Dataset Information

Heralded Spectroscopy Reveals Exciton-Exciton Correlations in Single Colloidal Quantum Dots.

ABSTRACT: Multiply excited states in semiconductor quantum dots feature intriguing physics and play a crucial role in nanocrystal-based technologies. While photoluminescence provides a natural probe to investigate these states, room-temperature single-particle spectroscopy of their emission has proved elusive due to the temporal and spectral overlap with emission from the singly excited and charged states. Here, we introduce biexciton heralded spectroscopy enabled by a single-photon avalanche diode array based spectrometer. This allows us to directly observe biexciton-exciton emission cascades and measure the biexciton binding energy of single quantum dots at room temperature, even though it is well below the scale of thermal broadening and spectral diffusion. Furthermore, we uncover correlations hitherto masked in ensembles of the biexciton binding energy with both charge-carrier confinement and fluctuations of the local electrostatic potential. Heralded spectroscopy has the potential of greatly extending our understanding of charge-carrier dynamics in multielectron systems and of parallelization of quantum optics protocols.

SUBMITTER: Lubin G

PROVIDER: S-EPMC8397400 | biostudies-literature | 2021 Aug

REPOSITORIES: biostudies-literature

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Heralded Spectroscopy Reveals Exciton-Exciton Correlations in Single Colloidal Quantum Dots.

Lubin Gur G Tenne Ron R Ulku Arin Can AC Antolovic Ivan Michel IM Burri Samuel S Karg Sean S Yallapragada Venkata Jayasurya VJ Bruschini Claudio C Charbon Edoardo E Oron Dan D

Nano letters 20210816 16

Multiply excited states in semiconductor quantum dots feature intriguing physics and play a crucial role in nanocrystal-based technologies. While photoluminescence provides a natural probe to investigate these states, room-temperature single-particle spectroscopy of their emission has proved elusive due to the temporal and spectral overlap with emission from the singly excited and charged states. Here, we introduce biexciton heralded spectroscopy enabled by a single-photon avalanche diode array ...[more]

PMID: 34398604

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Project description:Pairs of coupled quantum dots with controlled coupling between the two potential wells serve as an extremely rich system, exhibiting a plethora of optical phenomena that do not exist in each of the isolated constituent dots. Over the past decade, coupled quantum systems have been under extensive study in the context of epitaxially grown quantum dots (QDs), but only a handful of examples have been reported with colloidal QDs. This is mostly due to the difficulties in controllably growing nanoparticles that encapsulate within them two dots separated by an energetic barrier via colloidal synthesis methods. Recent advances in colloidal synthesis methods have enabled the first clear demonstrations of colloidal double quantum dots and allowed for the first exploratory studies into their optical properties. Nevertheless, colloidal double QDs can offer an extended level of structural manipulation that allows not only for a broader range of materials to be used as compared with epitaxially grown counterparts but also for more complex control over the coupling mechanisms and coupling strength between two spatially separated quantum dots. The photophysics of these nanostructures is governed by the balance between two coupling mechanisms. The first is via dipole-dipole interactions between the two constituent components, leading to energy transfer between them. The second is associated with overlap of excited carrier wave functions, leading to charge transfer and multicarrier interactions between the two components. The magnitude of the coupling between the two subcomponents is determined by the detailed potential landscape within the nanocrystals (NCs). One of the hallmarks of double QDs is the observation of dual-color emission from a single nanoparticle, which allows for detailed spectroscopy of their properties down to the single particle level. Furthermore, rational design of the two coupled subsystems enables one to tune the emission statistics from single photon emission to classical emission. Dual emission also provides these NCs with more advanced functionalities than the isolated components. The ability to better tailor the emission spectrum can be advantageous for color designed LEDs in lighting and display applications. The different response of the two emission colors to external stimuli enables ratiometric sensing. Control over hot carrier dynamics within such structures allows for photoluminescence upconversion. This Account first provides a description of the main hurdles toward the synthesis of colloidal double QDs and an overview of the growing library of synthetic pathways toward constructing them. The main discoveries regarding their photophysical properties are then described in detail, followed by an overview of potential applications taking advantage of the double-dot structure. Finally, a perspective and outlook for their future development is provided.

Dataset Information

Heralded Spectroscopy Reveals Exciton-Exciton Correlations in Single Colloidal Quantum Dots.

Publications

Heralded Spectroscopy Reveals Exciton-Exciton Correlations in Single Colloidal Quantum Dots.

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