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Nanocrystals: Synthesis, Properties and Applications

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A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Synthesis, Interfaces and Nanostructures".

Deadline for manuscript submissions: closed (26 February 2021) | Viewed by 38611

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Special Issue Editors

Dr. Dmitry Aldakov

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Guest Editor

SyMMES UMR-5819, Univ. Grenoble Alpes, CNRS, IRIG, SyMMES, F-38000 Grenoble, France
Interests: semiconductor nanocrystals; quantum dots; perovskite halides; solar cells; photocatalysis; non-toxic materials

Dr. Benoît Mahler

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Co-Guest Editor

iLM, UMR5306 - UCBL - CNRS, 10 rue Ada Byron, 69622 Villeurbanne, France
Interests: semiconductor nanocrystals; colloidal synthesis; two-dimensional nanocrystals; monolayers

Special Issue Information

Dear Colleagues,

Colloidal semiconductor nanocrystals represent a very dynamic field, both from a fundamental and applications viewpoint. Numerous efforts have been made to produce stable nanocrystals with controlled size, surface, and electronic properties. Their unique properties, such as their excellent size- and composition-related electronic and optical properties, stability, and limited toxicity make them very appealing materials for a variety of applications, such as solar cells, light-emitting devices, field-effect transistors, photocatalytic systems, photodetectors, and bioimaging, to name a few.

We invite authors to contribute original research articles or comprehensive review articles covering the most recent progress and new developments in the design, synthesis, study, and utilization of colloidal semiconductor nanocrystals for efficient and novel devices.

This Special Issue aims to cover a broad range of subjects, from nanocrystal synthesis and study of their fundamental properties, to the fabrication and characterization of devices and technologies with nanocrystals integration. The format of welcomed articles includes full papers, communications, and reviews. Potential topics include, but are not limited to, the following:

Novel colloidal nanocrystals (quantum dots) design and synthesis with a special focus on sustainable materials and technologies
Perovskite halide nanocrystals: synthesis and applications
Experimental and/or theoretical study of the synthesis mechanisms as well as fundamental properties of the nanocrystals
Fabrication and characterisation of the optoelectronic devices based on nanocrystals: solar cells, photodetectors, LEDs, TFTs, photoelectrocatalytical systems, and so.
Utilisation of nanocrystals for biological applications: bioimaging, drug delivery, and so on.

Dr. Dmitry Aldakov
Dr. Benoît Mahler
Guest Editors

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Keywords

Semiconductor nanocrystals
Quantum dots
Optoelectronic applications
Solar cells
Photodetectors
Bioimaging
LEDs
Perovskite nanocrystals

Published Papers (11 papers)

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Research

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14 pages, 2560 KiB

Open AccessArticle

Large-Scale Synthesis of Semiconducting Cu(In,Ga)Se₂ Nanoparticles for Screen Printing Application

by Bruna F. Gonçalves, Alec P. LaGrow, Sergey Pyrlin, Bryan Owens-Baird, Gabriela Botelho, Luis S. A. Marques, Marta M. D. Ramos, Kirill Kovnir, Senentxu Lanceros-Mendez and Yury V. Kolen’ko

Nanomaterials 2021, 11(5), 1148; https://doi.org/10.3390/nano11051148 - 28 Apr 2021

Cited by 10 | Viewed by 2791

Abstract

During the last few decades, the interest over chalcopyrite and related photovoltaics has been growing due the outstanding structural and electrical properties of the thin-film Cu(In,Ga)Se₂ photoabsorber. More recently, thin film deposition through solution processing has gained increasing attention from the industry, due to the potential low-cost and high-throughput production. To this end, the elimination of the selenization procedure in the synthesis of Cu(In,Ga)Se₂ nanoparticles with following dispersion into ink formulations for printing/coating deposition processes are of high relevance. However, most of the reported syntheses procedures give access to tetragonal chalcopyrite Cu(In,Ga)Se₂ nanoparticles, whereas methods to obtain other structures are scarce. Herein, we report a large-scale synthesis of high-quality Cu(In,Ga)Se₂ nanoparticles with wurtzite hexagonal structure, with sizes of 10–70 nm, wide absorption in visible to near-infrared regions, and [Cu]/[In + Ga] ≈ 0.8 and [Ga]/[Ga + In] ≈ 0.3 metal ratios. The inclusion of the synthesized NPs into a water-based ink formulation for screen printing deposition results in thin films with homogenous thickness of ≈4.5 µm, paving the way towards environmentally friendly roll-to-roll production of photovoltaic systems. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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10 pages, 1870 KiB

