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Amrutha Manoj Lena, Mitsuaki Yamauchi, Hideyuki Murakami, Naoki Kubo, Sadahiro Masuo, Kyohei Matsuo, [Hironobu Hayashi](https://orcid.org/0000-0002-7872-3052), Naoki Aratani, Hiroko Yamada

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[Orderly Arranged Cubic Quantum Dots along Supramolecular Templates of Naphthalenediimide Aggregates](https://mdr.nims.go.jp/datasets/9b165e27-f918-48d6-a75d-ccc571cffc19)

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Orderly Arranged Cubic Quantum Dots along Supramolecular Templates of Naphthalenediimide AggregatesSupramolecular ChemistryOrderly Arranged Cubic Quantum Dots along SupramolecularTemplates of Naphthalenediimide AggregatesAmrutha Manoj Lena, Mitsuaki Yamauchi,* Hideyuki Murakami, Naoki Kubo,Sadahiro Masuo, Kyohei Matsuo, Hironobu Hayashi, Naoki Aratani,* and Hiroko Yamada*Abstract: Precise control of assembled structures of quantum dots (QDs) is crucial for realizing the desired photophysicalproperties, but this remains challenging. Especially, the one-dimensional (1D) control is rare due to the nearly isotropicnature of QDs. Herein, we propose a novel strategy for controlling the 1D-arrangement range of cubic perovskite QDsin solution based on the morphological modification of a supramolecular polymer (SP) template. The original templatewith a short and tangled fibrous structure is prepared in a low-polarity solvent mixture via self-assembly of anaphthalenediimide-functionalized cholesterol derivative with an adhesion group for QDs. Mixing this template withQDs leads to the co-aggregation into short-range 1D-arrays of QDs on the templates. Notably, subsequent heating andcooling of the co-aggregate solution forms longer-range 1D-arrays of QDs with lateral growth, where arranged QDs aresandwiched between reconstructed SP templates. Furthermore, the longer-range 1D-array of QDs is achieved via analternative route involving the pre-organization of templates into longer and dispersed fibers by heating and cooling ofthe original template, succeeded by co-assembly with QDs. Finally, we reveal continuous fluorescence resonance energytransfer between 1D-arranged QDs by an in-depth analysis of the photoluminescence decay curves.IntroductionSemiconductor nanocrystals, called quantum dots (QDs),are regarded as outstanding photoluminescent (PL) nano-materials that have potential for a wide range of applicationsin interdisciplinary research areas, such as opto-electronics,[1–2] bioimaging,[3–4] catalysis,[5–6] displays,[7–9] andso on. Among QDs, perovskite QDs, specifically cesiumlead halide-based QDs (CsPbX3, X=Cl, Br, I), have gainedprominence in the field of luminescent materials. They offerhigh luminous efficiency, narrow PL linewidths that givehigh color purity, tunable PL wavelengths (by manipulatingthe halide composition), and high photodurability.[10–12]Recent researches have focused on the ordered spatialintegration of individual QDs. This is because their assemblyaffords advanced photophysical properties, such as long-range exciton diffusion,[13–14] collective PL (superfluore-scence),[15–16] and quantum resonance,[17–18] that cannot berealized in single and randomly assembled states. Theseproperties are attributed to the ordered array structures ofQDs, which exhibit efficient exciton transfer and/or elec-tron- and exciton-coupling interactions. In previous studies,QD array structures have been constructed mainly bysolvent-evaporation-induced self-assembly on a substrate,leading to two-dimensional (2D)- and three-dimensional(3D)-ordered assemblies of QDs, such as superlattices.[15] Incontrast to these structures, one-dimensional (1D) orderedassemblies of QDs do not form spontaneously because ofthe difficulty in the anisotropic arrangement of isotropicQDs.Several research groups,[19–22] including ours[23–26] havereported template methods for forming anisotropic 1D-arrays of spherical QDs using supramolecular assemblies ofpolymers, small organic molecules, and inorganic nano-structures. The template methods have been also utilized forthe arrangement of metal nanoparticles.