Atypical dependence of excited exciton energy levels and electron-hole correlation on emission energy in pyramidal InP-based quantum dots

We calculate the spectrum of excited exciton states in application-relevant self-assembled pyramidal quantum dots grown in InAs/InP and InAs/AlGaInAs material systems. These types of dots have been recently shown to combine the emission in the third optical fiber window with low surface density and a reasonable level of in-plane symmetry of emitters, which predestines them for studies on single- and entangled-photon emission and for corresponding applications. The spectrum of optically active excited states is crucial for successful resonant and quasi-resonant excitation of emitters, allowing for conservation of angular momentum and addressing individual selected quantum states. Here, we show that in both types of studied dots, due to their specific morphology of truncated pyramid, the density of excited-state ladder, especially the s–p shell splitting may follow an unconventional dependence on emission energy, opposite to the one typically met in regular quantum dots. We obtain this result via modeling based on available morphological data and calculation within the multi-band [Formula: see text] envelope-function theory combined with the configuration-interaction method used to calculate exciton states. Then, we explain this observation in purely geometric terms, as a result of an increasing effective quantum confinement width in a pyramid that is progressively cut from the top. Additionally, we show that the inverted trend is also manifested in the amount of electron-hole correlation in the exciton ground state, which also shows an anomalous dependence on emission energy and quantum dot volume.