Open AccessArticle

Development of Quantum Dot (QD) Based Color Converters for Multicolor Display

by Muhammad T. Sajjad, Ashu K. Bansal, Francesco Antolini, Eduard Preis, Lenuta Stroea, Stefano Toffanin, Michele Muccini, Luca Ortolani, Andrea Migliori, Sybille Allard, Ullrich Scherf and Ifor D. W. Samuel

Nanomaterials 2021, 11(5), 1089; https://doi.org/10.3390/nano11051089 - 23 Apr 2021

Cited by 5 | Viewed by 2506

Abstract

Many displays involve the use of color conversion layers. QDs are attractive candidates as color converters because of their easy processability, tuneable optical properties, high photoluminescence quantum yield, and good stability. Here, we show that emissive QDs with narrow emission range can be made in-situ in a polymer matrix, with properties useful for color conversion. This was achieved by blending the blue-emitting pyridine based polymer with a cadmium selenide precursor and baking their films at different temperatures. To achieve efficient color conversion, blend ratio and baking temperature/time were varied. We found that thermal decomposition of the precursor leads to highly emissive QDs whose final size and emission can be controlled using baking temperature/time. The formation of the QDs inside the polymer matrix was confirmed through morphological studies using atomic force microscopy (AFM) and transmission electron microscopy (TEM). Hence, our approach provides a cost-effective route to making highly emissive color converters for multi-color displays. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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13 pages, 4610 KiB

Open AccessEditor’s ChoiceArticle

Organic-to-Aqueous Phase Transfer of Alloyed AgInS₂-ZnS Nanocrystals Using Simple Hydrophilic Ligands: Comparison of 11-Mercaptoundecanoic Acid, Dihydrolipoic Acid and Cysteine

by Patrycja Kowalik, Piotr Bujak, Mateusz Penkala and Adam Pron

Nanomaterials 2021, 11(4), 843; https://doi.org/10.3390/nano11040843 - 25 Mar 2021

Cited by 6 | Viewed by 2624

Abstract

The exchange of primary hydrophobic ligands for hydrophilic ones was studied for two types of alloyed AgInS₂-ZnS nanocrystals differing in composition and by consequence exhibiting two different emission colors: red (R) and green (G). Three simple hydrophilic ligands were tested, namely, 11-mercaptoundecanoic acid, dihydrolipoic acid and cysteine. In all cases, stable aqueous colloidal dispersions were obtained. Detailed characterization of the nanocrystal surface before and after the ligand exchange by NMR spectroscopy unequivocally showed that the exchange process was the most efficient in the case of dihydrolipoic acid, leading to the complete removal of the primary ligands with a relatively small photoluminescence quantum yield drop from 68% to 40% for nanocrystals of the R type and from 48% to 28% for the G ones. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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12 pages, 4833 KiB

Open AccessArticle

Synthesis and Characterization of CuIn_1−xGa_xSe₂ Semiconductor Nanocrystals

by Yu-Tai Shih, Yu-Ching Tsai and Der-Yu Lin

Nanomaterials 2020, 10(10), 2066; https://doi.org/10.3390/nano10102066 - 19 Oct 2020

Cited by 13 | Viewed by 1880

Abstract

In this paper, the synthesis and characterization of CuIn_1−xGa_xSe₂ (0 ≤ x ≤ 1) nanocrystals are reported with the influences of x value on the structural, morphological, and optical properties of the nanocrystals. The X-ray diffraction (XRD) results showed that the nanocrystals were of chalcopyrite structure with particle size in the range of 11.5–17.4 nm. Their lattice constants decreased with increasing Ga content. Thus, the x value of the CuIn_1−xGa_xSe₂ nanocrystals was estimated by Vegard’s law. Transmission electron microscopy (TEM) analysis revealed that the average particle size of the nanocrystals agreed with the results of XRD. Well-defined lattice fringes were shown in the TEM images. An analysis of the absorption spectra indicated that the band gap energy of these CuIn_1−xGa_xSe₂ nanocrystals was tuned from 1.11 to 1.72 eV by varying the x value from 0 to 1. The Raman spectra indicated that the A₁ optical vibrational mode of the nanocrystals gradually shifted to higher wavenumber with increasing x value. A simple theoretical equation for the A₁ mode frequency was proposed. The plot of this equation showed the same trend as the experimental data. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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15 pages, 3992 KiB

Open AccessArticle

Charge Carrier Relaxation in Colloidal FAPbI₃ Nanostructures Using Global Analysis

by Carolina Villamil Franco, Benoît Mahler, Christian Cornaggia, Thomas Gustavsson and Elsa Cassette

Nanomaterials 2020, 10(10), 1897; https://doi.org/10.3390/nano10101897 - 23 Sep 2020

