Large shift current via in-gap and charge-neutral exciton excitations in BN nanotubes and single BN layer (2305.12439v1)

Abstract: We perform {\it ab initio} many-body calculations to investigate the exciton shift current in small diameter zigzag BN nanotubes and also single BN sheet, using the GW plus Bethe-Salpeter equation (GW-BSE) method with the newly developed efficient algorithms. Our GW-BSE calculations reveal a giant in-gap peak in the shift current spectrum in all the studied BN systems due to the excitation of the A exciton. The peak value of the excitonic shift current is more than three times larger than that of the quasiparticle shift current, and is attributed to the gigantic enhancement of the optical dipole matrix element by the A exciton resonance. The effective exciton shift current conductivity is nearly ten times larger than the largest shift conductivity observed in ferroelectric semiconductors. Importantly, the direction of the shift current in the BN nanotubes is found to be independent of the tube chirality ($n,0$) (or diameter), contrary to the simple rule of $ sgn(J_\text{shift})=\text{mod}(n,3)$ predicted by previous model Hamiltonian studies. Finally, our {\it ab initio} calculations also show that the exciton excitation energies decrease significantly with the decreasing diameter due to the curvature-induced orbital rehybridization in small diameter zigzag BN nanotubes.