Super-resolution photoluminescence lifetime and intensity mapping of interacting CdSe/CdS quantum dots

Journal Article · 13 January 2020 · Applied Physics Letters

DOI: https://doi.org/10.1063/1.5132563 · OSTI ID:1630862

Dunlap, Megan K.  ^[1]; Ryan, Duncan P.  ^[2]; Goodwin, Peter M.  ^[2]; Werner, James H.  ^[2]; Majumder, Somak  ^[2]; Hollingsworth, Jennifer A.  ^[2]; Gelfand, Martin P.  ^[1]; Van Orden, Alan  ^[1]

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1. Colorado State Univ., Fort Collins, CO (United States)
2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

We report an optical imaging method that simultaneously achieves nanometer-scale spatial resolution and records single-photon arrival times with subnanosecond temporal resolution, allowing for visualization of nanoscale photoluminescence dynamics. The technique combines time-correlated single-photon counting with single-molecule localization microscopy by monitoring the emission centroid location with a 2 × 2 array of optical fibers that are coupled to four single-photon counting detectors. We applied this method to image isolated and clustered CdSe/CdS core/shell quantum dots (QDs). Single QDs were localized with ~5 nm precision using 10⁴ detected photons. We note within clusters, emission centroids separated by ~12 nm were resolved, and spatial mapping of both the emission intensity and lifetime provided evidence of energy transport pathways among the QDs.

• Research Organization: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
• Sponsoring Organization: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC); Gary E. Maciel Fellowship Foundation
• Grant/Contract Number: 89233218CNA000001
• OSTI ID: 1630862
• Alternate ID(s): OSTI ID: 1582485
• Report Number(s): LA-UR-19-30441; TRN: US2200702
• Journal Information: Applied Physics Letters, Vol. 116, Issue 2; ISSN 0003-6951
• Publisher: American Institute of Physics (AIP)Copyright Statement
• Country of Publication: United States
• Language: English