Electron Delocalization versus Emission Coherence of Quantum Dot Superlattices

Abstract

Cooperative emission is a collective quantum optical process that requires macroscopic phase coherence among coupled emitters. Recent observations of cooperative emission in QD superlattices have renewed interest in how such coherence emerges in nanostructured solids. Meanwhile, theoretical studies have long discussed the relationship between electronic delocalization and coherence, particularly whether delocalized states necessarily give rise to cooperative emission. This study addresses this question through power-dependent steady-state PL and time-resolved PL decay measurements. The findings indicate that, although the quantum resonance peak exhibits delocalized excitonic characteristics, it shows no signatures of cooperative radiation. In particular, neither superlinear intensity scaling nor power-dependent emission delay was observed, indicating the absence of cooperative-radiation signatures. This can be understood from two disorder-related aspects. Temperature-dependent spectroscopy reveals pronounced inhomogeneous broadening and low-temperature dark-exciton participation, pointing to intra-domain static disorder and exciton-state mixing. These effects collectively hinder the establishment of macroscopic coherence. The temperature dependence of the quantum resonance peak decay lifetime is consistent with two-dimensional exciton dynamics. This work provides direct experimental evidence that electronic delocalization can be decoupled from cooperative coherence in CdSe quantum dot superlattices.