[27–28] Among thesetemplates, supramolecular assembly templates can accu-rately control the location of the QDs based on the templatestructure. Recently, we have succeeded in the 1D-arrayformation of spherical CdSe and CdSe/ZnS QDs using asupramolecular polymer (SP) template composed of acholesterol derivative with hydrogen bonding moieties and[*] A. Manoj Lena, Prof. Dr. N. ArataniDivision of Materials ScienceNara Institute of Science and Technology (NAIST)8916-5 Takayama-cho, Ikoma, Nara 630-0192 (Japan)E-mail: aratani@ms.naist.jpDr. M. Yamauchi, H. Murakami, Dr. K. Matsuo, Prof. Dr. H. YamadaInstitute for Chemical ResearchKyoto UniversityGokasho, Uji, Kyoto 611-0011 (Japan)E-mail: yamauchi.mitsuaki.4u@kyoto-u.ac.jphyamada@scl.kyoto-u.ac.jpN. Kubo, Prof. Dr. S. MasuoDepartment of Applied Chemistry for EnvironmentKwansei Gakuin University1 Gakuen, Uegahara, Sanda, Hyogo 669-1330 (Japan)Dr. H. HayashiCenter for Basic Research on MaterialsNational Institute for Materials Science (NIMS)1-2-1 Sengen, Tsukuba, Ibaraki 305-0047 (Japan)© 2025 The Author(s). Angewandte Chemie International Editionpublished by Wiley-VCH GmbH. This is an open access article underthe terms of the Creative Commons Attribution Non-CommercialNoDerivs License, which permits use and distribution in any med-ium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made.AngewandteChemieResearch Articlewww.angewandte.orgHow to cite: Angew. Chem. Int. Ed. 2025, 64, e202423912doi.org/10.1002/anie.202423912Angew. Chem. Int. Ed. 2025, 64, e202423912 (1 of 9) © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbHhttp://orcid.org/0000-0003-0005-5960http://orcid.org/0000-0003-4828-5968http://orcid.org/0000-0002-2472-9459http://orcid.org/0000-0002-7872-3052http://orcid.org/0000-0002-3181-6526http://orcid.org/0000-0002-2138-5902https://doi.org/10.1002/anie.202423912http://crossmark.crossref.org/dialog/?doi=10.1002%2Fanie.202423912&domain=pdf&date_stamp=2025-01-17an adhesion moiety (carboxyl group) for QDs (Figure 1a).[26]However, the rational methodology to control the arrange-ment range of QDs using SP templates has not yet beenestablished. In addition, the 1D-arrangement of cubic QDsremains challenging.[29] As a rare example, Pan et al.reported the 1D-array of cubic CsPbBr3 QDs using a pod-shaped PdSO4 scaffold.[30] If this methodology using SPtemplates is established, more effective interactions betweencubic QDs can occur via their flat surfaces.Herein, we report a new strategy to control the 1D-arraystructures of cubic CsPbBr3 QDs, achieving short- andlonger-range organization through fine-tuning of the SPtemplate morphology (Figures 1c,d). This template consistsof chiral self-assemblies of naphthalenediimide (NDI)-functionalized cholesterol derivative 1 (Figure 1b), possess-ing a pyridyl group as adhesion moiety for QDs. Figure 1dsummarizes the co-aggregation routes into short- andlonger-range 1D-array of QDs based on transmissionelectron microscopy (TEM) observation. Upon adding poorsolvent to the monomeric solution, 1 self-assembled intoshort and tangled fibrils (template A). Subsequently, mixingthem with QDs resulted in short-range 1D-arrays of QDsvia the adhesion of QDs on the templates. Notably, uponconsecutive heating and cooling of the co-aggregate solution(thermal treatment), longer-range 1D-arrays of QDs withlateral growth, in which they are sandwiched between thereconstructed SP template, were formed. In addition, wefound that the longer-range 1D-array of QDs could beformed also via an alternative co-aggregation route. In thisroute, longer and dispersed fibrils of 1 (template B) werepre-organized by thermal treatment of the template A insolution and then co-assembled with QDs to form thelonger-range 1D-array. An in-depth analysis of the PL decaycurves revealed continuous efficient fluorescence resonanceenergy transfer (FRET) among the 1D-arranged QDs. Tothe best of our knowledge, this study is the first example ofmanaging the 1D-array range of cubic QDs utilizing SPtemplates.Results and DiscussionIn this work, the adhesion between the SP template andQDs was essential for the formation of arranged QDs. Inthe previous work, the use of carboxyl group as adhesionmoiety for QDs (Figure 1a)[26] can form unfavorable hydro-gen-bonded dimers without exposed adhesion sites for QDs.Therefore, we newly designed a cholesterol derivative 1 witha pyridyl group at the end of the molecule as a moreappropriate adhesion moiety for QDs (Figure 1b). Thecholesterol group was introduced at the other end as asoluble substituent in low-polarity solvents and a chiralmoiety. Amide and carbamate groups were introduced topromote self-assembly by hydrogen bonds. NDI coreunit,[31–33] a well-established class of molecules insupramolecular chemistry, is used as a π–π stacking moietyand their aggregation behaviors can be monitored byspectroscopic analyses. To confirm the adhesion effect ofthe pyridyl group indirectly, a reference compound 2 wassynthesized by replacing the pyridyl group with a phenylgroup (Figure 1b). 