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• W3120604977 abstract "•Assembling uniform superstructures at all scales is achieved via transient emulsions•Partial solvent miscibility produces transient emulsion to facilitate templated assembly•Uniform superstructures can be precisely positioned at the desired location•The superstructuring process is controllable, tunable, and generally applicable The assembly of primary particles into uniform superstructures represents a compelling strategy to create new functionalities by utilizing interparticle electromagnetic coupling or other synergistic effects. However, many previous assembly approaches were limited to specific materials or the narrow dimension of the building blocks used or the superstructures produced. This work demonstrates a robust and straightforward assembly strategy to create uniform superstructures at defined positions by introducing primary particles into templating holes via a transient emulsion. This strategy, which applies broadly from nano to bulk scales, is expected to have an immediate impact on the future development of nanotechnology by providing a platform for integrating building blocks of various length scales into novel functioning devices critical to many areas, such as metasurfaces, data storage, drug delivery and release, bio- and chemical sensing, and electro-optical devices. Controllable assembly of molecular and nanoscale building blocks into uniform superstructures up to bulk dimensions remains a key challenge in the next phase of nanotechnology development. Here, we report the self-assembly of superstructures at all scales by taking advantage of the partial miscibility of water and 1-butanol to generate transient aqueous emulsion droplets that can encapsulate the target materials and introduce them into template holes. Further diffusion of water into 1-butanol depletes the emulsion droplets, assembling the building blocks into one well-defined superstructure in each hole. Superstructuring of various types and shapes of nanoparticles, biomolecules, and inorganic compounds could be achieved without the need for surfactants and chemical modifications. The versatility, scalability, low-cost, and accurate positioning are crucial advantages for the future development of advanced precision manufacturing. Controllable assembly of molecular and nanoscale building blocks into uniform superstructures up to bulk dimensions remains a key challenge in the next phase of nanotechnology development. Here, we report the self-assembly of superstructures at all scales by taking advantage of the partial miscibility of water and 1-butanol to generate transient aqueous emulsion droplets that can encapsulate the target materials and introduce them into template holes. Further diffusion of water into 1-butanol depletes the emulsion droplets, assembling the building blocks into one well-defined superstructure in each hole. Superstructuring of various types and shapes of nanoparticles, biomolecules, and inorganic compounds could be achieved without the need for surfactants and chemical modifications. The versatility, scalability, low-cost, and accurate positioning are crucial advantages for the future development of advanced precision manufacturing. The ability to self-assemble individual building blocks into ordered superstructures is a phenomenon known in natural systems (e.g., proteins) to gain new functionalities.1Freeman R. Han M. Álvarez Z. Lewis J.A. Wester J.R. Stephanopoulos N. McClendon M.T. Lynsky C. Godbe J.M. Sangji H. Reversible self-assembly of superstructured networks.Science. 2018; 362: 808-813Crossref PubMed Scopus (138) Google Scholar, 2Huang P. Boyken S.E. Baker D. The coming of age of de novo protein design.Nature. 2016; 537: 320-327Crossref PubMed Scopus (602) Google Scholar, 3King N.P. Bale J.B. Sheffler W. McNamara D.E. Gonen S. Gonen T. Yeates T.O. Baker D. Accurate design of co-assembling multi-component protein nanomaterials.Nature. 2014; 510: 103-108Crossref PubMed Scopus (368) Google Scholar, 4Wang T. Zhuang J. Lynch J. Chen O. Wang Z. Wang X. LaMontagne D. Wu H. Wang Z. Cao Y.C. Self-assembled colloidal superparticles from nanorods.Science. 