Elucidation of the Mechanism of Quantum Dot Arrangement Based on Self-Assembly of an Azobenzene Derivative

Kubo, Naoki; Yamauchi, Mitsuaki; Yamamoto, Seiya; Masuo, Sadahiro

doi:10.1246/bcsj.20210127

Cited by 5 publications

(5 citation statements)

References 23 publications

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“…An exception is the use of templates to form 1D assemblies of QDs. [17] Several research groups succeeded in fabricating 1D-arranged QDs by mixing dispersed QDs with appropriate templates comprising adhesion groups for QDs, such as molecular assemblies of a double-crossover DNA, [18] an amphiphilic block copolymer [19][20] and small organic molecules produced by our group, [21][22][23] and inorganic nano-sized substrates. [24] However, pure inter-QD interactions in 1D-arranged QDs have not been reported because of the presence of electronic and excitonic interactions between the arranged QDs and their templates and the absence of closely arranged QDs.…”

Section: Introductionmentioning

confidence: 99%

One‐Dimensionally Arranged Quantum‐Dot Superstructures Guided by a Supramolecular Polymer Template

Yamauchi,

Nakatsukasa,

Kubo

et al. 2023

Angew Chem Int Ed

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Colloidal quantum dots (QDs) exhibit important photophysical properties, such as long‐range energy diffusion, miniband formation, and collective photoluminescence, when aggregated into well‐defined superstructures, such as three‐dimensional (3D) and two‐dimensional (2D) superlattices. However, the construction of one‐dimensional (1D) QD superstructures, which have a simpler arrangement, is challenging; therefore, the photophysical properties of 1D‐arranged QDs have not been studied previously. Herein, we report a versatile strategy to obtain 1D‐arranged QDs using a supramolecular polymer (SP) template. The SP is composed of self‐assembling cholesterol derivatives containing two amide groups for hydrogen bonding and a carboxyl group as an adhesion moiety on the QDs. Upon mixing the SP and dispersed QDs in low‐polarity solvents, the QDs self‐adhered to the SP and self‐arranged into 1D superstructures through van der Waals interactions between the surface organic ligands of the QDs, as confirmed by transmission electron microscopy. Furthermore, we revealed efficient photoinduced fluorescence resonance energy transfer between the 1D‐arranged QDs by an in‐depth analysis of the emission spectra and decay curves.

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Section: Introductionmentioning

confidence: 99%

One‐Dimensionally Arranged Quantum‐Dot Superstructures Guided by a Supramolecular Polymer Template

Yamauchi,

Nakatsukasa,

Kubo

et al. 2023

Angew Chem Int Ed

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“…27,28,29,30 Inspired by the controllable self-assembly behavior different from NCs, we previously proposed a new methodology to form NC aggregated structures in solution using supramolecular aggregates of organic molecules with adhesion moieties to NCs as a template. 16,31,32 For example, when perylene bisimide derivatives having thiol groups that can be adsorbed onto NCs were used, mixing them with dot-shaped CdSe/ZnS NCs in an apolar solvent resulted in the coaggregation into a low-order structure of arranged NCs along a sheet-like aggregate. 31 Unexpectedly, when using azobenzene derivatives with an amino group for adhesion to NCs and amide group for hydrogen bonds, the coaggregation formed a high-order structure of arranged NCs in which the one-dimensionally aggregated NCs and azobenzene derivatives were alternately arranged.…”

Section: Introductionmentioning

confidence: 99%

Controlled coaggregation pathways of perovskite nanocrystals and supramolecular dye assemblies

Yamauchi,

Kubo,

Aratani

et al. 2023

Preprint

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High-order aggregates of semiconductor nanocrystals (NCs), known as superlattices, enable the fabrication of exceptional nanomaterials with structure-related physical properties and functionalities. The achievement of a heterogeneous superlattice composed of NCs and functional organic dyes leads to distinctive photophysical properties arising from the interaction between the NCs and dyes, thus activating multicomponent material chemistry. However, a methodology for controlling their heterostructures is yet to be established. Herein, we report a novel supramolecularly controlled coaggregation system involving perovskite NCs and perylene bisimide derivatives (PBIs) that form disorder, low-order, or high-order heterostructures. Their heterostructures were determined by the aggregation conditions of the PBIs (monomers, small aggregates, or large aggregates) before mixing with the NC. Notably, the high-order heterostructure exhibits an exceptional arrangement structure, such as Roman pavement, in which one-dimensionally arranged NCs and one-dimensionally stacked PBIs are alternately arranged at nanometer-scale intervals, as visualized using transmission electron microscopy. Spectroscopic analysis revealed that a high-order heterostructure (heterogeneous superlattice) was formed via an alteration in the π−π stacking interactions between the PBIs on the flat surface of the NC. Moreover, the high-order heterogeneous superlattice exhibited more efficient energy transfer from the NC to the assembled PBIs compared to the low-order heterostructure.