1 and 2 were synthesized in two stepsusing naphthalene-tetracarboxylic dianhydride as the start-ing reagent. The synthetic schemes and characterizationdata of 1 and 2 using 1H- and 13C-nuclear magneticresonance (NMR) spectroscopy and high-resolution massspectrometry (HRMS) are described in the SupportingInformation (Schemes S1, S2, Figures S1–S9).First, the absorption characteristics of 1 ([1]=3.0×10� 4 M) were evaluated in chloroform (CHCl3), where 1was expected to exist predominantly in its monomeric state.The UV/Vis absorption spectrum demonstrated sharp peakswith absorption maxima at 380, 360, and 342 nm, corre-sponding to the π–πS transitions of the NDI core inmonomeric 1 (Figure 2a). To form aggregates of 1 in a low-polarity solvent mixture ([1]=3.0×10� 4 M), a solution of 1 inCHCl3/methylcyclohexane (MCH) (2 :5, v/v) was preparedby adding 0.75 mL of MCH as a poor solvent into 0.30 mLof a CHCl3 solution ([1]=1.1×10� 3 M). The spectrum of theaggregates in solution showed broader peaks with a loss ofvibronic structure and a slight increase in a new red-shiftedabsorption at approximately 400 nm (Figure 2a) indicatingπ–π stacking interactions between the NDI cores of theaggregate.[33] To obtain evidence of hydrogen bonding, werecorded the Fourier transform infrared (FT-IR) spectra ofFigure 1. Molecular structures of (a) the previous compound and (b) 1and 2. (c) Chemical structure of CsPbBr3 QD. (d) Schematic illustrationof the 1D-array formation of QDs on different templates of 1.AngewandteChemieResearch ArticleAngew. Chem. Int. Ed. 2025, 64, e202423912 (2 of 9) © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH 15213773, 2025, 13, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/anie.202423912 by National Institute For, Wiley Online Library on [24/08/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons Licensethe same solutions (monomeric 1 in CHCl3 and aggregated 1in CHCl3:MCH (2 :5, v/v)). The FT-IR spectra are shown inFigure S10a. Monomeric 1 showed a free N� H peak at3452 cm� 1, while aggregated 1 showed the emergence ofextra broad N� H peaks in the shorter wavenumber region at3345 and 3262 cm� 1. This result indicates the existence oftwo types of hydrogen bonding modes for amide andcarbamate groups, attributed to different hydrogen bondstrengths.The supramolecular chirality of aggregated 1 based onthe chiral exciton coupling between the NDI cores, wasdetermined from the variations in circular dichroism (CD)signals from the monomeric to the aggregated state.Although the CD signal of monomeric 1 in CHCl3 wasnegligible in the absorption region of the NDI cores becauseof the absence of chiral π–π stacking, aggregated 1 exhibitedclear CD signals with two sharp positive peaks at 368 and390 nm (Figure 2b). These CD signals suggest that 1 under-goes self-assembly via one-handed biased helical stacking.The morphological features of the aggregates of 1 wereassessed using TEM and atomic force microscopy (AFM).The TEM images reveal predominant formation of shortand tangled nanofibrils (Figures 2c,d and S10b, c). Theaverage width of a single nanofibril was measured to be ca.10 nm. The AFM analysis revealed a height of ca. 9 nm(Figures 2e and S10d). Considering the above results, thenanofibril was expected to be a cylindrical structure with adiameter of 9–10 nm. This diameter is nearly twice themolecular length of 1 (4.7 nm) estimated from the energy-optimized structure using density functional theory (DFT)calculation (Figure 2f). Also, the nanofibril was expected tobe formed via helical stacking of 1 based on the CD activity(Figure 2b). According to the results, we can exclude thepossibility of a simpler single helical-growth with rotationalstacks maintaining the molecular length, known as twistedribbon[34] (Figure S10e). To be twice the molecular length,an offset stacking event should be involved in the helical-growth. Therefore, we conclude that multiple helical-growths into a tightly coiled ribbon or a tube-likestructure[34] occurred as the major self-aggregation processrather than a single helical-growth (Figures 2f and S10e).Occasionally, the helical nanostructures with pitch wereobserved as a screwed tube structure (Figure 2d inset),which supported the helical-growth mechanism.Similarly, we investigated the self-assembly behavior ofthe reference compound 2. In CHCl3/MCH (2 :5, v/v), inwhich 1 self-assembled, 2 existed as monomers, as confirmedby the sharp absorption peaks, absence of CD signals, andpresence of an IR peak corresponding to free N� H moietiesonly (Figures S11a–c). This result indicates that 2 has alower self-assembling ability than 1, presumably because ofthe higher solubility of the phenyl group in 2 compared tothe pyridyl group in 1 in