2012; 338: 358-363Crossref PubMed Scopus (268) Google Scholar, 5Hsia Y. Bale J.B. Gonen S. Shi D. Sheffler W. Fong K.K. Nattermann U. Xu C. Huang P.-S. Ravichandran R. Design of a hyperstable 60-subunit protein icosahedron.Nature. 2016; 535: 136-139Crossref PubMed Scopus (206) Google Scholar Modulating the self-assembly of superstructures in a precise and controlled manner will not only help in realizing their potential applications but also advance the fundamental understanding of self-assembly in nature.6Jones M.R. Seeman N.C. Mirkin C.A. Programmable materials and the nature of the DNA bond.Science. 2015; 347: 1260901Crossref PubMed Scopus (813) Google Scholar, 7Kotov N.A. Particle self-assembly: superstructures simplified.Nat. Nanotechnol. 2016; 11: 1002Crossref PubMed Scopus (8) Google Scholar, 8Nagaoka Y. Tan R. Li R. Zhu H. Eggert D. Wu Y.A. Liu Y. Wang Z. Chen O. Superstructures generated from truncated tetrahedral quantum dots.Nature. 2018; 561: 378-382Crossref PubMed Scopus (88) Google Scholar, 9Lin H. Lee S. Sun L. Spellings M. Engel M. Glotzer S.C. Mirkin C.A. 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Hovden R. Jiang Y. Riccio M. Muller D.A. Elser V. Estroff L.A. Hierarchical porous polymer scaffolds from block copolymers.Science. 2013; 341: 530-534Crossref PubMed Scopus (207) Google Scholar, 15Peinemann K.-V. Abetz V. Simon P.F. Asymmetric superstructure formed in a block copolymer via phase separation.Nat. Mater. 2007; 6: 992-996Crossref PubMed Scopus (557) Google Scholar Despite recent developments, creating a universal, scalable, and robust self-assembly method of superstructures at scales ranging from nano- to macroscopic lengths remain elusive. Current approaches are usually size limited,4Wang T. Zhuang J. Lynch J. Chen O. Wang Z. Wang X. LaMontagne D. Wu H. Wang Z. Cao Y.C. Self-assembled colloidal superparticles from nanorods.Science. 2012; 338: 358-363Crossref PubMed Scopus (268) Google Scholar,16Wasio N.A. Quardokus R.C. Forrest R.P. Lent C.S. Corcelli S.A. Christie J.A. Henderson K.W. Kandel S.A. Self-assembly of hydrogen-bonded two-dimensional quasicrystals.Nature. 2014; 507: 86-89Crossref PubMed Scopus (156) Google Scholar, 17Li P. Vermeulen N.A. Malliakas C.D. Gómez-Gualdrón D.A. Howarth A.J. Mehdi B.L. Dohnalkova A. Browning N.D. O’Keeffe M. Farha O.K. Bottom-up construction of a superstructure in a porous uranium-organic crystal.Science. 2017; 356: 624-627Crossref PubMed Scopus (198) Google Scholar, 18Lee S.Y. Gradon L. Janeczko S. Iskandar F. Okuyama K. Formation of highly ordered nanostructures by drying micrometer colloidal droplets.ACS Nano. 2010; 4: 4717-4724Crossref PubMed Scopus (92) Google Scholar require chemical modifications of building blocks and tedious fabrication procedures,19Chou L.Y. Zagorovsky K. Chan W.C. DNA assembly of nanoparticle superstructures for controlled biological delivery and elimination.Nat. Nanotechnol. 2014; 9: 148Crossref PubMed Scopus (329) Google Scholar, 20Gerling T. Wagenbauer K.F. Neuner A.M. Dietz H. Dynamic DNA devices and assemblies formed by shape-complementary, non–base pairing 3D components.Science. 2015; 347: 1446-1452Crossref PubMed Scopus (350) Google Scholar, 21Lin Q. Mason J.A. Li Z. Zhou W. O’Brien M.N. Brown K.A. Jones M.R. Butun S. Lee B. Dravid V.P. Building superlattices from individual nanoparticles via template-confined DNA-mediated assembly.Science. 2018; 359: 669-672Crossref PubMed Scopus (119) Google Scholar, 22Macfarlane R.J. Lee B. Jones M.R. Harris N. Schatz G.C. Mirkin C.A. Nanoparticle superlattice engineering with DNA.Science. 2011; 334: 204-208Crossref PubMed Scopus (814) Google Scholar, 23Zhang Y. Lu F. Yager K.G. Van Der Lelie D. Gang O. A general strategy for the DNA-mediated self-assembly of functional nanoparticles into heterogeneous systems.Nat. Nanotechnol. 2013; 8: 865Crossref PubMed Scopus (222) Google Scholar, 24Guo J. Tardy B.L. Christofferson A.J. Dai Y. Richardson J.J. Zhu W. Hu M. Ju Y. Cui J. Dagastine R.R. Modular assembly of superstructures from polyphenol-functionalized building blocks.Nat. Nanotechnol. 