Charge-Transfer-Driven Phase Transition of Two-Dimensional MoTe2 in Donor-Acceptor Heterostructures

In this work, based on first-principles calculations, we propose that electrene can be considered as an electrondonating substrate to drive the phase transition of MoTe2 from the H to T' phase, which is a topic of long-standing interest and importance. In particular, new electrenes Ca2XN2 (X = Zr, Hf) are predicted with the existence of a nearly free two-dimensional (2D) electron gas and ultralow work functions. In MoTe2/Ca2XN2. donor-acceptor heterostructures, we find significantly large charge transfer (similar to 0.4e per MoTe2 unit cell) from Ca2XN2 to MoTe2, which stabilizes the T' phase and decreases the phase transition barrier (from similar to 0.9 to similar to 0.5 eV per unit cell). In addition, the phase transition of MoTe2 on Ca2XN2 remains effective as the interlayer distance varies. It therefore can be confirmed conclusively that our results open a new avenue for phase transition study and provide new insights for the large-scale synthesis of metastable high-quality T'-phase MoTe2.