Cited by 5 | Viewed by 2919

Abstract

We study the hot charge carrier relaxation process in weakly confined hybrid lead iodide perovskite colloidal nanostructures, FAPbI₃ (FA = formaminidium), using femtosecond transient absorption (TA). We compare the conventional analysis method based on the extraction of the carrier temperature (T_c) by fitting the high-energy tail of the band-edge bleach with a global analysis method modeling the continuous evolution of the spectral lineshape in time using a simple sequential kinetic model. This practical approach results in a more accurate way to determine the charge carrier relaxation dynamics. At high excitation fluence (density of charge carriers above 10¹⁸ cm⁻³), the cooling time increases up to almost 1 ps in thick nanoplates (NPs) and cubic nanocrystals (NCs), indicating the hot phonon bottleneck effect. Furthermore, Auger heating resulting from the multi-charge carrier recombination process slows down the relaxation even further to tens and hundreds of picoseconds. These two processes could only be well disentangled by analyzing simultaneously the spectral lineshape and amplitude evolution. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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24 pages, 6982 KiB

Open AccessFeature PaperArticle

Mixed Mercaptocarboxylic Acid Shells Provide Stable Dispersions of InPZnS/ZnSe/ZnS Multishell Quantum Dots in Aqueous Media

by Benjamin Heyne, Kristin Arlt, André Geßner, Alexander F. Richter, Markus Döblinger, Jochen Feldmann, Andreas Taubert and Armin Wedel

Nanomaterials 2020, 10(9), 1858; https://doi.org/10.3390/nano10091858 - 17 Sep 2020

Cited by 7 | Viewed by 3627

Abstract

Highly luminescent indium phosphide zinc sulfide (InPZnS) quantum dots (QDs), with zinc selenide/zinc sulfide (ZnSe/ZnS) shells, were synthesized. The QDs were modified via a post-synthetic ligand exchange reaction with 3-mercaptopropionic acid (MPA) and 11-mercaptoundecanoic acid (MUA) in different MPA:MUA ratios, making this study the first investigation into the effects of mixed ligand shells on InPZnS QDs. Moreover, this article also describes an optimized method for the correlation of the QD size vs. optical absorption of the QDs. Upon ligand exchange, the QDs can be dispersed in water. Longer ligands (MUA) provide more stable dispersions than short-chain ligands. Thicker ZnSe/ZnS shells provide a better photoluminescence quantum yield (PLQY) and higher emission stability upon ligand exchange. Both the ligand exchange and the optical properties are highly reproducible between different QD batches. Before dialysis, QDs with a ZnS shell thickness of ~4.9 monolayers (ML), stabilized with a mixed MPA:MUA (mixing ratio of 1:10), showed the highest PLQY, at ~45%. After dialysis, QDs with a ZnS shell thickness of ~4.9 ML, stabilized with a mixed MPA:MUA and a ratio of 1:10 and 1:100, showed the highest PLQYs, of ~41%. The dispersions were stable up to 44 days at ambient conditions and in the dark. After 44 days, QDs with a ZnS shell thickness of ~4.9 ML, stabilized with only MUA, showed the highest PLQY, of ~34%. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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11 pages, 2054 KiB

Open AccessArticle

Effects of Copper Dopants on the Magnetic Property of Lightly Cu-Doped ZnO Nanocrystals

by Zhi Wang, Wenzhen Xiao, Mengmeng Tian, Neng Qin, Haidong Shi, Xiwei Zhang, Wenke Zha, Jiahua Tao and Junlong Tian

Nanomaterials 2020, 10(8), 1578; https://doi.org/10.3390/nano10081578 - 11 Aug 2020

Cited by 13 | Viewed by 2326

Abstract

To explore the origin of magnetism, the effect of light Cu-doping on ferromagnetic and photoluminescence properties of ZnO nanocrystals was investigated. These Cu-doped ZnO nanocrystals were prepared using a facile solution method. The Cu²⁺ and Cu⁺ ions were incorporated into Zn sites, as revealed by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). At the Cu concentration of 0.25 at.%, the saturated magnetization reached the maximum and then decreased with increasing Cu concentration. With increasing Cu concentration, the photoluminescence (PL) spectroscopy indicated the distribution of V_O⁺ and V_O⁺⁺ vacancies nearly unchanged. These results indicate that Cu ions can enhance the long-range ferromagnetic ordering at an ultralow concentration, but antiferromagnetic “Cu⁺-Vo-Cu²⁺” couples may also be generated, even at a very low Cu-doping concentration. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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14 pages, 5015 KiB

Open AccessArticle

Hydrothermal Synthesis of Aqueous-Soluble Copper Indium Sulfide Nanocrystals and Their Use in Quantum Dot Sensitized Solar Cells

by Calink I. L. Santos, Wagner S. Machado, Karl David Wegner, Leiriana A. P. Gontijo, Jefferson Bettini, Marco A. Schiavon, Peter Reiss and Dmitry Aldakov