the low-polarity solvent mixture.To induce the self-assembly of 2, we attempted itsaggregation at a higher ratio of MCH (CHCl3 :MCH=1 :7,v/v). The aggregate formation was confirmed by the broad-ening of absorption peaks, emergence of CD signals, andpresence of new IR peaks corresponding to the hydrogen-bonded amide and carbamate groups (Figures S11a–c).Unlike 1, 2 displayed increased light scattering effects on theabsorbance towards longer wavelengths (Figure S11a), in-dicating the formation of larger aggregates. As predicted,larger tangled fibrils were confirmed using TEM (Fig-ure S11d).Cubic CsPbBr3 QDs coated with surface ligands (oleicacid and oleylamine) were synthesized according to pre-viously reported procedures (Figure 1c and SupportingInformation).[10] TEM analysis of the QDs, spin-coated fromthe solution onto a grid, revealed the cube-shape of the QDswith an average edge-to-edge length of 7.8�1.0 nm (Figur-es S12a,b). The TEM images showed assembled structuresof the QDs formed by drying their dispersed solution on thesubstrate. The molar concentration of QD solution, assum-ing a single QD as a molecule, was estimated using anabsorption spectrum in solution according to the reportedmethod.[35]Previously, the interaction between nitrogen atoms ofthe pyridyl group and Pb atoms of formamidinium (ormethylammonium) lead halide perovskite crystals has beenreported in the solid state.[36–37] However, the dynamicinteraction in solution has not been revealed. To obtaininsight into the adhesion of 1 to QD, we compared the 1HFigure 2. (a) UV/Vis absorption and (b) CD spectral changes of 1([1]=3.0×10� 4 M) in CHCl3 and CHCl3/MCH (2 :5, v/v). (c,d) TEM and(e) AFM images of the nanofibrils of 1. Inset in (d) is a magnifiedimage of helical structure. (f) Schematic illustration of a possibleaggregate structure of 1.AngewandteChemieResearch ArticleAngew. Chem. Int. Ed. 2025, 64, e202423912 (3 of 9) © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH 15213773, 2025, 13, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/anie.202423912 by National Institute For, Wiley Online Library on [24/08/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons LicenseNMR spectra of 1, QD, and their mixture ([1] : [QD]=100 :1) in [D8]toluene (Figure S13). Upon mixing 1 with QD,the original proton signal of the pyridyl group of 1 showed aslight shift with a signal broadening, while the proton signalsof the NDI and cholesterol moieties did not change. Thisimplies the adhesion of the pyridyl moiety on the QDsurface.The short and tangled nanofibrils of 1 can serve as SPtemplates (referred to as template A) because their surfacescontain pyridyl groups as adsorption sites for QDs. Thus,the arrangement of QDs using the SP template wasattempted by mixing the fibrous aggregate of 1 and QDs insolution. First, we prepared a QD solution ([QD]=ca.1×10� 7 M) in CHCl3/MCH (2 :5, v/v) and dried it to be a filmunder argon flow. Subsequently, it was mixed with anaggregate solution of 1 (CHCl3 :MCH=2 :5, v/v, [1]=3.0×10� 4 M). The molar ratio of 1 :QD in the mixture wasmaintained at 3000 :1. To confirm the adhesion of the QDsonto the template, TEM observation of the co-aggregateswas carried out (Figures 3a–d). The images revealed theadhesion of the QDs to the tangled fibrous template A, inwhich 1D-arrangement of several QDs (short-range 1D-array) was observed along the surfaces of the templates(Figure 3e). In addition, we can infer that the adsorption ofQDs on the template was highly favorable, as no free orself-assembled QDs were observed on other areas (Figur-es S14a,b). In the adhesion process, the exposed pyridylgroups on the template interchange with the original surfaceligands, oleic acid and oleylamine, of QDs, via a ligand-exchange reaction[38] and/or contact to a site without ligandsor a halide vacancy on the surface.[39]In contrast, the TEM images of a mixture of self-assembled 2 and QDs revealed mainly isolated regions of 2and QDs, namely phase separation via narcissistic self-sorting (Figure S15a). Unlike the combination of 1 and QD,self-assembled QDs formed by the evaporation of solventson the substrate were also observed (Figure S15b). Thus, weindirectly conclude that the pyridyl groups on the SPtemplate of 1 serve as effective adhesion moieties for QDs.Next, we investigated the photophysical interactionsbetween the SP template A of 1 and QDs. The UV/Visabsorption spectrum after mixing them was nearly consistentwith the sum of their individual spectra (Figure 4a). Thisresult excludes electronic interactions between QD and 1 inthe ground state. In addition, no clear CD spectral changeswere