Bandedge-state-limited single-photon emission from volumetric quantum design of 2D colloidal quantum wells

Abstract

Present-day solution-processable single-photon sources are dominated by three-dimensionally confined colloidal quantum dot emitters, yet their particle-to-particle variation in single-exciton properties limits reproducibility and scalability. Here, to avoid such heterogeneity, we demonstrate reliable room-temperature single-photon emission from atomically flat two-dimensional (2D) colloidal quantum wells (CQWs) with inherently uniform one-dimensional quantum confinement, despite their long-standing limitations of efficient multiexciton emission and pronounced exciton-surface susceptibility. We resolve these challenges through volumetric quantum design (VQD) of CQWs, yielding a highly localized, single bandedge state. This design laterally confines the bandedge excitonic domain within the exciton coherent area and vertically decouples it from surface states via a thick, strain-relieved quantum-barrier shell that preserves strong confinement, overcoming the daunting thickness-confinement trade-off in 2D CQWs. Statistical single-particle spectroscopy reveals that VQD-CQWs deliver near-blinking-free (on-time >99.5%) and fluence-insensitive antibunching (g(2)(0): 0.041), protected by a bandedge-state-filling bottleneck, together with linear polarization of up to 73% under cavity-free conditions, originating from synergistic transition-dipole and electric-field anisotropies. These advances establish 2D CQWs as a viable, homogenous and scalable platform for quantum technologies.