2016; 11: 1105Crossref PubMed Scopus (218) Google Scholar, 25Lu F. Yager K.G. Zhang Y. Xin H. Gang O. Superlattices assembled through shape-induced directional binding.Nat. Commun. 2015; 6: 1-10Crossref Scopus (157) Google Scholar, 26Utgenannt A. Maspero R. Fortini A. Turner R. Florescu M. Jeynes C. Kanaras A.G. Muskens O.L. Sear R.P. Keddie J.L. Fast assembly of gold nanoparticles in large-area 2D nanogrids using a one-step, near-infrared radiation-assisted evaporation process.ACS Nano. 2016; 10: 2232-2242Crossref PubMed Scopus (34) Google Scholar and significantly differ based on the utilized building blocks.10Talapin D.V. Shevchenko E.V. Bodnarchuk M.I. Ye X. Chen J. Murray C.B. Quasicrystalline order in self-assembled binary nanoparticle superlattices.Nature. 2009; 461: 964-967Crossref PubMed Scopus (453) Google Scholar,27Yang Y. Wang B. Shen X. Yao L. Wang L. Chen X. Xie S. Li T. Hu J. Yang D. Scalable assembly of crystalline binary nanocrystal superparticles and their enhanced magnetic and electrochemical properties.J. Am. Chem. Soc. 2018; 140: 15038-15047Crossref PubMed Scopus (48) Google Scholar, 28Nagaoka Y. Zhu H. Eggert D. Chen O. Single-component quasicrystalline nanocrystal superlattices through flexible polygon tiling rule.Science. 2018; 362: 1396-1400Crossref PubMed Scopus (44) Google Scholar, 29Utgenannt A. Keddie J.L. Muskens O.L. Kanaras A.G. Directed organization of gold nanoparticles in polymer coatings through infrared-assisted evaporative lithography.Chem. Commun. 2013; 49: 4253-4255Crossref PubMed Google Scholar Emulsion-based self-assembly strategies are ideal for superstructuring because of their simplicity and unnecessity of chemical modifications.30Dinsmore A. Hsu M.F. Nikolaides M. Marquez M. Bausch A. Weitz D. Colloidosomes: selectively permeable capsules composed of colloidal particles.Science. 2002; 298: 1006-1009Crossref PubMed Scopus (1761) Google Scholar, 31Velev O. Furusawa K. Nagayama K. Assembly of latex particles by using emulsion droplets as templates. 1. Microstructured hollow spheres.Langmuir. 1996; 12: 2374-2384Crossref Scopus (549) Google Scholar, 32Liu D. Zhou F. Li C. Zhang T. Zhang H. Cai W. Li Y. Black gold: plasmonic colloidosomes with broadband absorption self-assembled from monodispersed gold nanospheres by using a reverse emulsion system.Angew. Chem. Int. Ed. 2015; 54: 9596-9600Crossref PubMed Scopus (139) Google Scholar, 33Fan W. Yan B. Wang Z. Wu L. Three-dimensional all-dielectric metamaterial solid immersion lens for subwavelength imaging at visible frequencies.Sci. Adv. 2016; 2: e1600901Crossref PubMed Scopus (96) Google Scholar However, their long-standing disadvantages comprise a polydisperse size distribution of emulsion droplets caused by using emulsifiers (e.g., surfactants) and the difficulty to accurately position them because of their unfixed fluid properties, which overall hinder the control of size, uniformity, and applications of the self-assembled superstructures. Here, we present the emulsion-based template-assisted self-assembly of superstructures unrestricted to the nature of the building blocks. We tackle the problem of distribution and positioning of emulsion droplets by using uniform holes patterned on a template film as a collective and size-controllable platform for superstructures. This emulsion strategy allowed the superstructuring of various shapes and types of building blocks at all scales without the need for any additional surfactants to the system. Figure 1A presents a schematic diagram of the superstructuring strategy based on the template-assisted emulsion approach. A honeycomb microhole array polystyrene (PS) film fabricated using a breath figure technique is used as a typical template in this study34Zhang A. Bai H. Li L. Breath figure: a nature-inspired preparation method for ordered porous films.Chem. Rev. 2015; 115: 9801-9868Crossref PubMed Scopus (267) Google Scholar,35Zhu C. Tian L. Liao J. Zhang X. Gu Z. Fabrication of bioinspired hierarchical functional structures by using honeycomb films as templates.Adv. Funct. Mater. 