Culling a Self-Assembled Quantum Dot as a Single-Photon Source Using X-ray Microscopy

ACS Nano. 2023 Aug 22;17(16):16080-16088. doi: 10.1021/acsnano.3c04835. Epub 2023 Jul 31.

Abstract

Epitaxially grown self-assembled semiconductor quantum dots (QDs) with atom-like optical properties have emerged as the best choice for single-photon sources required for the development of quantum technology and quantum networks. Nondestructive selection of a single QD having desired structural, compositional, and optical characteristics is essential to obtain noise-free, fully indistinguishable single or entangled photons from single-photon emitters. Here, we show that the structural orientations and local compositional inhomogeneities within a single QD and the surrounding wet layer can be probed in a screening fashion by scanning X-ray diffraction microscopy and X-ray fluorescence with a few tens of nanometers-sized synchrotron radiation beam. The presented measurement protocol can be used to cull the best single QD from the enormous number of self-assembled dots grown simultaneously. The obtained results show that the elemental composition and resultant strain profiles of a QD are sensitive to in-plane crystallographic directions. We also observe that lattice expansion after a certain composition-limit introduces shear strain within a QD, enabling the possibility of controlled chiral-QD formation. Nanoscale chirality and compositional anisotropy, contradictory to common assumptions, need to be incorporated into existing theoretical models to predict the optical properties of single-photon sources and to further tune the epitaxial growth process of self-assembled quantum structures.

Keywords: X-ray fluorescence (XRF); compositional inhomogeneities; epitaxially grown quantum dots; nanoscale chirality; scanning X-ray diffraction microscopy (SXDM); single quantum dot; single-photon sources.