Ligand-stabilized CdSe nanoplatelet hybrid structures with tailored geometric and electronic properties. New insights from theory

Szemjonov, Alexandra; Pauporté, Thierry; Ithurria, Sandrine; Lequeux, Nicolas; Dubertret, Benoît; Ciofini, Ilaria; Labat, Frédèric

doi:10.1039/c4ra10082d

Cited by 19 publications

(42 citation statements)

References 59 publications

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“…3d), with 6 on each of the 6 {100} ZB facets [73, 74]. This bridging structure has been widely reported to be the preferred conformation of thiolates and carboxylates on cationic facets [22, 77, 78]. This is unlike DMF, which binds through its electron-donating tertiary amine as a σ-bond donor to a single CN=3 cadmium atom on {111} ZB cationic facets, which have lower charge density.…”

Section: Quantum Dot Ligand Coordinationmentioning

confidence: 99%

“…QDs absorb and emit light through transitions of electrons between energy levels that can shift when they mix with ligand orbitals [99], much like the effect of ligand field strength on electronic transitions of metal coordination complexes. However, changes in electronic absorption spectra due to ligand binding are usually not substantial (<50 meV shift) except in the case of in very small QDs (<2 nm) [100] and thin QD sheets (nanoplatelets) [77] for which a large fraction of atoms are on the surface. The impact is much lower for the more common larger QDs for which the energy levels of the transitioning electron primarily arise from the fully coordinated atoms within the crystal.…”

Section: Optical Properties Dictated By the Surfacementioning

confidence: 99%

“…This may be a viable approximation for large QDs where surface curvature may not need to be explicitly taken into account and for nanoplatelets with very large surfaces [28, 77]. It is important to note that many assumptions enter into these calculations that are not fully supported by robust evidence, especially the use of single ligand types, as a mixture of different types are usually bound.…”

Section: Modeling Of Quantum Dot Surfacesmentioning

confidence: 99%

“…Calculations of surface energies and binding energies can therefore vary widely. Nevertheless, DFT studies have been invaluable for understanding the facet-specificity of ligand binding [51, 157], the ordering of ligand binding energies [26, 154, 155, 158], and the optimum binding geometries of ligands to specific facets [54, 77]. …”

Section: Modeling Of Quantum Dot Surfacesmentioning

confidence: 99%

See 3 more Smart Citations

Quantum dot surface engineering: Toward inert fluorophores with compact size and bright, stable emission

Lim

Schleife

et al. 2016

Coordination Chemistry Reviews

109

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The surfaces of colloidal nanocrystals are complex interfaces between solid crystals, coordinating ligands, and liquid solutions. For fluorescent quantum dots, the properties of the surface vastly influence the efficiency of light emission, stability, and physical interactions, and thus determine their sensitivity and specificity when they are used to detect and image biological molecules. But after more than 30 years of study, the surfaces of quantum dots remain poorly understood and continue to be an important subject of both experimental and theoretical research. In this article, we review the physics and chemistry of quantum dot surfaces and describe approaches to engineer optimal fluorescent probes for applications in biomolecular imaging and sensing. We describe the structure and electronic properties of crystalline facets, the chemistry of ligand coordination, and the impact of ligands on optical properties. We further describe recent advances in compact coatings that have significantly improved their properties by providing small hydrodynamic size, high stability and fluorescence efficiency, and minimal nonspecific interactions with cells and biological molecules. While major progress has been made in both basic and applied research, many questions remain in the chemistry and physics of quantum dot surfaces that have hindered key breakthroughs to fully optimize their properties.

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Section: Quantum Dot Ligand Coordinationmentioning

confidence: 99%

Section: Optical Properties Dictated By the Surfacementioning

confidence: 99%

Section: Modeling Of Quantum Dot Surfacesmentioning

confidence: 99%

Section: Modeling Of Quantum Dot Surfacesmentioning

confidence: 99%

See 2 more Smart Citations

Quantum dot surface engineering: Toward inert fluorophores with compact size and bright, stable emission

Lim

Schleife

et al. 2016

Coordination Chemistry Reviews

109

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“…During synthesis, both the surface orientation and the thickness of CdSe NPLs are precisely controlled . In consequence and due to the quantum confinement effects, their excitonic and charge carrier properties can be easily tuned . Therefore, they provide an excellent basis for studying how the quantum confinement in the sensitizers affect the performance of QDSCs.…”

Section: Introductionmentioning

confidence: 99%

Ex situ and in situ sensitized quantum dot solar cells

Szemjonov

Ithurria

Dubertret

et al. 2016

Physica Status Solidi (b)

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Although quantum dot‐sensitized solar cells (QDSCs) prepared with in situ sensitized wide‐band gap semiconductor nanorods are commonly reported, very few examples of the ex situ sensitization of these nanorods are known. They usually result in poor solar cell performance parameters. In this work, we have tested the photovoltaic application of both ex situ and in situ sensitized ZnO nanorods by linker‐assisted attachment and by the successive ionic layer adsorption and reaction (SILAR) technique, respectively. For the ex situ sensitization, instead of classical spherical QDs, we used quasi two‐dimensional CdSe nanoplatelets (NPLs) of controlled thicknesses, the photovoltaic application of which has never been reported before. Regarding the in situ sensitization, the photoanodes were characterized by XRD, UV–VIS absorption, and Raman spectroscopy during deposition, which helped to better understand the formation of CdSe QDs nanostructured ZnO surface. Devices incorporating in situ sensitized ZnO nanorods demonstrated superior performance compared to the best measured efficiencies of QDSCs prepared with ex situ sensitization, and their J–V characteristics were more reproducible.

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Manipulation of the Optical Properties of Colloidal 2D CdSe Nanoplatelets

Zhang

Sun

2021

Advanced Photonics Research

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Driven by the unique optoelectronic features arising from the strong quantum confinement along the thickness direction, rapid development of CdSe‐based nanoplatelets (NPL) has accomplished facile bandgap tunability over a broad spectrum via different preparation protocols or various postsynthesis treatments. The anisotropic geometry of NPLs also stimulates the exploitation of self‐assembled CdSe NPL superstructures to enhance light extraction efficiency in display technologies and achieves polarized lasing performance or even electrically pumped laser by adjusting the transition dipole orientation. Although several review articles about the general optical properties of CdSe NPLs have been published, none of them focus on the ability of spectral tunability and precise control of orientations in the solid‐state phase of CdSe NPLs. Herein, the band structure engineering approaches in the CdSe NPL family are systematically summarized and the optical properties and device performance metrics of these deliberately engineered NPLs are compared. Then, the recent advanced studies of the motivation and assembly methods of geometrically anisotropic CdSe NPL superlattices are discussed. Finally, the current challenges and future outlook on the controlled modification of optical features and the influences of the approaches in the aspect of CdSe NPL–based devices’ performance are highlighted.

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Ligand-stabilized CdSe nanoplatelet hybrid structures with tailored geometric and electronic properties. New insights from theory

Abstract: A theoretical protocol for the investigation of the properties of CdSe zinc blende nanoplatelets with different thicknesses in the (100) direction and stabilized by various ligands is proposed and validated with respect to experimental data.

Cited by 19 publications

References 59 publications

Quantum dot surface engineering: Toward inert fluorophores with compact size and bright, stable emission

Quantum dot surface engineering: Toward inert fluorophores with compact size and bright, stable emission

Ex situ and in situ sensitized quantum dot solar cells

Manipulation of the Optical Properties of Colloidal 2D CdSe Nanoplatelets

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