2018; 28: 1803194Crossref Scopus (19) Google Scholar; the strategy also works in holes fabricated using lithography or other methods. These films are composed of monodisperse, quasi-spherical, but top-opening microholes (approximately 10 μm in diameter) in a hexagonal close-packed arrangement of at least 1 cm in length (Figure S1). In principle, to deposit objects from the dispersion into the holes, the solvent needs to wet the template surface so that the dispersion can spread over and fill the holes, which, however, leads to random deposition of the objects all over the template surface (as shown in Figures S2A and S2B, by sweeping an aqueous dispersion of SiO2 nanoparticles over a hydrophilic surface). In contrast, if the dispersed phase conveys an opposing wettability to the template surface, it cannot reach into the holes occupied by air (Figures S2C and S2D), which is known as the Cassie-Baxter wetting model.36Cassie A. Baxter S. Wettability of porous surfaces.Trans. Faraday Soc. 1944; 40: 546-551Crossref Scopus (10230) Google Scholar Neither approach can achieve selective deposition/assembly only in the microholes. We addressed this issue by using a partially miscible system in the self-assembly process. The honeycomb microhole array with a hydrophobic surface is first wetted with 1-butanol to fill the microholes (Figure 1A). An aqueous solution is then dropped onto the film trapping the 1-butanol inside the microholes. Since 1-butanol is partially miscible in water, these trapped 1-butanol phases can diffuse into the water phase leading to a phase exchange in the microholes. After filling these microholes with water, a large volume of pure 1-butanol solvent is used to sweep the water surplus from the template surface, which simultaneously emulsifies the water into small emulsion droplets confined within the microholes. The resulting droplets are highly uniform and size-controllable by controlling the distribution of hole sizes. They gradually shrink as water diffuses into the 1-butanol phase. If building blocks (e.g., nanostructures, biological systems, or ions) of a proper concentration are pre-dispersed in the water phase, they will assemble into uniform superstructures (e.g., colloidosomes, biological structures, and crystals) within the template holes. The operating process is shown in Video S1. https://www.cell.com/cms/asset/2f6982dd-b87c-4c82-8e89-279f83529b99/mmc2.mp4Loading ... Download .mp4 (10.67 MB) Help with .mp4 files Video S1. The whole operation procedure of the template-assisted emulsion strategy Figure 1B schematically shows the template-assisted emulsion self-assembly of an example of nanoparticles that superstructured into colloidosomes. When a water droplet containing the nanoparticles is emulsified inside the microhole, the water/1-butanol (W/O) interface shrinks inward as the water phase diffuse into the 1-butanol phase. During this shrinking process, the water droplet maintains a quasi-spherical shape tangent to the inner wall of the microhole due to the hydrophobic property of the film, reaching a dynamic balance on the substrate. Meanwhile, the nanoparticles in the water droplet tend to spontaneously accumulate and self-assemble at the water/1-butanol interface, driven by the principle of minimum free energy at the interface.32Liu D. Zhou F. Li C. Zhang T. Zhang H. Cai W. Li Y. Black gold: plasmonic colloidosomes with broadband absorption self-assembled from monodispersed gold nanospheres by using a reverse emulsion system.Angew. Chem. Int. Ed. 2015; 54: 9596-9600Crossref PubMed Scopus (139) Google Scholar,37Velev O. Nagayama K. Assembly of latex particles by using emulsion droplets. 3. Reverse (water in oil) system.Langmuir. 