observed after mixing (Figure 4b), indicating that theadhesion of QDs did not disrupt the chiral stacking of 1. Incontrast, the PL spectra of QDs under an irradiation of470 nm, at which only QDs are excited, showed a decreasein the PL intensity upon mixing with template A (Figure 4a).This result suggests an increase in other nonradiativeprocesses via interactions between QD and 1 and/orarranged QDs in the excited state.To investigate the thermal reversibility of the 1D-arranged structure of QDs along the SP template, weprepared an original solution ([1] : [QD]=3000 :1, [1]=3.0×10� 4 M) by mixing an aggregate solution of 1(CHCl3 :MCH=2 :5, v/v, [1]=3.0×10� 4 M) and a film pre-pared by drying a QD solution ([QD]=ca. 1×10� 7 M). Afterheating the original solution at 90 °C and subsequent coolingto 20 °C, the arrangement level of QDs on the templatechanged (Figures 5a–c and S16). The TEM images revealedthe formation of not only short-range 1D-arrays, but alsolonger-range ordered 1D-arrays of QDs, compared to theoriginal arrangement structures before heating and coolingFigure 3. (a) TEM image and (b–d) the magnified images of 1D-arranged QDs along the SP template A of 1. (e) Schematic illustrationof the co-aggregate model structure.Figure 4. (a) UV/Vis absorption, PL, and (b) CD spectra of thedispersed QDs ([QD]=ca. 1×10� 7 M), the SP template A of 1([1]=3.0×10� 4 M), and co-aggregates of the SP template A of 1 andQD ([1] : [QD]=3000 :1; [1]=3.0×10� 4 M) in CHCl3/MCH (2 :5, v/v).The excitation wavelength of PL spectra was 470 nm.AngewandteChemieResearch ArticleAngew. Chem. Int. Ed. 2025, 64, e202423912 (4 of 9) © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH 15213773, 2025, 13, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/anie.202423912 by National Institute For, Wiley Online Library on [24/08/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License(Figures 3a–c). The longest 1D-array consisted of 21 QDswith length ~200 nm (Figure 5b). In these TEM images,longer SPs of 1 were observed as templates for the longer-range 1D-array of QDs, suggesting that the templatestructure was re-constructed via the heat-cool treatment.Notably, the 1D-arranged QDs were found to be sand-wiched between the re-constructed SP templates (Figure 5e).The model co-aggregate structure is shown in Figure 5f.The QDs were orderly arranged in 1D-array orientingtheir flat facets in the same direction, namely, face-to-faceoverlapping configuration (Figures 5c, f). To compare thislonger-range and the original short-range 1D-arrays (beforeheat-cool), we measured the center-to-center distance (d1)between the arranged QDs for more than 100 array points.The histograms are shown in Figure 5d. The average valueof d1 for the longer-range 1D-array was 10.3�1.3 nm. Thisstandard deviation was derived from the size distribution ofQDs (7.8�1.0 nm). For the original 1D-array, the averagevalue of d1 was 10.5�1.6 nm, which was slightly larger thanthat of the longer-range 1D-array. This result implies thatthe heat-cool treatment induces not only the formation of alonger-range 1D-array of QDs, but also a more uniformface-to-face overlapping configuration. Furthermore, theedge-to-edge distance (d2) between the 1D-arranged QDswas estimated to be ~2 nm from the TEM images. Consider-ing that this distance is less than twice the lengths of surfaceligands oleic acid and oleylamine, interdigitation betweenthe surface ligands occurs via van der Waals interactions(Figure 5f). This interdigitation can lead to face-to-faceoverlapping of the arranged QDs.Notably, we found a lateral growth of 1D-arranged QDsperpendicular to the 1D-array direction by TEM imaging(Figures 5g and S16). This means the formation of a multi-layer sandwich structure with repeated alternate arrange-ment of 1D-array of QDs and SP of 1. The lateralinteraction is presumably because the SP template has anadhesion ability on both sides, which is derived from thehelical morphology.Next, we increased the concentration of QDs in the co-aggregate to approximately 3×10� 7 M ([1] : [QD]=3000 :3)and performed heat-cool treatment. TEM images displayedmore densely adsorbed QDs with long-range 1D-arraystructures along the SP template (Figures S17a–c). One ofthe longest 1D-arrays of QDs measured ~400 nm. Free QDsthat were not adsorbed on the template were also observed,suggesting that this concentration of QDs was over thecapacity of the templates.We then investigated the thermal effect on the change of1D-array structures of QDs along the templates of 1 byfurther heat-cool treatments. However, the TEM imagesshowed only a few 1D-array structures after twice