Electrohydrodynamic Printing‐Based Heterointegration of Quantum Dots on Suspended Nanophotonic Cavities

Guymon, Gregory G.; Sharp, David; Cohen, Theodore A.; Gibbs, Stephen L.; Manna, Arnab; Tzanetopoulos, Eden; Gamelin, Daniel R.; Majumdar, Arka; MacKenzie, J. Devin

doi:10.1002/admt.202301921

Cited by 3 publications

(3 citation statements)

References 60 publications

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“…Due to their remarkable size and high stability under electron beams and excitation, these colossal core/shell QDs are poised to be highly effective for the deterministic positioning of single-photon emitters using solution-processable techniques such as template-assisted self-assembly 17 and electrohydrodynamic inkjet printing. 63,64 Additionally, our findings regarding particle morphologies and properties throughout the shelling process at this large particle size regime provide valuable insights into precision crystal growth and size-dependent optical properties.…”

Section: Discussionmentioning

confidence: 91%

Colossal Core/Shell CdSe/CdS Quantum Dot Emitters

Nguyen,

Hammel,

Sharp

et al. 2024

Preprint

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Single-photon sources are essential for advancing quantum technologies, with scalable integration being a crucial requirement. To date, deterministic positioning of single-photon sources in large-scale photonic structures remains a challenge. In this context, colloidal quantum dots (QDs), particularly core/shell configurations, are attractive due to their solution processability. However, traditional QDs are typically small, about 3 to 6 nm, which restricts their deterministic placement and utility in large-scale photonic devices. The largest existing core/shell QDs are the family of giant CdSe/CdS QDs, with total diameters ranging from about 20 to 50 nm. Pushing beyond this size limit, we introduce a synthesis strategy for colossal CdSe/CdS QDs, with sizes ranging from 30 to 100 nm, using a stepwise high-temperature continuous injection method. Electron microscopy reveals a consistent hexagonal diamond morphology composed of twelve semipolar {101 ̅1} facets and one polar (0001) facet. We also identify conditions where shell growth is disrupted, leading to defects, islands, and mechanical instability, which suggest synthetic requirements for growing crystalline particles beyond 100 nm. The stepwise growth of thick CdS shells on CdSe cores enables the synthesis of emissive QDs with long photoluminescence lifetimes of a few microseconds and suppressed blinking at room temperature. Notably, QDs with 100 CdS monolayers exhibit high single-photon emission purity with second-order photon correlation g(2)(0) values below 0.2. Our findings indicate that colossal core/shell QDs can efficiently emit single photons, which paves the way for quantum photonic applications that require deterministic placement of single-photon sources.

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Section: Discussionmentioning

confidence: 91%

Colossal Core/Shell CdSe/CdS Quantum Dot Emitters

Nguyen,

Hammel,

Sharp

et al. 2024

Preprint

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“…Compared to the previously reported giant CdSe/CdS QDs (Table ), colossal QDs are poised to be highly effective for scalable and deterministic single-particle positioning and ultimately precise coupling with optical cavities using solution-processable techniques, including template-assisted self-assembly, electrohydrodynamic inkjet printing, , and those that have been used for other particles with sub-100 nm diameters …”

Section: Results and Discussionmentioning

confidence: 97%

Colossal Core/Shell CdSe/CdS Quantum Dot Emitters

Nguyen,

Hammel,

Sharp

et al. 2024

ACS Nano

Self Cite

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Single-photon sources are essential for advancing quantum technologies with scalable integration being a crucial requirement. To date, deterministic positioning of singlephoton sources in large-scale photonic structures remains a challenge. In this context, colloidal quantum dots (QDs), particularly core/shell configurations, are attractive due to their solution processability. However, traditional QDs are typically small, about 3 to 6 nm, which restricts their deterministic placement and utility in large-scale photonic devices, particularly within optical cavities. The largest existing core/shell QDs are a family of giant CdSe/CdS QDs, with total diameters ranging from about 20 to 50 nm. Pushing beyond this size limit, we introduce a synthesis strategy for colossal CdSe/CdS QDs, with sizes ranging from 30 to 100 nm, using a stepwise high-temperature continuous injection method. Electron microscopy reveals a consistent hexagonal diamond morphology composed of 12 semipolar {101̅ 1} facets and one polar (0001) facet. We also identify conditions where shell growth is disrupted, leading to defects, islands, and mechanical instability, which suggest synthetic requirements for growing crystalline particles beyond 100 nm. The stepwise growth of thick CdS shells on CdSe cores enables the synthesis of emissive QDs with long photoluminescence lifetimes of a few microseconds and suppressed blinking at room temperature. Notably, QDs with 80 and 100 CdS monolayers exhibit high single-photon emission purity with second-order photon correlation g (2) (0) values below 0.2.

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“…Upon evaporation of the solvent, particles or molecules coagulate to form nanostructures. This method allows for precise subwavelength placement of the nano-object and is applicable to a wide range of materials, including gold nanoparticles, , quantum dots, , and organic molecules . In this work, we explore the spectral behavior of DBT molecules in printed Ac crystals at cryogenic temperatures.…”

Section: Resultsmentioning

confidence: 99%

High-Resolution Cryogenic Spectroscopy of Single Molecules in Nanoprinted Crystals

Musavinezhad,

Renger,

Zirkelbach

et al. 2024

ACS Nano

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We perform laser spectroscopy at liquid helium temperatures (T = 2 K) to investigate single dibenzoterrylene (DBT) molecules doped in anthracene crystals of nanoscopic height fabricated by electrohydrodynamic dripping. Using highresolution fluorescence excitation spectroscopy, we show that zero-phonon lines of single molecules in printed nanocrystals are nearly as narrow as the Fourier-limited transitions observed for the same guest−host system in the bulk. Moreover, the spectral instabilities are comparable to or less than one line width. By recording super-resolution images of DBT molecules and varying the polarization of the excitation beam, we determine the dimensions of the printed crystals and the orientation of the crystals' axes. Electrohydrodynamic printing of organic nano-and microcrystals is of interest for a series of applications, where controlled positioning of quantum emitters with narrow optical transitions is desirable.

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Electrohydrodynamic Printing‐Based Heterointegration of Quantum Dots on Suspended Nanophotonic Cavities

Cited by 3 publications

References 60 publications

Colossal Core/Shell CdSe/CdS Quantum Dot Emitters

Colossal Core/Shell CdSe/CdS Quantum Dot Emitters

Colossal Core/Shell CdSe/CdS Quantum Dot Emitters

High-Resolution Cryogenic Spectroscopy of Single Molecules in Nanoprinted Crystals

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