Negative quasiparticle shifts in phosphorene quantum dots

It is commonly believed that electron correlations would open up a quasiparticle gap in semiconductors. Contrary to this intuitive expectation, here we reveal that phosphorene quantum dots (PQDs) may exhibit just the opposite effect. By using a configuration interaction approach beyond the conventional double-excitation scheme, quasiparticle energies are calculated for hexagonal and rectangular PQDs in various dielectric environments. For the hexagonal PQD with a nominal gap of 2.26 eV, it is found that the quasiparticle shift decreases by more than 500 meV and eventually becomes negative when the effective dielectric constant is reduced from 20.0 to 5.0. For other trapezoidal, triangular, and rectangular PQDs, the quasiparticle shift exhibits a similar amount of decrement after the same change in the dielectric environment. Furthermore, the calculation by adopting the Rytova-Keldysh potential, which may be more suitable to describe two-dimensional screening, also shows a very similar result, although with smaller decrement of the quasiparticle shift. The origin of this anomalous quasiparticle shift is believed to be related to the long-range electron-electron interactions in the distinctive lattice structure of PQDs, as a similar phenomenon has never been found in graphene quantum dots.