heat-cooltreatment of the solution. In addition, fibrous templateswithout QDs and largely fused QDs were mainly observed(Figures S18a–c). This is probably due to the thermallyinduced agglomeration or decomposition of QDs.Here, we discuss the mechanism for the formation of alonger-range 1D-array of QDs by the heat-cool process. Wemeasured the CD spectrum of the co-aggregate ([1]:[QD]=3000 :1, [1]=3.0×10� 4 M) at 90 °C to investigate the changein the stacking nature of 1 upon heating. The CD signals ofthe co-aggregates decreased but did not completely dis-appear (Figure S19a), indicating the presence of monomersand aggregates of 1 at 90 °C. In contrast, the self-aggregatesof 1 showed a more pronounced decrease in CD signalsupon heating to 90 °C (Figure S19b). The higher thermalstability of the co-aggregates was probably due to theadsorption of QDs onto the template of 1. This hot solutionFigure 5. (a–c) TEM images of longer-range 1D-arranged QDs ontemplates of 1 after heat-cool treatment. (d) Histogram of the center-to-center distance between 1D-arranged QDs. Top and bottom histo-grams correspond to the short- and longer-range 1D-arranged QDs,respectively. (e) TEM image of 1D-arranged QDs sandwiched betweenthe templates, obtained under a different focus mode. (f) Schematicillustration of the 1D-arranged nanostructure of QDs, in which d1 andd2 are the center-to-center and edge-to-edge distance, respectively.(g) TEM image of 1D-arranged QDs with lateral growth and the modelstructure.AngewandteChemieResearch ArticleAngew. Chem. Int. Ed. 2025, 64, e202423912 (5 of 9) © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH 15213773, 2025, 13, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/anie.202423912 by National Institute For, Wiley Online Library on [24/08/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons Licensewas directly spin-coated onto a grid, and the samples wereobserved using TEM. The images revealed that the short-range 1D-array of QDs on the template of 1 persisted evenat high temperatures (Figures S19c,d). Additionally, shortfibers of 1, randomly assembled QDs, and free QDs wereobserved. After cooling to 20 °C, the CD signals recovereddue to the reassembly of 1 (Figure S19a). Consequently,cooling led to the formation of longer-range 1D-arrays ofQDs (Figure 5a). Based on these results, we propose thefollowing reconstruction mechanism. At high temperatures,short-range 1D-arrays of QDs along the template of 1coexist with the monomers of 1 and free QDs. During thecooling process, the monomers are consumed for theformation of more extended SP templates, and then freeQDs are adsorbed and arranged along the re-constructedlonger template.From the above results, the formation of longertemplates of 1 is a key factor to realize the longer-range 1D-array of QDs. We predicted that if a longer SP template canbe prepared and then mixed with free QDs, a similar longer-range 1D-array of QDs can be formed. Therefore, weverified whether a longer fiber of 1 is formed in the absenceof QDs by heat-cool treatment of the aggregate solution of 1(CHCl3 :MCH (2 :5, v/v), [1]=3.0×10� 4 M). As confirmed byTEM, longer and dispersed fibrils (referred to as templa-te B), compared to the tangled short fibrils (template A)prepared by the original method, were formed upon coolingof a hot solution (~80 °C) (Figures 6a and S20). Subse-quently, upon mixing them with QDs, longer-range 1D-arrangement of QDs along the longer template B wasachieved as expected (Figures 6b, c and S21). The co-aggregates contained 1D-arranged QDs sandwiched be-tween the templates and their lateral growth perpendicularto the 1D-array direction, similar to that obtained by theheat-cool treatment of the mixture (Figure 5a). This coag-gregation method via pre-tuning of the template morphol-ogy was also effective at a lower concentration of 1 ([1]=2.0×10� 4 M), where longer-range 1D-arrays of QDs wasobtained along the longer SP template (Figures 6d,e, andS22, S23). This result supports the usefulness and reproduci-bility of this method. As this method did not include theheating process of QDs, the QDs in the longer-range 1D-array structure did not suffer any thermal effects.Finally, we discuss the interactions between an excitedQD and templates of 1 or neighboring QDs. DFT calcu-lations revealed the highest occupied molecular orbital(HOMO= � 7.3 eV) and lowest unoccupied molecular orbi-tal (LUMO= � 3.8 eV) energy levels of the NDI core.Considering the conduction (� 3.1 eV) and valence band(� 5.6 eV) energy levels of CsPbBr3 QDs from previouslyreported experimental values,[40] photoinduced electrontransfer (eT) from the excited arranged QDs to NDI wasanticipated (Figure 7a). Previously, eT from QD to mono-meric NDI derivatives has been reported.