Ultrathin One- and Two-Dimensional Colloidal Semiconductor Nanocrystals: Pushing Quantum Confinement to the Limit

Berends, Anne C.; Donegá, Celso de Mello

doi:10.1021/acs.jpclett.7b01640

Cited by 66 publications

(87 citation statements)

References 89 publications

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“…Nanoparticle self-assembly is an emerging route with tremendous potential to build novel nanostructured materials [1,2]. In the past two decades, increasing interest has been devoted toward the formation of 3D [3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20] and 2D [21][22][23][24][25][26][27][28][29][30][31][32] nanogeometric materials for optoelectronic applications [33][34][35][36][37][38][39][40][41][42][43][44][45][46][47]. These nanomaterials are formed by the self-assembly of semiconductor nanocrystals (NCs) with the size of a few nanometers, and often with a roughly spherical shape, into various types of superstructures.…”

Section: Introductionmentioning

confidence: 99%

Understanding the Formation of PbSe Honeycomb Superstructures by Dynamics Simulations

Soligno

Vanmaekelbergh

2019

Phys. Rev. X

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Using a coarse-grained molecular dynamics model, we simulate the self-assembly of PbSe nanocrystals (NCs) adsorbed at a flat fluid-fluid interface. The model includes all key forces involved: NC-NC shortrange facet-specific attractive and repulsive interactions, entropic effects, and forces due to the NC adsorption at fluid-fluid interfaces. Realistic values are used for the input parameters regulating the various forces. The interface-adsorption parameters are estimated using a recently introduced sharpinterface numerical method which includes capillary deformation effects. We find that the final structure in which the NCs self-assemble is drastically affected by the input values of the parameters of our coarsegrained model. In particular, by slightly tuning just a few parameters of the model, we can induce NC selfassembly into either silicene-honeycomb superstructures, where all NCs have a f111g facet parallel to the fluid-fluid interface plane, or square superstructures, where all NCs have a f100g facet parallel to the interface plane. Both of these nanostructures have been observed experimentally. However, it is still not clear their formation mechanism, and, in particular, which are the factors directing the NC self-assembly into one or another structure. In this work, we identify and quantify such factors, showing illustrative assembled-phase diagrams obtained from our simulations. In addition, with our model, we can study the self-assembly dynamics, simulating how the NCs' structures evolve from few-NCs aggregates to gradually larger domains. For example, we observe linear chains, where all NCs have a f110g facet parallel to the interface plane as typical precursors of the square superstructure, and zigzag aggregates, where all NCs have a f111g facet parallel to the interface plane as typical precursors of the silicene-honeycomb superstructure. Both of these aggregates have also been observed experimentally. Finally, we show indications that our method can be applied to study defects of the obtained superstructures.

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Section: Introductionmentioning

confidence: 99%

Understanding the Formation of PbSe Honeycomb Superstructures by Dynamics Simulations

Soligno

Vanmaekelbergh

2019

Phys. Rev. X

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“…Since the report by Kovalenko's group in 2015, 1 ILHPs nanocrystals have attracted much attention because of not only their excellent optical performances, that is, bright and adjustable photoluminescence (PL) controlled by halide anions or particle size, but also because of their cost-effective fabrication approaches such as the high-regulation hot injection synthesis, the facile room-temperature synthesis, and the fast anion exchange methods. 2−6 So far, a bunch of different nanostructures of the ILHPs including nanocubes, 7 nanorods, 8 nanowires, 9 nanoplatelets, 10 nanosheets 11 have been extensively studied and reported. Especially, the utilization of ILHP nanocrystals has led to the development of promising optoelectronic devices, 12 such as light-emitting diodes (LEDs), 13−16 photodetectors, 2,17,18 solar cells, 19,20 and lasers.…”

Section: ■ Introductionmentioning

confidence: 99%

Solvent-Assisted Surface Engineering for High-Performance All-Inorganic Perovskite Nanocrystal Light-Emitting Diodes

Wang

Liu

Zhao

et al. 2018

ACS Appl. Mater. Interfaces

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All-inorganic cesium halide perovskite nanocrystals have attracted much interest in optoelectronic applications for the sake of the readily adjustable band gaps, high photoluminescence quantum yield, pure color emission, and affordable cost. However, because of the ineluctable utilization of organic surfactants during the synthesis, the structural and optical properties of CsPbBr nanocrystals degrade upon transforming from colloidal solutions to solid thin films, which plagues the device operation. Here, we develop a novel solvent-assisted surface engineering strategy, producing high-quality CsPbBr thin films for device applications. A good solvent is first introduced as an assembly trigger to conduct assembly in a one-dimensional direction, which is then interrupted by adding a nonsolvent. The nonsolvent drives the adjacent nanoparticles connecting in a two-dimensional direction. Assembled CsPbBr nanocrystal thin films are densely packed and very smooth with a surface roughness of ∼4.8 nm, which is highly desirable for carrier transport in a light-emitting diode (LED) device. Meanwhile, the film stability is apparently improved. Benefiting from this facile and reliable strategy, we have achieved remarkably improved performance of CsPbBr nanocrystal-based LEDs. Our results not only enrich the methods of nanocrystal surface engineering but also shed light on developing high-performance LEDs.

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“…Moreover, the endless electronic products and the constant updating of science and technology also require the energy materials with high performance to be used as electrode materials in electrochemical devices . In 2004, Geim and co‐workers first successfully separated graphene (a single‐layer graphite material), and started the research boom of two‐dimensional (2D) materials …”

Section: Introductionmentioning

confidence: 99%

Two‐Dimensional MOF and COF Nanosheets: Synthesis and Applications in Electrochemistry

et al. 2020

Chemistry A European J

198

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Metal–organic framework (MOF) and covalent organic framework (COF) nanosheets are a new type of two‐dimensional (2D) materials with unique design principles and various synthesis methods. They are considered ideal electrochemical devices due to the ultrathin thickness, easily tunable molecular structure, large porosity and other unique properties. There are two common methods to synthesize 2D MOF/COF nanosheets: bottom‐up and top‐down. The top‐down strategy mainly includes ultrasonic assisted exfoliation, electrochemical exfoliation and mechanical exfoliation. Another strategy mainly includes interface synthesis, modulation synthesis, surfactant‐assisted synthesis. In this Review, the development of ultrathin 2D nanosheets in the field of electrochemistry (supercapacitors, batteries, oxygen reduction, and hydrogen evolution) is introduced, and their unique dimensional advantages are highlighted.

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Ultrathin One- and Two-Dimensional Colloidal Semiconductor Nanocrystals: Pushing Quantum Confinement to the Limit

Cited by 66 publications

References 89 publications

Understanding the Formation of PbSe Honeycomb Superstructures by Dynamics Simulations

Understanding the Formation of PbSe Honeycomb Superstructures by Dynamics Simulations

Solvent-Assisted Surface Engineering for High-Performance All-Inorganic Perovskite Nanocrystal Light-Emitting Diodes

Two‐Dimensional MOF and COF Nanosheets: Synthesis and Applications in Electrochemistry

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