1997; 13: 1856-1859Crossref Scopus (138) Google Scholar The adsorbed nanoparticles are forced to closely pack in the interface as the water/liquid interface continues to collapse. A superstructured particle begins to form when the nanoparticles occupy the entire droplet surface. Quasi-spherical and well-ordered colloidosomes will ultimately form after the complete diffusion of the water droplet into the 1-butanol phase. To validate this working principle, the diffusion process of the water droplets into 1-butanol was directly recorded under an optical microscope (Figure 1C; Video S2). The water droplets were observed to quickly shrink in the 1-butanol phase as the 1-butanol solvent swept over the film until they completely vanished in less than 3.10 s (as indicated by the yellow dashed circle in Figure 1C). These results clearly support the above-mentioned mechanism of template-assisted emulsion self-assembly. https://www.cell.com/cms/asset/471dcb04-ec24-4df7-9930-7e35823e46e9/mmc3.mp4Loading ... Download .mp4 (2.59 MB) Help with .mp4 files Video S2. The observation of water diffusion from a microhole into 1-butanol using an optical microscope The assembly of monodisperse SiO2 nanoparticles (220 ± 16.7 nm in diameter) into superstructured colloidosomes was used as a model system to obtain more insights on the template-assisted emulsion self-assembly. Figures 2A and 2B show the typical SEM images of the SiO2 colloidosomes assembled inside a microhole array film. No free SiO2 nanoparticles were found on the film surface, where a large number of uniform colloidosomes were well positioned inside the microholes with a yield reaching 99%. Oxygen plasma treatment was performed to remove the top layer of the PS film to obtain a clear view of the colloidosomes (Figure 2C). The colloidosomes were found in a tangent contact with the interior wall of the microholes, as further confirmed in a cross-sectional image (Figure 2D). The colloidosomes can be easily collected by complete removal of the template (Figure 2E). Interestingly, the uniform colloidosomes have a blue colored appearance, as revealed in their dark-field optical image (Figure 2E), which is ascribed to the optical diffraction of the well-ordered arrangement of SiO2 nanoparticles in the colloidosomes (Figures 2F and 2G). The colloidosomes demonstrate a monodisperse size distribution with an average diameter of 4.3 ± 0.23 μm (Figures 2H and S3). Each colloidosome consists of SiO2 nanoparticles in a hexagonally ordered closely packed arrangement. This emulsion-based superstructuring strategy allows precise control of the size and uniformity of superstructures, and it can be applied to the assembly of building blocks of a wide range of compositions and sizes. The size of the superstructured SiO2 colloidosomes can be controlled by two main parameters: template size and concentration of nanoparticles in the solution. These two parameters are directly correlated. For example, Figures 3A and 3B depict the relationship between the size of the SiO2 colloidosomes and the concentrations of the microholes and nanoparticles, respectively. When the concentration of the nanoparticles is fixed, the diameter of the colloidosomes increases with increasing microhole size, as measured from the SEM results presented in Figure S4 and summarized in Figure 3A. Similarly, increasing the nanoparticle concentration while fixing the microhole size led to an increase in the size of the colloidosomes (Figures 3B and S5). In addition, temperature has a negligible effect on the size and morphology of the assembled superstructures (Figure S6). Figure 3C shows three different sizes of typical SiO2 colloidosomes after removal of the template by heating at 450°C for 3 h. Moreover, Figures 3D and 3E show the superstructuring of nanoparticles on 5-mm and 500-nm hole array films, respectively. The SiO2 colloidosomes assembled in the 5-mm holes achieved diameters of approximately 1.43 mm. The red diffraction observed indicates a highly ordered arrangement of SiO2 nanoparticles in these colloidosomes (Figures 3D and S7). In contrast, colloidosomes assembled from Fe3O4 nanoparticles (approximately 10 nm) in 500-nm holes display an average size of approximately 170 nm (Figure 3E). These results indicate that the template-assisted emulsion self-assembly strategy applies to all scales and can be used to prepare superstructures with sizes ranging from nanometers to millimeters by directly controlling the size of the templates and the concentration of the building blocks. As well as the honeycomb hole array film, the template-assisted self-assembly method is also suitable for various shapes of hole array films, such as cylindrical (Figures 3F and S8), cylindrical dimer (Figures 3G and S9), inverted pyramid (Figures 3H and S10), and even irregularly shaped holes (Figure S11). Despite their significant differences in morphology and periodicity, similar quasi-spherical SiO2 colloidosomes have been successfully assembled in all microhole array films. Almost all of the assembled colloidosomes were preferentially deposited at the inner boundaries of the microhole walls to reduce their surface energies effectively (Figures 3F–3H). For example, the superstructured colloidosomes are deposited at the bottom tip of the inverted pyramid holes where the lowest potential energy is attained (Figure 3H). These results demonstrate an effective strategy for preferentially depositing the superstructures into targeted positions, which only requires pre-designing the hole arrays. Further complexation of the superstructure shape can be achieved by introducing magnetic nanoparticles into the self-assembly system. The transition from quasi-spherical to ellipsoidal superstructures can be achieved by assembling magnetic Fe3O4 nanoparticles in an external magnetic field with increasing field strength, as shown in Figure 4A. Elongation of the superstructures is driven by the assembly of magnetic nanoparticles into one-dimensional (1D) chains along the field direction inside the emulsion droplets, with a larger aspect ratio (L/D, length to diameter) in a stronger field (Figure 4A). These 1D chains of magnetic nanoparticles are then tightly packed into an anisotropic ellipsoidal structure as the emulsion droplet collapses. Moreover, when released from the template and re-dispersed in 1-butanol, these ellipsoidal colloidosomes remain structurally stable and can be further aligned into a series of 1D long and head-to-tail chains along the magnetic field (Figures 4B and S12). Figure 4C depicts the relationship between the aspect ratio of the ellipsoidal colloidosomes and the intensity of the applied magnetic field. The aspect ratio increases slightly at the initial stage before ascending rapidly with increased magnetic field intensity. In contrast, when the intensity of the magnetic field is much higher, the increase of aspect ratio slows owing to the concentration of the local nanoparticles reaching a saturated balance in the finite space of the microholes. The combination of magnetic and non-magnetic nanoparticles offers an opportunity to further alter the superstructures from an ellipsoid to a tumbler-like shape. Figures 4D and 4E show the typical tumbler-like superstructures from a mixture of Fe3O4 nanoparticles (115 ± 27 nm) and SiO2 nanoparticles (220 ± 16.7 nm) assembled under a magnetic field. The tumbler-like colloidosomes consist of an anisotropic bundle of Fe3O4 nanoparticles as the inner core and SiO2 nanoparticles as the outer shell (artificially colored in Figure 4E), with their aspect ratio being determined by the relative concentration of the two building blocks after their assembly. Figures S13 and S14 demonstrate the evolution of the shapes of the tumbler-like colloidosomes by tuning the applied magnetic field intensity and the initial aqueous concentration ratio of Fe3O4 to polydopamine (PDA) nanoparticles, respectively. We used PDA instead of SiO2 nanoparticles in this case because of their convenient removal through calcination in air, which allows the observation of the structure of the inner Fe3O4 core. The monotonic increase of the intensity of the magnetic field or the original concentration ratio of Fe3O4 to PDA nanoparticles generated a shape change from a “plump” to a “slim” tumbler-like superstructure, caused by the dynamical increase of the relative nanoparticle concentration ratio of Fe3O4 to PDA. The overall self-assembly mechanism of the tumbler-like superstructures is depicted in Figure 4F. When an emulsion droplet containing non-magnetic and magnetic nanoparticles is introduced into the microhole, the two types of nanoparticles exhibit different assembly behaviors. The magnetic ones tend to align along the external magnetic field, and the non-magnetic ones are pushed to the droplet surface spontaneously to reduce