial charge transfer of thermoelectric SLs to further enhance thermoelectric performances.