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“…Coupling nanoparticles to information-rich linkers that are stable in organic media would offer the possibility of accessing new hybrid materials with unique functionality. Assemblies in organic media have been explored, typically with self-assembling polymers as the structure-directing agent and show promise to not only organize nanoparticles but to do in a predictive manner to access a wide variety of morphologies [24][25][26][27] .Peptoids, or poly-N-substituted glycines, are peptide analogs that are functionalized on the nitrogen rather than carbon in the backbone sequence [28][29][30] . Through functionalization of the nitrogen, the monomers can be made soluble in a wide range of solvents, including organics, and the hydrogen-bonding interactions that often dominate secondary structure in peptides are absent [28][29][30] .…”

mentioning

confidence: 99%

“…Coupling nanoparticles to information-rich linkers that are stable in organic media would offer the possibility of accessing hybrid materials with functionality that has been previously unobtainable. Assemblies in organic media have been explored, typically with self-assembling polymers as the structure-directing agent and show promise to not only organize nanoparticles but to do so in a predictive manner to access a wide variety of morphologies. − …”

mentioning

confidence: 99%

Impact of Nanoparticle Size and Surface Chemistry on Peptoid Self-Assembly

et al. 2022

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Self-assembled organic nanomaterials can be generated by bottom-up assembly pathways where the structure is controlled by the organic sequence and altered using pH, temperature, and solvation. In contrast, self-assembled structures based on inorganic nanoparticles typically rely on physical packing and drying effects to achieve uniform superlattices. By combining these two chemistries to access inorganic-organic nanostructures, we aim to understand the key factors that govern the assembly pathway and structural outcomes in hybrid systems. In this work, we outline two assembly regimes between quantum dots (QDs) and reversibly binding peptoids. These regimes can be accessed by changing the solubility and size of the hybrid (peptoid-QD) monomer unit. The hybrid monomers are prepared via ligand exchange, assembled, and resulting assemblies are studied using ex-situ transmission electron microscopy as a function of assembly time. In aqueous conditions, QDs were found to stabilize certain morphologies of peptoid intermediates and generate a unique final product consisting of multilayers of small peptoid sheets linked by QDs. The QDs were also seen to facilitate or inhibit assembly in organic solvents based on the relative hydrophobicity of the surface ligands, which ultimately dictated the solubility of the hybrid monomer unit. Increasing the size of the QDs led to large hybrid sheets with regions of highly ordered square-packed QDs. A second, smaller QD species can also be integrated to create binary hybrid lattices. These results create a set of design principles for controlling the structure and structural evolution of hybrid peptoid-QD assemblies and contribute to the predictive synthesis of complex hybrid matter. TOC Graphic. Introduction.Hierarchically organized nanomaterials are often generated by mimicking natural systems wherein functional properties emerge due to order and organization across multiple length scales 1-3 . To predictively generate such materials, we must understand and systematize the atomic-level interactions that lead to organization of the functional building blocks across length scales. Traditionally, hybrid organic-inorganic nanomaterials are synthesized via bottom-up assembly or through templated assembly on a scaffold [4][5][6][7] . In these approaches, organic molecules, which are typically DNA, peptides (or peptoids), polymers, or small multitopic organic molecules, are used as the structure-directing elements with covalent and non-covalent interactions dictating the possible assembly outcomes 1,5-13 . These interactions are dependent on the sequence used and can often be controlled using pH, temperature, electrolytes, solvent, and/or pendant groups [14][15][16][17][18] . When inorganic nanoparticles act as the driving force for assembly, the generated structures are often a result of particle packing and drying effects. In these systems, the structures can be tuned through size, surface chemistry, ligand packing or morphology of the nanoparticles but frequently lack precision and are ...

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Elucidation of the Mechanism of Quantum Dot Arrangement Based on Self-Assembly of an Azobenzene Derivative

Cited by 5 publications

References 23 publications

One‐Dimensionally Arranged Quantum‐Dot Superstructures Guided by a Supramolecular Polymer Template

One‐Dimensionally Arranged Quantum‐Dot Superstructures Guided by a Supramolecular Polymer Template

Controlled coaggregation pathways of perovskite nanocrystals and supramolecular dye assemblies

Impact of Nanoparticle Size and Surface Chemistry on Peptoid Self-Assembly

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