[41] However, thepossibility of eT in this case is low since the distancebetween the NDI core and edge of QD is not sufficientlyshort due to the presence of a long alkyl linkage betweenthe pyridyl group and NDI core (2.4 nm, Figure 2f).Alternately, FRET between 1D-arranged QDs can occurthrough dipole–dipole interactions, as observed in the caseof arranged spherical CdSe QDs.[25–26] The potential occur-rence of FRET was supported by the sufficient spectraloverlap between the PL and absorption spectra of the QDs(Figure S12c). This spectral overlap integral (J(λ)) value wasestimated to be 1.06×1017 M� 1 (cm)� 1 (nm)4 according to themethod shown in Figure S12 caption, which is suitably largeenough for FRET interactions. Förster radius (R0), at whichthe FRET efficiency is 0.5, was estimated to be ca. 10 nm,which is comparable to d1 (Figure 5d). In contrast, thepossibility of FRET from QD to 1 was excluded due to theenergy mismatch (Figure 4a). Therefore, it is expected thatthe arranged QDs along the SP templates of 1 predom-inately possess inter-QD FRET, rather than eT from QD to1, in the excited state of QDs (Figure 7b).To evaluate the exciton dynamics of QDs among the co-aggregates in CHCl3:MCH (2 :5, v/v), we analyzed the PLdecay curves of co-aggregates under an irradiation of 470nm. The timing of measurements was set to 15 min aftermixing SP with QDs to accurately compare the PL decaycurves. Here, short-range 1D-array of QDs along templateA (referred to as Coagg-A) and longer-range 1D-array ofFigure 6. (a–c) TEM images of (a) SP template B ([1]=3.0×10� 4 M) (b)longer-range 1D-arranged QDs on the template, and (c) the magnifiedimage. (d,e) TEM images of (d) SP template B at lower concentrationof 1 ([1]=2.0×10� 4 M) and (e) longer-range 1D-arranged QDs on thetemplate. (f) Schematic illustration of the co-aggregation process viatemplate B.AngewandteChemieResearch ArticleAngew. Chem. Int. Ed. 2025, 64, e202423912 (6 of 9) © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH 15213773, 2025, 13, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/anie.202423912 by National Institute For, Wiley Online Library on [24/08/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons LicenseQDs along template B (referred to as Coagg-B) werecompared in the same conditions except for preparationroutes ([1] : [QD]=3000 :1, [1]=3.0×10� 4 M). As a reference,the decay curve of dispersed QDs ([QD]=ca. 1×10� 7 M)was measured. The PL decay curves are shown in Figure 7c.The curves were fitted using two exponential equations toestimate the PL lifetime (Figures S24a–c and Table S1). Theresults reveal a decrease in the average PL lifetime (τ) forQDs from 5.0 ns (τQD, dispersed QDs) to 3.1 ns (τCoagg-A,Coagg-A) and 3.6 ns (τCoagg-B, Coagg-B). Similar changeswere reproducibly confirmed (Figures S25a–c and Table S2).The shortening of the PL lifetimes in Coagg-A and Coagg-Bindicates the occurrence of nonradiative processes by thearrangement of QDs.To unveil pure interactions between QDs, we measuredPL spectrum and PL decay curve at 10 times higherconcentration of QDs ([QD]=ca. 1×10� 6 M). A red-shiftedPL peak by 6 nm was observed compared to the original QDsolution ([QD]=ca. 1×10� 7 M) (Figure S26a). Unlike thecase of original concentration, single component and longerPL lifetime (10.9 ns) was obtained with more delayed risetime (Figures 7e, f, S26b, and Table S3). These changes canbe explained by multiple re-absorption and re-emission ofphoton, so-called photon recycling via radiative energytransfer (ET) process that is different mechanism fromnonradiative FRET.[42–43] This photon recycling predomi-nately occurs from smaller QD with larger band gap tolarger QD with smaller band gap, resulting in the red-shiftedPL. The red-shifted PL peak due to the re-absorption wasalso revealed in their superlattice.