Nanomaterials 2020, 10(7), 1252; https://doi.org/10.3390/nano10071252 - 28 Jun 2020

Cited by 13 | Viewed by 4351

Abstract

A facile hydrothermal method to synthesize water-soluble copper indium sulfide (CIS) nanocrystals (NCs) at 150 °C is presented. The obtained samples exhibited three distinct photoluminescence peaks in the red, green and blue spectral regions, corresponding to three size fractions, which could be separated by means of size-selective precipitation. While the red and green emitting fractions consist of 4.5 and 2.5 nm CIS NCs, the blue fraction was identified as in situ formed carbon nanodots showing excitation wavelength dependent emission. When used as light absorbers in quantum dot sensitized solar cells, the individual green and red fractions yielded power conversion efficiencies of 2.9% and 2.6%, respectively. With the unfractionated samples, the efficiency values approaching 5% were obtained. This improvement was mainly due to a significantly enhanced photocurrent arising from complementary panchromatic absorption. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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11 pages, 2538 KiB

Open AccessArticle

Structural and Enhanced Optical Properties of Stabilized γ‒Bi₂O₃ Nanoparticles: Effect of Oxygen Ion Vacancies

by Ashish Chhaganlal Gandhi, Chia-Liang Cheng and Sheng Yun Wu

Nanomaterials 2020, 10(6), 1023; https://doi.org/10.3390/nano10061023 - 27 May 2020

Cited by 17 | Viewed by 3340

Abstract

We report the synthesis of room temperature (RT) stabilized γ–Bi₂O₃ nanoparticles (NPs) at the expense of metallic Bi NPs through annealing in an ambient atmosphere. RT stability of the metastable γ–Bi₂O₃ NPs is confirmed using synchrotron radiation powder X-ray diffraction and Raman spectroscopy. γ–Bi₂O₃ NPs exhibited a strong red-band emission peaking at ~701 nm, covering 81% integrated intensity of photoluminescence spectra. Our findings suggest that the RT stabilization and enhanced red-band emission of γ‒Bi₂O₃ is mediated by excess oxygen ion vacancies generated at the octahedral O(2) sites during the annealing process. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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Review

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17 pages, 3310 KiB

Open AccessEditor’s ChoiceReview

Revealing the Exciton Fine Structure in Lead Halide Perovskite Nanocrystals

by Lei Hou, Philippe Tamarat and Brahim Lounis

Nanomaterials 2021, 11(4), 1058; https://doi.org/10.3390/nano11041058 - 20 Apr 2021

Cited by 22 | Viewed by 5871

Abstract

Lead-halide perovskite nanocrystals (NCs) are attractive nano-building blocks for photovoltaics and optoelectronic devices as well as quantum light sources. Such developments require a better knowledge of the fundamental electronic and optical properties of the band-edge exciton, whose fine structure has long been debated. In this review, we give an overview of recent magneto-optical spectroscopic studies revealing the entire excitonic fine structure and relaxation mechanisms in these materials, using a single-NC approach to get rid of their inhomogeneities in morphology and crystal structure. We highlight the prominent role of the electron-hole exchange interaction in the order and splitting of the bright triplet and dark singlet exciton sublevels and discuss the effects of size, shape anisotropy and dielectric screening on the fine structure. The spectral and temporal manifestations of thermal mixing between bright and dark excitons allows extracting the specific nature and strength of the exciton–phonon coupling, which provides an explanation for their remarkably bright photoluminescence at low temperature although the ground exciton state is optically inactive. We also decipher the spectroscopic characteristics of other charge complexes whose recombination contributes to photoluminescence. With the rich knowledge gained from these experiments, we provide some perspectives on perovskite NCs as quantum light sources. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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20 pages, 13319 KiB

Open AccessReview

Sulvanites: The Promise at the Nanoscale

by Roberto Prado-Rivera, Chen-Yu Chang, Mimi Liu, Cheng-Yu Lai and Daniela R. Radu

Nanomaterials 2021, 11(3), 823; https://doi.org/10.3390/nano11030823 - 23 Mar 2021

Cited by 8 | Viewed by 5261

Abstract

The class of ternary copper chalcogenides Cu₃MX₄ (M = V, Nb, Ta; X = S, Se, Te), also known as the sulvanite family, has attracted attention in the past decade as featuring promising materials for optoelectronic devices, including solar photovoltaics. Experimental and theoretical studies of these semiconductors have provided much insight into their properties, both in bulk and at the nanoscale. The recent realization of sulvanites at the nanoscale opens new avenues for the compounds toward printable electronics. This review is aimed at the consideration of synthesis methods, relevant properties and the recent developments of the most important sulvanites. Full article

(This article belongs to the Special Issue Nanocrystals: Synthesis, Properties and Applications)

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