Single-Photon Emission from Organic Dye Molecules Adsorbed on a Quantum Dot via Energy Transfer

Yoshioka, Miyu; Yamauchi, Mitsuaki; Tamai, Naoto; Masuo, Sadahiro

doi:10.1021/acs.nanolett.3c03279

Cited by 1 publication

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References 54 publications

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“…PBI molecules can act as photoredox catalysts for reactions including C–H bromination, fluoroalkylation, or arylations. , Figure b displays ensemble PL spectra of CsPbBr 3 QDs in the presence of increasing concentrations of the PBI dye. The PL peak above 550 nm corresponds to the emission from the PBI dye , which is sensitized by the QD, as identified by the shortened donor lifetime in time-resolved PL measurements (Figure c). At the single-particle level, intensity time traces of the green donor and red acceptor emission show (anti)correlated behavior signaling the occurrence of ET (Figure d).…”

Section: Resultsmentioning

confidence: 99%

Quantifying Förster Resonance Energy Transfer from Single Perovskite Quantum Dots to Organic Dyes

Feld,

Boehme,

Morad

et al. 2024

ACS Nano

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Colloidal quantum dots (QDs) are promising regenerable photoredox catalysts offering broadly tunable redox potentials along with high absorption coefficients. QDs have thus far been examined for various organic transformations, water splitting, and CO 2 reduction. Vast opportunities emerge from coupling QDs with other homogeneous catalysts, such as transition metal complexes or organic dyes, into hybrid nanoassemblies exploiting energy transfer (ET), leveraging a large absorption cross-section of QDs and long-lived triplet states of cocatalysts. However, a thorough understanding and further engineering of the complex operational mechanisms of hybrid nanoassemblies require simultaneously controlling the surface chemistry of the QDs and probing dynamics at sufficient spatiotemporal resolution. Here, we probe the ET from single lead halide perovskite QDs, capped by alkylphospholipid ligands, to organic dye molecules employing single-particle photoluminescence spectroscopy with singlephoton resolution. We identify a Forster-type ET by spatial, temporal, and photon−photon correlations in the QD and dye emission. Discrete quenching steps in the acceptor emission reveal stochastic photobleaching events of individual organic dyes, allowing a precise quantification of the transfer efficiency, which is >70% for QD−dye complexes with strong donor− acceptor spectral overlap. Our work explores the processes occurring at the QD/molecule interface and demonstrates the feasibility of sensitizing organic photocatalysts with QDs.

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