[44] Difference between thetwo ET mechanisms is whether there is a nonradiativeprocess or not. Although FRET induces shortening of PLlifetime of donors, it is difficult to analyze PL lifetimecomponents of donors because of the large PL overlap ofdonor and acceptor like this study’s system. To obtain moreaccurate insight into interactions between QDs, we eval-uated an aggregated QD film, in which QDs were locatedclosely as mixture of randomly and orderly aggregated QDs.The film was prepared by drop-cast and drying of the QDsolution ([QD]=ca. 1×10� 7) on a substrate. The PL decaycurve afforded PL average lifetime (τQD-film) of 3.6 ns (Fig-ure S26c and Table S3), which was shorter than that ofdispersed QDs (5.0 ns). As the change was induced by theaggregation of QDs, this shortening of the PL lifetimes wasassignable to continuous FRET between aggregated QDs,so-called exciton diffusion. Due to the continuous FRET,the probability of exciton trapping by defects of QD canincrease, resulting in the decrease of PL lifetimes.Notably, the τQD-film value of QD films (3.6 ns), which is asuitable condition for continuous FRET, is consistent withthe τCoagg-B value. Thus, we conclude that the longer-range1D-array of QDs in the Coagg-B exhibits continuous FRETin solution, comparable to the QD films. In addition, Coagg-A exhibited a slightly shorter PL lifetime (3.1 ns) comparedto that of the QD films (3.6 ns). This can be possiblyexplained due to the competitive eT from QD to SP inCoagg-A exhibiting FRET among short-range QD-arrays.When the contribution of eT increases, further shortening ofPL lifetime can occur as observed. Especially, non-arranged(adsorbed) QDs on SP templates can show eT. Anotherexplanation for the longer lifetime of Coagg-B than that ofCoagg-A could be the efficient photon recycling acrosslonger-range 1D-array of QDs, which enhances the PLlifetime.ConclusionIn summary, we succeeded in controlling the short- andlonger-range 1D-array structures of cubic perovskite QDs insolution by a new strategy of morphological tuning of SPtemplate composed of NDI-functionalized cholesterol deriv-ative with a pyridyl adhesion group. Upon mixing thedispersed QDs and SP templates with short and tangledfibrous structure in solution, the QDs self-arranged on thetemplate into a short-range 1D-array, as revealed by TEM.A longer-range 1D-array of QDs was formed by usingthermally tuned SP templates with longer and dispersedfibrous structure. Finally, we revealed continuous FRETbetween arranged QDs on the SP template by analyzing thePL decay curves. Our versatile strategy for efficiently self-Figure 7. (a) Energy diagram of NDI and CsPbBr3 QDs, where FRETand electron transfer (eT) upon excitation of QD are shown.(b) Schematic illustration of an exciton dynamics model among thearranged QDs on the SP template. (c) PL decay curves and(d) magnified curves of the dispersed QDs ([QD]=ca. 1×10� 7 M) andco-aggregates of 1 and QD in CHCl3/MCH (2 :5, v/v). (e) PL decaycurves and (f) magnified curves of dispersed QDs at differentconcentrations ([QD]=ca. 1×10� 7 and 1×10� 6 M) and the film of QD.The excitation wavelength was 470 nm.AngewandteChemieResearch ArticleAngew. Chem. Int. Ed. 2025, 64, e202423912 (7 of 9) © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH 15213773, 2025, 13, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/anie.202423912 by National Institute For, Wiley Online Library on [24/08/2025]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons Licensearranging QDs has the potential to contribute to thecreation of long-range 1D-arranged superstructures of nano-particles, enabling 1D anisotropic exciton and electrontransfer among the assembled nanoparticles.Supporting InformationFull details of synthesis, additional spectra, details of datacollections are available in the Supporting Information.AcknowledgementsThis work was supported by Japan Society for thePromotion of Science (JSPS) KAKENHI Grant NumbersJP22K14556 to M.Y., JP24H01714 (Transformative Re-search Areas “Meso-Hierarchical Materials”) to M.Y.,JP24K01576 to H.H., JP23K26480 to N.A., JP20H00379 toH.Y., JP20H05833 (Transformative Research Areas “Dy-namic Exciton”) to H.Y., JP23K21106 to S.M., andJP23H04875 (Transformative Research Areas “Meso-Hier-archical Materials”) to S.M.. A.M.L. thanks NAIST Graniteprogram and NAIST University Fellowships for the Crea-tion of Innovation in Science and Technology. This workwas partially supported by NAIST-ARIM Program ofMEXT, Japan. The TEM measurements were supported bythe Advanced Research Infrastructure for Materials andNanotechnology (JPMXP1222MS1029) of MEXT, Institutefor Molecular Science, Instrument Center, Okazaki, Japan.We would like to thank Editage (www.editage.jp) forEnglish language editing.Conflict of InterestThe authors declare no conflict of interest.Data Availability StatementThe data that support the findings of this study are availablefrom the corresponding author upon reasonable request.Keywords: perovskite quantum dot · supramolecularchemistry · self-assembly · naphthalenediimide · templatedassembly[1] S. Lee, M.-J. Choi, G. Sharma, M. Biondi, B. Chen, S.-W.Baek, A. M. Najarian, M. Vafaie, J. Wicks, L. K. Sagar, S.Hoogland, F. P. G. de Arquer, O. Voznyy, E. H. 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