Quantitative Excited State Spectroscopy of a Single InGaAs Quantum Dot Molecule through Multi-million Atom Electronic Structure Calculations

Atomistic electronic structure calculations are performed to study the coherent inter-dot couplings of the electronic states in a single InGaAs quantum dot molecule. The experimentally observed excitonic spectrum [12] is quantitatively reproduced, and the correct energy states are identified based on a previously validated atomistic tight binding model. The extended devices are represented explicitly in space with 15 million atom structures. An excited state spectroscopy technique is presented in which the externally applied electric field is swept to probe the ladder of the electronic energy levels (electron or hole) of one quantum dot through anti-crossings with the energy levels of the other quantum dot in a two quantum dot molecule. This technique can be applied to estimate the spatial electron-hole spacing inside the quantum dot molecule as well as to reverse engineer quantum dot geometry parameters such as the quantum dot separation. Crystal deformation induced piezoelectric effects have been discussed in the literature as minor perturbations lifting degeneracies of the electron excited (P and D) states, thus affecting polarization alignment of wave function lobes for III-V Heterostructures such as single InAs/GaAs quantum dots. In contrast this work demonstrates the crucial importance of piezoelectricity to resolve the symmetries and energies of the excited states through matching the experimentally measured spectrum in an InGaAs quantum dot molecule under the influence of an electric field. Both linear and quadratic piezoelectric effects are studied for the first time for a quantum dot molecule and demonstrated to be indeed important. The net piezoelectric contribution is found to be critical in determining the correct energy spectrum, which is in contrast to recent studies reporting vanishing net piezoelectric contributions.

💡 Research Summary

This paper presents a comprehensive atomistic study of the excited‑state spectrum of a single InGaAs quantum‑dot molecule (QDM) using multi‑million‑atom electronic‑structure calculations. The authors construct a realistic three‑dimensional model containing approximately 15 million atoms that explicitly represents the two InGaAs quantum dots, the surrounding GaAs matrix, alloy composition fluctuations, and the exact geometric parameters (height, base diameter, and inter‑dot separation) reported in the experimental work they reference (Ref.