the total free energy of the system. These two different responses prompt the phase separation of the two mixed nanoparticles inside the emulsion droplet. As the droplet contracts, the nearby 1D chains of the magnetic nanoparticles gradually assemble to form a standing bundle-like structure driven by the magnetic force. Meanwhile, the non-magnetic nanoparticles gather along with the direction of the shrinking droplet. Since the droplet maintains its dynamic balance at the bottom of the microhole wall, the top part of the standing bundle starts to penetrate into the 1-butanol phase as the interface diminishes, while the non-magnetic nanoparticles gradually gather at the bottom part of the standing bundle. These accumulated non-magnetic nanoparticles continue to assemble into an ordered shell while embodying the chain bundle. The template-assisted emulsion technique demonstrates excellent practicality for superstructuring various types and shapes of building blocks without any previous modifications or emulsifiers. For instance, Au nanoparticles, PDA nanoparticles, FeOOH nanorods, Fe2O3 nanodiscs (Figure 5A), and CdTe quantum dots (Figure S15), have all been assembled into uniform colloidosomes using the same approach. In addition, biopolymer molecules (e.g., chitosan, casein proteins, fish sperm DNA, and live micrococcus cells) have also been self-assembled into unique superstructures using the same approach (Figures 5B, S16, and S17). The self-assembly of biological systems (i.e., living cells) with high uniformity and yields exemplifies the potentials of the technique for numerous biological applications, including cell culture technology,38Lecault V. VanInsberghe M. Sekulovic S. Knapp D.J. Wohrer S. Bowden W. Viel F. McLaughlin T. Jarandehei A. Miller M. High-throughput analysis of single hematopoietic stem cell proliferation in microfluidic cell culture arrays.Nat. Methods. 2011; 8: 581Crossref PubMed Scopus (241) Google Scholar drugs and vaccine development,5Hsia Y. Bale J.B. Gonen S. Shi D. Sheffler W. Fong K.K. Nattermann U. Xu C. Huang P.-S. Ravichandran R. Design of a hyperstable 60-subunit protein icosahedron.Nature. 2016; 535: 136-139Crossref PubMed Scopus (206) Google Scholar and cell and gene engineering.1Freeman R. Han M. Álvarez Z. Lewis J.A. Wester J.R. Stephanopoulos N. McClendon M.T. Lynsky C. Godbe J.M. Sangji H. Reversible self-assembly of superstructured networks.Science. 2018; 362: 808-813Crossref PubMed Scopus (138) Google Scholar,19Chou L.Y. Zagorovsky K. Chan W.C. DNA assembly of nanoparticle superstructures for controlled biological delivery and elimination.Nat. Nanotechnol. 2014; 9: 148Crossref PubMed Scopus (329) Google Scholar Moreover, this superstructuring strategy is not limited to the self-assembly of nanostructures or polymeric molecules but can also be applied to the crystallization of ionic compounds in the confined space provided by the template. Figure 5C shows the growth of “cube-like” microcrystals of NaCl, “rice-like” microcrystals of Na2SO3, and “flower-like” microcrystals of Na2SO4, which represent the cubic, monoclinic, and orthorhombic lattice systems, respectively. Their corresponding low-magnification images containing multiple microcrystals are shown in Figures S18–S20. The multi-grain superstructures in the cases of Na2SO3 and Na2SO4 are believed to be associated with their anisotropic crystal lattices and multiple nucleation and merging events during their growth. According to the Young-Laplace law, the Laplace pressure inside an emulsion droplet is determined by the interfacial surface tension of the droplet divided by its radius.39Berthier J. Brakke K.A. The Physics of Microdroplets. John Wiley & Sons, 2012Crossref Scopus (124) Google Scholar As water and 1-butanol display a partially miscible system, the inter" @default.
• W3120604977 created "2021-01-18" @default.
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• W3120604977 date "2021-03-01" @default.
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• W3120604977 title "Self-assembly of superstructures at all scales" @default.
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