The broken mirror symmetry of two-dimensional (2D) Janus materials brings novel quantum properties and various application prospects. Particularly, when stacking into heterostructures, their intrinsic dipole moments and large band offsets… Click to show full abstract
The broken mirror symmetry of two-dimensional (2D) Janus materials brings novel quantum properties and various application prospects. Particularly, when stacking into heterostructures, their intrinsic dipole moments and large band offsets are very favorable to the photoexcited properties concerning electron-hole pairs, i.e., excitons. However, the effect of the intrinsic dipole moments on the interlayer excitons in the heterostructures composed of 2D Janus materials is still unclear. Here we use the GW/BSE methods to explore the effect of the intrinsic dipole moments on the interlayer excitons via varying the stacking configuration of MoSSe/WSSe heterostructures. Surprisingly, our results reveal that the parallel-arranged intrinsic dipole moments enhance the interlayer coupling in the heterostructures, and hence make the lowest interlayer exciton have an intensity comparable to the bright excitons while accompanied by a large binding energy and a radiative lifetime as long as 10-7 s at 300 K, though it is almost a spin-forbidden process, and with the out-of-plane light polarization, long lifetime interlayer excitons are observed under the effect of selection rules. More intriguingly, we found that the photoexcited properties of the interlayer excitons considering the momentum in the stacking configuration with parallel-arranged intrinsic dipole moments are greatly tunable through hydrostatic pressure. These explorations provide a basic perspective for optoelectronic applications by means of engineering the intrinsic dipole moments in Janus heterostructures.
               
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