2021
DOI: 10.1021/acs.nanolett.1c02540
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Tuning the Dimensionality of Excitons in Colloidal Quantum Dot Molecules

Abstract: Electrically coupled quantum dots (QDs) can support unique optoelectronic properties arising from the superposition of single-particle excited states. Experimental methods for integrating colloidal QDs within the same nano-object, however, have remained elusive to the rational design. Here, we demonstrate a chemical strategy that allows for the assembling of colloidal QDs into coupled composites, where proximal interactions give rise to unique optoelectronic behavior. The assembly method employing “adhesive” s… Show more

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Cited by 9 publications
(9 citation statements)
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“…One-dimensional assemblies of CdSe NCs achieved in OLAM/Se reaction mixture (Figure a) represent an interesting type of semiconductor quantum dots (QDs), where the fine structure of lowest-energy excitons differs from that of zero-dimensional QDs. As illustrated in Figure d, eight lowest-energy transitions in CdSe NCs shift lower in energy and reorder when several dots are fused into a 1D assembly of the same diameter . In spherical CdSe NCs, the upper F = ±1 bright states ( F = S + J is the total angular momentum) carry most of the dipole strength for optical absorption, while the lower F = ±1 bright states are responsible for the room-temperature emission.…”
Section: Resultsmentioning
confidence: 99%
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“…One-dimensional assemblies of CdSe NCs achieved in OLAM/Se reaction mixture (Figure a) represent an interesting type of semiconductor quantum dots (QDs), where the fine structure of lowest-energy excitons differs from that of zero-dimensional QDs. As illustrated in Figure d, eight lowest-energy transitions in CdSe NCs shift lower in energy and reorder when several dots are fused into a 1D assembly of the same diameter . In spherical CdSe NCs, the upper F = ±1 bright states ( F = S + J is the total angular momentum) carry most of the dipole strength for optical absorption, while the lower F = ±1 bright states are responsible for the room-temperature emission.…”
Section: Resultsmentioning
confidence: 99%
“…F is the total angular momentum of an excitonic state (b = bright, d = dark). Adapted from ref . Copyright 2021 American Chemical Society.…”
Section: Resultsmentioning
confidence: 99%
“…In the case of colloidal semiconductor NCs, the simplest two-qubit exciton system could be realized by using a pair of coupled nanoparticles (Figure ). Such a hetero-dimer can be assembled via colloidal routes , and is characterized by four possible states corresponding to an exciton being present (1) or absent (0) on each dot (Figure a). Using this nomenclature, we can define the four states of a nanocrystal hetero-dimer as |00⟩, |10⟩, |01⟩, and |11⟩, with the first digit referring to dot 1 and the second to dot 2 …”
Section: Resultsmentioning
confidence: 99%
“…4,5 Many fabrication strategies have been proposed to couple different types of quantum dots, not only PQDs. [6][7][8][9][10][11] Assembling quantum dots and studying their quantum coupling in solution would greatly simplify such studies. Furthermore, by assembling in solution, it is possible to study the individual dots prior to assembly, and then study the impact of coupling in the near-field, which is not possible with pre-assembled pairs.…”
Section: Introductionmentioning
confidence: 99%
“…Perovskite quantum dots (PQDs) show intriguing properties for quantum technologies, such as bright and highly coherent single-photon emission , and superfluorescence in ensembles of dots . Coupled quantum dots have long been investigated for quantum computing. , Many fabrication strategies have been proposed to couple different types of quantum dots, not only PQDs. Assembling quantum dots and studying their quantum coupling in solution would greatly simplify such studies. Furthermore, by assembling in solution, it is possible to study the individual dots prior to assembly and then study the impact of coupling in the near-field, which is not possible with preassembled pairs.…”
mentioning
confidence: 99%